Tractable theory of nonlinear response and multidimensional nonlinear spectroscopy.
Nonlinear spectroscopy provides insights into dynamics, but the response functions required for its interpretation pose a challenge to theorists. We proposed an approach in which the fifth-order response function [R5( t1, t2)] was expressed as a two-time classical time correlation function (TCF). Here, we present TCF theory results for R5( t1, t2) in liquid xenon. Using a first-order dipole-induced dipole polarizability model, the result is compared to an exact numerical calculation showing remarkable agreement. In addition, R5( t1, t2) is calculated using the exactly solved polarizability model, yielding different results and predicting an echo signal.
DeVane
Russell
R
Department of Chemistry, University of South Florida, 4202 E. Fowler Avenue, SCA400, Tampa, FL 33620-5250, USA.
Ridley
Christina
C
Space
Brian
B
Keyes
T
T