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<front>
<journal-meta>
<journal-id journal-id-type="publisher-id">Front. Mar. Sci.</journal-id>
<journal-title>Frontiers in Marine Science</journal-title>
<abbrev-journal-title abbrev-type="pubmed">Front. Mar. Sci.</abbrev-journal-title>
<issn pub-type="epub">2296-7745</issn>
<publisher>
<publisher-name>Frontiers Media S.A.</publisher-name>
</publisher>
</journal-meta>
<article-meta>
<article-id pub-id-type="doi">10.3389/fmars.2024.1304193</article-id>
<article-categories>
<subj-group subj-group-type="heading">
<subject>Marine Science</subject>
<subj-group>
<subject>Original Research</subject>
</subj-group>
</subj-group>
</article-categories>
<title-group>
<article-title>Modulation of regional carbon uptake by AMOC and alkalinity changes in the subpolar North Atlantic under a warming climate</article-title>
</title-group>
<contrib-group>
<contrib contrib-type="author" corresp="yes">
<name>
<surname>Zhang</surname>
<given-names>Qi</given-names>
</name>
<xref ref-type="author-notes" rid="fn001">
<sup>*</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/1740161"/>
<role content-type="https://credit.niso.org/contributor-roles/conceptualization/"/>
<role content-type="https://credit.niso.org/contributor-roles/data-curation/"/>
<role content-type="https://credit.niso.org/contributor-roles/software/"/>
<role content-type="https://credit.niso.org/contributor-roles/validation/"/>
<role content-type="https://credit.niso.org/contributor-roles/visualization/"/>
<role content-type="https://credit.niso.org/contributor-roles/writing-original-draft/"/>
<role content-type="https://credit.niso.org/contributor-roles/writing-review-editing/"/>
<role content-type="https://credit.niso.org/contributor-roles/methodology/"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Ito</surname>
<given-names>Takamitsu</given-names>
</name>
<uri xlink:href="https://loop.frontiersin.org/people/1405378"/>
<role content-type="https://credit.niso.org/contributor-roles/conceptualization/"/>
<role content-type="https://credit.niso.org/contributor-roles/formal-analysis/"/>
<role content-type="https://credit.niso.org/contributor-roles/funding-acquisition/"/>
<role content-type="https://credit.niso.org/contributor-roles/methodology/"/>
<role content-type="https://credit.niso.org/contributor-roles/software/"/>
<role content-type="https://credit.niso.org/contributor-roles/supervision/"/>
<role content-type="https://credit.niso.org/contributor-roles/validation/"/>
<role content-type="https://credit.niso.org/contributor-roles/writing-review-editing/"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Bracco</surname>
<given-names>Annalisa</given-names>
</name>
<uri xlink:href="https://loop.frontiersin.org/people/290125"/>
<role content-type="https://credit.niso.org/contributor-roles/conceptualization/"/>
<role content-type="https://credit.niso.org/contributor-roles/formal-analysis/"/>
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<role content-type="https://credit.niso.org/contributor-roles/writing-review-editing/"/>
</contrib>
</contrib-group>
<aff id="aff1">
<institution>Earth and Atmospheric Sciences, Georgia Institute of Technology</institution>, <addr-line>Atlanta, GA</addr-line>, <country>United States</country>
</aff>
<author-notes>
<fn fn-type="edited-by">
<p>Edited by: Matthias Gr&#xf6;ger, Leibniz Institute for Baltic Sea Research (LG), Germany</p>
</fn>
<fn fn-type="edited-by">
<p>Reviewed by: J&#xf6;rg Schwinger, Bjerknes Centre for Climate Research, Norway</p>
<p>Jinlin Liu, Tongji University, China</p>
</fn>
<fn fn-type="corresp" id="fn001">
<p>*Correspondence: Qi Zhang, <email xlink:href="mailto:qzhang459@gatech.edu">qzhang459@gatech.edu</email>
</p>
</fn>
</author-notes>
<pub-date pub-type="epub">
<day>08</day>
<month>04</month>
<year>2024</year>
</pub-date>
<pub-date pub-type="collection">
<year>2024</year>
</pub-date>
<volume>11</volume>
<elocation-id>1304193</elocation-id>
<history>
<date date-type="received">
<day>29</day>
<month>09</month>
<year>2023</year>
</date>
<date date-type="accepted">
<day>25</day>
<month>03</month>
<year>2024</year>
</date>
</history>
<permissions>
<copyright-statement>Copyright &#xa9; 2024 Zhang, Ito and Bracco</copyright-statement>
<copyright-year>2024</copyright-year>
<copyright-holder>Zhang, Ito and Bracco</copyright-holder>
<license xlink:href="http://creativecommons.org/licenses/by/4.0/">
<p>This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.</p>
</license>
</permissions>
<abstract>
<p>The slowdown of the Atlantic Meridional Overturning Circulation (AMOC) and associated consequences on ocean carbon uptake could have large implications for the Earth's climate system and its global carbon cycle. This study analyzes ten Earth System Models from the Coupled Model Intercomparison Project Phase 6 (CMIP6) and reveals that the regional carbon uptake in the subpolar North Atlantic under a high CO<sub>2</sub> emission scenario moderately correlates with the decline in AMOC at 40&#xb0;N. AMOC transports warm and salty subtropical waters to the subpolar regions. Models with stronger AMOC slowdown generally exhibit weaker surface warming and larger decline of surface salinity and alkalinity. We consider two plausible mechanisms linking the AMOC slowdown to the decline of regional CO<sub>2</sub> uptake: the reduction in surface alkalinity and diminished subduction. The decline of surface salinity and alkalinity reduces the ocean's capacity to buffer acids leading to a reduced CO<sub>2</sub> uptake. This important contribution is unique to the North Atlantic. Diminished convective mixing and subduction of surface water can further decrease the downward transport of anthropogenic carbon, as also shown in previous research. The centennial trends of <italic>p</italic>CO<sub>2</sub> are decomposed into four components driven by temperature, salinity, alkalinity and dissolved inorganic carbon, revealing that alkalinity and dissolved inorganic carbon are both significant contributors. The alkalinity-driven <italic>p</italic>CO<sub>2</sub> essentially follows surface salinity, establishing the linkage between AMOC slowdown and alkalinity decline. Our results indicate that alkalinity changes are important for the interplay between AMOC and the regional carbon sequestration ability across the late 20<sup>th</sup> and the entirety of the 21<sup>st</sup> century in the subpolar North Atlantic.</p>
</abstract>
<kwd-group>
<kwd>AMOC</kwd>
<kwd>alkalinity</kwd>
<kwd>carbon uptake</kwd>
<kwd>CMIP6</kwd>
<kwd>climate change</kwd>
<kwd>subpolar North Atlantic</kwd>
</kwd-group>
<counts>
<fig-count count="7"/>
<table-count count="2"/>
<equation-count count="2"/>
<ref-count count="103"/>
<page-count count="14"/>
<word-count count="7589"/>
</counts>
<custom-meta-wrap>
<custom-meta>
<meta-name>section-in-acceptance</meta-name>
<meta-value>Global Change and the Future Ocean</meta-value>
</custom-meta>
</custom-meta-wrap>
</article-meta>
</front>
<body>
<sec id="s1" sec-type="intro">
<label>1</label>
<title>Introduction</title>
<p>The Atlantic Meridional Overturning Circulation (AMOC) plays a significant role in the climate system, by transporting oceanic heat northward from the South Atlantic to the North Atlantic (<xref ref-type="bibr" rid="B91">Trenberth et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B95">Weijer et&#xa0;al., 2020</xref>). It also transports heat and carbon from the surface to the deep ocean in the North Atlantic and helps redistribute ocean heat vertically (<xref ref-type="bibr" rid="B43">Kostov et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B8">Buckley and Marshall, 2016</xref>; <xref ref-type="bibr" rid="B7">Bronselaer and Zanna, 2020</xref>). Its contribution is key to the ocean&#x2019;s ability to absorb the excess heat and carbon from greenhouse gas emissions and its evolution will be fundamental to the overall response of the climate system moving forward (<xref ref-type="bibr" rid="B3">Bellomo et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B75">Schwinger et&#xa0;al., 2022</xref>). The analysis of both observational and modeling datasets suggests that AMOC may have weakened after the 1980s (<xref ref-type="bibr" rid="B57">Menary et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B102">Zhu et&#xa0;al., 2023</xref>), and models indicate that it will further decline in the future (<xref ref-type="bibr" rid="B19">Drijfhout, 2015</xref>; <xref ref-type="bibr" rid="B9">Caesar et&#xa0;al., 2018</xref>; <xref ref-type="bibr" rid="B44">Latif et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B48">Liu et&#xa0;al., 2020</xref>). The AMOC weakening impacts regional and global climate by changing surface temperature, precipitation patterns and teleconnections (<xref ref-type="bibr" rid="B3">Bellomo et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B61">Orihuela-Pinto et&#xa0;al., 2022</xref>). While a reduction in the AMOC may have mitigated the rate of historical global warming (<xref ref-type="bibr" rid="B4">Bonnet et&#xa0;al., 2021</xref>), it also modifies the distribution of heat within the climate system, potentially retaining excess heat in the tropical South Atlantic (<xref ref-type="bibr" rid="B61">Orihuela-Pinto et&#xa0;al., 2022</xref>). This underscores the intricate role of the AMOC in the Earth&#x2019;s climate system and its potential influence on climate tipping points. Under greenhouse gas (GHG) forcing, the weakening of the AMOC can be caused by a combination of surface warming and increasing freshwater fluxes at high latitudes, both contributing towards increasing stratification in the upper ocean (<xref ref-type="bibr" rid="B88">Thorpe et&#xa0;al., 2001</xref>; <xref ref-type="bibr" rid="B83">Stouffer et&#xa0;al., 2006</xref>; <xref ref-type="bibr" rid="B52">Marshall et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B8">Buckley and Marshall, 2016</xref>; <xref ref-type="bibr" rid="B98">Yang et&#xa0;al., 2016</xref>) which can suppress deep convection (<xref ref-type="bibr" rid="B100">Zhang, 2010</xref>). In observational reanalyses, however, the trend in AMOC was positive between the 1960s and 1975 (<xref ref-type="bibr" rid="B1">Balmaseda et&#xa0;al., 2013</xref>) likely due to the increase in anthropogenic aerosol forcing which counteracted the effect of GHGs (<xref ref-type="bibr" rid="B10">Cai et&#xa0;al., 2006</xref>; <xref ref-type="bibr" rid="B17">Delworth and Dixon, 2006</xref>; <xref ref-type="bibr" rid="B31">Hassan et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B71">Robson et&#xa0;al., 2022</xref>). As a note of caution, the attribution of AMOC changes remains subject to intense scrutiny and conclusive statements are hard to make given the underestimation of decadal-scale variability by climate models (<xref ref-type="bibr" rid="B97">Yan et&#xa0;al., 2018</xref>) and the short time-span of the direct observational records (<xref ref-type="bibr" rid="B8">Buckley and Marshall, 2016</xref>).</p>
