Pub Date : 2026-03-24DOI: 10.1021/acs.jpclett.6c00645
Juan Zhan,Wei Lin
Here, we employed ab initio nonadiabatic molecular dynamics simulations to investigate the carrier dynamics in methylammonium lead iodide (MAPbI3) perovskites with lead vacancies under tensile strain. Our results reveal that moderate strain effectively suppresses nonradiative recombination and extends carrier lifetimes, while excessive strain accelerates carrier recombination due to the formation of deeper trap states, negatively affecting device performance. Significant tensile strain induces the formation of I-I dimers, leading to severe local lattice distortion characterized by the elongation of Pb-I bonds and the shortening of I-I bonds at the lead vacancy sites. Furthermore, the bandgap increases with tensile strain, attributed to the stronger antibonding character in the valence band compared to the conduction band. This work provides valuable insights into defect-mediated carrier relaxation dynamics and offers theoretical guidance for defect engineering in perovskite solar cells and related devices.
{"title":"Nonmonotonic Strain Dependence of Defect-Assisted Nonradiative Recombination in MAPbI3 Revealed by Nonadiabatic Dynamics.","authors":"Juan Zhan,Wei Lin","doi":"10.1021/acs.jpclett.6c00645","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00645","url":null,"abstract":"Here, we employed ab initio nonadiabatic molecular dynamics simulations to investigate the carrier dynamics in methylammonium lead iodide (MAPbI3) perovskites with lead vacancies under tensile strain. Our results reveal that moderate strain effectively suppresses nonradiative recombination and extends carrier lifetimes, while excessive strain accelerates carrier recombination due to the formation of deeper trap states, negatively affecting device performance. Significant tensile strain induces the formation of I-I dimers, leading to severe local lattice distortion characterized by the elongation of Pb-I bonds and the shortening of I-I bonds at the lead vacancy sites. Furthermore, the bandgap increases with tensile strain, attributed to the stronger antibonding character in the valence band compared to the conduction band. This work provides valuable insights into defect-mediated carrier relaxation dynamics and offers theoretical guidance for defect engineering in perovskite solar cells and related devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-24DOI: 10.1021/acs.jpclett.6c00444
Yuqi Wu,Xiaodan Yan,Ting Meng,Jinlu He
Experimental studies have demonstrated that doping magnetic ions into halide perovskites offers a promising route to tailor electron spin dynamics and suppress nonradiative charge recombination, yet the underlying atomistic mechanism remains elusive. Using nonadiabatic molecular dynamics simulations, we demonstrate that Mn doping in CsPbBr3 enhances spin polarization without introducing midgap trap states compared to the pristine system. This spin polarization reduces nonadiabatic coupling between band-edge states while activating additional spin-orbit coupling (SOC)-mediated spin-flip channels within CBM↑/CBM↓ and VBM↑/VBM↓. These channels enable dynamic charge redistribution among spin-resolved orbitals, thereby prolonging carrier lifetimes. Our study reveals how band-edge SOC governs charge recombination and spin relaxation dynamics in halide perovskites, providing design principles for high-performance optoelectronic devices.
{"title":"Tuning Band-Edge Spin-Orbit Coupling to Prolong Carrier Lifetime in CsPbBr3 Perovskites.","authors":"Yuqi Wu,Xiaodan Yan,Ting Meng,Jinlu He","doi":"10.1021/acs.jpclett.6c00444","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00444","url":null,"abstract":"Experimental studies have demonstrated that doping magnetic ions into halide perovskites offers a promising route to tailor electron spin dynamics and suppress nonradiative charge recombination, yet the underlying atomistic mechanism remains elusive. Using nonadiabatic molecular dynamics simulations, we demonstrate that Mn doping in CsPbBr3 enhances spin polarization without introducing midgap trap states compared to the pristine system. This spin polarization reduces nonadiabatic coupling between band-edge states while activating additional spin-orbit coupling (SOC)-mediated spin-flip channels within CBM↑/CBM↓ and VBM↑/VBM↓. These channels enable dynamic charge redistribution among spin-resolved orbitals, thereby prolonging carrier lifetimes. Our study reveals how band-edge SOC governs charge recombination and spin relaxation dynamics in halide perovskites, providing design principles for high-performance optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"270 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502185","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hydrated imidazolium hemimelitate with helical hydrogen bonding network is the first amphidynamic organic crystal observed in a group of imidazolium and carboxylic acid compounds. The sublattice of acid ions forms a static network, while the dynamic part comprises imidazole ions and water molecules. A transition from positional to orientational disorder of water molecules is observed as the temperature closes to room temperature and the spatial arrangement of cations leads to an order–disorder phase transition at a temperature of 150 K, which we analyzed in a wide spectral range using THz, FIR, MIR, and Raman spectroscopies. Furthermore, DFT calculations were employed to understand the molecular dynamics and the phase transition mechanism of the studied compound. The temperature-dependent spectra also revealed proton–phonon coupling to occur below 100 K. Our findings provide valuable information, such as temperature behavior of hydrogen bonds, anharmonicity, and coupling effects for the targeted design of amphidynamic materials.
