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Dynamic theory of nanophotonic control of two-dimensional semiconductor nonlinearities

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Title: Dynamic theory of nanophotonic control of two-dimensional semiconductor nonlinearities
Authors: Guazzotti, S
Pusch, A
Reiter, DE
Hess, O
Item Type: Journal Article
Abstract: We introduce a Maxwell-Bloch simulation approach which self-consistently combines a microscopic description of the carrier and polarization dynamics of a transition-metal-dichalcogenide (TMDC) monolayer with a spatiotemporal full-wave time-domain simulation of Maxwell's equations on the basis of a finite-difference time-domain (FDTD) method beyond the slowly varying amplitude or paraxial approximations. This offers a platform to realistically model, in particular, the typical ultrafast optical excitation experiments in micro- and nanocavities. Our simulations confirm that the weak screening of the Coulomb interaction in TMDC monolayers yields pronounced exciton lines in the linear spectrum and we uncover the second-order nonlinearity represented in the semiconductor Maxwell-Bloch equations by an intraband dipole moment. This allows us to calculate the spectral shape of the exceptionally strong second-harmonic generation around the exciton lines of TMDC monolayers. We demonstrate that the second-harmonic signal can remarkably be further enhanced by several orders of magnitude through a suitably designed (one-dimensional) photonic microcavity. Due to its self-consistency, flexibility, explicit spatio-temporal resolution on the nanoscale and the ready access to light field and electron dynamics, our theory and computational approach is an ideal platform to design and explore spatiotemporal nonlinear and quantum dynamics in complex photonic or plasmonic micro- and nanostructures for optoelectronic, nanophotonic and quantum applications of TMDC monolayers.
Issue Date: 15-Dec-2018
Date of Acceptance: 3-Nov-2018
URI: http://hdl.handle.net/10044/1/66153
DOI: https://dx.doi.org/10.1103/PhysRevB.98.245307
ISSN: 2469-9950
Publisher: American Physical Society
Journal / Book Title: Physical Review B
Volume: 98
Issue: 24
Copyright Statement: © 2018 American Physical Society.
Sponsor/Funder: European Office Of Aerospace Research & Developmen
Engineering & Physical Science Research Council (E
Engineering and Physical Sciences Research Council
US Air Force
Funder's Grant Number: FA9550-14-1-0181
German Academic Exchange Service
Keywords: Science & Technology
Physical Sciences
Materials Science, Multidisciplinary
Physics, Applied
Physics, Condensed Matter
Materials Science
Publication Status: Published
Article Number: 245307
Online Publication Date: 2018-12-17
Appears in Collections:Condensed Matter Theory
Faculty of Natural Sciences