<p>Changes in sea surface temperature (SST) and sea surface salinity (SSS) in the North Atlantic are linked to fluctuations in AMOC (<xref ref-type="bibr" rid="B18">Deser et&#xa0;al., 2010</xref>; <xref ref-type="bibr" rid="B21">Estella-Perez et&#xa0;al., 2020</xref>). Carbon uptake, on the other hand, is primarily driven by the rate of increase in the atmospheric CO<sub>2</sub> levels, thus depends on the trajectory of anthropogenic carbon emission. A significant fraction of anthropogenic CO<sub>2</sub> emissions is absorbed by oceans, increasing the concentrations of dissolved inorganic carbon (DIC) and thus causing acidification (<xref ref-type="bibr" rid="B65">Perez et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B36">Jiang et&#xa0;al., 2023</xref>; <xref ref-type="bibr" rid="B50">Ma et&#xa0;al., 2023</xref>). The increase in DIC affects the ability of the ocean to continue absorbing CO<sub>2</sub> from the atmosphere, as the ocean becomes more saturated with CO<sub>2</sub> (<xref ref-type="bibr" rid="B46">Le Qu&#xe9;r&#xe9; et&#xa0;al., 2007</xref>; <xref ref-type="bibr" rid="B40">Keppler et&#xa0;al., 2023</xref>). AMOC contributes to the vertical transport of DIC from the surface to interior ocean, which modulates the air-sea difference in partial pressure of CO<sub>2</sub> (<italic>p</italic>CO<sub>2</sub>) (<xref ref-type="bibr" rid="B69">Riebesell et&#xa0;al., 2009</xref>; <xref ref-type="bibr" rid="B6">Brix et&#xa0;al., 2013</xref>; <xref ref-type="bibr" rid="B90">Tjiputra et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B27">Goris et&#xa0;al., 2018</xref>). <xref ref-type="bibr" rid="B27">Goris et&#xa0;al. (2018)</xref> found that simulated anthropogenic carbon uptake in the North Atlantic is significantly correlated to seasonal <italic>p</italic>CO<sub>2</sub> amplitude, reflecting the role of vertical DIC transport and deep mixing (<xref ref-type="bibr" rid="B16">DeGrandpre et&#xa0;al., 2006</xref>) in the sequestration of anthropogenic carbon. Using this correlation, they were able to constrain the regional carbon uptake from the 1990s to 2100. However, the application of this approach to constrain future North Atlantic carbon uptake included large uncertainties by 2100 (<xref ref-type="bibr" rid="B26">Goris et&#xa0;al., 2023</xref>). Using model selection based on observational constraints of AMOC, previous studies narrow down the projected spread in ocean carbon uptake by CMIP5/CMIP6 models for the 21<sup>st</sup> century, leading to an increased and more precise projection of the global ocean&#x2019;s carbon uptake and acidification over the 21<sup>st</sup> century&#x200b;&#x200b; (<xref ref-type="bibr" rid="B93">Wang et&#xa0;al., 2016</xref>; <xref ref-type="bibr" rid="B87">Terhaar et&#xa0;al., 2022</xref>).</p>
<p>There are other factors that modulate the surface ocean <italic>p</italic>CO<sub>2</sub> and regional carbon uptake such as SST and alkalinity (ALK). Earlier work suggested that the weakening of AMOC can cause a decrease in ocean carbon uptake due to the reduced biological activity and altered ventilation (<xref ref-type="bibr" rid="B73">Schmittner and Galbraith, 2008</xref>; <xref ref-type="bibr" rid="B59">Nielsen et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B38">Katavouta and Williams, 2021</xref>). Moreover, alkalinity&#x2019;s role in CO<sub>2</sub> uptake and its contribution to the long-term buffering capacity of oceans have been highlighted in recent studies (<xref ref-type="bibr" rid="B86">Takahashi et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B58">Middelburg et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B13">Chikamoto et&#xa0;al., 2023</xref>). A decrease in ocean ALK negatively impacts the ocean&#x2019;s capacity to absorb CO<sub>2</sub>, thereby affecting its role as a carbon sink. The reduction of surface ALK accelerates the acidification of seawater, which in turn affects the marine ecosystem. The amount of CO<sub>2</sub> uptake reduction contributed by the above processes, however, remains highly uncertain.</p>
<p>In this study, we investigate the sources of this carbon uptake uncertainty focusing on the subpolar North Atlantic using simulations from the Coupled Model Intercomparison Project Phase 6 (CMIP6). Model outputs for various physical and biogeochemical variables are examined in their relationships with AMOC in the historical period as well as in future scenarios. Regarding AMOC, several studies examined how its representation in IPCC-class models has evolved across successive model generations (<xref ref-type="bibr" rid="B35">Jackson et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B70">Roberts et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B95">Weijer et&#xa0;al., 2020</xref>). On average, the CMIP6 multi-model ensemble exhibits a stronger AMOC decline after the 1980s than Phase 5 of CMIP (CMIP5) in all future CO<sub>2</sub> emission scenarios (<xref ref-type="bibr" rid="B57">Menary et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B95">Weijer et&#xa0;al., 2020</xref>). The decline between 1980 and 2015 compares reasonably well with observations of the Rapid Climate Change-Meridional Overturning Circulation (RAPID) array, the Overturning in the Subpolar North Atlantic Program (OSNAP), and the South Atlantic MOC Basin-wide Array (SAMBA), notwithstanding their limited time coverage (<xref ref-type="bibr" rid="B23">Frajka-Williams et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B49">Lozier et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B81">Smeed et&#xa0;al., 2019</xref>).</p>
<p>First, we provide an overview of the trends in AMOC, ALK, and ocean carbon uptake in the subpolar North Atlantic region, and then we discuss how they relate to physical variables from the late 20<sup>th</sup> century to the end of the 21<sup>st</sup> century. An essential aspect of our investigation involves probing the relationships between the factors that control the representation of carbon uptake and the weakening of the AMOC and ALK in ten CMIP6 Earth System Models under a high CO<sub>2</sub> emissions scenario (the Shared Socio-economic Pathways SSP5-8.5). Additionally, we seek to identify key processes and metrics that may effectively reduce uncertainty in future model projections. By exploring the relationships among AMOC trends, ALK, ocean carbon uptake, and various other physical variables, our study provides insights that are crucial for improving projections of the future global climate system and for identifying key variables to monitor to reduce uncertainty in carbon cycle feedbacks and their role in shaping the transient climate response to cumulative carbon emissions (TCRE).</p>
</sec>
<sec id="s2" sec-type="materials|methods">
<label>2</label>
<title>Materials and methods</title>
<sec id="s2_1">
<label>2.1</label>
<title>The ten CMIP6 Earth System Models and variables analyzed</title>
<p>We analyze four CMIP6 Earth System Models in the historical scenario (<xref ref-type="bibr" rid="B22">Eyring et&#xa0;al., 2016</xref>) and in the high CO<sub>2</sub> emission scenario, SSP5-8.5 (<xref ref-type="bibr" rid="B96">Wilbanks and Ebi, 2013</xref>; <xref ref-type="bibr" rid="B67">Riahi et&#xa0;al., 2017</xref>). These ten Earth System Models are listed in <xref ref-type="table" rid="T1">
<bold>Table&#xa0;1</bold>
</xref> and includes CESM2 (<xref ref-type="bibr" rid="B15">Danabasoglu et&#xa0;al., 2020</xref>), NorESM2-LM (<xref ref-type="bibr" rid="B78">Seland et&#xa0;al., 2020</xref>), ACCESS-ESM1-5 (<xref ref-type="bibr" rid="B103">Ziehn et&#xa0;al., 2020</xref>), MPI-ESM1-2-LR (<xref ref-type="bibr" rid="B53">Mauritsen et&#xa0;al., 2019</xref>), CMCC-ESM2 (<xref ref-type="bibr" rid="B11">Cherchi et&#xa0;al., 2019</xref>), CNRM-ESM2-1 (<xref ref-type="bibr" rid="B77">S&#xe9;f&#xe9;rian et&#xa0;al., 2019</xref>), UKESM1-0-LL (<xref ref-type="bibr" rid="B79">Sellar et&#xa0;al., 2019</xref>), MIROC-ES2L (<xref ref-type="bibr" rid="B30">Hajima et&#xa0;al., 2020</xref>), CanESM5 (<xref ref-type="bibr" rid="B84">Swart et&#xa0;al., 2019</xref>), and IPSL-CM6A-LR (<xref ref-type="bibr" rid="B5">Boucher et&#xa0;al., 2020</xref>). They have been selected for the availability of the physical and chemical variables (<xref ref-type="table" rid="T2">
<bold>Table&#xa0;2</bold>
