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

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4934231· OSTI ID:1469573
 [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

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.

Research Organization:
Univ. of California, Irvine, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
FG02-04ER15571
OSTI ID:
1469573
Alternate ID(s):
OSTI ID: 1224331
Journal Information:
Journal of Chemical Physics, Vol. 143, Issue 16; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 16 works
Citation information provided by
Web of Science

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Cited By (5)

Perspective: Quantum Hamiltonians for optical interactions journal January 2018
Quantum transition probabilities during a perturbing pulse: Differences between the nonadiabatic results and Fermi’s golden rule forms journal May 2018
Nonadiabatic transition probabilities in a time-dependent Gaussian pulse or plateau pulse: Toward experimental tests of the differences from Dirac’s transition probabilities journal November 2018
Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction journal December 2018
Perspective: Quantum Hamiltonians for Optical Interactions text January 2018