Thermal conductivity in large - J two-dimensional antiferromagnets: Role of phonon scattering

DOE PAGES

Chernyshev, A. L.; Brenig, Wolfram

2015-08-05

Different types of relaxation processes for magnon heat current are discussed, with a particular focus on coupling to three-dimensional phonons. There is thermal conductivity by these in-plane magnetic excitations using two distinct techniques: Boltzmann formalism within the relaxation-time approximation and memory-function approach. Also considered are the scattering of magnons by both acoustic and optical branches of phonons. We demonstrate an accord between the two methods, regarding the asymptotic behavior of the effective relaxation rates. It is strongly suggested that scattering from optical or zone-boundary phonons is important for magnon heat current relaxation in a high-temperature window of ΘD≲T<< J.

Tailorable stimulated Brillouin scattering in nanoscale silicon waveguides

PubMed Central

Shin, Heedeuk; Qiu, Wenjun; Jarecki, Robert; Cox, Jonathan A.; Olsson, Roy H.; Starbuck, Andrew; Wang, Zheng; Rakich, Peter T.

2013-01-01

Nanoscale modal confinement is known to radically enhance the effect of intrinsic Kerr and Raman nonlinearities within nanophotonic silicon waveguides. By contrast, stimulated Brillouin-scattering nonlinearities, which involve coherent coupling between guided photon and phonon modes, are stifled in conventional nanophotonics, preventing the realization of a host of Brillouin-based signal-processing technologies in silicon. Here we demonstrate stimulated Brillouin scattering in silicon waveguides, for the first time, through a new class of hybrid photonic–phononic waveguides. Tailorable travelling-wave forward-stimulated Brillouin scattering is realized—with over 1,000 times larger nonlinearity than reported in previous systems—yielding strong Brillouin coupling to phonons from 1 to 18 GHz. Experiments show that radiation pressures, produced by subwavelength modal confinement, yield enhancement of Brillouin nonlinearity beyond those of material nonlinearity alone. In addition, such enhanced and wideband coherent phonon emission paves the way towards the hybridization of silicon photonics, microelectromechanical systems and CMOS signal-processing technologies on chip. PMID:23739586

Electron-phonon interaction model and prediction of thermal energy transport in SOI transistor.

PubMed

Jin, Jae Sik; Lee, Joon Sik

2007-11-01

An electron-phonon interaction model is proposed and applied to thermal transport in semiconductors at micro/nanoscales. The high electron energy induced by the electric field in a transistor is transferred to the phonon system through electron-phonon interaction in the high field region of the transistor. Due to this fact, a hot spot occurs, which is much smaller than the phonon mean free path in the Si-layer. The full phonon dispersion model based on the Boltzmann transport equation (BTE) with the relaxation time approximation is applied for the interactions among different phonon branches and different phonon frequencies. The Joule heating by the electron-phonon scattering is modeled through the intervalley and intravalley processes for silicon by introducing average electron energy. The simulation results are compared with those obtained by the full phonon dispersion model which treats the electron-phonon scattering as a volumetric heat source. The comparison shows that the peak temperature in the hot spot region is considerably higher and more localized than the previous results. The thermal characteristics of each phonon mode are useful to explain the above phenomena. The optical mode phonons of negligible group velocity obtain the highest energy density from electrons, and resides in the hot spot region without any contribution to heat transport, which results in a higher temperature in that region. Since the acoustic phonons with low group velocity show the higher energy density after electron-phonon scattering, they induce more localized heating near the hot spot region. The ballistic features are strongly observed when phonon-phonon scattering rates are lower than 4 x 10(10) S(-1).

Time Evolution of Charge Carriers & Phonons after Photo-Excitation by an Ultra-Short Light Pulse in Bulk Germanium

NASA Astrophysics Data System (ADS)

Fahy, Stephen; Murphy-Armando, Felipe; Trigo, Mariano; Savic, Ivana; Murray, Eamonn; Reis, David

We have calculated the time-evolution of carriers and generated phonons in Ge after ultrafast photo-excitation above the direct band-gap. The relevant electron-phonon and anharmonic phonon scattering rates are obtained from first-principles electronic structure calculations. Measurements of the x-ray diffuse scattering after excitation near the L point in the Brillouin zone find a relatively slow (5 ps, compared to the typical electron-phonon energy relaxation of the Gamma-L phonon) increase of the phonon population. We find this is due to emission caused by the scattering of electrons between the Delta and L valleys, after the initial depopulation of the Gamma valley. The relative slowness of this process is due to a combination of causes: (i) the finite time for the initial depopulation of the conduction Gamma valley; (ii) the associated electron-phonon coupling is relatively weaker (compared to Gamma-L, Gamma-Delta and Delta-Delta couplings) ; (iii) the TA associated phonon has a long lifetime and (iv) the depopulation of the Delta valley suppresses the phonon emission. Supported by Science Foundation Ireland, Grant 12/1A/1601.

Transient thermal and nonthermal electron and phonon relaxation after short-pulsed laser heating of metals

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

Giri, Ashutosh; Hopkins, Patrick E., E-mail: phopkins@virginia.edu

2015-12-07

Several dynamic thermal and nonthermal scattering processes affect ultrafast heat transfer in metals after short-pulsed laser heating. Even with decades of measurements of electron-phonon relaxation, the role of thermal vs. nonthermal electron and phonon scattering on overall electron energy transfer to the phonons remains unclear. In this work, we derive an analytical expression for the electron-phonon coupling factor in a metal that includes contributions from equilibrium and nonequilibrium distributions of electrons. While the contribution from the nonthermal electrons to electron-phonon coupling is non-negligible, the increase in the electron relaxation rates with increasing laser fluence measured by thermoreflectance techniques cannot bemore » accounted for by only considering electron-phonon relaxations. We conclude that electron-electron scattering along with electron-phonon scattering have to be considered simultaneously to correctly predict the transient nature of electron relaxation during and after short-pulsed heating of metals at elevated electron temperatures. Furthermore, for high electron temperature perturbations achieved at high absorbed laser fluences, we show good agreement between our model, which accounts for d-band excitations, and previous experimental data. Our model can be extended to other free electron metals with the knowledge of the density of states of electrons in the metals and considering electronic excitations from non-Fermi surface states.« less

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

Stochastic treatment of electron multiplication without scattering in dielectrics

NASA Technical Reports Server (NTRS)

Lin, D. L.; Beers, B. L.

1981-01-01

By treating the emission of optical phonons as a Markov process, a simple analytic method is developed for calculating the electronic ionization rate per unit length for dielectrics. The effects of scattering from acoustic and optical phonons are neglected. The treatment obtains universal functions in recursive form, the theory depending on only two dimensionless energy ratios. A comparison of the present work with other numerical approaches indicates that the effect of scattering becomes important only when the electric potential energy drop in a mean free path for optical-phonon emission is less than about 25% of the ionization potential. A comparison with Monte Carlo results is also given for Teflon.

Using resistive readout to probe ultrafast dynamics of a plasmonic sensor

NASA Astrophysics Data System (ADS)

Cheney, Alec; Chen, Borui; Cartwright, Alexander; Thomay, Tim

2018-02-01

Surface plasmons in a DC current lead to an increase in scattering processes, resulting in a measurable increase in electrical resistance of a plasmonic nano-grating. This enables a purely electronic readout of plasmonically mediated optical absorption. We show that there is a time-dependence in these resistance changes on the order of 100ps that we attribute to electron-phonon and phonon-phonon scattering processes in the metal of the nano-gratings. Since plasmonic responses are strongly structurally dependent, an appropriately designed plasmoelectronic detector could potentially offer an extremely fast response at communication wavelengths in a fully CMOS compatible system.

Microstructure-Induced Phonon Focusing Effects and Opportunities for Improved Material Quantification (Postprint)

DTIC Science & Technology

2012-02-01

phonon interactions with electrons , electron -hole pairs, defects, super- lattices, and interfaces [1-4]. As pointed out by Hauser et. al. [3], and...phonon-phonon and electron - phonon scattering processes placed limits on the methods applicability. More recently, the advantages of using lower...texture effects. In particular, the elongated grains result in colonies that are largely cigar -shaped or cylindrical in their form, where elastic

Büttiker probes for dissipative phonon quantum transport in semiconductor nanostructures

NASA Astrophysics Data System (ADS)

Miao, K.; Sadasivam, S.; Charles, J.; Klimeck, G.; Fisher, T. S.; Kubis, T.

2016-03-01

Theoretical prediction of phonon transport in modern semiconductor nanodevices requires atomic resolution of device features and quantum transport models covering coherent and incoherent effects. The nonequilibrium Green's function method is known to serve this purpose well but is numerically expensive in simulating incoherent scattering processes. This work extends the efficient Büttiker probe approach widely used in electron transport to phonons and considers salient implications of the method. Different scattering mechanisms such as impurity, boundary, and Umklapp scattering are included, and the method is shown to reproduce the experimental thermal conductivity of bulk Si and Ge over a wide temperature range. Temperature jumps at the lead/device interface are captured in the quasi-ballistic transport regime consistent with results from the Boltzmann transport equation. Results of this method in Si/Ge heterojunctions illustrate the impact of atomic relaxation on the thermal interface conductance and the importance of inelastic scattering to activate high-energy channels for phonon transport. The resultant phonon transport model is capable of predicting the thermal performance in the heterostructure efficiently.

Attenuation process of the longitudinal phonon mode in a TeO2 crystal in the 20-GHz range

NASA Astrophysics Data System (ADS)

Ohno, S.; Sonehara, T.; Tatsu, E.; Koreeda, A.; Saikan, S.

2017-06-01

We experimentally investigated the hypersonic attenuation process of a longitudinal mode (L-mode) sound wave in TeO2 from room temperature to a lower temperature using Brillouin scattering and impulsive stimulated thermal scattering (ISTS) measurements. For precise measurement of the Brillouin linewidth at low temperatures, whereby the mean free path of the phonon becomes longer than the sample length, it is indispensable that the phonon should propagate along the phonon-resonance direction. To figure out the suitable direction, we defined two indices characterizing a degree of phonon divergence and a purity of propagation direction. The best direction that we found from these indices is [110] direction in TeO2, and it was used to discuss the temperature and frequency dependences of Brillouin spectra. We extracted the temperature dependence of the attenuation rate of T4 from the modulated Brillouin spectra due to the phonon resonance below Debye temperature. The frequency dependence ω1 of the hypersonic attenuation was also estimated from the polarization dependence of the Brillouin linewidth. Theoretically, it predicted that the L-mode phonon attenuation at low temperatures in TeO2 is a result of Herring's process, which shows the attenuation behavior of ω2T3 . The ω1T4 dependence is not allowed in Herring's process but is allowed by the L +L →L process, which has been considered to be forbidden so far. We evaluated the thermal phonon lifetime using ISTS and established that it was finite even at 20 K, thereby allowing the L +L →L process. Therefore, we conclude that the L +L →L process dominates the attenuation of an L-mode phonon in TeO2 in the low-temperature region.

Temperature-dependent thermal conductivity and diffusivity of a Mg-doped insulating β-Ga2O3 single crystal along [100], [010] and [001

NASA Astrophysics Data System (ADS)

Handwerg, M.; Mitdank, R.; Galazka, Z.; Fischer, S. F.

2016-12-01

The monoclinic crystal structure of β-{{Ga}}2{{{O}}}3 leads to significant anisotropy of the thermal properties. The 2ω-method is used to measure the thermal diffusivity D in [010] and [001] direction respectively and to determine the thermal conductivity values λ of the [100], [010] and [001] direction from the same insulating Mg-doped β-{{Ga}}2{{{O}}}3 single crystal. We detect a temperature independent anisotropy factor of both the thermal diffusivity and conductivity values of {D}[010]/{D}[001]={λ }[010]/{λ }[001]=1.4+/- 0.1. The temperature dependence is in accord with phonon-phonon-Umklapp-scattering processes from 300 K down to 150 K. Below 150 K point-defect-scattering lowers the estimated phonon-phonon-Umklapp-scattering values.

Phonon Lifetime Observation in Epitaxial ScN Film with Inelastic X-Ray Scattering Spectroscopy.

PubMed

Uchiyama, H; Oshima, Y; Patterson, R; Iwamoto, S; Shiomi, J; Shimamura, K

2018-06-08

Phonon-phonon scattering dominates the thermal properties in nonmetallic materials, and it directly influences device performance in applications. The understanding of the scattering has been progressing using computational approaches, and the direct and systematic observation of phonon modes that include momentum dependences is desirable. We report experimental data on the phonon dispersion curves and lifetimes in an epitaxially grown ScN film using inelastic x-ray scattering measurements. The momentum dependence of the optical phonon lifetimes is estimated from the spectral width, and the highest-energy phonon mode around the zone center is found to possess a short lifetime of 0.21 ps. A comparison with first-principles calculations shows that our observed phonon lifetimes are quantitatively explained by three-body phonon-phonon interactions.

Phonon Lifetime Observation in Epitaxial ScN Film with Inelastic X-Ray Scattering Spectroscopy

NASA Astrophysics Data System (ADS)

Uchiyama, H.; Oshima, Y.; Patterson, R.; Iwamoto, S.; Shiomi, J.; Shimamura, K.

2018-06-01

Phonon-phonon scattering dominates the thermal properties in nonmetallic materials, and it directly influences device performance in applications. The understanding of the scattering has been progressing using computational approaches, and the direct and systematic observation of phonon modes that include momentum dependences is desirable. We report experimental data on the phonon dispersion curves and lifetimes in an epitaxially grown ScN film using inelastic x-ray scattering measurements. The momentum dependence of the optical phonon lifetimes is estimated from the spectral width, and the highest-energy phonon mode around the zone center is found to possess a short lifetime of 0.21 ps. A comparison with first-principles calculations shows that our observed phonon lifetimes are quantitatively explained by three-body phonon-phonon interactions.

Lattice Waves, Spin Waves, and Neutron Scattering

DOE R&D Accomplishments Database

Brockhouse, Bertram N.

1962-03-01

Use of neutron inelastic scattering to study the forces between atoms in solids is treated. One-phonon processes and lattice vibrations are discussed, and experiments that verified the existence of the quantum of lattice vibrations, the phonon, are reviewed. Dispersion curves, phonon frequencies and absorption, and models for dispersion calculations are discussed. Experiments on the crystal dynamics of metals are examined. Dispersion curves are presented and analyzed; theory of lattice dynamics is considered; effects of Fermi surfaces on dispersion curves; electron-phonon interactions, electronic structure influence on lattice vibrations, and phonon lifetimes are explored. The dispersion relation of spin waves in crystals and experiments in which dispersion curves for spin waves in Co-Fe alloy and magnons in magnetite were obtained and the reality of the magnon was demonstrated are discussed. (D.C.W)

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.

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.

Brillouin light scattering as a probe for low frequency quasiparticles in solids

NASA Astrophysics Data System (ADS)

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

2015-03-01

In increasingly small electronic and spintronic devices, electrons, optical phonons, acoustic phonons, and magnons are often driven out of local thermal equilibrium. Thermal transport based on equilibrium dynamics does not adequately describe these systems necessitating a better understanding of non-equilibrium transport processes. Measuring the specific temperatures of the different energy carriers is therefore crucial in understanding the thermal transport. Brillouin light scattering (BLS) has recently been explored as a temperature sensor for low frequency acoustic phonons in glass, and also magnons in metallic and insulating ferromagnetic materials. We report the measured BLS spectra of acoustic phonons in Silicon at different temperatures. The temperature dependence of the BLS peak frequency, linewidth, and integrated intensity are examined to evaluate their potential uses as temperature sensors of acoustic phonons. We also observe a large nonequilibrium in phonon-magnon temperature in YIG under the effects of laser heating and thereby extract a value for the phonon-magnon coupling coefficient. This work is funded by the National Science Foundation and the Army Research Office.

Electron-phonon coupling and thermal transport in the thermoelectric compound Mo 3Sb 7–xTe x

DOE PAGES

Bansal, Dipanshu; Li, Chen W.; Said, Ayman H.; ...

2015-12-07

Phonon properties of Mo 3Sb 7–xTe x (x = 0, 1.5, 1.7), a potential high-temperature thermoelectric material, have been studied with inelastic neutron and x-ray scattering, and with first-principles simulations. The substitution of Te for Sb leads to pronounced changes in the electronic struc- ture, local bonding, phonon density of states (DOS), dispersions, and phonon lifetimes. Alloying with tellurium shifts the Fermi level upward, near the top of the valence band, resulting in a strong suppression of electron-phonon screening, and a large overall stiffening of interatomic force- constants. The suppression in electron-phonon coupling concomitantly increases group velocities and suppresses phononmore » scattering rates, surpassing the effects of alloy-disorder scattering, and re- sulting in a surprising increased lattice thermal conductivity in the alloy. We also identify that the local bonding environment changes non-uniformly around different atoms, leading to variable perturbation strengths for different optical phonon branches. The respective roles of changes in phonon group velocities and phonon lifetimes on the lattice thermal conductivity are quantified. Lastly, our results highlight the importance of the electron-phonon coupling on phonon mean-free-paths in this compound, and also estimates the contributions from boundary scattering, umklapp scattering, and point-defect scattering.« less

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 .

Coherent Control of Scattering Processes in Semiconductors

NASA Astrophysics Data System (ADS)

Wehner, M. U.

1998-03-01

On a timescale which compares to the duration of single scattering events, the relaxation of optical excitations in semiconductors has to be described by the quantum kinetic theory. Instead of simple scattering rates this theory delivers a non-Markovian dephasing. Related memory effects have so far been observed for the case of electron-LO-phonon scattering in four-wave-mixing experiments on GaAs at T = 77 K using 15 fs pulses (L. Bányai, D.B. Tran Thoai, E. Reitsamer, H. Haug, D. Steinbach, M.U. Wehner, T. Marschner, M. Wegener and W. Stolz, Phys. Rev. Lett. 75), 2188 (1995). It is crucial for the quantum kinetic time regime that scattering processes must not be considered as completed and irreversibel. The reversibility of the scattering shortly after optical excitation is demonstrated in four-wave-mixing experiments using coherent control. By adjusting the relative phase of two phase-locked pulses, the non-Markovian phonon oscillations observed in Ref.1 can be either suppressed or amplified (M. U. Wehner, M. H. Ulm, D. S. Chemla and M. Wegener, Phys. Rev. Lett. submitted). The behavior of the coherently controlled scattering amplitude is discussed using a simple model Hamiltonian, which describes the variation of the phonon oscillations in amplitude and phase very well.

Thermal transport across metal silicide-silicon interfaces: First-principles calculations and Green's function transport simulations

NASA Astrophysics Data System (ADS)

Sadasivam, Sridhar; Ye, Ning; Feser, Joseph P.; Charles, James; Miao, Kai; Kubis, Tillmann; Fisher, Timothy S.

2017-02-01

Heat transfer across metal-semiconductor interfaces involves multiple fundamental transport mechanisms such as elastic and inelastic phonon scattering, and electron-phonon coupling within the metal and across the interface. The relative contributions of these different transport mechanisms to the interface conductance remains unclear in the current literature. In this work, we use a combination of first-principles calculations under the density functional theory framework and heat transport simulations using the atomistic Green's function (AGF) method to quantitatively predict the contribution of the different scattering mechanisms to the thermal interface conductance of epitaxial CoSi2-Si interfaces. An important development in the present work is the direct computation of interfacial bonding from density functional perturbation theory (DFPT) and hence the avoidance of commonly used "mixing rules" to obtain the cross-interface force constants from bulk material force constants. Another important algorithmic development is the integration of the recursive Green's function (RGF) method with Büttiker probe scattering that enables computationally efficient simulations of inelastic phonon scattering and its contribution to the thermal interface conductance. First-principles calculations of electron-phonon coupling reveal that cross-interface energy transfer between metal electrons and atomic vibrations in the semiconductor is mediated by delocalized acoustic phonon modes that extend on both sides of the interface, and phonon modes that are localized inside the semiconductor region of the interface exhibit negligible coupling with electrons in the metal. We also provide a direct comparison between simulation predictions and experimental measurements of thermal interface conductance of epitaxial CoSi2-Si interfaces using the time-domain thermoreflectance technique. Importantly, the experimental results, performed across a wide temperature range, only agree well with predictions that include all transport processes: elastic and inelastic phonon scattering, electron-phonon coupling in the metal, and electron-phonon coupling across the interface.

Monte Carlo Calculation of Thermal Neutron Inelastic Scattering Cross Section Uncertainties by Sampling Perturbed Phonon Spectra

NASA Astrophysics Data System (ADS)

Holmes, Jesse Curtis

Nuclear data libraries provide fundamental reaction information required by nuclear system simulation codes. The inclusion of data covariances in these libraries allows the user to assess uncertainties in system response parameters as a function of uncertainties in the nuclear data. Formats and procedures are currently established for representing covariances for various types of reaction data in ENDF libraries. This covariance data is typically generated utilizing experimental measurements and empirical models, consistent with the method of parent data production. However, ENDF File 7 thermal neutron scattering library data is, by convention, produced theoretically through fundamental scattering physics model calculations. Currently, there is no published covariance data for ENDF File 7 thermal libraries. Furthermore, no accepted methodology exists for quantifying or representing uncertainty information associated with this thermal library data. The quality of thermal neutron inelastic scattering cross section data can be of high importance in reactor analysis and criticality safety applications. These cross sections depend on the material's structure and dynamics. The double-differential scattering law, S(alpha, beta), tabulated in ENDF File 7 libraries contains this information. For crystalline solids, S(alpha, beta) is primarily a function of the material's phonon density of states (DOS). Published ENDF File 7 libraries are commonly produced by calculation and processing codes, such as the LEAPR module of NJOY, which utilize the phonon DOS as the fundamental input for inelastic scattering calculations to directly output an S(alpha, beta) matrix. To determine covariances for the S(alpha, beta) data generated by this process, information about uncertainties in the DOS is required. The phonon DOS may be viewed as a probability density function of atomic vibrational energy states that exist in a material. Probable variation in the shape of this spectrum may be established that depends on uncertainties in the physics models and methodology employed to produce the DOS. Through Monte Carlo sampling of perturbations from the reference phonon spectrum, an S(alpha, beta) covariance matrix may be generated. In this work, density functional theory and lattice dynamics in the harmonic approximation are used to calculate the phonon DOS for hexagonal crystalline graphite. This form of graphite is used as an example material for the purpose of demonstrating procedures for analyzing, calculating and processing thermal neutron inelastic scattering uncertainty information. Several sources of uncertainty in thermal neutron inelastic scattering calculations are examined, including sources which cannot be directly characterized through a description of the phonon DOS uncertainty, and their impacts are evaluated. Covariances for hexagonal crystalline graphite S(alpha, beta) data are quantified by coupling the standard methodology of LEAPR with a Monte Carlo sampling process. The mechanics of efficiently representing and processing this covariance information is also examined. Finally, with appropriate sensitivity information, it is shown that an S(alpha, beta) covariance matrix can be propagated to generate covariance data for integrated cross sections, secondary energy distributions, and coupled energy-angle distributions. This approach enables a complete description of thermal neutron inelastic scattering cross section uncertainties which may be employed to improve the simulation of nuclear systems.

Invited review article: physics and Monte Carlo techniques as relevant to cryogenic, phonon, and ionization readout of Cryogenic Dark Matter Search radiation detectors.

PubMed

Leman, Steven W

2012-09-01

This review discusses detector physics and Monte Carlo techniques for cryogenic, radiation detectors that utilize combined phonon and ionization readout. A general review of cryogenic phonon and charge transport is provided along with specific details of the Cryogenic Dark Matter Search detector instrumentation. In particular, this review covers quasidiffusive phonon transport, which includes phonon focusing, anharmonic decay, and isotope scattering. The interaction of phonons in the detector surface is discussed along with the downconversion of phonons in superconducting films. The charge transport physics include a mass tensor which results from the crystal band structure and is modeled with a Herring-Vogt transformation. Charge scattering processes involve the creation of Neganov-Luke phonons. Transition-edge-sensor (TES) simulations include a full electric circuit description and all thermal processes including Joule heating, cooling to the substrate, and thermal diffusion within the TES, the latter of which is necessary to model normal-superconducting phase separation. Relevant numerical constants are provided for these physical processes in germanium, silicon, aluminum, and tungsten. Random number sampling methods including inverse cumulative distribution function (CDF) and rejection techniques are reviewed. To improve the efficiency of charge transport modeling, an additional second order inverse CDF method is developed here along with an efficient barycentric coordinate sampling method of electric fields. Results are provided in a manner that is convenient for use in Monte Carlo and references are provided for validation of these models.

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.

Intrinsic Charge Carrier Mobility in Single-Layer Black Phosphorus.

PubMed

Rudenko, A N; Brener, S; Katsnelson, M I

2016-06-17

We present a theory for single- and two-phonon charge carrier scattering in anisotropic two-dimensional semiconductors applied to single-layer black phosphorus (BP). We show that in contrast to graphene, where two-phonon processes due to the scattering by flexural phonons dominate at any practically relevant temperatures and are independent of the carrier concentration n, two-phonon scattering in BP is less important and can be considered negligible at n≳10^{13}  cm^{-2}. At smaller n, however, phonons enter in the essentially anharmonic regime. Compared to the hole mobility, which does not exhibit strong anisotropy between the principal directions of BP (μ_{xx}/μ_{yy}∼1.4 at n=10^{13} cm^{-2} and T=300  K), the electron mobility is found to be significantly more anisotropic (μ_{xx}/μ_{yy}∼6.2). Absolute values of μ_{xx} do not exceed 250 (700)  cm^{2} V^{-1} s^{-1} for holes (electrons), which can be considered as an upper limit for the mobility in BP at room temperature.

Ab initio phonon point defect scattering and thermal transport in graphene

NASA Astrophysics Data System (ADS)

Polanco, Carlos A.; Lindsay, Lucas

2018-01-01

We study the scattering of phonons from point defects and their effect on lattice thermal conductivity κ using a parameter-free ab initio Green's function methodology. Specifically, we focus on the scattering of phonons by boron (B), nitrogen (N), and phosphorus substitutions as well as single- and double-carbon vacancies in graphene. We show that changes of the atomic structure and harmonic interatomic force constants locally near defects govern the strength and frequency trends of the scattering of out-of-plane acoustic (ZA) phonons, the dominant heat carriers in graphene. ZA scattering rates due to N substitutions are nearly an order of magnitude smaller than those for B defects despite having similar mass perturbations. Furthermore, ZA phonon scattering rates from N defects decrease with increasing frequency in the lower-frequency spectrum in stark contrast to expected trends from simple models. ZA phonon-vacancy scattering rates are found to have a significantly softer frequency dependence (˜ω0 ) in graphene than typically employed in phenomenological models. The rigorous Green's function calculations demonstrate that typical mass-defect models do not adequately describe ZA phonon-defect scattering rates. Our ab initio calculations capture well the trend of κ vs vacancy density from experiments, though not the magnitudes. This work elucidates important insights into phonon-defect scattering and thermal transport in graphene, and demonstrates the applicability of first-principles methods toward describing these properties in imperfect materials.

X-ray Diffuse Scattering from Ultrafast Laser Excited Solids

NASA Astrophysics Data System (ADS)

Trigo, Mariano; Sheu, Yu-Miin; Chen, Jian; Reis, David; Fahy, Stephen; Murray, Eamonn; Graber, Timothy; Henning, Robert

2009-03-01

Intense, ultrashort laser pulses can be used to excite and detect coherent phonons in solids. However, optical experiments can only probe a reduced fraction of the Brillouin zone and hence most of the decay channels of such coherent phonons become invisible. In contrast, time-resolved x-ray diffuse scattering (TRXDS) has the potential to be the ultimate tool to study these phonon decay processes throughout the Brillouin-zone of the crystal. In our work, performed at the BioCARS beamline at the Advanced Photon Source, we use synchrotron time-resolved diffuse x-ray scattering to study Si and Bi under intense laser excitation with 100 ps resolution. We show that reasonable signal levels can be achieved with incident flux of 10^12 photons comparable to the flux that will be available at future 4th generation sources such as the LCLS in a single pulse. These sources will also provide three orders of magnitude shorter pulses; thus, this experiment serves as a test of the feasibility of time-resolved X-ray diffuse scattering as a tool for studying nonequilibrium phonon dynamics in solids.

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

Unexpectedly Fast Phonon-Assisted Exciton Hopping between Carbon Nanotubes

DOE PAGES

Davoody, A. H.; Karimi, F.; Arnold, M. S.; ...

2017-06-05

Carbon-nanotube (CNT) aggregates are promising light-absorbing materials for photovoltaics. The hopping rate of excitons between CNTs directly affects the efficiency of these devices. We theoretically investigate phonon-assisted exciton hopping, where excitons scatter with phonons into a same-tube transition state, followed by intertube Coulomb scattering into the final state. Second-order hopping between bright excitonic states is as fast as the first-order process (~1 ps). For perpendicular CNTs, the high rate stems from the high density of phononic states; for parallel CNTs, the reason lies in relaxed selection rules. Moreover, second-order exciton transfer between dark and bright states, facilitated by phonons withmore » large angular momentum, has rates comparable to bright-to-bright transfer, so dark excitons provide an additional pathway for energy transfer in CNT composites. Furthermore, as dark excitons are difficult to probe in experiment, predictive theory is critical for understanding exciton dynamics in CNT composites.« less

Unexpectedly Fast Phonon-Assisted Exciton Hopping between Carbon Nanotubes

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

Davoody, A. H.; Karimi, F.; Arnold, M. S.

Carbon-nanotube (CNT) aggregates are promising light-absorbing materials for photovoltaics. The hopping rate of excitons between CNTs directly affects the efficiency of these devices. We theoretically investigate phonon-assisted exciton hopping, where excitons scatter with phonons into a same-tube transition state, followed by intertube Coulomb scattering into the final state. Second-order hopping between bright excitonic states is as fast as the first-order process (~1 ps). For perpendicular CNTs, the high rate stems from the high density of phononic states; for parallel CNTs, the reason lies in relaxed selection rules. Moreover, second-order exciton transfer between dark and bright states, facilitated by phonons withmore » large angular momentum, has rates comparable to bright-to-bright transfer, so dark excitons provide an additional pathway for energy transfer in CNT composites. Furthermore, as dark excitons are difficult to probe in experiment, predictive theory is critical for understanding exciton dynamics in CNT composites.« less

Fuchs-Kliewer phonons of H-covered and clean GaN(1 1 bar 00)

NASA Astrophysics Data System (ADS)

Rink, M.; Himmerlich, M.; Krischok, S.; Kröger, J.

2018-01-01

Inelastic electron scattering is used to study surface phonon polaritons on H-covered and clean GaN(1 1 bar 00) surfaces. The Fuchs-Kliewer phonon of GaN(1 1 bar 00) -H gives rise to characteristic signatures of its single and multiple excitation in specular electron energy loss spectra. The loss intensities for multi-phonon scattering processes decrease according to a Poisson distribution. Vibrational spectra of this surface are invariant on the time scale of days reflecting its chemical passivation by the H layer. In contrast, vibrational spectra of pristine GaN(1 1 bar 00) are subject to a pronounced temporal evolution where spectroscopic weight is gradually shifted towards the multiple excitation of the Fuchs-Kliewer phonon. As a consequence, the monotonous decrease of the cross section for multiple quantum excitation as observed for the H-covered surface is not applicable. This remarkable effect is particularly strong in spectra acquired at low primary energies of incident electrons, which hints at processes occurring in the very surface region. Scenarios that may contribute to these observations are discussed.

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 deformation-potential of confined acoustic phonons is derived by quantizing the appropriate, experimentally verified approximate compressional acoustic-phonon modes in a free-standing rectangular quantum wire. The scattering rate is obtained for GaAs quantum wires with a range of cross-sectional dimensions. The results demonstrate that a proper treatment of confined acoustic phonons may be essential to correctly model electron scattering rates at low energies in nanoscale structures.

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 less than 100 nm was observed. The longitudinal acoustic phonon transport in silicon (Si) nanorod with confined diameter and length was investigated. The guided phonon modes in Si nanorod with different frequencies and wave vectors were observed. The mean-free-path of the guided phonons in Si nanorod was found to be larger than the effective phonon mean-free-path in Si film, because of the limited phonon scattering channels in Si nanorod. The phonon density of states and dispersion relation strongly depend on the size and boundary conditions of nanorod. Our work demonstrates the possibility of modifying the phonon transport properties in nanoscale materials by designing the size and boundary conditions, hence the control of thermal conductivity. In addition, the periodicity effect of nanostructures on acoustic phonon transport was investigated in silicon dioxide (SiO2) nanorod arrays. The lattice modes and mechanical eigenmodes were observed, and the pitch effect on lattice modes was discussed. A narrowband acoustic phonon spectroscopic technique with tunable frequency and spectral width throughout GHz frequency range has been developed to investigate the frequency-dependent acoustic phonon transport in nanoscale materials. The quadratic frequency dependence of acoustic attenuation of SiO2 and indium tin oxide (ITO) thin films was observed, and the acoustic attenuation of ITO was found to be larger than SiO2. Moreover, the acoustic control on mechanical resonance of nanoscale materials using the narrowband acoustic phonon source was demonstrated in tungsten thin film.

Ab initio phonon point defect scattering and thermal transport in graphene

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

Polanco, Carlos A.; Lindsay, Lucas R.

Here, we study the scattering of phonons from point defects and their effect on lattice thermal conductivity κ using a parameter-free ab initio Green's function methodology. Specifically, we focus on the scattering of phonons by boron (B), nitrogen (N), and phosphorus substitutions as well as single- and double-carbon vacancies in graphene. We show that changes of the atomic structure and harmonic interatomic force constants locally near defects govern the strength and frequency trends of the scattering of out-of-plane acoustic (ZA) phonons, the dominant heat carriers in graphene. ZA scattering rates due to N substitutions are nearly an order of magnitudemore » smaller than those for B defects despite having similar mass perturbations. Furthermore, ZA phonon scattering rates from N defects decrease with increasing frequency in the lower-frequency spectrum in stark contrast to expected trends from simple models. ZA phonon-vacancy scattering rates are found to have a significantly softer frequency dependence (~ω 0) in graphene than typically employed in phenomenological models. The rigorous Green's function calculations demonstrate that typical mass-defect models do not adequately describe ZA phonon-defect scattering rates. Our ab initio calculations capture well the trend of κ vs vacancy density from experiments, though not the magnitudes. In conclusion, this work elucidates important insights into phonon-defect scattering and thermal transport in graphene, and demonstrates the applicability of first-principles methods toward describing these properties in imperfect materials.« less

Ab initio phonon point defect scattering and thermal transport in graphene

DOE PAGES

Polanco, Carlos A.; Lindsay, Lucas R.

2018-01-04

Here, we study the scattering of phonons from point defects and their effect on lattice thermal conductivity κ using a parameter-free ab initio Green's function methodology. Specifically, we focus on the scattering of phonons by boron (B), nitrogen (N), and phosphorus substitutions as well as single- and double-carbon vacancies in graphene. We show that changes of the atomic structure and harmonic interatomic force constants locally near defects govern the strength and frequency trends of the scattering of out-of-plane acoustic (ZA) phonons, the dominant heat carriers in graphene. ZA scattering rates due to N substitutions are nearly an order of magnitudemore » smaller than those for B defects despite having similar mass perturbations. Furthermore, ZA phonon scattering rates from N defects decrease with increasing frequency in the lower-frequency spectrum in stark contrast to expected trends from simple models. ZA phonon-vacancy scattering rates are found to have a significantly softer frequency dependence (~ω 0) in graphene than typically employed in phenomenological models. The rigorous Green's function calculations demonstrate that typical mass-defect models do not adequately describe ZA phonon-defect scattering rates. Our ab initio calculations capture well the trend of κ vs vacancy density from experiments, though not the magnitudes. In conclusion, this work elucidates important insights into phonon-defect scattering and thermal transport in graphene, and demonstrates the applicability of first-principles methods toward describing these properties in imperfect materials.« less

Electromagnon dispersion probed by inelastic X-ray scattering in LiCrO2

PubMed Central

Tóth, Sándor; Wehinger, Björn; Rolfs, Katharina; Birol, Turan; Stuhr, Uwe; Takatsu, Hiroshi; Kimura, Kenta; Kimura, Tsuyoshi; Rønnow, Henrik M.; Rüegg, Christian

2016-01-01

Inelastic X-ray scattering with meV energy resolution (IXS) is an ideal tool to measure collective excitations in solids and liquids. In non-resonant scattering condition, the cross-section is strongly dominated by lattice vibrations (phonons). However, it is possible to probe additional degrees of freedom such as magnetic fluctuations that are strongly coupled to the phonons. The IXS spectrum of the coupled system contains not only the phonon dispersion but also the so far undetected magnetic correlation function. Here we report the observation of strong magnon–phonon coupling in LiCrO2 that enables the measurement of magnetic correlations throughout the Brillouin zone via IXS. We find electromagnon excitations and electric dipole active two-magnon excitations in the magnetically ordered phase and heavily damped electromagnons in the paramagnetic phase of LiCrO2. We predict that several (frustrated) magnets with dominant direct exchange and non-collinear magnetism show surprisingly large IXS cross-section for magnons and multi-magnon processes. PMID:27882928

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.

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

Thermal conductance at atomically clean and disordered silicon/aluminum interfaces: A molecular dynamics simulation study

NASA Astrophysics Data System (ADS)

Ih Choi, Woon; Kim, Kwiseon; Narumanchi, Sreekant

2012-09-01

Thermal resistance between layers impedes effective heat dissipation in electronics packaging applications. Thermal conductance for clean and disordered interfaces between silicon (Si) and aluminum (Al) was computed using realistic Si/Al interfaces and classical molecular dynamics with the modified embedded atom method potential. These realistic interfaces, which include atomically clean as well as disordered interfaces, were obtained using density functional theory. At 300 K, the magnitude of interfacial conductance due to phonon-phonon scattering obtained from the classical molecular dynamics simulations was approximately five times higher than the conductance obtained using analytical elastic diffuse mismatch models. Interfacial disorder reduced the thermal conductance due to increased phonon scattering with respect to the atomically clean interface. Also, the interfacial conductance, due to electron-phonon scattering at the interface, was greater than the conductance due to phonon-phonon scattering. This indicates that phonon-phonon scattering is the bottleneck for interfacial transport at the semiconductor/metal interfaces. The molecular dynamics modeling predictions for interfacial thermal conductance for a 5-nm disordered interface between Si/Al were in-line with recent experimental data in the literature.

Band gap structures for 2D phononic crystals with composite scatterer

NASA Astrophysics Data System (ADS)

Qi, Xiao-qiao; Li, Tuan-jie; Zhang, Jia-long; Zhang, Zhen; Tang, Ya-qiong

2018-05-01

We investigated the band gap structures in two-dimensional phononic crystals with composite scatterer. The composite scatterers are composed of two materials (Bragg scattering type) or three materials (locally resonance type). The finite element method is used to calculate the band gap structure, eigenmodes and transmission spectrum. The variation of the location and width of band gap are also investigated as a function of material ratio in the scatterer. We have found that the change trends the widest band gap of the two phononic crystals are different as the material ratio changing. In addition to this, there are three complete band gaps at most for the Bragg-scattering-type phononic crystals in the first six bands; however, the locally resonance-type phononic crystals exist only two complete band gap at most in the first six bands. The gap-tuning effect can be controlled by the material ratio in the scatterer.

Effect of confinement on anharmonic phonon scattering and thermal conductivity in pristine silicon nanowires

NASA Astrophysics Data System (ADS)

Rashid, Zahid; Zhu, Liyan; Li, Wu

2018-02-01

The effect of confinement on the anharmonic phonon scattering rates and the consequences thereof on the thermal transport properties in ultrathin silicon nanowires with a diameter of 1-4 nm have been characterized using atomistic simulations and the phonon Boltzmann transport equation. The phonon density of states (PDOS) for ultrathin nanowires approaches a constant value in the vicinity of the Γ point and increases with decreasing diameter, which indicates the increasing importance of the low-frequency phonons as heat carriers. The anharmonic phonon scattering becomes dramatically enhanced with decreasing thickness of the nanowires. In the thinnest nanowire, the scattering rates for phonons above 1 THz are one order of magnitude higher than those in the bulk Si. Below 1 THz, the increase in scattering rates is even much more appreciable. Our numerical calculations revealed that the scattering rates for transverse (longitudinal) acoustic modes follow √{ω } (1 /√{ω } ) dependence at the low-frequency limit, whereas those for the degenerate flexural modes asymptotically approach a constant value. In addition, the group velocities of phonons are reduced compared with bulk Si except for low-frequency phonons (<1 -2 THz depending on the thickness of the nanowires). The increased scattering rates combined with reduced group velocities lead to a severely reduced thermal conductivity contribution from the high-frequency phonons. Although the thermal conductivity contributed by those phonons with low frequencies is instead increased mainly due to the increased PDOS, the total thermal conductivity is still reduced compared to that of the bulk. This work reveals an unexplored mechanism to understand the measured ultralow thermal conductivity of silicon nanowires.

Magnon and phonon thermometry with inelastic light scattering

NASA Astrophysics Data System (ADS)

Olsson, Kevin S.; An, Kyongmo; Li, Xiaoqin

2018-04-01

Spin caloritronics investigates the interplay between the transport of spin and heat. In the spin Seebeck effect, a thermal gradient across a magnetic material generates a spin current. A temperature difference between the energy carriers of the spin and lattice subsystems, namely the magnons and phonons, is necessary for such thermal nonequilibrium generation of spin current. Inelastic light scattering is a powerful method that can resolve the individual temperatures of magnons and phonons. In this review, we discuss the thermometry capabilities of inelastic light scattering for measuring optical and acoustic phonons, as well as magnons. A scattering spectrum offers three temperature sensitive parameters: frequency shift, linewidth, and integrated intensity. We discuss the temperatures measured via each of these parameters for both phonon and magnons. Finally, we discuss inelastic light scattering experiments that have examined the magnon and phonon temperatures in thermal nonequilibrium which are particularly relevant to spin caloritronic phenomena.

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.

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

Thermal conductivity of hexagonal Si, Ge, and Si1-xGex alloys from first-principles

NASA Astrophysics Data System (ADS)

Gu, Xiaokun; Zhao, C. Y.

2018-05-01

Hexagonal Si and Ge with a lonsdaleite crystal structure are allotropes of silicon and germanium that have recently been synthesized. These materials as well as their alloys are promising candidates for novel applications in optoelectronics. In this paper, we systematically study the phonon transport and thermal conductivity of hexagonal Si, Ge, and their alloys by using the first-principle-based Peierls-Boltzmann transport equation approach. Both three-phonon and four-phonon scatterings are taken into account in the calculations as the phonon scattering mechanisms. The thermal conductivity anisotropy of these materials is identified. While the thermal conductivity parallel to the hexagonal plane for hexagonal Si and Ge is found to be larger than that perpendicular to the hexagonal plane, alloying effectively tunes the thermal conductivity anisotropy by suppressing the thermal conductivity contributions from the middle-frequency phonons. The importance of four-phonon scatterings is assessed by comparing the results with the calculations without including four-phonon scatterings. We find that four-phonon scatterings cannot be ignored in hexagonal Si and Ge as the thermal conductivity would be overestimated by around 10% (40%) at 300 K (900) K. In addition, the phonon mean free path distribution of hexagonal Si, Ge, and their alloys is also discussed.

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.

Isotope scattering and phonon thermal conductivity in light atom compounds: LiH and LiF

DOE PAGES

Lindsay, Lucas R.

2016-11-08

Engineered isotope variation is a pathway toward modulating lattice thermal conductivity (κ) of a material through changes in phonon-isotope scattering. The effects of isotope variation on intrinsic thermal resistance is little explored, as varying isotopes have relatively small differences in mass and thus do not affect bulk phonon dispersions. However, for light elements isotope mass variation can be relatively large (e.g., hydrogen and deuterium). Using a first principles Peierls-Boltzmann transport equation approach the effects of isotope variance on lattice thermal transport in ultra-low-mass compound materials LiH and LiF are characterized. The isotope mass variance modifies the intrinsic thermal resistance viamore » modulation of acoustic and optic phonon frequencies, while phonon-isotope scattering from mass disorder plays only a minor role. This leads to some unusual cases where values of isotopically pure systems ( 6LiH, 7Li 2H and 6LiF) are lower than the values from their counterparts with naturally occurring isotopes and phonon-isotope scattering. However, these differences are relatively small. The effects of temperature-driven lattice expansion on phonon dispersions and calculated κ are also discussed. This work provides insight into lattice thermal conductivity modulation with mass variation and the interplay of intrinsic phonon-phonon and phonon-isotope scattering in interesting light atom systems.« less

Synchrotron x-ray thermal diffuse scattering probes for phonons in Si/SiGe/Si trilayer nanomembranes

DOE PAGES

McElhinny, Kyle M.; Gopalakrishnan, Gokul; Savage, Donald E.; ...

2016-05-17

Nanostructures offer the opportunity to control the vibrational properties of via the scattering of phonons due to boundaries and mass disorder as well as through changes in the phonon dispersion due to spatial confinement. Advances in understanding these effects have the potential to lead to thermoelectrics with an improved figure of merit by lowering the thermal conductivity and to provide insight into electron-phonon scattering rates in nanoelectronics. However, characterizing the phonon population in nanomaterials has been challenging because of their small volume and because optical techniques probe only a small fraction of reciprocal space. Recent developments in x-ray scattering nowmore » allow the phonon population to be evaluated across all of reciprocal space in samples with volumes as small as several cubic micrometers. We apply this approach, synchrotron x-ray thermal diffuse scattering (TDS), to probe the population of phonons within a Si/SiGe/Si trilayer nanomembrane. The distributions of scattered intensity from Si/SiGe/Si trilayer nanomembranes and Si nanomembranes with uniform composition are qualitatively similar, with features arising from the elastic anisotropy of the diamond structure. The TDS signal for the Si/SiGe/Si nanomembrane, however, has higher intensity than the Si membrane of the same total thickness by approximately 3.75%. Possible origins of the enhancement in scattering from SiGe in comparison with Si include the larger atomic scattering factor of Ge atoms within the SiGe layer or reduced phonon frequencies due to alloying.« less

Ultrafast carrier thermalization and cooling dynamics in few-layer MoS2.

PubMed

Nie, Zhaogang; Long, Run; Sun, Linfeng; Huang, Chung-Che; Zhang, Jun; Xiong, Qihua; Hewak, Daniel W; Shen, Zexiang; Prezhdo, Oleg V; Loh, Zhi-Heng

2014-10-28

Femtosecond optical pump-probe spectroscopy with 10 fs visible pulses is employed to elucidate the ultrafast carrier dynamics of few-layer MoS2. A nonthermal carrier distribution is observed immediately following the photoexcitation of the A and B excitonic transitions by the ultrashort, broadband laser pulse. Carrier thermalization occurs within 20 fs and proceeds via both carrier-carrier and carrier-phonon scattering, as evidenced by the observed dependence of the thermalization time on the carrier density and the sample temperature. The n(-0.37 ± 0.03) scaling of the thermalization time with carrier density suggests that equilibration of the nonthermal carrier distribution occurs via non-Markovian quantum kinetics. Subsequent cooling of the hot Fermi-Dirac carrier distribution occurs on the ∼ 0.6 ps time scale via carrier-phonon scattering. Temperature- and fluence-dependence studies reveal the involvement of hot phonons in the carrier cooling process. Nonadiabatic ab initio molecular dynamics simulations, which predict carrier-carrier and carrier-phonon scattering time scales of 40 fs and 0.5 ps, respectively, lend support to the assignment of the observed carrier dynamics.

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.

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.

Advances in heat conduction models and approaches for the prediction of lattice thermal conductivity of dielectric materials

NASA Astrophysics Data System (ADS)

Saikia, Banashree

2017-03-01

An overview of predominant theoretical models used for predicting the thermal conductivities of dielectric materials is given. The criteria used for different theoretical models are explained. This overview highlights a unified theory based on temperature-dependent thermal-conductivity theories, and a drifting of the equilibrium phonon distribution function due to normal three-phonon scattering processes causes transfer of phonon momentum to (a) the same phonon modes (KK-S model) and (b) across the phonon modes (KK-H model). Estimates of the lattice thermal conductivities of LiF and Mg2Sn for the KK-H model are presented graphically.

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.

Scattering of an electronic wave packet by a one-dimensional electron-phonon-coupled structure

NASA Astrophysics Data System (ADS)

Brockt, C.; Jeckelmann, E.

2017-02-01

We investigate the scattering of an electron by phonons in a small structure between two one-dimensional tight-binding leads. This model mimics the quantum electron transport through atomic wires or molecular junctions coupled to metallic leads. The electron-phonon-coupled structure is represented by the Holstein model. We observe permanent energy transfer from the electron to the phonon system (dissipation), transient self-trapping of the electron in the electron-phonon-coupled structure (due to polaron formation and multiple reflections at the structure edges), and transmission resonances that depend strongly on the strength of the electron-phonon coupling and the adiabaticity ratio. A recently developed TEBD algorithm, optimized for bosonic degrees of freedom, is used to simulate the quantum dynamics of a wave packet launched against the electron-phonon-coupled structure. Exact results are calculated for a single electron-phonon site using scattering theory and analytical approximations are obtained for limiting cases.

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.

Thermal and thermoelectric transport measurements of an individual boron arsenide microstructure

NASA Astrophysics Data System (ADS)

Kim, Jaehyun; Evans, Daniel A.; Sellan, Daniel P.; Williams, Owen M.; Ou, Eric; Cowley, Alan H.; Shi, Li

2016-05-01

Recent first principles calculations have predicted that boron arsenide (BAs) can possess an unexpectedly high thermal conductivity that depends sensitively on the crystal size and defect concentration. However, few experimental results have been obtained to verify these predictions. In the present work, we report four-probe thermal and thermoelectric transport measurements of an individual BAs microstructure that was synthesized via a vapor transport method. The measured thermal conductivity was found to decrease slightly with temperature in the range between 250 K and 350 K. The temperature dependence suggests that the extrinsic phonon scattering processes play an important role in addition to intrinsic phonon-phonon scattering. The room temperature value of (186 ± 46) W m-1 K-1 is higher than that of bulk silicon but still a factor of four lower than the calculated result for a defect-free, non-degenerate BAs rod with a similar diameter of 1.15 μm. The measured p-type Seebeck coefficient and thermoelectric power factor are comparable to those of bismuth telluride, which is a commonly used thermoelectric material. The foregoing results also suggest that it is necessary to not only reduce defect and boundary scatterings but also to better understand and control the electron scattering of phonons in order to achieve the predicted ultrahigh intrinsic lattice thermal conductivity of BAs.

Intrinsic to extrinsic phonon lifetime transition in a GaAs-AlAs superlattice.

PubMed

Hofmann, F; Garg, J; Maznev, A A; Jandl, A; Bulsara, M; Fitzgerald, E A; Chen, G; Nelson, K A

2013-07-24

We have measured the lifetimes of two zone-center longitudinal acoustic phonon modes, at 320 and 640 GHz, in a 14 nm GaAs/2 nm AlAs superlattice structure. By comparing measurements at 296 and 79 K we separate the intrinsic contribution to phonon lifetime determined by phonon-phonon scattering from the extrinsic contribution due to defects and interface roughness. At 296 K, the 320 GHz phonon lifetime has approximately equal contributions from intrinsic and extrinsic scattering, whilst at 640 GHz it is dominated by extrinsic effects. These measurements are compared with intrinsic and extrinsic scattering rates in the superlattice obtained from first-principles lattice dynamics calculations. The calculated room-temperature intrinsic lifetime of longitudinal phonons at 320 GHz is in agreement with the experimentally measured value of 0.9 ns. The model correctly predicts the transition from predominantly intrinsic to predominantly extrinsic scattering; however the predicted transition occurs at higher frequencies. Our analysis indicates that the 'interfacial atomic disorder' model is not entirely adequate and that the observed frequency dependence of the extrinsic scattering rate is likely to be determined by a finite correlation length of interface roughness.

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.

