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<front>
<journal-meta>
<journal-id journal-id-type="publisher-id">Front. Earth Sci.</journal-id>
<journal-title>Frontiers in Earth Science</journal-title>
<abbrev-journal-title abbrev-type="pubmed">Front. Earth Sci.</abbrev-journal-title>
<issn pub-type="epub">2296-6463</issn>
<publisher>
<publisher-name>Frontiers Media S.A.</publisher-name>
</publisher>
</journal-meta>
<article-meta>
<article-id pub-id-type="publisher-id">680180</article-id>
<article-id pub-id-type="doi">10.3389/feart.2021.680180</article-id>
<article-categories>
<subj-group subj-group-type="heading">
<subject>Earth Science</subject>
<subj-group>
<subject>Brief Research Report</subject>
</subj-group>
</subj-group>
</article-categories>
<title-group>
<article-title>Asian Winter Monsoon Imprint on the Water Column Structure at the Northern South China Sea Coast</article-title>
<alt-title alt-title-type="left-running-head">Zhang et&#x20;al.</alt-title>
<alt-title alt-title-type="right-running-head">Monsoon Impacts SCS Coastal Waters</alt-title>
</title-group>
<contrib-group>
<contrib contrib-type="author" corresp="yes">
<name>
<surname>Zhang</surname>
<given-names>Yancheng</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="corresp" rid="c001">&#x2a;</xref>
<uri xlink:href="https://loop.frontiersin.org/people/1266570/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Zhu</surname>
<given-names>Kai</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Huang</surname>
<given-names>Chao</given-names>
</name>
<xref ref-type="aff" rid="aff3">
<sup>3</sup>
</xref>
<xref ref-type="aff" rid="aff4">
<sup>4</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/1141549/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Kong</surname>
<given-names>Deming</given-names>
</name>
<xref ref-type="aff" rid="aff4">
<sup>4</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/923733/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>He</surname>
<given-names>Yuxin</given-names>
</name>
<xref ref-type="aff" rid="aff5">
<sup>5</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/290522/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Wang</surname>
<given-names>Huanye</given-names>
</name>
<xref ref-type="aff" rid="aff6">
<sup>6</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/98394/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Liu</surname>
<given-names>Weiguo</given-names>
</name>
<xref ref-type="aff" rid="aff6">
<sup>6</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/86877/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Xie</surname>
<given-names>Zhouqing</given-names>
</name>
<xref ref-type="aff" rid="aff7">
<sup>7</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/114122/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Wei</surname>
<given-names>Gangjian</given-names>
</name>
<xref ref-type="aff" rid="aff3">
<sup>3</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/809271/overview"/>
</contrib>
<contrib contrib-type="author">
<name>
<surname>Liu</surname>
<given-names>Zhonghui</given-names>
</name>
<xref ref-type="aff" rid="aff2">
<sup>2</sup>
</xref>
<uri xlink:href="https://loop.frontiersin.org/people/933659/overview"/>
</contrib>
</contrib-group>
<aff id="aff1">
<label>
<sup>1</sup>
</label>School of Marine Sciences, Sun Yat-sen University, <addr-line>Zhuhai</addr-line>, <country>China</country>
</aff>
<aff id="aff2">
<label>
<sup>2</sup>
</label>Department of Earth Sciences, The University of Hong Kong, <addr-line>Hong Kong</addr-line>, <country>China</country>
</aff>
<aff id="aff3">
<label>
<sup>3</sup>
</label>State Key Laboratory of Isotope Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, <addr-line>Guangzhou</addr-line>, <country>China</country>
</aff>
<aff id="aff4">
<label>
<sup>4</sup>
</label>Guangdong Province Key Laboratory for Coastal Ocean Variation and Disaster Prediction, Guangdong Ocean University, <addr-line>Zhanjiang</addr-line>, <country>China</country>
</aff>
<aff id="aff5">
<label>
<sup>5</sup>
</label>School of Earth Sciences, Zhejiang University, <addr-line>Hangzhou</addr-line>, <country>China</country>
</aff>
<aff id="aff6">
<label>
<sup>6</sup>
</label>State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, <addr-line>Xi&#x2019;an</addr-line>, <country>China</country>
</aff>
<aff id="aff7">
<label>
<sup>7</sup>
</label>Anhui Key Laboratory of Polar Environment and Global Change, Department of Environmental Science and Engineering, University of Science and Technology of China, <addr-line>Hefei</addr-line>, <country>China</country>
</aff>
<author-notes>
<fn fn-type="edited-by">
<p>
<bold>Edited by:</bold> <ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/1075615/overview">Shengfa Liu</ext-link>, Ministry of Natural Resources, China</p>
</fn>
<fn fn-type="edited-by">
<p>
<bold>Reviewed by:</bold> <ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/406117/overview">Kefu Yu</ext-link>, Guangxi University, China</p>
<p>
<ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/828875/overview">Hong Yan</ext-link>, Institute of Earth Environment (CAS), China</p>
<p>
<ext-link ext-link-type="uri" xlink:href="https://loop.frontiersin.org/people/1390562/overview">Qian Li</ext-link>, Qingdao National Laboratory for Marine Science and Technology, China</p>
</fn>
<corresp id="c001">&#x2a;Correspondence: Yancheng Zhang, <email>zhangych99@mail.sysu.edu.cn</email>
</corresp>
<fn fn-type="other">
<p>This article was submitted to Quaternary Science, Geomorphology and Paleoenvironment, a section of the journal Frontiers in Earth Science</p>
</fn>
</author-notes>
<pub-date pub-type="epub">
<day>23</day>
<month>08</month>
<year>2021</year>
</pub-date>
<pub-date pub-type="collection">
<year>2021</year>
</pub-date>
<volume>9</volume>
<elocation-id>680180</elocation-id>
<history>
<date date-type="received">
<day>13</day>
<month>03</month>
<year>2021</year>
</date>
<date date-type="accepted">
<day>12</day>
<month>07</month>
<year>2021</year>
</date>
</history>
<permissions>
<copyright-statement>Copyright &#xa9; 2021 Zhang, Zhu, Huang, Kong, He, Wang, Liu, Xie, Wei and Liu.</copyright-statement>
<copyright-year>2021</copyright-year>
<copyright-holder>Zhang, Zhu, Huang, Kong, He, Wang, Liu, Xie, Wei and Liu</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&#x20;terms.</p>
</license>
</permissions>
<abstract>
<p>Coastal regions of the northern South China Sea (SCS) strongly interact with the Asian monsoon circulation (AMC). Thus, variations of sea surface temperature (SST) here are newly suggested to document AMC changes in an effective manner, but additional physical parameters of oceanic conditions, probably also in relation to the AMC system, remain poorly understood. In this study, we analyzed glycerol dialkyl glycerol tetraethers (GDGTs) from a well-dated sediment core YJ, retrieved at the northern SCS coast, to further scrutinize the intrinsic response of water column to winter AMC strength. It shows that within the time frame of past &#x223c;1,000&#xa0;years, the tetraether index of lipids with 86 carbon atoms (<inline-formula id="inf1">
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</inline-formula>) and published alkenone (<inline-formula id="inf2">
