Sample records for absorption phonon raman

  1. Terahertz Sum-Frequency Excitation of a Raman-Active Phonon.

    PubMed

    Maehrlein, Sebastian; Paarmann, Alexander; Wolf, Martin; Kampfrath, Tobias

    2017-09-22

    In stimulated Raman scattering, two incident optical waves induce a force oscillating at the difference of the two light frequencies. This process has enabled important applications such as the excitation and coherent control of phonons and magnons by femtosecond laser pulses. Here, we experimentally and theoretically demonstrate the so far neglected up-conversion counterpart of this process: THz sum-frequency excitation of a Raman-active phonon mode, which is tantamount to two-photon absorption by an optical transition between two adjacent vibrational levels. Coherent control of an optical lattice vibration of diamond is achieved by an intense terahertz pulse whose spectrum is centered at half the phonon frequency of 40 THz. Remarkably, the carrier-envelope phase of the THz pulse is directly transferred into the phase of the lattice vibration. New prospects in general infrared spectroscopy, action spectroscopy, and lattice trajectory control in the electronic ground state emerge.

  2. Theory of Raman scattering in coupled electron-phonon systems

    NASA Astrophysics Data System (ADS)

    Itai, K.

    1992-01-01

    The Raman spectrum is calculated for a coupled conduction-electron-phonon system in the zero-momentum-transfer limit. The Raman scattering is due to electron-hole excitations and phonons as well. The phonons of those branches that contribute to the electron self-energy and the correction of the electron-phonon vertex are assumed to have flat energy dispersion (the Einstein phonons). The effect of electron-impurity scattering is also incorporated. Both the electron-phonon interaction and the electron-impurity interaction cause the fluctuation of the electron distribution between different parts of the Fermi surface, which results in overdamped zero-sound modes of various symmetries. The scattering cross section is obtained by solving the Bethe-Salpeter equation. The spectrum shows a lower threshold at the smallest Einstein phonon energy when only the electron-phonon interaction is taken into consideration. When impurities are also taken into consideration, the threshold disappears.

  3. Phononic glass: a robust acoustic-absorption material.

    PubMed

    Jiang, Heng; Wang, Yuren

    2012-08-01

    In order to achieve strong wide band acoustic absorption under high hydrostatic pressure, an interpenetrating network structure is introduced into the locally resonant phononic crystal to fabricate a type of phononic composite material called "phononic glass." Underwater acoustic absorption coefficient measurements show that the material owns high underwater sound absorption coefficients over 0.9 in 12-30 kHz. Moreover, the quasi-static compressive behavior shows that the phononic glass has a compressive strength over 5 MPa which is crucial for underwater applications.

  4. Quantum Theory of Conditional Phonon States in a Dual-Pumped Raman Optical Frequency Comb

    NASA Astrophysics Data System (ADS)

    Mondloch, Erin

    In this work, we theoretically and numerically investigate nonclassical phonon states created in the collective vibration of a Raman medium by the generation of a dual-pumped Raman optical frequency comb in an optical cavity. This frequency comb is generated by cascaded Raman scattering driven by two phase-locked pump lasers that are separated in frequency by three times the Raman phonon frequency. We characterize the variety of conditioned phonon states that are created when the number of photons in all optical frequency modes except the pump modes are measured. Almost all of these conditioned phonon states are extremely well approximated as three-phonon-squeezed states or Schrodinger-cat states, depending on the outcomes of the photon number measurements. We show how the combinations of first-, second-, and third-order Raman scattering that correspond to each set of measured photon numbers determine the fidelity of the conditioned phonon state with model three-phonon-squeezed states and Schrodinger-cat states. All of the conditioned phonon states demonstrate preferential growth of the phonon mode along three directions in phase space. That is, there are three preferred phase values that the phonon state takes on as a result of Raman scattering. We show that the combination of Raman processes that produces a given set of measured photon numbers always produces phonons in multiples of three. In the quantum number-state representation, these multiples of three are responsible for the threefold phase-space symmetry seen in the conditioned phonon states. With a semiclassical model, we show how this three-phase preference can also be understood in light of phase correlations that are known to spontaneously arise in single-pumped Raman frequency combs. Additionally, our semiclassical model predicts that the optical modes also grow preferentially along three phases, suggesting that the dual-pumped Raman optical frequency comb is partially phase-stabilized.

  5. Temperature induced phonon behaviour in germanium selenide thin films probed by Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Taube, A.; Łapińska, A.; Judek, J.; Wochtman, N.; Zdrojek, M.

    2016-08-01

    Here we report a detailed study of temperature-dependent phonon properties of exfoliated germanium selenide thin films (several tens of nanometers thick) probed by Raman spectroscopy in the 70-350 K temperature range. The temperature-dependent behavior of the positions and widths of the Raman modes was nonlinear. We concluded that the observed effects arise from anharmonic phonon-phonon interactions and are explained by the phenomenon of optical phonon decay into acoustic phonons. At temperatures above 200 K, the position of the Raman modes tended to be linearly dependent, and the first order temperature coefficients χ were  -0.0277, -0.0197 and  -0.031 cm-1 K-1 for B 3g , A g(1) and A g(2) modes, respectively.

  6. Fine Structure of the Low-Frequency Raman Phonon Bands of Single-Wall Carbon Nanotubes

    NASA Technical Reports Server (NTRS)

    Iliev, M. N.; Litvinchuk, A. P.; Arepalli, S.; Nikolaev, P.; Scott, C. D.

    1999-01-01

    The Raman spectra of singled-wall carbon nanotubes (SWNT) produced by laser and are process were studied between 5 and 500 kappa. The line width vs. temperature dependence of the low-frequency Raman bands between 150 and 200/ cm deviates from that expected for phonon decay through phonon-phonon scattering mechanism. The experimental results and their analysis provided convincing evidence that each of the low-frequency Raman lines is a superposition of several narrower Raman lines corresponding to tubes of nearly the same diameter. The application of Raman spectroscopy to probe the distribution of SWNT by both diameter and chirality is discussed.

  7. Raman scattering from TO phonons in (GaAs)n/(AlAs)n superlattices

    NASA Astrophysics Data System (ADS)

    Wang, Z. P.; Han, H. X.; Li, G. H.; Jiang, D. S.; Ploog, K.

    1988-10-01

    (GaAS)n/(AlAs)n superlattices with n=4, 6, and 8 grown by molecular-beam epitaxy on (001)-oriented GaAs substrates were investigated by Raman scattering. In a strict backscattering geometry, confined TO-phonon modes with E symmetry are Raman forbidden. However, the effects due to near-Brewster-angle incidence and a large aperture of the scattering-light collecting lens create a small wave-vector component along the (110) orientation, and thus induce a Raman activity of TO phonons. When we take X∥[11¯0], Y∥[110], and Z∥[001], in the near-Z(YX)Z¯ backscattering configuration confined LO-phonon modes are Raman inactive. Using this configuration, we have for the first time observed both GaAs-like and AlAs-like confined TO-phonon modes at room temperature and under off-resonance conditions.

  8. Electron phonon couplings in 2D perovskite probed by ultrafast photoinduced absorption spectroscopy

    NASA Astrophysics Data System (ADS)

    Huynh, Uyen; Ni, Limeng; Rao, Akshay

    We use the time-resolved photoinduced absorption (PIA) spectroscopy with 20fs time resolution to investigate the electron phonon coupling in the self-assembled hybrid organic layered perovskite, the hexyl ammonium lead iodide compound (C6H13NH3)2 (PbI4) . The coupling results in the broadening and asymmetry of its temperature-dependence photoluminescence spectra. The exact time scale of this coupling, however, wasn't reported experimentally. Here we show that using an ultrashort excitation pulse allows us to resolve from PIA kinetics the oscillation of coherent longitudinal optical phonons that relaxes and self-traps electrons to lower energy states within 200 fs. The 200fs relaxation time is equivalent to a coupling strength of 40meV. Two coupled phonon modes are also identified as about 100 cm-1 and 300 cm-1 from the FFT spectrum of the PIA kinetics. The lower energy mode is consistent with previous reports and Raman spectrum but the higher energy one hasn't been observed before.

  9. Raman analysis of phonon modes in a short period AlN/GaN superlattice

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Sarkar, Ketaki; Datta, Debopam; Gosztola, David J.

    AlN/GaN-based optoelectronic devices have been the subject of intense research underlying the commercialization of efficient devices. Areas of considerable interest are the study of their lattice dynamics, phonon transport, and electron-phonon interactions specific to the interface of these heterostructures which results in additional optical phonon modes known as interface phonon modes. In this study, the framework of the dielectric continuum model (DCM) has been used to compare and analyze the optical phonon modes obtained from experimental Raman scattering measurements on AlN/GaN short-period superlattices. We have observed the localized E2(high), A1(LO) and the E1(TO) modes in superlattice measurements at frequencies shiftedmore » from their bulk values. To the best of our knowledge, the nanostructures used in these studies are among the smallest yielding useful Raman signatures for the interface modes. In addition, we have also identified an additional spread of interface phonon modes in the TO range resulting from the superlattice periodicity. The Raman signature contribution from the underlying AlxGa1-xN ternary has also been observed and analyzed. A temperature calibrationwas done based on Stokes/anti-Stokes ratio of A1(LO) using Raman spectroscopy in a broad operating temperature range. Good agreement between the experimental results and theoretically calculated calibration plot predicted using Bose-Einstein statistics was obtained.« less

  10. Raman analysis of phonon modes in a short period AlN/GaN superlattice

    NASA Astrophysics Data System (ADS)

    Sarkar, Ketaki; Datta, Debopam; Gosztola, David J.; Shi, Fengyuan; Nicholls, Alan; Stroscio, Michael A.; Dutta, Mitra

    2018-03-01

    AlN/GaN-based optoelectronic devices have been the subject of intense research underlying the commercialization of efficient devices. Areas of considerable interest are the study of their lattice dynamics, phonon transport, and electron-phonon interactions specific to the interface of these heterostructures which results in additional optical phonon modes known as interface phonon modes. In this study, the framework of the dielectric continuum model (DCM) has been used to compare and analyze the optical phonon modes obtained from experimental Raman scattering measurements on AlN/GaN short-period superlattices. We have observed the localized E2(high), A1(LO) and the E1(TO) modes in superlattice measurements at frequencies shifted from their bulk values. To the best of our knowledge, the nanostructures used in these studies are among the smallest yielding useful Raman signatures for the interface modes. In addition, we have also identified an additional spread of interface phonon modes in the TO range resulting from the superlattice periodicity. The Raman signature contribution from the underlying AlxGa1-xN ternary has also been observed and analyzed. A temperature calibration was done based on Stokes/anti-Stokes ratio of A1(LO) using Raman spectroscopy in a broad operating temperature range. Good agreement between the experimental results and theoretically calculated calibration plot predicted using Bose-Einstein statistics was obtained.

  11. Phonon-Assisted Optical Absorption in Silicon from First Principles

    NASA Astrophysics Data System (ADS)

    Noffsinger, Jesse; Kioupakis, Emmanouil; Van de Walle, Chris G.; Louie, Steven G.; Cohen, Marvin L.

    2012-04-01

    The phonon-assisted interband optical absorption spectrum of silicon is calculated at the quasiparticle level entirely from first principles. We make use of the Wannier interpolation formalism to determine the quasiparticle energies, as well as the optical transition and electron-phonon coupling matrix elements, on fine grids in the Brillouin zone. The calculated spectrum near the onset of indirect absorption is in very good agreement with experimental measurements for a range of temperatures. Moreover, our method can accurately determine the optical absorption spectrum of silicon in the visible range, an important process for optoelectronic and photovoltaic applications that cannot be addressed with simple models. The computational formalism is quite general and can be used to understand the phonon-assisted absorption processes in general.

  12. Size dependent Raman and absorption studies of single walled carbon nanotubes synthesized by pulse laser deposition at room temperature

    NASA Astrophysics Data System (ADS)

    Dixit, Saurabh; Singhal, Sonal; Vankar, V. D.; Shukla, A. K.

    2017-10-01

    In this article, size dependent correlation of acoustic states is established for radial breathing mode (RBM). Single walled carbon nanotubes (SWCNTs) are synthesized along with carbon encapsulated iron nanoparticles by pulse laser deposition at room temperature. Ferrocene is used as a catalyst for growth of SWCNTs. Various studies such as HR-TEM, X-Ray Diffraction (XRD), Raman spectroscopy and NIR-Absorption spectroscopy are utilized to confirm the presence of SWCNTs in the as-synthesized and purified samples. RBM of SWCNTs can be differentiated here from Raman modes of carbon encapsulated iron nanoparticles by comparing their line shape asymmetry as well as oscillator strength. Furthermore, a quantum confinement model is proposed for RBM. It is invoked here that RBM is manifestation of quantum confinement of acoustic phonons. Well reported analytical relation of RBM is utilized to explore the nature of phonons responsible for RBM on the basis of quantum confinement model. Diameters of SWCNTs estimated by Raman studies are found to be in reasonably good agreement with that of NIR-absorption studies.

  13. Enhancement of multiple-phonon resonant Raman scattering in Co-doped ZnO nanorods

    NASA Astrophysics Data System (ADS)

    Phan, The-Long; Vincent, Roger; Cherns, David; Dan, Nguyen Huy; Yu, Seong-Cho

    2008-08-01

    We have studied Raman scattering in Co-doped ZnO nanorods prepared by thermal diffusion. Experimental results show that the features of their non-resonant spectra are similar to Raman spectra from Co-doped ZnO materials investigated previously. Under resonant conditions, however, there is a strong enhancement of multiple-phonon Raman scattering processes. Longitudinal optical (LO)-phonon overtones up to eleventh order are observed. The modes become more obvious when the Co concentration diffused into ZnO nanorods goes to an appropriate value. This phenomenon is explained due to the shift of the band-gap energy and also due to the decrease in the intensity of near-band-edge luminescence. Our observation is in agreement with the prediction [J. F. Scott, Phys. Rev. B 2, 1209 (1970)] that the number of LO-phonon lines in ZnO is higher than that observed for CdS.

  14. Raman scattering from phonons and magnons in magnetic semiconductors, MnTe

    NASA Technical Reports Server (NTRS)

    Mobasser, S. R.; Hart, T. R.

    1985-01-01

    Comparisons are made between theoretical and experimental data on laser Raman scattering by phonons and two-magnons in antiferromagnetic and paramagnetic phases of MnTe. The study was performed specifically to characterize the magnetic exchange coupling constants of the Mn ions in the samples. Crystal MnTe samples were bombarded with an Ar ion laser beam to obtain spectrometer and photon counter data. One E(2g) phonon with a room temperature energy of 178/cm and a two-magnon peak of 360/cm were observed in the Raman spectrum. A spin wave dispersion relation is presented for the spectrum. Finally, a Monte Carlo technique was used to calculate the two-magnon joint density of states that best fits the experimental data.

  15. Phonon-assisted optical absorption in BaSnO 3 from first principles

    NASA Astrophysics Data System (ADS)

    Monserrat, Bartomeu; Dreyer, Cyrus E.; Rabe, Karin M.

    2018-03-01

    The perovskite BaSnO3 provides a promising platform for the realization of an earth-abundant n -type transparent conductor. Its optical properties are dominated by a dispersive conduction band of Sn 5 s states and by a flatter valence band of O 2 p states, with an overall indirect gap of about 2.9 eV . Using first-principles methods, we study the optical properties of BaSnO3 and show that both electron-phonon interactions and exact exchange, included using a hybrid functional, are necessary to obtain a qualitatively correct description of optical absorption in this material. In particular, the electron-phonon interaction drives phonon-assisted optical absorption across the minimum indirect gap and therefore determines the absorption onset, and it also leads to the temperature dependence of the absorption spectrum. Electronic correlations beyond semilocal density functional theory are key to determine the dynamical stability of the cubic perovskite structure, as well as the correct energies of the conduction bands that dominate absorption. Our work demonstrates that phonon-mediated absorption processes should be included in the design of novel transparent conductor materials.

  16. First-principles calculations of phonons and Raman and infrared spectra in Cd-IV-N2 compounds

    NASA Astrophysics Data System (ADS)

    Lyu, Sai; Lambrecht, Walter R. L.

    2018-05-01

    A first-principles study of the phonons at the zone center in Cd-IV-N2 compounds is presented with IV = Si, Ge, Sn. The calculations are performed for the most likely Pbn21 crystal structure, after showing that it is indeed lower in total energy compared to the closely related Pmc21 structure. The normal mode frequencies are calculated using density functional perturbation theory and symmetry labeled. The longitudinal optical-transverse optical splittings are determined using the Born effective charges which are also reported. These are used to simulate polarized Raman spectra for different scattering configurations as well as the infrared absorption and reflection spectra. The mode frequencies are found to decrease from Si to Ge to Sn as group-IV cation. The spectra show a wide variety of number of prominent peaks and relative intensities in spite of the great similarities of these three materials. Phonon densities of states and their analysis in atom by atom contributions are also reported.

  17. Folded Optical Phonons in Twisted Bilayer Graphene: Raman Signature of Graphene Superlattices

    NASA Astrophysics Data System (ADS)

    Wang, Yanan; Su, Zhihua; Wu, Wei; Xing, Sirui; Lu, Xiaoxiang; Lu, Xinghua; Pei, Shin-Shem; Robles-Hernandez, Francisco; Hadjiev, Viktor; Bao, Jiming

    2013-03-01

    In contrast to Bernal-stacked graphene exfoliated from HOPG, twisted bilayer graphene are widely observed in the samples prepared by silicon sublimation of SiC or chemical vapor deposition (CVD). However, many of its basic properties still remain unrevealed. In this work, hexagon-shaped bilayer graphene islands synthesized by CVD method were systematically studied using Raman spectroscopy. A series of folded phonons were observed in the range from 1375 cm-1 to 1525 cm-1. The frequency of folded phonon modes doesn't shift with laser excitation energy, but it is highly dependent on the rotational angle between two layers. In general, the frequency of folded phonon decreases with the increase of rotation angle. This rotation dependence can be qualitatively explained by the folding of phonon dispersion curve of single layer graphene into the reduced Brillouin zone of bilayer superlattice. The obseravtion of folded phonon is an important indication of superlattice band structure.

  18. Experimental study on the sound absorption characteristics of continuously graded phononic crystals

    NASA Astrophysics Data System (ADS)

    Zhang, X. H.; Qu, Z. G.; He, X. C.; Lu, D. L.

    2016-10-01

    Novel three-dimensional (3D) continuously graded phononic crystals (CGPCs) have been designed, and fabricated by 3D printing. Each of the CGPCs is an entity instead of a combination of several other samples, and the porosity distribution of the CGPC along the incident direction is nearly linear. The sound absorption characteristics of CGPCs were experimentally investigated and compared with those of uniform phononic crystals (UPCs) and discretely stepped phononic crystals (DSPCs). Experimental results show that CGPCs demonstrate excellent sound absorption performance because of their continuously graded structures. CGPCs have higher sound absorption coefficients in the large frequency range and more sound absorption coefficient peaks in a specific frequency range than UPCs and DSPCs. In particular, the sound absorption coefficients of the CGPC with a porosity of 0.6 and thickness of 30 mm are higher than 0.56 when the frequency is 1350-6300 Hz and are all higher than 0.2 in the studied frequency range (1000-6300 Hz). CGPCs are expected to have potential application in noise control, especially in the broad frequency and low-frequency ranges.

  19. Raman spectroscopy of magneto-phonon resonances in graphene and graphite

    NASA Astrophysics Data System (ADS)

    Goler, Sarah; Yan, Jun; Pellegrini, Vittorio; Pinczuk, Aron

    2012-08-01

    The magneto-phonon resonance or MPR occurs in semiconductor materials when the energy spacing between Landau levels is continuously tuned to cross the energy of an optical phonon mode. MPRs have been largely explored in bulk semiconductors, in two-dimensional systems and in quantum dots. Recently there has been significant interest in the MPR interactions of the Dirac fermion magneto-excitons in graphene, and a rich splitting and anti-crossing phenomena of the even parity E2g long wavelength optical phonon mode have been theoretically proposed and experimentally observed. The MPR has been found to crucially depend on disorder in the graphene layer. This is a feature that creates new venues for the study of interplays between disorder and interactions in the atomic layers. We review here the fundamentals of MRP in graphene and the experimental Raman scattering works that have led to the observation of these phenomena in graphene and graphite.

  20. Magneto-optical absorption and cyclotron-phonon resonance in graphene monolayer

    NASA Astrophysics Data System (ADS)

    Hoi, Bui Dinh; Phuong, Le Thi Thu; Phong, Tran Cong

    2018-03-01

    The optical absorption power by Dirac fermions in a graphene monolayer subjected to a perpendicular magnetic field is calculated using a projection operator technique. The electron-optical phonon interaction with optical deformation potential is taken into account. By varying the photon frequency (energy), we observe in the absorption power a series of cyclotron-phonon resonance (CPR) peaks (i.e., the phonon-assisted cyclotron resonance). It is seen that the resonant photon energy is linearly proportional to the square root of the magnetic field. Also, the half width at half maximum (HWHM) of CPR peaks depends on the magnetic field by the law HWHM = 7.42 √{B } but does not depend on the temperature. In particular, the magnetic field and temperature dependences of the position and HWHM of CPR peaks are in good agreement with those obtained recently by the perturbation theory and an experiment in graphene.

  1. First-principles modeling of resonant Raman scattering for the understanding of phonons and electrons in nanomaterials

    NASA Astrophysics Data System (ADS)

    Liang, Liangbo; Meunier, Vincent; Yan, Jia-An; Sumpter, Bobby

    Raman spectroscopy is a popular tool that can probe both phonons and electrons of the materials. First-principles modeling is important in aiding the understanding of experimental data. Raman modeling is typically based on the classical Placzek approximation and limited to the non-resonant condition, and thus the laser energy dependence of Raman intensities could not be captured. Here we showed that resonant Raman scattering could be captured by upgrading the classical approach, i.e., by calculating the dynamic dielectric tensor at the laser energy instead of the commonly used static value at zero energy. Our method was successfully applied to recently synthesized atomically precise graphene nanoribbons, and revealed the photon-energy-dependent Raman intensity of the radial breathing like mode (RBLM), which explained experimental observations that RBLM can be only observed in certain laser energies. Additionally, we also explored anisotropic 2D material, ReS2, and found that the angle-resolved Raman polarization dependence of its Raman modes is sensitive to the laser energy, as confirmed by recent experiments. The intricate electron-phonon coupling could lead to no simple rule for using Raman polarization dependence to determine the crystalline orientation. LL is supported by Eugene P. Wigner Fellowship at Oak Ridge National Laboratory and CNMS (a DOE Office of Science User Facility).

  2. Angular dependence of Raman scattering selection rules for long-wavelength optical phonons in short-period GaAs/AlAs superlattices

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Volodin, V. A., E-mail: volodin@isp.nsc.ru; Sachkov, V. A.; Sinyukov, M. P.

    2016-07-15

    The angular dependence of Raman scattering selection rules for optical phonons in short-period (001) GaAs/AlAs superlattices is calculated and experimentally studied. Experiments are performed using a micro-Raman setup, in the scattering geometry with the wavevectors of the incident and scattered light lying in the plane of superlattices (so-called in-plane geometry). Phonon frequencies are calculated using the Born model taking the Coulomb interaction into account in the rigid-ion approximation. Raman scattering spectra are calculated in the framework of the deformation potential and electro-optical mechanisms. Calculations show an angular dependence of the selection rules for optical phonons with different directions of themore » wavevectors. Drastic differences in the selection rules are found for experimental and calculated spectra. Presumably, these differences are due to the Fröhlich mechanism in Raman scattering for short-period superlattices.« less

  3. Single nanowire thermal conductivity measurements by Raman thermography.

    PubMed

    Doerk, Gregory S; Carraro, Carlo; Maboudian, Roya

    2010-08-24

    A facile, rapid, and nondestructive technique for determining the thermal conductivity of individual nanowires based on Raman temperature mapping has been demonstrated. Using calculated absorption efficiencies, the thermal conductivities of single cantilevered Si nanowires grown by the vapor-liquid-solid method are measured and the results agree well with values predicted by diffuse phonon boundary scattering. As a measurement performed on the wire, thermal contact effects are avoided and ambient air convection is found to be negligible for the range of diameters measured. The method's versatility is further exemplified in the reverse measurement of a single nanowire absorption efficiency assuming diffuse phonon boundary scattering. The results presented here outline the broad utility that Raman thermography may have for future thermoelectric and photovoltaic characterization of nanostructures.

  4. Fully ab initio calculation of the resonant one-phonon Raman intensity of graphene

    NASA Astrophysics Data System (ADS)

    Reichardt, Sven; Wirtz, Ludger

    We developed a fully ab initio, many-body perturbation theory approach for the calculation of resonant, one-phonon Raman spectra. Our general approach is applicable to any material and here we present its application to the case of graphene. Our diagrammatic, first-principles approach allows us to go beyond and improve on an earlier theoretical study by Basko, which relied on an analytical calculation in certain limits. We investigate the dependence of the G peak intensity on both the excitation energy and Fermi level. Furthermore, our method allows us to identify the relevant electronic quantum pathways and to demonstrate the importance of the contributions from non-resonant electronic transitions. We also applied our approach to the calculation of the resonant one-phonon Raman spectrum of MoS2, with our results being in good agreement with experimental data. SR acknowledges financial support from the National Research Fund (FNR) Luxembourg.

  5. Temperature dependence of the Urbach optical absorption edge: A theory of multiple phonon absorption and emission sidebands

    NASA Astrophysics Data System (ADS)

    Grein, C. H.; John, Sajeev

    1989-01-01

    The optical absorption coefficient for subgap electronic transitions in crystalline and disordered semiconductors is calculated by first-principles means with use of a variational principle based on the Feynman path-integral representation of the transition amplitude. This incorporates the synergetic interplay of static disorder and the nonadiabatic quantum dynamics of the coupled electron-phonon system. Over photon-energy ranges of experimental interest, this method predicts accurate linear exponential Urbach behavior of the absorption coefficient. At finite temperatures the nonlinear electron-phonon interaction gives rise to multiple phonon emission and absorption sidebands which accompany the optically induced electronic transition. These sidebands dominate the absorption in the Urbach regime and account for the temperature dependence of the Urbach slope and energy gap. The physical picture which emerges is that the phonons absorbed from the heat bath are then reemitted into a dynamical polaronlike potential well which localizes the electron. At zero temperature we recover the usual polaron theory. At high temperatures the calculated tail is qualitatively similar to that of a static Gaussian random potential. This leads to a linear relationship between the Urbach slope and the downshift of the extrapolated continuum band edge as well as a temperature-independent Urbach focus. At very low temperatures, deviations from these rules are predicted arising from the true quantum dynamics of the lattice. Excellent agreement is found with experimental data on c-Si, a-Si:H, a-As2Se3, and a-As2S3. Results are compared with a simple physical argument based on the most-probable-potential-well method.

  6. Scattering Tools for Nanostructure Phonon Engineering

    DTIC Science & Technology

    2013-09-25

    characterization of phonons in nanomaterials, such as Raman scattering, are sensitive only to phonon modes with wavevectors of extremely small magnitude...Fundamentally the wavevectors that can be probed by Raman scattering are limited by the small momentum of photons in the visible spectrum. Our work...serious characterization challenge because existing experimental techniques for the characterization of phonons in nanomaterials, such as Raman

  7. Optical phonon modes of III-V nanoparticles and indium phosphide/II-VI core-shell nanoparticles: A Raman and infrared study

    NASA Astrophysics Data System (ADS)

    Manciu, Felicia Speranta

    The prospects for realizing efficient nanoparticle light emitters in the visible/near IR for communications and bio-medical applications have benefited from progress in chemical fabrication of nanoparticles. III-V semiconductor nanopaticles such as GaP and InP are promising materials for the development of "blue" and "green" emitters, respectively, due to their large effective bandgaps. Enhanced emission efficiency has been achieved for core-shell nanoparticles, since inorganic shell materials increase electronic tunability and may decrease surface defects that often occur for nanoparticles capped with organic molecules. Also, the emission wavelength of InP nanoparticle cores can be tuned from green to red by changing the shell material in InP/II-VI core-shell nanoparticles. Investigations of phonon modes in nanocrystals are of both fundamental and applied interest. In the former case the optical phonon modes, such as surface/interface modes, are dependent on the nanoparticle dimensions, and also can provide information about dynamical properties of the nanoparticles and test the validity of various theoretical approaches. In the latter case the vibronic properties of nanoparticle emitters are controlled by confined phonons and modifications of the electron-phonon interaction by the confinement. Thus, the objective of the present thesis is the detailed study of the phonon modes of III-V nanoparticles (GaP and InP) and InP/II-VI core-shell nanoparticles by IR absorption and Raman scattering spectroscopies, and an elucidation of their complex vibrational properties. With the exception of three samples (two GaP and one InP), all samples were synthesized by a novel colloidal chemistry method, which does not requires added surfactant, but rather treatment of the corresponding precursors in octadecene noncoordinative solvent. Sample quality was characterized by ED, TEM and X-ray diffraction. Based on a comparison with a dielectric continuum model, the observed features

  8. Phonon Self-Energy Corrections to Nonzero Wave-Vector Phonon Modes in Single-Layer Graphene

    NASA Astrophysics Data System (ADS)

    Araujo, P. T.; Mafra, D. L.; Sato, K.; Saito, R.; Kong, J.; Dresselhaus, M. S.

    2012-07-01

    Phonon self-energy corrections have mostly been studied theoretically and experimentally for phonon modes with zone-center (q=0) wave vectors. Here, gate-modulated Raman scattering is used to study phonons of a single layer of graphene originating from a double-resonant Raman process with q≠0. The observed phonon renormalization effects are different from what is observed for the zone-center q=0 case. To explain our experimental findings, we explored the phonon self-energy for the phonons with nonzero wave vectors (q≠0) in single-layer graphene in which the frequencies and decay widths are expected to behave oppositely to the behavior observed in the corresponding zone-center q=0 processes. Within this framework, we resolve the identification of the phonon modes contributing to the G⋆ Raman feature at 2450cm-1 to include the iTO+LA combination modes with q≠0 and also the 2iTO overtone modes with q=0, showing both to be associated with wave vectors near the high symmetry point K in the Brillouin zone.

  9. The Influence of Phonons and Phonon Decay on the Optical Properties of GaN

    NASA Astrophysics Data System (ADS)

    Song, D. Y.; Basavaraj, M.; Nikishin, S. A.; Holtz, M.; Soukhoveev, V.; Usikov, A.; Dmitriev, V.

    2006-03-01

    The temperature dependences of vibrational and optical properties of high-quality GaN are studied using Raman and photoluminescence (PL) spectroscopies in the range 20 to 325 K. The Raman-active A1(LO) phonon has temperature dependence described well by combined two- and three-phonon decay. The temperature dependences of E2^2 phonon are almost entirely dominated by the thermal expansion, and the contribution of three-phonon decay process is very small throughout interested temperature range. The shallow neutral donor-bound exciton (D^0,X) and two free excitons (XA and XB) are observed at low temperatrue PL spectra. Also seen are two A1(LO) phonon sidebands (PSBs), originating from the XB free exciton, with the characteristic asymmetry attributed to interactions between discrete and continuum states. Analysis of the band-edge excitons reveals that energy gap shrinkage and exciton linewidths are completely described based on electron-phonon interactions with phonon properties consistent with the Raman analysis. First and second PSBs have temperature dependence associated with the A1(LO) phonon. The shift, broadening, and asymmetry of the PSBs are explained by Segall-Mahan theory adding the decay mechanism of A1(LO) phonon and the exciton broadening from electron-phonon interactions. Work at Texas Tech University supported by National Science Foundation grant ECS-0323640.

  10. Anisotropic Electron-Photon and Electron-Phonon Interactions in Black Phosphorus

    DOE PAGES

    Ling, Xi; Huang, Shengxi; Hasdeo, Eddwi; ...

    2016-03-10

    Orthorhombic black phosphorus (BP) and other layered materials, such as gallium telluride (GaTe) and tin selenide (SnSe), stand out among two-dimensional (2D) materials owing to their anisotropic in-plane structure. This anisotropy adds a new dimension to the properties of 2D materials and stimulates the development of angle-resolved photonics and electronics. However, understanding the effect of anisotropy has remained unsatisfactory to-date, as shown by a number of inconsistencies in the recent literatures. We use angle-resolved absorption and Raman spectroscopies to investigate the role of anisotropy on the electron-photon and electron-phonon interactions in BP. We highlight a non-trivial dependence between anisotropies andmore » flake thickness, photon and phonon energies. We show that once understood, the anisotropic optical absorption appears to be a reliable and simple way to identify the crystalline orientation of BP, which cannot be determined from Raman spectroscopy without the explicit consideration of excitation wavelength and flake thickness, as commonly used previously.« less

  11. Phonon self-energy corrections to non-zero wavevector phonon modes in single-layer graphene

    NASA Astrophysics Data System (ADS)

    Araujo, Paulo; Mafra, Daniela; Sato, Kentaro; Saito, Richiiro; Kong, Jing; Dresselhaus, Mildred

    2012-02-01

    Phonon self-energy corrections have mostly been studied theoretically and experimentally for phonon modes with zone-center (q = 0) wave-vectors. Here, gate-modulated Raman scattering is used to study phonons of a single layer of graphene (1LG) in the frequency range from 2350 to 2750 cm-1, which shows the G* and the G'-band features originating from a double-resonant Raman process with q 0. The observed phonon renormalization effects are different from what is observed for the zone-center q = 0 case. To explain our experimental findings, we explored the phonon self-energy for the phonons with non-zero wave-vectors (q 0) in 1LG in which the frequencies and decay widths are expected to behave oppositely to the behavior observed in the corresponding zone-center q = 0 processes. Within this framework, we resolve the identification of the phonon modes contributing to the G* Raman feature at 2450 cm-1 to include the iTO+LA combination modes with q 0 and the 2iTO overtone modes with q = 0, showing both to be associated with wave-vectors near the high symmetry point K in the Brillouin zone.

  12. Reliability of Raman measurements of thermal conductivity of single-layer graphene due to selective electron-phonon coupling: A first-principles study

    NASA Astrophysics Data System (ADS)

    Vallabhaneni, Ajit K.; Singh, Dhruv; Bao, Hua; Murthy, Jayathi; Ruan, Xiulin

    2016-03-01

    Raman spectroscopy has been widely used to measure thermal conductivity (κ ) of two-dimensional (2D) materials such as graphene. This method is based on a well-accepted assumption that different phonon polarizations are in near thermal equilibrium. However, in this paper, we show that, in laser-irradiated single-layer graphene, different phonon polarizations are in strong nonequilibrium, using predictive simulations based on first principles density functional perturbation theory and a multitemperature model. We first calculate the electron cooling rate due to phonon scattering as a function of the electron and phonon temperatures, and the results clearly illustrate that optical phonons dominate the hot electron relaxation process. We then use these results in conjunction with the phonon scattering rates computed using perturbation theory to develop a multitemperature model and resolve the spatial temperature distributions of the energy carriers in graphene under steady-state laser irradiation. Our results show that electrons, optical phonons, and acoustic phonons are in strong nonequilibrium, with the flexural acoustic (ZA) phonons showing the largest nonequilibrium to other phonon modes, mainly due to their weak coupling to other carriers in suspended graphene. Since ZA phonons are the main heat carriers in graphene, we estimate that neglecting this nonequilibrium leads to underestimation of thermal conductivity in experiments at room temperature by a factor of 1.35 to 2.6, depending on experimental conditions and assumptions used. Underestimation is also expected in Raman measurements of other 2D materials when the optical-acoustic phonon coupling is weak.

  13. Effects of acoustic- and optical-phonon sidebands on the fundamental optical-absorption edge in crystals and disordered semiconductors

    NASA Astrophysics Data System (ADS)

    Grein, C. H.; John, Sajeev

    1990-04-01

    We present the results of a parameter-free first-principles theory for the fine structure of the Urbach optical-absorption edge in crystalline and disordered semiconductors. The dominant features are recaptured by means of a simple physical argument based on the most probable potential-well analogy. At finite temperatures, the overall linear exponential Urbach behavior of the subgap optical-absorption coefficient is a consequence of multiple LA-phonon emission and absorption sidebands that accompany the electronic transition. The fine structure of subgap absorption spectra observed in some materials is accounted for by multiple TO-, LO-, and TA-phonon absorption and emission sidebands. Good agreement is found with experimental data on crystalline silicon. The effects of nonadiabaticity in the electron-phonon interaction are calculated.

  14. Enhanced light scattering of the forbidden longitudinal optical phonon mode studied by micro-Raman spectroscopy on single InN nanowires.

    PubMed

    Schäfer-Nolte, E O; Stoica, T; Gotschke, T; Limbach, F A; Sutter, E; Sutter, P; Grützmacher, D; Calarco, R

    2010-08-06

    In the literature, there are controversies on the interpretation of the appearance in InN Raman spectra of a strong scattering peak in the energy region of the unscreened longitudinal optical (LO) phonons, although a shift caused by the phonon-plasmon interaction is expected for the high conductance observed in this material. Most measurements on light scattering are performed on ensembles of InN nanowires (NWs). However, it is important to investigate the behavior of individual nanowires and here we report on micro-Raman measurements on single nanowires. When changing the polarization direction of the incident light from parallel to perpendicular to the wire, the expected reduction of the Raman scattering was observed for transversal optical (TO) and E(2) phonon scattering modes, while a strong symmetry-forbidden LO mode was observed independently on the laser polarization direction. Single Mg- and Si-doped crystalline InN nanowires were also investigated. Magnesium doping results in a sharpening of the Raman peaks, while silicon doping leads to an asymmetric broadening of the LO peak. The results can be explained based on the influence of the high electron concentration with a strong contribution of the surface accumulation layer and the associated internal electric field.

  15. Raman Scattering Study of the Soft Phonon Mode in the Hexagonal Ferroelectric Crystal KNiCl 3

    NASA Astrophysics Data System (ADS)

    Machida, Ken-ichi; Kato, Tetsuya; Chao, Peng; Iio, Katsunori

    1997-10-01

    Raman spectra of some phonon modes of the hexagonal ferroelectriccrystal KNiCl3are obtained in the temperature range between 290 K and 590 K, which includes the structural phase transition point T2(=561 K) at which previous measurements of dielectric constant and spontaneouspolarization as a function of temperature had shown that KNiCl3 undergoes a transition between polar phases II and III. An optical birefringence measurement carried outas a complement to the present Raman scattering revealed that this transition is of second order. Towards this transition point, the totally symmetric phonon mode with the lowest frequency observed in the room-temperature phasewas found to soften with increasing temperature.The present results provide new information on the phase-transitionmechanism and the space groups of thehigher (II)- and lower (III)-symmetric phases around T2.

  16. Phonon Raman spectra of colloidal CdTe nanocrystals: effect of size, non-stoichiometry and ligand exchange

    PubMed Central

    2011-01-01

    Resonant Raman study reveals the noticeable effect of the ligand exchange on the nanocrystal (NC) surface onto the phonon spectra of colloidal CdTe NC of different size and composition. The oleic acid ligand exchange for pyridine ones was found to change noticeably the position and width of the longitudinal optical (LO) phonon mode, as well as its intensity ratio to overtones. The broad shoulder above the LO peak frequency was enhanced and sharpened after pyridine treatment, as well as with decreasing NC size. The low-frequency mode around 100 cm-1 which is commonly related with the disorder-activated acoustical phonons appears in smaller NCs but is not enhanced after pyridine treatment. Surprisingly, the feature at low-frequency shoulder of the LO peak, commonly assigned to the surface optical phonon mode, was not sensitive to ligand exchange and concomitant close packing of the NCs. An increased structural disorder on the NC surface, strain and modified electron-phonon coupling is discussed as the possible reason of the observed changes in the phonon spectrum of ligand-exchanged CdTe NCs. PACS: 63.20.-e, 78.30.-j, 78.67.-n, 78.67.Bf PMID:21711581

  17. Novel Electron-Phonon Relaxation Pathway in Graphite Revealed by Time-Resolved Raman Scattering and Angle-Resolved Photoemission Spectroscopy.

    PubMed

    Yang, Jhih-An; Parham, Stephen; Dessau, Daniel; Reznik, Dmitry

    2017-01-19

    Time dynamics of photoexcited electron-hole pairs is important for a number of technologies, in particular solar cells. We combined ultrafast pump-probe Raman scattering and photoemission to directly follow electron-hole excitations as well as the G-phonon in graphite after an excitation by an intense laser pulse. This phonon is known to couple relatively strongly to electrons. Cross-correlating effective electronic and phonon temperatures places new constraints on model-based fits. The accepted two-temperature model predicts that G-phonon population should start to increase as soon as excited electron-hole pairs are created and that the rate of increase should not depend strongly on the pump fluence. Instead we found that the increase of the G-phonon population occurs with a delay of ~65 fs. This time-delay is also evidenced by the absence of the so-called self-pumping for G phonons. It decreases with increased pump fluence. We show that these observations imply a new relaxation pathway: Instead of hot carriers transferring energy to G-phonons directly, the energy is first transferred to optical phonons near the zone boundary K-points, which then decay into G-phonons via phonon-phonon scattering. Our work demonstrates that phonon-phonon interactions must be included in any calculations of hot carrier relaxation in optical absorbers even when only short timescales are considered.

  18. Raman spectroscopy and electron-phonon coupling in Eu3+ doped Gd2Zr2O7 nanopowders

    NASA Astrophysics Data System (ADS)

    Krizan, G.; Gilic, M.; Ristic-Djurovic, J. L.; Trajic, J.; Romcevic, M.; Krizan, J.; Hadzic, B.; Vasic, B.; Romcevic, N.

    2017-11-01

    The Raman spectra of Eu3+ doped Gd2Zr2O7 nanopowders were measured. We registered three phonons at 177 cm-1, 268 cm-1, and 592 cm-1, as well as their overtones at 354 cm-1, 445 cm-1, 708 cm-1, 1062 cm-1, 1184 cm-1, ∼1530 cm-1, and ∼1720 cm-1. The phonon at 592 cm-1 is known to be characteristic for Gd2Zr2O7 fluorite-type structure; however, the other two have not been registered so far. We found that the position of the newly detected phonons agrees well with the observed electron-phonon interaction. On the other hand, the registered multiphonon processes were a consequence of miniaturization that further induced changes in electronic structure of Eu3+ doped Gd2Zr2O7 nanopowders.

  19. A transform from absorption to Raman excitation profile. A time-dependent approach

    NASA Astrophysics Data System (ADS)

    Lee, Soo-Y.; Yeo, Robert C. K.

    1994-04-01

    An alternative time-frame approach, which is canonically conjugate to the energy-frame approach, for implementing the transform relations for calculating Raman excitation profiles directly from the optical absorption spectrum is presented. Practical and efficient fast Fourier transformation in the time frame replaces the widely used Chan and Page algorithm for evaluating the Hilbert transform in the energy frame. The time-frame approach is applied to: (a) a two-mode model which illustrates the missing mode effect in both absorption and Raman excitation profiles, (b) carotene, in which both the absorption spectrum and the Raman excitation profile show vibrational structure and (c) hexamethylbenzene: TCNE electron donor—acceptor complex where the same spectra are structureless and the Raman excitation profile for the 168 cm -1 mode poses a problem for the energy-frame approach. A similar time-frame approach can be used for the inverse transform from the Raman excitation profile to the optical absorption spectrum.

  20. Isotope effect on superconductivity and Raman phonons of Pyrochlore Cd2Re2O7

    NASA Astrophysics Data System (ADS)

    Razavi, F. S.; Hajialamdari, M.; Reedyk, M.; Kremer, R. K.

    2018-06-01

    Cd2Re2O7 is the only α-Pyrochlore exhibiting superconductivity with a transition temperature (Tc) of ∼ 1 K. In this study, we present the effect of oxygen isotope (18O) as well as combined 18O and cadmium isotope (116Cd) substitution on the superconductivity and Raman scattering spectrum of Cd2Re2O7. The change of Tc and the energy gap Δ(T) are reported using various techniques including point contact spectroscopy. The shift in Raman phonon frequencies upon isotope substitution will be compared with measurement of the isotope effect on the superconducting transition temperature.

  1. Electric-dipole absorption resonating with longitudinal optical phonon-plasmon system and its effect on dispersion relations of interface phonon polariton modes in metal/semiconductor-stripe structures

    NASA Astrophysics Data System (ADS)

    Sakamoto, Hironori; Takeuchi, Eito; Yoshida, Kouki; Morita, Ken; Ma, Bei; Ishitani, Yoshihiro

    2018-01-01

    Interface phonon polaritons (IPhPs) in nano-structures excluding metal components are thoroughly investigated because they have lower loss in optical emission or absorption and higher quality factors than surface plasmon polaritons. In previous reports, it is found that strong infrared (IR) absorption is based on the interaction of p-polarized light and materials, and the resonance photon energy highly depends on the structure size and angle of incidence. We report the optical absorption by metal/semiconductor (bulk-GaAs and thin film-AlN)-stripe structures in THz to mid-IR region for the electric field of light perpendicular to the stripes, where both of s- and p-polarized light are absorbed. The absorption resonates with longitudinal optical (LO) phonon or LO phonon-plasmon coupling (LOPC) modes, and thus is independent of the angle of incidence or structure size. This absorption is attributed to the electric dipoles by the optically induced polarization charges at the metal/semiconductor, heterointerfaces, or interfaces of high electron density layers and depression ones. The electric permittivity is modified by the formation of these dipoles. It is found to be indispensable to utilize our form of altered permittivity to explain the experimental dispersion relations of metal/semiconductor-IPhP and SPhP in these samples. This analysis reveals that the IPhPs in the stripe structures of metal/AlN-film on a SiC substrate are highly confined in the AlN film, while the permittivity of the structures of metal/bulk-GaAs is partially affected by the electric-dipoles. The quality factors of the electric-dipole absorption are found to be 42-54 for undoped samples, and the value of 62 is obtained for Al/AlN-IPhP. It is thought that metal-contained structures are not obstacles to mode energy selectivity in phonon energy region of semiconductors.

  2. Dominant phonon wave vectors and strain-induced splitting of the 2D Raman mode of graphene

    NASA Astrophysics Data System (ADS)

    Narula, Rohit; Bonini, Nicola; Marzari, Nicola; Reich, Stephanie

    2012-03-01

    The dominant phonon wave vectors q* probed by the 2D Raman mode of pristine and uniaxially strained graphene are determined via a combination of ab initio calculations and a full two-dimensional integration of the transition matrix. We show that q* are highly anisotropic and rotate about K with the polarizer and analyzer condition relative to the lattice. The corresponding phonon-mediated electronic transitions show a finite component along K-Γ that sensitively determines q*. We invalidate the notion of “inner” and “outer” processes. The characteristic splitting of the 2D mode of graphene under uniaxial tensile strain and given polarizer and analyzer setting is correctly predicted only if the strain-induced distortion and red-shift of the in-plane transverse optical (iTO) phonon dispersion as well as the changes in the electronic band structure are taken into account.

  3. Comparison of three empirical force fields for phonon calculations in CdSe quantum dots

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Kelley, Anne Myers

    Three empirical interatomic force fields are parametrized using structural, elastic, and phonon dispersion data for bulk CdSe and their predictions are then compared for the structures and phonons of CdSe quantum dots having average diameters of ~2.8 and ~5.2 nm (~410 and ~2630 atoms, respectively). The three force fields include one that contains only two-body interactions (Lennard-Jones plus Coulomb), a Tersoff-type force field that contains both two-body and three-body interactions but no Coulombic terms, and a Stillinger-Weber type force field that contains Coulombic interactions plus two-body and three-body terms. While all three force fields predict nearly identical peak frequencies formore » the strongly Raman-active “longitudinal optical” phonon in the quantum dots, the predictions for the width of the Raman peak, the peak frequency and width of the infrared absorption peak, and the degree of disorder in the structure are very different. The three force fields also give very different predictions for the variation in phonon frequency with radial position (core versus surface). The Stillinger-Weber plus Coulomb type force field gives the best overall agreement with available experimental data.« less

  4. Phonons in self-assembled Ge/Si structures

    NASA Astrophysics Data System (ADS)

    Milekhin, A. G.; Nikiforov, A. I.; Pchelyakov, O. P.; Schulze, S.; Zahn, D. R. T.

    2002-03-01

    We present the results of an investigation dealing with fundamental vibrations in periodical Ge/Si structures with small-size Ge quantum dots (QDs) performed using macro- and micro-Raman spectroscopy under resonant and off-resonant conditions. Samples with different number of repetition of Ge and Si layers contain Ge QDs with an average dot base size of 15 nm and a QD height of 2 nm. Periodic oscillations observed in the low-frequency region of the Raman spectra are assigned to folded LA phonons in the Ge QD superlattices. The measured phonon frequencies are in a good agreement with those calculated using the Rytov model. These oscillations are superimposed with a broad continuous emission originating from the whole acoustic dispersion branch due to a breaking up of translational invariance. The Raman spectra of the structure with single Ge QD layer reveal a series of peaks corresponding to LA phonons localized in the Si layer. Using the measured phonon frequencies and corresponding wave vectors the dispersion of the LA phonons in the Si is obtained. The longitudinal-acoustic wave velocity determined from the dispersion is 8365 ms-1 and in excellent agreement with that derived from the Brillouin study. In the optical phonon range, the LO and TO phonons localized in Ge QDs are observed. The position of the LO Ge phonons shifts downwards with increasing excitation energy (from 2.5 to 2.7 eV) indicating the presence of a QD size distribution in Ge dot superlattices. Raman scattering from Ge QDs is size-selectively enhanced by the resonance of the exciting laser energy and the confined excitonic states.

  5. Raman scattering and anti-Stokes luminescence in poly-paraphenylene vinylene/carbon nanotubes composites

    NASA Astrophysics Data System (ADS)

    Baibarac, M.; Massuyeau, F.; Wery, J.; Baltog, I.; Lefrant, S.

    2012-04-01

    In this paper, we present Raman scattering and luminescence of poly-paraphenylene vinylene/single-walled carbon nanotubes composites, focused on data recorded in the anti-Stokes branch. We demonstrate that, when the excitation energy is in the long wavelength tail of the fundamental absorption edge, an anti-Stokes signal is generated, whose origin is a photon absorption accompanied by a phonon process from lower to upper vibronic states. The efficiency of this anti-Stokes photo-luminescence is increased when composites films are deposited onto an Au rough surface acting as a surface enhanced Raman scattering substrate. This mechanism is explained by a coherent anti-Stokes Raman scattering-like process, as observed in other nano-structured materials.

  6. Laboratory investigation on the role of tubular shaped micro resonators phononic crystal insertion on the absorption coefficient of profiled sound absorber

    NASA Astrophysics Data System (ADS)

    Yahya, I.; Kusuma, J. I.; Harjana; Kristiani, R.; Hanina, R.

    2016-02-01

    This paper emphasizes the influence of tubular shaped microresonators phononic crystal insertion on the sound absorption coefficient of profiled sound absorber. A simple cubic and two different bodies centered cubic phononic crystal lattice model were analyzed in a laboratory test procedure. The experiment was conducted by using transfer function based two microphone impedance tube method refer to ASTM E-1050-98. The results show that sound absorption coefficient increase significantly at the mid and high-frequency band (600 - 700 Hz) and (1 - 1.6 kHz) when tubular shaped microresonator phononic crystal inserted into the tested sound absorber element. The increment phenomena related to multi-resonance effect that occurs when sound waves propagate through the phononic crystal lattice model that produce multiple reflections and scattering in mid and high-frequency band which increases the sound absorption coefficient accordingly

  7. Symmetry-adapted tight-binding calculations of the totally symmetric A1 phonons of single-walled carbon nanotubes and their resonant Raman intensity

    NASA Astrophysics Data System (ADS)

    Popov, Valentin N.; Lambin, Philippe

    2007-03-01

    The atomistic calculations of the physical properties of perfect single-walled carbon nanotubes based on the use of the translational symmetry of the nanotubes face increasing computational difficulties for most of the presently synthesized nanotubes with up to a few thousand atoms in the unit cell. This difficulty can be circumvented by use of the helical symmetry of the nanotubes and a two-atom unit cell. We present the results of such symmetry-adapted tight-binding calculations of the totally symmetric A1 phonons (the RBM and the G-band modes) and their resonant Raman intensity for several hundred nanotubes. In particular, we show that (1) the frequencies and the resonant Raman intensity of the RBM and the G-band modes show diameter and chirality dependence and family patterns, (2) the strong electron- A1LO phonon interactions in metallic nanotubes lead to Kohn anomalies at the zone center, (3) the G-band consists of a subband due to A1LO phonons of semiconducting tubes centered at ∼1593 cm -1, a subband of A1TO phonons at ∼1570 cm -1, and a subband of A1LO phonons of metallic tubes at ∼1540 cm -1. The latter prediction confirms previous theoretical results but disagrees with the commonly adopted assignment of the G-band features.

  8. Interaction between confined phonons and photons in periodic silicon resonators

    NASA Astrophysics Data System (ADS)

    Iskandar, A.; Gwiazda, A.; Younes, J.; Kazan, M.; Bruyant, A.; Tabbal, M.; Lerondel, G.

    2018-03-01

    In this paper, we demonstrate that phonons and photons of different momenta can be confined and interact with each other within the same nanostructure. The interaction between confined phonons and confined photons in silicon resonator arrays is observed by means of Raman scattering. The Raman spectra from large arrays of dielectric silicon resonators exhibited Raman enhancement accompanied with a downshift and broadening. The analysis of the Raman intensity and line shape using finite-difference time-domain simulations and a spatial correlation model demonstrated an interaction between photons confined in the resonators and phonons confined in highly defective regions prompted by the structuring process. It was shown that the Raman enhancement is due to collective lattice resonance inducing field confinement in the resonators, while the spectra downshift and broadening are signatures of the relaxation of the phonon wave vector due to phonon confinement in defective regions located in the surface layer of the Si resonators. We found that as the resonators increase in height and their shape becomes cylindrical, the amplitude of their coherent oscillation increases and hence their ability to confine the incoming electric field increases.

  9. Micro-Raman study on the softening and stiffening of phonons in rutile titanium dioxide film: Competing effects of structural defects, crystallite size, and lattice strain

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Gautam, Subodh K.; Singh, Fouran, E-mail: fouran@gmail.com; Sulania, I.

    2014-04-14

    Softening and stiffening of phonons in rutile titanium dioxide films are investigated by in situ micro-Raman studies during energetic ion irradiation. The in situ study minimized other possible mechanisms of phonon dynamics. Initial softening and broadening of Raman shift are attributed to the phonon confinement by structural defects and loss of stoichiometry. The stiffening of A{sub 1g} mode is ascribed to large distortion of TiO{sub 6} octahedra under the influence of lattice strain in the (110) plane, which gives rise to lengthening of equatorial Ti-O bond and shortening of apical Ti-O bond. The shortening of apical Ti-O bond induces stiffeningmore » of A{sub 1g} mode in the framework of the bond-order-length-strength correlation mechanism.« less

  10. Observation of Raman active phonon with Fano lineshape in quasi-one-dimensional superconductor K2Cr3As3

    NASA Astrophysics Data System (ADS)

    Zhang, W.-L.; Li, H.; Dai, X.; L, H. W.; Shi, Y.-G.; Luo, J. L.; Hu, Jiangping; Richard, P.; Ding, H.; Extreme Condition Team; Condensed Matter Theory Team

    We study the polarization-resolved phononic Raman scattering in the recent discovered quasi-one-dimensional superconductor K2Cr3As3. With support from first-principles calculations, we characterize several phonons, among which one mode has a Fano lineshape, indicative of an electron-phonon coupling. While the common expectation of an electron-phonon coupling is the conventional superconducting mechanism, we show that this mode is related to the in-plane Cr vibration, which modulates the exchange coupling between the first nearest Cr neighbors. Our result support the presence of magnetic fluctuations coupled to the electrons via the lattice. We acknowledge MOST (2010CB923000, 2011CBA001000, 2011CBA00102, 2012CB821403 and 2013CB921703), NSFC (11004232, 11034011/A0402, 11234014, 11274362 and 11474330) of China and by the Strategic Priority Research Program (B) of the Chinese Academy of Sciences, Grant No. XDB07020100.

  11. Polarized micro Raman spectroscopy of bilayer graphene

    NASA Astrophysics Data System (ADS)

    Moon, Hyerim; Yoon, Duhee; Son, Young-Woo; Cheong, Hyeonsik

    2009-03-01

    The frequency of Raman 2D band of the graphite depends on the excitation laser energy. This phenomenon is explained with double resonance Raman process. In polarized micro-Raman spectroscopy of single layer graphene, Raman G band (˜1586 cm-1) is isotropic, and 2D band (˜2686 cm-1) strongly depends on relative polarizations of the incident and scattered photons. This strong polarization dependence originates from inhomogeneous optical absorption and emission mediated by resonant electron-phonon interaction. In bi-layer graphene, Raman 2D band can be decomposed into four Lorenztian peaks which can be interpreted in terms of the four transition paths in the double resonance Raman process. We investigated the polarization dependence of each Lorenztian peak in the Raman 2D band of bi-layer graphene for different excitation laser energies. Strong polarization dependence of the Raman 2D band, similar to the case of single layer graphene, is observed. The excitation energy dependence of the polarized Raman scattering is analyzed in terms of the band structure of bi-layer graphene.

  12. Acoustical phonon anomaly in the Raman spectra of intermediate valent TmSe 1-xTe x and Tm xSe

    NASA Astrophysics Data System (ADS)

    Treindl, A.; Wachter, P.

    1980-12-01

    In the Raman spectra of intermediate valent TmSe 1- xTe x the same anomaly within the acoustical phonon band at 60 cm -1 is found as in Tm xSe. The connection of this anomaly with the valence mixing is confirmed. In a one-dimensional model calculation it is shown that a renormalized LA dispersion curve can produce the observed anomalous peak in the phonon DOS. As an alternative interpretation the possibility of a low energy electronic excitation at 60 cm -1 is discussed.

  13. Unusual exciton–phonon interactions at van der Waals engineered interfaces

    DOE PAGES

    Chow, Colin M.; Yu, Hongyi; Jones, Aaron M.; ...

    2017-01-13

    Raman scattering is a ubiquitous phenomenon in light–matter interactions, which reveals a material’s electronic, structural, and thermal properties. Controlling this process would enable new ways of studying and manipulating fundamental material properties. Here, we report a novel Raman scattering process at the interface between different van der Waals (vdW) materials as well as between a monolayer semiconductor and 3D crystalline substrates. We find that interfacing a WSe 2 monolayer with materials such as SiO 2, sapphire, and hexagonal boron nitride (hBN) enables Raman transitions with phonons that are either traditionally inactive or weak. This Raman scattering can be amplified bymore » nearly 2 orders of magnitude when a foreign phonon mode is resonantly coupled to the A exciton in WSe 2 directly or via an A 1' optical phonon from WSe 2. We further showed that the interfacial Raman scattering is distinct between hBN-encapsulated and hBN-sandwiched WSe 2 sample geometries. Finally, this cross-platform electron–phonon coupling, as well as the sensitivity of 2D excitons to their phononic environments, will prove important in the understanding and engineering of optoelectronic devices based on vdW heterostructures.« less

  14. Unusual exciton–phonon interactions at van der Waals engineered interfaces

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Chow, Colin M.; Yu, Hongyi; Jones, Aaron M.

    Raman scattering is a ubiquitous phenomenon in light–matter interactions, which reveals a material’s electronic, structural, and thermal properties. Controlling this process would enable new ways of studying and manipulating fundamental material properties. Here, we report a novel Raman scattering process at the interface between different van der Waals (vdW) materials as well as between a monolayer semiconductor and 3D crystalline substrates. We find that interfacing a WSe 2 monolayer with materials such as SiO 2, sapphire, and hexagonal boron nitride (hBN) enables Raman transitions with phonons that are either traditionally inactive or weak. This Raman scattering can be amplified bymore » nearly 2 orders of magnitude when a foreign phonon mode is resonantly coupled to the A exciton in WSe 2 directly or via an A 1' optical phonon from WSe 2. We further showed that the interfacial Raman scattering is distinct between hBN-encapsulated and hBN-sandwiched WSe 2 sample geometries. Finally, this cross-platform electron–phonon coupling, as well as the sensitivity of 2D excitons to their phononic environments, will prove important in the understanding and engineering of optoelectronic devices based on vdW heterostructures.« less

  15. Temperature Dependence of Raman-Active In-Plane E2g Phonons in Layered Graphene and h-BN Flakes

    NASA Astrophysics Data System (ADS)

    Li, Xiaoli; Liu, Jian; Ding, Kai; Zhao, Xiaohui; Li, Shuai; Zhou, Wenguang; Liang, Baolai

    2018-01-01

    Thermal properties of sp2 systems such as graphene and hexagonal boron nitride (h-BN) have attracted significant attention because of both systems being excellent thermal conductors. This research reports micro-Raman measurements on the in-plane E2g optical phonon peaks ( 1580 cm-1 in graphene layers and 1362 cm-1 in h-BN layers) as a function of temperature from - 194 to 200 °C. The h-BN flakes show higher sensitivity to temperature-dependent frequency shifts and broadenings than graphene flakes. Moreover, the thermal effect in the c direction on phonon frequency in h-BN layers is more sensitive than that in graphene layers but on phonon broadening in h-BN layers is similar as that in graphene layers. These results are very useful to understand the thermal properties and related physical mechanisms in h-BN and graphene flakes for applications of thermal devices.

  16. High-pressure Raman scattering studies of magnon-phonon interactions and ferroelastic phase transitions

    NASA Astrophysics Data System (ADS)

    Rosenblum, Steven S.

    1997-11-01

    Using high-pressure Raman spectroscopy, this dissertation investigates several areas of condensed matter physics. With metal thiophosphates (MnPSsb3, NiPSsb3) as our reference systems, we investigate coupling between phonons and two-magnon continua. We find that MnPSsb3's two-magnon excitation can be tuned into resonance with the 155 cmsp{-1} phonon at a temperature near 60 K. In NiPSsb3, we find that the two-magnon excitation has a linewidth broader than that predicted by standard two-magnon theory, reminiscent of the similar linewidth observed in the undoped cuprate superconductors. This observation calls into question the role quantum fluctuations associated with spin 1/2 play in the cuprates' two-magnon spectrum. Additionally, high-pressure Raman measurements of NiPSsb3 yielded evidence of resonant enhancement of the two-magnon excitation-previously only observed in the cuprate superconductors. Additionally, we investigated the rutile-to-CaClsb2 ferroelastic phase transition occurring in RuOsb2. We observed the splitting of the (rutile) Esb{g} mode, and used this to find a transition pressure of 11.8 GPa. Based on the lower transition pressure found in previous work and on other results in the literature, we speculate that stoichiometry plays a critical role in determining the stability of the rutile or CaClsb2 phase of the metal dioxides. These experiments were performed with a variety of single-, double-, and triple-grating spectrometers (Renishaw, SPEX, and Dilor, respectively). The excitation sources used were primarily ion lasers (either argon or helium-neon). Pressures up to 35 GPa were achieved via a Mao-Bell style Diamond Anvil Cell.

  17. Phase analysis of coherent radial-breathing-mode phonons in carbon nanotubes: Implications for generation and detection processes

    NASA Astrophysics Data System (ADS)

    Shimura, Akihiko; Yanagi, Kazuhiro; Yoshizawa, Masayuki

    2018-01-01

    In time-resolved pump-probe spectroscopy of carbon nanotubes, the fundamental understanding of the optical generation and detection processes of radial-breathing-mode (RBM) phonons has been inconsistent among the previous reports. In this study, the tunable-pumping/broadband-probing scheme was used to fully reveal the amplitude and phase of the phonon-modulated signals. We observed that signals detected off resonantly to excitonic transitions are delayed by π /2 radians with respect to resonantly detected signals, which demonstrates that RBM phonons are detected through dynamically modulating the linear response, not through adiabatically modulating the light absorption. Furthermore, we found that the initial phases are independent of the pump detuning across the first (E11) and the second (E22) excitonic resonances, evidencing that the RBM phonons are generated by the displacive excitation rather than stimulated Raman process.

  18. Temperature dependence Infrared and Raman studies of III-V/II-VI core-shell nanostructures

    NASA Astrophysics Data System (ADS)

    Manciu, Felicia S.; McCombe, Bruce D.; Lucey, Derrick

    2005-03-01

    The temperature dependence (8 K < T < 300 K) of optical phonon modes confined in InP/II-VI core-shell nanostructures have been investigated by far-infrared (FIR) and Raman scattering spectroscopies. The core-shell nanostructures were fabricated by colloidal chemistry and characterized by transmission electron microscopy and X-ray diffraction prior to being embedded in a polycrystalline CsI matrix for the present studies. The FIR measurements of InP/ZnSe sample exhibits three absorption features, one clearly due to the Froelich mode of the InP cores, and the others related to modes associated with the shell layer and its coupling to the matrix. Strong mixing of the characteristic vibrations of each constituent material was observed for InP/ZnS sample. Raman scattering (457.9 nm excitation) features were determined without polarization selection in the backscattering geometry. Interesting T-dependent resonant Raman effect of the surface optical phonon modes has been discovered in InP/ZnSe sample. Reasonable agreement is obtained between the Raman and FIR results, as well as with theoretical calculations.

  19. Anharmonic phonon decay in cubic GaN

    NASA Astrophysics Data System (ADS)

    Cuscó, R.; Domènech-Amador, N.; Novikov, S.; Foxon, C. T.; Artús, L.

    2015-08-01

    We present a Raman-scattering study of optical phonons in zinc-blende (cubic) GaN for temperatures ranging from 80 to 750 K. The experiments were performed on high-quality, cubic GaN films grown by molecular-beam epitaxy on GaAs (001) substrates. The observed temperature dependence of the optical phonon frequencies and linewidths is analyzed in the framework of anharmonic decay theory, and possible decay channels are discussed in the light of density-functional-theory calculations. The longitudinal-optical (LO) mode relaxation is found to occur via asymmetric decay into acoustic phonons, with an appreciable contribution of higher-order processes. The transverse-optical mode linewidth shows a weak temperature dependence and its frequency downshift is primarily determined by the lattice thermal expansion. The LO phonon lifetime is derived from the observed Raman linewidth and an excellent agreement with previous theoretical predictions is found.

  20. Blue- and red-shifts of V2O5 phonons in NH3 environment by in situ Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Adeleke Akande, Amos; Machatine, Augusto Goncalo Jose; Masina, Bathusile; Chimowa, George; Matsoso, Boitumelo; Roro, Kittessa; Duvenhage, Mart-Mari; Swart, Hendrik; Bandyopadhyay, Jayita; Sinha Ray, Suprakas; Wakufwa Mwakikunga, Bonex

    2018-01-01

    A layer of ~30 nm V2O5/100 nm-SiO2 on Si was employed in the in situ Raman spectroscopy in the presence of NH3 effluent from a thermal decomposition of ammonium acetate salt with the salt heated at 100 °C. When the layer is placed at 25 °C, we observe a reversible red-shift of 194 cm-1 V2O5 phonon by 2 cm-1 upon NH3 gas injection to saturation, as well as a reversible blue-shift of the 996 cm-1 by 4 cm-1 upon NH3 injection. However when the sensing layer is placed at 100 °C, the 194 cm-1 remains un-shifted while the 996 cm-1 phonon is red-shifted. There is a decrease/increase in intensity of the 145 cm-1 phonon at 25 °C/100 °C when NH3 interacts with V2O5 surface. Using the traditional and quantitative gas sensor tester system, we find that the V2O5 sensor at 25 °C responds faster than at 100 °C up to 20 ppm of NH3 beyond which it responds faster at 100 °C than at 25 °C. Overall rankings of the NH3 gas sensing features between the two techniques showed that the in situ Raman spectroscopy is faster in response compared with the traditional chemi-resistive tester. Hooke’s law, phonon confinement in ~51 nm globular particles with ~20 nm pore size and physisorption/chemisorption principles have been employed in the explanation of the data presented.

  1. Phonon anomalies in FeS

    DOE PAGES

    Baum, A.; Milosavljevic, A.; Lazarevic, N.; ...

    2018-02-12

    Here, we present results from light scattering experiments on tetragonal FeS with the focus placed on lattice dynamics. We identify the Raman active A 1g and B 1g phonon modes, a second order scattering process involving two acoustic phonons, and contributions from potentially defect-induced scattering. The temperature dependence between 300 and 20 K of all observed phonon energies is governed by the lattice contraction. Below 20 K the phonon energies increase by 0.5–1 cm -1 , thus indicating putative short range magnetic order. Additionally, along with the experiments we performed lattice-dynamical simulations and a symmetry analysis for the phonons andmore » potential overtones and find good agreement with the experiments. In particular, we argue that the two-phonon excitation observed in a gap between the optical branches becomes observable due to significant electron-phonon interaction.« less

  2. Phonon anomalies in FeS

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Baum, A.; Milosavljevic, A.; Lazarevic, N.

    Here, we present results from light scattering experiments on tetragonal FeS with the focus placed on lattice dynamics. We identify the Raman active A 1g and B 1g phonon modes, a second order scattering process involving two acoustic phonons, and contributions from potentially defect-induced scattering. The temperature dependence between 300 and 20 K of all observed phonon energies is governed by the lattice contraction. Below 20 K the phonon energies increase by 0.5–1 cm -1 , thus indicating putative short range magnetic order. Additionally, along with the experiments we performed lattice-dynamical simulations and a symmetry analysis for the phonons andmore » potential overtones and find good agreement with the experiments. In particular, we argue that the two-phonon excitation observed in a gap between the optical branches becomes observable due to significant electron-phonon interaction.« less

  3. High-performance dispersive Raman and absorption spectroscopy as tools for drug identification

    NASA Astrophysics Data System (ADS)

    Pawluczyk, Olga; Andrey, Sam; Nogas, Paul; Roy, Andrew; Pawluczyk, Romuald

    2009-02-01

    Due to increasing availability of pharmaceuticals from many sources, a need is growing to quickly and efficiently analyze substances in terms of the consistency and accuracy of their chemical composition. Differences in chemical composition occur at very low concentrations, so that highly sensitive analytical methods become crucial. Recent progress in dispersive spectroscopy with the use of 2-dimensional detector arrays, permits for signal integration along a long (up to 12 mm long) entrance slit of a spectrometer, thereby increasing signal to noise ratio and improving the ability to detect small concentration changes. This is achieved with a non-scanning, non-destructive system. Two different methods using P&P Optica high performance spectrometers were used. High performance optical dispersion Raman and high performance optical absorption spectroscopy were employed to differentiate various acetaminophen-containing drugs, such as Tylenol and other generic brands, which differ in their ingredients. A 785 nm excitation wavelength was used in Raman measurements and strong Raman signals were observed in the spectral range 300-1800 cm-1. Measurements with the absorption spectrometer were performed in the wavelength range 620-1020 nm. Both Raman and absorption techniques used transmission light spectrometers with volume phase holographic gratings and provided sufficient spectral differences, often structural, allowing for drug differentiation.

