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Annual review of physical chemistry最新文献

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Generating Superrotors and Dynamics of Molecules in Extremely High Rotational States.
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-14 DOI: 10.1146/annurev-physchem-082423-012311
Amy S Mullin
{"title":"Generating Superrotors and Dynamics of Molecules in Extremely High Rotational States.","authors":"Amy S Mullin","doi":"10.1146/annurev-physchem-082423-012311","DOIUrl":"https://doi.org/10.1146/annurev-physchem-082423-012311","url":null,"abstract":"<p><p>The optical centrifuge was demonstrated in 2000 as a tool for preparing ensembles of molecules in extreme rotational states. Highly rotationally excited molecules, so-called superrotors, are observed as products of photodissociation and molecular collisions, in high-temperature environments in the atmospheres of Earth and exoplanets, and in the interstellar medium. Traditional optical excitation is limited to small changes in rotation, limiting experiments to relatively low rotational states. In this review, I discuss the use of a tunable optical centrifuge to prepare molecules in selected ranges of excited rotational states and investigations of their collisional relaxation using state-resolved polarization-sensitive transient IR probing. I examine the decay dynamics of population, alignment, and translational energy release, focusing on experimental results, and compare them with simulations that overestimate observed relaxation rates. A clear picture of near-resonant and nonresonant energy transfer pathways emerges and establishes the means to distinguish superrotor and bath collision products.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424600","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: 0
Memory and Friction: From the Nanoscale to the Macroscale.
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-14 DOI: 10.1146/annurev-physchem-082423-031037
Benjamin A Dalton, Anton Klimek, Henrik Kiefer, Florian N Brünig, Hélène Colinet, Lucas Tepper, Amir Abbasi, Roland R Netz
{"title":"Memory and Friction: From the Nanoscale to the Macroscale.","authors":"Benjamin A Dalton, Anton Klimek, Henrik Kiefer, Florian N Brünig, Hélène Colinet, Lucas Tepper, Amir Abbasi, Roland R Netz","doi":"10.1146/annurev-physchem-082423-031037","DOIUrl":"https://doi.org/10.1146/annurev-physchem-082423-031037","url":null,"abstract":"<p><p>Friction is a phenomenon that manifests across all spatial and temporal scales, from the molecular to the macroscopic scale. It describes the dissipation of energy from the motion of particles or abstract reaction coordinates and arises in the transition from a detailed molecular-level description to a simplified, coarse-grained model. It has long been understood that time-dependent (non-Markovian) friction effects are critical for describing the dynamics of many systems, but that they are notoriously difficult to evaluate for complex physical, chemical, and biological systems. In recent years, the development of advanced numerical friction extraction techniques and methods to simulate the generalized Langevin equation has enabled exploration of the role of time-dependent friction across all scales. We discuss recent applications of these friction extraction techniques and the growing understanding of the role of friction in complex equilibrium and nonequilibrium dynamic many-body systems.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424605","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: 0
Femtosecond Extreme Ultraviolet Absorption Spectroscopy of Transition Metal Complexes.
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-14 DOI: 10.1146/annurev-physchem-082720-031657
Josh Vura-Weis
{"title":"Femtosecond Extreme Ultraviolet Absorption Spectroscopy of Transition Metal Complexes.","authors":"Josh Vura-Weis","doi":"10.1146/annurev-physchem-082720-031657","DOIUrl":"https://doi.org/10.1146/annurev-physchem-082720-031657","url":null,"abstract":"<p><p>In this review, we survey the use of extreme ultraviolet absorption spectroscopy to measure electronic and vibrational dynamics in transition metal complexes. Photons in this 30-100 eV energy range probe 3<i>p</i>$mbox{MVRightarrow}$ 3<i>d</i> transitions for 3<i>d</i> metals and 4<i>f</i>, 5<i>p</i>$mbox{MVRightarrow}$ 5<i>d</i> transitions in 5<i>d</i> metals, and the resulting spectra are sensitive to the spin state, oxidation state, and ligand field of the metal. Furthermore, the energy of the core level depends on the metal, providing elemental specificity. Use of tabletop high-harmonic sources allows these spectra to be measured with femtosecond to attosecond time resolution in a standard laser laboratory, revealing short-lived states in chromophores and photocatalysts that were unresolved using other techniques.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424583","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: 0
Flow of Energy and Information in Molecular Machines.