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</inline-formula>) temperature records together confirm a reduced thermal gradient during the Little Ice Age (LIA), in comparison to that during the Medieval Climate Anomaly (MCA). Considering concurrent variations of the branched and isoprenoid tetraether (BIT) and the ratio of archaeol to caldarchaeol (ACE), for example, with decreased values (&#x3c;&#x223c;0.3) for the former and relatively high values for the latter at the LIA, indicative of stratification and salinity changes, respectively, these multiple lines of evidence thereby call for well mixing of onsite water at site YJ correspondingly. Our results suggest that winter AMC strength is a critical factor for mixing subsurface waters and modifying thermal/saline conditions at the northern SCS coasts through the last millennium and also, perhaps, on longer timescales.</p>
</abstract>
<kwd-group>
<kwd>South China Sea</kwd>
<kwd>coastal conditions</kwd>
<kwd>GDGTs</kwd>
<kwd>last millennium</kwd>
<kwd>Asian winter monsoon</kwd>
</kwd-group>
</article-meta>
</front>
<body>
<sec id="s1">
<title>Introduction</title>
<p>The Asian monsoon circulation (AMC), as triggered by large-scale thermal contrast between ocean and land, characterizes a seasonal reversal of prevailing wind directions. In the summertime, it carries an enormous amount of moisture from the Indian and Pacific Oceans toward southern and northeastern Asia, and, consequently, exerts a considerable influence over the water cycle and the terrestrial ecosystem (<xref ref-type="bibr" rid="B47">Wang et&#x20;al., 2017</xref>; <xref ref-type="bibr" rid="B59">Zhang et&#x20;al., 2017</xref>). In this regard, much attention has been drawn until now to explore summer AMC variability and the physical mechanism(s) from seasonal to orbital timescales (e.g., <xref ref-type="bibr" rid="B11">Hu et&#x20;al., 2008</xref>; <xref ref-type="bibr" rid="B1">An et&#x20;al., 2011</xref>; <xref ref-type="bibr" rid="B28">Liu et&#x20;al., 2015</xref>; <xref ref-type="bibr" rid="B54">Xie et&#x20;al., 2015</xref>; <xref ref-type="bibr" rid="B6">Cheng et&#x20;al., 2016</xref>). In contrast, the winter component of the AMC itself often diverges cold-dry air from the Asian countries such as Siberia-Mongolia toward oceans, thus with little potential to deliver water vapor directly. Despite such fact, winter AMC is still of importance in transporting eolian dust and/or aerosol, and therefore in regulating the regional (and global) climate system (<xref ref-type="bibr" rid="B30">Maher et&#x20;al., 2010</xref>; <xref ref-type="bibr" rid="B19">Kok et&#x20;al., 2018</xref>). Combined with its impact upon the summer AMC precipitation subsequently (<xref ref-type="bibr" rid="B3">Bollasina et&#x20;al., 2011</xref>; <xref ref-type="bibr" rid="B26">Li et&#x20;al., 2016</xref>; <xref ref-type="bibr" rid="B4">Cai et&#x20;al., 2019</xref>), a complete understanding of winter AMC variations at present and, if possible, before the instrumental era (after &#x223c;1850 AD) (e.g., <xref ref-type="bibr" rid="B51">Wen et&#x20;al., 2016</xref>; <xref ref-type="bibr" rid="B17">Kang et&#x20;al., 2020</xref>) would provide constructive insight into their intrinsic link against both anthropogenic and natural backgrounds. Abundant analyses based on the grain size and geochemical proxies from Chinese loess sequences at available sparse sites (<xref ref-type="bibr" rid="B38">Stevens et&#x20;al., 2007</xref>; <xref ref-type="bibr" rid="B25">Li and Morrill 2015</xref>), on the one hand, have indeed advanced our knowledge about this topic, but on the other hand, these paleorecords, distributed across continental interiors, rather face difficulty to draw a clear picture of winter AMC behavior, for example, its far-field effect on terrestrial ecosystem especially. For example, at Huguangyan Maar Lake, winter AMC intensity, as inferred from diatom assemblages (<xref ref-type="bibr" rid="B45">Wang et&#x20;al., 2012</xref>) and magnetic susceptibility (<xref ref-type="bibr" rid="B57">Yancheva et&#x20;al., 2007</xref>), respectively, presents controversial temporal features during the Holocene (since &#x223c;11,700&#xa0;years ago before present, &#x201c;yr BP&#x201d; hereafter).</p>
<p>Next to Huguangyan Maar Lake, the South China Sea (SCS) is also strongly involved into the AMC coupling process (e.g., <xref ref-type="bibr" rid="B65">Xie et&#x20;al., 1998</xref>; <xref ref-type="bibr" rid="B23">Lau and Nath 2009</xref>; <xref ref-type="bibr" rid="B42">Wang et&#x20;al., 2009</xref>; <xref ref-type="bibr" rid="B27">Liu and Zhu 2016</xref>) and hence well suited to fingerprint its variability. In fact, along the SCS northern coasts, sea surface temperature (SST) apparently exhibits shore-parallel gradient and intensive vertical mixing in winter, while horizontal homogenization and vertical stratification in summer (<xref ref-type="fig" rid="F1">Figures 1A,B</xref>; <xref ref-type="bibr" rid="B52">Wang, 2007</xref>; <xref ref-type="bibr" rid="B16">Jing et&#x20;al., 2009</xref>). Such seasonality of SST variations and their difference, for example, at both horizontal and vertical scales, are readily capable of revealing winter AMC signals across different timescales (e.g., <xref ref-type="bibr" rid="B39">Tian et&#x20;al., 2010</xref>; <xref ref-type="bibr" rid="B13">Huang et&#x20;al., 2011</xref>; <xref ref-type="bibr" rid="B37">Steinke et&#x20;al., 2011</xref>; <xref ref-type="bibr" rid="B20">Kong, 2014a</xref>, <xref ref-type="bibr" rid="B22">Kong et&#x20;al., 2014b</xref>). Particularly, our recent study (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>), based on a well-dated sediment core YJ, &#x223c;200&#xa0;km far away from the Pearl River delta (<xref ref-type="fig" rid="F1">Figure&#x20;1</xref>), has shown extraordinary decrease (by up to &#x223c;4&#xb0;C) of alkenone SSTs and remarkable increase (by two to four orders of magnitude) of wind-borne terrigenous hopane contents during the Little Ice Age (LIA, &#x223c;150&#x2013;550&#xa0;years BP), consequently demonstrating an overall intensification of winter AMC, relative to the Medieval Climate Anomaly (MCA, &#x223c;700&#x2013;1,100&#xa0;years BP) and other intervals in the context of Holocene. This explanation, albeit well corroborated by a growing number of terrestrial paleorecords (e.g., <xref ref-type="bibr" rid="B57">Yancheva et&#x20;al., 2007</xref>; <xref ref-type="bibr" rid="B17">Kang et&#x20;al., 2020</xref>), still deserves independent evidence of oceanic conditions which, as inherently linked to SST change, would offer excellent opportunity to further illustrate the fundamental role of winter AMC variations in affecting coastal waters. To this end, the time window of last millennium covering both the LIA and MCA, two well-identified climate anomaly intervals during the late Holocene (<xref ref-type="bibr" rid="B31">Mann et&#x20;al., 2008</xref>), is specifically focused here for a tentative attempt to examine how the northern SCS coastal conditions, for example, in terms of both salinity and thermal properties, would have responded to winter AMC change at multi-centennial timescales.</p>
<fig id="F1" position="float">
<label>FIGURE 1</label>
<caption>