</xref>) necessary for our analysis under future scenarios. The climate model simulations are obtained via the Earth System Grid Federation (ESGF) archive of CMIP6 data (<ext-link ext-link-type="uri" xlink:href="https://esgf-node.llnl.gov">https://esgf-node.llnl.gov</ext-link>). The partial pressure of atmospheric CO<sub>2</sub> is obtained from the input and forcing datasets for the Model Intercomparison Projects (input4MIPs, <ext-link ext-link-type="uri" xlink:href="https://esgf-node.llnl.gov/search/input4mips/">https://esgf-node.llnl.gov/search/input4mips/</ext-link>) in CMIP6 (<xref ref-type="bibr" rid="B22">Eyring et&#xa0;al., 2016</xref>; <xref ref-type="bibr" rid="B55">Meinshausen et&#xa0;al., 2017</xref>, <xref ref-type="bibr" rid="B54">2020</xref>). The historical simulations cover the 1850 to 2014 period, and the future scenario simulation covers the period 2015 to 2100 with high radiative forcing under SSP5-8.5 (<xref ref-type="bibr" rid="B54">Meinshausen et&#xa0;al., 2020</xref>). Under the historical simulations, our analysis focuses on the period from 1950 to 2014. For all spatially-varying variables in <xref ref-type="table" rid="T2">
<bold>Table&#xa0;2</bold>
</xref>, the time series are computed as the area-weighted means within the defined sector of the subpolar North Atlantic basin, which encompasses the area from 40&#xb0;N to 65&#xb0;N latitude and from 55&#xb0;W to 15&#xb0;W longitude (<xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1</bold>
</xref>).</p>
<table-wrap id="T1" position="float">
<label>Table&#xa0;1</label>
<caption>
<p>Model components and resolution.</p>
</caption>
<table frame="hsides">
<thead>
<tr>
<th valign="middle" align="left">Model Name</th>
<th valign="middle" align="left">Atmospheric Component and Resolution</th>
<th valign="middle" align="left">Oceanic <break/>Component and Resolution</th>
<th valign="middle" align="left">References</th>
</tr>
</thead>
<tbody>
<tr>
<td valign="middle" align="left">CESM2</td>
<td valign="middle" align="left">CAM6, 0.9&#xb0;&#xd7;1.25&#xb0;, 32 levels</td>
<td valign="middle" align="left">POP2, ~1&#xb0;, 60 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B15">Danabasoglu et&#xa0;al., 2020</xref>)</td>
</tr>
<tr>
<td valign="middle" align="left">NorESM2-LM</td>
<td valign="middle" align="left">CAM6-Nor, ~2&#xb0;, 32 levels</td>
<td valign="middle" align="left">BLOM/iHAMOCC, ~1&#xb0;, 70 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B78">Seland et&#xa0;al., 2020</xref>)</td>
</tr>
<tr>
<td valign="middle" align="left">ACCESS-ESM1-5</td>
<td valign="middle" align="left">HadGAM2, 1.875&#xb0;&#xd7;1.25&#xb0;, 38 levels</td>
<td valign="middle" align="left">ACCESS-OM2, MOM5, tripolar primarily 1&#xb0;, 50 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B103">Ziehn et&#xa0;al., 2020</xref>)</td>
</tr>
<tr>
<td valign="middle" align="left">MPI-ESM1-2-LR</td>
<td valign="middle" align="left">ECHAM6.3, 1.875&#xb0;&#xd7;1.875&#xb0;, 47 levels</td>
<td valign="middle" align="left">MPIOM1.63, ~1.5&#xb0;, 40 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B53">Mauritsen et&#xa0;al., 2019</xref>)</td>
</tr>
<tr>
<td valign="middle" align="left">CMCC-ESM2</td>
<td valign="middle" align="left">CAM5.3, ~1&#xb0;, 30 levels</td>
<td valign="middle" align="left">NEMO3.6, ORCA1 tripolar grid, 1&#xb0; with refinement to 1/3&#xb0; within the tropics, 50 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B11">Cherchi et&#xa0;al., 2019</xref>)</td>
</tr>
<tr>
<td valign="middle" align="left">CNRM-ESM2-1</td>
<td valign="middle" align="left">ARPEGE 6.3, ~1&#xb0;, 91 levels</td>
<td valign="middle" align="left">NEMO3.6, eORCA1, tripolar primarily 1&#xb0;, 75 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B77">S&#xe9;f&#xe9;rian et&#xa0;al., 2019</xref>)</td>
</tr>
<tr>
<td valign="middle" align="left">UKESM1-0-LL</td>
<td valign="middle" align="left">MetUM-HadGEM3-GA7.1, 1.875&#xb0;&#xd7;1.25&#xb0;, 85 levels</td>
<td valign="middle" align="left">NEMO-HadGEM3-GO6.0, eORCA1, tripolar primarily 1&#xb0;, 75 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B79">Sellar et&#xa0;al., 2019</xref>)</td>
</tr>
<tr>
<td valign="middle" align="left">MIROC-ES2L</td>
<td valign="middle" align="left">CCSR AGCM, ~2.8&#xb0;, 40 levels</td>
<td valign="middle" align="left">COCO4.9, tripolar primarily 1&#xb0;, 63 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B30">Hajima et&#xa0;al., 2020</xref>)</td>
</tr>
<tr>
<td valign="middle" align="left">CanESM5</td>
<td valign="middle" align="left">CanAM5, ~2.8&#xb0;, 49 levels</td>
<td valign="middle" align="left">NEMO3.4.1, ORCA1 tripolar grid, 1&#xb0; with refinement to 1/3&#xb0; within 20&#xb0; of the equator, 41 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B84">Swart et&#xa0;al., 2019</xref>)</td>
</tr>
<tr>
<td valign="middle" align="left">IPSL-CM6A-LR</td>
<td valign="middle" align="left">LMDZ, 1.875&#xb0;&#xd7;1.25&#xb0;, 79 levels</td>
<td valign="middle" align="left">NEMO-OPA, eORCA1.3, tripolar primarily 1&#xb0;, 75 levels</td>
<td valign="middle" align="left">(<xref ref-type="bibr" rid="B5">Boucher et&#xa0;al., 2020</xref>)</td>
</tr>
</tbody>
</table>
</table-wrap>
<table-wrap id="T2" position="float">
<label>Table&#xa0;2</label>
<caption>
<p>Model variables and description.</p>
</caption>
<table frame="hsides">
<thead>
<tr>
<th valign="middle" align="left">Abbreviations</th>
<th valign="middle" align="left">Description</th>
<th valign="middle" align="center">Unit</th>
</tr>
</thead>
<tbody>
<tr>
<td valign="middle" align="left">AMOC</td>
<td valign="middle" align="left">Atlantic Meridional Overturning Circulation at 40&#xb0;N</td>
<td valign="middle" align="center">
<italic>Sv</italic>
</td>
</tr>
<tr>
<td valign="middle" align="left">SST</td>
<td valign="middle" align="left">Sea Surface Temperature</td>
<td valign="middle" align="center">&#xb0;C</td>
</tr>
<tr>
<td valign="middle" align="left">SSS</td>
<td valign="middle" align="left">Sea Surface Salinity</td>
<td valign="middle" align="center">&#x2030;</td>
</tr>
<tr>
<td valign="middle" align="left">DIC</td>
<td valign="middle" align="left">Surface Dissolved Inorganic Carbon</td>
<td valign="middle" align="center">
<italic>&#x3bc;mol</italic> kg<sup>-1</sup>
</td>
</tr>
<tr>
<td valign="middle" align="left">ALK</td>
<td valign="middle" align="left">Sea surface total alkalinity</td>
<td valign="middle" align="center">
<italic>&#x3bc;mol</italic> kg<sup>-1</sup>
</td>
</tr>
<tr>
<td valign="middle" align="left">KE</td>
<td valign="middle" align="left">Kinetic Energy, <inline-formula>
<mml:math display="inline" id="im1">
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</mml:mfrac>
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</inline-formula>, <italic>u</italic> and <italic>v</italic> represent the velocities in the horizontal and vertical planes, respectively.</td>
<td valign="middle" align="center">
<italic>J kg</italic>
<sup>-1</sup>
</td>
</tr>
<tr>
<td valign="middle" align="left">
<italic>p</italic>CO<sub>2</sub>
</td>
<td valign="middle" align="left">Partial Pressure of CO<sub>2</sub> in the ocean</td>
<td valign="middle" align="center">
<italic>&#x3bc;atm</italic>
</td>
</tr>
<tr>
<td valign="middle" align="left">d<italic>p</italic>CO<sub>2</sub>
</td>
<td valign="middle" align="left">Difference of partial pressure of CO<sub>2</sub> in the atmosphere and the ocean</td>
<td valign="middle" align="center">
<italic>&#x3bc;atm</italic>
</td>
</tr>
<tr>
<td valign="middle" align="left">fgCO<sub>2</sub>
</td>
<td valign="middle" align="left">Surface downward flux of total CO<sub>2</sub> (positive: air to sea)</td>
<td valign="middle" align="center">
<italic>kg m</italic>
<sup>-2</sup> <italic>yr</italic>
<sup>-1</sup>
</td>
</tr>
</tbody>
</table>
</table-wrap>
<fig id="f1" position="float">
<label>Figure&#xa0;1</label>
<caption>
<p>Map of the subpolar North Atlantic with major topographic features. The red box delimits the region where the analysis in this study is performed.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-11-1304193-g001.tif"/>
</fig>
<p>As an indicator of simulated AMOC intensity, we use the definition of maximum meridional overturning stream function at 40&#xb0;N and analyze its evolution over time, as commonly done in modeling studies (<xref ref-type="bibr" rid="B42">Knight et&#xa0;al., 2005</xref>; <xref ref-type="bibr" rid="B99">Zhang, 2008</xref>). The choice of 40&#xb0; N is based on the fact that variations in AMOC exhibit their highest anomalies near this latitude (<xref ref-type="bibr" rid="B8">Buckley and Marshall, 2016</xref>). We verified that this is indeed the case in all models considered (<xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Figure&#xa0;1</bold>
</xref>). Kinetic Energy is calculated based on velocities in the horizontal and vertical planes (<xref ref-type="table" rid="T2">
<bold>Table&#xa0;2</bold>
</xref>).</p>
</sec>
<sec id="s2_2">
<label>2.2</label>
<title>
<italic>p</italic>CO<sub>2</sub> decomposition</title>
<p>Variations in the ocean surface <italic>p</italic>CO<sub>2</sub> can be described as a combined effect of alterations in sea surface DIC, and alkalinity, as well as changes in SST and SSS (<xref ref-type="bibr" rid="B72">Sarmiento and Gruber, 2006</xref>), as follows:</p>
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<p>where <italic>&#x3b4;</italic> represents change over time and <inline-formula>
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</inline-formula>X are partial derivative of surface ocean <italic>p</italic>CO<sub>2</sub> with respect to X. SST is sea surface temperature (&#xb0;C), SSS is sea surface salinity (&#x2030;), DIC and ALK are ocean surface DIC and alkalinity (&#xb5;mol kg<sup>-1</sup>), respectively. This decomposition can be applied to understand the trends of surface ocean <italic>p</italic>CO<sub>2</sub>. The temporal change of air-sea CO<sub>2</sub> flux critically depends on the air-sea difference in <italic>p</italic>CO<sub>2</sub>. There would be a decline (increase) in air-sea CO<sub>2</sub> flux if ocean <italic>p</italic>CO<sub>2</sub> increases faster (slower) than atmospheric <italic>p</italic>CO<sub>2</sub>. This analysis uses the CO2SYS program (<xref ref-type="bibr" rid="B47">Lewis and Wallace, 1998</xref>) to calculate each term in <xref ref-type="disp-formula" rid="eq1">Equations 1</xref>, <xref ref-type="disp-formula" rid="eq2">2</xref>. The partial derivatives are calculated by making finite perturbations, and they quantify the sensitivity of ocean <italic>p</italic>CO2 to SST, SSS, DIC or ALK, while the terms <inline-formula>
