Title: Transient Second-Order Nonlinear Media: Breaking the Spatial Symmetry in the Time Domain via Hot-Electron Transfer

Journal Article · · Physical Review Letters

Second-order optical effects are essential to the active control of light and the generation of new spectral components. The inversion symmetry, however, prevents achieving a bulk $$χ^{(2)}$$ response, limiting the portfolio of the second-order nonlinear materials. Here, we demonstrate subpicosecond conversion of a statically passive dielectric to a transient second-order nonlinear medium upon the ultrafast transfer of hot electrons. Induced by an optical switching signal, the amorphous dielectric with vanishing intrinsic $$χ^{(2)}$$ develops dynamically tunable second-order nonlinear responses. By taking the second-harmonic generation as an example, we show that breaking the inversion symmetry through hot-electron dynamics can be leveraged to address the critical need for all-optical control of second-order nonlinearities in nanophotonics. We report our approach can be generically adopted in a variety of material and device platforms, offering a new class of complex nonlinear media with promising potentials for all-optical information processing.

Research Organization:
Emory Univ., Atlanta, GA (United States)
Sponsoring Organization:
National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0008798
OSTI ID:
1801887
Journal Information:
Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 1 Vol. 124; ISSN 0031-9007
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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