<p>Regional setting and the site of core YJ, existing paleorecords in the northern South China Sea (black dots) and at Huguang Maar Lake (orange star) as mentioned in the main text, are plotted against long-term (1985&#x2013;2006 AD) averaged January <bold>(A)</bold> and July <bold>(B)</bold> sea surface temperature (SST, color scale) from the AVHRR dataset (<xref ref-type="bibr" rid="B5">Casey, 2013</xref>). Chronology <bold>(C)</bold> and lithology <bold>(D)</bold> of core YJ are cited from <xref ref-type="bibr" rid="B12">Huang et&#x20;al. (2018)</xref> and <xref ref-type="bibr" rid="B62">Zhang et&#x20;al. (2019)</xref>. Note that the core-top <bold>(C)</bold> is calculated based on <sup>210</sup>Pb/<sup>137</sup>Cs dates, to be 2013 AD when our core YJ was retrieved.</p>
</caption>
<graphic xlink:href="feart-09-680180-g001.tif"/>
</fig>
<p>Taking the advantage of sediment core YJ, including i) high-quality control of the chronological framework (<xref ref-type="fig" rid="F1">Figures 1C,D</xref>) and ii) limited influence of the Pearl River freshwater discharge (<xref ref-type="fig" rid="F2">Figure&#x20;2</xref>), we hence directly analyzed glycerol dialkyl glycerol tetraether (GDGT) lipid biomarkers on its uppermost &#x223c;65&#xa0;cm section. Together with the existing measurements of the alkenone unsaturation index (<inline-formula id="inf3">
<mml:math id="m3">
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</inline-formula>, see definition in <xref ref-type="bibr" rid="B32">Prahl et&#x20;al., 1988</xref>) and hopane components, as earlier reported by <xref ref-type="bibr" rid="B62">Zhang et&#x20;al. (2019)</xref>, this study aimed to investigate the hydrological properties of the onsite water column. We hereby present proxy records of the ratio of archaeol to caldarchaeol (ACE), the branched and isoprenoid tetraether (BIT), respectively, and the tetraether index of lipids with 86 carbon atoms (<inline-formula id="inf4">
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</inline-formula>) over the past &#x223c;1,000&#xa0;years. These results, although potentially associated with various parameters in view of their original interpretations, are utilized to manifest salinity (<xref ref-type="bibr" rid="B40">Turich and Freeman 2011</xref>; <xref ref-type="bibr" rid="B43">Wang et&#x20;al., 2013</xref>), stratification (<xref ref-type="bibr" rid="B56">Yamamoto et&#x20;al., 2013</xref>; <xref ref-type="bibr" rid="B46">Wang et&#x20;al., 2021</xref>), and integrated temperature of the whole water column (<xref ref-type="bibr" rid="B55">Xing et&#x20;al., 2015</xref>; <xref ref-type="bibr" rid="B49">Wei et&#x20;al., 2020</xref>), respectively. On this basis, the difference of our paired <inline-formula id="inf5">
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</inline-formula>-<inline-formula id="inf6">
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</inline-formula> values, a rough measure of vertical thermal gradient, could be used to infer the water column structure changes induced by the winter AMC. Overall, this study helps clarify the dynamical interplay between winter AMC strength and northern SCS coastal conditions throughout the last millennium and, as a result, evoke a careful consideration of regional environmental settings in properly interpreting proxy-based temperature signals.</p>
<fig id="F2" position="float">
<label>FIGURE 2</label>
<caption>
<p>Comparison between temperature estimates at the topmost sample based on <inline-formula id="inf7">
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</inline-formula> and <inline-formula id="inf8">
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</inline-formula> proxies, respectively. Observational SSTs and salinity near the core site (112.125&#xb0;N, 21.625&#xb0;E, <xref ref-type="bibr" rid="B5">Casey, 2013</xref>; <xref ref-type="bibr" rid="B64">Zweng et&#x20;al., 2013</xref>) are also shown. The dashed line represents the annual mean SST&#x20;value.</p>
</caption>
<graphic xlink:href="feart-09-680180-g002.tif"/>
</fig>
</sec>
<sec sec-type="materials|methods" id="s2">
<title>Material and Methods</title>
<sec id="s2-1">
<title>Core Site and Chronology</title>
<p>Geographically, sediment core YJ (112&#xb0;8.08&#x2032; E, 21&#xb0;31.44&#x2032; N) is raised at a water depth of &#x223c;21&#xa0;m from the inner continental shelf offshore Yangjiang city with a distance of &#x223c;200&#xa0;km to the southwest of the Pearl River estuary. This site, according to modern observations (e.g., <xref ref-type="bibr" rid="B7">Dunn and Ridgway 2002</xref>; <xref ref-type="bibr" rid="B5">Casey, 2013</xref>), characterizes prominent SST variations between &#x223c;28.3&#xb0;C in summer (June-July-August, JJA) and &#x223c;20.9&#xb0;C in winter (December&#x2013;January&#x2013;February, DJF), but small changes in sea surface salinity (i.e.,&#x20;&#x223c;32.4&#xa0;psu in JJA and &#x223c;33.4&#xa0;psu in DJF; <xref ref-type="fig" rid="F2">Figure&#x20;2</xref>) due to limited influence of the Pearl River discharge. Most importantly, it is located at the coastal sector outside &#x223c;1&#xb0;C cooling effect of summer upwelling (e.g., to the east of the Pearl River delta and northeast of the Hainan Island, <xref ref-type="fig" rid="F1">Figure&#x20;1B</xref>), while surface cooling here is largely determined by vertical mixing of the onsite water column in winter (<xref ref-type="fig" rid="F1">Figure&#x20;1A</xref>). This site is hence well suited to examine the response of northern SCS coastal conditions to winter AMC changes, for example, by using the <inline-formula id="inf9">
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<mml:mtext>U</mml:mtext>
<mml:mrow>
<mml:mn>37</mml:mn>
</mml:mrow>
<mml:mrow>
<mml:mtext>K</mml:mtext>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
</mml:msubsup>
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</inline-formula> SST record in our previous study (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>).</p>
<p>The age model of this core, as already published before by <xref ref-type="bibr" rid="B12">Huang et&#x20;al. (2018)</xref> and <xref ref-type="bibr" rid="B62">Zhang et&#x20;al. (2019)</xref>, was achieved by combining both lead (<sup>210</sup>Pb)/cesium (<sup>137</sup>Cs) and radiocarbon (<sup>14</sup>C) methods. To summarize, measurements of 13&#x20;<sup>210</sup>Pb/<sup>137</sup>Cs radionuclide activity and 18&#x20;<sup>14</sup>C dates (at Beta Analytic Inc., United&#x20;States) were implemented on samples of bulk sediments above 13&#xa0;cm and complete shells below this depth, respectively. These age control points were then operated within R script BACON software (version 2.2, <xref ref-type="bibr" rid="B2">Blaauw and Christen 2011</xref>) and the Marine 13 calibration curve (<xref ref-type="bibr" rid="B33">Reimer et&#x20;al., 2013</xref>), using default parameters and a 252-year correction of regional reservoir age (<xref ref-type="bibr" rid="B36">Southon et&#x20;al., 2002</xref>; <xref ref-type="bibr" rid="B58">Yu et&#x20;al., 2010</xref>), to compute the mean age and 2&#x3c3; uncertainty at 1&#xa0;cm resolution. Such a chronological framework hints a possible hiatus of sedimentary deposit at the depth between &#x223c;65 and 85&#xa0;cm (<xref ref-type="fig" rid="F1">Figure&#x20;1C</xref>; see details in <xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>). Hence, we mainly focus on the topmost 65&#xa0;cm of the core YJ, roughly spanning the past &#x223c;1,000&#xa0;years, to analyze GDGT biomarkers for detecting the AMC signal across the LIA and&#x20;MCA.</p>
</sec>
<sec id="s2-2">
<title>Organic Biomarkers</title>