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</inline-formula> are the contributions of SST, SSS, DIC or ALK to <italic>p</italic>CO<sub>2</sub> changes.</p>
<p>In order to emphasize the salinity impact on ALK and DIC, we separate ALK and DIC into salinity normalized (sALK and sDIC, affected by dynamics, biology and air-sea exchange), and diluted parts (dALK and dDIC, affected by freshwater) (<xref ref-type="bibr" rid="B6">Brix et&#xa0;al., 2013</xref>; <xref ref-type="bibr" rid="B12">Chikamoto and DiNezio, 2021</xref>; <xref ref-type="bibr" rid="B13">Chikamoto et&#xa0;al., 2023</xref>):</p>
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</mml:math>
</disp-formula>
<p>where 35 is the standard salinity value which normalizes DIC and ALK. <xref ref-type="disp-formula" rid="eq2">Equation 2</xref> includes three terms multiplied by &#x3b4;SSS. The first term is the direct effect of salinity, and the second and third terms are the dilution components for DIC and ALK. By design, these two terms tend to cancel out each other. In this study we pay attention to sALK and dALK terms to assess their relative importance in driving <italic>p</italic>CO<sub>2</sub> changes.</p>
</sec>
</sec>
<sec id="s3" sec-type="results">
<label>3</label>
<title>Results</title>
<sec id="s3_1">
<label>3.1</label>
<title>The CO<sub>2</sub> uptake and AMOC change in the subpolar North Atlantic</title>
<p>We investigate the difference between the CO<sub>2</sub> flux (positive from air to sea) among models by considering the spatial patterns of two 31-year periods: 1970-2000 within the historical time and 2070-2100 in the SSP5-8.5 scenario as representative for a high emission future (<xref ref-type="fig" rid="f2">
<bold>Figure&#xa0;2</bold>
</xref>). In most models, the CO<sub>2</sub> flux shows a decrease in the western part of the SPNA while increasing in the eastern and northern parts (<xref ref-type="fig" rid="f2">
<bold>Figure&#xa0;2</bold>
</xref>). One primary factor is the weakening of the AMOC (<xref ref-type="fig" rid="f3">
<bold>Figure&#xa0;3</bold>
</xref>), which has been linked to strengthening stratification and shoaling mixing between density layers, both observed in recent decades and predicted for the future (<xref ref-type="bibr" rid="B41">Kim et&#xa0;al., 2023</xref>). There are, however, significant inter-model differences in the pattern of air-sea CO<sub>2</sub> flux change, some of which may be driven by the thermodynamic change due to the different SST responses to climate warming and AMOC slowdown. In the eastern and northern parts of SPNA, there are patches of cooling known as the North Atlantic Warming Hole (NAWH) (<xref ref-type="bibr" rid="B20">Drijfhout et&#xa0;al., 2012</xref>; <xref ref-type="bibr" rid="B66">Rahmstorf et&#xa0;al., 2015</xref>; <xref ref-type="bibr" rid="B24">Gervais et&#xa0;al., 2018</xref>; <xref ref-type="bibr" rid="B56">Menary et&#xa0;al., 2018</xref>; <xref ref-type="bibr" rid="B39">Keil et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B62">Oudar et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B3">Bellomo et&#xa0;al., 2021</xref>). AMOC weakening changes the relative proportions of warm subtropical waters and cold subpolar waters being transported into the eastern and western SPNA respectively. The weakening Labrador Current and the shift of the Gulf Stream result in colder and fresher waters south of Greenland due to the reduced transport of warm, salty water from the tropics and much lower SSS and higher sea surface height in the subpolar region (<xref ref-type="bibr" rid="B14">Claret et&#xa0;al., 2018</xref>; <xref ref-type="bibr" rid="B3">Bellomo et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B25">Gon&#xe7;alves Neto et&#xa0;al., 2021</xref>). This alteration in water mass distribution can lead to significant CO<sub>2</sub> uptake changes.</p>
<fig id="f2" position="float">
<label>Figure&#xa0;2</label>
<caption>
<p>Maps of fgCO<sub>2</sub> (<italic>kg m</italic>
<sup>-2</sup> <italic>yr</italic>
<sup>-1</sup>) difference between 31-year averages over 2070-2100 in the SSP585 scenario and that of 1970-2000 in the historical run for ten models <bold>(A-J)</bold>, and in the multi-model mean <bold>(K)</bold> in the SPNA. In <bold>(K)</bold> dots indicate whenever changes in at least 8 out of the 10 models agree in the sign.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-11-1304193-g002.tif"/>
</fig>
<fig id="f3" position="float">
<label>Figure&#xa0;3</label>
<caption>
<p>Maps of AMOC difference (in <italic>Sv</italic>) between 31-year averages over 2070-2100 in the SSP585 scenario and 1970-2000 in the historical runs for ten models <bold>(A-J)</bold> and the the multi-model mean <bold>(K)</bold>, visualized as basin-wide zonal-and time-integrated stream function.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-11-1304193-g003.tif"/>
</fig>
<p>
<xref ref-type="fig" rid="f3">
<bold>Figure&#xa0;3</bold>
</xref> presents the differences in AMOC stream functions from the CMIP6 models. Here we provide a comparative analysis of the mean AMOC magnitude between two timeframes: the historical period of 1970-2000 and the projected period of 2070-2100 in SSP5-8.5. All models exhibit a weakening of the AMOC by the end of the 21<sup>st</sup> century. The magnitudes of AMOC decrease vary among the models, but broadly correlates with the initial AMOC strength (<xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Figure&#xa0;1</bold>
</xref>): models with a stronger AMOC in historical times show a more pronounced decrease in the projections, especially in CESM2 and NorESM2-LM (<xref ref-type="fig" rid="f3">
<bold>Figures&#xa0;3A,B</bold>
</xref>; <xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Figures&#xa0;1A, B</bold>
</xref>). While in models with a weak AMOC in the historical period, such as in IPSL-CM6A-LR (<xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Figure&#xa0;1J</bold>
</xref>), the reduction is moderate in the future (<xref ref-type="fig" rid="f3">
<bold>Figure&#xa0;3J</bold>
</xref>). The AMOC exhibits its maximum strength at around 40&#xb0;N both during the historical period (1970-2000) (<xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Figure&#xa0;1</bold>
</xref>) and in the projected future period (2070-2100), and the greatest reduction in AMOC strength occurs at this latitude according to the model simulations (<xref ref-type="fig" rid="f3">
<bold>Figure&#xa0;3</bold>
</xref>). These findings about the AMOC trends in CMIP6 are consistent with the earlier study by <xref ref-type="bibr" rid="B95">Weijer et&#xa0;al. (2020)</xref>.</p>
</sec>
<sec id="s3_2">
<label>3.2</label>
<title>Time series of physical and chemical variables</title>
<p>Temporal trajectories of the physical variables from the ten CMIP6 Earth System Models are displayed in <xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4</bold>
</xref>. Robust changes across all ten models in the high CO<sub>2</sub> emission scenario include AMOC weakening, surface freshening, and increasing SST, DIC and sea surface <italic>p</italic>CO<sub>2</sub> (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4A&#x2013;E, G</bold>
</xref>). These changes can be attributed to the increasing atmospheric <italic>p</italic>CO<sub>2</sub> and the greenhouse effect but the rates of warming and DIC increases are model-dependent. Surface DIC generally increases due to the absorption of anthropogenic CO<sub>2</sub>, but this is not the only factor controlling its growth. Warming can reduce the solubility of gases, leading to higher <italic>p</italic>CO<sub>2</sub> at the sea surface. Additionally, increased ocean stratification can impact the circulation, contributing to AMOC weakening.</p>
<fig id="f4" position="float">
<label>Figure&#xa0;4</label>
<caption>
<p>Annual time series of anomalies of physical and chemical variables in the SPNA. <bold>(A)</bold> AMOC anomaly at 40&#xb0;N in units of <italic>Sv</italic>. <bold>(B)</bold> SST anomaly in &#xb0;C. <bold>(C)</bold> SSS anomaly in units of &#x2030;. <bold>(D)</bold> DIC anomaly in units of <italic>&#x3bc;mol kg</italic>
<sup>-1</sup>. <bold>(E)</bold> ALK anomaly in units of <italic>&#x3bc;mol kg</italic>
<sup>-1</sup>. <bold>(F)</bold> KE anomaly in units of <italic>J kg</italic>
<sup>-1</sup>. <bold>(G)</bold> <italic>p</italic>CO<sub>2</sub> anomaly in units of <italic>&#x3bc;atm</italic>. <bold>(H)</bold> d<italic>p</italic>CO<sub>2</sub> anomaly in units of <italic>&#x3bc;atm</italic>. <bold>(I)</bold> fgCO<sub>2</sub> anomaly in units of <italic>kg m</italic>
<sup>-2</sup> <italic>yr</italic>
<sup>-1</sup>. The time series include two periods - the historical period (1950-2014) and the future scenario (2015-2100, SSP5-8.5). The colored lines represent each model while the thick black line represents the ten models ensemble average.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-11-1304193-g004.tif"/>
</fig>
<p>In terms of AMOC, all models but MIROC-ES2L show a moderate increase in AMOC strength in the ~1950-1980 period, likely due to the aerosol forcing (<xref ref-type="bibr" rid="B57">Menary et&#xa0;al., 2020</xref>), followed by a decrease after the 1980s (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4A</bold>
</xref>). In the multi-model mean sense, AMOC weakens by about 9 <italic>Sv</italic> by the end of the 21<sup>st</sup> century (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4A</bold>
