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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.2023.1197977</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>Spatial symmetry and contrasting controls of surface pH and aragonite saturation state in the western North Pacific</article-title>
</title-group>
<contrib-group>
<contrib contrib-type="author">
<name>
<surname>Li</surname>
<given-names>Cheng-long</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/1052160"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Wu</surname>
<given-names>Yingxu</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/1155128"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Chen</surname>
<given-names>Kui</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Lin</surname>
<given-names>Hongmei</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Chen</surname>
<given-names>Liqi</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/686739"/>
</contrib>
<contrib contrib-type="author" corresp="yes">
<name>
<surname>Qi</surname>
<given-names>Di</given-names>
</name>
<xref ref-type="aff" rid="aff1">
<sup>1</sup>
</xref>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
<xref ref-type="author-notes" rid="fn001">
<sup>*</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/1781205"/>
</contrib>
</contrib-group>
<aff id="aff1">
<sup>1</sup>
<institution>Polar and Marine Research Institute, Jimei University</institution>, <addr-line>Xiamen</addr-line>, <country>China</country>
</aff>
<aff id="aff2">
<sup>2</sup>
<institution>Key Laboratory of Global Change and Marine-Atmospheric Chemistry of Ministry of Natural Resources (MNR), Third Institute of Oceanography, MNR</institution>, <addr-line>Xiamen</addr-line>, <country>China</country>
</aff>
<author-notes>
<fn fn-type="edited-by">
<p>Edited by: Khan M. G. Mostofa, Tianjin University, China</p>
</fn>
<fn fn-type="edited-by">
<p>Reviewed by: Li-Qing Jiang, University of Maryland, College Park, United States; Ruifeng Zhang, Shanghai Jiao Tong University, China</p>
</fn>
<fn fn-type="corresp" id="fn001">
<p>*Correspondence: Di Qi, <email xlink:href="mailto:qidi@jmu.edu.cn">qidi@jmu.edu.cn</email>
</p>
</fn>
</author-notes>
<pub-date pub-type="epub">
<day>01</day>
<month>12</month>
<year>2023</year>
</pub-date>
<pub-date pub-type="collection">
<year>2023</year>
</pub-date>
<volume>10</volume>
<elocation-id>1197977</elocation-id>
<history>
<date date-type="received">
<day>31</day>
<month>03</month>
<year>2023</year>
</date>
<date date-type="accepted">
<day>15</day>
<month>11</month>
<year>2023</year>
</date>
</history>
<permissions>
<copyright-statement>Copyright &#xa9; 2023 Li, Wu, Chen, Lin, Chen and Qi</copyright-statement>
<copyright-year>2023</copyright-year>
<copyright-holder>Li, Wu, Chen, Lin, Chen and Qi</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>Oceanic uptake of anthropogenic CO<sub>2</sub> causes a decrease in seawater pH and aragonite saturation state (&#x3a9;<sub>arag</sub>), a process known as ocean acidification (OA). The western North Pacific is a hotspot for anthropogenic CO<sub>2</sub> sinks; however, the spatiotemporal variability of pH and &#x3a9;<sub>arag</sub> and their controlling mechanisms remain unexplored. In this study, we provide high-frequency and high-precision underway measurements of sea surface <italic>p</italic>CO<sub>2</sub> and pH to investigate the distribution and drivers of OA metrics across different hydrochemical gradients in the western North Pacific in late spring 2018, a season with the highest primary production in the year. Our results show that the surface pH reached near air-sea equilibrium in the subtropical zone but gradually increased northward across the Kuroshio Recirculation (KR) zone and peaked in the Kuroshio Extension (KE) zone. We found that sea surface temperature played the most prominent role in regulating pH, which was also counteracted by the effects of air&#x2013;sea gas exchange and vertical mixing. In contrast, the distribution of &#x3a9;<sub>arag</sub> largely mirrored the pH and was governed by air&#x2013;sea gas exchange and vertical mixing, the effects of which on &#x3a9;<sub>arag</sub> were enhanced by temperature. Biological activity thrived in the KE zone to increase both pH and &#x3a9;<sub>arag</sub>, which further reinforced the latitudinal pattern of pH, but weakened that of &#x3a9;<sub>arag</sub>. These findings are based on direct <italic>in situ</italic> measurements of pH and improve our understanding of the spatiotemporal variability of OA metrics in the western North Pacific region.</p>
</abstract>
<kwd-group>
<kwd>ocean acidification</kwd>
<kwd>underway pH</kwd>
<kwd>aragonite saturation state</kwd>
<kwd>temperature effect</kwd>
<kwd>western North Pacific</kwd>
</kwd-group>
<counts>
<fig-count count="6"/>
<table-count count="1"/>
<equation-count count="3"/>
<ref-count count="62"/>
<page-count count="13"/>
<word-count count="5893"/>
</counts>
<custom-meta-wrap>
<custom-meta>
<meta-name>section-in-acceptance</meta-name>
<meta-value>Marine Biogeochemistry</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 ocean absorbs approximately a quarter of the anthropogenic CO<sub>2</sub> emissions annually, effectively alleviating global climate change (<xref ref-type="bibr" rid="B17">Gruber et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B16">Friedlingstein et&#xa0;al., 2022</xref>). However, absorbed anthropogenic CO<sub>2</sub> causes a decrease in seawater pH and aragonite saturation state (&#x3a9;<sub>arag</sub>), a process commonly known as ocean acidification (OA) (<xref ref-type="bibr" rid="B9">Doney et&#xa0;al., 2009</xref>; <xref ref-type="bibr" rid="B14">Feely et&#xa0;al., 2009</xref>), which endangers marine organisms and ecosystems (<xref ref-type="bibr" rid="B45">Orr et&#xa0;al., 2005</xref>; <xref ref-type="bibr" rid="B53">Waldbusser et&#xa0;al., 2015</xref>; <xref ref-type="bibr" rid="B10">Doney et&#xa0;al., 2020</xref>). In general, the decline rates of global open ocean surface OA metrics (e.g., pH and &#x3a9;<sub>arag</sub>) have followed an increase in atmospheric CO<sub>2</sub> over the past few decades (<xref ref-type="bibr" rid="B2">Bates et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B49">Takahashi et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B26">Jiang et&#xa0;al., 2023</xref>). Efforts have been made to investigate the global or hemispheric-scale distributions of OA metrics and their controlling processes (e.g., <xref ref-type="bibr" rid="B49">Takahashi et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B24">Jiang et&#xa0;al., 2015</xref>; <xref ref-type="bibr" rid="B12">Fassbender et&#xa0;al., 2017</xref>; <xref ref-type="bibr" rid="B33">Lauvset et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B57">Wu et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B59">Xue et&#xa0;al., 2021</xref>). These studies have suggested that the spatiotemporal variabilities and drivers of OA metrics are geographically diverse due to regional differences in physical and biogeochemical processes, primarily related to the combined effects of temperature, air&#x2013;sea gas exchange, water mixing, biological activity, and sea ice melt.</p>
<p>The western North Pacific, a highly dynamic region that includes the Kuroshio Extension (KE), Kuroshio Recirculation (KR), and southern subtropical regions (<xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1A</bold>