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-14 DOI: 10.1146/annurev-physchem-082423-030023
Matthew P Leighton, David A Sivak
{"title":"Flow of Energy and Information in Molecular Machines.","authors":"Matthew P Leighton, David A Sivak","doi":"10.1146/annurev-physchem-082423-030023","DOIUrl":"https://doi.org/10.1146/annurev-physchem-082423-030023","url":null,"abstract":"<p><p>Molecular machines transduce free energy between different forms throughout all living organisms. Unlike their macroscopic counterparts, molecular machines are characterized by stochastic fluctuations, overdamped dynamics, and soft components, and operate far from thermodynamic equilibrium. In addition, information is a relevant free energy resource for molecular machines, leading to new modes of operation for nanoscale engines. Toward the objective of engineering synthetic nanomachines, an important goal is to understand how molecular machines transduce free energy to perform their functions in biological systems. In this review, we discuss the nonequilibrium thermodynamics of free energy transduction within molecular machines, with a focus on quantifying energy and information flows between their components. We review results from theory, modeling, and inference from experiments that shed light on the internal thermodynamics of molecular machines, and ultimately explore what we can learn from considering these interactions.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424517","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: 0
Physical Considerations in Memory and Information Storage.
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-14 DOI: 10.1146/annurev-physchem-083122-010308
Matthew Du, Agnish Kumar Behera, Suriyanarayanan Vaikuntanathan
{"title":"Physical Considerations in Memory and Information Storage.","authors":"Matthew Du, Agnish Kumar Behera, Suriyanarayanan Vaikuntanathan","doi":"10.1146/annurev-physchem-083122-010308","DOIUrl":"https://doi.org/10.1146/annurev-physchem-083122-010308","url":null,"abstract":"<p><p>Information is an important resource. Storing and retrieving information faithfully are huge challenges and many methods have been developed to understand the principles behind robust information processing. In this review, we focus on information storage and retrieval from the perspective of energetics, dynamics, and statistical mechanics. We first review the Hopfield model of associative memory, the classic energy-based model of memory. We then discuss generalizations and physical realizations of the Hopfield model. Finally, we highlight connections to energy-based neural networks used in deep learning. We hope this review inspires new directions along the lines of information storage and retrieval in physical systems.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424531","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: 0
Chirality-Induced Spin Selectivity in Hybrid Organic-Inorganic Perovskite Semiconductors.
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-14 DOI: 10.1146/annurev-physchem-082423-032933
Yifan Dong, Matthew P Hautzinger, Md Azimul Haque, Matthew C Beard
{"title":"Chirality-Induced Spin Selectivity in Hybrid Organic-Inorganic Perovskite Semiconductors.","authors":"Yifan Dong, Matthew P Hautzinger, Md Azimul Haque, Matthew C Beard","doi":"10.1146/annurev-physchem-082423-032933","DOIUrl":"https://doi.org/10.1146/annurev-physchem-082423-032933","url":null,"abstract":"<p><p>The movement of charges through a chiral medium results in a spin-polarized charge current. This phenomenon, known as the chirality-induced spin selectivity (CISS) effect, enables control over spin populations without the need for magnetic components and operates at room temperature. CISS has been discovered in a range of chiral media and most prominently studied in chiral organic molecular species. Chiral hybrid organic-inorganic perovskite semiconductors combine the unique and functional aspects of inorganic semiconductors with chiral molecules. The inorganic component borrows the homochirality of the organic component to yield a unique family of highly tunable chiral semiconductors, where the enantiomeric purity is defined by the organic component. Semiconductors already form the backbone of modern-day technologies. Adding chirality and control over spin through CISS provides new avenues for creative technological development. This review is intended to be an introduction to these unique systems and the demonstrations of CISS and spin control.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424574","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: 0
Structure-Photophysical Property Relationships in Noncanonical and Synthetic Nucleobases.
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-14 DOI: 10.1146/annurev-physchem-082423-022427
Sean J Hoehn, Sarah E Krul, Sourav Kanti Seth, Carlos E Crespo-Hernández
{"title":"Structure-Photophysical Property Relationships in Noncanonical and Synthetic Nucleobases.","authors":"Sean J Hoehn, Sarah E Krul, Sourav Kanti Seth, Carlos E Crespo-Hernández","doi":"10.1146/annurev-physchem-082423-022427","DOIUrl":"https://doi.org/10.1146/annurev-physchem-082423-022427","url":null,"abstract":"<p><p>This review provides a focused coverage of the photophysical properties of noncanonical and synthetic nucleobases reported over the past decade. It emphasizes key research findings and physical insights gathered for prebiotic and fluorescent nucleobase analogs, sulfur- and selenium-substituted nucleobases, aza-substituted nucleobases, epigenetic nucleobases and their oxidation products, and nucleobases utilized for expanding DNA/RNA to reveal central structure-photophysical property relationships. Further research and development in this emerging field, coupled with machine learning methods, will enable the effective harnessing of nucleobases' modifications for applications in biotechnology, biomedicine, therapeutics, and even the creation of live semisynthetic organisms.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424553","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: 0
Emerging Mechanisms of Metal-Catalyzed RNA and DNA Modifications.
