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Understanding Organic Photovoltaic Materials Using Simple Thermal Analysis Methodologies Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-03-01 Aditi Khirbat, Oded Nahor, Sara Marina Barbier, Artem Levitsky, Jaime Martín, Gitti Frey, Natalie Stingelin
Large strides have been made in designing an ever-increasing set of modern organic materials of high functionality and thus, often, of high complexity, including semiconducting polymers, organic ferroelectrics, light-emitting small molecules, and beyond. Here, we review how broadly applied thermal analysis methodologies, especially differential scanning calorimetry, can be utilized to provide unique
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Photon Upconversion at Organic-Inorganic Interfaces Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-22 Zhiyuan Huang, Tsumugi Miyashita, Ming Lee Tang
Photon upconversion is a process that combines low-energy photons to form useful high-energy photons. There are potential applications in photovoltaics, photocatalysis, biological imaging, etc. Semiconductor quantum dots (QDs) are promising for the absorption of these low-energy photons due to the high extinction coefficient of QDs, especially in the near infrared (NIR). This allows the intriguing
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Phase Transitions in Organic and Organic/Inorganic Aerosol Particles Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-22 Miriam Arak Freedman, Qishen Huang, Kiran R. Pitta
The phase state of aerosol particles can impact numerous atmospheric processes, including new particle growth, heterogeneous chemistry, cloud condensation nucleus formation, and ice nucleation. In this article, the phase transitions of inorganic, organic, and organic/inorganic aerosol particles are discussed, with particular focus on liquid-liquid phase separation (LLPS). The physical chemistry that
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Enhanced Sampling with Machine Learning Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-22 Shams Mehdi, Zachary Smith, Lukas Herron, Ziyue Zou, Pratyush Tiwary
Molecular dynamics (MD) enables the study of physical systems with excellent spatiotemporal resolution but suffers from severe timescale limitations. To address this, enhanced sampling methods have been developed to improve the exploration of configurational space. However, implementing these methods is challenging and requires domain expertise. In recent years, integration of machine learning (ML)
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Oxygenic Photosynthesis in Far-Red Light: Strategies and Mechanisms Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-22 Eduard Elias, Thomas J. Oliver, Roberta Croce
Oxygenic photosynthesis, the process that converts light energy into chemical energy, is traditionally associated with the absorption of visible light by chlorophyll molecules. However, recent studies have revealed a growing number of organisms capable of using far-red light (700–800 nm) to drive oxygenic photosynthesis. This phenomenon challenges the conventional understanding of the limits of this
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Prebiotic Astrochemistry from Astronomical Observations and Laboratory Spectroscopy Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-22 Lucy M. Ziurys
The discovery of more than 200 gas-phase chemical compounds in interstellar space has led to the speculation that this nonterrestrial synthesis may play a role in the origin of life. These identifications were possible because of laboratory spectroscopy, which provides the molecular fingerprints for astronomical observations. Interstellar chemistry produces a wide range of small, organic molecules
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Lipid Landscapes: Vibrational Spectroscopy for Decoding Membrane Complexity Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-22 Xiaobing Chen, Ziareena A. Al-Mualem, Carlos R. Baiz
Cell membranes are incredibly complex environments containing hundreds of components. Despite substantial advances in the past decade, fundamental questions related to lipid-lipid interactions and heterogeneity persist. This review explores the complexity of lipid membranes, showcasing recent advances in vibrational spectroscopy to characterize the structure, dynamics, and interactions at the membrane
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Single-Macromolecule Studies of Eukaryotic Genomic Maintenance Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-22 Sergei Rudnizky, Peter J. Murray, Clara H. Wolfe, Taekjip Ha
Genomes are self-organized and self-maintained as long, complex macromolecules of chromatin. The inherent heterogeneity, stochasticity, phase separation, and chromatin dynamics of genome operation make it challenging to study genomes using ensemble methods. Various single-molecule force-, fluorescent-, and sequencing-based techniques rooted in different disciplines have been developed to fill critical
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Chemical Kinetics in Microdroplets Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-22 Kevin R. Wilson, Alexander M. Prophet