Impact of internal crystalline boundaries on lattice thermal conductivity: Importance of boundary structure and spacing

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

Aghababaei, Ramin, E-mail: ramin.aghababaei@epfl.ch; Anciaux, Guillaume; Molinari, Jean-François

2014-11-10

The low thermal conductivity of nano-crystalline materials is commonly explained via diffusive scattering of phonons by internal boundaries. In this study, we have quantitatively studied phonon-crystalline boundaries scattering and its effect on the overall lattice thermal conductivity of crystalline bodies. Various types of crystalline boundaries such as stacking faults, twins, and grain boundaries have been considered in FCC crystalline structures. Accordingly, the specularity coefficient has been determined for different boundaries as the probability of the specular scattering across boundaries. Our results show that in the presence of internal boundaries, the lattice thermal conductivity can be characterized by two parameters: (1)more » boundary spacing and (2) boundary excess free volume. We show that the inverse of the lattice thermal conductivity depends linearly on a non-dimensional quantity which is the ratio of boundary excess free volume over boundary spacing. This shows that phonon scattering across crystalline boundaries is mainly a geometrically favorable process rather than an energetic one. Using the kinetic theory of phonon transport, we present a simple analytical model which can be used to evaluate the lattice thermal conductivity of nano-crystalline materials where the ratio can be considered as an average density of excess free volume. While this study is focused on FCC crystalline materials, where inter-atomic potentials and corresponding defect structures have been well studied in the past, the results would be quantitatively applicable for semiconductors in which heat transport is mainly due to phonon transport.« less

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

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

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

Electron-phonon scattering rates in complex polar crystals

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

Prange, M. P.; Campbell, L. W.; Kerisit, S.

2017-09-01

The thermalization of fast electrons by phonons is studied in CsI, NaI, SrI2, and YAP. This numerical study uses an improvement to a recently developed ab initio method based on a density functional perturbation theoretical description of the phonon modes that provides a way to go beyond widely used phonon models based on binary crystals. Improvements to this method are described, and scattering rates are presented and discussed. The results here treat polar and nonpolar scattering on equal footing and allow an assessment of the relative importance of the two types of scattering. The relative activity of the numerous phononmore » modes in materials with complicated structures is discussed, and a simple criterion for finding the modes that scatter strongly is presented.« less

Revisiting PbTe to identify how thermal conductivity is really limited

NASA Astrophysics Data System (ADS)

Ju, Shenghong; Shiga, Takuma; Feng, Lei; Shiomi, Junichiro

2018-05-01

Due to the long range interaction in lead telluride (PbTe), the transverse optical (TO) phonon becomes soft around the Brillouin zone center. Previous studies have postulated that this zone-center softening causes the low thermal conductivity of PbTe through either enlarged phonon scattering phase space and/or strengthened lattice anharmonicity. In this paper, we reported an extensive sensitivity analysis of the PbTe thermal conductivity to various factors: range and magnitude of harmonic and anharmonic interatomic force constants and phonon wave vectors in the three-phonon scattering processes. The analysis reveals that the softening by long range harmonic interaction itself does not reduce thermal conductivity, and it is the large magnitude of the anharmonic (cubic) force constants that realizes low thermal conductivity, however, not through the TO phonons around the zone center but dominantly through the ones with larger wave vectors in the middle of Brillion zone. The paper clarifies that local band softening cannot be a direct finger print for low thermal conductivity and that the entire Brillion zone needs to be characterized on exploring low thermal conductivity materials.

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.

Probing Electron-Phonon Interaction through Two-Photon Interference in Resonantly Driven Semiconductor Quantum Dots

NASA Astrophysics Data System (ADS)

Reigue, Antoine; Iles-Smith, Jake; Lux, Fabian; Monniello, Léonard; Bernard, Mathieu; Margaillan, Florent; Lemaitre, Aristide; Martinez, Anthony; McCutcheon, Dara P. S.; Mørk, Jesper; Hostein, Richard; Voliotis, Valia

2017-06-01

We investigate the temperature dependence of photon coherence properties through two-photon interference (TPI) measurements from a single quantum dot (QD) under resonant excitation. We show that the loss of indistinguishability is related only to the electron-phonon coupling and is not affected by spectral diffusion. Through these measurements and a complementary microscopic theory, we identify two independent separate decoherence processes, both of which are associated with phonons. Below 10 K, we find that the relaxation of the vibrational lattice is the dominant contribution to the loss of TPI visibility. This process is non-Markovian in nature and corresponds to real phonon transitions resulting in a broad phonon sideband in the QD emission spectra. Above 10 K, virtual phonon transitions to higher lying excited states in the QD become the dominant dephasing mechanism, this leads to a broadening of the zero phonon line, and a corresponding rapid decay in the visibility. The microscopic theory we develop provides analytic expressions for the dephasing rates for both virtual phonon scattering and non-Markovian lattice relaxation.

Semiclassical multi-phonon theory for atom-surface scattering: Application to the Cu(111) system

NASA Astrophysics Data System (ADS)

Daon, Shauli; Pollak, Eli

2015-05-01

The semiclassical perturbation theory of Hubbard and Miller [J. Chem. Phys. 80, 5827 (1984)] is further developed to include the full multi-phonon transitions in atom-surface scattering. A practically applicable expression is developed for the angular scattering distribution by utilising a discretized bath of oscillators, instead of the continuum limit. At sufficiently low surface temperature good agreement is found between the present multi-phonon theory and the previous one-, and two-phonon theory derived in the continuum limit in our previous study [Daon, Pollak, and Miret-Artés, J. Chem. Phys. 137, 201103 (2012)]. The theory is applied to the measured angular distributions of Ne, Ar, and Kr scattered from a Cu(111) surface. We find that the present multi-phonon theory substantially improves the agreement between experiment and theory, especially at the higher surface temperatures. This provides evidence for the importance of multi-phonon transitions in determining the angular distribution as the surface temperature is increased.

Phonon Scattering in Thermoelectrics: Thermal Transport, Strong Anharmonicity, and Emergent Quasiparticles

NASA Astrophysics Data System (ADS)

Delaire, Olivier

Modern neutron and x-ray spectrometers can map phonon dispersions and scattering rates throughout reciprocal space, providing unique insights into microscopic scattering mechanisms, including anharmonicity, electron-phonon coupling, or scattering by defects and nanostructures. In addition, first-principles simulations enable the rationalization of extensive experimental datasets. In particular, ab-initio molecular dynamics simulations can capture striking effects of anharmonicity near lattice instabilities. A number of high-performance thermoelectric materials are found in the vicinity of lattice instabilities, including Pb chalcogenides PbX, SnSe, Cu2Se, among others. The large phonon anharmonicity found in such compounds suppresses the lattice thermal conductivity, enhancing their thermoelectric efficiency. In this presentation, I will present results from our investigations of phonons in these materials using neutron and x-ray scattering combined with first-principles simulations, focusing on anharmonic effects near lattice instabilities. I will show how strong anharmonicity can lead to emergent quasiparticles qualitatively different from harmonic phonons, which we probe in our measurements and simulations of the phonon self-energy. Commonalities between systems will be highlighted, including connections between strong anharmonicity and the electronic structure. Funding from US DOE, Office of Basic Energy Sciences, Materials Science and Engineering Division, Office of Science Early Career program (DE-SC0016166), and as part of the S3TEC EFRC (DE-SC0001299).

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

Nanostructure design for drastic reduction of thermal conductivity while preserving high electrical conductivity.

PubMed

Nakamura, Yoshiaki

2018-01-01

The design and fabrication of nanostructured materials to control both thermal and electrical properties are demonstrated for high-performance thermoelectric conversion. We have focused on silicon (Si) because it is an environmentally friendly and ubiquitous element. High bulk thermal conductivity of Si limits its potential as a thermoelectric material. The thermal conductivity of Si has been reduced by introducing grains, or wires, yet a further reduction is required while retaining a high electrical conductivity. We have designed two different nanostructures for this purpose. One structure is connected Si nanodots (NDs) with the same crystal orientation. The phonons scattering at the interfaces of these NDs occurred and it depended on the ND size. As a result of phonon scattering, the thermal conductivity of this nanostructured material was below/close to the amorphous limit. The other structure is Si films containing epitaxially grown Ge NDs. The Si layer imparted high electrical conductivity, while the Ge NDs served as phonon scattering bodies reducing thermal conductivity drastically. This work gives a methodology for the independent control of electron and phonon transport using nanostructured materials. This can bring the realization of thermoelectric Si-based materials that are compatible with large scale integrated circuit processing technologies.

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.

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

Phononic thermal conductivity in silicene: the role of vacancy defects and boundary scattering

NASA Astrophysics Data System (ADS)

Barati, M.; Vazifehshenas, T.; Salavati-fard, T.; Farmanbar, M.

2018-04-01

We calculate the thermal conductivity of free-standing silicene using the phonon Boltzmann transport equation within the relaxation time approximation. In this calculation, we investigate the effects of sample size and different scattering mechanisms such as phonon–phonon, phonon-boundary, phonon-isotope and phonon-vacancy defect. We obtain some similar results to earlier works using a different model and provide a more detailed analysis of the phonon conduction behavior and various mode contributions. We show that the dominant contribution to the thermal conductivity of silicene, which originates from the in-plane acoustic branches, is about 70% at room temperature and this contribution becomes larger by considering vacancy defects. Our results indicate that while the thermal conductivity of silicene is significantly suppressed by the vacancy defects, the effect of isotopes on the phononic transport is small. Our calculations demonstrate that by removing only one of every 400 silicon atoms, a substantial reduction of about 58% in thermal conductivity is achieved. Furthermore, we find that the phonon-boundary scattering is important in defectless and small-size silicene samples, especially at low temperatures.

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.

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.

Time Resolved X-Ray Diffraction Study of Acoustoelectrically Amplified Phonons.

NASA Astrophysics Data System (ADS)

Chapman, Leroy Dean

X-rays diffracted by nearly perfect crystals of n-type InSb have been investigated in the presence of intense acoustoelectrically (A.E.) amplified phonons. The fact that these phonons are nearly monochromatic and have a well defined propagation and polarization direction presents an excellent opportunity to investigate the nature of x -ray photon-phonon scattering in a diffracting crystal. The Debye-Waller factor which accounts for the attenuation of diffracted x-ray intensities due to thermal phonons is reflection dependent owing to its sin (theta)/(lamda) dependence. We have performed experiments comparing the (004) and (008) anomalously transmitted intensities as a function of A.E. amplified flux. The attenuation of both reflections due to the amplified phonons was the same in direct contradiction to an expected sin (theta)/(lamda) dependence. Some possible reasons for this failure are discussed. In a Bragg reflection scattering geometry, the intense monochromatic amplified phonons give rise to satellite peaks symmetrically located about the central elastic Brag peak in a rocking profile. We report in this thesis on the first observation of satellites in a thin crystal Laue transmission geometry. We have theoretically simulated the rocking profiles with some success. The A.E. amplification process in InSb is strongly favored for {110} propagation fast transverse (FT) phonons. In earlier experiments it was found that non-{110} FT phonons were also produced during the amplification process. We have developed a time resolved x-ray counting system which, in conjunction with a spatially resolved x-ray beam and a localized, traveling A.E. phonon distribution, allow the time evolution of the amplified distribution to be followed. We report on time resolved measurements for both the symmetric Bragg and Laue geometries from which we can determine when and where non-{110 } FT flux is generated and restrict the possible mechanisms for its generation.

Low lattice thermal conductivity of stanene

NASA Astrophysics Data System (ADS)

Peng, Bo; Zhang, Hao; Shao, Hezhu; Xu, Yuchen; Zhang, Xiangchao; Zhu, Heyuan

2016-02-01

A fundamental understanding of phonon transport in stanene is crucial to predict the thermal performance in potential stanene-based devices. By combining first-principle calculation and phonon Boltzmann transport equation, we obtain the lattice thermal conductivity of stanene. A much lower thermal conductivity (11.6 W/mK) is observed in stanene, which indicates higher thermoelectric efficiency over other 2D materials. The contributions of acoustic and optical phonons to the lattice thermal conductivity are evaluated. Detailed analysis of phase space for three-phonon processes shows that phonon scattering channels LA + LA/TA/ZA ↔ TA/ZA are restricted, leading to the dominant contributions of high-group-velocity LA phonons to the thermal conductivity. The size dependence of thermal conductivity is investigated as well for the purpose of the design of thermoelectric nanostructures.

Dependence of mobility on the electron concentration upon scattering at polar optical phonons in A{sup III}–N nitrides

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

Borisenko, S. I., E-mail: sib@tpu.ru

2016-04-15

The dependence of the effective relaxation time on the electron concentration in A{sup III}–N nitrides in the case of electron scattering at polar longitudinal optical phonons is calculated by the marching method. The method takes into account the inelasticity of electron scattering at polar optical phonons for nitrides in the zinc-blende approximation. The calculations show a substantial increase in mobility in samples with a degenerate electron gas, if screening of the long-range potential of polar longitudinal optical phonons is taken into account.

Effect of Al doping on thermoelectric power of Mg1-xAlxB2 phonon drag and carrier diffusion contribution

NASA Astrophysics Data System (ADS)

Singh, Namita; Sharma, Roopam; Khenata, R.; Varshney, Dinesh

2018-05-01

The carrier diffusion contribution to the thermoelectric power (Scdiff) is calculated for MgB2, Mg0.9A10.1B2 and drag Mg0.8Al0.2B2 within two energy gap method. The phonon drag thermoelectric power (Sphdrag) in normal state dominate and is an artifact of strong phonon-impurity and phonon scattering mechanism. The conductivity within the relaxation time approximation for π and σ band carriers has been taken into account ignoring a possible energy dependence of the scattering rates. Both these channels for heat transfer are clubbed to get total thermoelectric power (Stotal) which starts departing from linear temperature dependence at about 150 K, before increasing at higher temperatures weakly. The anomalies reported are well accounted in terms of the scattering mechanism by phonon drag and carrier scattering with impurities, shows similar results as those revealed from experiments.

Influence of point defects on the thermal conductivity in FeSi

NASA Astrophysics Data System (ADS)

Stern, Robin; Wang, Tao; Carrete, Jesús; Mingo, Natalio; Madsen, Georg K. H.

2018-05-01

The unique transport properties of B20 FeSi have been investigated for decades. The progress in theoretical calculations allows the explanation and prediction of more and more of such properties. In this paper we investigate the lattice thermal conductivity of FeSi. Calculation for pristine FeSi severely overestimates the lattice thermal conductivity compared to experiment. We point out that the defect concentration can be considerably larger than indicated by the Hall coefficient. The defect formation energies are calculated and it is found that a substantial amount of iron vacancies can form at thermal equilibrium. These will lead to an increased phonon scattering. To explain the thermal conductivity of FeSi, we consider phonon-phonon, isotope, and phonon-defect scattering to assess possible scattering mechanisms. The calculated thermal conductivities indicate that phonon-defect scattering is important in order to explain the reported experimental values.

Size effect on thermoelectric properties of Bi2Te3 nanoparticles

NASA Astrophysics Data System (ADS)

Choudhary, K. K.; Sharma, Uttam; Lodhi, Pavitra Devi; Kaurav, Netram

2018-05-01

Bi2Te3 nanoparticles exhibit size dependent thermoelectric properties which gives an opportunity to tune the size for optimization of the thermoelectric figure of merit (ZT). We have quantitatively analyzed the thermoelectric properties of Bi2Te3 using phonon scattering mechanism by incorporating the scattering of phonons with defects, grain boundaries, electrons and Umklapp phonon scatterings. The maximum value of ZT = 0.92 is obtained at T = 400 K for 30 nm Bi2Te3 nanoparticles in comparison to ZT = 0.45 for 150 nm nanoparticles at the same temperature. With decrease in size of nanoparticles interface volume ratio increases which increase the phonon scatterings with grain boundaries and point defects, results in decrease in thermal conductivity due to reduction in mean free path of phonons. As a result of decrease in thermal conductivity (κ), Seeback coefficient (S) and ZT increases.

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.

A numerical study of the nanoribbon field-effect transistors under the ballistic and dissipative transport

NASA Astrophysics Data System (ADS)

Ghoreishi, Seyed Saleh; Yousefi, Reza; Saghafi, Kamyar; Aderang, Habib

2017-08-01

In this article, a detailed performance comparison is made between ballistic and dissipative quantum transport of metal oxide semicondutor-like graphene nanoribbon field-effect transistor, in ON and OFF-state conditions. By the self-consistent mode-space non-equilibrium Green's function approach, inter- and intraband scattering is accounted and the role of acoustic and optical phonon scattering on the performance of the devices is evaluated. We found that in this structure the dominant mechanism of scattering changes according to the ranges of voltage bias. Under large biasing conditions, the influence of optical phonon scattering becomes important. Also, the ambipolar and OFF-current are impressed by the phonon-assisted band-to-band tunneling and increased considerably compared to the ballistic conditions, although sub-threshold swing degrades due to optical phonon scattering.

First-principles prediction of phononic thermal conductivity of silicene: A comparison with graphene

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

Gu, Xiaokun; Yang, Ronggui, E-mail: Ronggui.Yang@Colorado.Edu

2015-01-14

There has been great interest in two-dimensional materials, beyond graphene, for both fundamental sciences and technological applications. Silicene, a silicon counterpart of graphene, has been shown to possess some better electronic properties than graphene. However, its thermal transport properties have not been fully studied. In this paper, we apply the first-principles-based phonon Boltzmann transport equation to investigate the thermal conductivity of silicene as well as the phonon scattering mechanisms. Although both graphene and silicene are two-dimensional crystals with similar crystal structure, we find that phonon transport in silicene is quite different from that in graphene. The thermal conductivity of silicenemore » shows a logarithmic increase with respect to the sample size due to the small scattering rates of acoustic in-plane phonon modes, while that of graphene is finite. Detailed analysis of phonon scattering channels shows that the linear dispersion of the acoustic out-of-plane (ZA) phonon modes, which is induced by the buckled structure, makes the long-wavelength longitudinal acoustic phonon modes in silicene not as efficiently scattered as that in graphene. Compared with graphene, where most of the heat is carried by the acoustic out-of-plane (ZA) phonon modes, the ZA phonon modes in silicene only have ∼10% contribution to the total thermal conductivity, which can also be attributed to the buckled structure. This systematic comparison of phonon transport and thermal conductivity of silicene and graphene using the first-principle-based calculations shed some light on other two-dimensional materials, such as two-dimensional transition metal dichalcogenides.« less

Ab initio phonon thermal transport in monolayer InSe, GaSe, GaS, and alloys

NASA Astrophysics Data System (ADS)

Pandey, Tribhuwan; Parker, David S.; Lindsay, Lucas

2017-11-01

We compare vibrational properties and phonon thermal conductivities (κ) of monolayer InSe, GaSe, and GaS systems using density functional theory and Peierls-Boltzmann transport methods. In going from InSe to GaSe to GaS, system mass decreases giving both increasing acoustic phonon velocities and decreasing scattering of these heat-carrying modes with optic phonons, ultimately giving {κ }{InSe}< {κ }{GaSe}< {κ }{GaS}. This behavior is demonstrated by correlating the scattering phase space limited by fundamental conservation conditions with mode scattering rates and phonon dispersions for each material. We also show that, unlike flat monolayer systems such as graphene, in InSe, GaSe and GaS thermal transport is governed by in-plane vibrations. Alloying of InSe, GaSe, and GaS systems provides an effective method for modulating their κ through intrinsic vibrational modifications and phonon scattering from mass disorder giving reductions ˜2-3.5 times. This disorder also suppresses phonon mean free paths in the alloy systems compared to those in their crystalline counterparts. This work provides fundamental insights of lattice thermal transport from basic vibrational properties for an interesting set of two-dimensional materials.

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.

Bogolon-mediated electron capture by impurities in hybrid Bose-Fermi systems

NASA Astrophysics Data System (ADS)

Boev, M. V.; Kovalev, V. M.; Savenko, I. G.

2018-04-01

We investigate the processes of electron capture by a Coulomb impurity center residing in a hybrid system consisting of spatially separated two-dimensional layers of electron and Bose-condensed dipolar exciton gases coupled via the Coulomb forces. We calculate the probability of the electron capture accompanied by the emission of a single Bogoliubov excitation (bogolon), similar to regular phonon-mediated scattering in solids. Furthermore, we study the electron capture mediated by the emission of a pair of bogolons in a single capture event and show that these processes not only should be treated in the same order of the perturbation theory, but also they give a more important contribution than single-bogolon-mediated capture, in contrast with regular phonon scattering.

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

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

Bolmatov, Dima; Zhernenkov, Mikhail; Zav’yalov, Dmitry

Here in this work we report on terahertz phononic excitations in 2D gold nanoparticle arrays in a water matrix through a series of large-scale molecular dynamics simulations. For the first time, we observe acoustic Dirac-like crossings in H (H 2O) atomic (molecular) networks which emerge due to an intraband phononic scattering. These crossings are the phononic fingerprints of ice-like arrangements of H (H 2O) atomic (molecular) networks at nanometer scale. We reveal how phononic excitations in metallic nanoparticles and the water matrix reciprocally impact on one another providing the mechanism for the THz phononics manipulation via structural engineering. In addition,more » we show that by tuning the arrangement of 2D gold nanoparticle assemblies the Au phononic polarizations experience sub-terahertz hybridization (Kohn anomaly) due to surface electron-phonon relaxation processes. This opens the way for the sound control and manipulation in soft matter metamaterials at nanoscale.« less

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.

Thermally Driven Electronic Topological Transition in FeTi

NASA Astrophysics Data System (ADS)

Yang, F. C.; Muñoz, J. A.; Hellman, O.; Mauger, L.; Lucas, M. S.; Tracy, S. J.; Stone, M. B.; Abernathy, D. L.; Xiao, Yuming; Fultz, B.

2016-08-01

Ab initio molecular dynamics, supported by inelastic neutron scattering and nuclear resonant inelastic x-ray scattering, showed an anomalous thermal softening of the M5- phonon mode in B 2 -ordered FeTi that could not be explained by phonon-phonon interactions or electron-phonon interactions calculated at low temperatures. A computational investigation showed that the Fermi surface undergoes a novel thermally driven electronic topological transition, in which new features of the Fermi surface arise at elevated temperatures. The thermally induced electronic topological transition causes an increased electronic screening for the atom displacements in the M5- phonon mode and an adiabatic electron-phonon interaction with an unusual temperature dependence.

Ultracold-neutron production and up-scattering in superfluid helium between 1.1 K and 2.4 K

NASA Astrophysics Data System (ADS)

Leung, K. K. H.; Ivanov, S.; Piegsa, F. M.; Simson, M.; Zimmer, O.

2016-02-01

Ultracold neutrons (UCNs) were produced in superfluid helium using the PF1B cold-neutron beam facility at the Institut Laue-Langevin. A 4-liter beryllium-coated converter volume with a mechanical valve and windowless stainless-steel extraction system were used to accumulate and guide UCNs to a detector at room temperature. At a converter temperature of 1.08 K the total storage time constant in the vessel was (20.3 ±1.2 )s and the number of UCNs counted after accumulated was 91 700 ±300 . From this, we derive a volumetric UCN production rate of (6.9 ±1.7 ) cm-3s-1 , which includes a correction for losses in the converter during UCN extraction caused by the short storage time, but not accounting for UCN transport and detection efficiencies. The up-scattering rate of UCNs caused by excitations in the superfluid was studied by scanning the temperature between 1.2 K and 2.4 K . Using the temperature-dependent UCN production rate calculated from inelastic neutron scattering data, the only UCN up-scattering process found to occur was from two-phonon scattering. Our analysis for T <1.95 K rules out the contributions from roton-phonon scattering to <29 % (95% C.I.) and from one-phonon absorption to <47 % (95% C.I.) of their predicted levels.

Increased Phonon Scattering by Nanograins and Point Defects in Nanostructured Silicon with a Low Concentration of Germanium

NASA Astrophysics Data System (ADS)

Zhu, G. H.; Lee, H.; Lan, Y. C.; Wang, X. W.; Joshi, G.; Wang, D. Z.; Yang, J.; Vashaee, D.; Guilbert, H.; Pillitteri, A.; Dresselhaus, M. S.; Chen, G.; Ren, Z. F.

2009-05-01

The mechanism for phonon scattering by nanostructures and by point defects in nanostructured silicon (Si) and the silicon germanium (Ge) alloy and their thermoelectric properties are investigated. We found that the thermal conductivity is reduced by a factor of 10 in nanostructured Si in comparison with bulk crystalline Si. However, nanosize interfaces are not as effective as point defects in scattering phonons with wavelengths shorter than 1 nm. We further found that a 5at.% Ge replacing Si is very efficient in scattering phonons shorter than 1 nm, resulting in a further thermal conductivity reduction by a factor of 2, thereby leading to a thermoelectric figure of merit 0.95 for Si95Ge5, similar to that of large grained Si80Ge20 alloys.

Low lattice thermal conductivity of stanene

PubMed Central

Peng, Bo; Zhang, Hao; Shao, Hezhu; Xu, Yuchen; Zhang, Xiangchao; Zhu, Heyuan

2016-01-01

A fundamental understanding of phonon transport in stanene is crucial to predict the thermal performance in potential stanene-based devices. By combining first-principle calculation and phonon Boltzmann transport equation, we obtain the lattice thermal conductivity of stanene. A much lower thermal conductivity (11.6 W/mK) is observed in stanene, which indicates higher thermoelectric efficiency over other 2D materials. The contributions of acoustic and optical phonons to the lattice thermal conductivity are evaluated. Detailed analysis of phase space for three-phonon processes shows that phonon scattering channels LA + LA/TA/ZA ↔ TA/ZA are restricted, leading to the dominant contributions of high-group-velocity LA phonons to the thermal conductivity. The size dependence of thermal conductivity is investigated as well for the purpose of the design of thermoelectric nanostructures. PMID:26838731

Excitonic luminescence upconversion in a two-dimensional semiconductor

DOE PAGES

Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.; ...

2015-12-21

Photon upconversion is an elementary light-matter interaction process in which an absorbed photon is re-emitted at higher frequency after extracting energy from the medium. Furthermore, this phenomenon lies at the heart of optical refrigeration in solids(1), where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities(2) or exciton-phonon coupling(3). We demonstrate a luminescence upconversion process from a negatively charged exciton to a neutral exciton resonance in monolayer WSe2, producing spontaneous anti-Stokes emission with an energy gain of 30 meV. Polarization-resolved measurements find this process to be valley selective, unique to monolayer semiconductors(4). Since the charged exciton binding energy(5) closelymore » matches the 31 meV A(1)' optical phonon(6-9), we ascribe the spontaneous excitonic anti-Stokes to doubly resonant Raman scattering, where the incident and outgoing photons are in resonance with the charged and neutral excitons, respectively. Additionally, we resolve a charged exciton doublet with a 7 meV splitting, probably induced by exchange interactions, and show that anti-Stokes scattering is efficient only when exciting the doublet peak resonant with the phonon, further confirming the excitonic doubly resonant picture.« less

Nanostructure design for drastic reduction of thermal conductivity while preserving high electrical conductivity

PubMed Central

Nakamura, Yoshiaki

2018-01-01

Abstract The design and fabrication of nanostructured materials to control both thermal and electrical properties are demonstrated for high-performance thermoelectric conversion. We have focused on silicon (Si) because it is an environmentally friendly and ubiquitous element. High bulk thermal conductivity of Si limits its potential as a thermoelectric material. The thermal conductivity of Si has been reduced by introducing grains, or wires, yet a further reduction is required while retaining a high electrical conductivity. We have designed two different nanostructures for this purpose. One structure is connected Si nanodots (NDs) with the same crystal orientation. The phonons scattering at the interfaces of these NDs occurred and it depended on the ND size. As a result of phonon scattering, the thermal conductivity of this nanostructured material was below/close to the amorphous limit. The other structure is Si films containing epitaxially grown Ge NDs. The Si layer imparted high electrical conductivity, while the Ge NDs served as phonon scattering bodies reducing thermal conductivity drastically. This work gives a methodology for the independent control of electron and phonon transport using nanostructured materials. This can bring the realization of thermoelectric Si-based materials that are compatible with large scale integrated circuit processing technologies. PMID:29371907

Impact of optical phonon scattering on inversion channel mobility in 4H-SiC trenched MOSFETs

NASA Astrophysics Data System (ADS)

Kutsuki, Katsuhiro; Kawaji, Sachiko; Watanabe, Yukihiko; Onishi, Toru; Fujiwara, Hirokazu; Yamamoto, Kensaku; Yamamoto, Toshimasa

2017-04-01

Temperature characteristics of the channel mobility were investigated for 4H-SiC trenched MOSFETs in the range from 30 to 200 °C. The conventional model of channel mobility limited by carrier scattering is based on Si-MOSFETs and shows a greatly different channel mobility from the experimental value, especially at high temperatures. On the other hand, our improved mobility model taking into account optical phonon scattering yielded results in excellent agreement with experimental results. Moreover, the major factors limiting the channel mobility were found to be Coulomb scattering in a low effective field (<0.7 MV/cm) and optical phonon scattering in a high effective field.

Ab initio phonon thermal transport in monolayer InSe, GaSe, GaS, and alloys

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

Pandey, Tribhuwan; Parker, David S.; Lindsay, Lucas

We compare vibrational properties and phonon thermal conductivities (κ) of monolayer InSe, GaSe and GaS systems using density functional theory and Peierls-Boltzmann transport methods. In going from InSe to GaSe to GaS, system mass decreases giving both increasing acoustic phonon velocities and decreasing scattering of these heat-carrying modes with optic phonons, ultimately giving κInSe< κGaSe< κGaS. This behavior is demonstrated by correlating the scattering phase space limited by fundamental conservation conditions with mode scattering rates and phonon dispersions for each material. We also show that, unlike flat monolayer systems such as graphene, thermal transport is governed by in-plane vibrations inmore » InSe, GaSe and GaS, similar to buckled monolayer materials such as silicene. Alloying of InSe, GaSe and GaS systems provides an effective method for modulating their κ through intrinsic vibrational modifications and phonon scattering from mass disorder giving reductions ~2-3.5 times. This disorder also suppresses phonon mean free paths in the alloy systems compared to those in their crystalline counterparts. This work provides fundamental insights of lattice thermal transport from basic vibrational properties for an interesting set of two-dimensional materials.« less

Temperature-dependent spectral linewidths of terahertz Bloch oscillations in biased semiconductor superlattices

NASA Astrophysics Data System (ADS)

Unuma, Takeya; Matsuda, Aleph

2018-04-01

We investigate temperature-dependent spectral linewidths of Bloch oscillations in biased semiconductor superlattices experimentally and theoretically. The spectral linewidth in a GaAs-based superlattice determined by terahertz emission spectroscopy becomes larger gradually as temperature increases from 80 to 320 K. This behavior can be quantitatively reproduced by a microscopic theory of the spectral linewidth that has been extended to treat the phonon scattering and interface roughness scattering of electrons on a Wannier-Stark ladder. A detailed comparison between the terahertz measurements and theoretical simulations reveals that the LO phonon absorption process governs the increase in the spectral linewidth with increasing temperature.

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.

Phonon-mediated spin-flipping mechanism in the spin ices Dy 2 Ti 2 O 7 and Ho 2 Ti 2 O 7

DOE PAGES

Ruminy, M.; Chi, S.; Calder, S.; ...

2017-02-21

To understand emergent magnetic monopole dynamics in the spin ices Ho 2Ti 2O 7 and Dy 2Ti 2O 7, it is necessary to investigate the mechanisms by which spins flip in these materials. Presently there are thought to be two processes: quantum tunneling at low and intermediate temperatures and thermally activated at high temperatures. We identify possible couplings between crystal field and optical phonon excitations and construct a strictly constrained model of phonon-mediated spin flipping that quantitatively describes the high-temperature processes in both compounds, as measured by quasielastic neutron scattering. We support the model with direct experimental evidence of themore » coupling between crystal field states and optical phonons in Ho 2Ti 2O 7.« less

Thermally Driven Electronic Topological Transition in FeTi

DOE PAGES

Yang, F. C.; Muñoz, J. A.; Hellman, O.; ...

2016-08-08

In this paper, ab initio molecular dynamics, supported by inelastic neutron scattering and nuclear resonant inelastic x-ray scattering, showed an anomalous thermal softening of the M 5 - phonon mode in B2-ordered FeTi that could not be explained by phonon-phonon interactions or electron-phonon interactions calculated at low temperatures. A computational investigation showed that the Fermi surface undergoes a novel thermally driven electronic topological transition, in which new features of the Fermi surface arise at elevated temperatures. Finally, the thermally induced electronic topological transition causes an increased electronic screening for the atom displacements in the M 5 - phonon mode andmore » an adiabatic electron-phonon interaction with an unusual temperature dependence.« less

Inelastic x-ray scattering measurements of phonon dynamics in URu 2Si 2

DOE PAGES

Gardner, D. R.; Bonnoit, C. J.; Chisnell, R.; ...

2016-02-11

In this paper, we study high-resolution inelastic x-ray scattering measurements of the acoustic phonons of URu 2Si 2. At all temperatures, the longitudinal acoustic phonon linewidths are anomalously broad at small wave vectors revealing a previously unknown anharmonicity. The phonon modes do not change significantly upon cooling into the hidden order phase. In addition, our data suggest that the increase in thermal conductivity in the hidden order phase cannot be driven by a change in phonon dispersions or lifetimes. Hence, the phonon contribution to the thermal conductivity is likely much less significant compared to that of the magnetic excitations inmore » the low temperature phase.« less

Phonon transport control by nanoarchitecture including epitaxial Ge nanodots for Si-based thermoelectric materials

PubMed Central

Yamasaka, Shuto; Nakamura, Yoshiaki; Ueda, Tomohiro; Takeuchi, Shotaro; Sakai, Akira

2015-01-01

Phonon transport in Si films was controlled using epitaxially-grown ultrasmall Ge nanodots (NDs) with ultrahigh density for the purpose of developing Si-based thermoelectric materials. The Si/Ge ND stacked structures, which were formed by the ultrathin SiO2 film technique, exhibited lower thermal conductivities than those of the conventional nanostructured SiGe bulk alloys, despite the stacked structures having a smaller Ge fraction. This came from the large thermal resistance caused by phonon scattering at the Si/Ge ND interfaces. The phonon scattering can be controlled by the Ge ND structure, which was independent of Si layer structure for carrier transport. These results demonstrate the effectiveness of ultrasmall epitaxial Ge NDs as phonon scattering sources, opening up a route for the realisation of Si-based thermoelectric materials. PMID:26434678

Ballistic and Diffusive Thermal Conductivity of Graphene

NASA Astrophysics Data System (ADS)

Saito, Riichiro; Masashi, Mizuno; Dresselhaus, Mildred S.

2018-02-01

This paper is a contribution to the Physical Review Applied collection in memory of Mildred S. Dresselhaus. Phonon-related thermal conductivity of graphene is calculated as a function of the temperature and sample size of graphene in which the crossover of ballistic and diffusive thermal conductivity occurs at around 100 K. The diffusive thermal conductivity of graphene is evaluated by calculating the phonon mean free path for each phonon mode in which the anharmonicity of a phonon and the phonon scattering by a 13C isotope are taken into account. We show that phonon-phonon scattering of out-of-plane acoustic phonon by the anharmonic potential is essential for the largest thermal conductivity. Using the calculated results, we can design the optimum sample size, which gives the largest thermal conductivity at a given temperature for applying thermal conducting devices.

Temperature-dependent thermal conductivities of 1D semiconducting nanowires via four-point-probe 3-ω method.

PubMed

Lee, Seung-Yong; Lee, Mi-Ri; Park, No-Won; Kim, Gil-Sung; Choi, Heon-Jin; Choi, Tae-Youl; Lee, Sang-Kwon

2013-12-13

We report on a systematic study of the thermal transport characteristics of both as-grown zinc oxide and gallium nitride nanowires (NWs) via the four-point-probe 3-ω method in the temperature range 130-300 K. Both as-grown NWs were synthesized by a vapor-liquid-solid growth mechanism, and show clear n-type semiconducting behavior without any defects, which enables both the NWs to be promising candidates for thermoelectric materials. To measure the thermal conductivities of both NWs with lower heat loss and measurement errors, the suspended structures were formed by a combination of an e-beam lithography process and a random dispersion method. The measured thermal conductivities of both NWs are greatly reduced compared to their bulk materials due to the enhanced phonon scattering via the size effect and dopants (impurities). Furthermore, we observed that the Umklapp peaks of both NWs are shifted to a higher temperature than those of their bulk counterparts, indicating that phonon-boundary scattering dominates over other phonon scattering due to the size effect.

Thermal transport in nanocrystalline Si and SiGe by ab initio based Monte Carlo simulation.

PubMed

Yang, Lina; Minnich, Austin J

2017-03-14

Nanocrystalline thermoelectric materials based on Si have long been of interest because Si is earth-abundant, inexpensive, and non-toxic. However, a poor understanding of phonon grain boundary scattering and its effect on thermal conductivity has impeded efforts to improve the thermoelectric figure of merit. Here, we report an ab-initio based computational study of thermal transport in nanocrystalline Si-based materials using a variance-reduced Monte Carlo method with the full phonon dispersion and intrinsic lifetimes from first-principles as input. By fitting the transmission profile of grain boundaries, we obtain excellent agreement with experimental thermal conductivity of nanocrystalline Si [Wang et al. Nano Letters 11, 2206 (2011)]. Based on these calculations, we examine phonon transport in nanocrystalline SiGe alloys with ab-initio electron-phonon scattering rates. Our calculations show that low energy phonons still transport substantial amounts of heat in these materials, despite scattering by electron-phonon interactions, due to the high transmission of phonons at grain boundaries, and thus improvements in ZT are still possible by disrupting these modes. This work demonstrates the important insights into phonon transport that can be obtained using ab-initio based Monte Carlo simulations in complex nanostructured materials.

Thermal transport in nanocrystalline Si and SiGe by ab initio based Monte Carlo simulation

PubMed Central

Yang, Lina; Minnich, Austin J.

2017-01-01

Nanocrystalline thermoelectric materials based on Si have long been of interest because Si is earth-abundant, inexpensive, and non-toxic. However, a poor understanding of phonon grain boundary scattering and its effect on thermal conductivity has impeded efforts to improve the thermoelectric figure of merit. Here, we report an ab-initio based computational study of thermal transport in nanocrystalline Si-based materials using a variance-reduced Monte Carlo method with the full phonon dispersion and intrinsic lifetimes from first-principles as input. By fitting the transmission profile of grain boundaries, we obtain excellent agreement with experimental thermal conductivity of nanocrystalline Si [Wang et al. Nano Letters 11, 2206 (2011)]. Based on these calculations, we examine phonon transport in nanocrystalline SiGe alloys with ab-initio electron-phonon scattering rates. Our calculations show that low energy phonons still transport substantial amounts of heat in these materials, despite scattering by electron-phonon interactions, due to the high transmission of phonons at grain boundaries, and thus improvements in ZT are still possible by disrupting these modes. This work demonstrates the important insights into phonon transport that can be obtained using ab-initio based Monte Carlo simulations in complex nanostructured materials. PMID:28290484

Using high pressure to study thermal transport and phonon scattering mechanisms

NASA Astrophysics Data System (ADS)

Hohensee, Gregory Thomas

The aerospace industry studies nanocomposites for heat dissipation and moderation of thermal expansion, and the semiconductor industry faces a Joule heating barrier in devices with high power density. My primary experimental tools are the diamond anvil cell (DAC) coupled with time-domain thermoreflectance (TDTR). TDTR is a precise optical method well-suited to measuring thermal conductivities and conductances at the nanoscale and across interfaces. The DAC-TDTR method yields thermal property data as a function of pressure, rather than temperature. This relatively unexplored independent variable can separate the components of thermal conductance and serve as an independent test for phonon-defect scattering models. I studied the effect of non-equilibrium thermal transport at the aluminum-coated surface of an exotic cuprate material Ca9La5Cu 24O41, which boasts a tenfold enhanced thermal conductivity along one crystalline axis where two-leg copper-oxygen spin-ladder structures carry heat in the form of thermalized magnetic excitations. Highly anisotropic materials are of interest for controlled thermal management applications, and the spin-ladder magnetic heat carriers ("magnons") are not well understood. I found that below room temperature, the apparent thermal conductivity of Ca9La5Cu24O41 depends on the frequency of the applied surface heating in TDTR. This occurs because the thermal penetration depth in the TDTR experiment is comparable to the length-scale for the equilibration of the magnons that are the dominant channel for heat conduction and the phonons that dominate the heat capacity. I applied a two-temperature model to analyze the TDTR data and extracted an effective volumetric magnon-phonon coupling parameter g for Ca9La5Cu24O 41 at temperatures from 75 K to 300 K; g varies by approximately two orders of magnitude over this range of temperature and has the value g = 1015 W m-3 K-1 near the peak of the thermal conductivity at T ≈ 180 K. To examine intrinsic phonon-mediated interface conductance between dissimilar materials, I applied DAC-TDTR to measure the thermal conductance of a series of metal-diamond interfaces as a function of pressure up to 50 GPa. The thermal conductance of interfaces between metals and diamond, which has a comparatively high Debye temperature, is often greater than can be accounted for by two phonon-processes, and the nature of heat transport between such dissimilar materials is central to the thermal design of composite materials. The high pressures achievable in a diamond anvil cell can significantly extend the metal phonon density of states to higher frequencies, and can also suppress extrinsic effects by greatly stiffening interface bonding. I measured the interface thermal conductances of Pb, Au0.95Pd0.05, Pt, and Al films deposited on Type 1A natural [100] and Type 2A synthetic [110] diamond anvils, from ambient pressure to 50 GPa. In all cases, the thermal conductances increase weakly or saturate to similar values at high pressure. My results suggest that anharmonic conductance at metal-diamond interfaces is controlled by partial transmission processes, where a diamond phonon that inelastically scatters at the interface absorbs or emits a metal phonon. The thermal conductivity and absolute electrical resistivity of metallic silicon have not been measured previously. I performed regular and beam-offset TDTR to establish the thermal conductivities of Si and Si0.991Ge 0.009 across the semiconductor-metal phase transition and up to 45 GPa. The thermal conductivities of metallic Si and Si(Ge) are comparable to aluminum and indicative of predominantly electronic heat carriers. Metallic Si and Si(Ge) have a transport anisotropy of approximately 1.4, similar to that of beryllium, due to the primitive hexagonal crystal structure. I used the Wiedemann-Franz law to derive the associated electrical resistivity, and found it consistent with the Bloch-Gruneisen model. Not all crystalline point defects are alike in how they scatter phonons and reduce the thermal conductivity of mixed crystals. Heat-carrying phonons in iron (Fe) doped MgO, or [Mg,Fe]O ferropericlase, are known to be resonantly scattered by interaction with a 3.3 THz electronic transition in the high-spin state of the Fe impurities. At sufficiently high pressures, the Fe atoms transition from a high-spin to a low-spin state, which eliminates the resonant interaction and reduces the Fe atoms to simpler point defect phonon scatterers. To study the behavior of phonon-defect scattering with and without this resonant scattering process, I measured the thermal conductivity of Mg0.92Fe0.08 O ferropericlase up to and above the 40--60 GPa spin transition. Fe-doped MgO (ferropericlase) is also a model system relevant to geophysical modeling of the Earth's core-mantle boundary, so data on its thermal transport under pressure is valuable in itself. (Abstract shortened by UMI.).

Thermal conductivity model for nanoporous thin films

NASA Astrophysics Data System (ADS)

Huang, Congliang; Zhao, Xinpeng; Regner, Keith; Yang, Ronggui

2018-03-01

Nanoporous thin films have attracted great interest because of their extremely low thermal conductivity and potential applications in thin thermal insulators and thermoelectrics. Although there are some numerical and experimental studies about the thermal conductivity of nanoporous thin films, a simplified model is still needed to provide a straightforward prediction. In this paper, by including the phonon scattering lifetimes due to film thickness boundary scattering, nanopore scattering and the frequency-dependent intrinsic phonon-phonon scattering, a fitting-parameter-free model based on the kinetic theory of phonon transport is developed to predict both the in-plane and the cross-plane thermal conductivities of nanoporous thin films. With input parameters such as the lattice constants, thermal conductivity, and the group velocity of acoustic phonons of bulk silicon, our model shows a good agreement with available experimental and numerical results of nanoporous silicon thin films. It illustrates that the size effect of film thickness boundary scattering not only depends on the film thickness but also on the size of nanopores, and a larger nanopore leads to a stronger size effect of the film thickness. Our model also reveals that there are different optimal structures for getting the lowest in-plane and cross-plane thermal conductivities.

Compliant energy and momentum conservation in NEGF simulation of electron-phonon scattering in semiconductor nano-wire transistors

NASA Astrophysics Data System (ADS)

Barker, J. R.; Martinez, A.; Aldegunde, M.

2012-05-01

The modelling of spatially inhomogeneous silicon nanowire field-effect transistors has benefited from powerful simulation tools built around the Keldysh formulation of non-equilibrium Green function (NEGF) theory. The methodology is highly efficient for situations where the self-energies are diagonal (local) in space coordinates. It has thus been common practice to adopt diagonality (locality) approximations. We demonstrate here that the scattering kernel that controls the self-energies for electron-phonon interactions is generally non-local on the scale of at least a few lattice spacings (and thus within the spatial scale of features in extreme nano-transistors) and for polar optical phonon-electron interactions may be very much longer. It is shown that the diagonality approximation strongly under-estimates the scattering rates for scattering on polar optical phonons. This is an unexpected problem in silicon devices but occurs due to strong polar SO phonon-electron interactions extending into a narrow silicon channel surrounded by high kappa dielectric in wrap-round gate devices. Since dissipative inelastic scattering is already a serious problem for highly confined devices it is concluded that new algorithms need to be forthcoming to provide appropriate and efficient NEGF tools.

Interface-facilitated energy transport in coupled Frenkel-Kontorova chains

NASA Astrophysics Data System (ADS)

Su, Rui-Xia; Yuan, Zong-Qiang; Wang, Jun; Zheng, Zhi-Gang

2016-04-01

The role of interface couplings on the energy transport of two coupled Frenkel-Kontorova (FK) chains is explored through numerical simulations. In general, it is expected that the interface couplings result in the suppression of heat conduction through the coupled system due to the additional interface phonon-phonon scattering. In the present paper, it is found that the thermal conductivity increases with increasing intensity of interface interactions for weak inter-chain couplings, whereas the heat conduction is suppressed by the interface interaction in the case of strong inter-chain couplings. Based on the phonon spectral energy density method, we demonstrate that the enhancement of energy transport results from the excited phonon modes (in addition to the intrinsic phonon modes), while the strong interface phonon-phonon scattering results in the suppressed energy transport.

Resonant-phonon-assisted THz quantum cascade lasers with metal-metal waveguides.

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

Callebaut, Hans; Kohen, Stephen; Kumar, Sushil

2004-06-01

We report our development of terahertz (THz) quantum-cascade lasers (QCLs) based on two novel features. First, the depopulation of the lower radiative level is achieved through resonant longitudinal optical (LO-)phonon scattering. This depopulation mechanism is robust at high temperatures and high injection levels. In contrast to infrared QCLs that also use LO-phonon scattering for depopulation, in our THz lasers the selectivity of the depopulation scattering is achieved through a combination of resonant tunneling and LO-phonon scattering, hence the term resonant phonon. This resonant-phonon scheme allows a highly selective depopulation of the lower radiative level with a sub-picosecond lifetime, while maintainingmore » a relatively long upper level lifetime (>5 ps) that is due to upper-to-ground-state scattering. The second feature of our lasers is that mode confinement is achieved by using a novel double-sided metal-metal waveguide, which yields an essentially unity mode confinement factor and therefore a low total cavity loss at THz frequencies. Based on these two unique features, we have achieved some record performance, including, but not limited to, the highest pulsed operating temperature of 137 K, the highest continuous-wave operating temperature of 97 K, and the longest wavelength of 141 {micro}m (corresponding to 2.1 THz) without the assistance of a magnetic field.« less

Phonon-interface scattering in multilayer graphene on an amorphous support

PubMed Central

Sadeghi, Mir Mohammad; Jo, Insun; Shi, Li

2013-01-01

The recent studies of thermal transport in suspended, supported, and encased graphene just began to uncover the richness of two-dimensional phonon physics, which is relevant to the performance and reliability of graphene-based functional materials and devices. Among the outstanding questions are the exact causes of the suppressed basal-plane thermal conductivity measured in graphene in contact with an amorphous material, and the layer thickness needed for supported or embedded multilayer graphene (MLG) to recover the high thermal conductivity of graphite. Here we use sensitive in-plane thermal transport measurements of graphene samples on amorphous silicon dioxide to show that full recovery to the thermal conductivity of the natural graphite source has yet to occur even after the MLG thickness is increased to 34 layers, considerably thicker than previously thought. This seemingly surprising finding is explained by long intrinsic scattering mean free paths of phonons in graphite along both basal-plane and cross-plane directions, as well as partially diffuse scattering of MLG phonons by the MLG-amorphous support interface, which is treated by an interface scattering model developed for highly anisotropic materials. Based on the phonon transmission coefficient calculated from reported experimental thermal interface conductance results, phonons emerging from the interface consist of a large component that is scattered across the interface, making rational choice of the support materials a potential approach to increasing the thermal conductivity of supported MLG. PMID:24067656

Observing non-equilibrium state of transport through graphene channel at the nano-second time-scale

NASA Astrophysics Data System (ADS)

Mishra, Abhishek; Meersha, Adil; Raghavan, Srinivasan; Shrivastava, Mayank

2017-12-01

Electrical performance of a graphene FET is drastically affected by electron-phonon inelastic scattering. At high electric fields, the out-of-equilibrium population of optical phonons equilibrates by emitting acoustic phonons, which dissipate the energy to heat sinks. The equilibration time of the process is governed by thermal diffusion time, which is few nano-seconds for a typical graphene FET. The nano-second time-scale of the process keeps it elusive to conventional steady-state or DC measurement systems. Here, we employ a time-domain reflectometry-based technique to electrically probe the device for few nano-seconds and investigate the non-equilibrium state. For the first time, the transient nature of electrical transport through graphene FET is revealed. A maximum change of 35% in current and 50% in contact resistance is recorded over a time span of 8 ns, while operating graphene FET at a current density of 1 mA/μm. The study highlights the role of intrinsic heating (scattering) in deciding metal-graphene contact resistance and transport through the graphene channel.

Hot electron energy relaxation in lattice-matched InAlN/AlN/GaN heterostructures: The sum rules for electron-phonon interactions and hot-phonon effect

NASA Astrophysics Data System (ADS)

Zhang, J.-Z.; Dyson, A.; Ridley, B. K.

2015-01-01

Using the dielectric continuum (DC) and three-dimensional phonon (3DP) models, energy relaxation (ER) of the hot electrons in the quasi-two-dimensional channel of lattice-matched InAlN/AlN/GaN heterostructures is studied theoretically, taking into account non-equilibrium polar optical phonons, electron degeneracy, and screening from the mobile electrons. The electron power dissipation (PD) and ER time due to both half-space and interface phonons are calculated as functions of the electron temperature Te using a variety of phonon lifetime values from experiment, and then compared with those evaluated by the 3DP model. Thereby, particular attention is paid to examination of the 3DP model to use for the hot-electron relaxation study. The 3DP model yields very close results to the DC model: With no hot phonons or screening, the power loss calculated from the 3DP model is 5% smaller than the DC power dissipation, whereas slightly larger 3DP power loss (by less than 4% with a phonon lifetime from 0.1 to 1 ps) is obtained throughout the electron temperature range from room temperature to 2500 K after including both the hot-phonon effect (HPE) and screening. Very close results are obtained also for ER time with the two phonon models (within a 5% of deviation). However, the 3DP model is found to underestimate the HPE by 9%. The Mori-Ando sum rule is restored by which it is proved that the PD values obtained from the DC and 3DP models are in general different in the spontaneous phonon emission process, except when scattering with interface phonons is sufficiently weak, or when the degenerate modes condition is imposed, which is also consistent with Register's scattering rate sum rule. The discrepancy between the DC and 3DP results is found to be caused by how much the high-energy interface phonons contribute to the ER: their contribution is enhanced in the spontaneous emission process but is dramatically reduced after including the HPE. Our calculation with both phonon models has obtained a great fall in ER time at low electron temperatures (Te < 750 K) and slow decrease at the high temperatures with the use of decreasing phonon lifetime with Te. The calculated temperature dependence of the relaxation time and the high-temperature relaxation time ˜0.09 ps are in good agreement with experimental results.