<p>Core YJ was sampled continuously with a step of 1&#xa0;cm down its uppermost 65&#xa0;cm, which, based on our chronology as stated in <italic>Core Site and Chronology</italic> section, guaranteed a temporal resolution of &#x223c;10&#x2013;15&#xa0;years per sample for the past &#x223c;1,000&#xa0;years. Afterward, bulk sediment samples (&#x223c;5&#xa0;g) were freeze-dried, then grounded, and soaked to extract total lipids by solvent dichloromethane (DCM): methanol (MeOH) (9:1; v/v) in 60&#xa0;ml vials, under an ultrasonic wave in the 40&#xb0;C water bath for three cycles (&#x223c;15&#xa0;min each). The extract was subsequently hydrolyzed with 6% KOH in MeOH to remove alkenoates and separated into three fractions <italic>via</italic> silica gel column chromatography with successive eluents of <italic>n</italic>-hexane, DCM, and MeOH, respectively. Finally, GDGTs were isolated in MeOH fraction, alkenones in DCM fraction, and <italic>n</italic>-alkanes in hexane fraction.</p>
<p>Analyses of MeOH fraction were conducted on high-performance liquid chromatography atmospheric pressure chemical ionization (HPLC-APCI)-mass spectrometry (e.g., <xref ref-type="bibr" rid="B29">Liu et&#x20;al., 2013</xref>). An aliquot of the fraction was directly dried under N<sub>2</sub>, and then redissolved in hexane: isopropanol (99:1; v/v) and filtered after mixing with a known amount of C<sub>46</sub> internal standard (<xref ref-type="bibr" rid="B14">Huguet et&#x20;al., 2006</xref>). Selected ion monitoring (SIM), which targets specific mass numbers for GDGT components (membrane lipids biosynthesized as multiple homolog series of isoprenoid or methyl-branched isomers, termed isoprenoid-GDGTs, and branched-GDGTs, respectively, see detailed description in <xref ref-type="bibr" rid="B35">Schouten et&#x20;al., 2013</xref>), was used to enhance the detection sensitivity. Quantification was carried out by integrating the peak area of [M &#x2b; H]<sup>&#x2b;</sup> ions in the extracted ion chromatogram and comparing with the C<sub>46</sub> internal standard. We then calculated the ACE, BIT, and <inline-formula id="inf10">
<mml:math id="m10">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
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<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> indices using equations as given below:</p>
<p>
<inline-formula id="inf11">
<mml:math id="m11">
<mml:mrow>
<mml:mtext>ACE</mml:mtext>
<mml:mo>&#x3d;</mml:mo>
<mml:mtext>&#xa0;</mml:mtext>
<mml:mfrac>
<mml:mrow>
<mml:mtext>archaeol</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mtext>archaeol</mml:mtext>
<mml:mo>&#x2b;</mml:mo>
<mml:mtext>caldarchaeol</mml:mtext>
<mml:mo>&#xd7;</mml:mo>
<mml:mn>10</mml:mn>
</mml:mrow>
</mml:mfrac>
<mml:mtext>&#xa0;</mml:mtext>
<mml:mo>&#xd7;</mml:mo>
<mml:mn>100</mml:mn>
</mml:mrow>
</mml:math>
</inline-formula> (<xref ref-type="bibr" rid="B40">Turich and Freeman 2011</xref>; <xref ref-type="bibr" rid="B43">Wang et&#x20;al., 2013</xref>),</p>
<p>
<inline-formula id="inf12">
<mml:math id="m12">
<mml:mrow>
<mml:mtext>BIT</mml:mtext>
<mml:mo>&#x3d;</mml:mo>
<mml:mtext>&#xa0;</mml:mtext>
<mml:mfrac>
<mml:mrow>
<mml:mtext>I</mml:mtext>
<mml:mo>&#x2b;</mml:mo>
<mml:mtext>II</mml:mtext>
<mml:mo>&#x2b;</mml:mo>
<mml:mtext>III</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mtext>I</mml:mtext>
<mml:mo>&#x2b;</mml:mo>
<mml:mtext>II</mml:mtext>
<mml:mo>&#x2b;</mml:mo>
<mml:mo>&#x2b;</mml:mo>
<mml:mtext>III</mml:mtext>
<mml:mo>&#x2b;</mml:mo>
<mml:mtext>cren</mml:mtext>
</mml:mrow>
</mml:mfrac>
<mml:mo>&#xa0;</mml:mo>
</mml:mrow>
</mml:math>
</inline-formula> (<xref ref-type="bibr" rid="B10">Hopmans et&#x20;al., 2004</xref>),</p>
<p>
<inline-formula id="inf13">
<mml:math id="m13">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
<mml:mo>&#x3d;</mml:mo>
<mml:mtext>&#xa0;</mml:mtext>
<mml:mfrac>
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>GDGT</mml:mtext>
</mml:mrow>
<mml:mn>2</mml:mn>
</mml:msub>
<mml:mo>&#x2b;</mml:mo>
<mml:msub>
<mml:mrow>
<mml:mtext>GDGT</mml:mtext>
</mml:mrow>
<mml:mn>3</mml:mn>
</mml:msub>
<mml:mo>&#x2b;</mml:mo>
<mml:mrow>
<mml:mtext>cren</mml:mtext>
</mml:mrow>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>GDGT</mml:mtext>
</mml:mrow>
<mml:mn>1</mml:mn>
</mml:msub>
<mml:mo>&#x2b;</mml:mo>
<mml:msub>
<mml:mrow>
<mml:mtext>GDGT</mml:mtext>
</mml:mrow>
<mml:mn>2</mml:mn>
</mml:msub>
<mml:mo>&#x2b;</mml:mo>
<mml:msub>
<mml:mrow>
<mml:mtext>GDGT</mml:mtext>
</mml:mrow>
<mml:mn>3</mml:mn>
</mml:msub>
<mml:mo>&#x2b;</mml:mo>
<mml:mrow>
<mml:mtext>cren</mml:mtext>
</mml:mrow>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
</mml:mfrac>
</mml:mrow>
</mml:math>
</inline-formula> (<xref ref-type="bibr" rid="B34">Schouten et&#x20;al., 2002</xref>).&#x2003;<inline-formula id="inf14">
<mml:math id="m14">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> values were then converted to temperature estimates, using the calibration equation: SST &#x3d; 68.4 &#xd7;log (<inline-formula id="inf15">
<mml:math id="m15">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula>)&#x2b;38.6 (<xref ref-type="bibr" rid="B18">Kim et&#x20;al., 2010</xref>). Analytical uncertainties for our laboratory standards are typically less than 5% for the BIT and ACE values and 0.01 unit for <inline-formula id="inf16">
<mml:math id="m16">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula>.</p>
</sec>
</sec>
<sec sec-type="results" id="s3">
<title>Results</title>
<p>Throughout the past millennium, ACE values appear to be relatively high during the LIA, especially at its onset (centered around &#x223c;500&#xa0;years BP), as compared to the MCA (<xref ref-type="fig" rid="F3">Figure&#x20;3A</xref>). In contrast, the BIT index generally experiences a gradual declining trend from &#x223c;0.3 during the MCA (and the earlier epochs, marked by a possible hiatus in sediment accumulation and hence not shown here) toward &#x223c;0.15 in the recent years (<xref ref-type="fig" rid="F3">Figure&#x20;3B</xref>). Unlike these two modes, <inline-formula id="inf17">
<mml:math id="m17">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula>-based temperatures, although fluctuated within a large range (nearly about 3&#xb0;C in terms of magnitude, <xref ref-type="fig" rid="F3">Figure&#x20;3C</xref>), are apparently trendless over the investigated interval. However, when placed together with the existing <inline-formula id="inf18">
<mml:math id="m18">
<mml:mrow>
<mml:msubsup>
<mml:mtext>U</mml:mtext>
<mml:mrow>
<mml:mn>37</mml:mn>
</mml:mrow>
<mml:mrow>
<mml:mtext>K</mml:mtext>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
</mml:msubsup>
</mml:mrow>
</mml:math>
</inline-formula>-based SST record of the same core YJ (<xref ref-type="fig" rid="F3">Figures&#x20;3D,E</xref>), there exists certain similarity in the overall temporal patterns between SST (despite a substantial cooling of up to &#x223c;4&#xb0;C, <xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>) and <inline-formula id="inf19">
<mml:math id="m19">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
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</mml:msub>
</mml:mrow>
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</inline-formula> temperatures over the LIA (e.g., increase at the first half and decrease at the second half), but for the MCA, variations of these two independent records are clearly featured by different structures. Collectively, the LIA interval characterizes increase in ACE values and wind-borne hopane compounds (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>), and decrease in BIT ratios, SST, and vertical temperature gradient (<inline-formula id="inf20">