Micrometer-sized compartments play significant roles in driving heterogeneous transformations within atmospheric and biochemical systems as well as providing vehicles for drug delivery and novel reaction environments for the synthesis of industrial chemicals. Many reports now indicate that reaction kinetics are accelerated under microconfinement, for example, in sprays, thin films, droplets, aerosols
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Single-Molecule Spectroscopy and Super-Resolution Mapping of Physicochemical Parameters in Living Cells Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-16 Megan A. Steves, Changdong He, Ke Xu
By superlocalizing the positions of millions of single molecules over many camera frames, a class of super-resolution fluorescence microscopy methods known as single-molecule localization microscopy (SMLM) has revolutionized how we understand subcellular structures over the past decade. In this review, we highlight emerging studies that transcend the outstanding structural (shape) information offered
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Molecular Insights into Chemical Reactions at Aqueous Aerosol Interfaces Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-02-16 David T. Limmer, Andreas W. Götz, Timothy H. Bertram, Gilbert M. Nathanson
Atmospheric aerosols facilitate reactions between ambient gases and dissolved species. Here, we review our efforts to interrogate the uptake of these gases and the mechanisms of their reactions both theoretically and experimentally. We highlight the fascinating behavior of N2O5 in solutions ranging from pure water to complex mixtures, chosen because its aerosol-mediated reactions significantly impact
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Dynamics of Anions: From Bound to Unbound States and Everything In Between Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-01-26 Connor J. Clarke, Jan R.R. Verlet
Gas-phase anions present an ideal playground for the exploration of excited-state dynamics. They offer control in terms of the mass, extent of solvation, internal temperature, and conformation. The application of a range of ion sources has opened the field to a vast array of anionic systems whose dynamics are important in areas ranging from biology to star formation. Here, we review recent experimental
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Aqueous Titania Interfaces Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2024-01-25 Annabella Selloni
Water–metal oxide interfaces are central to many phenomena and applications, ranging from material corrosion and dissolution to photoelectrochemistry and bioengineering. In particular, the discovery of photocatalytic water splitting on TiO2 has motivated intensive studies of water-TiO2 interfaces for decades. So far, a broad understanding of the interaction of water vapor with several TiO2 surfaces
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Reinvented: An Attosecond Chemist Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-11-28 Stephen R. Leone
Attosecond science requires a substantial rethinking of how to make measurements on very short timescales; how to acquire the necessary equipment, technology, and personnel; and how to build a set of laboratories for such experiments. This entails a rejuvenation of the author in many respects, in the laboratory itself, with regard to students and postdocs, and in generating funding for research. It
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Many-Body Effects in Aqueous Systems: Synergies Between Interaction Analysis Techniques and Force Field Development Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-04-24 Joseph P. Heindel, Kristina M. Herman, Sotiris S. Xantheas
Interaction analysis techniques, including the many-body expansion (MBE), symmetry-adapted perturbation theory, and energy decomposition analysis, allow for an intuitive understanding of complex molecular interactions. We review these methods by first providing a historical context for the study of many-body interactions and discussing how nonadditivities emerge from Hamiltonians containing strictly
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Ultrafast X-Ray Probes of Elementary Molecular Events Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-04-24 Daniel Keefer, Stefano M. Cavaletto, Jérémy R. Rouxel, Marco Garavelli, Haiwang Yong, Shaul Mukamel
Elementary events that determine photochemical outcomes and molecular functionalities happen on the femtosecond and subfemtosecond timescales. Among the most ubiquitous events are the nonadiabatic dynamics taking place at conical intersections. These facilitate ultrafast, nonradiative transitions between electronic states in molecules that can outcompete slower relaxation mechanisms such as fluorescence
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Photodarkening, Photobrightening, and the Role of Color Centers in Emerging Applications of Lanthanide-Based Upconverting Nanomaterials Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-04-24 Changhwan Lee, P. James Schuck
Upconverting nanoparticles (UCNPs) compose a class of luminescent materials that utilize the unique wavelength-converting properties of lanthanide (Ln) ions for light-harvesting applications, photonics technologies, and biological imaging and sensing experiments. Recent advances in UCNP design have shed light on the properties of local color centers, both intrinsic and controllably induced, within