</xref>), is the largest annual net CO<sub>2</sub> sink in the Pacific Ocean (<xref ref-type="bibr" rid="B50">Takahashi et&#xa0;al., 2009</xref>). Seasonally, the KE and KR waters are CO<sub>2</sub> sinks in winter&#x2013;spring and weak sources in summer&#x2013;autumn, mainly driven by seasonal temperature variations (<xref ref-type="bibr" rid="B51">Takahashi et&#xa0;al., 2002</xref>). Consequently, the surface OA metrics in the KE and KR waters also showed significant seasonal variations, mainly controlled by temperature and its induced air&#x2013;sea gas exchange (<xref ref-type="bibr" rid="B21">Ishii et&#xa0;al., 2011</xref>; <xref ref-type="bibr" rid="B27">Kim et&#xa0;al., 2015</xref>). In general, the OA metrics in the southern subtropical region are annually in equilibrium with atmospheric CO<sub>2</sub> (<xref ref-type="bibr" rid="B44">Ono et&#xa0;al., 2019</xref>), whereas the spatial variability and drivers of OA metrics across the KE, KR, and southern subtropical regions remain poorly constrained.</p>
<fig id="f1" position="float">
<label>Figure&#xa0;1</label>
<caption>
<p>
<bold>(A)</bold> Sampling sites in the western North Pacific during May&#x2013;June 2018. Squares and diamonds represent CTD and underway sampling stations, respectively. The color indicates the monthly mean sea surface temperature (SST) in May 2018. The approximate locations of the Oyashio, Kuroshio, Kuroshio Extension (KE), Kuroshio Recirculation (KR), Subtropical Countercurrent (STCC), Kuroshio front (KF) and subtropical front (SF) were also sketched (<xref ref-type="bibr" rid="B30">Kobashi et&#xa0;al., 2006</xref>). <bold>(B)</bold> Monthly mean mixed layer depth (MLD) in May 2018 and cruise tracks (black lines). <bold>(C&#x2212;H)</bold> Monthly mean chlorophyll <italic>a</italic> (Chl <italic>a</italic>) concentrations from January to November 2018. SST, MLD, and Chl <italic>a</italic> were obtained from the website (<uri xlink:href="https://marine.copernicus.eu">https://marine.copernicus.eu</uri>).</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-10-1197977-g001.tif"/>
</fig>
<p>To investigate the spatial distributions and their controls on the OA metrics across the large temperature and physical and biological gradients in the western North Pacific (<xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1</bold>
</xref>), we simultaneously measured the underway sea surface pH and partial pressure of CO<sub>2</sub> (<italic>p</italic>CO<sub>2</sub>), with other auxiliary parameters in late spring 2018 (<xref ref-type="fig" rid="f1">
<bold>Figures&#xa0;1A, B</bold>
</xref>). During the cruise, we also investigated discrete carbonate parameters in surface waters for data comparison and validation (<xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1</bold>
</xref>). In addition, chlorophyll <italic>a</italic> (Chl <italic>a</italic>) data from satellites in 2018 were used to validate the underway Chl <italic>a</italic> and indicate seasonal variations in primary production (<xref ref-type="fig" rid="f1">
<bold>Figures&#xa0;1C&#x2013;H</bold>
</xref>). The objectives of this study were to (1) provide high-frequency-precision distributions of pH and &#x3a9;<sub>arag</sub>, (2) elucidate the spatial variations of pH and &#x3a9;<sub>arag</sub> and their controlling factors (e.g., temperature effect, air&#x2013;sea exchange, biological activities, and water mixing), and (3) quantify the contribution of these factors to the spatial variations of pH and &#x3a9;<sub>arag</sub>.</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>Study area</title>
<p>The surveying area was divided into three zones from north to south by the Kuroshio front (~35&#xb0;N) and the subtropical front (~27&#xb0;N), such as the KE (35&#xb0;&#x2212;39&#xb0;N), KR (27&#xb0;&#x2212;35&#xb0;N) and subtropical (21&#xb0;&#x2212;27&#xb0;N) zones (<xref ref-type="bibr" rid="B30">Kobashi et&#xa0;al., 2006</xref>; <xref ref-type="bibr" rid="B43">Oka et&#xa0;al., 2018</xref>; <xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1A</bold>
</xref>). The western North Pacific is stired by two strong Pacific western boundary currents: the Kuroshio and Oyashio. The southward-flowing Oyashio Current carries the low-salinity/cold subarctic water and meets the high-salinity/warm Kuroshio water (<xref ref-type="bibr" rid="B61">Yasuda et&#xa0;al., 1996</xref>) to form the interfrontal zone with a relatively high Chl <italic>a</italic> concentration in spring (<xref ref-type="fig" rid="f1">
<bold>Figures&#xa0;1C-H</bold>
</xref>). The northeastward-flowing Kuroshio Current separates from the coast of Japan at approximately 35&#xb0;N, 140&#xb0;E and turns eastward (<xref ref-type="bibr" rid="B47">Qiu and Chen, 2011</xref>), forming the KE (<xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1A</bold>
</xref>). South of the KE, the KR has a deepened mixed layer in winter owing to oceanic heat loss to the atmosphere (<xref ref-type="bibr" rid="B28">Kitamura et&#xa0;al., 2016</xref>). Even in late spring, the mixed layer depth (MLD) in the KR and KE zones was deeper than that in the subtropical zone (<xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1B</bold>
</xref>). In winter and spring, sea surface heat loss causes surface <italic>p</italic>CO<sub>2</sub> to be significantly lower than the air-equilibrated value in the KE and KR zones; thus, the region is a strong net annual CO<sub>2</sub> sink (<xref ref-type="bibr" rid="B50">Takahashi et&#xa0;al., 2009</xref>; <xref ref-type="bibr" rid="B36">Li et&#xa0;al., 2022a</xref>). Further south of the KR, an eastward-flowing Subtropical Countercurrent (STCC) occupies the area (<xref ref-type="bibr" rid="B63">Yoshida and Kidokoro, 1967</xref>).</p>
</sec>
<sec id="s2_2">
<label>2.2</label>
<title>Underway observations</title>
<p>The survey was conducted in the western North Pacific onboard R/V <italic>Xiangyanghong</italic> 3 from 10 May to 7 June 2018 (<xref ref-type="fig" rid="f1">
<bold>Figures&#xa0;1A, B</bold>
</xref>). We conducted pumping analyses of sea surface temperature (SST), salinity, fluorescence, pH and <italic>p</italic>CO<sub>2</sub>. The seawater sample was pumped approximately ~5 m below the sea surface. The underway SST was recorded every 5 s along the cruise path using an onboard SeaBird flow-through thermosalinograph (SBE 38, Sea-Bird Scientific, USA). An automated flow measuring system (AS-P2, Apollo SciTech, Inc., USA) was used for sea surface salinity (SSS), fluorescence, pH, and <italic>p</italic>CO<sub>2</sub> analyses, which were recorded continuously every 29 s along the cruise track.</p>
<p>A Honeywell Durafet<sup>&#xae;</sup> pH sensor was used to measure the pH of the flowing water. The Durafet pH electrode features an integral automatic temperature compensator in a one-piece construction and is suitable for varying pH and temperature ranges. The Durafet pH electrode was calibrated using three standard buffers (pH<sub>NBS</sub> = 4.01, 7.00 and 10.01 at 25.0&#xb0;C, Thermo Fisher Scientific Inc., USA). NBS stands for the National Bureau of Standards, which is now the National Institute of Standards and Technology of the U.S. Department of Commerce. The Durafet pH sensor operates with a short-term precision of &#xb1;0.0005 pH over periods of several hours and exhibits stability better than 0.005 pH over periods of weeks to months (<xref ref-type="bibr" rid="B40">Martz et&#xa0;al., 2010</xref>). Considering that the Durafet-electrode temperature was slightly different from the SST due to the effects of water pumping and room temperature, a temperature-dependent coefficient of 0.0128 pH &#xb0;C<sup>&#x2212;1</sup> was derived from the surface waters in the cruise by varying the temperature from 15.0 to 30.0&#xb0;C at a salinity of 34.6, TA of 2,268 &#x3bc;mol kg<sup>&#x2212;1</sup>, and DIC of 1,966 &#x3bc;mol kg<sup>&#x2212;1</sup>. Thus, the coefficient was used to calculate the sea surface pH (pH <sup>in_situ</sup>) as,</p>
<disp-formula>
<label>(1)</label>
<mml:math display="block" id="M1">
<mml:mrow>
<mml:msup>
<mml:mrow>
