The Journal of Physical Chemistry Letters最新文献_第9页

Controlling Structural Dimensionality in 2D Perovskites through A-Site Cation Enrichment 通过a位阳离子富集控制二维钙钛矿的结构维度

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-12 DOI: 10.1021/acs.jpclett.6c02668

Zhongqi Xie,Pingyuan Yan,Hou Wang,Heng Li,Qing-Song Jiang,Xiao Yang,Chuanxiang Sheng

{"title":"Controlling Structural Dimensionality in 2D Perovskites through A-Site Cation Enrichment","authors":"Zhongqi Xie,Pingyuan Yan,Hou Wang,Heng Li,Qing-Song Jiang,Xiao Yang,Chuanxiang Sheng","doi":"10.1021/acs.jpclett.6c02668","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02668","url":null,"abstract":"Two-dimensional (2D) Ruddlesden–Popper (RP) lead halide perovskites exhibit tunable structures, compositions, and optoelectronic properties, yet achieving precise control over their structural dimensionality in solution-processed thin films remains a significant challenge. Here, we report a simple strategy to regulate the dimensionality of 2D RP perovskites by enriching the A-site cations (FA+/Cs+) in the precursor solution, where FA = formamidinium. Based on a nominal n = 3 composition, systematic increase of the A-site cation ratio yields films with the general formula (4FPEA)2(FA0.3xCs0.7x)2Pb3X8+2x (X = I, Br; x = 1.5–3.0), where 4FPEA = 4-fluorophenylethylammonium. Within an optimal range, excess A-site cations promote the progressive formation of smaller-n phases without compromising film quality or triggering bulk three-dimensional (3D) perovskite formation. This tuning the n-value distribution effect is evidenced by UV–vis absorption, X-ray diffraction (XRD), steady-state photoluminescence (PL), and femtosecond transient absorption spectroscopy (TAS). As the A-site enrichment increases, the dominant phases shift from mixed high-n (quasi-3D) toward lower-n phases and energy funneling to large-n phases is suppressed, resulting in a continuous blue shift of the PL emission─from red to green for iodide-based perovskites and from green to blue for bromide-based analogues. This A-site stoichiometry engineering approach provides a straightforward, scalable route for tailoring the structural dimensionality and emission color of 2D perovskites via solution processing, with potential applications in light-emitting diodes and other optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"43 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152175","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}

引用次数: 0

Electrochemical State Reconfiguration in Vertical Opto-ionic Transistors for Adaptive Optoelectronic Computing 用于自适应光电计算的垂直光离子晶体管的电化学状态重构

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-12 DOI: 10.1021/acs.jpclett.6c02980

Xiaolong Li,Yang Liu,Xinmu Chen,Zihong Yang,Yujie Yang,Yali Yu,Jiayang Jiang,Yu Zhang,Yufeng Hu,Feng Teng

{"title":"Electrochemical State Reconfiguration in Vertical Opto-ionic Transistors for Adaptive Optoelectronic Computing","authors":"Xiaolong Li,Yang Liu,Xinmu Chen,Zihong Yang,Yujie Yang,Yali Yu,Jiayang Jiang,Yu Zhang,Yufeng Hu,Feng Teng","doi":"10.1021/acs.jpclett.6c02980","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02980","url":null,"abstract":"The ability to dynamically reconfigure a single device between sensing and computing functions could fundamentally simplify in-sensor vision architectures, yet achieving electrically programmable transitions between volatile photodetection and persistent synaptic processing remains challenging. Here, we establish an electrochemical state-reconfiguration strategy in a vertical opto-ionic electrochemical transistor (VOET) that enables reversible transformation between these two information-processing modes. The VOET integrates a porous sol–gel-derived ZnO semiconductor with an ionic-liquid gate in a vertically stacked multifinger architecture, enabling efficient volumetric electrochemical doping and coupling ionic dynamics with electronic transport throughout the channel. In the undoped state, the device exhibits volatile ultraviolet photodetection with an ON/OFF current ratio of 6 × 103, a responsivity of 132 mA/W, and a peak shot-noise-limited specific detectivity of 3.9 × 1010 Jones. Electrochemical ion doping switches the same transistor into a persistent photoconductive state, enabling nonvolatile optoelectronic synaptic operation with a post-tetanic potentiation index of up to 1100% and multidimensional spike-dependent plasticity governed by stimulus rate, duration, number, and intensity. Neural-network simulations using experimentally measured synaptic characteristics further demonstrate handwritten-digit recognition. These results reveal electrochemical state reconfiguration as a route to programmable transformation of transistor functionality, providing a compact platform for adaptive optoelectronic sensing, memory, and neuromorphic computing.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"295 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152177","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}