  4. Si/Ge elatform for lasers, amplifiers, and nonlinear optical devices based on the Raman Effect

    NASA Astrophysics Data System (ADS)

    Claps, Ricardo; Dimitropoulos, Dimitrios; Raghunathan, Varun; Fathpour, Sasan; Jalali, Bahram; Jusserand, Bernard

    2007-02-01

    The use of a silicon-germanium platform for the development of optically active devices will be discussed in this paper, from the perspective of Raman and Brillouin scattering phenomena. Silicon-Germanium is becoming a prevalent technology for the development of high speed CMOS transistors, with advances in several key parameters as high carrier mobility, low cost, and reduced manufacturing logistics. Traditionally, Si-Ge structures have been used in the optoelectronics arena as photodetectors, due to the enhanced absorption of Ge in the telecommunications band. Recent developments in Raman-based nonlinearities for devices based on a silicon-on-insulator platform have shed light on the possibility of using these effects in Si-Ge architectures. Lasing and amplification have been demonstrated using a SiGe alloy structure, and Brillouin/Raman activity from acoustic phonon modes in SiGe superlattices has been predicted. Moreover, new Raman-active branches and inhomogeneously broadened spectra result from optical phonon modes, offering new perspectives for optical device applications. The possibilities for an electrically-pumped Raman laser will be outlined, and the potential for design and development of silicon-based, Tera-Hertz wave emitters and/or receivers.

  5. Absorption and resonance Raman characteristics of β-carotene in water-ethanol mixtures, emulsion and hydrogel

    NASA Astrophysics Data System (ADS)

    Meinhardt-Wollweber, Merve; Suhr, Christian; Kniggendorf, Ann-Kathrin; Roth, Bernhard

    2018-05-01

    Absorption or resonance Raman scattering are often used to identify and even quantify carotenoids in situ. We studied the absorption spectra, the Raman spectra and their resonance behavior of β-carotene in different molecular environments set up as mixtures from lipid (emulsion) and non-polar (ethanol) solvents and a polar component (water) with regard to their application as references for in situ measurement. We show how both absorption profiles and resonance spectra of β-carotene strongly depend on the molecular environment. Most notably, our data suggests that the characteristic bathochromic absorption peak of J-aggregates does not contribute to carotenoid resonance conditions, and show how the Raman shift of the C=C stretching mode is dependent on both, the molecular environment and the excitation wavelength. Overall, the spectroscopic data collected here is highly relevant for the interpretation of in situ spectroscopic data in terms of carotenoid identification and quantification by resonance Raman spectroscopy as well as the preparation of reference samples. In particular, our data promotes careful consideration of appropriate molecular environment for reference samples.

  6. Negative refraction with low absorption using Raman transitions with magnetoelectric coupling

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Sikes, D. E.; Yavuz, D. D.

    2010-07-15

    We suggest a scheme for obtaining negative refraction that does not require the simultaneous presence of an electric-dipole and a magnetic-dipole transition near the same transition frequency. The key idea of the scheme is to obtain a strong electric response by using far-off-resonant Raman transitions. We propose to use a pair of electric-dipole Raman transitions and utilize magneto-electric cross coupling to achieve a negative index of refraction without requiring negative permeability. The interference of the two Raman transitions allows tunable negative refraction with low absorption.

  7. Hot-phonon generation in THz quantum cascade lasers

    NASA Astrophysics Data System (ADS)

    Spagnolo, V.; Vitiello, M. S.; Scamarcio, G.; Williams, B. S.; Kumar, S.; Hu, Q.; Reno, J. L.

    2007-12-01

    Observation of non-equilibrium optical phonons population associated with electron transport in THz quantum cascade lasers is reported. The phonon occupation number was measured by using a combination of micro-probe photoluminescence and Stokes/Anti-Stokes Raman spectroscopy. Energy balance analysis allows us to estimate the phonon relaxation rate, that superlinearly increases with the electrical power in the range 1.5 W - 1.95 W, above laser threshold. This observation suggests the occurrence of stimulated emission of optical phonons.

  8. Angular dispersion of oblique phonon modes in BiFeO3 from micro-Raman scattering

    NASA Astrophysics Data System (ADS)

    Hlinka, J.; Pokorny, J.; Karimi, S.; Reaney, I. M.

    2011-01-01

    The angular dispersion of oblique phonon modes in a multiferroic BiFeO3 has been obtained from a micro-Raman spectroscopic investigation of a coarse grain ceramic sample. Continuity of the measured angular dispersion curves allows conclusive identification of all pure zone-center polar modes. The method employed here to reconstruct the anisotropic crystal property from a large set of independent local measurements on a macroscopically isotropic ceramic sample profits from the considerable dispersion of the oblique modes in ferroelectric perovskites and it can be in principle conveniently applied to any other optically uniaxial ferroelectric material.

  9. Raman scattering in crystals

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Edwards, D.F.

    1988-09-30

    A tutorial presentation is given of Raman scattering in crystals. The physical concepts are emphasized rather than the detailed mathematical formalism. Starting with an introduction to the concepts of phonons and conservation laws, the effects of photon-phonon interactions are presented. This interaction concept is shown for a simple cubic crystal and is extended to a uniaxial crystal. The correlation table method is used for determining the number and symmetry of the Raman active modes. Finally, examples are given to illustrate the relative ease of using this group theoretical method and the predictions are compared with measured Raman spectra. 37 refs.,more » 17 figs., 6 tabs.« less

  10. Phonon-assisted nonlinear optical processes in ultrashort-pulse pumped optical parametric amplifiers

    NASA Astrophysics Data System (ADS)

    Isaienko, Oleksandr; Robel, István

    2016-03-01

    Optically active phonon modes in ferroelectrics such as potassium titanyl phosphate (KTP) and potassium titanyl arsenate (KTA) in the ~7-20 THz range play an important role in applications of these materials in Raman lasing and terahertz wave generation. Previous studies with picosecond pulse excitation demonstrated that the interaction of pump pulses with phonons can lead to efficient stimulated Raman scattering (SRS) accompanying optical parametric oscillation or amplification processes (OPO/OPA), and to efficient polariton-phonon scattering. In this work, we investigate the behavior of infrared OPAs employing KTP or KTA crystals when pumped with ~800-nm ultrashort pulses of duration comparable to the oscillation period of the optical phonons. We demonstrate that under conditions of coherent impulsive Raman excitation of the phonons, when the effective χ(2) nonlinearity cannot be considered instantaneous, the parametrically amplified waves (most notably, signal) undergo significant spectral modulations leading to an overall redshift of the OPA output. The pump intensity dependence of the redshifted OPA output, the temporal evolution of the parametric gain, as well as the pump spectral modulations suggest the presence of coupling between the nonlinear optical polarizations PNL of the impulsively excited phonons and those of parametrically amplified waves.

  11. Observation of chiral phonons

    NASA Astrophysics Data System (ADS)

    Zhu, Hanyu; Yi, Jun; Li, Ming-Yang; Xiao, Jun; Zhang, Lifa; Yang, Chih-Wen; Kaindl, Robert A.; Li, Lain-Jong; Wang, Yuan; Zhang, Xiang

    2018-02-01

    Chirality reveals symmetry breaking of the fundamental interaction of elementary particles. In condensed matter, for example, the chirality of electrons governs many unconventional transport phenomena such as the quantum Hall effect. Here we show that phonons can exhibit intrinsic chirality in monolayer tungsten diselenide. The broken inversion symmetry of the lattice lifts the degeneracy of clockwise and counterclockwise phonon modes at the corners of the Brillouin zone. We identified the phonons by the intervalley transfer of holes through hole-phonon interactions during the indirect infrared absorption, and we confirmed their chirality by the infrared circular dichroism arising from pseudoangular momentum conservation. The chiral phonons are important for electron-phonon coupling in solids, phonon-driven topological states, and energy-efficient information processing.

  12. Temperature Dependence of Brillouin Light Scattering Spectra of Acoustic Phonons in Silicon

    NASA Astrophysics Data System (ADS)

    Somerville, Kevin; Klimovich, Nikita; An, Kyongmo; Sullivan, Sean; Weathers, Annie; Shi, Li; Li, Xiaoqin

    2015-03-01

    Thermal management represents an outstanding challenge in many areas of technology. Electrons, optical phonons, and acoustic phonons are often driven out of local equilibrium in electronic devices or during laser-material interaction processes. Interest in non-equilibrium transport processes has motivated the development of Raman spectroscopy as a local temperature sensor of optical phonons and intermediate frequency acoustic phonons, whereas Brillouin light scattering (BLS) has recently been explored as a temperature sensor of low-frequency acoustic phonons. Here, we report temperature dependent BLS spectra of silicon, with Raman spectra taken simultaneously for comparison. The origins of the observed temperature dependence of the BLS peak position, linewidth, and intensity are examined in order to evaluate their potential use as temperature sensors for acoustic phonons. We determine that the integrated BLS intensity can be used measure the temperature of specific acoustic phonon modes. This work is supported by National Science Foundation (NSF) Thermal Transport Processes Program under Grant CBET-1336968.

  13. Wafer-scale metasurface for total power absorption, local field enhancement and single molecule Raman spectroscopy

    PubMed Central

    Wang, Dongxing; Zhu, Wenqi; Best, Michael D.; Camden, Jon P.; Crozier, Kenneth B.

    2013-01-01

    The ability to detect molecules at low concentrations is highly desired for applications that range from basic science to healthcare. Considerable interest also exists for ultrathin materials with high optical absorption, e.g. for microbolometers and thermal emitters. Metal nanostructures present opportunities to achieve both purposes. Metal nanoparticles can generate gigantic field enhancements, sufficient for the Raman spectroscopy of single molecules. Thin layers containing metal nanostructures (“metasurfaces”) can achieve near-total power absorption at visible and near-infrared wavelengths. Thus far, however, both aims (i.e. single molecule Raman and total power absorption) have only been achieved using metal nanostructures produced by techniques (high resolution lithography or colloidal synthesis) that are complex and/or difficult to implement over large areas. Here, we demonstrate a metasurface that achieves the near-perfect absorption of visible-wavelength light and enables the Raman spectroscopy of single molecules. Our metasurface is fabricated using thin film depositions, and is of unprecedented (wafer-scale) extent. PMID:24091825

  14. Raman gain and nonlinear optical absorption measurements in a low-loss silicon waveguide

    NASA Astrophysics Data System (ADS)

    Rong, Haisheng; Liu, Ansheng; Nicolaescu, Remus; Paniccia, Mario; Cohen, Oded; Hak, Dani

    2004-09-01

    We fabricated a low-loss (˜0.22dB/cm) rib waveguide (WG) in silicon-on-insulator with a small effective core area of ˜1.57μm2 and measured the stimulated Raman scattering gain in the WG. We obtained 2.3dB Raman gain in a 4.8-cm-long S-shaped WG using a 1455nm pump laser with a cw power of 0.9W measured before the WG. In addition, we observed nonlinear dependence of Raman gain and optical propagation loss as a function of the pump power. Our study shows that this mainly is due to two-photon absorption (TPA) induced free carrier absorption in the silicon WG. We experimentally determined the TPA induced free carrier lifetime of 25ns, which agrees well with our modeling.

  15. Phonon-assisted nonlinear optical processes in ultrashort-pulse pumped optical parametric amplifiers

    DOE PAGES

    Isaienko, Oleksandr; Robel, Istvan

    2016-03-15

    Optically active phonon modes in ferroelectrics such as potassium titanyl phosphate (KTP) and potassium titanyl arsenate (KTA) in the ~7–20 THz range play an important role in applications of these materials in Raman lasing and terahertz wave generation. Previous studies with picosecond pulse excitation demonstrated that the interaction of pump pulses with phonons can lead to efficient stimulated Raman scattering (SRS) accompanying optical parametric oscillation or amplification processes (OPO/OPA), and to efficient polariton-phonon scattering. In this work, we investigate the behavior of infrared OPAs employing KTP or KTA crystals when pumped with ~800-nm ultrashort pulses of duration comparable to themore » oscillation period of the optical phonons. We demonstrate that under conditions of coherent impulsive Raman excitation of the phonons, when the effective χ (2) nonlinearity cannot be considered instantaneous, the parametrically amplified waves (most notably, signal) undergo significant spectral modulations leading to an overall redshift of the OPA output. Furthermore, the pump intensity dependence of the redshifted OPA output, the temporal evolution of the parametric gain, as well as the pump spectral modulations suggest the presence of coupling between the nonlinear optical polarizations P NL of the impulsively excited phonons and those of parametrically amplified waves.« less

  16. Polarized Raman scattering of epitaxial vanadium dioxide films with low-temperature monoclinic phase

    NASA Astrophysics Data System (ADS)

    Shibuya, Keisuke; Sawa, Akihito

    2017-07-01

    A polarized Raman scattering study was carried out on epitaxial VO2 thin films on MgF2(001) and (110) substrates to investigate the Raman symmetry and tensor elements of the phonon modes of the films in a low-temperature monoclinic phase. From the polarization angular dependence of the Raman intensity, we assigned the phonon modes at 137, 194, 310, 340, 499, 612, and 663 cm-1 to Ag symmetry and the phonon modes at 143, 262, 442, 480, 582, and 820 cm-1 to Bg symmetry. The angular-dependence measurements also revealed that two phonon modes with Ag and Bg symmetries are present at about 224 and 393 cm-1, although only a single peak was observed in the Raman spectra at around these wavenumbers. On the basis of the experimental results, we evaluated the Raman tensors of the identified phonon modes. From the Raman tensors, we found that the atomic displacements of the 194 and 340 cm-1 phonon modes are approximately perpendicular and parallel, respectively, to the V-V dimer direction. This is consistent with a previous theoretical prediction, i.e., these modes are attributable to the tilting motion and the stretching vibration of the V-V dimers, respectively.

  17. Vacancy and curvature effects on the phonon properties of single wall carbon nanotube

    NASA Astrophysics Data System (ADS)

    Hossain Howlader, Ashraful; Sherajul Islam, Md.; Tanaka, Satoru; Makino, Takayuki; Hashimoto, Akihiro

    2018-02-01

    Single wall carbon nanotube (SWCNT) is considered as an ideal candidate for next-generation nanoelectronics owing to its unusual properties. Here we have performed an in-depth theoretical analysis of the effect of vacancy defects and curvature on the phonon properties of (10,0) and (10,10) SWCNTs using the forced vibrational method. We report that Raman active E2g mode softens towards the low-frequency region with increasing vacancies and curvature in both types of CNTs. Vacancy induces some new peaks at low-frequency region of the phonon density of states. Phonon localization properties are also manifested. Our calculated mode pattern and localization length show that optical phonon at Raman D-band frequency is strongly localized in vacancy defected and large curved CNTs. Our findings will be helpful in explaining the thermal conductivity, specific heat capacity, and Raman spectra in vacancy type disordered CNTs, as well as electron transport properties of CNT-based nanoelectronic devices.

  18. Renormalisation of Nonequilibrium Phonons Under Strong Perturbative Influences.

    NASA Astrophysics Data System (ADS)

    Mehta, Sushrut Madhukar

    Effects of strong perturbative influences, namely the presence of a narrow distribution of acoustic phonons, and the presence of an electron plasma, on the dynamics of nonequilibrium, near zone center, longitudinal optical phonons in GaP have been investigated in two separate experiments. The study of the effects of the interaction between the LO phonons and a heavily populated, narrow distribution of acoustic phonons lead to the observation of a new optically driven nonequilibrium phonon state. Time Resolved Coherent Antistokes Raman Scattering (TR-CARS), with picosecond resolution, was used to investigate the new mode. In order to achieve high occupation numbers in the acoustic branch, the picosecond laser pulses used were amplified up to 1.0 GW/cm^2 peak power per laser beam. An important characteristic property of the new state which differentiates it from the well known LO phonon state is the fact that rather than having the single decay rate observed under thermal equilibrium, the new state has two decay rates. Moreover, these two decay rates depend strongly on the distribution of the acoustic phonon occupation number. The coupling of the LO phonons with an electron plasma, on the other hand, was investigated by measurements of the shape of the Raman scattered line associated with the phonon-plasmon coupled mode. The plasma was generated by thermal excitation of carriers in doped samples. It was possible to study a large variety of plasma excitations by controlling the concentration of the dopant and the ambient temperature. A complete, self consistant model based on standard dielectric response theory is presented, and applied to the measurements of the phonon-plasmon coupled mode. It is possible to recover, via this model, the effective coupled mode damping rate, the plasma damping rate, and the plasma frequency as functions of ambient temperature, or the carrier concentration.

  19. Observation of chiral phonons.

    PubMed

    Zhu, Hanyu; Yi, Jun; Li, Ming-Yang; Xiao, Jun; Zhang, Lifa; Yang, Chih-Wen; Kaindl, Robert A; Li, Lain-Jong; Wang, Yuan; Zhang, Xiang

    2018-02-02

    Chirality reveals symmetry breaking of the fundamental interaction of elementary particles. In condensed matter, for example, the chirality of electrons governs many unconventional transport phenomena such as the quantum Hall effect. Here we show that phonons can exhibit intrinsic chirality in monolayer tungsten diselenide. The broken inversion symmetry of the lattice lifts the degeneracy of clockwise and counterclockwise phonon modes at the corners of the Brillouin zone. We identified the phonons by the intervalley transfer of holes through hole-phonon interactions during the indirect infrared absorption, and we confirmed their chirality by the infrared circular dichroism arising from pseudoangular momentum conservation. The chiral phonons are important for electron-phonon coupling in solids, phonon-driven topological states, and energy-efficient information processing. Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.

  20. Raman tensor elements of β-Ga2O3.

    PubMed

    Kranert, Christian; Sturm, Chris; Schmidt-Grund, Rüdiger; Grundmann, Marius

    2016-11-03

    The Raman spectrum and particularly the Raman scattering intensities of monoclinic β-Ga 2 O 3 are investigated by experiment and theory. The low symmetry of β-Ga 2 O 3 results in a complex dependence of the Raman intensity for the individual phonon modes on the scattering geometry which is additionally affected by birefringence. We measured the Raman spectra in dependence on the polarization direction for backscattering on three crystallographic planes of β-Ga 2 O 3 and modelled these dependencies using a modified Raman tensor formalism which takes birefringence into account. The spectral position of all 15 Raman active phonon modes and the Raman tensor elements of 13 modes were determined and are compared to results from ab-initio calculations.

  1. Raman tensor elements of β-Ga2O3

    PubMed Central

    Kranert, Christian; Sturm, Chris; Schmidt-Grund, Rüdiger; Grundmann, Marius

    2016-01-01

    The Raman spectrum and particularly the Raman scattering intensities of monoclinic β-Ga2O3 are investigated by experiment and theory. The low symmetry of β-Ga2O3 results in a complex dependence of the Raman intensity for the individual phonon modes on the scattering geometry which is additionally affected by birefringence. We measured the Raman spectra in dependence on the polarization direction for backscattering on three crystallographic planes of β-Ga2O3 and modelled these dependencies using a modified Raman tensor formalism which takes birefringence into account. The spectral position of all 15 Raman active phonon modes and the Raman tensor elements of 13 modes were determined and are compared to results from ab-initio calculations. PMID:27808113

  2. Phonon spectra, electronic, and thermodynamic properties of WS2 nanotubes.

    PubMed

    Evarestov, Robert A; Bandura, Andrei V; Porsev, Vitaly V; Kovalenko, Alexey V

    2017-11-15

    Hybrid density functional theory calculations are performed for the first time on the phonon dispersion and thermodynamic properties of WS 2 -based single-wall nanotubes. Symmetry analysis is presented for phonon modes in nanotubes using the standard (crystallographic) factorization for line groups. Symmetry and the number of infra-red and Raman active modes in achiral WS 2 nanotubes are given for armchair and zigzag chiralities. It is demonstrated that a number of infrared and Raman active modes is independent on the nanotube diameter. The zone-folding approach is applied to find out an impact of curvature on electron and phonon band structure of nanotubes rolled up from the monolayer. Phonon frequencies obtained both for layers and nanotubes are used to compute the thermal contributions to their thermodynamic functions. The temperature dependences of energy, entropy, and heat capacity of nanotubes are estimated with respect to those of the monolayer. The role of phonons in the stability estimation of nanotubes is discussed based on Helmholtz free energy calculations. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

  3. Probing the experimental phonon dispersion of graphene using 12C and 13C isotopes

    NASA Astrophysics Data System (ADS)

    Bernard, S.; Whiteway, E.; Yu, V.; Austing, D. G.; Hilke, M.

    2012-08-01

    Using very uniform large-scale chemical vapor deposition grown graphene transferred onto silicon, we were able to identify 15 distinct Raman lines associated with graphene monolayers. This was possible thanks to a combination of different carbon isotopes and different Raman laser energies and extensive averaging without increasing the laser power. This allowed us to obtain a detailed experimental phonon dispersion relation for many points in the Brillouin zone. We further identified a D+D' peak corresponding to a double-phonon process involving both an inter- and intravalley phonon.

  4. Two-Color Pump-Probe Measurement of Photonic Quantum Correlations Mediated by a Single Phonon

    NASA Astrophysics Data System (ADS)

    Anderson, Mitchell D.; Tarrago Velez, Santiago; Seibold, Kilian; Flayac, Hugo; Savona, Vincenzo; Sangouard, Nicolas; Galland, Christophe

    2018-06-01

    We propose and demonstrate a versatile technique to measure the lifetime of the one-phonon Fock state using two-color pump-probe Raman scattering and spectrally resolved, time-correlated photon counting. Following pulsed laser excitation, the n =1 phonon Fock state is probabilistically prepared by projective measurement of a single Stokes photon. The detection of an anti-Stokes photon generated by a second, time-delayed laser pulse probes the phonon population with subpicosecond time resolution. We observe strongly nonclassical Stokes-anti-Stokes correlations, whose decay maps the single phonon dynamics. Our scheme can be applied to any Raman-active vibrational mode. It can be modified to measure the lifetime of n ≥1 Fock states or the phonon quantum coherences through the preparation and detection of two-mode entangled vibrational states.

  5. Two-Color Pump-Probe Measurement of Photonic Quantum Correlations Mediated by a Single Phonon.

    PubMed

    Anderson, Mitchell D; Tarrago Velez, Santiago; Seibold, Kilian; Flayac, Hugo; Savona, Vincenzo; Sangouard, Nicolas; Galland, Christophe

    2018-06-08

    We propose and demonstrate a versatile technique to measure the lifetime of the one-phonon Fock state using two-color pump-probe Raman scattering and spectrally resolved, time-correlated photon counting. Following pulsed laser excitation, the n=1 phonon Fock state is probabilistically prepared by projective measurement of a single Stokes photon. The detection of an anti-Stokes photon generated by a second, time-delayed laser pulse probes the phonon population with subpicosecond time resolution. We observe strongly nonclassical Stokes-anti-Stokes correlations, whose decay maps the single phonon dynamics. Our scheme can be applied to any Raman-active vibrational mode. It can be modified to measure the lifetime of n≥1 Fock states or the phonon quantum coherences through the preparation and detection of two-mode entangled vibrational states.

  6. The graphene phonon dispersion with C12 and C13 isotopes

    NASA Astrophysics Data System (ADS)

    Whiteway, Eric; Bernard, Simon; Yu, Victor; Austing, D. Guy; Hilke, Michael

    2013-12-01

    Using very uniform large scale chemical vapor deposition grown graphene transferred onto silicon, we were able to identify 15 distinct Raman lines associated with graphene monolayers. This was possible thanks to a combination of different carbon isotopes and different Raman laser energies and extensive averaging without increasing the laser power. This allowed us to obtain a detailed experimental phonon dispersion relation for many points in the Brillouin zone. We further identified a D+D' peak corresponding to a double phonon process involving both an inter- and intra-valley phonon. In order to both eliminate substrate effects and to probe large areas, we undertook to study Raman scattering for large scale chemical vapor deposition (CVD) grown graphene using two different isotopes (C12 and C13) so that we can effectively exclude and subtract the substrate contributions, since a heavier mass downshifts only the vibrational properties, while keeping all other properties the same.

  7. Theoretical studies on absorption, emission, and resonance Raman spectra of Coumarin 343 isomers

    NASA Astrophysics Data System (ADS)

    Wu, Wenpeng; Cao, Zexing; Zhao, Yi

    2012-03-01

    The vibrationally resolved spectral method and quantum chemical calculations are employed to reveal the structural and spectral properties of Coumarin 343 (C343), an ideal candidate for organic dye photosensitizers, in vacuum and solution. The results manifest that the ground-state energies are dominantly determined by different placements of hydrogen atom in carboxylic group of C343 conformations. Compared to those in vacuum, the electronic absorption spectra in methanol solvent show a hyperchromic property together with the redshift and blueshift for the neutral C343 isomers and their deprotonated anions, respectively. From the absorption, emission, and resonance Raman spectra, it is found that the maximal absorption and emission come from low-frequency modes whereas the high-frequency modes have high Raman activities. The detailed spectra are further analyzed for the identification of the conformers and understanding the potential charge transfer mechanism in their photovoltaic applications.

  8. Sensitive Phonon-Based Probe for Structure Identification of 1T' MoTe 2

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Zhou, Lin; Huang, Shengxi; Tatsumi, Yuki

    In this work, by combining transmission electron microscopy and polarized Raman spectroscopy for the 1T' MoTe 2 flakes with different thicknesses, we found that the polarization dependence of Raman intensity is given as a function of excitation laser wavelength, phonon symmetry, and phonon frequency, but has weak dependence on the flake thickness from few-layer to multilayer. Additionally, the frequency of Raman peaks and the relative Raman intensity are sensitive to flake thickness, which manifests Raman spectroscopy as an effective probe for thickness of 1T' MoTe 2. This work demonstrates that polarized Raman spectroscopy is a powerful and nondestructive method tomore » quickly identify the crystal structure and thickness of 1T' MoTe 2 simultaneously, which opens up opportunities for the in situ probe of anisotropic properties and broad applications of this novel material.« less

  9. Sensitive Phonon-Based Probe for Structure Identification of 1T' MoTe 2

    DOE PAGES

    Zhou, Lin; Huang, Shengxi; Tatsumi, Yuki; ...

    2017-05-25

    In this work, by combining transmission electron microscopy and polarized Raman spectroscopy for the 1T' MoTe 2 flakes with different thicknesses, we found that the polarization dependence of Raman intensity is given as a function of excitation laser wavelength, phonon symmetry, and phonon frequency, but has weak dependence on the flake thickness from few-layer to multilayer. Additionally, the frequency of Raman peaks and the relative Raman intensity are sensitive to flake thickness, which manifests Raman spectroscopy as an effective probe for thickness of 1T' MoTe 2. This work demonstrates that polarized Raman spectroscopy is a powerful and nondestructive method tomore » quickly identify the crystal structure and thickness of 1T' MoTe 2 simultaneously, which opens up opportunities for the in situ probe of anisotropic properties and broad applications of this novel material.« less

  10. Evidence of superconductivity-induced phonon spectra renormalization in alkali-doped iron selenides

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Opačić, M.; Lazarević, N.; Šćepanović, M.

    2015-11-16

    Polarized Raman scattering spectra of superconducting K xFe 2-ySe 2 and nonsuperconducting K 0.8Fe 1.8Co 0.2Se 2 single crystals were measured in a temperature range from 10 K up to 300 K. Two Raman active modes from the I4/mmm phase and seven from the I4/m phase are observed in frequency range from 150 to 325 cm -1 in both compounds, suggesting that K 0.8Fe 1.8Co 0.2Se 2 single crystal also has two-phase nature. Temperature dependence of Raman mode energy is analyzed in terms of lattice thermal expansion and phonon-phonon interaction. Temperature dependence of Raman mode linewidth is considered as temperature-inducedmore » anharmonic effects. It is shown that change of Raman mode energy with temperature is dominantly driven by thermal expansion of the crystal lattice. Abrupt change of the A 1g mode energy near T C was observed in K xFe 2-ySe 2 , whereas it is absent in K 0.8Fe 1.8Co 0.2Se 2. Phonon energy hardening at low temperatures in the superconducting sample is a consequence of superconductivity-induced redistribution of the electronic states below critical temperature.« less

  11. Phonons in Confinement and the Boson Peak Using Nuclear Inelastic Absorption

    NASA Astrophysics Data System (ADS)

    Asthalter, T.; Bauer, M.; van Bürck, U.; Sergueev, I.; Franz, H.; Chumakov, A. I.

    2002-12-01

    We have applied nuclear inelastic absorption (NIA) to the molecular glass former dibutylphthalate/ferrocene, both in bulk and in nanoporous matrices having pore sizes of 50 and 25 Å, respectively. The quantity g(E)/E 2, where g(E) is the vibrational phonon density of states (VDOS) of the resonant nuclei, exhibits a pronounced maximum at low energies. Confinement in pores leads to a suppression of the VDOS below 1.5 meV, independent of the pore size. Also in the scaled heat capacity C(T)/T 3, we observe a decrease of the peak maximum for low temperatures. Our observations are discussed in the light of experimental and theoretical results on nanocrystals and a recent theoretical model for the boson peak.

  12. IR absorption and surface-enhanced Raman spectra of the isoquinoline alkaloid berberine

    NASA Astrophysics Data System (ADS)

    Strekal', N. D.; Motevich, I. G.; Nowicky, J. W.; Maskevich, S. A.

    2007-01-01

    We present the IR absorption and surface-enhanced Raman scattering (SERS) spectra of the isoquinoline alkaloid berberine adsorbed on a silver hydrosol and on the surface of a silver electrode for different potentials. Based on quantum chemical calculations, for the first time we have assigned the vibrations in the berberine molecule according to vibrational mode. The effect of the potential of the silver electrode on the geometry of sorption of the molecule on the surface is considered, assuming a short-range mechanism for enhancement of Raman scattering.

  13. Theoretical study of the Raman active CDW gap mode in manganites.

    PubMed

    Rout, G C; Panda, Saswati; Behera, S N

    2010-09-22

    We report here the microscopic theory of the Raman spectra of the colossal magnetoresistive (CMR) manganite systems. The system is described by a model Hamiltonian consisting of the double exchange interaction in addition to the charge ordering interaction in the e(g) band and spin-spin interaction among the t(2g) core electrons. Further the phonon coupling to the conduction electron density is incorporated in the model for phonons in the harmonic approximation. The spectral density function for the Raman spectra is calculated from the imaginary part of the phonon Green's function. The calculated spectra display the Raman active bare phonon peak along with the charge ordering peak. The magnetic field and temperature dependence of the charge ordering peak agrees with the 480 cm(-1) JT mode observed in the experiments. The evolution of this mode is investigated in the report.

  14. Dynamics of monochromatically generated nonequilibrium phonons in LaF3:Pr3+

    NASA Astrophysics Data System (ADS)

    Tolbert, W. A.; Dennis, W. M.; Yen, W. M.

    1990-07-01

    The temporal evolution of nonequilibrium phonon populations in LaF3:Pr3+ is investigated at low temperatures (1.8 K) utilizing pulsed, tunable, monochromatic generation and time-resolved, tunable, narrow-band detection. High occupation number, narrow-band phonon populations are generated via far-infrared pumping of defect-induced one-phonon absorption. Time-resolved, frequency-selective detection is provided by optical sideband absorption. Nonequilibrium phonon decay times are measured and attributed to anharmonic decay.

  15. Mechanism of asymmetric lineshape broadening in GaAs1-xNx Raman spectra

    NASA Astrophysics Data System (ADS)

    Mialitsin, Aleksej; Fluegel, Brian; Ptak, Aaron; Mascarenhas, Angelo

    2012-07-01

    Resonance Raman spectroscopy is used to probe the asymmetric broadening of the LO phonon linewidth in a dilute GaAs1-xNx alloy (x=0.41%). Electronic Raman scattering from a broad continuum is observed that gets enhanced concurrently with the LO phonon linewidth under resonance. The Fano interaction between the LO phonon and the electronic continuum is used to develop a model that satisfactorily explains the origin of the asymmetric LO phonon linewidth broadening in this abnormal alloy as arising due to coupling between the discrete and the continuum configurations.

  16. Calculation of the Raman intensity in graphene and carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Moutinho, Marcus; Venezuela, Pedro

    2014-03-01

    Raman spectroscopy is one of the most important experimental techniques for characterization of carbon materials because it can give a lot of information about electronic and phonon structure in a non destructive way. We use a third-order quantum field model to obtain the theoretical Raman intensity for graphene and carbon nanotubes (CNT). The most important Raman peaks in graphitic materials comes from to the iLo and iTo phonon branches near to Γ and K points and, in this work, we focus our attention on some of these peaks, like the G, D and 2D bands, as a function of laser energy. The electronic and phonon dispersion used in our calculations reproduces the graphene ab initio results with GW corrections and the zone folding method is used to obtain the CNT ones. Our results show that the experimental G band Raman excitation profile for CNT can be reproduced if we use the proper electronic and phonon dispersions. We also show that the phonon dispersion may influence the shape of the graphene D band and the dispersive behavior of the 2D band for graphene and CNT. This work was supported by the Brazilian Nanocarbon Institute of Science and Technology (INCT/Nanocarbono), the Brazilian Network on Carbon Nanotube Research and the Brazilian agency CAPES

  17. Phonon dynamics of graphene on metals

    NASA Astrophysics Data System (ADS)

    Taleb, Amjad Al; Farías, Daniel

    2016-03-01

    The study of surface phonon dispersion curves is motivated by the quest for a detailed understanding of the forces between the atoms at the surface and in the bulk. In the case of graphene, additional motivation comes from the fact that thermal conductivity is dominated by contributions from acoustic phonons, while optical phonon properties are essential to understand Raman spectra. In this article, we review recent progress made in the experimental determination of phonon dispersion curves of graphene grown on several single-crystal metal surfaces. The two main experimental techniques usually employed are high-resolution electron energy loss spectroscopy (HREELS) and inelastic helium atom scattering (HAS). The different dispersion branches provide a detailed insight into the graphene-substrate interaction. Softening of optical modes and signatures of the substrate‧s Rayleigh wave are observed for strong graphene-substrate interactions, while acoustic phonon modes resemble those of free-standing graphene for weakly interacting systems. The latter allows determining the bending rigidity and the graphene-substrate coupling strength. A comparison between theory and experiment is discussed for several illustrative examples. Perspectives for future experiments are discussed.

  18. Probing lattice dynamics and electron-phonon coupling in the topological nodal-line semimetal ZrSiS

    NASA Astrophysics Data System (ADS)

    Singha, Ratnadwip; Samanta, Sudeshna; Chatterjee, Swastika; Pariari, Arnab; Majumdar, Dipanwita; Satpati, Biswarup; Wang, Lin; Singha, Achintya; Mandal, Prabhat

    2018-03-01

    Topological materials provide an exclusive platform to study the dynamics of relativistic particles in table-top experiments and offer the possibility of wide-scale technological applications. ZrSiS is a newly discovered topological nodal-line semimetal and has drawn enormous interests. In this paper, we have investigated the lattice dynamics and electron-phonon interaction in single-crystalline ZrSiS using Raman spectroscopy. Polarization and angle-resolved Raman data have been analyzed using crystal symmetries and theoretically calculated atomic vibrational patterns along with phonon dispersion spectra. Wavelength- and temperature-dependent measurements show the complex interplay of electron and phonon degrees of freedom, resulting in resonant phonon and quasielastic electron scattering through interband transition. Our high-pressure Raman studies reveal vibrational anomalies, which are the signature of structural phase transitions. Further investigations through high-pressure synchrotron x-ray diffraction clearly show pressure-induced structural transitions and coexistence of multiple phases, which also indicate possible electronic topological transitions in ZrSiS. This study not only provides the fundamental information on the phonon subsystem, but also sheds some light in understanding the topological nodal-line phase in ZrSiS and other isostructural systems.

  19. Chemical composition of matrix-embedded ternary II-VI nanocrystals derived from first- and second-order Raman spectra

    NASA Astrophysics Data System (ADS)

    Azhniuk, Yu. M.; Hutych, Yu. I.; Lopushansky, V. V.; Prymak, M. V.; Gomonnai, A. V.; Zahn, D. R. T.

    2016-12-01

    A one- and multiphonon Raman scattering study is performed for an extensive set of CdS1-xSex, Cd1-yZnyS, Cd1-yZnySe, and CdSe1-xTex nanocrystals to investigate the applicability of first- and second-order Raman spectra for the determination of the matrix-embedded ternary nanocrystal composition. For one-mode ternary systems both the LO and 2LO phonon frequencies in the Raman spectra are shown to be a good measure of the nanocrystal composition. For two-mode systems, the approaches based on the difference of the LO phonon frequencies (first-order Raman spectra) or double LO overtone and combination tone frequencies (second-order Raman spectra) as well as on the LO phonon band intensity ratios are analysed. The weak electron-phonon coupling in the II-VI nanocrystals and the polaron constant values for the nanocrystal sublattices are discussed.

  20. Optical phonon behavior of columbite MgNb2O6 single crystals

    NASA Astrophysics Data System (ADS)

    Xu, Dapeng; Liu, Wenqiang; Zhou, Qiang; Cui, Tian; Yuan, Hongming; Wang, Wenquan; Liu, Ying; Shi, Zhan; Li, Liang

    2014-08-01

    To explore potential applications, MgNb2O6 single crystal grown previously by optical floating zone method was used as a prototype for optical phonon behavior investigation. Polarized Raman spectra obtained in adequate parallel and crossed polarization were presented. All the obtained Raman modes were identified for the MgNb2O6, in good agreement with previous theory analysis. The selection rules of Raman for the columbite group were validated. Additionally, in-site temperature-dependent Raman spectra of MgNb2O6 were also investigated in the range from 83 to 803 K. The strong four Ag phonon modes all exhibits red shift with the temperature increasing. But thermal expansion of spectra is sectional linear with inflection points at about 373 K. And the absolute value of dω/dT at high temperature is higher than the one at lower temperature.

  1. The dependence of graphene Raman D-band on carrier density.

    PubMed

    Liu, Junku; Li, Qunqing; Zou, Yuan; Qian, Qingkai; Jin, Yuanhao; Li, Guanhong; Jiang, Kaili; Fan, Shoushan

    2013-01-01

    Raman spectroscopy has been an integral part of graphene research and can provide information about graphene structure, electronic characteristics, and electron-phonon interactions. In this study, the characteristics of the graphene Raman D-band, which vary with carrier density, are studied in detail, including the frequency, full width half-maximum, and intensity. We find the Raman D-band frequency increases for hole doping and decreases for electron doping. The Raman D-band intensity increases when the Fermi level approaches half of the excitation energy and is higher in the case of electron doping than that of hole doping. These variations can be explained by electron-phonon interaction theory and quantum interference between different Raman pathways in graphene. The intensity ratio of Raman D- and G-band, which is important for defects characterization in graphene, shows a strong dependence on carrier density.

  2. A multimode vibronic treatment of absorption, resonance Raman, and hyper-Rayleigh scattering of excitonically coupled molecular dimers

    NASA Astrophysics Data System (ADS)

    Myers Kelley, Anne

    2003-08-01

    The linear absorption spectra, resonance Raman excitation profiles and depolarization dispersion curves, and hyper-Rayleigh scattering profiles are calculated for excitonically coupled homodimers of a model electron donor-acceptor "push-pull" conjugated chromophore as a function of dimer geometry. The vibronic eigenstates of the dimer are calculated by diagonalizing the matrix of transition dipole couplings among the vibronic transitions of the constituent monomers. The absorption spectra show the usual red- or blueshifted transitions for J-type or H-type dimers, respectively. When the electronic coupling is large compared with the vibronic width of the monomer spectrum, the dimer absorption spectra exhibit simple Franck-Condon progressions having reduced vibronic intensities compared with the monomer, and the resonance Raman excitation profiles are shifted but otherwise only weakly perturbed. When the coupling is comparable to the vibronic width, the H-dimer absorption spectra exhibit irregular vibronic frequency spacings and intensity patterns and the effects on the Raman excitation profiles are larger. There is strong dispersion in the Raman depolarization ratios for dimer geometries in which both transitions carry oscillator strength. The first hyperpolarizabilities are somewhat enhanced in J-dimers and considerably reduced in H-dimers. These effects on the molecular β will amplify the effects of dimerization on the ground-state dipole moment in electro-optic materials formed from chromophore-doped polymers that must be electric field poled to obtain the net alignment needed for a macroscopic χ(2).

  3. Temperature dependence of Brillouin light scattering spectra of acoustic phonons in silicon

    NASA Astrophysics Data System (ADS)

    Olsson, Kevin S.; Klimovich, Nikita; An, Kyongmo; Sullivan, Sean; Weathers, Annie; Shi, Li; Li, Xiaoqin

    2015-02-01

    Electrons, optical phonons, and acoustic phonons are often driven out of local equilibrium in electronic devices or during laser-material interaction processes. The need for a better understanding of such non-equilibrium transport processes has motivated the development of Raman spectroscopy as a local temperature sensor of optical phonons and intermediate frequency acoustic phonons, whereas Brillouin light scattering (BLS) has recently been explored as a temperature sensor of low-frequency acoustic phonons. Here, we report the measured BLS spectra of silicon at different temperatures. The origins of the observed temperature dependence of the BLS peak position, linewidth, and intensity are examined in order to evaluate their potential use as temperature sensors for acoustic phonons.

  4. Temperature dependence of Brillouin light scattering spectra of acoustic phonons in silicon

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Olsson, Kevin S.; Klimovich, Nikita; An, Kyongmo

    2015-02-02

    Electrons, optical phonons, and acoustic phonons are often driven out of local equilibrium in electronic devices or during laser-material interaction processes. The need for a better understanding of such non-equilibrium transport processes has motivated the development of Raman spectroscopy as a local temperature sensor of optical phonons and intermediate frequency acoustic phonons, whereas Brillouin light scattering (BLS) has recently been explored as a temperature sensor of low-frequency acoustic phonons. Here, we report the measured BLS spectra of silicon at different temperatures. The origins of the observed temperature dependence of the BLS peak position, linewidth, and intensity are examined in ordermore » to evaluate their potential use as temperature sensors for acoustic phonons.« less

  5. Decoupling of epitaxial graphene via gold intercalation probed by dispersive Raman spectroscopy

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Pillai, P. B., E-mail: p.pillai@sheffield.ac.uk, E-mail: m.desouza@sheffield.ac.uk; DeSouza, M., E-mail: p.pillai@sheffield.ac.uk, E-mail: m.desouza@sheffield.ac.uk; Narula, R.

    Signatures of a superlattice structure composed of a quasi periodic arrangement of atomic gold clusters below an epitaxied graphene (EG) layer are examined using dispersive Raman spectroscopy. The gold-graphene system exhibits a laser excitation energy dependant red shift of the 2D mode as compared to pristine epitaxial graphene. The phonon dispersions in both the systems are mapped using the experimentally observed Raman signatures and a third-nearest neighbour tight binding electronic band structure model. Our results reveal that the observed excitation dependent Raman red shift in gold EG primarily arise from the modifications of the phonon dispersion in gold-graphene and showsmore » that the extent of decoupling of graphene from the underlying SiC substrate can be monitored from the dispersive nature of the Raman 2D modes. The intercalated gold atoms restore the phonon band structure of epitaxial graphene towards free standing graphene.« less

  6. Probing Phonon Dynamics in Individual Single-Walled Carbon Nanotubes.

    PubMed

    Jiang, Tao; Hong, Hao; Liu, Can; Liu, Wei-Tao; Liu, Kaihui; Wu, Shiwei

    2018-04-11

    Interactions between elementary excitations, such as carriers, phonons, and plasmons, are critical for understanding the optical and electronic properties of materials. The significance of these interactions is more prominent in low-dimensional materials and can dominate their physical properties due to the enhanced interactions between these excitations. One-dimensional single-walled carbon nanotubes provide an ideal system for studying such interactions due to their perfect physical structures and rich electronic properties. Here we investigated G-mode phonon dynamics in individual suspended chirality-resolved single-walled carbon nanotubes by time-resolved anti-Stokes Raman spectroscopy. The improved technique allowed us to probe the intrinsic phonon information on a single-tube level and exclude the influences of tube-tube and tube-substrate interactions. We found that the G-mode phonon lifetime ranges from 0.75-2.25 ps and critically depends on whether the tube is metallic or semiconducting. In comparison with the phonon lifetimes in graphene and graphite, we revealed structure-dependent carrier-phonon and phonon-phonon interactions in nanotubes. Our results provide new information for optimizing the design of nanotube electronic/optoelectronic devices by better understanding and utilizing their phonon decay channels.

  7. Charge tuning of nonresonant magnetoexciton phonon interactions in graphene.

    PubMed

    Rémi, Sebastian; Goldberg, Bennett B; Swan, Anna K

    2014-02-07

    Far from resonance, the coupling of the G-band phonon to magnetoexcitons in single layer graphene displays kinks and splittings versus filling factor that are well described by Pauli blocking and unblocking of inter- and intra-Landau level transitions. We explore the nonresonant electron-phonon coupling by high-magnetic field Raman scattering while electrostatic tuning of the carrier density controls the filling factor. We show qualitative and quantitative agreement between spectra and a linearized model of electron-phonon interactions in magnetic fields. The splitting is caused by dichroism of left- and right-handed circular polarized light due to lifting of the G-band phonon degeneracy, and the piecewise linear slopes are caused by the linear occupancy of sequential Landau levels versus ν.

  8. Effective electron mass and phonon modes in n-type hexagonal InN

    NASA Astrophysics Data System (ADS)

    Kasic, A.; Schubert, M.; Saito, Y.; Nanishi, Y.; Wagner, G.

    2002-03-01

    Infrared spectroscopic ellipsometry and micro-Raman scattering are used to study vibrational and electronic properties of high-quality hexagonal InN. The 0.22-μm-thick highly n-conductive InN film was grown on c-plane sapphire by radio-frequency molecular-beam epitaxy. Combining our results from the ellipsometry data analysis with Hall-effect measurements, the isotropically averaged effective electron mass in InN is determined as 0.14m0. The resonantly excited zone center E1 (TO) phonon mode is observed at 477 cm-1 in the ellipsometry spectra. Despite the high electron concentration in the film, a strong Raman mode occurs in the spectral range of the unscreened A1(LO) phonon. Because an extended carrier-depleted region at the sample surface can be excluded from the ellipsometry-model analysis, we assign this mode to the lower branch of the large-wave-vector LO-phonon-plasmon coupled modes arising from nonconserving wave-vector scattering processes. The spectral position of this mode at 590 cm-1 constitutes a lower limit for the unscreened A1(LO) phonon frequency.

  9. Femtosecond transient absorption, Raman, and electrochemistry studies of tetrasulfonated copper phthalocyanine in water solutions.

    PubMed

    Abramczyk, H; Brozek-Płuska, B; Kurczewski, K; Kurczewska, M; Szymczyk, I; Krzyczmonik, P; Błaszczyk, T; Scholl, H; Czajkowski, W

    2006-07-20

    Ultrafast time-resolved electronic spectra of the primary events induced in the copper tetrasulfonated phthalocyanine Cu(tsPc)4-) in aqueous solution has been measured by femtosecond pump-probe transient absorption spectroscopy. The primary events initiated by the absorption of a photon occurring within the femtosecond time scale are discussed on the basis of the electron transfer mechanism between the adjacent phthalocyanine rings proposed recently in our laboratory. The femtosecond transient absorption results are compared with the low temperature emission spectra obtained with Raman spectroscopy and the voltammetric curves.

  10. Influence of electronic band topology on phonon properties in Dirac materials

    NASA Astrophysics Data System (ADS)

    Garate, Ion; Saha, Kush; Légaré, Katherine

    2015-03-01

    In Dirac materials, the interaction between electrons and long-wavelength phonons has been shown to induce and stabilize topological insulation [1-2]. Here report on a theoretical study of the converse effect, namely the influence of band topology on phonon properties. We calculate how electron-phonon interactions change the bulk phonon dispersion as a function of pressure and temperature, in both trivial and topological phases. We find that (i) topological insulators are more prone to lattice instabilities than trivial insulators, and (ii) Raman and neutron scattering measurements can be used to determine the electronic band topology. Research funded by Canada's NSERC and Québec's RQMP.

  11. Electron-electron correlations in Raman spectra of VO2

    NASA Astrophysics Data System (ADS)

    Goncharuk, I. N.; Ilinskiy, A. V.; Kvashenkina, O. E.; Shadrin, E. B.

    2013-01-01

    It has been shown that, in single crystals and films of a strongly correlated material, namely, vanadium dioxide, upon a thermally stimulated phase transition from the low-temperature monoclinic phase to the high-temperature tetragonal phase, the narrow-line Raman spectrum of the insulating (monoclinic) phase transforms into the broad-band Raman spectrum, which contains two peaks at 500 and 5000 cm-1 with widths of 400 and 3500 cm-1, respectively. It has been found that, as the temperature of the monoclinic phase approaches the structural phase transition temperature (340 K), the line profile of soft-mode phonons at a frequency of 149 cm-1 with A g symmetry and the line profile of phonons at a frequency of 201 cm-1 with A g symmetry acquire an asymmetric shape with a Fano antiresonance that is characteristic of the interaction of a single phonon vibration with a continuum of strongly correlated electrons. It has been demonstrated that the thermal transformation of peaks in the Raman spectra of the VO2 metallic phase is in quantitative agreement with the theory of Raman scattering in strongly correlated materials.

  12. Phonon anharmonicity of monoclinic zirconia and yttrium-stabilized zirconia

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Li, Chen W.; Smith, Hillary L.; Lan, Tian

    2015-04-13

    Inelastic neutron scattering measurements on monoclinic zirconia (ZrO 2) and 8 mol% yttrium-stabilized zirconia were performed at temperatures from 300 to 1373 ωK. We reported temperature-dependent phonon densities of states (DOS) and Raman spectra obtained at elevated temperatures. First-principles lattice dynamics calculations with density functional theory gave total and partial phonon DOS curves and mode Grüneisen parameters. These mode Grüneisen parameters were used to predict the experimental temperature dependence of the phonon DOS with partial success. However, substantial anharmonicity was found at elevated temperatures, especially for phonon modes dominated by the motions of oxygen atoms. Yttrium-stabilized zirconia (YSZ) was somewhatmore » more anharmonic and had a broader phonon spectrum at low temperatures, owing in part to defects in its structure. YSZ also has a larger vibrational entropy than monoclinic zirconia.« less

  13. Surface phonons in the topological insulators Bi2Se3 and Bi2Te3

    NASA Astrophysics Data System (ADS)

    Boulares, Ibrahim; Shi, Guangsha; Kioupakis, Emmanouil; Lošťák, Petr; Uher, Ctirad; Merlin, Roberto

    2018-03-01

    Raman scattering [K. M. F. Shahil et al., Appl. Phys. Lett. 96, 153103 (2010), V. Gnezdilov et al., Phys. Rev. B 84, 195118 (2011) and H. -H. Kung et al., Phys. Rev. B 95, 245406 (2017)], inelastic helium scattering [X. Zhu et al., Phys. Rev. Lett. 107, 186102 (2011)] and photoemission experiments [J. A. Sobota et al., Phys. Rev. Lett. 113, 157401 (2014)] on the topological insulators Bi2Se3 and Bi2Te3 show features in the range ∼ 50-160 cm-1, which have been assigned alternatively to Raman-forbidden, bulk infrared modes arising from symmetry breaking at the surface or to surface phonons, which couple to the topologically protected electronic states. Here, we present temperature- and wavelength- dependent Raman studies showing additional modes we ascribe to surface phonons in both Bi2Se3 and Bi2Te3. Our assignment is supported by density functional theory calculations revealing surface phonons at frequencies close to those of the extra peaks in the Raman data. The theoretical results also indicate that these modes are not a consequence of spin-orbit coupling and, thus, that their occurrence is unrelated to the topological properties of these materials.

  14. Characterization of Materials by Raman Scattering

    NASA Astrophysics Data System (ADS)

    Kozielski, M.

    2007-03-01

    The paper reports on the use of phonon spectra obtained with the Raman spectroscopy for characterization of different materials. The Raman scattering spectra obtained for zinc selenide crystals, mixed crystals zinc selenide admixtured with magnesium or beryllium, oxide crystals including strontium lanthanum gallate, molecular crystals of triammonium hydrogen diseleniate and a homologous series of polyoxyethylene glycols are analysed.

  15. Sensing coherent phonons with two-photon interference

    NASA Astrophysics Data System (ADS)

    Ding, Ding; Yin, Xiaobo; Li, Baowen

    2018-02-01

    Detecting coherent phonons pose different challenges compared to coherent photons due to the much stronger interaction between phonons and matter. This is especially true for high frequency heat carrying phonons, which are intrinsic lattice vibrations experiencing many decoherence events with the environment, and are thus generally assumed to be incoherent. Two photon interference techniques, especially coherent population trapping (CPT) and electromagnetically induced transparency (EIT), have led to extremely sensitive detection, spectroscopy and metrology. Here, we propose the use of two photon interference in a three-level system to sense coherent phonons. Unlike prior works which have treated phonon coupling as damping, we account for coherent phonon coupling using a full quantum-mechanical treatment. We observe strong asymmetry in absorption spectrum in CPT and negative dispersion in EIT susceptibility in the presence of coherent phonon coupling which cannot be accounted for if only pure phonon damping is considered. Our proposal has application in sensing heat carrying coherent phonons effects and understanding coherent bosonic multi-pathway interference effects in three coupled oscillator systems.

  16. Electron-Phonon and Electron-Electron Interactions in Individual Suspended Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Cronin, Stephen

    2010-03-01

    The fabrication of pristine, nearly defect-free, suspended carbon nanotubes (CNTs) enables the observation of several phenomena not seen before in carbon nanotubes, including breakdown of the Born-Oppenheimer approximation^1, mode selective electron-phonon coupling^2, and a Mott insulator transition^3. Raman spectroscopy of these nanotubes under applied gate and bias potentials reveals exceptionally strong electron-phonon coupling, arising from Kohn anomalies, which result in mode selective electron-phonon coupling, negative differential conductance (NDC), and non-equilibrium phonon populations^2,4. Due to the extremely long electron lifetimes, we observe a breakdown of the Born-Oppenheimer approximation, as deduced from the gate voltage-induced changes in the vibrational energies of suspended carbon nanotubes^1. We also report strikingly large variations in the Raman intensity of pristine metallic CNTs in response to gate voltages, which are attributed to a Mott insulating state of the strongly correlated electrons^3. As will be shown, preparing clean, defect-free devices is an essential prerequisite for studying the rich low-dimensional physics of CNTs. (1.) Bushmaker, A.W., Deshpande, V.V., Hsieh, S., Bockrath, M.W., and Cronin, S.B., ``Direct Observation of Born-Oppenheimer Approximation Breakdown in Carbon Nanotubes.'' Nano Letters, 9, 607 (2009). (2.) Bushmaker, A.W., Deshpande, V.V., Bockrath, M.W., and Cronin, S.B., ``Direct Observation of Mode Selective Electron-Phonon Coupling in Suspended Carbon Nanotubes.'' Nano Letters, 7, 3618 (2007) (3.) Bushmaker, A.W., Deshpande, V.V., Hsieh, S., Bockrath, M.W., and Cronin, S.B., ``Large Modulations in the Intensity of Raman-Scattered Light from Pristine Carbon Nanotubes.'' Physical Review Letters, 103, 067401 (2009). (4.) Bushmaker, A.W., Deshpande, V.V., Hsieh, S., Bockrath, M.W., and Cronin, S.B., ``Gate Voltage Controlled Non-Equilibrium and Non-Ohmic Behavior in Suspended Carbon Nanotubes.'' Nano Letters, 9

  17. Evidence of spin phonon coupling in magnetoelectric NiFe{sub 2}O{sub 4}/PMN-PT composite

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Ahlawat, Anju; Satapathy, S., E-mail: srinu73@rrcat.gov.in, E-mail: srinusatapathy@gmail.com; Gupta, P. K.

    2013-12-16

    The coupling of phonon with spin in strain coupled magnetoelectric NiFe{sub 2}O{sub 4} (NFO)/0.65Pb(Mg{sub 1/3}Nb{sub 2/3})O{sub 3}–0.35PbTiO{sub 3} (PMN-PT) composite was investigated by temperature-dependent Raman spectroscopy and magnetic measurements in the range 30–350 °C. Pure NFO shows usual ferromagnetic behaviour in this temperature range while NFO/PMN-PT composite show dramatic change in magnetic moment across ferroelectric transition temperature (T{sub c} ∼ 180 °C) of PMN-PT. The temperature evolution of the Raman spectra for the composite shows significant phonon anomalies in T-site (Fe-O) and O-site (Ni/Fe-O) phonon modes at ferroelectric transition temperature is attributed to spin phonon coupling in NFO/PMN-PT composite. The strain mediated magnetoelectric couplingmore » mechanism in this composite is apparent from the observed spin phonon interaction.« less

  18. The effect of n- and p-type doping on coherent phonons in GaN.

    PubMed

    Ishioka, Kunie; Kato, Keiko; Ohashi, Naoki; Haneda, Hajime; Kitajima, Masahiro; Petek, Hrvoje

    2013-05-22

    The effect of doping on the carrier-phonon interaction in wurtzite GaN is investigated by pump-probe reflectivity measurements using 3.1 eV light in near resonance with the fundamental band gap of 3.39 eV. Coherent modulations of the reflectivity due to the E2 and A1(LO) modes, as well as the 2A1(LO) overtone are observed. Doping of acceptor and donor atoms enhances the dephasing of the polar A1(LO) phonon via coupling with plasmons, with the effect of donors being stronger. Doping also enhances the relative amplitude of the coherent A1(LO) phonon with respect to that of the high-frequency E2 phonon, though it does not affect the relative intensity in Raman spectroscopic measurements. We attribute this enhanced coherent amplitude to the transient depletion field screening (TDFS) excitation mechanism, which, in addition to impulsive stimulated Raman scattering (ISRS), contributes to the generation of coherent polar phonons even for sub-band gap excitation. Because the TDFS mechanism requires photoexcitation of carriers, we argue that the interband transition is made possible at a surface with photon energies below the bulk band gap through the Franz-Keldysh effect.

  19. Investigation of Ferroelectric Domain Walls by Raman Spectroscopy

    NASA Astrophysics Data System (ADS)

    Stone, Gregory A.

    Ferroelectric materials are characterized by an intrinsic spontaneous electric dipole moment that can be manipulated by the application of an electric field. Regions inside the crystal, known as domains, can have the spontaneous dipole moments oriented in a different direction than the surrounding crystal. Due to favorable piezoelectric, pyroelectric, electro-optic, and nonlinear optical properties, ferroelectric materials are attractive for commercial applications. Many devices, such as nonlinear frequency converters, require precisely engineered domain patterns. The properties of domains and their boundaries, known as domain walls, are vital to the performance and limitations of these devices. As a result, ferroelectric domains and the domain walls have been the focus of many scientific studies. Despite all this work, questions remain regarding their properties. This work is aimed at developing a better understanding of the properties of the domain wall using confocal Raman spectroscopy. Raman spectra taken from domain walls in Lithium Niobate and Lithium Tantalate reveal two distinct changes in the Raman spectra: (1) Shifts in frequency of the bulk Raman modes, which persists over a range of 0.2-0.5 mu m from the domain wall. The absence of this effect in defect free stoichiometric Lithium Tantalate indicates that the shifts are related to defects inside the crystal. (2) The presence of Raman modes corresponding to phonons propagating orthogonal to the laser beam axis, which are not collected in the bulk crystal. The phonons also preferential propagate normal to the domain wall. These modes are detected up to 0.35 mum from the domain wall. The observation and separation of these effects was made possible by the optimized spatial resolution (0.23 mum) of a home-built scanning confocal microscope and the fact that degeneracy of the transverse and longitudinal phonon polarization is lifted by polar phonons in Lithium Niobate and Lithium Tantalate. Raman

  20. Intricate Resonant Raman Response in Anisotropic ReS2.

    PubMed

    McCreary, Amber; Simpson, Jeffrey R; Wang, Yuanxi; Rhodes, Daniel; Fujisawa, Kazunori; Balicas, Luis; Dubey, Madan; Crespi, Vincent H; Terrones, Mauricio; Hight Walker, Angela R

    2017-10-11

    The strong in-plane anisotropy of rhenium disulfide (ReS 2 ) offers an additional physical parameter that can be tuned for advanced applications such as logic circuits, thin-film polarizers, and polarization-sensitive photodetectors. ReS 2 also presents advantages for optoelectronics, as it is both a direct-gap semiconductor for few-layer thicknesses (unlike MoS 2 or WS 2 ) and stable in air (unlike black phosphorus). Raman spectroscopy is one of the most powerful characterization techniques to nondestructively and sensitively probe the fundamental photophysics of a 2D material. Here, we perform a thorough study of the resonant Raman response of the 18 first-order phonons in ReS 2 at various layer thicknesses and crystal orientations. Remarkably, we discover that, as opposed to a general increase in intensity of all of the Raman modes at excitonic transitions, each of the 18 modes behave differently relative to each other as a function of laser excitation, layer thickness, and orientation in a manner that highlights the importance of electron-phonon coupling in ReS 2 . In addition, we correct an unrecognized error in the calculation of the optical interference enhancement of the Raman signal of transition metal dichalcogenides on SiO 2 /Si substrates that has propagated through various reports. For ReS 2 , this correction is critical to properly assessing the resonant Raman behavior. We also implemented a perturbation approach to calculate frequency-dependent Raman intensities based on first-principles and demonstrate that, despite the neglect of excitonic effects, useful trends in the Raman intensities of monolayer and bulk ReS 2 at different laser energies can be accurately captured. Finally, the phonon dispersion calculated from first-principles is used to address the possible origins of unexplained peaks observed in the Raman spectra, such as infrared-active modes, defects, and second-order processes.

  1. Spectroscopy of infrared-active phonons in high-temperature superconductors

    NASA Technical Reports Server (NTRS)

    Litvinchuk, A. P.; Thomsen, C.; Cardona, M.; Borjesson, L.

    1995-01-01

    For a large variety of superconducting materials both experimental and theoretical lattice dynamical studies have been performed to date. The assignment of the observed infrared- and Raman-active phonon modes to the particular lattice eigenmodes is generally accepted. We will concentrate here upon the analysis of the changes of the infrared-phonon parameters (frequency and linewidth) upon entering the superconducting state which, as will be shown, may provide information on the magnitude of the superconductivity-related gap and its dependence on the superconducting transition temperature Tc.

  2. Resonant-Raman Intensities of N-layer Transition Metal Dichalcogenides from First Principles

    NASA Astrophysics Data System (ADS)

    Miranda, Henrique; Froehlicher, Guillaume; Lorchat, Ettienne; Fernique, François; Molina-Sánchez, Alejandro; Berciaud, Stéphane; Wirtz, Ludger

    Transition metal dichalcogenides (TMDs) have interesting optical and electronic properties that make them good candidates for nano-engineering applications. Raman spectroscopy provides information about the vibrational modes and optical spectrum at the same time: when the laser energy is close to an electronic transition, the intensity is increased due to resonance. We investigate these effects combining different ab initio methods: we obtain ground-state and vibrational properties from density functional theory and the optical absorption spectrum using GW corrections and the Bethe-Salpeter equation to account for the excitonic effects which are known to play an important role in TMDs. Using a quasi-static finite differences approach, we calculate the dielectric susceptibility for different light polarizations and different phonon modes in order to determine the Raman tensor of TMDs, in particular of multi-layer and bulk MoTe2. We explain recent experimental results for the splitting of high-frequency modes and deviations from the non-resonant Raman model. We also give a brief outlook on possible improvements of the methodology.

  3. Two-Phonon Absorption

    ERIC Educational Resources Information Center

    Hamilton, M. W.

    2007-01-01

    A nonlinear aspect of the acousto-optic interaction that is analogous to multi-photon absorption is discussed. An experiment is described in which the second-order acousto-optically scattered intensity is measured and found to scale with the square of the acoustic intensity. This experiment using a commercially available acousto-optic modulator is…

  4. Reshaping the phonon energy landscape of nanocrystals inside a terahertz plasmonic nanocavity.

    PubMed

    Jin, Xin; Cerea, Andrea; Messina, Gabriele C; Rovere, Andrea; Piccoli, Riccardo; De Donato, Francesco; Palazon, Francisco; Perucchi, Andrea; Di Pietro, Paola; Morandotti, Roberto; Lupi, Stefano; De Angelis, Francesco; Prato, Mirko; Toma, Andrea; Razzari, Luca

    2018-02-22

    Phonons (quanta of collective vibrations) are a major source of energy dissipation and drive some of the most relevant properties of materials. In nanotechnology, phonons severely affect light emission and charge transport of nanodevices. While the phonon response is conventionally considered an inherent property of a nanomaterial, here we show that the dipole-active phonon resonance of semiconducting (CdS) nanocrystals can be drastically reshaped inside a terahertz plasmonic nanocavity, via the phonon strong coupling with the cavity vacuum electric field. Such quantum zero-point field can indeed reach extreme values in a plasmonic nanocavity, thanks to a mode volume well below λ 3 /10 7 . Through Raman measurements, we find that the nanocrystals within a nanocavity exhibit two new "hybridized" phonon peaks, whose spectral separation increases with the number of nanocrystals. Our findings open exciting perspectives for engineering the optical phonon response of functional nanomaterials and for implementing a novel platform for nanoscale quantum optomechanics.

  5. Experimental evidence of zone-center optical phonon softening by accumulating holes in thin Ge

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Kabuyanagi, Shoichi; Nishimura, Tomonori; Yajima, Takeaki

    2016-01-15

    We discuss the impact of free carriers on the zone-center optical phonon frequency in germanium (Ge). By taking advantage of the Ge-on-insulator structure, we measured the Raman spectroscopy by applying back-gate bias. Phonon softening by accumulating holes in Ge film was clearly observed. This fact strongly suggests that the phonon softening in heavily-doped Ge is mainly attributed to the free carrier effect rather than the dopant atom counterpart. Furthermore, we propose that the free carrier effect on phonon softening is simply understandable from the viewpoint of covalent bonding modification by free carriers.

  6. Phonon stiffen and soften at zigzag- and armchair-dominated edges of exfoliated bilayer graphene ribbon presented by Raman spectra

    NASA Astrophysics Data System (ADS)

    Xia, Minggang; Zhou, Xiaohua; Xin, Duqiang; Xu, Qiang

    2018-01-01

    The Raman spectra at the edge of the exfoliated bilayer graphene ribbon (GR) were investigated in detail. Results show that both G and 2D phonons stiffen (wave number increases) at zigzag-dominated edge, while they soften at armchair-dominated edge compared with those at the middle position in the GR. Furthermore, the full widths at half maximum intensity of both G and 2D Raman peaks narrow at the zigzag-dominated edge, while they broaden at the armchair-dominated edge. The stiffness and softness are attributed to the C-C bonds at the edge. For zigzag-dominated edge, the stiffness may originate in the increase of the force constant induced by the shrinking of C-C bond. For armchair-dominated edge, the softness may be due to the decrease of the force constant induced by the unsaturated hanging bonds at edge, which is different from Kohn anomaly and charge doping. The analysis is in agreement well with others calculation results about C-C bonds and the edge energy. These results may be useful to understand physical properties at the bilayer graphene edge and for applications in the device by taking advantage of the edge states in bilayer graphene.

  7. Unified Description of the Optical Phonon Modes in N-Layer MoTe2

    NASA Astrophysics Data System (ADS)

    Froehlicher, Guillaume; Lorchat, Etienne; Fernique, François; Joshi, Chaitanya; Molina-Sánchez, Alejandro; Wirtz, Ludger; Berciaud, Stéphane

    N -layer transition metal dichalcogenides (denoted MX2) provide a unique platform to investigate the evolution of the physical properties between the bulk (3D) and monolayer (quasi-2D) limits. Here, we present a unified analysis of the optical phonon modes in N-layer 2 H -MX2. The 2 H -phase (or hexagonal phase) is the most common polytype for semiconducting MX2 (such as MoS2). Using Raman spectroscopy, we have measured the manifold of low-frequency (rigid layer), mid-frequency (involving intralayer displacement of the chalcogen atoms only), and high-frequency (involving intralayer displacements of all atoms) Raman-active modes in N = 1 to 12 layer 2 H -molybdenenum ditelluride (MoTe2). For each monolayer mode, the N-dependent phonon frequencies give rise to fan diagrams that are quantitatively fit to a force constant model. This analysis allows us to deduce the frequencies of all the bulk (including silent) optical phonon modes.

  8. Raman scattering of IrTe2

    NASA Astrophysics Data System (ADS)

    Lee, Alexander; Thorsmolle, Verner; Artyukhin, Sergey; Yang, Jun; Cheong, Sang-Wook; Blumberg, Girsh

    2014-03-01

    IrTe2 presents a layered compound with a triangular lattice. It is known to exhibit a first order structural phase transition at approximately 260 K which is of a first order, corresponding to a formation of a superstructure with a period of five unit cells. Using polarized Raman spectroscopy we have studied the temperature dependence of 14 observed Raman allowed phononic modes. These phonons couple strongly to this transition and one additional first order transition at approximately 170 K. In the high-temperature phase only 3 modes are observed, while below approximately 280 K all 14 modes become visible. Below approximately 170 K only 11 modes are observed. Our results shed light on the possible mechanism driving the transitions. ACL, VKT and GB acknowledge support by NSF DMR-1104884.

  9. Optical phonon modes in rhombohedral boron monosulfide under high pressure

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Cherednichenko, Kirill A.; IMPMC, UPMC Sorbonne Universités, CNRS UMR 7590, 75005 Paris; LSPM–CNRS, Université Paris Nord, 93430 Villetaneuse

    2015-05-14

    Raman spectra of rhombohedral boron monosulfide (r-BS) were measured under pressures up to 34 GPa at room temperature. No pressure-induced structural phase transition was observed, while strong pressure shift of Raman bands towards higher wavenumbers has been revealed. IR spectroscopy as a complementary technique has been used in order to completely describe the phonon modes of r-BS. All experimentally observed bands have been compared with theoretically calculated ones and modes assignment has been performed. r-BS enriched by {sup 10}B isotope was synthesized, and the effect of boron isotopic substitution on Raman spectra was observed and analyzed.

