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

Double-Wavelength-Switchable Molecular Self-Assembly of a Photoacid and Spirooxazine in an Aqueous Solution 水溶液中光酸和螺恶嗪的双波长可切换分子自组装。

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-20 DOI: 10.1021/acs.jpclett.3c02392

Alexander Zika, Mohit Agarwal, Ralf Schweins and Franziska Gröhn*,

引用次数: 0

Long Electron Spin Coherence Times of Atomic Hydrogen Trapped in Silsesquioxane Cages 原子氢在倍半硅氧烷笼中的长电子自旋相干时间。

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-20 DOI: 10.1021/acs.jpclett.3c02626

George Mitrikas*,

引用次数: 0

Mn-Modified ZnO Nanoflakes for Optimal Photoelectrochemical Performance Under Visible Light: Experimental Design and Theoretical Rationalization Mn修饰ZnO纳米片在可见光下的最佳光电化学性能：实验设计和理论合理化。

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-20 DOI: 10.1021/acs.jpclett.3c02730

Abinash Das, Dongyu Liu, Riu Riu Wary, Andrey S. Vasenko, Oleg V. Prezhdo* and Ranjith G. Nair*,

引用次数: 0

Physics-Inspired Equivariant Descriptors of Nonbonded Interactions 受物理学启发的非键合相互作用等变描述符。

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-20 DOI: 10.1021/acs.jpclett.3c02375

Kevin K. Huguenin-Dumittan, Philip Loche, Ni Haoran and Michele Ceriotti*,

引用次数: 2

Reconciling Imbalanced and Nonadiabatic Reactivity in Transition Metal–Oxo-Mediated Concerted Proton Electron Transfer (CPET) 过渡金属氧介导的协同质子-电子转移（CPET）中不平衡和非绝热反应性的协调。

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-19 DOI: 10.1021/acs.jpclett.3c02318

Joseph E. Schneider, and , John S. Anderson*,

{"title":"Reconciling Imbalanced and Nonadiabatic Reactivity in Transition Metal–Oxo-Mediated Concerted Proton Electron Transfer (CPET)","authors":"Joseph E. Schneider,  and , John S. Anderson*, ","doi":"10.1021/acs.jpclett.3c02318","DOIUrl":"10.1021/acs.jpclett.3c02318","url":null,"abstract":"Recently, there have been several experimental demonstrations of how the rates of concerted proton electron transfer (CPET) are affected by stepwise thermodynamic parameters of only proton (ΔG°PT) or electron (ΔG°ET) transfer. Semiclassical structure–activity relationships have been invoked to rationalize these linear free energy relationships, but it is not clear how they would manifest in a nonadiabatic reaction. Using density functional theory calculations, we demonstrate how a decrease in ΔG°PT can lead to transition state imbalance in a nonadiabatic framework. We then use these calculations to anchor a theoretical model that reproduces experimental trends with ΔG°PT and ΔG°ET. Our results reconcile predictions from semiclassical transition state theory with models that treat proton transfer quantum mechanically in CPET reactivity, make new predictions about the importance of basicity for uphill CPET reactions, and suggest similar treatments may be possible for other nonadiabatic reactions.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 43","pages":"9548–9555"},"PeriodicalIF":5.7,"publicationDate":"2023-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49671650","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

Stereoelectronic Switches of Single-Molecule Junctions through Conformation-Modulated Intramolecular Coupling Approaches 通过构象调制分子内耦合方法实现单分子连接的立体电子开关。

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-19 DOI: 10.1021/acs.jpclett.3c02577

Zhuan-Yun Cai, Zi-Wei Ma, Wen-Kai Wu, Jian-De Lin, Lin-Qi Pei, Jia-Zheng Wang, Tai-Rui Wu, Shan Jin, De-Yin Wu* and Zhong-Qun Tian,

