The Journal of Physical Chemistry Letters最新文献

Operating Mechanism Principles and Advancements for Halide Perovskite-Based Memristors and Neuromorphic Devices 基于卤化物过氧化物的记忆晶体和神经形态设备的运行机制原理与进展

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-27 DOI: 10.1021/acs.jpclett.4c02170

So-Yeon Kim, Heyi Zhang, Jenifer Rubio-Magnieto

{"title":"Operating Mechanism Principles and Advancements for Halide Perovskite-Based Memristors and Neuromorphic Devices","authors":"So-Yeon Kim, Heyi Zhang, Jenifer Rubio-Magnieto","doi":"10.1021/acs.jpclett.4c02170","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02170","url":null,"abstract":"With the advent of the generation of artificial intelligence (AI) based on big data-processing technologies, next-generation memristor and memristive neuromorphic devices have been actively studied with great interest to overcome the von Neumann bottleneck limits. Among various candidates, halide perovskites (HPs) have been in the spotlight as potential candidates for these devices due to their unique switching characteristics with low energy consumption and flexible integration compatibility across various sources for scalability. We outline the characteristics and operating principles of HP-based memristors and their neuromorphic devices. We explain filamentary- and interface-type switching according to the type of conducting pathway occurring inside the active HP layer and the operating mechanisms depending on the species that make up this conducting pathway. We summarize the types and mechanisms of current changes beneficial for neuromorphic device applications and finally organize various suggested analysis tools and physical models to enable experimental determination of switching mechanisms from various perspectives.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325821","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

Strategies To Achieve Long-Term Stability in Lead Halide Perovskite Nanocrystals and Its Optoelectronic Applications 实现卤化铅过氧化物纳米晶体的长期稳定性及其光电应用的战略

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-27 DOI: 10.1021/acs.jpclett.4c02240

Shovon Chatterjee, Subarna Biswas, Smruti Sourav, Jyotisman Rath, Syed Akhil, Nimai Mishra

引用次数: 0

Diverse Excitonic Phenomena in Asymmetric Trilayer Transition Metal Dichalcogenide Heterostructures 不对称三层过渡金属二卤化物异质结构中的多种激子现象

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-27 DOI: 10.1021/acs.jpclett.4c02526

Zhe Zhang, Shudong Wang

{"title":"Diverse Excitonic Phenomena in Asymmetric Trilayer Transition Metal Dichalcogenide Heterostructures","authors":"Zhe Zhang, Shudong Wang","doi":"10.1021/acs.jpclett.4c02526","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02526","url":null,"abstract":"Interlayer excitons formed in two-dimensional transition metal dichalcogenide (TMD) heterostructures can be easily tuned due to the large spatial separation. In this work, we discuss the electronic and excitonic optical properties of trilayer heterostructures MoS2/MoSSe/WSe2 and MoS2/MoSSe/MoSe2 using state-of-the-art GW+BSE calculations. In both trilayer geometries, we discover a variety of exciton states, including interlayer excitons, every-other-layer excitons, and their hybridized states, h-IX. Importantly, the h-IXs are optically bright through hybridizing with the intralayer excitons, and the radiative lifetimes of h-IXs range from subnanoseconds to tens of microseconds at 77 K, depending on their compositions. We also reveal that the diversity of the low-lying IXs in MoS2/MoSSe/MoSe2 is higher than that of MoS2/MoSSe/WSe2, because more energy levels participate in transitions in MoS2/MoSSe/MoSe2. Our findings demonstrate that the appropriate energy alignment via manipulating the Janus layer is crucial for realizing rich excitonic states in trilayer TMD heterostructures.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325792","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

Mechanistic Study on Oxygen Reduction Reaction in High-Concentrated Electrolytes for Aprotic Lithium–Oxygen Batteries 锂氧电池高浓度电解质中氧还原反应的机理研究

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-27 DOI: 10.1021/acs.jpclett.4c02455

Yuwei Su, Zhiwei Zhao, Erkang Wang, Zhangquan Peng

{"title":"Mechanistic Study on Oxygen Reduction Reaction in High-Concentrated Electrolytes for Aprotic Lithium–Oxygen Batteries","authors":"Yuwei Su, Zhiwei Zhao, Erkang Wang, Zhangquan Peng","doi":"10.1021/acs.jpclett.4c02455","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02455","url":null,"abstract":"Highly concentrated electrolytes (HCEs) have energized the development of high-energy-density lithium metal batteries by facilitating the formation of robust inorganic-derived solid electrolyte interfaces on the lithium anode. However, the oxygen reduction reaction (ORR) occurring on the cathode side remains ambiguous in HCE-based lithium–oxygen (Li–O2) batteries. Herein, we investigate the ORR mechanism in a highly concentrated LiTFSI-CH3CN electrolyte using ultra-microelectrode voltammetry coupled with in situ spectroscopies. It is found that, compared to the dilute electrolyte, the HCE prolongs the lifespan of superoxide intermediates and decelerates their migration rate to the bulk solution, resulting in a change in growth mode for the discharge product of Li2O2 from traditional two-dimensional film growth to surface three-dimensional expansion growth. This alteration reduces the cathode passivation and thus delivers the enhanced discharge capacity. Additionally, the HCE also increases the reaction energy barrier between superoxide and solvent molecules, thereby minimizing parasitic reactions and improving the cycle performance of Li–O2 batteries. Our study reveals the intricate interplay between electrolytes and oxygen intermediates and provides important insights into electrolyte chemistries for better Li–O2 batteries.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325794","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

