Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 1, Issue 19, Pages 2876-2880Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz101064j
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Funding
- NSF MRSEC [DMR 08-00254]
- AFOSR [FA9550-09-1-0117]
- Searle Foundation
- Institute for Complex Adaptive Matter (ICAM)
- DOE SCGF
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We report the demonstration of single-quantum 3D electronic spectroscopy. Utilizing the recently introduced gradient assisted photon echo (GRAPE) methodology, the fifth-order nonlinear polarization of the solvatochromatic dye IR144 corresponding to evolution through three sequential single-quantum coherences is measured. GRAPE, which allows a 2D slice of data to be acquired in parallel, permits a practical i mplementation of 3D spectroscopy at optical frequencies in a matter of minutes instead of hours. By spreading frequencies into a third spectral dimension, we can resolve features in the spectra that are otherwise obscured. For IR144, a previously unresolved cross peak originating from high frequency vibronic modes is observed in the spectrum. Theoretical modeling based on the cumulant expansion truncated at second order reproduces the main features of the experimental results. This experimental approach will enable further high dimensional spectroscopic experiments.
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