Bao-Ying Wen, Qing-Qi Chen, Petar M Radjenovic, Jin-Chao Dong, Zhong-Qun Tian, Jian-Feng Li
{"title":"In Situ Surface-Enhanced Raman Spectroscopy Characterization of Electrocatalysis with Different Nanostructures.","authors":"Bao-Ying Wen, Qing-Qi Chen, Petar M Radjenovic, Jin-Chao Dong, Zhong-Qun Tian, Jian-Feng Li","doi":"10.1146/annurev-physchem-090519-034645","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090519-034645","url":null,"abstract":"<p><p>As energy demands increase, electrocatalysis serves as a vital tool in energy conversion. Elucidating electrocatalytic mechanisms using in situ spectroscopic characterization techniques can provide experimental guidance for preparing high-efficiency electrocatalysts. Surface-enhanced Raman spectroscopy (SERS) can provide rich spectral information for ultratrace surface species and is extremely well suited to studying their activity. To improve the material and morphological universalities, researchers have employed different kinds of nanostructures that have played important roles in the development of SERS technologies. Different strategies, such as so-called borrowing enhancement from shell-isolated modes and shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS)-satellite structures, have been proposed to obtain highly effective Raman enhancement, and these methods make it possible to apply SERS to various electrocatalytic systems. Here, we discuss the development of SERS technology, focusing on its applications in different electrocatalytic reactions (such as oxygen reduction reactions) and at different nanostructure surfaces, and give a brief outlook on its development.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"331-351"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38842056","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}
{"title":"Droplet Interfacial Tensions and Phase Transitions Measured in Microfluidic Channels.","authors":"Priyatanu Roy, Shihao Liu, Cari S Dutcher","doi":"10.1146/annurev-physchem-090419-105522","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090419-105522","url":null,"abstract":"<p><p>Measurements of droplet phase and interfacial tension (IFT) are important in the fields of atmospheric aerosols and emulsion science. Bulk macroscale property measurements with similar constituents cannot capture the effect of microscopic length scales and highly curved surfaces on the transport characteristics and heterogeneous chemistry typical in these applications. Instead, microscale droplet measurements ensure properties are measured at the relevant length scale. With recent advances in microfluidics, customized multiphase fluid flows can be created in channels for the manipulation and observation of microscale droplets in an enclosed setting without the need for large and expensive control systems. In this review, we discuss the applications of different physical principles at the microscale and corresponding microfluidic approaches for the measurement of droplet phase state, viscosity, and IFT.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"73-97"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25386244","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}
Karwan Ali Omar, Karim Hasnaoui, Aurélien de la Lande
{"title":"First-Principles Simulations of Biological Molecules Subjected to Ionizing Radiation.","authors":"Karwan Ali Omar, Karim Hasnaoui, Aurélien de la Lande","doi":"10.1146/annurev-physchem-101419-013639","DOIUrl":"https://doi.org/10.1146/annurev-physchem-101419-013639","url":null,"abstract":"<p><p>Ionizing rays cause damage to genomes, proteins, and signaling pathways that normally regulate cell activity, with harmful consequences such as accelerated aging, tumors, and cancers but also with beneficial effects in the context of radiotherapies. While the great pace of research in the twentieth century led to the identification of the molecular mechanisms for chemical lesions on the building blocks of biomacromolecules, the last two decades have brought renewed questions, for example, regarding the formation of clustered damage or the rich chemistry involving the secondary electrons produced by radiolysis. Radiation chemistry is now meeting attosecond science, providing extraordinary opportunities to unravel the very first stages of biological matter radiolysis. This review provides an overview of the recent progress made in this direction, focusing mainly on the atto- to femto- to picosecond timescales. We review promising applications of time-dependent density functional theory in this context.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"445-465"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38899064","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}
Delphine K Farmer, Erin K Boedicker, Holly M DeBolt