<mml:math id="m20">
<mml:mrow>
<mml:msubsup>
<mml:mtext>U</mml:mtext>
<mml:mrow>
<mml:mn>37</mml:mn>
</mml:mrow>
<mml:mrow>
<mml:mtext>K</mml:mtext>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula>values), relative to those during the MCA (<xref ref-type="fig" rid="F3">Figure&#x20;3</xref> and <xref ref-type="fig" rid="F4">Figure&#x20;4</xref>).</p>
<fig id="F3" position="float">
<label>FIGURE 3</label>
<caption>
<p>GDGT proxies of sediment core YJ during the last millennium, for example, <bold>(A)</bold> ratio of archaeol to caldarchaeol (ACE) (higher values downward), <bold>(B)</bold> the branched and isoprenoid tetraether (BIT), <bold>(C)</bold> <inline-formula id="inf21">
<mml:math id="m21">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula>-based temperatures, <bold>(D)</bold> <inline-formula id="inf22">
<mml:math id="m22">
<mml:mrow>
<mml:msubsup>
<mml:mtext>U</mml:mtext>
<mml:mrow>
<mml:mn>37</mml:mn>
</mml:mrow>
<mml:mrow>
<mml:mtext>K</mml:mtext>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
</mml:msubsup>
</mml:mrow>
</mml:math>
</inline-formula>-SST record, and <bold>(E)</bold> sedimentation rates (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>). Color bars outline the Little Ice Age (LIA, &#x223c;150&#x2013;550&#xa0;years BP) (green) and Medieval Climate Anomaly (MCA, &#x223c;700&#x2013;1,100&#xa0;years BP) (red), and triangles denote <sup>14</sup>C age control points.</p>
</caption>
<graphic xlink:href="feart-09-680180-g003.tif"/>
</fig>
<fig id="F4" position="float">
<label>FIGURE 4</label>
<caption>
<p>Organic geochemical proxies of core YJ over the last millennium, including <bold>(A)</bold> <inline-formula id="inf23">
<mml:math id="m23">
<mml:mrow>
<mml:msubsup>
<mml:mtext>U</mml:mtext>
<mml:mrow>
<mml:mn>37</mml:mn>
</mml:mrow>
<mml:mrow>
<mml:mtext>K</mml:mtext>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
</mml:msubsup>
</mml:mrow>
</mml:math>
</inline-formula>-SST record (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>), <bold>(B)</bold> <inline-formula id="inf24">
<mml:math id="m24">
<mml:mrow>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula>-based temperature, <bold>(C)</bold> vertical thermal gradient at site YJ (<inline-formula id="inf25">
<mml:math id="m25">
<mml:mrow>
<mml:msubsup>
<mml:mtext>U</mml:mtext>
<mml:mrow>
<mml:mn>37</mml:mn>
</mml:mrow>
<mml:mrow>
<mml:mtext>K</mml:mtext>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
<mml:msub>
<mml:mrow>
<mml:mtext>TEX</mml:mtext>
</mml:mrow>
<mml:mrow>
<mml:mn>86</mml:mn>
</mml:mrow>
</mml:msub>
</mml:mrow>
</mml:math>
</inline-formula> values), <bold>(D)</bold> <inline-formula id="inf26">
<mml:math id="m26">
<mml:mrow>
<mml:msubsup>
<mml:mtext>U</mml:mtext>
<mml:mrow>
<mml:mn>37</mml:mn>
</mml:mrow>
<mml:mrow>
<mml:mtext>K</mml:mtext>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
</mml:msubsup>
</mml:mrow>
</mml:math>
</inline-formula>-SST difference between two sites YJ and NS02G (YJ minus NS02G), <bold>(E)</bold> hopane compounds (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>), <bold>(F)</bold> the branched and isoprenoid tetraether (BIT), and <bold>(G)</bold> the ratio of archaeol to caldarchaeol (ACE). Note that magnetic susceptibility at Lake Huguangyan Maar (higher values downward, <xref ref-type="bibr" rid="B57">Yancheva et&#x20;al., 2007</xref>) is also plotted <bold>(H)</bold> for comparison (with a possible shift of their peaks due to the age uncertainty). Color bars mark the same intervals as in <xref ref-type="fig" rid="F3">Figure&#x20;3</xref> (two cold epochs within the LIA, e.g., &#x223c;250&#xa0;years BP and &#x223c;500&#xa0;years BP, are further highlighted).</p>
</caption>
<graphic xlink:href="feart-09-680180-g004.tif"/>
</fig>
</sec>
<sec sec-type="discussion" id="s4">
<title>Discussion</title>
<p>Recent studies have shown that the possible source of brGDGTs, for example, terrigenous originated (e.g., soil) or <italic>in situ</italic> synthesized (mainly at subsurface waters), is critical to determine the BIT index and thus its proper explanation (<xref ref-type="bibr" rid="B50">Weijers et&#x20;al., 2014</xref>; <xref ref-type="bibr" rid="B53">Xiao et&#x20;al., 2016</xref>; <xref ref-type="bibr" rid="B46">Wang et&#x20;al., 2021</xref>). For example, more subsurface production of brGDGTs in the Qiongzhou Strait is suggested to be responsible for higher BIT values (&#x223c;0.4&#x2013;0.6), which, as a result, reflect enhanced stratification of the onsite water column and thus change in summer AMC strength (<xref ref-type="bibr" rid="B46">Wang et&#x20;al., 2021</xref>). At our study site YJ, BIT values, primarily subjected to crenarchaeol (one major component of isoGDGTs) rather than brGDGT variations (<xref ref-type="sec" rid="s11">Supplementary Figure&#x20;1</xref>), also imply water column stratification. A set of field surveys, based on collection of both the sediment trap and core-top samples, show that, at the transition zones between the Pearl River estuary and the SCS northern coast, the bloom of autotrophic ammonia-oxidizing <italic>Thaumarchaeota</italic>, main producers of isoGDGTs with limited brGDGTs, tends to preferably occur under the hydrological conditions in the coldest months, like low light levels (e.g., <xref ref-type="bibr" rid="B60">Zhang et&#x20;al., 2013</xref>; <xref ref-type="bibr" rid="B44">Wang et&#x20;al., 2015</xref>; <xref ref-type="bibr" rid="B15">Jia et&#x20;al., 2017</xref>) and less stratified water. Meanwhile, at normal marine settings, including those on the continental shelf, light and redox conditions can also yield redistribution of <italic>Euryarchaeota</italic>/<italic>Archaea</italic> community, leading to stratification of archaeal membrane lipids (with relatively high archaeol in subsurface waters, <xref ref-type="bibr" rid="B41">Turich et&#x20;al., 2007</xref>; <xref ref-type="bibr" rid="B50">Weijers et&#x20;al., 2014</xref>; <xref ref-type="bibr" rid="B53">Xiao et&#x20;al., 2016</xref>; <xref ref-type="bibr" rid="B63">Zhu et&#x20;al., 2016</xref>). In this sense, the coeval variations of isoGDGTs and archaeol abundance in our particular case may cause opposite temporal patterns of BIT and ACE indices (<xref ref-type="sec" rid="s11">Supplementary Figures 1, 2</xref>). This fact, in contrary to a recent study presented by <xref ref-type="bibr" rid="B46">Wang et&#x20;al. (2021)</xref> who have applied the concomitant increase in these two proxies to represent enhanced stratification of the northern SCS coastal water, thereby calls for other interpretation(s) to reconcile competing patterns of our BIT and ACE proxies (<xref ref-type="fig" rid="F3">Figures 3A,B</xref>). Considering the small variations of BIT values and brGDGTs (<xref ref-type="sec" rid="s11">Supplementary Figure&#x20;1</xref>), we thus interpret relatively low BIT ratios during the LIA as increased production of the ubiquitous <italic>Thaumarchaeota</italic>, relative to other <italic>Euryarchaeota</italic>/<italic>Archaea</italic>. Besides, it is also worth stressing that despite similar features of changes in crenarchaeol and caldarchaeol (GDGT-0) (<xref ref-type="sec" rid="s11">Supplementary Figures 1, 2</xref>), two most abundant components of isoGDGTs, the observed ACE values here may still primarily respond to <italic>Euryarchaeota</italic>/<italic>Archaea</italic> community changes, therefore no longer being an indicator of water column stratification (e.g., <xref ref-type="bibr" rid="B46">Wang et&#x20;al., 2021</xref>).</p>
