title: Femtosecond Soft X-ray Spectroscopy of Solvated Transition-Metal Complexes: Deciphering the Interplay of Electronic and Structural Dynamics.
abstract: 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.
authors: †Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
authors: Nils
authors: N
authors: Huse
authors: †Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.|‡Department of Chemistry and Chemistry Institute of Functional Materials, Pusan National University, Busan 609-735, Republic of Korea.
authors: Hana
authors: H
authors: Cho
authors: ‡Department of Chemistry and Chemistry Institute of Functional Materials, Pusan National University, Busan 609-735, Republic of Korea.
authors: Kiryong
authors: K
authors: Hong
authors: §Department of Chemistry, Michigan State University, East Lansing, Michigan 48824, United States.
authors: Lindsey
authors: L
authors: Jamula
authors: ⊥Department of Chemistry, Utrecht University, 3584 Utrecht, Netherlands.
authors: Frank M F
authors: FM
authors: de Groot
authors: ‡Department of Chemistry and Chemistry Institute of Functional Materials, Pusan National University, Busan 609-735, Republic of Korea.
authors: Tae Kyu
authors: TK
authors: Kim
authors: §Department of Chemistry, Michigan State University, East Lansing, Michigan 48824, United States.
authors: James K
authors: JK
authors: McCusker
authors: †Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
authors: Robert W
authors: RW
authors: Schoenlein
keywords: X-ray absorption spectroscopy; charge transfer; femtochemistry; spin crossover; structural dynamics; transition metals