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.

Neutron inelastic scattering measurements of low-energy phonons in the multiferroic BiFeO 3

DOE PAGES

Schneeloch, John A.; Xu, Zhijun; Wen, Jinsheng; ...

2015-02-10

In this study, we present neutron inelastic scattering measurements of the low-energy phonons in single crystal BiFeO 3. The dispersions of the three acoustic phonon modes (LA along [100], TA 1 along [010], and TA 2 along [110]) and two low-energy optic phonon modes (LO and TO 1) have been mapped out between 300 and 700 K. Elastic constants are extracted from the phonon measurements. The energy linewidths of both TA phonons at the zone boundary clearly broaden when the system is warmed toward the magnetic ordering temperature T N=640 K. In conclusion, this suggests that the magnetic order andmore » low-energy lattice dynamics in this multiferroic material are coupled.« less

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 numbers of scatterers. Also, since both extended methods provide analytic solutions, they may give further insights into the factors that govern the behaviour of time-varying phononic crystals. These extended methods may now be used to design an active phononic crystal that could demonstrate new or enhanced properties.

Ultrafast Spectral Photoresponse of Bilayer Graphene: Optical Pump-Terahertz Probe Spectroscopy.

PubMed

Kar, Srabani; Nguyen, Van Luan; Mohapatra, Dipti R; Lee, Young Hee; Sood, A K

2018-02-27

Photoinduced terahertz conductivity Δσ(ω) of Bernal stacked bilayer graphene (BLG) with different dopings is measured by time-resolved optical pump terahertz probe spectroscopy. The real part of photoconductivity Δσ(ω) (Δσ Re (ω)) is positive throughout the spectral range 0.5-2.5 THz in low-doped BLG. This is in sharp contrast to Δσ(ω) for high-doped bilayer graphene where Δσ Re (ω) is negative at low frequency and positive on the high frequency side. We use Boltzmann transport theory to understand quantitatively the frequency dependence of Δσ(ω), demanding the energy dependence of different scattering rates such as short-range impurity scattering, Coulomb scattering, carrier-acoustic phonon scattering, and substrate surface optical phonon scattering. We find that the short-range disorder scattering dominates over other processes. The calculated photoconductivity captures very well the experimental conductivity spectra as a function of lattice temperature varying from 300 to 4 K, without any empirical fitting procedures adopted so far in the literature. This helps us to understand the intraband conductivity of photoexcited hot carriers in 2D materials.

Terasonic Excitations in 2D Gold Nanoparticle Arrays in a Water Matrix as Revealed by Atomistic Simulations

DOE PAGES

Bolmatov, Dima; Zhernenkov, Mikhail; Zav’yalov, Dmitry; ...

2016-08-19

Here in this work we report on terahertz phononic excitations in 2D gold nanoparticle arrays in a water matrix through a series of large-scale molecular dynamics simulations. For the first time, we observe acoustic Dirac-like crossings in H (H 2O) atomic (molecular) networks which emerge due to an intraband phononic scattering. These crossings are the phononic fingerprints of ice-like arrangements of H (H 2O) atomic (molecular) networks at nanometer scale. We reveal how phononic excitations in metallic nanoparticles and the water matrix reciprocally impact on one another providing the mechanism for the THz phononics manipulation via structural engineering. In addition,more » we show that by tuning the arrangement of 2D gold nanoparticle assemblies the Au phononic polarizations experience sub-terahertz hybridization (Kohn anomaly) due to surface electron-phonon relaxation processes. This opens the way for the sound control and manipulation in soft matter metamaterials at nanoscale.« less

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.

Anharmonic Effects on the Electron-Energy Spectra of Surface Vibrations

NASA Astrophysics Data System (ADS)

Ariyasu, Janice Carol

First, we consider the effect of lateral interactions on double losses and overtones in electron-energy-loss studies of surface vibrations. We develop a theory of two-phonon losses in the dipole-dominated regime of small -angle scattering. Our calculation employs the simple model of an ordered overlayer of molecules adsorbed on a crystal surface. With this model, we can identify two features; one which corresponds to the double loss and another which corresponds the excitation of an overtone. We then study the role of lateral interactions in each. We find that the presence of lateral interactions affects the position of the overtone relative to the double loss, and influences both its width and shape. The implications of these results are discussed, particularly as they relate to estimates of dissociation energies by the Birge-Sponer procedure. Next, we consider the anharmonic damping of adsorbate vibrations, with specific applications to species (S, O, and CO) adsorbed on the Ni(100) and Ni(111) surfaces. Our attention is restricted to adsorbate modes that can decay by two-phonon processes to one substrate phonon and either another substrate mode phonon or to a phonon of a mode that is localized on the adsorbate. The magnitude and temperature variation of the linewidth of adsorbate modes by this mechanism is explored; we find that near room temperature the calculated linewidths vary linearly with temperature. We also simulate the inhomogeneous broadening produced by disorder by considering the eigenfrequencies of infrared -active modes. Finally, we consider the diffuse scattering of electrons from surfaces by long-wavelength, acoustic phonons. The mechanism that we explore is the modulation of the image potential from ripples induced in the surface profile by thermally-excited surface and bulk phonons. We compare our results with earlier studies, and with the scattering produced by the dynamic-dipole moment of the surface atoms.

Ferrite Materials for Advanced Multifunction Microwave Systems Applications

DTIC Science & Technology

2006-07-05

practical theoretical models of the two magnon Past CSU work has addressed and solved numerous scattering interaction and calculations of the resulting...zero frequency. Ahk in the first place derive from fundamental magnon - If the data in Fig. 3 are assumed to represent intrinsic magnon and magnon -phonon...Patton, J. Appl. Phys. 93, 9195 (2003).] 5 al., 1999). Magnon -phonon processes derive from spin end result is that fine grains give a corresponding high

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

Jana, R. N.; Meikap, A. K.

The results of a comprehensive study of weak electron localization (WEL) and electron-electron interaction (EEI) effects in disordered V{sub 75}X{sub 25} (X = Pd, Al) alloys has been reported. The resistivity in absence of magnetic field shows a minimum at temperature T = T{sub m} and follows T{sup 1/2} law within the temperature range 5 K ≤ T ≤ T{sub m}, which suggests predominant EEI effect. Magnetoresistivity is positive due to strong spin-orbit interaction. The dephasing scattering time is dominated by the electron-phonon scattering. The electron-phonon scattering rate shows quadratic temperature dependence behavior, which is explained by the theory ofmore » incomplete dragging at the random scattering potential by phonons. The zero temperature scattering time strongly depends on the disorder and its magnitude decreases with increasing disorder.« less

Interfacial phonon scattering and transmission loss in >1 μm thick silicon-on-insulator thin films

NASA Astrophysics Data System (ADS)

Jiang, Puqing; Lindsay, Lucas; Huang, Xi; Koh, Yee Kan

2018-05-01

Scattering of phonons at boundaries of a crystal (grains, surfaces, or solid/solid interfaces) is characterized by the phonon wavelength, the angle of incidence, and the interface roughness, as historically evaluated using a specularity parameter p formulated by Ziman [Electrons and Phonons (Clarendon Press, Oxford, 1960)]. This parameter was initially defined to determine the probability of a phonon specularly reflecting or diffusely scattering from the rough surface of a material. The validity of Ziman's theory as extended to solid/solid interfaces has not been previously validated. To better understand the interfacial scattering of phonons and to test the validity of Ziman's theory, we precisely measured the in-plane thermal conductivity of a series of Si films in silicon-on-insulator (SOI) wafers by time-domain thermoreflectance (TDTR) for a Si film thickness range of 1-10 μm and a temperature range of 100-300 K. The Si /SiO2 interface roughness was determined to be 0.11 ±0.04 nm using transmission electron microscopy (TEM). Furthermore, we compared our in-plane thermal conductivity measurements to theoretical calculations that combine first-principles phonon transport with Ziman's theory. Calculations using Ziman's specularity parameter significantly overestimate values from the TDTR measurements. We attribute this discrepancy to phonon transmission through the solid/solid interface into the substrate, which is not accounted for by Ziman's theory for surfaces. The phonons that are specularly transmitted into an amorphous layer will be sufficiently randomized by the time they come back to the crystalline Si layer, the effect of which is practically equivalent to a diffuse reflection at the interface. We derive a simple expression for the specularity parameter at solid/amorphous interfaces and achieve good agreement between calculations and measurement values.

Electron–phonon coupling in hybrid lead halide perovskites

PubMed Central

Wright, Adam D.; Verdi, Carla; Milot, Rebecca L.; Eperon, Giles E.; Pérez-Osorio, Miguel A.; Snaith, Henry J.; Giustino, Feliciano; Johnston, Michael B.; Herz, Laura M.

2016-01-01

Phonon scattering limits charge-carrier mobilities and governs emission line broadening in hybrid metal halide perovskites. Establishing how charge carriers interact with phonons in these materials is therefore essential for the development of high-efficiency perovskite photovoltaics and low-cost lasers. Here we investigate the temperature dependence of emission line broadening in the four commonly studied formamidinium and methylammonium perovskites, HC(NH2)2PbI3, HC(NH2)2PbBr3, CH3NH3PbI3 and CH3NH3PbBr3, and discover that scattering from longitudinal optical phonons via the Fröhlich interaction is the dominant source of electron–phonon coupling near room temperature, with scattering off acoustic phonons negligible. We determine energies for the interacting longitudinal optical phonon modes to be 11.5 and 15.3 meV, and Fröhlich coupling constants of ∼40 and 60 meV for the lead iodide and bromide perovskites, respectively. Our findings correlate well with first-principles calculations based on many-body perturbation theory, which underlines the suitability of an electronic band-structure picture for describing charge carriers in hybrid perovskites. PMID:27225329

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.

Disorder dependence electron phonon scattering rate of V82Pd18 - xFex alloys at low temperature

NASA Astrophysics Data System (ADS)

Jana, R. N.; Meikap, A. K.

2018-04-01

We have systematically investigated the disorder dependence electron phonon scattering rate in three dimensional disordered V82Pd18 - xFex alloys. A minimum in temperature dependence resistivity curve has been observed at low temperature T =Tm. In the temperature range 5 K ≤ T ≤Tm the resistivity correction follows ρo 5 / 2T 1 / 2 law. The dephasing scattering time has been calculated from analysis of magnetoresistivity by weak localization theory. The electron dephasing time is dominated by electron-phonon scattering and follows anomalous temperature (T) and disorder (ρ0) dependence behaviour like τe-ph-1 ∝T2 /ρ0, where ρ0 is the impurity resistivity. The magnitude of the saturated dephasing scattering time (τ0) at zero temperature decreases with increasing disorder of the samples. Such anomalous behaviour of dephasing scattering rate is still unresolved.

Phonon coupling to dynamic short-range polar order in a relaxor ferroelectric near the morphotropic phase boundary

DOE PAGES

John A. Schneeloch; Xu, Zhijun; Winn, B.; ...

2015-12-28

We report neutron inelastic scattering experiments on single-crystal PbMg 1/3Nb 2/3O 3 doped with 32% PbTiO 3, a relaxor ferroelectric that lies close to the morphotropic phase boundary. When cooled under an electric field E∥ [001] into tetragonal and monoclinic phases, the scattering cross section from transverse acoustic (TA) phonons polarized parallel to E weakens and shifts to higher energy relative to that under zero-field-cooled conditions. Likewise, the scattering cross section from transverse optic (TO) phonons polarized parallel to E weakens for energy transfers 4 ≤ ℏω ≤ 9 meV. However, TA and TO phonons polarized perpendicular to E showmore » no change. This anisotropic field response is similar to that of the diffuse scattering cross section, which, as previously reported, is suppressed when polarized parallel to E but not when polarized perpendicular to E. Lastly, our findings suggest that the lattice dynamics and dynamic short-range polar correlations that give rise to the diffuse scattering are coupled.« less

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.

Heat conduction in one-dimensional lattices with on-site potential.

PubMed

Savin, A V; Gendelman, O V

2003-04-01

The process of heat conduction in one-dimensional lattices with on-site potential is studied by means of numerical simulation. Using the discrete Frenkel-Kontorova, phi(4), and sinh-Gordon models we demonstrate that contrary to previously expressed opinions the sole anharmonicity of the on-site potential is insufficient to ensure the normal heat conductivity in these systems. The character of the heat conduction is determined by the spectrum of nonlinear excitations peculiar for every given model and therefore depends on the concrete potential shape and the temperature of the lattice. The reason is that the peculiarities of the nonlinear excitations and their interactions prescribe the energy scattering mechanism in each model. For sine-Gordon and phi(4) models, phonons are scattered at a dynamical lattice of topological solitons; for sinh-Gordon and for phi(4) in a different parameter regime the phonons are scattered at localized high-frequency breathers (in the case of phi(4) the scattering mechanism switches with the growth of the temperature).

Dynamic Displacement Disorder of Cubic BaTiO3

NASA Astrophysics Data System (ADS)

Paściak, M.; Welberry, T. R.; Kulda, J.; Leoni, S.; Hlinka, J.

2018-04-01

The three-dimensional distribution of the x-ray diffuse scattering intensity of BaTiO3 has been recorded in a synchrotron experiment and simultaneously computed using molecular dynamics simulations of a shell model. Together, these have allowed the details of the disorder in paraelectric BaTiO3 to be clarified. The narrow sheets of diffuse scattering, related to the famous anisotropic longitudinal correlations of Ti ions, are shown to be caused by the overdamped anharmonic soft phonon branch. This finding demonstrates that the occurrence of narrow sheets of diffuse scattering agrees with a displacive picture of the cubic phase of this textbook ferroelectric material. The presented methodology allows one to go beyond the harmonic approximation in the analysis of phonons and phonon-related scattering.

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.

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.

Ultrafast electronic dynamics in unipolar n-doped indium gallium arsenide/gallium arsenide self-assembled quantum dots

NASA Astrophysics Data System (ADS)

Wu, Zong-Kwei J.

2006-12-01

Photodetectors based on intraband infrared absorption in the quantum dots have demonstrated improved performance over its quantum well counterpart by lower dark current, relative temperature insensitivity, and its ability for normal incidence operation. Various scattering processes, including phonon emission/absorption and carrier-carrier scattering, are critical in understanding device operation on the fundamental level. In previous studies, our group has investigated carrier dynamics in both low- and high-density regime. Ultrafast electron-hole scattering and the predicted phonon bottleneck effect in intrinsic quantum dots have been observed. Further examination on electron dynamics in unipolar structures is presented in this thesis. We used n-doped quantum dot in mid-infrared photodetector device structure to study the electron dynamics in unipolar structure. Differential transmission spectroscopy with mid-infrared intraband pump and optical interband probe was implemented to measure the electron dynamics directly without creating extra electron-hole pair, Electron relaxation after excitation was measured under various density and temperature conditions. Rapid capture into quantum dot within ˜ 10 ps was observed due to Auger-type electron-electron scattering. Intradot relaxation from the quantum dot excited state to the ground state was also observed on the time scale of 100 ps. With highly doped electron density in the structure, the inter-sublevel relaxation is dominated by Auger-type electron-electron scattering and the phonon bottleneck effect is circumvented. Nanosecond-scale recovery in larger-sized quantum dots was observed, not intrinsic to electron dynamics but due to band-bending and built-in voltage drift. An ensemble Monte Carlo simulation was also established to model the dynamics in quantum dots and in goad agreement with the experimental results. We presented a comprehensive picture of electron dynamics in the unipolar quantum dot structure. Although the phonon bottleneck is circumvented with high doped electron density, relaxation processes in unipolar quantum dots have been measured with time scales longer than that of bipolar systems. The results explain the operation principles of the quantum dot infrared photodetector on a microscopic level and provide basic understanding for future applications and designs.

Anomalous Hall effect scaling in ferromagnetic thin films

NASA Astrophysics Data System (ADS)

Grigoryan, Vahram L.; Xiao, Jiang; Wang, Xuhui; Xia, Ke

2017-10-01

We propose a scaling law for anomalous Hall effect in ferromagnetic thin films. Our approach distinguishes multiple scattering sources, namely, bulk impurity, phonon for Hall resistivity, and most importantly the rough surface contribution to longitudinal resistivity. In stark contrast to earlier laws that rely on temperature- and thickness-dependent fitting coefficients, this scaling law fits the recent experimental data excellently with constant parameters that are independent of temperature and film thickness, strongly indicating that this law captures the underlying physical processes. Based on a few data points, this scaling law can even fit all experimental data in full temperature and thickness range. We apply this law to interpret the experimental data for Fe, Co, and Ni and conclude that (i) the phonon-induced skew scattering is unimportant as expected; (ii) contribution from the impurity-induced skew scattering is negative; (iii) the intrinsic (extrinsic) mechanism dominates in Fe (Co), and both the extrinsic and intrinsic contributions are important in Ni.

Theory of the Lattice Thermal Conductivity of Nanowires

NASA Astrophysics Data System (ADS)

Broido, D. A.; Mingo, N.

2004-03-01

Thermal transport in semiconductor nanowires is of considerable scientific interest, and its understanding is important as well for potential applications[1]. We present a theory of the lattice thermal conductivity along semiconductor nanowires which includes anharmonic phonon-phonon scattering as well as defect and boundary scattering. These latter two scattering mechanisms are treated in relaxation time approximations. Our theory provides an iterative solution [2] of the phonon Boltzmann equation in which the full nanowire phonon dispersions and modes obtained from lattice dynamics calculations are included consistently in treating the anharmonic three-phonon scattering. We calculate the lattice thermal conductivity of Si nanowires as a function of temperature and wire thickness, and we compare our results with recent measurements [3], and with previous calculations in the relaxation time approximation [4].-------- [1] D. Cahill, W. ford, K. Goodson, G. D. Mahan, A. Majumdar, H. J. Maris, R. Merlin and S. Phillpot, J. Appl. Phys. 93, 793 (2003). [2] M. Omini and A. Sparavigna, Nuovo Cimento, D 19, 1537 (1997). [3] D. Li, Y. Wu, P. Kim, L. Shi, P. Yang and A. Majumdar, Appl. Phys. Lett. 83, 2934 (2003). [4] N. Mingo, Phys. Rev. B 68, 113308 (2003).

Equilibrium limit of thermal conduction and boundary scattering in nanostructures.

PubMed

Haskins, Justin B; Kınacı, Alper; Sevik, Cem; Çağın, Tahir

2014-06-28

Determining the lattice thermal conductivity (κ) of nanostructures is especially challenging in that, aside from the phonon-phonon scattering present in large systems, the scattering of phonons from the system boundary greatly influences heat transport, particularly when system length (L) is less than the average phonon mean free path (MFP). One possible route to modeling κ in these systems is through molecular dynamics (MD) simulations, inherently including both phonon-phonon and phonon-boundary scattering effects in the classical limit. Here, we compare current MD methods for computing κ in nanostructures with both L ⩽ MFP and L ≫ MFP, referred to as mean free path constrained (cMFP) and unconstrained (uMFP), respectively. Using a (10,0) CNT (carbon nanotube) as a benchmark case, we find that while the uMFP limit of κ is well-defined through the use of equilibrium MD and the time-correlation formalism, the standard equilibrium procedure for κ is not appropriate for the treatment of the cMFP limit because of the large influence of boundary scattering. To address this issue, we define an appropriate equilibrium procedure for cMFP systems that, through comparison to high-fidelity non-equilibrium methods, is shown to be the low thermal gradient limit to non-equilibrium results. Further, as a means of predicting κ in systems having L ≫ MFP from cMFP results, we employ an extrapolation procedure based on the phenomenological, boundary scattering inclusive expression of Callaway [Phys. Rev. 113, 1046 (1959)]. Using κ from systems with L ⩽ 3 μm in the extrapolation, we find that the equilibrium uMFP κ of a (10,0) CNT can be predicted within 5%. The equilibrium procedure is then applied to a variety of carbon-based nanostructures, such as graphene flakes (GF), graphene nanoribbons (GNRs), CNTs, and icosahedral fullerenes, to determine the influence of size and environment (suspended versus supported) on κ. Concerning the GF and GNR systems, we find that the supported samples yield consistently lower values of κ and that the phonon-boundary scattering remains dominant at large lengths, with L = 0.4 μm structures exhibiting a third of the periodic result. We finally characterize the effect of shape in CNTs and fullerenes on κ, showing the angular components of conductivity in CNTs and icosahedral fullerenes are similar for a given circumference.

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

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

Effects of Mass Fluctuation on Thermal Transport Properties in Bulk Bi2Te3

NASA Astrophysics Data System (ADS)

Huang, Ben; Zhai, Pengcheng; Yang, Xuqiu; Li, Guodong

2017-05-01

In this paper, we applied large-scale molecular dynamics and lattice dynamics to study the influence of mass fluctuation on thermal transport properties in bulk Bi2Te3, namely thermal conductivity ( K), phonon density of state (PDOS), group velocity ( v g), and mean free path ( l). The results show that total atomic mass change can affect the relevant vibrational frequency on the micro level and heat transfer rate in the macro statistic, hence leading to the strength variation of the anharmonic phonon processes (Umklapp scattering) in the defect-free Bi2Te3 bulk. Moreover, it is interesting to find that the anharmonicity of Bi2Te3 can be also influenced by atomic differences of the structure such as the mass distribution in the primitive cell. Considering the asymmetry of the crystal structure and interatomic forces, it can be concluded by phonon frequency, lifetime, and velocity calculation that acoustic-optical phonon scattering shows the structure-sensitivity to the mass distribution and complicates the heat transfer mechanism, hence resulting in the low lattice thermal conductivity of Bi2Te3. This study is helpful for designing the material with tailored thermal conductivity via atomic substitution.

First-principles study of thermal transport in nitrogenated holey graphene.

PubMed

Ouyang, Tao; Xiao, Huaping; Tang, Chao; Zhang, Xiaoliang; Hu, Ming; Zhong, Jianxin

2017-01-27

Nitrogenated holey graphene (NHG), a new two-dimensional graphene variant with a large fundamental direct band gap, has recently been successfully synthesized via a simple wet-chemical reaction. Motivated by its unique geometry and novel properties, we investigated the phonon transport properties of the material by combining first-principle calculations and the phonon Boltzmann transport equation. The lattice thermal conductivity of NHG at room temperature is predicted to be about 82.22 W mK -1 , which is almost two orders of magnitude lower than that of graphene (about 3500 W mK -1 ). Deviating from the traditional understanding that thermal transport is usually largely contributed by the acoustic phonon modes for most suspended 2D materials, both out-of-plane flexural acoustic (ZA) and optical phonon modes make a more or less equal contribution, and their combination abnormally dominates the overall thermal transport in NHG. The major three-phonon process in NHG is further analyzed and the scattering between the acoustic and optical phonon modes like [Formula: see text] is the main phonon process channel. Meanwhile, the mean free path distribution of different phonon modes is calculated for the purpose of the thermal management of NHG-based devices. Our results elucidate the unusual thermal transport properties of NHG as compared with the representative case of graphene, and underpin its potential application for use by the thermal management community.

First-principles study of thermal transport in nitrogenated holey graphene

NASA Astrophysics Data System (ADS)

Ouyang, Tao; Xiao, Huaping; Tang, Chao; Zhang, Xiaoliang; Hu, Ming; Zhong, Jianxin

2017-01-01

Nitrogenated holey graphene (NHG), a new two-dimensional graphene variant with a large fundamental direct band gap, has recently been successfully synthesized via a simple wet-chemical reaction. Motivated by its unique geometry and novel properties, we investigated the phonon transport properties of the material by combining first-principle calculations and the phonon Boltzmann transport equation. The lattice thermal conductivity of NHG at room temperature is predicted to be about 82.22 W mK-1, which is almost two orders of magnitude lower than that of graphene (about 3500 W mK-1). Deviating from the traditional understanding that thermal transport is usually largely contributed by the acoustic phonon modes for most suspended 2D materials, both out-of-plane flexural acoustic (ZA) and optical phonon modes make a more or less equal contribution, and their combination abnormally dominates the overall thermal transport in NHG. The major three-phonon process in NHG is further analyzed and the scattering between the acoustic and optical phonon modes like {{ZA}}/{{TA}}/{{LA}}+{{O}}≤ftrightarrow {{O}} is the main phonon process channel. Meanwhile, the mean free path distribution of different phonon modes is calculated for the purpose of the thermal management of NHG-based devices. Our results elucidate the unusual thermal transport properties of NHG as compared with the representative case of graphene, and underpin its potential application for use by the thermal management community.

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

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

Thermal and thermoelectric transport measurements of an individual boron arsenide microstructure

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

Kim, Jaehyun; Sellan, Daniel P.; Ou, Eric

2016-05-16

Recent first principles calculations have predicted that boron arsenide (BAs) can possess an unexpectedly high thermal conductivity that depends sensitively on the crystal size and defect concentration. However, few experimental results have been obtained to verify these predictions. In the present work, we report four-probe thermal and thermoelectric transport measurements of an individual BAs microstructure that was synthesized via a vapor transport method. The measured thermal conductivity was found to decrease slightly with temperature in the range between 250 K and 350 K. The temperature dependence suggests that the extrinsic phonon scattering processes play an important role in addition to intrinsic phonon-phononmore » scattering. The room temperature value of (186 ± 46) W m{sup −1 }K{sup −1} is higher than that of bulk silicon but still a factor of four lower than the calculated result for a defect-free, non-degenerate BAs rod with a similar diameter of 1.15 μm. The measured p-type Seebeck coefficient and thermoelectric power factor are comparable to those of bismuth telluride, which is a commonly used thermoelectric material. The foregoing results also suggest that it is necessary to not only reduce defect and boundary scatterings but also to better understand and control the electron scattering of phonons in order to achieve the predicted ultrahigh intrinsic lattice thermal conductivity of BAs.« less

THz Acoustic Spectroscopy by using Double Quantum Wells and Ultrafast Optical Spectroscopy.

PubMed

Wei, Fan Jun; Yeh, Yu-Hsiang; Sheu, Jinn-Kong; Lin, Kung-Hsuan

2016-06-27

GaN is a pivotal material for acoustic transducers and acoustic spectroscopy in the THz regime, but its THz phonon properties have not been experimentally and comprehensively studied. In this report, we demonstrate how to use double quantum wells as a THz acoustic transducer for measuring generated acoustic phonons and deriving a broadband acoustic spectrum with continuous frequencies. We experimentally investigated the sub-THz frequency dependence of acoustic attenuation (i.e., phonon mean-free paths) in GaN, in addition to its physical origins such as anharmonic scattering, defect scattering, and boundary scattering. A new upper limit of attenuation caused by anharmonic scattering, which is lower than previously reported values, was obtained. Our results should be noteworthy for THz acoustic spectroscopy and for gaining a fundamental understanding of heat conduction.

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.

Subterahertz Longitudinal Phonon Modes Propagating in a Lipid Bilayer Immersed in an Aqueous Medium

NASA Astrophysics Data System (ADS)

Zakhvataev, V. E.

2018-04-01

The properties of subterahertz longitudinal acoustic phonon modes in the hydrophobic region of a lipid bilayer immersed in a compressible viscous aqueous medium are investigated theoretically. An approximate expression is obtained for the Mandelstam-Brillouin components of the dynamic structure factor of a bilayer. The analysis is based on a generalized hydrodynamic model of the "two-dimensional lipid bilayer + three-dimensional fluid medium" system, as well as on known sharp estimates for the frequencies and lifetimes of long-wavelength longitudinal acoustic phonons in a free hydrated lipid bilayer and in water, obtained from inelastic X-ray scattering experiments and molecular dynamics simulations. It is shown that, for characteristic values of the parameters of the membrane system, subterahertz longitudinal phonon-like excitations in the hydrophobic part of the bilayer are underdamped. In this case, the contribution of the viscous flow of the aqueous medium to the damping of a longitudinal membrane mode is small compared with the contribution of the lipid bilayer. Quantitative estimates of the damping ratio agree well with the experimental results for the vibration mode of the enzyme lysozyme in aqueous solution [1]. It is also shown that a coupling between longitudinal phonon modes of the bilayer and relaxation processes in its fluid environment gives rise to an additional peak in the scattering spectrum, which corresponds to a non-propagating mode.

Thermal conductance of metal–diamond interfaces at high pressure

DOE PAGES

Hohensee, Gregory T.; Wilson, R. B.; Cahill, David G.

2015-03-06

The thermal conductance of interfaces between metals and diamond, which has a comparatively high Debye temperature, is often greater than can be accounted for by two phonon-processes. The high pressures achievable in a diamond anvil cell can significantly extend the metal phonon density of states to higher frequencies, and can also suppress extrinsic effects by greatly stiffening interface bonding. Here we report time-domain thermoreflectance measurements of metal-diamond interface thermal conductance up to 50 GPa in the DAC for Pb, Au 0.95Pd 0.05, Pt, and Al films deposited on Type 1A natural [100] and Type 2A synthetic [110] diamond anvils. Inmore » all cases, the thermal conductances increase weakly or saturate to similar values at high pressure. Lastly, our results suggest that anharmonic conductance at metal-diamond interfaces is controlled by partial transmission processes, where a diamond phonon that inelastically scatters at the interface absorbs or emits a metal phonon.« less

Extraction-controlled terahertz frequency quantum cascade lasers with a diagonal LO-phonon extraction and injection stage.

PubMed

Han, Y J; Li, L H; Grier, A; Chen, L; Valavanis, A; Zhu, J; Freeman, J R; Isac, N; Colombelli, R; Dean, P; Davies, A G; Linfield, E H

2016-12-12

We report an extraction-controlled terahertz (THz)-frequency quantum cascade laser design in which a diagonal LO-phonon scattering process is used to achieve efficient current injection into the upper laser level of each period and simultaneously extract electrons from the adjacent period. The effects of the diagonality of the radiative transition are investigated, and a design with a scaled oscillator strength of 0.45 is shown experimentally to provide the highest temperature performance. A 3.3 THz device processed into a double-metal waveguide configuration operated up to 123 K in pulsed mode, with a threshold current density of 1.3 kA/cm² at 10 K. The QCL structures are modeled using an extended density matrix approach, and the large threshold current is attributed to parasitic current paths associated with the upper laser levels. The simplicity of this design makes it an ideal platform to investigate the scattering injection process.

Interfacial phonon scattering and transmission loss in > 1 µm thick silicon-on-insulator thin films

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

Jiang, Puqing; Lindsay, Lucas R.; Huang, Xi

Scattering of phonons at boundaries of a crystal (grains, surfaces, or solid/solid interfaces) is characterized by the phonon wavelength, the angle of incidence, and the interface roughness, as historically evaluated using a specularity parameter p formulated by Ziman [Electrons and Phonons (Clarendon Press, Oxford, 1960)]. This parameter was initially defined to determine the probability of a phonon specularly reflecting or diffusely scattering from the rough surface of a material. The validity of Ziman's theory as extended to solid/solid interfaces has not been previously validated. Here, to better understand the interfacial scattering of phonons and to test the validity of Ziman'smore » theory, we precisely measured the in-plane thermal conductivity of a series of Si films in silicon-on-insulator (SOI) wafers by time-domain thermoreflectance (TDTR) for a Si film thickness range of 1–10 μm and a temperature range of 100–300 K. The Si/SiO 2 interface roughness was determined to be 0.11±0.04nm using transmission electron microscopy (TEM). Furthermore, we compared our in-plane thermal conductivity measurements to theoretical calculations that combine first-principles phonon transport with Ziman's theory. Calculations using Ziman's specularity parameter significantly overestimate values from the TDTR measurements. We attribute this discrepancy to phonon transmission through the solid/solid interface into the substrate, which is not accounted for by Ziman's theory for surfaces. The phonons that are specularly transmitted into an amorphous layer will be sufficiently randomized by the time they come back to the crystalline Si layer, the effect of which is practically equivalent to a diffuse reflection at the interface. Finally, we derive a simple expression for the specularity parameter at solid/amorphous interfaces and achieve good agreement between calculations and measurement values.« less

Interfacial phonon scattering and transmission loss in > 1 µm thick silicon-on-insulator thin films

DOE PAGES

Jiang, Puqing; Lindsay, Lucas R.; Huang, Xi; ...

2018-05-17

Scattering of phonons at boundaries of a crystal (grains, surfaces, or solid/solid interfaces) is characterized by the phonon wavelength, the angle of incidence, and the interface roughness, as historically evaluated using a specularity parameter p formulated by Ziman [Electrons and Phonons (Clarendon Press, Oxford, 1960)]. This parameter was initially defined to determine the probability of a phonon specularly reflecting or diffusely scattering from the rough surface of a material. The validity of Ziman's theory as extended to solid/solid interfaces has not been previously validated. Here, to better understand the interfacial scattering of phonons and to test the validity of Ziman'smore » theory, we precisely measured the in-plane thermal conductivity of a series of Si films in silicon-on-insulator (SOI) wafers by time-domain thermoreflectance (TDTR) for a Si film thickness range of 1–10 μm and a temperature range of 100–300 K. The Si/SiO 2 interface roughness was determined to be 0.11±0.04nm using transmission electron microscopy (TEM). Furthermore, we compared our in-plane thermal conductivity measurements to theoretical calculations that combine first-principles phonon transport with Ziman's theory. Calculations using Ziman's specularity parameter significantly overestimate values from the TDTR measurements. We attribute this discrepancy to phonon transmission through the solid/solid interface into the substrate, which is not accounted for by Ziman's theory for surfaces. The phonons that are specularly transmitted into an amorphous layer will be sufficiently randomized by the time they come back to the crystalline Si layer, the effect of which is practically equivalent to a diffuse reflection at the interface. Finally, we derive a simple expression for the specularity parameter at solid/amorphous interfaces and achieve good agreement between calculations and measurement values.« less

A model for the high-temperature transport properties of heavily doped n-type silicon-germanium alloys

NASA Technical Reports Server (NTRS)

Vining, Cronin B.

1991-01-01

A model is presented for the high-temperature transport properties of large-grain-size, heavily doped n-type silicon-germanium alloys. Electron and phonon transport coefficients are calculated using standard Boltzmann equation expressions in the relaxation time approximation. Good agreement with experiment is found by considering acoustic phonon and ionized impurity scattering for electrons, and phonon-phonon, point defect, and electron-phonon scattering for phonons. The parameters describing electron transport in heavily doped and lightly doped materials are significantly different and suggest that most carriers in heavily doped materials are in a band formed largely from impurity states. The maximum dimensionless thermoelectric figure of merit for single-crystal, n-type Si(0.8)Ge(0.2) at 1300 K is estimated at ZT about 1.13 with an optimum carrier concentration of n about 2.9 x 10 to the 20th/cu cm.

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.

Ultrafast electron-optical phonon scattering and quasiparticle lifetime in CVD-grown graphene.

PubMed

Shang, Jingzhi; Yu, Ting; Lin, Jianyi; Gurzadyan, Gagik G

2011-04-26

Ultrafast quasiparticle dynamics in graphene grown by chemical vapor deposition (CVD) has been studied by UV pump/white-light probe spectroscopy. Transient differential transmission spectra of monolayer graphene are observed in the visible probe range (400-650 nm). Kinetics of the quasiparticle (i.e., low-energy single-particle excitation with renormalized energy due to electron-electron Coulomb, electron-optical phonon (e-op), and optical phonon-acoustic phonon (op-ap) interactions) was monitored with 50 fs resolution. Extending the probe range to near-infrared, we find the evolution of quasiparticle relaxation channels from monoexponential e-op scattering to double exponential decay due to e-op and op-ap scattering. Moreover, quasiparticle lifetimes of mono- and randomly stacked graphene films are obtained for the probe photon energies continuously from 1.9 to 2.3 eV. Dependence of quasiparticle decay rate on the probe energy is linear for 10-layer stacked graphene films. This is due to the dominant e-op intervalley scattering and the linear density of states in the probed electronic band. A dimensionless coupling constant W is derived, which characterizes the scattering strength of quasiparticles by lattice points in graphene.

Phonon anharmonicity and negative thermal expansion in SnSe

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

Bansal, Dipanshu; Hong, Jiawang; Li, Chen W.

In this paper, the anharmonic phonon properties of SnSe in the Pnma phase were investigated with a combination of experiments and first-principles simulations. Using inelastic neutron scattering (INS) and nuclear resonant inelastic X-ray scattering (NRIXS), we have measured the phonon dispersions and density of states (DOS) and their temperature dependence, which revealed a strong, inhomogeneous shift and broadening of the spectrum on warming. First-principles simulations were performed to rationalize these measurements, and to explain the previously reported anisotropic thermal expansion, in particular the negative thermal expansion within the Sn-Se bilayers. Including the anisotropic strain dependence of the phonon free energy,more » in addition to the electronic ground state energy, is essential to reproduce the negative thermal expansion. From the phonon DOS obtained with INS and additional calorimetry measurements, we quantify the harmonic, dilational, and anharmonic components of the phonon entropy, heat capacity, and free energy. Finally, the origin of the anharmonic phonon thermodynamics is linked to the electronic structure.« less

Phonon anharmonicity and negative thermal expansion in SnSe

DOE PAGES

Bansal, Dipanshu; Hong, Jiawang; Li, Chen W.; ...

2016-08-09

In this paper, the anharmonic phonon properties of SnSe in the Pnma phase were investigated with a combination of experiments and first-principles simulations. Using inelastic neutron scattering (INS) and nuclear resonant inelastic X-ray scattering (NRIXS), we have measured the phonon dispersions and density of states (DOS) and their temperature dependence, which revealed a strong, inhomogeneous shift and broadening of the spectrum on warming. First-principles simulations were performed to rationalize these measurements, and to explain the previously reported anisotropic thermal expansion, in particular the negative thermal expansion within the Sn-Se bilayers. Including the anisotropic strain dependence of the phonon free energy,more » in addition to the electronic ground state energy, is essential to reproduce the negative thermal expansion. From the phonon DOS obtained with INS and additional calorimetry measurements, we quantify the harmonic, dilational, and anharmonic components of the phonon entropy, heat capacity, and free energy. Finally, the origin of the anharmonic phonon thermodynamics is linked to the electronic structure.« less

Glass-like phonon scattering from a spontaneous nanostructure in AgSbTe2.

PubMed

Ma, J; Delaire, O; May, A F; Carlton, C E; McGuire, M A; VanBebber, L H; Abernathy, D L; Ehlers, G; Hong, Tao; Huq, A; Tian, Wei; Keppens, V M; Shao-Horn, Y; Sales, B C

2013-06-01

Materials with very low thermal conductivity are of great interest for both thermoelectric and optical phase-change applications. Synthetic nanostructuring is most promising for suppressing thermal conductivity through phonon scattering, but challenges remain in producing bulk samples. In crystalline AgSbTe2 we show that a spontaneously forming nanostructure leads to a suppression of thermal conductivity to a glass-like level. Our mapping of the phonon mean free paths provides a novel bottom-up microscopic account of thermal conductivity and also reveals intrinsic anisotropies associated with the nanostructure. Ground-state degeneracy in AgSbTe2 leads to the natural formation of nanoscale domains with different orderings on the cation sublattice, and correlated atomic displacements, which efficiently scatter phonons. This mechanism is general and suggests a new avenue for the nanoscale engineering of materials to achieve low thermal conductivities for efficient thermoelectric converters and phase-change memory devices.

Phonon-driven electron scattering and magnetothermoelectric effect in two-dimensional tin selenide

NASA Astrophysics Data System (ADS)

Yang, Kaike; Ren, Ji-Chang; Qiu, Hongfei; Wang, Jian-Sheng

2018-02-01

The bulk tin selenide (SnSe) is the best thermoelectric material currently with the highest figure-of-merit due to strong phonon-phonon interactions. We investigate the effect of electron-phonon coupling (EPC) on the transport properties of a two-dimensional (2D) SnSe sheet. We demonstrate that EPC plays a key role in the scattering rate when the constant relaxation time approximation is deficient. The EPC strength is especially large in contrast to that of pristine graphene. The scattering rate depends sensitively on the system temperatures and the carrier densities when the Fermi energy approaches the band edge. We also investigate the magnetothermoelectric effect of the 2D SnSe. It is found that at low temperatures there is enormous magnetoelectrical resistivity and magnetothermal resistivity above 200%, suggesting possible potential applications in device design. Our results agree qualitatively well with the experimental data.

Effect of rattling motion without cage structure on lattice thermal conductivity in LaOBiS2-xSex

NASA Astrophysics Data System (ADS)

Lee, C. H.; Nishida, A.; Hasegawa, T.; Nishiate, H.; Kunioka, H.; Ohira-Kawamura, S.; Nakamura, M.; Nakajima, K.; Mizuguchi, Y.

2018-01-01

Low energy phonons in LaOBiS2-xSex are studied using inelastic neutron scattering. Dispersionless flat phonon branches that are mainly associated with a large vibration of Bi atoms are observed at a relatively low energy of E = 6-6.7 meV. The phonon energy softens upon Se doping presumably owing to its heavier atomic mass than the S atom and the expansion of the lattice constant. Simultaneously, the lattice thermal conductivity lowered upon Se doping as the same manner of the phonon softening. These suggest that despite the lack of an oversized cage in LaOBiS2-xSex, rattling motions of Bi atoms can scatter phonon like rattling in cage compounds, contributing to enhance the thermoelectric property.

Effect of polarization field on mean free path of phonons in indium nitride

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

Sahoo, Sushant Kumar

2016-05-06

The effect of built-in-polarization field on mean free path of acoustic phonons in bulk wurtzite indium nitride (InN) has been theoretically investigated. The elastic constant of the material gets modified due to the existence of polarization field. As a result velocity and Debye frequency of phonons get enhanced. The various scattering rates of phonons are suppressed by the effect of polarization field, which implies an enhanced combined relaxation time. Thus phonons travel freely for a longer distance between two successive scatterings. This would enhance the thermal transport properties of the material when built-in-polarization field taken into account. Hence by themore » application of electric field the transport properties of such materials can be controlled as and when desired.« less

Lattice dynamics in Sn nanoislands and cluster-assembled films

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

Houben, Kelly; Couet, Sebastien; Trekels, Maarten

2017-04-01

To unravel the effects of phonon confinement, the influence of size and morphology on the atomic vibrations is investigated in Sn nanoislands and cluster-assembled films. Nuclear resonant inelastic x-ray scattering is used to probe the phonon densities of states of the Sn nanostructures which show significant broadening of the features compared to bulk phonon behavior. Supported by ab initio calculations, the broadening is attributed to phonon scattering and can be described within the damped harmonic oscillator model. Contrary to the expectations based on previous research, the appearance of high-energy modes above the cutoff energy is not observed. From the thermodynamicmore » properties extracted from the phonon densities of states, it was found that grain boundary Sn atoms are bound by weaker forces than bulk Sn atoms.« less

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.

Strong magnon-phonon coupling in NaFeAs studied by neutron scattering

NASA Astrophysics Data System (ADS)

Li, Yu; Yamani, Zahra; Song, Yu; Zhang, Chenglin; Dai, Pengcheng

We carried on inelastic neutron scattering experiment on the triple axis spectrometer in CNBC in Chalk River. We measured both the phonon and magnon in NaFeAs single crystals and their temperature dependence. Since structural transition temperature (TS) and the magnetic transition temperature (T N) are well separated in NaFeAs, it provides us an unique chance to exclude the consequence or magnetic order and focus on the so called nematic phase. As the previous paper on BaFe2As2, we observed the strong phonon softening nearby the structural transition temperature at very small q (q<0.1). This makes the phonon in NaFeAs deviate from the classical linear dispersion relationship for acoustic phonons. Besides the phonon softening, we also observe phonon hardening at a larger q range when the temperature goes down. This is accompanied by the stiffening of the magnons which can be represented by the linewidth of the low energy magnetic peaks. Our results suggest that there is strong coupling between the phonons and magnons in NaFeAs.

Guided wave opto-acoustic device

DOEpatents

Jarecki, Jr., Robert L.; Rakich, Peter Thomas; Camacho, Ryan; Shin, Heedeuk; Cox, Jonathan Albert; Qiu, Wenjun; Wang, Zheng

2016-02-23

The various technologies presented herein relate to various hybrid phononic-photonic waveguide structures that can exhibit nonlinear behavior associated with traveling-wave forward stimulated Brillouin scattering (forward-SBS). The various structures can simultaneously guide photons and phonons in a suspended membrane. By utilizing a suspended membrane, a substrate pathway can be eliminated for loss of phonons that suppresses SBS in conventional silicon-on-insulator (SOI) waveguides. Consequently, forward-SBS nonlinear susceptibilities are achievable at about 3000 times greater than achievable with a conventional waveguide system. Owing to the strong phonon-photon coupling achievable with the various embodiments, potential application for the various embodiments presented herein cover a range of radiofrequency (RF) and photonic signal processing applications. Further, the various embodiments presented herein are applicable to applications operating over a wide bandwidth, e.g. 100 MHz to 50 GHz or more.

Charge transport in organic molecular semiconductors from first principles: The bandlike hole mobility in a naphthalene crystal

NASA Astrophysics Data System (ADS)

Lee, Nien-En; Zhou, Jin-Jian; Agapito, Luis A.; Bernardi, Marco

2018-03-01

Predicting charge transport in organic molecular crystals is notoriously challenging. Carrier mobility calculations in organic semiconductors are dominated by quantum chemistry methods based on charge hopping, which are laborious and only moderately accurate. We compute from first principles the electron-phonon scattering and the phonon-limited hole mobility of naphthalene crystal in the framework of ab initio band theory. Our calculations combine GW electronic bandstructures, ab initio electron-phonon scattering, and the Boltzmann transport equation. The calculated hole mobility is in very good agreement with experiment between 100 -300 K , and we can predict its temperature dependence with high accuracy. We show that scattering between intermolecular phonons and holes regulates the mobility, though intramolecular phonons possess the strongest coupling with holes. We revisit the common belief that only rigid molecular motions affect carrier dynamics in organic molecular crystals. Our paper provides a quantitative and rigorous framework to compute charge transport in organic crystals and is a first step toward reconciling band theory and carrier hopping computational methods.

Lattice thermal conductivity of borophene from first principle calculation

NASA Astrophysics Data System (ADS)

Xiao, Huaping; Cao, Wei; Ouyang, Tao; Guo, Sumei; He, Chaoyu; Zhong, Jianxin

2017-04-01

The phonon transport property is a foundation of understanding a material and predicting the potential application in mirco/nano devices. In this paper, the thermal transport property of borophene is investigated by combining first-principle calculations and phonon Boltzmann transport equation. At room temperature, the lattice thermal conductivity of borophene is found to be about 14.34 W/mK (error is about 3%), which is much smaller than that of graphene (about 3500 W/mK). The contributions from different phonon modes are qualified, and some phonon modes with high frequency abnormally play critical role on the thermal transport of borophene. This is quite different from the traditional understanding that thermal transport is usually largely contributed by the low frequency acoustic phonon modes for most of suspended 2D materials. Detailed analysis further reveals that the scattering between the out-of-plane flexural acoustic mode (FA) and other modes likes FA + FA/TA/LA/OP ↔ TA/LA/OP is the predominant phonon process channel. Finally the vibrational characteristic of some typical phonon modes and mean free path distribution of different phonon modes are also presented in this work. Our results shed light on the fundamental phonon transport properties of borophene, and foreshow the potential application for thermal management community.

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 .

Phonovoltaic. I. Harvesting hot optical phonons in a nanoscale p -n junction

NASA Astrophysics Data System (ADS)

Melnick, Corey; Kaviany, Massoud

2016-03-01

The phonovoltaic (pV) cell is similar to the photovoltaic. It harvests nonequilibrium (hot) optical phonons (Ep ,O) more energetic than the band gap (Δ Ee ,g) to generate power in a p-n junction. We examine the theoretical electron-phonon and phonon-phonon scattering rates, the Boltzmann transport of electrons, and the diode equation and hydrodynamic simulations to describe the operation of a pV cell and develop an analytic model predicting its efficiency. Our findings indicate that a pV material with Ep ,O≃Δ Ee ,g≫kBT , where kBT is the thermal energy, and a strong interband electron-phonon coupling surpasses the thermoelectric limit, provided the optical phonon population is excited in a nanoscale cell, enabling the ensuing local nonequilibrium. Finding and tuning a material with these properties is challenging. In Paper II [C. Melnick and M. Kaviany, Phys. Rev. B 93, 125203 (2016), 10.1103/PhysRevB.93.125203], we tune the band gap of graphite within density functional theory through hydrogenation and the application of isotropic strains. The band gap is tuned to resonate with its energetic optical phonon modes and calculate the ab initio electron-phonon and phonon-phonon scattering rates. While hydrogenation degrades the strong electron-phonon coupling in graphene such that the figure of merit vanishes, we outline the methodology for a continued material search.

Thermoelectric study of Ag doped SnSe-Sb2Se3 based alloy

NASA Astrophysics Data System (ADS)

Das, Anish; Talukdar, M.; Kumar, Aparabal; Sarkar, Kalyan Jyoti; Dhama, P.; Banerji, P.

2018-05-01

In this article we have synthesized p-type alloy of SnSe and Sb2Se3 (10 atomic %) to study the thermoelectric transport properties. The alloy was prepared by melt grown technique followed by spark plasma sintering and latter doped with 2 atomic % Ag to compensate the carrier density in order to achieve higher electrical conductivity (σ). Out of these, the doped sample resulted in the maximum figure of merit, ZT˜0.7 at 773 K due to the existence of the secondary phase AgSbSe2 and reduced lattice thermal conductivity (0.61 W m-1 K-1 at 300 K). The fitted lattice thermal conductivity shows that point defect and Umklapp scattering are the primary process of phonon scattering for all the samples whereas the fitted mobility data confirms acoustic phonon scattering along with point defect and grain boundary scattering to be the main carrier scattering mechanism. More over room temperature carrier density and electrical conductivity are found to increase for the doped sample which further corroborate (90%)SnSe-(10%)Sb2Se3:2%Ag to be a potential candidate for highly efficient thermoelectric materials.

Understanding lattice thermal conductivity in thermoelectric clathrates: A density functional theory study on binary Si-based type-I clathrates

NASA Astrophysics Data System (ADS)

Euchner, Holger; Pailhès, Stéphane; Giordano, Valentina M.; de Boissieu, Marc

2018-01-01

Despite their crystalline nature, thermoelectric clathrates exhibit a strongly reduced lattice thermal conductivity. While the reason for this unexpected behavior is known to lie in the peculiarities of the complex crystal structure and the interplay of the underlying guest-host framework, their respective roles are still not fully disentangled and understood. Our ab initio study of the most simple type-I clathrate phase, the binary compound Ba8Si46 and its derivatives Ba8 -xSi46 seeks to identify these mechanisms and provides insight into their origin. Indeed, the strongly decreased lattice thermal conductivity in thermoelectric clathrates is a consequence of a reduction of the acoustic phonon bandwidth, a lowering of the acoustic phonon group velocities, and the amplification of three-phonon-scattering processes. While the complexity of the crystal structure is demonstrated not to be the leading factor, the reasons are manifold. A modified Si-Si interaction causes a first decrease of the sound velocity, whereas the presence of flat Ba modes results in an additional lowering. These modes correspond to confined Bloch states that are localized on the Ba atoms and significantly increase the scattering phase space and, together with an increased anharmonicity of the interatomic interactions, strongly affect the phonon lifetimes.

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.