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In Situ Measurement of Evolving Excited-State Dynamics During Deposition and Processing of Organic Films by Single-Shot Transient Absorption Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-28 Zachary S. Walbrun, Cathy Y. Wong
A significant advantage of organic semiconductors over many of their inorganic counterparts is solution processability. However, solution processing commonly yields heterogeneous films with properties that are highly sensitive to the conditions and parameters of casting and processing. Measuring the key properties of these materials in situ, during film production, can provide new insight into the
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The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-28 Hao Li, S.A. Shah, Ajay Ram Srimath Kandada, Carlos Silva, Andrei Piryatinski, Eric R. Bittner
We review our recent quantum stochastic model for spectroscopic lineshapes in the presence of a coevolving and nonstationary background population of excitations. Starting from a field theory description for interacting bosonic excitons, we derive a reduced model whereby optical excitons are coupled to an incoherent background via scattering as mediated by their screened Coulomb coupling. The Heisenberg
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Isotope Effects and the Atmosphere Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-16 Julia M. Carlstad, Kristie A. Boering
Chemical physics plays a large role in determining the isotopic compositions of gases in Earth's atmosphere, which in turn provide fundamental insights into the sources, sinks, and transformations of atmospheric gases and particulates and their influence on climate. This review focuses on the kinetic and photolysis isotope effects relevant to understanding the isotope compositions of atmospheric ozone
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Ultrafast Dynamics of Photosynthetic Light Harvesting: Strategies for Acclimation Across Organisms Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-16 Olivia C. Fiebig, Dvir Harris, Dihao Wang, Madeline P. Hoffmann, Gabriela S. Schlau-Cohen
Photosynthetic light harvesting exhibits near-unity quantum efficiency. The high efficiency is achieved through a series of energy and charge transfer steps within a network of pigment-containing proteins. Remarkably, high efficiency is conserved across many organisms despite differences in the protein structures and organization that allow each organism to respond to its own biological niche and the
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Modeling Excited States of Molecular Organic Aggregates for Optoelectronics Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-16 Federico J. Hernández, Rachel Crespo-Otero
Light-driven phenomena in organic molecular aggregates underpin several mechanisms relevant to optoelectronic applications. Modeling these processes is essential for aiding the design of new materials and optimizing optoelectronic devices. In this review, we cover the use of different atomistic models, excited-state dynamics, and transport approaches for understanding light-activated phenomena in molecular
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Mechanisms of Photothermalization in Plasmonic Nanostructures: Insights into the Steady State Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-16 Shengxiang Wu, Matthew Sheldon
Localized surface plasmon resonances (LSPRs) in metallic nanostructures result in subwavelength optical confinement that enhances light–matter interactions, for example, aiding the sensitivity of surface spectroscopies. The dissipation of surface plasmons as electronic and vibrational excitations sets the limit for field confinement but also provides opportunities for photochemistry, photocatalysis
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Surface-Mediated Formation of Stable Glasses Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-08 Peng Luo, Zahra Fakhraai
Surfaces mediate the formation of stable glasses (SGs) upon physical vapor deposition (PVD) for a wide range of glass formers. The thermodynamic and kinetic stability of SGs and their anisotropic packing structures are controlled through the deposition parameters (deposition temperature and rate) as well as the chemical structure and composition of the glass former. The resulting PVD glass properties
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Interactive Quantum Chemistry Enabled by Machine Learning, Graphical Processing Units, and Cloud Computing Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-08 Umberto Raucci, Hayley Weir, Sukolsak Sakshuwong, Stefan Seritan, Colton B. Hicks, Fabio Vannucci, Francesco Rea, Todd J. Martínez
Modern quantum chemistry algorithms are increasingly able to accurately predict molecular properties that are useful for chemists in research and education. Despite this progress, performing such calculations is currently unattainable to the wider chemistry community, as they often require domain expertise, computer programming skills, and powerful computer hardware. In this review, we outline methods
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3D Super-Resolution Fluorescence Imaging of Microgels Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-08 Oleksii Nevskyi, Dominik Wöll
Super-resolution fluorescence microscopy techniques are powerful tools to investigate polymer systems. In this review, we address how these techniques have been applied to hydrogel nano- and microparticles, so-called nano- or microgels. We outline which research questions on microgels could be addressed and what new insights could be achieved. Studies of the morphology, shape, and deformation of microgels;
