657 results match your criteria Annual Review Of Physical Chemistry[Journal]


Excited-State Imaging of Single Particles on the Subnanometer Scale.

Annu Rev Phys Chem 2020 Apr;71:415-433

Department of Chemistry and Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.

At the intersection of spectroscopy and microscopy lie techniques that are capable of providing subnanometer imaging of excited states of individual molecules or nanoparticles. Such approaches are particularly important for imaging macromolecules or nanoparticles large enough to have a high probability of containing a defect. These inevitable defects often control properties and function despite an otherwise ideal structure. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-071119-040108DOI Listing

Accelerated Reaction Kinetics in Microdroplets: Overview and Recent Developments.

Annu Rev Phys Chem 2020 Apr;71:31-51

Department of Chemistry, Texas A&M University, College Station, Texas 77842, USA; email:

Various organic reactions, including important synthetic reactions involving C-C, C-N, and C-O bond formation as well as reactions of biomolecules, are accelerated when the reagents are present in sprayed or levitated microdroplets or in thin films. The reaction rates increase by orders of magnitude with decreasing droplet size or film thickness. The effect is associated with reactions at the solution-air interface. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-121319-110654DOI Listing

Low-Frequency Protein Motions Coupled to Catalytic Sites.

Annu Rev Phys Chem 2020 Apr;71:267-288

Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, USA; email:

This review examines low-frequency vibrational modes of proteins and their coupling to enzyme catalytic sites. That protein motions are critical to enzyme function is clear, but the kinds of motions present in proteins and how they are involved in function remain unclear. Several models of enzyme-catalyzed reaction suggest that protein dynamics may be involved in the chemical step of the catalyzed reaction, but the evidence in support of such models is indirect. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-014308DOI Listing

Biomolecular Phase Separation: From Molecular Driving Forces to Macroscopic Properties.

Annu Rev Phys Chem 2020 Apr;71:53-75

Department of Chemical and Biomolecular Engineering, Lehigh University, Bethlehem, Pennsylvania 18015, USA; email:

Biological phase separation is known to be important for cellular organization, which has recently been extended to a new class of biomolecules that form liquid-like droplets coexisting with the surrounding cellular or extracellular environment. These droplets are termed membraneless organelles, as they lack a dividing lipid membrane, and are formed through liquid-liquid phase separation (LLPS). Elucidating the molecular determinants of phase separation is a critical challenge for the field, as we are still at the early stages of understanding how cells may promote and regulate functions that are driven by LLPS. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-071819-113553DOI Listing

Nonstatistical Reaction Dynamics.

Annu Rev Phys Chem 2020 Apr;71:289-313

Department of Chemistry and Biochemistry, Texas Tech University, Lubbock, Texas 79409, USA; email:

Nonstatistical dynamics is important for many chemical reactions. The Rice-Ramsperger-Kassel-Marcus (RRKM) theory of unimolecular kinetics assumes a reactant molecule maintains a statistical microcanonical ensemble of vibrational states during its dissociation so that its unimolecular dynamics are time independent. Such dynamics results when the reactant's atomic motion is chaotic or irregular. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-112519-110208DOI Listing

Hydration Mimicry by Membrane Ion Channels.

Annu Rev Phys Chem 2020 Apr 9;71:461-484. Epub 2020 Mar 9.

Department of Computational Biology and Biophysics, Sandia National Laboratories, Albuquerque, New Mexico 87185, USA; email:

Ions transiting biomembranes might pass readily from water through ion-specific membrane proteins if these protein channels provide environments similar to the aqueous solution hydration environment. Indeed, bulk aqueous solution is an important reference condition for the ion permeation process. Assessment of this hydration mimicry concept depends on understanding the hydration structure and free energies of metal ions in water in order to provide a comparison for the membrane channel environment. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-012320-015457DOI Listing

Bose-Einstein Condensation of Exciton-Polaritons in Organic Microcavities.

Annu Rev Phys Chem 2020 Apr 3;71:435-459. Epub 2020 Mar 3.

Department of Engineering Physics, École Polytechnique de Montréal, Montréal H3T 1J4, Canada; email:

Bose-Einstein condensation describes the macroscopic occupation of a single-particle mode: the condensate. This state can in principle be realized for any particles obeying Bose-Einstein statistics; this includes hybrid light-matter excitations known as polaritons. Some of the unique optoelectronic properties of organic molecules make them especially well suited for the realization of polariton condensates. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-010920-102509DOI Listing

The Exploration of Chemical Reaction Networks.

Annu Rev Phys Chem 2020 Apr 19;71:121-142. Epub 2020 Feb 19.

