Chemical physics reviews最新文献_第5页

Visible-light photoredox catalysis with organic polymers 有机聚合物的可见光光氧化还原催化

Chemical physics reviews Pub Date : 2023-03-01 DOI: 10.1063/5.0123282

G. Kumar, B. Cai, S. Ott, H. Tian

引用次数: 1

Layer-by-layer assembly of metal-organic framework thin films: Fabrication and advanced applications 金属有机骨架薄膜的逐层组装:制造和先进应用

Chemical physics reviews Pub Date : 2023-03-01 DOI: 10.1063/5.0135019

Dong-Hui Chen, H. Gliemann, C. Wöll

{"title":"Layer-by-layer assembly of metal-organic framework thin films: Fabrication and advanced applications","authors":"Dong-Hui Chen, H. Gliemann, C. Wöll","doi":"10.1063/5.0135019","DOIUrl":"https://doi.org/10.1063/5.0135019","url":null,"abstract":"Metal-organic frameworks (MOFs) are a class of crystalline porous coordination materials, which are assembled from inorganic nodes and organic linkers. Numerous applications, such as gas storage, molecule separation, catalysis, optical sensing, and charge transport, benefit from the outstanding properties of MOF materials. More advanced applications, e.g., in the electronics and optoelectronics area, demand homogeneous and monolithic MOF thin films. Recent studies demonstrated that surface-mounted MOFs (SURMOFs) are well suited to fulfill the requirements for the integration of MOFs into devices. As a crystalline thin-film material with tunable thickness, SURMOFs have been widely used in the optimization of chromophore stacking, electrical transport, stimuli-response, etc. The fabrication of SURMOFs is carried out employing a layer-by-layer (LbL) assembly technique, and it can yield MOF thin films with a well-defined orientation, tunable thickness, and editable crystalline heterostructure. We summarize the LbL assembly methods for SURMOF fabrication and the realization of advanced SURMOF architectures, including optical and electronic applications as well as the integration of photoactive SURMOFs and SURMOF-derived materials in technical devices. We conclude with a discussion of the challenges and prediction of the future of SURMOF materials.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44149619","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 7

Effects of electrolyte anion adsorption on the activity and stability of single atom electrocatalysts 电解质阴离子吸附对单原子电催化剂活性和稳定性的影响

Chemical physics reviews Pub Date : 2023-03-01 DOI: 10.1063/5.0125654

Tipaporn Patniboon, H. Hansen

{"title":"Effects of electrolyte anion adsorption on the activity and stability of single atom electrocatalysts","authors":"Tipaporn Patniboon, H. Hansen","doi":"10.1063/5.0125654","DOIUrl":"https://doi.org/10.1063/5.0125654","url":null,"abstract":"A single metal site incorporated in N-doped carbon (M/N/C) is a promising electrocatalyst. Here, we perform a computation investigation of the effect of electrolyte anion adsorption on the activity and stability of single-atom catalysts (MN4) with M as transition metal and p-block metal. The MN4 site on two different graphene structures (bulk graphene and graphene edge) is studied under electrochemical conditions for the oxygen reduction reaction (ORR) and the CO2 reduction reaction (CO2RR). Because of the two-dimensional nature of the catalyst, reaction intermediates and electrolyte ions can interact with both sides of the single-atom catalyst. As a result, the electrolyte anions compete with water and adsorbate on the single metal site, in some cases either poisoning or modifying the catalyst activity and thermodynamic stability. We find most electrolyte anions adsorbs on the single metal site under ORR conditions but not at the lower potentials for the CO2RR. Still, the adsorption of water and gas molecules can occur under CO2RR conditions. For example, under ORR conditions, the thermodynamic driving force of the *SO4-FeN4 site in the 0.1 M H2SO4 solution is about 0.47–0.56 eV lower than the *O-FeN4 site in water, depending on the local carbon structure. Additionally, the stabilization by electrolyte anions depends on the nature of the metal atom. Our study demonstrates the important role of electrolytes and the coordination environment for the activity and stability of the M/N/C catalyst.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"48658820","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 1

A guide to small fluorescent probes for single-molecule biophysics 用于单分子生物物理学的小荧光探针指南