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Adsorption at Nanoconfined Solid–Water Interfaces Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-02-04 Anastasia G. Ilgen, Kevin Leung, Louise J. Criscenti, Jeffery A. Greathouse
Reactions at solid–water interfaces play a foundational role in water treatment systems, catalysis, and chemical separations, and in predicting chemical fate and transport in the environment. Over the last century, experimental measurements and computational models have made tremendous progress in capturing reactions at solid surfaces. The interfacial reactivity of a solid surface, however, can change
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Remembering the Work of Phillip L. Geissler: A Coda to His Scientific Trajectory Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-01-31 Gregory R. Bowman, Stephen J. Cox, Christoph Dellago, Kateri H. DuBay, Joel D. Eaves, Daniel A. Fletcher, Layne B. Frechette, Michael Grünwald, Katherine Klymko, JiYeon Ku, Ahmad K. Omar, Eran Rabani, David R. Reichman, Julia R. Rogers, Andreana M. Rosnik, Grant M. Rotskoff, Anna R. Schneider, Nadine Schwierz, David A. Sivak, Suriyanarayanan Vaikuntanathan, Stephen Whitelam, Asaph Widmer-Cooper
Phillip L. Geissler made important contributions to the statistical mechanics of biological polymers, heterogeneous materials, and chemical dynamics in aqueous environments. He devised analytical and computational methods that revealed the underlying organization of complex systems at the frontiers of biology, chemistry, and materials science. In this retrospective we celebrate his work at these frontiers
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Toward Ab Initio Reaction Discovery Using the Artificial Force Induced Reaction Method Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-01-31 Satoshi Maeda, Yu Harabuchi, Hiroki Hayashi, Tsuyoshi Mita
Predicting the whole process of a chemical reaction while solving kinetic equations presents an opportunity to realize an on-the-fly kinetic simulation that directly discovers chemical reactions with their product yields. Such a simulation avoids the combinatorial explosion of reaction patterns to be examined by narrowing the search space based on the kinetic analysis of the reaction path network,
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Photochemical Upconversion Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-01-25 Jiale Feng, Jessica Alves, Damon M. de Clercq, Timothy W. Schmidt
Photochemical upconversion is a process whereby two lower-energy photons are converted into a higher-energy photon by sensitized triplet–triplet annihilation. While recent interest in this process has been motivated by improving the efficiencies of solar cells, many applications are being explored. In this review, we address the underlying physicochemical phenomena that are responsible for photochemical
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Modeling Anharmonic Effects in the Vibrational Spectra of High-Frequency Modes Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-01-25 Edwin L. Sibert
High-resolution vibrational spectra of C–H, O–H, and N–H stretches depend on both molecular conformation and environment as well as provide a window into the frequencies of many other vibrational degrees of freedom as a result of mode mixing. We review current theoretical strategies that are being deployed to both aid and guide the analysis of the data that are encoded in these spectra. The goal is
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Spectroscopic Studies of Clusters of Atmospheric Relevance Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-01-25 Nicoline C. Frederiks, Annapoorani Hariharan, Christopher J. Johnson
Atmospheric aerosols exert a significant but highly uncertain effect on the global climate, and roughly half of these particles originate as small clusters formed by collisions between atmospheric trace vapors. These particles typically consist of acids, bases, and water, stabilized by salt bridge formation and a network of strong hydrogen bonds. We review spectroscopic studies of this process, focusing
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The Predictive Power of Exact Constraints and Appropriate Norms in Density Functional Theory Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-01-25 Aaron D. Kaplan, Mel Levy, John P. Perdew
Ground-state Kohn-Sham density functional theory provides, in principle, the exact ground-state energy and electronic spin densities of real interacting electrons in a static external potential. In practice, the exact density functional for the exchange-correlation (xc) energy must be approximated in a computationally efficient way. About 20 mathematical properties of the exact xc functional are known
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Magneto-Optical Properties of Noble Metal Nanostructures Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-01-25 Juniper Foxley, Kenneth L. Knappenberger
The magneto-optical signatures of colloidal noble metal nanostructures, spanning both discrete nanoclusters (<2 nm) and plasmonic nanoparticles (>2 nm), exhibit rich structure-property correlations, impacting applications including photonic integrated circuits, light modulation, applied spectroscopy, and more. For nanoclusters, electron doping and single-atom substitution modify both the intensity
