【 Abstract 】 Stimulated by the discovery of high-TC superconductivity in 1986, band-filling-control of strongly-correlated electron systems have been a persistent challenge for past three decades in condensed matter science. Especially, recent efforts have been focused on electrostatic carrier doping of such materials utilizing field-effect transistor (FET) structures to find novel superconductivity. In this presentation, recent results on the development of novel superconducting (SC) organic FETs, such as strain-tunable SC FET and light-controllable SC FET are summarized. The techniques and knowledge described here will contribute to the advances in future superconducting electronics as well as the understanding of superconductivity in strongly-correlated electron systems.
{"title":"Development of Novel Phase Transition Devices Utilizing Strongly-correlated Molecular Conductors","authors":"M. Suda","doi":"10.3175/MOLSCI.11.A0092","DOIUrl":"https://doi.org/10.3175/MOLSCI.11.A0092","url":null,"abstract":"【 Abstract 】 Stimulated by the discovery of high-TC superconductivity in 1986, band-filling-control of strongly-correlated electron systems have been a persistent challenge for past three decades in condensed matter science. Especially, recent efforts have been focused on electrostatic carrier doping of such materials utilizing field-effect transistor (FET) structures to find novel superconductivity. In this presentation, recent results on the development of novel superconducting (SC) organic FETs, such as strain-tunable SC FET and light-controllable SC FET are summarized. The techniques and knowledge described here will contribute to the advances in future superconducting electronics as well as the understanding of superconductivity in strongly-correlated electron systems.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"36 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"91381609","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}
Microbial rhodopsin is a photo-receptive membrane protein of micro-organisms. The most ubiquitous microbial rhodopsins are light-driven ion pumps which actively transport H+ or Clagainst membrane chemical potential. In 2013, we reported a new class of ion pump rhodopsin, sodium pump rhodopsin (KR2) which outwardly transports Na+ ion by the use of light energy. The mechanism of Na+ transport by KR2 was investigated in spectroscopic and crystallographic studies. The results showed that the H+ transfer between photoisomerized retinal Schiff base and its counter ion, Asp116, is a critical process for the Na+-transport function. After this H+ transfer, the protonated Asp116 sequesters the H+ from the ion-transport pathway, and then immediately Na+ is taken up from the cytoplasmic side. The Na+ binds to the site composed of Asn112 and Asp251, and simultaneously H+ goes back to the retinal Schiff base. Then, positive charge of the reprotonated retinal Schiff-base prevents the back flow of Na+ to the cytoplasmic side. Finally, the Na+ is released to the extracellular side. Furthermore, on the basis of structural insights about KR2, we have succeeded to develop new artificial K+ and Cs+ pumping KR2 mutants, KR2K+ and KR2Cs+, respectively. Wildtype KR2 and these mutants are expected to provide new ways of the application to optogenetics.
{"title":"The Study on a Novel Light-driven Sodium Pump and Creation of New Functional Molecules","authors":"Keiichi Inoue","doi":"10.3175/MOLSCI.10.A0086","DOIUrl":"https://doi.org/10.3175/MOLSCI.10.A0086","url":null,"abstract":"Microbial rhodopsin is a photo-receptive membrane protein of micro-organisms. The most ubiquitous microbial rhodopsins are light-driven ion pumps which actively transport H+ or Clagainst membrane chemical potential. In 2013, we reported a new class of ion pump rhodopsin, sodium pump rhodopsin (KR2) which outwardly transports Na+ ion by the use of light energy. The mechanism of Na+ transport by KR2 was investigated in spectroscopic and crystallographic studies. The results showed that the H+ transfer between photoisomerized retinal Schiff base and its counter ion, Asp116, is a critical process for the Na+-transport function. After this H+ transfer, the protonated Asp116 sequesters the H+ from the ion-transport pathway, and then immediately Na+ is taken up from the cytoplasmic side. The Na+ binds to the site composed of Asn112 and Asp251, and simultaneously H+ goes back to the retinal Schiff base. Then, positive charge of the reprotonated retinal Schiff-base prevents the back flow of Na+ to the cytoplasmic side. Finally, the Na+ is released to the extracellular side. Furthermore, on the basis of structural insights about KR2, we have succeeded to develop new artificial K+ and Cs+ pumping KR2 mutants, KR2K+ and KR2Cs+, respectively. Wildtype KR2 and these mutants are expected to provide new ways of the application to optogenetics.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"10 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2016-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"89357421","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}
{"title":"Reports from a Tiny Science Lab of Hands-on Activities for School Kids","authors":"N. Mikami","doi":"10.3175/MOLSCI.10.A0083","DOIUrl":"https://doi.org/10.3175/MOLSCI.10.A0083","url":null,"abstract":"","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"27 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2016-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"89602704","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}