<p>Based on the results of previous studies (<xref ref-type="bibr" rid="B40">Turich and Freeman, 2011</xref>; <xref ref-type="bibr" rid="B9">He et&#x20;al., 2020</xref>), the ACE index might represent salinity if it mainly responds to <italic>Euryarchaeota</italic>/<italic>Archaea</italic> community changes. This prerequisite indeed exists in our case, because one could apparently see a major control of <italic>Euryarchaeota</italic>/<italic>Archaea</italic> on the ACE record (<xref ref-type="sec" rid="s11">Supplementary Figure&#x20;2</xref>). Due to the different characteristics of BIT and ACE records that strongly exclude the latter as a tracer of stratification (<xref ref-type="bibr" rid="B46">Wang et&#x20;al., 2021</xref>), we instead assume ACE to manifest salinity. As such, multi-centennial&#x2013;scale variations in our ACE record, as depicted in <xref ref-type="fig" rid="F4">Figure&#x20;4G</xref>, suggest increased (decreased) salinity of the onsite water column across the LIA (MCA) (<xref ref-type="bibr" rid="B40">Turich and Freeman, 2011</xref>). Together with the inference of the available <inline-formula id="inf27">
<mml:math id="m27">
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<mml:mtext>U</mml:mtext>
<mml:mrow>
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</inline-formula>-SST record and wind-borne hopane contents, as earlier reported (<xref ref-type="fig" rid="F4">Figures 4A,E</xref>), relatively saline conditions at our site, although only qualitatively estimated (if also taking into account the small range of vertical salinity gradient, <xref ref-type="fig" rid="F2">Figure&#x20;2</xref>), took place along with an intensification of winter AMC strength during the LIA, and <italic>vice versa</italic> for the MCA. Indeed, observational datasets confirm that, on seasonal timescales, there is a homogeneous structure of <italic>in situ</italic> salinity and temperature changes in winter (i.e.,&#x20;&#x223c;33.4&#xa0;psu and &#x223c;20&#xb0;C down the entire water column, respectively, <xref ref-type="sec" rid="s11">Supplementary Figure&#x20;3</xref>), relative to those in summer (i.e.,&#x20;&#x223c;32.4&#xa0;psu/28.3&#xb0;C at surface and &#x223c;33.4&#xa0;psu/27.1&#xb0;C at &#x223c;10&#x2013;15&#xa0;m water depth; <xref ref-type="bibr" rid="B64">Zweng et&#x20;al., 2013</xref>). In analogy with this scenario, it is possible that a stronger winter AMC during the LIA would have promoted vertical mixing of the onsite water column which; as a result, it would have brought more cold waters and production of (halophilic) <italic>Euryarchaeota</italic>/<italic>Archaea</italic> community (archaeol, the major driver of ACE values) at the subsurface layers toward upward, thereby decreasing SSTs while increasing its salinity. Notably, during the LIA cold interval, a less input of riverine discharge like the Pearl River drainage, due to the concomitant reduction of summer AMC intensity, as effectively corroborated by a growing body of compelling and independent evidence (e.g., <xref ref-type="bibr" rid="B8">Dykoski et&#x20;al., 2005</xref>; <xref ref-type="bibr" rid="B48">Wang et&#x20;al., 2005</xref>; <xref ref-type="bibr" rid="B61">Zhang et&#x20;al., 2008</xref>; <xref ref-type="bibr" rid="B45">Wang et&#x20;al., 2012</xref>; <xref ref-type="bibr" rid="B24">Lee et&#x20;al., 2019</xref>), may have also somewhat contributed to the inferred salinity increase here. Because these two processes are naturally coupled together from a climatological perspective, it is still difficult to assuredly claim which should play a major role in driving the higher salinity during the LIA. Still, an in-depth examination of winter (<italic>via</italic> mixing of subsurface waters) and/or summer (<italic>via</italic> decrease of riverine discharge) AMC impact on <italic>in situ</italic> salinity will need additional work in the future, for example, model simulations in particular. Regardless, variations in winter AMC strength, as inferred from both magnetic susceptibility at Huguangyan Maar Lake (<xref ref-type="bibr" rid="B57">Yancheva et&#x20;al., 2007</xref>) (<xref ref-type="fig" rid="F4">Figure&#x20;4H</xref>), the <inline-formula id="inf28">
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</inline-formula> SST record and wind-borne hopane contents at site YJ, are strongly suggested to modulate the water column structure at the SCS northern coasts, for example, by superimposing additional cooling effect on the top of the LIA cold climate background (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>).</p>
<p>The physical mechanism for our inference is further substantiated by the BIT index and <inline-formula id="inf29">
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</inline-formula>-derived temperature records (<xref ref-type="fig" rid="F3">Figures 3B,C</xref>). Based on the observations of i) more isoGDGT abundance at the northern SCS shelf in winter (e.g., roughly three times higher than in summer, <xref ref-type="bibr" rid="B15">Jia et&#x20;al., 2017</xref>) and ii) its primary role (without contribution of terrigenous lipid input as represented by hopane contents, <xref ref-type="fig" rid="F4">Figure&#x20;4E</xref>, and brGDGTs, <xref ref-type="sec" rid="s11">Supplementary Figure&#x20;1</xref>) in regulating variations in the BIT index in our case, lower (higher) BIT values during the LIA (MCA) hence probably result from increased (decreased) production of the <italic>Thaumarchaeota</italic>, which is in good support of more (less) prevalence of wintertime conditions (<xref ref-type="bibr" rid="B60">Zhang et&#x20;al., 2013</xref>; <xref ref-type="bibr" rid="B44">Wang et&#x20;al., 2015</xref>; <xref ref-type="bibr" rid="B15">Jia et&#x20;al., 2017</xref>). Combined with small BIT values downcore (roughly &#x3c;0.3), terrigenous materials thus exert little (if any) impact on the <inline-formula id="inf30">
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</inline-formula> proxy (and its calibrated temperature). For the <inline-formula id="inf31">
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</inline-formula> thermometer, recent studies by <xref ref-type="bibr" rid="B15">Jia et&#x20;al. (2017)</xref> and <xref ref-type="bibr" rid="B49">Wei et&#x20;al. (2020)</xref> have also suggested that at the northern SCS coast, its estimates are commonly comparable to or slightly lower than winter SSTs, hence indicative of temperature signals in cold season (<xref ref-type="fig" rid="F2">Figure&#x20;2</xref>). This interpretation, if true in our case, could explain the overall resemblance between our <inline-formula id="inf32">
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</inline-formula> values and the <inline-formula id="inf33">
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</inline-formula> SST record over the LIA (<xref ref-type="fig" rid="F3">Figure&#x20;3</xref>), as it strongly indicates the homogeneity of thermal signals, in line with enhanced vertical mixing of onsite water due to a stronger AMC then. However, we still note that prior to the LIA interval, there existed slightly cooler (&#x223c;0.5&#xb0;C) values of <inline-formula id="inf34">