Intrinsic phonon-limited charge carrier mobilities in thermoelectric SnSe

NASA Astrophysics Data System (ADS)

Ma, Jinlong; Chen, Yani; Li, Wu

2018-05-01

Within the past few years, tin selenide (SnSe) has attracted intense interest due to its remarkable thermoelectric potential for both n - and p -type crystals. In this work, the intrinsic phonon-limited electron/hole mobilities of SnSe are investigated using a Boltzmann transport equation based on first-principles calculated electron-phonon interactions. We find that the electrons have much larger mobilities than the holes. At room temperature, the mobilities of electrons along the a , b , and c axes are 325, 801, and 623 cm2/V s, respectively, whereas those of holes are 100, 299, and 291 cm2/V s, respectively. The anisotropy of mobilities is consistent with the reciprocal effective mass at band edges. The mode-specific analysis shows that the highest longitudinal optical phonons, rather than previously assumed acoustic phonons, dominate the scattering processes and consequently the mobilities in SnSe. The room-temperature largest mean free paths of electrons and holes in SnSe are about 21 and 13 nm, respectively.

Slow Noncollinear Coulomb Scattering in the Vicinity of the Dirac Point in Graphene.

PubMed

König-Otto, J C; Mittendorff, M; Winzer, T; Kadi, F; Malic, E; Knorr, A; Berger, C; de Heer, W A; Pashkin, A; Schneider, H; Helm, M; Winnerl, S

2016-08-19

The Coulomb scattering dynamics in graphene in energetic proximity to the Dirac point is investigated by polarization resolved pump-probe spectroscopy and microscopic theory. Collinear Coulomb scattering rapidly thermalizes the carrier distribution in k directions pointing radially away from the Dirac point. Our study reveals, however, that, in almost intrinsic graphene, full thermalization in all directions relying on noncollinear scattering is much slower. For low photon energies, carrier-optical-phonon processes are strongly suppressed and Coulomb mediated noncollinear scattering is remarkably slow, namely on a ps time scale. This effect is very promising for infrared and THz devices based on hot carrier effects.

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

Nunes, O. A. C., E-mail: oacn@unb.br

We study the interaction of Dirac Fermions in monolayer graphene on a GaAs substrate in an applied electric field by the combined action of the extrinsic potential of piezoelectric surface acoustical phonons of GaAs (piezoelectric acoustical (PA)) and of the intrinsic deformation potential of acoustical phonons in graphene (deformation acoustical (DA)). We find that provided the dc field exceeds a threshold value, emission of piezoelectric (PA) and deformation (DA) acoustical phonons can be obtained in a wide frequency range up to terahertz at low and high temperatures. We found that the phonon amplification rate R{sup PA,DA} scales with T{sub BG}{supmore » S−1} (S=PA,DA), T{sub BG}{sup S} being the Block−Gru{sup ¨}neisen temperature. In the high-T Block−Gru{sup ¨}neisen regime, extrinsic PA phonon scattering is suppressed by intrinsic DA phonon scattering, where the ratio R{sup PA}/R{sup DA} scales with ≈1/√(n), n being the carrier concentration. We found that only for carrier concentration n≤10{sup 10}cm{sup −2}, R{sup PA}/R{sup DA}>1. In the low-T Block−Gru{sup ¨}neisen regime, and for n=10{sup 10}cm{sup −2}, the ratio R{sup PA}/R{sup DA} scales with T{sub BG}{sup DA}/T{sub BG}{sup PA}≈7.5 and R{sup PA}/R{sup DA}>1. In this regime, PA phonon dominates the electron scattering and R{sup PA}/R{sup DA}<1 otherwise. This study is relevant to the exploration of the acoustic properties of graphene and to the application of graphene as an acoustical phonon amplifier and a frequency-tunable acoustical phonon device.« less

Magnetic scattering effects in two-band superconductor: the ferromagnetic dopants in MgB₂.

PubMed

Li, W X; Zeng, R; Poh, C K; Li, Y; Dou, S X

2010-04-07

This paper demonstrates the magnetic scattering effects on the electron-phonon interaction in two-band superconductors based on the transition-metal-doped MgB₂ to clarify the effects of magnetic dopants on multi-band superconductivity. The phonon properties of polycrystalline Mg(1-x)M(x)B₂ (M = Fe, Ni and Co), with x up to 0.05, were studied, with the investigation based on the normal state Raman spectra, especially the variation of the E(2g) mode. The magnetic scattering effect of Fe is much weaker than that of Mn in MgB₂, while it is stronger than that of Ni. The weak magnetic scattering effects are responsible for the superconducting behaviors of Mg(1 - x)Fe(x)B₂ and Mg(1 - x)Ni(x)B₂. Co shows almost no magnetic scattering effects on the superconductivity, while the depression of the critical temperature, T(c), in Mg(1 - x)Co(x)B₂ is attributed to the phonon behavior and is independent of the ferromagnetic nature of cobalt.

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.

Orbitally driven low thermal conductivity of monolayer gallium nitride (GaN) with planar honeycomb structure: a comparative study.

PubMed

Qin, Zhenzhen; Qin, Guangzhao; Zuo, Xu; Xiong, Zhihua; Hu, Ming

2017-03-23

Two-dimensional (2D) materials with graphene as a representative have been intensively studied for a long time. Recently, monolayer gallium nitride (ML GaN) with honeycomb structure was successfully fabricated in experiments, generating enormous research interest for its promising applications in nano- and opto-electronics. Considering all these applications are inevitably involved with thermal transport, systematic investigation of the phonon transport properties of 2D GaN is in demand. In this paper, by solving the Boltzmann transport equation (BTE) based on first-principles calculations, we performed a comprehensive study of the phonon transport properties of ML GaN, with detailed comparison to bulk GaN, 2D graphene, silicene and ML BN with similar honeycomb structure. Considering the similar planar structure of ML GaN to graphene, it is quite intriguing to find that the thermal conductivity (κ) of ML GaN (14.93 W mK -1 ) is more than two orders of magnitude lower than that of graphene and is even lower than that of silicene with a buckled structure. Systematic analysis is performed based on the study of the contribution from phonon branches, comparison among the mode level phonon group velocity and lifetime, the detailed process and channels of phonon-phonon scattering, and phonon anharmonicity with potential energy well. We found that, different from graphene and ML BN, the phonon-phonon scattering selection rule in 2D GaN is slightly broken by the lowered symmetry due to the large difference in the atomic radius and mass between Ga and N atoms. Further deep insight is gained from the electronic structure. Resulting from the special sp orbital hybridization mediated by the Ga-d orbital in ML GaN, the strongly polarized Ga-N bond, localized charge density, and its inhomogeneous distribution induce large phonon anharmonicity and lead to the intrinsic low κ of ML GaN. The orbitally driven low κ of ML GaN unraveled in this work would make 2D GaN prospective for applications in energy conversion such as thermoelectrics. Our study offers fundamental understanding of phonon transport in ML GaN within the framework of BTE and further electronic structure, which will enrich the studies of nanoscale phonon transport in 2D materials and shed light on further studies.

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.

Influence of phonon-assisted tunneling on the linear thermoelectric transport through molecular quantum dots

NASA Astrophysics Data System (ADS)

Khedri, A.; Meden, V.; Costi, T. A.

2017-11-01

We investigate the effect of vibrational degrees of freedom on the linear thermoelectric transport through a single-level quantum dot described by the spinless Anderson-Holstein impurity model. To study the effects of strong electron-phonon coupling, we use the nonperturbative numerical renormalization group approach. We also compare our results, at weak to intermediate coupling, with those obtained by employing the functional renormalization group method, finding good agreement in this parameter regime. When applying a gate voltage at finite temperatures, the inelastic scattering processes, induced by phonon-assisted tunneling, result in an interesting interplay between electrical and thermal transport. We explore different parameter regimes and identify situations for which the thermoelectric power as well as the dimensionless figure of merit are significantly enhanced via a Mahan-Sofo type of mechanism. We show, in particular, that this occurs at strong electron-phonon coupling and in the antiadiabatic regime.

Spatial Distortion of Vibration Modes via Magnetic Correlation of Impurities

NASA Astrophysics Data System (ADS)

Krasniqi, F. S.; Zhong, Y.; Epp, S. W.; Foucar, L.; Trigo, M.; Chen, J.; Reis, D. A.; Wang, H. L.; Zhao, J. H.; Lemke, H. T.; Zhu, D.; Chollet, M.; Fritz, D. M.; Hartmann, R.; Englert, L.; Strüder, L.; Schlichting, I.; Ullrich, J.

2018-03-01

Long wavelength vibrational modes in the ferromagnetic semiconductor Ga0.91 Mn0.09 As are investigated using time resolved x-ray diffraction. At room temperature, we measure oscillations in the x-ray diffraction intensity corresponding to coherent vibrational modes with well-defined wavelengths. When the correlation of magnetic impurities sets in, we observe the transition of the lattice into a disordered state that does not support coherent modes at large wavelengths. Our measurements point toward a magnetically induced broadening of long wavelength vibrational modes in momentum space and their quasilocalization in the real space. More specifically, long wavelength vibrational modes cannot be assigned to a single wavelength but rather should be represented as a superposition of plane waves with different wavelengths. Our findings have strong implications for the phonon-related processes, especially carrier-phonon and phonon-phonon scattering, which govern the electrical conductivity and thermal management of semiconductor-based devices.

Multiphonon: Phonon Density of States tools for Inelastic Neutron Scattering Powder Data

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

Y. Y. Lin, Jiao; Islam, Fahima; Kresh, Max

The multiphonon python package calculates phonon density of states, a reduced representation of vibrational property of condensed matter (see, for example, Section “Density of Normal Modes” in Chapter 23 “Quantum Theory of the Harmonic Crystal” of (Ashcroft and Mermin 2011)), from inelastic neutron scattering (see, for example (B. Fultz et al. 2006–2016)) spectrum from a powder sample. Inelastic neutron spectroscopy (INS) is a probe of excitations in solids of vibrational or magnetic origins. In INS, neutrons can lose(gain) energy to(from) the solid in the form of quantized lattice vibrations – phonons. Measuring phonon density of states is usually the firstmore » step in determining the phonon properties of a material experimentally. Phonons play a very important role in understanding the physical properties of a solid, including thermal conductivity and electrical conductivity. Hence, INS is an important tool for studying thermoelectric materials (Budai et al. 2014, Li et al. (2015)), where low thermal conductivity and high electrical conductivity are desired. Study of phonon entropy also made important contributions to the research of thermal dynamics and phase stability of materials (B. Fultz 2010, bogdanoff2002phonon, swan2006vibrational).« less

Tunable heat conduction through coupled Fermi-Pasta-Ulam chains

NASA Astrophysics Data System (ADS)

Su, Ruixia; Yuan, Zongqiang; Wang, Jun; Zheng, Zhigang

2015-01-01

We conduct a study on heat conduction through coupled Fermi-Pasta-Ulam (FPU) chains by using classical molecular dynamics simulations. Our attention is dedicated to showing how the phonon transport is affected by the interchain coupling. It has been well accepted that the heat conduction could be impeded by the interchain interaction due to the interface phonon scattering. However, recent theoretical and experimental studies suggest that the thermal conductivity of nanoscale materials can be counterintuitively enhanced by the interaction with the substrate. In the present paper, by consecutively varying the interchain coupling intensity, we observed both enhancement and suppression of thermal transport through the coupled FPU chains. For weak interchain couplings, it is found that the heat flux increases with the coupling intensity, whereas in the case of strong interchain couplings, the energy transport is found to be suppressed by the interchain interaction. Based on the phonon spectral energy density method, we attribute the enhancement of the energy transport to the excited phonon modes (in addition to the intrinsic phonon modes), while the upward shift of the high-frequency phonon branch and the interface phonon-phonon scattering account for the suppressed heat conduction.

Multiphonon: Phonon Density of States tools for Inelastic Neutron Scattering Powder Data

DOE PAGES

Y. Y. Lin, Jiao; Islam, Fahima; Kresh, Max

2018-01-29

The multiphonon python package calculates phonon density of states, a reduced representation of vibrational property of condensed matter (see, for example, Section “Density of Normal Modes” in Chapter 23 “Quantum Theory of the Harmonic Crystal” of (Ashcroft and Mermin 2011)), from inelastic neutron scattering (see, for example (B. Fultz et al. 2006–2016)) spectrum from a powder sample. Inelastic neutron spectroscopy (INS) is a probe of excitations in solids of vibrational or magnetic origins. In INS, neutrons can lose(gain) energy to(from) the solid in the form of quantized lattice vibrations – phonons. Measuring phonon density of states is usually the firstmore » step in determining the phonon properties of a material experimentally. Phonons play a very important role in understanding the physical properties of a solid, including thermal conductivity and electrical conductivity. Hence, INS is an important tool for studying thermoelectric materials (Budai et al. 2014, Li et al. (2015)), where low thermal conductivity and high electrical conductivity are desired. Study of phonon entropy also made important contributions to the research of thermal dynamics and phase stability of materials (B. Fultz 2010, bogdanoff2002phonon, swan2006vibrational).« less

Revisiting the temperature dependence of the homogeneous R 1 linewidth in ruby

NASA Astrophysics Data System (ADS)

Riesen, Hans; Szabo, Alex

2010-01-01

Transient spectral-hole-burning studies of the R 1(±3/2) line ( E¯ ( 2E) ← 4A 2(±3/2)) in 20 ppm ruby were conducted between 2.4 and 50 K in a low magnetic field ( B|| = 9.15 mT) and the results were supplemented with the original data of McCumber and Sturge. A direct one-phonon process, 2A¯←E¯, is the main contribution to the linewidth up to 50 K whereas at higher temperatures two-phonon Raman scattering becomes dominant. The two processes are well described by ΔΓdirect=Γ0/(exp(Δ/kT)-1) and a non-perturbative expression for the electron-phonon interaction developed by Hsu and Skinner. The value of Γ0 = 141 (±4) MHz is in excellent agreement with the result of 142 ± 6 MHz previously obtained for the R 2 line.

Trigonal LaF3: a novel SRS-active crystal

NASA Astrophysics Data System (ADS)

Kaminskii, A. A.; Lux, O.; Hanuza, J.; Rhee, H.; Eichler, H. J.; Zhang, J.; Tang, D.; Shen, D.; Yoneda, H.; Shirakawa, A.

2014-12-01

Trigonal fluoride LaF3, widely known as a host crystal for Ln3+-lasants, was found to be an attractive many-phonon Raman material and a subject for the investigation of different χ(3)-nonlinear optical effects. We present the manifestation of photon-phonon interactions related to stimulated Raman scattering (SRS) and Raman-induced four-wave mixing (RFWM) processes, initiated by picosecond exсitation at room temperature. Sesqui-octave-spanning Stokes and anti-Stokes frequency comb generation as well as many-step cascaded and cross-cascaded up-conversion χ(3)-nonlinear processes have been observed. The recorded spectral lines originated by SRS and RFWM are identified and attributed to the three observed SRS-promoting phonon modes. The lower limit of the steady-state Raman gain coefficient for near-IR first Stokes generation was estimated. Moreover, a brief review of known Ln3+ : LaF3 laser crystals and SRS-active fluorides is given.

Ultralow Thermal Conductivity in Diamond-Like Semiconductors: Selective Scattering of Phonons from Antisite Defects

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

Gorai, Prashun; Stevanovic, Vladan; Toberer, Eric

In this work, we discover anomalously low lattice thermal conductivity (<0.25 W/mK at 300 degrees C) in the Hg-containing quaternary diamond-like semiconductors within the Cu2IIBIVTe4 (IIB: Zn, Cd, Hg) (IV: Si, Ge, Sn) set of compositions. Using high-temperature X-ray diffraction, resonant ultrasound spectroscopy, and transport properties, we uncover the critical role of the antisite defects HgCu and CuHg on phonon transport within the Hg-containing systems. Despite the differences in chemistry between Hg and Cu, the high concentration of these antisite defects emerges from the energetic proximity of the kesterite and stannite cation motifs. Our phonon calculations reveal that heavier groupmore » IIB elements not only introduce low-lying optical modes, but the subsequent antisite defects also possess unusually strong point defect phonon scattering power. The scattering strength stems from the fundamentally different vibrational modes supported by the constituent elements (e.g., Hg and Cu). Despite the significant impact on the thermal properties, antisite defects do not negatively impact the mobility (>50 cm2/(Vs) at 300 degrees C) in Hg-containing systems, leading to predicted zT > 1.5 in Cu2HgGeTe4 and Cu2HgSnTe4 under optimized doping. In addition to introducing a potentially new p-type thermoelectric material, this work provides (1) a strategy to use the proximity of phase transitions to increase point defect phonon scattering, and (2) a means to quantify the power of a given point defect through inexpensive phonon calculations.« less

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.

Lattice dynamics and thermal transport in multiferroic CuCrO 2

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

Bansal, Dipanshu; Niedziela, Jennifer L.; May, Andrew F.

Inelastic neutron and x-ray scattering measurements of phonons and spin waves in CuCrO 2 were performed over a wide range of temperature, and complemented with first-principles simulations. The phonon dispersions and density of states are well reproduced by our density functional cal- culations, and reveal a strong anisotropy of Cu vibrations, with large amplitudes of low-frequency in-plane motions. In addition, we find that spin fluctuations persist above 300 K, far above the N eel temperature for long-range antiferromagnetic order, TN. Modeling of the thermal conductivity, based on our phonon measurements and simulations, reveals a significant anisotropy and indicates that themore » spin fluctuations above TN constitute a strong source of phonon scattering.« less

Lattice dynamics and thermal transport in multiferroic CuCrO 2

DOE PAGES

Bansal, Dipanshu; Niedziela, Jennifer L.; May, Andrew F.; ...

2017-02-09

Inelastic neutron and x-ray scattering measurements of phonons and spin waves in CuCrO 2 were performed over a wide range of temperature, and complemented with first-principles simulations. The phonon dispersions and density of states are well reproduced by our density functional cal- culations, and reveal a strong anisotropy of Cu vibrations, with large amplitudes of low-frequency in-plane motions. In addition, we find that spin fluctuations persist above 300 K, far above the N eel temperature for long-range antiferromagnetic order, TN. Modeling of the thermal conductivity, based on our phonon measurements and simulations, reveals a significant anisotropy and indicates that themore » spin fluctuations above TN constitute a strong source of phonon scattering.« less

Polar rotor scattering as atomic-level origin of low mobility and thermal conductivity of perovskite CH3NH3PbI3

PubMed Central

Li, Bing; Kawakita, Yukinobu; Liu, Yucheng; Wang, Mingchao; Matsuura, Masato; Shibata, Kaoru; Ohira-Kawamura, Seiko; Yamada, Takeshi; Lin, Shangchao; Nakajima, Kenji; Liu, Shengzhong (Frank)

2017-01-01

Perovskite CH3NH3PbI3 exhibits outstanding photovoltaic performances, but the understanding of the atomic motions remains inadequate even though they take a fundamental role in transport properties. Here, we present a complete atomic dynamic picture consisting of molecular jumping rotational modes and phonons, which is established by carrying out high-resolution time-of-flight quasi-elastic and inelastic neutron scattering measurements in a wide energy window ranging from 0.0036 to 54 meV on a large single crystal sample, respectively. The ultrafast orientational disorder of molecular dipoles, activated at ∼165 K, acts as an additional scattering source for optical phonons as well as for charge carriers. It is revealed that acoustic phonons dominate the thermal transport, rather than optical phonons due to sub-picosecond lifetimes. These microscopic insights provide a solid standing point, on which perovskite solar cells can be understood more accurately and their performances are perhaps further optimized. PMID:28665407

Three-dimensional phonon population anisotropy in silicon nanomembranes

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

McElhinny, Kyle M.; Gopalakrishnan, Gokul; Holt, Martin V.

Nanoscale single crystals possess modified phonon dispersions due to the truncation of the crystal. The introduction of surfaces alters the population of phonons relative to the bulk and introduces anisotropy arising from the breaking of translational symmetry. Such modifications exist throughout the Brillouin zone, even in structures with dimensions of several nanometers, posing a challenge to the characterization of vibrational properties and leading to uncertainty in predicting the thermal, optical, and electronic properties of nanomaterials. Synchrotron x-ray thermal diffuse scattering studies find that freestanding Si nanomembranes with thicknesses as large as 21 nm exhibit a higher scattering intensity per unitmore » thickness than bulk silicon. In addition, the anisotropy arising from the finite thickness of these membranes produces particularly intense scattering along reciprocal-space directions normal to the membrane surface compared to corresponding in-plane directions. These results reveal the dimensions at which calculations of materials properties and device characteristics based on bulk phonon dispersions require consideration of the nanoscale size of the crystal.« less

Lattice dynamics and thermal transport in multiferroic CuCrO2

NASA Astrophysics Data System (ADS)

Bansal, Dipanshu; Niedziela, Jennifer L.; May, Andrew F.; Said, Ayman; Ehlers, Georg; Abernathy, Douglas L.; Huq, Ashfia; Kirkham, Melanie; Zhou, Haidong; Delaire, Olivier

2017-02-01

Inelastic neutron and x-ray scattering measurements of phonons and spin waves were performed in the delafossite compound CuCrO2 over a wide range of temperature, and complemented with first-principles lattice dynamics simulations. The phonon dispersions and density of states are well reproduced by our density functional calculations, and reveal a strong anisotropy of Cu vibrations, which exhibit low-frequency modes of large amplitude parallel to the basal plane of the layered delafossite structure. The low frequency in-plane modes also show a systematic temperature dependence of neutron and x-ray scattering intensities. In addition, we find that spin fluctuations persist above 300 K, far above the Néel temperature for long-range antiferromagnetic order, TN≃24 K . Our modeling of the thermal conductivity, based on our phonon measurements and simulations, reveals a significant anisotropy and indicates that spin fluctuations above TN constitute an important source of phonon scattering, considerably suppressing the thermal conductivity compared to that of the isostructural but nonmagnetic compound CuAlO2.

Modeling of phonon scattering in n-type nanowire transistors using one-shot analytic continuation technique

NASA Astrophysics Data System (ADS)

Bescond, Marc; Li, Changsheng; Mera, Hector; Cavassilas, Nicolas; Lannoo, Michel

2013-10-01

We present a one-shot current-conserving approach to model the influence of electron-phonon scattering in nano-transistors using the non-equilibrium Green's function formalism. The approach is based on the lowest order approximation (LOA) to the current and its simplest analytic continuation (LOA+AC). By means of a scaling argument, we show how both LOA and LOA+AC can be easily obtained from the first iteration of the usual self-consistent Born approximation (SCBA) algorithm. Both LOA and LOA+AC are then applied to model n-type silicon nanowire field-effect-transistors and are compared to SCBA current characteristics. In this system, the LOA fails to describe electron-phonon scattering, mainly because of the interactions with acoustic phonons at the band edges. In contrast, the LOA+AC still well approximates the SCBA current characteristics, thus demonstrating the power of analytic continuation techniques. The limits of validity of LOA+AC are also discussed, and more sophisticated and general analytic continuation techniques are suggested for more demanding cases.

Crossover from incoherent to coherent phonon scattering in epitaxial oxide superlattices.

PubMed

Ravichandran, Jayakanth; Yadav, Ajay K; Cheaito, Ramez; Rossen, Pim B; Soukiassian, Arsen; Suresha, S J; Duda, John C; Foley, Brian M; Lee, Che-Hui; Zhu, Ye; Lichtenberger, Arthur W; Moore, Joel E; Muller, David A; Schlom, Darrell G; Hopkins, Patrick E; Majumdar, Arun; Ramesh, Ramamoorthy; Zurbuchen, Mark A

2014-02-01

Elementary particles such as electrons or photons are frequent subjects of wave-nature-driven investigations, unlike collective excitations such as phonons. The demonstration of wave-particle crossover, in terms of macroscopic properties, is crucial to the understanding and application of the wave behaviour of matter. We present an unambiguous demonstration of the theoretically predicted crossover from diffuse (particle-like) to specular (wave-like) phonon scattering in epitaxial oxide superlattices, manifested by a minimum in lattice thermal conductivity as a function of interface density. We do so by synthesizing superlattices of electrically insulating perovskite oxides and systematically varying the interface density, with unit-cell precision, using two different epitaxial-growth techniques. These observations open up opportunities for studies on the wave nature of phonons, particularly phonon interference effects, using oxide superlattices as model systems, with extensive applications in thermoelectrics and thermal management.

Inelastic neutron scattering study of phonon density of states in nanostructured Si1 xGex thermoelectrics

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

Dhital, Chetan; Abernathy, Douglas L; Zhu, Gaohua

2012-01-01

Inelastic neutron scattering measurements are utilized to explore relative changes in the generalized phonon density of states of nanocrystalline Si1 xGex thermoelectric materials prepared via ball-milling and hot-pressing techniques. Dynamic signatures of Ge clustering can be inferred from the data by referencing the resulting spectra to a density functional theoretical model assuming homogeneous alloying via the virtual-crystal approximation. Comparisons are also presented between as-milled Si nanopowder and bulk, polycrystalline Si where a preferential low-energy enhancement and lifetime broadening of the phonon density of states appear in the nanopowder. Negligible differences are however observed between the phonon spectra of bulk Simore » andhot-pressed, nanostructured Si samples suggesting that changes to the single-phonon dynamics above 4 meV play only a secondary role in the modified heat conduction of this compound.« less

Impurity and phonon scattering in silicon nanowires

NASA Astrophysics Data System (ADS)

Zhang, W.; Persson, M. P.; Mera, H.; Delerue, C.; Niquet, Y. M.; Allan, G.; Wang, E.

2011-03-01

We model the scattering of electrons by phonons and dopant impurities in ultimate [110]-oriented gate-all-around silicon nanowires with an atomistic valence force field and tight-binding approach. All electron-phonons interactions are included. We show that impurity scattering can reduce with decreasing nanowire diameter due to the enhanced screening by the gate. Donors and acceptors however perform very differently : acceptors behave as tunnel barriers for the electrons, while donors behave as quantum wells which introduce Fano resonances in the conductance. As a consequence the acceptors are much more limiting the mobility than the donors. The resistances of single acceptors are also very dependent on their radial position in the nanowire, which might be a significant source of variability in ultimate silicon nanowire devices. Concerning phonons, we show that, as a result of strong confinement, i) electrons couple to a wide and complex distribution of phonons modes, and ii) the mobility has a non-monotonic variation with wire diameter and is strongly reduced with respect to bulk. French National Research Agency ANR project QUANTAMONDE Contract No. ANR-07-NANO-023-02 and by the Délégation Générale pour l'Armement, French Ministry of Defense under Grant No. 2008.34.0031.

Superparamagnetic enhancement of thermoelectric performance.

PubMed

Zhao, Wenyu; Liu, Zhiyuan; Sun, Zhigang; Zhang, Qingjie; Wei, Ping; Mu, Xin; Zhou, Hongyu; Li, Cuncheng; Ma, Shifang; He, Danqi; Ji, Pengxia; Zhu, Wanting; Nie, Xiaolei; Su, Xianli; Tang, Xinfeng; Shen, Baogen; Dong, Xiaoli; Yang, Jihui; Liu, Yong; Shi, Jing

2017-09-13

The ability to control chemical and physical structuring at the nanometre scale is important for developing high-performance thermoelectric materials. Progress in this area has been achieved mainly by enhancing phonon scattering and consequently decreasing the thermal conductivity of the lattice through the design of either interface structures at nanometre or mesoscopic length scales or multiscale hierarchical architectures. A nanostructuring approach that enables electron transport as well as phonon transport to be manipulated could potentially lead to further enhancements in thermoelectric performance. Here we show that by embedding nanoparticles of a soft magnetic material in a thermoelectric matrix we achieve dual control of phonon- and electron-transport properties. The properties of the nanoparticles-in particular, their superparamagnetic behaviour (in which the nanoparticles can be magnetized similarly to a paramagnet under an external magnetic field)-lead to three kinds of thermoelectromagnetic effect: charge transfer from the magnetic inclusions to the matrix; multiple scattering of electrons by superparamagnetic fluctuations; and enhanced phonon scattering as a result of both the magnetic fluctuations and the nanostructures themselves. We show that together these effects can effectively manipulate electron and phonon transport at nanometre and mesoscopic length scales and thereby improve the thermoelectric performance of the resulting nanocomposites.

Intrinsic and extrinsic electrical and thermal transport of bulk black phosphorus

NASA Astrophysics Data System (ADS)

Hu, Sile; Xiang, Junsen; Lv, Meng; Zhang, Jiahao; Zhao, Hengcan; Li, Chunhong; Chen, Genfu; Wang, Wenhong; Sun, Peijie

2018-01-01

We report a comprehensive investigation of the electrical, thermal, and thermoelectric transport properties of bulk single-crystalline black phosphorus in wide temperature (2-300 K) and field (0-9 T) ranges. Electrical transport below T ≈ 250 K is found to be dominated by extrinsic hole-type charge carriers with large mobility exceeding 104 cm2/V s at low temperatures. While thermal transport measurements reveal an enhanced in-plane thermal conductivity maximum κ = 180 W/m K at T ≈ 25 K, it appears still to be largely constrained by extrinsic phonon scattering processes, e.g., the electron-phonon process, in addition to intrinsic umklapp scattering. The thermoelectric power and Nernst effect seem to be strongly influenced by ambipolar transport of charge carriers with opposite signs in at least the high-temperature region above 200 K, which diminishes the thermoelectric power factor of this material. Our results provide a timely update to the transport properties of bulk black phosphorus for future fundamental and applied research.

A chip-integrated coherent photonic-phononic memory.

PubMed

Merklein, Moritz; Stiller, Birgit; Vu, Khu; Madden, Stephen J; Eggleton, Benjamin J

2017-09-18

Controlling and manipulating quanta of coherent acoustic vibrations-phonons-in integrated circuits has recently drawn a lot of attention, since phonons can function as unique links between radiofrequency and optical signals, allow access to quantum regimes and offer advanced signal processing capabilities. Recent approaches based on optomechanical resonators have achieved impressive quality factors allowing for storage of optical signals. However, so far these techniques have been limited in bandwidth and are incompatible with multi-wavelength operation. In this work, we experimentally demonstrate a coherent buffer in an integrated planar optical waveguide by transferring the optical information coherently to an acoustic hypersound wave. Optical information is extracted using the reverse process. These hypersound phonons have similar wavelengths as the optical photons but travel at five orders of magnitude lower velocity. We demonstrate the storage of phase and amplitude of optical information with gigahertz bandwidth and show operation at separate wavelengths with negligible cross-talk.Optical storage implementations based on optomechanical resonator are limited to one wavelength. Here, exploiting stimulated Brillouin scattering, the authors demonstrate a coherent optical memory based on a planar integrated waveguide, which can operate at different wavelengths without cross-talk.

Quantum non-demolition phonon counter with a hybrid optomechnical system

NASA Astrophysics Data System (ADS)

Song, Qiao; Zhang, KeYe; Dong, Ying; Zhang, WeiPing

2018-05-01

A phonon counting scheme based on the control of polaritons in an optomechanical system is proposed. This approach permits us to measure the number of phonons in a quantum non-demolition (QND) manner for arbitrary modes not limited by the frequency matching condition as in usual photon-phonon scattering detections. The performance on phonon number transfer and quantum state transfer of the counter are analyzed and simulated numerically by taking into account all relevant sources of noise.

High-Field Quasiballistic Transport in Short Carbon Nanotubes

NASA Astrophysics Data System (ADS)

Javey, Ali; Guo, Jing; Paulsson, Magnus; Wang, Qian; Mann, David; Lundstrom, Mark; Dai, Hongjie

2004-03-01

Single walled carbon nanotubes with Pd Ohmic contacts and lengths ranging from several microns down to 10nm are investigated by electron transport experiments and theory. The mean-free path (MFP) for acoustic phonon scattering is estimated to be lap˜300 nm, and that for optical phonon scattering is lop˜15 nm. Transport through very short (˜10 nm) nanotubes is free of significant acoustic and optical phonon scattering and thus ballistic and quasiballistic at the low- and high-bias voltage limits, respectively. High currents of up to 70 μA can flow through a short nanotube. Possible mechanisms for the eventual electrical breakdown of short nanotubes at high fields are discussed. The results presented here have important implications to high performance nanotube transistors and interconnects.

Evidence for anisotropic polar nanoregions in relaxor Pb(Mg1/3Nb2/3)O3: A neutron study of the elastic constants and anomalous TA phonon damping in PMN

NASA Astrophysics Data System (ADS)

Stock, C.; Gehring, P. M.; Hiraka, H.; Swainson, I.; Xu, Guangyong; Ye, Z.-G.; Luo, H.; Li, J.-F.; Viehland, D.

2012-09-01

We use neutron inelastic scattering to characterize the acoustic phonons in the relaxor Pb(Mg1/3Nb2/3)O3 (PMN) and demonstrate the presence of a highly anisotropic damping mechanism that is directly related to short-range polar correlations. For a large range of temperatures above Tc˜210 K, where dynamic, short-range polar correlations are present, acoustic phonons propagating along [11¯0] and polarized along [110] (TA2 phonons) are overdamped and softened across most of the Brillouin zone. By contrast, acoustic phonons propagating along [100] and polarized along [001] (TA1 phonons) are overdamped and softened for a more limited range of wave vectors q. The anisotropy and temperature dependence of the acoustic phonon energy linewidth Γ are directly correlated with neutron diffuse scattering cross section, indicating that polar nanoregions are the cause of the anomalous behavior. The damping and softening vanish for q→0, i.e., for long-wavelength acoustic phonons near the zone center, which supports the notion that the anomalous damping is a result of the coupling between the relaxational component of the diffuse scattering and the harmonic TA phonons. Therefore, these effects are not due to large changes in the elastic constants with temperature because the elastic constants correspond to the long-wavelength limit. We compare the elastic constants we measure to those from Brillouin scattering experiments and to values reported for pure PbTiO3. We show that while the values of C44 are quite similar, those for C11 and C12 are significantly less in PMN and result in a softening of (C11-C12) over PbTiO3. The elastic constants also show an increased elastic anisotropy [2C44/(C11-C12)] in PMN versus that in PbTiO3. These results are suggestive of an instability to TA2 acoustic fluctuations in PMN and other relaxor ferroelectrics. We discuss our results in the context of the current debate over the “waterfall” effect and show that they are inconsistent with acoustic-optic phonon coupling or other models that invoke the presence of a second, low-energy optic mode.

Heat transport by phonons in crystalline materials and nanostructures

NASA Astrophysics Data System (ADS)

Koh, Yee Kan

This dissertation presents experimental studies of heat transport by phonons in crystalline materials and nanostructures, and across solid-solid interfaces. Particularly, this dissertation emphasizes advancing understanding of the mean-free-paths (i.e., the distance phonons propagate without being scattered) of acoustic phonons, which are the dominant heat carriers in most crystalline semiconductor nanostructures. Two primary tools for the studies presented in this dissertation are time-domain thermoreflectance (TDTR) for measurements of thermal conductivity of nanostructures and thermal conductance of interfaces; and frequency-domain thermoreflectance (FDTR), which I developed as a direct probe of the mean-free-paths of dominant heat-carrying phonons in crystalline solids. The foundation of FDTR is the dependence of the apparent thermal conductivity on the frequency of periodic heat sources. I find that the thermal conductivity of semiconductor alloys (InGaP, InGaAs, and SiGe) measured by TDTR depends on the modulation frequency, 0.1 ≤ f ≤ 10 MHz, used in TDTR measurements. Reduction in the thermal conductivity of the semiconductor alloys at high f compares well to the reduction in the thermal conductivity of epitaxial thin films, indicating that frequency dependence and thickness dependence of thermal conductivity are fundamentally equivalent. I developed the frequency dependence of thermal conductivity into a convenient probe of phonon mean-free-paths, a technique which I call frequency-domain thermoreflectance (FDTR). In FDTR, I monitor the changes in the intensity of the reflected probe beam as a function of the modulation frequency. To facilitate the analysis of FDTR measurements, I developed a nonlocal theory for heat conduction by phonons at high heating frequencies. Calculations of the nonlocal theory confirm my experimental findings that phonons with mean-free-paths longer than two times the penetration depth do not contribute to the apparent thermal conductivity. I employed FDTR to study the mean-free-paths of acoustic phonons in Si1-xGex. I experimentally demonstrate that 40% of heat is carried in Si1-xGe x alloys by phonons with mean-free-path 0.5 ≤ ℓ ≤ 5 mum, and phonons with > 2 mum do not contribute to the thermal conductivity of Si. I employed TDTR and frequency-dependent TDTR to study scattering of long- and medium-wavelength phonons in two important thermoelectric materials embedded with nanoscale precipitates. I find that the through-thickness lattice thermal conductivity of (PbTe)1-x/(PbSe)x nanodot superlattices (NDSLs) approaches the thermal conductivity of bulk homogenous PbTe1-x Sex alloys with the same average composition. On the other hand, I find that 3% of ErAs nanoparticles embedded in InGaAs is sufficient to scatter most of the phonons in InGaAs that have intermediate mean-free-paths, and thus reduces the thermal conductivity of InGaAs below the alloy limit. I find that scattering by nanoparticles approach the geometrical limit and can be readily accounted for by an additional boundary scattering which depends on the concentration of nanoparticles. Finally, I studied the thermal conductance of Au/Ti/Graphene/SiO 2 interfaces by TDTR. I find that heat transport across the interface is dominated by phonons. Even though graphene is only one atomic layer thick, graphene interfaces should be treated as two discrete interfaces instead of one diffuse interface in thermal analysis, suggesting that direct transmission of phonons from Au to SiO2 is negligible. My study is important for thermal management of graphene devices.

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.

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

Mikheev, Evgeny; Himmetoglu, Burak; Kajdos, Adam P.

We analyze and compare the temperature dependence of the electron mobility of two- and three-dimensional electron liquids in SrTiO{sub 3}. The contributions of electron-electron scattering must be taken into account to accurately describe the mobility in both cases. For uniformly doped, three-dimensional electron liquids, the room temperature mobility crosses over from longitudinal optical (LO) phonon-scattering-limited to electron-electron-scattering-limited as a function of carrier density. In high-density, two-dimensional electron liquids, LO phonon scattering is completely screened and the mobility is dominated by electron-electron scattering up to room temperature. The possible origins of the observed behavior and the consequences for approaches to improvemore » the mobility are discussed.« less

Hierarchical thermoelectrics: crystal grain boundaries as scalable phonon scatterers

NASA Astrophysics Data System (ADS)

Selli, Daniele; Boulfelfel, Salah Eddine; Schapotschnikow, Philipp; Donadio, Davide; Leoni, Stefano

2016-02-01

Thermoelectric materials are strategically valuable for sustainable development, as they allow for the generation of electrical energy from wasted heat. In recent years several strategies have demonstrated some efficiency in improving thermoelectric properties. Dopants affect carrier concentration, while thermal conductivity can be influenced by alloying and nanostructuring. Features at the nanoscale positively contribute to scattering phonons, however those with long mean free paths remain difficult to alter. Here we use the concept of hierarchical nano-grains to demonstrate thermal conductivity reduction in rocksalt lead chalcogenides. We demonstrate that grains can be obtained by taking advantage of the reconstructions along the phase transition path that connects the rocksalt structure to its high-pressure form. Since grain features naturally change as a function of size, they impact thermal conductivity over different length scales. To understand this effect we use a combination of advanced molecular dynamics techniques to engineer grains and to evaluate thermal conductivity in PbSe. By affecting grain morphologies only, i.e. at constant chemistry, two distinct effects emerge: the lattice thermal conductivity is significantly lowered with respect to the perfect crystal, and its temperature dependence is markedly suppressed. This is due to an increased scattering of low-frequency phonons by grain boundaries over different size scales. Along this line we propose a viable process to produce hierarchical thermoelectric materials by applying pressure via a mechanical load or a shockwave as a novel paradigm for material design.

Generalized Elliott-Yafet spin-relaxation time for arbitrary spin mixing

NASA Astrophysics Data System (ADS)

Vollmar, Svenja; Hilton, David J.; Schneider, Hans Christian

2017-08-01

We extend our recent result for the spin-relaxation time due to acoustic electron-phonon scattering in degenerate bands with spin mixing [New J. Phys. 18, 023012 (2016), 10.1088/1367-2630/18/2/023012] to include interactions with optical phonons, and present a numerical evaluation of the spin-relaxation time for intraband hole-phonon scattering in the heavy-hole (HH) bands of bulk GaAs. Comparing our computed spin-relaxation times to the conventional Elliott-Yafet result quantitatively demonstrates that the latter underestimates the spin-relaxation time because it does not correctly describe how electron-phonon interactions change the (vector) spin expectation value of the single-particle states. We show that the conventional Elliott-Yafet spin relaxation time is a special case of our result for weak spin mixing.

Phonon scattering in nanoscale systems: lowest order expansion of the current and power expressions

NASA Astrophysics Data System (ADS)

Paulsson, Magnus; Frederiksen, Thomas; Brandbyge, Mads

2006-04-01

We use the non-equilibrium Green's function method to describe the effects of phonon scattering on the conductance of nano-scale devices. Useful and accurate approximations are developed that both provide (i) computationally simple formulas for large systems and (ii) simple analytical models. In addition, the simple models can be used to fit experimental data and provide physical parameters.

Model for Ultrafast Carrier Scattering in Semiconductors

DTIC Science & Technology

2012-11-14

energy transfer between semi-classical carrier drift-diffusion under an electric field and quantum kinetics of interband /intersubband transitions...from an electron during each phonon-emission event. The net rate of phonon emission is determined by the Boltzmann scattering equation which depends ...energy-drift term under a strong dc field was demonstrated to reduce the field- dependent drift velocity and mobility. The Doppler shift in the energy

Kinetics of Electrons from Plasma Discharge in a Latent Track Region Induced by Swift Heavy ION Irradiation

NASA Astrophysics Data System (ADS)

Minárik, Stanislav

2015-08-01

While passing swift heavy ion through a material structure, it produces a region of radiation affected material which is known as a "latent track". Scattering motions of electrons interacting with a swift heavy ion are dominant in the latent track region. These phenomena include the electron impurity and phonon scattering processes modified by the interaction with the ion projectile as well as the Coulomb scattering between two electrons. In this paper, we provide detailed derivation of a 3D Boltzmann scattering equation for the description of the relative scattering motion of such electrons. Phase-space distribution function for this non-equilibrioum system of scattering electrons can be found by the solution of mentioned equation.

Intrinsic electronic transport and thermoelectric power factor in n-type doped monolayer MoS2

NASA Astrophysics Data System (ADS)

Zhao, Yinchang; Dai, Zhenhong; Zhang, Chao; Lian, Chao; Zeng, Shuming; Li, Geng; Meng, Sheng; Ni, Jun

2018-04-01

The electronic transport and thermoelectric properties in n-type doped monolayer MoS2 are investigated by a parameter-free method based on first-principles calculations, electron–phonon coupling (EPC), and Boltzmann transport equation (BTE). Remarkably, the calculated electron mobility μ ∼ 47 cm2 V‑1s‑1 and thermoelectric power factor σS 2 ∼ 2.93 × 10‑3 W m‑1 K‑2 at room temperature are much lower than the previous theoretical values (e.g. μ ∼ 130–410 cm2 V‑1 s‑1 and σS 2 ∼ 2.80 × 10‑2 W m‑1 K‑2), but agree well with the most recent experimental findings of μ ∼ 37 cm2 V‑1 s‑1 and σS 2 ∼ 3.00 × 10‑3 W m‑1 K‑2. The EPC projections on phonon dispersion and the phonon branch dependent scattering rates indicate that the acoustic phonons, especially the longitudinal acoustic phonons, dominate the carrier scattering. Therefore, a mobility of 68 cm2 V‑1 s‑1 is achieved if only the acoustic phonons induced scattering is included, in accordance with the result of 72 cm2 V‑1 s‑1 estimated from the deformation potential driven by acoustic modes. Furthermore, via excluding the scattering from the out-of-plane modes to simulate the EPC suppression, the obtained mobility of 258 cm2 V‑1 s‑1 is right in the range of 200–700 cm2 V‑1 s‑1 measured in the samples with top deposited dielectric layer. In addition, we also compute the lattice thermal conductivity κ L of monolayer MoS2 using phonon BTE, and obtain a κ L ∼ 123 W m‑1 K‑1 at 300 K.

Piezoelectric substrate effect on electron-acoustic phonon scattering in bilayer graphene

NASA Astrophysics Data System (ADS)

Ansari, Mohd Meenhaz; Ashraf, SSZ

2018-05-01

We have studied the effect of piezoelectric scattering as a function of electron temperature and distance between the sample and the substrate on electron-acoustic phonon scattering rate in Bilayer Graphene sitting on a piezoelectric substrate. We obtain approximate analytical result by neglecting the chiral nature of carriers and then proceed to obtain unapproximated numerical results for the scattering rate incorporating chirality of charge carriers. We find that on the incorporation of full numerical computation the magnitude as well as the power exponent both is affected with the power exponent changed from T3 to T3.31 in the low temperature range and to T6.98 dependence in the temperature range (>5K). We also find that the distance between the sample and substrate begins to strongly affect the scattering rate at temperatures above 10K. These calculation not only suggest the influencing effect of piezoelectric substrate on the transport properties of Dirac Fermions at very low temperatures but also open a channel to study low dimension structures by probing piezoelectric acoustical phonons.

Ultrahigh thermal conductivity of isotopically enriched silicon

NASA Astrophysics Data System (ADS)

Inyushkin, Alexander V.; Taldenkov, Alexander N.; Ager, Joel W.; Haller, Eugene E.; Riemann, Helge; Abrosimov, Nikolay V.; Pohl, Hans-Joachim; Becker, Peter

2018-03-01

Most of the stable elements have two and more stable isotopes. The physical properties of materials composed of such elements depend on the isotopic abundance to some extent. A remarkably strong isotope effect is observed in the phonon thermal conductivity, the principal mechanism of heat conduction in nonmetallic crystals. An isotopic disorder due to random distribution of the isotopes in the crystal lattice sites results in a rather strong phonon scattering and, consequently, in a reduction of thermal conductivity. In this paper, we present new results of accurate and precise measurements of thermal conductivity κ(T) for silicon single crystals having three different isotopic compositions at temperatures T from 2.4 to 420 K. The highly enriched crystal containing 99.995% of 28Si, which is one of the most perfect crystals ever synthesized, demonstrates a thermal conductivity of about 450 ± 10 W cm-1 K-1 at 24 K, the highest measured value among bulk dielectrics, which is ten times greater than the one for its counterpart natSi with the natural isotopic constitution. For highly enriched crystal 28Si and crystal natSi, the measurements were performed for two orientations [001] and [011], a magnitude of the phonon focusing effect on thermal conductivity was determined accurately at low temperatures. The anisotropy of thermal conductivity disappears above 31 K. The influence of the boundary scattering on thermal conductivity persists sizable up to much higher temperatures (˜80 K). The κ(T) measured in this work gives the most accurate approximation of the intrinsic thermal conductivity of single crystal silicon which is determined solely by the anharmonic phonon processes and diffusive boundary scattering over a wide temperature range.

Temperature dependence of the chromium(III) R1 linewidth in emerald

NASA Astrophysics Data System (ADS)

Carceller-Pastor, Ivana; Hutchison, Wayne D.; Riesen, Hans

2013-03-01

The temperature dependent contribution to the R1 (2E ← 4A2) linewidth in emerald, Be3Al2Si6O18:Cr3, has been measured by employing spectral hole-burning, fluorescence line narrowing and conventional luminescence experiments. The contribution varies from 0.6 MHz at 6.5 K to ˜420 GHz at 240 K and the line red-shifts by ˜570 GHz. Above 60 K, the dependence is well described by a non-perturbative formalism for two-phonon Raman scattering. Below this temperature the direct one-phonon process between the levels of the split 2E excited state dominates. However, it appears that a localized low-energy phonon leads to a deviation from the standard pattern at lowest temperatures.

Neutron and x-ray scattering study of phonon dispersion and diffuse scattering in (Na ,Bi ) Ti O3-x BaTi O3 single crystals near the morphotropic phase boundary

NASA Astrophysics Data System (ADS)

Luo, Chengtao; Bansal, Dipanshu; Li, Jiefang; Viehland, Dwight; Winn, Barry; Ren, Yang; Li, Xiaobing; Luo, Haosu; Delaire, Olivier

2017-11-01

Neutron and x-ray scattering measurements were performed on (N a1 /2B i1 /2 ) Ti O3-x at %BaTi O3 (NBT-x BT ) single crystals (x =4 , 5, 6.5, and 7.5) across the morphotropic phase boundary (MPB), as a function of both composition and temperature, and probing both structural and dynamical aspects. In addition to the known diffuse scattering pattern near the Γ points, our measurements revealed new, faint superlattice peaks, as well as an extensive diffuse scattering network, revealing a short-range ordering of polar nanoregions (PNR) with a static stacking morphology. In samples with compositions closest to the MPB, our inelastic neutron scattering investigations of the phonon dynamics showed two unusual features in the acoustic phonon branches, between the superlattice points, and between the superlattice points and Γ points, respectively. These critical elements are not present in the other compositions away from the MPB, which suggests that these features may be related to the tilt modes coupling behavior near the MPB.

Phonon thermal transport through tilt grain boundaries in strontium titanate

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

Zheng, Zexi; Chen, Xiang; Yang, Shengfeng

2014-08-21

In this work, we perform nonequilibrium molecular dynamics simulations to study phonon scattering at two tilt grain boundaries (GBs) in SrTiO{sub 3}. Mode-wise energy transmission coefficients are obtained based on phonon wave-packet dynamics simulations. The Kapitza conductance is then quantified using a lattice dynamics approach. The obtained results of the Kapitza conductance of both GBs compare well with those obtained by the direct method, except for the temperature dependence. Contrary to common belief, the results of this work show that the optical modes in SrTiO{sub 3} contribute significantly to phonon thermal transport, accounting for over 50% of the Kapitza conductance.more » To understand the effect of the GB structural disorder on phonon transport, we compare the local phonon density of states of the atoms in the GB region with that in the single crystalline grain region. Our results show that the excess vibrational modes introduced by the structural disorder do not have a significant effect on phonon scattering at the GBs, but the absence of certain modes in the GB region appears to be responsible for phonon reflections at GBs. This work has also demonstrated phonon mode conversion and simultaneous generation of new modes. Some of the new modes have the same frequency as the initial wave packet, while some have the same wave vector but lower frequencies.« less

Computational Study of In-Plane Phonon Transport in Si Thin Films

PubMed Central

Wang, Xinjiang; Huang, Baoling

2014-01-01

We have systematically investigated the in-plane thermal transport in Si thin films using an approach based on the first-principles calculations and lattice dynamics. The effects of phonon mode depletion induced by the phonon confinement and the corresponding variation in interphonon scattering, which may be important for the thermal conductivities of ultra-thin films but are often neglected in precedent studies, are considered in this study. The in-plane thermal conductivities of Si thin films with different thicknesses have been predicted over a temperature range from 80 K to 800 K and excellent agreements with experimental results are found. The validities of adopting the bulk phonon properties and gray approximation of surface specularity in thin film studies have been clarified. It is found that in ultra-thin films, while the phonon depletion will reduce the thermal conductivity of Si thin films, its effect is largely offset by the reduction in the interphonon scattering rate. The contributions of different phonon modes to the thermal transport and isotope effects in Si films with different thicknesses under various temperatures are also analyzed. PMID:25228061

Thermoelectrics. Dense dislocation arrays embedded in grain boundaries for high-performance bulk thermoelectrics.

PubMed

Kim, Sang Il; Lee, Kyu Hyoung; Mun, Hyeon A; Kim, Hyun Sik; Hwang, Sung Woo; Roh, Jong Wook; Yang, Dae Jin; Shin, Weon Ho; Li, Xiang Shu; Lee, Young Hee; Snyder, G Jeffrey; Kim, Sung Wng

2015-04-03

The widespread use of thermoelectric technology is constrained by a relatively low conversion efficiency of the bulk alloys, which is evaluated in terms of a dimensionless figure of merit (zT). The zT of bulk alloys can be improved by reducing lattice thermal conductivity through grain boundary and point-defect scattering, which target low- and high-frequency phonons. Dense dislocation arrays formed at low-energy grain boundaries by liquid-phase compaction in Bi(0.5)Sb(1.5)Te3 (bismuth antimony telluride) effectively scatter midfrequency phonons, leading to a substantially lower lattice thermal conductivity. Full-spectrum phonon scattering with minimal charge-carrier scattering dramatically improved the zT to 1.86 ± 0.15 at 320 kelvin (K). Further, a thermoelectric cooler confirmed the performance with a maximum temperature difference of 81 K, which is much higher than current commercial Peltier cooling devices. Copyright © 2015, American Association for the Advancement of Science.

