The Journal of Physical Chemistry Letters最新文献_第2页

Light-Powered Transport of Organic Anions by Microbial Rhodopsins. 微生物紫红质对有机阴离子的光传输。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-02 DOI: 10.1021/acs.jpclett.5c02551

Simiao Shen,Shoichiro Akita,Joji Wada,Mako Eguchi,Takashi Tsukamoto,Kwang-Hwan Jung,Yuki Sudo,Takashi Kikukawa

引用次数: 0

Suppression of Exciton Fine-Structure Splitting in Anisotropic Colloidal Quantum Dots for Applications in Quantum Communications. 抑制各向异性胶体量子点激子细结构分裂在量子通信中的应用。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-01 DOI: 10.1021/acs.jpclett.5c02582

Serguei V Goupalov

引用次数: 0

Formation of Larger Solvation Shells in a LiFSI Salt Solution for Enhanced Li+ Transport. 在LiFSI盐溶液中形成更大的溶剂化壳层以增强Li+输运。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-01 DOI: 10.1021/acs.jpclett.5c02445

Naresh C Osti,Eugene Mamontov

{"title":"Formation of Larger Solvation Shells in a LiFSI Salt Solution for Enhanced Li+ Transport.","authors":"Naresh C Osti,Eugene Mamontov","doi":"10.1021/acs.jpclett.5c02445","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02445","url":null,"abstract":"Electrodes and electrolytes in Li-ion batteries (LIBs) are crucial for their electrochemical performance, and fabricating these materials to achieve the desired properties for improved efficiency is challenging. A recent study published in Nature ( Nature 2024, 627, 101-107) outlined guidelines for designing an electrolyte using fluoroacetonitrile (FACN), a small-molecule solvent with low solvation energy. This characteristic enables the formation of an anion-rich inorganic interphase in a 1.3 M lithium bis(fluorosulfonyl)imide (LiFSI) solution, facilitating higher ionic conductivity, even at low temperatures. The formation of a ligand channel was postulated and demonstrated in the simulation due to the attraction of small solvent molecules from the secondary solvation shell to the Li+ ion in the primary solvation shell, thereby enhancing Li+ transport. While that study primarily focused on Li+ ion behavior in LIBs, the behavior of FACN in solutions with different lithium salts and what makes LiFSI in FACN outperform other systems remain to be explored. Using an experimental technique sensitive to FACN molecules, here we directly observe formation of larger solvation shells in a LiFSI solution compared to the Li salts with different anions, consistent with the postulated ligand-channel-mechanism and potentially paving the way to achieving enhanced ionic conductivity and energy density during LIB operation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"20 1","pages":"10434-10439"},"PeriodicalIF":6.475,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194507","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

Disulfide-Centered Hydrogen Bonding: Insights from Protein Structure Analysis and IR-UV Double Resonance Spectroscopy. 以二硫化物为中心的氢键：来自蛋白质结构分析和红外-紫外双共振光谱的见解。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-01 DOI: 10.1021/acs.jpclett.5c02737

Akshay Kumar Sahu,Anant Ram Satpathi,Saiprakash Rout,Radharaman Samanta,Laxmipriya Dash,Himansu S Biswal

{"title":"Disulfide-Centered Hydrogen Bonding: Insights from Protein Structure Analysis and IR-UV Double Resonance Spectroscopy.","authors":"Akshay Kumar Sahu,Anant Ram Satpathi,Saiprakash Rout,Radharaman Samanta,Laxmipriya Dash,Himansu S Biswal","doi":"10.1021/acs.jpclett.5c02737","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02737","url":null,"abstract":"Despite the importance of disulfide bonds in proteins, direct experimental characterization of noncovalent interactions involving their sulfur atoms, particularly sulfur-centered hydrogen bonds (H-bonds), remains underexplored. Here, we present an integrated study combining Protein Data Bank (PDB) analysis, quantum chemical calculations, and gas-phase vibrational spectroscopy. PDB screening revealed disulfide bonds in ∼20% of protein structures, with nearly 20 000 potential O-H···S and N-H···S H-bonds. The O-H···S H-bonds are shorter and more directional than the N-H···S H-bonds, consistent with the topological and energetic analyses of model systems. Mass-selective electronic and IR spectroscopy on the jet-cooled p-cresol-dimethyl disulfide (pCR-DMDS) complex confirmed disulfide-centered H-bonds through red-shifts in S1 → S0 electronic transitions and O-H stretching frequencies (ΔνO-H). The experimental ΔνO-H shift and comparative analysis with other H-bond acceptors (H2S, H2O, and dimethylsulfide) provide benchmark data on the intrinsic strength of disulfide-centered H-bonds, crucial for refining computational models and enhancing the understanding of their role in protein structure and function.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"24 1","pages":"10455-10465"},"PeriodicalIF":6.475,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194509","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

Hidden Effects of Anharmonic Bath on the Excitation Energy Transfer in the Light Harvesting 2 Complex of Purple Bacteria. 非调和浴对紫色细菌光收集复合物激发能传递的隐性影响。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-01 DOI: 10.1021/acs.jpclett.5c02414