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Studies of Local DNA Backbone Conformation and Conformational Disorder Using Site-Specific Exciton-Coupled Dimer Probe Spectroscopy Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-01-25 Andrew H. Marcus, Dylan Heussman, Jack Maurer, Claire S. Albrecht, Patrick Herbert, Peter H. von Hippel
The processes of genome expression, regulation, and repair require direct interactions between proteins and DNA at specific sites located at and near single-stranded–double-stranded DNA (ssDNA–dsDNA) junctions. Here, we review the application of recently developed spectroscopic methods and analyses that combine linear absorbance and circular dichroism spectroscopy with nonlinear 2D fluorescence spectroscopy
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Photoacid Dynamics in the Green Fluorescent Protein Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2023-01-25 Jasper J. van Thor, Paul M. Champion
The photoacid dynamics of fluorescent proteins include both electronic excited- and ground-state mechanisms of proton transfer. The associated characteristic timescales of these reactions range over many orders of magnitude, and the tunneling, barrier crossing, and relevant thermodynamics have in certain cases been linked to coherent nuclear motion. We review the literature and summarize the experiments
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Gas-Phase Computational Spectroscopy: The Challenge of the Molecular Bricks of Life Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-11-22 Vincenzo Barone, Cristina Puzzarini
Gas-phase molecular spectroscopy is a natural playground for accurate quantum-chemical computations. However, the molecular bricks of life (e.g., DNA bases or amino acids) are challenging systems because of the unfavorable scaling of quantum-chemical models with the molecular size (active electrons) and/or the presence of large-amplitude internal motions. From the theoretical point of view, both aspects
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Quantitative Surface-Enhanced Spectroscopy Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-04-20 Ryan D. Norton, Hoa T. Phan, Stephanie N. Gibbons, Amanda J. Haes
Surface-enhanced Raman scattering (SERS), a powerful technique for trace molecular detection, depends on chemical and electromagnetic enhancements. While recent advances in instrumentation and substrate design have expanded the utility, reproducibility, and quantitative capabilities of SERS, some challenges persist. In this review, advances in quantitative SERS detection are discussed as they relate
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Double and Charge-Transfer Excitations in Time-Dependent Density Functional Theory Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-04-20 Neepa T. Maitra
Time-dependent density functional theory has emerged as a method of choice for calculations of spectra and response properties in physics, chemistry, and biology, with its system-size scaling enabling computations on systems much larger than otherwise possible. While increasingly complex and interesting systems have been successfully tackled with relatively simple functional approximations, there has
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eScience Infrastructures in Physical Chemistry Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-04-20 Samantha Kanza, Cerys Willoughby, Colin Leonard Bird, Jeremy Graham Frey
As the volume of data associated with scientific research has exploded over recent years, the use of digital infrastructures to support this research and the data underpinning it has increased significantly. Physical chemists have been making use of eScience infrastructures since their conception, but in the last five years their usage has increased even more. While these infrastructures have not greatly
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Bimolecular Chemistry in the Ultracold Regime Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-04-20 Yu Liu, Kang-Kuen Ni
Advances in atomic, molecular, and optical physics techniques allowed the cooling of simple molecules down to the ultracold regime (1 mK) and opened opportunities to study chemical reactions with unprecedented levels of control. This review covers recent developments in studying bimolecular chemistry at ultralow temperatures. We begin with a brief overview of methods for producing, manipulating, and
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Molecular Polaritonics: Chemical Dynamics Under Strong Light–Matter Coupling Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-04-20 Tao E. Li, Bingyu Cui, Joseph E. Subotnik, Abraham Nitzan
Chemical manifestations of strong light–matter coupling have recently been a subject of intense experimental and theoretical studies. Here we review the present status of this field. Section 1 is an introduction to molecular polaritonics and to collective response aspects of light–matter interactions. Section 2 provides an overview of the key experimental observations of these effects, while Section
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Ultrafast Imaging of Molecules with Electron Diffraction Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-04-20 Martin Centurion, Thomas J.A. Wolf, Jie Yang