<mml:mtext>pH</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mtext>in</mml:mtext>
<mml:mo>_</mml:mo>
<mml:mtext>situ</mml:mtext>
</mml:mrow>
</mml:msup>
<mml:mo>=</mml:mo>
<mml:msup>
<mml:mrow>
<mml:mtext>pH</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mtext>Durafet</mml:mtext>
</mml:mrow>
</mml:msup>
<mml:mo>&#x2212;</mml:mo>
<mml:mn>0.0128</mml:mn>
<mml:mo>&#xd7;</mml:mo>
<mml:mo stretchy="false">(</mml:mo>
<mml:mtext>SST</mml:mtext>
<mml:mo>&#x2212;</mml:mo>
<mml:msup>
<mml:mtext>T</mml:mtext>
<mml:mrow>
<mml:mtext>Durafet</mml:mtext>
</mml:mrow>
</mml:msup>
<mml:mo stretchy="false">)</mml:mo>
</mml:mrow>
</mml:math>
</disp-formula>
<p>where pH<sup>Durafet</sup> and T<sup>Durafet</sup> are Durafet pH and temperature in the system, respectively.</p>
<p>Chl <italic>a</italic> was translated from underway water fluorescence and validated against field-measured Chl <italic>a</italic> (<xref ref-type="bibr" rid="B36">Li et&#xa0;al., 2022a</xref>). The underway <italic>p</italic>CO<sub>2</sub> measurement and calibration were described in detail by <xref ref-type="bibr" rid="B36">Li et&#xa0;al. (2022a)</xref>, and the overall uncertainty of <italic>p</italic>CO<sub>2</sub> was less than 1%.</p>
</sec>
<sec id="s2_3">
<label>2.3</label>
<title>Discrete sampling and analyses</title>
<p>Discrete water samples for dissolved oxygen (DO), dissolved inorganic carbon (DIC), and total alkalinity (TA) were collected using 10-L Niskin bottles at a surface layer of ~2 m. Depth profiles of temperature and salinity (Practical Salinity Scale of 1978) were obtained using calibrated conductivity-temperature-depth/pressure (CTD) probes (SBE911 plus, Sea-Bird Scientific, USA).</p>
<p>Water samples for DO analyses were collected, fixed, and titrated onboard the vessel following the classic Winkler procedure (<xref ref-type="bibr" rid="B29">Knap et&#xa0;al., 1996</xref>). Any potential nitrite interference in DO titration was removed by adding 0.01% NaN<sub>3</sub> during subsample fixation (<xref ref-type="bibr" rid="B55">Wong, 2012</xref>). To quantify the effects of net community metabolism, the apparent oxygen utilization (AOU) was calculated by subtracting the field-measured DO concentration from the air-equilibrated DO concentration. Assuming that DO was initially in equilibrium with the atmosphere, an AOU &gt;0 implies net community respiration, whereas an AOU&lt;0 implies net community production.</p>
<p>Following the procedure recommended by <xref ref-type="bibr" rid="B7">Dickson et&#xa0;al. (2007)</xref>, water samples for DIC and TA analyses were collected and stored in 250 mL borosilicate glass bottles. Prior to sealing with greased (Apiezon-L) ground-glass stoppers, 1 mL of seawater was removed from each sample bottle to allow for thermal expansion and 100 &#xb5;L of saturated HgCl<sub>2</sub> was added to the water samples to halt biological activity. The samples were then stored at room temperature until further analysis. DIC was measured using an infrared CO<sub>2</sub> detector-based DIC analyzer (AS-C3, Apollo SciTech Inc., USA), and TA was determined at 25.0 &#xb0;C by Gran&#x2019;s acidimetric titration using a semi-automated titrator (AS-ALK2, Apollo SciTech Inc., USA). The reproducibility of the DIC and TA measurements was within 0.1% (<xref ref-type="bibr" rid="B5">Cai et&#xa0;al., 2004</xref>). DIC and TA measurements were referenced to certified reference materials from the laboratory of Andrew G. Dickson (Scripps Institute of Oceanography, USA), with a precision of &#xb1;2 &#xb5;mol kg<sup>&#x2212;1</sup>.</p>
</sec>
<sec id="s2_4">
<label>2.4</label>
<title>Calculation of carbonate parameters</title>
<p>For discrete samples, <italic>p</italic>CO<sub>2</sub>, &#x3a9;<sub>arag</sub>, and NBS scale pH (pH<sub>NBS</sub>; for simplicity, &#x2018;pH&#x2019; in the following text refers to the NBS scale) were calculated from DIC, TA, seawater temperature, salinity, and pressure values using CO2SYS.xls (version 24) (<xref ref-type="bibr" rid="B46">Pelletier et&#xa0;al., 2015</xref>), an updated version of the original CO2SYS.EXE (<xref ref-type="bibr" rid="B34">Lewis and Wallace, 1998</xref>). Here, &#x3a9;<sub>arag</sub> is defined as the product of calcium (Ca<sup>2+</sup>) and carbonate (CO<sub>3</sub>
<sup>2&#x2212;</sup>) ion concentrations divided by the apparent solubility product for aragonite (<italic>K</italic>
<sub>sp</sub>*<sub>arag</sub>), i.e., &#x3a9;<sub>arag</sub> = [Ca<sup>2+</sup>] &#xd7; [CO<sub>3</sub>
<sup>2&#x2212;</sup>]/<italic>K</italic>
<sub>sp</sub>*<sub>arag</sub>. The DIC and &#x3a9;<sub>arag</sub> values were calculated using the program from the underway <italic>p</italic>CO<sub>2</sub>, salinity-based TA (<xref ref-type="fig" rid="f2">
<bold>Figure&#xa0;2A</bold>
</xref>), and other auxiliary parameters. The carbonic acid dissociation constants from <xref ref-type="bibr" rid="B41">Millero et&#xa0;al. (2006)</xref>, total boron/salinity (B<sub>T</sub>/S) from <xref ref-type="bibr" rid="B52">Uppstr&#xf6;m (1974)</xref>, and dissociation constant of HSO<sub>4</sub>
<sup>&#x2212;</sup> from <xref ref-type="bibr" rid="B8">Dickson (1990)</xref> were used to calculate the carbonate system parameters. Although the carbonic acid dissociation constants of Luecker et&#xa0;al. (2000) and the B<sub>T</sub>/S of <xref ref-type="bibr" rid="B35">Lee et&#xa0;al. (2010)</xref> are recommended (<xref ref-type="bibr" rid="B56">Woosley, 2021</xref>; <xref ref-type="bibr" rid="B25">Jiang et&#xa0;al., 2022</xref>), <xref ref-type="bibr" rid="B36">Li et&#xa0;al. (2022a)</xref> found that the measured <italic>p</italic>CO<sub>2</sub> in the western North Pacific agreed with the values calculated from the combination of <xref ref-type="bibr" rid="B41">Millero et&#xa0;al. (2006)</xref> and <xref ref-type="bibr" rid="B52">Uppstr&#xf6;m (1974)</xref>. The measured <italic>p</italic>CO<sub>2</sub> was approximately 8 &#x3bc;atm lower than the calculated values when using the combination of <xref ref-type="bibr" rid="B39">Lueker et&#xa0;al. (2000)</xref> and <xref ref-type="bibr" rid="B35">Lee et&#xa0;al. (2010)</xref>. During the calculation, the surface phosphate and silicate concentrations required by the program were replaced with zero. Given that surface phosphate and silicate concentrations in the surveying area are typically very low (&lt;0.1 &#x3bc;mol kg<sup>&#x2212;1</sup> and&lt;1 &#x3bc;mol kg<sup>&#x2212;1</sup>, respectively) (<xref ref-type="bibr" rid="B37">Li et&#xa0;al., 2022b</xref>), ignoring these nutrients results in minor errors in <italic>p</italic>CO<sub>2</sub> (0.2 &#x3bc;atm), pH (0.0002), and &#x3a9;<sub>arag</sub> (0.0005) values.</p>
<fig id="f2" position="float">
<label>Figure&#xa0;2</label>
<caption>
<p>
<bold>(A)</bold> Sea surface salinity (SSS) versus TA, <bold>(B)</bold> underway <italic>p</italic>CO<sub>2</sub> (<italic>p</italic>CO<sub>2</sub>
<sup>UW</sup>) versus calculated <italic>p</italic>CO<sub>2</sub> from DIC and TA (<italic>p</italic>CO<sub>2</sub>
<sup>DIC-TA</sup>), <bold>(C)</bold> calculated &#x3a9;<sub>arag</sub> from DIC and TA (&#x3a9;<sub>arag</sub> <sup>DIC-TA</sup>) versus calculated &#x3a9;<sub>arag</sub> from <italic>p</italic>CO<sub>2</sub>
<sup>UW</sup> and SSS-based TA (TA<sup>SSS</sup>), <bold>(D)</bold> underway pH (pH<sup>UW</sup>) versus calculated pH from DIC and TA (pH<sup>DIC-TA</sup>), <bold>(E&#x2212;H)</bold> differnce between pH<sup>DIC-TA</sup> and pH<sup>UW</sup> versus temperature, salinity, chlorophyll <italic>a</italic> (Chl <italic>a</italic>), and cruise time (day), respectively, <bold>(I)</bold> corrected pH<sup>UW</sup> versus pH<sup>DIC-TA</sup> at stations.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-10-1197977-g002.tif"/>
</fig>
