35 research outputs found

    Highly efficient, tunable single photon source based on single molecules

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    The authors studied spatially isolated terrylene molecules immobilized in a quasiplanar optical λ/2-microresonator using confocal microscopy and spectroscopy at variable temperatures. At T = 1.8 K, they observed individual molecules relaxing into microresonator-allowed vibronic levels of their electronic ground state by emission of single fluorescence photons. Coupling the purely electronic transition of embedded molecules to the longitudinal photonic mode of the microresonator resulted in an ultimate spectral narrowing and an increased collection efficiency of the emitted single photon wave trains

    Anisotropy and phonon modes from analysis of the dielectric function tensor and inverse dielectric function tensor of monoclinic yttrium orthosilicate

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    We determine the frequency dependence of the four independent Cartesian tensor elements of the dielectric function for monoclinic symmetry Y2_2SiO5_5 using generalized spectroscopic ellipsometry from 40-1200 cm−1^{-1}. Three different crystal cuts, each perpendicular to a principle axis, are investigated. We apply our recently described augmentation of lattice anharmonicity onto the eigendielectric displacement vector summation approach [A. Mock et al., Phys. Rev. B 95, 165202 (2017)], and we present and demonstrate the application of an eigendielectric displacement loss vector summation approach with anharmonic broadening. We obtain excellent match between all measured and model calculated dielectric function tensor elements and all dielectric loss function tensor elements. We obtain 23 Au_{\mathrm{u}} and 22 Bu_{\mathrm{u}} symmetry long wavelength active transverse and longitudinal optical mode parameters including their eigenvector orientation within the monoclinic lattice. We perform density functional theory calculations and obtain 23 Au_{\mathrm{u}} symmetry and 22 Bu_{\mathrm{u}} transverse and longitudinal optical mode parameters and their orientation within the monoclincic lattice. We compare our results from ellipsometry and density functional theory and find excellent agreement. We also determine the static and above reststrahlen spectral range dielectric tensor values and find a recently derived generalization of the Lyddane-Sachs-Teller relation for polar phonons in monoclinic symmetry materials satisfied [M. Schubert, Phys. Rev. Lett. 117, 215502 (2016)]

    Anisotropy, phonon modes, and lattice anharmonicity from dielectric function tensor analysis of monoclinic cadmium tungstate

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    We determine the frequency dependence of four independent CdWO4_4 Cartesian dielectric function tensor elements by generalized spectroscopic ellipsometry within mid-infrared and far-infrared spectral regions. Single crystal surfaces cut under different angles from a bulk crystal, (010) and (001), are investigated. From the spectral dependencies of the dielectric function tensor and its inverse we determine all long wavelength active transverse and longitudinal optic phonon modes with AuA_u and BuB_u symmetry as well as their eigenvectors within the monoclinic lattice. We thereby demonstrate that such information can be obtained completely without physical model line shape analysis in materials with monoclinic symmetry. We then augment the effect of lattice anharmonicity onto our recently described dielectric function tensor model approach for materials with monoclinic and triclinic crystal symmetries [Phys. Rev. B, 125209 (2016)], and we obtain excellent match between all measured and modeled dielectric function tensor elements. All phonon mode frequency and broadening parameters are determined in our model approach. We also perform density functional theory phonon mode calculations, and we compare our results obtained from theory, from direct dielectric function tensor analysis, and from model lineshape analysis, and we find excellent agreement between all approaches. We also discuss and present static and above reststrahlen spectral range dielectric constants. Our data for CdWO4_4 are in excellent agreement with a recently proposed generalization of the Lyddane-Sachs-Teller relation for materials with low crystal symmetry [Phys. Rev. Lett. 117, 215502 (2016)].Comment: arXiv admin note: text overlap with arXiv:1512.0859

    Electron effective mass in Sn-doped monoclinic single crystal β\beta-gallium oxide determined by mid-infrared optical Hall effect

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    The isotropic average conduction band minimum electron effective mass in Sn-doped monoclinic single crystal β\beta-Ga2_2O3_3 is experimentally determined by mid-infrared optical Hall effect to be (0.284±0.013)m0(0.284\pm0.013)m_{0} combining investigations on (010010) and (2ˉ01\bar{2}01) surface cuts. This result falls within the broad range of values predicted by theoretical calculations for undoped β\beta-Ga2_2O3_3. The result is also comparable to recent density functional calculations using the Gaussian-attenuation-Perdue-Burke-Ernzerhof hybrid density functional, which predict an average effective mass of 0.267m00.267m_{0} (arXiv:1704.06711 [cond-mat.mtrl-sci]). Within our uncertainty limits we detect no anisotropy for the electron effective mass, which is consistent with most previous theoretical calculations. We discuss upper limits for possible anisotropy of the electron effective mass parameter from our experimental uncertainty limits, and we compare our findings with recent theoretical results

    Laterally extended atomically precise graphene nanoribbons with improved electrical conductivity for efficient gas sensing

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    Narrow atomically precise graphene nanoribbons hold great promise for electronic and optoelectronic applications, but the previously demonstrated nanoribbon-based devices typically suffer from low currents and mobilities. In this study, we explored the idea of lateral extension of graphene nanoribbons for improving their electrical conductivity. We started with a conventional chevron graphene nanoribbon, and designed its laterally extended variant. We synthesized these new graphene nanoribbons in solution and found that the lateral extension results in decrease of their electronic bandgap and improvement in the electrical conductivity of nanoribbon-based thin films. These films were employed in gas sensors and an electronic nose system, which showed improved responsivities to low molecular weight alcohols compared to similar sensors based on benchmark graphitic materials, such as graphene and reduced graphene oxide, and a reliable analyte recognition. This study shows the methodology for designing new atomically precise graphene nanoribbons with improved properties, their bottom-up synthesis, characterization, processing and implementation in electronic devices

    Anisotropy, Phonon Modes, and Free Charge Carrier Parameters in Monoclinic β-Gallium Oxide Single Crystals

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    We derive a dielectric function tensor model approach to render the optical response of monoclinic and triclinic symmetry materials with multiple uncoupled infrared and far-infrared active modes. We apply our model approach to monoclinic β-Ga2O3 single-crystal samples. Surfaces cut under different angles from a bulk crystal, (010) and (2̅01), are investigated by generalized spectroscopic ellipsometry within infrared and far-infrared spectral regions. We determine the frequency dependence of 4 independent β-Ga2O3 Cartesian dielectric function tensor elements by matching large sets of experimental data using a point-by-point data inversion approach. From matching our monoclinic model to the obtained 4 dielectric function tensor components, we determine all infrared and far-infrared active transverse optic phonon modes with Au and Bu symmetry, and their eigenvectors within the monoclinic lattice. We find excellent agreement between our model results and results of density functional theory calculations. We derive and discuss the frequencies of longitudinal optical phonons in β-Ga2O3. We derive and report density and anisotropic mobility parameters of the free charge carriers within the tin-doped crystals. We discuss the occurrence of longitudinal phonon plasmon coupled modes in β-Ga2O3 and provide their frequencies and eigenvectors. We also discuss and present monoclinic dielectric constants for static electric fields and frequencies above the reststrahlen range, and we provide a generalization of the Lyddane-Sachs-Teller relation for monoclinic lattices with infrared and far-infrared active modes.We find that the generalized Lyddane-Sachs-Teller relation is fulfilled excellently for β-Ga2O3
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