Dynamics of electron solvation in methanol: Excited state relaxation and generation by charge-transfer-to-solvent

Abstract

The charge-transfer-to-solvent dynamics (CTTS) and excited state relaxation mechanism of the solvated electron in methanol are studied by time-resolved photoelectron spectroscopy on a liquid methanol microjet by means of two-pulse and three-pulse experiments. In the two-pulse experiment, CTTS excitation is followed by a probe photoejection pulse. The resulting time-evolving photoelectron spectrum reveals multiple time scales characteristic of relaxation and geminate recombination of the initially generated electron which are consistent with prior results from transient absorption. In the three-pulse experiment, the relaxation dynamics of the solvated electron following electronic excitation are measured. The internal conversion lifetime of the excited electron is found to be 130 ± 40 fs, in agreement with extrapolated results from clusters and the non-adiabatic relaxation mechanism.

Document Details

Document Type
Pub Defense Publication
Publication Date
Jun 15, 2015
Source ID
10.1063/1.4922441

Entities

People

  • Daniel Neumark
  • Holly L. Williams
  • Madeline H Elkins

Organizations

  • Air Force Office of Scientific Research
  • Lawrence Berkeley National Laboratory
  • National Science Foundation
  • University of California

Tags

Fields of Study

  • Physics

Readers

  • Quantum Chemistry
  • Quantum Dot Semiconductor Device Photonics and Graphene Optoelectronic Materials and THz Physics.

Technology Areas

  • Microelectronics