Soft x-ray spectroscopies which utilize electronic transition of core electrons are known as a powerful tool for observing electronic structures, and are extensively applied to solid and gaseous samples in vacuum. While soft x-ray requires a vacuum because of its low penetration ability, one cannot hold liquid phase samples in vacuum due to the vaporization of liquids. Therefore, soft x-ray measurement of liquid samples was one of the difficult experiments only a decade ago. Recently, extensive developments in experimental techniques have enabled the application of x-ray emission and absorption spectroscopy to liquid and solution samples. In this article, our recent investigations on electronic state concerning liquid structure of water using soft x-ray beamline BL17SU in third generation synchrotron facility SPring-8 are reviewed. In addition, the development of experimental apparatus dedicated to the research of liquid and solution samples is presented.
{"title":"Developments of a Liquid Flow Cell for Soft x-ray Spectroscopy and Observations of Water Molecules in Liquid Solutions","authors":"T. Tokushima","doi":"10.3175/molsci.9.a0077","DOIUrl":"https://doi.org/10.3175/molsci.9.a0077","url":null,"abstract":"Soft x-ray spectroscopies which utilize electronic transition of core electrons are known as a powerful tool for observing electronic structures, and are extensively applied to solid and gaseous samples in vacuum. While soft x-ray requires a vacuum because of its low penetration ability, one cannot hold liquid phase samples in vacuum due to the vaporization of liquids. Therefore, soft x-ray measurement of liquid samples was one of the difficult experiments only a decade ago. Recently, extensive developments in experimental techniques have enabled the application of x-ray emission and absorption spectroscopy to liquid and solution samples. In this article, our recent investigations on electronic state concerning liquid structure of water using soft x-ray beamline BL17SU in third generation synchrotron facility SPring-8 are reviewed. In addition, the development of experimental apparatus dedicated to the research of liquid and solution samples is presented.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"305 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2015-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79816511","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}
Laser desorption supersonic jet spectroscopy, which can enable the conformer-selected measurements, was improved by optimizing the matrix substances and introducing a high-pressure supersonic jet expansion to obtain high desorption efficiency and high jet-cooling effect. The improved laser desorption supersonic jet technique was applied to catecholamine neurotransmitters and their relevant molecules. By using resonance enhanced multiphoton ionization and UV-UV hole burning spectroscopies, the number of conformers of each molecule was determined. By comparing them, we found a propensity rule, named as “doubling rule”, in the conformational evolution of relevant molecules. However, the numbers of conformers of catecholamines are much less than the expected ones by the doubling rule. Thus we concluded that the numbers of conformers of catecholamines are specifically small. We discussed the reason of decreasing the number of conformers of catecholamines, and which was interpreted as due to the specific flexibility of catecholamines.
{"title":"Gas Phase Spectroscopy of Catecholamines and Relevant Molecules by Laser Desorption Supersonic Jet Technique","authors":"S. Ishiuchi","doi":"10.3175/molsci.9.a0075","DOIUrl":"https://doi.org/10.3175/molsci.9.a0075","url":null,"abstract":"Laser desorption supersonic jet spectroscopy, which can enable the conformer-selected measurements, was improved by optimizing the matrix substances and introducing a high-pressure supersonic jet expansion to obtain high desorption efficiency and high jet-cooling effect. The improved laser desorption supersonic jet technique was applied to catecholamine neurotransmitters and their relevant molecules. By using resonance enhanced multiphoton ionization and UV-UV hole burning spectroscopies, the number of conformers of each molecule was determined. By comparing them, we found a propensity rule, named as “doubling rule”, in the conformational evolution of relevant molecules. However, the numbers of conformers of catecholamines are much less than the expected ones by the doubling rule. Thus we concluded that the numbers of conformers of catecholamines are specifically small. We discussed the reason of decreasing the number of conformers of catecholamines, and which was interpreted as due to the specific flexibility of catecholamines.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"90 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2015-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"91463218","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":"Being Charmed by Mysterious High-resolution Spectra of Molecules","authors":"Koichi M. T. Yamada","doi":"10.3175/molsci.9.a0074","DOIUrl":"https://doi.org/10.3175/molsci.9.a0074","url":null,"abstract":"","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"59 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2015-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"78718220","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}
In recent years much of interest in atmospheric chemistry has been focused on atmospheric aerosols. In this article, laboratory kinetic studies and related quantum chemical theoretical studies on typical processes of formation and transformation of organic aerosols have been reviewed. Specifically, it targets on the topics of heterogeneous reactions of atmospheric O3 and OH with organic compounds at the surface of aerosols, and aqueous-phase reactions of dialdehydes (glyoxal and methylglyoxal) in cloud and aerosol particles. In order to attain better understanding on such processes, fundamental studies based on molecular science are needed, and closer collaboration between atmospheric chemistry and theoretical computational chemistry is proposed.