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</inline-formula> proxy during the MCA (<xref ref-type="fig" rid="F3">Figure&#x20;3</xref>). Such observation, based on the winter temperature signals as earlier asserted (<xref ref-type="bibr" rid="B15">Jia et&#x20;al., 2017</xref>; <xref ref-type="bibr" rid="B49">Wei et&#x20;al., 2020</xref>), should necessitate a strengthening of winter AMC strength during the MCA (relative to the LIA), evidently contradicting not only our <inline-formula id="inf35">
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</inline-formula> SST and hopane records (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>) but also other terrestrial paleorecords (e.g., <xref ref-type="bibr" rid="B57">Yancheva et&#x20;al., 2007</xref>; <xref ref-type="bibr" rid="B17">Kang et&#x20;al., 2020</xref>). Therefore, additional parameter(s) must also be included here for completely understanding our <inline-formula id="inf36">
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</inline-formula> record.</p>
<p>In our case, downcore <inline-formula id="inf37">
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</inline-formula> values, calculated to be &#x223c;18.8 &#xb1;&#x20;1.2&#xb0;C (<xref ref-type="fig" rid="F3">Figure&#x20;3C</xref>, and roughly &#x223c;2&#xb0;C higher if using regional equation developed by <xref ref-type="bibr" rid="B15">Jia et&#x20;al., 2017</xref>), are obviously lower than the <italic>in situ</italic> instrumental SST in winter (<xref ref-type="fig" rid="F2">Figure&#x20;2</xref>) considering that &#x223c;20% of <italic>Thaumarchaeota</italic> is actually produced in other seasons (<xref ref-type="bibr" rid="B44">Wang et&#x20;al., 2015</xref>; <xref ref-type="bibr" rid="B15">Jia et&#x20;al., 2017</xref>; <xref ref-type="bibr" rid="B49">Wei et&#x20;al., 2020</xref>). Further, in light of i) its different features with the <inline-formula id="inf38">
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</inline-formula> SST record, ii) lower BIT values (&#x3c;&#x223c;0.3), and iii) use of the <inline-formula id="inf39">
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</inline-formula> proxy to manifest the temperature of subsurface rather than surface waters, for example, over the western Pacific marginal sea (<xref ref-type="bibr" rid="B55">Xing et&#x20;al., 2015</xref>), we here apply <inline-formula id="inf40">
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</inline-formula> values as temperature indicators of an integrated water column but also biased toward winter season and subsurface waters (<xref ref-type="fig" rid="F2">Figure&#x20;2</xref>). Although it is quite difficult to differentiate the inhabit depths of <italic>Haptophyceae algae</italic> (alkenone-producing species) and <italic>Thaumarchaeota</italic> at site YJ with &#x223c;21&#xa0;m water depth, the use of <inline-formula id="inf41">
<mml:math id="m41">
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<mml:mtext>U</mml:mtext>
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</mml:mrow>
<mml:mrow>
<mml:mtext>K</mml:mtext>
<mml:mtext>&#x2032;</mml:mtext>
</mml:mrow>
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</mml:mrow>
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</inline-formula>- and <inline-formula id="inf42">
<mml:math id="m42">
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</inline-formula>-derived temperatures to reflect the surface and subsurface thermal signals has been confirmed at the shallow water column in the northern SCS coast (e.g., &#x223c;50&#xa0;m in <xref ref-type="bibr" rid="B46">Wang et&#x20;al., 2021</xref>). Following such interpretation, within the LIA, an overall similarity in the temporal patterns of these two paired records (<xref ref-type="fig" rid="F3">Figure&#x20;3C</xref> and <xref ref-type="fig" rid="F4">Figure&#x20;4A</xref>) indicates the homogeneity of thermal signature down the entire water column here, thus calling for an intensification of vertical mixing due to a stronger winter AMC influence (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>). In contrast, during the MCA, a weaker winter AMC would have reduced vertical mixing which, together with a stronger summer AMC simultaneously (<xref ref-type="bibr" rid="B8">Dykoski et&#x20;al., 2005</xref>; <xref ref-type="bibr" rid="B61">Zhang et&#x20;al., 2008</xref>), intensified stratification of the water column and then eliminated the similar imprint of thermal conditions at different water depths, as extracted by <inline-formula id="inf43">
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</inline-formula>-SST and <inline-formula id="inf44">
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</inline-formula> temperature records, respectively (<xref ref-type="fig" rid="F3">Figure&#x20;3C</xref> and <xref ref-type="fig" rid="F4">Figure&#x20;4A</xref>).</p>
<p>Since <inline-formula id="inf45">
<mml:math id="m45">
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</inline-formula> mainly documents annual mean SST toward summer biases (<xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>) while the <inline-formula id="inf46">
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</inline-formula> index is largely controlled by winter temperature and the subsurface signal (<xref ref-type="fig" rid="F2">Figure&#x20;2</xref>), the difference between our paired <inline-formula id="inf47">
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</inline-formula>- and <inline-formula id="inf48">
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</inline-formula>-values, roughly &#x223c;6&#x2013;7&#xb0;C, can be used as a rough measure to represent thermal contrast at both seasonal and vertical scales (<xref ref-type="fig" rid="F4">Figure&#x20;4C</xref>). As such, it shows that thermal gradient at the LIA was relatively small, for example, particularly down to &#x223c;4&#xb0;C at a few short-lived epochs such as &#x223c;250&#xa0;years BP, and &#x223c;500&#xa0;years BP when the <inline-formula id="inf49">
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</inline-formula>-SST record underwent abnormal cooling (of up &#x223c;4&#xb0;C, <xref ref-type="fig" rid="F4">Figure&#x20;4A</xref>), in comparison to that at the MCA (e.g., roughly &#x223c;8&#xb0;C, <xref ref-type="fig" rid="F4">Figure&#x20;4C</xref>). Together with similar variations of <inline-formula id="inf50">
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</inline-formula> and <inline-formula id="inf51">
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</inline-formula> records during the LIA, these multiple lines of independent evidence call for more influence of stronger AMC on the vertical mixing of subsurface water and thereby reduced stratification of the water column. Notably, considering the evolutionary role of winter AMC in regulating vertical mixing of subsurface waters at multi-centennial timescales, as discussed above, it is reasonable that, at our site YJ, the <inline-formula id="inf52">
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</mml:mrow>
</mml:msubsup>
<mml:mo>&#x2212;</mml:mo>
