How to turn your pump-probe instrument into a multidimensional spectrometer

2D IR and Vis spectroscopies via pulse shaping

Sang-Hee Shim, Martin T. Zanni

Research output: Contribution to journalReview article

224 Citations (Scopus)

Abstract

We have recently developed a new and simple way of collecting 2D infrared and visible spectra that utilizes a pulse shaper and a partly collinear beam geometry. 2D IR and Vis spectroscopies are powerful tools for studying molecular structures and their dynamics. They can be used to correlate vibrational or electronic eigenstates, measure energy transfer rates, and quantify the dynamics of lineshapes, for instance, all with femtosecond time-resolution. As a result, they are finding use in systems that exhibit fast dynamics, such as sub-millisecond chemical and biological dynamics, and in hard-to-study environments, such as in membranes. While powerful, these techniques have been difficult to implement because they require a series of femtosecond pulses to be spatially and temporally overlapped with precise time-resolution and interferometric phase stability. However, many of the difficulties associated with implementing 2D spectroscopies are eliminated by using a pulse shaper and a simple beam geometry, which substantially lowers the technical barriers required for researchers to enter this exciting field while simultaneously providing many new capabilities. The aim of this paper is to provide an overview of the methods for collecting 2D spectra so that an outsider considering using 2D spectroscopy in their own research can judge which approach would be most suitable for their research aims. This paper focuses primarily on 2D IR spectroscopy, but also includes our recent work on adapting this technology to collecting 2D Vis spectra. We review work that has already been published as well as cover several topics that we have not reported previously, including phase cycling methods to remove background signals, eliminate unwanted scatter, and shift data collection into the rotating frame.

Original languageEnglish
Pages (from-to)748-761
Number of pages14
JournalPhysical Chemistry Chemical Physics
Volume11
Issue number5
DOIs
Publication statusPublished - 2009 Jan 29
Externally publishedYes

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Pulse shaping
Infrared spectrometers
Spectrum Analysis
Pumps
Spectroscopy
spectrometers
pumps
shapers
probes
pulses
spectroscopy
Phase stability
Geometry
Energy Transfer
geometry
visible spectrum
Molecular Structure
Ultrashort pulses
Research
Energy transfer

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

How to turn your pump-probe instrument into a multidimensional spectrometer : 2D IR and Vis spectroscopies via pulse shaping. / Shim, Sang-Hee; Zanni, Martin T.

In: Physical Chemistry Chemical Physics, Vol. 11, No. 5, 29.01.2009, p. 748-761.

Research output: Contribution to journalReview article

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