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Engineering Heterointerface to Synergistically Regulate Kinetics and Stress of Copper-Cobalt Selenide toward Reversible Magnesium/Lithium Hybrid Batteries. 设计异质界面以协同调节硒化铜钴的动力学和应力,从而实现可逆的镁/锂混合电池。
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-19 DOI: 10.1021/acs.nanolett.4c04123
Wenlong Wang, Miao Tian, Zhitao Wang, Heping Ma, Yibo Du, Wenhui Si, Wenming Zhang, Hui Ying Yang, Song Chen
{"title":"Engineering Heterointerface to Synergistically Regulate Kinetics and Stress of Copper-Cobalt Selenide toward Reversible Magnesium/Lithium Hybrid Batteries.","authors":"Wenlong Wang, Miao Tian, Zhitao Wang, Heping Ma, Yibo Du, Wenhui Si, Wenming Zhang, Hui Ying Yang, Song Chen","doi":"10.1021/acs.nanolett.4c04123","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c04123","url":null,"abstract":"<p><p>Metal chalcogenide-based cathodes are crucial for the development of rechargeable magnesium batteries, yet the strong electrostatic interactions of Mg<sup>2</sup><sup>+</sup> result in slow ion transport and high polarization. The Mg<sup>2</sup><sup>+</sup>/Li<sup>+</sup> hybrid battery holds promise for enhancing the energy storage capability. Herein, we establish a system that utilizes (Co,Cu)Se<sub>2</sub>/CoSe<sub><i>x</i></sub> heterostructure grown on carbon cloth as the cathode and APC-LiCl as a dual-salt electrolyte to achieve high reversible capacity, enhanced cyclic stability, and impressive rate performance. First-principles calculations and kinetic analyses are employed to uncover that constructing the heterointerface stimulates the formation of an intrinsic electric field and high-density electron flows, thereby accelerating charge transfer and ion diffusion processes. Finite element simulations further demonstrate that the heterostructure effectively alleviates stresses associated with magnesiation/lithiation to enhance the structural integrity of the material. Moreover, the multistep reaction unveils a stepwise structural transformation pathway. This study initiates a new chapter in designing heterointerface strategies for advanced energy storage devices.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666484","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Core-Sheath Heterogenous Interlocked Stretchable Conductive Fiber Induced by Adhesive MXene Modulated Interfacial Soldering. 粘合剂 MXene 调制界面焊接诱导的芯-鞘异质互锁可伸缩导电纤维
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.nanolett.4c04731
Zhichao Hou, Yifan He, Lijun Qu, Xueji Zhang, Tingting Fan, Jinlei Miao
{"title":"Core-Sheath Heterogenous Interlocked Stretchable Conductive Fiber Induced by Adhesive MXene Modulated Interfacial Soldering.","authors":"Zhichao Hou, Yifan He, Lijun Qu, Xueji Zhang, Tingting Fan, Jinlei Miao","doi":"10.1021/acs.nanolett.4c04731","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c04731","url":null,"abstract":"<p><p>Whereas high electrical conductivity and mechanical stretchability are both essentially required for flexible electronics, simultaneously achieving them remains a great challenge due to the \"trade-off\" effect. Herein, an ultrastretchable conductor with core-sheath heterogeneous interlocked structure was developed, induced by interfacial soldering silver nanowires (AgNWs) which gradually evolved into elastic conductive fiber. Adhesive polydopamine-functionalized MXene (PDM) was proposed as an interfacial solder to assemble AgNWs along fibers while induced strong cold-welding effect soldered them into superelastic interconnected network. <i>In situ</i> coaxial heterogeneous interlocking between core AgNWs and sheath PDM network gradually formed during the interfacial soldering process, which enables elastic conductor simultaneously owning large mechanical stretchability and high electrical conductivity. Stretchable conductive fiber with core-sheath heterogeneous interlocking structure not only exhibits excellent electrical conductivity (1.13 × 10<sup>5</sup> S/m) but also could maintain stability (Δ<i>R</i>/<i>R</i><sub>0</sub> < 0.19) even under large mechanical deformations (300%). Ultrastretchable fibrous conductor with core-sheath heterogeneous interlocked microstructure induced by adhesive PDM interfacial soldering holds great promise in soft electronics.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646501","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Landau-Level Quantization and Band Splitting of FeSe Monolayers Revealed by Scanning Tunneling Spectroscopy. 扫描隧道光谱法揭示的 FeSe 单层朗道级量子化和带分裂。
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.nanolett.4c04461
Wantong Huang, Haicheng Lin, Yuguo Yin, Cheng Zheng, Wei Chen, Lichen Ji, Jack Hughes, Fedor Kusmartsev, Anna Kusmartseva, Qi-Kun Xue, Xi Chen, Shuai-Hua Ji
