Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering

Chen, Hsing-Ta; Li, Tao E.; Sukharev, Maxim; Nitzan, Abraham; Subotnik, Joseph E.

doi:10.1063/1.5057366

Title: Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering

Journal Article · 24 January 2019 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5057366 · OSTI ID:1613217

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^[2]; Subotnik, Joseph E. ^[2]

Univ. of Pennsylvania, Philadelphia, PA (United States); DOE/OSTI
Univ. of Pennsylvania, Philadelphia, PA (United States)
Arizona State Univ., Mesa, AZ (United States); Arizona State Univ., Tempe, AZ (United States)

In Paper I [Chen et al., J. Chem. Phys. 150, 044102 (2019)], we introduced Ehrenfest+R dynamics for a two-level system and showed how spontaneous emission can be heuristically included such that, after averaging over an ensemble of Ehrenfest+R trajectories, one can recover both coherent and incoherent electromagnetic fields. In the present paper, we now show that Ehrenfest+R dynamics can also correctly describe Raman scattering, whose features are completely absent from standard Ehrenfest dynamics. Ehrenfest+R dynamics appear to be quantitatively accurate both for resonant and off-resonant Raman signals, as compared with Kramers–Heisenberg–Dirac theory.

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Research Organization:: Univ. of Pennsylvania, Philadelphia, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0019397

OSTI ID:: 1613217

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 4 Vol. 150; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (39)

