Two-Dimensional Superconductivity and Anomalous Vortex Dissipation in Newly Discovered Transition Metal Dichalcogenide-Based Superlattices

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-11-25 DOI:10.1021/jacs.4c09248
Mengzhu Shi, Kaibao Fan, Houpu Li, Senyang Pan, Jiaqiang Cai, Nan Zhang, Hongyu Li, Tao Wu, Jinglei Zhang, Chuanying Xi, Ziji Xiang, Xianhui Chen
{"title":"Two-Dimensional Superconductivity and Anomalous Vortex Dissipation in Newly Discovered Transition Metal Dichalcogenide-Based Superlattices","authors":"Mengzhu Shi, Kaibao Fan, Houpu Li, Senyang Pan, Jiaqiang Cai, Nan Zhang, Hongyu Li, Tao Wu, Jinglei Zhang, Chuanying Xi, Ziji Xiang, Xianhui Chen","doi":"10.1021/jacs.4c09248","DOIUrl":null,"url":null,"abstract":"Properties of layered superconductors can vary drastically when thinned down from bulk to monolayer owing to the reduced dimensionality and weakened interlayer coupling. In transition metal dichalcogenides (TMDs), the inherent symmetry breaking effect in atomically thin crystals prompts novel states of matter such as Ising superconductivity with an extraordinary in-plane upper critical field. Here, we demonstrate that two-dimensional (2D) superconductivity resembling those in atomic layers but with more fascinating behaviors can be realized in the bulk crystals of two new TMD-based superconductors Ba<sub>0.75</sub>ClTaS<sub>2</sub> and Ba<sub>0.75</sub>ClTaSe<sub>2</sub> with superconducting transition temperatures 2.75 and 1.75 K, respectively. They comprise an alternating stack of H-type TMD layers and Ba–Cl layers. In both materials, intrinsic 2D superconductivity develops below a Berezinskii–Kosterlitz–Thouless transition. The upper critical field along <i>the ab</i> plane (<i></i><span style=\"color: inherit;\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"&gt;&lt;msubsup&gt;&lt;mrow&gt;&lt;mi&gt;H&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mrow&gt;&lt;mo stretchy=\"false\"&gt;|&lt;/mo&gt;&lt;mo stretchy=\"false\"&gt;|&lt;/mo&gt;&lt;/mrow&gt;&lt;mi&gt;a&lt;/mi&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;/mrow&gt;&lt;/msubsup&gt;&lt;/math&gt;' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"><nobr aria-hidden=\"true\"><span overflow=\"scroll\" style=\"width: 2.446em; display: inline-block;\"><span style=\"display: inline-block; position: relative; width: 2.219em; height: 0px; font-size: 110%;\"><span style=\"position: absolute; clip: rect(1.026em, 1002.22em, 2.673em, -999.997em); top: -2.156em; left: 0em;\"><span><span><span style=\"display: inline-block; position: relative; width: 2.219em; height: 0px;\"><span style=\"position: absolute; clip: rect(3.185em, 1000.91em, 4.151em, -999.997em); top: -3.974em; left: 0em;\"><span><span style=\"font-family: STIXMathJax_Normal-italic;\">𝐻<span style=\"display: inline-block; overflow: hidden; height: 1px; width: 0.06em;\"></span></span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; clip: rect(3.298em, 1001.2em, 4.264em, -999.997em); top: -4.429em; left: 0.969em;\"><span><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Variants;\">|</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Variants;\">|</span></span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑎</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑏</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; clip: rect(3.355em, 1000.74em, 4.151em, -999.997em); top: -3.634em; left: 0.855em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑐</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\">2</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span></span></span></span><span style=\"display: inline-block; width: 0px; height: 2.162em;\"></span></span></span><span style=\"display: inline-block; overflow: hidden; vertical-align: -0.434em; border-left: 0px solid; width: 0px; height: 1.566em;\"></span></span></nobr><span role=\"presentation\"><math display=\"inline\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><msubsup><mrow><mi>H</mi></mrow><mrow><mi>c</mi><mn>2</mn></mrow><mrow><mrow><mo stretchy=\"false\">|</mo><mo stretchy=\"false\">|</mo></mrow><mi>a</mi><mi>b</mi></mrow></msubsup></math></span></span><script