  10. Phonon Confinement Effect in TiO2 Nanoparticles as Thermosensor Materials

    DTIC Science & Technology

    2018-01-24

    TiO2 or ZnO nanoparticles (NPs) have a very strong finite-size dependency in their Raman spectra or photoluminescence (PL) spectra due to the phonon...spectrometers were used to establish the particle size versus the Raman/PL peak position master curves. Systematic isothermal and temperature- dependent heat...Thermosensor Materials", Workshop on Time- Dependent Temperature Measurements in Energy Release Processes, Chicago, IL, 2012. 11 3) Ashish Kumar Mishra

  11. Isotopic effects on phonon anharmonicity in layered van der Waals crystals: Isotopically pure hexagonal boron nitride

    NASA Astrophysics Data System (ADS)

    Cuscó, Ramon; Artús, Luis; Edgar, James H.; Liu, Song; Cassabois, Guillaume; Gil, Bernard

    2018-04-01

    Hexagonal boron nitride (h -BN) is a layered crystal that is attracting a great deal of attention as a promising material for nanophotonic applications. The strong optical anisotropy of this crystal is key to exploit polaritonic modes for manipulating light-matter interactions in 2D materials. h -BN has also great potential for solid-state neutron detection and neutron imaging devices, given the exceptionally high thermal neutron capture cross section of the boron-10 isotope. A good knowledge of phonons in layered crystals is essential for harnessing long-lived phonon-polariton modes for nanophotonic applications and may prove valuable for developing solid-state 10BN neutron detectors with improved device architectures and higher detection efficiencies. Although phonons in graphene and isoelectronic materials with a similar hexagonal layer structure have been studied, the effect of isotopic substitution on the phonons of such lamellar compounds has not been addressed yet. Here we present a Raman scattering study of the in-plane high-energy Raman active mode on isotopically enriched single-crystal h -BN. Phonon frequency and lifetime are measured in the 80-600-K temperature range for 10B-enriched, 11B-enriched, and natural composition high quality crystals. Their temperature dependence is explained in the light of perturbation theory calculations of the phonon self-energy. The effects of crystal anisotropy, isotopic disorder, and anharmonic phonon-decay channels are investigated in detail. The isotopic-induced changes in the phonon density of states are shown to enhance three-phonon anharmonic decay channels in 10B-enriched crystals, opening the possibility of isotope tuning of the anharmonic phonon decay processes.

  12. Estimation of electron–phonon coupling and Urbach energy in group-I elements doped ZnO nanoparticles and thin films by sol–gel method

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Vettumperumal, R.; Kalyanaraman, S., E-mail: mayura_priya2003@yahoo.co.in; Santoshkumar, B.

    Highlights: • Comparison of group-I elements doped ZnO nanoparticles and thin films. • Calculation of electron–phonon coupling and phonon lifetime from Raman spectroscopy. • Estimation of interband states from Urbach energy. - Abstract: Group-I (Li, Na, K & Cs) elements doped ZnO nanoparticles (NPs) and thin films were prepared using sol–gel method. XRD data and TEM images confirm the absence of any other secondary phase different from wurtzite type ZnO. Spherical shapes of grains are observed from the surfaces of doped ZnO films by atomic force microscope images (AFM) and presences of dopants are confirmed from energy dispersive X-ray spectra.more » The Raman active E{sub 2} (high), E{sub 2} (low), E{sub 1} and A{sub 1} (LO) modes are observed from both ZnO NPs and thin films. First-order longitudinal optical (LO) phonon is found to have contributions from direct band transition and localized excitons. Electron–phonon coupling, phonon lifetime and deformation energy of ZnO are calculated based on the effect of dopants with respect to the multiple Raman LO phonon scattering. Presence of localized interbands states in doped ZnO NPs and thin films are found from the Urbach energy calculations.« less

  13. Dielectric and phonon spectroscopy of Nb-doped Pb(Zr1-yTiy)O3-CoFe2O4 composites

    NASA Astrophysics Data System (ADS)

    Sakanas, Aurimas; Nuzhnyy, Dmitry; Grigalaitis, Robertas; Banys, Juras; Borodavka, Fedir; Kamba, Stanislav; Ciomaga, Cristina Elena; Mitoseriu, Liliana

    2017-06-01

    Broad-band dielectric and phonon response of Nb-doped (1-x)Pb(Zr1-yTiy)O3-xCoFe2O4 composites with x = 10%-30% was investigated between 0.1 MHz and 100 THz. At room temperature, a broad distribution of relaxation times causes a constant dielectric loss below 1 GHz. Above room temperature, a strong Maxwell-Wagner relaxation process dominates below 1 GHz due to the conductivity of CoFe2O4 (CF). Two additional relaxation processes are seen between 1 GHz and 1 THz. The lower-frequency one, coming from domain wall motion, disappears above TC ≈ 650 K. The higher-frequency component slows down on heating towards TC, because it is the central mode, which drives the ferroelectric phase transition. Time-domain THz transmission and infrared reflectivity spectra reveal a mixture of polar phonons from both ferroelectric Nb-doped Pb(Zr,Ti)O3 (PZTN) and magnetic CoFe2O4 (CF) components, while the micro-Raman scattering spectra allow to study phonons from both components separately. Similar temperature behavior of phonons as in the pure PZTN and CF was observed. While in CoFe2O4 the Raman-active phonons gradually reduce their intensities on heating due to increasing conductivity and related reduced Raman-scattering volume, some phonons in PZTN disappear above TC due to change of selection rules in the paraelectric phase. Like in the pure Pb(Zr,Ti)O3, the soft phonon and central modes were also observed.

  14. Electron-phonon interaction in efficient perovskite blue emitters

    NASA Astrophysics Data System (ADS)

    Gong, Xiwen; Voznyy, Oleksandr; Jain, Ankit; Liu, Wenjia; Sabatini, Randy; Piontkowski, Zachary; Walters, Grant; Bappi, Golam; Nokhrin, Sergiy; Bushuyev, Oleksandr; Yuan, Mingjian; Comin, Riccardo; McCamant, David; Kelley, Shana O.; Sargent, Edward H.

    2018-06-01

    Low-dimensional perovskites have—in view of their high radiative recombination rates—shown great promise in achieving high luminescence brightness and colour saturation. Here we investigate the effect of electron-phonon interactions on the luminescence of single crystals of two-dimensional perovskites, showing that reducing these interactions can lead to bright blue emission in two-dimensional perovskites. Resonance Raman spectra and deformation potential analysis show that strong electron-phonon interactions result in fast non-radiative decay, and that this lowers the photoluminescence quantum yield (PLQY). Neutron scattering, solid-state NMR measurements of spin-lattice relaxation, density functional theory simulations and experimental atomic displacement measurements reveal that molecular motion is slowest, and rigidity greatest, in the brightest emitter. By varying the molecular configuration of the ligands, we show that a PLQY up to 79% and linewidth of 20 nm can be reached by controlling crystal rigidity and electron-phonon interactions. Designing crystal structures with electron-phonon interactions in mind offers a previously underexplored avenue to improve optoelectronic materials' performance.

  15. A MEMS Infrared Thermopile Fabricated from Silicon-On-Insulator with Phononic Crystal Structures and Carbon Nanotube Absorption Layer

    NASA Astrophysics Data System (ADS)

    Gray, Kory Forrest

    The goal of this project was to examine the possibility of creating a novel thermal infrared detector based on silicon CMOS technology that has been enhanced by the latest nano-engineering discoveries. Silicon typically is not thought as an efficient thermoelectric material. However recent advancements in nanotechnology have improved the potential for a highly sensitive infrared detector based on nano-structured silicon. The thermal conductivity of silicon has been shown to be reduced from 150 W/mK down to 60 W/mK just by decreasing the scale of the silicon from bulk down to the sub-micron scale. Further reduction of the thermal conductivity has been shown by patterning silicon with a phonon crystal structure which has been reported to have thermal conductivities down to 10 W/mK. The phonon crystal structure consists of a 2D array of holes that are etched into the silicon. The size and pitch of the holes are on the order of the mean free path of the phonons in silicon which is approximately 200-500nm. This particular device had 200nm holes on a 400nm pitch. The Seebeck coefficient of silicon can also be enhanced by the reduction of the material from the bulk to sub-micron scale and with degenerate level doping. The combination of decreased thermal conductivity and increased Seebeck coefficient allow silicon to be a promising material for thermoelectric infrared detectors. The highly doped silicon is desired to reduce the electrical resistance of the device. The low electrical resistance is required to reduce the Johnson noise of the device which is the dominant noise source for most thermal detectors. This project designed a MEMS thermopile using a silicon-on-insulator substrate, and a CMOS compatible process. The basic thermopile consists of a silicon dioxide membrane with phononic crystal patterned silicon thermocouples around the edges of the membrane. Vertical aligned, multi-walled, carbon nanotubes were used as the infrared absorption layer. A MEMS

  16. Evidence of superconductivity-induced phonon spectra renormalization in alkali-doped iron selenides

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Opačić, M.; Lazarević, N.; Šćepanović, M.

    2015-11-16

    Polarized Raman scattering spectra of superconducting K x Fe2-y Se2 and non-superconducting K0.8Fe1.8Co0.2Se2 single crystals were measured in the temperature range from 10 K up to 300 K. Two Raman active modes from the I4/mmm phase and seven from the I4/m phase are observed in the frequency range from 150 to 325 cm-1 in both compounds, suggesting that the K0.8Fe1.8Co0.2Se2 single crystal also has a two-phase nature. The temperature dependence of the Raman mode energy is analyzed in terms of lattice thermal expansion and phonon–phonon interaction. The temperature dependence of the Raman mode linewidth is dominated by temperature-induced anharmonic effects. It is shown that the change in Raman mode energy with temperature is dominantly driven by thermal expansion of the crystal lattice. An abrupt change of the A1g mode energy nearmore » $${{T}_{\\text{C}}}$$ was observed in K x Fe2-y Se2, whereas it is absent in non-superconducting K0.8Fe1.8Co0.2Se2. Phonon energy hardening at low temperatures in the superconducting sample is a consequence of superconductivity-induced redistribution of the electronic states below the critical temperature.« less

  17. Imaginary parts of coupled electron and phonon propagators

    NASA Astrophysics Data System (ADS)

    Schwartzman, K.; Lawrence, W. E.

    1988-01-01

    Quasiparticle and phonon damping rates due to the electron-phonon and Coulomb interactions are obtained directly from the self-energy formalism of strong-coupling theory. This accounts for all processes involving phonon or quasiparticle decay into a single particle-hole pair, or quasiparticle decay by emission or absorption of a single real phonon. The two quasiparticle decay modes are treated on a common footing, without ad hoc separation, by accounting fully for the dynamics of the phonon propagator and the Coulomb vertex-the latter by expansion of the four-point Coulomb vertex function. The results are shown to be expressible in terms of only the physical (i.e., fully renormalized) energies and coupling constants, and are written in terms of spectral functions such as α2F(ω) and its generalizations. Expansion of these in powers of a phonon linewidth parameter distinguishes (in lowest orders) between quasiparticle decay modes involving real and virtual phonons. However, the simplest prescription for calculating decay rates involves an effective scattering amplitude in which this distinction is not made.

  18. Nonbolometric bottleneck in electron-phonon relaxation in ultrathin WSi films

    NASA Astrophysics Data System (ADS)

    Sidorova, Mariia V.; Kozorezov, A. G.; Semenov, A. V.; Korneeva, Yu. P.; Mikhailov, M. Yu.; Devizenko, A. Yu.; Korneev, A. A.; Chulkova, G. M.; Goltsman, G. N.

    2018-05-01

    We developed the model of the internal phonon bottleneck to describe the energy exchange between the acoustically soft ultrathin metal film and acoustically rigid substrate. Discriminating phonons in the film into two groups, escaping and nonescaping, we show that electrons and nonescaping phonons may form a unified subsystem, which is cooled down only due to interactions with escaping phonons, either due to direct phonon conversion or indirect sequential interaction with an electronic system. Using an amplitude-modulated absorption of the sub-THz radiation technique, we studied electron-phonon relaxation in ultrathin disordered films of tungsten silicide. We found an experimental proof of the internal phonon bottleneck. The experiment and simulation based on the proposed model agree well, resulting in τe -ph˜14 0 -19 0 ps at TC=3.4 K , supporting the results of earlier measurements by independent techniques.

  19. Interlayer electron-phonon coupling in WSe2/hBN heterostructures

    NASA Astrophysics Data System (ADS)

    Jin, Chenhao; Kim, Jonghwan; Suh, Joonki; Shi, Zhiwen; Chen, Bin; Fan, Xi; Kam, Matthew; Watanabe, Kenji; Taniguchi, Takashi; Tongay, Sefaattin; Zettl, Alex; Wu, Junqiao; Wang, Feng

    2017-02-01

    Engineering layer-layer interactions provides a powerful way to realize novel and designable quantum phenomena in van der Waals heterostructures. Interlayer electron-electron interactions, for example, have enabled fascinating physics that is difficult to achieve in a single material, such as the Hofstadter's butterfly in graphene/boron nitride (hBN) heterostructures. In addition to electron-electron interactions, interlayer electron-phonon interactions allow for further control of the physical properties of van der Waals heterostructures. Here we report an interlayer electron-phonon interaction in WSe2/hBN heterostructures, where optically silent hBN phonons emerge in Raman spectra with strong intensities through resonant coupling to WSe2 electronic transitions. Excitation spectroscopy reveals the double-resonance nature of such enhancement, and identifies the two resonant states to be the A exciton transition of monolayer WSe2 and a new hybrid state present only in WSe2/hBN heterostructures. The observation of an interlayer electron-phonon interaction could open up new ways to engineer electrons and phonons for device applications.

  20. Effect of particle size and laser power on the Raman spectra of CuAlO2 delafossite nanoparticles

    NASA Astrophysics Data System (ADS)

    Yassin, O. A.; Alamri, S. N.; Joraid, A. A.

    2013-06-01

    A transparent conductive oxide CuAlO2 delafossite is studied using x-ray powder diffraction (XRD) and micro-Raman spectroscopy measurements as a function of the particle size and laser power from 2 to 20 mW. The XRD results indicate that the lattice parameters and the cell volume expand as the particle size reduces. Large red shifts (˜60 cm-1) and line broadening (˜50 cm-1) are observed as the particle size becomes of the order of 13 nm. These huge values can only be justified if collective effects on the Raman spectra created by the lattice expansion, confinement of phonons and enhanced phonon-phonon interactions are included in the interpretations of the Raman spectra of the CuAlO2 nanoparticles.

  1. Studies of Phonon Anharmonicity in Solids

    NASA Astrophysics Data System (ADS)

    Lan, Tian

    Today our understanding of the vibrational thermodynamics of materials at low temperatures is emerging nicely, based on the harmonic model in which phonons are independent. At high temperatures, however, this understanding must accommodate how phonons interact with other phonons or with other excitations. We shall see that the phonon-phonon interactions give rise to interesting coupling problems, and essentially modify the equilibrium and non-equilibrium properties of materials, e.g., thermodynamic stability, heat capacity, optical properties and thermal transport of materials. Despite its great importance, to date the anharmonic lattice dynamics is poorly understood and most studies on lattice dynamics still rely on the harmonic or quasiharmonic models. There have been very few studies on the pure phonon anharmonicity and phonon-phonon interactions. The work presented in this thesis is devoted to the development of experimental and computational methods on this subject. Modern inelastic scattering techniques with neutrons or photons are ideal for sorting out the anharmonic contribution. Analysis of the experimental data can generate vibrational spectra of the materials, i.e., their phonon densities of states or phonon dispersion relations. We obtained high quality data from laser Raman spectrometer, Fourier transform infrared spectrometer and inelastic neutron spectrometer. With accurate phonon spectra data, we obtained the energy shifts and lifetime broadenings of the interacting phonons, and the vibrational entropies of different materials. The understanding of them then relies on the development of the fundamental theories and the computational methods. We developed an efficient post-processor for analyzing the anharmonic vibrations from the molecular dynamics (MD) calculations. Currently, most first principles methods are not capable of dealing with strong anharmonicity, because the interactions of phonons are ignored at finite temperatures. Our method adopts

  2. Micro-Raman investigations of InN-GaN core-shell nanowires on Si (111) substrate

    NASA Astrophysics Data System (ADS)

    Sangeetha, P.; Jeganathan, K.; Ramakrishnan, V.

    2013-06-01

    The electron-phonon interactions in InN-GaN core-shell nanowires grown by plasma assisted- molecular beam epitaxy (MBE) on Si (111) substrate have been analysed using micro-Raman spectroscopic technique with the excitation wavelength of 633, 488 and 325 nm. The Raman scattering at 633 nm reveals the characteristic E2 (high) and A1 (LO) phonon mode of InN core at 490 and 590 cm-1 respectively and E2 (high) phonon mode of GaN shell at 573 cm-1. The free carrier concentration of InN core is found to be low in the order ˜ 1016 cm-3 due to the screening of charge carriers by thin GaN shell. Diameter of InN core evaluated using the spatial correlation model is consistent with the transmission electron microscopic measurement of ˜15 nm. The phonon-life time of core-shell nanowire structure is estimated to be ˜0.4 ps. The micro-Raman mapping and its corresponding localised spectra for 325 nm excitation exhibit intense E2 (high) phonon mode of GaN shell at 573 cm-1 as the decrease of laser interaction length and the signal intensity is quenched at the voids due to high spacing of NWs.

  3. "Anomalous" excitation in hydrogen-bonded molecular crystals - a Raman scattering study of specifically deuterated acetanilide (C 6D 5-CONH-CD 3)

    NASA Astrophysics Data System (ADS)

    Sauvajol, J. L.; De Nunzio, G.; Almairac, R.; Moret, J.; Barthés, M.; Bataillon, Place E.

    1991-01-01

    The focus of experimental and theoretical works about crystalline Acetanilide has been the "anomalous" temperature-dependent ir absorption and Raman peaks at about 1650 cm -1 and the multiband structure in the N-H stretch region. A lively discussion about the assignment of these "anomalous" bands has arisen and is still in progress. The present Raman experiments should be placed in this context as an attempt to identify the molecular degrees of freedom which originate the "anomalous" bands. In this aim Raman experiments have been performed on specifically deuterated Acetanilide [C 6D 5-CONH-CD 3] single crystal in the low-frequency (phonon) and C=O stretching regions. On cooling a distinct band at about 1495 cm -1 increases in intensity. We assign this peak to the equivalent of the 1650 cm -1 band in Acetanilide. The temperature dependence of this Raman line was studied. The results are discussed in the light of the models proposed to explain the anomalous behaviour of the 1650 cm -1 Raman line in Acetanilide.

  4. Strain mapping in single-layer two-dimensional crystals via Raman activity

    NASA Astrophysics Data System (ADS)

    Yagmurcukardes, M.; Bacaksiz, C.; Unsal, E.; Akbali, B.; Senger, R. T.; Sahin, H.

    2018-03-01

    By performing density functional theory-based ab initio calculations, Raman-active phonon modes of single-layer two-dimensional (2D) materials and the effect of in-plane biaxial strain on the peak frequencies and corresponding activities of the Raman-active modes are calculated. Our findings confirm the Raman spectrum of the unstrained 2D crystals and provide expected variations in the Raman-active modes of the crystals under in-plane biaxial strain. The results are summarized as follows: (i) frequencies of the phonon modes soften (harden) under applied tensile (compressive) strains; (ii) the response of the Raman activities to applied strain for the in-plane and out-of-plane vibrational modes have opposite trends, thus, the built-in strains in the materials can be monitored by tracking the relative activities of those modes; (iii) in particular, the A peak in single-layer Si and Ge disappears under a critical tensile strain; (iv) especially in mono- and diatomic single layers, the shift of the peak frequencies is a stronger indication of the strain rather than the change in Raman activities; (v) Raman-active modes of single-layer ReX2 (X =S , Se) are almost irresponsive to the applied strain. Strain-induced modifications in the Raman spectrum of 2D materials in terms of the peak positions and the relative Raman activities of the modes could be a convenient tool for characterization.

  5. Direct Observation of Electron-Phonon Coupling and Slow Vibrational Relaxation in Organic-Inorganic Hybrid Perovskites.

    PubMed

    Straus, Daniel B; Hurtado Parra, Sebastian; Iotov, Natasha; Gebhardt, Julian; Rappe, Andrew M; Subotnik, Joseph E; Kikkawa, James M; Kagan, Cherie R

    2016-10-05

    Quantum and dielectric confinement effects in 2D hybrid perovskites create excitons with a binding energy exceeding 150 meV. We exploit the large exciton binding energy to study exciton and carrier dynamics as well as electron-phonon coupling in hybrid perovskites using absorption and photoluminescence (PL) spectroscopies. At temperatures below 75 K, we resolve splitting of the excitonic absorption and PL into multiple regularly-spaced resonances every 40-46 meV, consistent with electron-phonon coupling to phonons located on the organic cation. We also resolve resonances with a 14 meV spacing, in accord with coupling to phonons with mixed organic and inorganic character, and these assignments are supported by density-functional theory calculations. Hot exciton PL and time-resolved PL measurements show that vibrational relaxation occurs on a picosecond timescale competitive with that for PL. At temperatures above 75 K, excitonic absorption and PL exhibit homogeneous broadening. While absorption remains homogeneous, PL becomes inhomogeneous below 75K, which we speculate is caused by the formation and subsequent dynamics of a polaronic exciton.

  6. Conservation law of angular momentum in helicity-dependent Raman and Rayleigh scattering

    NASA Astrophysics Data System (ADS)

    Tatsumi, Yuki; Kaneko, Tomoaki; Saito, Riichiro

    2018-05-01

    In first-order Raman scattering, helicity of circularly polarized incident light is either conserved or changed depending on the Raman modes. When the helicity of incident light changes in the scattered light, the angular momentum of a photon is transferred to the material. Here, we present the conservation law of pseudoangular momentum in the helicity-dependent Raman scattering for a N -fold (N =1 -4 ,6 ) rotational symmetry of a crystal. Furthermore, the conservation law of electron-phonon interaction is discussed by considering the vibration direction of a phonon that has the same or lower symmetry than the symmetry of the crystal, which is essential to allow the helicity change in Raman scattering in a highly symmetric material, such as graphene. We also discuss the conservation law of pseudoangular momentum in Rayleigh scattering and show that the helicity change is allowed only in the crystal with one- or twofold rotational symmetry.

  7. Structure, phonons and related properties in zinc-IV-nitride (IV = silicon, germanium, tin), scandium nitride, and rare-earth nitrides

    NASA Astrophysics Data System (ADS)

    Paudel, Tula R.

    This thesis presents a study of the phonons and related properties in two sets of nitride compounds, whose properties are until now relatively poorly known. The Zn-IV-N2 group of compounds with the group IV elements Si, Ge and Sn, form a series analogous to the well known III-N nitride series with group III element Al, Ga, In. Structurally, they can be derived by doubling the period of III-V compounds in the plane in two directions and replacing the group-III elements with Zn and a group-IV element in a particular ordered pattern. Even though they are similar to the well-known III-V nitride compounds, the study of the properties of these materials is in its early stages. The phonons in these materials and their relation to the phonons in the corresponding group-III nitrides are of fundamental interest. They are also of practical interest because the phonon related spectra such as infrared absorption and Raman spectroscopy are sensitive to the structural quality of the material and can thus be used to quantify the degree of crystalline perfection of real samples. First-principles calculations of the phonons and related ground state properties of these compounds were carried out using Density Functional Perturbation Theory (DFPT) with the Local Density Approximation (LDA) for exchange and correlation and using a pseudopotential plane wave implementation which was developed by several authors over the last decades. The main focus of our study is on the phonons at the center of the Brillouin zone because the latter are most directly related to commonly used spectroscopies to probe the vibrations in a solid: infrared reflectivity and Raman spectroscopy. For a semiconducting or insulating compound, a splitting occurs between transverse and longitudinal phonons at the Gamma-point because of the long-range nature of electrostatic forces. The concepts required to handle this problem are reviewed. Our discussion emphasizes how the various quantities required are related to

  8. Phonon Spectrum in Hydroxyapatite: Calculations and EPR Study at Low Temperatures

    NASA Astrophysics Data System (ADS)

    Biktagirov, Timur; Gafurov, Marat; Iskhakova, Kamila; Mamin, Georgy; Orlinskii, Sergei

    2016-12-01

    Density functional theory-based calculations within the framework of the plane-wave pseudopotential approach are carried out to define the phonon spectrum of hydroxyapatite Ca_{10}(PO4)6(OH)2 (HAp). It allows to describe the temperature dependence of the electronic spin-lattice relaxation time T_{1e} of the radiation-induced stable radical NO3^{2-} in HAp, which was measured in X-band (9 GHz, magnetic field strength of 0.34 T) in the temperature range T = (10-300) K. It is shown that the temperature behavior of T_{1e} at T> 20 K can be fitted via two-phonon Raman type processes with the Debye temperature Θ D ≈ 280 {K} evaluated from the phonon spectrum.

  9. Raman spectroscopy and atomic force microscopy study of interfacial polytypism in GaP/Ge(111) heterostructures

    NASA Astrophysics Data System (ADS)

    Aggarwal, R.; Ingale, Alka A.; Dixit, V. K.

    2018-01-01

    Effects of lattice and polar/nonpolar mismatch between the GaP layer and Ge(111) substrate are investigated by spatially resolved Raman spectroscopy. The red shifted transverse optical (TO) and longitudinal optical (LO) phonons due to residual strain, along with asymmetry to TO phonon ∼358 cm-1 are observed in GaP/Ge(111). The peak intensity variation of mode ∼358 cm-1 with respect to TO phonon across the crystallographic morphed surface of GaP micro structures is associated with the topographical variations using atomic force microscopy mapping and Raman spectroscopy performed on both in plane and cross-sectional surface. Co-existence of GaP allotropes, i.e. wurtzite phase near heterojunction interface and dominant zinc-blende phase near surface is established using the spatially resolved polarized Raman spectroscopy from the cross sectional surface of heterostructures. This consistently explains effect of surface morphology on Raman spectroscopy from GaP(111). The study shows the way to identify crystalline phases in other advanced semiconductor heterostructures without any specific sample preparation.

  10. Simulation of Phonon Spectra in Three-Component Two-Dimensional Crystals of Refractory-Metal Dichalcogenides

    NASA Astrophysics Data System (ADS)

    Alexeev, A. Yu.; Krivosheeva, A. V.; Shaposhnikov, V. L.; Borisenko, V. E.

    2017-09-01

    A model for ab initio calculation of the phonon properties of three-component solid solutions of refractory-metal dichalcogenides was developed based on the assumption that displacements of the same type of chalcogen atoms and decoupled displacements of the metal atoms were identical. The calculated phonon frequencies at the Γ-point for monomolecular layers of MoS2-xSex and MoS2-xTex agreed with existing experimental Raman spectra.

  11. Raman scattering spectra of superconducting Bi2Sr2CaCu2O8 single crystals

    NASA Astrophysics Data System (ADS)

    Kirillov, D.; Bozovic, I.; Geballe, T. H.; Kapitulnik, A.; Mitzi, D. B.

    1988-12-01

    Raman spectra of Bi2Sr2CaCu2O8 single crystals with superconducting phase-transition temperature of 90 K have been studied. The spectra contained phonon lines and electronic continuum. Phonon energies and polarization selection rules were measured. A gap in the electronic continuum spectrum was observed in a superconducting state. Noticeable similarity between Raman spectra of Bi2Sr2CaCu2O8 and YBa2Cu3O7 was found.

  12. Layer-dependent second-order Raman intensity of Mo S2 and WS e2 : Influence of intervalley scattering

    NASA Astrophysics Data System (ADS)

    Qian, Qingkai; Zhang, Zhaofu; Chen, Kevin J.

    2018-04-01

    Acoustic-phonon Raman scattering, as a defect-induced second-order Raman scattering process (with incident photon scattered by one acoustic phonon at the Brillouin-zone edge and the momentum conservation fulfilled by defect scattering), is used as a sensitive tool to study the defects of transition-metal dichalcogenides (TMDs). Moreover, second-order Raman scattering processes are closely related to the valley depolarization of single-layer TMDs in potential valleytronic applications. Here, the layer dependence of second-order Raman intensity of Mo S2 and WS e2 is studied. The electronic band structures of Mo S2 and WS e2 are modified by the layer thicknesses; hence, the resonance conditions for both first-order and second-order Raman scattering processes are tuned. In contrast to the first-order Raman scattering, second-order Raman scattering of Mo S2 and WS e2 involves additional intervalley scattering of electrons by phonons with large momenta. As a result, the electron states that contribute most to the second-order Raman intensity are different from that to first-order process. A weaker layer-tuned resonance enhancement of second-order Raman intensity is observed for both Mo S2 and WS e2 . Specifically, when the incident laser has photon energy close to the optical band gap and the Raman spectra are normalized by the first-order Raman peaks, single-layer Mo S2 or WS e2 has the strongest second-order Raman intensity. This layer-dependent second-order Raman intensity can be further utilized as an indicator to identify the layer number of Mo S2 and WS e2 .

  13. Monitoring electrostatically-induced deflection, strain and doping in suspended graphene using Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Metten, Dominik; Froehlicher, Guillaume; Berciaud, Stéphane

    2017-03-01

    Electrostatic gating offers elegant ways to simultaneously strain and dope atomically thin membranes. Here, we report on a detailed in situ Raman scattering study on graphene, suspended over a Si/SiO2 substrate. In such a layered structure, the intensity of the Raman G- and 2D-mode features of graphene are strongly modulated by optical interference effects and allow an accurate determination of the electrostatically-induced membrane deflection, up to irreversible collapse. The membrane deflection is successfully described by an electromechanical model, which we also use to provide useful guidelines for device engineering. In addition, electrostatically-induced tensile strain is determined by examining the softening of the Raman features. Due to a small residual charge inhomogeneity, we find that non-adiabatic anomalous phonon softening is negligible compared to strain-induced phonon softening. These results open perspectives for innovative Raman scattering-based readout schemes in two-dimensional nanoresonators.

  14. Scattering of phonons by dislocations

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Anderson, A. C.

    1979-01-01

    By 1950, an explicit effort had been launched to use lattice thermal conductivity measurements in the investigation of defect structures in solids. This technique has been highly successful, especially when combined with the measurements of other properties such as optical absorption. One exception has been the study of dislocations. Although dislocations have a profound effect on the phonon thermal conductivity, the mechanisms of the phonon-dislocation interaction are poorly understood. The most basic questions are still debated in the literature. It therefore is pointless to attempt a quantitative comparison between an extensive accumulation of experimental data on the one hand, andmore » the numerous theoretical models on the other. Instead, this chapter will attempt to glean a few qualitative conclusions from the existing experimental data. These results will then be compared with two general models which incorporate, in a qualitative manner, most of the proposed theories of the phonon-dislocation interaction. Until very recently, measurement of thermal conductivity was the only means available to probe the interaction between phonons and defects at phonon frequencies above the standard ultrasonic range of approx. = 10/sup 9/ Hz. The introductory paragraphs provide a brief review of the thermal-conductivity technique and the problems which are encountered in practice. There is also a brief presentation of the theoretical models and the complications that may occur in more realistic situations.« less

  15. Differential absorption and Raman lidar for water vapor profile measurements - A review

    NASA Technical Reports Server (NTRS)

    Grant, William B.

    1991-01-01

    Differential absorption lidar and Raman lidar have been applied to the range-resolved measurements of water vapor density for more than 20 years. Results have been obtained using both lidar techniques that have led to improved understanding of water vapor distributions in the atmosphere. This paper reviews the theory of the measurements, including the sources of systematic and random error; the progress in lidar technology and techniques during that period, including a brief look at some of the lidar systems in development or proposed; and the steps being taken to improve such lidar systems.

  16. Spin-phonon coupling in BaFe{sub 12}O{sub 19} M-type hexaferrite

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Silva Júnior, Flávio M.; Paschoal, Carlos W. A., E-mail: paschoal.william@gmail.com

    2014-12-28

    The spin-phonon coupling in magnetic materials is due to the modulation of the exchange integral by lattice vibrations. BaFe{sub 12}O{sub 19} M-type hexaferrite, which is the most used magnetic material as permanent magnet, transforms into ferrimagnet at high temperatures, but no spin-phonon coupling was previously observed at this transition. In this letter, we investigated the temperature-dependent Raman spectra of polycrystalline BaFe{sub 12}O{sub 19} M-type hexaferrite from room temperature up to 780 K to probe spin-phonon coupling at the ferrimagnetic transition. An anomaly was observed in the position of the phonon attributed to the Fe{sup (4)}O{sub 6}, Fe{sup (5)}O{sub 6}, and Fe{supmore » (1)}O{sub 6} octahedra, evidencing the presence of a spin-phonon coupling in BaM in the ferrimagnetic transition at 720 K. The results also confirmed the spin-phonon coupling is different for each phonon even when they couple with the same spin configuration.« less

  17. Influence of polarity of solvents on IR absorption and Raman spectra of ascorbic acid

    NASA Astrophysics Data System (ADS)

    Kutsenko, S. A.; Danyaeva, Y. S.; Maximova, S. V.

    2018-04-01

    The results of numerical calculations of IR absorption and Raman spectra of ascorbic acid in polar and nonpolar solutions are presented. The dependence of the change in the total energy and the dipole moment of the molecule on the characteristics of the solvents was investigated using the two solvation models. Spectral bands and the corresponding structural groups of the molecule are found, the characteristics of which are most vulnerable to solvents.

  18. Combination of surface- and interference-enhanced Raman scattering by CuS nanocrystals on nanopatterned Au structures

    PubMed Central

    Yeryukov, Nikolay A; Sveshnikova, Larisa L; Duda, Tatyana A; Rodyakina, Ekaterina E; Gridchin, Victor A; Sheremet, Evgeniya S; Zahn, Dietrich R T

    2015-01-01

    Summary We present the results of a Raman study of optical phonons in CuS nanocrystals (NCs) with a low areal density fabricated through the Langmuir–Blodgett technology on nanopatterned Au nanocluster arrays using a combination of surface- and interference-enhanced Raman scattering (SERS and IERS, respectively). Micro-Raman spectra of one monolayer of CuS NCs deposited on a bare Si substrate reveal only features corresponding to crystalline Si. However, a new relatively strong peak occurs in the Raman spectrum of CuS NCs on Au nanocluster arrays at 474 cm−1. This feature is related to the optical phonon mode in CuS NCs and manifests the SERS effect. For CuS NCs deposited on a SiO2 layer this phonon mode is also observed due to the IERS effect. Its intensity changes periodically with increasing SiO2 layer thickness for different laser excitation lines and is enhanced by a factor of about 30. CuS NCs formed on Au nanocluster arrays fabricated on IERS substrates combine the advantages of SERS and IERS and demonstrate stronger SERS enhancement allowing for the observation of Raman signals from CuS NCs with an ultra-low areal density. PMID:25977845

  19. Dispersion of folded phonons in {Si}/{Si xGe1- x} superlattices

    NASA Astrophysics Data System (ADS)

    Brugger, H.; Reiner, H.; Abstreiter, G.; Jorke, H.; Herzog, H. J.; Kasper, E.

    Zone folding effects on acoustic phonons in {Si}/{Si xGe1- x} strained layer superlattices are studied by Raman spectroscopy. A quantitative explanation of the measured frequencies is given in terms of the elastic continuum theory. The scattering wavevector q s is varied by use of different laser lines to probe directly the phonon dispersion curve in the superlattices. For large period samples q s can be shifted through the new Brillouin zone boundary. We report on observation of a finite doublet splitting corresponding to the first zone-edge gap.

  20. Dephasing of LO-phonon-plasmon hybrid modes in n-type GaAs

    NASA Astrophysics Data System (ADS)

    Vallée, F.; Ganikhanov, F.; Bogani, F.

    1997-11-01

    The relaxation dynamics of coherent phononlike LO-phonon-plasmon hybrid modes is investigated in n-doped GaAs using an infrared time-resolved coherent anti-Stokes Raman scattering technique. Measurements performed for different crystal temperatures in the range 10-300 K as a function of the electron density injected by doping show a large reduction of the hybrid mode dephasing time compared to the bare LO-phonon one for densities larger than 1016 cm-3. The results are interpreted in terms of coherent decay of the LO-phonon-plasmon mixed mode in the weak-coupling regime and yield information on the plasmon and electron relaxation. The estimated average electron momentum relaxation times are smaller than those deduced from Hall mobility measurements, as expected from our theoretical model.

  1. Enhanced Raman Scattering from InSb Nanodots; Temperature and Laser-Power Dependent Studies

    NASA Astrophysics Data System (ADS)

    Wada, Noboru; Takayama, Haruki; Morohashi, Satoshi

    2010-03-01

    InSb nanodots were uniquely fabricated by vapor-transport on a Si substrate which had previously been bombarded by FBI Ga ions. The InSb nanodots were then examined by spatially-resolved Raman scattering using an Ar-ion laser (λ= 514.5 and 488 nm with P=1˜15 mW) with an optical microscope and CCD detector. In addition to the TO and LO peaks of InSb observed at ˜180 and 191 cm-1 respectively, two peaks were observed at ˜110 and 150 cm-1. Those Raman peaks were tentatively attributed to the 2TA and TO-TA second-order Raman processes. Those two peak intensities appeared to grow at the expense of the TO and LO Raman peak intensities with increasing the sample temperature from 10 K to 450 K. Also, the two-phonon peak intensities increased non-linearly with the probing laser power used. Hot carriers and their interactions with phonons in the restricted regions will be discussed together with Raman scattering results obtained from single-crystal InSb.

  2. Raman and Brillouin scattering studies of bulk 2H-WSe2

    NASA Astrophysics Data System (ADS)

    Akintola, K.; Andrews, G. T.; Curnoe, S. H.; Koehler, M. R.; Keppens, V.

    2015-10-01

    Raman and Brillouin spectroscopy were used to probe optic and acoustic phonons in bulk 2H-WSe2. Raman spectra collected under different polarization conditions allowed assignment of spectral peaks to various first- and second-order processes. In contrast to some previous studies, a Raman peak at  ˜259 cm-1was found not to be due to the A1g mode but to a second-order process involving phonons at either the M or K point of the Brillouin zone. Resonance effects due to excitons were also observed in the Raman spectra. Brillouin spectra of 2H-WSe2 contain a single peak doublet arising from a Rayleigh surface mode propagating with a velocity of 1340+/- 20 m s-1. This value is comparable to that estimated from Density Functional Theory calculations and also to those for the transition metal diselenides 2H-TaSe2 and 2H-NbSe2. Unlike these two materials, however, peaks arising from scattering via the elasto-optic mechanism were not observed in Brillouin spectra of WSe2 despite its lower opacity.

  3. Molecular Solid EOS based on Quasi-Harmonic Oscillator approximation for phonons

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Menikoff, Ralph

    2014-09-02

    A complete equation of state (EOS) for a molecular solid is derived utilizing a Helmholtz free energy. Assuming that the solid is nonconducting, phonon excitations dominate the specific heat. Phonons are approximated as independent quasi-harmonic oscillators with vibrational frequencies depending on the specific volume. The model is suitable for calibrating an EOS based on isothermal compression data and infrared/Raman spectroscopy data from high pressure measurements utilizing a diamond anvil cell. In contrast to a Mie-Gruneisen EOS developed for an atomic solid, the specific heat and Gruneisen coefficient depend on both density and temperature.

  4. Alcohol-catalyzed photoreduction of iron-porphyrin complexes revealed by resonance raman and absorption spectroscopies

    NASA Astrophysics Data System (ADS)

    Ogura, T.; Fidler, V.; Ozaki, Y.; Kitagawa, T.

    1990-06-01

    Photoreduction of Fe III(OEP) (2-MeIm) (OEP is octaethylporphyrin; 2-MeIm is 2-methylimidazole) was found to be catalyzed by a trace amount of MeOH present in Ch 2Cl 2 as a stabilizer. The absence of either 2-MeIm or MeOH in the CH 2Cl 2 solution of Fe III(OEP) X (X is Cl -, Br - or I -) leads to no photoreduction. The presence of MeOH in the Fe III(OEP) (2-MeIm) solution results in the appearance of a new absorption band at 585 nm, and when Raman scattering was excited at 590 nm, a new Raman band appeared at 524 cm -. This band exhibited an upshift by 4 cm - with 54Fe(OEP) (2-MeIm)(CH 3OH) and a downshift by 12 cm -1 with 56Fe(OEP)(2-MeIm) (CD 3OD) and was therefore assigned to the Fe III-MeOH stretching vibration. The excitation profile of this band gave a peak around 585 nm and accordingly, the new absorption band at 584 nm was assigned to a charge-transfer (CT) band from MeOH to the Fe III ion. It was most unexpected that the photoreduction did not occur upon laser illumination within the CT band.

  5. Raman scattering of rare earth hexaborides

    NASA Astrophysics Data System (ADS)

    Ogita, Norio; Hasegawa, Takumi; Udagawa, Masayuki; Iga, Fumitoshi; Kunii, Satoru

    2009-06-01

    Raman scattering spectra were measured for the rare-earth hexaborides RB6 (R = Ce, Gd, or Dy). All Raman-active phonons due to B6 vibrations were observed in the range 600 - 1400 cm-1. Anomalous peaks were detected below 200 cm-1, which correspond to vibrations of rare-earth ion excited by second-order Raman scattering process. The intensity and energy of the rare-earth mode decrease with decreasing temperature. This suggests that the rare-earth ion vibrates in a shallow and anharmonic potential due to the boron cage. Using the reported values of mean square displacement of rare-earth ion, we estimated the anharmonic contribution for the rare-earth vibrations.

  6. Phonons, defects and optical damage in crystalline acetanilide

    NASA Astrophysics Data System (ADS)

    Kosic, Thomas J.; Hill, Jeffrey R.; Dlott, Dana D.

    1986-04-01

    Intense picosecond pulses cause accumulated optical damage in acetanilide crystals at low temperature. Catastrophic damage to the irradiated volume occurs after an incubation period where defects accumulate. The optical damage is monitored with subanosecond time resolution. The generation of defects is studied with damage-detected picosecond spectroscopy. The accumulation of defects is studied by time-resolved coherent Raman scattering, which is used to measure optical phonon scattering from the accumulating defects.

  7. Phonon properties and slow organic-to-inorganic sub-lattice thermalization in hybrid perovskites

    NASA Astrophysics Data System (ADS)

    Chan, Maria; Chang, Angela; Xia, Yi; Sadasivam, Sridhar; Guo, Peijun; Kinaci, Alper; Lin, Hao-Wu; Darancet, Pierre; Schaller, Richard

    Organic-inorganic hybrid perovskite halide compounds have been investigated extensively for photovoltaics (PVs) and related applications. The thermal transport properties of hybrid perovskites, including phonon-carrier and phonon-phonon interactions, are of significance for their PV and solar thermoelectric applications. The interlocking organic and inorganic sublattices can be thought of as an extreme form of nanostructuring. A result of this nanostructuring is the large gap in phonon frequencies between the organic and inorganic sublattices, which is expected to create bottlenecks in phonon equilibration. In this work, we use a combination of ultrafast spectroscopy including photoluminescence and transient absorption, as well as first principles density functional theory (DFT), ab initio molecular dynamics calculations, phonon lifetimes derived from DFT force constants, and non-equilibrium phonon dynamics accounting for phonon lifetimes, to determine the phonon and charge interaction processes. We find evidence that thermalization of carriers occur at an atypically slow 50-100 ps time scale owing to the complex interplay between electronic and phonon excitations.

  8. Potential drug - nanosensor conjugates: Raman, infrared absorption, surface - enhanced Raman, and density functional theory investigations of indolic molecules

    NASA Astrophysics Data System (ADS)

    Pięta, Ewa; Paluszkiewicz, Czesława; Oćwieja, Magdalena; Kwiatek, Wojciech M.

    2017-05-01

    An extremely important aspect of planning cancer treatment is not only the drug efficiency but also a number of challenges associated with the side effects and control of this process. That is why it is worth paying attention to the promising potential of the gold nanoparticles combined with a compound treated as a potential drug. This work presents Raman (RS), infrared absorption (IR) and surface-enhanced Raman scattering (SERS) spectroscopic investigations of N-acetyl-5-methoxytryptamine (melatonin) and α-methyl-DL-tryptophan, regarding as anti breast cancer agents. The experimental spectroscopic analysis was supported by the quantum-chemical calculations based on the B3LYP hybrid density functional theory (DFT) at the B3LYP 6-311G(d,p) level of theory. The studied compounds were adsorbed onto two colloidal gold nanosensors synthesized by a chemical reduction method using sodium borohydride (SB) and trisodium citrate (TC), respectively. Its morphology characteristics were obtained using transmission electron microscopy (TEM). It has been suggested that the NH moiety from the aromatic ring, a well-known proton donor, causes the formation of hydrogen bonds with the negatively charged gold surface.

  9. Raman mapping probing of tip-induced anomalous polarization behavior in V2O5 waveguiding nanoribbons

    NASA Astrophysics Data System (ADS)

    Yan, Bin; Du, Chaoling; Liao, Lei; You, Yumeng; Cheng, Hao; Shen, Zexiang; Yu, Ting

    2010-02-01

    Spatially resolved and polarized micro-Raman spectroscopy has been performed on individual V2O5 waveguiding nanoribbons. The experimental results establish that the Raman-antenna patterns are strongly correlated with the local positions of the sample, which gives rise to a pronounced intensity contrast in the polarized mapping for certain phonon modes. The suppressed phonon signals at the body of a ribbon can be enhanced at the end facets, resulting from the effective waveguiding propagation along the nanoribbon and strong local electric field intensity at the ends. The phenomena reported here, in addition to providing insight into the tip effects on optoelectronic nanodevices, will facilitate the rational design of Raman detection in nanostructures.

  10. Statistical Fine Structure in Inhomogeneously Broadened Absorption Lines in Solids.

    DTIC Science & Technology

    1987-12-22

    the inhomogeneously broadened zero-phonon SijSo (0-0) absorption of pentacene molecules in crystals of p-terphenyl at liquid helium temperatures. SFS...structure (SFS) in the inhomogeneously broadened zero-phonon S, +- So (0-0) absorption of pentacene molecules in crystals of p-terphenyl at liquid helium...tile large multiplicity of local environments. Inhomogeneously broadened absorption lines are usually treated as smooth, Gaussian profiles. In recent

  11. Multiphonon Raman scattering and photoluminescence studies of CdS nanocrystals grown by thermal evaporation

    NASA Astrophysics Data System (ADS)

    Farid, Sidra; Stroscio, Michael A.; Dutta, Mitra

    2018-03-01

    Thermal evaporation growth technique is presented as a route to grow cost effective high quality CdS thin films. We have successfully grown high quality CdS thin films on ITO coated glass substrates by thermal evaporation technique and analyzed the effects of annealing and excitation dependent input of CdS thin film using Raman and photoluminescence spectroscopy. LO phonon modes have been analyzed quantitatively considering the contributions due to anneal induced effects on film quality using phonon spatial correlation model, line shape and defect state analysis. Asymmetry in the Raman line shape towards the low frequency side is related to the phonon confinement effects and is modeled by spatial correlation model. Calculations of width (FWHM), integrated intensity, and line shape for the longitudinal (LO) optical phonon modes indicate improved crystalline quality for the annealed films as compared to the as grown films. With increase in laser power, intensity ratio of 2-LO to 1-LO optical phonon modes is found to increase while multiple overtones upto fourth order are observed. Power dependent photoluminescence data indicates direct band-to-band transition in CdS thin films.

  12. Phonon renormalization and anharmonicity in Al-doped MgB2

    NASA Astrophysics Data System (ADS)

    Ortiz, Filiberto; Aguayo, Aarón

    2005-03-01

    We have studied the evolution of the E2g phonon mode dynamics in Mg1-xAlxB2 as a function of doping using the Frozen Phonon Approximation (FPA). The doping was modeled in the ab-initio Virtual Crystal Approximation (VCA). The results were obtained by means of first-principles total-energy calculations using the full potential Linearized Augmented Plane Wave (LAPW) method and the Generalized Gradient Approximation (GGA) for the exchange-correlation potential. We present results for the evolution of the phonon frequency and anharmonicity of the E2g mode as a function of Al concentration (x). From a comparison of the experimental data with the calculated E2g phonon frequency we show that the VCA-FPA reproduces the observed phonon renormalization in the whole range of Al concentrations. More interestingly, we find that the anharmonicity gradually decreases with Al doping and vanishes for x(Al)>0.5, that behaviour correlates with the evolution of the measured Raman linewidth in Al-doped MgB2. The significance of these results are discussed in the light of the experimentally observed loss of superconductivity in Mg1- xAlxB2.This work was supported by Consejo Nacional de Ciencia y Tecnolog'ia (CONACYT, M'exico) under Grant. No. 43830-F.

  13. Temperature-Dependent Thermal Boundary Conductance of Monolayer MoS 2 by Raman Thermometry

    DOE PAGES

    Yalon, Eilam; Aslan, Ozgur Burak; Smithe, Kirby K. H.; ...

    2017-10-20

    The electrical and thermal behavior of nanoscale devices based on two-dimensional (2D) materials is often limited by their contacts and interfaces. Here we report the temperature-dependent thermal boundary conductance (TBC) of monolayer MoS 2 with AlN and SiO 2, using Raman thermometry with laser-induced heating. The temperature-dependent optical absorption of the 2D material is crucial in such experiments, which we characterize here for the first time above room temperature. We obtain TBC ~ 15 MW m –2 K –1 near room temperature, increasing as ~ T 0.65 in the range 300–600 K. The similar TBC of MoS 2 with themore » two substrates indicates that MoS 2 is the “softer” material with weaker phonon irradiance, and the relatively low TBC signifies that such interfaces present a key bottleneck in energy dissipation from 2D devices. As a result, our approach is needed to correctly perform Raman thermometry of 2D materials, and our findings are key for understanding energy coupling at the nanoscale.« less

  14. Temperature-Dependent Thermal Boundary Conductance of Monolayer MoS 2 by Raman Thermometry

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Yalon, Eilam; Aslan, Ozgur Burak; Smithe, Kirby K. H.

    The electrical and thermal behavior of nanoscale devices based on two-dimensional (2D) materials is often limited by their contacts and interfaces. Here we report the temperature-dependent thermal boundary conductance (TBC) of monolayer MoS 2 with AlN and SiO 2, using Raman thermometry with laser-induced heating. The temperature-dependent optical absorption of the 2D material is crucial in such experiments, which we characterize here for the first time above room temperature. We obtain TBC ~ 15 MW m –2 K –1 near room temperature, increasing as ~ T 0.65 in the range 300–600 K. The similar TBC of MoS 2 with themore » two substrates indicates that MoS 2 is the “softer” material with weaker phonon irradiance, and the relatively low TBC signifies that such interfaces present a key bottleneck in energy dissipation from 2D devices. As a result, our approach is needed to correctly perform Raman thermometry of 2D materials, and our findings are key for understanding energy coupling at the nanoscale.« less

  15. Line width resonance of the longitudinal optical phonon in GaAs:N

    NASA Astrophysics Data System (ADS)

    Mialitsin, Aleksej; Mascarenhas, Angelo

    2013-03-01

    We extend resonant Raman scattering studies of Mascarenhas et al. [PRB68, 233201 (2003)] of GaAs1-xNx to the ultra-dilute nitrogen doping concentrations, whereby we unambiguously resolve the line width resonances of the LO phonon. A discontinuity is observed in the LO phonon line width resonance energy as a function of concentration. With decreasing nitrogen concentration the EW line width resonance energy reduces by ca. 40 meV at x = 0 . 4 % . This value corresponds to the concentration, at which the localized to delocalized transition manifests itself in the electro-reflectance signature line widths.

  16. Anharmonicities in phonon combinations and overtones in bilayered graphene: A temperature-dependent approach

    NASA Astrophysics Data System (ADS)

    Araujo, P. T.

    2018-05-01

    This paper studies phonon anharmonicities related to the phonon combination LOZO' and phonon overtone 2ZO in a A B -stacked bilayer graphene (2LG). The results explain in detail the rule of the ZO' layer breathing mode in the 2LG electron and phonon relaxations, especially at temperatures above 543 K, where anomalous behaviors are observed for the LOZO' frequencies, linewidths (and therefore, lifetimes), and integrated areas. Surprisingly, the 2ZO frequencies and linewidths do not show any dependence with temperature (ZO is the out-of-phase vibration of the layers). This result is explained via nonsymmetric lattice distortions and via the almost null Gr üneisen parameter associated to the ZO mode. Recently, the correct assignments for the phonon combination and overtone modes studied here have been put in debate once again in a theoretical work by Popov [Carbon 91, 436 (2015), 10.1016/j.carbon.2015.05.020]. This work shows how temperature-dependent Raman spectroscopy is used to propose a solution for these recent assignment problems. Finally, although 2LG is the system used here, the measurements and discussions to approach electron and phonon relaxations have the potential to be extended to any other multilayered structure that presents ZO'- and ZO-like phonon modes.

  17. The effect of external magnetic field on the Raman peaks in manganites

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Sahu, A. K., E-mail: ajitsahu@seemantaengg.ac.in; Rout, G. C.

    2014-04-24

    We report here a microscopic theoretical model study exhibiting the effect of external magnetic field on the Raman excitation peaks in the CMR manganite system. The Hamiltonian consists of Jahn-Teller (J-T) distortion in e{sub g} band, the double exchange interaction and the Heisenberg spin-spin interaction. Further the phonons are coupled to e{sub g} band electrons, J-T distorted e{sub g} band and the double exchange interaction. The Raman spectral intensity is calculated from the imaginary part of the phonon Green function. The spectra exhibits three peaks besides a very weak high energy peak. The magnetic field effect on these peaks aremore » reported.« less

  18. Spin Qubits in Germanium Structures with Phononic Gap

    NASA Technical Reports Server (NTRS)

    Smelyanskiy, V. N.; Vasko, F. T.; Hafiychuk, V. V.; Dykman, M. I.; Petukhov, A. G.

    2014-01-01

    We propose qubits based on shallow donor electron spins in germanium structures with phononic gap. We consider a phononic crystal formed by periodic holes in Ge plate or a rigid cover / Ge layer / rigid substrate structure with gaps approximately a few GHz. The spin relaxation is suppressed dramatically, if the Zeeman frequency omegaZ is in the phononic gap, but an effective coupling between the spins of remote donors via exchange of virtual phonons remains essential. If omegaZ approaches to a gap edge in these structures, a long-range (limited by detuning of omegaZ) resonant exchange interaction takes place. We estimate that ratio of the exchange integral to the longitudinal relaxation rate exceeds 10(exp 5) and lateral scale of resonant exchange 0.1 mm. The exchange contribution can be verified under microwave pumping through oscillations of spin echo signal or through the differential absorption measurements. Efficient manipulation of spins due to the Rabi oscillations opens a new way for quantum information applications.

  19. Intrinsic phonon properties of double-walled carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Tran, H. N.; Levshov, D. I.; Nguyen, V. C.; Paillet, M.; Arenal, R.; Than, X. T.; Zahab, A. A.; Yuzyuk, Y. I.; Phan, N. M.; Sauvajol, J.-L.; Michel, T.

    2017-03-01

    Double-walled carbon nanotubes (DWNT) are made of two concentric and weakly van der Waals coupled single-walled carbon nanotubes (SWNT). DWNTs are the simplest systems for studying the mechanical and electronic interactions between concentric carbon layers. In this paper we review recent results concerning the intrinsic features of phonons of DWNTs obtained from Raman experiments performed on index-identified DWNTs. The effect of the interlayer distance on the strength of the mechanical and electronic coupling between the layers, and thus on the frequencies of the Raman-active modes, namely the radial breathing-like modes (RBLMs) and G-modes, are evidenced and discussed. Invited talk at 8th International Workshop on Advanced Materials Science and Nanotechnology (IWAMSN2016), 8-12 November 2016, Ha Long City, Vietnam.

  20. The role of electron-phonon interactions on the coherence lifetime of monolayer transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Stevens, C. E.; Dey, P.; Paul, J.; Wang, Z.; Zhang, H.; Romero, A. H.; Shan, J.; Hilton, D. J.; Karaiskaj, D.

    2017-10-01

    We investigate the excitonic dephasing of transition metal dichalcogenides, namely MoS2, MoSe2 and WSe2 atomic monolayer thick and bulk crystals, in order to understand the factors that determine the optical coherence in these materials. Coherent nonlinear optical spectroscopy, temperature dependent absorption combined with theoretical calculations of the phonon spectra, reveal the important role electron-phonon interactions plat in dephasing process. The temperature dependence of the electronic band gap and the excitonic linewidth combined with 'ab initio' calculations of the phonon energies and the phonon density of state reveal strong interaction with the E‧ and E″ phonon modes.

  1. The role of electron-phonon interactions on the coherence lifetime of monolayer transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Stevens, C. E.; Dey, P.; Paul, J.; Wang, Z.; Zhang, H.; Romero, A. H.; Shan, J.; Hilton, D. J.; Karaiskaj, D.

    2017-06-01

    We investigate the excitonic dephasing of transition metal dichalcogenides, namely MoS2, MoSe2 and WSe2 atomic monolayer thick and bulk crystals, in order to understand the factors that determine the optical coherence in these materials. Coherent nonlinear optical spectroscopy, temperature dependent absorption combined with theoretical calculations of the phonon spectra, reveal the important role electron-phonon interactions plat in dephasing process. The temperature dependence of the electronic band gap and the excitonic linewidth combined with ‘ab initio’ calculations of the phonon energies and the phonon density of state reveal strong interaction with the E’ and E” phonon modes.

  2. Phonon vibrational frequencies of all single-wall carbon nanotubes at the lambda point: reduced matrix calculations.

    PubMed

    Wang, Yufang; Wu, Yanzhao; Feng, Min; Wang, Hui; Jin, Qinghua; Ding, Datong; Cao, Xuewei

    2008-12-01

    With a simple method-the reduced matrix method, we simplified the calculation of the phonon vibrational frequencies according to SWNTs structure and their phonon symmetric property and got the dispersion properties of all SWNTs at Gamma point in Brillouin zone, whose diameters lie between 0.6 and 2.5 nm. The calculating time is shrunk about 2-4 orders. A series of the dependent relationships between the diameters of SWNTs and the frequencies of Raman and IR active modes are given. Several fine structures including "glazed tile" structures in omega approximately d figures are found, which might predict a certain macro-quantum phenomenon of the phonons in SWNTs.

  3. X-ray diffraction, Raman, and photoacoustic studies of ZnTe nanocrystals

    NASA Astrophysics Data System (ADS)

    Ersching, K.; Campos, C. E. M.; de Lima, J. C.; Grandi, T. A.; Souza, S. M.; da Silva, D. L.; Pizani, P. S.

    2009-06-01

    Nanocrystalline ZnTe was prepared by mechanical alloying. X-ray diffraction (XRD), energy dispersive spectroscopy, Raman spectroscopy, and photoacoustic absorption spectroscopy techniques were used to study the structural, chemical, optical, and thermal properties of the as-milled powder. An annealing of the mechanical alloyed sample at 590 °C for 6 h was done to investigate the optical properties in a defect-free sample (close to bulk form). The main crystalline phase formed was the zinc-blende ZnTe, but residual trigonal tellurium and hexagonal ZnO phases were also observed for both as-milled and annealed samples. The structural parameters, phase fractions, average crystallite sizes, and microstrains of all crystalline phases were obtained from Rietveld analyses of the X-ray patterns. Raman results corroborate the XRD results, showing the longitudinal optical phonons of ZnTe (even at third order) and those modes of trigonal Te. Nonradiative surface recombination and thermal bending heat transfer mechanisms were proposed from photoacoustic analysis. An increase in effective thermal diffusivity coefficient was observed after annealing and the carrier diffusion coefficient, the surface recombination velocity, and the recombination time parameters remained the same.

  4. Raman spectroscopy of KxCo2-ySe2 single crystals near the ferromagnet-paramagnet transition

    DOE PAGES

    Opacic, M.; Lazarevic, N.; Radonjic, M. M.; ...

    2016-10-05

    Polarized Raman scattering spectra of the K xCo 2-ySe 2 (x = :::; y = :::) single crystals reveal the presence of two phonon modes, assigned as of the A1g and B1g symmetry. Absence of additional modes excludes the possibility of vacancy ordering, unlike in K xCo 2-ySe 2 . The ferromagnetic (FM) phase transition at Tc 74 K leaves a clear fingerprint on the temperature dependence of the Raman mode energy and linewidth. For T > Tc the temperature dependence looks conventional, driven by the thermal expansion and anharmonicity. The Raman modes are rather broad due to the electron-phononmore » coupling increased by the disorder and spin fluctuation e ects. In the FM phase the phonon frequency of both modes increases, while an opposite trend is seen in their linewidth: the A1g mode narrows in the FM phase, whereas the B 1g mode broadens. We argue that the large asymmetry and anomalous frequency shift of the B 1g mode is due to the coupling of spin fluctuations and vibration. Our density functional theory (DFT) calculations for the phonon frequencies agree rather well with the Raman measurements, with some discrepancy being expected since the DFT calculations neglect the spin fluctuations.« less

  5. Quantitative Probes of Electron-Phonon Coupling in an Organic Charge-Transfer Material

    NASA Astrophysics Data System (ADS)

    Rury, Aaron; Sorenson, Shayne; Driscoll, Eric; Dawlaty, Jahan

    While organic charge transfer (CT) materials may provide alternatives to inorganic materials in electronics and photonics applications, properties central to applications remain understudied in these organic materials. Specifically, electron-phonon coupling plays a pivotal role in electronic applications yet this coupling in CT materials remains difficult to directly characterize. To better understand the suitability of organic CT materials for electronic applications, we have devised an experimental technique that can directly assess electron-phonon coupling in a model organic CT material. Upon non-resonant interaction with an ultrafast laser pulse, we show that coherent excitation of Raman-active lattice vibrations of quinhydrone, a 1:1 co-crystal of the hydroquinone and p-benzoquinone, modulates the energies of electronic transitions probed by a white light pulse. Using a well-established theoretical framework of vibrational quantum beat spectra across the probe bandwidth, we quantitatively extract the parameters describing these electronic transitions to characterize electron-phonon coupling in this material. In conjunction with temperature-dependent resonance Raman measurements, we assess the hypothesis that several sharp transitions in the near-IR correspond to previously unknown excitonic states of this material. These results and their interpretation set the foundation for further elucidation of the one of the most important parameters in the application of organic charge-transfer materials to electronics and photonics.

  6. Optical phonon characteristics of an orthorhombic-transformed polymorph of CaTa2O6 single crystal fibre

    NASA Astrophysics Data System (ADS)

    Almeida, R. M.; Andreeta, M. R. B.; Hernandes, A. C.; Dias, A.; Moreira, R. L.

    2014-03-01

    Infrared-reflectivity spectroscopy and micro-Raman scattering were used to determine the optical phonon features of orthorhombic calcium tantalite (CaTa2O6) single crystal fibres. The fibres, obtained by the Laser-Heated Pedestal Growth method, grew into an ordered cubic structure \\left( Pm\\bar{3} \\right). Long-time annealing was used to induce a polymorphic transformation to an aeschynite orthorhombic structure (Pnma space group). The phase transformation led to the appearance of structural domains and micro-cracks, responsible for diffuse scattering and depolarization of the scattered light in the visible range, but not in the infrared region. Thus, polarized infrared spectroscopy could be performed within oriented single domains, with an appropriate microscope, allowing us to determine all relevant polar phonons of the orthorhombic CaTa2O6. The obtained phononic dielectric response, {{\\epsilon }_{r}} = 22.4 and = 86 × 103 GHz, shows the appropriateness of the material for microwave applications. Totally symmetric Raman modes could be resolved by polarization, after re-polishing the cracked sample surface.

  7. DFT-Assisted Polymorph Identification from Lattice Raman Fingerprinting

    PubMed Central

    2017-01-01

    A combined experimental and theoretical approach, consisting of lattice phonon Raman spectroscopy and density functional theory (DFT) calculations, is proposed as a tool for lattice dynamics characterization and polymorph phase identification. To illustrate the reliability of the method, the lattice phonon Raman spectra of two polymorphs of the molecule 2,7-dioctyloxy[1]benzothieno[3,2-b]benzothiophene are investigated. We show that DFT calculations of the lattice vibrations based on the known crystal structures, including many-body dispersion van der Waals (MBD-vdW) corrections, predict experimental data within an accuracy of ≪5 cm–1 (≪0.6 meV). Due to the high accuracy of the simulations, they can be used to unambiguously identify different polymorphs and to characterize the nature of the lattice vibrations and their relationship to the structural properties. More generally, this work implies that DFT-MBD-vdW is a promising method to describe also other physical properties that depend on lattice dynamics like charge transport. PMID:28731723

  8. Raman investigation of ro-vibrational modes of interstitial H2 in Si

    NASA Astrophysics Data System (ADS)

    Koch, S. G.; Lavrov, E. V.; Weber, J.

    2012-08-01

    A Raman scattering study of ro-vibrational transitions Q(J) of the interstitial H2 in Si is presented. It is shown that the Q(2) mode of para hydrogen is coupled to the TAX phonon of Si. The mode appears in the spectra at temperatures above 200 K. The results presented also suggest that the Q(3) transition of ortho hydrogen is resonantly coupled to the OΓ phonon.

  9. New explanation of Raman peak redshift in nanoparticles

    NASA Astrophysics Data System (ADS)

    Meilakhs, A. P.; Koniakhin, S. V.

    2017-10-01

    In this letter, we propose a new model that explains the Raman peak downshift observed in nanoparticles with respect to bulk materials. The proposed model takes into account discreteness of the vibrational spectra of nanoparticles. For crystals with a cubic lattice (Diamond, Silicon, Germanium) we give a relation between the displacement of Raman peak position and the size of nanoparticles. The proposed model does not include any uncertain parameters, unlike the conventionally used phonon confinement model (PCM), and can be employed for unambiguous nanoparticles size estimation.

  10. Phonon-induced ultrafast band gap control in LaTiO3

    NASA Astrophysics Data System (ADS)

    Gu, Mingqiang; Rondinelli, James M.

    We propose a route for ultrafast band gap engineering in correlated transition metal oxides by using optically driven phonons. We show that the ∖Gamma-point electron band energies can be deterministically tuned in the nonequilibrium state. Taking the Mott insulator LaTiO3 as an example, we show that such phonon-assisted processes dynamically induce an indirect-to-direct band gap transition or even a metal-to-insulator transition, depending on the electron correlation strength. We explain the origin of the dynamical band structure control and also establish its generality by examining related oxides. Lastly, we describe experimental routes to realize the band structure control with impulsive stimulated Raman scattering.

  11. Quantification of irradiation defects in beta-silicon carbide using Raman spectroscopy

    DOE PAGES

    Koyanagi, T.; Lance, M. J.; Katoh, Y.

    2016-08-11

    Raman spectra from polycrystalline beta-silicon carbide (SiC) were collected following neutron irradiation at 380–1180 °C to 0.011–1.87 displacement per atom. The longitudinal optical (LO) peak shifted to a lower frequency and broadened as a result of the irradiation. The changes observed in the LO phonon line shape and position in neutron-irradiated SiC are explained by a combination of changes in the lattice constant and Young's modulus, and the phonon confinement effect. The phonon confinement model reasonably estimates the defect-defect distance in the irradiated SiC, which is consistent with results from previous experimental studies and simulations.

  12. A new on-axis micro-spectrophotometer for combining Raman, fluorescence and UV/Vis absorption spectroscopy with macromolecular crystallography at the Swiss Light Source.

    PubMed

    Pompidor, Guillaume; Dworkowski, Florian S N; Thominet, Vincent; Schulze-Briese, Clemens; Fuchs, Martin R

    2013-09-01

    The combination of X-ray diffraction experiments with optical methods such as Raman, UV/Vis absorption and fluorescence spectroscopy greatly enhances and complements the specificity of the obtained information. The upgraded version of the in situ on-axis micro-spectrophotometer, MS2, at the macromolecular crystallography beamline X10SA of the Swiss Light Source is presented. The instrument newly supports Raman and resonance Raman spectroscopy, in addition to the previously available UV/Vis absorption and fluorescence modes. With the recent upgrades of the spectral bandwidth, instrument stability, detection efficiency and control software, the application range of the instrument and its ease of operation were greatly improved. Its on-axis geometry with collinear X-ray and optical axes to ensure optimal control of the overlap of sample volumes probed by each technique is still unique amongst comparable facilities worldwide and the instrument has now been in general user operation for over two years.

  13. A new on-axis micro-spectrophotometer for combining Raman, fluorescence and UV/Vis absorption spectroscopy with macromolecular crystallography at the Swiss Light Source

    PubMed Central

    Pompidor, Guillaume; Dworkowski, Florian S. N.; Thominet, Vincent; Schulze-Briese, Clemens; Fuchs, Martin R.

    2013-01-01

    The combination of X-ray diffraction experiments with optical methods such as Raman, UV/Vis absorption and fluorescence spectroscopy greatly enhances and complements the specificity of the obtained information. The upgraded version of the in situ on-axis micro-spectrophotometer, MS2, at the macromolecular crystallography beamline X10SA of the Swiss Light Source is presented. The instrument newly supports Raman and resonance Raman spectroscopy, in addition to the previously available UV/Vis absorption and fluorescence modes. With the recent upgrades of the spectral bandwidth, instrument stability, detection efficiency and control software, the application range of the instrument and its ease of operation were greatly improved. Its on-axis geometry with collinear X-ray and optical axes to ensure optimal control of the overlap of sample volumes probed by each technique is still unique amongst comparable facilities worldwide and the instrument has now been in general user operation for over two years. PMID:23955041

  14. Raman Antenna Effect in Semiconducting Nanowires.

    NASA Astrophysics Data System (ADS)

    Chen, Gugang; Xiong, Qihua; Eklund, Peter

    2007-03-01

    A novel Raman antenna effect has been observed in Raman scattering experiments recently carried out on individual GaP nanowires [1]. The Raman antenna effect is perfectly general and should appear in all semiconducting nanowires. It is characterized by an anomalous increase in the Raman cross section for scattering from LO or TO phonons when the electric field of the incident laser beam is parallel to the nanowire axis. We demonstrate that the explanation for the effect lies in the polarization dependence of the Mie scattering from the nanowire and the concomitant polarization-dependent electric field set up inside the wire. Our analysis involves calculations of the internal electric field using the discrete dipole approximation (DDA). We find that the Raman antenna effect happens only for nanowire diameters d<λ/4, where λ is the excitation laser wavelength. Our calculations are found in good agreement with recent experimental results for scattering from individual GaP nanowires. [1] Q. Xiong, G. Chen, G. D. Mahan, P. C. Eklund, in preparation, 2006.