{"title":"Atmospheric Heterogeneous Reaction Chemistry and Theoretical Molecular Science","authors":"H. Akimoto","doi":"10.3175/MOLSCI.9.A0079","DOIUrl":"https://doi.org/10.3175/MOLSCI.9.A0079","url":null,"abstract":"In recent years much of interest in atmospheric chemistry has been focused on atmospheric aerosols. In this article, laboratory kinetic studies and related quantum chemical theoretical studies on typical processes of formation and transformation of organic aerosols have been reviewed. Specifically, it targets on the topics of heterogeneous reactions of atmospheric O3 and OH with organic compounds at the surface of aerosols, and aqueous-phase reactions of dialdehydes (glyoxal and methylglyoxal) in cloud and aerosol particles. In order to attain better understanding on such processes, fundamental studies based on molecular science are needed, and closer collaboration between atmospheric chemistry and theoretical computational chemistry is proposed.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"263 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2015-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"73559934","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 functional crystals with novel π-electronic states such as (super)conductivity, (anti-/ferro)magnetism, etc. have been vigorously developed. On the other hand, researches of hydrogen-related functionalities such as (anti-/ferro) electrics, proton (super)conductivity, etc. have been also extensively performed. In this article, the novel π-electronhydrogen concerted organic materials and their functionalities are introduced. This phenomenon with dynamically coupled π electron-hydrogen might be related to biochemical cascade reactions and applicable to novel organic surface and devices.
{"title":"Development of novel functional properties of organic crystals in concert of π-electrons and hydrogens: —π電子と水素の協奏—","authors":"H. Mori","doi":"10.3175/molsci.9.a0081","DOIUrl":"https://doi.org/10.3175/molsci.9.a0081","url":null,"abstract":"Organic functional crystals with novel π-electronic states such as (super)conductivity, (anti-/ferro)magnetism, etc. have been vigorously developed. On the other hand, researches of hydrogen-related functionalities such as (anti-/ferro) electrics, proton (super)conductivity, etc. have been also extensively performed. In this article, the novel π-electronhydrogen concerted organic materials and their functionalities are introduced. This phenomenon with dynamically coupled π electron-hydrogen might be related to biochemical cascade reactions and applicable to novel organic surface and devices.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"33 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2015-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"74489667","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}
Single-walled carbon nanotubes are one of the candidate materials for the next generation electronics, such as printed, flexible, stretchable and wearable electronics due to their chemical stability, printability, flexibility, light-weight, and unique mechanical properties. In particularly, a combination of single-walled carbon nanotubes with electrolytes reveals rich and novel functionalities. This review describes recently demonstrated functional devices, such as inkjet-printed, extremely flexible, electrolyte-gated transistors.
{"title":"Novel Functional Devices of Single-walled Carbon Nanotubes","authors":"T. Takenobu","doi":"10.3175/MOLSCI.9.A0080","DOIUrl":"https://doi.org/10.3175/MOLSCI.9.A0080","url":null,"abstract":"Single-walled carbon nanotubes are one of the candidate materials for the next generation electronics, such as printed, flexible, stretchable and wearable electronics due to their chemical stability, printability, flexibility, light-weight, and unique mechanical properties. In particularly, a combination of single-walled carbon nanotubes with electrolytes reveals rich and novel functionalities. This review describes recently demonstrated functional devices, such as inkjet-printed, extremely flexible, electrolyte-gated transistors.","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"50 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2015-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"78366286","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":"Looking Back Fifty Years of Collaboration with Experimentalists","authors":"K. Morokuma","doi":"10.3175/MOLSCI.8.A0065","DOIUrl":"https://doi.org/10.3175/MOLSCI.8.A0065","url":null,"abstract":"","PeriodicalId":19105,"journal":{"name":"Molecular Science","volume":"56 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2014-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"87748707","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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