Laboratory for Physical Chemistry, ETH Zurich, 8093 Zurich, Switzerland; email:

Modern computational chemistry has reached a stage at which massive exploration into chemical reaction space with unprecedented resolution with respect to the number of potentially relevant molecular structures has become possible. Various algorithmic advances have shown that such structural screenings must and can be automated and routinely carried out. This will replace the standard approach of manually studying a selected and restricted number of molecular structures for a chemical mechanism. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-071119-040123DOI Listing

Single-Molecule FRET of Intrinsically Disordered Proteins.

Annu Rev Phys Chem 2020 Apr 25;71:391-414. Epub 2020 Feb 25.

Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA; email:

Intrinsically disordered proteins (IDPs) are now widely recognized as playing critical roles in a broad range of cellular functions as well as being implicated in diverse diseases. Their lack of stable secondary structure and tertiary interactions, coupled with their sensitivity to measurement conditions, stymies many traditional structural biology approaches. Single-molecule Förster resonance energy transfer (smFRET) is now widely used to characterize the physicochemical properties of these proteins in isolation and is being increasingly applied to more complex assemblies and experimental environments. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-012420-104917DOI Listing

Machine Learning for Molecular Simulation.

Annu Rev Phys Chem 2020 Apr 24;71:361-390. Epub 2020 Feb 24.

Department of Mathematics and Computer Science, Freie Universität Berlin, 14195 Berlin, Germany; email:

Machine learning (ML) is transforming all areas of science. The complex and time-consuming calculations in molecular simulations are particularly suitable for an ML revolution and have already been profoundly affected by the application of existing ML methods. Here we review recent ML methods for molecular simulation, with particular focus on (deep) neural networks for the prediction of quantum-mechanical energies and forces, on coarse-grained molecular dynamics, on the extraction of free energy surfaces and kinetics, and on generative network approaches to sample molecular equilibrium structures and compute thermodynamics. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052331DOI Listing

Photoemission from Free Particles and Droplets.

Annu Rev Phys Chem 2020 Apr 19;71:315-334. Epub 2020 Feb 19.

Department of Chemistry and Applied Biosciences, ETH Zürich, 8093 Zürich, Switzerland; email:

Intriguing properties of photoemission from free, unsupported particles and droplets were predicted nearly 50 years ago, though experiments were a technical challenge. The last few decades have seen a surge of research in the field, due to advances in aerosol technology (generation, characterization, and transfer into vacuum), the development of photoelectron imaging spectrometers, and advances in vacuum ultraviolet and ultrafast light sources. Particles and droplets offer several advantages for photoemission studies. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-071719-022655DOI Listing

The Maximum Caliber Variational Principle for Nonequilibria.

Annu Rev Phys Chem 2020 Apr 19;71:213-238. Epub 2020 Feb 19.

Laufer Center for Physical and Quantitative Biology, Stony Brook University, Stony Brook, New York 11794, USA; email:

Ever since Clausius in 1865 and Boltzmann in 1877, the concepts of entropy and of its maximization have been the foundations for predicting how material equilibria derive from microscopic properties. But, despite much work, there has been no equally satisfactory general variational principle for nonequilibrium situations. However, in 1980, a new avenue was opened by E. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-071119-040206DOI Listing

Mapping Structural Dynamics of Proteins with Femtosecond Stimulated Raman Spectroscopy.

Annu Rev Phys Chem 2020 Apr 19;71:239-265. Epub 2020 Feb 19.

Department of Chemistry, Oregon State University, Corvallis, Oregon 97331, USA; email:

The structure-function relationships of biomolecules have captured the interest and imagination of the scientific community and general public since the field of structural biology emerged to enable the molecular understanding of life processes. Proteins that play numerous functional roles in cellular processes have remained in the forefront of research, inspiring new characterization techniques. In this review, we present key theoretical concepts and recent experimental strategies using femtosecond stimulated Raman spectroscopy (FSRS) to map the structural dynamics of proteins, highlighting the flexible chromophores on ultrafast timescales. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-071119-040154DOI Listing

High-Field Dynamic Nuclear Polarization.

Authors:
Björn Corzilius

Annu Rev Phys Chem 2020 Apr 19;71:143-170. Epub 2020 Feb 19.