<p>To eliminate the dilution and concentration effects of precipitation and evaporation on the seawater carbonate system, we normalized the water TA (NTA) and DIC (NDIC) to a uniform salinity of 35. Salinity-normalized parameters were calculated as NTA = TA &#xd7; 35/salinity and NDIC = DIC &#xd7; 35/salinity. The temperature normalized <italic>p</italic>CO<sub>2</sub> at 28.0&#xb0;C was calculated by <italic>p</italic>CO<sub>2</sub>
<sup>28.0&#xb0;C</sup> (&#x3bc;atm) = <italic>p</italic>CO<sub>2</sub> &#xd7; e<sup>[0.0423 &#xd7; (28.0&#x2212;SST)]</sup> (<xref ref-type="bibr" rid="B51">Takahashi et&#xa0;al., 2002</xref>).</p>
</sec>
<sec id="s2_5">
<label>2.5</label>
<title>Quality-control of carbonate parameters</title>
<p>Durafet pH has a constrained uncertainty of 0.005 (<xref ref-type="bibr" rid="B40">Martz et&#xa0;al., 2010</xref>) and is therefore used as a reference to assess the quality of the underway and calculate the pH data. To further assess the quality of the underway pH/<italic>p</italic>CO<sub>2</sub> and discrete DIC/TA datasets, the underway pH/<italic>p</italic>CO<sub>2</sub> (pH<sup>UW</sup>/<italic>p</italic>CO<sub>2</sub>
<sup>UW</sup>) data collected at the stations were compared to the calculated pH/<italic>p</italic>CO<sub>2</sub> from the measured DIC and TA (pH<sup>DIC-TA</sup>/<italic>p</italic>CO<sub>2</sub>
<sup>DIC-TA</sup>). The &#x3a9;<sub>arag</sub> values calculated from DIC and TA (&#x3a9;<sub>arag</sub>
<sup>DIC-TA</sup>) were compared with those calculated from <italic>p</italic>CO<sub>2</sub>
<sup>UW</sup> and salinity-based TA (&#x3a9;<sub>arag</sub>
<italic>
<sup>p</sup>
</italic>
<sup>CO2UW-TAsss</sup>). The results showed that <italic>p</italic>CO<sub>2</sub>
<sup>UW</sup> versus <italic>p</italic>CO<sub>2</sub>
<sup>DIC-TA</sup> and &#x3a9;<sub>arag</sub>
<sup>DIC-TA</sup> versus &#x3a9;<sub>arag</sub>
<italic>
<sup>p</sup>
</italic>
<sup>CO2UW-TAsss</sup> agreed with each other, following a 1:1 line within &#xb1;6 &#x3bc;atm for <italic>p</italic>CO<sub>2</sub> and &#xb1;0.03 for &#x3a9;<sub>arag</sub> (n = 66), respectively (<xref ref-type="fig" rid="f2">
<bold>Figures&#xa0;2B, C</bold>
</xref>). These comparisons indicate that the measured and calculated <italic>p</italic>CO<sub>2</sub>, DIC, TA and &#x3a9;<sub>arag</sub> results were reliable.</p>
<p>However, the pH<sup>UW</sup> value was lower than that of pH<sup>DIC-TA</sup> by 0.015 &#xb1; 0.004 (n = 66) (<xref ref-type="fig" rid="f2">
<bold>Figure&#xa0;2D</bold>
</xref>), which was higher than the uncertainty of Durafet pH. We found that the differences between pH<sup>DIC-TA</sup> and pH<sup>UW</sup> were discrete relative to SST, SSS, and Chl <italic>a</italic> (<xref ref-type="fig" rid="f2">
<bold>Figures&#xa0;2E&#x2013;G</bold>
</xref>), but were significantly related to cruise time (day) (<xref ref-type="fig" rid="f2">
<bold>Figure&#xa0;2H</bold>
</xref>), indicating that the Durafet pH electrode had a time-dependent baseline drift. Therefore, we corrected pH<sup>UW</sup> according to the linear relationship between the differences and cruise time. The results showed that the corrected pH<sup>UW</sup> and pH<sup>DIC-TA</sup> were consistent with each other, following a 1:1 line within &#xb1;0.004 (n = 66) (<xref ref-type="fig" rid="f2">
<bold>Figure&#xa0;2I</bold>
</xref>). Note that &#x2018;pH&#x2019; in the following text refers to corrected pH.</p>
</sec>
<sec id="s2_6">
<label>2.6</label>
<title>Decomposition of pH and &#x3a9;<sub>arag</sub> changes</title>
<p>In this study, we aimed to quantify the contribution of the controlling factors to &#x394;pH and &#x394;&#x3a9;<sub>arag</sub> in the western North Pacific. We used a systematic approach based on first-order Taylor series deconvolution (<xref ref-type="bibr" rid="B42">Murata and Shu, 2012</xref>; <xref ref-type="bibr" rid="B19">Hagens and Middelburg, 2016</xref>) to decompose the &#x394;pH and &#x394;&#x3a9;<sub>arag</sub> into the contributions of individual water chemistry parameter changes in temperature (&#x394;T), salinity (&#x394;S), NDIC (&#x394;NDIC), NTA (&#x394;NTA), and residual (Res). The residual term represents contributions from other acid&#x2013;base systems, although these may be negligible. Therefore, we used this method to decompose &#x394;pH and &#x394;&#x3a9;<sub>arag</sub> as follows,</p>
<disp-formula>
<label>(2)</label>
<mml:math display="block" id="M2">
<mml:mrow>
<mml:mi>&#x394;</mml:mi>
<mml:mi>V</mml:mi>
<mml:mo>=</mml:mo>
<mml:mo stretchy="false">(</mml:mo>
<mml:mi>&#x259;</mml:mi>
<mml:mi>V</mml:mi>
<mml:mo stretchy="false">/</mml:mo>
<mml:mi>&#x259;</mml:mi>
<mml:mtext>T</mml:mtext>
<mml:mo stretchy="false">)</mml:mo>
<mml:mi>&#x394;</mml:mi>
<mml:mtext>T</mml:mtext>
<mml:mo>+</mml:mo>
<mml:mo stretchy="false">(</mml:mo>
<mml:mi>&#x259;</mml:mi>
<mml:mi>V</mml:mi>
<mml:mo stretchy="false">/</mml:mo>
<mml:mi>&#x259;</mml:mi>
<mml:mtext>S</mml:mtext>
<mml:mo stretchy="false">)</mml:mo>
<mml:mi>&#x394;</mml:mi>
<mml:mtext>S</mml:mtext>
<mml:mo>+</mml:mo>
<mml:mo stretchy="false">(</mml:mo>
<mml:mi>&#x259;</mml:mi>
<mml:mi>V</mml:mi>
<mml:mo stretchy="false">/</mml:mo>
<mml:mi>&#x259;</mml:mi>
<mml:mtext>NDIC</mml:mtext>
<mml:mo stretchy="false">)</mml:mo>
<mml:mi>&#x394;</mml:mi>
<mml:mtext>NDIC</mml:mtext>
<mml:mo>+</mml:mo>
<mml:mo stretchy="false">(</mml:mo>
<mml:mi>&#x259;</mml:mi>
<mml:mi>V</mml:mi>
<mml:mo stretchy="false">/</mml:mo>
<mml:mi>&#x259;</mml:mi>
<mml:mtext>NTA</mml:mtext>
<mml:mo stretchy="false">)</mml:mo>
<mml:mi>&#x394;</mml:mi>
<mml:mtext>NTA</mml:mtext>
<mml:mo>+</mml:mo>
<mml:mtext>Res</mml:mtext>
</mml:mrow>
</mml:math>
</disp-formula>
<p>where <italic>V</italic> indicates the pH and &#x3a9;<sub>arag</sub>. &#x394;<italic>V</italic> was calculated from the real-time value relative to the mean value in the subtropical zone (temperature = 28.0&#xb0;C, salinity = 34.4, TA = 2,260 &#x3bc;mol kg<sup>&#x2212;1</sup> and DIC = 1,945 &#x3bc;mol kg<sup>&#x2212;1</sup>), where sea surface pH and &#x3a9;<sub>arag</sub> were close to the air equilibrium. &#x394;T, &#x394;S, &#x394;NDIC, and &#x394;NTA were calculated based on the differences in water chemistry parameters between the real-time and mean values in the subtropical zone. On the right-hand side of equation (2), four partial derivative terms were calculated based on the observed data, assuming a 1&#x2030; change in the relative parameters, while the other three parameters were held constant.</p>
</sec>
</sec>
<sec id="s3" sec-type="results">
<label>3</label>
<title>Results</title>
<sec id="s3_1">
<label>3.1</label>
<title>Environmental settings</title>
<p>The spatial distributions of SST and Chl <italic>a</italic> are shown in <xref ref-type="fig" rid="f3">
<bold>Figures&#xa0;3A, B</bold>
</xref>, and the variations in SST, SSS, Chl <italic>a</italic>, and AOU are shown in <xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4A, B</bold>
</xref>. Overall, SST, Chl <italic>a</italic>, and AOU showed strong spatial variations from the subtropical zone, through the KR zone, to the KE zone (<xref ref-type="fig" rid="f3">
<bold>Figures&#xa0;3A, B</bold>
</xref>, <xref ref-type="fig" rid="f4">
<bold>4A, B</bold>
</xref>). Briefly, SST decreased from 27.93&#xb0;C &#xb1; 0.99&#xb0;C in the subtropical zone to 22.65&#xb0;C &#xb1; 1.45&#xb0;C in the KR zone and to 18.27&#xb0;C &#xb1; 2.37&#xb0;C in the KE zone. This strong gradient may be related to oceanic heat loss due to the northeastward flow of the Kuroshio Current (<xref ref-type="bibr" rid="B47">Qiu and Chen, 2011</xref>; <xref ref-type="bibr" rid="B28">Kitamura et&#xa0;al., 2016</xref>). However, SSS varied within a limited range of 34&#x2212;35 in the open ocean of the surveyed area (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4A</bold>
