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

Nils Huse; Hana Cho; Kiryong Hong; Lindsey Jamula; Frank M. F. de Groot; Tae Kyu Kim; James K. McCusker; Robert W. Schoenlein

doi:10.1021/jz200168m

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

Nils Huse^*, Hana Cho, Kiryong Hong, Lindsey Jamula, Frank M. F. de Groot, Tae Kyu Kim, James K. McCusker, Robert W. Schoenlein

^*Corresponding author for this work

Sub Inorganic Chemistry and Catalysis

Research output: Contribution to journal › Article › Academic › peer-review

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.

Original language	English
Pages (from-to)	880-884
Number of pages	5
Journal	Journal of Physical Chemistry Letters
Volume	2
Issue number	8
DOIs	https://doi.org/10.1021/jz200168m
Publication status	Published - 21 Apr 2011

Funding

This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, the Chemical Sciences, Geosciences, and Biosciences Division under the Department of Energy, Contract No. DE-AC02-05CH11231 (N.H., H.C., and R.W.S.) and Grant No. DE-FG02-01ER15282 (J.K.M.), as well as the Basic Science Research Program 2009-0068446 and 2010-0006570 through the National Research Foundation of Korea (NRF) funded by the Ministry of Education, Science and Technology (T.K.K.). The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.

Keywords

HIGH-SPIN STATE
CHARGE-TRANSFER
WATER

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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.",

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author = "Nils Huse and Hana Cho and Kiryong Hong and Lindsey Jamula and {de Groot}, {Frank M. F.} and Kim, {Tae Kyu} and McCusker, {James K.} and Schoenlein, {Robert W.}",

year = "2011",

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doi = "10.1021/jz200168m",

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AU - Huse, Nils

AU - Cho, Hana

AU - Hong, Kiryong

AU - Jamula, Lindsey

AU - de Groot, Frank M. F.

AU - Kim, Tae Kyu

AU - McCusker, James K.

AU - Schoenlein, Robert W.

PY - 2011/4/21

Y1 - 2011/4/21

N2 - 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.

AB - 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.

KW - HIGH-SPIN STATE

KW - CHARGE-TRANSFER

KW - WATER

U2 - 10.1021/jz200168m

DO - 10.1021/jz200168m

M3 - Article

SN - 1948-7185

VL - 2

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EP - 884

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

IS - 8

ER -

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

Abstract

Funding

Keywords

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