Dynamics of solvent molecules around a solute molecule plays a crucial role in chemical and biological processes, such as chemical reactivity, biological recognition, and hydrophobic interaction. Though extensive studies on the solvation dynamics have been carried out, the single molecular level information about the dynamics is hard to obtain in the condensed phase suffered by averaging effects over solvent molecules in various environments. In this study, gas phase hydrated clusters, for which size and orientation of hydration can be specifically defined, are utilized as a model system to elucidate the solvation dynamics in a molecular specific fashion by complementary use of picosecond time resolved IR spectroscopy and on-the-fly DFT MD simulation. An ionization induced CO → NH water reorientation in the CO bound acetanilide–water cluster was investigated as the first example of solvent reorientation. The time resolved IR spectra revealed that the reaction has an intermediate and takes ca. 6 ps to finish the reorientation. The MD simulation showed that the reaction is composed of two different channels; one is a fast channel in which the water molecule travels around the CH 3 group and the other is a slow channel in which water molecule once stays above the molecular plane. This detailed information about the water reorientation dynamics is first obtained by introducing a new dimen-sion, i.e. time, into the established method of determining static cluster structures, IR spectroscopy + quantum chemical calculations. This concept would open a new stage to study dynamic processes in the molecular level using gas phase solvated clusters.
{"title":"Revealing Single Molecular Solvent Reorientation Dynamics by Complementary Use of Picosecond Time Resolved IR Spectroscopy and MD Simulation","authors":"M. Miyazaki","doi":"10.3175/MOLSCI.10.A0087","DOIUrl":"https://doi.org/10.3175/MOLSCI.10.A0087","url":null,"abstract":"Dynamics of solvent molecules around a solute molecule plays a crucial role in chemical and biological processes, such as chemical reactivity, biological recognition, and hydrophobic interaction. Though extensive studies on the solvation dynamics have been carried out, the single molecular level information about the dynamics is hard to obtain in the condensed phase suffered by averaging effects over solvent molecules in various environments. In this study, gas phase hydrated clusters, for which size and orientation of hydration can be specifically defined, are utilized as a model system to elucidate the solvation dynamics in a molecular specific fashion by complementary use of picosecond time resolved IR spectroscopy and on-the-fly DFT MD simulation. An ionization induced CO → NH water reorientation in the CO bound acetanilide–water cluster was investigated as the first example of solvent reorientation. The time resolved IR spectra revealed that the reaction has an intermediate and takes ca. 6 ps to finish the reorientation. The MD simulation showed that the reaction is composed of two different channels; one is a fast channel in which the water molecule travels around the CH 3 group and the other is a slow channel in which water molecule once stays above the molecular plane. This detailed information about the water reorientation dynamics is first obtained by introducing a new dimen-sion, i.e. time, into the established method of determining static cluster structures, IR spectroscopy + quantum chemical calculations. This concept would open a new stage to study dynamic processes in the molecular level using gas phase solvated clusters.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"16 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2016-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"90832818","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}
{"title":"Nuclear and Electron Wave Packet Molecular Dynamics Simulation Method and Its Application to Liquid, Solid and Supercooled Hydrogens: ―分子から固体まで―","authors":"Hyeon-Deuk Kim","doi":"10.3175/MOLSCI.10.A0084","DOIUrl":"https://doi.org/10.3175/MOLSCI.10.A0084","url":null,"abstract":"","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"15 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2016-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"85476227","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}
Vibrational spectroscopy is a viable tool to reveal the mechanism of various molecular systems at the atomic and molecular resolution; yet the interpretation of the observed spectrum is often non-trivial and requires a theoretical assistance. Although it is rather common to calculate the vibrational spectrum based on the harmonic approximation, anharmonicity plays a crucial role, in particular, for the OH and NH stretching vibrations that lie in a high frequency region. In this article, recent advances in the vibrational structure theory are reviewed regarding: (1) The generation of anharmonic potential energy surface by the electronic structure calculation, (2) An efficient solver of vibrational Schrödinger equation by the vibrational quasi-degenerate perturbation theory based on variationally optimized coordinates, (3) A weight average approach to simulate the vibrational spectrum of condensed phase systems.