</xref>). Surface freshening (salinity decrease) may be driven by the freshwater fluxes including precipitation, ice melt, and runoff as well as internal dynamics including changing transport of salty subtropical waters to the SPNA by the weakened AMOC. A significant decline of surface alkalinity (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4E</bold>
</xref>) is linked to the reduction in SSS and AMOC (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4A, C</bold>
</xref>) in all models. The reduction in alkalinity accelerates the acidification of the surface water and decrease the buffering capacity. In the SPNA, all models show some decline of surface alkalinity associated with freshening (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4C, E</bold>
</xref>). Under the warming climate, the reduction in AMOC transport and the stronger freshwater fluxes together act to decrease the surface alkalinity by freshening or dilution, which tends to increase surface ocean <italic>p</italic>CO<sub>2</sub>. On interannual and longer timescale, surface ocean <italic>p</italic>CO<sub>2</sub> increases, following the rising atmospheric <italic>p</italic>CO<sub>2</sub>. All models exhibit increasing ocean <italic>p</italic>CO<sub>2</sub> of about 800 <italic>&#xb5;atm</italic> at the end of the 21<sup>st</sup> century in SSP5-8.5 (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4G</bold>
</xref>). Air-sea CO<sub>2</sub> exchange adjusts surface ocean <italic>p</italic>CO<sub>2</sub> to the atmospheric <italic>p</italic>CO<sub>2</sub> with some lag as determined by the air-sea equilibration timescale. Carbonate chemistry dictates that the increase must be achieved by the combination of the four factors in <xref ref-type="disp-formula" rid="eq2">Equation 2</xref>. The increase in surface ocean <italic>p</italic>CO<sub>2</sub> induced by alkalinity decrease reduces the regional carbon sink by limiting the ocean <italic>p</italic>CO<sub>2</sub> growth by the air-sea equilibration and resultant DIC increase. This effect is especially strong in models with significant freshening (SSS decline) which is mechanistically linked to the AMOC slowdown. The pattern of temporal changes in the air-sea <italic>p</italic>CO<sub>2</sub> difference (d<italic>p</italic>CO<sub>2</sub>) generally matches that of air-sea CO<sub>2</sub> flux (fgCO<sub>2</sub>) because d<italic>p</italic>CO<sub>2</sub> drives fgCO<sub>2</sub> (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4H, I</bold>
</xref>). Thus, any factor that increases the d<italic>p</italic>CO<sub>2</sub> gradient can also increase the magnitude of fgCO<sub>2</sub>, assuming other conditions remain the same. The trends in fgCO<sub>2</sub> are influenced by several factors beyond the d<italic>p</italic>CO<sub>2</sub> due to the dependence of air-sea gas transfer on wind speed and seaice cover in polar regions. Hence, there are some small discrepancies between the trends and variability of fgCO<sub>2</sub> and that of d<italic>p</italic>CO<sub>2</sub> (<xref ref-type="bibr" rid="B37">Jing et&#xa0;al., 2022</xref>).</p>
<p>CESM2 and NorESM2-LM exhibit similar trends in terms of AMOC and SST (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4A, B</bold>
</xref>). The strong AMOC weakening (~18 <italic>Sv</italic>) in CESM2 and NorESM2-LM is associated with the formation of a strong NAWH by the end of 2050. However, despite their similar model components, trends in SSS, DIC, and alkalinity differ between CESM2 and NorESM2-LM. Those differences could be attributed to how each model simulates ocean biogeochemical processes, freshwater inputs, and atmospheric CO<sub>2</sub> exchange dynamics (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4</bold>
</xref>). The less pronounced increase in DIC and the strong decrease in alkalinity in CESM2 might suggest a different representation of the freshwater fluxes, ocean circulation and mixing patterns, which can affect the regional carbon cycle. Even with the similar SST trends, the stronger freshening and alkalinity loss would weaken the regional carbon uptake, explaining the relatively weaker growth of surface simulated DIC and weaker carbon uptake (fgCO<sub>2</sub>) in CESM2 compared to NorESM2-LM (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4B&#x2013;E, I</bold>
</xref>). Differences in precipitation, evaporation, river runoff, and ice melt could cause variations in SSS and consequently influence CO<sub>2</sub> uptake and alkalinity levels. While CESM2 and NorESM2-LM exhibit similar AMOC and kinetic energy (KE) changes, there are indeed some minor differences in the evolution of kinetic energy (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4A, F</bold>
</xref>). Here, the KE is calculated as a measure of ocean transport strength in addition to AMOC intensity, and it includes other aspects of the ocean circulation system such as boundary currents (Irminger and Labrador Current), wind-driven subpolar gyre, as well as AMOC. The KE decrease in CESM2 is less pronounced after 2060s in comparison to NorESM2-LM indicating somewhat different circulation changes in the late 21<sup>st</sup> century. This could reflect the potential regional variations in freshwater fluxes and wind stress, and different parameterizations choices in the two models.</p>
<p>CanESM5 exhibits both the lowest d<italic>p</italic>CO<sub>2</sub> trend for most of the 21<sup>st</sup> century, and the most significant SST rise (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4B, H</bold>
</xref>) thus reduced CO<sub>2</sub> solubility. This model exhibits some reduction in fgCO<sub>2</sub>, though it is not the most substantial, and the fgCO<sub>2</sub> decrease occurs in conjunction with an increase in KE in the projections (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4F, I</bold>
</xref>).</p>
<p>Conversely, ACCESS-ESM1-5 shows the most considerable increase in fgCO<sub>2</sub>, consistent with minimal projected change in SSS (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4C, I</bold>
</xref>). This model&#x2019;s moderate AMOC attenuation (~7 <italic>Sv</italic>) and limited ocean freshening suggest that atmospheric <italic>p</italic>CO<sub>2</sub> increase predominantly drives the ocean CO<sub>2</sub> uptake with no opposing effects from alkalinity.</p>
</sec>
<sec id="s3_3">
<label>3.3</label>
<title>ALK contribution to <italic>p</italic>CO<sub>2</sub> change</title>
<p>So far, our discussion focused on interpreting different evolution of physical and biogeochemical variables. Here we decompose ocean <italic>p</italic>CO<sub>2</sub> and quantify the effect of SST, SSS, DIC and ALK on the change of d<italic>p</italic>CO<sub>2</sub> with the purpose of quantitatively assessing different drivers of <italic>p</italic>CO<sub>2</sub> increase on centennial timescale (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5F</bold>
</xref>). <italic>p</italic>CO<sub>2</sub> decomposition indicates that the overall change in <italic>p</italic>CO<sub>2</sub> can be expressed as the sum of four factors (SST, SSS, DIC, ALK) where each factor is multiplied by its respective sensitivity (<xref ref-type="disp-formula" rid="eq1">Equations 1</xref>, <xref ref-type="disp-formula" rid="eq2">2</xref>). <xref ref-type="fig" rid="f6">
<bold>Figure&#xa0;6A</bold>
</xref> shows the trends in oceanic <italic>p</italic>CO<sub>2</sub> over time in the SPNA, alongside contributions from various factors that influence <italic>p</italic>CO<sub>2</sub> levels. The increasing trend in <italic>p</italic>CO<sub>2</sub> signifies a growing partial pressure of CO<sub>2</sub> in the ocean&#x2019;s surface. ALK contributes to this increasing trend and, by the end of the 21<sup>st</sup> century, ALK becomes the most important contributor to <italic>p</italic>CO<sub>2</sub> change in the multi-model mean sense. The influence of sALK is close to zero, suggesting that changes in salinity-normalized ALK alone do not account for the change in <italic>p</italic>CO<sub>2</sub> trend. ALK affects <italic>p</italic>CO<sub>2</sub> due to dilution effects from freshwater fluxes and the weakened ocean salinity transport. The SST contribution to the increasing <italic>p</italic>CO<sub>2</sub> trend shows a moderate contribution by the warming-induced solubility decrease. The DIC contribution indicates that increases in DIC are driving <italic>p</italic>CO<sub>2</sub> upward, as more CO<sub>2</sub> is being added to the ocean. The SSS contribution is less significant but slightly negative, implying that a decrease in salinity impacts carbonate chemistry and CO<sub>2</sub> solubility. Overall, the increasing <italic>p</italic>CO<sub>2</sub> trend appears to be driven by ALK, DIC and SST changes, with SSS playing a minimal role.</p>
<fig id="f5" position="float">
<label>Figure&#xa0;5</label>
<caption>
<p>Correlation among various variables in the CMPI6 models analyzed. Differences are computed based on annual means over the region within the red box in <xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1</bold>
</xref> (poleward of 40&#xb0;N to 65&#xb0;N and eastward of 55&#xb0;W to 15&#xb0;W) and calculated between 31-year average in SSP5-8.5 (2070-2100) and corresponding in the historical period (1970-2000) <bold>(A)</bold> Correlation of SSS (&#x2030;) and ALK (<italic>&#x3bc;mol</italic> kg<sup>-1</sup>) difference. <bold>(B)</bold> Correlation of ALK (<italic>&#x3bc;mol</italic> kg<sup>-1</sup>) and AMOC difference. <bold>(C)</bold> Correlation of carbon uptake (PgC) in future projections (2070-2100) and ALK (<italic>&#x3bc;mol</italic> kg<sup>-1</sup>) difference. <bold>(D)</bold> Correlation of carbon uptake (PgC) in future projections (2070-2100) and SST (&#xb0;C) difference. <bold>(E)</bold> Correlation of fgCO<sub>2</sub> trend difference (<italic>kg m</italic>
