skip to main content

Title: Pulse-shaping assisted multidimensional coherent electronic spectroscopy

Understanding nuclear and electronic dynamics of molecular systems has advanced considerably by probing their nonlinear responses with a suitable sequence of pulses. Moreover, the ability to control crucial parameters of the excitation pulses, such as duration, sequence, frequency, polarization, slowly varying envelope, or carrier phase, has led to a variety of advanced time-resolved spectroscopic methodologies. Recently, two-dimensional electronic spectroscopy with ultrashort pulses has become a more and more popular tool since it allows to obtain information on energy and coherence transfer phenomena, line broadening mechanisms, or the presence of quantum coherences in molecular complexes. Here, we present a high fidelity two-dimensional electronic spectroscopy setup designed for molecular systems in solution. It incorporates the versatility of pulse-shaping methods to achieve full control on the amplitude and phase of the individual exciting and probing pulses. Selective and precise amplitude- and phase-modulation is shown and applied to investigate electronic dynamics in several reference molecular systems.
Authors:
; ; ;  [1]
  1. Institute of Applied Physics, University of Bern, Sidlerstasse 5, CH-3012 Bern (Switzerland)
Publication Date:
OSTI Identifier:
22415917
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 21; Other Information: (c) 2015 Author(s); Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; AMPLITUDES; CONTROL; ELECTRON SPECTROSCOPY; EXCITATION; LINE BROADENING; MODULATION; NONLINEAR PROBLEMS; POLARIZATION; PROBES; PULSES; TIME RESOLUTION; TWO-DIMENSIONAL CALCULATIONS; TWO-DIMENSIONAL SYSTEMS