Pulse shaping based two-dimensional electronic spectroscopy in a background free geometry

Opt Express. 2014 Jan 13;22(1):1018-27. doi: 10.1364/OE.22.001018.

Abstract

We demonstrate a "drop-in" modification of the pulse-shaped pump-probe geometry two-dimensional Fourier transform spectrometer that significantly improves its performance by making the measurement background-free. The modification uses a hybrid diffractive optic/pulse-shaping approach that combines the advantages of background-free detection with the precise timing and phase-cycling capabilities enabled by pulse-shaping. In addition, we present a simple new method for accurate phasing of optically heterodyned two-dimensional spectra. We demonstrate the high quality of data obtainable with this approach by reporting two-dimensional Fourier transform electronic spectra of chlorophyll a in glycerol/water at 77 K.

Publication types

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

MeSH terms

  • Algorithms*
  • Chlorophyll / analysis*
  • Chlorophyll / chemistry
  • Chlorophyll A
  • Glycerol / chemistry*
  • Refractometry / instrumentation*
  • Refractometry / methods
  • Spectroscopy, Fourier Transform Infrared / instrumentation*
  • Spectroscopy, Fourier Transform Infrared / methods
  • Water / chemistry*

Substances

  • Water
  • Chlorophyll
  • Glycerol
  • Chlorophyll A