{"title":"Amphidynamic Molecular Crystal with Temperature-Controlled Helical Hydrogen-Bonded Network: Proton Dynamics and Order–Disorder Phase Transition","authors":"Sylwia Zięba,Christelle Kadlec,Savita Priya,Yayi Lin,Adam Mizera,Martin Dressel,Petr Kužel","doi":"10.1021/acs.jpclett.6c00289","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00289","url":null,"abstract":"Hydrated imidazolium hemimelitate with helical hydrogen bonding network is the first amphidynamic organic crystal observed in a group of imidazolium and carboxylic acid compounds. The sublattice of acid ions forms a static network, while the dynamic part comprises imidazole ions and water molecules. A transition from positional to orientational disorder of water molecules is observed as the temperature closes to room temperature and the spatial arrangement of cations leads to an order–disorder phase transition at a temperature of 150 K, which we analyzed in a wide spectral range using THz, FIR, MIR, and Raman spectroscopies. Furthermore, DFT calculations were employed to understand the molecular dynamics and the phase transition mechanism of the studied compound. The temperature-dependent spectra also revealed proton–phonon coupling to occur below 100 K. Our findings provide valuable information, such as temperature behavior of hydrogen bonds, anharmonicity, and coupling effects for the targeted design of amphidynamic materials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"20 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147506439","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-24DOI: 10.1021/acs.jpclett.6c00197
Surajit Metya,Daniel González,Iakov A. Medvedkov,Mateus X. Silva,Breno R. L. Galvão,Ralf I. Kaiser
Substituting silicon for carbon in reactive molecular frameworks profoundly influences bonding characteristics, electronic structure, and reaction pathways, making silicon-containing systems a topic of sustained interest in fundamental and applied chemistry. Elucidating how silicon incorporation modulates elementary reaction dynamics is essential for establishing predictive principles relevant to organosilicon synthesis, materials chemistry, and heterocycle design. In this context, the reaction of the silicon nitride radical (SiN) with propene (C3H6) serves as an ideal model system to probe these effects. Previous studies have shown that reactions of SiN with two-carbon unsaturated hydrocarbons such as ethylene (C2H4) and acetylene (C2H2) predominantly yield acyclic silaisonitrile derivatives, whereas reactions with four-carbon systems, exemplified by 1,3-butadiene (C4H6), favor the formation of cyclic products. As a three-carbon unsaturated hydrocarbon, propene (C3H6) occupies a critical borderline position, offering a unique opportunity to determine whether silicon nitride reactivity preferentially promotes cyclic or acyclic product formation in this borderline case. Crossed molecular beam experiments, combined with high-level electronic structure calculations and Rice–Ramsperger–Kassel–Marcus (RRKM) statistical analysis, reveal that the reaction proceeds via indirect dynamics involving long-lived intermediates and tight exit transition states. Although the potential energy surface features multiple competing pathways, reaction energetics, and barrier heights strongly favor the formation of acyclic products, while cyclic Si–N heterocycles emerge only as minor channels. Together, these results provide fundamental insight into how main-group substitution governs reaction selectivity and pathway control, establishing general principles for silicon-centered reaction dynamics and expanding the conceptual framework of silicon–nitrogen chemistry.
