The structure of a protein is closely related to its biological function. In this regard, structural changes, as well as static structures, have been scrutinized as essential elements in understanding and controlling the function of a protein. In particular, the structural change in the solution phase needs to be elucidated to properly understand protein functions under physiological conditions. Time-resolved x-ray liquidography (TRXL), also known as time-resolved x-ray solution scattering, has attracted attention as a powerful experimental method for studying the structural dynamics of proteins in the solution phase. Initially, TRXL was used to study the structural dynamics of small molecules in the solution phase, and later, its application was extended to probe the structural changes in proteins. Via TRXL, structural changes ranging from large quaternary movements to subtle rearrangements of the tertiary structures have been successfully elucidated. In this review, we introduce various studies using TRXL to investigate the structural dynamics of proteins. These include early TRXL studies on model systems, those on photoreceptor proteins, and recent studies using stimuli beyond the direct photoexcitation of proteins.
{"title":"Structural dynamics of proteins explored via time-resolved x-ray liquidography","authors":"Yunbeom Lee, Hyosub Lee, H. Ihee","doi":"10.1063/5.0101155","DOIUrl":"https://doi.org/10.1063/5.0101155","url":null,"abstract":"The structure of a protein is closely related to its biological function. In this regard, structural changes, as well as static structures, have been scrutinized as essential elements in understanding and controlling the function of a protein. In particular, the structural change in the solution phase needs to be elucidated to properly understand protein functions under physiological conditions. Time-resolved x-ray liquidography (TRXL), also known as time-resolved x-ray solution scattering, has attracted attention as a powerful experimental method for studying the structural dynamics of proteins in the solution phase. Initially, TRXL was used to study the structural dynamics of small molecules in the solution phase, and later, its application was extended to probe the structural changes in proteins. Via TRXL, structural changes ranging from large quaternary movements to subtle rearrangements of the tertiary structures have been successfully elucidated. In this review, we introduce various studies using TRXL to investigate the structural dynamics of proteins. These include early TRXL studies on model systems, those on photoreceptor proteins, and recent studies using stimuli beyond the direct photoexcitation of proteins.","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":"44250086","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}
Photocatalytic CO2 reduction is one of the ideal means to realize the carbon cycle. Metal–organic frameworks (MOFs) have received great attention as catalysts for photocatalytic CO2RR in recent years. The adjustable metal nodes and organic ligands in MOFs make them multifunctional catalysts. Therefore, they can participate in photocatalytic CO2RR in different roles. MOFs can be used as primary photocatalysts or be coupled with other active species to form composite materials. They can also act as co-catalysts to cooperate with photosensitizers. Moreover, MOFs can be used as precursors or templates for the preparation of derived nanomaterials. These derivatives are also promising candidates in photocatalytic CO2RR. This review aims to outline multiple roles of MOFs and their derivatives in photocatalytic CO2RR. Meanwhile, the corresponding modification strategies are summarized. At the end of the manuscript, the present problems of MOFs applied in photocatalytic CO2RR are summarized and the future development and challenges are also proposed.
{"title":"Multiple roles of metal–organic framework-based catalysts in photocatalytic CO2 reduction","authors":"Yaping Zhang, Jixiang Xu, Lei Wang, Banglin Chen","doi":"10.1063/5.0099758","DOIUrl":"https://doi.org/10.1063/5.0099758","url":null,"abstract":"Photocatalytic CO2 reduction is one of the ideal means to realize the carbon cycle. Metal–organic frameworks (MOFs) have received great attention as catalysts for photocatalytic CO2RR in recent years. The adjustable metal nodes and organic ligands in MOFs make them multifunctional catalysts. Therefore, they can participate in photocatalytic CO2RR in different roles. MOFs can be used as primary photocatalysts or be coupled with other active species to form composite materials. They can also act as co-catalysts to cooperate with photosensitizers. Moreover, MOFs can be used as precursors or templates for the preparation of derived nanomaterials. These derivatives are also promising candidates in photocatalytic CO2RR. This review aims to outline multiple roles of MOFs and their derivatives in photocatalytic CO2RR. Meanwhile, the corresponding modification strategies are summarized. At the end of the manuscript, the present problems of MOFs applied in photocatalytic CO2RR are summarized and the future development and challenges are also proposed.","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":"48250081","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}
Iontronics is an artificial platform using ions or molecules as signal carriers in an aqueous environment and is inspired by biological systems and their operating principles. Applications of iontronics have been primarily developed to mimic the characteristics of biological systems or to form seamless biointerfaces for communication. This review provides a comprehensive description of such endeavors in iontronics over the recent decades, as well as demonstrations pertaining to biomimetic nonlinear behaviors and ionic chemical delivery devices. The research highlights and applications are discussed based on the types of charge-selective materials used and their underlying principles. As iontronics is still at the early stage of development and diversification, a brief overview of its historical aspects and origin is first provided, followed by theoretical discussions regarding each iontronic material and its related applications. Finally, the review is concluded with some perspectives regarding future developments of iontronics in relation to natural systems in living organisms.