{"title":"Stereoelectronic Switches of Single-Molecule Junctions through Conformation-Modulated Intramolecular Coupling Approaches","authors":"Zhuan-Yun Cai, Zi-Wei Ma, Wen-Kai Wu, Jian-De Lin, Lin-Qi Pei, Jia-Zheng Wang, Tai-Rui Wu, Shan Jin, De-Yin Wu* and Zhong-Qun Tian, ","doi":"10.1021/acs.jpclett.3c02577","DOIUrl":"10.1021/acs.jpclett.3c02577","url":null,"abstract":"Stereoelectronic effects in single-molecule junctions have been widely utilized to achieve a molecular switch, but high-efficiency and reproducible switching remain challenging. Here, we demonstrate that there are three stable intramolecular conformations in the 9,10-diphenyl-9,10-methanoanthracen-11-one (DPMAO) systems due to steric effect. Interestingly, different electronic coupling approaches including weak coupling (through-space), decoupling, and strong coupling (through-bond) between two terminal benzene rings are accomplished in the three stable conformations, respectively. Theoretical calculations show that the molecular conductance of three stable conformations differs by more than 1 order of magnitude. Furthermore, the populations of the three stable conformations are highly dependent on the solvent effect and the external electric field. Therefore, an excellent molecular switch can be achieved using the DPMAO molecule junctions and external stimuli. Our findings reveal that modulating intramolecular electronic coupling approaches may be a useful manner to enable molecular switches with high switching ratios. This opens up a new route for building high-efficiency molecular switches in single-molecular junctions.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 43","pages":"9539–9547"},"PeriodicalIF":5.7,"publicationDate":"2023-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49671651","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

Nuclear–Electronic Orbital Quantum Mechanical/Molecular Mechanical Real-Time Dynamics 核电子轨道量子力学/分子力学实时动力学。

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-19 DOI: 10.1021/acs.jpclett.3c02275

Mathew Chow, Tao E. Li and Sharon Hammes-Schiffer*,

{"title":"Nuclear–Electronic Orbital Quantum Mechanical/Molecular Mechanical Real-Time Dynamics","authors":"Mathew Chow, Tao E. Li and Sharon Hammes-Schiffer*, ","doi":"10.1021/acs.jpclett.3c02275","DOIUrl":"10.1021/acs.jpclett.3c02275","url":null,"abstract":"Simulating the nuclear–electronic quantum dynamics of large-scale molecular systems in the condensed phase is key for studying biologically and chemically important processes such as proton transfer and proton-coupled electron transfer reactions. Herein, the real-time nuclear–electronic orbital time-dependent density functional theory (RT-NEO-TDDFT) approach is combined with a hybrid quantum mechanical/molecular mechanical (QM/MM) strategy to enable the accurate description of coupled nuclear–electronic quantum dynamics in the presence of heterogeneous environments such as solvent or proteins. The densities of the electrons and quantum protons are propagated in real time, while the other nuclei are propagated classically on the instantaneous electron–proton vibronic surface. This approach is applied to phenol bound to lysozyme, intramolecular proton transfer in malonaldehyde, and nonequilibrium excited-state intramolecular proton transfer in o-hydroxybenzaldehyde. These examples illustrate that the RT-NEO-TDDFT framework, coupled with an atomistic representation of the environment, allows the simulation of condensed-phase systems that exhibit significant nuclear quantum effects.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 43","pages":"9556–9562"},"PeriodicalIF":5.7,"publicationDate":"2023-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49671702","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

Ammonia Cracking Catalyzed by Ni Nanoparticles Confined in the Framework of CeO2 Support CeO2载体框架内Ni纳米粒子催化氨裂解

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-18 DOI: 10.1021/acs.jpclett.3c02446

Hiroshi Mizoguchi*, Yuta Osawa, Masato Sasase, Naoki Ohashi, Masaaki Kitano and Hideo Hosono*,

引用次数: 0

Halide Ions Regulating the Morphologies of PbS and Au@PbS Core–Shell Nanocrystals: Synthesis, Self-Assembly, and Electrical Transport Properties 卤化物离子对PbS和Au@PbS核壳纳米晶体：合成、自组装和电输运性质。