</xref>). In the KE zone, the SSS was only slightly lower than that in the subtropical and KR zones, suggesting a limited influence of the low-salinity Oyashio current on the hydrological characteristics of the KE surface waters during the surveying cruise.</p>
<fig id="f3" position="float">
<label>Figure&#xa0;3</label>
<caption>
<p>Distributions of <bold>(A)</bold> underway sea surface temperature (SST, &#xb0;C), <bold>(B)</bold> chlorophyll <italic>a</italic> (Chl <italic>a</italic>, mg m<sup>&#x2212;3</sup>), <bold>(C)</bold> pH and <bold>(D)</bold> &#x3a9;<sub>arag</sub> during May&#x2013;June 2018. <bold>(A, B)</bold> were obtained from <xref ref-type="bibr" rid="B36">Li et&#xa0;al. (2022a)</xref>. Subtropical front, SF; Kuroshio front, KF.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-10-1197977-g003.tif"/>
</fig>
<fig id="f4" position="float">
<label>Figure&#xa0;4</label>
<caption>
<p>Underway and discrete sea surface <bold>(A)</bold> temperature (SST, &#xb0;C) and salinity (SSS), <bold>(B)</bold> chlorophyll <italic>a</italic> (Chl <italic>a</italic>, mg m<sup>&#x2212;3</sup>) and AOU (&#x3bc;mol kg<sup>&#x2212;1</sup>), <bold>(C)</bold> NDIC (&#x3bc;mol kg<sup>&#x2212;1</sup>), <bold>(D)</bold> <italic>in situ p</italic>CO<sub>2</sub> (&#x3bc;atm) and temperature normalized <italic>p</italic>CO<sub>2</sub> at 28.0 &#xb0;C (&#x3bc;atm), <bold>(E)</bold> pH and <bold>(F)</bold> &#x3a9;<sub>arag</sub> during May&#x2013;June 2018. Discrete parameters (blue dots) are collected from the stations. In <bold>(C&#x2212;F)</bold>, the red lines indicate the air-equilibrated values. Color shading indicates the subtropical, Kuroshio Recirculation (KR) and Kuroshio Extension (KE) zones, respectively. Subtropical front, SF; Kuroshio front, KF.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-10-1197977-g004.tif"/>
</fig>
<p>The Chl <italic>a</italic> concentration is relatively low at 0.2&#x2212;0.4 mg m<sup>&#x2212;3</sup> in the subtropical and KR zones (<xref ref-type="fig" rid="f3">
<bold>Figures&#xa0;3B</bold>
</xref>, <xref ref-type="fig" rid="f4">
<bold>4B</bold>
</xref>) due to the limited nutrient availability that restricted phytoplankton growth (<xref ref-type="bibr" rid="B54">Wong et&#xa0;al., 2002</xref>; <xref ref-type="bibr" rid="B62">Yasunaka et&#xa0;al., 2014</xref>). However, the KE zone has a high Chl <italic>a</italic> concentration of 0.4&#x2212;0.9 mg m<sup>&#x2212;3</sup>, suggesting that biological activity may influence OA metrics in this region. Correspondingly, the AOU value of &#x2212;9 &#xb1; 3 &#x3bc;mol kg<sup>&#x2212;1</sup> in the subtropical and KR zones was slightly lower than the air&#x2013;sea equilibrated value (0 &#x3bc;mol kg<sup>&#x2212;1</sup>), probably related to the low primary production. However, the KE zone had a relatively low AOU value of &#x2212;26 &#xb1; 6 &#x3bc;mol kg<sup>&#x2212;1</sup> (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4B</bold>
</xref>), indicating the effect of relatively intense biological oxygen production in the KE surface waters.</p>
</sec>
<sec id="s3_2">
<label>3.2</label>
<title>Spatial variability of carbonate system parameters</title>
<p>The variations in the surface NDIC and <italic>p</italic>CO<sub>2</sub> are shown in <xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4C, D</bold>
</xref>. The variations of surface NDIC were generally mirrored the SST (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4C</bold>
</xref>), and the NDIC value increased from 1975 &#xb1; 11 &#x3bc;mol kg<sup>&#x2212;1</sup> in the subtropical zone, to 2,017 &#xb1; 10 &#x3bc;mol kg<sup>&#x2212;1</sup> in the KR zone, and to 2,076 &#xb1; 7 &#x3bc;mol kg<sup>&#x2212;1</sup> in the KE zone. The surface NDIC was close to the air equilibrium in the subtropical zone and lower than the air-equilibrated NDIC by 17 &#xb1; 7 &#x3bc;mol kg<sup>&#x2212;1</sup> in the KR zone and 38 &#xb1; 7 &#x3bc;mol kg<sup>&#x2212;1</sup> in the KE zone (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4C</bold>
</xref>). In contrast to the distinct variation in surface NDIC, surface TA and SSS generally followed a linear relationship (<xref ref-type="fig" rid="f2">
<bold>Figure&#xa0;2A</bold>
</xref>), and surface NTA showed a uniform value of 2,295 &#xb1; 4 &#x3bc;mol kg<sup>&#x2212;1</sup> in the study area, which is consistent with the previously reported mean NTA value of 2,297 &#xb1; 5 &#x3bc;mol kg<sup>&#x2212;1</sup> in the western North Pacific (<xref ref-type="bibr" rid="B44">Ono et&#xa0;al., 2019</xref>). This uniformity of NTA further supports the limited influence of the Oyashio current on the KE surface waters during the survey cruise, as the Oyashio water has a relatively high NTA of ~2,400 &#x3bc;mol kg<sup>&#x2212;1</sup> (<xref ref-type="bibr" rid="B20">Ishii et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B49">Takahashi et&#xa0;al., 2014</xref>). <xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4D</bold>
</xref> shows that the distribution of sea surface <italic>p</italic>CO<sub>2</sub> in late spring is similar to that of SST, as previously described in detail by <xref ref-type="bibr" rid="B36">Li et&#xa0;al. (2022a)</xref>. In addition, the temperature normalized <italic>p</italic>CO<sub>2</sub> at 28.0&#xb0;C mirrored <italic>in situ p</italic>CO<sub>2</sub> but was similar to that of Chl <italic>a</italic> (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4B, D</bold>
</xref>), suggesting a relatively weak effect of biological CO<sub>2</sub> drawdown.</p>
<p>The variations in surface pH and &#x3a9;<sub>arag</sub> are shown in <xref ref-type="fig" rid="f3">
<bold>Figures&#xa0;3C, D</bold>
</xref>, <xref ref-type="fig" rid="f4">
<bold>4E, F</bold>
</xref>, and they also show large environmental gradients. Surface pH variations were similar to those of NDIC but mirrored &#x3a9;<sub>arag</sub>, SST and <italic>p</italic>CO<sub>2</sub>. The pH (&#x3a9;<sub>arag</sub>) increased (decreased) from 8.18 &#xb1; 0.01 (3.57 &#xb1; 0.12) in the subtropical zone to 8.21 &#xb1; 0.01 (3.25 &#xb1; 0.12) in the KR zone and to 8.24 &#xb1; 0.02 (2.95 &#xb1; 0.16) in the KE zone. Similar to NDIC and <italic>p</italic>CO<sub>2</sub>, the surface pH and &#x3a9;<sub>arag</sub> were close to the air equilibrium in the subtropical zone, which is consistent with the results of <xref ref-type="bibr" rid="B44">Ono et&#xa0;al. (2019)</xref>. They found that the surface pH and &#x3a9;<sub>arag</sub> in the area have been in air equilibrium annually over the past three decades. In contrast, the surface pH and &#x3a9;<sub>arag</sub> were higher than the air-equilibrated values in the KR and KE zones (<xref ref-type="fig" rid="f4">
<bold>Figures&#xa0;4E, F</bold>
</xref>). Especially in the KE zone, the low surface <italic>p</italic>CO<sub>2</sub> and high pH corresponded to the relatively high Chl <italic>a</italic> content and negative AOU, indicating the effects of photosynthesis-induced oxygen addition, <italic>p</italic>CO<sub>2</sub> decrease, and pH increase. However, the surface &#x3a9;<sub>arag</sub> is the lowest in the KE zone, which is contradictory to the photosynthesis-induced &#x3a9;<sub>arag</sub> increase. These results indicate that photosynthesis was not the only factor controlling surface pH and &#x3a9;<sub>arag</sub> distributions.</p>
</sec>
</sec>
<sec id="s4" sec-type="discussion">
<label>4</label>
<title>Discussion</title>
<sec id="s4_1">
<label>4.1</label>
<title>Controls of surface pH and &#x3a9;<sub>arag</sub> variations</title>
<p>To reveal the mechanisms governing the distributions of sea surface pH and &#x3a9;<sub>arag</sub> in late spring, we investigated the relationship between surface pH, &#x3a9;<sub>arag</sub>, and SST (<xref ref-type="fig" rid="f5">
<bold>Figures&#xa0;5A, B</bold>
