Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 3, Issue 22, Pages 3353-3359Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz3015327
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Funding
- Major Thematic Grant from Peter Wall Institute for Advanced Studies of the University of British Columbia
- US DoD DTRA program
- NSERC Discovery Grant
- NSERC Alexander Graham Bell CGS award
- Walter C. Sumner Memorial Fellowship
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We present a reference-free robust method for the nondestructive imaging of complex time-evolving molecular wave functions using as input the time-resolved fluorescence signal. The method is based on expanding the evolving wave function in a set of bound stationary states and determining the set of complex expansion coefficients by calculating a series of Fourier integrals of the signal. As illustrated for the A(1)Sigma(+)(u) electronic state of Na-upsilon the method faithfully reconstructs the time-dependent complex wave function of the nuclear motion. Moreover, using perturbation theory to connect the excitation pulse and the material expansion coefficients, our method is used to determine the electromagnetic field of the excitation pulse, thus providing a simple technique for pulse characterization that obviates the additional measurements and iterative solutions that beset other techniques. The approach, which is found to be quite robust against errors in the experimental data, can be readily generalized to the reconstruction of polyatomic vibrational wave functions.
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