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Bauer, Jonas M. ; Chen, Lijue ; Wilhelm, Philipp ; Watanabe, Kenji ; Taniguchi, Takashi ; Bange, Sebastian ; Lupton, John M. ; Lin, Kai-Qiang

Excitonic resonances control the temporal dynamics of nonlinear optical wave mixing in monolayer semiconductors

Bauer, Jonas M., Chen, Lijue , Wilhelm, Philipp, Watanabe, Kenji , Taniguchi, Takashi, Bange, Sebastian, Lupton, John M. und Lin, Kai-Qiang (2022) Excitonic resonances control the temporal dynamics of nonlinear optical wave mixing in monolayer semiconductors. Nature Photonics.

Veröffentlichungsdatum dieses Volltextes: 21 Okt 2022 13:06
Artikel
DOI zum Zitieren dieses Dokuments: 10.5283/epub.53081


Zusammenfassung

Researchers show that resonant coupling of light pulses with excitonic transitions affects the optimal time difference between pulses for sum-frequency generation and four-wave mixing in monolayer WSe2. Monolayer semiconductors are an emerging platform for strong nonlinear light-matter interactions that are enhanced by the giant oscillator strength of tightly bound excitons. Little attention has ...

Researchers show that resonant coupling of light pulses with excitonic transitions affects the optimal time difference between pulses for sum-frequency generation and four-wave mixing in monolayer WSe2. Monolayer semiconductors are an emerging platform for strong nonlinear light-matter interactions that are enhanced by the giant oscillator strength of tightly bound excitons. Little attention has been paid to the impact of excitonic resonances on the temporal dynamics of such nonlinearities, since harmonic generation and optical wave mixing are generally considered instantaneous processes. We find that a significant time difference, ranging from -40 to +120 fs, is necessary between two light pulses for optimal sum-frequency generation (SFG) and four-wave mixing (FWM) to occur from monolayer WSe2 when one of the pulses is in resonance with an excitonic transition. These resonances involve both band-edge A excitons and high-lying excitons that comprise electrons from conduction bands far above the bandgap. Numerical simulations in the density-matrix formalism rationalize the distinct dynamics of SFG and FWM. The interpulse delays for maximal SFG and FWM are governed primarily by the lifetime of the one-photon and two-photon resonant states, respectively. The method therefore offers an unconventional probe of the dynamics of excitonic states accessible with either one-photon or two-photon transitions. Remarkably, the longest delay times occur at the lowest excitation powers, indicating a strong nonlinearity that offers exploration potential for excitonic quantum nonlinear optics.



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Details

DokumentenartArtikel
Titel eines Journals oder einer ZeitschriftNature Photonics
Verlag:Nature
Ort der Veröffentlichung:BERLIN
Datum17 Oktober 2022
InstitutionenPhysik > Institut für Experimentelle und Angewandte Physik > Lehrstuhl Professor Lupton > Arbeitsgruppe John Lupton
Projekte
Gefördert von: Deutsche Forschungsgemeinschaft (DFG) (314695032)
Identifikationsnummer
WertTyp
10.1038/s41566-022-01080-1DOI
Stichwörter / KeywordsQUANTUM; PHOTON
Dewey-Dezimal-Klassifikation500 Naturwissenschaften und Mathematik > 530 Physik
StatusVeröffentlicht
BegutachtetJa, diese Version wurde begutachtet
An der Universität Regensburg entstandenJa
URN der UB Regensburgurn:nbn:de:bvb:355-epub-530819
Dokumenten-ID53081

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