The Raman Effect Long, Derek A. John Wiley & Sons, Ltd https://doi.org/10.1002/0470845767	book	January 2002
Über die Streuung von Strahlung durch Atome Kramers, H. A.; Heisenberg, W. Zeitschrift für Physik, Vol. 31, Issue 1 https://doi.org/10.1007/bf02980624	journal	February 1925
Semiclassical and quantum-electrodynamical approaches in nonrelativistic radiation theory Milonni, P. W. Physics Reports, Vol. 25, Issue 1 https://doi.org/10.1016/0370-1573(76)90037-5	journal	May 1976
Surface- and Tip-Enhanced Raman Spectroscopy in Catalysis Hartman, Thomas; Wondergem, Caterina S.; Kumar, Naresh The Journal of Physical Chemistry Letters, Vol. 7, Issue 8 https://doi.org/10.1021/acs.jpclett.6b00147	journal	April 2016
Strong Light–Matter Interaction in Quantum Emitter/Metal Hybrid Nanostructures Vasa, Parinda; Lienau, Christoph ACS Photonics, Vol. 5, Issue 1 https://doi.org/10.1021/acsphotonics.7b00650	journal	October 2017
The semiclassical way to molecular spectroscopy Heller, Eric J. Accounts of Chemical Research, Vol. 14, Issue 12 https://doi.org/10.1021/ar00072a002	journal	December 1981
Theoretical Studies of Plasmonics using Electronic Structure Methods Morton, Seth M.; Silverstein, Daniel W.; Jensen, Lasse Chemical Reviews, Vol. 111, Issue 6 https://doi.org/10.1021/cr100265f	journal	June 2011
Simple aspects of Raman scattering Heller, Eric J.; Sundberg, Robert; Tannor, David The Journal of Physical Chemistry, Vol. 86, Issue 10 https://doi.org/10.1021/j100207a018	journal	May 1982
Surface Plasmon-Driven Water Reduction: Gold Nanoparticle Size Matters Qian, Kun; Sweeny, Brendan C.; Johnston-Peck, Aaron C. Journal of the American Chemical Society, Vol. 136, Issue 28 https://doi.org/10.1021/ja504097v	journal	July 2014
Surface-Enhanced Raman Nanoparticle Beacons Based on Bioconjugated Gold Nanocrystals and Long Range Plasmonic Coupling Qian, Ximei; Zhou, Xi; Nie, Shuming Journal of the American Chemical Society, Vol. 130, Issue 45 https://doi.org/10.1021/ja8062502	journal	November 2008
Symmetrical Windowing for Quantum States in Quasi-Classical Trajectory Simulations Cotton, Stephen J.; Miller, William H. The Journal of Physical Chemistry A, Vol. 117, Issue 32 https://doi.org/10.1021/jp401078u	journal	March 2013
Simplified Sum-Over-States Approach for Predicting Resonance Raman Spectra. Application to Nucleic Acid Bases Rappoport, Dmitrij; Shim, Sangwoo; Aspuru-Guzik, Alán The Journal of Physical Chemistry Letters, Vol. 2, Issue 11 https://doi.org/10.1021/jz200413g	journal	May 2011
Single-Molecule Surface-Enhanced Raman Scattering: Can STEM/EELS Image Electromagnetic Hot Spots? Mirsaleh-Kohan, Nasrin; Iberi, Vighter; Simmons, Philip D. The Journal of Physical Chemistry Letters, Vol. 3, Issue 16 https://doi.org/10.1021/jz300967q	journal	August 2012
Metallic Nanoparticle Arrays: A Common Substrate for Both Surface-Enhanced Raman Scattering and Surface-Enhanced Infrared Absorption Le, Fei; Brandl, Daniel W.; Urzhumov, Yaroslav A. ACS Nano, Vol. 2, Issue 4 https://doi.org/10.1021/nn800047e	journal	March 2008
Using Raman spectroscopy to characterize biological materials Butler, Holly J.; Ashton, Lorna; Bird, Benjamin Nature Protocols, Vol. 11, Issue 4 https://doi.org/10.1038/nprot.2016.036	journal	March 2016
Resonance Raman spectra of uracil based on Kramers–Kronig relations using time-dependent density functional calculations and multireference perturbation theory Neugebauer, Johannes; Hess, Bernd A. The Journal of Chemical Physics, Vol. 120, Issue 24 https://doi.org/10.1063/1.1697371	journal	June 2004
On the Theory of Raman Intensities Albrecht, Andreas C. The Journal of Chemical Physics, Vol. 34, Issue 5 https://doi.org/10.1063/1.1701032	journal	May 1961
Finite lifetime effects on the polarizability within time-dependent density-functional theory Jensen, L.; Autschbach, J.; Schatz, G. C. The Journal of Chemical Physics, Vol. 122, Issue 22 https://doi.org/10.1063/1.1929740	journal	June 2005
Theory and method for calculating resonance Raman scattering from resonance polarizability derivatives Jensen, L.; Zhao, L. L.; Autschbach, J. The Journal of Chemical Physics, Vol. 123, Issue 17 https://doi.org/10.1063/1.2046670	journal	November 2005
Quantum-classical Liouville dynamics in the mapping basis Kim, Hyojoon; Nassimi, Ali; Kapral, Raymond The Journal of Chemical Physics, Vol. 129, Issue 8 https://doi.org/10.1063/1.2971041	journal	August 2008
A classical/semiclassical theory for the interaction of infrared radiation with molecular systems Miller, William H. The Journal of Chemical Physics, Vol. 69, Issue 5 https://doi.org/10.1063/1.436793	journal	September 1978
Time-dependent theory of Raman scattering Lee, Soo-Y.; Heller, E. J. The Journal of Chemical Physics, Vol. 71, Issue 12 https://doi.org/10.1063/1.438316	journal	January 1979
Electromagnetic theory of enhanced Raman scattering by molecules adsorbed on rough surfaces Gersten, Joel; Nitzan, Abraham The Journal of Chemical Physics, Vol. 73, Issue 7 https://doi.org/10.1063/1.440560	journal	October 1980
Polyatomic Raman scattering for general harmonic potentials Tannor, David J.; Heller, Eric J. The Journal of Chemical Physics, Vol. 77, Issue 1 https://doi.org/10.1063/1.443643	journal	July 1982
The enhancement of Raman scattering, resonance Raman scattering, and fluorescence from molecules adsorbed on a rough silver surface Weitz, D. A.; Garoff, S.; Gersten, J. I. The Journal of Chemical Physics, Vol. 78, Issue 9 https://doi.org/10.1063/1.445486	journal	May 1983
Toward preresonant impulsive Raman preparation of large amplitude vibrational motion Smith, T. J.; Cina, J. A. The Journal of Chemical Physics, Vol. 104, Issue 4 https://doi.org/10.1063/1.470786	journal	January 1996
Can chirp enhance cumulative pre‐resonant impulsive stimulated Raman excitation? Hiller, Eric M.; Cina, Jeffrey A. The Journal of Chemical Physics, Vol. 105, Issue 9 https://doi.org/10.1063/1.472212	journal	September 1996
Consistent schemes for non-adiabatic dynamics derived from partial linearized density matrix propagation Huo, Pengfei; Coker, David F. The Journal of Chemical Physics, Vol. 137, Issue 22 https://doi.org/10.1063/1.4748316	journal	December 2012
Symmetrical windowing for quantum states in quasi-classical trajectory simulations: Application to electronically non-adiabatic processes Cotton, Stephen J.; Miller, William H. The Journal of Chemical Physics, Vol. 139, Issue 23 https://doi.org/10.1063/1.4845235	journal	December 2013
Ehrenfest+R dynamics. I. A mixed quantum–classical electrodynamics simulation of spontaneous emission Chen, Hsing-Ta; Li, Tao E.; Sukharev, Maxim The Journal of Chemical Physics, Vol. 150, Issue 4 https://doi.org/10.1063/1.5057365	journal	January 2019
Optics of exciton-plasmon nanomaterials Sukharev, Maxim; Nitzan, Abraham Journal of Physics: Condensed Matter, Vol. 29, Issue 44 https://doi.org/10.1088/1361-648x/aa85ef	journal	October 2017
The Quantum Theory of the Emission and Absorption of Radiation Dirac, P. A. M. Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 114, Issue 767 https://doi.org/10.1098/rspa.1927.0039	journal	March 1927
Many-body theory of surface-enhanced Raman scattering Masiello, David J.; Schatz, George C. Physical Review A, Vol. 78, Issue 4 https://doi.org/10.1103/physreva.78.042505	journal	October 2008
Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy Li, Tao E.; Nitzan, Abraham; Sukharev, Maxim Physical Review A, Vol. 97, Issue 3 https://doi.org/10.1103/physreva.97.032105	journal	March 2018
The Raman Effect Nielsen, J. Rud School Science and Mathematics, Vol. 29, Issue 6 https://doi.org/10.1111/j.1949-8594.1929.tb02459.x	journal	June 1929
Surface-Enhanced Raman Spectroscopy Stiles, Paul L.; Dieringer, Jon A.; Shah, Nilam C. Annual Review of Analytical Chemistry, Vol. 1, Issue 1, p. 601-626 https://doi.org/10.1146/annurev.anchem.1.031207.112814	journal	July 2008
Localized Surface Plasmon Resonance Spectroscopy and Sensing Willets, Katherine A.; Van Duyne, Richard P. Annual Review of Physical Chemistry, Vol. 58, Issue 1 https://doi.org/10.1146/annurev.physchem.58.032806.104607	journal	May 2007
Quantum-Classical Liouville Dynamics in the Mapping Basis Kim, Hyojoon; Nassimi, Ali; Kapral, Raymond arXiv https://doi.org/10.48550/arxiv.0903.0847	text	January 2009
Ehrenfest+R Dynamics I: A Mixed Quantum-Classical Electrodynamics Simulation of Spontaneous Emission Chen, Hsing-Ta; Li, Tao E.; Sukharev, Maxim arXiv https://doi.org/10.48550/arxiv.1806.04662	text	January 2018

