Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 2, Issue 8, Pages 880-884Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz200168m
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Funding
- Office of Science, Office of Basic Energy Sciences, the Chemical Sciences, Geosciences, and Biosciences Division under the Department of Energy [AC02-05CH11231, DE-FG02-01ER15282]
- Ministry of Education, Science and Technology [2009-0068446, 2010-0006570]
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
- National Research Foundation of Korea [2010-0006570, 2009-0068446] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- U.S. Department of Energy (DOE) [DE-FG02-01ER15282] Funding Source: U.S. Department of Energy (DOE)
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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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