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DOI | 10.1038/s41467-018-07833-3 |
Transient metal-centered states mediate isomerization of a photochromic rutheniumsulfoxide complex | |
Cordones, Amy A.1; Lee, Jae Hyuk2; Hong, Kiryong3; Cho, Hana4; Garg, Komal5; Boggio-Pasqua, Martial6,7; Rack, Jeffrey J.5,8; Huse, Nils9,10,11; Schoenlein, Robert W.1,12; Kim, Tae Kyu13,14 | |
2018-05-18 | |
发表期刊 | NATURE COMMUNICATIONS |
ISSN | 2041-1723 |
出版年 | 2018 |
卷号 | 9 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; South Korea; France; Germany |
英文摘要 | Ultrafast isomerization reactions underpin many processes in (bio)chemical systems and molecular materials. Understanding the coupled evolution of atomic and molecular structure during isomerization is paramount for control and rational design in molecular science. Here we report transient X-ray absorption studies of the photo-induced linkage isomerization of a Ru-based photochromic molecule. X-ray spectra reveal the spin and valence charge of the Ru atom and provide experimental evidence that metal-centered excited states mediate isomerization. Complementary X-ray spectra of the functional ligand S atoms probe the nuclear structural rearrangements, highlighting the formation of two metal-centered states with different metal-ligand bonding. These results address an essential open question regarding the relative roles of transient charge-transfer and metal-centered states in mediating photoisomerization. Global temporal and spectral data analysis combined with time-dependent density functional theory reveals a complex mechanism for photoisomerization with atomic details of the transient molecular and electronic structure not accessible by other means. |
领域 | 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000432444100003 |
WOS关键词 | RAY-ABSORPTION-SPECTROSCOPY ; DENSITY-FUNCTIONAL THEORY ; SULFOXIDE COMPLEXES ; EXCITED-STATE ; CONICAL INTERSECTION ; ELECTRONIC-STRUCTURE ; PHOTOISOMERIZATION MECHANISM ; FEMTOSECOND ISOMERIZATION ; MOLECULAR-STRUCTURE ; NITROSYL COMPLEX |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/204133 |
专题 | 资源环境科学 |
作者单位 | 1.Stanford Univ, PULSE Inst, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA; 2.Pohang Accelerator Lab, Pohang 37673, South Korea; 3.Korea Res Inst Stand & Sci, Ctr Gas Anal, Div Chem & Med Metrol, Daejeon 34113, South Korea; 4.Korea Res Inst Stand & Sci, Ctr Analyt Chem, Div Chem & Med Metrol, Daejeon 34113, South Korea; 5.Ohio Univ, Nanoscale & Quantum Phenomena Inst, Dept Chem & Biochem, Athens, OH 45701 USA; 6.CNRS, Lab Chim & Phys Quant, F-31062 Toulouse, France; 7.Univ Toulouse, IRSAMC, UMR 5626, 118 Route Narbonne, F-31062 Toulouse, France; 8.Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA; 9.Univ Hamburg, Dept Phys, Inst Nanostruct & Solid State Phys, D-22761 Hamburg, Germany; 10.Max Planck Inst Struct & Dynam Matter, D-22761 Hamburg, Germany; 11.Ctr Free Elect Laser Sci, D-22761 Hamburg, Germany; 12.SLAC Natl Accelerator, LCLS, Menlo Pk, CA 94025 USA; 13.Pusan Natl Univ, Dept Chem, Busan 46241, South Korea; 14.Pusan Natl Univ, Chem Inst Funct Mat, Busan 46241, South Korea |
推荐引用方式 GB/T 7714 | Cordones, Amy A.,Lee, Jae Hyuk,Hong, Kiryong,et al. Transient metal-centered states mediate isomerization of a photochromic rutheniumsulfoxide complex[J]. NATURE COMMUNICATIONS,2018,9. |
APA | Cordones, Amy A..,Lee, Jae Hyuk.,Hong, Kiryong.,Cho, Hana.,Garg, Komal.,...&Kim, Tae Kyu.(2018).Transient metal-centered states mediate isomerization of a photochromic rutheniumsulfoxide complex.NATURE COMMUNICATIONS,9. |
MLA | Cordones, Amy A.,et al."Transient metal-centered states mediate isomerization of a photochromic rutheniumsulfoxide complex".NATURE COMMUNICATIONS 9(2018). |
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