引用次数: 0

Dark-State-MediatedLow-Energy Electron Attachmentto Molecular Oxygen: Symmetry Adapted Decomposition of the DEA Resonancethrough Dyson-Orbitals’ Incoherent Mixing 暗态介导的低能电子依附于分子氧：戴森-轨道非相干混合对DEA共振的对称适应分解

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-11 DOI: 10.1021/acs.jpclett.6c02057

Narayan Kundu,Ayan Bhowmick,Aryya Ghosh,Dhananjay Nandi,Sourav Pal

{"title":"Dark-State-Mediated\u0000Low-Energy Electron Attachment\u0000to Molecular Oxygen: Symmetry Adapted Decomposition of the DEA Resonance\u0000through Dyson-Orbitals’ Incoherent Mixing","authors":"Narayan Kundu,Ayan Bhowmick,Aryya Ghosh,Dhananjay Nandi,Sourav Pal","doi":"10.1021/acs.jpclett.6c02057","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02057","url":null,"abstract":"Abstract Dissociative electron attachment (DEA) to O2 exhibits a prominent resonance peak at ∼6.5 eV, producing O– with a single kinetic energy band (∼1.5 eV) and a distinct four-lobed angular distribution. Using velocity-map imaging and complex absorbing potential equation-of-motion electron-attachment coupled-cluster singles and doubles (CAP-EOM-EA-CCSD) calculations, we notice that this resonance is mediated by electron-impact excitation to the optically dark a1Δg and b1Σg+ states, which suggests electron impact excitation to these optically dark excited states provides an appropriate electronic structure for electron attachment forming 2Πu, 2Πg and 2,4Σu Feshbach resonances. The measured angular distribution is reproduced by an incoherent superposition of three symmetry channels: 2Πu (66.5%); 2Πg (25.1%); and 2,4Σu (8.5%). The Dyson orbitals computed from the CAP-EOM-EA-CCSD calculations quantitatively reproduce the channel weights and their energy dependencies. This dark-state-mediated mechanism pinpointedly resolves the experimental observations and provides a general symmetry-adapted framework for decomposing DEA resonances from the fragmented anions angular distributions.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"7 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151120","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}

引用次数: 0

Computational Study of Gas-Phase Reactions to ProduceSulfite Esters: A New Class of Sulfur Containing Molecules in theAtmosphere? 气相反应生成亚硫酸盐酯的计算研究：大气中一类新的含硫分子

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-11 DOI: 10.1021/acs.jpclett.6c02217

Christopher David Daub,Avinash Kumar,Matti Rissanen

引用次数: 0

SuppressingNonradiative Voltage Losses in TernaryOrganic Solar Cells via Additional CT States 通过附加CT态抑制三元有机太阳能电池的非辐射电压损失

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-10 DOI: 10.1021/acs.jpclett.6c03080

Botao Wang,Yuan Xiao,Fanghao Cheng,Yaru Dong,Sun Yin

引用次数: 0

PhotogeneratedCharge Injection-Modulated Ultralow-PowerZnO/Sb2S3 Heterojunction Memristors for ArtificialVisual Nociception and Persistence Systems 光致电荷注入调制的超低功率zno /Sb2S3异质结记忆电阻器用于人工视觉痛觉和持久系统