在反应性分子框架中用硅代替碳会深刻地影响成键特性、电子结构和反应途径，使含硅体系成为基础化学和应用化学领域持续关注的话题。阐明硅掺入如何调节基本反应动力学对于建立与有机硅合成、材料化学和杂环设计相关的预测原理至关重要。在这种情况下，氮化硅自由基（SiN）与丙烯（C3H6）的反应可以作为探测这些效应的理想模型体系。先前的研究表明，SiN与乙烯（C2H4）和乙炔（C2H2）等二碳不饱和烃反应，主要生成无环硅腈衍生物，而与四碳体系反应，如1,3-丁二烯（C4H6），有利于形成环产物。作为一种三碳不饱和烃，丙烯（C3H6）占据了一个临界的边界位置，这就提供了一个独特的机会来确定在这个边界情况下，氮化硅的反应性是优先促进环产物还是非环产物的形成。交叉分子束实验，结合高能级电子结构计算和rice - ramspberger - kassel - marcus （RRKM）统计分析，揭示了反应是通过间接动力学进行的，涉及长寿命中间体和紧密的出口过渡态。虽然势能表面具有多种竞争途径，但反应能量和势垒高度强烈地有利于非环产物的形成，而环Si-N杂环仅作为次要通道出现。总之，这些结果为主基团取代如何控制反应选择性和途径控制提供了基本的见解，建立了以硅为中心的反应动力学的一般原理，并扩展了硅氮化学的概念框架。
{"title":"Can a Three-Carbon Olefin Close a Five-Membered Ring on Reaction with the Silicon Nitride Radical (SiN, X2Σ+)? A Crossed Molecular Beams and Ab Initio Study","authors":"Surajit Metya,Daniel González,Iakov A. Medvedkov,Mateus X. Silva,Breno R. L. Galvão,Ralf I. Kaiser","doi":"10.1021/acs.jpclett.6c00197","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00197","url":null,"abstract":"Substituting silicon for carbon in reactive molecular frameworks profoundly influences bonding characteristics, electronic structure, and reaction pathways, making silicon-containing systems a topic of sustained interest in fundamental and applied chemistry. Elucidating how silicon incorporation modulates elementary reaction dynamics is essential for establishing predictive principles relevant to organosilicon synthesis, materials chemistry, and heterocycle design. In this context, the reaction of the silicon nitride radical (SiN) with propene (C3H6) serves as an ideal model system to probe these effects. Previous studies have shown that reactions of SiN with two-carbon unsaturated hydrocarbons such as ethylene (C2H4) and acetylene (C2H2) predominantly yield acyclic silaisonitrile derivatives, whereas reactions with four-carbon systems, exemplified by 1,3-butadiene (C4H6), favor the formation of cyclic products. As a three-carbon unsaturated hydrocarbon, propene (C3H6) occupies a critical borderline position, offering a unique opportunity to determine whether silicon nitride reactivity preferentially promotes cyclic or acyclic product formation in this borderline case. Crossed molecular beam experiments, combined with high-level electronic structure calculations and Rice–Ramsperger–Kassel–Marcus (RRKM) statistical analysis, reveal that the reaction proceeds via indirect dynamics involving long-lived intermediates and tight exit transition states. Although the potential energy surface features multiple competing pathways, reaction energetics, and barrier heights strongly favor the formation of acyclic products, while cyclic Si–N heterocycles emerge only as minor channels. Together, these results provide fundamental insight into how main-group substitution governs reaction selectivity and pathway control, establishing general principles for silicon-centered reaction dynamics and expanding the conceptual framework of silicon–nitrogen chemistry.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"83 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147506440","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-24DOI: 10.1021/acs.jpclett.6c00519
S Swaminathan, J Berger, M K Mahato, T W Ebbesen, G Jung
Proton transfer reactions are ubiquitous in chemistry and biology. Here we explore the consequences of vibrational strong coupling (VSC) on excited state proton transfer in solution. The rates of proton transfer, as well as the internal dynamics and quantum yields, are significantly modified when the solvent and the photoacid are coupled cooperatively. These findings confirm that VSC can act on excited state reactivity and not just on ground state processes reported so far.
