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Nonlinear Response of Solids and Molecules in Intense Infrared Radiation

Published online by Cambridge University Press:  10 February 2011

Sokrates T. Pantelides ,
Roland Winkler ,
Maurizio Ferconil  and
J. J. Vicente Alvarez
Sokrates T. Pantelides
Affiliation:
Department of Physics and Astronomy, Vanderbilt University, Nashville, TN 37235 Solid State Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831
Roland Winkler
Affiliation:
Department of Physics and Astronomy, Vanderbilt University, Nashville, TN 37235
Maurizio Ferconil
Affiliation:
Department of Physics and Astronomy, Vanderbilt University, Nashville, TN 37235
J. J. Vicente Alvarez
Affiliation:
Department of Physics and Astronomy, Vanderbilt University, Nashville, TN 37235
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Abstract

Infrared radiation, which couples with vibrations in molecules and solids, has long been considered as a promising way to selectively control chemical reactions, materials processing, and biomedical applications. The expectation is that particular frequencies couple to specific atomic motions, in contrast to heat which imparts energy indiscriminately. The promise has yet to be fulfilled, but recent successes and the development of new lasers have rekindled interest. We report calculations of the dynamics of solids and molecules under intense infrared radiation. In solids, using a model calculation, we find that narrowly-defined “windows of opportunity” exist for resonant enhancement of impurity diffusion at moderate intensities. In molecules, using a generalization of Car-Parrinello dynamics, we find that, for very intense fields, energy absorption at normal modes is not very efficient and that selective bond-breaking may occur at nonresonant frequencies by “concerted kicks”. Finally, time-dependent density functional theory is used to show that the effect of very intense infrared radiation on atoms and molecules is to produce very high harmonics as found experimentally.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 538: Symposium J – Multiscale Modelling of Materials , 1998 , 453
Copyright
Copyright © Materials Research Society 1999

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