Phonon spectroscopy with sub-meV resolution by femtosecond x-ray diffuse scattering

DOE PAGES

Zhu, Diling; Robert, Aymeric; Henighan, Tom; ...

2015-08-10

We present a reconstruction of the transverse acoustic phonon dispersion of germanium from femtosecond time-resolved x-ray diffuse scattering measurements at the Linac Coherent Light Source. We demonstrate an energy resolution of 0.3 meV with a momentum resolution of 0.01 nm -1 using 10-keV x rays with a bandwidth of ~ 1 eV. This high resolution was achieved simultaneously for a large section of reciprocal space including regions closely following three of the principal symmetry directions. The phonon dispersion was reconstructed with less than 3 h of measurement time, during which neither the x-ray energy, the sample orientation, nor the detectormore » position were scanned. In conclusion, these results demonstrate how time-domain measurements can complement conventional frequency domain inelastic-scattering techniques.« less

Temperature and frequency dependent mean free paths of renormalized phonons in nonlinear lattices

NASA Astrophysics Data System (ADS)

Li, Nianbei; Liu, Junjie; Wu, Changqin; Li, Baowen

2018-02-01

Unraveling general properties of renormalized phonons are of fundamental relevance to the heat transport in the regime of strong nonlinearity. In this work, we directly study the temperature and frequency dependent mean free path (MFP) of renormalized phonons with the newly developed numerical tuning fork method. The typical 1D nonlinear lattices such as Fermi-Pasta-Ulam β lattice and {φ }4 lattice are investigated in detail. Interestingly, it is found that the MFPs are inversely proportional to the frequencies of renormalized phonons rather than the square of phonon frequencies predicted by existing phonon scattering theory.

Kapitza resistance of Si/SiO2 interface

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

Bowen Deng; Aleksandr Chenatynskiy; Marat Khafizov

2014-02-01

A phonon wave packet dynamics method is used to characterize the Kapitza resistance of a Si/SiO2 interface in a Si/SiO2/Si heterostructure. By varying the thickness of SiO2 layer sandwiched between two Si layers, we determine the Kapitza resistance for the Si/SiO2 interface from both wave packet dynamics and a direct, non-equilibrium molecular dynamics approach. The good agreement between the two methods indicates that they have each captured the anharmonic phonon scatterings at the interface. Moreover, detailed analysis provides insights as to how individual phonon mode scatters at the interface and their contribution to the Kapitza resistance.

Anisotropic confinement effects in a two-dimensional plasma crystal.

PubMed

Laut, I; Zhdanov, S K; Räth, C; Thomas, H M; Morfill, G E

2016-01-01

The spectral asymmetry of the wave-energy distribution of dust particles during mode-coupling-induced melting, observed for the first time in plasma crystals by Couëdel et al. [Phys. Rev. E 89, 053108 (2014)PLEEE81539-375510.1103/PhysRevE.89.053108], is studied theoretically and by molecular-dynamics simulations. It is shown that an anisotropy of the well confining the microparticles selects the directions of preferred particle motion. The observed differences in intensity of waves of opposed directions are explained by a nonvanishing phonon flux. Anisotropic phonon scattering by defects and Umklapp scattering are proposed as possible reasons for the mean phonon flux.

Impact of metal gates on remote phonon scattering in titanium nitride/hafnium dioxide n-channel metal-oxide-semiconductor field effect transistors-low temperature electron mobility study

NASA Astrophysics Data System (ADS)

Maitra, Kingsuk; Frank, Martin M.; Narayanan, Vijay; Misra, Veena; Cartier, Eduard A.

2007-12-01

We report low temperature (40-300 K) electron mobility measurements on aggressively scaled [equivalent oxide thickness (EOT)=1 nm] n-channel metal-oxide-semiconductor field effect transistors (nMOSFETs) with HfO2 gate dielectrics and metal gate electrodes (TiN). A comparison is made with conventional nMOSFETs containing HfO2 with polycrystalline Si (poly-Si) gate electrodes. No substantial change in the temperature acceleration factor is observed when poly-Si is replaced with a metal gate, showing that soft optical phonons are not significantly screened by metal gates. A qualitative argument based on an analogy between remote phonon scattering and high-resolution electron energy-loss spectroscopy (HREELS) is provided to explain the underlying physics of the observed phenomenon. It is also shown that soft optical phonon scattering is strongly damped by thin SiO2 interface layers, such that room temperature electron mobility values at EOT=1 nm become competitive with values measured in nMOSFETs with SiON gate dielectrics used in current high performance processors.

Resonant inelastic light scattering and photoluminescence in isolated nc-Si/SiO{sub 2} quantum dots

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

Bairamov, F. B., E-mail: Bairamov@mail.ioffe.ru; Toporov, V. V.; Poloskin, E. D.

2013-05-15

Observation at the room temperature the spectra of the resonant inelastic light scattering by the spatially confined optical phonons as well as the excitonic luminescence caused by confinement effects in the ensemble of isolated quantum dots (QDs) nc-Si/SiO{sub 2} is reported. It is shown that the samples investigated are high purity and high crystalline perfection quality nc-Si/SiO{sub 2} QDs without amorphous phase {alpha}-Si and contaminants. Comparison between the experimental data obtained and phenomenological model of the strong space confinement of optical phonons revealed the need of the more accurate form of the weighted function for the confinement of optical phonons.more » It is shown that simultaneous detection of the inelastic light scattering by the confinement of phonons and the excitonic luminescence spectra by the confined electron-hole pairs in the nc-Si/SiO{sub 2} QDs allows selfconsistently to determine more accurate values of the diameter of the nc-Si/SiO{sub 2} QDs.« less

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.

Highly localized distributed Brillouin scattering response in a photonic integrated circuit

NASA Astrophysics Data System (ADS)

Zarifi, Atiyeh; Stiller, Birgit; Merklein, Moritz; Li, Neuton; Vu, Khu; Choi, Duk-Yong; Ma, Pan; Madden, Stephen J.; Eggleton, Benjamin J.

2018-03-01

The interaction of optical and acoustic waves via stimulated Brillouin scattering (SBS) has recently reached on-chip platforms, which has opened new fields of applications ranging from integrated microwave photonics and on-chip narrow-linewidth lasers, to phonon-based optical delay and signal processing schemes. Since SBS is an effect that scales exponentially with interaction length, on-chip implementation on a short length scale is challenging, requiring carefully designed waveguides with optimized opto-acoustic overlap. In this work, we use the principle of Brillouin optical correlation domain analysis to locally measure the SBS spectrum with high spatial resolution of 800 μm and perform a distributed measurement of the Brillouin spectrum along a spiral waveguide in a photonic integrated circuit. This approach gives access to local opto-acoustic properties of the waveguides, including the Brillouin frequency shift and linewidth, essential information for the further development of high quality photonic-phononic waveguides for SBS applications.

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

DOE PAGES

Selig, Malte; Berghäuser, Gunnar; Raja, Archana; ...

2016-11-07

Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. We investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS 2 and MoSe 2) through a study combining microscopic theory with spectroscopic measurements. We also show that the excitonicmore » coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. Particularly, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures, in WS 2.« less

Thermal conductivity of magnetic insulators with strong spin-orbit coupling

NASA Astrophysics Data System (ADS)

Stamokostas, Georgios; Lapas, Panteleimon; Fiete, Gregory A.

We study the influence of spin-orbit coupling on the thermal conductivity of various types of magnetic insulators. In the absence of spin-orbit coupling and orbital-degeneracy, the strong-coupling limit of Hubbard interactions at half filling can often be adequately described in terms of a pure spin Hamiltonian of the Heisenberg form. However, in the presence of spin-orbit coupling the resulting exchange interaction can become highly anisotropic. The effect of the atomic spin-orbit coupling, taken into account through the effect of magnon-phonon interactions and the magnetic order and excitations, on the lattice thermal conductivity of various insulating magnetic systems is studied. We focus on the regime of low temperatures where the dominant source of scattering is two-magnon scattering to one-phonon processes. The thermal current is calculated within the Boltzmann transport theory. We are grateful for financial support from NSF Grant DMR-0955778.

Thermal conductivity of magnetic insulators with strong spin-orbit coupling

NASA Astrophysics Data System (ADS)

Lapas, Panteleimon; Stamokostas, Georgios; Fiete, Gregory

2015-03-01

We study the influence of spin-orbit coupling on the thermal conductivity of various types of magnetic insulators. In the absence of spin-orbit coupling and orbital-degeneracy, the strong-coupling limit of Hubbard interactions at half filling can often be adequately described in terms of a pure spin Hamiltonian of the Heisenberg form. However, in the presence of spin-orbit coupling the resulting exchange interaction can become highly anisotropic. The effect of the atomic spin-orbit coupling, taken into account through the effect of magnon-phonon interactions and the magnetic order and excitations, on the lattice thermal conductivity of various insulating magnetic systems is studied. We focus on the regime of low temperatures where the dominant source of scattering is two-magnon scattering to one-phonon processes. The thermal current is calculated within the Boltzmann transport theory. We are grateful for financial support from NSF Grant DMR-0955778.

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.

Survey of background scattering from materials found in small-angle neutron scattering.

PubMed

Barker, J G; Mildner, D F R

2015-08-01

Measurements and calculations of beam attenuation and background scattering for common materials placed in a neutron beam are presented over the temperature range of 300-700 K. Time-of-flight (TOF) measurements have also been made, to determine the fraction of the background that is either inelastic or quasi-elastic scattering as measured with a 3 He detector. Other background sources considered include double Bragg diffraction from windows or samples, scattering from gases, and phonon scattering from solids. Background from the residual air in detector vacuum vessels and scattering from the 3 He detector dome are presented. The thickness dependence of the multiple scattering correction for forward scattering from water is calculated. Inelastic phonon background scattering at small angles for crystalline solids is both modeled and compared with measurements. Methods of maximizing the signal-to-noise ratio by material selection, choice of sample thickness and wavelength, removal of inelastic background by TOF or Be filters, and removal of spin-flip scattering with polarized beam analysis are discussed.

Survey of background scattering from materials found in small-angle neutron scattering

PubMed Central

Barker, J. G.; Mildner, D. F. R.

2015-01-01

Measurements and calculations of beam attenuation and background scattering for common materials placed in a neutron beam are presented over the temperature range of 300–700 K. Time-of-flight (TOF) measurements have also been made, to determine the fraction of the background that is either inelastic or quasi-elastic scattering as measured with a 3He detector. Other background sources considered include double Bragg diffraction from windows or samples, scattering from gases, and phonon scattering from solids. Background from the residual air in detector vacuum vessels and scattering from the 3He detector dome are presented. The thickness dependence of the multiple scattering correction for forward scattering from water is calculated. Inelastic phonon background scattering at small angles for crystalline solids is both modeled and compared with measurements. Methods of maximizing the signal-to-noise ratio by material selection, choice of sample thickness and wavelength, removal of inelastic background by TOF or Be filters, and removal of spin-flip scattering with polarized beam analysis are discussed. PMID:26306088

Effects of Electron Scattering at Metal-Nonmetal Interfaces on Electron-Phonon Equilibration in Gold Films

DTIC Science & Technology

2009-01-26

dielectrics is a major concern in thermal boundary conductance studies . This aspect of energy transfer has been extensively studied and modeled on long...electron-phonon coupling in the particle. There have been only a small number of studies looking at electron-phonon relaxation around interfaces in thin...film systems. These studies avoid complications due to nanopar- ticle geometries i.e., capillary modes on determining the electron-phonon-interfacial

On-chip magnetic cooling of a nanoelectronic device.

PubMed

Bradley, D I; Guénault, A M; Gunnarsson, D; Haley, R P; Holt, S; Jones, A T; Pashkin, Yu A; Penttilä, J; Prance, J R; Prunnila, M; Roschier, L

2017-04-04

We demonstrate significant cooling of electrons in a nanostructure below 10 mK by demagnetisation of thin-film copper on a silicon chip. Our approach overcomes the typical bottleneck of weak electron-phonon scattering by coupling the electrons directly to a bath of refrigerated nuclei, rather than cooling via phonons in the host lattice. Consequently, weak electron-phonon scattering becomes an advant- age. It allows the electrons to be cooled for an experimentally useful period of time to temperatures colder than the dilution refrigerator platform, the incoming electrical connections, and the host lattice. There are efforts worldwide to reach sub-millikelvin electron temperatures in nanostructures to study coherent electronic phenomena and improve the operation of nanoelectronic devices. On-chip magnetic cooling is a promising approach to meet this challenge. The method can be used to reach low, local electron temperatures in other nanostructures, obviating the need to adapt traditional, large demagnetisation stages. We demonstrate the technique by applying it to a nanoelectronic primary thermometer that measures its internal electron temperature. Using an optimised demagnetisation process, we demonstrate cooling of the on-chip electrons from 9 mK to below 5 mK for over 1000 seconds.

On-chip magnetic cooling of a nanoelectronic device

NASA Astrophysics Data System (ADS)

Bradley, D. I.; Guénault, A. M.; Gunnarsson, D.; Haley, R. P.; Holt, S.; Jones, A. T.; Pashkin, Yu. A.; Penttilä, J.; Prance, J. R.; Prunnila, M.; Roschier, L.

2017-04-01

We demonstrate significant cooling of electrons in a nanostructure below 10 mK by demagnetisation of thin-film copper on a silicon chip. Our approach overcomes the typical bottleneck of weak electron-phonon scattering by coupling the electrons directly to a bath of refrigerated nuclei, rather than cooling via phonons in the host lattice. Consequently, weak electron-phonon scattering becomes an advant- age. It allows the electrons to be cooled for an experimentally useful period of time to temperatures colder than the dilution refrigerator platform, the incoming electrical connections, and the host lattice. There are efforts worldwide to reach sub-millikelvin electron temperatures in nanostructures to study coherent electronic phenomena and improve the operation of nanoelectronic devices. On-chip magnetic cooling is a promising approach to meet this challenge. The method can be used to reach low, local electron temperatures in other nanostructures, obviating the need to adapt traditional, large demagnetisation stages. We demonstrate the technique by applying it to a nanoelectronic primary thermometer that measures its internal electron temperature. Using an optimised demagnetisation process, we demonstrate cooling of the on-chip electrons from 9 mK to below 5 mK for over 1000 seconds.

Intervalley double resonance processes in MoS2

NASA Astrophysics Data System (ADS)

Wang, Yuanxi; Carvalho, Bruno; Malard, Leandro; Fantini, Cristiano; Crespi, Vincent; Pimenta, Marcos

Intervalley scattering plays a significant role in electronic energy dissipation in semiconductors. We investigate the intervalley scattering of monolayer and few-layer MoS2, by combining density functional theory calculations and resonant Raman spectroscopy probed by up to 20 laser excitation energies. We observe that two Raman peaks within 420-460 cm-1 are dispersive over a small range of laser energy, a clear signature of second-order processes involving intervalley scattering. Both modes involve LA and TA phonons at or near the K point. A third Raman peak at 466 cm-1 shows a strong intensity dependence on the layer number and is assigned 2LA(M). Our results invalidate previous Raman peak assignment proposals and open up a better understanding of double resonance processes in transition metal dichalcogenides.

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.

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.

Spatial Distortion of Vibration Modes via Magnetic Correlation of Impurities

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

Krasniqi, Faton S.; Zhong, Yinpeng; Epp, S. W.

Long wavelength vibrational modes in the ferromagnetic semiconductor Ga 0.91M n0.09As are investigated using time resolved x-ray diffraction. At room temperature, we measure oscillations in the x-ray diffraction intensity corresponding to coherent vibrational modes with well-defined wavelengths. When the correlation of magnetic impurities sets in, we observe the transition of the lattice into a disordered state that does not support coherent modes at large wavelengths. Our measurements point toward a magnetically induced broadening of long wavelength vibrational modes in momentum space and their quasilocalization in the real space. More specifically, long wavelength vibrational modes cannot be assigned to a singlemore » wavelength but rather should be represented as a superposition of plane waves with different wavelengths. Lastly, our findings have strong implications for the phonon-related processes, especially carrier-phonon and phonon-phonon scattering, which govern the electrical conductivity and thermal management of semiconductor-based devices.« less

Spatial Distortion of Vibration Modes via Magnetic Correlation of Impurities

DOE PAGES

Krasniqi, Faton S.; Zhong, Yinpeng; Epp, S. W.; ...

2018-03-08

Long wavelength vibrational modes in the ferromagnetic semiconductor Ga 0.91M n0.09As are investigated using time resolved x-ray diffraction. At room temperature, we measure oscillations in the x-ray diffraction intensity corresponding to coherent vibrational modes with well-defined wavelengths. When the correlation of magnetic impurities sets in, we observe the transition of the lattice into a disordered state that does not support coherent modes at large wavelengths. Our measurements point toward a magnetically induced broadening of long wavelength vibrational modes in momentum space and their quasilocalization in the real space. More specifically, long wavelength vibrational modes cannot be assigned to a singlemore » wavelength but rather should be represented as a superposition of plane waves with different wavelengths. Lastly, our findings have strong implications for the phonon-related processes, especially carrier-phonon and phonon-phonon scattering, which govern the electrical conductivity and thermal management of semiconductor-based devices.« less

Electron-hole collision limited transport in charge-neutral bilayer graphene

NASA Astrophysics Data System (ADS)

Nam, Youngwoo; Ki, Dong-Keun; Soler-Delgado, David; Morpurgo, Alberto F.

2017-12-01

Ballistic transport occurs whenever electrons propagate without collisions deflecting their trajectory. It is normally observed in conductors with a negligible concentration of impurities, at low temperature, to avoid electron-phonon scattering. Here, we use suspended bilayer graphene devices to reveal a new regime, in which ballistic transport is not limited by scattering with phonons or impurities, but by electron-hole collisions. The phenomenon manifests itself in a negative four-terminal resistance that becomes visible when the density of holes (electrons) is suppressed by gate-shifting the Fermi level in the conduction (valence) band, above the thermal energy. For smaller densities, transport is diffusive, and the measured conductivity is reproduced quantitatively, with no fitting parameters, by including electron-hole scattering as the only process causing velocity relaxation. Experiments on a trilayer device show that the phenomenon is robust and that transport at charge neutrality is governed by the same physics. Our results provide a textbook illustration of a transport regime that had not been observed previously and clarify the nature of conduction through charge-neutral graphene under conditions in which carrier density inhomogeneity is immaterial. They also demonstrate that transport can be limited by a fully electronic mechanism, originating from the same microscopic processes that govern the physics of Dirac-like plasmas.

Excitons in Cuprous Oxide: Photoionization and Other Multiphoton Processes

NASA Astrophysics Data System (ADS)

Frazer, Nicholas Laszlo

In cuprous oxide (Cu2O), momentum from the absorption of two infrared photons to make an orthoexciton is conserved and detected through the photon component of a resulting mixed exciton/photon (quadrupole exciton polariton) state. I demonstrated that this process, which actually makes the photon momentum more precisely defined, is disrupted by photoionization of excitons. Some processes are known to affect exciton propagation in both the pump and exciton stages, such as phonon emission, exciton-exciton (Auger) scattering, and third harmonic generation. These processes alone were not able to explain all observed losses of excitons or all detected scattering products, which lead me to design an optical pump-probe experiment to measure the exciton photoionization cross section, which is (3.9+/-0.2) x 10-22 m2. This dissertation describes the synthesis of cuprous oxide crystals using oxidation of copper, crystallization from melt with the optical floating zone method, and annealing. The cuprous oxide crystals were characterized using time and space resolved luminescence, leading to the discovery of new defect properties. Selection rules and overall efficiency of third harmonic generation in these crystals were characterized. Exciton photoionization was demonstrated through the depletion of polariton luminescence by an optical probe, the production of phonon linked luminescence as a scattering product, temporal delay of the probe, and time resolved luminescence. The results are integrated with the traditional dynamical model of exciton densities. An additional investigation of copper/cuprous oxide/gold photovoltaic devices is appended.

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.

The p-wave superconductivity in the presence of Rashba interaction in 2DEG

PubMed Central

Weng, Ke-Chuan; Hu, C. D.

2016-01-01

We investigate the effect of the Rashba interaction on two dimensional superconductivity. The presence of the Rashba interaction lifts the spin degeneracy and gives rise to the spectrum of two bands. There are intraband and interband pairs scattering which result in the coupled gap equations. We find that there are isotropic and anisotropic components in the gap function. The latter has the form of cos φk where . The former is suppressed because the intraband and the interband scatterings nearly cancel each other. Hence, −the system should exhibit the p-wave superconductivity. We perform a detailed study of electron-phonon interaction for 2DEG and find that, if only normal processes are considered, the effective coupling strength constant of this new superconductivity is about one-half of the s-wave case in the ordinary 2DEG because of the angular average of the additional in the anisotropic gap function. By taking into account of Umklapp processes, we find they are the major contribution in the electron-phonon coupling in superconductivity and enhance the transition temperature Tc. PMID:27459677

Neutron and x-ray scattering study of phonon dispersion and diffuse scattering in ( Na , Bi ) Ti O 3 - x BaTi O 3 single crystals near the morphotropic phase boundary

DOE PAGES

Luo, Chengtao; Bansal, Dipanshu; Li, Jiefang; ...

2017-11-10

Neutron and x-ray scattering measurements were performed on (Na 1/2Bi 1/2)TiO 3-x at % BaTiO 3 (NBT-xBT) single crystals (x = 4, 5, 6.5, and 7.5) across the morphotropic phase boundary (MPB), as a function of both composition and temperature, and probing both structural and dynamical aspects. In addition to the known diffuse scattering pattern near the gamma points, our measurements revealed new, faint superlattice peaks, as well as an extensive diffuse scattering network, revealing a short-range ordering of polar nanoregions (PNR) with a static stacking morphology. Furthermore, in samples with compositions closest to the MPB, our inelastic neutron scatteringmore » investigations of the phonon dynamics showed two unusual features in the acoustic phonon branches, between the superlattice points, and between the superlattice points and gamma points, respectively. Finally, these critical elements are not present in the other compositions away from the MPB, which suggests that these features may be related to the tilt modes coupling behavior near the MPB.« less

Neutron and x-ray scattering study of phonon dispersion and diffuse scattering in ( Na , Bi ) Ti O 3 - x BaTi O 3 single crystals near the morphotropic phase boundary

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

Luo, Chengtao; Bansal, Dipanshu; Li, Jiefang

Neutron and x-ray scattering measurements were performed on (Na 1/2Bi 1/2)TiO 3-x at % BaTiO 3 (NBT-xBT) single crystals (x = 4, 5, 6.5, and 7.5) across the morphotropic phase boundary (MPB), as a function of both composition and temperature, and probing both structural and dynamical aspects. In addition to the known diffuse scattering pattern near the gamma points, our measurements revealed new, faint superlattice peaks, as well as an extensive diffuse scattering network, revealing a short-range ordering of polar nanoregions (PNR) with a static stacking morphology. Furthermore, in samples with compositions closest to the MPB, our inelastic neutron scatteringmore » investigations of the phonon dynamics showed two unusual features in the acoustic phonon branches, between the superlattice points, and between the superlattice points and gamma points, respectively. Finally, these critical elements are not present in the other compositions away from the MPB, which suggests that these features may be related to the tilt modes coupling behavior near the MPB.« less

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.

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.

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.

Spiral-Based Phononic Plates: From Wave Beaming to Topological Insulators

NASA Astrophysics Data System (ADS)

Foehr, André; Bilal, Osama R.; Huber, Sebastian D.; Daraio, Chiara

2018-05-01

Phononic crystals and metamaterials can sculpt elastic waves, controlling their dispersion using different mechanisms. These mechanisms are mostly Bragg scattering, local resonances, and inertial amplification, derived from ad hoc, often problem-specific geometries of the materials' building blocks. Here, we present a platform that ultilizes a lattice of spiraling unit cells to create phononic materials encompassing Bragg scattering, local resonances, and inertial amplification. We present two examples of phononic materials that can control waves with wavelengths much larger than the lattice's periodicity. (1) A wave beaming plate, which can beam waves at arbitrary angles, independent of the lattice vectors. We show that the beaming trajectory can be continuously tuned, by varying the driving frequency or the spirals' orientation. (2) A topological insulator plate, which derives its properties from a resonance-based Dirac cone below the Bragg limit of the structured lattice of spirals.

Electrical transport, electrothermal transport, and effective electron mass in single-crystalline In2O3 films

NASA Astrophysics Data System (ADS)

Preissler, Natalie; Bierwagen, Oliver; Ramu, Ashok T.; Speck, James S.

2013-08-01

A comprehensive study of the room-temperature electrical and electrothermal transport of single-crystalline indium oxide (In2O3) and indium tin oxide (ITO) films over a wide range of electron concentrations is reported. We measured the room-temperature Hall mobility μH and Seebeck coefficient S of unintentionally doped and Sn-doped high-quality, plasma-assisted molecular-beam-epitaxy-grown In2O3 for volume Hall electron concentrations nH from 7×1016 cm-3 (unintentionally doped) to 1×1021 cm-3 (highly Sn-doped, ITO). The resulting empirical S(nH) relation can be directly used in other In2O3 samples to estimate the volume electron concentration from simple Seebeck coefficient measurements. The mobility and Seebeck coefficient were modeled by a numerical solution of the Boltzmann transport equation. Ionized impurity scattering and polar optical phonon scattering were found to be the dominant scattering mechanisms. Acoustic phonon scattering was found to be negligible. Fitting the temperature-dependent mobility above room temperature of an In2O3 film with high mobility allowed us to find the effective Debye temperature (ΘD=700 K) and number of phonon modes (NOPML=1.33) that best describe the polar optical phonon scattering. The modeling also yielded the Hall scattering factor rH as a function of electron concentration, which is not negligible (rH≈1.4) at nondegenerate electron concentrations. Fitting the Hall-scattering-factor corrected concentration-dependent Seebeck coefficient S(n) for nondegenerate samples to the numerical solution of the Boltzmann transport equation and to widely used, simplified equations allowed us to extract an effective electron mass of m*=(0.30±0.03)me (with free electron mass me). The modeled mobility and Seebeck coefficient based on polar optical phonon and ionized impurity scattering describes the experimental results very accurately up to electron concentrations of 1019 cm-3, and qualitatively explains a mobility plateau or local maximum around 1020 cm-3. Ionized impurity scattering with doubly charged donors best describes the mobility in our unintentionally doped films, consistent with oxygen vacancies as unintentional shallow donors, whereas singly charged donors best describe our Sn-doped films. Our modeling yields a (phonon-limited) maximum theoretical drift mobility and Hall mobility of μ=190 cm2/Vs and μH=270 cm2/Vs, respectively. Simplified equations for the Seebeck coefficient describe the measured values in the nondegenerate regime using a Seebeck scattering parameter of r=-0.55 (which is consistent with the determined Debye temperature), and provide an estimate of the Seebeck coefficient to lower electron concentrations. The simplified equations fail to describe the Seebeck coefficient around the Mott transition (nMott=5.5×1018 cm-3) from nondegenerate to degenerate electron concentrations, whereas the numerical modeling accurately describes this region.

Terahertz quantum cascade lasers based on resonant phonon scattering for depopulation.

PubMed

Hu, Qing; Williams, Benjamin S; Kumar, Sushil; Callebaut, Hans; Reno, John L

2004-02-15

We report our development of terahertz (THz) quantum cascade lasers (QCLs), in which the depopulation of the lower radiative level is achieved through resonant longitudinal optical (LO) phonon scattering. This depopulation mechanism, similar to that implemented in all the QCLs operating at mid-infrared frequencies, is robust at high temperatures and high injection levels. The unique feature of resonant LO-phonon scattering in our THz QCL structures allows a highly selective depopulation of the lower radiative level with a sub-picosecond lifetime, while maintaining a relatively long upper level lifetime (more than 5 ps) that is due to upper-to-ground-state scattering. The first QCL based on this mechanism achieved lasing at 3.4 THz (lambda approximately 87 microm) up to 87 K for pulsed operations, with peak power levels exceeding 10 mW at ca. 40 K. Using a novel double-sided metal waveguide for mode confinement, which yields a unity mode confinement factor and therefore a low total cavity loss at THz frequencies, we have also achieved lasing at wavelengths longer than 100 microm.

Strong anharmonic phonon scattering induced giant reduction of thermal conductivity in PbTe nanotwin boundary

NASA Astrophysics Data System (ADS)

Zhou, Yanguang; Yang, Jia-Yue; Cheng, Long; Hu, Ming

2018-02-01

Lead telluride (PbTe) is a renowned thermoelectric material with high energy conversion efficiency in medium to high temperature range. However, the performance of PbTe at room temperature is poor due to its relatively high lattice thermal conductivity, which is difficult to be engineered due to its intrinsic very short phonon mean-free path. By performing systematic first-principles and molecular-dynamics simulations, we report that the room-temperature lattice thermal conductivity of PbTe can be reduced by almost one order of magnitude (86%) using the recent experimentally observed nanotwin structure. The mechanism responsible for the dramatic decrease of thermal conductivity strongly depends on the type and mass of atoms at the twin boundary. For PbTe nanotwinned structures with Te at the twin boundary, phonon transport is dominated by the phonon confinement effect and phonon-twin boundary scattering, and the thermal conductivity converges to the bulk value when half of the periodic length is larger than the dominant phonon mean-free path. The same phenomenon is found in another comparison system of KCl nanotwinned structures. However, when Pb is present at the twin boundary, a scattering mechanism occurs: anharmonicity induced by the twin boundary. Due to the mass difference between Pb and Te, the thermal resistance for Pb residing at the twin boundary is found to be one order of magnitude larger than the case with Te at the twin boundary, which results in much stronger phonon-twin boundary scattering. Consequently, the lowest thermal conductivity of such PbTe nanotwinned structure is only 0.4 W/mK, which is reduced by about sevenfold compared to the bulk value of 2.85 W/mK; finally, the converged thermal conductivity cannot restore the bulk value even when half of the periodic length is much larger than the dominant mean-free path. These results offer useful guidance for the development of PbTe-based thermoelectrics and also suggest that nanotwins are excellent building blocks for enhancing the performance of existing thermoelectrics.

Effects of counterion valency on the damping of phonons propagating along the axial direction of liquid-crystalline DNA

NASA Astrophysics Data System (ADS)

Liu, Yun; Chen, Sow-Hsin; Berti, Debora; Baglioni, Piero; Alatas, Ahmet; Sinn, Harald; Alp, Ercan; Said, Ayman

2005-12-01

The phonon propagation and damping along the axial direction of films of aligned 40wt% calf-thymus DNA rods are studied by inelastic x-ray scattering (IXS). The IXS spectra are analyzed with the generalized three effective eigenmode theory, from which we extract the dynamic structure factor S (Q,E) as a function of transferred energy E =ℏω, and the magnitude of the transferred wave vector Q. S (Q,E) of a DNA sample typically consists of three peaks, one central Rayleigh scattering peak, and two symmetric Stokes and anti-Stokes Brillouin side peaks. By analyzing the Brillouin peaks, the phonon excitation energy and damping can be extracted at different Q values from about 4 to 30nm-1. A high-frequency sound speed is obtained from the initial slope of the linear portion of the dispersion relation below Q =4nm-1. The high-frequency sound speed obtained in this Q range is 3100m /s, which is about twice faster than the ultrasound speed of 1800m/s, measured by Brillouin light scattering at Q ˜0.01nm-1 at the similar hydration level. Our observations provide further evidence of the strong coupling between the internal dynamics of a DNA molecule and the dynamics of the solvent. The effect on damping and propagation of phonons along the axial direction of DNA rods due to divalent and trivalent counterions has been studied. It is found that the added multivalent counterions introduce stronger phonon damping. The phonons at the range between ˜12.5 and ˜22.5nm-1 are overdamped by the added counterions according to our model analyses. The intermediate scattering function is extracted and it shows a clear two-step relaxation with the fast relaxation time ranging from 0.1 to 4ps.

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.

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.

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.

Electron and phonon transport in Co-doped FeV0.6Nb0.4Sb half-Heusler thermoelectric materials

NASA Astrophysics Data System (ADS)

Fu, Chenguang; Liu, Yintu; Xie, Hanhui; Liu, Xiaohua; Zhao, Xinbing; Jeffrey Snyder, G.; Xie, Jian; Zhu, Tiejun

2013-10-01

The electron and phonon transport characteristics of n-type Fe1-xCoxV0.6Nb0.4Sb half-Heusler thermoelectric compounds is analyzed. The acoustic phonon scattering is dominant in the carrier transport. The deformation potential of Edef = 14.1 eV and the density of state effective mass m* ≈ 2.0 me are derived under a single parabolic band assumption. The band gap is calculated to be ˜0.3 eV. Electron and phonon mean free paths are estimated based on the low and high temperature measurements. The electron mean free path is higher than the phonon one above room temperature, which is consistent with the experimental result that the electron mobility decreases more than the lattice thermal conductivity by grain refinement to enhance boundary scattering. A maximum ZT value of ˜0.33 is obtained at 650 K for x = 0.015, an increase by ˜60% compared with FeVSb. The optimal doping level is found to be ˜3.0 × 1020 cm-3 at 600 K.

Theory of electron-phonon-dislon interacting system—toward a quantized theory of dislocations

NASA Astrophysics Data System (ADS)

Li, Mingda; Tsurimaki, Yoichiro; Meng, Qingping; Andrejevic, Nina; Zhu, Yimei; Mahan, Gerald D.; Chen, Gang

2018-02-01

We provide a comprehensive theoretical framework to study how crystal dislocations influence the functional properties of materials, based on the idea of a quantized dislocation, namely a ‘dislon’. In contrast to previous work on dislons which focused on exotic phenomenology, here we focus on their theoretical structure and computational power. We first provide a pedagogical introduction that explains the necessity and benefits of taking the dislon approach and why the dislon Hamiltonian takes its current form. Then, we study the electron-dislocation and phonon-dislocation scattering problems using the dislon formalism. Both the effective electron and phonon theories are derived, from which the role of dislocations on electronic and phononic transport properties is computed. Compared with traditional dislocation scattering studies, which are intrinsically single-particle, low-order perturbation and classical quenched defect in nature, the dislon theory not only allows easy incorporation of quantum many-body effects such as electron correlation, electron-phonon interaction, and higher-order scattering events, but also allows proper consideration of the dislocation’s long-range strain field and dynamic aspects on equal footing for arbitrary types of straight-line dislocations. This means that instead of developing individual models for specific dislocation scattering problems, the dislon theory allows for the calculation of electronic structure and electrical transport, thermal transport, optical and superconducting properties, etc, under one unified theory. Furthermore, the dislon theory has another advantage over empirical models in that it requires no fitting parameters. The dislon theory could serve as a major computational tool to understand the role of dislocations on multiple materials’ functional properties at an unprecedented level of clarity, and may have wide applications in dislocated energy materials.

Phonon exchange by two-dimensional electrons in intermediate magnetic fields

NASA Astrophysics Data System (ADS)

Gopalakrishnan, Gokul

The discovery of the integer and fractional quantum Hall effects have broadened the exploration of the two-dimensional electron gas to regimes where complex and exciting physics lay previously hidden. While many experimental investigations have focused on the regime of large magnetic fields where transport properties are determined by contributions from a single Landau level, the regime of intermediate fields, where multiple Landau levels are involved, has been much less explored. This dissertation is a report on a previously unobserved interaction probed by a novel type of magneto-transport measurement performed in this intermediate regime, in bilayer two-dimensional electron systems. This measurement technique, known as electron drag, directly measures interlayer electron-electron scattering rates, by measuring the voltage induced in one of the layers when a current is driven through the other. The scattering mechanism, which may be Coulomb or phonon mediated, depends critically on both the separation between the layers and the electron density. When electron drag is measured in the presence of a perpendicular magnetic field in suitable samples, the resulting magnetodrag signal reveals new information about the electronic states as well as properties of a phonon mediated scattering mechanism. This phonon scattering mechanism is reflected in previously unobserved oscillations. These oscillations, which are periodic in the inverse field, are argued to arise from a resonant interlayer exchange of 2 kF phonons. Measurements of the temperature, density and layer-spacing dependences of magnetodrag resistivity are reported and are shown to confirm this particular mechanism. Additionally, analysis of the temperature dependence reveals a strong sensitivity to Landau level widths. Based on this analysis, a means of characterizing the broadening of Landau levels and hence, electronic lifetimes in this regime, which are otherwise difficult to characterize, is proposed.

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.

RAPID COMMUNICATION: Diffusion thermopower in graphene

NASA Astrophysics Data System (ADS)

Vaidya, R. G.; Kamatagi, M. D.; Sankeshwar, N. S.; Mulimani, B. G.

2010-09-01

The diffusion thermopower of graphene, Sd, is studied for 30 < T < 300 K, considering the electrons to be scattered by impurities, vacancies, surface roughness and acoustic and optical phonons via deformation potential couplings. Sd is found to increase almost linearly with temperature, determined mainly by vacancy and impurity scatterings. A departure from linear behaviour due to optical phonons is noticed. As a function of carrier concentration, a change in the sign of |Sd| is observed. Our analysis of recent thermopower data obtains a good fit. The limitations of Mott formula are discussed. Detailed analysis of data will enable a better understanding of the scattering mechanisms operative in graphene.

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.

Acoustic phonons in chrysotile asbestos probed by high-resolution inelastic x-ray scattering

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

Mamontov, Eugene; Vakhrushev, S. B.; Kumzerov, Yu. A,

Acoustic phonons in an individual, oriented fiber of chrysotile asbestos (chemical formula Mg{sub 3}Si{sub 2}O{sub 5}(OH){sub 4}) were observed at room temperature in the inelastic x-ray measurement with a very high (meV) resolution. The x-ray scattering vector was aligned along [1 0 0] direction of the reciprocal lattice, nearly parallel to the long axis of the fiber. The latter coincides with [1 0 0] direction of the direct lattice and the axes of the nano-channels. The data were analyzed using a damped harmonic oscillator model. Analysis of the phonon dispersion in the first Brillouin zone yielded the longitudinal sound velocitymore » of (9200 {+-} 600) m/s.« less

Hybridization and electron-phonon coupling in ferroelectric BaTiO3 probed by resonant inelastic x-ray scattering

NASA Astrophysics Data System (ADS)

Fatale, S.; Moser, S.; Miyawaki, J.; Harada, Y.; Grioni, M.

2016-11-01

We investigated the ferroelectric perovskite material BaTiO3 by resonant inelastic x-ray scattering (RIXS) at the Ti L3 edge. We observe with decreasing temperature a transfer of spectral weight from the elastic to the charge-transfer spectral features, indicative of increasing Ti 3 d -O 2 p hybridization. When the incident photon energy selects transitions to the Ti 3 d eg manifold, the quasielastic RIXS response exhibits a tail indicative of phonon excitations. A fit of the spectral line shape by a theoretical model allows us to estimate the electron-phonon coupling strength M ˜0.25 eV, which places BaTiO3 in the intermediate coupling regime.

Orbital angular momentum mode division filtering for photon-phonon coupling

PubMed Central

Zhu, Zhi-Han; Sheng, Li-Wen; Lv, Zhi-Wei; He, Wei-Ming; Gao, Wei

2017-01-01

Stimulated Brillouin scattering (SBS), a fundamental nonlinear interaction between light and acoustic waves occurring in any transparency material, has been broadly studied for several decades and gained rapid progress in integrated photonics recently. However, the SBS noise arising from the unwanted coupling between photons and spontaneous non-coherent phonons in media is inevitable. Here, we propose and experimentally demonstrate this obstacle can be overcome via a method called orbital angular momentum mode division filtering. Owing to the introduction of a new distinguishable degree-of-freedom, even extremely weak signals can be discriminated and separated from a strong noise produced in SBS processes. The mechanism demonstrated in this proof-of-principle work provides a practical way for quasi-noise-free photonic-phononic operation, which is still valid in waveguides supporting multi-orthogonal spatial modes, permits more flexibility and robustness for future SBS devices. PMID:28071736

Thermometry with Subnanometer Resolution in the Electron Microscope Using the Principle of Detailed Balancing.

PubMed

Lagos, Maureen J; Batson, Philip E

2018-06-13

We measure phonon energy gain and loss down to 20 meV in a single nanostructure using an atom-wide monochromatic electron beam. We show that the bulk and surface, energy loss and energy gain processes obey the principle of detailed balancing in nanostructured systems at thermal equilibrium. By plotting the logarithm of the ratio of the loss and gain bulk/surface scattering as a function of the excitation energy, we find a linear behavior, expected from detailed balance arguments. Since that universal linearity scales with the inverse of the nanosystem temperature only, we can measure the temperature of the probed object with precision down to about 1 K without reference to the nanomaterial. We also show that subnanometer spatial resolution (down to ∼2 Å) can be obtained using highly localized acoustic phonon scattering. The surface phonon polariton signal can also be used to measure the temperature near the nanostructure surfaces, but with unavoidable averaging over several nanometers. Comparison between transmission and aloof probe configurations suggests that our method exhibits noninvasive characteristics. Our work demonstrates the validity of the principle of detailed balancing within nanoscale materials at thermal equilibrium, and it describes a transparent method to measure nanoscale temperature, thus representing an advance in the development of a noninvasive method for measurements with angstrom resolution.

An Atomistic-Scale Study for Thermal Conductivity and Thermochemical Compatibility in (DyY)Zr2O7 Combining an Experimental Approach with Theoretical Calculation.

PubMed

Qu, Liu; Choy, Kwang-Leong; Wheatley, Richard

2016-02-18

Ceramic oxides that have high-temperature capabilities can be deposited on the superalloy components in aero engines and diesel engines to advance engine efficiency and reduce fuel consumption. This paper aims to study doping effects of Dy(3+) and Y(3+)on the thermodynamic properties of ZrO2 synthesized via a sol-gel route for a better control of the stoichiometry, combined with molecular dynamics (MD) simulation for the calculation of theoretical properties. The thermal conductivity is investigated by the MD simulation and Clarke's model. This can improve the understanding of the microstructure and thermodynamic properties of (DyY)Zr2O7 (DYZ) at the atomistic level. The phonon-defect scattering and phonon-phonon scattering processes are investigated via the theoretical calculation, which provides an effective way to study thermal transport properties of ionic oxides. The measured and predicted thermal conductivity of DYZ is lower than that of 4 mol % Y2O3 stabilized ZrO2 (4YSZ). It is discovered that DYZ is thermochemically compatible with Al2O3 at 1300 °C, whereas at 1350 °C DYZ reacts with Al2O3 forming a small amount of new phases.

An Atomistic-Scale Study for Thermal Conductivity and Thermochemical Compatibility in (DyY)Zr2O7 Combining an Experimental Approach with Theoretical Calculation

PubMed Central

Qu, Liu; Choy, Kwang-Leong; Wheatley, Richard

2016-01-01

Ceramic oxides that have high-temperature capabilities can be deposited on the superalloy components in aero engines and diesel engines to advance engine efficiency and reduce fuel consumption. This paper aims to study doping effects of Dy3+ and Y3+on the thermodynamic properties of ZrO2 synthesized via a sol-gel route for a better control of the stoichiometry, combined with molecular dynamics (MD) simulation for the calculation of theoretical properties. The thermal conductivity is investigated by the MD simulation and Clarke’s model. This can improve the understanding of the microstructure and thermodynamic properties of (DyY)Zr2O7 (DYZ) at the atomistic level. The phonon-defect scattering and phonon-phonon scattering processes are investigated via the theoretical calculation, which provides an effective way to study thermal transport properties of ionic oxides. The measured and predicted thermal conductivity of DYZ is lower than that of 4 mol % Y2O3 stabilized ZrO2 (4YSZ). It is discovered that DYZ is thermochemically compatible with Al2O3 at 1300 °C, whereas at 1350 °C DYZ reacts with Al2O3 forming a small amount of new phases. PMID:26888438

First-principles investigations on elastic, thermodynamic and lattice thermal conductivity of topological insulator LaAs

NASA Astrophysics Data System (ADS)

Zhou, Yu; Cheng, Yan; Chen, Xiang-Rong; Hu, Cui-E.; Chen, Qi-Feng

2018-07-01

Topological insulators are always a hot topic owing to their various peculiar physical effects, which are useful in spintronics and quantum information processing. Herein, we systematically investigate the elastic, thermodynamic and lattice thermal conductivity of a new typical topological insulator LaAs by combining the first-principles approach and an iterative solution of the Boltzmann transport equation. The obtained elastic constants and other lattice structural parameters of LaAs are well consistent with the experimental and other theoretical results. For the first time, the lattice thermal conductivity (5.46 W/(m•K)) and mean free path (14.4 nm) of LaAs are obtained, which manifests that the LaAs is more likely to be a desirable thermoelectric material. It is noted that the obtained mode-averaged Grüneisen parameters by different ab initio simulation packages are very similar, suggesting that our results are rather responsible. From the phonon scattering rates of LaAs, we speculate that the reduction of acoustic-optical gap and the larger phonon scattering may jointly result in reduction of thermal conductivity for LaAs. Meanwhile, the temperature dependence curves of the lattice thermal conductivity, heat capacity and phonon mean free path are also presented. We expect our work can provide more information for further experimental studies.

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.

Nonlinear optical response in narrow graphene nanoribbons

NASA Astrophysics Data System (ADS)

Karimi, Farhad; Knezevic, Irena

We present an iterative method to calculate the nonlinear optical response of armchair graphene nanoribbons (aGNRs) and zigzag graphene nanoribbons (zGNRs) while including the effects of dissipation. In contrast to methods that calculate the nonlinear response in the ballistic (dissipation-free) regime, here we obtain the nonlinear response of an electronic system to an external electromagnetic field while interacting with a dissipative environment (to second order). We use a self-consistent-field approach within a Markovian master-equation formalism (SCF-MMEF) coupled with full-wave electromagnetic equations, and we solve the master equation iteratively to obtain the higher-order response functions. We employ the SCF-MMEF to calculate the nonlinear conductance and susceptibility, as well as to calculate the dependence of the plasmon dispersion and plasmon propagation length on the intensity of the electromagnetic field in GNRs. The electron scattering mechanisms included in this work are scattering with intrinsic phonons, ionized impurities, surface optical phonons, and line-edge roughness. Unlike in wide GNRs, where ionized-impurity scattering dominates dissipation, in ultra-narrow nanoribbons on polar substrates optical-phonon scattering and ionized-impurity scattering are equally prominent. Support by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award DE-SC0008712.

The interpretation of polycrystalline coherent inelastic neutron scattering from aluminium

PubMed Central

Roach, Daniel L.; Ross, D. Keith; Gale, Julian D.; Taylor, Jon W.

2013-01-01

A new approach to the interpretation and analysis of coherent inelastic neutron scattering from polycrystals (poly-CINS) is presented. This article describes a simulation of the one-phonon coherent inelastic scattering from a lattice model of an arbitrary crystal system. The one-phonon component is characterized by sharp features, determined, for example, by boundaries of the (Q, ω) regions where one-phonon scattering is allowed. These features may be identified with the same features apparent in the measured total coherent inelastic cross section, the other components of which (multiphonon or multiple scattering) show no sharp features. The parameters of the model can then be relaxed to improve the fit between model and experiment. This method is of particular interest where no single crystals are available. To test the approach, the poly-CINS has been measured for polycrystalline aluminium using the MARI spectrometer (ISIS), because both lattice dynamical models and measured dispersion curves are available for this material. The models used include a simple Lennard-Jones model fitted to the elastic constants of this material plus a number of embedded atom method force fields. The agreement obtained suggests that the method demonstrated should be effective in developing models for other materials where single-crystal dispersion curves are not available. PMID:24282332

Light dark matter in superfluid helium: Detection with multi-excitation production

DOE PAGES

Knapen, Simon; Lin, Tongyan; Zurek, Kathryn M.

2017-03-22

We examine in depth a recent proposal to utilize superfluid helium for direct detection of sub-MeV mass dark matter. For sub-keV recoil energies, nuclear scattering events in liquid helium primarily deposit energy into long-lived phonon and roton quasiparticle excitations. If the energy thresholds of the detector can be reduced to the meV scale, then dark matter as light as ~MeV can be reached with ordinary nuclear recoils. If, on the other hand, two or more quasiparticle excitations are directly produced in the dark matter interaction, the kinematics of the scattering allows sensitivity to dark matter as light as ~keV atmore » the same energy resolution. We present in detail the theoretical framework for describing excitations in superfluid helium, using it to calculate the rate for the leading dark matter scattering interaction, where an off-shell phonon splits into two or more higher-momentum excitations. Here, we validate our analytic results against the measured and simulated dynamic response of superfluid helium. Finally, we apply this formalism to the case of a kinetically mixed hidden photon in the superfluid, both with and without an external electric field to catalyze the processes.« less

Near-Field Infrared Pump-Probe Imaging of Surface Phonon Coupling in Boron Nitride Nanotubes.

PubMed

Gilburd, Leonid; Xu, Xiaoji G; Bando, Yoshio; Golberg, Dmitri; Walker, Gilbert C

2016-01-21

Surface phonon modes are lattice vibrational modes of a solid surface. Two common surface modes, called longitudinal and transverse optical modes, exhibit lattice vibration along or perpendicular to the direction of the wave. We report a two-color, infrared pump-infrared probe technique based on scattering type near-field optical microscopy (s-SNOM) to spatially resolve coupling between surface phonon modes. Spatially varying couplings between the longitudinal optical and surface phonon polariton modes of boron nitride nanotubes are observed, and a simple model is proposed.

Vacancy-induced dislocations within grains for high-performance PbSe thermoelectrics

DOE PAGES

Chen, Zhiwei; Ge, Binghui; Li, Wen; ...

2017-01-04

To minimize the lattice thermal conductivity in thermoelectrics, strategies typically focus on the scattering of low-frequency phonons by interfaces and high-frequency phonons by point defects. In addition, scattering of mid-frequency phonons by dense dislocations, localized at the grain boundaries, has been shown to reduce the lattice thermal conductivity and improve the thermoelectric performance. Here we propose a vacancy engineering strategy to create dense dislocations in the grains. In Pb 1$-$xSb 2x/3Se solid solutions, cation vacancies are intentionally introduced, where after thermal annealing the vacancies can annihilate through a number of mechanisms creating the desired dislocations homogeneously distributed within the grains.more » This leads to a lattice thermal conductivity as low as 0.4Wm -1 K -1 and a high thermoelectric figure of merit, which can be explained by a dislocation scattering model. As a result, the vacancy engineering strategy used here should be equally applicable for solid solution thermoelectrics and provides a strategy for improving zT.« less

Reduction of thermal conductivity in phononic nanomesh structures.

PubMed

Yu, Jen-Kan; Mitrovic, Slobodan; Tham, Douglas; Varghese, Joseph; Heath, James R

2010-10-01

Controlling the thermal conductivity of a material independently of its electrical conductivity continues to be a goal for researchers working on thermoelectric materials for use in energy applications and in the cooling of integrated circuits. In principle, the thermal conductivity κ and the electrical conductivity σ may be independently optimized in semiconducting nanostructures because different length scales are associated with phonons (which carry heat) and electric charges (which carry current). Phonons are scattered at surfaces and interfaces, so κ generally decreases as the surface-to-volume ratio increases. In contrast, σ is less sensitive to a decrease in nanostructure size, although at sufficiently small sizes it will degrade through the scattering of charge carriers at interfaces. Here, we demonstrate an approach to independently controlling κ based on altering the phonon band structure of a semiconductor thin film through the formation of a phononic nanomesh film. These films are patterned with periodic spacings that are comparable to, or shorter than, the phonon mean free path. The nanomesh structure exhibits a substantially lower thermal conductivity than an equivalently prepared array of silicon nanowires, even though this array has a significantly higher surface-to-volume ratio. Bulk-like electrical conductivity is preserved. We suggest that this development is a step towards a coherent mechanism for lowering thermal conductivity.

