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Defect-mediated carrier dynamics and third-order nonlinear optical response of WS2 quantum dots

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Abstract

In this Letter, we report the third-order absorptive and refractive nonlinear optical response of highly luminescent WS2 quantum dots (QDs) in the off-resonant femtosecond and nanosecond pulses, which is beneficial for optical limiting and quantum information processing. For 800 nm femtosecond excitation, QDs show two-photon absorption (β = (107 ± 2)×10−3 cm/GW) with positive nonlinearity originating from bound carriers. This picture changes significantly for 532 nm nanosecond excitation, where it shows reverse saturable absorption with negative nonlinearity primarily originating from the sequential absorption of two single photons through the shallow defects, creating free carriers. Our results provide a promising route toward low-dimensional optoelectronic devices.

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Supplementary Material (1)

NameDescription
Supplement 1       In the Supplemental Document, we describe the detailed synthesis of sample preparation, basic characterization, Raman study, analysis of time-resolved PL, Z-scan measurements, and femtosecond transient absorption

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Data underlying the results presented in this paper are not publicly available at this time but may be obtained from the authors upon reasonable request.

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