<sup>-2</sup> <italic>yr</italic>
<sup>-2</sup>) and AMOC (<italic>Sv</italic>). <bold>(F)</bold> Correlation of fgCO<sub>2</sub> difference (<italic>kg m</italic>
<sup>-2</sup> <italic>yr</italic>
<sup>-1</sup>) and d<italic>p</italic>CO<sub>2</sub> (<italic>&#x3bc;atm</italic>).</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-11-1304193-g005.tif"/>
</fig>
<fig id="f6" position="float">
<label>Figure&#xa0;6</label>
<caption>
<p>Drivers of ocean surface <italic>p</italic>CO<sub>2</sub> trends and <italic>p</italic>CO<sub>2</sub> sensitivity. <bold>(A)</bold> Drivers of <italic>p</italic>CO<sub>2</sub> trends, calculated by <inline-formula>
<mml:math display="inline" id="im4">
<mml:mrow>
<mml:mfrac>
<mml:mrow>
<mml:mo>&#x2202;</mml:mo>
<mml:mi>p</mml:mi>
<mml:mi>C</mml:mi>
<mml:msub>
<mml:mi>O</mml:mi>
<mml:mn>2</mml:mn>
</mml:msub>
</mml:mrow>
<mml:mrow>
<mml:mo>&#x2202;</mml:mo>
<mml:mi>X</mml:mi>
</mml:mrow>
</mml:mfrac>
<mml:mtext>&#x3b4;</mml:mtext>
<mml:mi>X</mml:mi>
</mml:mrow>
</mml:math>
</inline-formula>, where <italic>X</italic> = SST, DIC, sDIC, ALK, sALK or SSS. The color lines show the ocean surface <italic>p</italic>CO<sub>2</sub> trend (blue solid), and the contributions of changes in SST (red solid), DIC (orange solid), sDIC(orange dotted), ALK (green solid), sALK (green dotted) and SSS (light blue) to the ocean <italic>p</italic>CO<sub>2</sub> trends, in addition to the sum of the four drivers (dark grey dotted). The transparent lines indicate the annual trends and the solid lines are the 20-year running average. <bold>(B)</bold> <italic>p</italic>CO<sub>2</sub> sensitivity, calculated by <inline-formula>
<mml:math display="inline" id="im5">
<mml:mrow>
<mml:mfrac>
<mml:mrow>
<mml:mo>&#x2202;</mml:mo>
<mml:mi>p</mml:mi>
<mml:mi>C</mml:mi>
<mml:msub>
<mml:mi>O</mml:mi>
<mml:mn>2</mml:mn>
</mml:msub>
</mml:mrow>
<mml:mrow>
<mml:mo>&#x2202;</mml:mo>
<mml:mi>X</mml:mi>
<mml:mo stretchy="false">/</mml:mo>
<mml:mi>X</mml:mi>
<mml:mo>_</mml:mo>
<mml:mi>s</mml:mi>
<mml:mi>t</mml:mi>
<mml:mi>d</mml:mi>
<mml:mi>e</mml:mi>
<mml:mi>v</mml:mi>
</mml:mrow>
</mml:mfrac>
</mml:mrow>
</mml:math>
</inline-formula>, where <italic>X_stdev</italic> is the standard deviation of each variable over 1950-2100. The color lines show the ocean surface <italic>p</italic>CO<sub>2</sub> sensitivity to SST (red solid), DIC (orange solid), sDIC(orange dotted), ALK (green solid), sALK (green dotted) and SSS (light blue). The standard deviation of SST, DIC, sDIC, ALK, sALK or SSS are 1.14 &#xb0;C, 38.78 <italic>&#x3bc;mol kg</italic>
<sup>-1</sup>, 64.54 <italic>&#x3bc;mol kg</italic>
<sup>-1</sup>, 21.41 <italic>&#x3bc;mol kg</italic>
<sup>-1</sup>, 4.92 <italic>&#x3bc;mol kg</italic>
<sup>-1</sup> and 0.40 &#x2030;, respectively.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-11-1304193-g006.tif"/>
</fig>
<p>By examining the temporal evolution of <italic>p</italic>CO<sub>2</sub> sensitivity to all components, the sensitivity increases over time due to the changing background states of carbonate chemistry over the centennial timescale considered (<xref ref-type="fig" rid="f6">
<bold>Figure&#xa0;6B</bold>
</xref>). The nearly opposite sensitivities to DIC and ALK indicate that mutually compensating <italic>p</italic>CO<sub>2</sub> response for synchronous changes in DIC and ALK. This can be easily understood considering the changes induced by a pulse of freshwater flux. An input of freshwater can decrease DIC and ALK at similar rates, leading to a muted response of surface ocean <italic>p</italic>CO<sub>2</sub> over a relatively short timescale. On the interannual and longer timescales, the gradual increase in atmospheric <italic>p</italic>CO<sub>2</sub> and the resultant ocean carbon uptake increase DIC but not ALK (<xref ref-type="fig" rid="f6">
<bold>Figure&#xa0;6B</bold>
</xref>). Thus, increasing DIC and decreasing ALK together increase the surface ocean <italic>p</italic>CO<sub>2</sub> on longer timescales. The increasing acidity of seawater increases the buffer factor which is approximately equal to [H<sup>+</sup>]/K<sub>2</sub> where K<sub>2</sub> is the equilibrium constant for the dissolution reaction of bicarbonate ion into carbonate ion. The acidification of seawater (increase in [H<sup>+</sup>]) directly causes the increase in buffer factor and the sensitivity of <italic>p</italic>CO<sub>2</sub> to DIC on centennial timescales.</p>
<p>We further investigate the difference of <italic>p</italic>CO<sub>2</sub> components between two 31-year periods: 1970-2000 as representative of the late 20<sup>th</sup> century and 2070-2100 in the SSP5-8.5 scenario as representative of the future towards the end of the 21<sup>st</sup> century (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7</bold>
</xref>). Over these two periods, all models show AMOC slowdown in the future scenario, together with increasing <italic>p</italic>CO<sub>2</sub> in the atmosphere and in the surface ocean (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7</bold>
</xref>). The contribution of SST to the surface ocean <italic>p</italic>CO<sub>2</sub> change is relatively small in comparison to alkalinity and DIC. ALK contributes the most to <italic>p</italic>CO<sub>2</sub> increase in CESM2, NorESM2-LM, CanESM5, MIROC-ES2L, UKESM1-0-LL, and CNRM-ESM2-1 while in the other four models&#x2019; the <italic>p</italic>CO<sub>2</sub> increase is mainly driven by DIC contributions (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7A</bold>
</xref>).</p>
<fig id="f7" position="float">
<label>Figure&#xa0;7</label>
<caption>
<p>
<bold>(A)</bold> Differences in ocean surface <italic>p</italic>CO<sub>2</sub> trends (blue) and its drivers, and differences in AMOC (black) and fgCO<sub>2</sub> trends (purple) between the average over 2070-2100 and the average over 1970-2000. The ocean <italic>p</italic>CO<sub>2</sub> drivers include ALK (green), sALK (<bold>B</bold>, green plaid), dALK (<bold>B</bold>, green strip), DIC (orange), sDIC (<bold>B</bold>, orange plaid), dDIC (<bold>B</bold>, orange strip) and SST (red).</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-11-1304193-g007.tif"/>
</fig>
<p>The <italic>p</italic>CO<sub>2</sub> trends associated with DIC and ALK are further decomposed using the salinity-normalized and the dilution (freshwater) components. The DIC contribution of <italic>p</italic>CO<sub>2</sub> trends can be understood as a residual between the increase in salinity-normalized DIC (affected by air-sea CO<sub>2</sub> exchange, dynamics and biology) and the decrease in the dilution component. For most models, the salinity-normalized DIC dominates except for CESM2 (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7B</bold>
</xref>).</p>
<p>ALK contribution to <italic>p</italic>CO<sub>2</sub> changes relies on the freshwater (dilution) component of ALK decrease except for IPSL-CM6A-LR. In models with stronger SSS decrease, ALK contributes more to increased surface ocean <italic>p</italic>CO<sub>2</sub> and weakened ocean CO<sub>2</sub> uptake. Thus, the mechanisms behind the representation of weakened CO<sub>2</sub> uptake in the late 21<sup>st</sup> century are model dependent. In ACCESS-ESM1-5, the ALK and dALK contributions are lower in 2070-2100 than that in 1970-2000. In this particular model, ALK makes a small contribution to <italic>p</italic>CO<sub>2</sub> change due to the sudden shift in SSS, DIC and ALK in the last 5 years of the 21<sup>st</sup> century (2096-2100, <xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4C&#x2013;E</bold>
</xref>). If we exclude this event by adjusting the analysis window to 2065-2095 in ACCESS-ESM1-5, the dilution component (dALK) clearly controls the <italic>p</italic>CO<sub>2</sub> change in this model, and its fgCO<sub>2</sub> decreases significantly (<xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Figure&#xa0;3</bold>
</xref>). CESM2 and NorESM2-LM both exhibit a pronounced AMOC slowdown, consistent with strong fgCO<sub>2</sub> decreasing trends (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7A</bold>
</xref>). What distinguish CESM2 and NorESM2-LM are the magnitude of the AMOC reduction, and the resultant ALK-driven pCO<sub>2</sub> increase is much greater than that of DIC in comparison to other models (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7</bold>
</xref>). IPSL-CM6A-LR and MPI-ESM1-2-LR, on the other hand, show the weakest AMOC slowdown associated with the least fgCO<sub>2</sub> decrease (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7A</bold>
</xref>). In these models, the ALK contributions to <italic>p</italic>CO<sub>2</sub> trend are also the weakest (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7B</bold>
</xref>, <xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Figure&#xa0;3</bold>
</xref>). The correlation between AMOC changes and ALK contribution to the fgCO<sub>2</sub> trends can be explained through salinity changes.</p>
</sec>
<sec id="s3_4">
<label>3.4</label>
<title>Correlations among ALK, AMOC and carbon uptake</title>
<p>To understand the relationship between ALK and AMOC with carbon uptake, we examine the differences between the two 31-year periods (1970-2000 vs 2070-2100) among the ten models. <xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5A</bold>
</xref> illustrates a strong positive correlation between changes in ALK and SSS across climate models, indicating that a decrease in ocean SSS is typically accompanied by a decrease in ALK. This means that the ALK change is mainly caused by the freshwater effect and by changes in the northward transport of salinity by the AMOC. This is reinforced by a notable positive correlation between ALK differences and changes in AMOC strength, suggesting that the decrease in ALK is associated with the reduction in AMOC (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5B</bold>
