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Extremely large third-order nonlinear optical effects caused by electron transport in quantum plasmonic metasurfaces with subnanometer gaps.

ABSTRACT: In this study, a third-order nonlinear optical responses in quantum plasmonic metasurfaces composed of metallic nano-objects with subnanometer gaps were investigated using time-dependent density functional theory, a fully quantum mechanical approach. At gap distances of???0.6 nm, the third-order nonlinearities monotonically increased as the gap distance decreased, owing to enhancement of the induced charge densities at the gaps between nano-objects. Particularly, when the third harmonic generation overlapped with the plasmon resonance, a large third-order nonlinearity was achieved. At smaller gap distances down to 0.1 nm, we observed the appearance of extremely large third-order nonlinearity without the assistance of the plasmon resonance. At a gap distance of 0.1 nm, the observed third-order nonlinearity was approximately three orders of magnitude larger than that seen at longer gap distances. The extremely large third-order nonlinearities were found to originate from electron transport by quantum tunneling and/or overbarrier currents through the subnanometer gaps.

SUBMITTER: Takeuchi T

PROVIDER: S-EPMC7718924 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature

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Extremely large third-order nonlinear optical effects caused by electron transport in quantum plasmonic metasurfaces with subnanometer gaps.

Takeuchi Takashi T Yabana Kazuhiro K

Scientific reports 20201204 1

In this study, a third-order nonlinear optical responses in quantum plasmonic metasurfaces composed of metallic nano-objects with subnanometer gaps were investigated using time-dependent density functional theory, a fully quantum mechanical approach. At gap distances of ≥ 0.6 nm, the third-order nonlinearities monotonically increased as the gap distance decreased, owing to enhancement of the induced charge densities at the gaps between nano-objects. Particularly, when the third harmonic generati ...[more]

PMID: 33277512

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Project description:In the present investigation, quantum chemical calculations have been performed in a systematic way to explore the optoelectronic, charge transfer, and nonlinear optical (NLO) properties of different bis(dicyanomethylene) end-functionalized quinoidal oligothiophenes. The effect of different conformations (linking modes of thiophene rings) on conformational, optoelectronic, and NLO properties are studied from the best-performed dimer to octamer. The optical and NLO properties of all the selected systems (1-7) are calculated by means of density functional theory (DFT) methods. Among all the designed compounds, the largest linear isotropic (αiso) polarizability value of 603.1 × 10-24 esu is shown by compound 7 which is ∼12, ∼16, ∼9, ∼11, ∼10, and ∼4 times larger as compared to compounds 1-6, respectively. A relative investigation is performed considering the expansion in third-order NLO polarizability as a function of size and conformational modes. Among all the investigated systems, system 7 shows the highest value of static second hyperpolarizability ⟨γ⟩ with an amplitude of 7607 × 10-36 esu at the M06/6-311G** level of theory, which is ∼521, ∼505, ∼38, ∼884, ∼185, and ∼15 times more than that of compounds 1-6, respectively. The extensively larger ⟨γ⟩ amplitude of compound 7 with higher oscillator strength and lower transition energy indicates that NLO properties are remarkably dependent upon linking modes of thiophene rings and its chain length. Furthermore, to trace the origin of higher nonlinearities, TD-DFT calculations are also performed at the same TD-M06/6-311G** level of theory. Additionally, a comprehensive understanding of the effect of structure/property relationship on the NLO polarizabilities of these investigated quinoidal oligothiophenes is obtained through the inspection of Frontier molecular orbitals, the density of states (TDOS and PDOS), and molecular electrostatic potential diagrams including the transition density matrix. Hence, the current examination will not just feature the NLO capability of entitled compounds yet additionally incite the interest of experimentalists to adequately modify the structure of these oligothiophenes for efficient optical and NLO applications.

Dataset Information

Extremely large third-order nonlinear optical effects caused by electron transport in quantum plasmonic metasurfaces with subnanometer gaps.

Publications

Extremely large third-order nonlinear optical effects caused by electron transport in quantum plasmonic metasurfaces with subnanometer gaps.

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