{"title":"Landau-Level Quantization and Band Splitting of FeSe Monolayers Revealed by Scanning Tunneling Spectroscopy.","authors":"Wantong Huang, Haicheng Lin, Yuguo Yin, Cheng Zheng, Wei Chen, Lichen Ji, Jack Hughes, Fedor Kusmartsev, Anna Kusmartseva, Qi-Kun Xue, Xi Chen, Shuai-Hua Ji","doi":"10.1021/acs.nanolett.4c04461","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c04461","url":null,"abstract":"<p><p>Two-dimensional (2D) superconductors that reside on substrates must be influenced by Rashba spin-orbit coupling (SOC). The intriguing effect of Rashba-type SOCs on iron-based superconductors (IBSs) has remained largely a mystery. In this work, we unveil modified Landau-level spectroscopy and the intricate band splitting of FeSe monolayers through the precision of scanning tunneling spectroscopy, which unequivocally demonstrates the presence of Rashba SOC. The discovery sheds light on a nonparabolic electron band at the X and/orY point, displaying a distinctive Landau quantization behavior characterized by <i>E</i><sub><i>n</i></sub> ∝ (<i>nB</i>)<sup>4/3</sup>. The theoretical model aligns with our experimental insights, positing that the <i>k</i><sup>4</sup>-term of the electron band becomes predominant and profoundly reshapes the band structure. Our results underscore the pivotal role of the Rashba SOC effect on 2D superconductors and set the stage to probe new quantum states in systems with remarkably low carrier concentrations.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646505","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Controlled Separation of Skyrmions and Antiskyrmions by Kitaev Interaction. 通过基塔耶夫相互作用控制天离子和反天离子的分离。
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.nanolett.4c04194
Shuhua Guan, Wenhui Duan, Xiaolong Zou
{"title":"Controlled Separation of Skyrmions and Antiskyrmions by Kitaev Interaction.","authors":"Shuhua Guan, Wenhui Duan, Xiaolong Zou","doi":"10.1021/acs.nanolett.4c04194","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c04194","url":null,"abstract":"<p><p>As topological quasi-particles in magnetic materials, skyrmions and antiskyrmions show potential in spintronics for information storage and computing. However, effectively controlling and separating these entities remain significantly challenging. Here, we demonstrate that anisotropic Kitaev exchange can distinctly influence the static and dynamic behaviors for skyrmions and antiskyrmions, thus aiding their manipulation and separation. Employing the monolayer frustrated magnet NiBr<sub>2</sub> as a model system, we construct a magnetic field-strain phase diagram to explore the strain-controlled stability of these topological structures. The introduction of the Kitaev term breaks the energy degeneracy among magnetic structures with various helicities, leading to a translation-rotation mode transition with an increase in current. Importantly, due to their different rotational symmetries, the skyrmion and antiskyrmion show distinct critical behaviors and rotational dynamics, which are governed by the Kitaev parameters. These phenomena enable the design of two proof-of-concept spintronics devices, i.e., a skyrmion separator and a non-gate logic unit.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646499","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Nanocluster Colloidal Electrolyte Enables Highly Stable and Reversible Zinc Anodes. 纳米团簇胶体电解质实现了高度稳定和可逆的锌阳极。
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.nanolett.4c03201
Jiahui Peng, Huanhuan Sun, Mengyao Wen, Yuming Chen, Zhixuan Luo, Yu Huyan, Yumeng Xue, Jian-Gan Wang
{"title":"A Nanocluster Colloidal Electrolyte Enables Highly Stable and Reversible Zinc Anodes.","authors":"Jiahui Peng, Huanhuan Sun, Mengyao Wen, Yuming Chen, Zhixuan Luo, Yu Huyan, Yumeng Xue, Jian-Gan Wang","doi":"10.1021/acs.nanolett.4c03201","DOIUrl":"10.1021/acs.nanolett.4c03201","url":null,"abstract":"<p><p>Aqueous zinc-ion batteries represent a favorable technology for stationary energy storage systems owing to their safety, reliability, and cost-effectiveness. However, Zn anodes suffer uncontrollable dendrite formation and harmful side reactions that lead to a short lifespan. Herein, we demonstrate a nanocluster colloidal electrolyte strategy for stabilizing the zinc anodes. A copper nanocluster (CuNC) is screened out to validate the efficient suppression of messy dendrites and side reactions. A CuNC could resurface a zincophilic and protective interlayer for interfacially steering uniform Zn stripping/plating and mitigating corrosion/hydrogen evolution reactions. Impressively, the colloidal electrolyte enables zinc anodes to show a high Coulombic efficiency of 99.8% over 2100 cycles and extended lifespans of 2200 and 1300 h under 0.5 and 5 mA cm<sup>-2</sup>, respectively. A full cell based on the modified electrolyte exhibits significantly improved cycling durability for more than 15 000 cycles. This work will aid in the design of nanocluser colloidal electrolytes with respect to stable zinc chemistry and beyond.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646495","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Nitrogen-Doped Graphene-Supported Tungsten Oxynitride Nanoparticles as an Efficient Bidirectional Polysulfide Convertor for Advanced Lithium-Sulfur Batteries. 氮掺杂石墨烯支撑的氮氧化钨纳米粒子作为先进锂硫电池的高效双向多硫化物转换器。