</xref>). Furthermore, a moderate positive correlation is observed between ALK differences and oceanic carbon uptake, implying that an increase (or less dilution) in ALK could increase the ocean&#x2019;s capacity to sequester carbon (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5C</bold>
</xref>). However, this correlation is relatively small (R<sup>2</sup> = 0.23) indicating that there are other mechanisms at play. Indeed, <xref ref-type="bibr" rid="B27">Goris et&#xa0;al. (2018)</xref> demonstrated that the vertical transport of DIC plays an important role, which is reflected in the seasonal amplitude of surface ocean <italic>p</italic>CO<sub>2</sub>. This factor alone, however, cannot explain the future evolution of carbon uptake in the North Atlantic in the models. Furthermore, the relationship between SST differences and carbon uptake is weak in the models considered, indicating that SST variations unlikely control carbon uptake changes (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5D</bold>
</xref>).</p>
<p>Our analysis identified the inter-model relationship modulating the centennial changes in ALK and AMOC, which are quite strongly correlated (R<sup>2</sup> = 0.65). AMOC changes may have a profound impact on ALK in the SPNA, through changes in freshwater fluxes and in the transport of subtropical water masses to SPNA (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5B</bold>
</xref>). AMOC-induced changes in ALK in turn influence the ocean&#x2019;s ability to absorb CO<sub>2</sub>, despite the moderate direct correlation between ALK and carbon uptake. Considering the above <italic>p</italic>CO<sub>2</sub> decomposition analysis, ALK changes can affect the regional <italic>p</italic>CO<sub>2</sub> significantly, and more so in the future than in historical times (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7</bold>
</xref>). Furthermore, the AMOC changes are moderately correlated (R<sup>2</sup> = 0.43) with trend in fgCO<sub>2</sub> indicating that a diminished convective mixing further decreases the carbon uptake (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5E</bold>
</xref>). This analysis highlights the importance of ALK reduction, which increases surface ocean <italic>p</italic>CO<sub>2</sub> and reduces the ocean&#x2019;s capacity to absorb CO<sub>2</sub>. These correlations underscore the interconnectedness of ocean circulation, chemical composition, and the carbon cycle in the Earth&#x2019;s climate system.</p>
</sec>
</sec>
<sec id="s4" sec-type="discussion">
<label>4</label>
<title>Discussion</title>
<sec id="s4_1">
<label>4.1</label>
<title>AMOC, ALK and carbon uptake</title>
<p>This study examined how the representation of the AMOC and its future evolution modulates ocean carbon uptake in the SPNA in ten of the CMIP6 Earth System Models through the analysis of physical and biogeochemical changes on centennial timescales. The AMOC slowdown is generally associated with SSS and ALK decrease, along with increased DIC in the multi-model mean sense, consistent with previous studies (<xref ref-type="bibr" rid="B34">Jackson et&#xa0;al., 2015</xref>; <xref ref-type="bibr" rid="B74">Schmittner and Lund, 2015</xref>; <xref ref-type="bibr" rid="B101">Zhang et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B13">Chikamoto et&#xa0;al., 2023</xref>; <xref ref-type="bibr" rid="B80">Sinet et&#xa0;al., 2023</xref>; <xref ref-type="bibr" rid="B92">van Westen and Dijkstra, 2023</xref>). The extent of these changes can vary across models. For example, CESM2 and NorESM2-LM project pronounced AMOC reductions, which are correlated with modest SST increases due to an intense NAWH (<xref ref-type="bibr" rid="B39">Keil et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B3">Bellomo et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B85">Swingedouw et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B60">No&#xeb;l et&#xa0;al., 2022</xref>; <xref ref-type="bibr" rid="B33">Iversen et&#xa0;al., 2023</xref>) and more significant reductions in SSS and ALK (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4</bold>
</xref>). Upper ocean currents weaken in these models, and these changes are aligned with a strong decrease in KE (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4F</bold>
</xref>) (<xref ref-type="bibr" rid="B29">Gregory and Tailleux, 2010</xref>). In contrast, CanESM5 displays weaker AMOC slowdown, notable SST increases and moderate reduction in SSS and ALK (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4</bold>
</xref>). This model shows a drop in d<italic>p</italic>CO<sub>2</sub>, suggesting that the intensified warming raises ocean <italic>p</italic>CO<sub>2</sub> (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4H</bold>
</xref>). The SPNA in CanESM5 continues to absorb CO<sub>2</sub> until the late 21st century while affected by strong warming, moderate reduction in ALK and moderate AMOC weakening (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4</bold>
</xref>).</p>
<p>The models characterized by strong AMOC mean states in the historical period exhibit both a more pronounced slowdown of AMOC (CESM2/NorESM2-LM) (<xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Figure&#xa0;1</bold>
</xref>) (<xref ref-type="bibr" rid="B28">Gregory et&#xa0;al., 2005</xref>; <xref ref-type="bibr" rid="B95">Weijer et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B3">Bellomo et&#xa0;al., 2021</xref>) and a considerably weaker cumulative CO<sub>2</sub> uptake compared to the models with weaker AMOC slowdown (IPSL-CM6A-LR/MPI-ESM1-2-LR) (<xref ref-type="fig" rid="f7">
<bold>Figure&#xa0;7A</bold>
</xref>). A recent study suggests that under high CO<sub>2</sub>-emission scenarios, the area to the southeast of Greenland is expected to reach the point of anthropogenic CO<sub>2</sub> uptake saturation earlier in the 21<sup>st</sup> century, while under low CO<sub>2</sub>-emission scenarios, it will transit from a carbon sink to a carbon source for the atmosphere around 2080 (<xref ref-type="bibr" rid="B68">Ridge and McKinley, 2021</xref>). Two mechanisms that link AMOC weakening and reduced CO<sub>2</sub> uptake include weakened subduction of surface water (<xref ref-type="bibr" rid="B16">DeGrandpre et&#xa0;al., 2006</xref>; <xref ref-type="bibr" rid="B27">Goris et&#xa0;al., 2018</xref>) and alkalinity decrease due to freshening of surface waters in the SPNA. These two mechanisms are not exclusive to one another, and both affect the air-sea CO<sub>2</sub> transfer. Their relative importance is model-dependent. Having said this, we can point to the most plausible explanation in the model context considering CESM2, which has the strongest AMOC of the ten models in the historical period, and displays the strongest decline as well. The high correlations between AMOC, SSS and ALK link the AMOC slowdown to the alkalinity decline and resultant weakened ocean carbon uptake (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5</bold>
</xref>), while also explaining the reduced rate of increase or even decline in surface DIC concentrations (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4D</bold>
</xref>). Warming-induced solubility decline is also sensitive to the magnitude of AMOC slowdown, but the SST difference has little correlation with carbon uptake in the future scenario (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5D</bold>
</xref>). In CESM2 (or NorESM2-LM), the strong AMOC slowdown causes the SPNA to reach the maximum rate of CO<sub>2</sub> uptake earlier than the inflection point of the transient atmospheric CO<sub>2</sub> levels (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4I</bold>
</xref>) (<xref ref-type="bibr" rid="B87">Terhaar et&#xa0;al., 2022</xref>). In the SSP5-8.5 scenario, where the global CO<sub>2</sub> emission is assumed to increase through the 2080s, their regional ocean carbon sink reaches its peak and then becomes less effective by ~ 2040-2060 (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4I</bold>
</xref>). The increasing contribution of ALK changes to the <italic>p</italic>CO<sub>2</sub> in the SPNA (<xref ref-type="fig" rid="f6">
<bold>Figure&#xa0;6A</bold>
</xref>) is unique to this region. The ALK contribution to <italic>p</italic>CO<sub>2</sub> increase is relatively modest both globally and in the Southern Ocean (<xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Figure&#xa0;3</bold>
</xref>), suggesting a distinct influence to the North Atlantic that may warrant further investigation.</p>
<p>Ocean carbon uptake can reach its peak at an earlier period when the biogeochemical response to physical climate changes (including the AMOC slowdown) further reduces the ocean&#x2019;s ability to absorb atmospheric CO<sub>2</sub> (<xref ref-type="bibr" rid="B51">Maier-Reimer et&#xa0;al., 1996</xref>; <xref ref-type="bibr" rid="B32">Humphreys et&#xa0;al., 2018</xref>; <xref ref-type="bibr" rid="B82">Stock et&#xa0;al., 2020</xref>). The surface ocean DIC concentrations increased during the 20<sup>th</sup> century due to the uptake of anthropogenic carbon (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4D</bold>
</xref>) (<xref ref-type="bibr" rid="B94">Wanninkhof et&#xa0;al., 2010</xref>; <xref ref-type="bibr" rid="B36">Jiang et&#xa0;al., 2023</xref>; <xref ref-type="bibr" rid="B40">Keppler et&#xa0;al., 2023</xref>; <xref ref-type="bibr" rid="B50">Ma et&#xa0;al., 2023</xref>). In the high emission scenario, the atmospheric <italic>p</italic>CO<sub>2</sub> levels continue to increase and the surface ocean DIC generally follows the atmospheric forcing trend (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4D, G</bold>