Photoexcited molecules convert light into chemical and mechanical energy through changes in electronic and nuclear structure that take place on femtosecond timescales. Gas phase ultrafast electron diffraction (GUED) is an ideal tool to probe the nuclear geometry evolution of the molecules and complements spectroscopic methods that are mostly sensitive to the electronic state. GUED is a weak and passive
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Protein Structure Prediction with Mass Spectrometry Data Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-04-20 Sarah E. Biehn, Steffen Lindert
Knowledge of protein structure is crucial to our understanding of biological function and is routinely used in drug discovery. High-resolution techniques to determine the three-dimensional atomic coordinates of proteins are available. However, such methods are frequently limited by experimental challenges such as sample quantity, target size, and efficiency. Structural mass spectrometry (MS) is a technique
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Imaging Dynamic Processes in Multiple Dimensions and Length Scales Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-02-04 Seth L. Filbrun, Fei Zhao, Kuangcai Chen, Teng-Xiang Huang, Meek Yang, Xiaodong Cheng, Bin Dong, Ning Fang
Optical microscopy has become an invaluable tool for investigating complex samples. Over the years, many advances to optical microscopes have been made that have allowed us to uncover new insights into the samples studied. Dynamic changes in biological and chemical systems are of utmost importance to study. To probe these samples, multidimensional approaches have been developed to acquire a fuller
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Photophysics of Two-Dimensional Semiconducting Organic–Inorganic Metal-Halide Perovskites Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-02-04 Daniel B. Straus, Cherie R. Kagan
Two-dimensional organic–inorganic hybrid perovskites (2DHPs) consist of alternating anionic metal-halide and cationic organic layers. They have widely tunable structural and optical properties. We review the role of the organic cation in defining the structural and optical properties of 2DHPs through the example of lead iodide 2DHPs. Even though excitons reside in the metal-halide layers, the organic
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Classical and Nonclassical Nucleation and Growth Mechanisms for Nanoparticle Formation Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-02-03 Young-Shin Jun, Yaguang Zhu, Ying Wang, Deoukchen Ghim, Xuanhao Wu, Doyoon Kim, Haesung Jung
All solid materials are created via nucleation. In this evolutionary process, nuclei form in solution or at interfaces, expand by monomeric growth and oriented attachment, and undergo phase transformation. Nucleation determines the location and size of nuclei, whereas growth controls the size, shape, and aggregation of newly formed nanoparticles. These physical properties of nanoparticles can affect
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Vibration-Cavity Polariton Chemistry and Dynamics Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-26 Adam D. Dunkelberger, Blake S. Simpkins, Igor Vurgaftman, Jeffrey C. Owrutsky
Molecular polaritons result from light-matter coupling between optical resonances and molecular electronic or vibrational transitions. When the coupling is strong enough, new hybridized states with mixed photon-material character are observed spectroscopically, with resonances shifted above and below the uncoupled frequency. These new modes have unique optical properties and can be exploited to promote
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Stochastic Vector Techniques in Ground-State Electronic Structure Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-26 Roi Baer, Daniel Neuhauser, Eran Rabani
We review a suite of stochastic vector computational approaches for studying the electronic structure of extended condensed matter systems. These techniques help reduce algorithmic complexity, facilitate efficient parallelization, simplify computational tasks, accelerate calculations, and diminish memory requirements. While their scope is vast, we limit our study to ground-state and finite temperature
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Path Integrals for Nonadiabatic Dynamics: Multistate Ring Polymer Molecular Dynamics Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-26 Nandini Ananth
This review focuses on a recent class of path-integral-based methods for the simulation of nonadiabatic dynamics in the condensed phase using only classical molecular dynamics trajectories in an extended phase space. Specifically, a semiclassical mapping protocol is used to derive an exact, continuous, Cartesian variable path-integral representation for the canonical partition function of a system
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Laser-Induced Coulomb Explosion Imaging of Aligned Molecules and Molecular Dimers Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-26 Constant A. Schouder, Adam S. Chatterley, James D. Pickering, Henrik Stapelfeldt
We discuss how Coulomb explosion imaging (CEI), triggered by intense femtosecond laser pulses and combined with laser-induced alignment and covariance analysis of the angular distributions of the recoiling fragment ions, provides new opportunities for imaging the structures of molecules and molecular complexes. First, focusing on gas phase molecules, we show how the periodic torsional motion of halogenated