{"title":"Excited-State Proton Transfer in Solution under Vibrational Strong Coupling.","authors":"S Swaminathan, J Berger, M K Mahato, T W Ebbesen, G Jung","doi":"10.1021/acs.jpclett.6c00519","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00519","url":null,"abstract":"<p><p>Proton transfer reactions are ubiquitous in chemistry and biology. Here we explore the consequences of vibrational strong coupling (VSC) on excited state proton transfer in solution. The rates of proton transfer, as well as the internal dynamics and quantum yields, are significantly modified when the solvent and the photoacid are coupled cooperatively. These findings confirm that VSC can act on excited state reactivity and not just on ground state processes reported so far.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502563","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-23DOI: 10.1021/acs.jpclett.6c00555
Ahmad Ostovari Moghaddam,Seyedsaeed Mehrabi-Kalajahi,Seyed Amir Hossein Vasigh,Hassan Yousefi Bavili,Behrouz Shaabani,Xue Bai,Wei Qin,Alexei Vagov,Andrey S Vasenko,Fu-Quan Bai,Mikhail A Varfolomeev
Water electrolysis is a key technology for sustainable energy conversion and hydrogen generation. Recently, high-entropy oxides (HEOs) have emerged as promising materials because they allow tuning of structural, electronic, and catalytic properties in multifunctional systems. Here, we report the synthesis of a multicomponent La(FeCoCuTiNiMnMgSnZn)O3 perovskite, and its hybridization with reduced graphene oxide (rGO) to form a robust La(FeCoCuTiNiMnMgSnZn)O3-rGO nanocomposite. Structural characterization confirms the formation of a single-phase cubic perovskite structure with a uniform cation distribution and a slight lattice expansion compared with LaTiO3. In addition, HEO nanoparticles are homogeneously dispersed on the rGO sheets. High-resolution XPS analysis also reveals a defect-rich surface with mixed metal valence states, which interact with the conductive carbon network. Electrochemical measurements show that the La(FeCoCuTiNiMnMgSnZn)O3-rGO nanocomposite exhibits superior oxygen evolution reaction (OER) activity. It reaches a current density of 30 mA cm-2 at a lower overpotential and shows a Tafel slope of 81.9 mV dec-1. The catalyst also demonstrates good stability during 8 h of continuous operation. The enhanced performance is attributed to the combined effect of multiple metal elements in the high-entropy lattice, improved charge transport through the rGO network, and the presence of many active sites created by surface defects. These results show that combining HEOs with conductive carbon materials is a useful strategy for developing efficient and durable electrocatalysts for the OER.
水电解是可持续能源转化和制氢的关键技术。最近，高熵氧化物（HEOs）作为一种很有前途的材料出现，因为它们允许在多功能系统中调整结构、电子和催化性能。在这里，我们报道了一种多组分La(FeCoCuTiNiMnMgSnZn)O3钙钛矿的合成，并将其与还原氧化石墨烯（rGO）杂化，形成了一种坚固的La(FeCoCuTiNiMnMgSnZn)O3-rGO纳米复合材料。结构表征证实形成了一种阳离子分布均匀的单相立方钙钛矿结构，与LaTiO3相比有轻微的晶格膨胀。此外，HEO纳米颗粒均匀地分散在氧化石墨烯薄片上。高分辨率XPS分析还揭示了具有混合金属价态的富含缺陷的表面，这些缺陷与导电碳网络相互作用。电化学测试表明，La(FeCoCuTiNiMnMgSnZn)O3-rGO纳米复合材料具有优异的析氧反应（OER）活性。在较低的过电位下，电流密度达到30 mA cm-2，塔非尔斜率为81.9 mV / dec1。催化剂在连续运行8 h时也表现出良好的稳定性。这种性能的增强是由于高熵晶格中多种金属元素的综合作用，通过还原氧化石墨烯网络的电荷传输的改善，以及表面缺陷产生的许多活性位点的存在。这些结果表明，将氢氧根与导电碳材料结合是开发高效、耐用的OER电催化剂的有效策略。
{"title":"Synergistic Multimetal Effects in a High-Entropy Perovskite Oxide Anchored on Reduced Graphene Oxide for Accelerated Water Oxidation.","authors":"Ahmad Ostovari Moghaddam,Seyedsaeed Mehrabi-Kalajahi,Seyed Amir Hossein Vasigh,Hassan Yousefi Bavili,Behrouz Shaabani,Xue Bai,Wei Qin,Alexei Vagov,Andrey S Vasenko,Fu-Quan Bai,Mikhail A Varfolomeev","doi":"10.1021/acs.jpclett.6c00555","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00555","url":null,"abstract":"Water electrolysis is a key technology for sustainable energy conversion and hydrogen generation. Recently, high-entropy oxides (HEOs) have emerged as promising materials because they allow tuning of structural, electronic, and catalytic properties in multifunctional systems. Here, we report the synthesis of a multicomponent La(FeCoCuTiNiMnMgSnZn)O3 perovskite, and its hybridization with reduced graphene oxide (rGO) to form a robust