</xref>). There are significant correlations between surface pH, &#x3a9;<sub>arag</sub>, and SST with correlation coefficients (<italic>r</italic>) of 0.84 (<italic>p&lt;</italic>0.001) and 0.93 (<italic>p&lt;</italic>0.001), respectively. We further divided the effect of temperature on pH and &#x3a9;<sub>arag</sub> into internal and external effects, both of which coexist in the contemporary ocean (<xref ref-type="bibr" rid="B23">Jiang et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B4">Cai et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B57">Wu et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B59">Xue et&#xa0;al., 2021</xref>). The internal temperature effect is computed based on the assumption that temperature is the only variable, because it is linked to shifts in the species in the CO<sub>2</sub> system as the temperature varies. The external temperature effect was calculated by varying the temperature and assuming a consistent air-sea equilibrium (<xref ref-type="bibr" rid="B4">Cai et&#xa0;al., 2020</xref>). Note that, for the internal temperature effect, the magnitude of the pH is initially much larger than that of &#x3a9;<sub>arag</sub> (<xref ref-type="bibr" rid="B23">Jiang et&#xa0;al., 2019</xref>).</p>
<fig id="f5" position="float">
<label>Figure&#xa0;5</label>
<caption>
<p>Schematic of the relationships between sea surface temperature and <bold>(A)</bold> pH and <bold>(B)</bold> &#x3a9;<sub>arag</sub>. The initial condition is set up with subtropical salinity = 34.4 and TA = 2,260 &#x3bc;mol kg<sup>&#x2212;1</sup> to generate the <italic>p</italic>CO<sub>2</sub> contours, with the dashed black line representing the air-sea equilibrium at <italic>p</italic>CO<sub>2</sub> = 390 &#x3bc;atm. The dashed gray line represents the internal temperature effect calculated from salinity = 34.4, TA = 2,260 &#x3bc;mol kg<sup>&#x2212;1</sup>, and DIC = 1,945 &#x3bc;mol kg<sup>&#x2212;1</sup> in the subtropical zone. Blue, yellow, and red dots indicate data obtained in the subtropical, Kuroshio Recirculation (KR) and Kuroshio Extension (KE) zone, respectively.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-10-1197977-g005.tif"/>
</fig>
<p>The results showed that surface pH generally followed the internal temperature effect but was lower than that predicted by the internal temperature effect and higher than the air&#x2013;sea equilibrated values in the KR and KE zones. This result indicates that the internal temperature dominated the latitudinal gradient in surface pH, although the air-sea gas exchange induced by temperature partially offsets the internal temperature-driven pH pattern. In contrast, the surface &#x3a9;<sub>arag</sub> generally followed the external temperature effect (air&#x2013;sea gas exchange induced by temperature) but was lower than that predicted by the internal temperature effect and higher than the air&#x2013;sea equilibrated values in the KR and KE zones. This result indicates that the surface &#x3a9;<sub>arag</sub> is mainly controlled by the external temperature effect, although the internal temperature effect enhances the external temperature-driven &#x3a9;<sub>arag</sub> gradient.</p>
<p>In addition to the effect of temperature on the surface pH and &#x3a9;<sub>arag</sub>, biological activities tend to increase the sea surface pH and &#x3a9;<sub>arag</sub> in the KE zone (<italic>Section 3.2</italic>), probably enhancing the surface pH gradient but counteracting the surface &#x3a9;<sub>arag</sub> gradient. In addition, entrainment of subsurface low-pH and &#x3a9;<sub>arag</sub> water decreases the surface pH and &#x3a9;<sub>arag</sub> in winter and spring (<xref ref-type="bibr" rid="B22">Ishii et&#xa0;al., 2001</xref>; <xref ref-type="bibr" rid="B51">Takahashi et&#xa0;al., 2002</xref>; <xref ref-type="bibr" rid="B27">Kim et&#xa0;al., 2015</xref>).</p>
</sec>
<sec id="s4_2">
<label>4.2</label>
<title>Contribution of controlling factors on pH and &#x3a9;<sub>arag</sub> variations</title>
<p>As mentioned above, the changes in surface pH (&#x394;pH) and &#x3a9;<sub>arag</sub> (&#x394;&#x3a9;<sub>arag</sub>) were affected by internal temperature, external temperature (air&#x2013;sea gas exchange induced by temperature), biological activities, and vertical mixing. The effects of these processes on the spatial and&#xa0;temporal variations in pH and &#x3a9;<sub>arag</sub> have also been previously reported by some studies (e.g., <xref ref-type="bibr" rid="B21">Ishii et&#xa0;al., 2011</xref>; <xref ref-type="bibr" rid="B49">Takahashi et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B24">Jiang et&#xa0;al., 2015</xref>; <xref ref-type="bibr" rid="B57">Wu et&#xa0;al., 2021</xref>; <xref ref-type="bibr" rid="B59">Xue et&#xa0;al., 2021</xref>). Here, we first decomposed &#x394;pH and &#x394;&#x3a9;<sub>arag</sub> into the contributions of changes in individual parameters.</p>
<p>Decomposition provides quantitative constraints on how the various drivers of pH and &#x3a9;<sub>arag</sub> change spatially (<xref ref-type="fig" rid="f6">
<bold>Figures&#xa0;6A, B</bold>
</xref>). Generally, among the different drivers, the &#x394;pH values were mainly attributed to &#x394;T, whereas the contribution of &#x394;NDIC to &#x394;pH offset approximately 61% &#xb1; 16% and 63% &#xb1; 8% of the &#x394;pH caused by &#x394;T in the KR and KE zones, respectively. With respect to &#x394;&#x3a9;<sub>arag</sub>, the values were primarily controlled by the &#x394;NDIC, whose contributions accounted for 69% &#xb1; 9% and 73% &#xb1; 3% of &#x394;&#x3a9;<sub>arag</sub> in the KR and KE zones, respectively. In addition, the contributions of &#x394;NDIC to &#x394;&#x3a9;<sub>arag</sub> were enhanced by &#x394;T, with contributions to &#x394;&#x3a9;<sub>arag</sub> of 34% &#xb1; 9% and 30% &#xb1; 3% in the KR and KE zones, respectively. Furthermore, the direct contributions of &#x394;S to &#x394;pH and &#x394;&#x3a9;<sub>arag</sub> were negligible, while the indirect contributions of &#x394;S via the variation of TA can also contribute to &#x394;pH and &#x394;&#x3a9;<sub>arag</sub> (<xref ref-type="bibr" rid="B31">Kuchinke et&#xa0;al., 2014</xref>; <xref ref-type="bibr" rid="B32">Kwiatkowski and Orr, 2018</xref>; <xref ref-type="bibr" rid="B38">Li and Zhai, 2019</xref>). However, the contributions of &#x394;S-induced TA changes to &#x394;&#x3a9;<sub>arag</sub> were offset by &#x394;S-induced DIC changes because the sensitivities of pH and &#x3a9;<sub>arag</sub> to DIC and TA are approximately equal and opposite, respectively (<xref ref-type="bibr" rid="B6">Cao et&#xa0;al., 2007</xref>; <xref ref-type="bibr" rid="B4">Cai et&#xa0;al., 2020</xref>; <xref ref-type="bibr" rid="B60">Xue and Cai, 2020</xref>).</p>
<fig id="f6" position="float">
<label>Figure&#xa0;6</label>
<caption>
<p>Spatiotemporal changes in pH (&#x394;pH) and &#x3a9;<sub>arag</sub> (&#x394;&#x3a9;<sub>arag</sub>) <bold>(A, B)</bold> due to individual parameter changes in NDIC (&#x394;NDIC), NTA (&#x394;NTA), and temperature (&#x394;T), salinity (&#x394;S), and residual (Res), and <bold>(C, D)</bold> due to individual processes of internal temperature effect, biological activity, air&#x2013;sea gas exchange and vertical mixing, and residual. These changes were calculated from the real-time values relative to the mean value in the subtropical zone (temperature = 28.0 &#xb0;C, salinity = 34.4, TA = 2,260 &#x3bc;mol kg<sup>&#x2212;1</sup>, and DIC = 1,945 &#x3bc;mol kg<sup>&#x2212;1</sup>). Color shading indicates the subtropical, Kuroshio Recirculation (KR) and Kuroshio Extension (KE) zones. Subtropical front, SF, Kuroshio front, KF.</p>
</caption>
<graphic mimetype="image" mime-subtype="tiff" xlink:href="fmars-10-1197977-g006.tif"/>
</fig>
