Femtosecond Soft X-ray Spectroscopy of Solvated Transition-Metal Complexes: Deciphering the Interplay of Electronic and Structural Dynamics

被引：168

作者：

Huse, Nils ^{[1
]}

Cho, Hana ^{[1
,2
,3
]}

Hong, Kiryong ^{[2
,3
]}

Jamula, Lindsey ^{[4
]}

de Groot, Frank M. F. ^{[5
]}

Kim, Tae Kyu ^{[2
,3
]}

McCusker, James K. ^{[4
]}

Schoenlein, Robert W. ^{[1
]}

机构：

[1] Univ Calif Berkeley, Lawrence Berkeley Lab, Ultrafast Xray Sci Lab, Div Chem Sci, Berkeley, CA 94720 USA

[2] Pusan Natl Univ, Dept Chem, Pusan 609735, South Korea

[3] Pusan Natl Univ, Chem Inst Funct Mat, Pusan 609735, South Korea

[4] Michigan State Univ, Dept Chem, E Lansing, MI 48824 USA

[5] Univ Utrecht, Dept Chem, NL-3584 Utrecht, Netherlands

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2011年 / 2卷 / 08期

关键词：

HIGH-SPIN STATE; WATER;

D O I：

10.1021/jz200168m

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

We present the first implementation of femtosecond soft X-ray spectroscopy as an ultrafast direct probe of the excited-state valence orbitals in solution phase molecules. This method is applied to photoinduced spin crossover of [Fe(tren(py)(3))](2+), where the ultrafast spin state conversion of the metal ion, initiated by metal-to-ligand charge transfer excitation, is directly measured using the intrinsic spin state selectivity of the soft X-ray L-edge transitions. Our results provide important experimental data concerning the mechanism of ultrafast spin state conversion and subsequent electronic and structural dynamics, highlighting the potential of this technique to study ultrafast phenomena in the solution phase.

引用

页码：880 / 884

页数：5

共 26 条

[1]

[Anonymous], SPIN CROSSOVER TRANS

[2]

Aziz EF, 2010, NAT CHEM, V2, P853, DOI [10.1038/NCHEM.768, 10.1038/nchem.768]

[3] Femtosecond XANES Study of the Light-Induced Spin Crossover Dynamics in an Iron(II) Complex [J].