{"title":"Iontronics: Aqueous ion-based engineering for bioinspired functionalities and applications","authors":"S. H. Han, M.-A. Oh, T. Chung","doi":"10.1063/5.0089822","DOIUrl":"https://doi.org/10.1063/5.0089822","url":null,"abstract":"Iontronics is an artificial platform using ions or molecules as signal carriers in an aqueous environment and is inspired by biological systems and their operating principles. Applications of iontronics have been primarily developed to mimic the characteristics of biological systems or to form seamless biointerfaces for communication. This review provides a comprehensive description of such endeavors in iontronics over the recent decades, as well as demonstrations pertaining to biomimetic nonlinear behaviors and ionic chemical delivery devices. The research highlights and applications are discussed based on the types of charge-selective materials used and their underlying principles. As iontronics is still at the early stage of development and diversification, a brief overview of its historical aspects and origin is first provided, followed by theoretical discussions regarding each iontronic material and its related applications. Finally, the review is concluded with some perspectives regarding future developments of iontronics in relation to natural systems in living organisms.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47668067","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}
Solar water splitting is a promising technique for harvesting solar energy and converting abundant sunlight into storable hydrogen fuel. The cuprous oxide photocathode, one of the best-performing oxide photocathodes, possesses a theoretical photocurrent density of up to 14.7 mA cm−2 and a photovoltage as large as 1.6 V, making it possible to convert solar energy into hydrogen energy in a low-cost way. Herein, a comprehensive review of improving the solar water splitting performance of the cuprous oxide photocathode is presented with a focus on the crucial issues of increasing photocurrent density, photovoltage, and durability from the aspects of solving the incompatibility between the electron diffusion length and optical absorption distances, improving interfacial band alignment, revealing the impact of deficiencies, and introducing protective overlayers. We also outline the development of unassisted solar water splitting tandem devices with the cuprous oxide photocathode as a component, emphasizing the critical strategies to enhance the transmittance of the cuprous oxide photocathode, laying a solid foundation to further boost solar to hydrogen conversion efficiency. Finally, a perspective regarding the future directions for further optimizing the solar water splitting performance of the cuprous oxide photocathode and boosting solar to hydrogen conversion efficiency of the unbiased tandem device is also presented.
太阳能水分解是一种很有前途的技术，可以收集太阳能并将丰富的阳光转化为可储存的氢燃料。氧化亚铜光电阴极是性能最好的氧化物光电阴极之一，其理论光电流密度高达14.7 mA cm−2，光电压高达1.6 V，使太阳能以低成本的方式转化为氢能成为可能。本文从解决电子扩散长度和光吸收距离的不相容、改善界面带对准、揭示缺陷的影响以及引入保护层等方面对提高氧化亚铜光电阴极的太阳能水分解性能进行了综述，重点讨论了提高光电流密度、光电压和耐用性的关键问题。概述了以氧化亚铜光电阴极为组件的无辅助太阳能水分解串联装置的发展，强调了提高氧化亚铜光电阴极透光率的关键策略，为进一步提高太阳能到氢的转换效率奠定了坚实的基础。最后，展望了进一步优化氧化亚铜光电阴极的太阳能水分解性能和提高无偏串联装置太阳能制氢效率的未来发展方向。
{"title":"Cuprous oxide photocathodes for solar water splitting","authors":"Jinshui Cheng, Linxiao Wu, Jingshan Luo","doi":"10.1063/5.0095088","DOIUrl":"https://doi.org/10.1063/5.0095088","url":null,"abstract":"Solar water splitting is a promising technique for harvesting solar energy and converting abundant sunlight into storable hydrogen fuel. The cuprous oxide photocathode, one of the best-performing oxide photocathodes, possesses a theoretical photocurrent density of up to 14.7 mA cm−2 and a photovoltage as large as 1.6 V, making it possible to convert solar energy into hydrogen energy in a low-cost way. Herein, a comprehensive review of improving the solar water splitting performance of the cuprous oxide photocathode is presented with a focus on the crucial issues of increasing photocurrent density, photovoltage, and durability from the aspects of solving the incompatibility between the electron diffusion length and optical absorption distances, improving interfacial band alignment, revealing the impact of deficiencies, and introducing protective overlayers. We also outline the development of unassisted solar water splitting tandem devices with the cuprous oxide photocathode as a component, emphasizing the critical strategies to enhance the transmittance of the cuprous oxide photocathode, laying a solid foundation to further boost solar to hydrogen conversion efficiency. Finally, a perspective regarding the future directions for further optimizing the solar water splitting performance of the cuprous oxide photocathode and boosting solar to hydrogen conversion efficiency of the unbiased tandem device is also presented.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"46939764","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}
