Abstract
We report two-dimensional electronic spectroscopy with a femtosecond stimulated Raman scattering probe. The method reveals correlations between excitation energy and excited state vibrational structure following photoexcitation. We demonstrate the method in rhodamine 6G.
Highlights
Two-dimensional electronic spectroscopy (2DES) has emerged as an attractive method for studying the ultrafast dynamics and electronic structure of a wide range of condensed matter systems [1]
We have previously demonstrated pulse-shaping-based 2DES in the pump probe geometry [9], enabling the straightforward use of a continuum probe to expand the frequency information available in 2DES [10]
A continuum probe pulse is created by focusing a small fraction of the 800 nm pulse into a 2 mm thick sapphire window with a 200 mm focal length lens and collimated using a 250 mm spherical mirror
Summary
Two-dimensional electronic spectroscopy (2DES) has emerged as an attractive method for studying the ultrafast dynamics and electronic structure of a wide range of condensed matter systems [1]. We combine these two methods, demonstrating 2DES with a FSRS probe (2DE-FSRS). We have previously demonstrated pulse-shaping-based 2DES in the pump probe geometry [9], enabling the straightforward use of a continuum probe to expand the frequency information available in 2DES [10]. In a standard FSRS experiment, a single actinic pump pulse is used.
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