{"title":"Dry Deposition of Atmospheric Aerosols: Approaches, Observations, and Mechanisms.","authors":"Delphine K Farmer, Erin K Boedicker, Holly M DeBolt","doi":"10.1146/annurev-physchem-090519-034936","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090519-034936","url":null,"abstract":"<p><p>Aerosols are liquid or solid particles suspended in the atmosphere, typically with diameters on the order of nanometers to microns. These particles impact air quality and the radiative balance of the planet. Dry deposition is a key process for the removal of aerosols from the atmosphere and plays an important role in controlling the lifetime of atmospheric aerosols. Dry deposition is driven by turbulence and shows a strong dependence on particle size. This review summarizes the mechanisms behind aerosol dry deposition, including measurement approaches, field observations, and modeling studies. We identify several gaps in the literature, including deposition over the cryosphere (i.e., snow and ice surfaces) and the ocean; in addition, we highlight new techniques to measure black carbon fluxes. While recent advances in aerosol instrumentation have enhanced our understanding of aerosol sources and chemistry, dry deposition and other loss processes remain poorly investigated.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"375-397"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38842057","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}
{"title":"Molecular Simulation of Electrode-Solution Interfaces.","authors":"Laura Scalfi, Mathieu Salanne, Benjamin Rotenberg","doi":"10.1146/annurev-physchem-090519-024042","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090519-024042","url":null,"abstract":"<p><p>Many key industrial processes, from electricity production, conversion, and storage to electrocatalysis or electrochemistry in general, rely on physical mechanisms occurring at the interface between a metallic electrode and an electrolyte solution, summarized by the concept of an electric double layer, with the accumulation/depletion of electrons on the metal side and of ions on the liquid side. While electrostatic interactions play an essential role in the structure, thermodynamics, dynamics, and reactivity of electrode-electrolyte interfaces, these properties also crucially depend on the nature of the ions and solvent, as well as that of the metal itself. Such interfaces pose many challenges for modeling because they are a place where quantum chemistry meets statistical physics. In the present review, we explore the recent advances in the description and understanding of electrode-electrolyte interfaces with classical molecular simulations, with a focus on planar interfaces and solvent-based liquids, from pure solvent to water-in-salt electrolytes.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"189-212"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39126537","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}
{"title":"Optical Properties and Excited-State Dynamics of Atomically Precise Gold Nanoclusters.","authors":"Meng Zhou, Rongchao Jin","doi":"10.1146/annurev-physchem-090419-104921","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090419-104921","url":null,"abstract":"<p><p>Understanding the excited-state dynamics of nanomaterials is essential to their applications in photoenergy storage and conversion. This review summarizes recent progress in the excited-state dynamics of atomically precise gold (Au) nanoclusters (NCs). We first discuss the electronic structure and typical relaxation pathways of Au NCs from subpicoseconds to microseconds. Unlike plasmonic Au nanoparticles, in which collective electron excitation dominates, Au NCs show single-electron transitions and molecule-like exciton dynamics. The size-, shape-, structure-, and composition-dependent dynamics in Au NCs are further discussed in detail. For small-sized Au NCs, strong quantum confinement effects give rise to relaxation dynamics that is significantly dependent on atomic packing, shape, and heteroatom doping. For relatively larger-sized Au NCs, strong size dependence can be observed in exciton and electron dynamics. We also discuss the origin of coherent oscillations and their roles in excited-state relaxation. Finally, we provide our perspective on future directions in this area.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"121-142"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1146/annurev-physchem-090419-104921","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38694057","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}
{"title":"Vibrational Sum-Frequency Generation Hyperspectral Microscopy for Molecular Self-Assembled Systems.","authors":"Haoyuan Wang, Wei Xiong","doi":"10.1146/annurev-physchem-090519-050510","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090519-050510","url":null,"abstract":"<p><p>In this review, we discuss the recent developments and applications of vibrational sum-frequency generation (VSFG) microscopy. This hyperspectral imaging technique can resolve systems without inversion symmetry, such as surfaces, interfaces and noncentrosymmetric self-assembled materials, in the spatial, temporal, and spectral domains. We discuss two common VSFG microscopy geometries: wide-field and confocal point-scanning. We then introduce the principle of VSFG and the relationships between hyperspectral imaging with traditional spectroscopy, microscopy, and time-resolved measurements. We further highlight crucial applications of VSFG microscopy in self-assembled monolayers, cellulose in plants, collagen fibers, and lattice self-assembled biomimetic materials. In these systems, VSFG microscopy reveals relationships between physical properties that would otherwise be hidden without being spectrally, spatially, and temporally resolved. Lastly, we discuss the recent development of ultrafast transient VSFG microscopy, which can spatially measure the ultrafast vibrational dynamics of self-assembled materials. The review ends with an outlook on the technical challenges of and scientific potential for VSFG microscopy.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"279-306"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38749446","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}