Organic polymer photocatalysts have garnered much interest in recent years, notably because of their photocatalytic activity toward hydrogen production from water. However, to rationalize the differences in activities between photocatalysts, it is crucial that their photodynamics are understood. Here, we provide an accessible introduction to the use of transient ultraviolet/visible absorption spectroscopy to study the photodynamics of linear polymeric photocatalysts through a review of literature studies. The principles of transient absorption (TA) spectroscopy, and the apparatus required, are briefly described. A step-by-step method to identify key species and unravel their kinetics is provided through exemplar spectra reported within the literature. This review provides the foundations for researchers new to the field of TA spectroscopy to design, perform, and interpret their own TA experiments to probe the photodynamics of organic photocatalysts.
{"title":"Transient absorption spectroscopic studies of linear polymeric photocatalysts for solar fuel generation","authors":"Chaoqi Li, Alexander J. Cowan, Adrian M. Gardner","doi":"10.1063/5.0098274","DOIUrl":"https://doi.org/10.1063/5.0098274","url":null,"abstract":"Organic polymer photocatalysts have garnered much interest in recent years, notably because of their photocatalytic activity toward hydrogen production from water. However, to rationalize the differences in activities between photocatalysts, it is crucial that their photodynamics are understood. Here, we provide an accessible introduction to the use of transient ultraviolet/visible absorption spectroscopy to study the photodynamics of linear polymeric photocatalysts through a review of literature studies. The principles of transient absorption (TA) spectroscopy, and the apparatus required, are briefly described. A step-by-step method to identify key species and unravel their kinetics is provided through exemplar spectra reported within the literature. This review provides the foundations for researchers new to the field of TA spectroscopy to design, perform, and interpret their own TA experiments to probe the photodynamics of organic photocatalysts.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49448345","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}
Organic-based solar cells have developed for the last three decades. Moving forward generally requires the assistance of useful models that are adapted to currently used materials and device architectures. The least understood part of the charge generation is the first step of the exciton dissociation, and new or refined models are being suggested. However, many of today's questions have been asked before, going back almost an entire century. We have gone to the 1930s and attempted to critically review significant contributions on equal footing. We find that Onsager's and Frenkel's models have a similar foundation but were developed to suit very different materials (ions in solutions vs electrons in semiconductors). The contribution by Braun or the Onsager–Braun model can be considered wrong, yet it was instrumental for the field's development. The community practically ignores one of the most promising models (Arkhipov–Baranovskii). Hot exciton dissociation has many faces due to “hot” being a relative term and/or the heat being stored in different ways (electronic, vibronic, etc.). Entropy considerations are instrumental in simplifying the picture, yet they add no physics compared to the full-3D models. We hope that by emphasizing the physical picture of the various models and the underlying assumptions, one could use them as a stepping stone to the next generation models.