<p>We further decomposed &#x394;NDIC into the contributions of fundamental biogeochemical processes to &#x394;pH and &#x394;&#x3a9;<sub>arag</sub>, e.g., the changes in biological activities (&#x394;NDIC<sup>Bio</sup>) and other &#x394;NDIC, which were mainly associated with air&#x2013;sea gas exchange and vertical mixing (&#x394;NDIC<sup>ASM</sup>). Therefore, we represent the contributions using the terms: &#x394;<italic>V</italic>
<sup>T</sup> = (<italic>&#x259;V/&#x259;</italic>T)&#x394;T, &#x394;<italic>V</italic>
<sup>&#x394;NDIC</sup> = (<italic>&#x259;V/&#x259;</italic>NDIC)&#x394;NDIC, &#x394;<italic>V</italic>
<sup>Bio</sup> = (&#x394;NDIC<sup>Bio/</sup>&#x394;NDIC)&#x394;<italic>V</italic>
<sup>&#x394;NDIC</sup>, and &#x394;<italic>V</italic>
<sup>ASM</sup> = &#x394;<italic>V</italic>
<sup>&#x394;NDIC</sup> &#x2212; &#x394;<italic>V</italic>
<sup>Bio</sup>. Therefore, we decompose &#x394;<italic>V</italic> as follows,</p>
<disp-formula>
<label>(3)</label>
<mml:math display="block" id="M3">
<mml:mrow>
<mml:mi>&#x394;</mml:mi>
<mml:mi>V</mml:mi>
<mml:mo>=</mml:mo>
<mml:mi>&#x394;</mml:mi>
<mml:msup>
<mml:mi>V</mml:mi>
<mml:mtext>T</mml:mtext>
</mml:msup>
<mml:mo>+</mml:mo>
<mml:mi>&#x394;</mml:mi>
<mml:msup>
<mml:mi>V</mml:mi>
<mml:mrow>
<mml:mtext>Bio</mml:mtext>
</mml:mrow>
</mml:msup>
<mml:mo>+</mml:mo>
<mml:mi>&#x394;</mml:mi>
<mml:msup>
<mml:mi>V</mml:mi>
<mml:mrow>
<mml:mtext>ASM</mml:mtext>
</mml:mrow>
</mml:msup>
<mml:mo>+</mml:mo>
<mml:mtext>Res</mml:mtext>
</mml:mrow>
</mml:math>
</disp-formula>
<p>where &#x394;<italic>V</italic>
<sup>Bio</sup> indicates the effect of biological activities. &#x394;NDIC<sup>Bio</sup> was calculated as &#x394;NDIC<sup>Bio</sup> = &#x394;AOU &#xd7; 117/170, where &#x394;AOU was calculated from the real-time value relative to the mean value in the subtropical zone (&#x2212;9 &#x3bc;mol kg<sup>&#x2212;1</sup>) and 117/170 is the C/O ratio (<xref ref-type="bibr" rid="B1">Anderson and Sarmiento, 1994</xref>). The discrete AOU values (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4B</bold>
</xref>) were linearly interpolated between the two stations and then adjusted to the underway time. &#x394;<italic>V</italic>
<sup>ASM</sup> was calculated from the difference between &#x394;<italic>V</italic>
<sup>&#x394;NDIC</sup> and &#x394;<italic>V</italic>
<sup>Bio</sup>, indicating the effects of temperature-induced air&#x2013;sea gas exchange and vertical mixing, both of which tend to decrease the surface pH and &#x3a9;<sub>arag</sub> in the KR and KE zones. We have included the minor contributions of &#x394;S and &#x394;NTA in the residual component in <xref ref-type="fig" rid="f6">
<bold>Figures&#xa0;6A, B</bold>
</xref>.</p>
<p>The contributions of the fundamental biogeochemical processes to &#x394;pH and &#x394;&#x3a9;<sub>arag</sub> are shown in <xref ref-type="fig" rid="f6">
<bold>Figures&#xa0;6C, D</bold>
</xref>. The contribution of &#x394;NDIC<sup>ASM</sup> to &#x394;pH offsets approximately 55% &#xb1; 20% and 77% &#xb1; 12% of &#x394;pH caused by &#x394;T in the KR and KE zones, respectively. In contrast, the contribution of &#x394;NDIC<sup>ASM</sup> accounts for 62% &#xb1; 15% and 87% &#xb1; 9% of &#x394;&#x3a9;<sub>arag</sub> in the KR and KE zones, respectively. This result indicates that the effect of air&#x2013;sea gas exchange and vertical mixing increased from the KR zone to the KE zone, probably related to the lower temperature-induced air&#x2013;sea gas exchange (<xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1A</bold>
</xref>) and deeper mixed layer depth (<xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1B</bold>
</xref>). The effect of biological activities was mainly constrained in the KE zone (<xref ref-type="fig" rid="f6">
<bold>Figures&#xa0;6C, D</bold>
</xref>), where waters with low AOU and high Chl <italic>a</italic> levels were located (<xref ref-type="fig" rid="f4">
<bold>Figure&#xa0;4B</bold>
</xref>). The contribution of biological activities accounted for 36% &#xb1; 26% of the &#x394;pH<sub>arag</sub> and offsets approximately 14% &#xb1; 9% of the &#x394;&#x3a9; in the KE zone. However, the contribution of biological activities offsets only about 17% &#xb1; 11% of the &#x394;NDIC<sup>ASM</sup>-induced &#x394;pH<sub>arag</sub> and 15% &#xb1; 9% of the &#x394;NDIC<sup>ASM</sup>-induced &#x394;&#x3a9; in the KE zone, respectively. Therefore, biological activities enhanced the temperature-driven pattern in pH but counteracted that in &#x3a9;<sub>arag</sub>. Moreover, the Chl <italic>a</italic> concentrations were highest in the late spring of the year (<xref ref-type="fig" rid="f1">
<bold>Figures&#xa0;1C&#x2013;H</bold>
</xref>), indicating that the influence of biological activity on the distribution of pH and &#x3a9;<sub>arag</sub> in late spring was the most notable and representative in the year. However, compared to the effect of temperature or air&#x2013;sea gas exchange on surface pH and &#x3a9;<sub>arag</sub> patterns, the degree of biological influence was relatively small, although primary production was highest in late spring (<xref ref-type="fig" rid="f1">
<bold>Figure&#xa0;1E</bold>
</xref>). This result was further supported by the results of <xref ref-type="bibr" rid="B36">Li et&#xa0;al. (2022a)</xref>, who found that the biological influence on the distribution pattern of surface <italic>p</italic>CO<sub>2</sub> was relatively minor.</p>
<p>In summary, these quantified results are consistent with the qualitative results, e.g., SST variations dominated the &#x394;pH, although air&#x2013;sea gas exchange and vertical mixing counteracted the temperature-driven pH pattern to a comparable extent. In contrast, &#x394;&#x3a9;<sub>arag</sub> was mainly controlled by air&#x2013;sea gas exchange and vertical mixing, the effects of which on the &#x3a9;<sub>arag</sub> pattern were enhanced by temperature. However, biological activities have a limited influence on the &#x394;pH and &#x394;&#x3a9;<sub>arag</sub> values.</p>
</sec>
<sec id="s4_3">
<label>4.3</label>
<title>Comparison with results from other studies</title>
<p>We showed that the surface pH and &#x3a9;<sub>arag</sub> were out of phase in late spring in the western North Pacific, e.g., the pH (&#x3a9;<sub>arag</sub>) was gradually decreased (increased) southward across the KE, KR, and subtropical zones. This latitudinal distribution pattern of surface pH and &#x3a9;<sub>arag</sub> is consistent with the climatological distribution of surface pH and &#x3a9;<sub>arag</sub> from low to mid-latitudes but is contrary to the distribution pattern from mid to high latitudes, where pH and&#xa0;&#x3a9;<sub>arag</sub> are generally in phase (<xref ref-type="bibr" rid="B24">Jiang et&#xa0;al., 2015</xref>; <xref ref-type="bibr" rid="B23">Jiang et&#xa0;al., 2019</xref>; <xref ref-type="bibr" rid="B59">Xue et&#xa0;al., 2021</xref>). In addition, we have presented the combined effects of temperature, air&#x2013;sea gas exchange, biological activities, and mixing on springtime pH and &#x3a9;<sub>arag</sub> distributions in the western North Pacific. Similarly combined effects have also been shown from East Asia to the Arctic Ocean, where <xref ref-type="bibr" rid="B57">Wu et&#xa0;al. (2021)</xref> found that biological activity counteracts the temperature-driven pattern in pH but reinforces that in &#x3a9;<sub>arag</sub> in the Bering and Chukchi Shelf, where the region has higher temperature and higher primary production relative to the Arctic Basin. This result contradicts with our result in the KE zone, where the region has a lower temperature and higher primary production than the subtropical zone (<xref ref-type="fig" rid="f6">
<bold>Figures&#xa0;6C, D</bold>