La(FeCoCuTiNiMnMgSnZn)O3-rGO nanocomposite. Structural characterization confirms the formation of a single-phase cubic perovskite structure with a uniform cation distribution and a slight lattice expansion compared with LaTiO3. In addition, HEO nanoparticles are homogeneously dispersed on the rGO sheets. High-resolution XPS analysis also reveals a defect-rich surface with mixed metal valence states, which interact with the conductive carbon network. Electrochemical measurements show that the La(FeCoCuTiNiMnMgSnZn)O3-rGO nanocomposite exhibits superior oxygen evolution reaction (OER) activity. It reaches a current density of 30 mA cm-2 at a lower overpotential and shows a Tafel slope of 81.9 mV dec-1. The catalyst also demonstrates good stability during 8 h of continuous operation. The enhanced performance is attributed to the combined effect of multiple metal elements in the high-entropy lattice, improved charge transport through the rGO network, and the presence of many active sites created by surface defects. These results show that combining HEOs with conductive carbon materials is a useful strategy for developing efficient and durable electrocatalysts for the OER.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147495051","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-23DOI: 10.1021/acs.jpclett.6c00372
Jiaren Huang,Xiaodong Shen,Yongqiang Zhao,Weixing Chen,Tao Huang,Bingsuo Zou
In this work, BaCl2:Eu2+,S2- is employed as model system to investigate the formation and tunable evolution of localized excitonic magnetic polarons (LEMPs) in Eu-S codoped divalent metal halides, in which Eu-S bonding in BaCl2 with Eu2+ 5d-f hybridization markedly enhances the band edge emission, shifting from 401 to 412 nm with rising EuS content, and the absorption band edge shifts from 3.02 to 2.85 eV, with EMP character. Moreover, EuS doped in different hosts (Ba < Sr < Ca) leads to a progressive red shift of EMP emission from 406 nm to the near-infrared region. Under high-energy laser excitation, these compounds can exhibit pronounced nonlinear emission with ASE-like behavior (n > 1), demonstrating the LEMP-cooperative radiative processes. This study establishes rare-earth-sulfur codoped halides as a promising materials platform for tuning luminescence through coupled spin-lattice-exciton interactions.
{"title":"Localized Excitonic Magnetic Polarons and Their Role in the Luminescence of Rare-Earth-Sulfur Codoped Divalent Metal Halides.","authors":"Jiaren Huang,Xiaodong Shen,Yongqiang Zhao,Weixing Chen,Tao Huang,Bingsuo Zou","doi":"10.1021/acs.jpclett.6c00372","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00372","url":null,"abstract":"In this work, BaCl2:Eu2+,S2- is employed as model system to investigate the formation and tunable evolution of localized excitonic magnetic polarons (LEMPs) in Eu-S codoped divalent metal halides, in which Eu-S bonding in BaCl2 with Eu2+ 5d-f hybridization markedly enhances the band edge emission, shifting from 401 to 412 nm with rising EuS content, and the absorption band edge shifts from 3.02 to 2.85 eV, with EMP character. Moreover, EuS doped in different hosts (Ba < Sr < Ca) leads to a progressive red shift of EMP emission from 406 nm to the near-infrared region. Under high-energy laser excitation, these compounds can exhibit pronounced nonlinear emission with ASE-like behavior (n > 1), demonstrating the LEMP-cooperative radiative processes. This study establishes rare-earth-sulfur codoped halides as a promising materials platform for tuning luminescence through coupled spin-lattice-exciton interactions.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"31 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502189","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-23DOI: 10.1021/acs.jpclett.6c00411
Yongjie Fan,RuiYa Xu,Wen Yang,Hongwei Xia,Yufang Liu