{"title":"Charge dissociation in organic solar cells—from Onsager and Frenkel to modern models","authors":"Dan Liraz, N. Tessler","doi":"10.1063/5.0099986","DOIUrl":"https://doi.org/10.1063/5.0099986","url":null,"abstract":"Organic-based solar cells have developed for the last three decades. Moving forward generally requires the assistance of useful models that are adapted to currently used materials and device architectures. The least understood part of the charge generation is the first step of the exciton dissociation, and new or refined models are being suggested. However, many of today's questions have been asked before, going back almost an entire century. We have gone to the 1930s and attempted to critically review significant contributions on equal footing. We find that Onsager's and Frenkel's models have a similar foundation but were developed to suit very different materials (ions in solutions vs electrons in semiconductors). The contribution by Braun or the Onsager–Braun model can be considered wrong, yet it was instrumental for the field's development. The community practically ignores one of the most promising models (Arkhipov–Baranovskii). Hot exciton dissociation has many faces due to “hot” being a relative term and/or the heat being stored in different ways (electronic, vibronic, etc.). Entropy considerations are instrumental in simplifying the picture, yet they add no physics compared to the full-3D models. We hope that by emphasizing the physical picture of the various models and the underlying assumptions, one could use them as a stepping stone to the next generation models.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"42868777","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}
S. Basak, K. Dzieciol, Y. E. Durmus, H. Tempel, H. Kungl, Chandramohan George, J. Mayer, Rüdiger-Albrecht Eichel
In situ transmission electron microscopy (TEM) research has enabled better understanding of various battery chemistries (Li-ion, Li–S, metal–O2, Li, and Na metal based, etc.), which fueled substantial developments in battery technologies. In this review, we highlight some of the recent developments shedding new light on battery materials and electrochemistry via TEM. Studying battery electrode processes depending on the type of electrolytes used and the nature of electrode–electrolyte interfaces established upon battery cycling conditions is key to further adoption of battery technologies. To this end, in situ/ operando TEM methodologies would require accommodating alongside correlation microscopy tools to predict battery interface evolution, reactivity, and stability, for which the use of x-ray computed tomography and image process via machine learning providing complementary information is highlighted. Such combined approaches have potential to translate TEM-based battery results into more direct macroscopic relevance for the optimization of real-world batteries.
{"title":"Characterizing battery materials and electrodes via in situ/operando transmission electron microscopy","authors":"S. Basak, K. Dzieciol, Y. E. Durmus, H. Tempel, H. Kungl, Chandramohan George, J. Mayer, Rüdiger-Albrecht Eichel","doi":"10.1063/5.0075430","DOIUrl":"https://doi.org/10.1063/5.0075430","url":null,"abstract":"In situ transmission electron microscopy (TEM) research has enabled better understanding of various battery chemistries (Li-ion, Li–S, metal–O2, Li, and Na metal based, etc.), which fueled substantial developments in battery technologies. In this review, we highlight some of the recent developments shedding new light on battery materials and electrochemistry via TEM. Studying battery electrode processes depending on the type of electrolytes used and the nature of electrode–electrolyte interfaces established upon battery cycling conditions is key to further adoption of battery technologies. To this end, in situ/ operando TEM methodologies would require accommodating alongside correlation microscopy tools to predict battery interface evolution, reactivity, and stability, for which the use of x-ray computed tomography and image process via machine learning providing complementary information is highlighted. Such combined approaches have potential to translate TEM-based battery results into more direct macroscopic relevance for the optimization of real-world batteries.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43646382","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}
Heterogeneous reactions are highly dependent upon the local structure and environment of the catalyst surface within a nanoscale. Among numerous techniques for monitoring heterogeneous reactions, dark-field microscopy offers reliable data regardless of specific reaction conditions. In addition, plasmonic nanoprobes provide high sensitivity in a sub-wavelength resolution due to localized surface plasmon resonances susceptible to the dielectric change of objects and surroundings. By clever reaction cell design and data analysis, nanoparticle signals can be parallelly analyzed under variable reaction conditions in a controlled manner. This technique effectively measures the heterogeneity of individual nanoparticles for reaction monitoring. A wide range of chemical and electrochemical reactions have been monitored in situ and in operando at a single-particle level in this way. The advancement of localized surface plasmon scatterometry with simulation techniques approaches sub-particle accuracy in a high temporal resolution up to microseconds. Combining other in situ spectroscopic methods would make dark-field scatterometry a versatile tool for various reaction monitoring and sensing applications.