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.nanolett.4c04791
Lulu Suo, Lei Feng, Juan Wang, Miaomiao Xing, Shuhua Lv, Hongyu Mou, Xing Gao, Deliang Zhang, Jibin Song
{"title":"Nitrogen-Doped Graphene-Supported Tungsten Oxynitride Nanoparticles as an Efficient Bidirectional Polysulfide Convertor for Advanced Lithium-Sulfur Batteries.","authors":"Lulu Suo, Lei Feng, Juan Wang, Miaomiao Xing, Shuhua Lv, Hongyu Mou, Xing Gao, Deliang Zhang, Jibin Song","doi":"10.1021/acs.nanolett.4c04791","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c04791","url":null,"abstract":"<p><p>Catalytic materials are considered pivotal in addressing the sluggish kinetics and shuttle effect in lithium-sulfur batteries (LSBs). However, effectively harnessing the utilization rate of active sites within catalytic materials remains a pivotal challenge. In this study, a novel conductive nitrogen-doped graphene-loaded tungsten oxynitride nanoparticle (WNO/NG) with abundant active sites is prepared through a polymer-assisted templating method for serving as a sulfur host. Electrochemical analysis coupled with <i>in situ</i> XRD confirm the dual-directional electrocatalytic behavior of WNO/NG for accelerating the conversion of lithium polysulfide (LiPSs). Theoretical calculations demonstrate that the intrinsic mechanism underlying the performance enhancement is attributed to the high inherent conductivity of WNO/NG and the efficient interface charge transfer with LiPSs. The assembled 500 mAh pouch cell delivers a 97% capacity retention after 25 cycles. This strategy provides valuable insights for designing catalytic materials with abundant activity sites and sheds light on the mechanisms of catalytic enhancement in Li-S chemistry.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666488","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Precise Control of Polyaniline Nanohelices with Chirality Continuum and Their Correlation on Catalytic Performance. 具有手性连续性的聚苯胺纳米螺旋的精确控制及其与催化性能的相关性。
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.nanolett.4c04816
Pengyuan Hang, Jiangbo Tong, Zheng Xi, Shixin Li, Shengyang Tao, Xiaohuan Sun, Jie Han
{"title":"Precise Control of Polyaniline Nanohelices with Chirality Continuum and Their Correlation on Catalytic Performance.","authors":"Pengyuan Hang, Jiangbo Tong, Zheng Xi, Shixin Li, Shengyang Tao, Xiaohuan Sun, Jie Han","doi":"10.1021/acs.nanolett.4c04816","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c04816","url":null,"abstract":"<p><p>Left- and right-handed chiral molecule inducers have been frequently used to guide the formation of chiral nanomaterials with binary chiral shapes. However, the transition of chiral nanomaterials from discrete to continuously tunable chiral shapes is imperative but challenging and will contribute to a deep understanding of the fundamental relations between chiral nanostructures and their chemical properties. This study shows that chiral polyaniline nanohelices (PANI NHs) with similar aspect ratios (∼5.0) but continuously tunable screw pitches (293 to ∞ nm) and tilt angles (33° to 0°) can be fabricated by adjusting the enantiomer excess of <i>S/R</i>-camphorsulfonic acid used as a chiral molecule inducer. After Au nanoparticles were loaded on the surface of chiral PANI NHs, the chiral morphology-dependent catalytic performances of PANI-Au NHs are studied in reduction, oxidation, and enantioselective catalytic reactions, showing that the larger the helical twist degree, the higher the catalytic activity and enantioselectivity of PANI-Au NHs.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646516","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Reconfiguring the Coordination Structure in Deep Eutectic Electrolytes for Enabling Stable Operation of Zinc-Ion Batteries. 重构深共晶电解质中的配位结构,实现锌-离子电池的稳定运行。
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.nanolett.4c03480
Qiang Guo, Weixing Mo, Jianhang Huang, Feng Liu
