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Giant nonlinear optical activity in two-dimensional palladium diselenide.

ABSTRACT: Nonlinear optical effects in layered two-dimensional transition metal chalcogenides have been extensively explored recently because of the promising prospect of the nonlinear optical effects for various optoelectronic applications. However, these materials possess sizable bandgaps ranging from visible to ultraviolet region, so the investigation of narrow-bandgap materials remains deficient. Here, we report our comprehensive study on the nonlinear optical processes in palladium diselenide (PdSe₂) that has a near-infrared bandgap. Interestingly, this material exhibits a unique thickness-dependent second harmonic generation feature, which is in contrast to other transition metal chalcogenides. Furthermore, the two-photon absorption coefficients of 1-3 layer PdSe₂ (??~?4.16?×?10⁵, 2.58?×?10⁵, and 1.51?×?10⁵?cm?GW^-1) are larger by two and three orders of magnitude than that of the conventional two-dimensional materials, and giant modulation depths (?_s?~?32%, 27%, and 24%) were obtained in 1-3 layer PdSe₂. Such unique nonlinear optical characteristics make PdSe₂ a potential candidate for technological innovations in nonlinear optoelectronic devices.

SUBMITTER: Yu J

PROVIDER: S-EPMC7889859 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Giant nonlinear optical activity in two-dimensional palladium diselenide.

Yu Juan J Kuang Xiaofei X Li Junzi J Zhong Jiahong J Zeng Cheng C Cao Lingkai L Liu Zongwen Z Zeng Zhouxiaosong Z Luo Ziyu Z He Tingchao T Pan Anlian A Liu Yanping Y

Nature communications 20210217 1

Nonlinear optical effects in layered two-dimensional transition metal chalcogenides have been extensively explored recently because of the promising prospect of the nonlinear optical effects for various optoelectronic applications. However, these materials possess sizable bandgaps ranging from visible to ultraviolet region, so the investigation of narrow-bandgap materials remains deficient. Here, we report our comprehensive study on the nonlinear optical processes in palladium diselenide (PdSe<s ...[more]

PMID: 33597512

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Project description:Nonlinear optical (NLO) pigments are compounds insoluble in solvents that exhibit phenomena related to nonlinear optical susceptibilities (χ(n) where n = 2,3,...), e.g., two-photon absorption (2PA) which is related to the imaginary part of χ(3). Determination of spectrally-resolved 2PA properties for NLO pigments of macromolecular nature, such as coordination polymers or crosslinked polymers, has long been a challenging issue due to their particulate form, precluding characterizations with standard techniques such as Z-scan. In this contribution, we investigate thus far unknown spectrally-resolved 2PA properties of a new subclass of NLO pigments-crosslinked conjugated polymers. The studied compounds are built up from electron-donating (triphenylamine) and electron-withdrawing (2,2'-bipyridine) structural fragments joined by vinylene (Pol1) or vinyl(4-ethynylphenyl) (Pol2) aromatic bridges. 2PA properties of these polymers have been characterized in broad spectral range by specially modified two-photon excited fluorescence (TPEF) techniques: solid state TPEF (SSTPEF) and internal standard TPEF (ISTPEF). The impact of self-aggregation of aromatic backbones on the 2PA properties of the polymers has been evaluated through extended comparisons of NLO parameters, i.e., 2PA cross sections (σ2) and molar-mass normalized 2PA merit factors (σ2/M) with those of small-molecular model compounds: Mod1 and Mod2. By doing this, we found that the 2PA response of Pol1 and Pol2 is improved 2-3 times versus respective model compounds in the solid state form. Further comparisons with 2PA results collected for diluted solutions of Mod1 and Mod2 supports the notion that self-aggregated structure contributes to the observed enhancement of 2PA response. On the other hand, it is clear that Pol1 and Pol2 suffer from aggregation-caused quenching phenomenon, well reflected in time-resolved fluorescence properties as well as in relatively low values of quantum yield of fluorescence. Accordingly, despite improved intrinsic 2PA response, the effective intensity of two-photon excited emission for Pol1 and Pol2 is slightly lower relative to Mod1 and Mod2. Finally, we explore temperature-resolved luminescence properties under one- (377 nm), two- (820 nm), and three-photon excitation (1020 nm) conditions of postsynthetically Eu3+-functionalized material, Pol1-Eu, and discuss its suitability for temperature sensing applications.

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Giant nonlinear optical activity in two-dimensional palladium diselenide.

Publications

Giant nonlinear optical activity in two-dimensional palladium diselenide.

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