Optimizing the thermoelectric performance of graphene nano-ribbons without degrading the electronic properties.

PubMed

Tran, Van-Truong; Saint-Martin, Jérôme; Dollfus, Philippe; Volz, Sebastian

2017-05-24

The enhancement of thermoelectric figure of merit ZT requires to either increase the power factor or reduce the phonon conductance, or even both. In graphene, the high phonon thermal conductivity is the main factor limiting the thermoelectric conversion. The common strategy to enhance ZT is therefore to introduce phonon scatterers to suppress the phonon conductance while retaining high electrical conductance and Seebeck coefficient. Although thermoelectric performance is eventually enhanced, all studies based on this strategy show a significant reduction of the electrical conductance. In this study we demonstrate that appropriate sources of disorder, including isotopes and vacancies at lowest electron density positions, can be used as phonon scatterers to reduce the phonon conductance in graphene ribbons without degrading the electrical conductance, particularly in the low-energy region which is the most important range for device operation. By means of atomistic calculations we show that the natural electronic properties of graphene ribbons can be fully preserved while their thermoelectric efficiency is strongly enhanced. For ribbons of width M = 5 dimer lines, room-temperature ZT is enhanced from less than 0.26 to more than 2.5. This study is likely to set the milestones of a new generation of nano-devices with dual electronic/thermoelectric functionalities.

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.

The conflicting role of buckled structure in phonon transport of 2D group-IV and group-V materials.

PubMed

Peng, Bo; Zhang, Dequan; Zhang, Hao; Shao, Hezhu; Ni, Gang; Zhu, Yongyuan; Zhu, Heyuan

2017-06-08

Controlling heat transport through material design is one important step toward thermal management in 2D materials. To control heat transport, a comprehensive understanding of how structure influences heat transport is required. It has been argued that a buckled structure is able to suppress heat transport by increasing the flexural phonon scattering. Using a first principles approach, we calculate the lattice thermal conductivity of 2D mono-elemental materials with a buckled structure. Somewhat counterintuitively, we find that although 2D group-V materials have a larger mass and higher buckling height than their group-IV counterparts, the calculated κ of blue phosphorene (106.6 W mK -1 ) is nearly four times higher than that of silicene (28.3 W mK -1 ), while arsenene (37.8 W mK -1 ) is more than fifteen times higher than germanene (2.4 W mK -1 ). We report for the first time that a buckled structure has three conflicting effects: (i) increasing the Debye temperature by increasing the overlap of the p z orbitals, (ii) suppressing the acoustic-optical scattering by forming an acoustic-optical gap, and (iii) increasing the flexural phonon scattering. The former two, corresponding to the harmonic phonon part, tend to enhance κ, while the last one, corresponding to the anharmonic part, suppresses it. This relationship between the buckled structure and phonon behaviour provides insight into how to control heat transport in 2D materials.

Heat-transport mechanisms in molecular building blocks of inorganic/organic hybrid superlattices

NASA Astrophysics Data System (ADS)

Giri, Ashutosh; Niemelä, Janne-Petteri; Tynell, Tommi; Gaskins, John T.; Donovan, Brian F.; Karppinen, Maarit; Hopkins, Patrick E.

2016-03-01

Nanomaterial interfaces and concomitant thermal resistances are generally considered as atomic-scale planes that scatter the fundamental energy carriers. Given that the nanoscale structural and chemical properties of solid interfaces can strongly influence this thermal boundary conductance, the ballistic and diffusive nature of phonon transport along with the corresponding phonon wavelengths can affect how energy is scattered and transmitted across an interfacial region between two materials. In hybrid composites composed of atomic layer building blocks of inorganic and organic constituents, the varying interaction between the phononic spectrum in the inorganic crystals and vibronic modes in the molecular films can provide a new avenue to manipulate the energy exchange between the fundamental vibrational energy carriers across interfaces. Here, we systematically study the heat transfer mechanisms in hybrid superlattices of atomic- and molecular-layer-grown zinc oxide and hydroquinone with varying thicknesses of the inorganic and organic layers in the superlattices. We demonstrate ballistic energy transfer of phonons in the zinc oxide that is limited by scattering at the zinc oxide/hydroquinone interface for superlattices with a single monolayer of hydroquinone separating the thicker inorganic layers. The concomitant thermal boundary conductance across the zinc oxide interfacial region approaches the maximal thermal boundary conductance of a zinc oxide phonon flux, indicative of the contribution of long wavelength vibrations across the aromatic molecular monolayers in transmitting energy across the interface. This transmission of energy across the molecular interface decreases considerably as the thickness of the organic layers are increased.

Thermal conductivity and phonon transport properties of silicon using perturbation theory and the environment-dependent interatomic potential

NASA Astrophysics Data System (ADS)

Pascual-Gutiérrez, José A.; Murthy, Jayathi Y.; Viskanta, Raymond

2009-09-01

Silicon thermal conductivities are obtained from the solution of the linearized phonon Boltzmann transport equation without the use of any parameter-fitting. Perturbation theory is used to compute the strength of three-phonon and isotope scattering mechanisms. Matrix elements based on Fermi's golden rule are computed exactly without assuming either average or mode-dependent Grüeisen parameters, and with no underlying assumptions of crystal isotropy. The environment-dependent interatomic potential is employed to describe the interatomic force constants and the perturbing Hamiltonians. A detailed methodology to accurately find three-phonon processes satisfying energy- and momentum-conservation rules is also described. Bulk silicon thermal conductivity values are computed across a range of temperatures and shown to match experimental data very well. It is found that about two-thirds of the heat transport in bulk silicon may be attributed to transverse acoustic modes. Effective relaxation times and mean free paths are computed in order to provide a more complete picture of the detailed transport mechanisms and for use with carrier transport models based on the Boltzmann transport equation.

Excited-state dynamics of size-dependent colloidal TiO2-Au nanocomposites

NASA Astrophysics Data System (ADS)

Karam, Tony E.; Khoury, Rami A.; Haber, Louis H.

2016-03-01

The ultrafast excited-state dynamics of size-dependent TiO2-Au nanocomposites synthesized by reducing gold nanoclusters to the surface of colloidal TiO2 nanoparticles are studied using pump-probe transient absorption spectroscopy with 400 nm excitation pulses. The results show that the relaxation processes of the plasmon depletion band, which are described by electron-phonon and phonon-phonon scattering lifetimes, are independent of the gold nanocluster shell size surrounding the TiO2 nanoparticle core. The dynamics corresponding to interfacial electron transfer between the gold nanoclusters and the TiO2 bandgap are observed to spectrally overlap with the gold interband transition signal, and the electron transfer lifetimes are shown to significantly decrease as the nanocluster shell size increases. Additionally, size-dependent periodic oscillations are observed and are attributed to acoustic phonons of a porous shell composed of aggregated gold nanoclusters around the TiO2 core, with frequencies that decrease and damping times that remain constant as the nanocluster shell size increases. These results are important for the development of improved catalytic nanomaterial applications.

Monoclinic β-BaY2F8—a novel crystal simultaneously active for SRS and Ln3+-ion lasing

NASA Astrophysics Data System (ADS)

Kaminskii, A. A.; Lux, O.; Hanuza, J.; Rhee, H.; Eichler, H. J.; Zhang, J.; Tang, D.; Shen, D.; Yu, H.; Wang, J.; Yoneda, H.; Shirakawa, A.

2015-01-01

This paper presents the first investigation of stimulated Raman scattering (SRS) in the monoclinic fluoride crystal β-BaY2F8, which is known as a promising host-material for trivalent lanthanide (Ln3+) lasant ions. Picosecond laser excitation in the visible and near-IR spectral range at room temperature revealed the manifestation of nine SRS-promoting phonon modes, which are related to Ag and Bg vibrations of the crystal. Besides multi-phonon Stokes and anti-Stokes generation, we observed cross-cascaded χ(3) ↔ χ(3) processes involving different pairs of SRS-active phonons. A comparative estimation of the first Stokes steady-state Raman gain coefficients, both in the visible and near-IR region related to the most active SRS-phonon mode ωSRS1 ≈ 208 cm-1 of β-BaY2F8, was also performed. Furthermore, a brief review of the pioneering papers on laser action of Ln3+-ions doped in β-BaY2F8 single crystals and other known SRS-active fluoride crystals is given in tabular form.

Photo-excited charge carriers suppress sub-terahertz phonon mode in silicon at room temperature

DOE PAGES

Liao, Bolin; Maznev, A. A.; Nelson, Keith A.; ...

2016-10-12

There is a growing interest in the mode-by-mode understanding of electron and phonon transport for improving energy conversion technologies, such as thermoelectrics and photovoltaics. Whereas remarkable progress has been made in probing phonon–phonon interactions, it has been a challenge to directly measure electron–phonon interactions at the single-mode level, especially their effect on phonon transport above cryogenic temperatures. Here in this paper, we use three-pulse photoacoustic spectroscopy to investigate the damping of a single sub-terahertz coherent phonon mode by free charge carriers in silicon at room temperature. Building on conventional pump–probe photoacoustic spectroscopy, we introduce an additional laser pulse to opticallymore » generate charge carriers, and carefully design temporal sequence of the three pulses to unambiguously quantify the scattering rate of a single-phonon mode due to the electron–phonon interaction. Our results confirm predictions from first-principles simulations and indicate the importance of the often-neglected effect of electron–phonon interaction on phonon transport in doped semiconductors.« less

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.

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 the impurity Cr^{4+} ions. Using rate equations to describe the electron -lattice system, the nonradiative relaxation time and the phonon lifetimes were estimated by fitting to the experimental data. The nonradiative relaxation time is estimated to be in the order of few ps while the phonon lifetimes are of the order of 10 ps. Best fit suggests the presence of an electronic bottleneck immediately after photoexcitation with an estimated lifetime of 3 ps at room temperature.

Reflection and extinction of light by self-assembled monolayers of a quinque-thiophene derivative: A coherent scattering approach

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

Gholamrezaie, Fatemeh; Meskers, Stefan C. J., E-mail: s.c.j.meskers@tue.nl; Leeuw, Dago M. de

Scattering matrix theory is used to describe resonant optical properties of molecular monolayers. Three types of coupling are included: exciton-exciton, exciton-photon, and exciton-phonon coupling. We use the K-matrix formalism, developed originally to describe neutron scattering spectra in nuclear physics to compute the scattering of polaritons by phonons. This perturbation approach takes into account the three couplings and allows one to go beyond molecular exciton theory without the need of introducing additional boundary conditions for the polariton. We demonstrate that reflection, absorption, and extinction of light by 2D self-assembled monolayers of molecules containing quinque-thiophene chromophoric groups can be calculated. The extractedmore » coherence length of the Frenkel exciton is discussed.« less

Evolution of the phonon density of states of LaCoO3 over the spin state transition

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

Golosova, N. O.; Kozlenko, D. P.; Kolesnikov, Alexander I

2011-01-01

The phonon spectra of LaCoO3 were studied by inelastic neutron scattering in the temperature range of 4 120 K. The DFT calculations of the lattice dynamics have been made for interpretation of the experimental data. The observed and calculated phonon frequencies were found to be in a reasonable agreement. The evolution of the phonon density of states over the spin state transition was analyzed. In the low-temperature range (T < 50 K), an increase in the energy of resolved breathing, stretching, and bending phonon modes was found, followed by their softening and broadening at higher temperatures due to the spinmore » state transition and relevant orbital-phonon coupling.« less

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

Kargar, Fariborz; Debnath, Bishwajit; Kakko, Joona -Pekko

Similar to electron waves, the phonon states in semiconductors can undergo changes induced by external boundaries. However, despite strong scientific and practical importance, conclusive experimental evidence of confined acoustic phonon polarization branches in individual free-standing nanostructures is lacking. Here we report results of Brillouin-Mandelstam light scattering spectroscopy, which reveal multiple (up to ten) confined acoustic phonon polarization branches in GaAs nanowires with a diameter as large as 128 nm, at a length scale that exceeds the grey phonon mean-free path in this material by almost an order-of-magnitude. The dispersion modification and energy scaling with diameter in individual nanowires are inmore » excellent agreement with theory. The phonon confinement effects result in a decrease in the phonon group velocity along the nanowire axis and changes in the phonon density of states. Furthermore, the obtained results can lead to more efficient nanoscale control of acoustic phonons, with benefits for nanoelectronic, thermoelectric and spintronic devices.« less

Soft phonon modes driven huge difference on lattice thermal conductivity between topological semimetal WC and WN

NASA Astrophysics Data System (ADS)

Guo, San-Dong; Chen, Peng

2018-04-01

Topological semimetals are currently attracting increasing interest due to their potential applications in topological qubits and low-power electronics, which are closely related to their thermal transport properties. Recently, the triply degenerate nodal points near the Fermi level of WC are observed by using angle-resolved photoemission spectroscopy. In this work, by solving the Boltzmann transport equation based on first-principles calculations, we systematically investigate the phonon transport properties of topological semimetals WC and WN. The predicted room-temperature lattice thermal conductivities of WC (WN) along the a and c directions are 1140.64 (7.47) W m-1 K-1 and 1214.69 (5.39) W m-1 K-1. Considering the similar crystal structure of WC and WN, it is quite interesting to find that the thermal conductivity of WC is more than two orders of magnitude higher than that of WN. It is found that, different from WN, the large acoustic-optical (a-o) gap prohibits the acoustic+acoustic → optical (aao) scattering, which gives rise to very long phonon lifetimes, leading to ultrahigh lattice thermal conductivity in WC. For WN, the lack of an a-o gap is due to soft phonon modes in optical branches, which can provide more scattering channels for aao scattering, producing very short phonon lifetimes. Further deep insight can be attained from their different electronic structures. Distinctly different from that in WC, the density of states of WN at the Fermi level becomes very sharp, which leads to destabilization of WN, producing soft phonon modes. It is found that the small shear modulus G and C44 limit the stability of WN, compared with WC. Our studies provide valuable information for phonon transports in WC and WN, and motivate further experimental studies to study their lattice thermal conductivities.

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

Trang Nghiêm, T. T.; Chapuis, Pierre-Olivier

The wave property of phonons is employed to explore the thermal transport across a finite periodic array of nano-scatterers such as circular and triangular holes. As thermal phonons are generated in all directions, we study their transmission through a single array for both normal and oblique incidences, using a linear dispersionless time-dependent acoustic frame in a two-dimensional system. Roughness effects can be directly considered within the computations without relying on approximate analytical formulae. Analysis by spatio-temporal Fourier transform allows us to observe the diffraction effects and the conversion of polarization. Frequency-dependent energy transmission coefficients are computed for symmetric and asymmetricmore » objects that are both subject to reciprocity. We demonstrate that the phononic array acts as an efficient thermal barrier by applying the theory of thermal boundary (Kapitza) resistances to arrays of smooth scattering holes in silicon for an exemplifying periodicity of 10 nm in the 5–100 K temperature range. It is observed that the associated thermal conductance has the same temperature dependence as that without phononic filtering.« less

Finite size effect on the magnetic excitations spectra, phonons and heat conduction of the quasi- one-dimensional spin chains system SrCuO2

NASA Astrophysics Data System (ADS)

Bounoua, Dalila; Saint-Martin, Romuald; Petit, Sylvain; Bourdarot, Frédéric; Pinsard-Gaudart, Loreynne

2018-05-01

We report inelastic neutron scattering measurements of the phonons modes, in the one-dimensional half integer spin chains cuprate SrCuO2. We study the longitudinal and the transverse modes propagating in the direction of the chains, along Q (0 0 L) and Q (2 0 L), respectively. On the other hand, we investigate the effect of substitution by impurities in the corresponding doped compounds, namely, SrCu0.99M0.01O2 with M=Mg or Zn, and La0.01Sr0.99CuO2. Our results evidence a systematic strong spinon-phonon interaction leading to an important decrease of the phonon scattered intensity as well as a decrease of the group velocity of the transverse acoustic modes upon substitution, and a shift of the transverse optical B3 u mode in the La-doped SrCuO2, in terms of energy.

Hot carrier dynamics in plasmonic transition metal nitrides

NASA Astrophysics Data System (ADS)

Habib, Adela; Florio, Fred; Sundararaman, Ravishankar

2018-06-01

Extraction of non-equilibrium hot carriers generated by plasmon decay in metallic nano-structures is an increasingly exciting prospect for utilizing plasmonic losses, but the search for optimum plasmonic materials with long-lived carriers is ongoing. Transition metal nitrides are an exciting class of new plasmonic materials with superior thermal and mechanical properties compared to conventional noble metals, but their suitability for plasmonic hot carrier applications remains unknown. Here, we present fully first principles calculations of the plasmonic response, hot carrier generation and subsequent thermalization of all group IV, V and VI transition metal nitrides, fully accounting for direct and phonon-assisted transitions as well as electron–electron and electron–phonon scattering. We find the largest frequency ranges for plasmonic response in ZrN, HfN and WN, between those of gold and silver, while we predict strongest absorption in the visible spectrum for the VN, NbN and TaN. Hot carrier generation is dominated by direct transitions for most of the relevant energy range in all these nitrides, while phonon-assisted processes dominate only below 1 eV plasmon energies primarily for the group IV nitrides. Finally, we predict the maximum hot carrier lifetimes to be around 10 fs for group IV and VI nitrides, a factor of 3–4 smaller than noble metals, due to strong electron–phonon scattering. However, we find longer carrier lifetimes for group V nitrides, comparable to silver for NbN and TaN, while exceeding 100 fs (twice that of silver) for VN, making them promising candidates for efficient hot carrier extraction.

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

Lattice thermal transport in L a 3 C u 3 X 4 compounds ( X = P , As , Sb , Bi ) : Interplay of anharmonicity and scattering phase space

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

None, None

Thermal conductivities of La 3Cu 3X 4(X=P,As,Sb,Bi) compounds are examined using first-principles density functional theory and Boltzmann transport methods. We observe a trend of increasing lattice thermal conductivity (κl) with increasing atomic mass, challenging our expectations, as lighter mass systems typically have larger sound speeds and weaker intrinsic scattering. In particular, we find that La 3Cu 3P 4 has the lowest κ l, despite having larger sound speed and the most restricted available phase space for phonon-phonon scattering, an important criterion for estimating and comparing κ l among like systems. The origin of this unusual behavior lies in the strengthmore » of the individual anharmonic phonon scattering matrix elements, which are much larger in La 3Cu 3P 4 than in the heavier La 3Cu 3Bi 4 system. Lastly, our finding provides insights into the interplay of harmonic and anharmonic properties of complex, low-thermal-conductivity compounds, of potential use for thermoelectric and thermal barrier coating applications.« less

Lattice thermal transport in L a 3 C u 3 X 4 compounds ( X = P , As , Sb , Bi ) : Interplay of anharmonicity and scattering phase space

DOE PAGES

None, None

2017-06-30

Thermal conductivities of La 3Cu 3X 4(X=P,As,Sb,Bi) compounds are examined using first-principles density functional theory and Boltzmann transport methods. We observe a trend of increasing lattice thermal conductivity (κl) with increasing atomic mass, challenging our expectations, as lighter mass systems typically have larger sound speeds and weaker intrinsic scattering. In particular, we find that La 3Cu 3P 4 has the lowest κ l, despite having larger sound speed and the most restricted available phase space for phonon-phonon scattering, an important criterion for estimating and comparing κ l among like systems. The origin of this unusual behavior lies in the strengthmore » of the individual anharmonic phonon scattering matrix elements, which are much larger in La 3Cu 3P 4 than in the heavier La 3Cu 3Bi 4 system. Lastly, our finding provides insights into the interplay of harmonic and anharmonic properties of complex, low-thermal-conductivity compounds, of potential use for thermoelectric and thermal barrier coating applications.« less

Lattice thermal transport in L a3C u3X4 compounds (X =P ,As ,Sb ,Bi ) : Interplay of anharmonicity and scattering phase space

NASA Astrophysics Data System (ADS)

Pandey, Tribhuwan; Polanco, Carlos A.; Lindsay, Lucas; Parker, David S.

2017-06-01

Thermal conductivities of L a3C u3X4 (X =P ,As ,Sb ,Bi ) compounds are examined using first-principles density functional theory and Boltzmann transport methods. We observe a trend of increasing lattice thermal conductivity (κl) with increasing atomic mass, challenging our expectations, as lighter mass systems typically have larger sound speeds and weaker intrinsic scattering. In particular, we find that L a3C u3P4 has the lowest κl, despite having larger sound speed and the most restricted available phase space for phonon-phonon scattering, an important criterion for estimating and comparing κl among like systems. The origin of this unusual behavior lies in the strength of the individual anharmonic phonon scattering matrix elements, which are much larger in L a3C u3P4 than in the heavier L a3C u3B i4 system. Our finding provides insights into the interplay of harmonic and anharmonic properties of complex, low-thermal-conductivity compounds, of potential use for thermoelectric and thermal barrier coating applications.

High mobility In0.75Ga0.25As quantum wells in an InAs phonon lattice

NASA Astrophysics Data System (ADS)

Chen, C.; Holmes, S. N.; Farrer, I.; Beere, H. E.; Ritchie, D. A.

2018-03-01

InGaAs based devices are great complements to silicon for CMOS, as they provide an increased carrier saturation velocity, lower operating voltage and reduced power dissipation (International technology roadmap for semiconductors (www.itrs2.net)). In this work we show that In0.75Ga0.25As quantum wells with a high mobility, 15 000 to 20 000 cm2 V-1 s-1 at ambient temperature, show an InAs-like phonon with an energy of 28.8 meV, frequency of 232 cm-1 that dominates the polar-optical mode scattering from  ˜70 K to 300 K. The measured optical phonon frequency is insensitive to the carrier density modulated with a surface gate or LED illumination. We model the electron scattering mechanisms as a function of temperature and identify mechanisms that limit the electron mobility in In0.75Ga0.25As quantum wells. Background impurity scattering starts to dominate for temperatures  <100 K. In the high mobility In0.75Ga0.25As quantum well, GaAs-like phonons do not couple to the electron gas unlike the case of In0.53Ga0.47As quantum wells.

Giant suppression of phononic heat transport in a quantum magnet BiCu2PO6

NASA Astrophysics Data System (ADS)

Jeon, Byung-Gu; Koteswararao, B.; Park, C. B.; Shu, G. J.; Riggs, S. C.; Moon, E. G.; Chung, S. B.; Chou, F. C.; Kim, Kee Hoon

2016-11-01

Thermal transport of quantum magnets has elucidated the nature of low energy elementary excitations and complex interplay between those excited states via strong scattering of thermal carriers. BiCu2PO6 is a unique frustrated spin-ladder compound exhibiting highly anisotropic spin excitations that contain both itinerant and localized dispersion characters along the b- and a-axes respectively. Here, we investigate thermal conductivity κ of BiCu2PO6 under high magnetic fields (H) of up to 30 tesla. A dip-feature in κ, located at ~15 K at zero-H along all crystallographic directions, moves gradually toward lower temperature (T) with increasing H, thus resulting in giant suppression by a factor of ~30 near the critical magnetic field of Hc ≅ 23.5 tesla. The giant H- and T-dependent suppression of κ can be explained by the combined result of resonant scattering of phononic heat carriers with magnetic energy levels and increased phonon scattering due to enhanced spin fluctuation at Hc, unequivocally revealing the existence of strong spin-phonon coupling. Moreover, we find an experimental indication that the remaining magnetic heat transport along the b-axis becomes almost gapless at the magnetic quantum critical point realized at Hc.

Giant suppression of phononic heat transport in a quantum magnet BiCu2PO6.

PubMed

Jeon, Byung-Gu; Koteswararao, B; Park, C B; Shu, G J; Riggs, S C; Moon, E G; Chung, S B; Chou, F C; Kim, Kee Hoon

2016-11-15

Thermal transport of quantum magnets has elucidated the nature of low energy elementary excitations and complex interplay between those excited states via strong scattering of thermal carriers. BiCu 2 PO 6 is a unique frustrated spin-ladder compound exhibiting highly anisotropic spin excitations that contain both itinerant and localized dispersion characters along the b- and a-axes respectively. Here, we investigate thermal conductivity κ of BiCu 2 PO 6 under high magnetic fields (H) of up to 30 tesla. A dip-feature in κ, located at ~15 K at zero-H along all crystallographic directions, moves gradually toward lower temperature (T) with increasing H, thus resulting in giant suppression by a factor of ~30 near the critical magnetic field of H c  ≅ 23.5 tesla. The giant H- and T-dependent suppression of κ can be explained by the combined result of resonant scattering of phononic heat carriers with magnetic energy levels and increased phonon scattering due to enhanced spin fluctuation at H c , unequivocally revealing the existence of strong spin-phonon coupling. Moreover, we find an experimental indication that the remaining magnetic heat transport along the b-axis becomes almost gapless at the magnetic quantum critical point realized at H c .

Fundamental limits on the electron mobility of β-Ga2O3

NASA Astrophysics Data System (ADS)

Kang, Youngho; Krishnaswamy, Karthik; Peelaers, Hartwin; Van de Walle, Chris G.

2017-06-01

We perform first-principles calculations to investigate the electronic and vibrational spectra and the electron mobility of β-Ga2O3. We calculate the electron-phonon scattering rate of the polar optical phonon modes using the Vogl model in conjunction with Fermi’s golden rule; this enables us to fully take the anisotropic phonon spectra of the monoclinic lattice of β-Ga2O3 into account. We also examine the scattering rate due to ionized impurities or defects using a Yukawa-potential-based model. We consider scattering due to donor impurities, as well as the possibility of compensation by acceptors such as Ga vacancies. We then calculate the room-temperature mobility of β-Ga2O3 using the Boltzmann transport equation within the relaxation time approximation, for carrier densities in the range from 1017 to 1020 cm-3. We find that the electron-phonon interaction dominates the mobility for carrier densities of up to 1019 cm-3. We also find that the intrinsic anisotropy in the mobility is small; experimental findings of large anisotropy must therefore be attributed to other factors. We attribute the experimentally observed reduction of the mobility with increasing carrier density to increasing levels of compensation, which significantly affect the mobility.

Fundamental limits on the electron mobility of β-Ga2O3.

PubMed

Kang, Youngho; Krishnaswamy, Karthik; Peelaers, Hartwin; Van de Walle, Chris G

2017-06-14

We perform first-principles calculations to investigate the electronic and vibrational spectra and the electron mobility of β-Ga 2 O 3 . We calculate the electron-phonon scattering rate of the polar optical phonon modes using the Vogl model in conjunction with Fermi's golden rule; this enables us to fully take the anisotropic phonon spectra of the monoclinic lattice of β-Ga 2 O 3 into account. We also examine the scattering rate due to ionized impurities or defects using a Yukawa-potential-based model. We consider scattering due to donor impurities, as well as the possibility of compensation by acceptors such as Ga vacancies. We then calculate the room-temperature mobility of β-Ga 2 O 3 using the Boltzmann transport equation within the relaxation time approximation, for carrier densities in the range from 10 17 to 10 20 cm -3 . We find that the electron-phonon interaction dominates the mobility for carrier densities of up to 10 19 cm -3 . We also find that the intrinsic anisotropy in the mobility is small; experimental findings of large anisotropy must therefore be attributed to other factors. We attribute the experimentally observed reduction of the mobility with increasing carrier density to increasing levels of compensation, which significantly affect the mobility.

Giant suppression of phononic heat transport in a quantum magnet BiCu2PO6

PubMed Central

Jeon, Byung-Gu; Koteswararao, B.; Park, C. B.; Shu, G. J.; Riggs, S. C.; Moon, E. G.; Chung, S. B.; Chou, F. C.; Kim, Kee Hoon

2016-01-01

Thermal transport of quantum magnets has elucidated the nature of low energy elementary excitations and complex interplay between those excited states via strong scattering of thermal carriers. BiCu2PO6 is a unique frustrated spin-ladder compound exhibiting highly anisotropic spin excitations that contain both itinerant and localized dispersion characters along the b- and a-axes respectively. Here, we investigate thermal conductivity κ of BiCu2PO6 under high magnetic fields (H) of up to 30 tesla. A dip-feature in κ, located at ~15 K at zero-H along all crystallographic directions, moves gradually toward lower temperature (T) with increasing H, thus resulting in giant suppression by a factor of ~30 near the critical magnetic field of Hc ≅ 23.5 tesla. The giant H- and T-dependent suppression of κ can be explained by the combined result of resonant scattering of phononic heat carriers with magnetic energy levels and increased phonon scattering due to enhanced spin fluctuation at Hc, unequivocally revealing the existence of strong spin-phonon coupling. Moreover, we find an experimental indication that the remaining magnetic heat transport along the b-axis becomes almost gapless at the magnetic quantum critical point realized at Hc. PMID:27845377

Giant suppression of phononic heat transport in a quantum magnet BiCu 2PO 6

DOE PAGES

Jeon, Byung-Gu; Koteswararao, B.; Park, C. B.; ...

2016-11-15

Thermal transport of quantum magnets has elucidated the nature of low energy elementary excitations and complex interplay between those excited states via strong scattering of thermal carriers. BiCu 2PO 6 is a unique frustrated spin-ladder compound exhibiting highly anisotropic spin excitations that contain both itinerant and localized dispersion characters along the b- and a-axes respectively. Here, we investigate thermal conductivity κ of BiCu 2PO 6 under high magnetic fields (H) of up to 30 tesla. A dip-feature in κ, located at ~15K at zero-H along all crystallographic directions, moves gradually toward lower temperature (T) with increasing H, thus resulting inmore » giant suppression by a factor of ~30 near the critical magnetic field of H c≅23.5 tesla. The giant H- and T-dependent suppression of κ can be explained by the combined result of resonant scattering of phononic heat carriers with magnetic energy levels and increased phonon scattering due to enhanced spin fluctuation at H c, unequivocally revealing the existence of strong spin-phonon coupling. Moreover, we find an experimental indication that the remaining magnetic heat transport along the b-axis becomes almost gapless at the magnetic quantum critical point realized at H c.« less

Resonant inelastic x-ray scattering probes the electron-phonon coupling in the spin liquid κ -(BEDT-TTF)2Cu2(CN) 3

NASA Astrophysics Data System (ADS)

Ilakovac, V.; Carniato, S.; Foury-Leylekian, P.; Tomić, S.; Pouget, J.-P.; Lazić, P.; Joly, Y.; Miyagawa, K.; Kanoda, K.; Nicolaou, A.

2017-11-01

Resonant inelastic x-ray scattering at the N K edge reveals clearly resolved harmonics of the anion plane vibrations in the κ -(BEDT-TTF) 2Cu2 (CN) 3 spin-liquid insulator. Tuning the incoming light energy at the K edge of two distinct N sites permits us to excite different sets of phonon modes. The cyanide (CN) stretching mode is selected at the edge of the ordered N sites which are more strongly connected to the bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF) molecules, while positionally disordered N sites show multimode excitation. Combining measurements with calculations on an anion plane cluster permits us to estimate the site-dependent electron-phonon coupling of the modes related to nitrogen excitation.

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.

Acoustic phonon spectrum and thermal transport in nanoporous alumina arrays

DOE PAGES

Kargar, Fariborz; Ramirez, Sylvester; Debnath, Bishwajit; ...

2015-10-28

We report results of a combined investigation of thermal conductivity and acoustic phonon spectra in nanoporous alumina membranes with the pore diameter decreasing from D=180 nm to 25 nm. The samples with the hexagonally arranged pores were selected to have the same porosity Ø ≈13%. The Brillouin-Mandelstam spectroscopy measurements revealed bulk-like phonon spectrum in the samples with D = 180 nm pores and spectral features, which were attributed to spatial confinement, in the samples with 25 nm and 40 nm pores. The velocity of the longitudinal acoustic phonons was reduced in the samples with smaller pores. As a result, analysismore » of the experimental data and calculated phonon dispersion suggests that both phonon-boundary scattering and phonon spatial confinement affect heat conduction in membranes with the feature sizes D < 40 nm.« less

Effect of electron-electron scattering on the conductance of a quantum wire studied with the Boltzman transport equation

NASA Astrophysics Data System (ADS)

Lyo, S. K.; Huang, Danhong

2006-05-01

Electron-electron scattering conserves total momentum and does not dissipate momentum directly in a low-density system where the umklapp process is forbidden. However, it can still affect the conductance through the energy relaxation of the electrons. We show here that this effect can be studied with arbitrary accuracy in a multisublevel one-dimensional (1D) single quantum wire system in the presence of roughness and phonon scattering using a formally exact solution of the Boltzmann transport equation. The intrasubband electron-electron scattering is found to yield no net effect on the transport of electrons in 1D with only one sublevel occupied. For a system with a multilevel occupation, however, we find a significant effect of intersublevel electron-electron scattering on the temperature and density dependence of the resistance at low temperatures.

Answer to Question {number_sign}30 [{open_quote}{open_quote}How are positrons moderated?,{close_quote}{close_quote} Thomas D. Rossing, Am. J. Phys. {bold 63}(12), 1065 (1995)

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

Weber, M.; Lynn, K.G.

1996-07-01

The positrons from {beta}{sup +} decaying sources loss energyat a much faster rate than they annihilate. As the energy of the positrons drops, core excitations, plasmon excitation, electron/hole pair creation, and phonon scattering are the dominant processes of further energy loss.

Theoretical treatment of the processes involving the dipole transitions to the lowest exciton states in hexagonal semiconductors

NASA Astrophysics Data System (ADS)

Semenova, L. E.

2018-04-01

The treatment of the two-photon transitions to the An=1 exciton level and the resonant Raman scattering of light by LO-phonons is given for the hexagonal semiconductors A2B6, taking into account the influence of the complex top valence band and anisotropy of the exciton effective mass.

Effects of lithium insertion on thermal conductivity of silicon nanowires

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

Xu, Wen; Institute of High Performance Computing, A*STAR, Singapore, Singapore 138632; Zhang, Gang, E-mail: zhangg@ihpc.a-star.edu.sg

2015-04-27

Recently, silicon nanowires (SiNWs) have been applied as high-performance Li battery anodes, since they can overcome the pulverization and mechanical fracture during lithiation. Although thermal stability is one of the most important parameters that determine safety of Li batteries, thermal conductivity of SiNWs with Li insertion remains unclear. In this letter, using molecular dynamics simulations, we study room temperature thermal conductivity of SiNWs with Li insertion. It is found that compared with the pristine SiNW, there is as much as 60% reduction in thermal conductivity with 10% concentration of inserted Li atoms, while under the same impurity concentration the reductionmore » in thermal conductivity of the mass-disordered SiNW is only 30%. With lattice dynamics calculations and normal mode decomposition, it is revealed that the phonon lifetimes in SiNWs decrease greatly due to strong scattering of phonons by vibrational modes of Li atoms, especially for those high frequency phonons. The observed strong phonon scattering phenomenon in Li-inserted SiNWs is similar to the phonon rattling effect. Our study serves as an exploration of thermal properties of SiNWs as Li battery anodes or weakly coupled with impurity atoms.« less

Development of interatomic potential of Ge(1- x - y )Si x Sn y ternary alloy semiconductors for classical lattice dynamics simulation

NASA Astrophysics Data System (ADS)

Tomita, Motohiro; Ogasawara, Masataka; Terada, Takuya; Watanabe, Takanobu

2018-04-01

We provide the parameters of Stillinger-Weber potentials for GeSiSn ternary mixed systems. These parameters can be used in molecular dynamics (MD) simulations to reproduce phonon properties and thermal conductivities. The phonon dispersion relation is derived from the dynamical structure factor, which is calculated by the space-time Fourier transform of atomic trajectories in an MD simulation. The phonon properties and thermal conductivities of GeSiSn ternary crystals calculated using these parameters mostly reproduced both the findings of previous experiments and earlier calculations made using MD simulations. The atomic composition dependence of these properties in GeSiSn ternary crystals obtained by previous studies (both experimental and theoretical) and the calculated data were almost exactly reproduced by our proposed parameters. Moreover, the results of the MD simulation agree with the previous calculations made using a time-independent phonon Boltzmann transport equation with complicated scattering mechanisms. These scattering mechanisms are very important in complicated nanostructures, as they allow the heat-transfer properties to be more accurately calculated by MD simulations. This work enables us to predict the phonon- and heat-related properties of bulk group IV alloys, especially ternary alloys.

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.

Phonon Surface Scattering and Thermal Energy Distribution in Superlattices.

PubMed

Kothari, Kartik; Maldovan, Martin

2017-07-17

Thermal transport at small length scales has attracted significant attention in recent years and various experimental and theoretical methods have been developed to establish the reduced thermal conductivity. The fundamental understanding of how phonons move and the physical mechanisms behind nanoscale thermal transport, however, remains poorly understood. Here we move beyond thermal conductivity calculations and provide a rigorous and comprehensive physical description of thermal phonon transport in superlattices by solving the Boltzmann transport equation and using the Beckman-Kirchhoff surface scattering theory with shadowing to precisely describe phonon-surface interactions. We show that thermal transport in superlattices can be divided in two different heat transport modes having different physical properties at small length scales: layer-restricted and extended heat modes. We study how interface conditions, periodicity, and composition can be used to manipulate the distribution of thermal energy flow among such layer-restricted and extended heat modes. From predicted frequency and mean free path spectra of superlattices, we also investigate the existence of wave effects. The results and insights in this paper advance the fundamental understanding of heat transport in superlattices and the prospects of rationally designing thermal systems with tailored phonon transport properties.

Effects of lithium insertion on thermal conductivity of silicon nanowires

NASA Astrophysics Data System (ADS)

Xu, Wen; Zhang, Gang; Li, Baowen

2015-04-01

Recently, silicon nanowires (SiNWs) have been applied as high-performance Li battery anodes, since they can overcome the pulverization and mechanical fracture during lithiation. Although thermal stability is one of the most important parameters that determine safety of Li batteries, thermal conductivity of SiNWs with Li insertion remains unclear. In this letter, using molecular dynamics simulations, we study room temperature thermal conductivity of SiNWs with Li insertion. It is found that compared with the pristine SiNW, there is as much as 60% reduction in thermal conductivity with 10% concentration of inserted Li atoms, while under the same impurity concentration the reduction in thermal conductivity of the mass-disordered SiNW is only 30%. With lattice dynamics calculations and normal mode decomposition, it is revealed that the phonon lifetimes in SiNWs decrease greatly due to strong scattering of phonons by vibrational modes of Li atoms, especially for those high frequency phonons. The observed strong phonon scattering phenomenon in Li-inserted SiNWs is similar to the phonon rattling effect. Our study serves as an exploration of thermal properties of SiNWs as Li battery anodes or weakly coupled with impurity atoms.

Phonon thermal transport in 2H, 4H and 6H silicon carbide from first principles

DOE PAGES

Protik, Nakib Haider; Katre, Ankita; Lindsay, Lucas R.; ...

2017-06-07

Here, silicon carbide (SiC) is a wide band gap semiconductor with a variety of industrial applications. Among its many useful properties is its high thermal conductivity, which makes it advantageous for thermal management applications. In this paper we present ab initio calculations of the in-plane and cross-plane thermal conductivities, κ in and κ out, of three common hexagonal polytypes of SiC: 2H, 4H and 6H. The phonon Boltzmann transport equation is solved iteratively using as input interatomic force constants determined from density functional theory. Both κ in and κ out decrease with increasing n in nH SiC because of additionalmore » low-lying optic phonon branches. These optic branches are characterized by low phonon group velocities, and they increase the phase space for phonon-phonon scattering of acoustic modes. Also, for all n, κ in is found to be larger than κ out in the temperature range considered. At electron concentrations present in experimental samples, scattering of phonons by electrons is shown to be negligible except well below room temperature where it can lead to a significant reduction of the lattice thermal conductivity. This work highlights the power of ab initio approaches in giving quantitative, predictive descriptions of thermal transport in materials. It helps explain the qualitative disagreement that exists among different sets of measured thermal conductivity data and provides information of the relative quality of samples from which measured data was obtained.« less

Phonon transport properties of two-dimensional group-IV materials from ab initio calculations

NASA Astrophysics Data System (ADS)

Peng, Bo; Zhang, Hao; Shao, Hezhu; Xu, Yuanfeng; Ni, Gang; Zhang, Rongjun; Zhu, Heyuan

2016-12-01

It has been argued that stanene has lowest lattice thermal conductivity among two-dimensional (2D) group-IV materials because of its largest atomic mass, weakest interatomic bonding, and enhanced ZA phonon scattering due to the breaking of an out-of-plane symmetry selection rule. However, we show that, although the lattice thermal conductivity κ for graphene, silicene, and germanene decreases monotonically with decreasing Debye temperature, unexpected higher κ is observed in stanene. By enforcing all the invariance conditions in 2D materials and including Ge 3 d and Sn 4 d electrons as valence electrons for germanene and stanene, respectively, the lattice dynamics in these materials are accurately described. A large acoustic-optical gap and the bunching of the acoustic-phonon branches significantly reduce phonon scattering in stanene, leading to higher thermal conductivity than germanene. The vibrational origin of the acoustic-optical gap can be attributed to the buckled structure. Interestingly, a buckled system has two competing influences on phonon transport: the breaking of the symmetry selection rule leads to reduced thermal conductivity, and the enlarging of the acoustic-optical gap results in enhanced thermal conductivity. The size dependence of thermal conductivity is investigated as well. In nanoribbons, the κ of silicene, germanene, and stanene is much less sensitive to size effect due to their short intrinsic phonon mean-free paths. This work sheds light on the nature of phonon transport in buckled 2D materials.

Phonon thermal transport in 2H, 4H and 6H silicon carbide from first principles

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

Protik, Nakib Haider; Katre, Ankita; Lindsay, Lucas R.

Here, silicon carbide (SiC) is a wide band gap semiconductor with a variety of industrial applications. Among its many useful properties is its high thermal conductivity, which makes it advantageous for thermal management applications. In this paper we present ab initio calculations of the in-plane and cross-plane thermal conductivities, κ in and κ out, of three common hexagonal polytypes of SiC: 2H, 4H and 6H. The phonon Boltzmann transport equation is solved iteratively using as input interatomic force constants determined from density functional theory. Both κ in and κ out decrease with increasing n in nH SiC because of additionalmore » low-lying optic phonon branches. These optic branches are characterized by low phonon group velocities, and they increase the phase space for phonon-phonon scattering of acoustic modes. Also, for all n, κ in is found to be larger than κ out in the temperature range considered. At electron concentrations present in experimental samples, scattering of phonons by electrons is shown to be negligible except well below room temperature where it can lead to a significant reduction of the lattice thermal conductivity. This work highlights the power of ab initio approaches in giving quantitative, predictive descriptions of thermal transport in materials. It helps explain the qualitative disagreement that exists among different sets of measured thermal conductivity data and provides information of the relative quality of samples from which measured data was obtained.« less

Influence of Scattering on Ballistic Nanotransistor Design

NASA Technical Reports Server (NTRS)

Anantram, M. P.; Svizhenko, Alexei; Biegel, Bryan, A. (Technical Monitor)

2002-01-01

Importance of this work: (1) This is the first work to model electron-phonon scattering within a quantum mechanical approach to nanotransistors. The simulations use the non equilibrium Green's function method. (2) A simple equation which captures the importance of scattering as a function of the spatial location from source to drain is presented. This equation helps interpret the numerical simulations. (3) We show that the resistance per unit length in the source side is much larger than in the drain side. Thus making scattering in the source side of the device much more important than scattering in the drain side. Numerical estimates of ballisticity for 10nm channel length devices in the presence of of electron-phonon scattering are given. Based on these calculations, we propose that to achieve a larger on-current in nanotransistors, it is crucial to keep the highly doped source extension region extremely small, even if this is at the cost of making the highly doped drain extension region longer.

Direct observation of confined acoustic phonon polarization branches in free-standing semiconductor nanowires

DOE PAGES

Kargar, Fariborz; Debnath, Bishwajit; Kakko, Joona -Pekko; ...

2016-11-10

Similar to electron waves, the phonon states in semiconductors can undergo changes induced by external boundaries. However, despite strong scientific and practical importance, conclusive experimental evidence of confined acoustic phonon polarization branches in individual free-standing nanostructures is lacking. Here we report results of Brillouin-Mandelstam light scattering spectroscopy, which reveal multiple (up to ten) confined acoustic phonon polarization branches in GaAs nanowires with a diameter as large as 128 nm, at a length scale that exceeds the grey phonon mean-free path in this material by almost an order-of-magnitude. The dispersion modification and energy scaling with diameter in individual nanowires are inmore » excellent agreement with theory. The phonon confinement effects result in a decrease in the phonon group velocity along the nanowire axis and changes in the phonon density of states. Furthermore, the obtained results can lead to more efficient nanoscale control of acoustic phonons, with benefits for nanoelectronic, thermoelectric and spintronic devices.« less

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

Khurgin, Jacob B., E-mail: jakek@jhu.edu; Bajaj, Sanyam; Rajan, Siddharth

Longitudinal optical (LO) phonons in GaN generated in the channel of high electron mobility transistors (HEMT) are shown to undergo nearly elastic scattering via collisions with hot electrons. The net result of these collisions is the diffusion of LO phonons in the Brillouin zone causing reduction of phonon and electron temperatures. This previously unexplored diffusion mechanism explicates how an increase in electron density causes reduction of the apparent lifetime of LO phonons, obtained from the time resolved Raman studies and microwave noise measurements, while the actual decay rate of the LO phonons remains unaffected by the carrier density. Therefore, themore » saturation velocity in GaN HEMT steadily declines with increased carrier density, in a qualitative agreement with experimental results.« less

Electron mobility in modulation-doped heterostructures

NASA Technical Reports Server (NTRS)

Walukiewicz, W.; Ruda, H. E.; Lagowski, J.; Gatos, H. C.

1984-01-01

A model for electron mobility in a two-dimensional electron gas confined in a triangular well was developed. All major scattering processes (deformation potential and piezoelectric acoustic, polar optical, ionized impurity, and alloy disorder) were included, as well as intrasubband and intersubband scattering. The model is applied to two types of modulation-doped heterostructures, namely GaAs-GaAlAs and In(0.53)Ga(0.47)As-Al(0.52)In(0.48)As. In the former case, phonons and remote ionized impurities ultimately limit the mobility, whereas in the latter, alloy disorder is a predominant scattering process at low temperatures. The calculated mobilities are in very good agreement with recently reported experimental characteristics for both GaAs-Ga(1-x)Al(x)As and In(0.53)Ga(0.47)As-Al(0.52)In(0.48)As modulation-doped heterostructures.

Thermal transport in bismuth telluride quintuple layer: mode-resolved phonon properties and substrate effects

PubMed Central

Shao, Cheng; Bao, Hua

2016-01-01

The successful exfoliation of atomically-thin bismuth telluride (Bi2Te3) quintuple layer (QL) attracts tremendous research interest in this strongly anharmonic quasi-two-dimensional material. The thermal transport properties of this material are not well understood, especially the mode-wise properties and when it is coupled with a substrate. In this work, we have performed molecular dynamics simulations and normal mode analysis to study the mode-resolved thermal transport in freestanding and supported Bi2Te3 QL. The detailed mode-wise phonon properties are calculated and the accumulated thermal conductivities with respect to phonon mean free path (MFP) are constructed. It is shown that 60% of the thermal transport is contributed by phonons with MFP longer than 20 nm. Coupling with a-SiO2 substrate leads to about 60% reduction of thermal conductivity. Through varying the interfacial coupling strength and the atomic mass of substrate, we also find that phonon in Bi2Te3 QL is more strongly scattered by interfacial potential and its transport process is less affected by the dynamics of substrate. Our study provides an in-depth understanding of heat transport in Bi2Te3 QL and is helpful in further tailoring its thermal property through nanostructuring. PMID:27263656

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.

Defects Enable Dark Exciton Photoluminescence in Single-Walled Carbon Nanotubes

DOE PAGES

Amori, Amanda R.; Rossi, Jamie E.; Landi, Brian J.; ...

2018-01-24

Variable temperature photoluminescence excitation spectroscopy of three (n,m) species of single-walled carbon nanotubes revealed that at resonant S 22 excitation, in addition to allowed excitonic optical transitions, several sidebands that should be forbidden based on selection rules were observed and appeared to have a strong temperature dependence. In particular, we found that a sideband located approximately 130 meV away from the bright S 11 exciton peak relating to the K-momentum dark exciton state, called X 1, decreased in intensity five-fold as the samples were cooled. Direct optical excitation of this dark state is nominally forbidden, thus calling into question howmore » the state is populated, and why it is so prominent in the photoluminescence spectrum. Interestingly, the ratio of the integrated photoluminescence intensities of X 1 to S 11 scales with a Boltzmann factor unrelated to the phonon that is thought to be responsible for depopulating the K-momentum dark exciton state: an in-plane transverse optical phonon, A 1’. Furthermore, photoluminescence spectra from individual (7,5) nanotubes show that only a small fraction exhibit the X 1 feature, with varying oscillator strength, thus suggesting that intrinsic processes such as phonon scattering are not responsible for populating the dark state. Alternatively, we suggest that populating the K-momentum dark exciton state requires scattering from defects, which is consistent with the increased magnitude of the X 1 feature for samples with increased sample purification and processing. Thus, the presence of an X 1 peak in photoluminescence is an extremely sensitive spectroscopic indicator of defects on single-walled carbon nanotubes.« less

Defects Enable Dark Exciton Photoluminescence in Single-Walled Carbon Nanotubes

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

Amori, Amanda R.; Rossi, Jamie E.; Landi, Brian J.

Variable temperature photoluminescence excitation spectroscopy of three (n,m) species of single-walled carbon nanotubes revealed that at resonant S 22 excitation, in addition to allowed excitonic optical transitions, several sidebands that should be forbidden based on selection rules were observed and appeared to have a strong temperature dependence. In particular, we found that a sideband located approximately 130 meV away from the bright S 11 exciton peak relating to the K-momentum dark exciton state, called X 1, decreased in intensity five-fold as the samples were cooled. Direct optical excitation of this dark state is nominally forbidden, thus calling into question howmore » the state is populated, and why it is so prominent in the photoluminescence spectrum. Interestingly, the ratio of the integrated photoluminescence intensities of X 1 to S 11 scales with a Boltzmann factor unrelated to the phonon that is thought to be responsible for depopulating the K-momentum dark exciton state: an in-plane transverse optical phonon, A 1’. Furthermore, photoluminescence spectra from individual (7,5) nanotubes show that only a small fraction exhibit the X 1 feature, with varying oscillator strength, thus suggesting that intrinsic processes such as phonon scattering are not responsible for populating the dark state. Alternatively, we suggest that populating the K-momentum dark exciton state requires scattering from defects, which is consistent with the increased magnitude of the X 1 feature for samples with increased sample purification and processing. Thus, the presence of an X 1 peak in photoluminescence is an extremely sensitive spectroscopic indicator of defects on single-walled carbon nanotubes.« less

An analysis of phonon emission as controlled by the combined interaction with the acoustic and piezoelectric phonons in a degenerate III-V compound semiconductor using an approximated Fermi-Dirac distribution at low lattice temperatures

NASA Astrophysics Data System (ADS)

Basu, A.; Das, B.; Middya, T. R.; Bhattacharya, D. P.

2018-03-01

Compound semiconductors being piezoelectric in nature, the intrinsic thermal vibration of the lattice atoms at any temperature gives rise to an additional potential field that perturbs the periodic potential field of the atoms. This is over and above the intrinsic deformation acoustic potential field which is always produced in every material. The scattering of the electrons through the piezoelectric perturbing potential is important in all compound semiconductors, particularly at the low lattice temperatures. Thus, the electrical transport in such materials is principally controlled by the combined interaction of the electrons with the deformation potential acoustic and piezoelectric phonons at low lattice temperatures. The study here, deals with the problem of phonon growth characteristics, considering the combined scattering of the non-equilibrium electrons in compound semiconductors, at low lattice temperatures. Beside degeneracy, other low temperature features, like the inelasticity of the electron-phonon collisions, and the full form of the phonon distribution have been duly considered. The distribution function of the degenerate ensemble of carriers, as given by the heated Fermi-Dirac function, has been approximated by a simplified, well-tested model. The model which has been proposed earlier, makes it much easier to carry out analytically the integrations without usual oversimplified approximations.