  15. Coherent Excitation of Optical Phonons in GaAs by Broadband Terahertz Pulses

    PubMed Central

    Fu, Zhengping; Yamaguchi, Masashi

    2016-01-01

    Coherent excitation and control of lattice motion by electromagnetic radiation in optical frequency range has been reported through variety of indirect interaction mechanisms with phonon modes. However, coherent phonon excitation by direct interaction of electromagnetic radiation and nuclei has not been demonstrated experimentally in terahertz (THz) frequency range mainly due to the lack of THz emitters with broad bandwidth suitable for the purpose. We report the experimental observation of coherent phonon excitation and detection in GaAs using ultrafast THz-pump/optical-probe scheme. From the results of THz pump field dependence, pump/probe polarization dependence, and crystal orientation dependence, we attributed THz wave absorption and linear electro-optic effect to the excitation and detection mechanisms of coherent polar TO phonons. Furthermore, the carrier density dependence of the interaction of coherent phonons and free carriers is reported. PMID:27905563

  16. Modification of the G-phonon mode of graphene by nitrogen doping

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Lukashev, Pavel V., E-mail: pavel.lukashev@uni.edu; Hurley, Noah; Zhao, Liuyan

    2016-01-25

    The effect of nitrogen doping on the phonon spectra of graphene is analyzed. In particular, we employ first-principles calculations and scanning Raman analysis to investigate the dependence of phonon frequencies in graphene on the concentration of nitrogen dopants. We demonstrate that the G phonon frequency shows oscillatory behavior as a function of nitrogen concentration. We analyze different mechanisms which could potentially be responsible for this behavior, such as Friedel charge oscillations around the localized nitrogen impurity atom, the bond length change between nitrogen impurity and its nearest neighbor carbon atoms, and the long-range interactions of the nitrogen point defects. Wemore » show that the bond length change and the long range interaction of point defects are possible mechanisms responsible for the oscillatory behavior of the G frequency as a function of nitrogen concentration. At the same time, Friedel charge oscillations are unlikely to contribute to this behavior.« less

  17. THz acoustic phonon spectroscopy and nanoscopy by using piezoelectric semiconductor heterostructures.

    PubMed

    Mante, Pierre-Adrien; Huang, Yu-Ru; Yang, Szu-Chi; Liu, Tzu-Ming; Maznev, Alexei A; Sheu, Jinn-Kong; Sun, Chi-Kuang

    2015-02-01

    Thanks to ultrafast acoustics, a better understanding of acoustic dynamics on a short time scale has been obtained and new characterization methods at the nanoscale have been developed. Among the materials that were studied during the development of ultrafast acoustics, nitride based heterostructures play a particular role due to their piezoelectric properties and the possibility to generate phonons with over-THz frequency and bandwidth. Here, we review some of the work performed using this type of structure, with a focus on THz phonon spectroscopy and nanoscopy. First, we present a brief description of the theory of coherent acoustic phonon generation by piezoelectric heterostructure. Then the first experimental observation of coherent acoustic phonon generated by the absorption of ultrashort light pulses in piezoelectric heterostructures is presented. From this starting point, we then present some methods developed to realize customizable phonon generation. Finally we review some more recent applications of these structures, including imaging with a nanometer resolution, broadband attenuation measurements with a frequency up to 1THz and phononic bandgap characterization. Copyright © 2014 Elsevier B.V. All rights reserved.

  18. Resonant Raman scattering study of BexZn1-xO thin films grown on sapphire by molecular beam epitaxy

    NASA Astrophysics Data System (ADS)

    Wang, Yu-Chao; Su, Long-Xing; Zhao, Yu; Liu, Jian-Feng; Shen, Zheng-Chuan; Feng, Yu-Hua; Wu, Tian-Zhun; Tang, Zi-Kang

    2017-07-01

    Resonance Raman spectra of BexZn1-xO alloy materials were studied using 325 nm Laser. The research showed that the Raman spectra of BexZn1-xO alloys presents a dual-mode vibration. Compare BexZn1-xO alloy with ZnO single crystal, the A1 (LO) phonon vibration mode of BexZn1-xO alloy moved to the larger wave number direction. The position of A1 (LO) phonon vibration modes of Be0.08Zn0.92O and Be0.12Zn0.88O was 580 cm-1 and 582 cm-1, respectively. In addition, the temperature-dependent Raman spectroscopy was employed for Be0.12Zn0.88O, and the phonon mode frequency shift with temperature was studied in detail. Finally, the stability of the polar and nonpolar BexZn1-xO alloy materials was studied using resonance Raman spectroscopy. The results showed that the A1 (LO) phonon mode frequency of polar BexZn1-xO alloy remained in the same position, while the nonpolar BexZn1-xO alloys moved nearly 3.5 cm-1 to larger direction after being placed in the air for two years. The reason may be that the stability of the nonpolar BexZn1-xO alloy is relatively poor upon interaction with molecule such as H2O, O2 in the air.

  19. Phonon-Mediated Exciton Stark Effect Enhanced by a Static Electric Field

    NASA Astrophysics Data System (ADS)

    Ivanov, A. L.

    1997-03-01

    The optical properties of semiconductor QW's change in the presence of coherent pump light. The exciton (phonon-mediated, biexciton-mediated, etc.) optical Stark effect is an effective shift of the exciton level that follow dynamically the intensity I0 ~= 0.1 div 1 GW/cm^2 of the pump light. In the present work we develop a theory of a low-intensity electric-field enhanced phonon-mediated optical Stark effect in polar semiconductors and semiconductor microstructures. The main point is that the exciton - LO-phonon Fröhlich interaction can be strongly enhanced by a (quasi-) static electric field F which polarizes the exciton in the geometry F | k | p, where k and p are the wavevectors of the pump and probe light, respectively. The electric field enhancement of spontaneous Raman scattering has been already analyzed (E. Burstein et al., 1971). Even a moderate electric field F ~= 10^3 V/cm reduces the intensity of the pump light to I0 ~= 1 div 10 MW/cm^2. Moreover, the phonon-mediated Stark effect enhanced by a static electric field F allow us to realize the both red and blue dynamical shifts of the exciton level.

  20. Flexural phonon limited phonon drag thermopower in bilayer graphene

    NASA Astrophysics Data System (ADS)

    Ansari, Mohd Meenhaz; Ashraf, SSZ

    2018-05-01

    We investigate the phonon drag thermopower from flexural phonons as a function of electron temperature and carrier concentration in the Bloch-Gruneisen regime in non-strained bilayer graphene using Boltzmann transport equation approach. The flexural phonons are expected to be the major source of intrinsic scattering mechanism in unstrained bilayer graphene due to their large density. The flexural phonon modes dispersion relation is quadratic so these low energy flexural phonons abound at room temperature and as a result deform the bilayer graphene sheet in the out of plane direction and affects the transport properties. We also produce analytical result for phonon-drag thermopower from flexural phonons and find that phonon-drag thermopower depicts T2 dependence on temperature and n-1 on carrier concentration.

  1. Raman spectroscopic determination of the length, strength, compressibility, Debye temperature, elasticity, and force constant of the C-C bond in graphene.

    PubMed

    Yang, X X; Li, J W; Zhou, Z F; Wang, Y; Yang, L W; Zheng, W T; Sun, Chang Q

    2012-01-21

    From the perspective of bond relaxation and bond vibration, we have formulated the Raman phonon relaxation of graphene, under the stimuli of the number-of-layers, the uni-axial strain, the pressure, and the temperature, in terms of the response of the length and strength of the representative bond of the entire specimen to the applied stimuli. Theoretical unification of the measurements clarifies that: (i) the opposite trends of the Raman shifts, which are due to the number-of-layers reduction, of the G-peak shift and arises from the vibration of a pair of atoms, while the D- and the 2D-peak shifts involve the z-neighbor of a specific atom; (ii) the tensile strain-induced phonon softening and phonon-band splitting arise from the asymmetric response of the C(3v) bond geometry to the C(2v) uni-axial bond elongation; (iii) the thermal softening of the phonons originates from bond expansion and weakening; and (iv) the pressure stiffening of the phonons results from bond compression and work hardening. Reproduction of the measurements has led to quantitative information about the referential frequencies from which the Raman frequencies shift as well as the length, energy, force constant, Debye temperature, compressibility and elastic modulus of the C-C bond in graphene, which is of instrumental importance in the understanding of the unusual behavior of graphene.

  2. Rotamer-Specific Photoisomerization of Difluorostilbenes from Transient Absorption and Transient Raman Spectroscopy.

    PubMed

    Quick, M; Dobryakov, A L; Ioffe, I N; Berndt, F; Mahrwald, R; Ernsting, N P; Kovalenko, S A

    2018-01-25

    Photoisomerization of 2,2'-, 3,3'-, and 4,4'-difluorostilbene (F2, F3, F4, respectively) in n-hexane, perfluoro-n-hexane, and acetonitrile is studied with broadband transient absorption (TA) and femtosecond stimulated Raman (FSR) spectroscopy and by DFT/TDDFT calculations. F2 and F3 possess three rotamers (rotational isomers) each, while F4 has one single conformation only. These differences are reflected in TA and FSR spectra. Thus F4 reveals a monoexponential decay of TA with τ 1 = 172 ps in n-hexane, as expected for a single species. For F2 and F3, the decays are biexponential in all solvents, corresponding to two distinctly discerned rotamers or rotamer fractions. Specifically, for F2 in n-hexane, τ 1 = 357 ps (83%) and τ 2 = 62 ps (17%), and for F3 in the same solvent, τ 1 = 222 ps (57%), and τ 2 = 81 ps (43%). The weights in brackets agree with theoretically estimated ground-state abundances of the rotamers. Furthermore, a global fit of the TA and FSR data allows us to extract the spectra of the pure rotamers. The Raman spectra of S 0 and S 1 are in qualitative agreement with calculations.

  3. Infrared dielectric functions and optical phonons of wurtzite Y x Al1-x N (0  ⩽  x  ⩽  0.22)

    NASA Astrophysics Data System (ADS)

    Ben Sedrine, N.; Zukauskaite, A.; Birch, J.; Jensen, J.; Hultman, L.; Schöche, S.; Schubert, M.; Darakchieva, V.

    2015-10-01

    YAlN is a new member of the group-III nitride family with potential for applications in next generation piezoelectric and light emitting devices. We report the infrared dielectric functions and optical phonons of wurtzite (0001) Y x Al1-x N epitaxial films with 0  ⩽  x  ⩽  0.22. The films are grown by magnetron sputtering epitaxy on c-plane Al2O3 and their phonon properties are investigated using infrared spectroscopic ellipsometry and Raman scattering spectroscopy. The infrared-active E 1(TO) and LO, and the Raman active E 2 phonons are found to exhibit one-mode behavior, which is discussed in the framework of the MREI model. The compositional dependencies of the E 1(TO), E 2 and LO phonon frequencies, the high-frequency limit of the dielectric constant, {{\\varepsilon}∞} , the static dielectric constant, {{\\varepsilon}0} , and the Born effective charge Z B are established and discussed.

  4. Tunable phonon-induced transparency in bilayer graphene nanoribbons.

    PubMed

    Yan, Hugen; Low, Tony; Guinea, Francisco; Xia, Fengnian; Avouris, Phaedon

    2014-08-13

    In the phenomenon of plasmon-induced transparency, which is a classical analogue of electromagnetically induced transparency (EIT) in atomic gases, the coherent interference between two plasmon modes results in an optical transparency window in a broad absorption spectrum. With the requirement of contrasting lifetimes, typically one of the plasmon modes involved is a dark mode that has limited coupling to the electromagnetic radiation and possesses relatively longer lifetime. Plasmon-induced transparency not only leads to light transmission at otherwise opaque frequency regions but also results in the slowing of light group velocity and enhanced optical nonlinearity. In this article, we report an analogous behavior, denoted as phonon-induced transparency (PIT), in AB-stacked bilayer graphene nanoribbons. Here, light absorption due to the plasmon excitation is suppressed in a narrow window due to the coupling with the infrared active Γ-point optical phonon, whose function here is similar to that of the dark plasmon mode in the plasmon-induced transparency. We further show that PIT in bilayer graphene is actively tunable by electrostatic gating and estimate a maximum slow light factor of around 500 at the phonon frequency of 1580 cm(-1), based on the measured spectra. Our demonstration opens an avenue for the exploration of few-photon nonlinear optics and slow light in this novel two-dimensional material.

  5. Localized magnetoplasmons in quantum dots: Magneto-optical absorption, Raman scattering, and inelastic electron scattering

    NASA Astrophysics Data System (ADS)

    Kushwaha, M. S.

    We investigate a one-component, quasi-zero dimensional, quantum plasma exposed to a parabolic potential and an applied magnetic field in the symmetric gauge. If the size of such a system as can be realized in the semiconducting quantum dots is on the order of the de-Broglie wavelength, the electronic and optical properties become highly tunable. Then the quantum size effects challenge the observation of many-particle phenomena such as the magneto-optical absorption, Raman intensity, and electron-energy-loss spectrum. An exact analytical solution of the problem leads us to infer that these many-particle phenomena are, in fact, dictated by the generalized Kohn's theorem in the long-wavelength limit. Maneuvering the confinement and/or the magnetic field furnishes the resonance energy capable of being explored with the FIR, Raman, or electron-energy-loss spectroscopy. This implies that either of these probes should be competent in observing the localized magnetoplasmons in the system. A deeper insight into the physics of quantum dots is paving the way for their implementation in such diverse fields as quantum computing and medical imaging.

  6. Quantitative analysis of domain texture in polycrystalline barium titanate by polarized Raman microprobe spectroscopy

    NASA Astrophysics Data System (ADS)

    Sakashita, Tatsuo; Chazono, Hirokazu; Pezzotti, Giuseppe

    2007-12-01

    A quantitative determination of domain distribution in polycrystalline barium titanate (BaTiO3, henceforth BT) ceramics has been pursued with the aid of a microprobe polarized Raman spectrometer. The crystallographic texture and domain orientation distribution of BT ceramics, which switched upon applying stress according to ferroelasticity principles, were determined from the relative intensity of selected phonon modes, taking into consideration a theoretical analysis of the angular dependence of phonon mode intensity for the tetragonal BT phase. Furthermore, the angular dependence of Raman intensity measured in polycrystalline BT depended on the statistical distribution of domain angles in the laser microprobe, which was explicitly taken into account in this work for obtaining a quantitative analysis of domain orientation for in-plane textured BT polycrystalline materials.

  7. Temperature- and Phase-Dependent Phonon Renormalization in 1T'-MoS2.

    PubMed

    Tan, Sherman Jun Rong; Sarkar, Soumya; Zhao, Xiaoxu; Luo, Xin; Luo, Yong Zheng; Poh, Sock Mui; Abdelwahab, Ibrahim; Zhou, Wu; Venkatesan, Thirumalai; Chen, Wei; Quek, Su Ying; Loh, Kian Ping

    2018-05-22

    Polymorph engineering of 2H-MoS 2 , which can be achieved by alkali metal intercalation to obtain either the mixed 2H/1T' phases or a homogeneous 1T' phase, has received wide interest recently, since this serves as an effective route to tune the electrical and catalytic properties of MoS 2 . As opposed to an idealized single crystal-to-single crystal phase conversion, the 2H to 1T' phase conversion results in crystal domain size reduction as well as strained lattices, although how these develop with composition is not well understood. Herein, the evolution of the phonon modes in Li-intercalated 1T'-MoS 2 (Li x MoS 2 ) are investigated as a function of different 1T'-2H compositions. We observed that the strain evolution in the mixed phases is revealed by the softening of four Raman modes, B g ( J 1 ), A g ( J 3 ), E 1 2g , and A 1g , with increasing 1T' phase composition. Additionally, the first-order temperature coefficients of the 1T' phonon mode vary linearly with increasing 1T' composition, which is explained by increased electron-phonon and strain-phonon coupling.

  8. Spin angular momentum induced by optical quasi-phonons activated in birefringent uniaxial crystals

    NASA Astrophysics Data System (ADS)

    Mohamadou, B.; Maïmounatou, B.; Erasmus, R. M.

    2017-09-01

    The present report formally establishes the expression of the angular momentum of the quasi-phonons induced by linearly polarized light. The transferred mechanical torque due to phonons is then determined from the spin angular momentum and is shown to be measurable from Raman scattering experiments. To investigate this, the electric field due the excited dipoles and the associated macroscopic dielectric polarization vectors were first calculated using a lattice dynamical model in order to derive in a second step the analytical expression of the angular momentum density arising from the inelastic light scattering by quasi-phonons. The numerical results of the calculated angle dependent mode electric fields and the induced spin angular moments as well as the transferred torques were analyzed with regard to some typical behaviors of the interacting modes and it is shown that the fluctuations of the effective charges is their main origin.

  9. Quantitative Analysis of Temperature Dependence of Raman shift of monolayer WS2

    NASA Astrophysics Data System (ADS)

    Huang, Xiaoting; Gao, Yang; Yang, Tianqi; Ren, Wencai; Cheng, Hui-Ming; Lai, Tianshu

    2016-08-01

    We report the temperature-dependent evolution of Raman spectra of monolayer WS2 directly CVD-grown on a gold foil and then transferred onto quartz substrates over a wide temperature range from 84 to 543 K. The nonlinear temperature dependence of Raman shifts for both and A1g modes has been observed. The first-order temperature coefficients of Raman shifts are obtained to be -0.0093 (cm-1/K) and -0.0122 (cm-1/K) for and A1g peaks, respectively. A physical model, including thermal expansion and three- and four-phonon anharmonic effects, is used quantitatively to analyze the observed nonlinear temperature dependence. Thermal expansion coefficient (TEC) of monolayer WS2 is extracted from the experimental data for the first time. It is found that thermal expansion coefficient of out-plane mode is larger than one of in-plane mode, and TECs of and A1g modes are temperature-dependent weakly and strongly, respectively. It is also found that the nonlinear temperature dependence of Raman shift of mode mainly originates from the anharmonic effect of three-phonon process, whereas one of A1g mode is mainly contributed by thermal expansion effect in high temperature region, revealing that thermal expansion effect cannot be ignored.

  10. Evidence of an Improper Displacive Phase Transition in Cd2 Re2 O7 via Time-Resolved Coherent Phonon Spectroscopy

    NASA Astrophysics Data System (ADS)

    Harter, J. W.; Kennes, D. M.; Chu, H.; de la Torre, A.; Zhao, Z. Y.; Yan, J.-Q.; Mandrus, D. G.; Millis, A. J.; Hsieh, D.

    2018-01-01

    We have used a combination of ultrafast coherent phonon spectroscopy, ultrafast thermometry, and time-dependent Landau theory to study the inversion symmetry breaking phase transition at Tc=200 K in the strongly spin-orbit coupled correlated metal Cd2 Re2 O7 . We establish that the structural distortion at Tc is a secondary effect through the absence of any softening of its associated phonon mode, which supports a purely electronically driven mechanism. However, the phonon lifetime exhibits an anomalously strong temperature dependence that decreases linearly to zero near Tc. We show that this behavior naturally explains the spurious appearance of phonon softening in previous Raman spectroscopy experiments and should be a prevalent feature of correlated electron systems with linearly coupled order parameters.

  11. Direct Observation of Electron-Phonon Coupling and Slow Vibrational Relaxation in Organic-Inorganic Hybrid Perovskites

    NASA Astrophysics Data System (ADS)

    Hurtado Parra, Sebastian; Straus, Daniel; Iotov, Natasha; Fichera, Bryan; Gebhardt, Julian; Rappe, Andrew; Subotnik, Joseph; Kikkawa, James; Kagan, Cherie

    Quantum and dielectric confinement effects in Ruddlesden-Popper 2D hybrid perovskites create excitons with a binding energy exceeding 150 meV. We exploit the large exciton binding energy to study exciton and carrier dynamics as well as electron-phonon coupling (EPC) in hybrid perovskites using absorption and photoluminescence (PL) spectroscopies. At temperatures <75 K, we resolve splitting of the excitonic absorption and PL into multiple regularly spaced resonances every 40-46 meV, consistent with EPC to phonons located on the organic cation. We also resolve resonances with a 14 meV spacing, in accord with coupling to phonons with mixed organic and inorganic character. These assignments are supported by density-functional theory calculations. Hot exciton PL and time-resolved PL measurements show that vibrational relaxation occurs on a picosecond time scale competitive with that for PL. At temperatures >75 K, excitonic absorption and PL exhibit homogeneous broadening. While absorption remains homogeneous, PL becomes inhomogeneous at temperatures <75K, which we speculate is caused by the formation and subsequent dynamics of a polaronic exciton. This work is supported by the U.S. Department of Energy, Office of Basic Energy Sciences Grant DE-SC0002158 and the National Science Foundation Graduate Research Fellowship Grant DGE-1321851.

  12. Experimental artifacts influencing polarization sensitive magneto-Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Thirunavukkuarasu, K.; Lu, Z.; Su, L.; Yu, Y.; Cao, L.; Ballotin, M. V.; Christianen, P. C. M.; Zhang, Y.; Smirnov, D.

    Since the discovery of graphene, there has been an explosion of research on 2D layered materials such as transition metal dichalcogenides (TMDs). Among several experimental techniques utilized for studying these materials, Raman spectroscopy has proven to be a very powerful tool due to it's sensitivity to layer numbers, interlayer coupling etc. Layered MoS2, member of TMD family, is a typical example with promising applications in nano-optoelectronics. A recent magneto-Raman investigations on MoS2 published by J. Ji etal reported an observation of giant magneto-optical effect. In this work, the intensity of Raman modes exhibited dramatic change in intensities and was attributed to field-induced broken symmetry on Raman scattering cross-section. Due to the ambiguous nature of the interpretation presented in this publication, we performed further Raman studies on MoS2 at high magnetic fields to illustrate the experimental factors overlooked by the previous study. It is highly important to consider the magnetic field-induced rotation of the polarization of the light and its effect on the Raman active phonon modes in anisotropic materials. A detailed report of our magneto-Raman experiments and their outcomes will be presented.

  13. High-pressure Raman study of vibrational spectra in crystalline acetanilide

    NASA Astrophysics Data System (ADS)

    Sakai, Masamichi; Kuroda, Noritaka; Nishina, Yuichiro

    1993-01-01

    We have studied the effect of pressure on the low-frequency lattice modes and the amide-I (N-CO stretching) vibrational modes in crystalline acetanilide (C6H5NHCOCH3) in the temperature range 80-300 K by means of Raman spectroscopy. The Raman intensity of the 1650-cm-1 band, which appears upon cooling, is enhanced by applying pressure. The energy difference between the amide-I phonon (Ag mode) and the 1650-cm-1 bands does not change appreciably under pressure up to at least 4 GPa. These results are analyzed in terms of the self-trapped model in which a single lattice mode couples with the amide-I excitation by taking into account the effect of pressure on the low-frequency lattice modes and on the dipole-dipole interactions associated with the amide-I vibration. A band is observed at 30 cm-1 below the amide-I phonon band at low temperatures with a pressure above ~2 GPa.

  14. Pressure dependence of the optical phonon frequencies and the transverse effective charge in AlSb

    NASA Astrophysics Data System (ADS)

    Ves, S.; Strössner, K.; Cardona, M.

    1986-02-01

    The first order Raman scattering by TO and LO phonons has been measured in AlSb under hydrostatic' pressures up to its phase transition. The Raman frequencies increase nearly linear while the transverse effective charge e ∗T are compared with estimates based on pseudopotential and on LCAO calculation. In order to obtain from the measured pressure dependence the corresponding volume coefficients the bulk modulus B O and its pressure derivative BOˌ = {dBO}/{dP} was measured by energy-dispersive X-ray diffraction (B O = 55.1 GPa and BOˌ = 4.55 ).

  15. Spin-phonon coupling and exchange interaction in Gd substituted YFe0.5Cr0.5O3

    NASA Astrophysics Data System (ADS)

    Singh, Karan; Sharma, Mohit K.; Mukherjee, K.

    2018-02-01

    We report the evolution of physical properties due to partial substitution of Gd on the Y site in a mixed metal oxide YFe0.5Cr0.5O3. This compound exhibits negative magnetization at low applied fields. Our investigations on Y1-xGdxFe0.5Cr0.5O3 (x = 0.0, 0.2, 0.4 and 0.6) compounds is carried out through magnetization and Raman spectroscopy studies. It is observed that even with 20% Gd substitution, the negative magnetization observed in YFe0.5Cr0.5O3 is suppressed. Due to magnetic rare earth ion Gd3+, additional exchange interaction of the form Gd-O-Fe/Cr dominates the magnetic interaction arising due to the transition metal ions. This results in positive magnetization in Gd-substituted compounds. Temperature dependent Raman spectroscopy along with magnetization studies revealed that the observed shifts of Raman mode is due to spin-phonon coupling. Hardening of Raman mode observed below 240 K in YFe0.5Cr0.5O3 weakens and softening of phonon modes was observed for Y0.4Gd0.6Fe0.5Cr0.5O3 compound. This implies that additional magnetic interactions due to Gd ions play a dominating role in dictating the behavior of the Gd-substituted compounds.

  16. Phononic crystal devices

    DOEpatents

    El-Kady, Ihab F [Albuquerque, NM; Olsson, Roy H [Albuquerque, NM

    2012-01-10

    Phononic crystals that have the ability to modify and control the thermal black body phonon distribution and the phonon component of heat transport in a solid. In particular, the thermal conductivity and heat capacity can be modified by altering the phonon density of states in a phononic crystal. The present invention is directed to phononic crystal devices and materials such as radio frequency (RF) tags powered from ambient heat, dielectrics with extremely low thermal conductivity, thermoelectric materials with a higher ratio of electrical-to-thermal conductivity, materials with phononically engineered heat capacity, phononic crystal waveguides that enable accelerated cooling, and a variety of low temperature application devices.

  17. Sensitivity Modulation of Upconverting Thermometry through Engineering Phonon Energy of a Matrix.

    PubMed

    Suo, Hao; Guo, Chongfeng; Zheng, Jiming; Zhou, Bo; Ma, Chonggeng; Zhao, Xiaoqi; Li, Ting; Guo, Ping; Goldys, Ewa M

    2016-11-09

    Investigation of the unclear influential factors to thermal sensing capability is the only way to achieve highly sensitive thermometry, which is greatly needed to meet the growing demand for potential sensing applications. Here, the effect from the phonon energy of a matrix on the sensitivity of upconversion (UC) microthermometers is elaborately discussed using a controllable method. Uniform truncated octahedral YF 3 :Er 3+ /Yb 3+ microcrystals were prepared by a hydrothermal approach, and phase transformation from YF 3 to YOF and Y 2 O 3 with nearly unchanged morphology and size was successfully realized by controlling the annealing temperature. The phonon energies of blank matrixes were determined by FT-IR spectra and Raman scattering. Upon 980 nm excitation, phonon energy-dependent UC emitting color was finely tuned from green to yellow for three samples, and the mechanisms were proposed. Thermal sensing behaviors based on the TCLs ( 2 H 11/2 / 4 S 3/2 ) were evaluated, and the sensitivities gradually grew with the increase in the matrix's phonon energy. According to chemical bond theory and first-principle calculations, the most intrinsic factors associated with thermometric ability were qualitatively demonstrated through analyzing the inner relation between the phonon energy and bond covalency. The exciting results provide guiding insights into employing appropriate host materials with desired thermometric ability while offering the possibility of highly accurate measurement of temperature.

  18. Effects of strain on phonon interactions and phase nucleation in several semiconductor and nano particle systems

    NASA Astrophysics Data System (ADS)

    Tallman, Robert E.

    Raman scattering is utilized to explore the effects of applied pressure and strain on anharmonic phonon interactions and nucleation of structural transitions in several bulk and nanoparticle semiconductor systems. The systems investigated are bulk ZnS and ZnSe in several isotopic compositions, InP/CdS core/shell nanoparticles exhibiting confined and surface optical Raman modes, and amorphous selenium films undergoing photo-induced crystallization. The anharmonic decay of long-wavelength optical modes into two-phonon acoustic combinations modes is studied in 64Zn32S, 64Zn34S, natZnatS bulk crystals by measuring the TO(Gamma) Raman line-shape as a function of applied hydrostatic pressure. The experiments are carried out at room temperature and 16K for pressures up to 150 kbars using diamond-anvil cells. The most striking effects occur in 68Zn32S where the TO(Gamma) peak narrows by a factor of 10 and increases in intensity at pressures for which the TO(Gamma) frequency has been tuned into a gap in the two-phonon density of states (DOS). In all the isotopic compositions, the observed phonon decay processes can be adequately explained by a second order perturbation treatment of the anharmonic coupling between TO(Gamma) and TA + LA combinations at various critical points, combined with an adiabatic bond-charge model for the phonon DOS and the known mode Gruneisen parameters. Bulk ZnSe crystals exhibit very different behavior. Here we find that anharmonic decay alone can not explain the excessive (˜ 60 cm-1 ) broadening in the TO(Gamma) Raman peak observed as the pressure approaches to within 50kbar of the ZB -> B1 phase transition (at P ˜ 137 kbar). Rather the broadening appears to arise from antecedent nucleation of structural changes within nanoscopic domains, with the mechanism for line-shape changes being mode mixing via localization and disorder instead of anharmonicity. To sort out these contributions, pressure experiments on natural ZnSe and on isotopically pure

  19. ``New'' energy states lead to phonon-less optoelectronic properties in nanostructured silicon

    NASA Astrophysics Data System (ADS)

    Singh, Vivek; Yu, Yixuan; Korgel, Brian; Nagpal, Prashant

    2014-03-01

    Silicon is arguably one of the most important technological material for electronic applications. However, indirect bandgap of silicon semiconductor has prevented optoelectronic applications due to phonon assistance required for photon light absorption/emission. Here we show, that previously unexplored surface states in nanostructured silicon can couple with quantum-confined energy levels, leading to phonon-less exciton-recombination and photoluminescence. We demonstrate size dependence (2.4 - 8.3 nm) of this coupling observed in small uniform silicon nanocrystallites, or quantum-dots, by direct measurements of their electronic density of states and low temperature measurements. To enhance the optical absorption of the these silicon quantum-dots, we utilize generation of resonant surface plasmon polariton waves, which leads to several fold increase in observed spectrally-resolved photocurrent near the quantum-confined bandedge states. Therefore, these enhanced light emission and absorption enhancement can have important implications for applications of nanostructured silicon for optoelectronic applications in photovoltaics and LEDs.

  20. Exploring the effect of hole localization on the charge-phonon dynamics of hole doped delafossite

    NASA Astrophysics Data System (ADS)

    Mazumder, Nilesh; Mandal, Prasanta; Roy, Rajarshi; Ghorai, Uttam Kumar; Saha, Subhajit; Chattopadhyay, Kalyan Kumar

    2017-09-01

    For weak or moderate doping, electrical measurement is not suitable for detecting changes in the charge localization inside a semiconductor. Here, to investigate the nature of charge-phonon coupling in the presence of gradually delocalized holes within a weak doping regime (~1016 cm-3), we examine the temperature dependent Raman spectra (303-817 K) of prototype hole doped delafossite CuC{{r}1-x}M{{g}x}{{O}2-y}{{S}y} (x  =  0/0.03, y  =  0/0.01). For both {{E}g} and {{A}1g} phonons, negative lineshape asymmetry and relative thermal hardening are distinctly observed upon SO× and (MgCr\\bullet+SO×) doping. Using Allen formalism, charge density of states at the Fermi level per spin and molecule, and charge delocalization associated to a - b plane, are estimated to increase appreciably upon codoping compared to the c -axis. We delineate the interdependence between charge-phonon coupling constant (λ ) and anharmonic phonon lifetime ({τanh} ), and deduce that excitation of delocalized holes weakly coupled with phonons of larger {τanh} is the governing feature of observed Fano asymmetry (q ) reversal.

  1. Raman studies of single-walled carbon nanotubes synthesized by pulsed laser ablation at room temperature

    NASA Astrophysics Data System (ADS)

    Dixit, Saurabh; Shukla, A. K.

    2018-06-01

    In this article, single-walled carbon nanotubes (SWCNTs) are synthesized at room temperature using pulsed laser ablation of ferrocene mixed graphitic target. Radial breathing mode (RBM) reveals the presence of semiconducting SWCNTs of multiple diameters. Quantum confinement model is developed for Raman line-shape of G - feature. It is invoked here that G-feature is the manifestation of TO phonons in the semiconducting SWCNTs. Disorder in the SWCNTs is studied here as a function of the concentration of ferrocene in the graphitic target using X-ray diffraction analysis, oscillator strength of G - feature and D mode and Raman line-shape model of G - feature. Furthermore, phonon softening of G - feature of semiconducting SWCNTs is observed as a function of the diameter of nanotube.

  2. Terahertz and infrared spectroscopic evidence of phonon-paramagnon coupling in hexagonal piezomagnetic YMnO3

    NASA Astrophysics Data System (ADS)

    Kadlec, C.; Goian, V.; Rushchanskii, K. Z.; Kužel, P.; Ležaić, M.; Kohn, K.; Pisarev, R. V.; Kamba, S.

    2011-11-01

    Terahertz and far-infrared electric and magnetic responses of hexagonal piezomagnetic YMnO3 single crystals are investigated. Antiferromagnetic resonance is observed in the spectra of magnetic permeability μa [H(ω) oriented within the hexagonal plane] below the Néel temperature TN. This excitation softens from 41 to 32 cm-1 upon heating and finally disappears above TN. An additional weak and heavily-damped excitation is seen in the spectra of complex dielectric permittivity ɛc within the same frequency range. This excitation contributes to the dielectric spectra in both antiferromagnetic and paramagnetic phases. Its oscillator strength significantly increases upon heating toward room temperature, thus providing evidence of piezomagnetic or higher-order couplings to polar phonons. Other heavily-damped dielectric excitations are detected near 100 cm-1 in the paramagnetic phase in both ɛc and ɛa spectra, and they exhibit similar temperature behavior. These excitations appearing in the frequency range of magnon branches well below polar phonons could remind electromagnons, however their temperature dependence is quite different. We have used density functional theory for calculating phonon dispersion branches in the whole Brillouin zone. A detailed analysis of these results and of previously published magnon dispersion branches brought us to the conclusion that the observed absorption bands stem from phonon-phonon and phonon-paramagnon differential absorption processes. The latter is enabled by strong short-range in-plane spin correlations in the paramagnetic phase.

  3. Resonance Raman scattering of β-carotene solution excited by visible laser beams into second singlet state.

    PubMed

    Lu, Luyao; Shi, Lingyan; Secor, Jeff; Alfano, Robert

    2018-02-01

    This study aimed to use self-absorption correction to determine the Raman enhancement of β-carotene. The Raman spectra of β-carotene solutions were measured using 488nm, 514nm, 532nm and 633nm laser beams, which exhibited significant resonance Raman (RR) enhancement when the laser energy approaches the electronic transition energy from S 0 to S 2 state. The Raman intensity and the actual resonance Raman gain without self-absorption from S 2 state by β-carotene were also obtained to evaluate the effect of self-absorption on RR scattering. Moreover, we observed the Raman intensity strength followed the absorption spectra. Our study found that, although 488nm and 514nm pumps seemed better for stronger RR enhancement, 532nm would be the optimum Raman pump laser with moderate RR enhancement due to reduced fluorescence and self-absorption. The 532nm excitation will be helpful for applying resonance Raman spectroscopy to investigate biological molecules in tissues. Copyright © 2017 Elsevier B.V. All rights reserved.

  4. Microscopic theory of multiple-phonon-mediated dephasing and relaxation of quantum dots near a photonic band gap

    NASA Astrophysics Data System (ADS)

    Roy, Chiranjeeb; John, Sajeev

    2010-02-01

    We derive a quantum theory of the role of acoustic and optical phonons in modifying the optical absorption line shape, polarization dynamics, and population dynamics of a two-level atom (quantum dot) in the “colored” electromagnetic vacuum of a photonic band-gap (PBG) material. This is based on a microscopic Hamiltonian describing both radiative and vibrational processes quantum mechanically. We elucidate the extent to which phonon-assisted decay limits the lifetime of a single photon-atom bound state and derive the modified spontaneous emission dynamics due to coupling to various phonon baths. We demonstrate that coherent interaction with undamped phonons can lead to an enhanced lifetime of a photon-atom bound state in a PBG. This results in reduction of the steady-state atomic polarization but an increase in the fractionalized upper state population in the photon-atom bound state. We demonstrate, on the other hand, that the lifetime of the photon-atom bound state in a PBG is limited by the lifetime of phonons due to lattice anharmonicities (breakup of phonons into lower energy phonons) and purely nonradiative decay. We also derive the modified polarization decay and dephasing rates in the presence of such damping. This leads to a microscopic, quantum theory of the optical absorption line shapes. Our model and formalism provide a starting point for describing dephasing and relaxation in the presence of external coherent fields and multiple quantum dot interactions in electromagnetic reservoirs with radiative memory effects.

  5. Detecting the phonon spin in magnon-phonon conversion experiments

    NASA Astrophysics Data System (ADS)

    Holanda, J.; Maior, D. S.; Azevedo, A.; Rezende, S. M.

    2018-05-01

    Recent advances in the emerging field of magnon spintronics have stimulated renewed interest in phenomena involving the interaction between spin waves, the collective excitations of spins in magnetic materials that quantize as magnons, and the elastic waves that arise from excitations in the crystal lattice, which quantize as phonons. In magnetic insulators, owing to the magnetostrictive properties of materials, spin waves can become strongly coupled to elastic waves, forming magnetoelastic waves—a hybridized magnon-phonon excitation. While several aspects of this interaction have been subject to recent scrutiny, it remains unclear whether or not phonons can carry spin. Here we report experiments on a film of the ferrimagnetic insulator yttrium iron garnet under a non-uniform magnetic field demonstrating the conversion of coherent magnons generated by a microwave field into phonons that have spin. While it is well established that photons in circularly polarized light carry a spin, the spin of phonons has had little attention in the literature. By means of wavevector-resolved Brillouin light-scattering measurements, we show that the magnon-phonon conversion occurs with constant energy and varying linear momentum, and that the light scattered by the phonons is circularly polarized, thus demonstrating that the phonons have spin.

  6. Room-Temperature Coherent Optical Phonon in 2D Electronic Spectra of CH 3NH 3PbI 3 Perovskite as a Possible Cooling Bottleneck

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Monahan, Daniele M.; Guo, Liang; Lin, Jia

    2017-06-29

    A hot phonon bottleneck may be responsible for slow hot carrier cooling in methylammonium lead iodide hybrid perovskite, creating the potential for more efficient hot carrier photovoltaics. In room-temperature 2D electronic spectra near the band edge, we observe in this paper amplitude oscillations due to a remarkably long lived 0.9 THz coherent phonon population at room temperature. This phonon (or set of phonons) is assigned to angular distortions of the Pb–I lattice, not coupled to cation rotations. The strong coupling between the electronic transition and the 0.9 THz mode(s), together with relative isolation from other phonon modes, makes it likelymore » to cause a phonon bottleneck. Finally, the pump frequency resolution of the 2D spectra also enables independent observation of photoinduced absorptions and bleaches independently and confirms that features due to band gap renormalization are longer-lived than in transient absorption spectra.« less

  7. Terahertz Time Domain Spectroscopy of Phonon-Depopulation Based Quantum Cascade Lasers

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Rungsawang, R.; Dhillon, S. S.; Jukam, N.

    2011-12-23

    A 3.1 THz phonon depopulation-based quantum-cascade-laser is investigated using terahertz time domain spectroscopy. A gain of 25 cm{sup -1} and absorption features due to the lower laser level being populated from a parasitic electronic channel are highlighted.

  8. Enhancement of phonon backscattering due to confinement of ballistic phonon pathways in silicon as studied with a microfabricated phonon spectrometer

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Otelaja, O. O.; Robinson, R. D., E-mail: rdr82@cornell.edu

    2015-10-26

    In this work, the mechanism for enhanced phonon backscattering in silicon is investigated. An understanding of phonon propagation through substrates has implications for engineering heat flow at the nanoscale, for understanding sources of decoherence in quantum systems, and for realizing efficient phonon-mediated particle detectors. In these systems, phonons that backscatter from the bottom of substrates, within the crystal or from interfaces, often contribute to the overall detector signal. We utilize a microscale phonon spectrometer, comprising superconducting tunnel junction emitters and detectors, to specifically probe phonon backscattering in silicon substrates (∼500 μm thick). By etching phonon “enhancers” or deep trenches (∼90 μm) aroundmore » the detectors, we show that the backscattered signal level increases by a factor of ∼2 for two enhancers versus one enhancer. Using a geometric analysis of the phonon pathways, we show that the mechanism of the backscattered phonon enhancement is due to confinement of the ballistic phonon pathways and increased scattering off the enhancer walls. Our result is applicable to the geometric design and patterning of substrates that are employed in phonon-mediated detection devices.« less

  9. A possible high-mobility signal in bulk MoTe2: Temperature independent weak phonon decay

    NASA Astrophysics Data System (ADS)

    Li, Titao; Zhang, Zhaojun; Zheng, Wei; Lv, Yangyang; Huang, Feng

    2016-11-01

    Layered transition metal dichalcogenides (TMDs) have attracted great attention due to their non-zero bandgap for potential application in high carrier mobility devices. Recent studies demonstrate that the carrier mobility of MoTe2 would decrease by orders of magnitude when used for few-layer transistors. As phonon scattering has a significant influence on carrier mobility of layered material, here, we first reported temperature-dependent Raman spectra of bulk 2H-MoTe2 from 80 to 300 K and discovered that the phonon lifetime of both E12g and A1g vibration modes are independent with temperature. These results were explained by the weak phonon decay in MoTe2. Our results imply the existence of a carrier mobility higher than the theoretical value in intrinsic bulk 2H-MoTe2 and the feasibility to obtain MoTe2-based transistors with sufficiently high carrier mobility.

  10. Heat guiding and focusing using ballistic phonon transport in phononic nanostructures

    NASA Astrophysics Data System (ADS)

    Anufriev, Roman; Ramiere, Aymeric; Maire, Jeremie; Nomura, Masahiro

    2017-05-01

    Unlike classical heat diffusion at macroscale, nanoscale heat conduction can occur without energy dissipation because phonons can ballistically travel in straight lines for hundreds of nanometres. Nevertheless, despite recent experimental evidence of such ballistic phonon transport, control over its directionality, and thus its practical use, remains a challenge, as the directions of individual phonons are chaotic. Here, we show a method to control the directionality of ballistic phonon transport using silicon membranes with arrays of holes. First, we demonstrate that the arrays of holes form fluxes of phonons oriented in the same direction. Next, we use these nanostructures as directional sources of ballistic phonons and couple the emitted phonons into nanowires. Finally, we introduce thermal lens nanostructures, in which the emitted phonons converge at the focal point, thus focusing heat into a spot of a few hundred nanometres. These results motivate the concept of ray-like heat manipulations at the nanoscale.

  11. Heat guiding and focusing using ballistic phonon transport in phononic nanostructures.

    PubMed

    Anufriev, Roman; Ramiere, Aymeric; Maire, Jeremie; Nomura, Masahiro

    2017-05-18

    Unlike classical heat diffusion at macroscale, nanoscale heat conduction can occur without energy dissipation because phonons can ballistically travel in straight lines for hundreds of nanometres. Nevertheless, despite recent experimental evidence of such ballistic phonon transport, control over its directionality, and thus its practical use, remains a challenge, as the directions of individual phonons are chaotic. Here, we show a method to control the directionality of ballistic phonon transport using silicon membranes with arrays of holes. First, we demonstrate that the arrays of holes form fluxes of phonons oriented in the same direction. Next, we use these nanostructures as directional sources of ballistic phonons and couple the emitted phonons into nanowires. Finally, we introduce thermal lens nanostructures, in which the emitted phonons converge at the focal point, thus focusing heat into a spot of a few hundred nanometres. These results motivate the concept of ray-like heat manipulations at the nanoscale.

  12. Suppression of Raman electron spin relaxation of radicals in crystals. Comparison of Cu2+ and free radical relaxation in triglycine sulfate and Tutton salt single crystals.

    PubMed

    Hoffmann, S K; Goslar, J; Lijewski, S

    2011-08-31

    Electron spin-lattice relaxation was measured by the electron spin echo method in a broad temperature range above 4.2 K for Cu(2+) ions and free radicals produced by ionizing radiation in triglycine sulfate (TGS) and Tutton salt (NH4)(2)Zn(SO4)2 ⋅ 6H2O crystals. Localization of the paramagnetic centres in the crystal unit cells was determined from continuous wave electron paramagnetic resonance spectra. Various spin relaxation processes and mechanisms are outlined. Cu(2+) ions relax fast via two-phonon Raman processes in both crystals involving the whole phonon spectrum of the host lattice. This relaxation is slightly slower for TGS where Cu(2+) ions are in the interstitial position. The ordinary Raman processes do not contribute to the radical relaxation which relaxes via the local phonon mode. The local mode lies within the acoustic phonon band for radicals in TGS but within the optical phonon range in (NH4)(2)Zn(SO4)2 ⋅ 6H2O. In the latter the cross-relaxation was considered. A lack of phonons around the radical molecules suggested a local crystal amorphisation produced by x- or γ-rays.

  13. Electron-phonon interaction in three-barrier nanosystems as active elements of quantum cascade detectors

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Tkach, N. V., E-mail: ktf@chnu.edu.ua; Seti, Ju. A.; Grynyshyn, Yu. B.

    2015-04-15

    The theory of electron tunneling through an open nanostructure as an active element of a quantum cascade detector is developed, which takes into account the interaction of electrons with confined and interface phonons. Using the method of finite-temperature Green’s functions and the electron-phonon Hamiltonian in the representation of second quantization over all system variables, the temperature shifts and electron-level widths are calculated and the contributions of different electron-phonon-interaction mechanisms to renormalization of the spectral parameters are analyzed depending on the geometrical configuration of the nanosystem. Due to weak electron-phonon coupling in a GaAs/Al{sub 0.34}Ga{sub 0.66}As-based resonant tunneling nanostructure, the temperaturemore » shift and rf field absorption peak width are not very sensitive to the electron-phonon interaction and result from a decrease in potential barrier heights caused by a difference in the temperature dependences of the well and barrier band gaps.« less

  14. Experimental and theoretical study of second-order Raman scattering in BaLiF 3

    NASA Astrophysics Data System (ADS)

    Mortier, M.; Gesland, J. Y.; Rousseau, M.

    1994-01-01

    Second-order Raman scattering is evidenced in the inverted cubic fluoroperovskite BaLiF 3. Spectra recorded from 300 to 20 K are interpreted from the thermally weighted two-phonons density-of- states calculated with a rigid ion model.

  15. Heat guiding and focusing using ballistic phonon transport in phononic nanostructures

    PubMed Central

    Anufriev, Roman; Ramiere, Aymeric; Maire, Jeremie; Nomura, Masahiro

    2017-01-01

    Unlike classical heat diffusion at macroscale, nanoscale heat conduction can occur without energy dissipation because phonons can ballistically travel in straight lines for hundreds of nanometres. Nevertheless, despite recent experimental evidence of such ballistic phonon transport, control over its directionality, and thus its practical use, remains a challenge, as the directions of individual phonons are chaotic. Here, we show a method to control the directionality of ballistic phonon transport using silicon membranes with arrays of holes. First, we demonstrate that the arrays of holes form fluxes of phonons oriented in the same direction. Next, we use these nanostructures as directional sources of ballistic phonons and couple the emitted phonons into nanowires. Finally, we introduce thermal lens nanostructures, in which the emitted phonons converge at the focal point, thus focusing heat into a spot of a few hundred nanometres. These results motivate the concept of ray-like heat manipulations at the nanoscale. PMID:28516909

  16. Raman spectra of Hg-based superconductors: Effect of oxygen defects

    NASA Astrophysics Data System (ADS)

    Zhou, Xingjiang; Cardona, M.; Chu, C. W.; Lin, Q. M.; Loureiro, S. M.; Marezio, M.

    1996-09-01

    Polarized micro-Raman scattering measurements have been performed on the five members of the HgBa2Can-1CunO2n+2+δ (n=1, 2, 3, 4, and 5) high-Tc superconductor family. A systematic evolution of the spectrum, which mainly involves oxygen-related phonons around 590, 570, 540, and 470 cm-1, with an increasing number of CuO2 layers, has been observed. Local laser annealing measurements clearly demonstrate that all these phonons are closely related to interstitial oxygen in the HgOδ planes. The origin of the spectrum evolution with the number of CuO2 layers lies in the variation of interstitial oxygen content.

  17. Effect of 10B isotope and vacancy defects on the phonon modes of two-dimensional hexagonal boron nitride

    NASA Astrophysics Data System (ADS)

    Sherajul Islam, Md.; Anindya, Khalid N.; Bhuiyan, Ashraful G.; Tanaka, Satoru; Makino, Takayuki; Hashimoto, Akihiro

    2018-02-01

    We report the details of the effects of the 10B isotope and those of B and N vacancies combined with the isotope on the phonon modes of two-dimensional hexagonal boron nitride (h-BN). The phonon density of states and localization problems are solved using the forced vibrational method, which is suitable for an intricate and disordered system. We observe an upward shift of Raman-active E2g-mode optical phonons (32 cm-1) for a 100% 10B isotope, which matches well with the experiment and simple harmonic oscillator model. However, a downward shift of E2g-mode phonons is observed for B or N vacancies and the combination of the isotope and vacancy-type disordered BN. Strong localized eigenmodes are found for all types of defects, and a typical localization length is on the order of ˜7 nm for naturally occurring BN samples. These results are very important for understanding the heat dissipation and electron transport properties of BN-based nanoelectronics.

  18. Resonant Raman spectra of diindenoperylene thin films

    NASA Astrophysics Data System (ADS)

    Scholz, R.; Gisslén, L.; Schuster, B.-E.; Casu, M. B.; Chassé, T.; Heinemeyer, U.; Schreiber, F.

    2011-01-01

    Resonant and preresonant Raman spectra obtained on diindenoperylene (DIP) thin films are interpreted with calculations of the deformation of a relaxed excited molecule with density functional theory (DFT). The comparison of excited state geometries based on time-dependent DFT or on a constrained DFT scheme with observed absorption spectra of dissolved DIP reveals that the deformation pattern deduced from constrained DFT is more reliable. Most observed Raman peaks can be assigned to calculated A_g-symmetric breathing modes of DIP or their combinations. As the position of one of the laser lines used falls into a highly structured absorption band, we have carefully analyzed the Raman excitation profile arising from the frequency dependence of the dielectric tensor. This procedure gives Raman cross sections in good agreement with the observed relative intensities, both in the fully resonant and in the preresonant case.

  19. Resonant Raman spectra of diindenoperylene thin films.

    PubMed

    Scholz, R; Gisslén, L; Schuster, B-E; Casu, M B; Chassé, T; Heinemeyer, U; Schreiber, F

    2011-01-07

    Resonant and preresonant Raman spectra obtained on diindenoperylene (DIP) thin films are interpreted with calculations of the deformation of a relaxed excited molecule with density functional theory (DFT). The comparison of excited state geometries based on time-dependent DFT or on a constrained DFT scheme with observed absorption spectra of dissolved DIP reveals that the deformation pattern deduced from constrained DFT is more reliable. Most observed Raman peaks can be assigned to calculated A(g)-symmetric breathing modes of DIP or their combinations. As the position of one of the laser lines used falls into a highly structured absorption band, we have carefully analyzed the Raman excitation profile arising from the frequency dependence of the dielectric tensor. This procedure gives Raman cross sections in good agreement with the observed relative intensities, both in the fully resonant and in the preresonant case.

  20. The temperature dependence of vibronic lineshapes: Linear electron-phonon coupling

    NASA Astrophysics Data System (ADS)

    Roos, Claudia; Köhn, Andreas; Gauss, Jürgen; Diezemann, Gregor

    2014-10-01

    We calculate the effect of a linear electron-phonon coupling on vibronic transitions of dye molecules of arbitrary complexity. With the assumption of known vibronic frequencies (for instance from quantum-chemical calculations), we give expressions for the absorption or emission lineshapes in a second-order cumulant expansion. We show that the results coincide with those obtained from generalized Redfield theory if one uses the time-local version of the theory and applies the secular approximation. Furthermore, the theory allows to go beyond the Huang-Rhys approximation and can be used to incorporate Dushinsky effects in the treatment of the temperature dependence of optical spectra. We consider both, a pure electron-phonon coupling independent of the molecular vibrations and a coupling bilinear in the molecular vibrational modes and the phonon coordinates. We discuss the behavior of the vibronic density of states for various models for the spectral density representing the coupling of the vibronic system to the harmonic bath. We recover some of the results that have been derived earlier for the spin-boson model and we show that the behavior of the spectral density at low frequencies determines the dominant features of the spectra. In case of the bilinear coupling between the molecular vibrations and the phonons we give analytical expressions for different spectral densities. The spectra are reminiscent of those obtained from the well known Brownian oscillator model and one finds a zero-phonon line and phonon-side bands located at vibrational frequencies of the dye. The intensity of the phonon-side bands diminishes with increasing vibrational frequencies and with decreasing coupling strength (Huang-Rhys factor). It vanishes completely in the Markovian limit where only a Lorentzian zero-phonon line is observed.

  1. Position sensitive detection of nuclear radiation mediated by non equilibrium phonons at low temperatures

    NASA Astrophysics Data System (ADS)

    Pröbst, F.; Peterreins, Th.; Feilitzsch, F. v.; Kraus, H.

    1990-03-01

    Many experiments in nuclear and particle physics would benefit from the development of a device capable of detecting non-ionizing events with a low energy threshold. In this context, we report on experimental tests of a detector based on the registration of nonequilibrium phonons. The device is composed of a silicon single crystal (size: 20×10×3 mm 3) and of an array of superconducting tunnel junctions evaporated onto the surface of the crystal. The junctions serve as sensors for phonons created by absorption of nuclear radiation in the crystal. We show how pulse height analysis and the investigation of time differences between correlated pulses in different junctions can be used to obtain information about the point of absorption.

  2. Effect of solution concentration on the structured order and optical properties of short-chain polyene biomolecules

    NASA Astrophysics Data System (ADS)

    Ouyang, Shunli; Sun, Chenglin; Zhou, Mi; Li, Dongfei; Wang, Weiwei; Qu, Guannan; Li, Zuowei; Gao, Shuqin; Yang, Jiange

    2010-09-01

    We have measured the Raman spectra and UV-Vis absorption spectra of linear polyene biomolecules (β-carotene and lycopene) in CS2 at low concentrations (10-6-10-10 mol/L). With decreasing concentration, all the carbon-carbon vibrations form a coherent mode in ordered β-carotene and lycopene due to extended π-conjugation that gives strong electron-phonon coupling, which leads to an anomalous experimental phenomenon. We observed an extremely high Raman scattering cross section( RSCS) and the Raman activities in β-carotene and lycopene are characterized by intensive overtones and combinations. Further, the UV-Vis absorption bands become narrower.

  3. Intrinsic Raman spectroscopy for quantitative biological spectroscopy Part II

    PubMed Central

    Bechtel, Kate L.; Shih, Wei-Chuan; Feld, Michael S.

    2009-01-01

    We demonstrate the effectiveness of intrinsic Raman spectroscopy (IRS) at reducing errors caused by absorption and scattering. Physical tissue models, solutions of varying absorption and scattering coefficients with known concentrations of Raman scatterers, are studied. We show significant improvement in prediction error by implementing IRS to predict concentrations of Raman scatterers using both ordinary least squares regression (OLS) and partial least squares regression (PLS). In particular, we show that IRS provides a robust calibration model that does not increase in error when applied to samples with optical properties outside the range of calibration. PMID:18711512

  4. Surface-enhanced Raman scattering on single-wall carbon nanotubes.

    PubMed

    Kneipp, Katrin; Kneipp, Harald; Dresselhaus, Mildred S; Lefrant, Serge

    2004-11-15

    Exploiting the effect of surface-enhanced Raman scattering (SERS), the Raman signal of single-wall carbon nanotubes (SWNTs) can be enhanced by up to 14 orders of magnitude when the tubes are in contact with silver or gold nanostructures and Raman scattering takes place predominantly in the enhanced local optical fields of the nanostructures. Such a level of enhancement offers exciting opportunities for ultrasensitive Raman studies on SWNTs and allows resonant and non-resonant Raman experiments to be done on single SWNTs at relatively high signal levels. Since the optical fields are highly localized within so-called "hot spots" on fractal silver colloidal clusters, lateral confinement of the Raman scattering can be as small as 5 nm, allowing spectroscopic selection of a single nanotube from a larger population. Moreover, since SWNTs are very stable "artificial molecules" with a high aspect ratio and a strong electron-phonon coupling, they are unique "test molecules" for investigating the SERS effect itself and for probing the "electromagnetic field contribution" and "charge transfer contribution" to the effect. SERS is also a powerful tool for monitoring the "chemical" interaction between the nanotube and the metal nanostructure.

  5. Enhancement of Raman scattering in dielectric nanostructures with electric and magnetic Mie resonances

    NASA Astrophysics Data System (ADS)

    Frizyuk, Kristina; Hasan, Mehedi; Krasnok, Alex; Alú, Andrea; Petrov, Mihail

    2018-02-01

    Resonantly enhanced Raman scattering in dielectric nanostructures has been recently proven to be an efficient tool for nanothermometry and for the experimental determination of their mode composition. In this paper we develop a rigorous analytical theory based on the Green's function approach to calculate the Raman emission from crystalline high-index dielectric nanoparticles. As an example, we consider silicon nanoparticles which have a strong Raman response due to active optical phonon modes. We relate enhancement of Raman signal emission to the Purcell effect due to the excitation of Mie modes inside the nanoparticles. We also employ our numerical approach to calculate inelastic Raman emission in more sophisticated geometries, which do not allow a straightforward analytical form of the Green's function. The Raman response from a silicon nanodisk has been analyzed with the proposed method, and the contribution of various Mie modes has been revealed.

  6. Strain effects on thermal conductivity of nanostructured silicon by Raman piezothermography

    NASA Astrophysics Data System (ADS)

    Murphy, Kathryn Fay

    A fundamental problem facing the rational design of materials is the independent control of electrical and thermal properties, with implications for a wide range of applications including thermoelectrics, solar thermal power generation, and thermal logic. One strategy for controlling transport involves manipulating the length scales which affect it. For instance, Si thermal conductivity may be reduced with relatively little change in electrical properties when the confining dimension (e.g., nanowire diameter) is small enough that heat carriers are preferentially scattered at free surfaces. However, tailoring properties by geometry or chemistry alone does not allow for on-demand modification, precluding applications which require responsive behavior such as thermal transistors, thermoelectric modules which adapt to their environmental temperature, or switchable thermal barriers. One means of tuning transport is elastic strain, which has long been exploited to improve carrier mobility in electronic devices. Uniform strain is predicted to affect thermal conductivity primarily via changes in heat capacity and phonon velocity, and crystalline defects such as vacancies or dislocations---which induce large strain gradients---should lower thermal conductivity by decreasing the phonon mean free path. Nanowires are ideal for the study of strain and defect effects due to the availability of a range of elastic strain an order of magnitude larger than in bulk and due to their small volumes. However, experimental measurements of strain-mediated thermal conductivity in nanowires have been limited due to the complexity of simultaneously applying and measuring stress or strain, heating, and measuring temperature. In this dissertation, we measure strain effects on thermal conductivity using a novel non-contact approach which we name Raman piezothermography. We apply a uniaxial load to individual Si nanowires, Si thin films, and Si micromeshes under a confocal mu-Raman microscope and

  7. Performance Modeling of an Airborne Raman Water Vapor Lidar

    NASA Technical Reports Server (NTRS)

    Whiteman, D. N.; Schwemmer, G.; Berkoff, T.; Plotkin, H.; Ramos-Izquierdo, L.; Pappalardo, G.

    2000-01-01

    A sophisticated Raman lidar numerical model had been developed. The model has been used to simulate the performance of two ground-based Raman water vapor lidar systems. After tuning the model using these ground-based measurements, the model is used to simulate the water vapor measurement capability of an airborne Raman lidar under both day-and night-time conditions for a wide range of water vapor conditions. The results indicate that, under many circumstances, the daytime measurements possess comparable resolution to an existing airborne differential absorption water vapor lidar while the nighttime measurement have higher resolution. In addition, a Raman lidar is capable of measurements not possible using a differential absorption system.

  8. Mid-infrared emission and Raman spectra analysis of Er(3+)-doped oxyfluorotellurite glasses.

    PubMed

    Chen, Fangze; Xu, Shaoqiong; Wei, Tao; Wang, Fengchao; Cai, Muzhi; Tian, Ying; Xu, Shiqing

    2015-04-10

    This paper reports on the spectroscopic and structural properties in Er(3+)-doped oxyfluorotellurite glasses. The compositional variation accounts for the evolutions of Raman spectra, Judd-Ofelt parameters, radiative properties, and fluorescent emission. It is found that, when maximum phonon energy changes slightly, phonon density plays a crucial role in quenching the 2.7 μm emission generated by the Er(3+):(4)I11/2→(4)I13/2 transition. The comparative low phonon density contributes strong 2.7 μm emission intensity. The high branching ratio (18.63%) and large emission cross section (0.95×10(-20)  cm(2)) demonstrate that oxyfluorotellurite glass contained with 50 mol.% TeO2 has potential application in the mid-infrared region laser.

  9. Inverse Edelstein effect induced by magnon-phonon coupling

    NASA Astrophysics Data System (ADS)

    Xu, Mingran; Puebla, Jorge; Auvray, Florent; Rana, Bivas; Kondou, Kouta; Otani, Yoshichika

    2018-05-01

    We demonstrate a spin to charge current conversion via magnon-phonon coupling and an inverse Edelstein effect on the hybrid device Ni/Cu (Ag )/Bi 2O3 . The generation of spin current (Js≈108A/m2 ) due to magnon-phonon coupling reveals the viability of acoustic spin pumping as a mechanism for the development of spintronic devices. A full in-plane magnetic field angle dependence of the power absorption and a combination of longitudinal and transverse voltage detection reveals the symmetric and asymmetric components of the inverse Edelstein effect voltage induced by Rayleigh-type surface acoustic waves. While the symmetric components are well studied, asymmetric components still need to be explored. We assign the asymmetric contributions to the interference between longitudinal and shear waves and an anisotropic charge distribution in our hybrid device.

  10. Temperature dependent Raman investigation of multiwall carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Dilawar Sharma, Nita; Singh, Jasveer; Vijay, Aditi

    2018-04-01

    We report anomalous observations in our investigations of the temperature dependent Raman spectroscopic measurement of multiwall carbon nanotubes. The Micro-Raman spectra were recorded with the laser source having 514.5 nm wavelength and within the temperature range of 80-440 K. The major Raman bands, the G and D band, are observed at 1584 and 1348 cm-1, respectively, at ambient. The absence of the radial breathing mode confirms the multiwall nature of carbon nanotubes. It has been observed that with an increase in the temperature above 120 K, there is a shift in Raman bands towards the higher wave-number region. However, a drop in the G and D bands is observed from 80 to 120 K which was not observed for the second order band. Thereafter, all Raman modes exhibited mode hardening up to about 320 K followed by mild softening of the phonon modes. Linear temperature coefficients were found to have higher contribution to mode hardening as compared to higher order terms. Total anharmonicity estimation shows a predominant effect of the quasi-harmonic term as compared to the true anharmonic term.

  11. Layer-Dependent Ultrafast Carrier and Coherent Phonon Dynamics in Black Phosphorus.

    PubMed

    Miao, Xianchong; Zhang, Guowei; Wang, Fanjie; Yan, Hugen; Ji, Minbiao

    2018-05-09

    Black phosphorus is a layered semiconducting material, demonstrating strong layer-dependent optical and electronic properties. Probing the photophysical properties on ultrafast time scales is of central importance in understanding many-body interactions and nonequilibrium quasiparticle dynamics. Here, we applied temporally, spectrally, and spatially resolved pump-probe microscopy to study the transient optical responses of mechanically exfoliated few-layer black phosphorus, with layer numbers ranging from 2 to 9. We have observed layer-dependent resonant transient absorption spectra with both photobleaching and red-shifted photoinduced absorption features, which could be attributed to band gap renormalization of higher subband transitions. Surprisingly, coherent phonon oscillations with unprecedented intensities were observed when the probe photons were in resonance with the optical transitions, which correspond to the low-frequency layer-breathing mode. Our results reveal strong Coulomb interactions and electron-phonon couplings in photoexcited black phosphorus, providing important insights into the ultrafast optical, nanomechanical, and optoelectronic properties of this novel two-dimensional material.

  12. Absorption and resonance Raman spectra of Pb2, Pb3 and Pb4 in xenon matrices

    NASA Technical Reports Server (NTRS)

    Stranz, D. D.; Khanna, R. K.

    1980-01-01

    Lead metal was vaporized and trapped in solid xenon at 12K. Electronic absorption and resonance Raman spectra were recorded of the resulting matrix, which was shown to contain Pb2, Pb3, and possibly Pb4 molecular species. The vibrational frequency for Pb2 is determined to be 108/cm for the ground state, with a dissociation energy of 82000/cm. Ad3h symmetry is indicated for the Pb3 species, with nu sub 1=117/cm and nu sub 2 = 96 /cm. The existence of Pb4 is suggested by a fundamental and overtone of 111/cm spacing.

  13. Raman scattering excitation spectroscopy of monolayer WS2.

    PubMed

    Molas, Maciej R; Nogajewski, Karol; Potemski, Marek; Babiński, Adam

    2017-07-11

    Resonant Raman scattering is investigated in monolayer WS 2 at low temperature with the aid of an unconventional technique, i.e., Raman scattering excitation (RSE) spectroscopy. The RSE spectrum is made up by sweeping the excitation energy, when the detection energy is fixed in resonance with excitonic transitions related to either neutral or charged excitons. We demonstrate that the shape of the RSE spectrum strongly depends on the selected detection energy. The resonance of outgoing light with the neutral exciton leads to an extremely rich RSE spectrum, which displays several Raman scattering features not reported so far, while no clear effect on the associated background photoluminescence is observed. Instead, when the outgoing photons resonate with the negatively charged exciton, a strong enhancement of the related emission occurs. Presented results show that the RSE spectroscopy can be a useful technique to study electron-phonon interactions in thin layers of transition metal dichalcogenides.

  14. Coherent Phonon Rabi Oscillations with a High-Frequency Carbon Nanotube Phonon Cavity.

    PubMed

    Zhu, Dong; Wang, Xin-He; Kong, Wei-Cheng; Deng, Guang-Wei; Wang, Jiang-Tao; Li, Hai-Ou; Cao, Gang; Xiao, Ming; Jiang, Kai-Li; Dai, Xing-Can; Guo, Guang-Can; Nori, Franco; Guo, Guo-Ping

    2017-02-08

    Phonon-cavity electromechanics allows the manipulation of mechanical oscillations similar to photon-cavity systems. Many advances on this subject have been achieved in various materials. In addition, the coherent phonon transfer (phonon Rabi oscillations) between the phonon cavity mode and another oscillation mode has attracted many interest in nanoscience. Here, we demonstrate coherent phonon transfer in a carbon nanotube phonon-cavity system with two mechanical modes exhibiting strong dynamical coupling. The gate-tunable phonon oscillation modes are manipulated and detected by extending the red-detuned pump idea of photonic cavity electromechanics. The first- and second-order coherent phonon transfers are observed with Rabi frequencies 591 and 125 kHz, respectively. The frequency quality factor product fQ m ∼ 2 × 10 12 Hz achieved here is larger than k B T base /h, which may enable the future realization of Rabi oscillations in the quantum regime.

  15. Direct observation of mode-specific phonon-band gap coupling in methylammonium lead halide perovskites.

    PubMed

    Kim, Heejae; Hunger, Johannes; Cánovas, Enrique; Karakus, Melike; Mics, Zoltán; Grechko, Maksim; Turchinovich, Dmitry; Parekh, Sapun H; Bonn, Mischa

    2017-09-25

    Methylammonium lead iodide perovskite is an outstanding semiconductor for photovoltaics. One of its intriguing peculiarities is that the band gap of this perovskite increases with increasing lattice temperature. Despite the presence of various thermally accessible phonon modes in this soft material, the understanding of how precisely these phonons affect macroscopic material properties and lead to the peculiar temperature dependence of the band gap has remained elusive. Here, we report a strong coupling of a single phonon mode at the frequency of ~ 1 THz to the optical band gap by monitoring the transient band edge absorption after ultrafast resonant THz phonon excitation. Excitation of the 1 THz phonon causes a blue shift of the band gap over the temperature range of 185 ~ 300 K. Our results uncover the mode-specific coupling between one phonon and the optical properties, which contributes to the temperature dependence of the gap in the tetragonal phase.Methylammonium lead iodide perovskite, a promising material for efficient photovoltaics, shows a unique temperature dependence of its optical properties. Kim et al. quantify the coupling between the optical gap and a lattice phonon at 1 THz, which favorably contributes to the thermal variation of the gap.

  16. Absorption and resonance Raman study of the pyromellitic diahydride anion via density functional theory

    NASA Astrophysics Data System (ADS)

    Andruniow, T.; Pawlikowski, M.

    2000-05-01

    The electronic structure of the low-energy states of the pyromellitic diahydride (PMDA) anion is investigated in terms of the VWN (Vosco-Wilk-Nusair) the BP (Becke-Perdew) and the B3LYP density functional (DF) methods employed with 6-31G * basis sets. All the methods are shown to reproduce correctly the absorption and resonance Raman spectra in the region corresponding to the low-energy 1 2Au→1 2B3g transition. The discrepancies between the theory and experiment are attributed to a (weak) Dushinsky effect predominately due to a mixing of the ν3=1593 cm -1 and ν4=1342 cm -1 vibrations in the 1 2B3 g state of the PMDA radical.

  17. Excitation of phonons in medium-energy electron diffraction

    NASA Astrophysics Data System (ADS)

    Alvarez, M. A. Vicente; Ascolani, H.; Zampieri, G.

    1996-03-01

    The ``elastic'' backscattering of electrons from crystalline surfaces presents two regimes: a low-energy regime, in which the characteristic low-energy electron diffraction (LEED) pattern is observed, and a medium-energy regime, in which the diffraction pattern is similar to those observed in x-ray photoemission diffraction (XPD) and Auger electron diffraction (AED) experiments. We present a model for the electron scattering which, including the vibrational degrees of freedom of the crystal, contains both regimes and explains the passage from one regime to the other. Our model is based on a separation of the electron and atomic motions (adiabatic approximation) and on a cluster-type formulation of the multiple scattering of the electron. The inelastic scattering events (excitation and/or absorption of phonons) are treated as coherent processes and no break of the phase relation between the incident and the exit paths of the electron is assumed. The LEED and the medium-energy electron diffraction regimes appear naturally in this model as the limit cases of completely elastic scattering and of inelastic scattering with excitation and/or absorption of multiple phonons. Intensity patterns calculated with this model are in very good agreement with recent experiments of electron scattering on Cu(001) at low and medium energies. We show that there is a correspondence between the type of intensity pattern and the mean number of phonons excited and/or absorbed during the scattering: a LEED-like pattern is observed when this mean number is less than 2, LEED-like and XPD/AED-like features coexist when this number is 3-4, and a XPD/AED-like pattern is observed when this number is greater than 5-6.

  18. Ab initio calculation of resonant Raman intensities of transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Miranda, Henrique; Reichardt, Sven; Molina-Sanchez, Alejandro; Wirtz, Ludger

    Raman spectroscopy is used to characterize optical and vibrational properties of materials. Its computational simulation is important for the interpretation of experimental results. Two approaches are the bond polarizability model and density functional perturbation theory. However, both are known to not capture resonance effects. These resonances and quantum interference effects are important to correctly reproduce the intensities as a function of laser energy as, e.g., reported for the case of multi-layer MoTe21.We present two fully ab initio approaches that overcome this limitation. In the first, we calculate finite difference derivatives of the dielectric susceptibility with the phonon displacements2. In the second we calculate electron-light and electron-phonon matrix elements from density functional theory and use them to evaluate expressions for the Raman intensity derived from time-dependent perturbation theory. These expressions are implemented in a computer code that performs the calculations as a post-processing step. We compare both methods and study the case of triple-layer MoTe2. Luxembourg National Research Fund (FNR).