{"title":"Cryogenic Super-Resolution Fluorescence and Electron Microscopy Correlated at the Nanoscale.","authors":"Peter D Dahlberg, W E Moerner","doi":"10.1146/annurev-physchem-090319-051546","DOIUrl":"https://doi.org/10.1146/annurev-physchem-090319-051546","url":null,"abstract":"<p><p>We review the emerging method of super-resolved cryogenic correlative light and electron microscopy (srCryoCLEM). Super-resolution (SR) fluorescence microscopy and cryogenic electron tomography (CET) are both powerful techniques for observing subcellular organization, but each approach has unique limitations. The combination of the two brings the single-molecule sensitivity and specificity of SR to the detailed cellular context and molecular scale resolution of CET. The resulting correlative data is more informative than the sum of its parts. The correlative images can be used to pinpoint the positions of fluorescently labeled proteins in the high-resolution context of CET with nanometer-scale precision and/or to identify proteins in electron-dense structures. The execution of srCryoCLEM is challenging and the approach is best described as a method that is still in its infancy with numerous technical challenges. In this review, we describe state-of-the-art srCryoCLEM experiments, discuss the most pressing challenges, and give a brief outlook on future applications.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"253-278"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8877847/pdf/nihms-1779529.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38749866","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Daisy Unsihuay, Daniela Mesa Sanchez, Julia Laskin
{"title":"Quantitative Mass Spectrometry Imaging of Biological Systems.","authors":"Daisy Unsihuay, Daniela Mesa Sanchez, Julia Laskin","doi":"10.1146/annurev-physchem-061020-053416","DOIUrl":"10.1146/annurev-physchem-061020-053416","url":null,"abstract":"<p><p>Mass spectrometry imaging (MSI) is a powerful, label-free technique that provides detailed maps of hundreds of molecules in complex samples with high sensitivity and subcellular spatial resolution. Accurate quantification in MSI relies on a detailed understanding of matrix effects associated with the ionization process along with evaluation of the extraction efficiency and mass-dependent ion losses occurring in the analysis step. We present a critical summary of approaches developed for quantitative MSI of metabolites, lipids, and proteins in biological tissues and discuss their current and future applications.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"307-329"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8161172/pdf/nihms-1699190.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38749868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Marc A Sprague-Piercy, Megan A Rocha, Ashley O Kwok, Rachel W Martin
{"title":"α-Crystallins in the Vertebrate Eye Lens: Complex Oligomers and Molecular Chaperones.","authors":"Marc A Sprague-Piercy, Megan A Rocha, Ashley O Kwok, Rachel W Martin","doi":"10.1146/annurev-physchem-090419-121428","DOIUrl":"10.1146/annurev-physchem-090419-121428","url":null,"abstract":"<p><p>α-Crystallins are small heat-shock proteins that act as holdase chaperones. In humans, αA-crystallin is expressed only in the eye lens, while αB-crystallin is found in many tissues. α-Crystallins have a central domain flanked by flexible extensions and form dynamic, heterogeneous oligomers. Structural models show that both the C- and N-terminal extensions are important for controlling oligomerization through domain swapping. α-Crystallin prevents aggregation of damaged β- and γ-crystallins by binding to the client protein using a variety of binding modes. α-Crystallin chaperone activity can be compromised by mutation or posttranslational modifications, leading to protein aggregation and cataract. Because of their high solubility and their ability to form large, functional oligomers, α-crystallins are particularly amenable to structure determination by solid-state nuclear magnetic resonance (NMR) and solution NMR, as well as cryo-electron microscopy.</p>","PeriodicalId":7967,"journal":{"name":"Annual review of physical chemistry","volume":"72 ","pages":"143-163"},"PeriodicalIF":14.7,"publicationDate":"2021-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8062273/pdf/nihms-1628487.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38713564","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}