type=\"math/mml\"><math display=\"inline\" overflow=\"scroll\"><msubsup><mrow><mi>H</mi></mrow><mrow><mi>c</mi><mn>2</mn></mrow><mrow><mrow><mo stretchy=\"false\">|</mo><mo stretchy=\"false\">|</mo></mrow><mi>a</mi><mi>b</mi></mrow></msubsup></math></script>) exceeds the Pauli limit (<i>μ</i><sub><i>0</i></sub><i>H</i><sub>p</sub>); in particular, Ba<sub>0.75</sub>ClTaSe<sub>2</sub> exhibits an extremely high <i></i><span style=\"color: inherit;\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;&amp;#x3BC;&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;0&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;msubsup&gt;&lt;mrow&gt;&lt;mi&gt;H&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mrow&gt;&lt;mo stretchy=\"false\"&gt;|&lt;/mo&gt;&lt;mo stretchy=\"false\"&gt;|&lt;/mo&gt;&lt;/mrow&gt;&lt;mi&gt;a&lt;/mi&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;/mrow&gt;&lt;/msubsup&gt;&lt;/math&gt;' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"><nobr aria-hidden=\"true\"><span overflow=\"scroll\" style=\"width: 3.582em; display: inline-block;\"><span style=\"display: inline-block; position: relative; width: 3.241em; height: 0px; font-size: 110%;\"><span style=\"position: absolute; clip: rect(1.026em, 1003.24em, 2.673em, -999.997em); top: -2.156em; left: 0em;\"><span><span><span style=\"display: inline-block; position: relative; width: 1.026em; height: 0px;\"><span style=\"position: absolute; clip: rect(3.355em, 1000.57em, 4.321em, -999.997em); top: -3.974em; left: 0em;\"><span><span style=\"font-family: STIXMathJax_Normal-italic;\">𝜇</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; top: -3.747em; left: 0.571em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\">0</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span></span></span><span><span style=\"display: inline-block; position: relative; width: 2.219em; height: 0px;\"><span style=\"position: absolute; clip: rect(3.185em, 1000.91em, 4.151em, -999.997em); top: -3.974em; left: 0em;\"><span><span style=\"font-family: STIXMathJax_Normal-italic;\">𝐻<span style=\"display: inline-block; overflow: hidden; height: 1px; width: 0.06em;\"></span></span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; clip: rect(3.298em, 1001.2em, 4.264em, -999.997em); top: -4.429em; left: 0.969em;\"><span><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Variants;\">|</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Variants;\">|</span></span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑎</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑏</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; clip: rect(3.355em, 1000.74em, 4.151em, -999.997em); top: -3.634em; left: 0.855em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑐</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\">2</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span></span></span></span><span style=\"display: inline-block; width: 0px; height: 2.162em;\"></span></span></span><span style=\"display: inline-block; overflow: hidden; vertical-align: -0.434em; border-left: 0px solid; width: 0px; height: 1.566em;\"></span></span></nobr><span role=\"presentation\"><math display=\"inline\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><msub><mrow><mi>μ</mi></mrow><mrow><mn>0</mn></mrow></msub><msubsup><mrow><mi>H</mi></mrow><mrow><mi>c</mi><mn>2</mn></mrow><mrow><mrow><mo stretchy=\"false\">|</mo><mo stretchy=\"false\">|</mo></mrow><mi>a</mi><mi>b</mi></mrow></msubsup></math></span></span><script type=\"math/mml\"><math display=\"inline\" overflow=\"scroll\"><msub><mrow><mi>μ</mi></mrow><mrow><mn>0</mn></mrow></msub><msubsup><mrow><mi>H</mi></mrow><mrow><mi>c</mi><mn>2</mn></mrow><mrow><mrow><mo stretchy=\"false\">|</mo><mo stretchy=\"false\">|</mo></mrow><mi>a</mi><mi>b</mi></mrow></msubsup></math></script>≈ 14 <i>μ</i><sub><i>0</i></sub><i>H</i><sub><i>p</i></sub> and a colossal superconducting anisotropy (<i></i><span style=\"color: inherit;\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"&gt;&lt;msubsup&gt;&lt;mrow&gt;&lt;mi&gt;H&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mrow&gt;&lt;mo