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:
-
- Wayne State Univ., Detroit, MI (United States). Department of Chemistry and Department of Mathematics
- 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)
- 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. https://doi.org/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. https://doi.org/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 = {Mon Oct 26 00:00:00 EDT 2015},
month = {Mon Oct 26 00:00:00 EDT 2015}
}
Web of Science
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