Institute of Chemistry and Department of Life, Light and Matter, University of Rostock, 18059 Rostock, Germany; email:

Dynamic nuclear polarization (DNP) is one of the most prominent methods of sensitivity enhancement in nuclear magnetic resonance (NMR). Even though solid-state DNP under magic-angle spinning (MAS) has left the proof-of-concept phase and has become an important tool for structural investigations of biomolecules as well as materials, it is still far from mainstream applicability because of the potentially overwhelming combination of unique instrumentation, complex sample preparation, and a multitude of different mechanisms and methods available. In this review, I introduce the diverse field and history of DNP, combining aspects of NMR and electron paramagnetic resonance. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-071119-040222DOI Listing

Electron Transfer from Semiconductor Nanocrystals to Redox Enzymes.

Annu Rev Phys Chem 2020 Apr 25;71:335-359. Epub 2020 Feb 25.

Department of Chemistry, University of Colorado Boulder, Boulder, Colorado 80309, USA; email:

This review summarizes progress in understanding electron transfer from photoexcited nanocrystals to redox enzymes. The combination of the light-harvesting properties of nanocrystals and the catalytic properties of redox enzymes has emerged as a versatile platform to drive a variety of enzyme-catalyzed reactions with light. Transfer of a photoexcited charge from a nanocrystal to an enzyme is a critical first step for these reactions. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-014232DOI Listing

Molecular Simulations of Gram-Negative Bacterial Membranes Come of Age.

Annu Rev Phys Chem 2020 Apr 18;71:171-188. Epub 2020 Feb 18.

School of Chemistry, University of Southampton, Southampton S017 1BJ, United Kingdom; email:

Gram-negative bacteria are protected by a multicompartmental molecular architecture known as the cell envelope that contains two membranes and a thin cell wall. As the cell envelope controls influx and efflux of molecular species, in recent years both experimental and computational studies of such architectures have seen a resurgence due to the implications for antibiotic development. In this article we review recent progress in molecular simulations of bacterial membranes. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-103019-033434DOI Listing

Roaming Reactions and Dynamics in the van der Waals Region.

Authors:
Arthur G Suits

Annu Rev Phys Chem 2020 Apr 18;71:77-100. Epub 2020 Feb 18.

Department of Chemistry, University of Missouri, Columbia, Missouri 65211, USA; email:

Roaming reactions were first clearly identified in photodissociation of formaldehyde 15 years ago, and roaming dynamics are now recognized as a universal aspect of chemical reactivity. These reactions typically involve frustrated near-dissociation of a quasibound system to radical fragments, followed by reorientation at long range and intramolecular abstraction. The consequences can be unexpected formation of molecular products, depletion of the radical pool in chemical systems, and formation of products with unusual internal state distributions. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-020929DOI Listing

Benchmark Experimental Gas-Phase Intermolecular Dissociation Energies by the SEP-R2PI Method.

Annu Rev Phys Chem 2020 Apr 18;71:189-211. Epub 2020 Feb 18.

Department of Chemistry and Biochemistry, University of Bern, 3012 Bern, Switzerland; email:

The gas-phase ground-state dissociation energy () of an isolated and cold bimolecular complex is a fundamental measure of the intermolecular interaction strength between its constituents. Accurate values are important for the understanding of intermolecular bonding, for benchmarking high-level theoretical calculations, and for the parameterization of dispersion-corrected density functionals or force-field models that are used in fields ranging from crystallography to biochemistry. We review experimental measurements of the gas-phase () and () values of 55 different M⋅S complexes, where M is a (hetero)aromatic molecule and S is a closed-shell solvent atom or molecule. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-014224DOI Listing

Chromatosome Structure and Dynamics from Molecular Simulations.

Annu Rev Phys Chem 2020 Apr 4;71:101-119. Epub 2020 Feb 4.

Molecular and Cellular Modeling Group, Heidelberg Institute for Theoretical Studies (HITS), 69118 Heidelberg, Germany; email:

Chromatosomes are fundamental units of chromatin structure that are formed when a linker histone protein binds to a nucleosome. The positioning of the linker histone on the nucleosome influences the packing of chromatin. Recent simulations and experiments have shown that chromatosomes adopt an ensemble of structures that differ in the geometry of the linker histone-nucleosome interaction. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-071119-040043DOI Listing

Spatially Resolved Photogenerated Exciton and Charge Transport in Emerging Semiconductors.

Annu Rev Phys Chem 2020 Apr 22;71:1-30. Epub 2019 Nov 22.

Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA; email:

We review recent advances in the characterization of electronic forms of energy transport in emerging semiconductors. The approaches described all temporally and spatially resolve the evolution of initially localized populations of photogenerated excitons or charge carriers. We first provide a comprehensive background for describing the physical origin and nature of electronic energy transport both microscopically and from the perspective of the observer. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-052516-050703DOI Listing

Imaging Quantum Vortices in Superfluid Helium Droplets.