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-18 DOI: 10.1021/acs.jpclett.3c02614

Feiyue Ge, Yingying Han, Changsheng Feng, Han Zhang, Feifan Chen, Dan Xu, Chen-Lei Tao, Fang Cheng* and Xue-Jun Wu*,

{"title":"Halide Ions Regulating the Morphologies of PbS and Au@PbS Core–Shell Nanocrystals: Synthesis, Self-Assembly, and Electrical Transport Properties","authors":"Feiyue Ge, Yingying Han, Changsheng Feng, Han Zhang, Feifan Chen, Dan Xu, Chen-Lei Tao, Fang Cheng* and Xue-Jun Wu*, ","doi":"10.1021/acs.jpclett.3c02614","DOIUrl":"10.1021/acs.jpclett.3c02614","url":null,"abstract":"The geometry and surface state of nanocrystals (NCs) strongly affect their physiochemical properties, self-assembly behaviors, and potential applications, but there is still a lack of a facile method to regulate the exposed facets of the NCs, especially metal@semiconductor core–shell NCs. Herein, we present a reproducible approach for tuning the morphology of PbS NCs from nanocubes to nano-octahedrons by introducing lead halides as precursors. Excitingly, the method can be easily extended to the synthesis of metal@PbS core–shell NCs with single-crystalline shells and specific exposed facets. In addition, the halide passivation layers on the NCs are found to greatly improve their antioxidant ability. Therefore, the Cl-passivated NCs can self-assemble into atomic-coupled monolayer films via oriented attachment under ambient conditions, which exhibit enhanced electrical conductivities compared with uncoupled counterparts. The precise synthesis of nanocrystals with tunable shapes and the construction of self-assembled films provide a way to expand their application in high-performance optoelectronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 42","pages":"9521–9530"},"PeriodicalIF":5.7,"publicationDate":"2023-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49671699","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

Data Driven Computational Design and Experimental Validation of Drugs for Accelerated Mitigation of Pandemic-like Scenarios 加速缓解类似流行病的药物的数据驱动计算设计和实验验证。

IF 5.7 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2023-10-18 DOI: 10.1021/acs.jpclett.3c01749

Samrendra K. Singh, Kelsie King, Cole Gannett, Christina Chuong, Soumil Y. Joshi, Charles Plate, Parisa Farzeen, Emily M. Webb, Lakshmi Kumar Kunche, James Weger-Lucarelli, Andrew N. Lowell, Anne M. Brown* and Sanket A. Deshmukh*,

{"title":"Data Driven Computational Design and Experimental Validation of Drugs for Accelerated Mitigation of Pandemic-like Scenarios","authors":"Samrendra K. Singh, Kelsie King, Cole Gannett, Christina Chuong, Soumil Y. Joshi, Charles Plate, Parisa Farzeen, Emily M. Webb, Lakshmi Kumar Kunche, James Weger-Lucarelli, Andrew N. Lowell, Anne M. Brown* and Sanket A. Deshmukh*, ","doi":"10.1021/acs.jpclett.3c01749","DOIUrl":"10.1021/acs.jpclett.3c01749","url":null,"abstract":"Emerging pathogens are a historic threat to public health and economic stability. Current trial-and-error approaches to identify new therapeutics are often ineffective due to their inefficient exploration of the enormous small molecule design space. Here, we present a data-driven computational framework composed of hybrid evolutionary algorithms for evolving functional groups on existing drugs to improve their binding affinity toward the main protease (Mpro) of SARS-CoV-2. We show that combinations of functional groups and sites are critical to design drugs with improved binding affinity, which can be easily achieved using our framework by exploring a fraction of the available search space. Atomistic simulations and experimental validation elucidate that enhanced and prolonged interactions between functionalized drugs and Mpro residues result in their improved therapeutic value over that of the parental compound. Overall, this novel framework is extremely flexible and has the potential to rapidly design inhibitors for any protein with available crystal structures.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 42","pages":"9490–9499"},"PeriodicalIF":5.7,"publicationDate":"2023-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41230405","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