{"title":"Development of Molecular Vibrational Structure Theory with an Explicit Account of Anharmonicity","authors":"K. Yagi","doi":"10.3175/MOLSCI.10.A0085","DOIUrl":"https://doi.org/10.3175/MOLSCI.10.A0085","url":null,"abstract":"Vibrational spectroscopy is a viable tool to reveal the mechanism of various molecular systems at the atomic and molecular resolution; yet the interpretation of the observed spectrum is often non-trivial and requires a theoretical assistance. Although it is rather common to calculate the vibrational spectrum based on the harmonic approximation, anharmonicity plays a crucial role, in particular, for the OH and NH stretching vibrations that lie in a high frequency region. In this article, recent advances in the vibrational structure theory are reviewed regarding: (1) The generation of anharmonic potential energy surface by the electronic structure calculation, (2) An efficient solver of vibrational Schrödinger equation by the vibrational quasi-degenerate perturbation theory based on variationally optimized coordinates, (3) A weight average approach to simulate the vibrational spectrum of condensed phase systems.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"24 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2016-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"86736249","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}
We performed femtosecond reflection spectroscopy on a series of perovskite-type cobalt oxide, R BaCo 2 O 6- d ( R = Sm, Gd, and Tb). The transient reflectivity as well as the optical conductivity just after photoirradiation shows ultrafast change within the time resolution (ca. 120 fs) at room temperature, implying appearance of a hidden state different from the high temperature phase. The transferred spectral weight in the optical conductivity by the photoexcitation sensitively depends on the R -species. i.e ., transfer of the d electron. Recent theoretical treatment which quantitatively succeeded in reproducing the transfer dependence of the excited state indicates that the photoirradiation causes locally ferromag-netic state via double-exchange interaction between the injected hole and spins of Co ion, which can be viewed as a novel example of photoinduced phase transition.
我们对一系列钙钛矿型氧化钴R BaCo 2 O 6- d (R = Sm, Gd和Tb)进行了飞秒反射光谱分析。光辐照后的瞬态反射率和光电导率在室温下表现出超快的时间分辨率(约120fs)变化，这意味着出现了不同于高温相的隐藏态。光激发引起的光电导率中传递的谱权敏感地依赖于R -基团。也就是d电子的转移。最近的理论处理成功地定量再现了激发态的转移依赖关系，表明光照射通过注入空穴和Co离子自旋之间的双重交换相互作用引起局部铁磁态，这可以看作是光诱导相变的一个新例子。
{"title":"Novel Photo-excited State and Femtosecond Dynamics in Perovskite-type Cobalt Oxides","authors":"Y. Okimoto","doi":"10.3175/MOLSCI.10.A0088","DOIUrl":"https://doi.org/10.3175/MOLSCI.10.A0088","url":null,"abstract":"We performed femtosecond reflection spectroscopy on a series of perovskite-type cobalt oxide, R BaCo 2 O 6- d ( R = Sm, Gd, and Tb). The transient reflectivity as well as the optical conductivity just after photoirradiation shows ultrafast change within the time resolution (ca. 120 fs) at room temperature, implying appearance of a hidden state different from the high temperature phase. The transferred spectral weight in the optical conductivity by the photoexcitation sensitively depends on the R -species. i.e ., transfer of the d electron. Recent theoretical treatment which quantitatively succeeded in reproducing the transfer dependence of the excited state indicates that the photoirradiation causes locally ferromag-netic state via double-exchange interaction between the injected hole and spins of Co ion, which can be viewed as a novel example of photoinduced phase transition.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2016-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"88801065","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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