</xref>). However, there are significant model differences in the surface DIC future trajectories. CESM2, for example, stands out for its weak DIC increase even in the highest emission scenario during the late 21<sup>st</sup> century (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4D</bold>
</xref>). A weakened biological pump may potentially explain the reduced ocean carbon uptake (<xref ref-type="bibr" rid="B64">Passow and Carlson, 2012</xref>; <xref ref-type="bibr" rid="B2">Barange et&#xa0;al., 2017</xref>), as a weakened export of organic matter from the surface ocean would leave behind higher DIC concentrations (<xref ref-type="bibr" rid="B89">Tian et&#xa0;al., 2015</xref>).</p>
<p>We complete this work by presenting the inter-model correlations of variables which reveal diverging behaviors among the ten models (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5</bold>
</xref>). There is generally a strong positive correlation between changes in ALK and SSS which are both declining in tandem, due to freshwater influences and weakened transport of saline subtropical waters to the SPNA region (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5A</bold>
</xref>) (<xref ref-type="bibr" rid="B45">Lauvset and Gruber, 2014</xref>). The ALK dependence extends to the AMOC, as a decrease in AMOC strength is associated with a reduction in ALK (<xref ref-type="fig" rid="f5">
<bold>Figure&#xa0;5B</bold>
</xref>). These alterations in ALK appear to moderately affect the ocean&#x2019;s capacity for carbon uptake (<xref ref-type="bibr" rid="B86">Takahashi et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B58">Middelburg et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B13">Chikamoto et&#xa0;al., 2023</xref>). The findings suggest that the interplay between AMOC and ALK is significant, as AMOC&#x2019;s role in transporting chemically distinct water masses directly impacts ALK levels, which in turn, indirectly influence the CO<sub>2</sub> sequestration capabilities of the ocean. Consistent with our work, previous studies have established that models simulating lower present-day SSS in the SPNA tend to reduce future carbon absorption (<xref ref-type="bibr" rid="B21">Estella-Perez et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B63">Park et&#xa0;al., 2023</xref>). As our results indicate, the likelihood that SSS and ALK will diminish in the future is very high, and consequently, the SPNA will not help mitigate global warming given the substantial reduction in its ability to uptake CO<sub>2</sub>.</p>
</sec>
<sec id="s4_2">
<label>4.2</label>
<title>Modal prediction reliability</title>
<p>This work analyzed CMIP6 models with the goal of identifying processes or quantities that could help us distinguish among behaviors that are indicative of the future evolution of ocean circulation and carbon cycling in the SPNA. There is indeed an urgent need to better quantify the carbon dioxide removal potential in the ocean.</p>
<p>In summary, this study underscores the complex relationship among AMOC dynamics, ALK, surface ocean salinity and the ocean&#x2019;s capacity to uptake atmospheric carbon, offering insights into the intricate interactions between physical variables in SPNA. Despite the different extent of the decline in AMOC in the ten of the CMIP6 models considered, all models agree on the trend direction (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4A</bold>
</xref>). A stronger AMOC slowdown correlates with less ocean carbon uptake (<xref ref-type="bibr" rid="B73">Schmittner and Galbraith, 2008</xref>; <xref ref-type="bibr" rid="B59">Nielsen et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B38">Katavouta and Williams, 2021</xref>). This study emphasized the relatively underappreciated role of diminishing ALK and its impact on regional carbon uptake. Despite the complexity of the relationships among the variables analyzed, it clearly emerges that changes in ALK are an important factor in the oceanic absorption of CO<sub>2</sub> (<xref ref-type="bibr" rid="B86">Takahashi et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B58">Middelburg et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B13">Chikamoto et&#xa0;al., 2023</xref>). Moving forward, a deeper dive into the mechanistic links between these variables is imperative to enhance our understanding of their collective impact on the carbon cycle within the Earth&#x2019;s climate system.</p>
<p>Observations are still limited, while being the best tool to identify specific quantities and relationships in both physics and biogeochemistry. Model simulations will continue to serve as a key tool to understand ocean physics and biogeochemistry under changing climate (<xref ref-type="bibr" rid="B57">Menary et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B82">Stock et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B95">Weijer et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B85">Swingedouw et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B71">Robson et&#xa0;al., 2022</xref>). The role of the biological pump on carbon uptake and its future evolution remains largely uncertain (<xref ref-type="bibr" rid="B58">Middelburg et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B76">Seferian et&#xa0;al., 2020</xref>). More work is needed to better understand what drives the observed export of particle organic carbon and why models generally misrepresent both mean and variability. A better characterization of the biological pump and of carbon export will enhance our ability to predict the evolution of the marine ecosystem in the SPNA and is especially important considering the monitoring, reporting, and verification (MRV) required for the deployment of carbon removal technologies.</p>
<p>As final note of caution, we should keep in mind that all climate models present biases that limit their reliability, and the robustness of common behaviors could be tested paying attention to the outliers. For instance, in our analysis ACCESS-ESM1-5 stands out for its strong correlation of carbon uptake with ALK or SST (<xref ref-type="fig" rid="f5">
<bold>Figures&#xa0;5C, D</bold>
</xref>), possibly indicating an anomaly or significant deviation in the model&#x2019;s simulation relative to others. This could be due to unique model parameterizations, sensitivities to specific inputs, or how ACCESS-ESM1-5 simulates the interactions between oceanic processes and the carbon cycle (<xref ref-type="bibr" rid="B103">Ziehn et&#xa0;al., 2020</xref>). To understand the cause of this outlier behavior, a detailed examination of the model&#x2019;s internal processes and assumptions is necessary, which may involve a closer look at the representation of ocean chemistry, circulation patterns, and their response to changing climatic conditions. Further diagnostic studies comparing ACCESS-ESM1-5 with other models and observational data would be beneficial to determine the reasons behind its distinctive response.</p>
</sec>
</sec>
<sec id="s5" sec-type="data-availability">
<title>Data availability statement</title>
<p>The original contributions presented in the study are included in the article/<xref ref-type="supplementary-material" rid="SM1">
<bold>Supplementary Material</bold>
</xref>. Further inquiries can be directed to the corresponding author.</p>
</sec>
<sec id="s6" sec-type="author-contributions">
<title>Author contributions</title>
<p>QZ: Conceptualization, Data curation, Software, Validation, Visualization, Writing &#x2013; original draft, Writing &#x2013; review &amp; editing, Methodology. TI: Conceptualization, Formal analysis, Funding acquisition, Methodology, Software, Supervision, Validation, Writing &#x2013; review &amp; editing. AB: Conceptualization, Formal analysis, Funding acquisition, Methodology, Supervision, Validation, Writing &#x2013; review &amp; editing.</p>
</sec>
</body>
<back>
<sec id="s7" sec-type="funding-information">
<title>Funding</title>
<p>The author(s) declare financial support was received for the research, authorship, and/or publication of this article. The study was funded by the U.S. Department of Energy (DE-SC0021300).</p>
</sec>
<ack>
<title>Acknowledgments</title>
<p>We acknowledge the World Climate Research Programme, which, through its Working Group on Coupled Modelling, coordinated and promoted CMIP6. We thank the climate modeling groups for producing and making available their model output, the Earth System Grid Federation (ESGF) for archiving the data and providing access, and the multiple funding agencies who support CMIP6 and ESGF. We acknowledge the support by the U.S. Department of Energy, through grant DE-SC0021300. The Generic Mapping Tools open-access software was used to produce the map in this paper.</p>
</ack>
<sec id="s8" sec-type="COI-statement">
<title>Conflict of interest</title>
<p>The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.</p>
</sec>
<sec id="s9" sec-type="disclaimer">
<title>Publisher&#x2019;s note</title>
<p>All claims expressed in this article are solely those of the authors and do not necessarily represent those of their affiliated organizations, or those of the publisher, the editors and the reviewers. Any product that may be evaluated in this article, or claim that may be made by its manufacturer, is not guaranteed or endorsed by the publisher.</p>
</sec>
<sec id="s10" sec-type="supplementary-material">
<title>Supplementary material</title>
<p>The Supplementary Material for this article can be found online at: <ext-link ext-link-type="uri" xlink:href="https://www.frontiersin.org/articles/10.3389/fmars.2024.1304193/full#supplementary-material">https://www.frontiersin.org/articles/10.3389/fmars.2024.1304193/full#supplementary-material</ext-link>
</p>
<supplementary-material xlink:href="Image_1.pdf" id="SM1" mimetype="application/pdf"/>
</sec>
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