stretchy=\"false\"&gt;|&lt;/mo&gt;&lt;mo stretchy=\"false\"&gt;|&lt;/mo&gt;&lt;/mrow&gt;&lt;mi&gt;a&lt;/mi&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;/mrow&gt;&lt;/msubsup&gt;&lt;/math&gt;' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"><nobr aria-hidden=\"true\"><span overflow=\"scroll\" style=\"width: 2.446em; display: inline-block;\"><span style=\"display: inline-block; position: relative; width: 2.219em; height: 0px; font-size: 110%;\"><span style=\"position: absolute; clip: rect(1.026em, 1002.22em, 2.673em, -999.997em); top: -2.156em; left: 0em;\"><span><span><span style=\"display: inline-block; position: relative; width: 2.219em; height: 0px;\"><span style=\"position: absolute; clip: rect(3.185em, 1000.91em, 4.151em, -999.997em); top: -3.974em; left: 0em;\"><span><span style=\"font-family: STIXMathJax_Normal-italic;\">𝐻<span style=\"display: inline-block; overflow: hidden; height: 1px; width: 0.06em;\"></span></span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; clip: rect(3.298em, 1001.2em, 4.264em, -999.997em); top: -4.429em; left: 0.969em;\"><span><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Variants;\">|</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Variants;\">|</span></span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑎</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑏</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; clip: rect(3.355em, 1000.74em, 4.151em, -999.997em); top: -3.634em; left: 0.855em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑐</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\">2</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span></span></span></span><span style=\"display: inline-block; width: 0px; height: 2.162em;\"></span></span></span><span style=\"display: inline-block; overflow: hidden; vertical-align: -0.434em; border-left: 0px solid; width: 0px; height: 1.566em;\"></span></span></nobr><span role=\"presentation\"><math display=\"inline\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><msubsup><mrow><mi>H</mi></mrow><mrow><mi>c</mi><mn>2</mn></mrow><mrow><mrow><mo stretchy=\"false\">|</mo><mo stretchy=\"false\">|</mo></mrow><mi>a</mi><mi>b</mi></mrow></msubsup></math></span></span><script type=\"math/mml\"><math display=\"inline\" overflow=\"scroll\"><msubsup><mrow><mi>H</mi></mrow><mrow><mi>c</mi><mn>2</mn></mrow><mrow><mrow><mo stretchy=\"false\">|</mo><mo stretchy=\"false\">|</mo></mrow><mi>a</mi><mi>b</mi></mrow></msubsup></math></script>/<i></i><span style=\"color: inherit;\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"&gt;&lt;msubsup&gt;&lt;mrow&gt;&lt;mi&gt;H&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo lspace=\"0.03em\" rspace=\"0.03em\"&gt;&amp;#x22A5;&lt;/mo&gt;&lt;mi&gt;a&lt;/mi&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;/mrow&gt;&lt;/msubsup&gt;&lt;/math&gt;' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"><nobr aria-hidden=\"true\"><span overflow=\"scroll\" style=\"width: 2.56em; display: inline-block;\"><span style=\"display: inline-block; position: relative; width: 2.332em; height: 0px; font-size: 110%;\"><span style=\"position: absolute; clip: rect(1.139em, 1002.33em, 2.616em, -999.997em); top: -2.156em; left: 0em;\"><span><span><span style=\"display: inline-block; position: relative; width: 2.332em; height: 0px;\"><span style=\"position: absolute; clip: rect(3.185em, 1000.91em, 4.151em, -999.997em); top: -3.974em; left: 0em;\"><span><span style=\"font-family: STIXMathJax_Normal-italic;\">𝐻<span style=\"display: inline-block; overflow: hidden; height: 1px; width: 0.06em;\"></span></span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; clip: rect(3.355em, 1001.31em, 4.151em, -999.997em); top: -4.372em; left: 0.969em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main; padding-left: 0.06em; padding-right: 0.06em;\">⊥</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑎</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑏</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; clip: rect(3.355em, 1000.74em, 4.151em, -999.997em); top: -3.69em; left: 0.855em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑐</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\">2</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span></span></span></span><span style=\"display: inline-block; width: 0px; height: 2.162em;\"></span></span></span><span style=\"display: inline-block; overflow: hidden; vertical-align: -0.372em; border-left: 0px solid; width: 0px; height: 1.378em;\"></span></span></nobr><span role=\"presentation\"><math display=\"inline\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><msubsup><mrow><mi>H</mi></mrow><mrow><mi>c</mi><mn>2</mn></mrow><mrow><mo lspace=\"0.03em\" rspace=\"0.03em\">⊥</mo><mi>a</mi><mi>b</mi></mrow></msubsup></math></span></span><script type=\"math/mml\"><math display=\"inline\" overflow=\"scroll\"><msubsup><mrow><mi>H</mi></mrow><mrow><mi>c</mi><mn>2</mn></mrow><mrow><mo lspace=\"0.03em\" rspace=\"0.03em\">⊥</mo><mi>a</mi><mi>b</mi></mrow></msubsup></math></script>) of ∼150. Moreover, the temperature-field phase diagram of Ba<sub>0.75</sub>ClTaSe<sub>2</sub> under an in-plane magnetic field contains a large phase regime of vortex dissipation, which can be ascribed to the Josephson vortex motion, signifying an unprecedentedly strong fluctuation effect in TMD-based superconductors. Our results provide a new path toward the establishment of 2D superconductivity and novel exotic quantum phases in bulk crystals of TMD-based superconductors.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"58 1","pages":""},"PeriodicalIF":14.4000,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c09248","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
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Abstract

Properties of layered superconductors can vary drastically when thinned down from bulk to monolayer owing to the reduced dimensionality and weakened interlayer coupling. In transition metal dichalcogenides (TMDs), the inherent symmetry breaking effect in atomically thin crystals prompts novel states of matter such as Ising superconductivity with an extraordinary in-plane upper critical field. Here, we demonstrate that two-dimensional (2D) superconductivity resembling those in atomic layers but with more fascinating behaviors can be realized in the bulk crystals of two new TMD-based superconductors Ba0.75ClTaS2 and Ba0.75ClTaSe2 with superconducting transition temperatures 2.75 and 1.75 K, respectively. They comprise an alternating stack of H-type TMD layers and Ba–Cl layers. In both materials, intrinsic 2D superconductivity develops below a Berezinskii–Kosterlitz–Thouless transition. The upper critical field along the ab plane (Hc2||ab) exceeds the Pauli limit (μ0Hp); in particular, Ba0.75ClTaSe2 exhibits an extremely high μ0Hc2||ab≈ 14 μ0Hp and a colossal superconducting anisotropy (Hc2||ab/Hc2ab) of ∼150. Moreover, the temperature-field phase diagram of Ba0.75ClTaSe2 under an in-plane magnetic field contains a large phase regime of vortex dissipation, which can be ascribed to the Josephson vortex motion, signifying an unprecedentedly strong fluctuation effect in TMD-based superconductors. Our results provide a new path toward the establishment of 2D superconductivity and novel exotic quantum phases in bulk crystals of TMD-based superconductors.

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新发现的过渡金属二掺杂超晶格中的二维超导性和反常涡流耗散
由于尺寸减小和层间耦合减弱,当层状超导体从块状变薄到单层时,其性质会发生巨大变化。在过渡金属二掺杂物(TMDs)中,原子薄晶体固有的对称破缺效应会产生新的物质状态,如具有非同寻常的面内上临界场的伊辛超导性。在这里,我们证明了在两种基于 TMD 的新型超导体 Ba0.75ClTaS2 和 Ba0.75ClTaSe2 的块状晶体中可以实现类似原子层的二维(2D)超导,但具有更迷人的行为,其超导转变温度分别为 2.75 和 1.75 K。它们由 H 型 TMD 层和 Ba-Cl 层交替堆叠而成。在这两种材料中,本征二维超导电性都发生在贝列津斯基-科斯特利兹-无穷转变以下。沿 ab 平面的临界上场(𝐻||𝑎𝑏𝑐2Hc2||abHc2||ab)超过了保利极限(μ0Hp);特别是,Ba0.75ClTaSe2表现出极高的𝜇0𝐻||𝑎𝑏𝑐2μ0Hc2||abμ0Hc2||ab≈14 μ0Hp和巨大的超导各向异性(𝐻||𝑎𝑏𝑐2Hc2||abHc2||ab/𝐻⊥𝑎𝑏𝑐2Hc2⊥abHc2⊥ab)∼150。此外,Ba0.75ClTaSe2在面内磁场作用下的温场相图包含一个大的涡旋耗散相机制,它可以归因于约瑟夫森涡旋运动,这标志着在基于TMD的超导体中出现了前所未有的强烈波动效应。我们的研究结果为在基于 TMD 的超导体块体晶体中建立二维超导电性和新型奇异量子相提供了一条新途径。
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CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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