skip to main content

SciTech ConnectSciTech Connect

Title: Lineshape analysis of coherent multidimensional optical spectroscopy using incoherent light

Coherent two-dimensional electronic spectroscopy using incoherent (noisy) light, I{sup (4)} 2D ES, holds intriguing challenges and opportunities. One challenge is to determine how I{sup (4)} 2D ES compares to femtosecond 2D ES. Here, we merge the sophisticated energy-gap Hamiltonian formalism that is often used to model femtosecond 2D ES with the factorized time-correlation formalism that is needed to describe I{sup (4)} 2D ES. The analysis reveals that in certain cases the energy-gap Hamiltonian is insufficient to model the spectroscopic technique correctly. The results using a modified energy-gap Hamiltonian show that I{sup (4)} 2D ES can reveal detailed lineshape information, but, contrary to prior reports, does not reveal dynamics during the waiting time.
Authors:
 [1] ;  [2]
  1. Department of Chemistry, Concordia College, Moorhead, Minnesota 56562 (United States)
  2. Department of Chemistry, New York University, New York, New York 10003 (United States)
Publication Date:
OSTI Identifier:
22415896
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 21; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; COMPARATIVE EVALUATIONS; CORRELATIONS; ELECTRON SPECTROSCOPY; ENERGY GAP; FACTORIZATION; HAMILTONIANS; TWO-DIMENSIONAL CALCULATIONS; TWO-DIMENSIONAL SYSTEMS; VISIBLE RADIATION