Facile collection of two-dimensional electronic spectra using femtosecond pulse-shaping technology

Erik M. Grumstrup, Sang Hee Shim, Matthew A. Montgomery, Niels H. Damrauer, Martin T. Zanni

Research output: Contribution to journalArticlepeer-review

130 Citations (Scopus)


This letter reports a straightforward means of collecting two-dimensional electronic (2D-E) spectra using optical tools common to many research groups involved in ultrafast spectroscopy and quantum control. In our method a femtosecond pulse shaper is used to generate a pair of phase stable collinear laser pulses which are then incident on a gas or liquid sample. The pulse pair is followed by an ultrashort probe pulse that is spectrally resolved. The delay between the collinear pulses is incremented using phase and amplitude shaping and a 2D-E spectrum is generated following Fourier transformation. The partially collinear beam geometry results in perfectly phased absorptive spectra without phase twist. Our approach is much simpler to implement than standard non-collinear beam geometries, which are challenging to phase stabilize and require complicated calibrations. Using pulse shaping, many new experiments are now also possible in both 2D-E spectroscopy and coherent control.

Original languageEnglish
Pages (from-to)16681-16689
Number of pages9
JournalOptics Express
Issue number25
Publication statusPublished - 2007 Dec 12
Externally publishedYes

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics


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