Annu Rev Phys Chem 2019 Jun;70:173-198

Department of Chemistry and Department of Physics and Astronomy, Unive rsity of Southern California , Los Angeles, California 90089, USA; email:

Free superfluid helium droplets constitute a versatile medium for a diverse range of experiments in physics and chemistry that extend from studies of the fundamental laws of superfluid motion to the synthesis of novel nanomaterials. In particular, the emergence of quantum vortices in rotating helium droplets is one of the most dramatic hallmarks of superfluidity and gives detailed access to the wave function describing the quantum liquid. This review provides an introduction to quantum vorticity in helium droplets, followed by a historical account of experiments on vortex visualization in bulk superfluid helium and a more detailed discussion of recent advances in the study of the rotational motion of isolated, nano- to micrometer-scale superfluid helium droplets. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052744DOI Listing
June 2019
11 Reads

Atmospheric Spectroscopy and Photochemistry at Environmental Water Interfaces.

Annu Rev Phys Chem 2019 Jun;70:45-69

Department of Chemistry, University of Nebraska, Lincoln, Nebraska 68566, USA.

The air-water interface is ubiquitous in nature, as manifested in the form of the surfaces of oceans, lakes, and atmospheric aerosols. The aerosol interface, in particular, can play a crucial role in atmospheric chemistry. The adsorption of atmospheric species onto and into aerosols modifies their concentrations and chemistries. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052311DOI Listing
June 2019
3 Reads

Triplet-Pair States in Organic Semiconductors.

Annu Rev Phys Chem 2019 Jun;70:323-351

Department of Physics and Astronomy, University of Sheffield, Sheffield S3 7RH, United Kingdom; email: ,

Entanglement of states is one of the most surprising and counterintuitive consequences of quantum mechanics, with potent applications in cryptography and computing. In organic semiconductor materials, one particularly significant manifestation is the spin-entangled triplet-pair state, which consists of a pair of localized triplet excitons coupled into an overall spin-0, -1, or -2 configuration. The most widely analyzed of these is the spin-0 pair, denoted (TT), which was initially invoked in the 1960s to explain delayed fluorescence in acene films. Read More

View Article

Download full-text PDF

Source
https://www.annualreviews.org/doi/10.1146/annurev-physchem-0
Publisher Site
http://dx.doi.org/10.1146/annurev-physchem-042018-052435DOI Listing
June 2019
2 Reads

Photochemistry of Organic Retinal Prostheses.

Annu Rev Phys Chem 2019 06;70:99-121

Center for Nano Science and Technology, Istituto Italiano di Tecnologia, 20133 Milan, Italy; email: ,

Organic devices are attracting considerable attention as prostheses for the recovery of retinal light sensitivity lost to retinal degenerative disease. The biotic/abiotic interface created when light-sensitive polymers and living tissues are placed in contact allows excitation of a response in blind laboratory rats exposed to visual stimuli. Although polymer retinal prostheses have proved to be efficient, their working mechanism is far from being fully understood. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052445DOI Listing
June 2019
19 Reads

Optical and Physical Probing of Thermal Processes in Semiconductor and Plasmonic Nanocrystals.

Annu Rev Phys Chem 2019 Jun 11;70:353-377. Epub 2019 Jan 11.

Center for Nanoscale Materials, Argonne National Laboratory, Lemont, Illinois 60439, USA; email:

This article reviews thermal properties of semiconductor and emergent plasmonic nanomaterials, focusing on mechanisms through which hot carriers and phonons are produced and dissipated as well as the related impacts on optoelectronic properties. Elevated equilibrium temperatures, of particular relevance for implementation of nanomaterials in devices, affect absorptive and radiative transitions as well as emission efficiency that can present reversible and irreversible changes with temperature. In noble metal or doped semiconductor/insulator nanomaterials, hot carriers and lattice heating can substantially influence localized surface plasmon resonances and yield large ultrafast changes in transmission or strongly oscillatory coherences. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052639DOI Listing
June 2019
1 Read

Chiral Plasmonic Nanostructures Enabled by Bottom-Up Approaches.

Annu Rev Phys Chem 2019 06 21;70:275-299. Epub 2019 May 21.

Max Planck Institute for Intelligent Systems, 70569 Stuttgart, Germany; email:

We present a comprehensive review of recent developments in the field of chiral plasmonics. Significant advances have been made recently in understanding the working principles of chiral plasmonic structures. With advances in micro- and nanofabrication techniques, a variety of chiral plasmonic nanostructures have been experimentally realized; these tailored chiroptical properties vastly outperform those of their molecular counterparts. Read More

View Article

Download full-text PDF

Source
https://www.annualreviews.org/doi/10.1146/annurev-physchem-0
Publisher Site
http://dx.doi.org/10.1146/annurev-physchem-050317-021332DOI Listing
June 2019
17 Reads

Interferometric Scattering Microscopy.