  19. Phonon shift in chemically exfoliated WS2 nanosheet

    NASA Astrophysics Data System (ADS)

    Sarkar, Abdus Salam; Pal, Suman Kalyan

    2018-04-01

    We have synthesized few layer WS2 nanosheets in a low boiling point solvent. Few layer of WS2 sheets are characterized by various techniques such as UV-visible and Raman spectroscopy, transmission electron microscopy (TEM), atomic force microscopy (AFM) and scanning electron microscopy (SEM). UV-Vis absorption spectra confirm the well dispersed in isopropyl alcohol. SEM and TEM images indicate the sheet like morphology of WS2. Atomic force microscopy image and room temperature Raman spectroscopy confirm the exfoliation of few layer (4-5 layer) of WS2. Further, Raman spectroscopy was used as a meteorology tool to determine the temperature co-efficient. We have systematically investigated the temperature dependent Raman spectroscopic behavior of few layer WS2. Our results depict the softening of the Raman modes E12g in plane vibration and A1g out of plane vibration with increasing the temperature from 77 K to 300 K. Softening of the Raman modes could be explained in terms of the double resonance which is active in the layered materials. The observed temperature coefficients for two Raman peaks E12g and A1g, are - 0.022 cm-1 and -0.009 cm-1, respectively.

  20. Surface-enhanced Raman spectroscopy of urine by an ingenious near-infrared Raman spectrometer

    NASA Astrophysics Data System (ADS)

    Feng, Shangyuan; Chen, Weiwei; Li, Yongzeng; Chen, Guannan; Huang, Zufang; Liao, Xiaohua; Xie, Zhiming; Chen, Rong

    2007-11-01

    This paper demonstrates the potential of an elaborately devised near-infrared Raman system in analysis of urine. The broad band in the long-wavelength region of the electronic absorption spectra of the sol with added adsorbent at certain concentrations has been explained in terms of the aggregation of the colloidal silver particles. We have reported the surface-enhanced Raman (SERS) spectra of urine, and studied the silver solution enhanced effects on the urine Raman scattering. The Raman bands of human's urine was assigned to certain molecule vibrations. We have found that different donators have dissimilar SERS of urine in different physiological condition. Comparatively few studies have explored the ability of Raman spectroscopy for the analysis of urine acid. In the present report, we investigated the ability of surface enhanced Raman spectroscopy to measure uric acid in the human urine. The results suggested that the present Raman system holds considerable promise for practical use. Practical applications such as the quantitative medical examination of urine metabolites may also be feasible in the near future.

  1. Correlated phonons and the Tc-dependent dynamical phonon anomalies

    NASA Astrophysics Data System (ADS)

    Hakioğlu, T.; Türeci, H.

    1997-11-01

    Anomalously large low-temperature phonon anharmonicities can lead to static as well as dynamical changes in the low-temperature properties of the electron-phonon system. In this work, we focus our attention on the dynamically generated low-temperature correlations in an interacting electron-phonon system using a self-consistent dynamical approach in the intermediate coupling range. In the context of the model, the polaron correlations are produced by the charge-density fluctuations which are generated dynamically by the electron-phonon coupling. Conversely, the latter is influenced in the presence of the former. The purpose of this work is to examine the dynamics of this dual mechanism between the two using the illustrative Fröhlich model. In particular, the influence of the low-temperature phonon dynamics on the superconducting properties in the intermediate coupling range is investigated. The influence on the Holstein reduction factor as well as the enhancement in the zero-point fluctuations and in the electron-phonon coupling are calculated numerically. We also examine these effects in the presence of superconductivity. Within this model, the contribution of the electron-phonon interaction as one of the important elements in the mechanisms of superconductivity can reach values as high as 15-20% of the characteristic scale of the lattice vibrational energy. The second motivation of this work is to understand the nature of the Tc-dependent temperature anomalies observed in the Debye-Waller factor, dynamical pair correlations, and average atomic vibrational energies for a number of high-temperature superconductors. In our approach we do not claim nor believe that the electron-phonon interaction is the primary mechanism leading to high-temperature superconductivity. Nevertheless, our calculations suggest that the dynamically induced low-temperature phonon correlation model can account for these anomalies and illustrates their possible common origin. Finally, the

  2. Red shifts of the Eg(1) Raman mode of nanocrystalline TiO2:Er monoliths grown by sol-gel process

    NASA Astrophysics Data System (ADS)

    Palomino-Merino, R.; Trejo-Garcia, P.; Portillo-Moreno, O.; Jiménez-Sandoval, S.; Tomás, S. A.; Zelaya-Angel, O.; Lozada-Morales, R.; Castaño, V. M.

    2015-08-01

    Nanocrystalline monoliths of Er doped TiO2 were prepared by the sol-gel technique, by controlling the Er-doping levels into the TiO2 precursor solution. As-prepared and annealed in air samples showed the anatase TiO2 phase. The average diameter of the nanoparticles ranged from 19 to 2.6 nm as the nominal concentration of Er varies from 0% to 7%, as revealed by EDS analysis in an electron microscope. Photo Acoustic Spectroscopy (PAS) allowed calculate the forbidden band gap, evidencing an absorption edge at around 300 nm, attributed to TiO2 and evidence of electronic transitions or Er3+. The Raman spectra, corresponding to the anatase phase, show the main phonon mode Eg(1) band position at 144 cm-1 with a red shift for the annealing samples.

  3. Fast Xe-129 relaxation in solid xenon near its melting point: Cross-over from Raman scattering of phonons to vacancy diffusion.

    NASA Astrophysics Data System (ADS)

    Kuzma, N. N.; Patton, B.; Raman, K.; Happer, W.

    2002-03-01

    NMR measurements of longitudinal relaxation times T1 in pure solid xenon were carried out using both natural-abundance and isotopically-enriched samples of hyperpolarized ^129Xe. At temperatures below 120 K and fields above 500 Gauss, the relaxation rate 1/T1 is field- and abundance-independent, consistent with the model of ^129Xe spin-flip Raman scattering of phonons(R. J. Fitzgerald et al.), Phys. Rev. B 59, 8795 (1999).. Above 120 K, vacancies invade the xenon lattice(P. R. Granfors et al.) Phys. Rev. B 24, 4753 (1981)., and a dramatic cross-over to the nuclear dipole-dipole relaxation due to the diffusion of vacancies is observed. As a result, the measured relaxation times of xenon near its melting point strongly depend on field and somewhat on ^129Xe abundance, and can be as short as several seconds, leading to potential difficulties in cryogenic applications of hyperpolarized ^129Xe. The data are analyzed using the theory of nuclear relaxation due to spin diffusion in cubic crystals(C. A. Sholl, J. Phys. C 21), 319 (1988)., and some estimates of the vacancy density and jump rates are discussed.

  4. Two-Magnon Raman Scattering and Pseudospin-Lattice Interactions in Sr_{2}IrO_{4} and Sr_{3}Ir_{2}O_{7}.

    PubMed

    Gretarsson, H; Sung, N H; Höppner, M; Kim, B J; Keimer, B; Le Tacon, M

    2016-04-01

    We have used Raman scattering to investigate the magnetic excitations and lattice dynamics in the prototypical spin-orbit Mott insulators Sr_{2}IrO_{4} and Sr_{3}Ir_{2}O_{7}. Both compounds exhibit pronounced two-magnon Raman scattering features with different energies, line shapes, and temperature dependencies, which in part reflect the different influence of long-range frustrating exchange interactions. Additionally, we find strong Fano asymmetries in the line shapes of low-energy phonon modes in both compounds, which disappear upon cooling below the antiferromagnetic ordering temperatures. These unusual phonon anomalies indicate that the spin-orbit coupling in Mott-insulating iridates is not sufficiently strong to quench the orbital dynamics in the paramagnetic state.

  5. Correlation of TEM data with confined phonons to determine strain and size of Ge nanocrystals embedded in SixNy matrix

    NASA Astrophysics Data System (ADS)

    Bahariqushchi, Rahim; Gündoğdu, Sinan; Aydinli, Atilla

    2017-11-01

    Models that use phonon confinement fail to provide consistent results for nanocrystal sizes in differing dielectric matrices due to varying stress experienced by nanocrystals in different dielectric environments. In cases where direct measurement of stress is difficult, the possibility of stress saturation as a function of size opens up a window for the use of phonon confinement to determine size. We report on a test of this possibility in Ge: SixNy system. Ge nanocrystals (NCs) embedded in silicon nitride matrix have been fabricated using plasma enhanced chemical vapor deposition (PECVD) followed by post annealing in Ar ambient. Nanocrystal size dependence of Raman spectra was studied taking into account associated stress and an improved phonon confinement approach. Our analysis show same stress for NCs which have sizes below 7.0 nm allowing the use of phonon confinement to determine the nanocrystal size. The results are compared with TEM data and good agreement is observed.

  6. Superlubrication by phonon confinement

    NASA Astrophysics Data System (ADS)

    Wada, Noriyuki; Ishikawa, Makoto; Shiga, Takuma; Shiomi, Junichiro; Suzuki, Masaru; Miura, Kouji

    2018-04-01

    The superlubrication described here, involving confined phonons, is easily achievable and very simple because it uses only submicron islands, smaller than the mean free path of the phonons, to confine phonons. We can achieve superlubrication with a friction force of piconewton order at the submicron island. We can call this phononic lubrication or self-lubrication because phonons induced by tip shearing are confined within the submicron islands and decrease the friction during the subsequent sliding. Phonon confinement should make it possible to directly develop applications for lubricants and ultimately to open a novel avenue of tribology.

  7. Universal link between the boson peak and transverse phonons in glass.

    PubMed

    Shintani, Hiroshi; Tanaka, Hajime

    2008-11-01

    The physical properties of a topologically disordered amorphous material (glass), such as heat capacity and thermal conductivity, are markedly different from those of its ordered crystalline counterpart. The understanding of these phenomena is a notoriously complex problem. One of the universal features of disordered glasses is the 'boson peak', which is observed in neutron and Raman scattering experiments. The boson peak is typically ascribed to an excess density of vibrational states. Here, we study the nature of the boson peak, using numerical simulations of several glass-forming systems. We discovered evidence suggestive of the equality of the boson peak frequency to the Ioffe-Regel limit for 'transverse' phonons, above which transverse phonons no longer propagate. Our results indicate a possibility that the origin of the boson peak is transverse vibrational modes associated with defective soft structures in the disordered state. Furthermore, we suggest a possible link between slow structural relaxation and fast boson peak dynamics in glass-forming systems.

  8. Phonon assisted electronic transition in telluric acid ammonium phosphate single crystals

    NASA Astrophysics Data System (ADS)

    El-Muraikhi, M.; Kassem, M. E.; Al-Houty, L.

    The effect of gamma-irradiation on the absorption optical spectra of telluric acid ammonium phosphate single crystals (TAAP) has been studied, in the wave length of 200-600 nm, for samples irradiated by various doses up to 10 Mrad. The results show that the electron phonon coupling constant increases with the irradiation dose.

  9. X-ray absorption and Raman spectroscopy studies of molybdenum environments in borosilicate waste glasses

    NASA Astrophysics Data System (ADS)

    McKeown, David A.; Gan, Hao; Pegg, Ian L.

    2017-05-01

    Mo-containing high-level nuclear waste borosilicate glasses were investigated as part of an effort to improve Mo loading while avoiding yellow phase crystallization. Previous work showed that additions of vanadium decrease yellow phase formation and increases Mo solubility. X-ray absorption spectroscopy (XAS) and Raman spectroscopy were used to characterize Mo environments in HLW borosilicate glasses and to investigate possible structural relationships between Mo and V. Mo XAS spectra for the glasses indicate isolated tetrahedral Mo6+O4 with Mo-O distances near 1.75 Å. V XANES indicate tetrahedral V5+O4 as the dominant species. Raman spectra show composition dependent trends, where Mo-O symmetrical stretch mode frequencies (ν1) are sensitive to the mix of alkali and alkaline earth cations, decreasing by up to 10 cm-1 for glasses that change from Li+ to Na+ as the dominant network-modifying species. This indicates that MoO4 tetrahedra are isolated from the borosilicate network and are surrounded, at least partly, by Na+ and Li+. Secondary ν1 frequency effects, with changes up to 7 cm-1, were also observed with increasing V2O5 and MoO3 content. These secondary trends may indicate MoO4-MoO4 and MoO4-VO4 clustering, suggesting that V additions may stabilize Mo in the matrix with respect to yellow phase formation.

  10. Optical and biological properties of plasma-treated Neurospora crassa spores as studied by absorption, circular dichroism, and Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Lee, Geon Joon; Park, Gyungsoon; Choi, Eun Ha

    2017-11-01

    We studied the effect of plasma treatment on the optical, structural and biological properties of Neurospora crassa ( N. crassa) spores. An atmospheric-pressure plasma jet (APPJ) was used to generate reactive oxygen and nitrogen species in aqueous solution. The APPJ treatment of N. crassa spores in water significantly reduced the viability of spores. The reduction in the spore viability can be attributed to the reactive species from the plasma itself and those derived from the reaction of plasma radicals with aqueous solution. These structural modifications were contingent on the medium in which N. crassa spores were suspended; plasma treatment of N. crassa spores in PBS did not significantly affect the viability of spores as compared with N. crassa spores in water. Scanning electron microscopy images and circular dichroism spectra indicated that the spore cell wall was damaged by plasma treatment. The optical absorption spectrum of untreated N. crassa spores exhibited two resonance absorption bands at approximately λ1 ≈ 260 nm and λ2 ≈ 472 nm, originating from deoxyribonucleic acid (DNA) and β-carotene. The Raman spectrum of untreated N. crassa spores exhibited three main peaks at 1519, 1157 and 1006 cm -1, attributed to β-carotene inside the cell wall. The Raman spectra showed that the APPJ treatment of N. crassa spores in water caused degradation of β-carotene, affecting the viability of spores.

  11. Enhanced Raman Scattering from NCM523 Cathodes Coated with Electrochemically Deposited Gold

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Tornheim, Adam; Maroni, Victor A.; He, Meinan

    Materials with the general composition LiMO2, where M is a mix of nickel, cobalt, and manganese, have been studied extensively as cathodes for lithium-based electrochemical cells. Some compositions, like LiNi0.5Co0.2Mn0.3O2 (NCM523), have already found application in commercial lithium-ion batteries. Pre-test and post-test analyses of these types of cathodes have benefited greatly from the use of Raman spectroscopy. Specifically, Raman spectroscopy can be used to investigate the phonons of the LiMO2 lattice. This is particularly useful for studies of the LiMO2 after it has been formed into the type of polymer-bonded laminate from which typical battery cathodes are cut. One ofmore » the problems that occurs in such studies is that the scattering from the LiMO2 phase gets progressively weaker as the nickel content increases. NCM523 poses one example of this behavior owing to the fact that half of the transition metal content is nickel. In this study we show that the intensity of the Raman scattering from the NCM523 phonons can be significantly increased by electroplating clusters of sub-micron gold particles on NCM523-containing laminate structures. The gold appears to plate somewhat selectively on the NCM523 particles in randomly sized clusters. These clusters stimulate the Raman scattering from the NCM523 to varying extents that can reach nearly 100 times the scattering intensity from uncoated pristine laminates.« less

  12. Raman study of transition-metal oxides with perovskite-like structure

    NASA Astrophysics Data System (ADS)

    Kolev, Nikolay Iliev

    Perovskite-like oxides exhibit a rich variety of properties of fundamental scientific interest and potential application value. The motivation for this work is to contribute to our knowledge of perovskite-like systems and strongly correlated systems in general. The polarized Raman spectra of single crystal and thin film CaCu3Ti4O12, single crystal and thin film CaRuO3, microcrystals of La0.5Ca 0.5MnO3, and ceramic and thin film CaMnO3 have been investigated. In close comparison to results from lattice dynamics calculations most of the Raman lines in the CaCu3Ti4O12, CaRuO3, La0.5Ca0.5MnO3 and CaMnO 3 spectra, have been assigned to definite phonon modes. The validity of the model for twin orientation in the Pnma structure for CaRuO3 and La0.5Ca0.5MnO3 is confirmed. The analysis of the CaMnO3 spectra contributed to the development of a model, based on four basic distortions of the (distorted) perovskite structure. The temperature behavior of the CaCu3Ti4O 12 spectra shows that there is no evidence for structural phase transition in the temperature range 20--600 K, so such a transition cannot be responsible for the sharp drop in the dielectric constant below 100 K. The Raman spectra indirectly support the mechanism of formation of barrier layer capacitances in CaCu3Ti4O12.The observation of additional Raman mode of nominal Ag symmetry is discussed in terms of coexistence of domains of different atomic arrangement, or alternatively of non-stoichiometry (Cu deficiency). In the case of the thin film, the tetragonal distortions could be responsible for the greater separation of the additional Ag line. No anomalies in the temperature behavior of the Raman lines of CaRuO3 is observed, which is an indirect evidence for its lack of long-range magnetic ordering at low temperatures (depending on whether this ordering would be observable by Raman spectroscopy through spin-phonon coupling). In La0.5Ca0.5MnO 3 the appearance of several Raman lines below TN is analyzed in terms of

  13. Raman tensor elements for tetragonal BaTiO3 and their use for in-plane domain texture assessments

    NASA Astrophysics Data System (ADS)

    Deluca, Marco; Higashino, Masayuki; Pezzotti, Giuseppe

    2007-08-01

    A quantitative assessment of c-axis oriented domains in a textured BaTiO3 (BT) single crystal has been carried out by polarized Raman microprobe spectroscopy. The relative intensity modulation of the Raman phonon modes has been theoretically modeled as a function of crystal rotation and linked to the volume fraction of c-axis oriented domains. Raman tensor elements have also been experimentally determined for the Ag and B1 vibrational modes. As an application, the internal in-plane texture and the volume fraction of c-oriented domains in the BT single crystal have been nondestructively visualized by monitoring the relative intensity of Ag and B1 Raman modes.

  14. Dynamically tunable extraordinary light absorption in monolayer graphene

    NASA Astrophysics Data System (ADS)

    Safaei, Alireza; Chandra, Sayan; Vázquez-Guardado, Abraham; Calderon, Jean; Franklin, Daniel; Tetard, Laurene; Zhai, Lei; Leuenberger, Michael N.; Chanda, Debashis

    2017-10-01

    The high carrier mobility of graphene makes it an attractive material for electronics, however, graphene's application for optoelectronic systems is limited due to its low optical absorption. We present a cavity-coupled nanopatterned graphene absorber designed to sustain temporal and spatial overlap between localized surface plasmon resonance and cavity modes, thereby resulting in enhanced absorption up to an unprecedented value of theoretically (60 %) and experimentally measured (45 %) monolayer graphene in the technologically relevant 8-12-μm atmospheric transparent infrared imaging band. We demonstrate a wide electrostatic tunability of the absorption band (˜2 μ m ) by modifying the Fermi energy. The proposed device design allows enhanced absorption and dynamic tunability of chemical vapor deposition grown low carrier mobility graphene which provides a significant advantage over previous strategies where absorption enhancement was limited to exfoliated high carrier mobility graphene. We developed an analytical model that incorporates the coupling of the graphene electron and substrate phonons, providing valuable and instructive insights into the modified plasmon-phonon dispersion relation necessary to interpret the experimental observations. Such gate voltage and cavity tunable enhanced absorption in chemical vapor deposited large area monolayer graphene paves the path towards the scalable development of ultrasensitive infrared photodetectors, modulators, and other optoelectronic devices.

  15. Dramatic Raman Gain Suppression in the Vicinity of the Zero Dispersion Point in a Gas-Filled Hollow-Core Photonic Crystal Fiber.

    PubMed

    Bauerschmidt, S T; Novoa, D; Russell, P St J

    2015-12-11

    In 1964 Bloembergen and Shen predicted that Raman gain could be suppressed if the rates of phonon creation and annihilation (by inelastic scattering) exactly balance. This is only possible if the momentum required for each process is identical, i.e., phonon coherence waves created by pump-to-Stokes scattering are identical to those annihilated in pump-to-anti-Stokes scattering. In bulk gas cells, this can only be achieved over limited interaction lengths at an oblique angle to the pump axis. Here we report a simple system that provides dramatic Raman gain suppression over long collinear path lengths in hydrogen. It consists of a gas-filled hollow-core photonic crystal fiber whose zero dispersion point is pressure adjusted to lie close to the pump laser wavelength. At a certain precise pressure, stimulated generation of Stokes light in the fundamental mode is completely suppressed, allowing other much weaker phenomena such as spontaneous Raman scattering to be explored at high pump powers.

  16. Some aspects of pulsed laser deposition of Si nanocrystalline films

    NASA Astrophysics Data System (ADS)

    Polyakov, B.; Petruhins, A.; Butikova, J.; Kuzmin, A.; Tale, I.

    2009-11-01

    Nanocrystalline silicon films were deposited by a picosecond laser ablation on different substrates in vacuum at room temperature. A nanocrystalline structure of the films was evidenced by atomic force microscopy (AFM), optical and Raman spectroscopies. A blue shift of the absorption edge was observed in optical absorption spectra, and a decrease of the optical phonon energy at the Brillouin zone centre was detected by Raman scattering. Early stages of nanocrystalline film formation on mica and HOPG substrates were studied by AFM. Mechanism of nanocrystal growth on substrate is discussed. in here

  17. Evidence of Longitudinal Acoustic Phonon Generation in Si Doping Superlattices by Ge Prism-Coupled THz Laser Radiation

    NASA Astrophysics Data System (ADS)

    Wilson, T.; Kasper, E.; Oehme, M.; Schulze, J.; Korolev, K.

    2014-11-01

    We report on the direct excitation of 246 GHz longitudinal acoustic phonons in silicon doping superlattices by the resonant absorption of nanosecond-pulsed far-infrared laser radiation of the same frequency. A longitudinally polarized evanescent laser light field is coupled to the superlattice through a germanium prism providing total internal reflection at the superlattice interface. The ballistic phonon signal is detected by a superconducting aluminum bolometer. The sample is immersed in low-temperature liquid helium.

  18. Raman structural studies of the nickel electrode

    NASA Technical Reports Server (NTRS)

    Cornilsen, Bahne C.

    1994-01-01

    The objectives of this investigation have been to define the structures of charged active mass, discharged active mass, and related precursor materials (alpha-phases), with the purpose of better understanding the chemical and electrochemical reactions, including failure mechanisms and cobalt incorporation, so that the nickel electrode may be improved. Although our primary tool has been Raman spectroscopy, the structural conclusions drawn from the Raman data have been supported and augmented by three other analysis methods: infrared spectroscopy, powder X-ray Diffraction (XRD), and x-ray absorption spectroscopy (in particular EXAFS, Extended X-ray Absorption Fine Structure spectroscopy).

  19. Negative refraction using Raman transitions and chirality

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Sikes, D. E.; Yavuz, D. D.

    2011-11-15

    We present a scheme that achieves negative refraction with low absorption in far-off resonant atomic systems. The scheme utilizes Raman resonances and does not require the simultaneous presence of an electric-dipole transition and a magnetic-dipole transition near the same wavelength. We show that two interfering Raman tran-sitions coupled to a magnetic-dipole transition can achieve a negative index of refraction with low absorption through magnetoelectric cross-coupling. We confirm the validity of the analytical results with exact numerical simulations of the density matrix. We also discuss possible experimental implementations of the scheme in rare-earth metal atomic systems.

  20. Femtosecond transient absorption spectroscopy of silanized silicon quantum dots

    NASA Astrophysics Data System (ADS)

    Kuntermann, Volker; Cimpean, Carla; Brehm, Georg; Sauer, Guido; Kryschi, Carola; Wiggers, Hartmut

    2008-03-01

    Excitonic properties of colloidal silicon quantum dots (Si qdots) with mean sizes of 4nm were examined using stationary and time-resolved optical spectroscopy. Chemically stable silicon oxide shells were prepared by controlled surface oxidation and silanization of HF-etched Si qdots. The ultrafast relaxation dynamics of photogenerated excitons in Si qdot colloids were studied on the picosecond time scale from 0.3psto2.3ns using femtosecond-resolved transient absorption spectroscopy. The time evolution of the transient absorption spectra of the Si qdots excited with a 150fs pump pulse at 390nm was observed to consist of decays of various absorption transitions of photoexcited electrons in the conduction band which overlap with both the photoluminescence and the photobleaching of the valence band population density. Gaussian deconvolution of the spectroscopic data allowed for disentangling various carrier relaxation processes involving electron-phonon and phonon-phonon scatterings or arising from surface-state trapping. The initial energy and momentum relaxation of hot carriers was observed to take place via scattering by optical phonons within 0.6ps . Exciton capturing by surface states forming shallow traps in the amorphous SiOx shell was found to occur with a time constant of 4ps , whereas deeper traps presumably localized in the Si-SiOx interface gave rise to exciton trapping processes with time constants of 110 and 180ps . Electron transfer from initially populated, higher-lying surface states to the conduction band of Si qdots (>2nm) was observed to take place within 400 or 700fs .

  1. Orientation-resolved domain mapping in tetragonal SrTiO 3 using polarized Raman spectroscopy

    DOE PAGES

    Gray, Jr., Dodd J.; Merz, Tyler A.; Hikita, Yasuyuki; ...

    2016-12-16

    Here, we present microscopically resolved, polarized spectroscopy of Raman scattering collected from tetragonal SrTiO 3. The anisotropic response of first-order Raman peaks within a single tetragonal domain has been measured. From these data, we assign symmetries to the phonons seen in the first-order Raman spectrum which is normally complicated by uncontrolled domain structure. Using a translation stage, we map the local domain orientation of a 3–μm 3 crystal volume near the laser focus and compare it to wide-field polarized images. This technique can be performed with readily available instruments and is relevant to the study of a wide range ofmore » related materials, interfaces, and devices.« less

  2. Low-Frequency Raman Modes of 2H-TaSe2 in the Charge Density Wave Phase

    NASA Astrophysics Data System (ADS)

    Chowdhury, Sugata; Simpson, J.; Einstein, T. L.; Hight Walker, A. R.; Theoretical Collaboration

    With changes in temperatures, tantalum diselenide (2H-TaSe2) , a layered, transition metal chalcogenides (TMD) exhibits unique super-lattice structures. The metallic ground state changes to an incommensurate charge density wave (CDW) state at 122?K followed by a commensurate CDW state at 90?K, and eventually a superconducting state 0.14 K. These phase transitions are driven by strong electron-phonon coupling and favored by the particular form of the Fermi surface of these systems. Here we theoretically studied the structural origin of low-frequency Raman modes of bulk 2H-TaSe2\\ in the CDW phases. Our calculations reveal that changes observed in the Raman modes are associated with the thermal expansion in the basal plane of 2H-TaSe2. The Grüneisen parameters of these two Raman modes increase in the CDW phases. Changes in the lattice parameter ``a'' are large compared to ``c'' which induces strain along the a-axis. We compared our results with experimental data which show low-frequency Raman phonon modes are very sensitive to temperature and are not observed in the metallic room-temperature state. In addition, we found that cation displacement is more than anion in CDW phase. Our results may shed more light on exact nature of the CDW instability and optical properties in this system.

  3. Efficient Surface Enhanced Raman Scattering substrates from femtosecond laser based fabrication

    NASA Astrophysics Data System (ADS)

    Parmar, Vinod; Kanaujia, Pawan K.; Bommali, Ravi Kumar; Vijaya Prakash, G.

    2017-10-01

    A fast and simple femtosecond laser based methodology for efficient Surface Enhanced Raman Scattering (SERS) substrate fabrication has been proposed. Both nano scaffold silicon (black silicon) and gold nanoparticles (Au-NP) are fabricated by femtosecond laser based technique for mass production. Nano rough silicon scaffold enables large electromagnetic fields for the localized surface plasmons from decorated metallic nanoparticles. Thus giant enhancement (approximately in the order of 104) of Raman signal arises from the mixed effects of electron-photon-phonon coupling, even at nanomolar concentrations of test organic species (Rhodamine 6G). Proposed process demonstrates the low-cost and label-less application ability from these large-area SERS substrates.

  4. Resonant stimulation of Raman scattering from single-crystal thiophene/phenylene co-oligomers

    NASA Astrophysics Data System (ADS)

    Yanagi, Hisao; Marutani, Yusuke; Matsuoka, Naoki; Hiramatsu, Toru; Ishizumi, Atsushi; Sasaki, Fumio; Hotta, Shu

    2013-12-01

    Amplified Raman scattering was observed from single crystals of thiophene/phenylene co-oligomers (TPCOs). Under ns-pulsed excitation, the TPCO crystals exhibited amplified spontaneous emission (ASE) at resonant absorption wavelengths. With increasing excitation wavelength to the 0-0 absorption edge, the stimulated resonant Raman peaks appeared both in the 0-1 and 0-2 ASE band regions. When the excitation wavelength coincided with the 0-1 ASE band energy, the Raman peaks selectively appeared in the 0-2 ASE band. Such unusual enhancement of the 0-2 Raman scattering was ascribed to resonant stimulation via vibronic coupling with electronic transitions in the uniaxially oriented TPCO molecules.

  5. Increased radiative lifetime of Tm{sup 3+}:{sup 3}F{sub 4} → {sup 3}H{sub 6} transition in oxyfluoride tellurite glasses

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Ma, Yaoyao, E-mail: xiaoqi_198863@126.com; Graduate School of Chinese Academy of Sciences, Beijing 100039; Wang, Xin

    2015-04-15

    Highlights: • We prepare Tm{sup 3+}-doped tellurite-zinc glasses with F{sup −} substitution. • Thermal stability becomes better with increasing F{sup −} in present glasses. • Tm{sup 3+} 1.8 μm radiative lifetime increases with F{sup −} concentration. • The origin of the increased lifetime has been discussed. - Abstract: The 1.8 μm emission properties of Tm{sup 3+}-doped zinc tellurite glasses modified by the substitution of ZnF{sub 2} are investigated in this paper. The thermal stability, Raman and phonon sideband spectra, transmission and absorption spectra, emission spectra and decay curves are discussed. It is found that substitution of fluoride ions into themore » zinc tellurite matrix produces dramatic increase in the emission lifetime of Tm{sup 3+} 1.8 μm emission. Absorption, Raman and phonon sideband spectra are used to estimate the local structure of Tm{sup 3+} ions. These analyses indicate structural change around Tm{sup 3+} ions caused by substitution of fluoride ions monitors the increased intrinsic radiative lifetimes. An increase in the measured radiative lifetimes of the Tm{sup 3+}:{sup 3}F{sub 4} → {sup 3}H{sub 6} transition is observed. The origin has been discussed and the reduction of OH{sup −} absorption, decrease of maximum phonon energy and phonon density are considered to be dominant in all of the nonradiative relaxations.« less

  6. Interplay of structure and magnetism in ruthenocuprates: a Raman scattering and dilatometry study

    NASA Astrophysics Data System (ADS)

    Fainstein, A.; Ramos, C. A.; Pregliasco, R. G.; Butera, A.; Trodahl, H. J.; Williams, G. V. M.; Tallon, J. L.

    2002-07-01

    We present a Raman scattering and dilatometry study of polycrystalline samples of the magnetic superconducting ruthenocuprates RuSr 2Gd 2- xCe xCu 2O 10+ δ (RuGd 1222) and RuSr 2GdCu 2O 8 (RuGd 1212). In the Raman spectra a high-temperature diffusive-like laser-tail develops below the magnetic ordering temperature ( TM) into an underdamped peak which shifts up to ˜130 cm-1. A line assigned to O(Ru) phonons hardens, narrows and strengthens strongly below TM. Finally, a phonon peak appears below TM at ˜590 cm-1. These three magnetic-order-dependent features are observed for RuGd 1212 and for RuGd 1222 with x=1.0, but do not appear for x=0.5. Dilatometry measurements, on the other hand, evidence a change of the expansion coefficient at TM. These results point to a structural effect accompanying the magnetic order, and suggest a complex interplay of spin and lattice degrees of freedom in these ruthenocuprates.

  7. Anharmonic phonon-polariton dynamics in ferroelectric LiNbO3 studied with single-shot pump-probe imaging spectroscopy

    NASA Astrophysics Data System (ADS)

    Kuribayashi, T.; Motoyama, T.; Arashida, Y.; Katayama, I.; Takeda, J.

    2018-05-01

    We demonstrate that single-shot pump-probe imaging spectroscopy with an echelon mirror enables us to disclose the ferroelectric phonon-polariton dynamics across a wide temperature range from 10 K to 375 K while avoiding the photorefractive effects that appear prominently at low temperatures. The E-mode phonon-polaritons corresponding to the two transverse optical modes, TO1 and TO3, up to ˜7 THz were induced in LiNbO3 through an impulsive stimulated Raman scattering process. Subsequently, using single-shot pump-probe imaging spectroscopy over a minimal cumulative time, we successfully visualized the phonon-polariton dynamics in time-wavelength space even at low temperatures. We found that the phase-matching condition significantly affected the observed temperature-dependent phonon-polariton frequency shift. The anharmonicity of the TO1 and TO3 modes was then evaluated based on an anharmonic model involving higher-order interactions with acoustic phonons while eliminating the influence of the frequency shift due to the phase-matching condition. The observed wavenumber-dependent damping rate was analyzed by considering the bilinear coupling of the TO1 or TO3 modes with the thermally activated relaxation mode. We found that the phonon-polariton with a higher frequency and wavenumber had a higher damping rate at high temperatures because of its frequent interaction with the thermally activated relaxation mode and acoustic phonons. The TO3 mode displayed greater bilinear coupling than the TO1 mode, which may also have contributed to the observed high damping rate. Thus, using our unique single-shot spectroscopy technique, we could reveal the overall anharmonic characteristics of the E-mode phonon-polaritons arising from both the acoustic phonons and the relaxation mode.

  8. Four-phonon scattering reduces intrinsic thermal conductivity of graphene and the contributions from flexural phonons

    NASA Astrophysics Data System (ADS)

    Feng, Tianli; Ruan, Xiulin

    2018-01-01

    We have developed a formalism of the exact solution to linearized phonon Boltzmann transport equation (BTE) for thermal conductivity calculation including three- and four-phonon scattering. We find strikingly high four-phonon scattering rates in single-layer graphene (SLG) based on the optimized Tersoff potential. The reflection symmetry in graphene, which forbids the three-ZA (out-of-plane acoustic) scattering, allows the four-ZA processes ZA +ZA ⇌ZA +ZA and ZA ⇌ZA +ZA + ZA. As a result, the large phonon population of the low-energy ZA branch originated from the quadratic phonon dispersion leads to high four-phonon scattering rates, even much higher than the three-phonon scattering rates at room temperature. These four-phonon processes are dominated by the normal processes, which lead to a failure of the single mode relaxation time approximation. Therefore, we have solved the exact phonon BTE using an iterative scheme and then calculated the length- and temperature-dependent thermal conductivities. We find that the predicted thermal conductivity of SLG is lower than the previously predicted value from the three-phonon scattering only. The relative contribution of the ZA branch is reduced from 70% to 30% when four-phonon scattering is included. Furthermore, we have demonstrated that the four-phonon scattering in multilayer graphene and graphite is not strong due to the ZA splitting by interlayer van der Waals interaction. We also demonstrate that the five-phonon process in SLG is not strong due to the restriction of reflection symmetry.

  9. Longitudinal optical phonon-plasmon coupled modes of degenerate Al-doped ZnO films

    NASA Astrophysics Data System (ADS)

    Ding, K.; Hu, Q. C.; Lin, W. W.; Huang, J. K.; Huang, F.

    2012-07-01

    We have investigated the interaction between carriers and polar phonons by using Raman scattering spectroscopy in highly conductive Al-doped ZnO films grown by metalorganic chemical vapor deposition. Different from the longitudinal optical phonon-plasmon coupled modes (LOPPCM) observed in nondegenerate ZnO, an A1(LO)-like mode appears at the low frequency side of the uncoupled A1(LO) mode, and it monotonically shifts to higher frequencies and approaches to the uncoupled A1(LO) mode as Al composition increases. Based on line shape calculations, the A1(LO)-like mode is assigned to the large wave-vector LOPPCM arising from nonconserving scattering dominated by the Al impurity-induced Fröhlich mechanism. Benefiting from the nonmonotonic Al composition dependence of the electron density, it is revealed that the LOPPCM depends mainly on the doping level but not the carrier concentration.

  10. Raman spectra and optical trapping of highly refractive and nontransparent particles

    NASA Astrophysics Data System (ADS)

    Xie, Changan; Li, Yong-qing

    2002-08-01

    We measured the Raman spectra of single optically trapped highly refractive and nontransparent microscopic particles suspended in a liquid using an inverted confocal laser-tweezers-Raman-spectroscopy system. A low-power diode-laser beam of TEM00 mode was used both for optical trapping and Raman excitation of refractive, absorptive, and reflective metal particles. To form a stable trap for a nontransparent particle, the beam focus was located near the top of the particle and the particle was pushed against a glass plate by the axial repulsive force. Raman spectra from single micron-sized crystals with high index of refraction including silicon, germanium, and KNbO3, and from absorptive particles of black and color paints were recorded. Surface-enhanced Raman scattering of R6G and phenylalanine molecules absorbed on the surface of a trapped cluster of silver particles was also demonstrated.

  11. Mapping momentum-dependent electron-phonon coupling and nonequilibrium phonon dynamics with ultrafast electron diffuse scattering

    NASA Astrophysics Data System (ADS)

    Stern, Mark J.; René de Cotret, Laurent P.; Otto, Martin R.; Chatelain, Robert P.; Boisvert, Jean-Philippe; Sutton, Mark; Siwick, Bradley J.

    2018-04-01

    Despite their fundamental role in determining material properties, detailed momentum-dependent information on the strength of electron-phonon and phonon-phonon coupling (EPC and PPC, respectively) across the entire Brillouin zone has remained elusive. Here we demonstrate that ultrafast electron diffuse scattering (UEDS) directly provides such information. By exploiting symmetry-based selection rules and time resolution, scattering from different phonon branches can be distinguished even without energy resolution. Using graphite as a model system, we show that UEDS patterns map the relative EPC and PPC strength through their profound sensitivity to photoinduced changes in phonon populations. We measure strong EPC to the K -point TO phonon of A1' symmetry (K -A1' ) and along the entire TO branch between Γ -K , not only to the Γ -E2 g phonon. We also determine that the subsequent phonon relaxation of these strongly coupled optical phonons involve three stages: decay via several identifiable channels to TA and LA phonons (1 -2 ps), intraband thermalization of the non-equilibrium TA/LA phonon populations (30 -40 ps) and interband relaxation of the TA/LA modes (115 ps). Combining UEDS with ultrafast angle-resolved photoelectron spectroscopy will yield a complete picture of the dynamics within and between electron and phonon subsystems, helping to unravel complex phases in which the intertwined nature of these systems has a strong influence on emergent properties.

  12. Optical Absorption and Raman Spectroscopy of Multiple Shocked Liquid Benzene to 10 GPa

    NASA Astrophysics Data System (ADS)

    Root, S.

    2005-07-01

    Liquid benzene samples were multiply shocked to peak pressures ranging from 3 GPa to 10 GPa to examine physical and chemical changes in benzene. A xenon flashlamp was used to probe the visible spectrum of benzene for loses in transmitted light intensity caused by changes in the electronic structure (absorption) or a possible liquid to solid phase transition (scattering). Raman spectroscopy was used to corroborate transmission measurements by examining changes in the benzene vibrational modes. The C-C symmetric ring breathing mode (992 cm-1), C-H symmetric stretch (3061 cm-1), along with several weaker modes at 607 cm-1, 1178 cm-1, 1586 cm-1, and 1606 cm-1 were monitored during shock loading. An EOS was developed to calculate the temperature of the shock compressed benzene. The present work has demonstrated that liquid benzene remains unchanged during multiple shock loading up to 10 GPa. Work supported by ONR and DOE.

  13. Optimizing phonon space in the phonon-coupling model

    NASA Astrophysics Data System (ADS)

    Tselyaev, V.; Lyutorovich, N.; Speth, J.; Reinhard, P.-G.

    2017-08-01

    We present a new scheme to select the most relevant phonons in the phonon-coupling model, named here the time-blocking approximation (TBA). The new criterion, based on the phonon-nucleon coupling strengths rather than on B (E L ) values, is more selective and thus produces much smaller phonon spaces in the TBA. This is beneficial in two respects: first, it curbs the computational cost, and second, it reduces the danger of double counting in the expansion basis of the TBA. We use here the TBA in a form where the coupling strength is regularized to keep the given Hartree-Fock ground state stable. The scheme is implemented in a random-phase approximation and TBA code based on the Skyrme energy functional. We first explore carefully the cutoff dependence with the new criterion and can work out a natural (optimal) cutoff parameter. Then we use the freshly developed and tested scheme for a survey of giant resonances and low-lying collective states in six doubly magic nuclei looking also at the dependence of the results when varying the Skyrme parametrization.

  14. X-ray absorption and Raman spectroscopy studies of molybdenum environments in borosilicate waste glasses

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    McKeown, David A.; Gan, Hao; Pegg, Ian L.

    2017-05-01

    Mo-containing high-level nuclear waste borosilicate glasses were investigated as part of an effort to improve Mo loading while avoiding yellow phase crystallization. Previous work showed that additions of vanadium decrease yellow phase formation and increases Mo solubility. X-ray absorption spectroscopy (XAS) and Raman spectroscopy were used to characterize Mo environments in HLW borosilicate glasses and to investigate possible structural relationships between Mo and V. Mo XAS spectra for the glasses indicate isolated tetrahedral Mo6+O4 with Mo-O distances near 1.75 Å. V XANES indicate tetrahedral V5+O4 as the dominant species. Raman spectra show composition dependent trends, where Mo-O symmetrical stretch modemore » frequencies (ν1) are sensitive to the mix of alkali and alkaline earth cations, decreasing by up to 10 cm-1 for glasses that change from Li+ to Na+ as the dominant network-modifying species. This indicates that MoO4 tetrahedra are isolated from the borosilicate network and are surrounded, at least partly, by Na+ and Li+. Secondary ν1 frequency effects, with changes up to 7 cm-1, were also observed with increasing V2O5 and MoO3 content. These secondary trends may indicate MoO4-MoO4 and MoO4-VO4 clustering, suggesting that V additions may stabilize Mo in the matrix with respect to yellow phase formation.« less

  15. Raman spectroscopy of white wines.

    PubMed

    Martin, Coralie; Bruneel, Jean-Luc; Guyon, François; Médina, Bernard; Jourdes, Michael; Teissedre, Pierre-Louis; Guillaume, François

    2015-08-15

    The feasibility of exploiting Raman scattering to analyze white wines has been investigated using 3 different wavelengths of the incoming laser radiation in the near-UV (325 nm), visible (532 nm) and near infrared (785 nm). To help in the interpretation of the Raman spectra, the absorption properties in the UV-visible range of two wine samples as well as their laser induced fluorescence have also been investigated. Thanks to the strong intensity enhancement of the Raman scattered light due to electronic resonance with 325 nm laser excitation, hydroxycinnamic acids may be detected and analyzed selectively. Fructose and glucose may also be easily detected below ca. 1000 cm(-1). This feasibility study demonstrates the potential of the Raman spectroscopic technique for the analysis of white wines. Copyright © 2015 Elsevier Ltd. All rights reserved.

  16. Dual-excitation wavelength resonance Raman explosives detector

    NASA Astrophysics Data System (ADS)

    Yellampalle, Balakishore; Sluch, Mikhail; Wu, Hai-Shan; Martin, Robert; McCormick, William; Ice, Robert; Lemoff, Brian E.

    2013-05-01

    Deep-ultraviolet resonance Raman spectroscopy (DUVRRS) is a promising approach to stand-off detection of explosive traces due to: 1) resonant enhancement of Raman cross-section, 2) λ-4-cross-section enhancement, and 3) fluorescence and solar background free signatures. For trace detection, these signal enhancements more than offset the small penetration depth due to DUV absorption. A key challenge for stand-off sensors is to distinguish explosives, with high confidence, from a myriad of unknown background materials that may have interfering spectral peaks. To address this, we are developing a stand-off explosive sensor using DUVRRS with two simultaneous DUV excitation wavelengths. Due to complex interplay of resonant enhancement, self-absorption and laser penetration depth, significant amplitude variation is observed between corresponding Raman bands with different excitation wavelengths. These variations with excitation wavelength provide an orthogonal signature that complements the traditional Raman signature to improve specificity relative to single-excitation-wavelength techniques. As part of this effort, we are developing two novel CW DUV lasers, which have potential to be compact, and a compact dual-band high throughput DUV spectrometer, capable of simultaneous detection of Raman spectra in two spectral windows. We have also developed a highly sensitive algorithm for the detection of explosives under low signal-to-noise situations.

  17. Au3+ ion implantation on FTO coated glasses: Effect on structural, electrical, optical and phonon properties

    NASA Astrophysics Data System (ADS)

    Sahu, Bindu; Dey, Ranajit; Bajpai, P. K.

    2017-06-01

    Effects of 11.00 MeV Au3+ ions implanted in FTO coated (thickness ≈300 nm) silicate glasses on structural, electrical optical and phonon behavior have been explored. It has been observed that metal clustering near the surface and sub-surface region below glass-FTO interface changes electrical and optical properties significantly. Ion implantation does not affect the crystalline structure of the coated films; however, the unit cell volume decreases with increase in fluence and the tetragonal distortion (c/a ratio) also decreases systematically in the implanted samples. The sheet resistivity of the films increases from 11 × 10-5 ohm-cm (in pristine) to 7.5 × 10-4 ohm-cm for highest ion beam fluence ≈1015 ions/cm2. The optical absorption decreases with increasing fluence whereas, the optical transmittance as well as reflectance increases with increasing fluence. The Raman spectra are observed at ∼530 cm-1 and ∼1103 cm-1 in pristine sample. The broad band at 530 cm-1 shifts towards higher wave number in the irradiated samples. This may be correlated with increased disorder and strain relaxation in the samples as a result of ion beam irradiation.

  18. Role of orbital filling on nonlinear ionic Raman scattering in perovskite titanates

    NASA Astrophysics Data System (ADS)

    Gu, Mingqiang; Rondinelli, James M.

    2017-01-01

    The linear and nonlinear phononic interactions between an optically excited infrared (IR) or hyper-Raman mode and a driven Raman mode are computed for the d0 (CaTiO3) and d1 (LaTiO3) titanates within a first-principles density functional framework. We calculate the potential energy surface expanded in terms of the Ag or B1 g mode amplitudes coupled to the Au or the B3 u mode and determine the coupling coefficients for these multimode interactions. We find that the linear-quadratic coupling dominates the anharmonicities over the quadratic-quadratic interaction in the perovskite titanates. The IR and Raman modes both modify the electronic structure with the former being more significant but occurring on a different time scale; furthermore, the coupled-mode interactions lead to sizable perturbations to the valence bandwidth (˜100 meV ) and band gap (˜50 meV). By comparing the coupling coefficients of undoped CaTiO3 and LaTiO3 to those for electron-doped (CaTiO3) and hole-doped (LaTiO3) titanates, we isolate the role of orbital filling in the nonlinear coupling process. We find that with increasing occupancy of the d manifold, the linear-quadratic interaction decreases by approximately 30% with minor changes induced by the cation chemistry (that mainly affect the phonon mode frequencies) or by electron correlation. We identify the importance of the Ti-O bond stiffness, which depends on the orbital filling, in governing the lattice anharmonicitiy. This microscopic understanding can be used to increase the nonlinear coupling coefficient to facilitate more facile access of nonequilibrium structures and properties through ionic Raman scattering processes.

  19. Coordinated EDX and micro-Raman analysis of presolar silicon carbide: A novel, nondestructive method to identify rare subgroup SiC

    NASA Astrophysics Data System (ADS)

    Liu, Nan; Steele, Andrew; Nittler, Larry R.; Stroud, Rhonda M.; De Gregorio, Bradley T.; Alexander, Conel M. O'D.; Wang, Jianhua

    2017-12-01

    We report the development of a novel method to nondestructively identify presolar silicon carbide (SiC) grains with high initial 26Al/27Al ratios (>0.01) and extreme 13C-enrichments (12C/13C ≤ 10) by backscattered electron-energy dispersive X-ray (EDX) and micro-Raman analyses. Our survey of a large number of presolar SiC demonstrates that (1) 80% of core-collapse supernova and putative nova SiC can be identified by quantitative EDX and Raman analyses with >70% confidence; (2) 90% of presolar SiC are predominantly 3C-SiC, as indicated by their Raman transverse optical (TO) peak position and width; (3) presolar 3C-SiC with 12C/13C ≤ 10 show lower Raman TO phonon frequencies compared to mainstream 3C-SiC. The downward shifted phonon frequencies of the 13C-enriched SiC with concomitant peak broadening are a natural consequence of isotope substitution. 13C-enriched SiC can therefore be identified by micro-Raman analysis; (4) larger shifts in the Raman TO peak position and width indicate deviations from the ideal 3C structure, including rare polytypes. Coordinated transmission electron microscopy analysis of one X and one mainstream SiC grain found them to be of 6H and 15R polytypes, respectively; (5) our correlated Raman and NanoSIMS study of mainstream SiC shows that high nitrogen content is a dominant factor in causing mainstream SiC Raman peak broadening without significant peak shifts; and (6) we found that the SiC condensation conditions in different stellar sites are astonishingly similar, except for X grains, which often condensed more rapidly and at higher atmospheric densities and temperatures, resulting in a higher fraction of grains with much downward shifted and broadened Raman TO peaks.

  20. Electron-phonon interactions in semiconductor nanostructures

    NASA Astrophysics Data System (ADS)

    Yu, Segi

    In this dissertation, electron-phonon interactions are studied theoretically in semiconductor nanoscale heterostructures. Interactions of electrons with interface optical phonons dominate over other electron-phonon interactions in narrow width heterostructures. Hence, a transfer matrix method is used to establish a formalism for determining the dispersion relations and electrostatic potentials of the interface phonons for multiple-interface heterostructure within the macroscopic dielectric continuum model. This method facilitates systematic calculations for complex structures where the conventional method is difficult to implement. Several specific cases are treated to illustrate advantages of the formalism. Electrophonon resonance (EPR) is studied in cylindrical quantum wires using the confined/interface optical phonons representation and bulk phonon representation. It has been found that interface phonon contribution to EPR is small compared with confined phonon. Different selection rules for bulk phonons and confined phonons result in different EPR behaviors as the radius of cylindrical wire changes. Experiment is suggested to test which phonon representation is appropriate for EPR. The effects of phonon confinement on elect ron-acoustic-phonon scattering is studied in cylindrical and rectangular quantum wires. In the macroscopic elastic continuum model, the confined-phonon dispersion relations are obtained for several crystallographic directions with free-surface and clamped-surface boundary conditions in cylindrical wires. The scattering rates due to the deformation potential are obtained for these confined phonons and are compared with those of bulk-like phonons. The results show that the inclusion of acoustic phonon confinement may be crucial for calculating accurate low-energy electron scattering rates. Furthermore, it has been found that there is a scaling rule governing the directional dependence of the scattering rates. The Hamiltonian describing the

  1. Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites

    PubMed Central

    Yang, Jianfeng; Wen, Xiaoming; Xia, Hongze; Sheng, Rui; Ma, Qingshan; Kim, Jincheol; Tapping, Patrick; Harada, Takaaki; Kee, Tak W.; Huang, Fuzhi; Cheng, Yi-Bing; Green, Martin; Ho-Baillie, Anita; Huang, Shujuan; Shrestha, Santosh; Patterson, Robert; Conibeer, Gavin

    2017-01-01

    The hot-phonon bottleneck effect in lead-halide perovskites (APbX3) prolongs the cooling period of hot charge carriers, an effect that could be used in the next-generation photovoltaics devices. Using ultrafast optical characterization and first-principle calculations, four kinds of lead-halide perovskites (A=FA+/MA+/Cs+, X=I−/Br−) are compared in this study to reveal the carrier-phonon dynamics within. Here we show a stronger phonon bottleneck effect in hybrid perovskites than in their inorganic counterparts. Compared with the caesium-based system, a 10 times slower carrier-phonon relaxation rate is observed in FAPbI3. The up-conversion of low-energy phonons is proposed to be responsible for the bottleneck effect. The presence of organic cations introduces overlapping phonon branches and facilitates the up-transition of low-energy modes. The blocking of phonon propagation associated with an ultralow thermal conductivity of the material also increases the overall up-conversion efficiency. This result also suggests a new and general method for achieving long-lived hot carriers in materials. PMID:28106061

  2. Raman scattering in the Mott insulators LaTiO3 and YTiO3: evidence for orbital excitations.

    PubMed

    Ulrich, C; Gössling, A; Grüninger, M; Guennou, M; Roth, H; Cwik, M; Lorenz, T; Khaliullin, G; Keimer, B

    2006-10-13

    Raman scattering is used to observe pronounced electronic excitations around 230 meV--well above the two-phonon range--in the Mott insulators LaTiO3 and YTiO3. Based on the temperature, polarization, and photon energy dependence, the modes are identified as orbital excitations. The observed profiles bear a striking resemblance to magnetic Raman modes in the insulating parent compounds of the superconducting cuprates, indicating an unanticipated universality of the electronic excitations in transition metal oxides.

  3. Rotating samples in FT-RAMAN spectrometers

    NASA Astrophysics Data System (ADS)

    De Paepe, A. T. G.; Dyke, J. M.; Hendra, P. J.; Langkilde, F. W.

    1997-11-01

    It is customary to rotate samples in Raman spectroscopy to avoid absorption or sample heating. In FT-Raman experiments the rotation is always shown (typically 30-60 rpm) because higher speeds are thought to generate noise in the spectra. In this article we show that more rapid rotation is possible. A tablet containing maleic acid and one made up of sub-millimetre silica particles with metoprolol succinate as active ingredient were rotated at different speeds, up to 6760 rpm. The FT-Raman spectra were recorded and studied. We conclude that it is perfectly acceptable to rotate samples up to 1500 rpm.

  4. Quantum random bit generation using energy fluctuations in stimulated Raman scattering.

    PubMed

    Bustard, Philip J; England, Duncan G; Nunn, Josh; Moffatt, Doug; Spanner, Michael; Lausten, Rune; Sussman, Benjamin J

    2013-12-02

    Random number sequences are a critical resource in modern information processing systems, with applications in cryptography, numerical simulation, and data sampling. We introduce a quantum random number generator based on the measurement of pulse energy quantum fluctuations in Stokes light generated by spontaneously-initiated stimulated Raman scattering. Bright Stokes pulse energy fluctuations up to five times the mean energy are measured with fast photodiodes and converted to unbiased random binary strings. Since the pulse energy is a continuous variable, multiple bits can be extracted from a single measurement. Our approach can be generalized to a wide range of Raman active materials; here we demonstrate a prototype using the optical phonon line in bulk diamond.

  5. Phonon anomalies in intermediate valent TmXSe and TmSe1 - yTey

    NASA Astrophysics Data System (ADS)

    Boppart, H.; Treindl, A.; Wachter, P.

    1981-03-01

    In TmxSe and TmSe1-yTey the degree of valence mixing can be adjusted between nearly 3+ for Tm0.87Se and 2.55+ for TmSe0.7Te0.3. The measurement of sound velocities vL, vTl and vT2 and the evaluation of the Raman effect for various compositions permit the derivation of LA [111] phonon dispersion at critical points in the Brillouin zone. vL decreases with increasing valence mixing. Near the middle of the zone the LA branch gets a dip for intermediate valent compositions, resulting in a characteristic peak in the Ramn spectrum at about 60 cm-1. The elastic constant c12 has been found negative for Tm0.99Se, also at 4.2 K. For uniaxial pressures c12 exhibits strong nonlinearities and even changes sign with pressure in an intermediate valent composition. The optical phonon frequencies, LO (L) also soften proportional with the degree of valence mixing.

  6. Temperature dependence of the fundamental optical absorption edge in crystals and disordered semiconductors

    NASA Astrophysics Data System (ADS)

    Grein, C. H.; John, Sajeev

    1989-04-01

    We present a first principles theory of the temperature dependence of the Urbach optical absorption edge in crystals and disordered semiconductors which incorporates the effects of short range correlated static disorder and the non-adiabatic quantum dynamics of the coupled electron-phonon system. At finite temperatures the dominant features of the Urbach tail are accounted for by multiple phonon absorption and emission side bands which accompany the optically induced electronic transition and which provide a dynamic polaronic potential well that localizes the electron. Excellent agreement is found with experimental data on both crystalline and amorphous silicon.

  7. Effect of oxygen vacancies and strain on the phonon spectrum of HfO2 thin films

    NASA Astrophysics Data System (ADS)

    Gao, Lingyuan; Yalon, Eilam; Chew, Annabel R.; Deshmukh, Sanchit; Salleo, Alberto; Pop, Eric; Demkov, Alexander A.

    2017-06-01

    The effect of strain and oxygen deficiency on the Raman spectrum of monoclinic HfO2 is investigated theoretically using first-principles calculations. 1% in-plane compressive strain applied to a and c axes is found to blue shift the phonon frequencies, while 1% tensile strain does the opposite. The simulations are compared, and good agreement is found with the experimental results of Raman frequencies greater than 110 cm-1 for 50 nm HfO2 thin films. Several Raman modes measured below 110 cm-1 and previously assigned to HfO2 are found to be rotational modes of gases present in air ambient (nitrogen and oxygen). However, localized vibrational modes introduced by threefold-coordinated oxygen (O3) vacancies are identified at 96.4 cm-1 computationally. These results are important for a deeper understanding of vibrational modes in HfO2, which has technological applications in transistors and particularly in resistive random-access memory whose operation relies on oxygen-deficient HfOx.

  8. Optical phonons in nanostructured thin films composed by zincblende zinc selenide quantum dots in strong size-quantization regime: Competition between phonon confinement and strain-related effects

    NASA Astrophysics Data System (ADS)

    Pejova, Biljana

    2014-05-01

    Raman scattering in combination with optical spectroscopy and structural studies by X-ray diffraction was employed to investigate the phonon confinement and strain-induced effects in 3D assemblies of variable-size zincblende ZnSe quantum dots close packed in thin film form. Nanostructured thin films were synthesized by colloidal chemical approach, while tuning of the nanocrystal size was enabled by post-deposition thermal annealing treatment. In-depth insights into the factors governing the observed trends of the position and half-width of the 1LO band as a function of the average QD size were gained. The overall shifts in the position of 1LO band were found to result from an intricate compromise between the influence of phonon confinement and lattice strain-induced effects. Both contributions were quantitatively and exactly modeled. Accurate assignments of the bands due to surface optical (SO) modes as well as of the theoretically forbidden transverse optical (TO) modes were provided, on the basis of reliable physical models (such as the dielectric continuum model of Ruppin and Englman). The size-dependence of the ratio of intensities of the TO and LO modes was studied and discussed as well. Relaxation time characterizing the phonon decay processes in as-deposited samples was found to be approximately 0.38 ps, while upon post-deposition annealing already at 200 °C it increases to about 0.50 ps. Both of these values are, however, significantly smaller than those characteristic for a macrocrystalline ZnSe sample.

  9. Interplay of valley selection and helicity exchange of light in Raman scattering for graphene and MoS2

    NASA Astrophysics Data System (ADS)

    Tatsumi, Yuki; Saito, Riichiro

    2018-03-01

    Raman spectra of graphene and MoS2 are calculated for incident and scattered circularly polarized light. In the case of graphene, the well known G -band Raman spectra have a not well known property that the helicity of the incident circularly polarized light changes to another helicity in the scattered light. Using the electron-photon and electron-phonon matrix elements by first-principles calculation, we calculate resonant Raman spectra of graphene and MoS2 for circularly polarized light which are compared with recent experiments. The Raman intensity for circularly polarized light is relevant to optical valley polarization in the case of MoS2. We also discuss how the helicity-selection rule can be modified by applying stress to graphene.

  10. Raman scattering in the RTiO3 family of Mott-Hubbard insulators

    NASA Astrophysics Data System (ADS)

    Reedyk, M.; Crandles, D. A.; Cardona, M.; Garrett, J. D.; Greedan, J. E.

    1997-01-01

    Raman-scattering measurements have been carried out for crystals of the RTiO3 (R=La,Ce,Pr,Nd,Sm,Gd) system whose members are Mott-Hubbard insulators. RTiO3 has an orthorhombically distorted perovskite unit cell. The distortion increases systematically from LaTiO3 to GdTiO3 and is accompanied by changes in electronic structure (decreasing W/U ratio). As a consequence of the changing electronic properties, the Raman spectrum shows an interesting evolution of both the phonon features and the electronic continuum. Most notable are (1) a redistribution in the spectral shape of the electronic background, (2) a systematic change in line shape, and a dramatic increase in the center frequency of one of the phonon modes from 287 cm-1 in LaTiO3 to 385 cm-1 in GdTiO3, and (3) the observation of resonance effects in the most insulating members of the series. The appearance of a free-carrier component in the electronic-scattering background, which seems to be related to systematic self-energy effects of the phonon near 300 cm-1, is unexpected. It is likely the result of increased doping due to a greater facility for rare-earth vacancies to form in large R3+ ionic radius members of the series. A systematic increase in the continuum scattering rate is also observed and indicates that the free carriers are not scattering off rare-earth vacancies but rather that the scattering mechanism originates from changes in electronic structure.

  11. Phonon counting and intensity interferometry of a nanomechanical resonator

    NASA Astrophysics Data System (ADS)

    Cohen, Justin D.; Meenehan, Seán M.; Maccabe, Gregory S.; Gröblacher, Simon; Safavi-Naeini, Amir H.; Marsili, Francesco; Shaw, Matthew D.; Painter, Oskar

    2015-04-01

    In optics, the ability to measure individual quanta of light (photons) enables a great many applications, ranging from dynamic imaging within living organisms to secure quantum communication. Pioneering photon counting experiments, such as the intensity interferometry performed by Hanbury Brown and Twiss to measure the angular width of visible stars, have played a critical role in our understanding of the full quantum nature of light. As with matter at the atomic scale, the laws of quantum mechanics also govern the properties of macroscopic mechanical objects, providing fundamental quantum limits to the sensitivity of mechanical sensors and transducers. Current research in cavity optomechanics seeks to use light to explore the quantum properties of mechanical systems ranging in size from kilogram-mass mirrors to nanoscale membranes, as well as to develop technologies for precision sensing and quantum information processing. Here we use an optical probe and single-photon detection to study the acoustic emission and absorption processes in a silicon nanomechanical resonator, and perform a measurement similar to that used by Hanbury Brown and Twiss to measure correlations in the emitted phonons as the resonator undergoes a parametric instability formally equivalent to that of a laser. Owing to the cavity-enhanced coupling of light with mechanical motion, this effective phonon counting technique has a noise equivalent phonon sensitivity of 0.89 +/- 0.05. With straightforward improvements to this method, a variety of quantum state engineering tasks using mesoscopic mechanical resonators would be enabled, including the generation and heralding of single-phonon Fock states and the quantum entanglement of remote mechanical elements.

  12. Quantum theory of phonon-mediated decoherence and relaxation of two-level systems in a structured electromagnetic reservoir

    NASA Astrophysics Data System (ADS)

    Roy, Chiranjeeb

    In this thesis we study the role of nonradiative degrees of freedom on quantum optical properties of mesoscopic quantum dots placed in the structured electromagnetic reservoir of a photonic crystal. We derive a quantum theory of the role of acoustic and optical phonons in modifying the optical absorption lineshape, polarization dynamics, and population dynamics of a two-level atom (quantum dot) in the "colored" electromagnetic vacuum of a photonic band gap (PBG) material. This is based on a microscopic Hamiltonian describing both radiative and vibrational processes quantum mechanically. Phonon sidebands in an ordinary electromagnetic reservoir are recaptured in a simple model of optical phonons using a mean-field factorization of the atomic and lattice displacement operators. Our formalism is then used to treat the non-Markovian dynamics of the same system within the structured electromagnetic density of states of a photonic crystal. We elucidate the extent to which phonon-assisted decay limits the lifetime of a single photon-atom bound state and derive the modified spontaneous emission dynamics due to coupling to various phonon baths. We demonstrate that coherent interaction with undamped phonons can lead to enhanced lifetime of a photon-atom bound state in a PBG by (i) dephasing and reducing the transition electric dipole moment of the atom and (ii) reducing the quantum mechanical overlap of the state vectors of the excited and ground state (polaronic shift). This results in reduction of the steady-state atomic polarization but an increase in the fractionalized upper state population in the photon-atom bound state. We demonstrate, on the other hand, that the lifetime of the photon-atom bound state in a PBG is limited by the lifetime of phonons due to lattice anharmonicities (break-up of phonons into lower energy phonons) and purely nonradiative decay. We demonstrate how these additional damping effects limit the extent of the polaronic (Franck-Condon) shift of

  13. Instant detection and identification of concealed explosive-related compounds: Induced Stokes Raman versus infrared.

    PubMed

    Elbasuney, Sherif; El-Sherif, Ashraf F

    2017-01-01

    The instant detection of explosives and explosive-related compounds has become an urgent priority in recent years for homeland security and counter-terrorism applications. Modern techniques should offer enhancement in selectivity, sensitivity, and standoff distances. Miniaturisation, portability, and field-ruggedisation are crucial requirements. This study reports on instant and standoff identification of concealed explosive-related compounds using customized Raman technique. Stokes Raman spectra of common explosive-related compounds were generated and spectrally resolved to create characteristic finger print spectra. The scattered Raman emissions over the band 400:2000cm -1 were compared to infrared absorption using FTIR. It has been demonstrated that the two vibrational spectroscopic techniques were opposite and completing each other. Molecular vibrations with strong absorption in infrared (those involve strong change in dipole moments) induced weak signals in Raman and vice versa. The tailored Raman offered instant detection, high sensitivity, and standoff detection capabilities. Raman demonstrated characteristic fingerprint spectra with stable baseline and sharp intense peaks. Complete correlations of absorption/scattered signals to certain molecular vibrations were conducted to generate an entire spectroscopic profile of explosive-related compounds. This manuscript shades the light on Raman as one of the prevailing technologies for instantaneous detection of explosive-related compounds. Copyright © 2016 Elsevier Ireland Ltd. All rights reserved.

  14. Stimulated Raman amplification, oscillation, and linewidth in barium nitrate

    NASA Technical Reports Server (NTRS)

    McCray, Christopher J.; Chyba, Thomas H.

    1998-01-01

    Measurements of Raman gain in a Ba(NO3)2 crystal are reported at 532 nm using a Raman oscillator/amplifier arrangement for differential absorption lidar measurements of ozone. The experimentally determined gain coefficient will be compared with theoretical results. The effect of single and multi-longitudinal mode pumping upon the amplification process will be discussed. Measurement of the Raman linewidth for 1st 2nd and 3d stokes shifts arc presented.

  15. Vacuum phonon tunneling.

    PubMed

    Altfeder, Igor; Voevodin, Andrey A; Roy, Ajit K

    2010-10-15

    Field-induced phonon tunneling, a previously unknown mechanism of interfacial thermal transport, has been revealed by ultrahigh vacuum inelastic scanning tunneling microscopy (STM). Using thermally broadened Fermi-Dirac distribution in the STM tip as in situ atomic-scale thermometer we found that thermal vibrations of the last tip atom are effectively transmitted to sample surface despite few angstroms wide vacuum gap. We show that phonon tunneling is driven by interfacial electric field and thermally vibrating image charges, and its rate is enhanced by surface electron-phonon interaction.

  16. Evaluation of quantum confinement effect in nanocrystal Si dot layer by Raman spectroscopy.

    PubMed

    Mizukami, Y; Kosemura, D; Numasawa, Y; Ohshita, Y; Ogura, A

    2012-11-01

    Quantum confinement effect in the nanocrystal-Si (nc-Si) was evaluated by Raman spectroscopy. The nc-Si dot layers were fabricated by the H2 plasma treatment for the nucleation site formation followed by the SiH4 irradiation for the nc-Si growth. Post-oxidation annealing was also performed to improve the crystalline quality. After post-oxidation annealing for 5 or 10 min, the asymmetric broadening on the lower frequency sides in Raman spectra were obtained, which can be attributed to the phonon confinement effect in nc-Si. Furthermore we confirmed that hydrostatic stress of approximately 500 MPa was induced in nc-Si after post-oxidation annealing.

  17. Spin-Orbital Excitation Continuum and Anomalous Electron-Phonon Interaction in the Mott Insulator LaTiO3

    NASA Astrophysics Data System (ADS)

    Ulrich, C.; Khaliullin, G.; Guennou, M.; Roth, H.; Lorenz, T.; Keimer, B.

    2015-10-01

    Raman scattering experiments on stoichiometric, Mott-insulating LaTiO3 over a wide range of excitation energies reveal a broad electronic continuum which is featureless in the paramagnetic state, but develops a gap of ˜800 cm-1 upon cooling below the Néel temperature TN=146 K . In the antiferromagnetic state, the spectral weight below the gap is transferred to well-defined spectral features due to spin and orbital excitations. Low-energy phonons exhibit pronounced Fano anomalies indicative of strong interaction with the electron system for T >TN , but become sharp and symmetric for T phonon lifetime by the onset of magnetic order are highly unusual for Mott insulators and indicate liquidlike correlations between spins and orbitals.

  18. Diffraction of electrons at intermediate energies: The role of phonons

    NASA Astrophysics Data System (ADS)

    Ascolani, H.; Zampieri, G.

    1996-07-01

    The intensity of electrons reflected ``elastically'' from crystalline surfaces presents two regimes: the low-energy or LEED regime (<500 eV), in which the electrons are reflected along the Bragg directions, and the intermediate-energy or XPD/AED regime (>500 eV), in which the maxima of intensity are along the main crystallographic axes. We present a model which explains this transition in terms of the excitation/absorption of phonons during the scattering.

  19. Preface: Phonons 2007

    NASA Astrophysics Data System (ADS)

    Perrin, Bernard

    2007-06-01

    Conference logo The conference PHONONS 2007 was held 15-20 July 2007 in the Conservatoire National des Arts et Métiers (CNAM) Paris, France. CNAM is a college of higher technology for training students in the application of science to industry, founded by Henri Grégoire in 1794. This was the 12th International Conference on Phonon Scattering in Condensed Matter. This international conference series, held every 3 years, started in France at Sainte-Maxime in 1972. It was then followed by meetings at Nottingham (1975), Providence (1979), Stuttgart (1983), Urbana-Champaign (1986), Heidelberg (1989), Ithaca (1992), Sapporo (1995), Lancaster (1998), Dartmouth (2001) and St Petersburg (2004). PHONONS 2007 was attended by 346 delegates from 37 different countries as follows: France 120, Japan 45, Germany 25, USA 25, Russia 21, Italy 13, Poland 9, UK 9, Canada 7, The Netherlands 7, Finland 6, Spain 6, Taiwan 6, Greece 4, India 4, Israel 4, Ukraine 4, Serbia 3, South Africa 3, Argentina 2, Belgium 2, China 2, Iran 2, Korea 2, Romania 2, Switzerland 2, and one each from Belarus, Bosnia-Herzegovina, Brazil, Bulgaria, Egypt, Estonia, Mexico, Moldova, Morocco, Saudi Arabia, Turkey. There were 5 plenary lectures, 14 invited talks and 84 oral contributions; 225 posters were presented during three poster sessions. The first plenary lecture was given by H J Maris who presented fascinating movies featuring the motion of a single electron in liquid helium. Robert Blick gave us a review on the new possibilities afforded by nanotechnology to design nano-electomechanical systems (NEMS) and the way to use them to study elementary and fundamental processes. The growing interest for phonon transport studies in nanostructured materials was demonstrated by Arun Majumdar. Andrey Akimov described how ultrafast acoustic solitons can monitor the optical properties of quantum wells. Finally, Maurice Chapellier told us how

  20. Electronic structures and abnormal phonon behaviors of cobalt-modified Na0.5Bi0.5TiO3-6%BaTiO3 single crystals

    NASA Astrophysics Data System (ADS)

    Huang, T.; Zhang, P.; Xu, L. P.; Chen, C.; Zhang, J. Z.; Hu, Z. G.; Luo, H. S.; Chu, J. H.

