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Broadband THz absorption spectrometer based on excitonic nonlinear optical effects.

ABSTRACT: A broadly tunable THz source is realized via difference frequency generation, in which an enhancement to χ(3) that is obtained via resonant excitation of III-V semiconductor quantum well excitons is utilized. The symmetry of the quantum wells (QWs) is broken by utilizing the built-in electric-field across a p-i-n junction to produce effective χ(2) processes, which are derived from the high χ(3). This χ(2) media exhibits an onset of nonlinear processes at ~4 W cm-2, thereby enabling area (and, hence, power) scaling of the THz emitter. Phase matching is realized laterally through normal incidence excitation. Using two collimated 130 mW continuous wave (CW) semiconductor lasers with ~1-mm beam diameters, we realize monochromatic THz emission that is tunable from 0.75 to 3 THz and demonstrate the possibility that this may span 0.2-6 THz with linewidths of ~20 GHz and efficiencies of ~1 × 10-5, thereby realizing ~800 nW of THz power. Then, transmission spectroscopy of atmospheric features is demonstrated, thereby opening the way for compact, low-cost, swept-wavelength THz spectroscopy.

SUBMITTER: Majeed A

PROVIDER: S-EPMC6414654 | biostudies-literature | 2019

REPOSITORIES: biostudies-literature

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Broadband THz absorption spectrometer based on excitonic nonlinear optical effects.

Majeed Avan A Ivanov Pavlo P Stevens Benjamin B Clarke Edmund E Butler Iain I Childs David D Kojima Osamu O Hogg Richard R

Light, science & applications 20190313

A broadly tunable THz source is realized via difference frequency generation, in which an enhancement to χ(3) that is obtained via resonant excitation of III-V semiconductor quantum well excitons is utilized. The symmetry of the quantum wells (QWs) is broken by utilizing the built-in electric-field across a p-i-n junction to produce effective χ(2) processes, which are derived from the high χ(3). This χ(2) media exhibits an onset of nonlinear processes ...[more]

PMID: 30886706

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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.

Dataset Information

Broadband THz absorption spectrometer based on excitonic nonlinear optical effects.

Publications

Broadband THz absorption spectrometer based on excitonic nonlinear optical effects.

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