The image data obtained from solid-state, two-dimensional (2D) broadband photodetectors enable enhanced object identification owing to the wide range of information residing beyond human vision capabilities. However, the widespread use of these photodetector devices is limited by narrow photoresponse ranges and low response speeds. The obtained 2D InSbSe3 photodetector devices exhibit comprehensively excellent optoelectronic properties with a high on/off ratio of 105, a high photoresponsivity of 5.14 A/W, and an ultrashort photoresponse time of 6 ms under laser illumination at a wavelength of 520 nm with an applied bias voltage of 0.2 V. These metrics represent a greater performance than those obtained by most previously reported photodetector devices composed of other 2D ternary materials. Furthermore, the InSbSe3-based photodetector devices demonstrate a favorable broadband photoresponse, with good performance obtained at wavelengths ranging from ultraviolet (265 nm) to near-infrared (940 nm). Finally, the developed photodetector devices facilitated optical imaging conducted at wavelengths of 375, 520, and 785 nm. Accordingly, the proposed 2D InSbSe3 nanosheet materials exhibit a substantial potential for the development of low-power, high-sensitivity multispectral imaging systems useful in a wide range of applications such as machine vision, environmental monitoring, and medical diagnosis.
从固态、二维（2D）宽带光电探测器获得的图像数据，由于人类视觉能力之外的广泛信息，能够增强物体识别。然而，这些光电探测器器件的广泛使用受到光响应范围窄和响应速度低的限制。所制得的二维InSbSe3光电探测器器件在520 nm波长、0.2 V偏置电压的激光照射下，具有105的高开/关比、5.14 a /W的高光响应率和6 ms的超短光响应时间等综合优异的光电性能。这些指标比以前报道的大多数由其他二维三元材料组成的光电探测器器件获得的性能更好。此外，基于insbse3的光电探测器器件表现出良好的宽带光响应，在紫外（265 nm）到近红外（940 nm）波长范围内都有良好的性能。最后，所开发的光电探测器装置有助于在375、520和785 nm波长下进行光学成像。因此，所提出的二维InSbSe3纳米片材料在开发低功耗、高灵敏度多光谱成像系统方面具有巨大潜力，可用于机器视觉、环境监测和医疗诊断等广泛应用。
{"title":"Atomically Thin InSbSe3 Layers for Multispectral Optical Imaging with Fast Photoresponse and Broadband Photodetection.","authors":"Yongjie Fan,RuiYa Xu,Wen Yang,Hongwei Xia,Yufang Liu","doi":"10.1021/acs.jpclett.6c00411","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00411","url":null,"abstract":"The image data obtained from solid-state, two-dimensional (2D) broadband photodetectors enable enhanced object identification owing to the wide range of information residing beyond human vision capabilities. However, the widespread use of these photodetector devices is limited by narrow photoresponse ranges and low response speeds. The obtained 2D InSbSe3 photodetector devices exhibit comprehensively excellent optoelectronic properties with a high on/off ratio of 105, a high photoresponsivity of 5.14 A/W, and an ultrashort photoresponse time of 6 ms under laser illumination at a wavelength of 520 nm with an applied bias voltage of 0.2 V. These metrics represent a greater performance than those obtained by most previously reported photodetector devices composed of other 2D ternary materials. Furthermore, the InSbSe3-based photodetector devices demonstrate a favorable broadband photoresponse, with good performance obtained at wavelengths ranging from ultraviolet (265 nm) to near-infrared (940 nm). Finally, the developed photodetector devices facilitated optical imaging conducted at wavelengths of 375, 520, and 785 nm. Accordingly, the proposed 2D InSbSe3 nanosheet materials exhibit a substantial potential for the development of low-power, high-sensitivity multispectral imaging systems useful in a wide range of applications such as machine vision, environmental monitoring, and medical diagnosis.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"7 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147495053","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-23DOI: 10.1021/acs.jpclett.6c00524
Mohamed Sabba, Christian Bengs, Urvashi D Heramun, Malcolm H Levitt
A modification of the widely used spin-lock-induced crossing (SLIC) procedure is proposed for the solution nuclear magnetic resonance (NMR) of strongly coupled nuclear spin systems, including singlet NMR and parahydrogen-enhanced hyperpolarized NMR experiments. The compensated-SLIC (cSLIC) scheme uses a repetitive sequence where the repeated element employs two different radio-frequency field amplitudes. Effective compensation for deviations in the radio-frequency field amplitude is achieved without increasing the overall duration of the SLIC sequence. The advantageous properties of cSLIC are demonstrated by numerical simulations and representative experiments.
