Annual review of physical chemistry最新文献_第9页

Atomic Force Microscopy: An Emerging Tool in Measuring the Phase State and Surface Tension of Individual Aerosol Particles. 原子力显微镜:测量单个气溶胶颗粒的相态和表面张力的新兴工具。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-11-01 DOI: 10.1146/annurev-physchem-090419-110133

Hansol D Lee, Alexei V Tivanski

引用次数: 15

Understanding and Controlling Intersystem Crossing in Molecules. 理解和控制分子间的系统交叉。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-02-19 DOI: 10.1146/annurev-physchem-061020-053433

Christel M Marian

{"title":"Understanding and Controlling Intersystem Crossing in Molecules.","authors":"Christel M Marian","doi":"10.1146/annurev-physchem-061020-053433","DOIUrl":"https://doi.org/10.1146/annurev-physchem-061020-053433","url":null,"abstract":"This review article focuses on the understanding of intersystem crossing (ISC) in molecules. It addresses readers who are interested in the phenomenon of intercombination transitions between states of different electron spin multiplicities but are not familiar with relativistic quantum chemistry. Among the spin-dependent interaction terms that enable a crossover between states of different electron spin multiplicities, spin-orbit coupling (SOC) is by far the most important. If SOC is small or vanishes by symmetry, ISC can proceed by electronic spin-spin coupling (SSC) or hyperfine interaction (HFI). Although this review discusses SSC- and HFI-based ISC, the emphasis is on SOC-based ISC. In addition to laying the theoretical foundations for the understanding of ISC, the review elaborates on the qualitative rules for estimating transition probabilities. Research on the mechanisms of ISC has experienced a major revival in recent years owing to its importance in organic light-emitting diodes (OLEDs). Exemplified by challenging case studies, chemical substitution and solvent environment effects are discussed with the aim of helping the reader to understand and thereby get a handle on the factors that steer the efficiency of ISC.","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"617-640"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25386245","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 57

Quantum Dynamics of Exciton Transport and Dissociation in Multichromophoric Systems. 多色系中激子输运和解离的量子动力学。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-02-26 DOI: 10.1146/annurev-physchem-090419-040306

Wjatscheslaw Popp, Dominik Brey, Robert Binder, Irene Burghardt

引用次数: 23

From Intermolecular Interaction Energies and Observable Shifts to Component Contributions and Back Again: A Tale of Variational Energy Decomposition Analysis. 从分子间相互作用能和可观察的位移到组分贡献再回来:一个变分能量分解分析的故事。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-02-26 DOI: 10.1146/annurev-physchem-090419-115149

Yuezhi Mao, Matthias Loipersberger, Paul R Horn, Akshaya Das, Omar Demerdash, Daniel S Levine, Srimukh Prasad Veccham, Teresa Head-Gordon, Martin Head-Gordon

{"title":"From Intermolecular Interaction Energies and Observable Shifts to Component Contributions and Back Again: A Tale of Variational Energy Decomposition Analysis.","authors":"Yuezhi Mao, Matthias Loipersberger, Paul R Horn, Akshaya Das, Omar Demerdash, Daniel S Levine, Srimukh Prasad Veccham, Teresa Head-Gordon, Martin Head-Gordon","doi":"10.1146/annurev-physchem-090419-115149","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090419-115149","url":null,"abstract":"Quantum chemistry in the form of density functional theory (DFT) calculations is a powerful numerical experiment for predicting intermolecular interaction energies. However, no chemical insight is gained in this way beyond predictions of observables. Energy decomposition analysis (EDA) can quantitatively bridge this gap by providing values for the chemical drivers of the interactions, such as permanent electrostatics, Pauli repulsion, dispersion, and charge transfer. These energetic contributions are identified by performing DFT calculations with constraints that disable components of the interaction. This review describes the second-generation version of the absolutely localized molecular orbital EDA (ALMO-EDA-II). The effects of different physical contributions on changes in observables such as structure and vibrational frequencies upon complex formation are characterized via the adiabatic EDA. Example applications include red- versus blue-shifting hydrogen bonds; the bonding and frequency shifts of CO, N2, and BF bound to a [Ru(II)(NH3)5]2 + moiety; and the nature of the strongly bound complexes between pyridine and the benzene and naphthalene radical cations. Additionally, the use of ALMO-EDA-II to benchmark and guide the development of advanced force fields for molecular simulation is illustrated with the recent, very promising, MB-UCB potential.","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"641-666"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25408808","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 34

