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Institute of Physics eBooks

Interaction of light pulses with ensembles of chromophores: polarization gratings

Joel Y. Yuen-Zhou, Jacob J. Krich, Ivan Kassal, Allan S. Johnson, Alán Aspuru‐Guzik

Published Sep 1, 2014• 0 citations
Publisher
DOI
10.1088/978-0-750-31062-8ch3

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In the regime of resonant coherent light-matter interaction, light pulses may interact with each other indirectly via a polarization wave created by the other pulse. We show that such interaction allows fast creation and erasing of high-contrast dynamic population density gratings, as well as control of their period in a few-cycle regime. Our scheme uses counter-propagating optical pulses, which do not cross each other in the medium. The mechanism is able to work with pulse durations up to the single-cycle limit. Somewhat surprisingly, ultrafast grating wave vector control requires the generation of polarization waves with the phase velocity much smaller than that of light.
The authors consider photochem. hole burning of an inhomogeneous and isotropic ensemble of chromophores through excitation with a narrow-bandwidth source of polarized light. The authors derive expressions for the depth and anisotropy of resonant and vibronic satellite spectral holes with increasing fluence. A fit of these satn. curves to exptl. data yields the Debye-Waller factor of the system. A simple rate equation model predicts that the anisotropy of a spectral hole depends only on the angle between the transition dipoles of the burnt and the probed transitions. In expts. with pulsed lasers strong deviations from this ideal behavior are obsd. An extended theory including satn. gives a satisfactory description of this phenomenon and provides a new method for the detn. of photochem. quantum yields.
Abstract Recently, the possibility of the creation, erasing and ultrafast control of polarization and population inversion gratings by sequences of few-cycle bipolar pulses interacting with a medium in a resonant and coherent way was predicted. In this case, the overlapping of pulses in the medium is not needed for the creation of gratings. In this paper, we study the possibility of the ultrafast creation and control of spatial periodic gratings in a resonant medium when subcycle unipolar pulses (that is ones containing the constant spectral component of an electric field) propagate in the coherent regime.