</xref>). In general, both spatial and seasonal variations in pH and &#x3a9;<sub>arag</sub> are larger in coastal oceans than in open oceans (<xref ref-type="bibr" rid="B15">Feely et&#xa0;al., 2008</xref>; <xref ref-type="bibr" rid="B3">Borges and Gypens, 2010</xref>; <xref ref-type="bibr" rid="B13">Feely et&#xa0;al., 2010</xref>; <xref ref-type="bibr" rid="B18">Gruber et&#xa0;al., 2012</xref>; <xref ref-type="bibr" rid="B58">Xu et&#xa0;al., 2020</xref>).</p>
<p>We found that temperature and its induced air&#x2013;sea gas exchange fundamentally controlled pH and &#x3a9;<sub>arag</sub> distributions from the subtropical zone to the KE zone. This is further supported by the results of <xref ref-type="bibr" rid="B59">Xue et&#xa0;al. (2021)</xref>, who found that when pH is mainly controlled by the internal temperature effect (thermal), surface pH and &#x3a9;<sub>arag</sub> tend to be out of phase because the effects of thermal and non-thermal (e.g., air&#x2013;sea gas exchange, biological activities, and mixing) on pH are out of phase; however, when pH is mainly controlled by non-thermal effects, surface pH and &#x3a9;<sub>arag</sub> will be in phase because their non-thermal effects are intrinsically in phase. Similarly, the variations in surface pH and &#x3a9;<sub>arag</sub> and their controls from low- to mid-latitudes agree with the seasonal variations in pH and &#x3a9;<sub>arag</sub> at mid-latitudes, which are also primarily driven by temperature and its induced air&#x2013;sea gas exchange (<xref ref-type="bibr" rid="B21">Ishii et&#xa0;al., 2011</xref>; <xref ref-type="bibr" rid="B27">Kim et&#xa0;al., 2015</xref>; <xref ref-type="bibr" rid="B11">Fassbender et&#xa0;al., 2018</xref>; <xref ref-type="bibr" rid="B32">Kwiatkowski and Orr, 2018</xref>). Taken together, these studies suggest that the spatiotemporal changes and drivers of the pH and &#x3a9;<sub>arag</sub> depend on the particular ocean environment.</p>
</sec>
</sec>
<sec id="s5">
<label>5</label>
<title>Summary</title>
<p>Based on the high-frequency-precision measurement of underway pH and <italic>p</italic>CO<sub>2</sub>, we demonstrated the distributions of surface pH and &#x3a9;<sub>arag</sub> and their controls across different hydrochemical gradients in the western North Pacific in late spring. The surface pH (&#x3a9;<sub>arag</sub>) was the highest (lowest) in the Kuroshio Extension zone, gradually decreased (increased) southward across the Kuroshio Recirculation zone and was close to the air&#x2013;sea equilibrium in the subtropical zone. Sea surface temperature dominated the pH distribution, although air&#x2013;sea gas exchange and vertical mixing counteracted the temperature-driven pH pattern to a comparable magnitude. The distribution of &#x3a9;<sub>arag</sub> was controlled by air&#x2013;sea gas exchange and vertical mixing and was enhanced by temperature. Biological activities enhanced the temperature-driven pattern of pH and counteracted that of &#x3a9;<sub>arag</sub>. However, compared to the effect of temperature or air-sea gas exchange, the degree of biological influence on surface pH and &#x3a9;<sub>arag</sub> patterns was relatively small in late spring, even though primary production was highest during the year. Overall, this work improves our understanding of the spatiotemporal variations in ocean acidification metrics in the western North Pacific, although more analyses from different seasons are still necessary to further explore the mechanisms controlling ocean acidification metrics.</p>
</sec>
<sec id="s6" sec-type="data-availability">
<title>Data availability statement</title>
<p>The datasets presented in this study can be found in online repositories. The names of the repository/repositories and accession number(s) can be found below: <ext-link ext-link-type="uri" xlink:href="https://figshare.com/articles/dataset/Underway-pumping_pCO2_and_auxiliary_data_along_the_cruise_track_over_the_Kuroshio_Extension_and_its_recirculation_regions_northwestern_North_Pacific_in_late_spring_2018/19807807?file=42541858">https://figshare.com/articles/dataset/Underway-pumping_pCO2_and_auxiliary_data_along_the_cruise_track_over_the_Kuroshio_Extension_and_its_recirculation_regions_northwestern_North_Pacific_in_late_spring_2018/19807807?file=42541858</ext-link>.</p>
</sec>
<sec id="s7" sec-type="author-contributions">
<title>Author contributions</title>
<p>DQ designed the study. C-LL performed the investigation, with assistance from KC and HL. C-LL performed experiments, analyzed the data, and wrote the original manuscript. DQ, YW, and LC provided comments on data analysis and revised the manuscript. All authors contributed to the article and approved the submitted version.</p>
</sec>
</body>
<back>
<sec id="s8" sec-type="funding-information">
<title>Funding</title>
<p>This research was financially supported by the National Key Research and Development Program of China (2019YFE0114800), the National Natural Science Foundation of China (91858210), and&#xa0;the Natural Science Foundation of Fujian Province, China (2019Jo5148).</p>
</sec>
<ack>
<title>Acknowledgments</title>
<p>We thank the crews of R/V <italic>Xiangyanghong</italic> 3 for their assistance and cooperation during the investigation. The sampling survey was supported by the Laboratory of Marine Isotopic Technology and Environmental Risk Assessment, Third Institute of Oceanography, Ministry of Natural Resources, <italic>via</italic> a survey of environmental radioactivity detection projects in the western Pacific.</p>
</ack>
<sec id="s9" 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="s10" 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>
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<glossary>
<title>Glossary</title>
<table-wrap position="anchor">
<table frame="hsides">
<tbody>
<tr>
<td>KR</td>
<td>Kuroshio Recirculation</td>
</tr>
<tr>
<td>KE</td>
<td>Kuroshio Extension</td>
</tr>
<tr>
<td>STCC</td>
<td>Subtropical Countercurrent</td>
</tr>
<tr>
<td>KF</td>
<td>Kuroshio front</td>
</tr>
<tr>
<td>SF</td>
<td>subtropical front</td>
</tr>
<tr>
<td>&#x3a9;<sub>arag</sub>
</td>
<td>aragonite saturation state</td>
</tr>
<tr>
<td>OA</td>
<td>ocean acidification</td>
</tr>
<tr>
<td>
<italic>p</italic>CO<sub>2</sub>
</td>
<td>partial pressure of CO<sub>2</sub>
</td>
</tr>
<tr>
<td>Chl <italic>a</italic>
</td>
<td>chlorophyll <italic>a</italic>
</td>
</tr>
<tr>
<td>MLD</td>
<td>mixed layer depth</td>
</tr>
<tr>
<td>SST</td>
<td>sea surface temperature</td>
</tr>
<tr>
<td>SSS</td>
<td>sea surface salinity</td>
</tr>
<tr>
<td>DO</td>
<td>dissolved oxygen</td>
</tr>
<tr>
<td>AOU</td>
<td>apparent oxygen utilization</td>
</tr>
<tr>
<td>DIC</td>
<td>dissolved inorganic carbon</td>
</tr>
<tr>
<td>TA</td>
<td>total alkalinity</td>
</tr>
<tr>
<td>NTA</td>
<td>salinity-normalized TA</td>
</tr>
<tr>
<td>NDIC</td>
<td>salinity-normalized DIC</td>
</tr>
<tr>
<td>pH<sup>UW</sup>
</td>
<td>underway pH</td>
</tr>
<tr>
<td>
<italic>p</italic>CO<sub>2</sub>
<sup>UW</sup>
</td>
<td>underway <italic>p</italic>CO<sub>2</sub>
</td>
</tr>
<tr>
<td>pH<sup>DIC-TA</sup>
</td>
<td>calculated pH from measured DIC and TA</td>
</tr>
<tr>
<td>
<italic>p</italic>CO<sub>2</sub>
<sup>DIC-TA</sup>
</td>
<td>calculated <italic>p</italic>CO<sub>2</sub> from measured DIC and TA</td>
</tr>
<tr>
<td>&#x3a9;<sub>arag</sub>
<sup>DIC-TA</sup>
</td>
<td>calculated &#x3a9;<sub>arag</sub> from measured DIC and TA</td>
</tr>
<tr>
<td>&#x3a9;<sub>arag</sub>
<italic>
<sup>p</sup>
</italic>
<sup>CO2UW-TAsss</sup>
</td>
<td>calculated &#x3a9;<sub>arag</sub> from underway <italic>p</italic>CO<sub>2</sub> and salinity-based TA</td>
</tr>
<tr>
<td>&#x394;NDIC<sup>Bio</sup>
</td>
<td>effect of biological activity on NDIC change</td>
</tr>
<tr>
<td>&#x394;NDIC<sup>ASM</sup>
</td>
<td>effect of air&#x2013;sea gas exchange and vertical mixing on NDIC change</td>
</tr>
</tbody>
</table>
</table-wrap>
</glossary>
</back>
</article>