Chemical physics reviews Pub Date : 2023-03-01 DOI: 10.1063/5.0131663

M. Leake, S. Quinn

{"title":"A guide to small fluorescent probes for single-molecule biophysics","authors":"M. Leake, S. Quinn","doi":"10.1063/5.0131663","DOIUrl":"https://doi.org/10.1063/5.0131663","url":null,"abstract":"The explosive growth of single-molecule techniques is transforming our understanding of biology, helping to develop new physics inspired by emergent biological processes, and leading to emerging areas of nanotechnology. Key biological and chemical processes can now be probed with new levels of detail, one molecule at a time, from the nanoscopic dynamics of nature's molecular machines to an ever-expanding range of exciting applications across multiple length and time scales. Their common feature is an ability to render the underlying distribution of molecular properties that ensemble averaging masks and to reveal new insights into complex systems containing spatial and temporal heterogeneity. Small fluorescent probes are among the most adaptable and versatile for single-molecule sensing applications because they provide high signal-to-noise ratios combined with excellent specificity of labeling when chemically attached to target biomolecules or embedded within a host material. In this review, we examine recent advances in probe designs, their utility, and applications and provide a practical guide to their use, focusing on the single-molecule detection of nucleic acids, proteins, carbohydrates, and membrane dynamics. We also present key challenges that must be overcome to perform successful single-molecule experiments, including probe conjugation strategies, identify tradeoffs and limitations for each probe design, showcase emerging applications, and discuss exciting future directions for the community.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44194670","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 3

Data-driven many-body potentials from density functional theory for aqueous phase chemistry 水相化学密度泛函理论中数据驱动的多体势

Chemical physics reviews Pub Date : 2023-03-01 DOI: 10.1063/5.0129613

Etienne Palos, Saswata Dasgupta, Eleftherios Lambros, F. Paesani

{"title":"Data-driven many-body potentials from density functional theory for aqueous phase chemistry","authors":"Etienne Palos, Saswata Dasgupta, Eleftherios Lambros, F. Paesani","doi":"10.1063/5.0129613","DOIUrl":"https://doi.org/10.1063/5.0129613","url":null,"abstract":"Density functional theory (DFT) has been applied to modeling molecular interactions in water for over three decades. The ubiquity of water in chemical and biological processes demands a unified understanding of its physics, from the single molecule to the thermodynamic limit and everything in between. Recent advances in the development of data-driven and machine-learning potentials have accelerated simulation of water and aqueous systems with DFT accuracy. However, anomalous properties of water in the condensed phase, where a rigorous treatment of both local and non-local many-body (MB) interactions is in order, are often unsatisfactory or partially missing in DFT models of water. In this review, we discuss the modeling of water and aqueous systems based on DFT and provide a comprehensive description of a general theoretical/computational framework for the development of data-driven many-body potentials from DFT reference data. This framework, coined MB-DFT, readily enables efficient many-body molecular dynamics (MD) simulations of small molecules, in both gas and condensed phases, while preserving the accuracy of the underlying DFT model. Theoretical considerations are emphasized, including the role that the delocalization error plays in MB-DFT potentials of water and the possibility to elevate DFT and MB-DFT to near-chemical-accuracy through a density-corrected formalism. The development of the MB-DFT framework is described in detail, along with its application in MB-MD simulations and recent extension to the modeling of reactive processes in solution within a quantum mechanics/MB molecular mechanics (QM/MB-MM) scheme, using water as a prototypical solvent. Finally, we identify open challenges and discuss future directions for MB-DFT and QM/MB-MM simulations in condensed phases.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44964396","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 3

Ultrafast laser spectroscopy uncovers mechanisms of light energy conversion in photosynthesis and sustainable energy materials 超快激光光谱揭示光合作用和可持续能源材料中的光能转换机制

Chemical physics reviews Pub Date : 2022-12-01 DOI: 10.1063/5.0092864

D. Zigmantas, T. Polívka, P. Persson, V. Sundström

{"title":"Ultrafast laser spectroscopy uncovers mechanisms of light energy conversion in photosynthesis and sustainable energy materials","authors":"D. Zigmantas, T. Polívka, P. Persson, V. Sundström","doi":"10.1063/5.0092864","DOIUrl":"https://doi.org/10.1063/5.0092864","url":null,"abstract":"The invention of the laser in 1960 gave us the ruby laser, which generally produced chaotic pulses of light. Six years later, in 1966, a concept called passive mode-locking applied to neodymium-glass lasers produced reasonably well-behaving picosecond pulses. This triggered an intense activity, with respect to developing improved laser pulse sources, measurement techniques, and application to chemistry, physics, and biology. Initially, only ∼10 –ps-long pulses at a few wavelengths were available. Nevertheless, insight into the function of complex biological systems, like photosynthetic proteins, and molecules of chemical interest was gained in very early studies. Today, both duration and color of ultrashort pulses can be tuned to almost any value. This has of course opened up possibilities to study almost any atomic, molecular, or solid-state system and any dynamic process. This review focuses on the use of laser spectroscopy to investigate light energy conversion mechanisms in both natural photosynthesis and a topical selection of novel materials for solar energy conversion. More specifically, in photosynthesis we will review light harvesting and primary electron transfer; materials for solar energy conversion that we discuss include sensitized semiconductors (dye sensitized solar cells), polymer:fullerene and polymer:polymer bulk heterojunctions (organic solar cells), organometal halide perovskites, as well as molecular and hybrid systems for production of solar fuel and valuable chemicals. All these scientific areas, and in particular photosynthesis and the solar cell materials, have been extensively studied with ultrafast spectroscopy, resulting in a vast literature; a comprehensive review of the individual materials is, therefore, not feasible, and we will limit our discussion to work that we think has been of particular importance for understanding the function of the respective systems.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44228421","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 6