{"title":"Nanoscale reaction monitoring using localized surface plasmon resonance scatterometry","authors":"Hyun-Soo Hwang, Hyunjoon Song","doi":"10.1063/5.0090949","DOIUrl":"https://doi.org/10.1063/5.0090949","url":null,"abstract":"Heterogeneous reactions are highly dependent upon the local structure and environment of the catalyst surface within a nanoscale. Among numerous techniques for monitoring heterogeneous reactions, dark-field microscopy offers reliable data regardless of specific reaction conditions. In addition, plasmonic nanoprobes provide high sensitivity in a sub-wavelength resolution due to localized surface plasmon resonances susceptible to the dielectric change of objects and surroundings. By clever reaction cell design and data analysis, nanoparticle signals can be parallelly analyzed under variable reaction conditions in a controlled manner. This technique effectively measures the heterogeneity of individual nanoparticles for reaction monitoring. A wide range of chemical and electrochemical reactions have been monitored in situ and in operando at a single-particle level in this way. The advancement of localized surface plasmon scatterometry with simulation techniques approaches sub-particle accuracy in a high temporal resolution up to microseconds. Combining other in situ spectroscopic methods would make dark-field scatterometry a versatile tool for various reaction monitoring and sensing applications.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47733102","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}
Entropy is one of the most fundamental quantities in physics. For systems with few degrees of freedom, the value of entropy provides a powerful insight into its microscopic dynamics, such as the number, degeneracy, and relative energies of electronic states, the value of spin, degree of localization and entanglement, and the emergence of exotic states such as non-Abelian anyons. As the size of a system decreases, the conventional methods for measuring entropy, based on heat capacity, quickly become infeasible due to the requirement of increasingly accurate measurements of heat. Several methods to directly measure entropy of mesoscopic quantum systems have recently been developed. These methods use electronic measurements of charge, conductance and thermocurrent, rather than heat, and have been successfully applied to a wide range of systems, from quantum dots and molecules, to quantum Hall states and twisted bilayer graphene. In this Review, we provide an overview of electronic direct entropy measurement methods, discuss their theoretical background, compare their ranges of applicability and look into the directions of their future extensions and applications.
{"title":"Electronic measurements of entropy in meso- and nanoscale systems","authors":"E. Pyurbeeva, J. Mol, P. Gehring","doi":"10.1063/5.0101784","DOIUrl":"https://doi.org/10.1063/5.0101784","url":null,"abstract":"Entropy is one of the most fundamental quantities in physics. For systems with few degrees of freedom, the value of entropy provides a powerful insight into its microscopic dynamics, such as the number, degeneracy, and relative energies of electronic states, the value of spin, degree of localization and entanglement, and the emergence of exotic states such as non-Abelian anyons. As the size of a system decreases, the conventional methods for measuring entropy, based on heat capacity, quickly become infeasible due to the requirement of increasingly accurate measurements of heat. Several methods to directly measure entropy of mesoscopic quantum systems have recently been developed. These methods use electronic measurements of charge, conductance and thermocurrent, rather than heat, and have been successfully applied to a wide range of systems, from quantum dots and molecules, to quantum Hall states and twisted bilayer graphene. In this Review, we provide an overview of electronic direct entropy measurement methods, discuss their theoretical background, compare their ranges of applicability and look into the directions of their future extensions and applications.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47334998","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}
Dong Yang, Norihiko Sasaki, Takuma Shimada, Zhehui Jin, M. Takeuchi, K. Sugiyasu
In this short review, we provide an overview of multistep molecular and macromolecular assembly in syntheses of higher-order structures that are unobtainable under thermodynamic control. As in the case of organic/macromolecular chemistry, a synthetic scheme is designed such that a series of assembly processes eventually leads to a complex structure. The recent progress in this research field has been made based on the mechanistic understandings from viewpoints of both thermodynamics and kinetics. We also describe relevant systems which make use of advanced experimental apparatuses such as optical tweezers, high-speed atomic force microscopy, and so on. The unprecedented structures obtainable in this way might play a pivotal role in bridging the hierarchical levels from the molecular scale to the macroscopic world, leading to new functional supramolecular materials.
{"title":"Multistep molecular and macromolecular assembly for the creation of complex nanostructures","authors":"Dong Yang, Norihiko Sasaki, Takuma Shimada, Zhehui Jin, M. Takeuchi, K. Sugiyasu","doi":"10.1063/5.0079750","DOIUrl":"https://doi.org/10.1063/5.0079750","url":null,"abstract":"In this short review, we provide an overview of multistep molecular and macromolecular assembly in syntheses of higher-order structures that are unobtainable under thermodynamic control. As in the case of organic/macromolecular chemistry, a synthetic scheme is designed such that a series of assembly processes eventually leads to a complex structure. The recent progress in this research field has been made based on the mechanistic understandings from viewpoints of both thermodynamics and kinetics. We also describe relevant systems which make use of advanced experimental apparatuses such as optical tweezers, high-speed atomic force microscopy, and so on. The unprecedented structures obtainable in this way might play a pivotal role in bridging the hierarchical levels from the molecular scale to the macroscopic world, leading to new functional supramolecular materials.","PeriodicalId":72559,"journal":{"name":"Chemical physics reviews","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"46220107","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}
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