{"title":"Error Compensation without a Time Penalty: Robust Spin-Lock-Induced Crossing in Solution NMR.","authors":"Mohamed Sabba, Christian Bengs, Urvashi D Heramun, Malcolm H Levitt","doi":"10.1021/acs.jpclett.6c00524","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00524","url":null,"abstract":"<p><p>A modification of the widely used spin-lock-induced crossing (SLIC) procedure is proposed for the solution nuclear magnetic resonance (NMR) of strongly coupled nuclear spin systems, including singlet NMR and parahydrogen-enhanced hyperpolarized NMR experiments. The compensated-SLIC (cSLIC) scheme uses a repetitive sequence where the repeated element employs two different radio-frequency field amplitudes. Effective compensation for deviations in the radio-frequency field amplitude is achieved without increasing the overall duration of the SLIC sequence. The advantageous properties of cSLIC are demonstrated by numerical simulations and representative experiments.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":""},"PeriodicalIF":4.6,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502595","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-23DOI: 10.1021/acs.jpclett.6c00410
Ulrich Leo,Maximilian A Gruber,Nina A Henke,Veronika Reisner,Sirri B Kalkan,Michael F Lichtenegger,Bert Nickel,Alexander S Urban
Lead halide perovskite nanocrystals (PNCs) exhibit outstanding optical and electronic properties for next-generation optoelectronics; however, their instability under ambient conditions severely hinders their practical implementation. Here, we demonstrate a versatile ligand cross-linking approach via electron-beam irradiation that effectively enhances nanocrystal stability without compromising their exceptional optical properties. Electron-beam exposure induces cross-linking reactions within the native oleylamine and oleic acid ligand shell, forming a robust, interconnected organic network that substantially increases hydrophobicity, long-term ambient stability, and resistance to various solvents. Unlike polymer or micelle encapsulation strategies, our cross-linking method preserves the structural integrity of the PNC layer and its optical properties without introducing additional layers or barriers that could impede charge transport. We further exploit this technique to create unprecedented heterostructures, achieving dual-emission spectra without ion exchange. Additionally, we present a novel method for producing mechanically stable, freestanding PNC films, which significantly simplifies device fabrication. These findings open up new avenues for integrating highly stable perovskite nanocrystal layers into commercial-scale photovoltaic and optoelectronic devices.
{"title":"Electron-Beam Cross-Linked Ligands Enable Highly Stable and Freestanding Perovskite Nanocrystal Films.","authors":"Ulrich Leo,Maximilian A Gruber,Nina A Henke,Veronika Reisner,Sirri B Kalkan,Michael F Lichtenegger,Bert Nickel,Alexander S Urban","doi":"10.1021/acs.jpclett.6c00410","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00410","url":null,"abstract":"Lead halide perovskite nanocrystals (PNCs) exhibit outstanding optical and electronic properties for next-generation optoelectronics; however, their instability under ambient conditions severely hinders their practical implementation. Here, we demonstrate a versatile ligand cross-linking approach via electron-beam irradiation that effectively enhances nanocrystal stability without compromising their exceptional optical properties. Electron-beam exposure induces cross-linking reactions within the native oleylamine and oleic acid ligand shell, forming a robust, interconnected organic network that substantially increases hydrophobicity, long-term ambient stability, and resistance to various solvents. Unlike polymer or micelle encapsulation strategies, our cross-linking method preserves the structural integrity of the PNC layer and its optical properties without introducing additional layers or barriers that could impede charge transport. We further exploit this technique to create unprecedented heterostructures, achieving dual-emission spectra without ion exchange. Additionally, we present a novel method for producing mechanically stable, freestanding PNC films, which significantly simplifies device fabrication. These findings open up new avenues for integrating highly stable perovskite nanocrystal layers into commercial-scale photovoltaic and optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"118 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147495052","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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