Abstract
A fundamental goal of chemical physics is an understanding of microscopic interactions in liquids at and away from equilibrium. In principle, this microscopic information is accessible by high-order and high-dimensionality nonlinear optical measurements. Unfortunately, the time required to execute such experiments increases exponentially with the dimensionality, while the signal decreases exponentially with the order of the nonlinearity. Recently, we demonstrated a non-uniform acquisition method based on radial sampling of the time-domain signal [W. O. Hutson et al., J. Phys. Chem. Lett. 9, 1034 (2018)]. The four-dimensional spectrum was then reconstructed by filtered back-projection using an inverse Radon transform. Here, we demonstrate an alternative reconstruction method based on the statistical analysis of different back-projected spectra which results in a dramatic increase in sensitivity and at least a 100-fold increase in dynamic range compared to conventional uniform sampling and Fourier reconstruction. These results demonstrate that alternative sampling and reconstruction methods enable applications of increasingly high-order and high-dimensionality methods toward deeper insights into the vibronic structure of liquids.
Original language | English (US) |
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Article number | 194201 |
Journal | Journal of Chemical Physics |
Volume | 148 |
Issue number | 19 |
DOIs | |
State | Published - May 21 2018 |
Funding
This work was supported by the Office of Naval Research (Grant No. N00014-16-1-2715-P00001).
ASJC Scopus subject areas
- General Physics and Astronomy
- Physical and Theoretical Chemistry