Annu Rev Phys Chem 2019 06 12;70:301-322. Epub 2019 Apr 12.

Physical and Theoretical Chemistry Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3QZ, United Kingdom; email: ,

Interferometric scattering microscopy (iSCAT) is an extremely sensitive imaging method based on the efficient detection of light scattered by nanoscopic objects. The ability to, at least in principle, maintain high imaging contrast independent of the exposure time or the scattering cross section of the object allows for unique applications in single-particle tracking, label-free imaging of nanoscopic (dis)assembly, and quantitative single-molecule characterization. We illustrate these capabilities in areas as diverse as mechanistic studies of motor protein function, viral capsid assembly, and single-molecule mass measurement in solution. Read More

View Article

Download full-text PDF

Source
https://www.annualreviews.org/doi/10.1146/annurev-physchem-0
Publisher Site
http://dx.doi.org/10.1146/annurev-physchem-050317-021247DOI Listing
June 2019
10 Reads

Multireference Theories of Electron Correlation Based on the Driven Similarity Renormalization Group.

Annu Rev Phys Chem 2019 Jun 20;70:245-273. Epub 2019 Mar 20.

Department of Chemistry and Cherry L. Emerson Center for Scientific Computation, Emory University, Atlanta, Georgia 30322, USA; emails: ,

The driven similarity renormalization group (DSRG) provides an alternative way to address the intruder state problem in quantum chemistry. In this review, we discuss recent developments of multireference methods based on the DSRG. We provide a pedagogical introduction to the DSRG and its various extensions and discuss its formal properties in great detail. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052416DOI Listing
June 2019
2 Reads

Ultrafast Dynamic Microscopy of Carrier and Exciton Transport.

Annu Rev Phys Chem 2019 Jun 18;70:219-244. Epub 2019 Mar 18.

Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, USA; email:

We highlight the recent progress in ultrafast dynamic microscopy that combines ultrafast optical spectroscopy with microscopy approaches, focusing on the application transient absorption microscopy (TAM) to directly image energy and charge transport in solar energy harvesting and conversion systems. We discuss the principles, instrumentation, and resolutions of TAM. The simultaneous spatial, temporal, and excited-state-specific resolutions of TAM unraveled exciton and charge transport mechanisms that were previously obscured in conventional ultrafast spectroscopy measurements for systems such as organic solar cells, hybrid perovskite thin films, and molecular aggregates. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052605DOI Listing
June 2019
1 Read

Microscopy and Cell Biology: New Methods and New Questions.

Annu Rev Phys Chem 2019 06 18;70:199-218. Epub 2019 Mar 18.

Department of Mechanical Engineering and Materials Science, Duke University, Durham, North Carolina 27708, USA; email:

Understanding the cellular basis of human health and disease requires the spatial resolution of microscopy and the molecular-level details provided by spectroscopy. This review highlights imaging methods at the intersection of microscopy and spectroscopy with applications in cell biology. Imaging methods are divided into three broad categories: fluorescence microscopy, label-free approaches, and imaging tools that can be applied to multiple imaging modalities. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052527DOI Listing
June 2019
1 Read

Kinetics of Drug Binding and Residence Time.

Annu Rev Phys Chem 2019 06 20;70:143-171. Epub 2019 Feb 20.

Department of Pharmacy and Biotechnology, University of Bologna, I-40126 Bologna, Italy.

The kinetics of drug binding and unbinding is assuming an increasingly crucial role in the long, costly process of bringing a new medicine to patients. For example, the time a drug spends in contact with its biological target is known as residence time (the inverse of the kinetic constant of the drug-target unbinding, 1/). Recent reports suggest that residence time could predict drug efficacy in vivo, perhaps even more effectively than conventional thermodynamic parameters (free energy, enthalpy, entropy). Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052340DOI Listing
June 2019
1 Read

Single Photon Sources in Atomically Thin Materials.

Annu Rev Phys Chem 2019 Jun 8;70:123-142. Epub 2019 Feb 8.

