Abstract

Multidimensional infrared spectroscopy is a robust tool for studying the structural dynamics of molecules. In particular, twodimensional infrared (2DIR) spectroscopy can reveal vibrational coupling among the internal modes of molecules, uncovering the transient structure of complex systems. While spectroscopically very powerful, current experimental techniques are time consuming to perform, requiring ~10⁶ laser shots for a single 2DIR spectrum. In this work, we demonstrate a new technique that can acquire a full 2DIR correlation spectrum using a single ultrafast laser pulse. This apparatus will allow 2DIR spectroscopy to be extended to systems that were unattainable with previous technology, including, irreversible chemical reactions, rapid flow experiments, or with low repetition rate laser systems.

© 2007 Optical Society of America

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History
Original Manuscript: October 25, 2006
Manuscript Accepted: December 19, 2006
Revised Manuscript: December 17, 2006
Published: January 8, 2007

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Author Affiliations

Matthew F. DeCamp, Lauren P. DeFlores, Kevin C. Jones, Andrei Tokmakoff

Massachusetts Institute of Technology

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