Monitoring membranes: The exploration of biological bilayers with second harmonic generation. 监测膜：利用二次谐波发生探索生物双层膜。

IF 6.1

Chemical physics reviews Pub Date : 2022-12-01 Epub Date: 2022-12-14 DOI: 10.1063/5.0120888

Eleanor F Page, Marea J Blake, Grant A Foley, Tessa R Calhoun

引用次数: 0

Publisher's Note: “Structural dynamics of proteins explored via time-resolved x-ray liquidography” [Chem. Phys. Rev. 3, 041304 (2022)] 出版商注释：“通过时间分辨x射线液相色谱法探索蛋白质的结构动力学”[Chem.Phys.Rev.304304（2022）]

Chemical physics reviews Pub Date : 2022-12-01 DOI: 10.1063/5.0135628

Yunbeom Lee, Hyosub Lee, H. Ihee

引用次数: 0

Negative inductor effects in nonlinear two-dimensional systems: Oscillatory neurons and memristors 非线性二维系统中的负电感效应:振荡神经元和忆阻器

Chemical physics reviews Pub Date : 2022-12-01 DOI: 10.1063/5.0124115

J. Bisquert

{"title":"Negative inductor effects in nonlinear two-dimensional systems: Oscillatory neurons and memristors","authors":"J. Bisquert","doi":"10.1063/5.0124115","DOIUrl":"https://doi.org/10.1063/5.0124115","url":null,"abstract":"Many chemical and physical systems show self-sustained oscillations that can be described by a set of nonlinear differential equations. The system enters oscillatory behavior by an intrinsic instability that leads to bifurcation. We analyze conducting systems that present oscillating response under application of external voltage or current. Phenomena like electrochemical corrosion and the spiking response of a biological neuron are well-known examples. These systems have applications in artificial neurons and synapses for neuromorphic computation. Their dynamical properties can be characterized by normal mode analysis of small expansion of the constituent nonlinear equations. The linearized model leads to the technique of ac frequency response impedance spectroscopy that can be obtained experimentally. We show a general description of two-variable systems formed by a combination of a fast variable (the voltage) and a slowing down internal variable, which produce a chemical inductor. A classification of bifurcations and stability is obtained in terms of the parameters of the intrinsic equivalent circuit including the case of a negative inductor. Thereafter, we describe a number of physical examples and establish the characterization of their properties: The electrocatalytic reaction with adsorbed intermediate species, an oscillating metal oxide memristor, and finally we discuss the signs of the equivalent circuit elements in the central model of neuroscience, the Hodgkin–Huxley model for an oscillating neuron.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"46411227","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 6

Sensitized triplet–triplet annihilation based photon upconversion in full organic and hybrid multicomponent systems 全有机和混合多组分系统中基于敏化三重态-三重态湮灭的光子上转换

Chemical physics reviews Pub Date : 2022-12-01 DOI: 10.1063/5.0112032

A. Ronchi, A. Monguzzi

{"title":"Sensitized triplet–triplet annihilation based photon upconversion in full organic and hybrid multicomponent systems","authors":"A. Ronchi, A. Monguzzi","doi":"10.1063/5.0112032","DOIUrl":"https://doi.org/10.1063/5.0112032","url":null,"abstract":"In the last 15 years, the attention dedicated to organic conjugated systems experienced outstanding growth because of the renewed interest in mechanisms involving triplet states such as singlet fission, thermally activated delayed fluorescence, and intersystem crossing enhanced phosphorescence. Photon upconversion via sensitized triplet–triplet annihilation ( sTTA) enables the conversion of low-energy photons into high-energy ones, and it has been proposed in multicomponent systems as an efficient managing strategy of non-coherent photons. This mechanism exploits the annihilation of two optically dark triplet states of emitter moieties to produce high-energy photons. The annihilating triplets are sensitized through Dexter energy transfer by a light-harvester, typically a conjugated molecule or a nanocrystal, so sTTA upconversion is usually performed in bi-component systems. The high yield observed at low excitation intensities stimulated thriving research in the field, leading to the development of a large family of fully organic and hybrid sTTA multicomponent upconverters. Here, we compare the evolution of these two families of systems with respect to the sTTA upconversion main figures of merit, highlighting the strengths and weaknesses of both approaches, according to the results reported in the literature. The data presented are also discussed in the perspective of future developments in the field, pointing out the challenges that are still to be faced for the technological use of the sTTA upconversion process.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47547216","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 4