Correction to “Role of H2O Adsorption in CO Oxidation over Cerium-Oxide Cluster Anions (CeO2)nO– (n = 1–4)” 更正 "氧化铈簇阴离子 (CeO2)nO- (n = 1-4) 在 CO 氧化过程中对 H2O 的吸附作用"

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-27 DOI: 10.1021/acs.jpclett.4c02726

Jiao-Jiao Chen, Si-Dun Wang, Xun-Lei Ding, Sheng-Gui He

引用次数: 0

The Challenging Conformational Landscape of Cysteamine···H2O Revealed by the Strong Interplay of Rotational Spectroscopy and Quantum Chemical Calculations 旋转光谱和量子化学计算的强相互作用揭示了半胱胺--H2O 的挑战性构象格局

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-26 DOI: 10.1021/acs.jpclett.4c02353

Wentao Song, Assimo Maris, Charlotte N. Cummings, Luca Evangelisti, Nicholas R. Walker, Sonia Melandri

{"title":"The Challenging Conformational Landscape of Cysteamine···H2O Revealed by the Strong Interplay of Rotational Spectroscopy and Quantum Chemical Calculations","authors":"Wentao Song, Assimo Maris, Charlotte N. Cummings, Luca Evangelisti, Nicholas R. Walker, Sonia Melandri","doi":"10.1021/acs.jpclett.4c02353","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02353","url":null,"abstract":"A 1:1 molecular complex of cysteamine with water is shown to adopt a cage-like structure where cysteamine accepts a relatively strong hydrogen bond from water while also engaging in two additional weaker interactions (SH···Ow and CH···Ow). Experimental and theoretical approaches confirm this conformer as the global minimum on the potential energy surface. Fitting of key structural parameters to experimentally determined moments of inertia yields consistent and accurate results for rotational and 14N nuclear quadrupole coupling constants which are shown to be challenging to calculate using ab initio methods. Comprehensive analysis of the intermolecular interactions and a thorough comparison with the properties of aminoethanol–water is presented, utilizing independent gradient models based on Hirshfeld partition, quantum theory of atoms-in-molecules, and symmetry-adapted perturbation theory approaches. As expected, the OH group of aminoethanol is a stronger hydrogen bond donor than the SH group in cysteamine, while the CH···Ow interaction is a key determining factor of the conformational landscape in both cysteamine–water and aminoethanol–water complexes. The results show very clearly that the synergy between theoretical calculations and experimental results is not only desirable but mandatory to get the right answers in such complex conformational surfaces. The results are also clear benchmarks for the accuracy of different theoretical methods in assessing the structures and energy order of the conformations.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321448","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

Topological Protection of Oxygen Redox in Li-Rich Cathodes 富锂阴极中氧氧化还原的拓扑保护

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-26 DOI: 10.1021/acs.jpclett.4c01929

Zhefeng Chen, Wentao Zhang, Shunning Li, Feng Pan

引用次数: 0

Singlet–Triplet Inversions in Through-Bond Charge-Transfer States 直通键电荷转移态中的单三反转

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-26 DOI: 10.1021/acs.jpclett.4c02317

J. Terence Blaskovits, Clémence Corminboeuf, Marc H. Garner

引用次数: 0

Structure and Dynamics of ATP and the ATP–Zn2+ Complex in Solution ATP 和 ATP-Zn2+ 复合物在溶液中的结构与动力学

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-26 DOI: 10.1021/acs.jpclett.4c02296

Emma Rossi, Achintya Kundu, Alberta Ferrarini, Thomas Elsaesser, Marialore Sulpizi

引用次数: 0

Chemically Reversible Translational Moiré Superlattice Formations in the Two-Dimensional Films of the Zinc Phthalate Complex 邻苯二甲酸锌复合物二维薄膜中的化学可逆平移莫伊尔超晶格形成

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-09-26 DOI: 10.1021/acs.jpclett.4c02284

Archismita Hajra, Arun Chattopadhyay

{"title":"Chemically Reversible Translational Moiré Superlattice Formations in the Two-Dimensional Films of the Zinc Phthalate Complex","authors":"Archismita Hajra, Arun Chattopadhyay","doi":"10.1021/acs.jpclett.4c02284","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02284","url":null,"abstract":"The exciting electronic properties of two-dimensional layered materials introduced by twist angle and lattice mismatch between two consecutive layers are well-recognized. The major challenge lies in the control over the moiré periodicity. Herein, we report a chemically directed way to achieve the desired precision over moiré periodicity of the assembly of a complex of zinc ions and o-phthalic acid utilizing soft bonds. The reaction of o-phthalic acid with zinc ions in the aqueous medium at 80 °C for 1 h followed by preserving the reaction mixture at ambient temperature (35 °C) resulted in translational moiré superlattices with precise periods. Those lattices are further stacked angularly to give rotational super-moiré lattices. Further, the role of the π–zinc ion interaction in the origin of moiré fringes was examined with the reaction with 8-hydroxyquinoline-5-sulfonic acid (HQS) that also established the reversible nature of the superlattices. The present observations also suggest the formation of moiré superlattice through ion insertion in a chemical lattice.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321446","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