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</inline-formula> gradient during the MCA is also likely amplified by an intensified stratification of the water column (and thus characterized by relatively larger errors) simultaneously. Reduction of vertical mixing, due to a weaker winter AMC (than during the LIA), would yield less influence of the subsurface cooling signal on surface temperature (generated by the <inline-formula id="inf53">
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</inline-formula> proxy, for example, <xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>). Water column stratification could also reshape <italic>Euryarchaeota</italic>/<italic>Archaea</italic> community and thus potentially drive <inline-formula id="inf54">
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</inline-formula> to lower values. This could have also contributed to the <inline-formula id="inf55">
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</inline-formula> values during the MCA, not particularly high as compared to the <inline-formula id="inf56">
<mml:math id="m56">
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</mml:mrow>
<mml:mrow>
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</mml:msubsup>
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</inline-formula>-SST values (<xref ref-type="fig" rid="F3">Figure&#x20;3C</xref>). On the other hand, the <inline-formula id="inf57">
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</mml:mrow>
</mml:math>
</inline-formula> proxy well captures the temporal pattern of temperature changes within the LIA. Despite the potential contribution from <italic>Euryarchaeota</italic>/<italic>Archaea</italic> community changes, our calculation of vertical thermal gradient apparently resembles the temporal patterns of SST difference between the coast and open ocean (e.g., using <inline-formula id="inf58">
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</inline-formula>-SST records at two sites YJ and NS02G, <xref ref-type="fig" rid="F4">Figure&#x20;4D</xref>), whereas the SST difference is used to track winter AMC variability (<xref ref-type="bibr" rid="B21">Kong et&#x20;al., 2017</xref>; <xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>). Assuming that the open sea SST represents &#x201c;original&#x201d; temperature signal that is not strongly impacted by the winter AMC, the temperature difference between the two locations could indicate the winter AMC impact. The difference of our <inline-formula id="inf59">
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</inline-formula> values captures most of the features in the two <inline-formula id="inf61">
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</inline-formula>-SST difference (<xref ref-type="fig" rid="F4">Figures 4C,D</xref>), suggesting that the <inline-formula id="inf62">
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</mml:math>
</inline-formula> proxy largely manifests the integrated water column/subsurface temperature at this site, despite its complicated nature. Hence, vertical thermal difference at the site YJ, associated with the strengthening (weakening) of onsite vertical mixing, facilitates our explanation of enhanced (reduced) winter AMC strength during the LIA (MCA). Altogether, secular changes in winter AMC intensity, for example, its intensification during the LIA, are capable of i) transporting terrigenous biomass, as substantiated by exponential increase of wind-borne hopane compounds (<xref ref-type="fig" rid="F4">Figure&#x20;4E</xref>); ii) exerting additional cooling signals upon typical cold climate background (through both atmospheric and oceanic processes, <xref ref-type="bibr" rid="B62">Zhang et&#x20;al., 2019</xref>), as seen by abnormal SST decrease (<xref ref-type="fig" rid="F4">Figure&#x20;4A</xref>); and iii) enhancing vertical mixing (thereby reducing stratification) of the onsite water column, as reinforced by the similarity in <inline-formula id="inf63">
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</inline-formula> temperatures and decrease in their difference (<xref ref-type="fig" rid="F4">Figure&#x20;4C</xref>), as well as lower BIT values.</p>
</sec>
<sec sec-type="conclusion" id="s5">
<title>Conclusion</title>
<p>We used a sediment core YJ, collected from the northern SCS coast, to analyze GDGT lipid biomarkers during the past millennium. These proxies, together with published alkenone (<inline-formula id="inf65">
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</inline-formula>)-SST and hopane records from the same core, help constrain the dynamical interplay between northern SCS coastal conditions and winter AMC intensity at multi-centennial timescales. In general, variations in ACE and BIT indices, although characterized by opposite features, indicate a more prevalent regime of the winter season at the LIA (than the MCA). Further comparison of paired <inline-formula id="inf66">
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<mml:msubsup>
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<mml:mrow>
<mml:mn>86</mml:mn>
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</mml:mrow>
</mml:math>
</inline-formula> temperature records, with the caution that the latter might be additionally affected by non-thermal factor, shows decrease (increase) in the vertical thermal gradient during the LIA (MCA), thereby calling for a well (less)-mixing of the onsite water column. Therefore, winter AMC changes would have greatly regulated both thermal and saline properties of the shallow waters at northern SCS coasts. Our results necessitate a careful examination of the AMC coupling processes for better understanding coastal environment in the past, for example, during the LIA and MCA, and also in the near future.</p>
</sec>
</body>
<back>
<sec id="s6">
<title>Data Availability Statement</title>
<p>The original contributions presented in the study are included in the article/<xref ref-type="sec" rid="s11">Supplementary Material</xref>; further inquiries can be directed to the corresponding author.</p>
</sec>
<sec id="s7">
<title>Author Contributions</title>
<p>Conceptualization: ZL; investigation: KZ, CH, DK, YH, HW, and ZX; formal analysis: YZ and ZL; resources: WL, GW, and ZL; funding acquisition: WL and ZL; writing: YZ and ZL led the writing with intellectual contributions from all coauthors.</p>
</sec>
<sec id="s8">
<title>Funding</title>
<p>This work was supported by the National Key Research and Development Program of China (2016YFA0601204) and Hong Kong RGC Grant 17325516.</p>
</sec>
<sec sec-type="COI-statement" id="s9">
<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>
<p>The reviewer (YH) declared a shared affiliation with several of the authors, (HW, WL, ZX), to the handling editor at time of review.</p>
</sec>
<sec sec-type="disclaimer" id="s10">
<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>
<ack>
<p>We sincerely thank guest editors for inviting contribution to this special issue and anonymous referees for providing insightful comments to improve our manuscript.</p>
</ack>
<sec id="s11">
<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/feart.2021.680180/full#supplementary-material">https://www.frontiersin.org/articles/10.3389/feart.2021.680180/full&#x23;supplementary-material</ext-link>
</p>
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<supplementary-material xlink:href="DataSheet2.xlsx" id="SM2" mimetype="application/xlsx" xmlns:xlink="http://www.w3.org/1999/xlink"/>
</sec>
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