Vibronic and Environmental Effects in Simulations of Optical Spectroscopy. 光谱学模拟中的振动和环境效应。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-01-04 DOI: 10.1146/annurev-physchem-090419-051350

Tim J Zuehlsdorff, Sapana V Shedge, Shao-Yu Lu, Hanbo Hong, Vincent P Aguirre, Liang Shi, Christine M Isborn

{"title":"Vibronic and Environmental Effects in Simulations of Optical Spectroscopy.","authors":"Tim J Zuehlsdorff, Sapana V Shedge, Shao-Yu Lu, Hanbo Hong, Vincent P Aguirre, Liang Shi, Christine M Isborn","doi":"10.1146/annurev-physchem-090419-051350","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090419-051350","url":null,"abstract":"Including both environmental and vibronic effects is important for accurate simulation of optical spectra, but combining these effects remains computationally challenging. We outline two approaches that consider both the explicit atomistic environment and the vibronic transitions. Both phenomena are responsible for spectral shapes in linear spectroscopy and the electronic evolution measured in nonlinear spectroscopy. The first approach utilizes snapshots of chromophore-environment configurations for which chromophore normal modes are determined. We outline various approximations for this static approach that assumes harmonic potentials and ignores dynamic system-environment coupling. The second approach obtains excitation energies for a series of time-correlated snapshots. This dynamic approach relies on the accurate truncation of the cumulant expansion but treats the dynamics of the chromophore and the environment on equal footing. Both approaches show significant potential for making strides toward more accurate optical spectroscopy simulations of complex condensed phase systems.","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"165-188"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39126539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 22

Quantum-State Control and Manipulation of Paramagnetic Molecules with Magnetic Fields. 具有磁场的顺磁分子的量子态控制和操纵。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-01-25 DOI: 10.1146/annurev-physchem-090419-053842

Brianna R Heazlewood

{"title":"Quantum-State Control and Manipulation of Paramagnetic Molecules with Magnetic Fields.","authors":"Brianna R Heazlewood","doi":"10.1146/annurev-physchem-090419-053842","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090419-053842","url":null,"abstract":"Since external magnetic fields were first employed to deflect paramagnetic atoms in 1921, a range of magnetic field-based methods have been introduced to state-selectively manipulate paramagnetic species. These methods include magnetic guides, which selectively filter paramagnetic species from all other components of a beam, and magnetic traps, where paramagnetic species can be spatially confined for extended periods of time. However, many of these techniques were developed for atomic-rather than molecular-paramagnetic species. It has proven challenging to apply some of these experimental methods developed for atoms to paramagnetic molecules. Thanks to the emergence of new experimental approaches and new combinations of existing techniques, the past decade has seen significant progress toward the manipulation and control of paramagnetic molecules. This review identifies the key methods that have been implemented for the state-selective manipulation of paramagnetic molecules-discussing the motivation, state of the art, and future prospects of the field. Key applications include the ability to control chemical interactions, undertake precise spectroscopic measurements, and challenge our understanding of chemical reactivity at a fundamental level.","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"353-373"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38857524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 8

Cascaded Biocatalysis and Bioelectrocatalysis: Overview and Recent Advances. 级联生物催化和生物电催化:综述和最新进展。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-01-27 DOI: 10.1146/annurev-physchem-090519-050109

