期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 7, 期 3, 页码 465-470出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.5b02509
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资金
- Office of Science, Office of Basic Energy Sciences, the Chemical Sciences, Geosciences, and Biosciences Division under the Department of Energy [DE-AC02-05CH11231]
- Office of Basic Energy Sciences of the U.S. Department of Energy [DE-SC0002190]
- National Research Foundation of Korea [2007-0056095, 2013S1A2A2035406, 2013R1A1A2009575, 2014R1A4A1001690]
- Global Research Laboratory Program [2009-00439]
- Max Planck POSTECH/KOREA Research Initiative Program through the National Research Foundation of Korea (NRF) - Ministry of Science, ICT AMP
- Future Planning [2011-0031558]
- Max Planck Society
- City of Hamburg
Time-resolved nitrogen-1s spectroscopy in the X-ray water window is presented as a novel probe of metal-ligand interactions and transient states in nitrogen containing organic compounds. New information on iron(II) polypyridyl complexes via nitrogen core-level transitions yields insight into the charge density of the photoinduced high-spin state by comparing experimental results with time-dependent density functional theory. In the transient high-spin state, the 3d electrons of the metal center are more delocalized over the nearest-neighbor nitrogen atoms despite increased bond lengths. Our findings point to a strong coupling of electronic states with charge-transfer character, facilitating the ultrafast intersystem crossing cascade in these systems. The study also highlights the importance of local charge density measures to complement chemical interaction concepts of charge donation and back-bonding with molecular orbital descriptions of states.
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