Kwang Hyun Cho,Seogjoo J Jang,Young Min Rhee

{"title":"Hidden Effects of Anharmonic Bath on the Excitation Energy Transfer in the Light Harvesting 2 Complex of Purple Bacteria.","authors":"Kwang Hyun Cho,Seogjoo J Jang,Young Min Rhee","doi":"10.1021/acs.jpclett.5c02414","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02414","url":null,"abstract":"Environmental effects in the excitation energy transfer (EET) processes have been predominantly modeled by baths of harmonic oscillators; however, the key features of anharmonicities that are overlooked in such descriptions remain poorly understood. Through detailed comparison of the dynamics of a realistic molecular bath with its best effective harmonic representation, here, we uncover new qualitative details of such effects accompanying EET in the light harvesting 2 (LH2) complex of purple bacteria. Results of mixed quantum-classical simulations demonstrate that the harmonic oscillator bath model can effectively reproduce major features of the EET dynamics of those for anharmonic bath with proper choice of initial conditions, confirming the validity of many spectroscopic data modeled by the harmonic oscillator bath. However, it falls short of representing the nonequilibrium nuclear dynamics, even at the qualitative level. In particular, we find that vibrational energy flow mechanisms due to anharmonic couplings between pigment vibrational modes cannot be captured by the harmonic oscillator bath. The importance of this observation in relation to biological mechanisms of heat dissipation are discussed. We also identify important signatures of anharmonicities in detailed features of bath spectral densities. These results demonstrate hidden roles and features of anharmonic effects that can be perceived through accurate representation of potential energy surfaces, which contribute to the robust and resilient functionality of natural light-harvesting complexes.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"35 1","pages":"10473-10482"},"PeriodicalIF":6.475,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145203685","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

Anharmonic Motion-Induced Self-Passivation of Hydrogen Defects in Hybrid Organic-Inorganic Perovskites: Ab Initio Quantum Dynamics. 杂化有机-无机钙钛矿中氢缺陷的非调和运动诱导自钝化：从头算量子动力学。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-01 DOI: 10.1021/acs.jpclett.5c02546

Xuesong Tian,Andrey S Vasenko,Evgueni V Chulkov,Run Long

引用次数: 0

The Role of Rigidity in Augmentation of Fluorescence and Room-Temperature Phosphorescence in Multinuclear Zn2+-Schiff Base Complexes. 刚性对多核Zn2+-席夫碱配合物荧光和室温磷光增强的作用。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-01 DOI: 10.1021/acs.jpclett.5c02185

Arkaprava Chowdhury,Souradip Dasgupta,Mirza Nasib Begg,Nrita Gaur,Dinesh Kabra,Anindya Datta

引用次数: 0

Multidimensional Quantum Dynamics of Double Hydrogen Transfer in Porphycene: Effects of Anharmonic Vibrational Mode Couplings. 卟啉中双氢转移的多维量子动力学：非谐波振动模式耦合的影响。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-01 DOI: 10.1021/acs.jpclett.5c02371

Xiaoxi Liu,Wei Liu,Wensheng Bian

引用次数: 0

Spin-to-Charge Conversion Modulated by Chiral Molecules. 手性分子调制的自旋-电荷转换。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-01 DOI: 10.1021/acs.jpclett.5c02519

Peng-Yi Liu, Tian-Yi Zhang, Ai-Min Guo, Yossi Paltiel, Qing-Feng Sun

引用次数: 0

Critical Role of Intermolecular-Interaction-Mediated Conformational Dynamics in Sensitized OLEDs. 分子间相互作用介导的构象动力学在敏化oled中的关键作用。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-10-01 DOI: 10.1021/acs.jpclett.5c02231

Cheng-Yu Yao,Qing-Yu Meng,Xue-Liang Wen,Hao-Yun Shao,Juan Qiao

{"title":"Critical Role of Intermolecular-Interaction-Mediated Conformational Dynamics in Sensitized OLEDs.","authors":"Cheng-Yu Yao,Qing-Yu Meng,Xue-Liang Wen,Hao-Yun Shao,Juan Qiao","doi":"10.1021/acs.jpclett.5c02231","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02231","url":null,"abstract":"Sensitized organic light-emitting diodes (OLEDs) based on a thermally activated delayed fluorescence sensitizer require high Förster resonance energy transfer efficiency (ΦFRET) to achieve high efficiency and color purity. Since the energy transfer process involves complex interactions between two distinct molecules in amorphous solid film, it remains far from being understood and needs deep insights. Herein, taking two representative sensitizers, nonrigid donor-π-acceptor type DMAC-TRZ and rigid donor-spiro-acceptor type ACRSA as examples, we first established a reliable multiscale model based on the picture of the energy transfer process and obtained experimentally verified energy transfer rates (kFRET∼107 s-1) and then performed molecular-level calculations to explore the interplay of intermolecular interactions and molecular rigidity in governing ΦFRET. For nonrigid DMAC-TRZ, it is not the commonly believed intrinsic conformer variation via the dihedral angle between the donor and π unit but strong intermolecular interactions with a terminal emitter at short distance that induce undesirable low-energy conformers with large variation in the dihedral angle between the acceptor and π unit, which further result in an anomalous reduction of Franck-Condon factor weighted density of states (FCWD) and thus lower-than-expected kFRET and ΦFRET. For ACRSA, it is a rigid spirocyclic structure that greatly weakens intermolecular interactions and preserves an almost distance-independent molecular conformation, thus facilitating nearly uniform FCWD parameters and superior kFRET and ΦFRET. Our study provides fresh insights into the critical role of intermolecular-interaction-mediated conformational dynamics in energy transfer, revealing a blind and vital point behind molecular rigidity in developing high-performance sensitized OLEDs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"175 1","pages":"10440-10448"},"PeriodicalIF":6.475,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194510","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