Yoo Seok Lee, Koun Lim, Shelley D Minteer

引用次数: 16

Electrochemical Tip-Enhanced Raman Spectroscopy: An In Situ Nanospectroscopy for Electrochemistry. 电化学尖端增强拉曼光谱:电化学的原位纳米光谱。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-05-01 DOI: 10.1146/annurev-physchem-061020-053442

Sheng-Chao Huang, Yi-Fan Bao, Si-Si Wu, Teng-Xiang Huang, Matthew M Sartin, Xiang Wang, Bin Ren

{"title":"Electrochemical Tip-Enhanced Raman Spectroscopy: An In Situ Nanospectroscopy for Electrochemistry.","authors":"Sheng-Chao Huang, Yi-Fan Bao, Si-Si Wu, Teng-Xiang Huang, Matthew M Sartin, Xiang Wang, Bin Ren","doi":"10.1146/annurev-physchem-061020-053442","DOIUrl":"https://doi.org/10.1146/annurev-physchem-061020-053442","url":null,"abstract":"Revealing the intrinsic relationships between the structure, properties, and performance of the electrochemical interface is a long-term goal in the electrochemistry and surface science communities because it could facilitate the rational design of electrochemical devices. Achieving this goal requires in situ characterization techniques that provide rich chemical information and high spatial resolution. Electrochemical tip-enhanced Raman spectroscopy (EC-TERS), which provides molecular fingerprint information with nanometer-scale spatial resolution, is a promising technique for achieving this goal. Since the first demonstration of this technique in 2015, EC-TERS has been developed for characterizing various electrochemical processes at the nanoscale and molecular level. Here, we review the development of EC-TERS over the past 5 years. We discuss progress in addressing the technical challenges, including optimizing the EC-TERS setup and solving tip-related issues, and provide experimental guidelines. We also survey the important applications of EC-TERS for probing molecular protonation, molecular adsorption, electrochemical reactions, and photoelectrochemical reactions. Finally, we discuss the opportunities and challenges in the future development of this young technique.","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"213-234"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38782809","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 11

Control of Chemical Reaction Pathways by Light-Matter Coupling. 光-物质耦合对化学反应途径的控制。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-01-22 DOI: 10.1146/annurev-physchem-090519-045502

Dinumol Devasia, Ankita Das, Varun Mohan, Prashant K Jain

{"title":"Control of Chemical Reaction Pathways by Light-Matter Coupling.","authors":"Dinumol Devasia, Ankita Das, Varun Mohan, Prashant K Jain","doi":"10.1146/annurev-physchem-090519-045502","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090519-045502","url":null,"abstract":"Because plasmonic metal nanostructures combine strong light absorption with catalytically active surfaces, they have become platforms for the light-assisted catalysis of chemical reactions. The enhancement of reaction rates by plasmonic excitation has been extensively discussed. This review focuses on a less discussed aspect: the induction of new reaction pathways by light excitation. Through commentary on seminal reports, we describe the principles behind the optical modulation of chemical reactivity and selectivity on plasmonic metal nanostructures. Central to these phenomena are excited charge carriers generated by plasmonic excitation, which modify the energy landscape available to surface reactive species and unlock pathways not conventionally available in thermal catalysis. Photogenerated carriers can trigger bond dissociation or desorption in an adsorbate-selective manner, drive charge transfer and multielectron redox reactions, and generate radical intermediates. Through one or more of these mechanisms, a specific pathway becomes favored under light. By improved control over these mechanisms, light-assisted catalysis can be transformational for chemical synthesis and energy conversion.","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"423-443"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38848220","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 23

Modeling Spin-Crossover Dynamics. 自旋交叉动力学建模。

IF 14.7 1区化学

Annual review of physical chemistry Pub Date : 2021-04-20 Epub Date: 2021-02-09 DOI: 10.1146/annurev-physchem-101419-012625

Saikat Mukherjee, Dmitry A Fedorov, Sergey A Varganov

引用次数: 15