{"title":"Reconfiguring the Coordination Structure in Deep Eutectic Electrolytes for Enabling Stable Operation of Zinc-Ion Batteries.","authors":"Qiang Guo, Weixing Mo, Jianhang Huang, Feng Liu","doi":"10.1021/acs.nanolett.4c03480","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c03480","url":null,"abstract":"<p><p>Highly stable aqueous Zn-ion batteries are of great importance for commercial applications. The challenging issues of interfacial side reactions and rampant dendrite growth cause short circuit and premature failure of aqueous Zn-ion batteries. Herein, a hydrated deep eutectic electrolyte is formulated to tackle such problems, which adopts 1,3-propanediol as a cosolvent. 1,3-Propanediol molecules can enter into the Zn<sup>2+</sup> solvation structure to from a lean-water electrolyte and drastically diminish the activity of water molecules through reinforcing the hydrogen bond network. Meanwhile, PDO molecules exclude the neighboring water to modulate the electric double layer configuration, thus impeding water-mediated side reactions and inducing an inorganic-rich interphase. Consequently, this hydrated deep eutectic electrolyte ensures long-term stability of Zn-Zn, Zn-Cu, and Zn-I<sub>2</sub> cells. The favorable influence exerted by PDO molecules provides the guidance for constructing high-performance aqueous Zn-ion batteries.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646517","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Strong and Stable Woody Triboelectric Materials Enabled by Biphase Blocking. 通过双相阻断技术实现强而稳定的木质三电材料。
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.nanolett.4c02802
Cong Gao, Jiamin Zhao, Tao Liu, Bin Luo, Mingchao Chi, Song Zhang, Chenchen Cai, Jinlong Wang, Yanhua Liu, Yuzheng Shao, Guoli Du, Chengrong Qin, Shuangxi Nie
{"title":"Strong and Stable Woody Triboelectric Materials Enabled by Biphase Blocking.","authors":"Cong Gao, Jiamin Zhao, Tao Liu, Bin Luo, Mingchao Chi, Song Zhang, Chenchen Cai, Jinlong Wang, Yanhua Liu, Yuzheng Shao, Guoli Du, Chengrong Qin, Shuangxi Nie","doi":"10.1021/acs.nanolett.4c02802","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c02802","url":null,"abstract":"<p><p>Driven by the \"Internet of Everything\" (IoE) vision, the demand for smart materials is growing. Wood, one of the most abundant and renewable resources, has long been a staple in construction and furnishing applications. To further expand its application range, this study developed a high-strength, stable wood-based triboelectric material through a synergistic biphasic mechanism. The in situ growth of flame retardants and the formation of a dense char layer significantly enhanced the fire resistance of the wood-based triboelectric material, reducing the heat release rate (HRR) by 95.4% and total heat release (THR) by 94.2%. The dense laminate structure provided an excellent impact toughness (126 kJ m<sup>-2</sup>). As a smart sensor, the wood-based triboelectric material demonstrated the ability to recognize human motion states and trajectories, exhibiting great potential for applications in smart homes. This study provides valuable insights for exploring the potential applications of wood as a smart material.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646518","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Exciton Enhanced Nonlinear Optical Responses in Monolayer h-BN and MoS2: Insight from First-Principles Exciton-State Coupling Formalism and Calculations. 单层 h-BN 和 MoS2 中的激子增强非线性光学响应:第一原理激子态耦合形式和计算的启示。
IF 9.6 1区 材料科学
Nano Letters Pub Date : 2024-11-18 DOI: 10.1021/acs.nanolett.4c03434
Jiawei Ruan, Yang-Hao Chan, Steven G Louie
{"title":"Exciton Enhanced Nonlinear Optical Responses in Monolayer h-BN and MoS<sub>2</sub>: Insight from First-Principles Exciton-State Coupling Formalism and Calculations.","authors":"Jiawei Ruan, Yang-Hao Chan, Steven G Louie","doi":"10.1021/acs.nanolett.4c03434","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c03434","url":null,"abstract":"<p><p>Excitons are vital in the photophysics of materials, especially in low-dimensional systems. The conceptual and quantitative understanding of excitonic effects in nonlinear optical (NLO) processes is more challenging compared to linear ones. Here, we present an ab initio approach to second-order NLO responses, incorporating excitonic effects, that employs an exciton-state coupling formalism and allows for a detailed analysis of the role of individual excitonic states. Taking monolayer h-BN and MoS<sub>2</sub> as two prototype 2D materials, we calculate their second harmonic generation (SHG) susceptibility and shift current conductivity tensor. We find strong excitonic enhancement in the NLO responses requires that the resonant excitons are not only optically bright themselves but also able to couple strongly to other bright excitons. Our results explain the occurrence of two strong peaks in the SHG of monolayer h-BN and why the A and B excitons of MoS<sub>2</sub> unexpectedly exhibit minimal excitonic enhancement in both SHG and shift current generation.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":" ","pages":""},"PeriodicalIF":9.6,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666486","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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