    2016-10-01

    Optical properties, electronic structures, and structural variations of x wt% cobalt (Co) doped Na0.5Bi0.5TiO3-6%BaTiO3 (x=0%, 0.5%, 0.8%) single crystals have been studied by temperature-dependent optical ellipsometry and Raman spectra from 250 to 650 K. Based on the temperature evolution of electronic transitions (Ecp1 and Ecp2) and the phonon modes involving Ti-O vibrations, two critical temperature points exhibit an increasing trend with Co dopants, which are related to structural variations for ferroelectric to anti-ferroelectric, and anti-ferroelectric to paraelectric transition, respectively. Additionally, distinguishing abnormal phonon behaviors can be observed from Raman spectra for the crystal of x=0.5% and 0.8%, which show reverse frequency shift of the modes involving Ti-O vibration. It can be ascribed to different relative concentration of Co2+ and Co3+ in the crystals, which has been confirmed by X-ray Photoelectron Spectroscopy data.

  1. Tip-Enhanced Raman Imaging and Nano Spectroscopy of Etched Silicon Nanowires

    PubMed Central

    Kazemi-Zanjani, Nastaran; Kergrene, Erwan; Liu, Lijia; Sham, Tsun-Kong; Lagugné-Labarthet, François

    2013-01-01

    Tip-enhanced Raman spectroscopy (TERS) is used to investigate the influence of strains in isolated and overlapping silicon nanowires prepared by chemical etching of a (100) silicon wafer. An atomic force microscopy tip made of nanocrystalline diamond coated with a thin layer of silver is used in conjunction with an excitation wavelength of 532 nm in order to probe the first order optical phonon mode of the [100] silicon nanowires. The frequency shift and the broadening of the silicon first order phonon are analyzed and compared to the topographical measurements for distinct configuration of nanowires that are disposed in straight, bent or overlapping configuration over a microscope coverslip. The TERS spatial resolution is close to the topography provided by the nanocrystalline diamond tip and subtle spectral changes are observed for different nanowire configurations. PMID:24072021

  2. Transient absorption phenomena and related structural transformations in femtosecond laser-excited Si

    NASA Astrophysics Data System (ADS)

    Kudryashov, Sergey I.

    2004-09-01

    Analysis of processes affecting transient optical absorption and photogeneration of electron-hole plasma in silicon pumped by an intense NIR or visible femtosecond laser pulse has been performed taking into account the most important electron-photon, electron-electron and electron-phonon interactions and, as a result, two main regimes of such laser-matter interaction have been revealed. The first regime is concerned with indirect interband optical absorption in Si, enhanced by a coherent shrinkage of its smallest indirect bandgap due to dynamic Franz-Keldysh effect (DFKE). The second regime takes place due to the critical renormalization of the Si direct bandgap along Λ-axis of its first Brillouin zone because of DFKE and the deformation potential electron-phonon interaction and occurs as intense direct single-photon excitation of electrons into one of the quadruplet of equivalent Λ-valleys in the lowest conduction band, which is split down due to the electron-phonon interaction.

  3. Phonon Counting and Intensity Interferometry of a Nanomechanical Resonator

    DTIC Science & Technology

    2014-10-04

    photon detectors, Γdark, and the residual pump laser light which is transmitted through the filters. In this work we use a cascaded pair of tunable...T. Gerrits, I. Vayshenker, B. Baek, M. D. Shaw, R. P. Mirin, and S. W. Nam, Nature Photon . 7, 210 6 a b 0 1 10−1 FIG. 5. FEM simulations . a, Electric... photon detection we have performed effective phonon counting measurements of the acoustic emission and absorption processes in a nanomechanical res

  4. Coherent generation of symmetry-forbidden phonons by light-induced electron-phonon interactions in magnetite

    NASA Astrophysics Data System (ADS)

    Borroni, S.; Baldini, E.; Katukuri, V. M.; Mann, A.; Parlinski, K.; Legut, D.; Arrell, C.; van Mourik, F.; Teyssier, J.; Kozlowski, A.; Piekarz, P.; Yazyev, O. V.; Oleś, A. M.; Lorenzana, J.; Carbone, F.

    2017-09-01

    Symmetry breaking across phase transitions often causes changes in selection rules and emergence of optical modes which can be detected via spectroscopic techniques or generated coherently in pump-probe experiments. In second-order or weakly first-order transitions, fluctuations of the ordering field are present above the ordering temperature, giving rise to intriguing precursor phenomena, such as critical opalescence. Here, we demonstrate that in magnetite (Fe3O4 ) light excitation couples to the critical fluctuations of the charge order and coherently generates structural modes of the ordered phase above the critical temperature of the Verwey transition. Our findings are obtained by detecting coherent oscillations of the optical constants through ultrafast broadband spectroscopy and analyzing their dependence on temperature. To unveil the coupling between the structural modes and the electronic excitations, at the origin of the Verwey transition, we combine our results from pump-probe experiments with spontaneous Raman scattering data and theoretical calculations of both the phonon dispersion curves and the optical constants. Our methodology represents an effective tool to study the real-time dynamics of critical fluctuations across phase transitions.

  5. High-Pressure Synchrotron Infrared Absorption and Raman Spectroscopy of ζ-N_2

    NASA Astrophysics Data System (ADS)

    Gregoryanz, E.; Goncharov, A. F.; Mao, H. K.; Hemley, R. J.

    2000-03-01

    Infrared mid-IR and Raman spectra of high-pressure, low-temperature phases of solid nitrogen have been measured to above 40 GPa. The transition to the lower-symmetry ordered phase ζ at 21 GPa, reported by Schiferl et al. [1]. has been confirmed. We observe three Raman-active and two IR components of the nu2 stretching mode (disk-like molecules) and only one Raman-active component of the nu1 mode (sphere-like molecules). All the vibron modes increase frequency with pressure. The structure of ζ-N2 phase is discussed. [1] Schiferl et al., J. Phys. Chem., 89, 2324 (1985).

  6. Phonon properties of lutetium pnictides

    NASA Astrophysics Data System (ADS)

    Arya, Balwant Singh; Aynyas, Mahendra; Sanyal, Sankar P.

    2018-05-01

    Phonon properties of Lutetium pnictides (LuX : X = P, As) have been studied by using breathing shell model (BSM) which includes breathing motion of electrons of the Lu atoms due to f-d hybridization to establish their predominant ionic nature. The calculated phonon dispersion curves of these compounds are presented follow the same trend as observed in ytterbium pnictides (YbP and YbAs). We also report one phonon density of states and specific heat for these compounds. We discuss the significance of this approach in predicting the phonon dispersion curves and examine the role of electron-phonon interaction.

  7. A novel micro-Raman technique to detect and characterize 4H-SiC stacking faults

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Piluso, N., E-mail: nicolo.piluso@imm.cnr.it; Camarda, M.; La Via, F.

    A novel Micro-Raman technique was designed and used to detect extended defects in 4H-SiC homoepitaxy. The technique uses above band-gap high-power laser densities to induce a local increase of free carriers in undoped epitaxies (n < 10{sup 16} at/cm{sup −3}), creating an electronic plasma that couples with the longitudinal optical (LO) Raman mode. The Raman shift of the LO phonon-plasmon-coupled mode (LOPC) increases as the free carrier density increases. Crystallographic defects lead to scattering or recombination of the free carriers which results in a loss of coupling with the LOPC, and in a reduction of the Raman shift. Given that the LOmore » phonon-plasmon coupling is obtained thanks to the free carriers generated by the high injection level induced by the laser, we named this technique induced-LOPC (i-LOPC). This technique allows the simultaneous determination of both the carrier lifetime and carrier mobility. Taking advantage of the modifications on the carrier lifetime induced by extended defects, we were able to determine the spatial morphology of stacking faults; the obtained morphologies were found to be in excellent agreement with those provided by standard photoluminescence techniques. The results show that the detection of defects via i-LOPC spectroscopy is totally independent from the stacking fault photoluminescence signals that cover a large energy range up to 0.7 eV, thus allowing for a single-scan simultaneous determination of any kind of stacking fault. Combining the i-LOPC method with the analysis of the transverse optical mode, the micro-Raman characterization can determine the most important properties of unintentionally doped film, including the stress status of the wafer, lattice impurities (point defects, polytype inclusions) and a detailed analysis of crystallographic defects, with a high spectral and spatial resolution.« less

  8. Effect of boron doping on first-order Raman scattering in superconducting boron doped diamond films

    NASA Astrophysics Data System (ADS)

    Kumar, Dinesh; Chandran, Maneesh; Ramachandra Rao, M. S.

    2017-05-01

    Aggregation of impurity levels into an impurity band in heavily boron doped diamond results in a background continuum and discrete zone centre phonon interference during the inelastic light scattering process. In order to understand the Raman scattering effect in granular BDD films, systematically heavily doped samples in the semiconducting and superconducting regimes have been studied using the excitation wavelengths in the UV and visible regions. A comprehensive analysis of the Fano resonance effect as a function of the impurity concentrations and the excitation frequencies is presented. Various Raman modes available in BDD including signals from the grain boundaries are discussed.

  9. Raman microscopic studies of PVD deposited hard ceramic coatings

    NASA Astrophysics Data System (ADS)

    Constable, Christopher Paul

    PVD hard ceramic coatings grown via the combined cathodic arc/unbalance magnetron deposition process were studied using Raman microscopy. Characteristic spectra from binary, multicomponent, multilayered and superlattice coatings were acquired to gain knowledge of the solid-state physics associated with Raman scattering from polycrystalline PVD coatings and to compile a comprehensive spectral database. Defect-induced first order scattering mechanisms were observed which gave rise to two pronounced groups of bands related to the acoustical (150-300cm[-1]) and optical (400-750cm[-1]) parts of the phonon spectrum. Evidence was gathered to support the theory that the optic modes were mainly due to the vibrations of the lighter elements and the acoustic modes due to the vibrations of the heavier elements within the lattice.A study into the deformation and disordering on the Raman spectral bands of PVD coatings was performed. TiAIN and TiZrN coatings were intentionally damaged via scratching methods. These scratches were then analysed by Raman mapping, both across and along, and a detailed spectral interpretation performed. Band broadening occurred which was related to "phonon relaxation mechanisms" as a direct result of the breaking up of coating grains resulting in a larger proportion of grain boundaries per-unit-volume. A direct correlation of the amount of damage with band width was observed. Band shifts were also found to occur which were due to the stresses caused by the scratching process. These shifts were found to be the largest at the edges of scratches. The Raman mapping of "droplets", a defect inherent to PVD deposition processes, found that higher compressive stresses and large amounts of disorder occurred for coating growth onto droplets.Strategies designed to evaluate the ability of Raman microscopy to monitor the extent of real wear on cutting tools were evaluated. The removal of a coating layer and subsequent detection of a base layer proved successful

  10. Ballistic phonon transport in holey silicon.

    PubMed

    Lee, Jaeho; Lim, Jongwoo; Yang, Peidong

    2015-05-13

    When the size of semiconductors is smaller than the phonon mean free path, phonons can carry heat with no internal scattering. Ballistic phonon transport has received attention for both theoretical and practical aspects because Fourier's law of heat conduction breaks down and the heat dissipation in nanoscale transistors becomes unpredictable in the ballistic regime. While recent experiments demonstrate room-temperature evidence of ballistic phonon transport in various nanomaterials, the thermal conductivity data for silicon in the length scale of 10-100 nm is still not available due to experimental challenges. Here we show ballistic phonon transport prevails in the cross-plane direction of holey silicon from 35 to 200 nm. The thermal conductivity scales linearly with the length (thickness) even though the lateral dimension (neck) is as narrow as 20 nm. We assess the impact of long-wavelength phonons and predict a transition from ballistic to diffusive regime using scaling models. Our results support strong persistence of long-wavelength phonons in nanostructures and are useful for controlling phonon transport for thermoelectrics and potential phononic applications.

  11. Intermolecular electron transfer from intramolecular excitation and coherent acoustic phonon generation in a hydrogen-bonded charge-transfer solid

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Rury, Aaron S., E-mail: arury@usc.edu; Sorenson, Shayne; Dawlaty, Jahan M.

    2016-03-14

    Organic materials that produce coherent lattice phonon excitations in response to external stimuli may provide next generation solutions in a wide range of applications. However, for these materials to lead to functional devices in technology, a full understanding of the possible driving forces of coherent lattice phonon generation must be attained. To facilitate the achievement of this goal, we have undertaken an optical spectroscopic study of an organic charge-transfer material formed from the ubiquitous reduction-oxidation pair hydroquinone and p-benzoquinone. Upon pumping this material, known as quinhydrone, on its intermolecular charge transfer resonance as well as an intramolecular resonance of p-benzoquinone,more » we find sub-cm{sup −1} oscillations whose dispersion with probe energy resembles that of a coherent acoustic phonon that we argue is coherently excited following changes in the electron density of quinhydrone. Using the dynamical information from these ultrafast pump-probe measurements, we find that the fastest process we can resolve does not change whether we pump quinhydrone at either energy. Electron-phonon coupling from both ultrafast coherent vibrational and steady-state resonance Raman spectroscopies allows us to determine that intramolecular electronic excitation of p-benzoquinone also drives the electron transfer process in quinhydrone. These results demonstrate the wide range of electronic excitations of the parent of molecules found in many functional organic materials that can drive coherent lattice phonon excitations useful for applications in electronics, photonics, and information technology.« less

  12. Intermolecular electron transfer from intramolecular excitation and coherent acoustic phonon generation in a hydrogen-bonded charge-transfer solid

    NASA Astrophysics Data System (ADS)

    Rury, Aaron S.; Sorenson, Shayne; Dawlaty, Jahan M.

    2016-03-01

    Organic materials that produce coherent lattice phonon excitations in response to external stimuli may provide next generation solutions in a wide range of applications. However, for these materials to lead to functional devices in technology, a full understanding of the possible driving forces of coherent lattice phonon generation must be attained. To facilitate the achievement of this goal, we have undertaken an optical spectroscopic study of an organic charge-transfer material formed from the ubiquitous reduction-oxidation pair hydroquinone and p-benzoquinone. Upon pumping this material, known as quinhydrone, on its intermolecular charge transfer resonance as well as an intramolecular resonance of p-benzoquinone, we find sub-cm-1 oscillations whose dispersion with probe energy resembles that of a coherent acoustic phonon that we argue is coherently excited following changes in the electron density of quinhydrone. Using the dynamical information from these ultrafast pump-probe measurements, we find that the fastest process we can resolve does not change whether we pump quinhydrone at either energy. Electron-phonon coupling from both ultrafast coherent vibrational and steady-state resonance Raman spectroscopies allows us to determine that intramolecular electronic excitation of p-benzoquinone also drives the electron transfer process in quinhydrone. These results demonstrate the wide range of electronic excitations of the parent of molecules found in many functional organic materials that can drive coherent lattice phonon excitations useful for applications in electronics, photonics, and information technology.

  13. Impact of Graphene-Metal Interfaces on the Raman and Transport Properties of Graphene Devices

    NASA Astrophysics Data System (ADS)

    Hsu, Allen; Hofmann, Mario; Fang, Wenjing; Kimg, Ki Kang; Kong, Jing; Palacios, Tomas

    2012-02-01

    Graphene is an amazing nano-material with many exciting properties and applications. However, due to its low dimensionality, the performance of this material is mainly limited by interfaces and surface properties. One of these interfaces, important for graphene field effect transistors and catalysts supported on graphene membranes, is that between the graphene and a metal layer. In this study, we experimentally examine the impact of various metals on graphene through Raman and Transmission Electron Microscopy. We find that strong graphene-metal interactions have significant impacts on the phonon structure in graphene. Furthermore, we observe changes in our Raman spectra relating to the crystallographic orientation between a metal and graphene.

  14. Effects of low energy E-beam irradiation on graphene and graphene field effect transistors and raman metrology of graphene on split gate test structures

    NASA Astrophysics Data System (ADS)

    Rao, Gayathri S.

    2011-12-01

    measured Raman ID/IG ratios. Additionally, the Raman G-band DeltaFWHM variation was strongly dependent on the nature of the e-beam irradiation and the presence of the substrate. Single-step irradiated, substrate-supported graphene exhibited substantial broadening while multi-step irradiation resulted in G-band narrowing. This behavior was not observed for suspended graphene which indicated the addition or elimination of substrate-induced phonon-relaxation mechanisms in response to each type of irradiation. The narrowing of the FWHM (G) in the multi-step case is attributed to doping consistent with the Dirac point shift of ˜ -16V and the removal of Landau phonon damping above Ef > ℏwG2 . In strong contrast, single step irradiation of substrate supported graphene yielded a broadening of the FWHM (G) accompanied by a CNP shift of ˜ -8V indicating appreciable n-doping. This reveals the presence of alternate phonon decay channels even when Landau damping above Ef > ℏwG2 is removed. It is proposed in this dissertation that this phenomenon is linked to hybridization of silicon oxide defect states (induced by single-step e-beam irradiation) and graphene electron states. This hybridization promotes a graphene phonon decay channel distinct from Landau damping, the latter being forbidden under sufficient doping. It is proposed that the alternate phonon decay channel involves two-component inelastic scattering, wherein the graphene phonons transfer energy to the carriers in the lattice which in turn couple to the polar phonons of the substrate resulting in mobility reduction. Furthermore, it is proposed that this defect-induced, graphene phonon decay channel is inhibited in multi-step e-beam irradiation due to the presence of adsorbates on the graphene introduced during ambient exposure between radiation cycles. On e-beam irradiation the adsorbates induce polar orientation of water dipoles at the graphene/SiO2 interface. This polar layer shifts the hybridized defect bands closer

  15. Wide-Stopband Aperiodic Phononic Filters

    NASA Technical Reports Server (NTRS)

    Rostem, Karwan; Chuss, David; Denis, K. L.; Wollack, E. J.

    2016-01-01

    We demonstrate that a phonon stopband can be synthesized from an aperiodic structure comprising a discrete set of phononic filter stages. Each element of the set has a dispersion relation that defines a complete bandgap when calculated under a Bloch boundary condition. Hence, the effective stopband width in an aperiodic phononic filter (PnF) may readily exceed that of a phononic crystal with a single lattice constant or a coherence scale. With simulations of multi-moded phononic waveguides, we discuss the effects of finite geometry and mode-converting junctions on the phonon transmission in PnFs. The principles described may be utilized to form a wide stopband in acoustic and surface wave media. Relative to the quantum of thermal conductance for a uniform mesoscopic beam, a PnF with a stopband covering 1.6-10.4 GHz is estimated to reduce the thermal conductance by an order of magnitude at 75 mK.

  16. Self-consistency in the phonon space of the particle-phonon coupling model

    NASA Astrophysics Data System (ADS)

    Tselyaev, V.; Lyutorovich, N.; Speth, J.; Reinhard, P.-G.

    2018-04-01

    In the paper the nonlinear generalization of the time blocking approximation (TBA) is presented. The TBA is one of the versions of the extended random-phase approximation (RPA) developed within the Green-function method and the particle-phonon coupling model. In the generalized version of the TBA the self-consistency principle is extended onto the phonon space of the model. The numerical examples show that this nonlinear version of the TBA leads to the convergence of results with respect to enlarging the phonon space of the model.

  17. Temperature performance analysis of intersubband Raman laser in quantum cascade structures

    NASA Astrophysics Data System (ADS)

    Yousefvand, Hossein Reza

    2017-06-01

    In this paper we investigate the effects of temperature on the output characteristics of the intersubband Raman laser (RL) that integrated monolithically with a quantum cascade (QC) laser as an intracavity optical pump. The laser bandstructure is calculated by a self-consistent solution of Schrodinger-Poisson equations, and the employed physical model of carrier transport is based on a five-level carrier scattering rates; a two-level rate equations for the pump laser and a three-level scattering rates to include the stimulated Raman process in the RL. The temperature dependency of the relevant physical effects such as thermal broadening of the intersubband transitions (ISTs), thermally activated phonon emission lifetimes, and thermal backfilling of the final lasing state of the Raman process from the injector are included in the model. Using the presented model, the steady-state, small-signal modulation response and transient device characteristics are investigated for a range of sink temperatures (80-220 K). It is found that the main characteristics of the device such as output power, threshold current, Raman modal gain, turn-on delay time and 3-dB optical bandwidth are remarkably affected by the temperature.

  18. Monolithic phononic crystals with a surface acoustic band gap from surface phonon-polariton coupling.

    PubMed

    Yudistira, D; Boes, A; Djafari-Rouhani, B; Pennec, Y; Yeo, L Y; Mitchell, A; Friend, J R

    2014-11-21

    We theoretically and experimentally demonstrate the existence of complete surface acoustic wave band gaps in surface phonon-polariton phononic crystals, in a completely monolithic structure formed from a two-dimensional honeycomb array of hexagonal shape domain-inverted inclusions in single crystal piezoelectric Z-cut lithium niobate. The band gaps appear at a frequency of about twice the Bragg band gap at the center of the Brillouin zone, formed through phonon-polariton coupling. The structure is mechanically, electromagnetically, and topographically homogeneous, without any physical alteration of the surface, offering an ideal platform for many acoustic wave applications for photonics, phononics, and microfluidics.

  19. Grain boundary-dominated electrical conduction and anomalous optical-phonon behaviour near the Neel temperature in YFeO3 ceramics

    NASA Astrophysics Data System (ADS)

    Raut, Subhajit; Babu, P. D.; Sharma, R. K.; Pattanayak, Ranjit; Panigrahi, Simanchalo

    2018-05-01

    We investigated the anomalous behaviour in the dielectric properties, occurring nearly at room temperature and at elevated temperatures (near the Neel temperature TN) of the polycrystalline samples of YFeO3 (YFO) ceramics. On the prepared YFO ceramics, the magnetic measurements showed the Neel temperature of YFO to be 650 K, below which the compound exhibited the weak ferromagnetic behaviour. X-ray photoelectron spectroscopy (XPS) shows the presence of Fe ions (Fe2+ and Fe3+ states) and also revealed the formation of the oxygen vacancies. The frequency dependence of the complex dielectric constant within the frequency domain of 100 Hz-1 MHz shows the presence of grain dominated dielectric relaxation over the thermal window of 300-373 K. The activation energy Eact.ɛ=0.611 eV extracted from the imaginary permittivity spectrum indicates the involvement of oxygen vacancies in the relaxation process. Above 493 K, the ac conductivity, complex impedance, and modulus studies revealed appreciable conduction and relaxation processes occurring in YFO ceramics with respective activation energies Eac t . σ=1.362 eV and Eac t . Z=1.345 eV , which suggests that the oxygen vacancies are also involved for the anomalous behaviour of the dielectric constant at elevated temperatures. The temperature dependent Raman spectroscopic measurements within the thermal window of 298-698 K showed anomalous variations of the line widths and frequencies of several Raman active modes above 473 K up to the vicinity of TN pointing towards the presence of admixtures of the electron-phonon and spin-phonon coupling in the system. A further study on the thermal variation of the B2g(4) mode frequency with [M(T)/MS]2 shows the occurrence of strong spin-phonon (s-p) coupling, while the line shape shows the presence of the Fano asymmetry, suggesting spin dependent electron-phonon (e-p) coupling in the system below TN.

  20. Nanoscale Phonon Transport as Probed with a Microfabricated Phonon Spectrometer for the Study of Nanoscale Energy Transport

    NASA Astrophysics Data System (ADS)

    Robinson, Richard; Otelaja, Obafemi; Hertzberg, Jared; Aksit, Mahmut; Stewart, Derek

    2013-03-01

    Phonons are the dominant heat carriers in dielectrics and a clear understanding of their behavior at the nanoscale is important for the development of efficient thermoelectric devices. In this work we show how acoustic phonon transport can be directly probed by the generation and detection of non-equilibrium phonons in microscale and nanoscale structures. Our technique employs a scalable method of fabricating phonon generators and detectors by forming Al-AlxOy-Al superconducting tunnel junctions on the sidewalls of a silicon mesa etched with KOH and an operating temperature of 0.3K. In the line-of-sight path along the width of these mesas, phonons with frequency ~100 GHz can propagate ballistically The phonons radiate into the mesa and are observed by the detector after passing through the mesa. We fabricated silicon nanosheets of width 100 to 300 nm along the ballistic path and observe surface scattering effects on phonon transmission when the characteristic length scale of a material is less than the phonon mean free path. We compare our results to the Casimir-Ziman theory. Our methods can be adapted for studying phonon transport in other nanostructures and will improve the understanding of phonon contribution to thermal transport. The work was supported in part by the National Science Foundation under Agreement No. DMR-1149036.

  1. Effect of incorporation of ethylene glycol into PEDOT:PSS on electron phonon coupling and conductivity

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Lin, Yow-Jon, E-mail: rzr2390@yahoo.com.tw; Ni, Wei-Shih; Lee, Jhe-You

    2015-06-07

    The effect of incorporation of ethylene glycol (EG) into poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) on electron phonon coupling and conductivity is investigated. It is shown that the carrier density (N{sub C}) increases significantly and the carrier mobility (μ) increases slightly at 300 K. The increased intensity of the Raman spectrum between 1400 and 1450 cm{sup −1}, following EG treatment (that is, the quinoid-dominated structures of the PEDOT chain), leads to an increase in the number of polarons (bipolarons), which leads to an increase in N{sub C}. In addition, μ in PEDOT:PSS samples with or without EG addition exhibits a strong temperature dependence, which demonstrates themore » dominance of tunneling (hopping) at low (high) temperatures. The high conductivity of PEDOT:PSS samples with the addition of EG is attributed to the combined effect of the modification of the electron-phonon coupling and the increase in N{sub C} (μ)« less

  2. 2D Raman band splitting in graphene: Charge screening and lifting of the K-point Kohn anomaly.

    PubMed

    Wang, Xuanye; Christopher, Jason W; Swan, Anna K

    2017-10-19

    Pristine graphene encapsulated in hexagonal boron nitride has transport properties rivalling suspended graphene, while being protected from contamination and mechanical damage. For high quality devices, it is important to avoid and monitor accidental doping and charge fluctuations. The 2D Raman double peak in intrinsic graphene can be used to optically determine charge density, with decreasing peak split corresponding to increasing charge density. We find strong correlations between the 2D 1 and 2D 2 split vs 2D line widths, intensities, and peak positions. Charge density fluctuations can be measured with orders of magnitude higher precision than previously accomplished using the G-band shift with charge. The two 2D intrinsic peaks can be associated with the "inner" and "outer" Raman scattering processes, with the counterintuitive assignment of the phonon closer to the K point in the KM direction (outer process) as the higher energy peak. Even low charge screening lifts the phonon Kohn anomaly near the K point for graphene encapsulated in hBN, and shifts the dominant intensity from the lower to the higher energy peak.

  3. Influence of piezoelectric strain on the Raman spectra of BiFeO{sub 3} films deposited on PMN-PT substrates

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Himcinschi, Cameliu, E-mail: himcinsc@physik.tu-freiberg.de; Talkenberger, Andreas; Kortus, Jens

    2016-01-25

    BiFeO{sub 3} epitaxial thin films were deposited on piezoelectric 0.72Pb(Mg{sub 1/3}Nb{sub 2/3})O{sub 3}-0.28PbTiO{sub 3} (PMN-PT) substrates with a conductive buffer layer (La{sub 0.7}Sr{sub 0.3}MnO{sub 3} or SrRuO{sub 3}) using pulsed laser deposition. The calibration of the strain values induced by the electric field applied on the piezoelectric PMN-PT substrates was realised using X-Ray diffraction measurements. The method of piezoelectrically induced strain allows one to directly obtain a quantitative correlation between the strain and the shift of the Raman-active phonons. This is a prerequisite for making Raman scattering a strong tool to probe the strain coupling in multiferroic nanostructures. Using themore » Poisson's number for BiFeO{sub 3}, one can determine the volume change induced by strain, and therefore the Grüneisen parameters for specific phonon modes.« less

  4. Spacetime representation of topological phononics

    NASA Astrophysics Data System (ADS)

    Deymier, Pierre A.; Runge, Keith; Lucas, Pierre; Vasseur, Jérôme O.

    2018-05-01

    Non-conventional topology of elastic waves arises from breaking symmetry of phononic structures either intrinsically through internal resonances or extrinsically via application of external stimuli. We develop a spacetime representation based on twistor theory of an intrinsic topological elastic structure composed of a harmonic chain attached to a rigid substrate. Elastic waves in this structure obey the Klein–Gordon and Dirac equations and possesses spinorial character. We demonstrate the mapping between straight line trajectories of these elastic waves in spacetime and the twistor complex space. The twistor representation of these Dirac phonons is related to their topological and fermion-like properties. The second topological phononic structure is an extrinsic structure composed of a one-dimensional elastic medium subjected to a moving superlattice. We report an analogy between the elastic behavior of this time-dependent superlattice, the scalar quantum field theory and general relativity of two types of exotic particle excitations, namely temporal Dirac phonons and temporal ghost (tachyonic) phonons. These phonons live on separate sides of a two-dimensional frequency space and are delimited by ghost lines reminiscent of the conventional light cone. Both phonon types exhibit spinorial amplitudes that can be measured by mapping the particle behavior to the band structure of elastic waves.

  5. Simultaneous measurement of temperature, stress, and electric field in GaN HEMTs with micro-Raman spectroscopy.

    PubMed

    Bagnall, Kevin R; Moore, Elizabeth A; Badescu, Stefan C; Zhang, Lenan; Wang, Evelyn N

    2017-11-01

    As semiconductor devices based on silicon reach their intrinsic material limits, compound semiconductors, such as gallium nitride (GaN), are gaining increasing interest for high performance, solid-state transistor applications. Unfortunately, higher voltage, current, and/or power levels in GaN high electron mobility transistors (HEMTs) often result in elevated device temperatures, degraded performance, and shorter lifetimes. Although micro-Raman spectroscopy has become one of the most popular techniques for measuring localized temperature rise in GaN HEMTs for reliability assessment, decoupling the effects of temperature, mechanical stress, and electric field on the optical phonon frequencies measured by micro-Raman spectroscopy is challenging. In this work, we demonstrate the simultaneous measurement of temperature rise, inverse piezoelectric stress, thermoelastic stress, and vertical electric field via micro-Raman spectroscopy from the shifts of the E 2 (high), A 1 longitudinal optical (LO), and E 2 (low) optical phonon frequencies in wurtzite GaN. We also validate experimentally that the pinched OFF state as the unpowered reference accurately measures the temperature rise by removing the effect of the vertical electric field on the Raman spectrum and that the vertical electric field is approximately the same whether the channel is open or closed. Our experimental results are in good quantitative agreement with a 3D electro-thermo-mechanical model of the HEMT we tested and indicate that the GaN buffer acts as a semi-insulating, p-type material due to the presence of deep acceptors in the lower half of the bandgap. This implementation of micro-Raman spectroscopy offers an exciting opportunity to simultaneously probe thermal, mechanical, and electrical phenomena in semiconductor devices under bias, providing unique insight into the complex physics that describes device behavior and reliability. Although GaN HEMTs have been specifically used in this study to

  6. Simultaneous measurement of temperature, stress, and electric field in GaN HEMTs with micro-Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Bagnall, Kevin R.; Moore, Elizabeth A.; Badescu, Stefan C.; Zhang, Lenan; Wang, Evelyn N.

    2017-11-01

    As semiconductor devices based on silicon reach their intrinsic material limits, compound semiconductors, such as gallium nitride (GaN), are gaining increasing interest for high performance, solid-state transistor applications. Unfortunately, higher voltage, current, and/or power levels in GaN high electron mobility transistors (HEMTs) often result in elevated device temperatures, degraded performance, and shorter lifetimes. Although micro-Raman spectroscopy has become one of the most popular techniques for measuring localized temperature rise in GaN HEMTs for reliability assessment, decoupling the effects of temperature, mechanical stress, and electric field on the optical phonon frequencies measured by micro-Raman spectroscopy is challenging. In this work, we demonstrate the simultaneous measurement of temperature rise, inverse piezoelectric stress, thermoelastic stress, and vertical electric field via micro-Raman spectroscopy from the shifts of the E2 (high), A1 longitudinal optical (LO), and E2 (low) optical phonon frequencies in wurtzite GaN. We also validate experimentally that the pinched OFF state as the unpowered reference accurately measures the temperature rise by removing the effect of the vertical electric field on the Raman spectrum and that the vertical electric field is approximately the same whether the channel is open or closed. Our experimental results are in good quantitative agreement with a 3D electro-thermo-mechanical model of the HEMT we tested and indicate that the GaN buffer acts as a semi-insulating, p-type material due to the presence of deep acceptors in the lower half of the bandgap. This implementation of micro-Raman spectroscopy offers an exciting opportunity to simultaneously probe thermal, mechanical, and electrical phenomena in semiconductor devices under bias, providing unique insight into the complex physics that describes device behavior and reliability. Although GaN HEMTs have been specifically used in this study to

  7. Time-varying phononic crystals

    NASA Astrophysics Data System (ADS)

    Wright, Derek Warren

    The primary objective of this thesis was to gain a deeper understanding of acoustic wave propagation in phononic crystals, particularly those that include materials whose properties can be varied periodically in time. This research was accomplished in three ways. First, a 2D phononic crystal was designed, created, and characterized. Its properties closely matched those determined through simulation. The crystal demonstrated band gaps, dispersion, and negative refraction. It served as a means of elucidating the practicalities of phononic crystal design and construction and as a physical verification of their more interesting properties. Next, the transmission matrix method for analyzing 1D phononic crystals was extended to include the effects of time-varying material parameters. The method was then used to provide a closed-form solution for the case of periodically time-varying material parameters. Some intriguing results from the use of the extended method include dramatically altered transmission properties and parametric amplification. New insights can be gained from the governing equations and have helped to identify the conditions that lead to parametric amplification in these structures. Finally, 2D multiple scattering theory was modified to analyze scatterers with time-varying material parameters. It is shown to be highly compatible with existing multiple scattering theories. It allows the total scattered field from a 2D time-varying phononic crystal to be determined. It was shown that time-varying material parameters significantly affect the phononic crystal transmission spectrum, and this was used to switch an incident monochromatic wave. Parametric amplification can occur under certain circumstances, and this effect was investigated using the closed-form solutions provided by the new 1D method. The complexity of the extended methods grows logarithmically as opposed linearly with existing methods, resulting in superior computational complexity for large

  8. Midinfrared absorption measured at a lambda/400 resolution with an atomic force microscope.

    PubMed

    Houel, Julien; Homeyer, Estelle; Sauvage, Sébastien; Boucaud, Philippe; Dazzi, Alexandre; Prazeres, Rui; Ortéga, Jean-Michel

    2009-06-22

    Midinfrared absorption can be locally measured using a detection combining an atomic force microscope and a pulsed excitation. This is illustrated for the midinfrared bulk GaAs phonon absorption and for the midinfrared absorption of thin SiO(2) microdisks. We show that the signal given by the cantilever oscillation amplitude of the atomic force microscope follows the spectral dependence of the bulk material absorption. The absorption spatial resolution achieved with microdisks is around 50 nanometer for an optical excitation around 22 micrometer wavelength.

  9. Raman spectroscopy in transition metals and alloys at ultrahigh pressures.

    NASA Astrophysics Data System (ADS)

    Goncharov, Alexander; Gregoryanz, Eugene; Struzhkin, Viktor; Hemley, Russell; Mao, Ho-Kwang; Merkel, Sebastien; Huang, Eugene

    2001-03-01

    We present the results of Raman measurements of hexagonal close-packed phases of Fe, Fe_(1-x)Nix (x=0.01-0.2), Re up to megabar pressures (>100 GPa). We compare frequencies and their pressure dependences of the Raman-active E_2g mode for different compositions. We find a substantial decrease in the phonon frequency for Fe:Ne alloy compared to pure Fe, which is tentatively attributed to magneto-elastic coupling. We also determine the mode Grüneisen parameters and compare them to other experimental results and theoretical calculations. The data for pure Fe and Re are used to determine the pressure dependence of the C_44 shear elastic modulus [1,2]. [1] A. P. Jephcoat, H. Olijnyk, K. Refson, Eos 80, F929 (1999). [2] S. Merkel et al., Science 288, 1626 (2000).

  10. First principles calculation of lattice thermal conductivity of metals considering phonon-phonon and phonon-electron scattering

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Wang, Yan; Lu, Zexi; Ruan, Xiulin, E-mail: ruan@purdue.edu

    2016-06-14

    The effect of phonon-electron (p-e) scattering on lattice thermal conductivity is investigated for Cu, Ag, Au, Al, Pt, and Ni. We evaluate both phonon-phonon (p-p) and p-e scattering rates from first principles and calculate the lattice thermal conductivity (κ{sub L}). It is found that p-e scattering plays an important role in determining the κ{sub L} of Pt and Ni at room temperature, while it has negligible effect on the κ{sub L} of Cu, Ag, Au, and Al. Specifically, the room temperature κ{sub L}s of Cu, Ag, Au, and Al predicted from density-functional theory calculations with the local density approximation aremore » 16.9, 5.2, 2.6, and 5.8 W/m K, respectively, when only p-p scattering is considered, while it is almost unchanged when p-e scattering is also taken into account. However, the κ{sub L} of Pt and Ni is reduced from 7.1 and 33.2 W/m K to 5.8 and 23.2 W/m K by p-e scattering. Even though Al has quite high electron-phonon coupling constant, a quantity that characterizes the rate of heat transfer from hot electrons to cold phonons in the two-temperature model, p-e scattering is not effective in reducing κ{sub L} owing to the relatively low p-e scattering rates in Al. The difference in the strength of p-e scattering in different metals can be qualitatively understood by checking the amount of electron density of states that is overlapped with the Fermi window. Moreover, κ{sub L} is found to be comparable to the electronic thermal conductivity in Ni.« less

  11. Cavity-enhanced Raman microscopy of individual carbon nanotubes

    PubMed Central

    Hümmer, Thomas; Noe, Jonathan; Hofmann, Matthias S.; Hänsch, Theodor W.; Högele, Alexander; Hunger, David

    2016-01-01

    Raman spectroscopy reveals chemically specific information and provides label-free insight into the molecular world. However, the signals are intrinsically weak and call for enhancement techniques. Here, we demonstrate Purcell enhancement of Raman scattering in a tunable high-finesse microcavity, and utilize it for molecular diagnostics by combined Raman and absorption imaging. Studying individual single-wall carbon nanotubes, we identify crucial structural parameters such as nanotube radius, electronic structure and extinction cross-section. We observe a 320-times enhanced Raman scattering spectral density and an effective Purcell factor of 6.2, together with a collection efficiency of 60%. Potential for significantly higher enhancement, quantitative signals, inherent spectral filtering and absence of intrinsic background in cavity-vacuum stimulated Raman scattering render the technique a promising tool for molecular imaging. Furthermore, cavity-enhanced Raman transitions involving localized excitons could potentially be used for gaining quantum control over nanomechanical motion and open a route for molecular cavity optomechanics. PMID:27402165

  12. Generalization of soft phonon modes

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Rudin, Sven P.

    Soft phonon modes describe a collective movement of atoms that transform a higher-symmetry crystal structure into a lower-symmetry crystal structure. Such structural transformations occur at finite temperatures, where the phonons (i.e., the low-temperature vibrational modes) and the static perfect crystal structures provide an incomplete picture of the dynamics. In this paper, principal vibrational modes (PVMs) are introduced as descriptors of the dynamics of a material system withmore » $N$ atoms. The PVMs represent the independent collective movements of the atoms at a given temperature. Molecular dynamics (MD) simulations, here in the form of quantum MD using density functional theory calculations, provide both the data describing the atomic motion and the data used to construct the PVMs. The leading mode, $${\\mathrm{PVM}}_{0}$$, represents the $3N$-dimensional direction in which the system moves with greatest amplitude. For structural phase transitions, $${\\mathrm{PVM}}_{0}$$ serves as a generalization of soft phonon modes. At low temperatures, $${\\mathrm{PVM}}_{0}$$ reproduces the soft phonon mode in systems where one phonon dominates the phase transformation. In general, multiple phonon modes combine to describe a transformation, in which case $${\\mathrm{PVM}}_{0}$$ culls these phonon modes. Moreover, while soft phonon modes arise in the higher-symmetry crystal structure, $${\\mathrm{PVM}}_{0}$$ can be equally well calculated on either side of the structural phase transition. Finally, two applications demonstrate these properties: first, transitions into and out of bcc titanium, and, second, the two crystal structures proposed for the $${\\beta}$$ phase of uranium, the higher-symmetry structure of which stabilizes with temperature.« less

  13. Generalization of soft phonon modes

    DOE PAGES

    Rudin, Sven P.

    2018-04-27

    Soft phonon modes describe a collective movement of atoms that transform a higher-symmetry crystal structure into a lower-symmetry crystal structure. Such structural transformations occur at finite temperatures, where the phonons (i.e., the low-temperature vibrational modes) and the static perfect crystal structures provide an incomplete picture of the dynamics. In this paper, principal vibrational modes (PVMs) are introduced as descriptors of the dynamics of a material system withmore » $N$ atoms. The PVMs represent the independent collective movements of the atoms at a given temperature. Molecular dynamics (MD) simulations, here in the form of quantum MD using density functional theory calculations, provide both the data describing the atomic motion and the data used to construct the PVMs. The leading mode, $${\\mathrm{PVM}}_{0}$$, represents the $3N$-dimensional direction in which the system moves with greatest amplitude. For structural phase transitions, $${\\mathrm{PVM}}_{0}$$ serves as a generalization of soft phonon modes. At low temperatures, $${\\mathrm{PVM}}_{0}$$ reproduces the soft phonon mode in systems where one phonon dominates the phase transformation. In general, multiple phonon modes combine to describe a transformation, in which case $${\\mathrm{PVM}}_{0}$$ culls these phonon modes. Moreover, while soft phonon modes arise in the higher-symmetry crystal structure, $${\\mathrm{PVM}}_{0}$$ can be equally well calculated on either side of the structural phase transition. Finally, two applications demonstrate these properties: first, transitions into and out of bcc titanium, and, second, the two crystal structures proposed for the $${\\beta}$$ phase of uranium, the higher-symmetry structure of which stabilizes with temperature.« less

  14. Generalization of soft phonon modes

    NASA Astrophysics Data System (ADS)

    Rudin, Sven P.

    2018-04-01

    Soft phonon modes describe a collective movement of atoms that transform a higher-symmetry crystal structure into a lower-symmetry crystal structure. Such structural transformations occur at finite temperatures, where the phonons (i.e., the low-temperature vibrational modes) and the static perfect crystal structures provide an incomplete picture of the dynamics. Here, principal vibrational modes (PVMs) are introduced as descriptors of the dynamics of a material system with N atoms. The PVMs represent the independent collective movements of the atoms at a given temperature. Molecular dynamics (MD) simulations, here in the form of quantum MD using density functional theory calculations, provide both the data describing the atomic motion and the data used to construct the PVMs. The leading mode, PVM0, represents the 3 N -dimensional direction in which the system moves with greatest amplitude. For structural phase transitions, PVM0 serves as a generalization of soft phonon modes. At low temperatures, PVM0 reproduces the soft phonon mode in systems where one phonon dominates the phase transformation. In general, multiple phonon modes combine to describe a transformation, in which case PVM0 culls these phonon modes. Moreover, while soft phonon modes arise in the higher-symmetry crystal structure, PVM0 can be equally well calculated on either side of the structural phase transition. Two applications demonstrate these properties: first, transitions into and out of bcc titanium, and, second, the two crystal structures proposed for the β phase of uranium, the higher-symmetry structure of which stabilizes with temperature.

  15. The Influence of Trace Gases Absorption on Differential Ring Cross Sections

    NASA Astrophysics Data System (ADS)

    Han, Dong; Zhao, Keyi

    2017-04-01

    The Ring effect refers to the filling in of Fraunhofer lines, which is known as solar absorption lines, caused almost entirely by rotational Raman scattering. The rotational Raman scattering by N2 and O2 in the atmosphere is the main factor that leads to Ring effect. The Ring effect is one significant limitation to the accuracy of the retrieval of trace gas constituents in atmosphere, while using satellite data with Differential Optical Absorption Spectroscopy technique. In this study, firstly the solar spectrum is convolved with rotational Raman cross sections of atmosphere, which is calculated with rotational Raman cross sections of N2 and O2, divided by the original solar spectrum, with a cubic polynomial subtracted off, to create differential Ring spectrum Ring1. Secondly, the Ring effect for pure Raman scattering of the Fraunhofer spectrum plus the contribution from interference by terrestrial absorption which always comes from a kind of trace gas (e.g., O3) are derived. To allow for more generality, the optically thin term as well as the next term in the expansion for the Beer-Lambert law are calculated.Ring1, Ring2, and Ring3are the Fraunhofer only, 1st terrestrial correction, and 2nd terrestrial correction for DOAS fitting.

  16. Sound and heat revolutions in phononics

    NASA Astrophysics Data System (ADS)

    Maldovan, Martin

    2013-11-01

    The phonon is the physical particle representing mechanical vibration and is responsible for the transmission of everyday sound and heat. Understanding and controlling the phononic properties of materials provides opportunities to thermally insulate buildings, reduce environmental noise, transform waste heat into electricity and develop earthquake protection. Here I review recent progress and the development of new ideas and devices that make use of phononic properties to control both sound and heat. Advances in sonic and thermal diodes, optomechanical crystals, acoustic and thermal cloaking, hypersonic phononic crystals, thermoelectrics, and thermocrystals herald the next technological revolution in phononics.

  17. Coherent Manipulation of Phonons at the Nanoscale

    NASA Astrophysics Data System (ADS)

    Yu, Shangjie; Ouyang, Min

    Phonons play a key role in almost every physical process, including for example dephasing phenomena of electronic quantum states, electric and heat transports. Therefore, understanding and even manipulating phonons represent a pre-requisite for tailoring phonons-mediated physical processes. In this talk, we will first present how to employ ultrafast optical spectroscopy to probe acoustic phonon modes in colloidal metallic nanoparticles. Furthermore, we have developed various phonon manipulation schemes that can be achieved by a train of optical pulses in time domain to allow selective control of phonon modes. Our theoretical modeling and simulation demonstrates an excellent agreement with experimental results, thus providing a future guideline on more complex phononic control at the nanoscale.

  18. Coherent acoustic phonons in nanostructures

    NASA Astrophysics Data System (ADS)

    Dekorsy, T.; Taubert, R.; Hudert, F.; Bartels, A.; Habenicht, A.; Merkt, F.; Leiderer, P.; Köhler, K.; Schmitz, J.; Wagner, J.

    2008-02-01

    Phonons are considered as a most important origin of scattering and dissipation for electronic coherence in nanostructures. The generation of coherent acoustic phonons with femtosecond laser pulses opens the possibility to control phonon dynamics in amplitude and phase. We demonstrate a new experimental technique based on two synchronized femtosecond lasers with GHz repetition rate to study the dynamics of coherently generated acoustic phonons in semiconductor heterostructures with high sensitivity. High-speed synchronous optical sampling (ASOPS) enables to scan a time-delay of 1 ns with 100 fs time resolution with a frequency in the kHz range without a moving part in the set-up. We investigate the dynamics of coherent zone-folded acoustic phonons in semiconductor superlattices (GaAs/AlAs and GaSb/InAs) and of coherent vibration of metallic nanostructures of non-spherical shape using ASOPS.

  19. Optical absorption of suspended graphene based metal plasmonic grating in the visible range

    NASA Astrophysics Data System (ADS)

    Han, Y. X.; Chen, B. B.; Yang, J. B.; He, X.; Huang, J.; Zhang, J. J.; Zhang, Z. J.

    2018-05-01

    We employ finite-difference time-domain ( FDTD) method and Raman spectroscopy to study the properties of graphene, which is suspended on a gold/SiO2/Si grating structure with different trench depth of SiO2 layer. The absorption enhancement of suspended graphene and plasmonic resonance of metal grating are investigated in the visible range using 2D FDTD method. Moreover, it is found that the intensity of the Raman features depends very sensitively on the trench depth of SiO2 layer. Raman enhancement in our experiments is attributed to the enhanced optical absorption of graphene by near-field coupling based metal plasmonic grating. The enhanced absorption of suspended graphene modulated by localized surface plasmon resonance (LSPR) offers a potential application for opto-electromechanical devices.

  20. Cross section of resonant Raman scattering of light by polyenes

    NASA Astrophysics Data System (ADS)

    Verdyugin, V. V.; Burshteyn, K. Ya.; Shorygin, P. P.

    1987-03-01

    An experimental study is presented of the resonant Raman spectra of beta carotene. Absolute differential cross sections are obtained for the most intensive Raman spectral lines with excitation at the absorption maximum. A theoretical analysis is presented of the variation in absolute differential cross section as a function of a number of conjunct double bonds in the polyenes.

  1. The contribution of Raman spectroscopy to the analysis of phase transformations in pharmaceutical compounds.

    PubMed

    Hédoux, Alain; Guinet, Yannick; Descamps, Marc

    2011-09-30

    We show in this paper the contribution of the whole Raman spectrum including the phonon spectrum, to detect, identify and characterize polymorphic forms of molecular compounds, and study their stability and transformation. Obtaining these kinds of information is important in the area of pharmaceutical compounds. Two different polymorphic systems are analyzed through investigations in indomethacin and caffeine exposed to variable environmental conditions and various stresses, as possibly throughout the production cycle of the active pharmaceutical ingredient. It is shown the capability of the low-frequency Raman spectroscopy to reveal disorder in the crystalline state, to detect small amorphous or crystalline material, and to elucidate ambiguous polymorphic or polyamorphic situations. Copyright © 2011 Elsevier B.V. All rights reserved.

  2. Strain, doping, and disorder effects in GaAs/Ge/Si heterostructures: A Raman spectroscopy investigation

    NASA Astrophysics Data System (ADS)

    Mlayah, A.; Carles, R.; Leycuras, A.

    1992-01-01

    The present work is devoted to a Raman study of GaAs/Ge/Si heterostructures grown by the vapor-phase epitaxy technique. We first show that the GaAs epilayers are submitted to a biaxial tensile strain. The strain relaxation generates misfit dislocations and thus disorder effects which we analyze in terms of translational invariance loss and Raman selection rules violation. The first-order Raman spectra of annealed samples exhibit an unexpected broadband we identify as due to scattering by a coupled LO phonon-damped plasmon mode. This is corroborated by an accurate line-shape analysis which accounts for the recorded spectra and makes evident the presence of free carriers within the GaAs layers. Their density is estimated from the deduced plasmon frequency and also using a method we have presented in a previous work.

  3. Raman scattering in the atmospheres of the major planets

    NASA Technical Reports Server (NTRS)

    Cochran, W. D.; Trafton, L. M.

    1978-01-01

    A technique is developed to calculate the detailed effects of Raman scattering in an inhomogeneous anisotropically scattering atmosphere. The technique is applied to evaluations of Raman scattering by H2 in the atmosphere of the major planets. It is noted that Raman scattering produces an insufficient decrease in the blue and ultraviolet regions to explain the albedos of all planets investigated. For all major planets, the filling-in of solar line cores and the generation of the Raman-shifted ghosts of the Fraunhofer spectrum are observed. With regard to Uranus and Neptune, Raman scattering is seen to exert a major influence on the formation and profile of strong red and near infrared CH4 bands, and Raman scattering by H2 explains the residual intensity in the cores of these bands. Raman scattering by H2 must also be taken into account in the scattering of photons into the cores of saturated absorption bands.

  4. On the interplay between phonon-boundary scattering and phonon-point-defect scattering in SiGe thin films

    NASA Astrophysics Data System (ADS)

    Iskandar, A.; Abou-Khalil, A.; Kazan, M.; Kassem, W.; Volz, S.

    2015-03-01

    This paper provides theoretical understanding of the interplay between the scattering of phonons by the boundaries and point-defects in SiGe thin films. It also provides a tool for the design of SiGe-based high-efficiency thermoelectric devices. The contributions of the alloy composition, grain size, and film thickness to the phonon scattering rate are described by a model for the thermal conductivity based on the single-mode relaxation time approximation. The exact Boltzmann equation including spatial dependence of phonon distribution function is solved to yield an expression for the rate at which phonons scatter by the thin film boundaries in the presence of the other phonon scattering mechanisms. The rates at which phonons scatter via normal and resistive three-phonon processes are calculated by using perturbation theories with taking into account dispersion of confined acoustic phonons in a two dimensional structure. The vibrational parameters of the model are deduced from the dispersion of confined acoustic phonons as functions of temperature and crystallographic direction. The accuracy of the model is demonstrated with reference to recent experimental investigations regarding the thermal conductivity of single-crystal and polycrystalline SiGe films. The paper describes the strength of each of the phonon scattering mechanisms in the full temperature range. Furthermore, it predicts the alloy composition and film thickness that lead to minimum thermal conductivity in a single-crystal SiGe film, and the alloy composition and grain size that lead to minimum thermal conductivity in a polycrystalline SiGe film.

  5. Two-Dimensional Heterostructure as a Platform for Surface-Enhanced Raman Scattering.

    PubMed

    Tan, Yang; Ma, Linan; Gao, Zhibin; Chen, Ming; Chen, Feng

    2017-04-12

    Raman enhancement on a flat nonmetallic surface has attracted increasing attention, ever since the discovery of graphene enhanced Raman scattering. Recently, diverse two-dimensional layered materials have been applied as a flat surface for the Raman enhancement, attributed to different mechanisms. Looking beyond these isolated materials, atomic layers can be reassembled to design a heterostructure stacked layer by layer with an arbitrary chosen sequence, which allows the flow of charge carriers between neighboring layers and offers novel functionalities. Here, we demonstrate the heterostructure as a novel Raman enhancement platform. The WSe 2 (W) monolayer and graphene (G) were stacked together to form a heterostructure with an area of 10 mm × 10 mm. Heterostructures with different stacked structuress are used as platforms for the enhanced Raman scattering, including G/W, W/G, G/W/G/W, and W/G/G/W. On the surface of the heterostructure, the intensity of the Raman scattering is much stronger compared with isolated layers, using the copper phthalocyanine (CuPc) molecule as a probe. It is found that the Raman enhancement effect on heterostructures depends on stacked methods. Phonon modes of CuPc have the strongest enhancement on G/W. W/G and W/G/G/W have a stronger enhancement than that on the isolated WSe 2 monolayer, while lower than the graphene monolayer. The G/W/G/W/substrate demonstrated a comparable Raman enhancement effect than the G/W/substrate. These differences are due to the different interlayer couplings in heterostructures related to electron transition probability rates, which are further proved by first-principle calculations and probe-pump measurements.

  6. Phononic crystal diffraction gratings

    NASA Astrophysics Data System (ADS)

    Moiseyenko, Rayisa P.; Herbison, Sarah; Declercq, Nico F.; Laude, Vincent

    2012-02-01

    When a phononic crystal is interrogated by an external source of acoustic waves, there is necessarily a phenomenon of diffraction occurring on the external enclosing surfaces. Indeed, these external surfaces are periodic and the resulting acoustic diffraction grating has a periodicity that depends on the orientation of the phononic crystal. This work presents a combined experimental and theoretical study on the diffraction of bulk ultrasonic waves on the external surfaces of a 2D phononic crystal that consists of a triangular lattice of steel rods in a water matrix. The results of transmission experiments are compared with theoretical band structures obtained with the finite-element method. Angular spectrograms (showing frequency as a function of angle) determined from diffraction experiments are then compared with finite-element simulations of diffraction occurring on the surfaces of the crystal. The experimental results show that the diffraction that occurs on its external surfaces is highly frequency-dependent and has a definite relation with the Bloch modes of the phononic crystal. In particular, a strong influence of the presence of bandgaps and deaf bands on the diffraction efficiency is found. This observation opens perspectives for the design of efficient phononic crystal diffraction gratings.

  7. Superradiance-Driven Phonon Laser

    NASA Astrophysics Data System (ADS)

    Jiang, Ya-Jing; Lü, Hao; Jing, Hui

    2018-04-01

    We propose to enhance the generation of a phonon laser by exploiting optical superradiance. In our scheme, the optomechanical cavity contains a movable membrane, which supports a mechanical mode, and the superradiance cavity can generate the coherent collective light emissions by applying a transverse pump to an ultracold intracavity atomic gas. The superradiant emission turns out to be capable of enhancing the phonon laser performance. This indicates a new way to operate a phonon laser with the assistance of coherent atomic gases trapped in a cavity or lattice potentials.

  8. Resonant Raman and FTIR spectra of carbon doped GaN

    NASA Astrophysics Data System (ADS)

    Ito, S.; Kobayashi, H.; Araki, K.; Suzuki, K.; Sawaki, N.; Yamashita, K.; Honda, Y.; Amano, H.

    2015-03-01

    Intentionally carbon (C) doped (0 0 0 1)GaN was grown using C2H2 on a sapphire substrate by metalorganic vapor phase epitaxy. Optical spectra of the heavily doped samples were investigated at room temperature. In Raman spectra excited by the 325 nm line of a He-Cd laser, multiple LO phonon scattering signals up to 7th order were observed, and the A1(LO) phonon energy was determined to be 737.5 cm-1 (91.45 meV). In infrared reflectance spectra, on the other hand, a local vibration mode was found at 777.5 cm-1, which is attributed to a Ga-C bond in the GaN matrix suggesting that the C sits on an N site (CN). In spite of the strong suggestion of CN, the samples did not show p-type conduction. Possible origin of the carrier compensation is discussed in relation to the enhancement of defect related yellow luminescence in the photoluminescence spectra.

  9. Spotting the differences in two-dimensional materials - the Raman scattering perspective.

    PubMed

    Zhang, Shishu; Zhang, Na; Zhao, Yan; Cheng, Ting; Li, Xiaobo; Feng, Rui; Xu, Hua; Liu, Zhirong; Zhang, Jin; Tong, Lianming

    2018-05-08

    Two-dimensional (2D) layered materials have attracted tremendous attention and led to a prosperous development in both fundamental investigation and device applications in various fields, such as nanoelectronics, flexible devices, sustainable energy and catalysts. The precise characterization of the structure and properties of 2D materials is in urgent need. Raman scattering spectroscopy is one of the most popular characterization tools that is convenient, rapid and non-invasive. It provides information on both the lattice structure from the frequency of phonon modes and the electronic band structure through the intensity due to electronic resonance Raman scattering. Although a few morphological characterization tools can image 2D materials with atomic resolution, Raman scattering measurements are more tolerant to the conditions of sample preparation such as the substrate and less technically demanding, and have been one of the routine tools for the characterization of 2D materials. In this review, we focus on the characterization of 2D materials using Raman scattering spectroscopy, in particular, the revealing of differences from primitive 2D materials, such as defects, doping effects, van der Waals heterostructures and the interaction with molecules. The characteristic Raman features of such differences and the corresponding interpretation will be discussed. We hope that this review will be useful for wide research communities of materials, physics, chemistry and engineering.

  10. Electron-Phonon Systems on a Universal Quantum Computer

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Macridin, Alexandru; Spentzouris, Panagiotis; Amundson, James

    We present an algorithm that extends existing quantum algorithms forsimulating fermion systems in quantum chemistry and condensed matter physics toinclude phonons. The phonon degrees of freedom are represented with exponentialaccuracy on a truncated Hilbert space with a size that increases linearly withthe cutoff of the maximum phonon number. The additional number of qubitsrequired by the presence of phonons scales linearly with the size of thesystem. The additional circuit depth is constant for systems with finite-rangeelectron-phonon and phonon-phonon interactions and linear for long-rangeelectron-phonon interactions. Our algorithm for a Holstein polaron problem wasimplemented on an Atos Quantum Learning Machine (QLM) quantum simulatoremployingmore » the Quantum Phase Estimation method. The energy and the phonon numberdistribution of the polaron state agree with exact diagonalization results forweak, intermediate and strong electron-phonon coupling regimes.« less

  11. Engineering dissipation with phononic spectral hole burning

    NASA Astrophysics Data System (ADS)

    Behunin, R. O.; Kharel, P.; Renninger, W. H.; Rakich, P. T.

    2017-03-01

    Optomechanics, nano-electromechanics, and integrated photonics have brought about a renaissance in phononic device physics and technology. Central to this advance are devices and materials supporting ultra-long-lived photonic and phononic excitations that enable novel regimes of classical and quantum dynamics based on tailorable photon-phonon coupling. Silica-based devices have been at the forefront of such innovations for their ability to support optical excitations persisting for nearly 1 billion cycles, and for their low optical nonlinearity. While acoustic phonon modes can persist for a similar number of cycles in crystalline solids at cryogenic temperatures, it has not been possible to achieve such performance in silica, as silica becomes acoustically opaque at low temperatures. We demonstrate that these intrinsic forms of phonon dissipation are greatly reduced (by >90%) by nonlinear saturation using continuous drive fields of disparate frequencies. The result is a form of steady-state phononic spectral hole burning that produces a wideband transparency window with optically generated phonon fields of modest (nW) powers. We developed a simple model that explains both dissipative and dispersive changes produced by phononic saturation. Our studies, conducted in a microscale device, represent an important step towards engineerable phonon dynamics on demand and the use of glasses as low-loss phononic media.

  12. Quantum Interference Effects in Resonant Raman Spectroscopy of Single- and Triple-Layer MoTe2 from First-Principles

    NASA Astrophysics Data System (ADS)

    Miranda, Henrique P. C.; Reichardt, Sven; Froehlicher, Guillaume; Molina-Sánchez, Alejandro; Berciaud, Stéphane; Wirtz, Ludger

    2017-04-01

    We present a combined experimental and theoretical study of resonant Raman spectroscopy in single- and triple-layer MoTe$_2$. Raman intensities are computed entirely from first principles by calculating finite differences of the dielectric susceptibility. In our analysis, we investigate the role of quantum interference effects and the electron-phonon coupling. With this method, we explain the experimentally observed intensity inversion of the $A^\\prime_1$ vibrational modes in triple-layer MoTe2 with increasing laser photon energy. Finally, we show that a quantitative comparison with experimental data requires the proper inclusion of excitonic effects.

  13. Quantitative detection of astaxanthin and cantaxanthin in Atlantic salmon by resonance Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Ermakov, Igor V.; Ermakova, Maia R.; Gellermann, Werner

    2006-02-01

    Two major carotenoids species found in salmonids muscle tissues are astaxanthin and cantaxanthin. They are taken up from fish food and are responsible for the attractive red-orange color of salmon filet. Since carotenoids are powerful antioxidants and biomarkers of nutrient consumption, they are thought to indicate fish health and resistance to diseases in fish farm environments. Therefore, a rapid, accurate, quantitative optical technique for measuring carotenoid content in salmon tissues is of economic interest. We demonstrate the possibility of using fast, selective, quantitative detection of astaxanthin and cantaxanthin in salmon muscle tissues, employing resonance Raman spectroscopy. Analyzing strong Raman signals originating from the carbon-carbon double bond stretch vibrations of the carotenoid molecules under blue laser excitation, we are able to characterize quantitatively the concentrations of carotenoids in salmon muscle tissue. To validate the technique, we compared Raman data with absorption measurements of carotenoid extracts in acetone. A close correspondence was observed in absorption spectra for tissue extract in acetone and a pure astaxanthin solution. Raman results show a linear dependence between Raman and absorption data. The proposed technique holds promise as a method of rapid screening of carotenoid levels in fish muscle tissues and may be attractive for the fish farm industry to assess the dietary status of salmon, risk for infective diseases, and product quality control.

  14. Theoretical investigation of the hyper-Raman scattering in hexagonal semiconductors under two-photon excitation near resonance with the An=2 exciton level

    NASA Astrophysics Data System (ADS)

    Semenova, L. E.

    2018-04-01

    The hyper-Raman scattering of light by LO-phonons under two-photon excitation near resonance with the An=2 exciton level in the wurtzite semiconductors A2B6 was theoretically investigated, taking into account the influence of the complex structure of the top valence band.

  15. Ultrafast Physics Behind the Nonradiative Relaxation Process of Chromium Ions in Forsterite Crystals.

    NASA Astrophysics Data System (ADS)

    Demos, Stavros Gregorios

    The nonradiative relaxation following photoexcitation has been studied in Cr^{4+} -doped forsterite (Mg_2SiO _4) using picosecond laser excitation and ultrasensitive photon counting detection. The experimental techniques utilized were time resolved antiStokes Raman scattering and up-converted hot and ordinary luminescence. The up-converted hot luminescence technique allowed the investigation of the upper state nonradiative relaxation of the excited state manifold of Cr^{4+ }-doped forsterite. The excitation involves the absorption of two photons per photoexcited ion in a two-step absorption. Discrete peaks are observed in the hot up-converted luminescence spectrum and are attributed to the population of nonequilibrium vibronic levels during the deexcitation of the ions by phonon emission. This work reveals that the phonon modes participating in the initial steps of the nonradiative relaxation of the photoexcited ions have energies 218 +/- 20, 325 +/- 20, 365 +/- 20 and 513 +/- 12 cm^ {-1}. The shape of the luminescence spectral envelope suggests two electronic bottlenecks at ~2.1 and ~2.45 eV associated with slower rates of vibrational relaxation at different parts of the excited state manifold. Time resolved measurements indicated that the average time for phonon emission is of the order of hundreds of fs. Information on the nonequilibrium phonon dynamics of the 225, 335 and 370 cm^{-1} modes of forsterite has been obtained using time resolved Raman scattering. Laser pulses of 450 fs in duration and 590 nm in wavelength were used to excite the Cr ions 2.1 eV above the ground state. The probe pulses (obtained from the same laser) are monitoring the nonequilibrium phonon population through the intensity of the antiStokes Raman lines at various pump-probe delay times. Experiments were performed at room and liquid nitrogen temperatures. The observed nonequilibrium phonon populations are associated with the overall complex nonradiative decay following the excitation of

  16. Splash, pop, sizzle: Information processing with phononic computing

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Sklan, Sophia R.

    2015-05-15

    Phonons, the quanta of mechanical vibration, are important to the transport of heat and sound in solid materials. Recent advances in the fundamental control of phonons (phononics) have brought into prominence the potential role of phonons in information processing. In this review, the many directions of realizing phononic computing and information processing are examined. Given the relative similarity of vibrational transport at different length scales, the related fields of acoustic, phononic, and thermal information processing are all included, as are quantum and classical computer implementations. Connections are made between the fundamental questions in phonon transport and phononic control and themore » device level approach to diodes, transistors, memory, and logic. .« less

  17. Experimental Study of Electron and Phonon Dynamics in Nanoscale Materials by Ultrafast Laser Time-Domain Spectroscopy

    NASA Astrophysics Data System (ADS)

    Shen, Xiaohan

    With the rapid advances in the development of nanotechnology, nowadays, the sizes of elementary unit, i.e. transistor, of micro- and nanoelectronic devices are well deep into nanoscale. For the pursuit of cheaper and faster nanoscale electronic devices, the size of transistors keeps scaling down. As the miniaturization of the nanoelectronic devices, the electrical resistivity increases dramatically, resulting rapid growth in the heat generation. The heat generation and limited thermal dissipation in nanoscale materials have become a critical problem in the development of the next generation nanoelectronic devices. Copper (Cu) is widely used conducting material in nanoelectronic devices, and the electron-phonon scattering is the dominant contributor to the resistivity in Cu nanowires at room temperature. Meanwhile, phonons are the main carriers of heat in insulators, intrinsic and lightly doped semiconductors. The thermal transport is an ensemble of phonon transport, which strongly depends on the phonon frequency. In addition, the phonon transport in nanoscale materials can behave fundamentally different than in bulk materials, because of the spatial confinement. However, the size effect on electron-phonon scattering and frequency dependent phonon transport in nanoscale materials remain largely unexplored, due to the lack of suitable experimental techniques. This thesis is mainly focusing on the study of carrier dynamics and acoustic phonon transport in nanoscale materials. The weak photothermal interaction in Cu makes thermoreflectance measurement difficult, we rather measured the reflectivity change of Cu induced by absorption variation. We have developed a method to separately measure the processes of electron-electron scattering and electron-phonon scattering in epitaxial Cu films by monitoring the transient reflectivity signal using the resonant probe with particular wavelengths. The enhancement on electron-phonon scattering in epitaxial Cu films with thickness

  18. In-pile Thermal Conductivity Characterization with Time Resolved Raman

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Wang, Xinwei; Hurley, David H.

    The project is designed to achieve three objectives: (1) Develop a novel time resolved Raman technology for direct measurement of fuel and cladding thermal conductivity. (2) Validate and improve the technology development by measuring ceramic materials germane to the nuclear industry. (3) Conduct instrumentation development to integrate optical fiber into our sensing system for eventual in-pile measurement. We have developed three new techniques: time-domain differential Raman (TD-Raman), frequency-resolved Raman (FR-Raman), and energy transport state-resolved Raman (ET-Raman). The TD-Raman varies the laser heating time and does simultaneous Raman thermal probing, the FR-Raman probes the material’s thermal response under periodical laser heatingmore » of different frequencies, and the ET-Raman probes the thermal response under steady and pulsed laser heating. The measurement capacity of these techniques have been fully assessed and verified by measuring micro/nanoscale materials. All these techniques do not need the data of laser absorption and absolute material temperature rise, yet still be able to measure the thermal conductivity and thermal diffusivity with unprecedented accuracy. It is expected they will have broad applications for in-pile thermal characterization of nuclear materials based on pure optical heating and sensing.« less

  19. Phonon spectra and the one-phonon and two-phonon densities of states of UO2 and PuO2

    NASA Astrophysics Data System (ADS)

    Poplavnoi, A. S.; Fedorova, T. P.; Fedorov, I. A.

    2017-04-01

    The vibrational spectra of uranium dioxide UO2 and plutonium dioxide PuO2, as well as the one-phonon densities of states and thermal occupation number weighted two-phonon densities of states, have been calculated within the framework of the phenomenological rigid ion model. It has been shown that the acoustic and optical branches of the spectra are predominantly determined by vibrations of the metal and oxygen atoms, respectively, because the atomic masses of the metal and oxygen differ from each other by an order of magnitude. On this basis, the vibrational spectra can be represented in two Brillouin zones, i.e., in the Brillouin zone of the crystal and the Brillouin zone of the oxygen sublattice. In this case, the number of optical branches decreases by a factor of two. The two-phonon densities of states consist of two broad structured peaks. The temperature dependences of the upper peak exhibit a thermal broadening of the phonon lines L01 and L02 in the upper part of the optical branches. The lower peak is responsible for the thermal broadening of the lowest two optical (T02, T01) and acoustic (LA, TA) branches.

