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Title: Non-linear non-local molecular electrodynamics with nano-optical fields

Abstract

The interaction of optical fields sculpted on the nano-scale with matter may not be described by the dipole approximation since the fields may vary appreciably across the molecular length scale. Rather than incrementally adding higher multipoles, it is advantageous and more physically transparent to describe the optical process using non-local response functions that intrinsically include all multi-poles. In this work, we present a semi-classical approach for calculating non-local response functions based on the minimal coupling Hamiltonian. The first, second, and third order response functions are expressed in terms of correlation functions of the charge and the current densities. Finally, this approach is based on the gauge invariant current rather than the polarization, and on the vector potential rather than the electric and magnetic fields.

Authors:
 [1];  [2];  [2]
  1. Wayne State Univ., Detroit, MI (United States). Department of Chemistry and Department of Mathematics
  2. Univ. of California, Irvine, CA (United States). Department of Chemistry
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1469573
Alternate Identifier(s):
OSTI ID: 1224331
Grant/Contract Number:  
FG02-04ER15571
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 16; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chernyak, Vladimir Y., Saurabh, Prasoon, and Mukamel, Shaul. Non-linear non-local molecular electrodynamics with nano-optical fields. United States: N. p., 2015. Web. doi:10.1063/1.4934231.
Chernyak, Vladimir Y., Saurabh, Prasoon, & Mukamel, Shaul. Non-linear non-local molecular electrodynamics with nano-optical fields. United States. doi:10.1063/1.4934231.
Chernyak, Vladimir Y., Saurabh, Prasoon, and Mukamel, Shaul. Mon . "Non-linear non-local molecular electrodynamics with nano-optical fields". United States. doi:10.1063/1.4934231. https://www.osti.gov/servlets/purl/1469573.
@article{osti_1469573,
title = {Non-linear non-local molecular electrodynamics with nano-optical fields},
author = {Chernyak, Vladimir Y. and Saurabh, Prasoon and Mukamel, Shaul},
abstractNote = {The interaction of optical fields sculpted on the nano-scale with matter may not be described by the dipole approximation since the fields may vary appreciably across the molecular length scale. Rather than incrementally adding higher multipoles, it is advantageous and more physically transparent to describe the optical process using non-local response functions that intrinsically include all multi-poles. In this work, we present a semi-classical approach for calculating non-local response functions based on the minimal coupling Hamiltonian. The first, second, and third order response functions are expressed in terms of correlation functions of the charge and the current densities. Finally, this approach is based on the gauge invariant current rather than the polarization, and on the vector potential rather than the electric and magnetic fields.},
doi = {10.1063/1.4934231},
journal = {Journal of Chemical Physics},
number = 16,
volume = 143,
place = {United States},
year = {2015},
month = {10}
}

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