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-14 DOI: 10.1146/annurev-physchem-082423-030241
Mohd Ahsan, Chinmai Pindi, Giulia Palermo
{"title":"Emerging Mechanisms of Metal-Catalyzed RNA and DNA Modifications.","authors":"Mohd Ahsan, Chinmai Pindi, Giulia Palermo","doi":"10.1146/annurev-physchem-082423-030241","DOIUrl":"https://doi.org/10.1146/annurev-physchem-082423-030241","url":null,"abstract":"<p><p>Metal ions play a critical role in various chemical, biological, and environmental processes. This review reports on emerging chemical mechanisms in the catalysis of DNA and RNA. We provide an overview of the metal-dependent mechanisms of DNA cleavage in CRISPR (clustered regularly interspaced short palindromic repeats)-Cas systems that are transforming life sciences through genome editing technologies, and showcase intriguing metal-dependent mechanisms of RNA cleavages. We show that newly discovered CRISPR-Cas complexes operate as protein-assisted ribozymes, highlighting RNA's versatility and the enhancement of CRISPR-Cas functions through strategic metal ion use. We demonstrate the power of computer simulations in observing chemical processes as they unfold and in advancing structural biology through innovative approaches for refining cryo-electron microscopy maps. Understanding metal ion involvement in nucleic acid catalysis is crucial for advancing genome editing, aiding therapeutic interventions for genetic disorders, and improving the editing tools' specificity and efficiency.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424579","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: 0
Quantum State-Resolved Structure and Dynamics of C60 Fullerenes. 量子态分辨的 C60 富勒烯结构与动力学。
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-04 DOI: 10.1146/annurev-physchem-082423-013137
Lee R Liu, Jun Ye
{"title":"Quantum State-Resolved Structure and Dynamics of C<sub>60</sub> Fullerenes.","authors":"Lee R Liu, Jun Ye","doi":"10.1146/annurev-physchem-082423-013137","DOIUrl":"https://doi.org/10.1146/annurev-physchem-082423-013137","url":null,"abstract":"<p><p>The C<sub>60</sub> fullerene molecule has been the subject of intense study for four decades, starting with its identification in the mass spectra of carbon soot in 1985. In this review, we focus on the achievement of ultra-high-resolution spectroscopy of gas phase neutral C<sub>60</sub>, heralded by the observation of quantum state-resolved infrared spectra in 2019. C<sub>60</sub> is now the largest and most symmetric molecule for which rovibrational quantum state resolution has been achieved, motivating the use of large molecules for studying complex quantum systems with symmetries and degrees of freedom not readily available in other composite systems. We discuss the theory, challenges, and experimental techniques of high-resolution C<sub>60</sub> spectroscopy and recent experimental results probing the structure, dynamics, and interactions of C<sub>60</sub> enabled by quantum state resolution.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143188073","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: 0
Reaction Coordinates Are Optimal Channels of Energy Flow.
IF 11.7 1区 化学
Annual review of physical chemistry Pub Date : 2025-02-04 DOI: 10.1146/annurev-physchem-082423-010652
Ao Ma, Huiyu Li
{"title":"Reaction Coordinates Are Optimal Channels of Energy Flow.","authors":"Ao Ma, Huiyu Li","doi":"10.1146/annurev-physchem-082423-010652","DOIUrl":"https://doi.org/10.1146/annurev-physchem-082423-010652","url":null,"abstract":"<p><p>Reaction coordinates (RCs) are the few essential coordinates of a protein that control its functional processes, such as allostery, enzymatic reaction, and conformational change. They are critical for understanding protein function and provide optimal enhanced sampling of protein conformational changes and states. Since the pioneering work in the late 1990s, identifying the correct and objectively provable RCs has been a central topic in molecular biophysics and chemical physics. This review summarizes the major advances in identifying RCs over the past 25 years, focusing on methods aimed at finding RCs that meet the rigorous committor criterion, widely accepted as the true RCs. Importantly, the newly developed physics-based energy flow theory and generalized work functional method provide a general and rigorous approach for identifying true RCs, revealing their physical nature as the optimal channels of energy flow in biomolecules.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":" ","pages":""},"PeriodicalIF":11.7,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143188088","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: 0
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