Full-dispersion Monte Carlo simulation of phonon transport in micron-sized graphene nanoribbons

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

Mei, S., E-mail: smei4@wisc.edu; Knezevic, I., E-mail: knezevic@engr.wisc.edu; Maurer, L. N.

2014-10-28

We simulate phonon transport in suspended graphene nanoribbons (GNRs) with real-space edges and experimentally relevant widths and lengths (from submicron to hundreds of microns). The full-dispersion phonon Monte Carlo simulation technique, which we describe in detail, involves a stochastic solution to the phonon Boltzmann transport equation with the relevant scattering mechanisms (edge, three-phonon, isotope, and grain boundary scattering) while accounting for the dispersion of all three acoustic phonon branches, calculated from the fourth-nearest-neighbor dynamical matrix. We accurately reproduce the results of several experimental measurements on pure and isotopically modified samples [S. Chen et al., ACS Nano 5, 321 (2011);S. Chenmore » et al., Nature Mater. 11, 203 (2012); X. Xu et al., Nat. Commun. 5, 3689 (2014)]. We capture the ballistic-to-diffusive crossover in wide GNRs: room-temperature thermal conductivity increases with increasing length up to roughly 100 μm, where it saturates at a value of 5800 W/m K. This finding indicates that most experiments are carried out in the quasiballistic rather than the diffusive regime, and we calculate the diffusive upper-limit thermal conductivities up to 600 K. Furthermore, we demonstrate that calculations with isotropic dispersions overestimate the GNR thermal conductivity. Zigzag GNRs have higher thermal conductivity than same-size armchair GNRs, in agreement with atomistic calculations.« less

Dissipative time-dependent quantum transport theory: Quantum interference and phonon induced decoherence dynamics

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

Zhang, Yu, E-mail: zhy@yangtze.hku.hk; Chen, GuanHua, E-mail: ghc@everest.hku.hk; Yam, ChiYung

2015-04-28

A time-dependent inelastic electron transport theory for strong electron-phonon interaction is established via the equations of motion method combined with the small polaron transformation. In this work, the dissipation via electron-phonon coupling is taken into account in the strong coupling regime, which validates the small polaron transformation. The corresponding equations of motion are developed, which are used to study the quantum interference effect and phonon-induced decoherence dynamics in molecular junctions. Numerical studies show clearly quantum interference effect of the transport electrons through two quasi-degenerate states with different couplings to the leads. We also found that the quantum interference can bemore » suppressed by the electron-phonon interaction where the phase coherence is destroyed by phonon scattering. This indicates the importance of electron-phonon interaction in systems with prominent quantum interference effect.« less

Femtosecond study of A1g phonons in the strong 3D topological insulators: From pump-probe to coherent control

NASA Astrophysics Data System (ADS)

Hu, Jianbo; Igarashi, Kyushiro; Sasagawa, Takao; Nakamura, Kazutaka G.; Misochko, Oleg V.

2018-01-01

Fully symmetric A1g phonons are expected to play a dominant role in electron scattering in strong topological insulators (TIs), thus limiting the ballistic transport of future electronic devices. Here, we report on femtosecond time-resolved observation of a pair of A1g coherent phonons and their optical control in two strong 3D TIs, Bi2Te3 and Bi2Se3, by using a second pump pulse in ultrafast spectroscopy measurements. Along with well-defined phonon properties such as frequency and lifetime, an obvious phonon chirp has been observed, implying a strong coupling between photo-carriers and lattices. The coherent phonon manipulation, on the other hand, allows us to change the phonon amplitude selectively but does not affect either the frequency or coherence lifetime of the chosen mode.

Theory and experimental evidence of phonon domains and their roles in pre-martensitic phenomena

NASA Astrophysics Data System (ADS)

Jin, Yongmei M.; Wang, Yu U.; Ren, Yang

2015-12-01

Pre-martensitic phenomena, also called martensite precursor effects, have been known for decades while yet remain outstanding issues. This paper addresses pre-martensitic phenomena from new theoretical and experimental perspectives. A statistical mechanics-based Grüneisen-type phonon theory is developed. On the basis of deformation-dependent incompletely softened low-energy phonons, the theory predicts a lattice instability and pre-martensitic transition into elastic-phonon domains via 'phonon spinodal decomposition.' The phase transition lifts phonon degeneracy in cubic crystal and has a nature of phonon pseudo-Jahn-Teller lattice instability. The theory and notion of phonon domains consistently explain the ubiquitous pre-martensitic anomalies as natural consequences of incomplete phonon softening. The phonon domains are characterised by broken dynamic symmetry of lattice vibrations and deform through internal phonon relaxation in response to stress (a particular case of Le Chatelier's principle), leading to previously unexplored new domain phenomenon. Experimental evidence of phonon domains is obtained by in situ three-dimensional phonon diffuse scattering and Bragg reflection using high-energy synchrotron X-ray single-crystal diffraction, which observes exotic domain phenomenon fundamentally different from usual ferroelastic domain switching phenomenon. In light of the theory and experimental evidence of phonon domains and their roles in pre-martensitic phenomena, currently existing alternative opinions on martensitic precursor phenomena are revisited.

Inequivalence of single-particle and population lifetimes in a cuprate superconductor

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

Yang, Shuolong; Sobota, J. A.; Leuenberger, D.

2015-06-15

We study optimally doped Bi-2212 (T c=96 K) using femtosecond time- and angle-resolved photoelectron spectroscopy. Energy-resolved population lifetimes are extracted and compared with single-particle lifetimes measured by equilibrium photoemission. The population lifetimes deviate from the single-particle lifetimes in the low excitation limit by 1–2 orders of magnitude. Fundamental considerations of electron scattering unveil that these two lifetimes are in general distinct, yet for systems with only electron-phonon scattering they should converge in the low-temperature, low-fluence limit. As a result, the qualitative disparity in our data, even in this limit, suggests that scattering channels beyond electron-phonon interactions play a significant rolemore » in the electron dynamics of cuprate superconductors.« less

Thermoelectric Transport in Nanocomposites

PubMed Central

Liu, Bin; Hu, Jizhu; Zhou, Jun; Yang, Ronggui

2017-01-01

Thermoelectric materials which can convert energies directly between heat and electricity are used for solid state cooling and power generation. There is a big challenge to improve the efficiency of energy conversion which can be characterized by the figure of merit (ZT). In the past two decades, the introduction of nanostructures into bulk materials was believed to possibly enhance ZT. Nanocomposites is one kind of nanostructured material system which includes nanoconstituents in a matrix material or is a mixture of different nanoconstituents. Recently, nanocomposites have been theoretically proposed and experimentally synthesized to be high efficiency thermoelectric materials by reducing the lattice thermal conductivity due to phonon-interface scattering and enhancing the electronic performance due to manipulation of electron scattering and band structures. In this review, we summarize the latest progress in both theoretical and experimental works in the field of nanocomposite thermoelectric materials. In particular, we present various models of both phonon transport and electron transport in various nanocomposites established in the last few years. The phonon-interface scattering, low-energy electrical carrier filtering effect, and miniband formation, etc., in nanocomposites are discussed. PMID:28772777

Thermoelectric Transport in Nanocomposites.

PubMed

Liu, Bin; Hu, Jizhu; Zhou, Jun; Yang, Ronggui

2017-04-15

Thermoelectric materials which can convert energies directly between heat and electricity are used for solid state cooling and power generation. There is a big challenge to improve the efficiency of energy conversion which can be characterized by the figure of merit ( ZT ). In the past two decades, the introduction of nanostructures into bulk materials was believed to possibly enhance ZT . Nanocomposites is one kind of nanostructured material system which includes nanoconstituents in a matrix material or is a mixture of different nanoconstituents. Recently, nanocomposites have been theoretically proposed and experimentally synthesized to be high efficiency thermoelectric materials by reducing the lattice thermal conductivity due to phonon-interface scattering and enhancing the electronic performance due to manipulation of electron scattering and band structures. In this review, we summarize the latest progress in both theoretical and experimental works in the field of nanocomposite thermoelectric materials. In particular, we present various models of both phonon transport and electron transport in various nanocomposites established in the last few years. The phonon-interface scattering, low-energy electrical carrier filtering effect, and miniband formation, etc., in nanocomposites are discussed.

Polariton effects in naphthalene crystals

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

Robinette, Susan Louise

1977-10-01

The experimental verification of the two-step nature of energy dissipation of photon energy by a crystal is the subject of this dissertation. The ..cap alpha..(O,O) Davydov component of the lowest energy singlet transition in pure strain-free napthalene single crystals is shown to exhibit an increase in absorption with increasing temperature, due to an increase in polariton damping via polariton-phonon scattering processes. (GHT)

Size Effects in Nanoscale Structural Phenomena

NASA Astrophysics Data System (ADS)

McElhinny, Kyle Matthew

The creation of nanostructures offers the opportunity to modify and tune properties in ways inaccessible in bulk materials. A key component in this development is the introduction of size effects which reduce the physical size, dimensionality, and increase the contribution of surface effects. The size effects strongly modify the structural dynamics in nanoscale systems and leads to changes in the vibrational, electrical, and optical properties. An increased level of understanding and control of nanoscale structural dynamics will enable more precise control over nanomaterial transport properties. My work has shown that 1D spatial confinement through the creation of semiconducting nanomembranes modifies the phonon population and dispersion. X ray thermal diffuse scattering distributions show an excess in intensity for nanomembranes less than 100 nm in thickness, for phonon modes with wavevectors spanning the entire Brillouin zone. This excess intensity indicates the development of new low energy phonon modes or the softening of elastic constants. Furthermore, an additional anisotropy in the phonon dispersion is observed with a symmetry matching the direction of spatial confinement. This work has also extended x ray thermal diffuse scattering for use in studying nanomaterials. In electro- and photoactive monolayers a structural reconfiguration can be produced by external optical stimuli. I have developed an electro and photoactive molecular monolayers on oxide surfaces. Using x ray reflectivity, I have evaluated the organization and reconfiguration of molecular monolayers deposited by Langmuir Blodgett technique. I have designed and probed the reconfiguration of optically reconfigurable monolayers of azobenzene donor molecules on semiconducting surfaces. These monolayers reconfigure through a cooperative switching process leading to the development of large isomeric domains. This work represents an advancement in the interpretation of x ray reflectivity from molecular monolayers and inhomogeneous surfaces. The growth 2D materials depends on the interactions between the substrate and the 2D material. I have studied the competition between kinetics and surface energetics which lead to a faceted Ge surface during the growth of Graphene nanoribbons. As part of this work, I have developed new methodologies for interpreting x ray reflectivity patterns from surfaces with multiple reflections. A systematic analysis of the temperature dependence of the faceting process indicates that the process is thermodynamically dominated at high temperatures.

Study of phonons in irradiated epitaxial thin films of UO2

NASA Astrophysics Data System (ADS)

Rennie, S.; Lawrence Bright, E.; Darnbrough, J. E.; Paolasini, L.; Bosak, A.; Smith, A. D.; Mason, N.; Lander, G. H.; Springell, R.

2018-06-01

We report experiments to determine the effect of radiation damage on the phonon spectra of the most common nuclear fuel, UO2. We irradiated thin (˜300 nm) epitaxial films of UO2 with 2.1 MeV He2 + ions to 0.15 displacements per atom and a lattice swelling of Δ a /a ˜0.6 % and then used grazing-incidence inelastic x-ray scattering to measure the phonon spectrum. We succeeded in observing the acoustic modes, both transverse and longitudinal, across the Brillouin zone. The phonon energies, in both the pristine and irradiated samples, are unchanged from those observed in bulk material. On the other hand, the phonon linewidths (inversely proportional to the phonon lifetimes) show a significant broadening when comparing the pristine and irradiated samples. This effect is shown to increase with phonon energy across the Brillouin zone. The decreases in the phonon lifetimes of the acoustic modes are roughly consistent with a 50% reduction in the thermal conductivity.

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.

Towards predictive many-body calculations of phonon-limited carrier mobilities in semiconductors

NASA Astrophysics Data System (ADS)

Poncé, Samuel; Margine, Elena R.; Giustino, Feliciano

2018-03-01

We probe the accuracy limit of ab initio calculations of carrier mobilities in semiconductors, within the framework of the Boltzmann transport equation. By focusing on the paradigmatic case of silicon, we show that fully predictive calculations of electron and hole mobilities require many-body quasiparticle corrections to band structures and electron-phonon matrix elements, the inclusion of spin-orbit coupling, and an extremely fine sampling of inelastic scattering processes in momentum space. By considering all these factors we obtain excellent agreement with experiment, and we identify the band effective masses as the most critical parameters to achieve predictive accuracy. Our findings set a blueprint for future calculations of carrier mobilities, and pave the way to engineering transport properties in semiconductors by design.

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.

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.

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.

First-principles analysis of anharmonic nuclear motion and thermal transport in thermoelectric materials

NASA Astrophysics Data System (ADS)

Tadano, Terumasa; Tsuneyuki, Shinji

2015-12-01

We show a first-principles approach for analyzing anharmonic properties of lattice vibrations in solids. We firstly extract harmonic and anharmonic force constants from accurate first-principles calculations based on the density functional theory. Using the many-body perturbation theory of phonons, we then estimate the phonon scattering probability due to anharmonic phonon-phonon interactions. We show the validity of the approach by computing the lattice thermal conductivity of Si, a typical covalent semiconductor, and selected thermoelectric materials PbTe and Bi2Te3 based on the Boltzmann transport equation. We also show that the phonon lifetime and the lattice thermal conductivity of the high-temperature phase of SrTiO3 can be estimated by employing the perturbation theory on top of the solution of the self-consistent phonon equation.

Peculiarities of both light and beta-particles scattering by ultrathin diamond-like semiconductor film.

PubMed

Rumyantsev, Vladimir V; Shtaerman, Esfir Y

2008-02-01

Peculiarities of scattering of TM-polarized light wave by a diamond-like crystalline nano-layer are studied. They are due to specific dispersion of n-phonon polaritons localized in the layer. The IR polaritons discussed here (relating to diamond and Si crystals which are nonpolar materials) will only appear if some of the vibration modes become polar, e.g., due to the presence of the surface. As a result of mixing of g- and u-modes of ion oscillations along the (111)-direction in the near-surface layer, it is possible to observe additional (with respect to bulk) scattering of coherent electromagnetic waves of the Stokes and anti-Stokes frequencies. beta-particles can be utilized as an independent tool of study of new semiconductors, in particular thin diamond films. The effect associated with response of a quasi-two-dimensional diamond-like layer to the moving electron field is considered. beta-particle field induces phonon excitation modes to arise in the material. Coupled with the beta-particle electromagnetic modes they generate polaritons. Spectral density of the radiation intensity of the flashed phonon polaritons has been estimated as a function of the layer thickness as well as of the scattering angle and the beta-particle velocity.

Phonon Scattering in Silicon by Multiple Morphological Defects: A Multiscale Analysis

NASA Astrophysics Data System (ADS)

Lorenzi, Bruno; Dettori, Riccardo; Dunham, Marc T.; Melis, Claudio; Tonini, Rita; Colombo, Luciano; Sood, Aditya; Goodson, Kenneth E.; Narducci, Dario

2018-05-01

Ideal thermoelectric materials should possess low thermal conductivity κ along with high electrical conductivity σ . Thus, strategies are needed to impede the propagation of phonons mostly responsible for thermal conduction while only marginally affecting charge carrier diffusion. Defect engineering may provide tools to fulfill this aim, provided that one can achieve an adequate understanding of the role played by multiple morphological defects in scattering thermal energy carriers. In this paper, we study how various morphological defects such as grain boundaries and dispersed nanovoids reduce the thermal conductivity of silicon. A blended approach has been adopted, using data from both simulations and experiments in order to cover a wide range of defect densities. We show that the co-presence of morphological defects with different characteristic scattering length scales is effective in reducing the thermal conductivity. We also point out that non-gray models (i.e. models with spectral resolution) are required to improve the accuracy of predictive models explaining the dependence of κ on the density of morphological defects. Finally, the application of spectral models to Matthiessen's rule is critically addressed with the aim of arriving at a compact model of phonon scattering in highly defective materials showing that non-local descriptors would be needed to account for lattice distortion due to nanometric voids.

Equilibrium Limit of Boundary Scattering in Carbon Nanostructures: Molecular Dynamics Calculations of Thermal Transport

NASA Technical Reports Server (NTRS)

Haskins, Justin; Kinaci, Alper; Sevik, Cem; Cagin, Tahir

2012-01-01

It is widely known that graphene and many of its derivative nanostructures have exceedingly high reported thermal conductivities (up to 4000 W/mK at 300 K). Such attractive thermal properties beg the use of these structures in practical devices; however, to implement these materials while preserving transport quality, the influence of structure on thermal conductivity should be thoroughly understood. For graphene nanostructures, having average phonon mean free paths on the order of one micron, a primary concern is how size influences the potential for heat conduction. To investigate this, we employ a novel technique to evaluate the lattice thermal conductivity from the Green-Kubo relations and equilibrium molecular dynamics in systems where phonon-boundary scattering dominates heat flow. Specifically, the thermal conductivities of graphene nanoribbons and carbon nanotubes are calculated in sizes up to 3 microns, and the relative influence of boundary scattering on thermal transport is determined to be dominant at sizes less than 1 micron, after which the thermal transport largely depends on the quality of the nanostructure interface. The method is also extended to carbon nanostructures (fullerenes) where phonon confinement, as opposed to boundary scattering, dominates, and general trends related to the influence of curvature on thermal transport in these materials are discussed.

Theory of intermediate- and high-field mobility in dilute nitride alloys

NASA Astrophysics Data System (ADS)

Seifikar, Masoud; O'Reilly, Eoin P.; Fahy, Stephen

2011-10-01

We have solved the steady-state Boltzmann transport equation in bulk GaAs1-xNx. Two different models of the conduction band structure have been studied to investigate the behavior of electrons with increasing electric field in these alloys: (1) carriers in parabolic Γ and L bands are scattered by resonant nitrogen substitutional defect states, polar optic and acoustic phonons, and intervalley optical phonons; (2) carriers, constrained in the lower band of the band-anticrossing (BAC) model, are scattered by phonons and by nitrogen states. We consider scattering both by isolated N atoms and also by a full distribution of N states. We find that it is necessary to include the full distribution of levels in order to account for the small low-field mobility and the absence of a negative differential velocity regime observed experimentally with increasing x. Model 2 breaks down at intermediate and high field, due to the unphysical constraint of limiting carriers to the lower BAC band. For model 1, carrier scattering into the L bands is reduced at intermediate electric fields but is comparable at high fields to that observed in GaAs, with the calculated high-field mobility and carrier distribution then also being comparable to GaAs. Overall the results account well for a wide range of experimental data.

Influence of defects and doping on phonon transport properties of monolayer MoSe2

NASA Astrophysics Data System (ADS)

Yan, Zhequan; Yoon, Mina; Kumar, Satish

2018-07-01

The doping of monolayer MoSe2 by tungsten (W) can suppress the Se vacancy concentration, but how doping and resulting change in defect concentration can tune its thermal properties is not understood yet. We use first-principles density functional theory (DFT) along with the phonon Boltzmann transport equation (BTE) to study the phonon transport properties of pristine MoSe2 and W doped MoSe2 with and without the presence of Se vacancies. We found that for samples without Se vacancy, the W doping could enhance the thermal transport of monolayer MoSe2 due to reduced three-phonon scattering phase space. For example, we observed that the 16.7% W doping increases the thermal conductivity of the monolayer MoSe2 with 2% Se vacancy by 80% if all vacancies can be suppressed by W-doping. However, the W doping in the defective MoSe2 amplifies the influence of the phonon scattering caused by the Se vacancies, which results in a further decrease in thermal conductivity of monolayer MoSe2 with defects. This is found to be related with higher phonon density of states of Mo0.83W0.17Se2 and larger mass difference between W and Se atoms compared to Mo and Se atoms. This study deciphers the effect of defects and doping on the thermal conductivity of monolayer MoSe2, which helps us understand the mechanism of defect-induced phonon transport, and provides insights into enhancing the heat dissipation in MoSe2-based electronic devices.

Soft-phonon dynamics of the thermoelectric β-SnSe at high temperatures

NASA Astrophysics Data System (ADS)

Chatterji, Tapan; Wdowik, Urszula D.; Jagło, Grzegorz; Rols, Stéphane; Wagner, Frank R.

2018-07-01

Results of inelastic neutron scattering experiments on SnSe single crystals at high temperatures along with theoretical studies based on the density functional theory are reported. Our experiments reveal significant softening of the transverse acoustic branch along the [ 0 , ξ , 0 ] direction in the low-temperature α-SnSe of Pbnm symmetry as temperature approaches Tc = 807 K from below. This process is followed by a condensation of the zone-boundary Y-phonon of the high-temperature β-SnSe with Cmcm symmetry at the onset of phase transition. The employed theoretical approach supports experimental observations and demonstrates that the phase change in SnSe is mediated by an unstable zone-boundary phonon with the Y2+ irreducible representation within the Cmcm symmetry space group of the high-temperature β-SnSe. The present work provides a detailed understanding of the soft-mode dynamics in SnSe and conclusively shows that the α ⇌ β structural transformation in this currently topical thermoelectric material is of displacive type.

Thermal Conductivity of Twisted Bilayer Graphene Nanoribbons from Non-equilibrium Molecular Dynamics Study.

NASA Astrophysics Data System (ADS)

Li, Chenyang; Su, Shanshan; Ge, Supeng; Lake, Roger

Misorientation of the two layers of bilayer graphene affects both the electronic properties and the vibrational modes or phonons. The phonon density of modes is little affected by misorientation, however, zone-folding can allow new Umklapp scattering processes that could affect the phonon transport and thermal conductivity. To investigate this, we use NEMD molecular dynamics simulations as implemented in LAMMPS to study the thermal conductivity of the misoriented graphene bilayers. Seven commensurate misorientation angles varying from 6.01º to 48.36º have modeled and analyzed to understand how the misorientation angle affects the thermal conductivity of relatively wide ( 10 nm) misoriented bilayer graphene nanoribbons (m-BLGNRs). Within numerical accuracy, we find that the thermal conductivity of the m-BLGNRs for all of the simulated commensurate angles have the same thermal conductivity with AB stacked and AA stacked BLGNRs. These results indicate that neither the misorientation angle nor the stacking order affect the thermal conductivity of BLGNRs. This work was supported as part by the NSF #1307671.

Measurements Of The Effects Of Grain Boundary And Alloy Scattering On Spectral Phonon Mean Free Path Distributions.

NASA Astrophysics Data System (ADS)

Lubner, Sean; Khan, Md. Imran; Dames, Chris

In the electronics and clean energy fields, it is increasingly necessary to reliably model the dissipation of heat from micro and nanostructures or nanostructured materials such as in batteries, computer chips, and thermoelectrics. In these regimes where length scales are comparable to the mean free paths (MFPs) of energy carriers, the diffusion law of heat conduction begins to break down. In this talk, I present our recent results from using a time domain thermoreflectance (TDTR) technique with laser spot 1/e-squared radii less than 2 microns to measure sub-diffusion thermal transport in silicon, nanograined-silicon (ng-Si), and silicon germanium (SiGe) alloys. Our results experimentally demonstrate that alloy scattering skews phonon spectra toward longer MFPs, while nanostructuring skews phonon spectra toward shorter MFPs. As a consequence, we show that a significant fraction of the heat-carrying phonons in SiGe have MFPs greater than 10 microns at room temperature, and that the thermal conductivity of ng-Si overtakes that of SiGe after microstructuring. NSF.

Coupling of Excitons and Discrete Acoustic Phonons in Vibrationally Isolated Quantum Emitters.

PubMed

Werschler, Florian; Hinz, Christopher; Froning, Florian; Gumbsheimer, Pascal; Haase, Johannes; Negele, Carla; de Roo, Tjaard; Mecking, Stefan; Leitenstorfer, Alfred; Seletskiy, Denis V

2016-09-14

The photoluminescence emission by mesoscopic condensed matter is ultimately dictated by the fine-structure splitting of the fundamental exciton into optically allowed and dipole-forbidden states. In epitaxially grown semiconductor quantum dots, nonradiative equilibration between the fine-structure levels is mediated by bulk acoustic phonons, resulting in asymmetric spectral broadening of the excitonic luminescence. In isolated colloidal quantum dots, spatial confinement of the vibrational motion is expected to give rise to an interplay between the quantized electronic and phononic degrees of freedom. In most cases, however, zero-dimensional colloidal nanocrystals are strongly coupled to the substrate such that the charge relaxation processes are still effectively governed by the bulk properties. Here we show that encapsulation of single colloidal CdSe/CdS nanocrystals into individual organic polymer shells allows for systematic vibrational decoupling of the semiconductor nanospheres from the surroundings. In contrast to epitaxially grown quantum dots, simultaneous quantization of both electronic and vibrational degrees of freedom results in a series of strong and narrow acoustic phonon sidebands observed in the photoluminescence. Furthermore, an individual analysis of more than 200 compound particles reveals that enhancement or suppression of the radiative properties of the fundamental exciton is controlled by the interaction between fine-structure states via the discrete vibrational modes. For the first time, pronounced resonances in the scattering rate between the fine-structure states are directly observed, in good agreement with a quantum mechanical model. The unambiguous assignment of mediating acoustic modes to the observed scattering resonances complements the experimental findings. Thus, our results form an attractive basis for future studies on subterahertz quantum opto-mechanics and efficient laser cooling at the nanoscale.

Fourier-transform-based model for carrier transport in semiconductor heterostructures: Longitudinal optical phonon scattering

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

Lü, X.; Schrottke, L.; Grahn, H. T.

We present scattering rates for electrons at longitudinal optical phonons within a model completely formulated in the Fourier domain. The total intersubband scattering rates are obtained by averaging over the intrasubband electron distributions. The rates consist of the Fourier components of the electron wave functions and a contribution depending only on the intersubband energies and the intrasubband carrier distributions. The energy-dependent part can be reproduced by a rational function, which allows for the separation of the scattering rates into a dipole-like contribution, an overlap-like contribution, and a contribution which can be neglected for low and intermediate carrier densities of themore » initial subband. For a balance between accuracy and computation time, the number of Fourier components can be adjusted. This approach facilitates an efficient design of complex heterostructures with realistic, temperature- and carrier density-dependent rates.« less

Electrical and Electron-Phonon Interactions in Graphene-Based Nanostructures and Aptamer-Based Electrical Sensors

NASA Astrophysics Data System (ADS)

Qian, Jun

This research work contains two main parts: the theoretical study of confined phonon modes and electron states in confined graphene nanostructures; the experimental part including two topics about fabricating a graphene-FET aptamer-sensor for cocaine detection and the study of the electronic transport properties of dsDNA. In the theory part, we study the confined optical phonon modes in graphene nanoribbons (GNR) and rectangular graphene quantum dots (RGQD) by the elastic continuum model. The carrier states are studied by effective mass approximation. The phonon bottleneck effect is expected in general for RGQDs. The scattering rates are calculated for specific RGQDs with carefully chosen dimensions to fulfill the momentum and energy conservation conditions. In the experimental part, we have developed a combined technique of semiconductor processes and molecular biological protocols to fabricate a signal-off graphene-FET aptamer-sensor for cocaine. In addition, DNA transport properties were studied by STM on GNP-dsDNA-Au conjugates in atmospheric condition. The dsDNA-complexes exhibit as a slightly n-type semiconductor by simulated with a Landauer-type model. A geometrical model is proposed to explain the distinct I-V spectra.

Prediction of Thermal Transport Properties of Materials with Microstructural Complexity

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

Chen, Youping

This project aims at overcoming the major obstacle standing in the way of progress in dynamic multiscale simulation, which is the lack of a concurrent atomistic-continuum method that allows phonons, heat and defects to pass through the atomistic-continuum interface. The research has led to the development of a concurrent atomistic-continuum (CAC) methodology for multiscale simulations of materials microstructural, mechanical and thermal transport behavior. Its efficacy has been tested and demonstrated through simulations of dislocation dynamics and phonon transport coupled with microstructural evolution in a variety of materials and through providing visual evidences of the nature of phonon transport, such asmore » showing the propagation of heat pulses in single and polycrystalline solids is partially ballistic and partially diffusive. In addition to providing understanding on phonon scattering with phase interface and with grain boundaries, the research has contributed a multiscale simulation tool for understanding of the behavior of complex materials and has demonstrated the capability of the tool in simulating the dynamic, in situ experimental studies of nonequilibrium transient transport processes in material samples that are at length scales typically inaccessible by atomistically resolved methods.« less

Broadband sound blocking in phononic crystals with rotationally symmetric inclusions.

PubMed

Lee, Joong Seok; Yoo, Sungmin; Ahn, Young Kwan; Kim, Yoon Young

2015-09-01

This paper investigates the feasibility of broadband sound blocking with rotationally symmetric extensible inclusions introduced in phononic crystals. By varying the size of four equally shaped inclusions gradually, the phononic crystal experiences remarkable changes in its band-stop properties, such as shifting/widening of multiple Bragg bandgaps and evolution to resonance gaps. Necessary extensions of the inclusions to block sound effectively can be determined for given incident frequencies by evaluating power transmission characteristics. By arraying finite dissimilar unit cells, the resulting phononic crystal exhibits broadband sound blocking from combinational effects of multiple Bragg scattering and local resonances even with small-numbered cells.

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

Peng, Hua; College of Physics and Optoelectronics, Taiyuan University of Technology, Taiyuan 030024; Kioussis, Nicholas, E-mail: nick.kioussis@csun.edu

Using ab initio based calculations, we have calculated the intrinsic lattice thermal conductivity of chiral tellurium. We show that the interplay between the strong covalent intrachain and weak van der Waals interchain interactions gives rise to the phonon band gap between the lower and higher optical phonon branches. The underlying mechanism of the large anisotropy of the thermal conductivity is the anisotropy of the phonon group velocities and of the anharmonic interatomic force constants (IFCs), where large interchain anharmonic IFCs are associated with the lone electron pairs. We predict that tellurium has a large three-phonon scattering phase space that resultsmore » in low thermal conductivity. The thermal conductivity anisotropy decreases under applied hydrostatic pressure.« less

Ballistic phonon transmission in quasiperiodic acoustic nanocavities

NASA Astrophysics Data System (ADS)

Mo, Yuan; Huang, Wei-Qing; Huang, Gui-Fang; Chen, Yuan; Hu, Wangyu; Wang, Ling-Ling; Pan, Anlian

2011-04-01

Ballistic phonon transport is investigated in acoustic nanocavities modulated in a quasiperiodic manner at low temperatures. Two different types of quasiperiodic acoustic nanocavities are considered: the lengths of nanocavities (QPL) and the lengths of the bridges (QPD) connecting two successive nanocavities are modulated according to the Fibonacci rule. We demonstrate that the transmission spectra and thermal conductance in both systems are similar, which is more prominent in QPD than in QPL. The transmission and thermal conductance of QPD are larger than those of QPL due to the fact that constant nanocavity length in QPD would strengthen ballistic phonon resonant transport, while varying nanocavity length in QPL lead to strong phonon scattering.

Wave excitations of drifting two-dimensional electron gas under strong inelastic scattering

NASA Astrophysics Data System (ADS)

Korotyeyev, V. V.; Kochelap, V. A.; Varani, L.

2012-10-01

We have analyzed low-temperature behavior of two-dimensional electron gas in polar heterostructures subjected to a high electric field. When the optical phonon emission is the fastest relaxation process, we have found existence of collective wave-like excitations of the electrons. These wave-like excitations are periodic in time oscillations of the electrons in both real and momentum spaces. The excitation spectra are of multi-branch character with considerable spatial dispersion. There are one acoustic-type and a number of optical-type branches of the spectra. Their small damping is caused by quasi-elastic scattering of the electrons and formation of relevant space charge. Also there exist waves with zero frequency and finite spatial periods—the standing waves. The found excitations of the electron gas can be interpreted as synchronous in time and real space manifestation of well-known optical-phonon-transient-time-resonance. Estimates of parameters of the excitations for two polar heterostructures, GaN/AlGaN and ZnO/MgZnO, have shown that excitation frequencies are in THz-frequency range, while standing wave periods are in sub-micrometer region.

Microscopic origins of the terahertz carrier relaxation and cooling dynamics in graphene

PubMed Central

Mihnev, Momchil T.; Kadi, Faris; Divin, Charles J.; Winzer, Torben; Lee, Seunghyun; Liu, Che-Hung; Zhong, Zhaohui; Berger, Claire; de Heer, Walt A.; Malic, Ermin; Knorr, Andreas; Norris, Theodore B.

2016-01-01

The ultrafast dynamics of hot carriers in graphene are key to both understanding of fundamental carrier–carrier interactions and carrier–phonon relaxation processes in two-dimensional materials, and understanding of the physics underlying novel high-speed electronic and optoelectronic devices. Many recent experiments on hot carriers using terahertz spectroscopy and related techniques have interpreted the variety of observed signals within phenomenological frameworks, and sometimes invoke extrinsic effects such as disorder. Here, we present an integrated experimental and theoretical programme, using ultrafast time-resolved terahertz spectroscopy combined with microscopic modelling, to systematically investigate the hot-carrier dynamics in a wide array of graphene samples having varying amounts of disorder and with either high or low doping levels. The theory reproduces the observed dynamics quantitatively without the need to invoke any fitting parameters, phenomenological models or extrinsic effects such as disorder. We demonstrate that the dynamics are dominated by the combined effect of efficient carrier–carrier scattering, which maintains a thermalized carrier distribution, and carrier–optical–phonon scattering, which removes energy from the carrier liquid. PMID:27221060

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.

Forbidden phonon: Dynamical signature of bond symmetry breaking in the iron chalcogenides

DOE PAGES

Fobes, David M.; Zaliznyak, Igor A.; Tranquada, John M.; ...

2016-09-01

Investigation of the inelastic neutron scattering spectra in Fe 1+yTe 1₋xSe x near a signature wave vector Q=(1,0,0) for the bond-order wave (BOW) formation of parent compound Fe 1+yTe reveals an acoustic-phonon-like dispersion present in all structural phases. While a structural Bragg peak accompanies the mode in the low-temperature phase of Fe 1+yTe, it is absent in the high-temperature tetragonal phase, where Bragg scattering at this Q is forbidden by symmetry. Notably, this mode is also observed in superconducting FeTe 0.55Se 0.45, where structural and magnetic transitions are suppressed, and no BOW has been observed. Lastly, the presence of thismore » “forbidden” phonon indicates that the lattice symmetry is dynamically or locally broken by magneto-orbital BOW fluctuations, which are strongly coupled to lattice in these materials.« less

Boron arsenide phonon dispersion from inelastic x-ray scattering: Potential for ultrahigh thermal conductivity

NASA Astrophysics Data System (ADS)

Ma, Hao; Li, Chen; Tang, Shixiong; Yan, Jiaqiang; Alatas, Ahmet; Lindsay, Lucas; Sales, Brian C.; Tian, Zhiting

2016-12-01

Cubic boron arsenide (BAs) was predicted to have an exceptionally high thermal conductivity (k ) ˜2000 W m-1K-1 at room temperature, comparable to that of diamond, based on first-principles calculations. Subsequent experimental measurements, however, only obtained a k of ˜200 W m-1K-1 . To gain insight into this discrepancy, we measured phonon dispersion of single-crystal BAs along high symmetry directions using inelastic x-ray scattering and compared these with first-principles calculations. Based on the measured phonon dispersion, we have validated the theoretical prediction of a large frequency gap between acoustic and optical modes and bunching of acoustic branches, which were considered the main reasons for the predicted ultrahigh k . This supports its potential to be a super thermal conductor if very-high-quality single-crystal samples can be synthesized.

Boron arsenide phonon dispersion from inelastic x-ray scattering: Potential for ultrahigh thermal conductivity

DOE PAGES

Ma, Hao; Li, Chen; Tang, Shixiong; ...

2016-12-14

Cubic boron arsenide (BAs) was predicted to have an exceptionally high thermal conductivity (k) ~2000 Wm -1K -1 at room temperature, comparable to that of diamond, based on first-principles calculations. Subsequent experimental measurements, however, only obtained a k of ~200 Wm-1K-1. To gain insight into this discrepancy, we measured phonon dispersion of single crystal BAs along high symmetry directions using inelastic x-ray scattering (IXS) and compared these with first-principles calculations. Based on the measured phonon dispersion, we have validated the theoretical prediction of a large frequency gap between acoustic and optical modes and bunching of acoustic branches, which were consideredmore » the main reasons for the predicted ultrahigh k. This supports its potential to be a super thermal conductor if very high-quality single crystal samples can be synthesized.« less

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.

Independent control of electrical and heat conduction by nanostructure designing for Si-based thermoelectric materials

PubMed Central

Yamasaka, Shuto; Watanabe, Kentaro; Sakane, Shunya; Takeuchi, Shotaro; Sakai, Akira; Sawano, Kentarou; Nakamura, Yoshiaki

2016-01-01

The high electrical and drastically-low thermal conductivities, a vital goal for high performance thermoelectric (TE) materials, are achieved in Si-based nanoarchitecture composed of Si channel layers and epitaxial Ge nanodots (NDs) with ultrahigh areal density (~1012 cm−2). In this nanoarchitecture, the ultrasmall NDs and Si channel layers play roles of phonon scattering sources and electrical conduction channels, respectively. Electron conductivity in n-type nanoacrhitecture shows high values comparable to those of epitaxial Si films despite the existence of epitaxial NDs. This is because Ge NDs mainly scattered not electrons but phonons selectively, which could be attributed to the small conduction band offset at the epitaxially-grown Si/Ge interface and high transmission probability through stacking faults. These results demonstrate an independent control of thermal and electrical conduction for phonon-glass electron-crystal TE materials by nanostructure designing and the energetic and structural interface control. PMID:26973092

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.

Nuclear resonant inelastic X-ray scattering at high pressure and low temperature

DOE PAGES

Bi, Wenli; Zhao, Jiyong; Lin, Jung -Fu; ...

2015-01-01

In this study, a new synchrotron radiation experimental capability of coupling nuclear resonant inelastic X-ray scattering with the cryogenically cooled high-pressure diamond anvil cell technique is presented. The new technique permits measurements of phonon density of states at low temperature and high pressure simultaneously, and can be applied to studies of phonon contribution to pressure- and temperature-induced magnetic, superconducting and metal–insulator transitions in resonant isotope-bearing materials. In this report, a pnictide sample, EuFe 2As 2, is used as an example to demonstrate this new capability at beamline 3-ID of the Advanced Photon Source, Argonne National Laboratory. A detailed description ofmore » the technical development is given. The Fe-specific phonon density of states and magnetism from the Fe sublattice in Eu 57Fe 2As 2 at high pressure and low temperature were derived by using this new capability.« less

Thermal Conductivity of Wurtzite Zinc-Oxide from First-Principles Lattice Dynamics - a Comparative Study with Gallium Nitride

NASA Astrophysics Data System (ADS)

Wu, Xufei; Lee, Jonghoon; Varshney, Vikas; Wohlwend, Jennifer L.; Roy, Ajit K.; Luo, Tengfei

2016-03-01

Wurtzite Zinc-Oxide (w-ZnO) is a wide bandgap semiconductor that holds promise in power electronics applications, where heat dissipation is of critical importance. However, large discrepancies exist in the literature on the thermal conductivity of w-ZnO. In this paper, we determine the thermal conductivity of w-ZnO using first-principles lattice dynamics and compare it to that of wurtzite Gallium-Nitride (w-GaN) - another important wide bandgap semiconductor with the same crystal structure and similar atomic masses as w-ZnO. However, the thermal conductivity values show large differences (400 W/mK of w-GaN vs. 50 W/mK of w-ZnO at room temperature). It is found that the much lower thermal conductivity of ZnO originates from the smaller phonon group velocities, larger three-phonon scattering phase space and larger anharmonicity. Compared to w-GaN, w-ZnO has a smaller frequency gap in phonon dispersion, which is responsible for the stronger anharmonic phonon scattering, and the weaker interatomic bonds in w-ZnO leads to smaller phonon group velocities. The thermal conductivity of w-ZnO also shows strong size effect with nano-sized grains or structures. The results from this work help identify the cause of large discrepancies in w-ZnO thermal conductivity and will provide in-depth understanding of phonon dynamics for the design of w-ZnO-based electronics.

Thermal Conductivity of Wurtzite Zinc-Oxide from First-Principles Lattice Dynamics – a Comparative Study with Gallium Nitride

PubMed Central

Wu, Xufei; Lee, Jonghoon; Varshney, Vikas; Wohlwend, Jennifer L.; Roy, Ajit K.; Luo, Tengfei

2016-01-01

Wurtzite Zinc-Oxide (w-ZnO) is a wide bandgap semiconductor that holds promise in power electronics applications, where heat dissipation is of critical importance. However, large discrepancies exist in the literature on the thermal conductivity of w-ZnO. In this paper, we determine the thermal conductivity of w-ZnO using first-principles lattice dynamics and compare it to that of wurtzite Gallium-Nitride (w-GaN) – another important wide bandgap semiconductor with the same crystal structure and similar atomic masses as w-ZnO. However, the thermal conductivity values show large differences (400 W/mK of w-GaN vs. 50 W/mK of w-ZnO at room temperature). It is found that the much lower thermal conductivity of ZnO originates from the smaller phonon group velocities, larger three-phonon scattering phase space and larger anharmonicity. Compared to w-GaN, w-ZnO has a smaller frequency gap in phonon dispersion, which is responsible for the stronger anharmonic phonon scattering, and the weaker interatomic bonds in w-ZnO leads to smaller phonon group velocities. The thermal conductivity of w-ZnO also shows strong size effect with nano-sized grains or structures. The results from this work help identify the cause of large discrepancies in w-ZnO thermal conductivity and will provide in-depth understanding of phonon dynamics for the design of w-ZnO-based electronics. PMID:26928396

Effect of small scattering centers on the thermoelectric properties of p-type SiGe alloys

NASA Technical Reports Server (NTRS)

Beaty, John S.; Rolfe, Jonathan L.; Vandersande, Jan W.

1991-01-01

Theory predicts that the addition of ultra-fine, inert, phonon-scattering centers to thermoelectric materials will reduce their thermal conductivity. To investigate this prediction, ultrafine particulates (20 to 120 A) of silicon nitride have been added to boron-doped, p-type, 80/20 SiGe. All of the SiGe samples produced from ultrafine powder have lower thermal conductivities than standard SiGe, but high-temperature heat treatment increases the thermal conductivity back to the value for standard SiGe. However, the SiGe samples with silicon nitride, inert, phonon-scattering centers retained the lower thermal conductivity after several heat treatments. A reduction of approximately 25 percent in thermal conductivity has been achieved in these samples. The magnitude of the reduction agrees with theoretical predictions.

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.

Thermal conductivity of III-V semiconductor superlattices

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

Mei, S., E-mail: song.mei@wisc.edu; Knezevic, I., E-mail: irena.knezevic@wisc.edu

2015-11-07

This paper presents a semiclassical model for the anisotropic thermal transport in III-V semiconductor superlattices (SLs). An effective interface rms roughness is the only adjustable parameter. Thermal transport inside a layer is described by the Boltzmann transport equation in the relaxation time approximation and is affected by the relevant scattering mechanisms (three-phonon, mass-difference, and dopant and electron scattering of phonons), as well as by diffuse scattering from the interfaces captured via an effective interface scattering rate. The in-plane thermal conductivity is obtained from the layer conductivities connected in parallel. The cross-plane thermal conductivity is calculated from the layer thermal conductivitiesmore » in series with one another and with thermal boundary resistances (TBRs) associated with each interface; the TBRs dominate cross-plane transport. The TBR of each interface is calculated from the transmission coefficient obtained by interpolating between the acoustic mismatch model (AMM) and the diffuse mismatch model (DMM), where the weight of the AMM transmission coefficient is the same wavelength-dependent specularity parameter related to the effective interface rms roughness that is commonly used to describe diffuse interface scattering. The model is applied to multiple III-arsenide superlattices, and the results are in very good agreement with experimental findings. The method is both simple and accurate, easy to implement, and applicable to complicated SL systems, such as the active regions of quantum cascade lasers. It is also valid for other SL material systems with high-quality interfaces and predominantly incoherent phonon transport.« less

Quantum transport properties of carbon nanotube field-effect transistors with electron-phonon coupling

NASA Astrophysics Data System (ADS)

Ishii, Hiroyuki; Kobayashi, Nobuhiko; Hirose, Kenji

2007-11-01

We investigated the electron-phonon coupling effects on the electronic transport properties of metallic (5,5)- and semiconducting (10,0)-carbon nanotube devices. We calculated the conductance and mobility of the carbon nanotubes with micron-order lengths at room temperature, using the time-dependent wave-packet approach based on the Kubo-Greenwood formula within a tight-binding approximation. We investigated the scattering effects of both longitudinal acoustic and optical phonon modes on the transport properties. The electron-optical phonon coupling decreases the conductance around the Fermi energy for the metallic carbon nanotubes, while the conductance of semiconductor nanotubes is decreased around the band edges by the acoustic phonons. Furthermore, we studied the Schottky-barrier effects on the mobility of the semiconducting carbon nanotube field-effect transistors for various gate voltages. We clarified how the electron mobilities of the devices are changed by the acoustic phonon.

Pressure dependence of transverse acoustic phonon energy in ferropericlase across the spin transition.

PubMed

Fukui, Hiroshi; Baron, Alfred Q R; Ishikawa, Daisuke; Uchiyama, Hiroshi; Ohishi, Yasuo; Tsuchiya, Taku; Kobayashi, Hisao; Matsuzaki, Takuya; Yoshino, Takashi; Katsura, Tomoo

2017-06-21

We investigated transverse acoustic (TA) phonons in iron-bearing magnesium oxide (ferropericlase) up to 56 GPa using inelastic x-ray scattering (IXS). The results show that the energy of the TA phonon far from the Brillouin zone center suddenly increases with increasing pressure above the spin transition pressure of ferropericlase. Ab initio calculations revealed that the TA phonon energy far from the Brillouin zone center is higher in the low-spin state than in the high spin state; that the TA phonon energy depend weakly on pressure; and that the energy gap between the TA and the lowest-energy-optic phonons is much narrower in the low-spin state than in the high-spin state. This allows us to conclude that the anomalous behavior of the TA mode in the present experiments is the result of gap narrowing due to the spin transition and explains contradictory results in previous experimental studies.

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

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

Ling, Meng-Chieh

Graphene, a two-dimensional (2D) honeycomb structure allotrope of carbon atoms, has a long history since the invention of the pencil [Petroski (1989)] and the linear dispersion band structure proposed by Wallace [Wal]; however, only after Novoselov et al. successively isolated graphene from graphite [Novoselov et al. (2004)], it has been studied intensively during the recent years. It draws so much attentions not only because of its potential application in future electronic devices but also because of its fundamental properties: its quasiparticles are governed by the two-dimensional Dirac equation, and exhibit a variety of phenomena such as the anomalous integer quantummore » Hall effect (IQHE) [Novoselov et al. (2005)] measured experimentally, a minimal conductivity at vanishing carrier concentration [Neto et al. (2009)], Kondo effect with magnetic element doping [Hentschel and Guinea (2007)], Klein tunneling in p-n junctions [Cheianov and Fal’ko (2006), Beenakker (2008)], Zitterbewegung [Katsnelson (2006)], and Schwinger pair production [Schwinger (1951); Dora and Moessner (2010)]. Although both electron-phonon coupling and photoconductivity in graphene also draws great attention [Yan et al. (2007); Satou et al. (2008); Hwang and Sarma (2008); Vasko and Ryzhii (2008); Mishchenko (2009)], the nonequilibrium behavior based on the combination of electronphonon coupling and Schwinger pair production is an intrinsic graphene property that has not been investigated. Our motivation for studying clean graphene at low temperature is based on the following effect: for a fixed electric field, below a sufficiently low temperature linear eletric transport breaks down and nonlinear transport dominates. The criteria of the strength of this field [Fritz et al. (2008)] is eE = T2/~vF (1.1) For T >√eE~vF the system is in linear transport regime while for T <√eE~vF the system is in nonlinear transport regime. From the scaling’s point of view, at the nonlinear transport regime the temperature T and electric field E are also related. In this thesis we show that the nontrivial electron distribution function can be associated with an effective temperature T which exhibits a dependence on electric field E and electron-phonon coupling g: T ∝ E1/4g(1.2) The anamolous exponent 1/4 may obtained from scaling. Meanwhile, yet we cannot obtain the distribution function, however, argument based on scaling gives us the current dependence on electric field: J ∝√Eg2 (1.3) which is a very different result compared with the results in which electrons do not experience scattering. This result provides us with important insighht into the correct nonequilibrium distribution function because now we know what the electric field dependence of current must be. Due to the applied field, the electronic system produces heat which prevents us from reaching a steady state. In order to remove Joule heat, we imagine that we have a graphene flake attached to a semiconductor substrate. Joule heat either transport to its environment or to the substrate as shown in 1.1. The red lines represent heat current flowing from high temperature sample to the low temperature reservoir. However, for a very large system, the temperature gradient is 0 in the plane so heat cannot be conducted outside in the horizontal direction, while the energy gap in semiconductor also forbids electron current from flowing into the substrate. But for phonon thermal current, the temperature gradient is large in the vertical direction, so heat can be transported into the substrate via phonons. There are two possible channels of phonon degrees of freedom, acoustic phonon and optical phonon. As we can see from Fig. 1.2 [Kusminskiy et al. (2009)], since the optical phonon excitation energy is too large for a low temperature system, it is note likely to be excited by the nonlinear electric field, so the possible way left is by electron-acoustic phonon scattering. Here acoustic phonon acts as a heat bath to absorb the Joule heat created by pair production process. Hence the scattering process is determined by electron-acoustic phonon interaction which will be introduced in section 3.3.« less

Coupled spin and electron-phonon interaction at the Tl/Si(111) surface from relativistic first-principles calculations

NASA Astrophysics Data System (ADS)

Garcia-Goiricelaya, Peio; Gurtubay, Idoia G.; Eiguren, Asier

2018-05-01

We investigate the role played by the electron spin and the spin-orbit interaction in the exceptional electron-phonon coupling at the Tl/Si(111) surface. Our first-principles calculations demonstrate that the particular spin pattern of this system dominates the whole low-energy electron-phonon physics, which is remarkably explained by forbidden spin-spin scattering channels. In particular, we show that the strength of the electron-phonon coupling appears drastically weakened for surface states close to the K ¯ and K'¯ valleys, which is unambiguously attributed to the spin polarization through the associated modulation due to the spinor overlaps. However, close to the Γ ¯ point, the particular spin pattern in this area is less effective in damping the electron-phonon matrix elements, and the result is an exceptional strength of the electron-phonon coupling parameter λ ˜1.4 . These results are rationalized by a simple model for the electron-phonon matrix elements including the spinor terms.

Hydrodynamic phonon drift and second sound in a (20,20) single-wall carbon nanotube

NASA Astrophysics Data System (ADS)

Lee, Sangyeop; Lindsay, Lucas

2017-05-01

Two hydrodynamic features of phonon transport, phonon drift and second sound, in a (20,20) single-wall carbon nanotube (SWCNT) are discussed using lattice dynamics calculations employing an optimized Tersoff potential for atomic interactions. We formally derive a formula for the contribution of drift motion of phonons to total heat flux at steady state. It is found that the drift motion of phonons carries more than 70 % and 90 % of heat at 300 and 100 K, respectively, indicating that phonon flow can be reasonably approximated as hydrodynamic if the SWCNT is long enough to avoid ballistic phonon transport. The dispersion relation of second sound is derived from the Peierls-Boltzmann transport equation with Callaway's scattering model and quantifies the speed of second sound and its relaxation. The speed of second sound is around 4000 m/s in a (20,20) SWCNT and the second sound can propagate more than 10 µm in an isotopically pure (20,20) SWCNT for frequency around 1 GHz at 100 K.