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Benchmarking semiclassical and perturbative methods for real-time simulations of cavity-bound emission and interference Hoffmann, Norah M.; Schäfer, Christian; Säkkinen, Niko The Journal of Chemical Physics, Vol. 151, Issue 24 https://doi.org/10.1063/1.5128076	journal	December 2019
Cumulant expansion for the treatment of light–matter interactions in arbitrary material structures Sánchez-Barquilla, M.; Silva, R. E. F.; Feist, J. The Journal of Chemical Physics, Vol. 152, Issue 3 https://doi.org/10.1063/1.5138937	journal	January 2020
Understanding detailed balance for an electron-radiation system through mixed quantum-classical electrodynamics Chen, Hsing-Ta; Li, Tao E.; Nitzan, Abraham Physical Review A, Vol. 100, Issue 1 https://doi.org/10.1103/physreva.100.010101	journal	July 2019
Capturing vacuum fluctuations and photon correlations in cavity quantum electrodynamics with multitrajectory Ehrenfest dynamics Hoffmann, Norah M.; Schäfer, Christian; Rubio, Angel Physical Review A, Vol. 99, Issue 6 https://doi.org/10.1103/physreva.99.063819	journal	June 2019
Ehrenfest+R Dynamics I: A Mixed Quantum-Classical Electrodynamics Simulation of Spontaneous Emission Chen, Hsing-Ta; Li, Tao E.; Sukharev, Maxim arXiv https://doi.org/10.48550/arxiv.1806.04662	text	January 2018
Understanding Detailed Balance for an Electron-Radiation System Through Mixed Quantum-Classical Electrodynamics Chen, Hsing-Ta; Li, Tao E.; Nitzan, Abraham arXiv https://doi.org/10.48550/arxiv.1904.02742	text	January 2019
Benchmarking Semiclassical and Perturbative Methods for Real-time Simulations of Cavity-Bound Emission and Interference Hoffmann, Norah M.; Schäfer, Christian; Säkkinen, Niko arXiv https://doi.org/10.48550/arxiv.1909.07177	text	January 2019

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Title: Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering

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References (39)

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