  20. Diffraction of electrons at intermediate energies: The role of phonons

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Ascolani, H.; Zampieri, G.

    1996-07-01

    The intensity of electrons reflected {open_quote}{open_quote}elastically{close_quote}{close_quote} from crystalline surfaces presents two regimes: the low-energy or LEED regime ({lt}500 eV), in which the electrons are reflected along the Bragg directions, and the intermediate-energy or XPD/AED regime ({gt}500 eV), in which the maxima of intensity are along the main crystallographic axes. We present a model which explains this transition in terms of the excitation/absorption of phonons during the scattering. {copyright} {ital 1996 American Institute of Physics.}

  1. Vibrational properties, phonon spectrum and related thermal parameters of β-octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine: a theoretical study.

    PubMed

    Qian, Wen; Zhang, Weibin; Zong, Hehou; Gao, Guofang; Zhou, Yang; Zhang, Chaoyang

    2016-01-01

    The vibrational spectrum, phonon dispersion curve, and phonon density of states (DOS) of β-octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (β-HMX) crystal were obtained by molecular simulation and calculations. As results, it was found that the peaks at low frequency (0-2.5 THz) are comparable with the experimental Terahertz absorption and the molecular vibrational modes are in agreement with previous reports. Thermodynamic properties including Gibbs free energy, enthalpy, and heat capacity as functions of temperature were obtained based on the calculated phonon spectrum. The heat capacity at normal temperature was calculated using linear fitting method, with a result consistent with experiments. Graphical Abstract Phonon spectrum and heat capacity of β-octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine from DFT calculation.

  2. Phonon properties of iron-based superconductors

    NASA Astrophysics Data System (ADS)

    Gupta, Yuhit; Goyal, Megha; Sinha, M. M.

    2018-05-01

    Earlier, it was thought there is antagonist relationship between superconductivity and ferromagnetic materials, But, a discovery of iron-based superconductors have removed this misconception. It gives an idea to make a review on the superconductivity properties of different materials. The new iron-based superconductors' present symmetry breaking competing phases in the form of tetragonal to orthorhombic transition. It consists of mainly four families [1111], [111], [122], and [11] type. Superconductivity of iron-based superconductors mainly related with the phonons and there is an excellent relation between phonons and superconductivity. Phonons properties are helpful in predicting the superconducting properties of materials. Phonon properties of iron-based superconductors in various phases are summarized in this study. We are presenting the review of phonon properties of iron-based superconductors.

  3. Electron-phonon coupling from finite differences

    NASA Astrophysics Data System (ADS)

    Monserrat, Bartomeu

    2018-02-01

    The interaction between electrons and phonons underlies multiple phenomena in physics, chemistry, and materials science. Examples include superconductivity, electronic transport, and the temperature dependence of optical spectra. A first-principles description of electron-phonon coupling enables the study of the above phenomena with accuracy and material specificity, which can be used to understand experiments and to predict novel effects and functionality. In this topical review, we describe the first-principles calculation of electron-phonon coupling from finite differences. The finite differences approach provides several advantages compared to alternative methods, in particular (i) any underlying electronic structure method can be used, and (ii) terms beyond the lowest order in the electron-phonon interaction can be readily incorporated. But these advantages are associated with a large computational cost that has until recently prevented the widespread adoption of this method. We describe some recent advances, including nondiagonal supercells and thermal lines, that resolve these difficulties, and make the calculation of electron-phonon coupling from finite differences a powerful tool. We review multiple applications of the calculation of electron-phonon coupling from finite differences, including the temperature dependence of optical spectra, superconductivity, charge transport, and the role of defects in semiconductors. These examples illustrate the advantages of finite differences, with cases where semilocal density functional theory is not appropriate for the calculation of electron-phonon coupling and many-body methods such as the GW approximation are required, as well as examples in which higher-order terms in the electron-phonon interaction are essential for an accurate description of the relevant phenomena. We expect that the finite difference approach will play a central role in future studies of the electron-phonon interaction.

  4. Hydrostatic pressure and temperature effect on the Raman spectra of the molecular crystal 2-amine-1,3,4-thiadiazole

    NASA Astrophysics Data System (ADS)

    de Toledo, T. A.; da Costa, R. C.; Bento, R. R. F.; Pizani, P. S.

    2018-03-01

    The structural, thermal and vibrational properties of the molecular crystal 2-amine-1,3,4-thiadiazole (ATD) were investigated combining X-ray diffraction, infrared spectroscopy, Raman scattering (in solid and in solution) and thermal analysis as experimental techniques and first principle calculations based on density functional theory using PZ, BLYP in condensed-phase and B3LYP/cc-pVTZ in isolated molecule methods. The structural stability and phonon anharmonicity were also studied using Raman spectroscopy at different temperatures and hydrostatic pressures. A reasonable agreement was obtained between calculated and experimental results. The main difference between experimental and computed structural and vibrational spectra occurred in the intermolecular bond distance Nsbnd H⋯N and stretching modes of NH2. The vibrational spectra were interpreted and assigned based on group theory and functional group analysis assisted by theoretical results, which led to a more comprehensive knowledge about external and internal modes at different thermodynamic conditions. As temperature increases, it was observed the line-width increases and red-shifts, indicating a phonon anharmonicity without a temperature-induced phase transition in the range 10-413 K. However, ATD crystal undergoes a phase transition in the temperature range 413-475 K, as indicated by thermal analysis curve and Raman spectra. Furthermore, increasing pressure from ambient to 3.1 GPa, it was observed the splitting of the external Raman bands centered at 122 cm-1 (at 0.2 GPa), 112 cm-1 (1.1 GPa), 93 cm-1 (2.4 GPa) in two components as well as the appearance of new band near 50 cm-1 at 1.1 GPa, indicating a possible phase-transition. The blue-shift of the Raman bands was associated to anharmonicity of the interatomic potential caused by unit cell contraction.

  5. Lattice anharmonicity, phonon dispersion, and thermal conductivity of PbTe studied by the phonon quasiparticle approach

    NASA Astrophysics Data System (ADS)

    Lu, Yong; Sun, Tao; Zhang, Dong-Bo

    2018-05-01

    We investigated the vibrational property of lead telluride (PbTe) with a focus on lattice anharmonicity at moderate temperatures (300 phonon quasiparticle approach which combines first-principles molecular dynamics and lattice dynamics. The calculated anharmonic phonon dispersions are strongly temperature dependent and some phonon modes adopt giant frequency shifts, e.g., transverse optical modes in the long-wavlength regime. As a result, we witness the avoided crossing between transverse optical modes and longitudinal acoustic modes at elevated temperature, in good agreement with experimentation and available theoretical studies. These results, together with the large root-mean-square displacements of atoms, reveal a strong anharmonic effect in PbTe. The obtained phonon lifetimes allow studies of transport properties. For considered temperatures, the phonon mean free paths can be shorter than lattice constants at relatively high temperature, especially for optical modes. This finding goes against the widely employed minimal phonon mean free path concept. As such, the calculated lattice thermal conductivity of PbTe, which is indeed relatively small, does not have the prescribed minima at high temperature, showcasing the breakdown of the minimal mean free path theory. Our study provides a basis for delineating vibrational and transport properties of PbTe and other thermoelectric materials within the framework of the phonon gas model.

  6. Directly Characterizing the Relative Strength and Momentum Dependence of Electron-Phonon Coupling Using Resonant Inelastic X-Ray Scattering

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Devereaux, T. P.; Shvaika, A. M.; Wu, K.

    The coupling between lattice and charge degrees of freedom in condensed matter materials is ubiquitous and can often result in interesting properties and ordered phases, including conventional superconductivity, charge-density wave order, and metal-insulator transitions. Angle-resolved photoemission spectroscopy and both neutron and nonresonant x-ray scattering serve as effective probes for determining the behavior of appropriate, individual degrees of freedom—the electronic structure and lattice excitation, or phonon dispersion, respectively. However, each provides less direct information about the mutual coupling between the degrees of freedom, usually through self-energy effects, which tend to renormalize and broaden spectral features precisely where the coupling is strong,more » impacting one’s ability to quantitatively characterize the coupling. Here, we demonstrate that resonant inelastic x-ray scattering, or RIXS, can be an effective tool to directly determine the relative strength and momentum dependence of the electron-phonon coupling in condensed matter systems. Using a diagrammatic approach for an eight-band model of copper oxides, we study the contributions from the lowest-order diagrams to the full RIXS intensity for a realistic scattering geometry, accounting for matrix element effects in the scattering cross section, as well as the momentum dependence of the electron-phonon coupling vertex. A detailed examination of these maps offers a unique perspective into the characteristics of electron-phonon coupling, which complements both neutron and nonresonant x-ray scattering, as well as Raman and infrared conductivity.« less

  7. Directly Characterizing the Relative Strength and Momentum Dependence of Electron-Phonon Coupling Using Resonant Inelastic X-Ray Scattering

    DOE PAGES

    Devereaux, T. P.; Shvaika, A. M.; Wu, K.; ...

    2016-10-25

    The coupling between lattice and charge degrees of freedom in condensed matter materials is ubiquitous and can often result in interesting properties and ordered phases, including conventional superconductivity, charge-density wave order, and metal-insulator transitions. Angle-resolved photoemission spectroscopy and both neutron and nonresonant x-ray scattering serve as effective probes for determining the behavior of appropriate, individual degrees of freedom—the electronic structure and lattice excitation, or phonon dispersion, respectively. However, each provides less direct information about the mutual coupling between the degrees of freedom, usually through self-energy effects, which tend to renormalize and broaden spectral features precisely where the coupling is strong,more » impacting one’s ability to quantitatively characterize the coupling. Here, we demonstrate that resonant inelastic x-ray scattering, or RIXS, can be an effective tool to directly determine the relative strength and momentum dependence of the electron-phonon coupling in condensed matter systems. Using a diagrammatic approach for an eight-band model of copper oxides, we study the contributions from the lowest-order diagrams to the full RIXS intensity for a realistic scattering geometry, accounting for matrix element effects in the scattering cross section, as well as the momentum dependence of the electron-phonon coupling vertex. A detailed examination of these maps offers a unique perspective into the characteristics of electron-phonon coupling, which complements both neutron and nonresonant x-ray scattering, as well as Raman and infrared conductivity.« less

  8. Intrinsic phonon bands in high quality monolayer T' molybdenum ditelluride

    NASA Astrophysics Data System (ADS)

    Chen, Shao-Yu; Naylor, Carl; Goldstein, Thomas; Johnson, Charlie; Yan, Jun

    Distorted octahedral (T') transition metal dichalcogenide (TMDC) is a type of layered semimetal that has attracted significant recent attention because of its fascination physical, chemical and nontrivial topological properties. Unlike its hexagonal counterpart, monolayer (1L) T'-TMDC is challenging to work with due to rapid sample degradation in air. In this talk, I will discuss well-protected 1L-T' - MoTe2 that exhibits sharp and robust intrinsic Raman bands, with intensities about one order of magnitude stronger than those from bulk T'-MoTe2. The high quality samples enable us to reveal for the first time the set of all nine even-parity zone-center optical phonons. Crystal angle and light polarization resolved measurements further indicate that all the intrinsic Raman modes belong to either z-mode (vibrating along the zigzag Mo atomic chain) or m-modes (vibrating in the mirror plane). Moreover, with the knowledge of vibrational symmetry, we can effectively distinguish the intrinsic modes from Te-metalloid-like modes with energy around 122 and 141 cm-1 which are associated to the sample degradation. Our studies offer a powerful non-destructive method for assessing sample quality, providing the fingerprint as well as key insights in understanding the fundamental properties of 1L T'-TMDCs.

  9. Electron-phonon Interactions in HTSC Cuprates

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Egami, T.; Chung, J.-H.; McQueeny, R. J.

    Phonons have been generally considered to be irrelevant to the high-temperature superconductivity in the cuprates. However, such a bias is usually based upon the assumption of conventional electron-phonon coupling, while in the cuprates the coupling can be rather unconventional because of strong electron correlation. We present the results of our recent measurements of phonon dispersion in YBa{sub 2}Cu{sub 3}O{sub 6+x} by inelastic neutron scattering. These suggest certain phonon modes interact strongly with electrons and are closely involved in the superconductivity phenomenon with possible contribution to pairing.

  10. Lattice dynamical investigation of the Raman and infrared wave numbers and heat capacity properties of the pyrochlores R2Zr2O7 (R = La, Nd, Sm, Eu)

    NASA Astrophysics Data System (ADS)

    Nandi, S.; Jana, Y. M.; Gupta, H. C.

    2018-04-01

    A short-range electrostatic forcefield model has been applied for the first time to investigate the Raman and infrared wave numbers in pyrochlore zirconates R2Zr2O7 (R3+ = La, Nd, Sm, Eu). The calculations of phonons involve five stretching and four bending force constants in the Wilson GF matrix method. The calculated phonon wave numbers are in reasonable agreement with the observed spectra in infrared and Raman excitation zones for all of these isomorphous compounds. The contributions of force constants to each mode show a similar trend of variation for all of these compounds. Furthermore, to validate the established forcefield model, we calculated the standard thermodynamic functions, e.g., molar heat capacity, entropy and enthalpy, and compared the results with the previous experimental data for each compound. Using the derived wave numbers for the acoustic and optical modes, the total phonon contribution to the heat capacity was calculated for all these zirconate compounds. The Schottky heat capacity contributions were also calculated for the magnetic compounds, Nd2Zr2O7, Sm2Zr2O7 and Eu2Zr2O7, taking account of crystal-field level schemes of the lanthanide ions. The derived total heat capacity and the integrated values of molar entropy and molar enthalpy showed satisfactory correlations at low temperatures with the experimental results available in the literature for these compounds. At higher temperatures, the discrepancies may be caused by the anharmonic effects of vibrations, phonon dispersion, distribution of phonon density of states, etc.

  11. Topological chiral phonons in center-stacked bilayer triangle lattices

    NASA Astrophysics Data System (ADS)

    Xu, Xifang; Zhang, Wei; Wang, Jiaojiao; Zhang, Lifa

    2018-06-01

    Since chiral phonons were found in an asymmetric two-dimensional hexagonal lattice, there has been growing interest in the study of phonon chirality, which were experimentally verified very recently in monolayer tungsten diselenide (2018 Science 359 579). In this work, we find chiral phonons with nontrivial topology in center-stacked bilayer triangle lattices. At the Brillouin-zone corners, (), circularly polarized phonons and nonzero phonon Berry curvature are observed. Moreover, we find that the phonon chirality remain robust with changing sublattice mass ratio and interlayer coupling. The chiral phonons at the valleys are demonstrated in doubler-layer sodium chloride along the [1 1 1] direction. We believe that the findings on topological chiral phonons in triangle lattices will give guidance in the study of chiral phonons in real materials and promote the phononic applications.

  12. Phononic Origins of Friction in Carbon Nanotube Oscillators.

    PubMed

    Prasad, Matukumilli V D; Bhattacharya, Baidurya

    2017-04-12

    Phononic coupling can have a significant role in friction between nanoscale surfaces. We find frictional dissipation per atom in carbon nanotube (CNT) oscillators to depend significantly on interface features such as contact area, commensurability, and by end-capping of the inner core. We perform large-scale phonon wavepacket MD simulations to study phonon coupling between a 250 nm long (10,10) outer tube and inner cores of four different geometries. Five different phonon polarizations known to have dominant roles in thermal transport are selected, and transmission coefficient plots for a range of phonon energies along with phonon scattering dynamics at specific energies are obtained. We find that the length of interface affects friction only through LA phonon scattering and has a significant nonlinear effect on total frictional force. Incommensurate contact does not always give rise to superlubricity: the net effect of two competing interaction mechanisms shown by longitudinal and transverse phonons decides the role of commensurability. Capping of the core has no effect on acoustic phonons but destroys the coherence of transverse optical phonons and creates diffusive scattering. In contrast, the twisting and radial breathing phonon modes have perfect transmission at all energies and can be deemed as the enablers of ultralow friction in CNT oscillators. Our work suggests that tuning of interface geometries can give rise to desirable friction properties in nanoscale devices.

  13. Unified Description of the Optical Phonon Modes inN-Layer MoTe2

    NASA Astrophysics Data System (ADS)

    Froehlicher, Guillaume; Lorchat, Etienne; Fernique, François; Joshi, Chaitanya; Molina-Sánchez, Alejandro; Wirtz, Ludger; Berciaud, Stéphane

    2015-10-01

    $N$-layer transition metal dichalcogenides provide a unique platform to investigate the evolution of the physical properties between the bulk (three dimensional) and monolayer (quasi two-dimensional) limits. Here, using high-resolution micro-Raman spectroscopy, we report a unified experimental description of the $\\Gamma$-point optical phonons in $N$-layer $2H$-molybdenum ditelluride (MoTe$_2$). We observe a series of $N$-dependent low-frequency interlayer shear and breathing modes (below $40~\\rm cm^{-1}$, denoted LSM and LBM) and well-defined Davydov splittings of the mid-frequency modes (in the range $100-200~\\rm cm^{-1}$, denoted iX and oX), which solely involve displacements of the chalcogen atoms. In contrast, the high-frequency modes (in the range $200-300~\\rm cm^{-1}$, denoted iMX and oMX), arising from displacements of both the metal and chalcogen atoms, exhibit considerably reduced splittings. The manifold of phonon modes associated with the in-plane and out-of-plane displacements are quantitatively described by a force constant model, including interactions up to the second nearest neighbor and surface effects as fitting parameters. The splittings for the iX and oX modes observed in $N$-layer crystals are directly correlated to the corresponding bulk Davydov splittings between the $E_{2u}/E_{1g}$ and $B_{1u}/A_{1g}$ modes, respectively, and provide a measurement of the frequencies of the bulk silent $E_{2u}$ and $B_{1u}$ optical phonon modes. Our analysis could readily be generalized to other layered crystals.

  14. Topological phonon modes in filamentary structures

    NASA Astrophysics Data System (ADS)

    Berg, Nina; Joel, Kira; Koolyk, Miriam; Prodan, Emil

    2011-02-01

    This work describes a class of topological phonon modes, that is, mechanical vibrations localized at the edges of special structures that are robust against the deformations of the structures. A class of topological phonons was recently found in two-dimensional structures similar to that of microtubules. The present work introduces another class of topological phonons, this time occurring in quasi-one-dimensional filamentary structures with inversion symmetry. The phenomenon is exemplified using a structure inspired from that of actin microfilaments, present in most live cells. The system discussed here is probably the simplest structure that supports topological phonon modes, a fact that allows detailed analysis in both time and frequency domains. We advance the hypothesis that the topological phonon modes are ubiquitous in the biological world and that living organisms make use of them during various processes.

  15. High-temperature Raman spectroscopy of solid oxide fuel cell materials and processes.

    PubMed

    Pomfret, Michael B; Owrutsky, Jeffrey C; Walker, Robert A

    2006-09-07

    Chemical and material processes occurring in high temperature environments are difficult to quantify due to a lack of experimental methods that can probe directly the species present. In this letter, Raman spectroscopy is shown to be capable of identifying in-situ and noninvasively changes in material properties as well as the formation and disappearance of molecular species on surfaces at temperatures of 715 degrees C. The material, yttria-stabilized zirconia or YSZ, and the molecular species, Ni/NiO and nanocrystalline graphite, factor prominently in the chemistry of solid oxide fuel cells (SOFCs). Experiments demonstrate the ability of Raman spectroscopy to follow reversible oxidation/reduction kinetics of Ni/NiO as well as the rate of carbon disappearance when graphite, formed in-situ, is exposed to a weakly oxidizing atmosphere. In addition, the Raman active phonon mode of YSZ shows a temperature dependent shift that correlates closely with the expansion of the lattice parameter, thus providing a convenient internal diagnostic for identifying thermal gradients in high temperature systems. These findings provide direct insight into processes likely to occur in operational SOFCs and motivate the use of in-situ Raman spectroscopy to follow chemical processes in these high-temperature, electrochemically active environments.

  16. Phonon thermodynamics of iron and cementite

    NASA Astrophysics Data System (ADS)

    Mauger, Lisa Mary

    The vibrational properties of materials are essential to understanding material stability and thermodynamics. In this thesis I outline vibrational thermodynamic models and the experimental tools that provide evidence on phonon behavior. The introductory section discusses the history of metallurgy and thermodynamic theory, with an emphasis on the role of iron and cementite, two important components of steels. The thermodynamic framework for understanding vibrational material behavior is provided alongside the growing body of experimental and computational tools that provide physical insight on vibrational properties. The high temperature vibrational behavior of iron and cementite are explored within this context in the final chapters. Body-centered-cubic iron exhibits decreasing phonon energies at elevated temperatures. The observed energy change in not uniform across phonon modes in iron, and specific phonon modes show significant decreases in energy that are not explained by simple vibrational models. This anomalously energy decrease is linked to the second-nearest-neighbor interactions in the bcc structure, through examination of fitted interatomic force constants. The large changes in phonon energy result in a significant increase in the vibrational entropy, called the nonharmonic vibrational entropy, which emulates the temperature behavior of the magnetic entropy across the Curie temperature. The nonharmonic vibrational entropy is attributed to interactions between the vibrations and state of magnetic disorder in the material, which persists above the magnetic transitions and extends the stability region of the bcc phase. Orthorombic cementite, Fe3C, exhibits anisotropic magneto-volume behavior in the ferromagnetic phase including regions very low thermal expansion. The phonon modes of cementite show anomalous temperature dependence, with low energy phonon modes increasing their energy at elevated temperatures in the ferromagnetic phase. This behavior is

  17. Mutual interactions of phonons, rotons, and gravity

    NASA Astrophysics Data System (ADS)

    Nicolis, Alberto; Penco, Riccardo

    2018-04-01

    We introduce an effective point-particle action for generic particles living in a zero-temperature superfluid. This action describes the motion of the particles in the medium at equilibrium as well as their couplings to sound waves and generic fluid flows. While we place the emphasis on elementary excitations such as phonons and rotons, our formalism applies also to macroscopic objects such as vortex rings and rigid bodies interacting with long-wavelength fluid modes. Within our approach, we reproduce phonon decay and phonon-phonon scattering as predicted using a purely field-theoretic description of phonons. We also correct classic results by Landau and Khalatnikov on roton-phonon scattering. Finally, we discuss how phonons and rotons couple to gravity, and show that the former tend to float while the latter tend to sink but with rather peculiar trajectories. Our formalism can be easily extended to include (general) relativistic effects and couplings to additional matter fields. As such, it can be relevant in contexts as diverse as neutron star physics and light dark matter detection.

  18. Variable-Range Hopping through Marginally Localized Phonons

    NASA Astrophysics Data System (ADS)

    Banerjee, Sumilan; Altman, Ehud

    2016-03-01

    We investigate the effect of coupling Anderson localized particles in one dimension to a system of marginally localized phonons having a symmetry protected delocalized mode at zero frequency. This situation is naturally realized for electrons coupled to phonons in a disordered nanowire as well as for ultracold fermions coupled to phonons of a superfluid in a one-dimensional disordered trap. To determine if the coupled system can be many-body localized we analyze the phonon-mediated hopping transport for both the weak and strong coupling regimes. We show that the usual variable-range hopping mechanism involving a low-order phonon process is ineffective at low temperature due to discreteness of the bath at the required energy. Instead, the system thermalizes through a many-body process involving exchange of a diverging number n ∝-log T of phonons in the low temperature limit. This effect leads to a highly singular prefactor to Mott's well-known formula and strongly suppresses the variable range hopping rate. Finally, we comment on possible implications of this physics in higher dimensional electron-phonon coupled systems.

  19. Raman effect in multiferroic Bi5Fe1+xTi3-xO15 solid solutions: A temperature study

    NASA Astrophysics Data System (ADS)

    Rodríguez Aranda, Ma. Del Carmen; Rodríguez-Vázquez, Ángel G.; Salazar-Kuri, Ulises; Mendoza, María Eugenia; Navarro-Contreras, Hugo R.

    2018-02-01

    In this work, a Raman study of powder samples of multiferroic Bi5Fe1+xTi3-xO15 solid solutions and Bi6Fe2Ti3O18 as a function of temperature from 27 °C (room temperature) to 850 °C is presented. The values of x (i.e., the Fe composition) for the solid solutions were 1.0, 1.1, 1.3, and 1.4. The temperature coefficients of eight phonon frequencies were determined for all the samples. The large observed phonon broadenings with increasing temperature precluded the observation of several of the phonon bands above defined temperatures in the range of 200-700 °C depending on the sample. These phonon broadenings were explained on the basis of the Klemens model, which considers that the broadenings are due to the thermal expansion of the lattice with a major contribution in terms of magnitude from anharmonic phonon-phonon interactions. However, some evidence for the presence of several of the phonons persisted up to 800-850 °C. These solid solutions are expected to exhibit a ferroelectric-paraelectric phase transition at 742 to 750 °C and a ferromagnetic-antiferromagnetic transition at 426 °C. We also observed changes in the slopes of the temperature dependence of the phonon frequencies for the lines at 228 cm-1 for Bi5FeTi3O15 and 330 cm-1 for Bi6Fe2Ti3O18 at temperatures of 247 °C and 347 °C, respectively. No similar temperature-frequency slope changes indicative of possible phase transitions were observed for any of the phonon lines of the other three Bi5Fe1+xTi3-xO15 solid solutions examined.

  20. Measuring phonon mean free path distributions by probing quasiballistic phonon transport in grating nanostructures

    DOE PAGES

    Zeng, Lingping; Collins, Kimberlee C.; Hu, Yongjie; ...

    2015-11-27

    Heat conduction in semiconductors and dielectrics depends upon their phonon mean free paths that describe the average travelling distance between two consecutive phonon scattering events. Nondiffusive phonon transport is being exploited to extract phonon mean free path distributions. Here, we describe an implementation of a nanoscale thermal conductivity spectroscopy technique that allows for the study of mean free path distributions in optically absorbing materials with relatively simple fabrication and a straightforward analysis scheme. We pattern 1D metallic grating of various line widths but fixed gap size on sample surfaces. The metal lines serve as both heaters and thermometers in time-domainmore » thermoreflectance measurements and simultaneously act as wiregrid polarizers that protect the underlying substrate from direct optical excitation and heating. We demonstrate the viability of this technique by studying length-dependent thermal conductivities of silicon at various temperatures. The thermal conductivities measured with different metal line widths are analyzed using suppression functions calculated from the Boltzmann transport equation to extract the phonon mean free path distributions with no calibration required. Furthermore, this table-top ultrafast thermal transport spectroscopy technique enables the study of mean free path spectra in a wide range of technologically important materials.« less

  1. The study of dispersive 'b'-mode in monolayer MoS2 in temperature dependent resonant Raman scattering experiments

    NASA Astrophysics Data System (ADS)

    Kutrowska-Girzycka, Joanna; Jadczak, Joanna; Bryja, Leszek

    2018-07-01

    We report on resonant Raman scattering studies of monolayer MoS2 as a function of the excitation laser energy (1.959-2.033 eV) and temperature (T = 7-295 K). In complementary reflectivity contrast experiments we determined the temperature evolution of the A exciton and trion resonances. We focus our studies on the dispersive, second order 'b' mode related to the resonant two phonon Raman process of successive emissions of the acoustic LA and TA phonons at K points. We found that when excitation laser energy is tuned across the A exciton level this mode shifts almost linearly to lower frequency with the rate equal -83 and -71 cm-1/eV at T = 7 and 295 K, respectively, which is about two times higher rate than those reported in the previous studies of monolayer MoS2 but very close the relevant rate recorded for bulk MoS2. We interpret this effect as related to the difference of concentration of two dimensional electron gas. We also determined, using excitation with the He-Ne laser the temperature shifts of the Raman peaks of dispersive 'b' and dispersionless E‧ and A1‧ modes. We found that absolute value of the temperature coefficient of 'b' mode, equals 3.5 × 10-2 cm-1/K, is much higher than those of E‧ and A1‧ modes, equal 0.4 × 10-2 and 0.8 × 10-2 cm-1/K, respectively.

  2. The dielectric properties of La(Mg0.5Ti0.5)O3 ceramics studied by Raman-scattering, infrared reflectivity spectroscopy, and first-principles calculations.

    PubMed

    Liu, Hsiang-Lin; Hsueh, Hung-Chung; Lin, I-Nan; Yang, Ming-Ti; Lee, Wei-Chung; Chen, Yi-Chun; Chia, Chia-Ta; Cheng, Hsiu-Fung

    2011-06-08

    La(Mg(0.5)Ti(0.5))O(3) (LMT) ceramics were prepared by either the solid-state reaction (LMT)(SS) or the citric-acid chemical method (LMT)(CA). A combination of Raman scattering, infrared reflectivity, and first-principles calculations was carried out to elucidate the correlation between lattice dynamics and the dielectric properties of these materials. Twelve Raman-active phonons are observed in both samples, displaying similar frequency positions. Interestingly, the A(g) phonon (g(11) mode) of (LMT)(SS) at about 717 cm(-1) involving the oxygen octahedron breathing vibrations demonstrates a narrower linewidth, suggesting its better crystallinity. Furthermore, an infrared-active u(2) phonon band due to the vibrations of O(I) and O(II) layers, which possesses the largest oscillator strength, exhibits stronger intensity for (LMT)(SS), as compared with those for (LMT)(CA). Additionally, the Q × f values (the product of dielectric Q values and measurement frequency) of (LMT)(SS) estimated from either microwave cavity or infrared spectroscopic measurements are larger than those of (LMT)(CA). These results indicate that the better coherence of lattice vibrations in (LMT)(SS) leads to its higher Q × f value, providing evidence for a strong connection between optical spectroscopic behavior and microwave dielectric characteristics in these materials.

  3. Contrast and Raman spectroscopy study of single- and few-layered charge density wave material: 2H-TaSe2

    PubMed Central

    Hajiyev, Parviz; Cong, Chunxiao; Qiu, Caiyu; Yu, Ting

    2013-01-01

    In this article, we report the first successful preparation of single- and few-layers of tantalum diselenide (2H-TaSe2) by mechanical exfoliation technique. Number of layers is confirmed by white light contrast spectroscopy and atomic force microscopy (AFM). Vibrational properties of the atomically thin layers of 2H-TaSe2 are characterized by micro-Raman spectroscopy. Room temperature Raman measurements demonstrate MoS2-like spectral features, which are reliable for thickness determination. E1g mode, usually forbidden in backscattering Raman configuration is observed in the supported TaSe2 layers while disappears in the suspended layers, suggesting that this mode may be enabled because of the symmetry breaking induced by the interaction with the substrate. A systematic in-situ low temperature Raman study, for the first time, reveals the existence of incommensurate charge density wave phase transition in single and double-layered 2H-TaSe2 as reflected by a sudden softening of the second-order broad Raman mode resulted from the strong electron-phonon coupling (Kohn anomaly). PMID:24005335

  4. Thermodynamic measurements in a high pressure hydrogen-oxygen flame using Raman scattering from a broadband excimer laser

    NASA Technical Reports Server (NTRS)

    Hartfield, Roy, Jr.

    1996-01-01

    Raman scattering is an inelastic molecular scattering process in which incident radiation is reemitted at a fixed change in frequency. Raman spectroscopy can be used to measure the number density and temperature of the irradiated species. The strength of the Raman signal is inversely proportional to the wavelength raised to the fourth power. Consequently, high signal to noise ratios are obtained by using ultraviolet (UV) excitation sources. Using UV sources for Raman Spectroscopy in flames is complicated by the fact that some of the primary constituents in hydrogen-oxygen combustion absorb and reemit light in the UV and these fluorescence processes interfere with the Raman signals. This problem has been handled in atmospheric pressure flames in some instances by using a narrowband tunable excimer laser as a source. This allows for detuning from absorption transitions and the elimination of interfering fluorescence signals at the Raman wavelengths. This approach works well in the atmospheric pressure flame; however, it has two important disadvantages. First, injection-locked narrowband tunable excimer lasers are very expensive. More importantly, however, is the fact that at the high pressures characteristic of rocket engine combustion chambers, the absorption transitions are broadened making it difficult to tune to a spectral location at which substantial absorption would not occur. The approach taken in this work is to separate the Raman signal from the fluorescence background by taking advantage of the fact that Raman signal has nonisotropic polarization characteristics while the fluorescence signals are unpolarized. Specifically, for scattering at right angles to the excitation beam path, the Raman signal is completely polarized. The Raman signal is separated from the fluorescence background by collecting both horizontally and vertically polarized signals separately. One of the polarizations has both the Raman signal and the fluorescence background while the

  5. Transmission eigenchannels for coherent phonon transport

    NASA Astrophysics Data System (ADS)

    Klöckner, J. C.; Cuevas, J. C.; Pauly, F.

    2018-04-01

    We present a procedure to determine transmission eigenchannels for coherent phonon transport in nanoscale devices using the framework of nonequilibrium Green's functions. We illustrate our procedure by analyzing a one-dimensional chain, where all steps can be carried out analytically. More importantly, we show how the procedure can be combined with ab initio calculations to provide a better understanding of phonon heat transport in realistic atomic-scale junctions. In particular, we study the phonon eigenchannels in a gold metallic atomic-size contact and different single-molecule junctions based on molecules such as an alkane chain, a brominated benzene-diamine, where destructive phonon interference effects take place, and a C60 junction.

  6. Multiphonon resonant Raman scattering in MoS{sub 2}

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Gołasa, K., E-mail: Katarzyna.Golasa@fuw.edu.pl; Grzeszczyk, M.; Wysmołek, A.

    2014-03-03

    Optical emission spectrum of a resonantly (λ = 632.8 nm) excited molybdenum disulfide (MoS{sub 2}) is studied at liquid helium temperature. More than 20 peaks in the energy range spanning up to 1400 cm{sup −1} from the laser line, which are related to multiphonon resonant Raman scattering processes, are observed. The attribution of the observed lines involving basic lattice vibrational modes of MoS{sub 2} and both the longitudinal (LA(M)) and the transverse (TA(M) and/or ZA(M)) acoustic phonons from the vicinity of the high-symmetry M point of the MoS{sub 2} Brillouin zone is proposed.

  7. Scanning Tunneling Microscopy Observation of Phonon Condensate

    PubMed Central

    Altfeder, Igor; Voevodin, Andrey A.; Check, Michael H.; Eichfeld, Sarah M.; Robinson, Joshua A.; Balatsky, Alexander V.

    2017-01-01

    Using quantum tunneling of electrons into vibrating surface atoms, phonon oscillations can be observed on the atomic scale. Phonon interference patterns with unusually large signal amplitudes have been revealed by scanning tunneling microscopy in intercalated van der Waals heterostructures. Our results show that the effective radius of these phonon quasi-bound states, the real-space distribution of phonon standing wave amplitudes, the scattering phase shifts, and the nonlinear intermode coupling strongly depend on the presence of defect-induced scattering resonance. The observed coherence of these quasi-bound states most likely arises from phase- and frequency-synchronized dynamics of all phonon modes, and indicates the formation of many-body condensate of optical phonons around resonant defects. We found that increasing the strength of the scattering resonance causes the increase of the condensate droplet radius without affecting the condensate fraction inside it. The condensate can be observed at room temperature. PMID:28225066

  8. Probing Pharmaceutical Mixtures during Milling: The Potency of Low-Frequency Raman Spectroscopy in Identifying Disorder.

    PubMed

    Walker, Greg; Römann, Philipp; Poller, Bettina; Löbmann, Korbinian; Grohganz, Holger; Rooney, Jeremy S; Huff, Gregory S; Smith, Geoffrey P S; Rades, Thomas; Gordon, Keith C; Strachan, Clare J; Fraser-Miller, Sara J

    2017-12-04

    This study uses a multimodal analytical approach to evaluate the rates of (co)amorphization of milled drug and excipient and the effectiveness of different analytical methods in detecting these changes. Indomethacin and tryptophan were the model substances, and the analytical methods included low-frequency Raman spectroscopy (785 nm excitation and capable of measuring both low- (10 to 250 cm -1 ) and midfrequency (450 to 1800 cm -1 ) regimes, and a 830 nm system (5 to 250 cm -1 )), conventional (200-3000 cm -1 ) Raman spectroscopy, Fourier transform infrared spectroscopy (FTIR), and X-ray powder diffraction (XRPD). The kinetics of amorphization were found to be faster for the mixture, and indeed, for indomethacin, only partial amorphization occurred (after 360 min of milling). Each technique was capable of identifying the transformations, but some, such as low-frequency Raman spectroscopy and XRPD, provided less ambiguous signatures than the midvibrational frequency techniques (conventional Raman and FTIR). The low-frequency Raman spectra showed intense phonon mode bands for the crystalline and cocrystalline samples that could be used as a sensitive probe of order. Multivariate analysis has been used to further interpret the spectral changes. Overall, this study demonstrates the potential of low-frequency Raman spectroscopy, which has several practical advantages over XRPD, for probing (dis-)order during pharmaceutical processing, showcasing its potential for future development, and implementation as an in-line process monitoring method.

  9. Magnons and magnetodielectric effects in CoCr2O4 : Raman scattering studies

    NASA Astrophysics Data System (ADS)

    Sethi, A.; Byrum, T.; McAuliffe, R. D.; Gleason, S. L.; Slimak, J. E.; Shoemaker, D. P.; Cooper, S. L.

    2017-05-01

    Magnetoelectric materials have generated wide technological and scientific interest because of the rich phenomena these materials exhibit, including the coexistence of magnetic and ferroelectric orders, magnetodielectric behavior, and exotic hybrid excitations such as electromagnons. The multiferroic spinel material CoCr2O4 is a particularly interesting example of a multiferroic material, because evidence for magnetoelectric behavior in the ferrimagnetic phase seems to conflict with traditional noncollinear-spin-driven mechanisms for inducing a macroscopic polarization. With the overall goal of clarifying the magnetodielectric behavior previously reported below TC in CoCr2O4 , in this paper we report an inelastic light scattering study of the magnon and phonon spectrum of CoCr2O4 as simultaneous functions of temperature, pressure, and magnetic field. Below the Curie temperature (TC=94 K ) of CoCr2O4 we observe a ω ˜16 cm-1 q =0 magnon having T1g-symmetry, which has the transformation properties of an axial vector. The anomalously large Raman intensity of the T1g-symmetry magnon is characteristic of materials with a large magneto-optical response and likely arises from large magnetic fluctuations that strongly modulate the dielectric response in CoCr2O4 . The Raman susceptibility of the T1g-symmetry magnon exhibits a strong magnetic-field dependence that is consistent with the magnetodielectric response observed in CoCr2O4 , suggesting that magnetodielectric behavior in CoCr2O4 primarily arises from the field-dependent suppression of magnetic fluctuations that are strongly coupled to long-wavelength phonons. Increasing the magnetic anisotropy in CoCr2O4 with applied pressure decreases the magnetic-field dependence of the T1g-symmetry magnon Raman susceptibility, suggesting that strain can be used to control the magnetodielectric response in CoCr2O4 .

  10. Absorption and resonance Raman spectra of Pb2, Pb3, and Pb4 in xenon matrices

    NASA Technical Reports Server (NTRS)

    Stranz, D. D.; Khanna, R. K.

    1981-01-01

    Matrix isolation techniques are used to investigate the spectra of lead molecules and, in particular, to obtain resonance Raman spectra of lead vapors isolated in solid xenon matrices. The presence of Pb2 is confirmed by the visible adsorption, and Raman spectra yield a vibrational frequency for the ground state of 108 per cm and a dissociation energy of 8200 per cm. A second resonance Raman progression indicates a Pb3 species of D3h symmetry. Finally, two additional Raman features at approximately 111 per cm spacing are evidence for a third species, tentatively identified as Pb4.

  11. Ocean Raman Scattering in Satellite Backscatter UV Measurements

    NASA Technical Reports Server (NTRS)

    Vasilkov, Alexander P.; Joiner, Joanna; Gleason, James; Bhartia, Pawan; Bhartia, P. K. (Technical Monitor)

    2002-01-01

    Ocean Raman scattering significantly contributes to the filling-in of solar Fraunhofer lines measured by satellite backscatter ultraviolet (buy) instruments in the cloudless atmosphere over clear ocean waters. A model accounting for this effect in buy measurements is developed and compared with observations from the Global Ozone Monitoring Experiment (GONE). The model extends existing models for ocean Raman scattering to the UV spectral range. Ocean Raman scattering radiance is propagated through the atmosphere using a concept of the Lambert equivalent reflectively and an accurate radiative transfer model for Rayleigh scattering. The model and observations can be used to evaluate laboratory measurements of pure water absorption in the UV. The good agreement between model and observations suggests that buy instruments may be useful for estimating chlorophyll content.

  12. Scanning Tunneling Microscopy Observation of Phonon Condensate

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Altfeder, Igor; Balatsky, Alexander V.; Voevodin, Andrey A.

    Using quantum tunneling of electrons into vibrating surface atoms, phonon oscillations can be observed on the atomic scale. Phonon interference patterns with unusually large signal amplitudes have been revealed by scanning tunneling microscopy in intercalated van der Waals heterostructures. Our results show that the effective radius of these phonon quasi-bound states, the real-space distribution of phonon standing wave amplitudes, the scattering phase shifts, and the nonlinear intermode coupling strongly depend on the presence of defect-induced scattering resonance. The observed coherence of these quasi-bound states most likely arises from phase- and frequency-synchronized dynamics of all phonon modes, and indicates the formationmore » of many-body condensate of optical phonons around resonant defects. We found that increasing the strength of the scattering resonance causes the increase of the condensate droplet radius without affecting the condensate fraction inside it. The condensate can be observed at room temperature.« less

  13. Scanning Tunneling Microscopy Observation of Phonon Condensate

    DOE PAGES

    Altfeder, Igor; Balatsky, Alexander V.; Voevodin, Andrey A.; ...

    2017-02-22

    Using quantum tunneling of electrons into vibrating surface atoms, phonon oscillations can be observed on the atomic scale. Phonon interference patterns with unusually large signal amplitudes have been revealed by scanning tunneling microscopy in intercalated van der Waals heterostructures. Our results show that the effective radius of these phonon quasi-bound states, the real-space distribution of phonon standing wave amplitudes, the scattering phase shifts, and the nonlinear intermode coupling strongly depend on the presence of defect-induced scattering resonance. The observed coherence of these quasi-bound states most likely arises from phase- and frequency-synchronized dynamics of all phonon modes, and indicates the formationmore » of many-body condensate of optical phonons around resonant defects. We found that increasing the strength of the scattering resonance causes the increase of the condensate droplet radius without affecting the condensate fraction inside it. The condensate can be observed at room temperature.« less

  14. Progress on Raman laser for sodium resonance fluorescence lidar

    NASA Astrophysics Data System (ADS)

    Li, Steven X.; Yu, Anthony W.; Krainak, Michael A.; Bai, Yingxin; Konoplev, Oleg; Fahey, Molly E.; Numata, Kenji

    2018-02-01

    We are developing a Q-switched narrow linewidth intra-cavity Raman laser for a space based sodium lidar application. A novel Raman laser injection seeding scheme is proposed and is experimentally verified. A Q-switched, diode pumped, c-cut Nd:YVO4 laser has been designed to emit a fundamental wavelength at 1066.6 nm. This fundamental wavelength is used as the pump in an intra-cavity Raman conversion in a Gd0.2Y0.8VO4 composite material. By tuning the temperature of the crystal, we tuned the Raman shifting to the desired sodium absorption line. A diode end pumped, T-shaped laser cavity has been built for experimental investigation. The fundamental pump laser cavity is a twisted mode cavity to eliminate the spatial hole burning for effective injection seeding. The Raman laser cavity is a linear standing wave cavity because Raman gain medium does not suffer spatial hole burning as traditional laser gain medium. The linewidth and temporal profile of the Raman laser is experimentally investigated with narrow and broadband fundamental pump emission. We have, for the first time, demonstrated an injection seeded, high peak power, narrow linewidth intra-cavity Raman laser for potential use in a sodium resonance fluorescence lidar.

  15. Effect of phonon-bath dimensionality on the spectral tuning of single-photon emitters in the Purcell regime

    NASA Astrophysics Data System (ADS)

    Chassagneux, Yannick; Jeantet, Adrien; Claude, Théo; Voisin, Christophe

    2018-05-01

    We develop a theoretical frame to investigate the spectral dependence of the brightness of a single-photon source made of a solid-state nanoemitter embedded in a high-quality factor microcavity. This study encompasses the cases of localized excitons embedded in a one-, two-, or three-dimensional matrix. The population evolution is calculated based on a spin-boson model, using the noninteracting blip approximation. We find that the spectral dependence of the single-photon source brightness (hereafter called spectral efficiency) can be expressed analytically through the free-space emission and absorption spectra of the emitter, the vacuum Rabi splitting, and the loss rates of the system. In other words, the free-space spectrum of the emitter encodes all the relevant information on the interaction between the exciton and the phonon bath to obtain the dynamics of the cavity-coupled system. We compute numerically the spectral efficiency for several types of localized emitters differing by the phonon bath dimensionality. In particular, in low-dimensional systems where this interaction is enhanced, a pronounced asymmetric energy exchange between the emitter and the cavity on the phonon sidebands yields a considerable extension of the tuning range of the source through phonon-assisted cavity feeding, possibly surpassing that of a purely resonant system.

  16. Electron-phonon coupling and phonon subbands in small, electrically heated metal wires

    NASA Astrophysics Data System (ADS)

    Perrin, N.; Wybourne, M. N.

    1996-02-01

    The initial work of Perrin and Budd is extended to small metal wires in which the usual bulk phonon spectrum is modified into a series of acoustic subbands at low temperature. We analyze the contribution of the subbands to the lack of equilibrium between the electrons and the phonons in the wire heated by an applied electric field. The resulting electrical behavior of the wire is also considered and compared to experimental results.

  17. Stimulated Raman photoacoustic imaging

    PubMed Central

    Yakovlev, Vladislav V.; Zhang, Hao F.; Noojin, Gary D.; Denton, Michael L.; Thomas, Robert J.; Scully, Marlan O.

    2010-01-01

    Achieving label-free, molecular-specific imaging with high spatial resolution in deep tissue is often considered the grand challenge of optical imaging. To accomplish this goal, significant optical scattering in tissues has to be overcome while achieving molecular specificity without resorting to extrinsic labeling. We demonstrate the feasibility of developing such an optical imaging modality by combining the molecularly specific stimulated Raman excitation with the photoacoustic detection. By employing two ultrashort excitation laser pulses, separated in frequency by the vibrational frequency of a targeted molecule, only the specific vibrational level of the target molecules in the illuminated tissue volume is excited. This targeted optical absorption generates ultrasonic waves (referred to as stimulated Raman photoacoustic waves) which are detected using a traditional ultrasonic transducer to form an image following the design of the established photoacoustic microscopy. PMID:21059930

  18. Controlling thermal emission of phonon by magnetic metasurfaces

    PubMed Central

    Zhang, X.; Liu, H.; Zhang, Z. G.; Wang, Q.; Zhu, S. N.

    2017-01-01

    Our experiment shows that the thermal emission of phonon can be controlled by magnetic resonance (MR) mode in a metasurface (MTS). Through changing the structural parameter of metasurface, the MR wavelength can be tuned to the phonon resonance wavelength. This introduces a strong coupling between phonon and MR, which results in an anticrossing phonon-plasmons mode. In the process, we can manipulate the polarization and angular radiation of thermal emission of phonon. Such metasurface provides a new kind of thermal emission structures for various thermal management applications. PMID:28157206

  19. Quantum many-body correlations in collective phonon-excitations

    NASA Astrophysics Data System (ADS)

    Droenner, Leon; Kabuss, Julia; Carmele, Alexander

    2018-02-01

    We present a theoretical study of a many-emitter phonon laser based on optically driven semiconductor quantum dots placed within an acoustic nanocavity. A transformation of the phonon laser Hamiltonian leads to a Tavis-Cummings type interaction with an unexpected additional many-emitter energy shift. This many-emitter interaction with the cavity mode results in a variety of phonon resonances which dependent strongly on the number of participating emitters. These collective resonances show the highest phonon output. Furthermore, we show that the output can be increased even more via lasing at the two phonon resonance.

  20. Tunable infrared reflectance by phonon modulation

    DOEpatents

    Ihlefeld, Jon F.; Sinclair, Michael B.; Beechem, III, Thomas E.

    2018-03-06

    The present invention pertains to the use of mobile coherent interfaces in a ferroelectric material to interact with optical phonons and, ultimately, to affect the material's optical properties. In altering the optical phonon properties, the optical properties of the ferroelectric material in the spectral range near-to the phonon mode frequency can dramatically change. This can result in a facile means to change to the optical response of the ferroelectric material in the infrared.

  1. Heterodyne x-ray diffuse scattering from coherent phonons

    DOE PAGES

    Kozina, M.; Trigo, M.; Chollet, M.; ...

    2017-08-10

    Here in this paper, we report Fourier-transform inelastic x-ray scattering measurements of photoexcited GaAs with embedded ErAs nanoparticles. We observe temporal oscillations in the x-ray scattering intensity, which we attribute to inelastic scattering from coherent acoustic phonons. Unlike in thermal equilibrium, where inelastic x-ray scattering is proportional to the phonon occupation, we show that the scattering is proportional to the phonon amplitude for coherent states. The wavevectors of the observed phonons extend beyond the excitation wavevector. The nanoparticles break the discrete translational symmetry of the lattice, enabling the generation of large wavevector coherent phonons. Elastic scattering of x-ray photons frommore » the nanoparticles provides a reference for heterodyne mixing, yielding signals proportional to the phonon amplitude.« less

  2. Strain Control of Exciton-Phonon Coupling in Atomically Thin Semiconductors.

    PubMed

    Niehues, Iris; Schmidt, Robert; Drüppel, Matthias; Marauhn, Philipp; Christiansen, Dominik; Selig, Malte; Berghäuser, Gunnar; Wigger, Daniel; Schneider, Robert; Braasch, Lisa; Koch, Rouven; Castellanos-Gomez, Andres; Kuhn, Tilmann; Knorr, Andreas; Malic, Ermin; Rohlfing, Michael; Michaelis de Vasconcellos, Steffen; Bratschitsch, Rudolf

    2018-03-14

    Semiconducting transition metal dichalcogenide (TMDC) monolayers have exceptional physical properties. They show bright photoluminescence due to their unique band structure and absorb more than 10% of the light at their excitonic resonances despite their atomic thickness. At room temperature, the width of the exciton transitions is governed by the exciton-phonon interaction leading to strongly asymmetric line shapes. TMDC monolayers are also extremely flexible, sustaining mechanical strain of about 10% without breaking. The excitonic properties strongly depend on strain. For example, exciton energies of TMDC monolayers significantly redshift under uniaxial tensile strain. Here, we demonstrate that the width and the asymmetric line shape of excitonic resonances in TMDC monolayers can be controlled with applied strain. We measure photoluminescence and absorption spectra of the A exciton in monolayer MoSe 2 , WSe 2 , WS 2 , and MoS 2 under uniaxial tensile strain. We find that the A exciton substantially narrows and becomes more symmetric for the selenium-based monolayer materials, while no change is observed for atomically thin WS 2 . For MoS 2 monolayers, the line width increases. These effects are due to a modified exciton-phonon coupling at increasing strain levels because of changes in the electronic band structure of the respective monolayer materials. This interpretation based on steady-state experiments is corroborated by time-resolved photoluminescence measurements. Our results demonstrate that moderate strain values on the order of only 1% are already sufficient to globally tune the exciton-phonon interaction in TMDC monolayers and hold the promise for controlling the coupling on the nanoscale.

  3. Beyond spatial correlation effect in micro-Raman light scattering: An example of zinc-blende GaN/GaAs hetero-interface

    NASA Astrophysics Data System (ADS)

    Ning, J. Q.; Zheng, C. C.; Zheng, L. X.; Xu, S. J.

    2015-08-01

    Spatially resolved Raman light scattering experiments were performed on a zinc-blende GaN/GaAs heterostructure with confocal micro-Raman scattering technique under the backscattering geometric configuration. By varying the illumination spot locations across the heterostructure interface, we found that the Raman light scattering spectral features change remarkably. The interface effect on the GaAs substrate manifested as a much broader lineshape of the transverse optical (TO) phonon mode. Two kinds of broadening mechanisms, namely, spatial correlation induced wave-vector relaxation effect and lattice-mismatch strain + compositional intermixing effect, have been identified. The former leads to the broadening of the TO mode at the low-energy side, whereas the latter accounts for the broadening at the high-energy side. The diffuse light scattering from the highly defective nucleation layer of GaN was found to produce a broad scattering background of the GaN TO mode. The methodology and conclusions of the present work could be applicable to Raman spectroscopic studies on other material interfaces.

  4. Ion beam induced optical and surface modification in plasmonic nanostructures

    NASA Astrophysics Data System (ADS)

    Singh, Udai B.; Gautam, Subodh K.; Kumar, Sunil; Hooda, Sonu; Ojha, Sunil; Singh, Fouran

    2016-07-01

    In present work, ion irradiation induced nanostructuring has been exploited as an efficient and effective tool for synthesis of coupled plasmonics nanostructures by using 1.2 MeV Xe ions on Au/ZnO/Au system deposited on glass substrate. The results are correlated on the basis of their optical absorption, surface morphologies and enhanced sensitivity of evolved phonon modes by using UV Visible spectroscopy, scanning electron microscopy (SEM), and Raman spectroscopy (RS), respectively. Optical absorbance spectra of plasmonic nanostructures (NSs) show a decrease in band gap, which may be ascribed to the formation of defects with ion irradiation. The surface morphology reveals the formation of percolated NSs upon ion irradiation and Rutherford backscattering spectrometry (RBS) study clearly shows the formation of multilayer system. Furthermore, RS measurements on samples are studied to understand the enhanced sensitivity of ion irradiation induced phonon mode at 573 cm-1 along with other modes. As compared to pristine sample, a stronger and pronounced evolution of these phonon modes is observed with further ion irradiation, which indicates localized surface plasmon results with enhanced intensity of phonon modes of Zinc oxide (ZnO) material. Thus, such plasmonic NSs can be used as surface enhanced Raman scattering (SERS) substrates.

  5. Nonperturbative Quantum Nature of the Dislocation–Phonon Interaction

    DOE PAGES

    Li, Mingda; Ding, Zhiwei; Meng, Qingping; ...

    2017-01-31

    Despite the long history of dislocation–phonon interaction studies, there are many problems that have not been fully resolved during this development. These include an incompatibility between a perturbative approach and the long-range nature of a dislocation, the relation between static and dynamic scattering, and their capability of dealing with thermal transport phenomena for bulk material only. Here in this paper, by utilizing a fully quantized dislocation field, which we called a “dislon”, a phonon interacting with a dislocation is renormalized as a quasi-phonon, with shifted quasi-phonon energy, and accompanied by a finite quasi-phonon lifetime, which are reducible to classical results.more » A series of outstanding legacy issues including those above can be directly explained within this unified phonon renormalization approach. For instance, a renormalized phonon naturally resolves the decade-long debate between dynamic and static dislocation–phonon scattering approaches, as two limiting cases. In particular, at nanoscale, both the dynamic and static approaches break down, while the present renormalization approach remains valid by capturing the size effect, showing good agreement with lattice dynamics simulations.« less

  6. Nonperturbative Quantum Nature of the Dislocation–Phonon Interaction

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Li, Mingda; Ding, Zhiwei; Meng, Qingping

    Despite the long history of dislocation–phonon interaction studies, there are many problems that have not been fully resolved during this development. These include an incompatibility between a perturbative approach and the long-range nature of a dislocation, the relation between static and dynamic scattering, and their capability of dealing with thermal transport phenomena for bulk material only. Here in this paper, by utilizing a fully quantized dislocation field, which we called a “dislon”, a phonon interacting with a dislocation is renormalized as a quasi-phonon, with shifted quasi-phonon energy, and accompanied by a finite quasi-phonon lifetime, which are reducible to classical results.more » A series of outstanding legacy issues including those above can be directly explained within this unified phonon renormalization approach. For instance, a renormalized phonon naturally resolves the decade-long debate between dynamic and static dislocation–phonon scattering approaches, as two limiting cases. In particular, at nanoscale, both the dynamic and static approaches break down, while the present renormalization approach remains valid by capturing the size effect, showing good agreement with lattice dynamics simulations.« less

  7. Raman-noise-induced noise-figure limit for chi (3) parametric amplifiers

    NASA Astrophysics Data System (ADS)

    Voss, Paul L.; Kumar, Prem

    2004-03-01

    The nonzero response time of the Kerr [chi (3)] nonlinearity determines the quantum-limited noise figure of c3 parametric amplifiers. This nonzero response time of the nonlinearity requires coupling of the parametric amplification process to a molecular-vibration phonon bath, causing the addition of excess noise through Raman gain or loss at temperatures above 0 K. The effect of this excess noise on the noise figure can be surprisingly significant. We derive analytical expressions for this quantum-limited noise figure for phase-insensitive operation of a chi (3) amplifier and show good agreement with published noise-figure measurements.

  8. Surface phononic graphene

    NASA Astrophysics Data System (ADS)

    Yu, Si-Yuan; Sun, Xiao-Chen; Ni, Xu; Wang, Qing; Yan, Xue-Jun; He, Cheng; Liu, Xiao-Ping; Feng, Liang; Lu, Ming-Hui; Chen, Yan-Feng

    2016-12-01

    Strategic manipulation of wave and particle transport in various media is the key driving force for modern information processing and communication. In a strongly scattering medium, waves and particles exhibit versatile transport characteristics such as localization, tunnelling with exponential decay, ballistic, and diffusion behaviours due to dynamical multiple scattering from strong scatters or impurities. Recent investigations of graphene have offered a unique approach, from a quantum point of view, to design the dispersion of electrons on demand, enabling relativistic massless Dirac quasiparticles, and thus inducing low-loss transport either ballistically or diffusively. Here, we report an experimental demonstration of an artificial phononic graphene tailored for surface phonons on a LiNbO3 integrated platform. The system exhibits Dirac quasiparticle-like transport, that is, pseudo-diffusion at the Dirac point, which gives rise to a thickness-independent temporal beating for transmitted pulses, an analogue of Zitterbewegung effects. The demonstrated fully integrated artificial phononic graphene platform here constitutes a step towards on-chip quantum simulators of graphene and unique monolithic electro-acoustic integrated circuits.

  9. Femtosecond coherent nuclear dynamics of excited tetraphenylethylene: Ultrafast transient absorption and ultrafast Raman loss spectroscopic studies

    NASA Astrophysics Data System (ADS)

    Kayal, Surajit; Roy, Khokan; Umapathy, Siva

    2018-01-01

    Ultrafast torsional dynamics plays an important role in the photoinduced excited state dynamics. Tetraphenylethylene (TPE), a model system for the molecular motor, executes interesting torsional dynamics upon photoexcitation. The photoreaction of TPE involves ultrafast internal conversion via a nearly planar intermediate state (relaxed state) that further leads to a twisted zwitterionic state. Here, we report the photoinduced structural dynamics of excited TPE during the course of photoisomerization in the condensed phase by ultrafast Raman loss (URLS) and femtosecond transient absorption (TA) spectroscopy. TA measurements on the S1 state reveal step-wise population relaxation from the Franck-Condon (FC) state → relaxed state → twisted state, while the URLS study provides insights on the vibrational dynamics during the course of the reaction. The TA spectral dynamics and vibrational Raman amplitudes within 1 ps reveal vibrational wave packet propagating from the FC state to the relaxed state. Fourier transformation of this oscillation leads to a ˜130 cm-1 low-frequency phenyl torsional mode. Two vibrational marker bands, Cet=Cet stretching (˜1512 cm-1) and Cph=Cph stretching (˜1584 cm-1) modes, appear immediately after photoexcitation in the URLS spectra. The initial red-shift of the Cph=Cph stretching mode with a time constant of ˜400 fs (in butyronitrile) is assigned to the rate of planarization of excited TPE. In addition, the Cet=Cet stretching mode shows initial blue-shift within 1 ps followed by frequency red-shift, suggesting that on the sub-picosecond time scale, structural relaxation is dominated by phenyl torsion rather than the central Cet=Cet twist. Furthermore, the effect of the solvent on the structural dynamics is discussed in the context of ultrafast nuclear dynamics and solute-solvent coupling.

  10. Femtosecond coherent nuclear dynamics of excited tetraphenylethylene: Ultrafast transient absorption and ultrafast Raman loss spectroscopic studies.

    PubMed

    Kayal, Surajit; Roy, Khokan; Umapathy, Siva

    2018-01-14

    Ultrafast torsional dynamics plays an important role in the photoinduced excited state dynamics. Tetraphenylethylene (TPE), a model system for the molecular motor, executes interesting torsional dynamics upon photoexcitation. The photoreaction of TPE involves ultrafast internal conversion via a nearly planar intermediate state (relaxed state) that further leads to a twisted zwitterionic state. Here, we report the photoinduced structural dynamics of excited TPE during the course of photoisomerization in the condensed phase by ultrafast Raman loss (URLS) and femtosecond transient absorption (TA) spectroscopy. TA measurements on the S 1 state reveal step-wise population relaxation from the Franck-Condon (FC) state → relaxed state → twisted state, while the URLS study provides insights on the vibrational dynamics during the course of the reaction. The TA spectral dynamics and vibrational Raman amplitudes within 1 ps reveal vibrational wave packet propagating from the FC state to the relaxed state. Fourier transformation of this oscillation leads to a ∼130 cm -1 low-frequency phenyl torsional mode. Two vibrational marker bands, C et =C et stretching (∼1512 cm -1 ) and C ph =C ph stretching (∼1584 cm -1 ) modes, appear immediately after photoexcitation in the URLS spectra. The initial red-shift of the C ph =C ph stretching mode with a time constant of ∼400 fs (in butyronitrile) is assigned to the rate of planarization of excited TPE. In addition, the C et =C et stretching mode shows initial blue-shift within 1 ps followed by frequency red-shift, suggesting that on the sub-picosecond time scale, structural relaxation is dominated by phenyl torsion rather than the central C et =C et twist. Furthermore, the effect of the solvent on the structural dynamics is discussed in the context of ultrafast nuclear dynamics and solute-solvent coupling.

  11. Spectroscopic (FT-IR, FT-Raman, UV absorption, 1H and 13C NMR) and theoretical (in B3LYP/6-311++G** level) studies on alkali metal salts of caffeic acid.

    PubMed

    Świsłocka, Renata

    2013-01-01

    The effect of some metals on the electronic system of benzoic and nicotinic acids has recently been investigated by IR, Raman and UV spectroscopy [1-3]. Benzoic and nicotinic acids are regarded model systems representing a wide group of aromatic ligands which are incorporated into enzymes. In this work the FT-IR (in solid state and in solution), FT-Raman, UV absorption and (1)H and (13)C NMR spectra of caffeic acid (3,4-dihydroxycinnamic acid) and its salts with lithium, sodium, potassium, rubidium and caesium were registered, assigned and analyzed. The effect of alkali metals on the electronic system of ligands was discussed. Studies of differences in the number and position of bands from the IR, Raman, UV absorption spectra and chemical shifts from NMR spectra allowed to conclude on the distribution of electronic charge in the molecules, the delocalization energy of π electrons and the reactivity of ligands in metal complexes. Optimized geometrical structures of studied compounds were calculated by B3LYP method using 6-311++G** basis set. Bond lengths, angles and dipole moments for the optimized structures of caffeic acid and lithium, sodium, potassium caffeinates were also calculated. The theoretical wavenumbers and intensities of IR spectra were obtained. The calculated parameters were compared to the experimental characteristics of investigated compounds. Microbial activity of studied compounds was tested against Escherichia coli, Pseudomonas aeruginosa, Staphylococcus aureus and Proteus vulgaris. Copyright © 2012 Elsevier B.V. All rights reserved.

  12. Micro-Raman scattering and dielectric investigations of phase transitions behavior in the PbHf0.7Sn0.3O3 single crystal

    NASA Astrophysics Data System (ADS)

    Jankowska-Sumara, Irena; Ko, Jae-Hyeon; Podgórna, Maria; Oh, Soo Han; Majchrowski, Andrzej

    2017-09-01

    Raman light scattering was used to detect the sequence of transitions in a PbHf1-xSnxO3 (PHS) single crystal with x = 0.30 in a temperature range of 77-873 K. Changes of Raman spectra were observed in the vicinity of structural phase transitions: between the antiferroelectric (AFE1)-antiferroelectric (AFE2)—intermediate—paraelectric phases. Light scattering and dielectric investigations were used to find out the nature and sequence of the phase transition, as well as the large dielectric permittivity values measured at the phase transition, by searching for the soft-phonon-mode behavior. The experimentally recorded spectra were analyzed in terms of the damped-harmonic oscillator model for the phonon bands. It is demonstrated that the structural phase transformations in PHS can be considered as the result of softening of many modes, not only the ferroelectric one. It was also proved that locally broken symmetry effects are present at temperatures far above the Curie temperature and are connected with the softening of two optic modes of different nature.

  13. Implementation of an Analytical Raman Scattering Correction for Satellite Ocean-Color Processing

    NASA Technical Reports Server (NTRS)

    McKinna, Lachlan I. W.; Werdell, P. Jeremy; Proctor, Christopher W.

    2016-01-01

    Raman scattering of photons by seawater molecules is an inelastic scattering process. This effect can contribute significantly to the water-leaving radiance signal observed by space-borne ocean-color spectroradiometers. If not accounted for during ocean-color processing, Raman scattering can cause biases in derived inherent optical properties (IOPs). Here we describe a Raman scattering correction (RSC) algorithm that has been integrated within NASA's standard ocean-color processing software. We tested the RSC with NASA's Generalized Inherent Optical Properties algorithm (GIOP). A comparison between derived IOPs and in situ data revealed that the magnitude of the derived backscattering coefficient and the phytoplankton absorption coefficient were reduced when the RSC was applied, whilst the absorption coefficient of colored dissolved and detrital matter remained unchanged. Importantly, our results show that the RSC did not degrade the retrieval skill of the GIOP. In addition, a timeseries study of oligotrophic waters near Bermuda showed that the RSC did not introduce unwanted temporal trends or artifacts into derived IOPs.

  14. Order and disorder and their influences on optical absorption of glasses in the gap region

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Baník, Ivan, E-mail: ivan.banik@stuba.sk; Kubliha, Marian, E-mail: marian.kubliha@stuba.sk; Lukovičová, Jozefa, E-mail: jozefa.lukovicova@stuba.sk

    2016-07-07

    The exponential increase of the absorption coefficient near the absorption edge is usually explained by existence of the density-of-states tails. Among the quoted theoretical models which are widely used to explain the manifestations of the Urbach rule in semiconductors, are the Sumi–Toyozava and the Dow–Redfield models and ab initio (from beginning) theory. Our barrier-cluster-heating model assumes the different creating mechanism of exponential tails. The energy by optical transition is provided to electrons except from photons also from vibration of microregion. It deals about the replenishment of absented photons energy, which is smaller as gap width. Absented energy needed for themore » transition by light absorption is accumulated in certain microregions of material in the form of vibrational energy. At absorption sufficiently big package of accumulated energy can be used. Energy of emptied microarea is filled by phonons from surrounding of microarea (as result of temperature status of surrounding), resp. phonons of optical background which are created in given microarea at non radiative recombination of carriers. In this work simplified process at derivating of Urbach rule is listed.« less

  15. Raman spectroscopic study of plasma-treated salmon DNA

    NASA Astrophysics Data System (ADS)

    Joon Lee, Geon; Kwon, Young-Wan; Hee Kim, Yong; Ha Choi, Eun

    2013-01-01

    In this research, we studied the effect of plasma treatment on the optical/structural properties of the deoxyribonucleic acid (DNA) extracted from salmon sperm. DNA-cetyltrimethylammonium (CTMA) films were obtained by complexation of DNA with CTMA. Circular dichroism (CD) and Raman spectra indicated that DNA retained its double helical structure in the solid film. The Raman spectra exhibited several vibration modes corresponding to the nuclear bases and the deoxyribose-phosphate backbones of the DNA, as well as the alkylchains of CTMA. Dielectric-barrier-discharge (DBD) plasma treatment induced structural modification and damage to the DNA, as observed by changes in the ultraviolet-visible absorption, CD, and Raman spectra. The optical emission spectra of the DBD plasma confirmed that DNA modification was induced by plasma ions such as reactive oxygen species and reactive nitrogen species.

  16. Surface induced phonon decay rates in thin film nano-structures

    NASA Astrophysics Data System (ADS)

    Photiadis, D. M.

    2007-12-01

    Nano-scale structure significantly impacts phonon transport and related phonon relaxation rates, with order of magnitude effects on the thermal conductivity of dielectric thin films and quantum wires, and even larger effects on the lifetimes of ultrasonic phonons of micro- (nano-) oscillators. In both cases, efforts to explain the data have been hampered by our lack of knowledge of the effects of confined dimensionality on phonon-phonon scattering rates. Using a phonon Boltzmann equation with appropriate boundary conditions on the free surfaces to take surface roughness into account, we have obtained an expression yielding phonon lifetimes in 2-D dielectric nanostructures(thin films) resulting from phonon-phonon scattering in conjunction with phonon-surface scattering. We present these theoretical results and, in the limit in which surface induced losses dominate, obtain explicit predictions for the phonon lifetimes. The predicted temperature dependence of the ultrason! ic loss does not explain the observed saturation of the loss at low temperatures(τ(T) → const), but does give results of the order of magnitude of measured ultrasonic lifetimes.

  17. Phonon optimized interatomic potential for aluminum

    NASA Astrophysics Data System (ADS)

    Muraleedharan, Murali Gopal; Rohskopf, Andrew; Yang, Vigor; Henry, Asegun

    2017-12-01

    We address the problem of generating a phonon optimized interatomic potential (POP) for aluminum. The POP methodology, which has already been shown to work for semiconductors such as silicon and germanium, uses an evolutionary strategy based on a genetic algorithm (GA) to optimize the free parameters in an empirical interatomic potential (EIP). For aluminum, we used the Vashishta functional form. The training data set was generated ab initio, consisting of forces, energy vs. volume, stresses, and harmonic and cubic force constants obtained from density functional theory (DFT) calculations. Existing potentials for aluminum, such as the embedded atom method (EAM) and charge-optimized many-body (COMB3) potential, show larger errors when the EIP forces are compared with those predicted by DFT, and thus they are not particularly well suited for reproducing phonon properties. Using a comprehensive Vashishta functional form, which involves short and long-ranged interactions, as well as three-body terms, we were able to better capture interactions that reproduce phonon properties accurately. Furthermore, the Vashishta potential is flexible enough to be extended to Al2O3 and the interface between Al-Al2O3, which is technologically important for combustion of solid Al nano powders. The POP developed here is tested for accuracy by comparing phonon thermal conductivity accumulation plots, density of states, and dispersion relations with DFT results. It is shown to perform well in molecular dynamics (MD) simulations as well, where the phonon thermal conductivity is calculated via the Green-Kubo relation. The results are within 10% of the values obtained by solving the Boltzmann transport equation (BTE), employing Fermi's Golden Rule to predict the phonon-phonon relaxation times.