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Intramolecular Vibrations in Excitation Energy Transfer: Insights from Real-Time Path Integral Calculations Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-26 Sohang Kundu, Nancy Makri
Excitation energy transfer (EET) is fundamental to many processes in chemical and biological systems and carries significant implications for the design of materials suitable for efficient solar energy harvest and transport. This review discusses the role of intramolecular vibrations on the dynamics of EET in nonbonded molecular aggregates of bacteriochlorophyll, a perylene bisimide, and a model system
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Calculating Multidimensional Optical Spectra from Classical Trajectories Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-21 Roger F. Loring
Multidimensional optical spectra are measured from the response of a material system to a sequence of laser pulses and have the capacity to elucidate specific molecular interactions and dynamics whose influences are absent or obscured in a conventional linear absorption spectrum. Interpretation of complex spectra is supported by theoretical modeling of the spectroscopic observable, requiring implementation
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Probing the Nature of the Transition-Metal-Boron Bonds and Novel Aromaticity in Small Metal-Doped Boron Clusters Using Photoelectron Spectroscopy Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-19 Teng-Teng Chen, Ling Fung Cheung, Lai-Sheng Wang
Photoelectron spectroscopy combined with quantum chemistry has been a powerful approach to elucidate the structures and bonding of size-selected boron clusters (B n−), revealing a prevalent planar world that laid the foundation for borophenes. Investigations of metal-doped boron clusters not only lead to novel structures but also provide important information about the metal-boron bonds that are critical
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Vibrational Spectroscopy of the Water Dimer at Jet-Cooled and Atmospheric Temperatures Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-19 Emil Vogt, Henrik G. Kjaergaard
The vibrational spectroscopy of the water dimer provides an understanding of basic hydrogen bonding in water clusters, and with about one water dimer for every 1,000 water molecules, it plays a critical role in atmospheric science. Here, we review how the experimental and theoretical progress of the past decades has improved our understanding of water dimer vibrational spectroscopy under both cold
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Capturing Atom-Specific Electronic Structural Dynamics of Transition-Metal Complexes with Ultrafast Soft X-Ray Spectroscopy Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-05 Raphael M. Jay, Kristjan Kunnus, Philippe Wernet, Kelly J. Gaffney
The atomic specificity of X-ray spectroscopies provides a distinct perspective on molecular electronic structure. For 3 d metal coordination and organometallic complexes, the combination of metal- and ligand-specific X-ray spectroscopies directly interrogates metal–ligand covalency—the hybridization of metal and ligand electronic states. Resonant inelastic X-ray scattering (RIXS), the X-ray analog
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Neural Network Potentials: A Concise Overview of Methods Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2022-01-04 Emir Kocer, Tsz Wai Ko, Jörg Behler
In the past two decades, machine learning potentials (MLPs) have reached a level of maturity that now enables applications to large-scale atomistic simulations of a wide range of systems in chemistry, physics, and materials science. Different machine learning algorithms have been used with great success in the construction of these MLPs. In this review, we discuss an important group of MLPs relying
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Demystifying the Diffuse Vibrational Spectrum of Aqueous Protons Through Cold Cluster Spectroscopy Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2021-04-20 Helen J. Zeng, Mark A. Johnson
The ease with which the pH is routinely determined for aqueous solutions masks the fact that the cationic product of Arrhenius acid dissolution, the hydrated proton, or H+(aq), is a remarkably complex species. Here, we review how results obtained over the past 30 years in the study of H+⋅(H2O)n cluster ions isolated in the gas phase shed light on the chemical nature of H+(aq). This effort has also
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From Intermolecular Interaction Energies and Observable Shifts to Component Contributions and Back Again: A Tale of Variational Energy Decomposition Analysis Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2021-04-20 Yuezhi Mao, Matthias Loipersberger, Paul R. Horn, Akshaya Das, Omar Demerdash, Daniel S. Levine, Srimukh Prasad Veccham, Teresa Head-Gordon, Martin Head-Gordon
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
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Understanding and Controlling Intersystem Crossing in Molecules Annu. Rev. Phys. Chem. (IF 14.7) Pub Date : 2021-04-20 Christel M. Marian
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