Institute of Biomedical Materials and Devices, University of Technology Sydney, Ultimo, New South Wales 2007, Australia; email: ,

Layered materials are very attractive for studies of light-matter interactions at the nanoscale. In particular, isolated quantum systems such as color centers and quantum dots embedded in these materials are gaining interest due to their potential use in a variety of quantum technologies and nanophotonics. Here, we review the field of nonclassical light emission from van der Waals crystals and atomically thin two-dimensional materials. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052628DOI Listing

Why Are DNA and Protein Electron Transfer So Different?

Authors:
David N Beratan

Annu Rev Phys Chem 2019 06 6;70:71-97. Epub 2019 Feb 6.

Department of Chemistry and Department of Physics, Duke University, Durham, North Carolina 27708, USA; email:

The corpus of electron transfer (ET) theory provides considerable power to describe the kinetics and dynamics of electron flow at the nanoscale. How is it, then, that nucleic acid (NA) ET continues to surprise, while protein-mediated ET is relatively free of mechanistic bombshells? I suggest that this difference originates in the distinct electronic energy landscapes for the two classes of reactions. In proteins, the donor/acceptor-to-bridge energy gap is typically several-fold larger than in NAs. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052353DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6591729PMC
June 2019
1 Read

Conical Intersections at the Nanoscale: Molecular Ideas for Materials.

Annu Rev Phys Chem 2019 Jun 11;70:21-43. Epub 2019 Jan 11.

Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, USA.

The ability to predict and describe nonradiative processes in molecules via the identification and characterization of conical intersections is one of the greatest recent successes of theoretical chemistry. Only recently, however, has this concept been extended to materials science, where nonradiative recombination limits the efficiencies of materials for various optoelectronic applications. In this review, we present recent advances in the theoretical study of conical intersections in semiconductor nanomaterials. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-042018-052425DOI Listing
June 2019
2 Reads

The Right Answer for the Right Reason: My Personal Goal for Quantum Chemistry.

Annu Rev Phys Chem 2019 06 2;70:1-20. Epub 2019 Jan 2.

Department of Chemistry, University of Washington, Seattle, Washington 98195, USA; email:

A brief history of quantum theory is given to illustrate the barriers to progress caused by preconceived ideas. The biases in my own thinking which I had to overcome to approach the right answer for the right reason are discussed. This is followed by a personal autobiography illustrating how I have led a life of serendipity with no real sense of purpose. Read More

View Article

Download full-text PDF

Source
https://www.annualreviews.org/doi/10.1146/annurev-physchem-0
Publisher Site
http://dx.doi.org/10.1146/annurev-physchem-042018-052300DOI Listing
June 2019
4 Reads

Exploring Energy Landscapes.

Authors:
David J Wales

Annu Rev Phys Chem 2018 04;69:401-425

Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, United Kingdom; email:

Recent advances in the potential energy landscapes approach are highlighted, including both theoretical and computational contributions. Treating the high dimensionality of molecular and condensed matter systems of contemporary interest is important for understanding how emergent properties are encoded in the landscape and for calculating these properties while faithfully representing barriers between different morphologies. The pathways characterized in full dimensionality, which are used to construct kinetic transition networks, may prove useful in guiding such calculations. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-021219DOI Listing
April 2018
2 Reads

Vibrational and Nonadiabatic Coherence in 2D Electronic Spectroscopy, the Jahn-Teller Effect, and Energy Transfer.

Authors:
David M Jonas

Annu Rev Phys Chem 2018 04;69:327-352

Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado 80309-0215, USA; email:

Femtosecond two-dimensional (2D) Fourier transform spectroscopy generates and probes several types of coherence that characterize the couplings between vibrational and electronic motions. These couplings have been studied in molecules with Jahn-Teller conical intersections, pseudo-Jahn-Teller funnels, dimers, molecular aggregates, photosynthetic light harvesting complexes, and photosynthetic reaction centers. All have closely related Hamiltonians and at least two types of vibrations, including one that is decoupled from the electronic dynamics and one that is nonadiabatically coupled. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-052516-050602DOI Listing
April 2018
1 Read

Measuring Electric Fields in Biological Matter Using the Vibrational Stark Effect of Nitrile Probes.

Annu Rev Phys Chem 2018 04;69:253-271

Department of Chemistry, University of Texas at Austin, Austin, Texas 78712-1224, USA; email:

Measurement of the electrostatic interactions that give rise to biological functions has been a longstanding challenge in biophysics. Advances in spectroscopic techniques over the past two decades have allowed for the direct measurement of electric fields in a wide variety of biological molecules and systems via the vibrational Stark effect (VSE). The frequency of the nitrile stretching oscillation has received much attention as an electric field reporter because of its sensitivity to electric fields and its occurrence in a relatively transparent region of the infrared spectrum. Read More

View Article

Download full-text PDF

Source
http://www.annualreviews.org/doi/10.1146/annurev-physchem-05
Publisher Site
http://dx.doi.org/10.1146/annurev-physchem-052516-045011DOI Listing
April 2018
3 Reads

Elementary Chemical Reactions in Surface Photocatalysis.