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-10 DOI: 10.1021/acs.jpclett.6c02683

Yuanhui Yang,Yuanfeng Sun,Kai Hu,Haoyuan Li,Shifu Xiong,Shixing Teng,Yuhang Wang,Chuanzhen Dong,Hongling Guo

{"title":"Photogenerated\u0000Charge Injection-Modulated Ultralow-Power\u0000ZnO/Sb2S3 Heterojunction Memristors for Artificial\u0000Visual Nociception and Persistence Systems","authors":"Yuanhui Yang,Yuanfeng Sun,Kai Hu,Haoyuan Li,Shifu Xiong,Shixing Teng,Yuhang Wang,Chuanzhen Dong,Hongling Guo","doi":"10.1021/acs.jpclett.6c02683","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02683","url":null,"abstract":"Abstract Bioinspired neuromorphic architectures featuring sensory-memory-computing integration offer a highly effective approach to overcoming the traditional von Neumann computing bottleneck. However, existing optoelectronic memristors universally face challenges such as high static power consumption and difficulties in modulating resistive switching behaviors during array-level integration. Here, an ultralow-power Ag/PMMA/ZnO/Sb2S3/FTO heterojunction memristor operating at the nanoampere scale is reported. By engineering a Type-II ZnO/Sb2S3 band alignment and incorporating an ultrathin PMMA tunneling barrier, the device achieves synergistic carrier regulation and broadband charge separation. Notably, light illumination significantly reduces the SET voltage from 5.0 to 2.65 V. A collaborative switching model, governed by photocarrier injection and electric-field-driven dynamics, is proposed to elucidate the mechanism of threshold modulation at the interface. Functionally, the device emulates essential synaptic plasticity and realizes an advanced artificial visual nociceptor featuring threshold-triggering, nonadaptation, and relaxation. Furthermore, simulation-based spatiotemporal image processing, including dynamic forgetting and visual persistence, is demonstrated. This work establishes a new mechanistic paradigm for ultralow-power, multimodal neuromorphic vision hardware, paving the way for next-generation energy-efficient bioinspired perception systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"165 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151123","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}

引用次数: 0

Ultrafast Dynamicsof Competing Dimethyl DisulfidePhotodissociation Pathways 竞争二甲基二硫化物光解途径的超快动力学

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-09 DOI: 10.1021/acs.jpclett.6c02772

Neil C. Cole-Filipiak,Varun Rishi,Jack Dalton,Jan Troß,Christopher J. Kliewer,Andrew R. Attar,Matthias C. Hoffmann,Fuhao Ji,Ming-Fu Lin,Yusong Liu,Duan Luo,Joao Pedro Figueira Nunes,Alexander H. Reid,Xiaozhe Shen,Xijie Wang,Thomas Wolf,Jie Yang,Susana Herrera,Vasilios G. Stavros,Laura M. McCaslin,Krupa Ramasesha

