Structural dynamics in floppy systems: ultrafast conformeric motions in Rydberg-excited triethylamine

J Phys Chem A. 2011 Mar 17;115(10):1804-9. doi: 10.1021/jp110905h. Epub 2011 Feb 22.

Abstract

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.

Publication types

  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Butylamines / chemistry
  • Ethylamines / chemistry*
  • Kinetics
  • Models, Molecular
  • Molecular Conformation*
  • Motion*
  • Spectrum Analysis
  • Thermodynamics

Substances

  • Butylamines
  • Ethylamines
  • N,N-dimethyl-2-butanamine
  • triethylamine