Annu Rev Phys Chem 2018 04 28;69:451-472. Epub 2018 Feb 28.

State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Dalian 116023, Liaoning, China; email: , , , , ,

Photocatalytic hydrogen evolution and organic degradation on oxide materials have been extensively investigated in the last two decades. Great efforts have been dedicated to the study of photocatalytic reaction mechanisms of a variety of molecules on TiO surfaces by using surface science methods under ultra-high vacuum (UHV) conditions, providing fundamental understanding of surface chemical reactions in photocatalysis. In this review, we summarize the recent progress in the study of photocatalysis of several important species (water, methanol, and aldehydes) on different TiO surfaces. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-052516-044933DOI Listing
April 2018
38 Reads

Characterization of Intermediate Oxidation States in CO Activation.

Annu Rev Phys Chem 2018 04 28;69:231-252. Epub 2018 Feb 28.

JILA and Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado 80309-0440, USA; email: ,

Redox chemistry during the activation of carbon dioxide involves changing the charge state in a CO molecular unit. However, such changes are usually not well described by integer formal charges, and one can think of COO functional units as being in intermediate oxidation states. In this article, we discuss the properties of CO and CO-based functional units in various charge states. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-021122DOI Listing
April 2018
12 Reads

Addressing the Challenge of Molecular Change: An Interim Report.

Authors:
Raphael D Levine

Annu Rev Phys Chem 2018 04 28;69:1-21. Epub 2018 Feb 28.

The Fritz Haber Research Center for Molecular Dynamics, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904, Israel; email:

Invited by the editorial committee of the Annual Review of Physical Chemistry to "contribute my autobiography," I present it here, as I understand the term. It is about my parents, my mentors, my coworkers, and my friends in learning and the scientific problems that we tried to address. Courtesy of the editorial assistance of Annual Reviews, some of the science is in the figure captions and sidebars. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-102717-010036DOI Listing
April 2018
1 Read

Sensing Chirality with Rotational Spectroscopy.

Annu Rev Phys Chem 2018 04 28;69:499-519. Epub 2018 Feb 28.

Deutsches Elektronen-Synchrotron, 22607 Hamburg, Germany.

Chiroptical spectroscopy techniques for the differentiation of enantiomers in the condensed phase are based on an established paradigm that relies on symmetry breaking using circularly polarized light. We review a novel approach for the study of chiral molecules in the gas phase using broadband rotational spectroscopy, namely microwave three-wave mixing, which is a coherent, nonlinear, and resonant process. This technique can be used to generate a coherent molecular rotational signal that can be detected in a manner similar to that in conventional Fourier transform microwave spectroscopy. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-052516-050629DOI Listing
April 2018
4 Reads

Enhancing Analytical Separations Using Super-Resolution Microscopy.

Annu Rev Phys Chem 2018 04 28;69:353-375. Epub 2018 Feb 28.

Department of Chemistry, Rice University, Houston, Texas 77251, USA; email:

Super-resolution microscopy is becoming an invaluable tool to investigate structure and dynamics driving protein interactions at interfaces. In this review, we highlight the applications of super-resolution microscopy for quantifying the physics and chemistry that occur between target proteins and stationary-phase supports during chromatographic separations. Our discussion concentrates on the newfound ability of super-resolved single-protein spectroscopy to inform theoretical parameters via quantification of adsorption-desorption dynamics, protein unfolding, and nanoconfined transport. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-052516-045018DOI Listing
April 2018
2 Reads

Computational Design of Clusters for Catalysis.

Annu Rev Phys Chem 2018 04 28;69:377-400. Epub 2018 Feb 28.

Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA; email:

When small clusters are studied in chemical physics or physical chemistry, one perhaps thinks of the fundamental aspects of cluster electronic structure, or precision spectroscopy in ultracold molecular beams. However, small clusters are also of interest in catalysis, where the cold ground state or an isolated cluster may not even be the right starting point. Instead, the big question is: What happens to cluster-based catalysts under real conditions of catalysis, such as high temperature and coverage with reagents? Myriads of metastable cluster states become accessible, the entire system is dynamic, and catalysis may be driven by rare sites present only under those conditions. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-014216DOI Listing
April 2018
3 Reads

Membrane-Mediated Cooperativity of Proteins.