{"title":"Ultrafast Dynamics\u0000of Competing Dimethyl Disulfide\u0000Photodissociation Pathways","authors":"Neil C. Cole-Filipiak,Varun Rishi,Jack Dalton,Jan Troß,Christopher J. Kliewer,Andrew R. Attar,Matthias C. Hoffmann,Fuhao Ji,Ming-Fu Lin,Yusong Liu,Duan Luo,Joao Pedro Figueira Nunes,Alexander H. Reid,Xiaozhe Shen,Xijie Wang,Thomas Wolf,Jie Yang,Susana Herrera,Vasilios G. Stavros,Laura M. McCaslin,Krupa Ramasesha","doi":"10.1021/acs.jpclett.6c02772","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02772","url":null,"abstract":"Abstract Disulfide photochemistry impacts a wide range of chemical processes from biological UV photodamage to polymer self-healing and green photocatalysis. Despite this, the response of disulfide bonds to deep-UV light remains poorly understood. Dimethyl disulfide serves as a model system for understanding the fundamental properties of this chemical motif, including its UV photodynamics. While 267-nm excitation exclusively cleaves the S–S bond on a subpicosecond time scale, 200 nm excites electronic states of Rydberg and antibonding character, resulting in competing C–S and S–S dissociation on an unknown time scale. Using mega-electron-volt ultrafast electron diffraction and time-resolved velocity-mapped ion imaging, we find subpicosecond as well as unexpectedly long, picosecond lifetimes. Nonadiabatic mixed quantum-classical dynamics reveal mechanisms and observables. We attribute the subpicosecond dynamics to bond dissociation on singlet states and the picosecond dynamics to dissociation after intersystem crossing. Our study reveals that deep-UV excitation in disulfide-containing molecules can induce complex, multi-time scale dynamics.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"82 1 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151126","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}

引用次数: 0

Ultrafast Core–ShellSpin Transfer and Spin-SelectiveRelaxation in an Endohedral Cage Cluster 内腔笼团簇中的超快核壳自旋转移和自旋选择弛豫

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-09 DOI: 10.1021/acs.jpclett.6c02587

Xueke Yu,Qi Gao,Yu Chen,Wei Pei,Xiuyun Zhang,Yan Su,Jijun Zhao

{"title":"Ultrafast Core–Shell\u0000Spin Transfer and Spin-Selective\u0000Relaxation in an Endohedral Cage Cluster","authors":"Xueke Yu,Qi Gao,Yu Chen,Wei Pei,Xiuyun Zhang,Yan Su,Jijun Zhao","doi":"10.1021/acs.jpclett.6c02587","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02587","url":null,"abstract":"Abstract Ultrafast optical control of spin states offers a promising route to molecular-scale magnetic manipulation, yet the mechanisms of laser-driven spin dynamics in atomically precise clusters remain poorly understood. Here, we investigate the ultrafast spin dynamics of the endohedral Mn@Sn12 cluster using real-time time-dependent density functional theory simulations. Strong Mn 3d–Sn 5p orbital hybridization couples the localized Mn center to the Sn12 cage. Upon femtosecond laser excitation, the Mn@Sn12 cluster exhibits a pronounced transient magnetic response within several femtoseconds, accompanied by changes in the local magnetic moments of both subsystems. Time-dependent analyses of spin-resolved electronic occupations, spin density, and density of states provide evidence for early time intersite redistribution of spin-polarized electronic populations between the Mn center and Sn12 cage. Excited-state relaxation analysis further shows that spin-conserving relaxation is substantially faster than spin-flip relaxation, reflecting efficient electron–vibration coupling and limited spin–orbit-mediated mixing between opposite-spin states. These results elucidate the microscopic origin of ultrafast spin dynamics in molecular nanoclusters and highlight endohedral metal clusters as promising platforms for atomic-scale optical spin control.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"20 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151130","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}

引用次数: 0

ConstructingMechanically Flexible Molecular Crystalswith Tunable Near-Full-Spectrum Emission via an α-CyanodiaryletheneScaffold 通过α-氰二芳烯支架构建具有可调谐近全光谱发射的机械柔性分子晶体

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-09 DOI: 10.1021/acs.jpclett.6c02667

Bo Jing,Jinhe Li,Yankuan Wei,Xuesong Yang,Songgu Wu,Hongyu Zhang,Junbo Gong

引用次数: 0

Simulating UVPhotolysis of Ibuprofen by Time-DependentExcited-State Molecular Dynamics 基于时间依赖性激发态分子动力学模拟布洛芬的紫外光解

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2026-10-09 DOI: 10.1021/acs.jpclett.6c02893

Tabassum Billah,Dauda Mohammed,Yulun Han,Dmitri Kilin,Jiale Xu

引用次数: 0