期刊
JOURNAL OF PHYSICAL CHEMISTRY A
卷 115, 期 10, 页码 1804-1809出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp110905h
关键词
-
资金
- Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy [DE-FG02-03ER15452]
Rotations about its three carbon nitrogen bonds give triethylamine a complex, 3-dimensional potential energy landscape of conformeric structures. Electronic excitation to Rydberg states prepares the molecule in a high-energy, nonequilibrium distribution of such conformers, initiating ultrafast transitions between them. Time-resolved Rydberg electron binding energy spectra, observed using photoionization-photoelectron spectroscopy with ultrashort laser pulses, reveal these time-evolving structures. The time-dependent structural fingerprint spectra are assigned with the aid of a computational analysis of the, potential energy landscape. Upon 209 nm electronic excitation to the 3p Rydberg state, triethylamine decays to 3s with a 200 fs time constant. The initially prepared conformer reacts to a mixture of structures with a time constant of 232 fs and settles into a final geometry distribution on a further subpicosecond time scale. The binding energy of the Rydberg electron is found to be an important determinant of the conformeric energy landscape.
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