Authors:
Thomas R Weikl

Annu Rev Phys Chem 2018 04 28;69:521-539. Epub 2018 Feb 28.

Department of Theory and Bio-Systems, Max Planck Institute of Colloids and Interfaces, 14424 Potsdam, Germany; email:

Besides direct protein-protein interactions, indirect interactions mediated by membranes play an important role for the assembly and cooperative function of proteins in membrane shaping and adhesion. The intricate shapes of biological membranes are generated by proteins that locally induce membrane curvature. Indirect curvature-mediated interactions between these proteins arise because the proteins jointly affect the bending energy of the membranes. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-052516-050637DOI Listing
April 2018
1 Read

Connections Between Theory and Experiment for Gold and Silver Nanoclusters.

Annu Rev Phys Chem 2018 04 28;69:205-229. Epub 2018 Feb 28.

Department of Chemistry, Kansas State University, Manhattan, Kansas 66506, USA; email:

Ligand-stabilized gold and silver nanoparticles are of tremendous current interest in sensing, catalysis, and energy applications. Experimental and theoretical studies have closely interacted to elucidate properties such as the geometric and electronic structures of these fascinating systems. In this review, the interplay between theory and experiment is described; areas such as optical absorption and doping, where the theory-experiment connections are well established, are discussed in detail; and the current status of these connections in newer fields of study, such as luminescence, transient absorption, and the effects of solvent and the surrounding environment, are highlighted. Read More

View Article

Download full-text PDF

Source
http://www.annualreviews.org/doi/10.1146/annurev-physchem-05
Publisher Site
http://dx.doi.org/10.1146/annurev-physchem-052516-050932DOI Listing
April 2018
13 Reads

Computational Photophysics in the Presence of an Environment.

Annu Rev Phys Chem 2018 04 28;69:473-497. Epub 2018 Feb 28.

Institute of Theoretical Chemistry, Faculty of Chemistry, University of Vienna, A-1090 Wien, Austria; email: ,

Most processes triggered by ultraviolet (UV) or visible (vis) light in nature take place in complex biological environments. The first step in these photophysical events is the excitation of the absorbing system or chromophore to an electronically excited state. Such an excitation can be monitored by the UV-vis absorption spectrum. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-021013DOI Listing
April 2018
3 Reads

Chemical Kinetics for Bridging Molecular Mechanisms and Macroscopic Measurements of Amyloid Fibril Formation.

Annu Rev Phys Chem 2018 04 28;69:273-298. Epub 2018 Feb 28.

Centre for Misfolding Diseases, Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, United Kingdom; email:

Understanding how normally soluble peptides and proteins aggregate to form amyloid fibrils is central to many areas of modern biomolecular science, ranging from the development of functional biomaterials to the design of rational therapeutic strategies against increasingly prevalent medical conditions such as Alzheimer's and Parkinson's diseases. As such, there is a great need to develop models to mechanistically describe how amyloid fibrils are formed from precursor peptides and proteins. Here we review and discuss how ideas and concepts from chemical reaction kinetics can help to achieve this objective. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-021322DOI Listing
April 2018
36 Reads

Dynamics at Conical Intersections.

Annu Rev Phys Chem 2018 04 28;69:427-450. Epub 2018 Feb 28.

National Research Council of Canada, Ottawa, Ontario K1A 06A, Canada; email:

The nonadiabatic coupling of electronic and vibrational degrees of freedom is the defining feature of electronically excited states of polyatomic molecules. Once considered a theoretical curiosity, conical intersections (CIs) are now generally accepted as being the dominant source of coupled charge and vibrational energy flow in molecular excited states. Passage through CIs leads to the conversion of electronic to vibrational energy, which drives the ensuing photochemistry, isomerization being a canonical example. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-052516-050721DOI Listing
April 2018
6 Reads

Electronic Transport in Two-Dimensional Materials.

Annu Rev Phys Chem 2018 04 20;69:299-325. Epub 2018 Feb 20.

Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA; email:

Two-dimensional (2D) materials have captured the attention of the scientific community due to the wide range of unique properties at nanometer-scale thicknesses. While significant exploratory research in 2D materials has been achieved, the understanding of 2D electronic transport and carrier dynamics remains in a nascent stage. Furthermore, because prior review articles have provided general overviews of 2D materials or specifically focused on charge transport in graphene, here we instead highlight charge transport mechanisms in post-graphene 2D materials, with particular emphasis on transition metal dichalcogenides and black phosphorus. Read More

View Article

Download full-text PDF

Source
http://dx.doi.org/10.1146/annurev-physchem-050317-021353DOI Listing
April 2018
1 Read