Direct Probing of Spin State Dynamics Coupled with Electronic and Structural Modifications by Picosecond Time-Resolved XAFS

被引:65
作者
Nozawa, Shunsuke [1 ,5 ]
Sato, Tokushi [2 ]
Chollet, Matthieu [2 ]
Ichiyanagi, Kouhei [5 ]
Tomita, Ayana [2 ]
Fujii, Hiroshi [3 ,4 ,5 ]
Adachi, Shin-ichi
Koshihara, Shin-ya [2 ]
机构
[1] Japan Sci & Technol Agcy, ERATO, Tsukuba, Ibaraki 3050801, Japan
[2] Tokyo Inst Technol, Meguro Ku, Tokyo 1528551, Japan
[3] Inst Mol Sci, Okazaki, Aichi 4448787, Japan
[4] Natl Inst Nat Sci, Okazaki Inst Integrat Biosci, Okazaki, Aichi 4448787, Japan
[5] High Energy Accelerator Res Org, Tsukuba, Ibaraki 3050801, Japan
关键词
TRANSIENT MOLECULAR-STRUCTURES; X-RAY; K-EDGE; PHOTODISSOCIATION; SPECTROSCOPY; TRANSITION; COMPLEXES; TRACKING;
D O I
10.1021/ja907460b
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The first direct observation of the transient spin-state in a disordered magnetic system with time-resolved XAFS is reported. By observing the evolution of the Fe-II 1s -3d transition, the spin crossover transition from the (1)A(1) low spin state to T-5(2) high spin state has been directly observed on a picosecond time scale. Moreover, observation of the transient spin state with time-resolved XAFS allows for the investigation of the variations in the electronic state and molecular structure. This unique experimental technique probes the excited states involved in the ultrafast photoinduced reactions in disordered magnetic systems.
引用
收藏
页码:61 / +
页数:5
相关论文
共 36 条
[1]   Novel photocatalyst: Titania-coated magnetite. Activity and photodissolution [J].
Beydoun, D ;
Amal, R ;
Low, GKC ;
McEvoy, S .
JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (18) :4387-4396
[3]   Ultrafast X-ray absorption spectroscopy [J].
Bressler, C ;
Chergui, M .
CHEMICAL REVIEWS, 2004, 104 (04) :1781-1812
[4]   Towards structural dynamics in condensed chemical systems exploiting ultrafast time-resolved x-ray absorption spectroscopy [J].
Bressler, C ;
Saes, M ;
Chergui, M ;
Grolimund, D ;
Abela, R ;
Pattison, P .
JOURNAL OF CHEMICAL PHYSICS, 2002, 116 (07) :2955-2966
[5]   Femtosecond XANES Study of the Light-Induced Spin Crossover Dynamics in an Iron(II) Complex [J].
Bressler, Ch. ;
Milne, C. ;
Pham, V. -T. ;
ElNahhas, A. ;
van der Veen, R. M. ;
Gawelda, W. ;
Johnson, S. ;
Beaud, P. ;
Grolimund, D. ;
Kaiser, M. ;
Borca, C. N. ;
Ingold, G. ;
Abela, R. ;
Chergui, M. .
SCIENCE, 2009, 323 (5913) :489-492
[6]   Importance of photoelectron multiple scattering in the iron K-edge X-ray absorption spectra of spin-crossover complexes: Full multiple scattering calculations for several iron(II) trispyrazolylborate and trispyrazolylmethane complexes [J].
Briois, V ;
Sainctavit, P ;
Long, GJ ;
Grandjean, F .
INORGANIC CHEMISTRY, 2001, 40 (05) :912-918
[7]   Tracking the structural dynamics of proteins in solution using time-resolved wide-angle X-ray scattering [J].
Cammarata, Marco ;
Levantino, Matteo ;
Schotte, Friedrich ;
Anfinrud, Philip A. ;
Ewald, Friederike ;
Choi, Jungkweon ;
Cupane, Antonio ;
Wulff, Michael ;
Ihee, Hyotcherl .
NATURE METHODS, 2008, 5 (10) :881-886
[8]   Tracking electrons and atoms in a photoexcited metalloporphyrin by X-ray transient absorption spectroscopy [J].
Chen, Lin X. ;
Zhang, Xiaoyi ;
Wasinger, Erik C. ;
Attenkofer, Klaus ;
Jennings, Guy ;
Muresan, Ana Z. ;
Lindsey, Jonathan S. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (31) :9616-+
[9]   Probing transient molecular structures in photochemical processes using laser-initiated time-resolved X-ray absorption spectroscopy [J].
Chen, LX .
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 2005, 56 :221-254
[10]   Taking snapshots of photoexcited molecules in disordered media by using pulsed synchrotron X-rays [J].
Chen, LX .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2004, 43 (22) :2886-2905