TY - JOUR
T1 - Ultrafast Four-Dimensional Coherent Spectroscopy by Projection Reconstruction
AU - Hutson, William O.
AU - Spencer, Austin P.
AU - Harel, Elad
N1 - Funding Information:
This work was supported by the Office of Naval Research (N00014-16-1-2715-P00001) and the Packard Foundation (2013-39272) in part.
Publisher Copyright:
© 2018 American Chemical Society.
PY - 2018/3/1
Y1 - 2018/3/1
N2 - Multidimensional coherent spectroscopy provides insights into the vibronic structure and dynamics of complex systems. In general, the higher the dimensionality, the better the spectral discrimination and the more information that may be extracted about the system. A major impediment to widespread implementation of these methods, however, is that the acquisition time generally increases exponentially with dimensionality, prohibiting practical implementation. We demonstrate the use of nonuniform sampling based on the projection-slice theorem and inverse Radon transform within the context of a fifth-order, 4D technique (GAMERS) designed to correlate the vibrational contributions to different electronic states. Projection-reconstruction (PRO GAMERS) greatly reduces the data sampling requirements without sacrificing frequency resolution. The sensitivity of this technique is demonstrated to surpass conventional uniform sampling by orders of magnitude. The incorporation of projection-reconstruction into multidimensional coherent spectroscopy opens up the possibility to study the structure of complex chemical, biological, and physical systems with unprecedented detail.
AB - Multidimensional coherent spectroscopy provides insights into the vibronic structure and dynamics of complex systems. In general, the higher the dimensionality, the better the spectral discrimination and the more information that may be extracted about the system. A major impediment to widespread implementation of these methods, however, is that the acquisition time generally increases exponentially with dimensionality, prohibiting practical implementation. We demonstrate the use of nonuniform sampling based on the projection-slice theorem and inverse Radon transform within the context of a fifth-order, 4D technique (GAMERS) designed to correlate the vibrational contributions to different electronic states. Projection-reconstruction (PRO GAMERS) greatly reduces the data sampling requirements without sacrificing frequency resolution. The sensitivity of this technique is demonstrated to surpass conventional uniform sampling by orders of magnitude. The incorporation of projection-reconstruction into multidimensional coherent spectroscopy opens up the possibility to study the structure of complex chemical, biological, and physical systems with unprecedented detail.
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U2 - 10.1021/acs.jpclett.8b00122
DO - 10.1021/acs.jpclett.8b00122
M3 - Article
C2 - 29432694
AN - SCOPUS:85042710330
VL - 9
SP - 1034
EP - 1040
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 5
ER -