  18. Phonon-mediated nuclear spin relaxation in H2O

    NASA Astrophysics Data System (ADS)

    Yamakawa, Koichiro; Azami, Shinya; Arakawa, Ichiro

    2017-03-01

    A theoretical model of the phonon-mediated nuclear spin relaxation in H2O trapped by cryomatrices has been established for the first time. In order to test the validity of this model, we measured infrared spectra of H2O trapped in solid Ar, which showed absorption peaks due to rovibrational transitions of ortho- and para-H2O in the spectral region of the bending vibration. We monitored the time evolution of the spectra and analyzed the rotational relaxation associated with the nuclear spin flip to obtain the relaxation rates of H2O at temperatures of 5-15 K. Temperature dependence of the rate is discussed in terms of the devised model.

  19. Magnetic and low temperature phonon studies of CoCr2O4 powders doped with Fe(III) and Ni(II) ions

    NASA Astrophysics Data System (ADS)

    Ptak, M.; Mączka, M.; Pikul, A.; Tomaszewski, P. E.; Hanuza, J.

    2014-04-01

    Extensive temperature-dependent phonon studies and low-temperature magnetic measurements of CoCr2-xFexO4 (for x=0.5, 1 and 2) and Co0.9Ni0.1Cr2O4 polycrystalline powders are presented. The main aim of these studies was to obtain information on phonon and structural properties of these compounds as well as strength of spin-phonon coupling in the magnetically ordered phases. IR and Raman spectra show that doping of CoCr2O4 with Fe(III) ions leads to broadening of bands and appearance of new bands due to the formation of inverted spinel structure. In contrast to this behavior, doping with 10 mol% of Ni(II) ions leads to weak increase of band width only. Magnetization measured as a function of temperature and external magnetic field showed that magnetic properties of Co0.9Ni0.1Cr2O4 sample are similar to those reported for pure CoCr2O4, i.e., partial substitution of Ni(II) for Co(II) leads to slight shift of the ferrimagnetic phase transition at TC and spiral spin order transition at TS towards lower values. The change of crystallization preference induced by incorporation of increasing concentration of Fe(III) ions in the spinel lattice causes significant increase of TC and decrease of TS. The latter transition disappears completely for higher concentrations of Fe(III). The performed temperature-dependent IR studies revealed interesting anomalous behavior of phonons below TC for CoCr1.5Fe0.5O4 and Co0.9Ni0.1Cr2O4, which was attributed to spin-phonon coupling.

  20. Bilayer graphene phonovoltaic-FET: In situ phonon recycling

    NASA Astrophysics Data System (ADS)

    Melnick, Corey; Kaviany, Massoud

    2017-11-01

    A new heat harvester, the phonovoltaic (pV) cell, was recently proposed. The device converts optical phonons into power before they become heat. Due to the low entropy of a typical hot optical phonon population, the phonovoltaic can operate at high fractions of the Carnot limit and harvest heat more efficiently than conventional heat harvesting technologies such as the thermoelectric generator. Previously, the optical phonon source was presumed to produce optical phonons with a single polarization and momentum. Here, we examine a realistic optical phonon source in a potential pV application and the effects this has on pV operation. Supplementing this work is our investigation of bilayer graphene as a new pV material. Our ab initio calculations show that bilayer graphene has a figure of merit exceeding 0.9, well above previously investigated materials. This allows a room-temperature pV to recycle 65% of a highly nonequilibrium, minimum entropy population of phonons. However, full-band Monte Carlo simulations of the electron and phonon dynamics in a bilayer graphene field-effect transistor (FET) show that the optical phonons emitted by field-accelerated electrons can only be recycled in situ with an efficiency of 50%, and this efficiency falls as the field strength grows. Still, an appropriately designed FET-pV can recycle the phonons produced therein in situ with a much higher efficiency than a thermoelectric generator can harvest heat produced by a FET ex situ.

  1. Specularity of longitudinal acoustic phonons at rough surfaces

    NASA Astrophysics Data System (ADS)

    Gelda, Dhruv; Ghossoub, Marc G.; Valavala, Krishna; Ma, Jun; Rajagopal, Manjunath C.; Sinha, Sanjiv

    2018-01-01

    The specularity of phonons at crystal surfaces is of direct importance to thermal transport in nanostructures and to dissipation in nanomechanical resonators. Wave scattering theory provides a framework for estimating wavelength-dependent specularity, but experimental validation remains elusive. Widely available thermal conductivity data presents poor validation since the involvement of the infinitude of phonon wavelengths in thermal transport presents an underconstrained test for specularity theory. Here, we report phonon specularity by measuring the lifetimes of individual coherent longitudinal acoustic phonon modes excited in ultrathin (36-205 nm) suspended silicon membranes at room temperature over the frequency range ˜20 -118 GHz. Phonon surface scattering dominates intrinsic Akhiezer damping at frequencies ≳60 GHz, enabling measurements of phonon boundary scattering time over wavelengths ˜72 -140 nm . We obtain detailed statistics of the surface roughness at the top and bottom surfaces of membranes using HRTEM imaging. We find that the specularity of the excited modes are in good agreement with solutions of wave scattering only when the TEM statistics are corrected for projection errors. The often-cited Ziman formula for phonon specularity also appears in good agreement with the data, contradicting previous results. This work helps to advance the fundamental understanding of phonon scattering at the surfaces of nanostructures.

  2. Electron-Mediated Phonon-Phonon Coupling Drives the Vibrational Relaxation of CO on Cu(100)

    NASA Astrophysics Data System (ADS)

    Novko, D.; Alducin, M.; Juaristi, J. I.

    2018-04-01

    We bring forth a consistent theory for the electron-mediated vibrational intermode coupling that clarifies the microscopic mechanism behind the vibrational relaxation of adsorbates on metal surfaces. Our analysis points out the inability of state-of-the-art nonadiabatic theories to quantitatively reproduce the experimental linewidth of the CO internal stretch mode on Cu(100) and it emphasizes the crucial role of the electron-mediated phonon-phonon coupling in this regard. The results demonstrate a strong electron-mediated coupling between the internal stretch and low-energy CO modes, but also a significant role of surface motion. Our nonadiabatic theory is also able to explain the temperature dependence of the internal stretch phonon linewidth, thus far considered a sign of the direct anharmonic coupling.

  3. Re-induced Raman active modes in HgBa2Can-1CunO2n+2+δ compounds

    NASA Astrophysics Data System (ADS)

    Poulakis, N.; Lampakis, D.; Liarokapis, E.; Yoshikawa, Akira; Shimoyama, Jun-Ich; Kishio, Kohji; Peacock, G. B.; Hodges, J. P.; Gameson, I.; Edwards, P. P.; Panagopoulos, C.

    1999-08-01

    A comparative Raman study of Re-free and Re-doped HgBa2Can-1CunO2n+2+δ with n=1,3,4,5 is presented in an attempt to further clarify the structural and phononic modifications brought about by Re substitution. A number of extra high-frequency phonon peaks show up in the spectra of the Re-doped samples and are attributed to the oxygen modes of a strongly bound, almost decoupled ReO6 octahedron. As regards the apex oxygen in the Hg site, a clear transfer of spectral weight from the 590 to the 570 cm-1 apex phonon band is observed upon Re substitution. Such a change may well be accounted for assuming increased excess oxygen content for the Re-doped samples. Another interesting result is the enhancement upon Re doping of a narrow peak probably attributed to c-axis vibrations of Ba whose frequency shows a distinctive change with the number n of the CuO2 layers, providing an easy way to identify the various phases in a sample.

  4. Electron-phonon superconductivity in YIn3

    NASA Astrophysics Data System (ADS)

    Billington, D.; Llewellyn-Jones, T. M.; Maroso, G.; Dugdale, S. B.

    2013-08-01

    First-principles calculations of the electron-phonon coupling were performed on the cubic intermetallic compound YIn3. The electron-phonon coupling constant was found to be λep = 0.42. Using the Allen-Dynes formula with a Coulomb pseudopotential of μ* = 0.10, a Tc of approximately 0.77 K is obtained which is reasonably consistent with the experimentally observed temperature (between 0.8 and 1.1 K). The results indicate that conventional electron-phonon coupling is capable of producing the superconductivity in this compound.

  5. Plasphonics: local hybridization of plasmons and phonons.

    PubMed

    Marty, Renaud; Mlayah, Adnen; Arbouet, Arnaud; Girard, Christian; Tripathy, Sudhiranjan

    2013-02-25

    We show that the interaction between localized surface plasmons sustained by a metallic nano-antenna and delocalized phonons lying at the surface of an heteropolar semiconductor can generate a new class of hybrid electromagnetic modes. These plasphonic modes are investigated using an analytical model completed by accurate Green dyadic numerical simulations. When surface plasmon and surface phonon frequencies match, the optical resonances exhibit a large Rabi splitting typical of strongly interacting two-level systems. Based on numerical simulations of the electric near-field maps, we investigate the nature of the plaphonic excitations. In particular, we point out a strong local field enhancement boosted by the phononic surface. This effect is interpreted in terms of light harvesting by the plasmonic antenna from the phononic surface. We thus introduce the concept of active phononic surfaces that may be exploited for far-infared optoelectronic devices and sensors.

  6. Study of nonlinear absorption properties of reduced graphene oxide by Z-scan technique

    NASA Astrophysics Data System (ADS)

    Sreeja, V. G.; Vinitha, G.; Reshmi, R.; Anila, E. I.; Jayaraj, M. K.

    2017-05-01

    Graphene has generated enormous research interest during the last decade due to its significant unique properties and wide applications in the field of optoelectronics and photonics. This research studied the structural and nonlinear absorption properties of reduced graphene oxide (rGO) synthesized by Modified Hummer's method. Structural and physiochemical properties of the rGO were explored with the help of Fourier transform infrared spectroscopy (FTIR) and Raman spectroscopy (Raman). Nonlinear absorption property in rGO, was investigated by open aperture Z-scan technique by using a continuous wave (CW) laser. The Z-scan results demonstrate saturable absorption property of rGO with a nonlinear absorption coefficient, β, of -2.62 × 10-4 cm/W, making it suitable for applications in Q switching, generation of ultra-fast high energy pulses in laser cavity and mode lockers.

  7. Electronic Raman scattering as an ultra-sensitive probe of strain effects in semiconductors.

    PubMed

    Fluegel, Brian; Mialitsin, Aleksej V; Beaton, Daniel A; Reno, John L; Mascarenhas, Angelo

    2015-05-28

    Semiconductor strain engineering has become a critical feature of high-performance electronics because of the significant device performance enhancements that it enables. These improvements, which emerge from strain-induced modifications to the electronic band structure, necessitate new ultra-sensitive tools to probe the strain in semiconductors. Here, we demonstrate that minute amounts of strain in thin semiconductor epilayers can be measured using electronic Raman scattering. We applied this strain measurement technique to two different semiconductor alloy systems using coherently strained epitaxial thin films specifically designed to produce lattice-mismatch strains as small as 10(-4). Comparing our strain sensitivity and signal strength in Al(x)Ga(1-x)As with those obtained using the industry-standard technique of phonon Raman scattering, we found that there was a sensitivity improvement of 200-fold and a signal enhancement of 4 × 10(3), thus obviating key constraints in semiconductor strain metrology.

  8. Electronic Raman scattering as an ultra-sensitive probe of strain effects in semiconductors

    PubMed Central

    Fluegel, Brian; Mialitsin, Aleksej V.; Beaton, Daniel A.; Reno, John L.; Mascarenhas, Angelo

    2015-01-01

    Semiconductor strain engineering has become a critical feature of high-performance electronics because of the significant device performance enhancements that it enables. These improvements, which emerge from strain-induced modifications to the electronic band structure, necessitate new ultra-sensitive tools to probe the strain in semiconductors. Here, we demonstrate that minute amounts of strain in thin semiconductor epilayers can be measured using electronic Raman scattering. We applied this strain measurement technique to two different semiconductor alloy systems using coherently strained epitaxial thin films specifically designed to produce lattice-mismatch strains as small as 10−4. Comparing our strain sensitivity and signal strength in AlxGa1−xAs with those obtained using the industry-standard technique of phonon Raman scattering, we found that there was a sensitivity improvement of 200-fold and a signal enhancement of 4 × 103, thus obviating key constraints in semiconductor strain metrology. PMID:26017853

  9. Temperature Dependence of Phonons in Pyrolitic Graphite

    DOE R&D Accomplishments Database

    Brockhouse, B. N.; Shirane, G.

    1977-01-01

    Dispersion curves for longitudinal and transverse phonons propagating along and near the c-axis in pyrolitic graphite at temperatures between 4?K and 1500?C have been measured by neutron spectroscopy. The observed frequencies decrease markedly with increasing temperature (except for the transverse optical ''rippling'' modes in the hexagonal planes). The neutron groups show interesting asymmetrical broadening ascribed to interference between one phonon and many phonon processes.

  10. Anomalous vibrational modes in few layer WTe 2 revealed by polarized Raman scattering and first-principles calculations

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Cao, Yan; Sheremetyeva, Natalya; Liang, Liangbo

    When layered transition-metal dichalcogenides (TMDs) are scaled down from a three- to a two-dimensional geometry, electronic and structural transitions occur, leading to the emergence of properties not usually found in the bulk. Here, we report a systematic Raman study of exfoliated semi-metallic WTe 2 flakes with thickness ranging from few layers down to a single layer. A dramatic change in the Raman spectra occurs between the monolayer and few-layer WTe 2 as a vibrational mode centered at ~86.9 cm -1 in the monolayer splits into two active modes at 82.9 and 89.6 cm -1 in the bilayer. Davydov splitting ofmore » these two modes is found in the bilayer, as further evidenced by polarized Raman measurements. Strong angular dependence of Raman modes on the WTe 2 film thickness reflects that the existence of directional interlayer interaction, rather than isotropic van der Waals (vdw) coupling, is playing an essential role affecting the phonon modes, especially in anisotropic 2D WTe 2 material. Therefore, the strong evolution of Raman modes with thickness and polarization direction, can not only be a reliable fingerprint for the determination of the thickness and the crystallographic orientation, but can also be an ideal probe for such strong and directional interlayer interaction.« less

  11. Graphitic carbon nanospheres: A Raman spectroscopic investigation of thermal conductivity and morphological evolution by pulsed laser irradiation

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Agarwal, Radhe; Sahoo, Satyaprakash, E-mail: satya504@gmail.com, E-mail: rkatiyar@hpcf.upr.edu; Chitturi, Venkateswara Rao

    2015-12-07

    Graphitic carbon nanospheres (GCNSs) were prepared by a unique acidic treatment of multi-walled nanotubes. Spherical morphology with a narrow size distribution was confirmed by transmission electron microscopy studies. The room temperature Raman spectra showed a clear signature of D- and G-peaks at around 1350 and 1591 cm{sup −1}, respectively. Temperature dependent Raman scattering measurements were performed to understand the phonon dynamics and first order temperature coefficients related to the D- and G-peaks. The temperature dependent Raman spectra in a range of 83–473 K were analysed, where the D-peak was observed to show a red-shift with increasing temperature. The relative intensity ratio ofmore » D- to G-peaks also showed a significant rise with increasing temperature. Such a temperature dependent behaviour can be attributed to lengthening of the C-C bond due to thermal expansion in material. The estimated value of the thermal conductivity of GCNSs ∼0.97 W m{sup −1} K{sup −1} was calculated using Raman spectroscopy. In addition, the effect of pulsed laser treatment on the GCNSs was demonstrated by analyzing the Raman spectra of post irradiated samples.« less

  12. Anomalous vibrational modes in few layer WTe 2 revealed by polarized Raman scattering and first-principles calculations

    DOE PAGES

    Cao, Yan; Sheremetyeva, Natalya; Liang, Liangbo; ...

    2017-08-02

    When layered transition-metal dichalcogenides (TMDs) are scaled down from a three- to a two-dimensional geometry, electronic and structural transitions occur, leading to the emergence of properties not usually found in the bulk. Here, we report a systematic Raman study of exfoliated semi-metallic WTe 2 flakes with thickness ranging from few layers down to a single layer. A dramatic change in the Raman spectra occurs between the monolayer and few-layer WTe 2 as a vibrational mode centered at ~86.9 cm -1 in the monolayer splits into two active modes at 82.9 and 89.6 cm -1 in the bilayer. Davydov splitting ofmore » these two modes is found in the bilayer, as further evidenced by polarized Raman measurements. Strong angular dependence of Raman modes on the WTe 2 film thickness reflects that the existence of directional interlayer interaction, rather than isotropic van der Waals (vdw) coupling, is playing an essential role affecting the phonon modes, especially in anisotropic 2D WTe 2 material. Therefore, the strong evolution of Raman modes with thickness and polarization direction, can not only be a reliable fingerprint for the determination of the thickness and the crystallographic orientation, but can also be an ideal probe for such strong and directional interlayer interaction.« less

  13. Phonon Recycling for Ultrasensitive Kinetic Inductance Detectors

    NASA Astrophysics Data System (ADS)

    Zmuidzinas, Jonas

    Initially proposed (Day et al. 2003; Zmuidzinas 2012) in 1999 by our Caltech/JPL group, and thanks to strong support from NASA, the superconducting (microwave) kinetic inductance detector (MKID or KID) technology continues to develop rapidly as it transitions into applications. The development effort worldwide is intensifying and NASA's continued support of KID development is essential in order to keep pace. Here we propose to investigate and demonstrate a new, low-TRL concept, which we call phonon recycling, that promises to open broad new avenues in KID design and performance. Briefly, phonon recycling allows the detector designer to tailor the responsivity and sensitivity of a KID to match the needs of the application by using geometry to restrict the rate at which recombination phonons are allowed to escape from the detector. In particular, phonon recycling should allow very low noise-equivalent power (NEP) to be achieved without requiring very low operating tem- peratures. Phonon recycling is analogous to the use of micromachined suspension legs to control the flow of heat in a bolometer, as measured by the thermal conductivity G. However, phonon recycling exploits the non-thermal distribution of recombination phonons as well as their very slow decay in crystals at low temperatures. These properties translate to geometrical and mechanical requirements for a phonon-recycled KID that are considerably more relaxed than for a bolometer operating at the same temperature and NEP. Our ultimate goal is to develop detector arrays suitable for a far-infrared (FIR) space mission, which will impose strict requirements on the array sensitivity, yield, uniformity, multiplexing density, etc. Through previous NASA support under the Strategic Astrophysics Technology (SAT) program, we have successfully demonstrated the MAKO submillimeter camera at the Caltech Submillimeter Observatory and have become familiar with these practical issues. If our demonstration of phonon recycling

  14. Phonon localization transition in relaxor ferroelectric PZN-5%PT

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Manley, Michael E.; Christianson, Andrew D.; Abernathy, Douglas L.

    Relaxor ferroelectric behavior occurs in many disordered ferroelectric materials but is not well understood at the atomic level. Recent experiments and theoretical arguments indicate that Anderson localization of phonons instigates relaxor behavior by driving the formation of polar nanoregions (PNRs). Here, we use inelastic neutron scattering to observe phonon localization in relaxor ferroelectric PZN-5%PT (0.95[Pb(Zn 1/3 Nb 2/3)O 3]–0.05PbTiO 3) and detect additional features of the localization process. In the lead, up to phonon localization on cooling, the local resonant modes that drive phonon localization increase in number. The increase in resonant scattering centers is attributed to a known increasemore » in the number of locally off centered Pb atoms on cooling. The transition to phonon localization occurs when these random scattering centers increase to a concentration where the Ioffe-Regel criterion is satisfied for localizing the phonon. Finally, we also model the effects of damped mode coupling on the observed phonons and phonon localization structure.« less

  15. Phonon localization transition in relaxor ferroelectric PZN-5%PT

    DOE PAGES

    Manley, Michael E.; Christianson, Andrew D.; Abernathy, Douglas L.; ...

    2017-03-27

    Relaxor ferroelectric behavior occurs in many disordered ferroelectric materials but is not well understood at the atomic level. Recent experiments and theoretical arguments indicate that Anderson localization of phonons instigates relaxor behavior by driving the formation of polar nanoregions (PNRs). Here, we use inelastic neutron scattering to observe phonon localization in relaxor ferroelectric PZN-5%PT (0.95[Pb(Zn 1/3 Nb 2/3)O 3]–0.05PbTiO 3) and detect additional features of the localization process. In the lead, up to phonon localization on cooling, the local resonant modes that drive phonon localization increase in number. The increase in resonant scattering centers is attributed to a known increasemore » in the number of locally off centered Pb atoms on cooling. The transition to phonon localization occurs when these random scattering centers increase to a concentration where the Ioffe-Regel criterion is satisfied for localizing the phonon. Finally, we also model the effects of damped mode coupling on the observed phonons and phonon localization structure.« less

  16. Optical Absorption and Emission Mechanisms of Single Defects in Hexagonal Boron Nitride

    NASA Astrophysics Data System (ADS)

    Jungwirth, Nicholas R.; Fuchs, Gregory D.

    2017-08-01

    We investigate the polarization selection rules of sharp zero-phonon lines (ZPLs) from isolated defects in hexagonal boron nitride (HBN) and compare our findings with the predictions of a Huang-Rhys model involving two electronic states. Our survey, which spans the spectral range ˜550 - 740 nm , reveals that, in disagreement with a two-level model, the absorption and emission dipoles are often misaligned. We relate the dipole misalignment angle (Δ θ ) of a ZPL to its energy shift from the excitation energy (Δ E ) and find that Δ θ ≈0 ° when Δ E corresponds to an allowed HBN phonon frequency and that 0 ° ≤Δ θ ≤90 ° when Δ E exceeds the maximum allowed HBN phonon frequency. Consequently, a two-level Huang-Rhys model succeeds at describing excitations mediated by the creation of one optical phonon but fails at describing excitations that require the creation of multiple phonons. We propose that direct excitations requiring the creation of multiple phonons are inefficient due to the low Huang-Rhys factors in HBN and that these ZPLs are instead excited indirectly via an intermediate electronic state. This hypothesis is corroborated by polarization measurements of an individual ZPL excited with two distinct wavelengths that indicate a single ZPL may be excited by multiple mechanisms. These findings provide new insight on the nature of the optical cycle of novel defect-based single-photon sources in HBN.

  17. Magneto-optical far-infrared absorption spectroscopy of the hole states of indium phosphide

    NASA Astrophysics Data System (ADS)

    Lewis, R. A.; Wang, Y.-J.

    2005-03-01

    Far-infrared absorption spectroscopy in magnetic fields of up to 30 T of the zinc acceptor impurity in indium phosphide has revealed for the first time a series of free-hole transitions (Landau-related series) in addition to the familiar bound-hole transitions (Lyman series) as well as hitherto unobserved phonon replicas of both series. Analysis of these data permits the simultaneous direct experimental determination of (i) the hole effective mass, (ii) the species-specific binding energy of the acceptor impurity, (iii) the absolute energy levels of the acceptor excited states of both odd and even parity, (iv) more reliable, and in some cases the only, g factors for acceptor states, through relaxation of the selection rules for phonon replicas, and (v) the LO phonon energy. The method is applicable to other semiconductors and may lead to the reappraisal of their physical parameters.

  18. Nonequilibrium dynamics of the phonon gas in ultrafast-excited antimony

    NASA Astrophysics Data System (ADS)

    Krylow, Sergej; Zijlstra, Eeuwe S.; Kabeer, Fairoja Cheenicode; Zier, Tobias; Bauerhenne, Bernd; Garcia, Martin E.

    2017-12-01

    The ultrafast relaxation dynamics of a nonequilibrium phonon gas towards thermal equilibrium involves many-body collisions that cannot be properly described by perturbative approaches. Here, we develop a nonperturbative method to elucidate the microscopic mechanisms underlying the decay of laser-excited coherent phonons in the presence of electron-hole pairs, which so far are not fully understood. Our theory relies on ab initio molecular dynamics simulations on laser-excited potential-energy surfaces. Those simulations are compared with runs in which the laser-excited coherent phonon is artificially deoccupied. We apply this method to antimony and show that the decay of the A1 g phonon mode at low laser fluences can be accounted mainly to three-body down-conversion processes of an A1 g phonon into acoustic phonons. For higher excitation strengths, however, we see a crossover to a four-phonon process, in which two A1 g phonons decay into two optical phonons.

  19. Solid-state Raman frequency converters for CO2-DIAL systems at 1.6 μm

    NASA Astrophysics Data System (ADS)

    Rhee, Hanjo; Lisinetskii, Victor; Kaminskii, Alexander A.; Eichler, Hans-Joachim

    2009-09-01

    Measurement of the three-dimensional distribution of atmospheric trace gases, especially CO2, is an important factor to improve the accuracy of climate models and to understand the global effects of the greenhouse effect. This can be achieved by differential absorption Lidar (DIAL). The absorption spectrum of CO2 features several suitable absorption lines for a ground-based or air-borne DIAL system working at wavelengths between 1.57 μm and 1.61 μm. An appropriate laser transmitter must emit laser pulses with pulse energies of more than 10 mJ and pulse duration in the nanosecond range. For high spectral purity the bandwidth is required to be less than 60 MHz. OPOs and Er-doped solid-state lasers emit around 1.6 μm, but we describe here alternatively Nd:YAG and Nd:glass laser systems with Raman converters. The use of stimulated Raman scattering in crystalline and ceramic materials is a possibility to shift the wavelength of existing lasers depending on the size of the Raman shift. After the investigation of a large number of Raman-active materials some of them could be identified as promising candidates for the conversion of typical Nd:YAG emission wavelengths, including LiNH2C6H4SO3•H2O, Ba(NO3)2, Li2SO4•H2O, Y(HCOO)3•2H2O, β-BBO and diamond. Our experiments with Ba(NO3)2 showed that the choice of the material should not be restricted to those with an adequate first order Stokes Raman line position, but also second or third order Raman shift should be considered. Development of Raman frequency converters for high pulse energies concentrates on linear and folded resonator designs and seeded Raman amplifiers using the Raman material as a direct amplifier. With Ba(NO3)2 pulse energy up to 116 mJ and 42 % quantum efficiency at the third Stokes wavelength with 1599 nm has been demonstrated. High power operation at 5 W with compensation of thermal lensing was achieved.

  20. Engineering thermal conductance using a two-dimensional phononic crystal.

    PubMed

    Zen, Nobuyuki; Puurtinen, Tuomas A; Isotalo, Tero J; Chaudhuri, Saumyadip; Maasilta, Ilari J

    2014-03-19

    Controlling thermal transport has become relevant in recent years. Traditionally, this control has been achieved by tuning the scattering of phonons by including various types of scattering centres in the material (nanoparticles, impurities, etc). Here we take another approach and demonstrate that one can also use coherent band structure effects to control phonon thermal conductance, with the help of periodically nanostructured phononic crystals. We perform the experiments at low temperatures below 1 K, which not only leads to negligible bulk phonon scattering, but also increases the wavelength of the dominant thermal phonons by more than two orders of magnitude compared to room temperature. Thus, phononic crystals with lattice constants ≥1 μm are shown to strongly reduce the thermal conduction. The observed effect is in quantitative agreement with the theoretical calculation presented, which accurately determined the ballistic thermal conductance in a phononic crystal device.

  1. Phonon quarticity induced by changes in phonon-tracked hybridization during lattice expansion and its stabilization of rutile TiO 2

    DOE PAGES

    Lan, Tian; Li, Chen W.; Hellman, O.; ...

    2015-08-11

    Although the rutile structure of TiO 2 is stable at high temperatures, the conventional quasiharmonic approximation predicts that several acoustic phonons decrease anomalously to zero frequency with thermal expansion, incorrectly predicting a structural collapse at temperatures well below 1000 K. In this paper, inelastic neutron scattering was used to measure the temperature dependence of the phonon density of states (DOS) of rutile TiO 2 from 300 to 1373 K. Surprisingly, these anomalous acoustic phonons were found to increase in frequency with temperature. First-principles calculations showed that with lattice expansion, the potentials for the anomalous acoustic phonons transform from quadratic tomore » quartic, stabilizing the rutile phase at high temperatures. In these modes, the vibrational displacements of adjacent Ti and O atoms cause variations in hybridization of 3d electrons of Ti and 2p electrons of O atoms. Finally, with thermal expansion, the energy variation in this “phonon-tracked hybridization” flattens the bottom of the interatomic potential well between Ti and O atoms, and induces a quarticity in the phonon potential.« less

  2. Ultrafast switching of valence and generation of coherent acoustic phonons in semiconducting rare-earth monosulfides

    NASA Astrophysics Data System (ADS)

    Punpongjareorn, Napat; He, Xing; Tang, Zhongjia; Guloy, Arnold M.; Yang, Ding-Shyue

    2017-08-01

    We report on the ultrafast carrier dynamics and generation of coherent acoustic phonons in YbS, a semiconducting rare-earth monochalcogenide, using two-color pump-probe reflectivity. Compared to the carrier relaxation processes and lifetimes of conventional semiconductors, recombination of photoexcited electrons with holes in localized f orbitals is found to take place rapidly with a density-independent time constant of <500 fs in YbS. Such carrier annihilation signifies the unique and ultrafast nature of valence restoration of ytterbium ions after femtosecond photoexcitation switching. Following transfer of the absorbed energy to the lattice, coherent acoustic phonons emerge on the picosecond timescale as a result of the thermal strain in the photoexcited region. By analyzing the electronic and structural dynamics, we obtain the physical properties of YbS including its two-photon absorption and thermooptic coefficients, the period and decay time of the coherent oscillation, and the sound velocity.

  3. Ternary mixed crystal effects on interface optical phonon and electron-phonon coupling in zinc-blende GaN/AlxGa1-xN spherical quantum dots

    NASA Astrophysics Data System (ADS)

    Huang, Wen Deng; Chen, Guang De; Yuan, Zhao Lin; Yang, Chuang Hua; Ye, Hong Gang; Wu, Ye Long

    2016-02-01

    The theoretical investigations of the interface optical phonons, electron-phonon couplings and its ternary mixed effects in zinc-blende spherical quantum dots are obtained by using the dielectric continuum model and modified random-element isodisplacement model. The features of dispersion curves, electron-phonon coupling strengths, and its ternary mixed effects for interface optical phonons in a single zinc-blende GaN/AlxGa1-xN spherical quantum dot are calculated and discussed in detail. The numerical results show that there are three branches of interface optical phonons. One branch exists in low frequency region; another two branches exist in high frequency region. The interface optical phonons with small quantum number l have more important contributions to the electron-phonon interactions. It is also found that ternary mixed effects have important influences on the interface optical phonon properties in a single zinc-blende GaN/AlxGa1-xN quantum dot. With the increase of Al component, the interface optical phonon frequencies appear linear changes, and the electron-phonon coupling strengths appear non-linear changes in high frequency region. But in low frequency region, the frequencies appear non-linear changes, and the electron-phonon coupling strengths appear linear changes.

  4. Pressure-enabled phonon engineering in metals

    PubMed Central

    Lanzillo, Nicholas A.; Thomas, Jay B.; Watson, Bruce; Washington, Morris; Nayak, Saroj K.

    2014-01-01

    We present a combined first-principles and experimental study of the electrical resistivity in aluminum and copper samples under pressures up to 2 GPa. The calculations are based on first-principles density functional perturbation theory, whereas the experimental setup uses a solid media piston–cylinder apparatus at room temperature. We find that upon pressurizing each metal, the phonon spectra are blue-shifted and the net electron–phonon interaction is suppressed relative to the unstrained crystal. This reduction in electron–phonon scattering results in a decrease in the electrical resistivity under pressure, which is more pronounced for aluminum than for copper. We show that density functional perturbation theory can be used to accurately predict the pressure response of the electrical resistivity in these metals. This work demonstrates how the phonon spectra in metals can be engineered through pressure to achieve more attractive electrical properties. PMID:24889627

  5. Raman Scattering Signature of a Localized-to-Delocalized Transition at the Inception of a Dilute Abnormal GaAs1-xNx Alloy

    NASA Astrophysics Data System (ADS)

    Mialitsin, Aleksej V.; Mascarenhas, Angelo

    2013-05-01

    We identify the signature of a localized-to-delocalized transition in the resonant Raman scattering spectra from GaAs1-xNx. Our measurements in the ultradilute nitrogen doping concentrations demonstrate an energy shift in the line width resonance of the LO phonon. With decreasing nitrogen concentration, the EW line width resonance energy reduces abruptly by ca. 47 meV at x≈0.35%. This value corresponds to the concentration at which GaAs1-xNx has been recently shown to transition from an impurity regime to an alloy regime. Our study elucidates the evolution of dilute abnormal alloys and their Raman response.

  6. Temperature dependence of resonant secondary emission in NaNO 2: Spectral behavior

    NASA Astrophysics Data System (ADS)

    Kato, Riso; Kawaguchi, Yoshizo; Ashida, Masaaki

    1990-05-01

    Spectral behavior of resonant secondary emission in NaNO 2 has been investigated in the temperature range from 2 to 30 K under the excitation near the v00 line of the lowest singlet absorption. With increasing temperature, luminescence lines separated from multiple-order Raman lines become detectable even under the excitation with the off-resonance energy Δ c ≳ 13 cm -1. The intensity of the luminescence line IL( T) increases with temperature in proportion to the phonon number n( hvp, T) in the temperature range T ≲ Δ c/ k, while it increases more steeply in the range T ≳ Δ c/ k. The temperature dependence of IL( T) is ascribed to the increase in the luminescence from the v00 level after the one-phonon assisted transition to the level induced by the off-resonant incident light. The intensity of the Raman line IR( T) decreases gradually in 2-12 K range and shows rapid drop above 12 K. The temperature dependence of IR( T) is ascribed to the dephasing of the intermediate state due to the two-phonon interaction with the reservoir.

  7. Seeing the invisible plasma with transient phonons in cuprous oxide

    DOE PAGES

    Frazer, Laszlo; Schaller, Richard D.; Chang, Kelvin B.; ...

    2016-12-12

    Here, the emission of phonons from electron–hole plasma is the primary limit on the efficiency of photovoltaic devices operating above the bandgap. In cuprous oxide (Cu 2O) there is no luminescence from electron–hole plasma. Therefore, we searched for optical phonons emitted by energetic charge carriers using phonon-to-exciton upconversion transitions. We found 14 meV phonons with a lifetime of 0.916 ± 0.008 ps and 79 meV phonons that are longer lived and overrepresented. It is surprising that the higher energy phonon has a longer lifetime.

  8. Dynamics of large-wave-vector magnons and phonons in MnF2:Er3+ using a far-infrared quantum-counter technique

    NASA Astrophysics Data System (ADS)

    Rotter, L. D.; Dennis, W. M.; Yen, W. M.

    1990-07-01

    Magnons near the Brillouin zone-edge were generated in antiferromagnetic MnF2:Er3+ at 1.9 K by exciting the intrinsic two-magnon absorption band using a pulsed far-infrared laser. The lowest Stark level of the Er3+ ground state was used as a 36-cm-1 magnon and phonon detector in a quantum-counter scheme. A simple set of rate equations was used to model the system. The decay time was found to be 2.9+/-0.6 μs for 55-cm-1, 3+/-2 μs for 47.6-cm-1 magnons, and 40+/-20 ns for 36-cm-1 phonons. The sum of the 36-cm-1 magnon decay rate and the Er3+-magnon decay rate was 0.9+/-0.2 μs-1. Possible mechanisms of magnon decay are discussed. The dominant mechanism is most likely thermal magnon-magnon scattering. No evidence of large-wave-vector magnon decay to 36-cm-1 phonons was found. We suggest that magnons do not decay to phonons until they scatter into the magnetoelastic modes. Implications with respect to recent magnon-transport experiments are discussed.

  9. Self-consistent description of a system of interacting phonons

    NASA Astrophysics Data System (ADS)

    Poluektov, Yu. M.

    2015-11-01

    A proposal for a method of self-consistent description of phonon systems. This method generalizes the Debye model to account for phonon-phonon interaction. The idea of "self-consistent" phonons is introduced; their speed depends on the temperature and is determined by solving a non-linear equation. The Debye energy is also a function of the temperature within the framework of the proposed approach. The thermodynamics of "self-consistent" phonon gas are built. It is shown that at low temperatures the cubic law temperature dependence of specific heat acquires an additional term that is proportional to the seventh power of the temperature. This seems to explain the reason why the cubic law for specific heat is observed only at relatively low temperatures. At high temperatures, the theory predicts a linear deviation with respect to temperature from the Dulong-Petit law, which is observed experimentally. A modification to the melting criteria is considered, to account for the phonon-phonon interaction.

  10. Excited-state structure and electronic dephasing time of Nile blue from absolute resonance Raman intensities

    NASA Astrophysics Data System (ADS)

    Lawless, Mary K.; Mathies, Richard A.

    1992-06-01

    Absolute resonance Raman cross sections are measured for Nile blue 690 perchlorate dissolved in ethylene glycol with excitation at 514, 531, and 568 nm. These values and the absorption spectrum are modeled using a time-dependent wave packet formalism. The excited-state equilibrium geometry changes are quantitated for 40 resonance Raman active modes, seven of which (590, 1141, 1351, 1429, 1492, 1544, and 1640 cm-1 ) carry 70% of the total resonance Raman intensity. This demonstrates that in addition to the prominent 590 and 1640 cm-1 modes, a large number of vibrational degrees of freedom are Franck-Condon coupled to the electronic transition. After exposure of the explicit vibrational progressions, the residual absorption linewidth is separated into its homogeneous [350 cm-1 half-width at half-maximum (HWHM)] and inhomogeneous (313 cm-1 HWHM) components through an analysis of the absolute Raman cross sections. The value of the electronic dephasing time derived from this study (25 fs) compares well to previously published results. These data should be valuable in multimode modeling of femtosecond experiments on Nile blue.

  11. H irradiation effects on the GaAs-like Raman modes in GaAs1-xNx/GaAs1-xNx:H planar heterostructures

    NASA Astrophysics Data System (ADS)

    Giulotto, E.; Geddo, M.; Patrini, M.; Guizzetti, G.; Felici, M.; Capizzi, M.; Polimeni, A.; Martelli, F.; Rubini, S.

    2014-12-01

    The GaAs-like longitudinal optical phonon frequency in two hydrogenated GaAs1-xNx/GaAs1-xNx:H microwire heterostructures—with similar N concentration, but different H dose and implantation conditions—has been investigated by micro-Raman mapping. In the case of GaAs0.991N0.009 wires embedded in barriers where GaAs-like properties are recovered through H irradiation, the phonon frequency in the barriers undergoes a blue shift with respect to the wires. In GaAs0.992N0.008 wires embedded in less hydrogenated barriers, the phonon frequency exhibits an opposite behavior (red shift). Strain, disorder, phonon localization effects induced by H-irradiation on the GaAs-like phonon frequency are discussed and related to different types of N-H complexes formed in the hydrogenated barriers. It is shown that the red (blue) character of the frequency shift is related to the dominant N-2H (N-3H) type of complexes. Moreover, for specific experimental conditions, an all-optical determination of the uniaxial strain field is obtained. This may improve the design of recently presented devices that exploit the correlation between uniaxial stress and the degree of polarization of photoluminescence.

  12. Phonon cross-plane transport and thermal boundary resistance: effect of heat source size and thermal boundary resistance on phonon characteristics

    NASA Astrophysics Data System (ADS)

    Ali, H.; Yilbas, B. S.

    2016-09-01

    Phonon cross-plane transport across silicon and diamond thin films pair is considered, and thermal boundary resistance across the films pair interface is examined incorporating the cut-off mismatch and diffusive mismatch models. In the cut-off mismatch model, phonon frequency mismatch for each acoustic branch is incorporated across the interface of the silicon and diamond films pair in line with the dispersion relations of both films. The frequency-dependent and transient solution of the Boltzmann transport equation is presented, and the equilibrium phonon intensity ratios at the silicon and diamond film edges are predicted across the interface for each phonon acoustic branch. Temperature disturbance across the edges of the films pair is incorporated to assess the phonon transport characteristics due to cut-off and diffusive mismatch models across the interface. The effect of heat source size, which is allocated at high-temperature (301 K) edge of the silicon film, on the phonon transport characteristics at the films pair interface is also investigated. It is found that cut-off mismatch model predicts higher values of the thermal boundary resistance across the films pair interface as compared to that of the diffusive mismatch model. The ratio of equilibrium phonon intensity due to the cut-off mismatch over the diffusive mismatch models remains >1 at the silicon edge, while it becomes <1 at the diamond edge for all acoustic branches.

  13. Edge waves and resonances in two-dimensional phononic crystal plates

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Hsu, Jin-Chen, E-mail: hsujc@yuntech.edu.tw; Hsu, Chih-Hsun

    2015-05-07

    We present a numerical study on phononic band gaps and resonances occurring at the edge of a semi-infinite two-dimensional (2D) phononic crystal plate. The edge supports localized edge waves coupling to evanescent phononic plate modes that decay exponentially into the semi-infinite phononic crystal plate. The band-gap range and the number of edge-wave eigenmodes can be tailored by tuning the distance between the edge and the semi-infinite 2D phononic lattice. As a result, a phononic band gap for simultaneous edge waves and plate waves is created, and phononic cavities beside the edge can be built to support high-frequency edge resonances. Wemore » design an L3 edge cavity and analyze its resonance characteristics. Based on the band gap, high quality factor and strong confinement of resonant edge modes are achieved. The results enable enhanced control over acoustic energy flow in phononic crystal plates, which can be used in designing micro and nanoscale resonant devices and coupling of edge resonances to other types of phononic or photonic crystal cavities.« less

  14. The effect of hot phonons and coupled phonon-plasmon modes on scattering-induced NDR in quantum wells

    NASA Astrophysics Data System (ADS)

    Ridley, B. K.; Al-Mudares, M.

    1988-04-01

    We have extended our Monte Carlo simulation of scattering-induced NDR in Al. 8Ga 2As/GaAs quantum wells by including (a) the effect of hot phonons (b) coupled phonon-plasmon modes (c) degeneracy. Hot phonons were modelled using a phenomenological lifetime which we ranged from 3ps to 10ps. Coupled modes were modelled in the antiscreening approximation. Bulk-like modes were assumed in both cases. NDR is quenched if the phonon lifetime exceeds 7ps, but is little affected if the lifetime is 3ps. The effect of coupled modes is appreciable at a doping density of 10 18cm -3, virtually eliminating NDR, but at 10 17cm -3 the effect is much smaller. Including degeneracy has only a small effect on the results. We conclude that NDR is still possible at electron densities around 10 17cm -3.

  15. Four-phonon scattering significantly reduces intrinsic thermal conductivity of solids

    NASA Astrophysics Data System (ADS)

    Feng, Tianli; Lindsay, Lucas; Ruan, Xiulin

    2017-10-01

    For decades, the three-phonon scattering process has been considered to govern thermal transport in solids, while the role of higher-order four-phonon scattering has been persistently unclear and so ignored. However, recent quantitative calculations of three-phonon scattering have often shown a significant overestimation of thermal conductivity as compared to experimental values. In this Rapid Communication we show that four-phonon scattering is generally important in solids and can remedy such discrepancies. For silicon and diamond, the predicted thermal conductivity is reduced by 30% at 1000 K after including four-phonon scattering, bringing predictions in excellent agreement with measurements. For the projected ultrahigh-thermal conductivity material, zinc-blende BAs, a competitor of diamond as a heat sink material, four-phonon scattering is found to be strikingly strong as three-phonon processes have an extremely limited phase space for scattering. The four-phonon scattering reduces the predicted thermal conductivity from 2200 to 1400 W/m K at room temperature. The reduction at 1000 K is 60%. We also find that optical phonon scattering rates are largely affected, being important in applications such as phonon bottlenecks in equilibrating electronic excitations. Recognizing that four-phonon scattering is expensive to calculate, in the end we provide some guidelines on how to quickly assess the significance of four-phonon scattering, based on energy surface anharmonicity and the scattering phase space. Our work clears the decades-long fundamental question of the significance of higher-order scattering, and points out ways to improve thermoelectrics, thermal barrier coatings, nuclear materials, and radiative heat transfer.

  16. Polarization-controlled coherent phonon generation in acoustoplasmonic metasurfaces

    NASA Astrophysics Data System (ADS)

    Lanzillotti-Kimura, Norberto D.; O'Brien, Kevin P.; Rho, Junsuk; Suchowski, Haim; Yin, Xiaobo; Zhang, Xiang

    2018-06-01

    Acoustic vibrations at the nanoscale (GHz-THz frequencies) and their interactions with electrons, photons, and other excitations are the heart of an emerging field in physics: nanophononics. The design of ultrahigh frequency acoustic-phonon transducers, with tunable frequency, and easy to integrate in complex systems is still an open and challenging problem for the development of acoustic nanoscopies and phonon lasers. Here we show how an optimized plasmonic metasurface can act as a high-frequency phonon transducer. We report pump-probe experiments in metasurfaces composed of an array of gold nanostructures, revealing that such arrays can act as efficient and tunable photon-phonon transducers, with a strong spectral dependence on the excitation rate and laser polarization. We anticipate our work to be the starting point for the engineering of phononic metasurfaces based on plasmonic nanostructures.

  17. Understanding photon sideband statistics and correlation for determining phonon coherence

    NASA Astrophysics Data System (ADS)

    Ding, Ding; Yin, Xiaobo; Li, Baowen

    2018-01-01

    Generating and detecting coherent high-frequency heat-carrying phonons have been topics of great interest in recent years. Although there have been successful attempts in generating and observing coherent phonons, rigorous techniques to characterize and detect phonon coherence in a crystalline material have been lagging compared to what has been achieved for photons. One main challenge is a lack of detailed understanding of how detection signals for phonons can be related to coherence. The quantum theory of photoelectric detection has greatly advanced the ability to characterize photon coherence in the past century, and a similar theory for phonon detection is necessary. Here, we reexamine the optical sideband fluorescence technique that has been used to detect high-frequency phonons in materials with optically active defects. We propose a quantum theory of phonon detection using the sideband technique and found that there are distinct differences in sideband counting statistics between thermal and coherent phonons. We further propose a second-order correlation function unique to sideband signals that allows for a rigorous distinction between thermal and coherent phonons. Our theory is relevant to a correlation measurement with nontrivial response functions at the quantum level and can potentially bridge the gap of experimentally determining phonon coherence to be on par with that of photons.

  18. Orbitally-driven giant phonon anharmonicity in SnSe

    DOE PAGES

    Li, Chen W.; Hong, Jiawang; May, Andrew F.; ...

    2015-10-19

    We understand that elementary excitations and their couplings in condensed matter systems is critical to develop better energy-conversion devices. In thermoelectric materials, the heat-to-electricity conversion efficiency is directly improved by suppressing the propagation of phonon quasiparticles responsible for macroscopic thermal transport. The material with the current record for thermoelectric conversion efficiency, SnSe, achieves an ultra-low thermal conductivity, but the mechanism enabling this strong phonon scattering remains largely unknown. Using inelastic neutron scattering measurements and first-principles simulations, we mapped the four-dimensional phonon dispersion surfaces of SnSe, and revealed the origin of ionic-potential anharmonicity responsible for the unique properties of SnSe. Wemore » show that the giant phonon scattering arises from an unstable electronic structure, with orbital interactions leading to a ferroelectric-like lattice instability. Our results provide a microscopic picture connecting electronic structure and phonon anharmonicity in SnSe, and offers precious insights on how electron-phonon and phononphonon interactions may lead to the realization of ultra-low thermal conductivity.« less

  19. Temperature-Induced Large Broadening and Blue Shift in the Electronic Band Structure and Optical Absorption of Methylammonium Lead Iodide Perovskite.

    PubMed

    Yang, Jia-Yue; Hu, Ming

    2017-08-17

    The power conversion efficiency of hybrid halide perovskite solar cells is profoundly influenced by the operating temperature. Here we investigate the temperature influence on the electronic band structure and optical absorption of cubic CH 3 NH 3 PbI 3 from first-principles by accounting for both the electron-phonon interaction and thermal expansion. Within the framework of density functional perturbation theory, the electron-phonon coupling induces slightly enlarged band gap and strongly broadened electronic relaxation time as temperature increases. The large broadening effect is mainly due to the presence of cation organic atoms. Consequently, the temperature-dependent absorption peak exhibits blue-shift position, decreased amplitude, and broadened width. This work uncovers the atomistic origin of temperature influence on the optical absorption of cubic CH 3 NH 3 PbI 3 and can provide guidance to design high-performance hybrid halide perovskite solar cells at different operating temperatures.

  20. Micro-Raman imaging on 4H-SiC in contact with the electrode at room temperature

    NASA Astrophysics Data System (ADS)

    Suda, Jun; Suwa, Satoshi; Mizuno, Shugo; Togo, Kouki; Mastuo, Yuya

    2018-03-01

    Raman images (30 μm × 30 μm × 180 μm) of a bulk 4H-SiC wafer in contact with a Ni/Au electrode film in 100 nm/200 nm thick were measured with Micro-Raman spectroscopy at room temperature. As the imaging area approached the interface between the SiC and electrode, the center frequency of the E2(TO) mode (778 cm- 1) immediately declined; in the Raman imaging, relative distribution of compressive residual stress around residual tensile stress, and linewidth were broadened due to crystal distortion. For LOPC (LO-phonon-plasmon-coupled) mode (970 cm- 1), center frequency showed variation right next to the interface, while linewidth decreased slowly as the imaging area approached the interface. We evaluated the temperature dependence of the line broadening and the center frequency of the LOPC mode in 4H-SiC in a high-temperature region. Free carrier concentration increased with temperature, and remained almost constant in the center frequency after impurities were ionized completely.

  1. The impact of inversion and mirror reflection symmetry on Raman scattering of T'transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Yan, Jun; Chen, Shao-Yu; Naylor, Carl; Goldstein, Thomas; Johnson, Charlie; Venkataraman, Dhandapani; Ramasubramaniam, Ashwin

    Distorted octahedral (T') transition metal dichalcogenides (TMDCs) are topologically interesting material systems. Inversion-symmetry-broken bulk T'-TMDCs are predicted to be type II Weyl semimetals and inversion-symmetric monolayer (1L) T'-TMDCs are shown to be 2D topological insulators. In this talk, I will show that both the inversion symmetry and the mirror symmetry are important for understanding the lattice dynamics and Raman scattering of T'-TMDCs. The mirror plane that is perpendicular to the zigzag transition metal atomic chain classifies lattice vibrations into z-modes and m-modes where ` z' stands for zigzag and ` m' stands for mirror. Raman active z- and m- modes can be experimentally determined with light-polarization and crystal angle-resolved Raman tensor analysis. We report observation of all 9 even-parity zone-center phonons in 1L-T'-MoTe2. In bulk T'-MoTe2, we monitor inversion symmetry breaking with the shear lattice vibrations, which is important for supporting Weyl fermions. This work is supported by the Armstrong Fund for Science and NSF EFRI 2DARE EFMA-1542879.

  2. Excitation energy dependent Raman spectrum of MoSe2

    PubMed Central

    Nam, Dahyun; Lee, Jae-Ung; Cheong, Hyeonsik

    2015-01-01

    Raman investigation of MoSe2 was carried out with eight different excitation energies. Seven peaks, including E1g, A1g, E2g1, and A2u2 peaks are observed in the range of 100–400 cm−1. The phonon modes are assigned by comparing the peak positions with theoretical calculations. The intensities of the peaks are enhanced at different excitation energies through resonance with different optical transitions. The A1g mode is enhanced at 1.58 and 3.82 eV, which are near the A exciton energy and the band-to-band transition between higher energy bands, respectively. The E2g1 mode is strongly enhanced with respect to the A1g mode for the 2.71- and 2.81-eV excitations, which are close to the C exciton energy. The different enhancements of the A1g and E2g1 modes are explained in terms of the symmetries of the exciton states and the exciton-phonon coupling. Other smaller peaks including E1g and A2u2 are forbidden but appear due to the resonance effect near optical transition energies. PMID:26601614

  3. Absorption coefficients of silicon: A theoretical treatment

    NASA Astrophysics Data System (ADS)

    Tsai, Chin-Yi

    2018-05-01

    A theoretical model with explicit formulas for calculating the optical absorption and gain coefficients of silicon is presented. It incorporates direct and indirect interband transitions and considers the effects of occupied/unoccupied carrier states. The indirect interband transition is calculated from the second-order time-independent perturbation theory of quantum mechanics by incorporating all eight possible routes of absorption or emission of photons and phonons. Absorption coefficients of silicon are calculated from these formulas. The agreements and discrepancies among the calculated results, the Rajkanan-Singh-Shewchun (RSS) formula, and Green's data are investigated and discussed. For example, the RSS formula tends to overestimate the contributions of indirect transitions for cases with high photon energy. The results show that the state occupied/unoccupied effect is almost negligible for silicon absorption coefficients up to the onset of the optical gain condition where the energy separation of Quasi-Femi levels between electrons and holes is larger than the band-gap energy. The usefulness of using the physics-based formulas, rather than semi-empirical fitting ones, for absorption coefficients in theoretical studies of photovoltaic devices is also discussed.

  4. Raman spectroscopic characterization of wood and pulp fibers

    Treesearch

    Umesh Prasad Agarwal

    2008-01-01

    This chapter reviews applications of Raman spectroscopy in the field of wood and pulp fibers. Most of the literature examined was published between 1998 and 2006. In addition to introduction, this chapter contains sections on wood and components, mechanical pulp, chemical pulp, modified/treated wood, cellulose I crystallinity of wood fibers, and the self-absorption...

  5. Electronic Raman scattering as an ultra-sensitive probe of strain effects in semiconductors

    DOE PAGES

    Fluegel., Brian; Mialitsin, Aleksej V.; Beaton, Daniel A.; ...

    2015-05-28

    In this study, the semiconductor strain engineering has become a critical feature of high-performance electronics because of the significant device performance enhancements that it enables. These improvements, which emerge from strain-induced modifications to the electronic band structure, necessitate new ultra-sensitive tools to probe the strain in semiconductors. Here, we demonstrate that minute amounts of strain in thin semiconductor epilayers can be measured using electronic Raman scattering. We applied this strain measurement technique to two different semiconductor alloy systems using coherently strained epitaxial thin films specifically designed to produce lattice-mismatch strains as small as 10 –4. Comparing our strain sensitivity andmore » signal strength in Al xGa 1–xAs with those obtained using the industry-standard technique of phonon Raman scattering, we found that there was a sensitivity improvement of 200-fold and a signal enhancement of 4 × 10 3, thus obviating key constraints in semiconductor strain metrology.« less

  6. Orbitally driven giant phonon anharmonicity in SnSe

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Li, C. W.; Hong, J.; May, A. F.

    Understanding elementary excitations and their couplings in condensed matter systems is critical for developing better energy-conversion devices. In thermoelectric materials, the heat-to-electricity conversion efficiency is directly improved by suppressing the propagation of phonon quasiparticles responsible for macroscopic thermal transport. The current record material for thermoelectric conversion efficiency, SnSe, has an ultralow thermal conductivity, but the mechanism behind the strong phonon scattering remains largely unknown. From inelastic neutron scattering measurements and first-principles simulations, we mapped the four-dimensional phonon dispersion surfaces of SnSe, and found the origin of the ionic-potential anharmonicity responsible for the unique properties of SnSe. We show that themore » giant phonon scattering arises from an unstable electronic structure, with orbital interactions leading to a ferroelectric-like lattice instability. The present results provide a microscopic picture connecting electronic structure and phonon anharmonicity in SnSe, and offers new insights on how electron–phonon and phonon–phonon interactions may lead to the realization of ultralow thermal conductivity.« less

  7. Phonons and elasticity of cementite through the Curie temperature

    NASA Astrophysics Data System (ADS)

    Mauger, L.; Herriman, J. E.; Hellman, O.; Tracy, S. J.; Lucas, M. S.; Muñoz, J. A.; Xiao, Yuming; Li, J.; Fultz, B.

    2017-01-01

    Phonon partial densities of states (pDOS) of Fe573C were measured from cryogenic temperatures through the Curie transition at 460 K using nuclear resonant inelastic x-ray scattering. The cementite pDOS reveal that low-energy acoustic phonons shift to higher energies (stiffen) with temperature before the magnetic transition. This unexpected stiffening suggests strongly nonharmonic vibrational behavior that impacts the thermodynamics and elastic properties of cementite. Density functional theory calculations reproduced the anomalous stiffening observed experimentally in cementite by accounting for phonon-phonon interactions at finite temperatures. The calculations show that the low-energy acoustic phonon branches with polarizations along the [010] direction are largely responsible for the anomalous thermal stiffening. The effect was further localized to the motions of the FeII site within the orthorhombic structure, which participates disproportionately in the anomalous phonon stiffening.

  8. Exciton-phonon system on a star graph: A perturbative approach.

    PubMed

    Yalouz, Saad; Pouthier, Vincent

    2016-05-01

    Based on the operatorial formulation of the perturbation theory, the properties of an exciton coupled with optical phonons on a star graph are investigated. Within this method, the dynamics is governed by an effective Hamiltonian, which accounts for exciton-phonon entanglement. The exciton is dressed by a virtual phonon cloud whereas the phonons are clothed by virtual excitonic transitions. In spite of the coupling with the phonons, it is shown that the energy spectrum of the dressed exciton resembles that of a bare exciton. The only differences originate in a polaronic mechanism that favors an energy shift and a decay of the exciton hopping constant. By contrast, the motion of the exciton allows the phonons to propagate over the graph so that the dressed normal modes drastically differ from the localized modes associated to bare phonons. They define extended vibrations whose properties depend on the state occupied by the exciton that accompanies the phonons. It is shown that the phonon frequencies, either red shifted or blue shifted, are very sensitive to the model parameter in general, and to the size of the graph in particular.

  9. Nanomesh phononic structures for low thermal conductivity and thermoelectric energy conversion materials

    DOEpatents

    Yu, Jen-Kan; Mitrovic, Slobodan; Heath, James R.

    2016-08-16

    A nanomesh phononic structure includes: a sheet including a first material, the sheet having a plurality of phononic-sized features spaced apart at a phononic pitch, the phononic pitch being smaller than or equal to twice a maximum phonon mean free path of the first material and the phononic size being smaller than or equal to the maximum phonon mean free path of the first material.

  10. Coherent phonon optics in a chip with an electrically controlled active device.

    PubMed

    Poyser, Caroline L; Akimov, Andrey V; Campion, Richard P; Kent, Anthony J

    2015-02-05

    Phonon optics concerns operations with high-frequency acoustic waves in solid media in a similar way to how traditional optics operates with the light beams (i.e. photons). Phonon optics experiments with coherent terahertz and sub-terahertz phonons promise a revolution in various technical applications related to high-frequency acoustics, imaging, and heat transport. Previously, phonon optics used passive methods for manipulations with propagating phonon beams that did not enable their external control. Here we fabricate a phononic chip, which includes a generator of coherent monochromatic phonons with frequency 378 GHz, a sensitive coherent phonon detector, and an active layer: a doped semiconductor superlattice, with electrical contacts, inserted into the phonon propagation path. In the experiments, we demonstrate the modulation of the coherent phonon flux by an external electrical bias applied to the active layer. Phonon optics using external control broadens the spectrum of prospective applications of phononics on the nanometer scale.

  11. Time-domain calculations of the polarized Raman spectra, the transient infrared absorption anisotropy, and the extent of delocalization of the OH stretching mode of liquid water.

    PubMed

    Torii, Hajime

    2006-08-03

    The polarized Raman spectrum and the time dependence of the transient infrared (TRIR) absorption anisotropy are calculated for the OH stretching mode of liquid water (neat liquid H2O) by using time-domain formulations, which include the effects of both the diagonal frequency modulations (of individual oscillators) induced by the interactions between the dipole derivatives and the intermolecular electric field, and the off-diagonal (intermolecular) vibrational coupling described by the transition dipole coupling (TDC) mechanism. The IR spectrum of neat liquid H2O and the TRIR anisotropy of a liquid mixture of H2O/HDO/D2O are also calculated. It is shown that the calculated features of these optical signals, including the temperature dependence of the polarized Raman and IR spectra, are in reasonable agreement with the experimental results, indicating that the frequency separation between the isotropic and anisotropic components of the polarized Raman spectrum and the rapid decay (approximately 0.1 ps) of the TRIR anisotropy of the OH stretching mode of neat liquid H2O are mainly controlled by the resonant intermolecular vibrational coupling described by the TDC mechanism. Comparing with the time evolution of vibrational excitations, it is suggested that the TRIR anisotropy decays in the time needed for the initially localized vibrational excitations to delocalize over a few oscillators. It is also shown that the enhancement of the dipole derivatives by the interactions with surrounding molecules is an important factor in generating the spectral profiles of the OH stretching Raman band. The time-domain behavior of the molecular motions that affect the spectroscopic features is discussed.

  12. Resonant Magnon-Phonon Polaritons in a Ferrimagnet

    DTIC Science & Technology

    2000-09-29

    UNCLASSIFIED Defense Technical Information Center Compilation Part Notice ADPO 11604 TITLE: Resonant Magnon -Phonon Polaritons in a Ferrimagnet...part numbers comprise the compilation report: ADP011588 thru ADP011680 UNCLASSIFIED 75 Resonant Magnon -Phonon Polaritons in a Ferrimagnet I. E...susceptibilities X"aa and X’m << X’m appear, where 77 xem - DPx igEo0 i_ Xxy - hy- C1 (0)2 _ 00t2) 4= -7• 4 3. Phonon and magnon polaritons We solve the

  13. Structural and dynamical properties of Bridgman-grown CdSexTe1-x (0

    NASA Astrophysics Data System (ADS)

    Talwar, Devki N.; Feng, Zhe Chuan; Lee, Jyh-Fu; Becla, P.

    2013-04-01

    Measurements of the Raman scattering and extended x-ray-absorption fine-structure (EXAFS) spectroscopy are reported on a series of Bridgman-grown zinc-blende CdTe1-xSex (0.35 ≥ x > 0.05) ternary alloys to empathize their lattice dynamical and structural properties. Low-temperature Raman spectra have revealed the classic CdTe-like (TO1, LO1) and CdSe-like (TO2, LO2) pairs of optical phonons. The composition-dependent peak positions of the LO2 modes exhibited shifts towards the higher-energy side, while those of the LO1 phonon frequencies have unveiled the slight redshifts. Detailed analyses of EXAFS data by using the first-principles bond orbital model have enabled us to estimate both the lattice relaxations and nearest-neighbor radial force constants around the Se/Te atoms in the CdTe/CdSe matrix. These results are methodically integrated in the “average t-matrix” formalism within the Green's-function theory for defining the impurity perturbations to comprehend the composition-dependent optical phonons in CdTe1-xSex alloys. Based on our comprehensive calculations of impurity modes in the low-composition regime x→ 0, we have assigned the weak phonon feature observed near ˜175 cm-1 in the low-temperature infrared reflectivity spectroscopy study to a SeTe localized vibrational mode.

  14. Investigating the Electron-Phonon Coupling of Molecular Beam Epitaxy-Grown Hg1-x Cd x Se Semiconductor Alloys

    NASA Astrophysics Data System (ADS)

    Peiris, F. C.; Lewis, M. V.; Brill, G.; Doyle, Kevin; Myers, T. H.

    2018-03-01

    Using spectroscopic ellipsometry, the temperature-dependence of the dielectric functions of a series of Hg1-x Cd x Se thin films deposited on both ZnTe/Si(112) and GaSb(112) substrates were investigated. Initially, for each sample, room-temperature ellipsometric spectra were obtained from 35 meV to 6 eV using two different ellipsometers. Subsequently, ellipsometry spectra were obtained from 10 K to 300 K by incorporating a cryostat to the ellipsometer. Using a standard inversion technique, the spectroscopic ellipsometric data were modeled in order to obtain the temperature-dependent dielectric functions of each of the Hg1-x Cd x Se thin films. The results indicate that the E 1 critical point blue-shifts as a function of Cd-alloy concentration. The temperature-dependence of E 1 was fitted to a Bose-Einstein occupation distribution function, which consequently allowed us to determine the electron-phonon coupling of Hg1-x Cd x Se alloys. From the fitting results, we obtain a value of 17 ± 2 meV for the strength of the electron-phonon coupling for Hg1-x Cd x Se alloy system, which compares nominally with the binary systems, such as CdSe and CdTe, which have values around 38 meV and 16 meV, respectively. This implies that the addition of Hg into the CdSe binary system does not significantly alter its electron-phonon coupling strength. Raman spectroscopy measurements performed on all the samples show the HgSe-like transverse optic (TO) and longitudinal optic (LO) phonons (˜ 130 cm-1 and ˜ 160 cm-1, respectively) for all the samples. While there is a slight red-shift of the HgSe-like TO peak as a function of the Cd-concentration, HgSe-like LO peak does not significantly change with the alloy concentration.

  15. A hybrid phononic crystal for roof application.

    PubMed

    Wan, Qingmian; Shao, Rong

    2017-11-01

    Phononic crystal is a type of acoustic material, and the study of phononic crystals has attracted great attention from national research institutions. Meanwhile, noise reduction in the low-frequency range has always encountered difficulties and troubles in the engineering field. In order to obtain a unique and effective low-frequency noise reduction method, in this paper a low frequency noise attenuation system based on phononic crystal structure is proposed and demonstrated. The finite element simulation of the band gap is consistent with the final test results. The effects of structure parameters on the band gaps were studied by changing the structure parameters and the band gaps can be controlled by suitably tuning structure parameters. The structure and results provide a good support for phononic crystal structures engineering application.

  16. Excited-state structure and isomerization dynamics of the retinal chromophore in rhodopsin from resonance Raman intensities.

    PubMed Central

    Loppnow, G R; Mathies, R A

    1988-01-01

    Resonance Raman excitation profiles have been measured for the bovine visual pigment rhodopsin using excitation wavelengths ranging from 457.9 to 647.1 nm. A complete Franck-Condon analysis of the absorption spectrum and resonance Raman excitation profiles has been performed using an excited-state, time-dependent wavepacket propagation technique. This has enabled us to determine the change in geometry upon electronic excitation of rhodopsin's 11-cis-retinal protonated Schiff base chromophore along 25 normal coordinates. Intense low-frequency Raman lines are observed at 98, 135, 249, 336, and 461 cm-1 whose intensities provide quantitative, mode-specific information about the excited-state torsional deformations that lead to isomerization. The dominant contribution to the width of the absorption band in rhodopsin results from Franck-Condon progressions in the 1,549 cm-1 ethylenic normal mode. The lack of vibronic structure in the absorption spectrum is shown to be caused by extensive progressions in low-frequency torsional modes and a large homogeneous linewidth (170 cm-1 half-width) together with thermal population of low-frequency modes and inhomogeneous site distribution effects. The resonance Raman cross-sections of rhodopsin are unusually weak because the excited-state wavepacket moves rapidly (approximately 35 fs) and permanently away from the Franck-Condon geometry along skeletal stretching and torsional coordinates. PMID:3416032

  17. Stimulated Raman spectroscopy of 13CF4

    NASA Astrophysics Data System (ADS)

    Martínez, R. Z.; Bermejo, D.; Boudon, V.

    2018-06-01

    CF4 is a powerful greenhouse gas, mostly released in the atmosphere by industries. A careful modeling of its absorption spectrum is required in order to allow accurate atmospheric concentration measurements. For this aim, high resolution Raman spectroscopy is of great help, since it gives access to rovibrational levels that are not directly reachable through dipolar absorption, although they are involved in hot band generation. Following our previous work on 12CF4, we present here a similar investigation of the second isotopologue, 13CF4. The spectra of the ν1 (909.21 cm-1), 2ν1 -ν1 (906.77 cm-1), ν1 +ν2 -ν2 (909.33 cm-1), ν2 (435.47 cm-1), 2ν2 (868.10 cm-1) and 3ν2 -ν2 (865.73 cm-1) bands were obtained with a quasi-continuous wave stimulated Raman spectrometer. These six bands were studied at temperatures of 140 and 298 K (for the hot bands). These spectra could be assigned and modeled thanks to the XTDS and SPVIEW software developed in the Dijon group.

  18. Phonon Mapping in Flowing Equilibrium

    NASA Astrophysics Data System (ADS)

    Ruff, J. P. C.

    2015-03-01

    When a material conducts heat, a modification of the phonon population occurs. The equilibrium Bose-Einstein distribution is perturbed towards flowing-equilibrium, for which the distribution function is not analytically known. Here I argue that the altered phonon population can be efficiently mapped over broad regions of reciprocal space, via diffuse x-ray scattering or time-of-flight neutron scattering, while a thermal gradient is applied across a single crystal sample. When compared to traditional transport measurements, this technique offers a superior, information-rich new perspective on lattice thermal conductivity, wherein the band and momentum dependences of the phonon thermal current are directly resolved. The proposed method is benchmarked using x-ray thermal diffuse scattering measurements of single crystal diamond under transport conditions. CHESS is supported by the NSF & NIH/NIGMS via NSF Award DMR-1332208.

  19. Phonon Effects on Charge Transport Through a Two State Molecule

    NASA Astrophysics Data System (ADS)

    Ulloa, Sergio E.; Yudiarsah, Efta

    2008-03-01

    We study the effect of local and non-local phonon on the transport properties of a molecule model described by two- electronic states. The local phonon interaction is tackled by means of a Lang Firsov transformation [1,2]. The interaction with non-local phonons (phonon-assisted hopping) is considered perturbatively up to the first nonzero order in the self energy. The presence of different kinds of electron-phonon interaction open new transmission channels. In addition to the polaron shift and replicas due to local phonons, non-local phonons cause the appearance of new satellite states around the initial states. In the weak coupling regime of non-local phonon and electrons, states are shifted an amount proportional to square of the interaction. However, in the strong coupling regime, the non-linear effects emerge and display more interesting features on transport properties. Additional features on transport properties due to new transmission channel are shown to appear at finite temperatures. [1] G. D. Mahan, Many-particle physics, 3rd ed. (Plenum Publishers, New York, 2000). [2] R. Gutierrez et al., Phys. Rev. B. 74, 235105 (2006).

  20. Band gap enhancement of glancing angle deposited TiO2 nanowire array

    NASA Astrophysics Data System (ADS)

    Chinnamuthu, P.; Mondal, A.; Singh, N. K.; Dhar, J. C.; Chattopadhyay, K. K.; Bhattacharya, Sekhar

    2012-09-01

    Vertically oriented TiO2 nanowire (NW) arrays were fabricated by glancing angle deposition technique. Field emission-scanning electron microscopy shows the formation of two different diameters ˜80 nm and ˜40 nm TiO2 NW for 120 and 460 rpm azimuthal rotation of the substrate. The x-ray diffraction and Raman scattering depicted the presence of rutile and anatase phase TiO2. The overall Raman scattering intensity decreased with nanowire diameter. The role of phonon confinement in anatase and rutile peaks has been discussed. The red (7.9 cm-1 of anatase Eg) and blue (7.4 cm-1 of rutile Eg, 7.8 cm-1 of rutile A1g) shifts of Raman frequencies were observed. UV-vis absorption measurements show the main band absorption at 3.42 eV, 3.48 eV, and ˜3.51 eV for thin film and NW prepared at 120 and 460 rpm, respectively. Three fold enhance photon absorption and intense light emission were observed for NW assembly. The photoluminescence emission from the NW assembly revealed blue shift in main band transition due to quantum confinement in NW structures.