Laser cooling and control of excitations in superfluid helium

NASA Astrophysics Data System (ADS)

Harris, G. I.; McAuslan, D. L.; Sheridan, E.; Sachkou, Y.; Baker, C.; Bowen, W. P.

2016-08-01

Superfluidity is a quantum state of matter that exists macroscopically in helium at low temperatures. The elementary excitations in superfluid helium have been probed with great success using techniques such as neutron and light scattering. However, measurements of phonon excitations have so far been limited to average thermodynamic properties or the driven response far out of thermal equilibrium. Here, we use cavity optomechanics to probe the thermodynamics of phonon excitations in real time. Furthermore, strong light-matter interactions allow both laser cooling and amplification. This represents a new tool to observe and control superfluid excitations that may provide insight into phonon-phonon interactions, quantized vortices and two-dimensional phenomena such as the Berezinskii-Kosterlitz-Thouless transition. The third sound modes studied here also offer a pathway towards quantum optomechanics with thin superfluid films, including the prospect of femtogram masses, high mechanical quality factors, strong phonon-phonon and phonon-vortex interactions, and self-assembly into complex geometries with sub-nanometre feature size.

Electron-phonon coupling and superconductivity in the (4/3)-monolayer of Pb on Si(111): Role of spin-orbit interaction

NASA Astrophysics Data System (ADS)

Sklyadneva, I. Yu.; Heid, R.; Bohnen, K.-P.; Echenique, P. M.; Chulkov, E. V.

2018-05-01

The effect of spin-orbit coupling on the electron-phonon interaction in a (4/3)-monolayer of Pb on Si(111) is investigated within the density-functional theory and linear-response approach in the mixed-basis pseudopotential representation. We show that the spin-orbit interaction produces a large weakening of the electron-phonon coupling strength, which appears to be strongly overestimated in the scalar relativistic calculations. The effect of spin-orbit interaction is largely determined by the induced modification of Pb electronic bands and a stiffening of the low-energy part of phonon spectrum, which favor a weakening of the electron-phonon coupling strength. The state-dependent strength of the electron-phonon interaction in occupied Pb electronic bands varies depending on binding energy rather than electronic momentum. It is markedly larger than the value averaged over electron momentum because substrate electronic bands make a small contribution to the phonon-mediated scattering and agrees well with the experimental data.

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

Kuleyev, I. G., E-mail: kuleev@imp.uran.ru; Kuleyev, I. I.; Bakharev, S. M.

We study the effect of anisotropy in elastic properties on the electron–phonon drag and thermoelectric phenomena in gapless semiconductors with degenerate charge-carrier statistics. It is shown that phonon focusing leads to a number of new effects in the drag thermopower at low temperatures, when diffusive phonon scattering from the boundaries is the predominant relaxation mechanism. We analyze the effect of phonon focusing on the dependences of the thermoelectromotive force (thermopower) in HgSe:Fe crystals on geometric parameters and the heat-flow directions relative to the crystal axes in the Knudsen regime of the phonon gas flow. The crystallographic directions that ensure themore » maximum and minimum values of the thermopower are determined and the role of quasi-longitudinal and quasi-transverse phonons in the drag thermopower in HgSe:Fe crystals at low temperatures is analyzed. It is shown that the main contribution to the drag thermopower comes from slow quasi-transverse phonons in the directions of focusing in long samples.« less

Magnetic moments induce strong phonon renormalization in FeSi.

PubMed

Krannich, S; Sidis, Y; Lamago, D; Heid, R; Mignot, J-M; Löhneysen, H v; Ivanov, A; Steffens, P; Keller, T; Wang, L; Goering, E; Weber, F

2015-11-27

The interactions of electronic, spin and lattice degrees of freedom in solids result in complex phase diagrams, new emergent phenomena and technical applications. While electron-phonon coupling is well understood, and interactions between spin and electronic excitations are intensely investigated, only little is known about the dynamic interactions between spin and lattice excitations. Noncentrosymmetric FeSi is known to undergo with increasing temperature a crossover from insulating to metallic behaviour with concomitant magnetic fluctuations, and exhibits strongly temperature-dependent phonon energies. Here we show by detailed inelastic neutron-scattering measurements and ab initio calculations that the phonon renormalization in FeSi is linked to its unconventional magnetic properties. Electronic states mediating conventional electron-phonon coupling are only activated in the presence of strong magnetic fluctuations. Furthermore, phonons entailing strongly varying Fe-Fe distances are damped via dynamic coupling to the temperature-induced magnetic moments, highlighting FeSi as a material with direct spin-phonon coupling and multiple interaction paths.

Acoustic scattering from phononic crystals with complex geometry.

PubMed

Kulpe, Jason A; Sabra, Karim G; Leamy, Michael J

2016-05-01

This work introduces a formalism for computing external acoustic scattering from phononic crystals (PCs) with arbitrary exterior shape using a Bloch wave expansion technique coupled with the Helmholtz-Kirchhoff integral (HKI). Similar to a Kirchhoff approximation, a geometrically complex PC's surface is broken into a set of facets in which the scattering from each facet is calculated as if it was a semi-infinite plane interface in the short wavelength limit. When excited by incident radiation, these facets introduce wave modes into the interior of the PC. Incorporation of these modes in the HKI, summed over all facets, then determines the externally scattered acoustic field. In particular, for frequencies in a complete bandgap (the usual operating frequency regime of many PC-based devices and the requisite operating regime of the presented theory), no need exists to solve for internal reflections from oppositely facing edges and, thus, the total scattered field can be computed without the need to consider internal multiple scattering. Several numerical examples are provided to verify the presented approach. Both harmonic and transient results are considered for spherical and bean-shaped PCs, each containing over 100 000 inclusions. This facet formalism is validated by comparison to an existing self-consistent scattering technique.

Scatterings and Quantum Effects in (Al ,In )N /GaN Heterostructures for High-Power and High-Frequency Electronics

NASA Astrophysics Data System (ADS)

Wang, Leizhi; Yin, Ming; Khan, Asif; Muhtadi, Sakib; Asif, Fatima; Choi, Eun Sang; Datta, Timir

2018-02-01

Charge transport in the wide-band-gap (Al ,In )N /GaN heterostructures with high carrier density approximately 2 ×1013 cm-2 is investigated over a large range of temperature (270 mK ≤T ≤280 K ) and magnetic field (0 ≤B ≤18 T ). We observe the first evidence of weak localization in the two-dimensional electron gas in this system. From the Shubnikov-de Haas (SdH) oscillations a relatively light effective mass of 0.23 me is determined. Furthermore, the linear dependence with temperature (T <20 K ) of the inelastic scattering rate (τi-1∝T ) is attributed to the phase breaking by electron-electron scattering. Also in the same temperature range the less-than unit ratio of quantum lifetime to Hall transport time (τq/τt<1 ) is taken to signify the dominance of small-angle scattering. Above 20 K, with increasing temperature scattering changes from acoustic phonon to optical phonon scattering, resulting in a rapid decrease in carrier mobility and increase in sheet resistance. Suppression of such scatterings will lead to higher mobility and a way forward to high-power and high-frequency electronics.

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.

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.

Microscale heat transfer in fusion welding of glass by ultra-short pulse laser using dual phase lag effects

NASA Astrophysics Data System (ADS)

Bag, Swarup

2018-04-01

The heat transfer in microscale has very different physical basis than macroscale where energy transport depends on collisions among energy carriers (electron and phonon), mean free path for the lattice (~ 10 – 100 nm) and mean free time between energy carriers. The heat transport is described on the basis of different types of energy carriers averaging over the grain scale in space and collations between them in time scale. The physical bases of heat transfer are developed by phonon-electron interaction for metals and alloys and phonon scattering for insulators and dielectrics. The non-Fourier effects in heating become more and more predominant as the duration of heating pulse becomes extremely small that is comparable with mean free time of the energy carriers. The mean free time for electron – phonon and phonon-phonon interaction is of the order of 1 and 10 picoseconds, respectively. In the present study, the mathematical formulation of the problem is defined considering dual phase lag i.e. two relaxation times in heat transport assuming a volumetric heat generation for ultra-short pulse laser interaction with dielectrics. The relaxation times are estimated based on phonon scattering model. A three dimensional finite element model is developed to find transient temperature distribution using quadruple ellipsoidal heat source model. The analysis is performed for single and multiple pulses to generate the time temperature history at different location and at different instant of time. The simulated results are validated with experiments reported in independent literature. The effect of two relaxation times and pulse width on the temperature profile is studied through numerical simulation.

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

Non-equilibrium Green's function calculation for GaN-based terahertz-quantum cascade laser structures

NASA Astrophysics Data System (ADS)

Yasuda, H.; Kubis, T.; Hosako, I.; Hirakawa, K.

2012-04-01

We theoretically investigated GaN-based resonant phonon terahertz-quantum cascade laser (QCL) structures for possible high-temperature operation by using the non-equilibrium Green's function method. It was found that the GaN-based THz-QCL structures do not necessarily have a gain sufficient for lasing, even though the thermal backfilling and the thermally activated phonon scattering are effectively suppressed. The main reason for this is the broadening of the subband levels caused by a very strong interaction between electrons and longitudinal optical (LO) phonons in GaN.

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.

Dynamical Cooper pairing in nonequilibrium electron-phonon systems

DOE PAGES

Knap, Michael; Babadi, Mehrtash; Refael, Gil; ...

2016-12-08

In this paper, we analyze Cooper pairing instabilities in strongly driven electron-phonon systems. The light-induced nonequilibrium state of phonons results in a simultaneous increase of the superconducting coupling constant and the electron scattering. We demonstrate that the competition between these effects leads to an enhanced superconducting transition temperature in a broad range of parameters. Finally, our results may explain the observed transient enhancement of superconductivity in several classes of materials upon irradiation with high intensity pulses of terahertz light, and may pave new ways for engineering high-temperature light-induced superconducting states.

Simulation of optically pumped intersubband laser in magnetic field

NASA Astrophysics Data System (ADS)

Erić, Marko; Milanović, Vitomir; Ikonić, Zoran; Indjin, Dragan

2007-06-01

Simulations of an optically pumped intersubband laser in magnetic field up to 60 T are performed within the steady-state rate equations model. The electron-polar optical phonon scattering is calculated using the confined and interface phonon model. A strong oscillatory optical gain vs. magnetic field dependence is found, with two dominant gain peaks occurring at 20 and 40 T, the fields which bring appropriate states into resonance with optical phonons and thus open additional relaxation paths. The peak at 20 T exceeds the value of gain achieved at zero field.

Lattice and magnetic dynamics in perovskite Y1 -xLaxTiO3

NASA Astrophysics Data System (ADS)

Li, Bing; Louca, Despina; Niedziela, Jennifer; Li, Zongyao; Zhang, Libin; Zhou, Jianshi; Goodenough, John B.

2016-12-01

Inelastic neutron scattering combined with the dynamic pair density function (DPDF) analysis were used to investigate the magnetic and lattice dynamics in the orbitally active Y1 -xLaxTiO3 as it crosses the antiferromagnetic (AFM) to ferromagnetic (FM) phase boundary. Upon doping, the FM state present in YTiO3 is suppressed on approaching a critical concentration of xc˜0.3 in which TC≃0 , and is replaced by the AFM phase of LaTiO3. Below xc, magnetic scattering from spin waves is dominant at low energies. At xc with a TC≃0 , magnetic scattering is also observed and is most likely due to AFM fluctuations. At the same time, local atomic fluctuations extending to 50 meV are observed above and below the magnetic transitions from 0 ≤x ≤1 that show distinct characteristics with x . From Y to La, a clear difference is observed in the phonon density of states as a function of doping as well. At x =0.15 and 0.3, low-energy modes involving predominantly the rare-earth ion become suppressed with increasing temperature, while in x =1 , strong suppression of phonon modes across a wide range in energy is observed above TN. It is likely that in the Y heavy samples, phonon modes below 20 meV have a stronger influence on the orbital excitations, while in LaTiO3, a strong phonon dependence is observed upon cooling up to TN.

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

Modeling inelastic phonon scattering in atomic- and molecular-wire junctions

NASA Astrophysics Data System (ADS)

Paulsson, Magnus; Frederiksen, Thomas; Brandbyge, Mads

2005-11-01

Computationally inexpensive approximations describing electron-phonon scattering in molecular-scale conductors are derived from the nonequilibrium Green’s function method. The accuracy is demonstrated with a first-principles calculation on an atomic gold wire. Quantitative agreement between the full nonequilibrium Green’s function calculation and the newly derived expressions is obtained while simplifying the computational burden by several orders of magnitude. In addition, analytical models provide intuitive understanding of the conductance including nonequilibrium heating and provide a convenient way of parameterizing the physics. This is exemplified by fitting the expressions to the experimentally observed conductances through both an atomic gold wire and a hydrogen molecule.

Observation of soft phonon mode in TbFe 3 ( BO 3 ) 4 by inelastic neutron scattering

DOE PAGES

Pavlovskiy, M. S.; Shaykhutdinov, Krill A.; Wu, L. S.; ...

2018-02-28

In this study, the phonon dispersion in terbium iron borate TbFe 3(BO 3) 4 has been measured by inelastic neutron scattering in a temperature range 180S=192.5 K and studied by ab initio calculations. Significant, but not complete, softening of the transverse acoustic (TA) branch has been observed at the corner of the Brillouin zone (Λ point) at temperatures T≳T S, in full agreement with theoretical calculations. Finally, the TA soft mode undergoes considerable broadening at the Λ point near the transition temperature that can be attributed to the anharmonic interference between transverse acoustic and optical modes.

Influence of trap-assisted tunneling on trap-assisted tunneling current in double gate tunnel field-effect transistor

NASA Astrophysics Data System (ADS)

Zhi, Jiang; Yi-Qi, Zhuang; Cong, Li; Ping, Wang; Yu-Qi, Liu

2016-02-01

Trap-assisted tunneling (TAT) has attracted more and more attention, because it seriously affects the sub-threshold characteristic of tunnel field-effect transistor (TFET). In this paper, we assess subthreshold performance of double gate TFET (DG-TFET) through a band-to-band tunneling (BTBT) model, including phonon-assisted scattering and acoustic surface phonons scattering. Interface state density profile (Dit) and the trap level are included in the simulation to analyze their effects on TAT current and the mechanism of gate leakage current. Project supported by the National Natural Science Foundation of China (Grant Nos. 61574109 and 61204092).

Observation of soft phonon mode in TbFe 3 ( BO 3 ) 4 by inelastic neutron scattering

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

Pavlovskiy, M. S.; Shaykhutdinov, Krill A.; Wu, L. S.

In this study, the phonon dispersion in terbium iron borate TbFe 3(BO 3) 4 has been measured by inelastic neutron scattering in a temperature range 180S=192.5 K and studied by ab initio calculations. Significant, but not complete, softening of the transverse acoustic (TA) branch has been observed at the corner of the Brillouin zone (Λ point) at temperatures T≳T S, in full agreement with theoretical calculations. Finally, the TA soft mode undergoes considerable broadening at the Λ point near the transition temperature that can be attributed to the anharmonic interference between transverse acoustic and optical modes.

Phonon focusing and temperature dependences of thermal conductivity of silicon nanofilms

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

Kuleyev, I. I., E-mail: kuleev@imp.uran.ru; Bakharev, S. M.; Kuleyev, I. G.

2015-04-15

The effect of phonon focusing on the anisotropy and temperature dependences of the thermal conductivities of silicon nanofilms is analyzed using the three-mode Callaway model. The orientations of the film planes and the directions of the heat flux for maximal or minimal heat removal from silicon chip elements at low temperatures, as well as at room temperature, are determined. It is shown that in the case of diffuse reflection of phonons from the boundaries, the plane with the (100) orientation exhibits the lowest scattering ability (and the highest thermal conductivity), while the plane with the (111) orientation is characterized bymore » the highest scattering ability (and the lowest thermal conductivity). The thermal conductivity of wide films is determined to a considerable extent by the orientation of the film plane, while for nanowires with a square cross section, the thermal conductivity is mainly determined by the direction of the heat flux. The effect of elastic energy anisotropy on the dependences of the thermal conductivity on the geometrical parameters of films is analyzed. The temperatures of transition from boundary scattering to bulk relaxation mechanisms are determined.« less

Plasmons in graphene nanoribbons

DOE PAGES

Karimi, F.; Knezevic, I.

2017-09-12

We calculate the dielectric function and plasmonic response of armchair (aGNRs) and zigzag (zGNRs) graphene nanoribbons using the self-consistent-field approach within the Markovian master equation formalism (SCF-MMEF). We accurately account for electron scattering with phonons, ionized impurities, and line-edge roughness and show that electron scattering with surface optical phonons is much more prominent in GNRs than in graphene. We calculate the loss function, plasmon dispersion, and the plasmon propagation length in supported GNRs. Midinfrared plasmons in supported (3N+2)-aGNRs can propagate as far as several microns at room temperature, with 4–5-nm-wide ribbons having the longest propagation length. In other types ofmore » aGNRs and in zGNRs, the plasmon propagation length seldom exceeds 100 nm. Plasmon propagation lengths are much longer on nonpolar (e.g., diamondlike carbon) than on polar substrates (e.g., SiO 2 or hBN), where electrons scatter strongly with surface optical phonons. In conclusion, we also show that the aGNR plasmon density is nearly uniform across the ribbon, while in zGNRs, because of the highly localized edge states, plasmons of different spin polarization are accumulated near the opposite edges.« less

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

Jeon, Byung-Gu; Koteswararao, B.; Park, C. B.

Thermal transport of quantum magnets has elucidated the nature of low energy elementary excitations and complex interplay between those excited states via strong scattering of thermal carriers. BiCu 2PO 6 is a unique frustrated spin-ladder compound exhibiting highly anisotropic spin excitations that contain both itinerant and localized dispersion characters along the b- and a-axes respectively. Here, we investigate thermal conductivity κ of BiCu 2PO 6 under high magnetic fields (H) of up to 30 tesla. A dip-feature in κ, located at ~15K at zero-H along all crystallographic directions, moves gradually toward lower temperature (T) with increasing H, thus resulting inmore » giant suppression by a factor of ~30 near the critical magnetic field of H c≅23.5 tesla. The giant H- and T-dependent suppression of κ can be explained by the combined result of resonant scattering of phononic heat carriers with magnetic energy levels and increased phonon scattering due to enhanced spin fluctuation at H c, unequivocally revealing the existence of strong spin-phonon coupling. Moreover, we find an experimental indication that the remaining magnetic heat transport along the b-axis becomes almost gapless at the magnetic quantum critical point realized at H c.« less

Ultra-low Thermal Conductivity in Si/Ge Hierarchical Superlattice Nanowire.

PubMed

Mu, Xin; Wang, Lili; Yang, Xueming; Zhang, Pu; To, Albert C; Luo, Tengfei

2015-11-16

Due to interfacial phonon scattering and nanoscale size effect, silicon/germanium (Si/Ge) superlattice nanowire (SNW) can have very low thermal conductivity, which is very attractive for thermoelectrics. In this paper, we demonstrate using molecular dynamics simulations that the already low thermal conductivity of Si/Ge SNW can be further reduced by introducing hierarchical structure to form Si/Ge hierarchical superlattice nanowire (H-SNW). The structural hierarchy introduces defects to disrupt the periodicity of regular SNW and scatters coherent phonons, which are the key contributors to thermal transport in regular SNW. Our simulation results show that periodically arranged defects in Si/Ge H-SNW lead to a ~38% reduction of the already low thermal conductivity of regular Si/Ge SNW. By randomizing the arrangement of defects and imposing additional surface complexities to enhance phonon scattering, further reduction in thermal conductivity can be achieved. Compared to pure Si nanowire, the thermal conductivity reduction of Si/Ge H-SNW can be as large as ~95%. It is concluded that the hierarchical structuring is an effective way of reducing thermal conductivity significantly in SNW, which can be a promising path for improving the efficiency of Si/Ge-based SNW thermoelectrics.

Ultra-low Thermal Conductivity in Si/Ge Hierarchical Superlattice Nanowire

PubMed Central

Mu, Xin; Wang, Lili; Yang, Xueming; Zhang, Pu; To, Albert C.; Luo, Tengfei

2015-01-01

Due to interfacial phonon scattering and nanoscale size effect, silicon/germanium (Si/Ge) superlattice nanowire (SNW) can have very low thermal conductivity, which is very attractive for thermoelectrics. In this paper, we demonstrate using molecular dynamics simulations that the already low thermal conductivity of Si/Ge SNW can be further reduced by introducing hierarchical structure to form Si/Ge hierarchical superlattice nanowire (H-SNW). The structural hierarchy introduces defects to disrupt the periodicity of regular SNW and scatters coherent phonons, which are the key contributors to thermal transport in regular SNW. Our simulation results show that periodically arranged defects in Si/Ge H-SNW lead to a ~38% reduction of the already low thermal conductivity of regular Si/Ge SNW. By randomizing the arrangement of defects and imposing additional surface complexities to enhance phonon scattering, further reduction in thermal conductivity can be achieved. Compared to pure Si nanowire, the thermal conductivity reduction of Si/Ge H-SNW can be as large as ~95%. It is concluded that the hierarchical structuring is an effective way of reducing thermal conductivity significantly in SNW, which can be a promising path for improving the efficiency of Si/Ge-based SNW thermoelectrics. PMID:26568511

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

Chen, S. L., E-mail: shuch@ist.hokudai.ac.jp; Takayama, J.; Murayama, A.

Time-resolved optical spin orientation spectroscopy was employed to investigate the temperature-dependent electron spin injection in In{sub 0.1}Ga{sub 0.9}As quantum well (QW) and In{sub 0.5}Ga{sub 0.5}As quantum dots (QDs) tunnel-coupled nanostructures with 4, 6, and 8 nm-thick GaAs barriers. The fast picosecond-ranged spin injection from QW to QD excited states (ES) was observed to speed up with temperature, as induced by pronounced longitudinal-optical (LO)-phonon-involved multiple scattering process, which contributes to a thermally stable and almost fully spin-conserving injection within 5–180 K. The LO-phonon coupling was also found to cause accelerated electron spin relaxation of QD ES at elevated temperature, mainly via hyperfine interactionmore » with random nuclear field.« less

Nonequilibrium Langevin approach to quantum optics in semiconductor microcavities

NASA Astrophysics Data System (ADS)

Portolan, S.; di Stefano, O.; Savasta, S.; Rossi, F.; Girlanda, R.

2008-01-01

Recently, the possibility of generating nonclassical polariton states by means of parametric scattering has been demonstrated. Excitonic polaritons propagate in a complex interacting environment and contain real electronic excitations subject to scattering events and noise affecting quantum coherence and entanglement. Here, we present a general theoretical framework for the realistic investigation of polariton quantum correlations in the presence of coherent and incoherent interaction processes. The proposed theoretical approach is based on the nonequilibrium quantum Langevin approach for open systems applied to interacting-electron complexes described within the dynamics controlled truncation scheme. It provides an easy recipe to calculate multitime correlation functions which are key quantities in quantum optics. As a first application, we analyze the buildup of polariton parametric emission in semiconductor microcavities including the influence of noise originating from phonon-induced scattering.

Thermal and thermoelectric transport in nanoscale systems

NASA Astrophysics Data System (ADS)

Murphy, Padraig Gerard

This thesis deals with transport in molecular junctions and nanowires. We show that a molecular junction can give large values of the thermoelectric figure of merit ZT, and so could be used as a solid state energy conversion device that operates close to the Carnot efficiency. The mechanism is similar to the Mahan-Sofo model for bulk thermoelectrics---the Lorenz ratio goes to zero, violating the Wiedemann-Franz law, while the thermopower remains non-zero. The molecular state through which charge is transported must be weakly coupled to the leads, and the energy level of the state must be of order kBT away from the Fermi energy of the leads. In practice, the figure of merit is limited by the phonon thermal conductance; we show that the largest possible ZT-G˜ph th-1/2 , where G˜phth is the phonon thermal conductance divided by the thermal conductance quantum. The thermal conductance by phonons of a quasi-one-dimensional solid with isotope or defect scattering is studied using the Landauer formalism for thermal transport. A scalable numerical transfer-matrix technique is developed and applied to model quasi-one-dimensional systems in order to confirm simple analytic predictions. We argue that existing thermal conductivity data on semiconductor nanowires, showing an unexpected linear temperature dependence, can be understood through a model that combines incoherent surface scattering for short-wavelength phonons with nearly ballistic long-wavelength phonons.

Diffusive charge transport in graphene on SiO 2

NASA Astrophysics Data System (ADS)

Chen, J.-H.; Jang, C.; Ishigami, M.; Xiao, S.; Cullen, W. G.; Williams, E. D.; Fuhrer, M. S.

2009-07-01

We review our recent work on the physical mechanisms limiting the mobility of graphene on SiO 2. We have used intentional addition of charged scattering impurities and systematic variation of the dielectric environment to differentiate the effects of charged impurities and short-range scatterers. The results show that charged impurities indeed lead to a conductivity linear in density ( σ(n)∝n) in graphene, with a scattering magnitude that agrees quantitatively with theoretical estimates; increased dielectric screening reduces the scattering from charged impurities, but increases the scattering from short-range scatterers. We evaluate the effects of the corrugations (ripples) of graphene on SiO 2 on transport by measuring the height-height correlation function. The results show that the corrugations cannot mimic long-range (charged impurity) scattering effects, and have too small an amplitude-to-wavelength ratio to significantly affect the observed mobility via short-range scattering. Temperature-dependent measurements show that longitudinal acoustic phonons in graphene produce a resistivity that is linear in temperature and independent of carrier density; at higher temperatures, polar optical phonons of the SiO 2 substrate give rise to an activated, carrier density-dependent resistivity. Together the results paint a complete picture of charge carrier transport in graphene on SiO 2 in the diffusive regime.

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.

Phonon Speed, Not Scattering, Differentiates Thermal Transport in Lead Halide Perovskites.

PubMed

Elbaz, Giselle A; Ong, Wee-Liat; Doud, Evan A; Kim, Philip; Paley, Daniel W; Roy, Xavier; Malen, Jonathan A

2017-09-13

Thermal management plays a critical role in the design of solid state materials for energy conversion. Lead halide perovskites have emerged as promising candidates for photovoltaic, thermoelectric, and optoelectronic applications, but their thermal properties are still poorly understood. Here, we report on the thermal conductivity, elastic modulus, and sound speed of a series of lead halide perovskites MAPbX 3 (X = Cl, Br, I), CsPbBr 3 , and FAPbBr 3 (MA = methylammonium, FA = formamidinium). Using frequency domain thermoreflectance, we find that the room temperature thermal conductivities of single crystal lead halide perovskites range from 0.34 to 0.73 W/m·K and scale with sound speed. These results indicate that regardless of composition, thermal transport arises from acoustic phonons having similar mean free path distributions. A modified Callaway model with Born von Karmen-based acoustic phonon dispersion predicts that at least ∼70% of thermal conductivity results from phonons having mean free paths shorter than 100 nm, regardless of whether resonant scattering is invoked. Hence, nanostructures or crystal grains with dimensions smaller than 100 nm will appreciably reduce thermal transport. These results are important design considerations to optimize future lead halide perovskite-based photovoltaic, optoelectronic, and thermoelectric devices.

Anomalous Thermal Diffusivity in Bad Metals

NASA Astrophysics Data System (ADS)

Zhang, Jiecheng; Levenson-Falk, Eli M.; Ramshaw, Brad J.; Bonn, Douglas A.; Liang, Ruixing; Hardy, Walter N.; Hartnoll, Sean A.; Kapitulnik, Aharon

Local measurements of thermal diffusivity are used to analyze the transport of heat in the bad metallic regime of several strongly correlated materials. In underdoped YBCO systems, we use the in-plane anisotropy to analyze transport in this system. Specifically, we find that the diffusivity anisotropy is comparable to reported values of the electrical resistivity anisotropy and drops sharply below the charge order transition, suggesting that both anisotropies have the same origin. We interpret our results through a strong electron-phonon scattering picture and find that both electronic and phononic contributions to the diffusivity exhibit a saturated scattering time of ℏ /kB T . Our results suggest that neither well-defined electron nor phonon quasiparticles are present in underdoped YBCO systems, and thermal transport exhibits a collective behavior of a ''soup'' of strongly coupled electrons and phonons which moves at a velocity that is smaller than the Fermi velocity, but larger than the speed of sound. We generalize this treatment to measurements of other bad metals and discuss its implications. Work supported by the Gordon and Betty Moore Foundation through the EPiQS Initiative, Grant GBMF4529, and by a Department of Energy Early Career Award (SAH).

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.

Evaluation of charge mobility in organic materials: from localized to delocalized descriptions at a first-principles level.

PubMed

Shuai, Zhigang; Wang, Linjun; Li, Qikai

2011-03-04

The carrier mobility for carbon electronic materials is an important parameter for optoelectronics. We report here some recently developed theoretical tools to predict the mobility without any free parameters. Carrier scatterings with phonons and traps are the key factors in evaluating the mobility. We consider three major scattering regimes: i) where the molecular internal vibration severely induces charge self-trapping and, thus, the hopping mechanism dominates; ii) where both intermolecular and intramolecular scatterings come to play roles, so the Holstein-Peierls polaron model is applied; and, iii) where charge is well delocalized with coherence length comparable with acoustic phonon wavelength, so that a deformation potential approach is more appropriate. We develop computational methods at the first-principles level for the three different cases that have extensive potential application in rationalizing material design.

Nuclear quantum effect with pure anharmonicity and the anomalous thermal expansion of silicon.

PubMed

Kim, D S; Hellman, O; Herriman, J; Smith, H L; Lin, J Y Y; Shulumba, N; Niedziela, J L; Li, C W; Abernathy, D L; Fultz, B

2018-02-27

Despite the widespread use of silicon in modern technology, its peculiar thermal expansion is not well understood. Adapting harmonic phonons to the specific volume at temperature, the quasiharmonic approximation, has become accepted for simulating the thermal expansion, but has given ambiguous interpretations for microscopic mechanisms. To test atomistic mechanisms, we performed inelastic neutron scattering experiments from 100 K to 1,500 K on a single crystal of silicon to measure the changes in phonon frequencies. Our state-of-the-art ab initio calculations, which fully account for phonon anharmonicity and nuclear quantum effects, reproduced the measured shifts of individual phonons with temperature, whereas quasiharmonic shifts were mostly of the wrong sign. Surprisingly, the accepted quasiharmonic model was found to predict the thermal expansion owing to a large cancellation of contributions from individual phonons.

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

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.

Novel approach for calculating the charge carrier mobility and Hall factor for semiconductor materials

NASA Astrophysics Data System (ADS)

Colibaba, G. V.

2018-06-01

The additive Matthiessen's rule is the simplest and most widely used rule for the rapid experimental characterization and modeling of the charge carrier mobility. However, the error when using this rule can be higher than 40% and the contribution of the assumed additional scattering channels due to the difference between the experimental data and results calculated based on this rule can be misestimated by several times. In this study, a universal semi-additive equation is proposed for the total mobility and Hall factor, which is applicable to any quantity of scattering mechanisms, where it considers the energy dependence of the relaxation time and the error is 10-20 times lower compared with Matthiessen's rule. Calculations with accuracy of 99% are demonstrated for materials with polar-optical phonon, acoustic phonon via the piezoelectric potential, ionized, and neutral impurity scattering. The proposed method is extended to the deformation potential, dislocation, localized defect, alloy potential, and dipole scattering, for nondegenerate and partially degenerate materials.

Effects of Fe3O4 Magnetic Nanoparticles on the Thermoelectric Properties of Heavy-Fermion YbAl3 Materials

NASA Astrophysics Data System (ADS)

He, Danqi; Mu, Xin; Zhou, Hongyu; Li, Cuncheng; Ma, Shifang; Ji, Pengxia; Hou, Weikang; Wei, Ping; Zhu, Wanting; Nie, Xiaolei; Zhao, Wenyu

2018-06-01

The magnetic nanocomposite thermoelectric materials xFe3O4/YbAl3 ( x = 0%, 0.3%, 0.6%, 1.0%, and 1.5%) have been prepared by the combination of ultrasonic dispersion and spark plasma sintering process. The nanocomposites retain good chemical stability in the presence of the second-phase Fe3O4. The second-phase Fe3O4 magnetic nanoparticles are distributed on the interfaces and boundaries of the matrix. The x dependences of thermoelectric properties indicate that Fe3O4 magnetic nanoparticles can significantly decrease the thermal conductivity and electrical conductivity. The magnetic nanoparticles embedded in YbAl3 matrix are not only the phonon scattering centers of nanostructures, but also the electron scattering centers due to the Kondo-like effect between the magnetic moment of Fe3O4 nanoparticles and the spin of electrons. The ZT values of the composites are first increased in the x range 0%-1.0% and then decreased when x > 1.0%. The highest ZT value reaches 0.3 at 300 K for the nanocomposite with x = 1.0%. Our work demonstrates that the Fe3O4 magnetic nanoparticles can greatly increase the thermoelectric performance of heavy-fermion YbAl3 thermoelectric materials through simultaneously scattering electrons and phonons.

Electrons and Phonons in Semiconductor Multilayers

NASA Astrophysics Data System (ADS)

Ridley, B. K.

1996-11-01

This book provides a detailed description of the quantum confinement of electrons and phonons in semiconductor wells, superlattices and quantum wires, and shows how this affects their mutual interactions. It discusses the transition from microscopic to continuum models, emphasizing the use of quasi-continuum theory to describe the confinement of optical phonons and electrons. The hybridization of optical phonons and their interactions with electrons are treated, as are other electron scattering mechanisms. The book concludes with an account of the electron distribution function in three-, two- and one-dimensional systems, in the presence of electrical or optical excitation. This text will be of great use to graduate students and researchers investigating low-dimensional semiconductor structures, as well as to those developing new devices based on these systems.

Anisotropic thermal transport in Weyl semimetal TaAs: a first principles calculation.

PubMed

Ouyang, Tao; Xiao, Huaping; Tang, Chao; Hu, Ming; Zhong, Jianxin

2016-06-22

A fundamental understanding of the phonon transport property is crucial to predict the thermal management performance in micro/nano-electronic devices. By combining first principle calculations and Boltzmann phonon transport equation, we investigate thermal transport in TaAs-a typical Weyl semimetal. The lattice thermal conductivity of TaAs at room temperature was found to be 39.26 W mK(-1) and 24.78 W mK(-1) along the a(b) and c crystal axis, respectively, showing obvious anisotropy. Detailed analyses of the mode level phonon properties further revealed that the three acoustic phonon modes dominate the overall thermal transport and the major phonon scattering channels in this typical Weyl semimetal were TA1/TA2/LA + O ↔ O and A + A ↔ O. The representative phonon mean free path of TaAs was also calculated in this paper, which provide helpful guidance for the thermal management of TaAs-based electronic devices.

Lattice thermal conductivity of multi-component alloys

DOE PAGES

Caro, Magdalena; Béland, Laurent K.; Samolyuk, German D.; ...

2015-06-12

High entropy alloys (HEA) have unique properties including the potential to be radiation tolerant. These materials with extreme disorder could resist damage because disorder, stabilized by entropy, is the equilibrium thermodynamic state. Disorder also reduces electron and phonon conductivity keeping the damage energy longer at the deposition locations, eventually favoring defect recombination. In the short time-scales related to thermal spikes induced by collision cascades, phonons become the relevant energy carrier. In this paper, we perform a systematic study of phonon thermal conductivity in multiple component solid solutions represented by Lennard-Jones (LJ) potentials. We explore the conditions that minimize phonon meanmore » free path via extreme alloy complexity, by varying the composition and the elements (differing in mass, atomic radii, and cohesive energy). We show that alloy complexity can be tailored to modify the scattering mechanisms that control energy transport in the phonon subsystem. Finally, our analysis provides a qualitative guidance for the selection criteria used in the design of HEA alloys with low phonon thermal conductivity.« less

Magnon and phonon dispersion, lifetime, and thermal conductivity of iron from spin-lattice dynamics simulations

NASA Astrophysics Data System (ADS)

Wu, Xufei; Liu, Zeyu; Luo, Tengfei

2018-02-01

In recent years, the fundamental physics of spin-lattice (e.g., magnon-phonon) interaction has attracted significant experimental and theoretical interests given its potential paradigm-shifting impacts in areas like spin-thermoelectrics, spin-caloritronics, and spintronics. Modelling studies of the transport of magnons and phonons in magnetic crystals are very rare. In this paper, we use spin-lattice dynamics (SLD) simulations to model ferromagnetic crystalline iron, where the spin and lattice systems are coupled through the atomic position-dependent exchange function, and thus the interaction between magnons and phonons is naturally considered. We then present a method combining SLD simulations with spectral energy analysis to calculate the magnon and phonon harmonic (e.g., dispersion, specific heat, and group velocity) and anharmonic (e.g., scattering rate) properties, based on which their thermal conductivity values are calculated. This work represents an example of using SLD simulations to understand the transport properties involving coupled magnon and phonon dynamics.

Thermal conductivity of graphene nanoribbons accounting for phonon dispersion and polarization

NASA Astrophysics Data System (ADS)

Wang, Yingjun; Xie, Guofeng

2015-12-01

The relative contribution to heat conduction by different phonon branches is still an intriguing and open question in phonon transport of graphene nanoribbons (GNRs). By incorporating the direction-dependent phonon-boundary scattering into the linearized phonon Boltzmann transport equation, we find that because of lower Grüneisen parameter, the TA phonons have the major contribution to thermal conductivity of GNRs, and in the case of smooth edge and micron-length of GNRS, the relative contribution of TA branch to thermal conductivity is over 50%. The length and edge roughness of GNRs have distinct influences on the relative contribution of different polarization branches to thermal conductivity. The contribution of TA branch to thermal conductivity increases with increasing the length or decreasing the edge roughness of GNRs. On the contrary, the contribution of ZA branch to thermal conductivity increases with decreasing the length or increasing the edge roughness of GNRs. The contribution of LA branch is length and roughness insensitive. Our findings are helpful for understanding and engineering the thermal conductivity of GNRs.

Phonon-assisted damping of plasmons in three- and two-dimensional metals

NASA Astrophysics Data System (ADS)

Caruso, Fabio; Novko, Dino; Draxl, Claudia

2018-05-01

We investigate the effects of crystal lattice vibrations on the dispersion of plasmons. The loss function of the homogeneous electron gas (HEG) in two and three dimensions is evaluated numerically in the presence of electronic coupling to an optical phonon mode. Our calculations are based on many-body perturbation theory for the dielectric function as formulated by the Hedin-Baym equations in the Fan-Migdal approximation. The coupling to phonons broadens the spectral signatures of plasmons in the electron-energy loss spectrum (EELS) and it induces the decay of plasmons on timescales shorter than 1 ps. Our results further reveal the formation of a kink in the plasmon dispersion of the two-dimensional HEG, which marks the onset of plasmon-phonon scattering. Overall, these features constitute a fingerprint of plasmon-phonon coupling in EELS of simple metals. It is shown that these effects may be accounted for by resorting to a simplified treatment of the electron-phonon interaction which is amenable to first-principles calculations.

Hydrodynamic phonon drift and second sound in a (20,20) single-wall carbon nanotube

DOE PAGES

Lee, Sangyeop; Lindsay, Lucas

2017-05-18

Here, two hydrodynamic features of phonon transport, phonon drift and second sound, in a (20,20) single wall carbon nanotube (SWCNT) are discussed using lattice dynamics calculations employing an optimized Tersoff potential for atomic interactions. We formally derive a formula for the contribution of drift motion of phonons to total heat flux at steady state. It is found that the drift motion of phonons carry more than 70% and 90% of heat at 300 K and 100 K, respectively, indicating that phonon flow can be reasonably approximated as hydrodynamic if the SWCNT is long enough to avoid ballistic phonon transport. Themore » dispersion relation of second sound is derived from the Peierls-Boltzmann transport equation with Callaway s scattering model and quantifies the speed of second sound and its relaxation. The speed of second sound is around 4000 m/s in a (20,20) SWCNT and the second sound can propagate more than 10 m in an isotopically pure (20,20) SWCNT for frequency around 1 GHz at 100 K.« less

Hydrodynamic phonon drift and second sound in a (20,20) single-wall carbon nanotube

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

Lee, Sangyeop; Lindsay, Lucas

Here, two hydrodynamic features of phonon transport, phonon drift and second sound, in a (20,20) single wall carbon nanotube (SWCNT) are discussed using lattice dynamics calculations employing an optimized Tersoff potential for atomic interactions. We formally derive a formula for the contribution of drift motion of phonons to total heat flux at steady state. It is found that the drift motion of phonons carry more than 70% and 90% of heat at 300 K and 100 K, respectively, indicating that phonon flow can be reasonably approximated as hydrodynamic if the SWCNT is long enough to avoid ballistic phonon transport. Themore » dispersion relation of second sound is derived from the Peierls-Boltzmann transport equation with Callaway s scattering model and quantifies the speed of second sound and its relaxation. The speed of second sound is around 4000 m/s in a (20,20) SWCNT and the second sound can propagate more than 10 m in an isotopically pure (20,20) SWCNT for frequency around 1 GHz at 100 K.« less

Phonon conduction in GaN-diamond composite substrates

NASA Astrophysics Data System (ADS)

Cho, Jungwan; Francis, Daniel; Altman, David H.; Asheghi, Mehdi; Goodson, Kenneth E.

2017-02-01

The integration of strongly contrasting materials can enable performance benefits for semiconductor devices. One example is composite substrates of gallium nitride (GaN) and diamond, which promise dramatically improved conduction cooling of high-power GaN transistors. Here, we examine phonon conduction in GaN-diamond composite substrates fabricated using a GaN epilayer transfer process through transmission electron microscopy, measurements using time-domain thermoreflectance, and semiclassical transport theory for phonons interacting with interfaces and defects. Thermoreflectance amplitude and ratio signals are analyzed at multiple modulation frequencies to simultaneously extract the thermal conductivity of GaN layers and the thermal boundary resistance across GaN-diamond interfaces at room temperature. Uncertainties in the measurement of these two properties are estimated considering those of parameters, including the thickness of a topmost metal transducer layer, given as an input to a multilayer thermal model, as well as those associated with simultaneously fitting the two properties. The volume resistance of an intermediate, disordered SiN layer between the GaN and diamond, as well as a presence of near-interfacial defects in the GaN and diamond, dominates the measured GaN-diamond thermal boundary resistances as low as 17 m2 K GW-1. The GaN thermal conductivity data are consistent with the semiclassical phonon thermal conductivity integral model that accounts for the size effect as well as phonon scattering on point defects at concentrations near 3 × 1018 cm-3.

A revisit to the temperature dependence of electrical resistivity of α - Titanium at low temperatures

NASA Astrophysics Data System (ADS)

Sharath Chandra, L. S.; Mondal, R.; Thamizhavel, A.; Dhar, S. K.; Roy, S. B.

2017-09-01

The temperature dependence of resistivity ρ(T) of a polycrystalline sample and a single crystal sample (current along the [0001] direction) of α - Titanium (Ti) at low temperatures is revisited to understand the electrical charge transport phenomena in this hexagonal closed pack metal. We show that the ρ(T) in single crystal Ti can be explained by considering the scattering of electrons due to electron-phonon, electron-electron, inter-band s-d and electron-impurity interactions, whereas the ρ(T) of polycrystalline Ti could not be explained by these interactions alone. We observed that the effects of the anisotropy of the hexagonal structure on the electronic band structure and the phonon dispersion need to be taken into account to explain ρ(T) of polycrystalline Ti. Two Debye temperatures corresponding to two different directions for the electron-phonon interactions and inter-band s-d scattering are needed to account the observed ρ(T) in polycrystalline Ti.

High Field Transport of Free Carriers at the SI-SIO2 Interface.

DTIC Science & Technology

1983-10-27

nuotbor) - Investigations of interface transport, ballistic transport and generally speaking high field transport in silicon and III-V compounds are...Tang and K. Hess, "Energy Diffusion Equation for an Electron Gas Interacting with Polar Optical Phonons: Non- Parabolic Case," Solid State...deformation potential electron-phonon scattering coeffi- cents is preented for elemental and compound semiconductors. Explesions for t acoustical defonoation

Thermodynamics of technetium: Reconciling theory and experiment using density functional perturbation analysis

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

Weck, Philippe F.; Kim, Eunja

The structure, lattice dynamics and thermodynamic properties of bulk technetium were investigated within the framework of density functional theory. The phonon density of states spectrum computed with density functional perturbation theory closely matches inelastic coherent neutron scattering measurements. The thermal properties of technetium were derived from phonon frequencies calculated within the quasi-harmonic approximation (QHA), which introduces a volume dependence of phonon frequencies as a part of the anharmonic effect. As a result, the predicted thermal expansion and isobaric heat capacity of technetium are in excellent agreement with available experimental data for temperatures up to ~1600 K.

Thermodynamics of technetium: Reconciling theory and experiment using density functional perturbation analysis

DOE PAGES

Weck, Philippe F.; Kim, Eunja

2015-06-11

The structure, lattice dynamics and thermodynamic properties of bulk technetium were investigated within the framework of density functional theory. The phonon density of states spectrum computed with density functional perturbation theory closely matches inelastic coherent neutron scattering measurements. The thermal properties of technetium were derived from phonon frequencies calculated within the quasi-harmonic approximation (QHA), which introduces a volume dependence of phonon frequencies as a part of the anharmonic effect. As a result, the predicted thermal expansion and isobaric heat capacity of technetium are in excellent agreement with available experimental data for temperatures up to ~1600 K.

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.

Temperature-insensitive long-wavelength (λ ≈14 µm) Quantum Cascade lasers with low threshold.

PubMed

Huang, Xue; Charles, William O; Gmachl, Claire

2011-04-25

We demonstrate high-performance, long-wavelength (λ ≈14 µm) Quantum Cascade (QC) lasers based on a diagonal optical transition and a "two-phonon-continuum" depletion scheme in which the lower laser level is depopulated by resonant longitudinal optical phonon scattering followed by scattering to a lower energy level continuum. A 2.8 mm long QC laser shows a low threshold current density of 2.0 kA/cm2, a peak output power of ~336 mW, and a slope efficiency of 375 mW/A, all at 300 K, with a high characteristic temperature T0 ~310 K over a wide temperature range from 240 K to 390 K.

Wideband spectrum analysis of ultra-high frequency radio-wave signals due to advanced one-phonon non-collinear anomalous light scattering.

PubMed

Shcherbakov, Alexandre S; Arellanes, Adan Omar

2017-04-20

We present a principally new acousto-optical cell providing an advanced wideband spectrum analysis of ultra-high frequency radio-wave signals. For the first time, we apply a recently developed approach with the tilt angle to a one-phonon non-collinear anomalous light scattering. In contrast to earlier cases, now one can exploit a regime with the fixed optical wavelength for processing a great number of acoustic frequencies simultaneously in the linear regime. The chosen rutile-crystal combines a moderate acoustic velocity with low acoustic attenuation and allows us wide-band data processing within GHz-frequency acoustic waves. We have created and experimentally tested a 6-cm aperture rutile-made acousto-optical cell providing the central frequency 2.0 GHz, frequency bandwidth ∼0.52  GHz with the frequency resolution about 68.3 kHz, and ∼7620 resolvable spots. A similar cell permits designing an advanced ultra-high-frequency arm within a recently developed multi-band radio-wave acousto-optical spectrometer for astrophysical studies. This spectrometer is intended to operate with a few parallel optical arms for processing the multi-frequency data flows within astrophysical observations. Keeping all the instrument's advantages of the previous schematic arrangement, now one can create the highest-frequency arm using the developed rutile-based acousto-optical cell. It permits optimizing the performances inherent in that arm via regulation of both the central frequency and the frequency bandwidth for spectrum analysis.

Electron drag in ferromagnetic structures separated by an insulating interface

NASA Astrophysics Data System (ADS)

Kozub, V. I.; Muradov, M. I.; Galperin, Y. M.

2018-06-01

We consider electron drag in a system of two ferromagnetic layers separated by an insulating interface. The source of it is expected to be magnon-electron interactions. Namely, we assume that the external voltage is applied to the "active" layer stimulating electric current through this layer. In its turn, the scattering of the current-carrying electrons by magnons leads to a magnon drag current within this layer. The 3-magnons interactions between magnons in the two layers (being of non-local nature) lead to magnon drag within the "passive" layer which, correspondingly, produce electron drag current via processes of magnon-electron scattering. We estimate the drag current and compare it to the phonon-induced one.

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.

Laser marking on microcrystalline silicon film.

PubMed

Park, Min Gyu; Choi, Se-Bum; Ruh, Hyun; Hwang, Hae-Sook; Yu, Hyunung

2012-07-01

We present a compact dot marker using a CW laser on a microcrystalline silicon (Si) thin film. A laser annealing shows a continuous crystallization transformation from nano to a large domain (> 200 nm) of Si nanocrystals. This microscale patterning is quite useful since we can manipulate a two-dimentional (2-D) process of Si structural forms for better and efficient thin-film transistor (TFT) devices as well as for photovoltaic application with uniform electron mobility. A Raman scattering microscope is adopted to draw a 2-D mapping of crystal Si film with the intensity of optical-phonon mode at 520 cm(-1). At a 300-nm spatial resolution, the position resolved the Raman scattering spectra measurements carried out to observe distribution of various Si species (e.g., large crystalline, polycrystalline and amorphous phase). The population of polycrystalline (poly-Si) species in the thin film can be analyzed with the frequency shift (delta omega) from the optical-phonon line since poly-Si distribution varies widely with conditions, such as an irradiated-laser power. Solid-phase crystallization with CW laser irradiation improves conductivity of poly-Si with micropatterning to develop the potential of the device application.

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.

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

Metric for strong intrinsic fourth-order phonon anharmonicity

NASA Astrophysics Data System (ADS)

Yue, Sheng-Ying; Zhang, Xiaoliang; Qin, Guangzhao; Phillpot, Simon R.; Hu, Ming

2017-05-01

Under the framework of Taylor series expansion for potential energy, we propose a simple and robust metric, dubbed "regular residual analysis," to measure the fourth-order phonon anharmonicity in crystals. The method is verified by studying the intrinsic strong higher-order anharmonic effects in UO2 and CeO2. Comparison of the thermal conductivity results, which calculated by the anharmonic lattice dynamics method coupled with the Boltzmann transport equation and the spectral energy density method coupled with ab initio molecular dynamics simulation further validates our analysis. Analysis of the bulk Si and Ge systems confirms that the fourth-order phonon anharmonicity is enhanced and cannot be neglected at high enough temperatures, which agrees with a previous study where the four-phonon scattering was explicitly determined. This metric will facilitate evaluating and interpreting the lattice thermal conductivity of crystals with strong fourth-order phonon anharmonicity.

Reflection thermal diffuse x-ray scattering for quantitative determination of phonon dispersion relations

DOE PAGES

Mei, A. B.; Hellman, O.; Schlepuetz, C. M.; ...

2015-11-03

Synchrotron reflection x-ray thermal diffuse scattering (TDS) measurements, rather than previously reported transmission TDS, are carried out at room temperature and analyzed using a formalism based upon second-order interatomic force constants and long-range Coulomb interactions to obtain quantitative determinations of MgO phonon dispersion relations (h) over bar omega(j) (q), phonon densities of states g((h) over bar omega), and isochoric temperature-dependent vibrational heat capacities c v (T). We use MgO as a model system for investigating reflection TDS due to its harmonic behavior as well as its mechanical and dynamic stability. Resulting phonon dispersion relations and densities of states are foundmore » to be in good agreement with independent reports from inelastic neutron and x-ray scattering experiments. Temperature-dependent isochoric heat capacities c v (T), computed within the harmonic approximation from (h) over bar omega(j) (q) values, increase with temperature from 0.4 x 10 -4 eV/atom K at 100 K to 1.4 x 10 -4 eV/atom K at 200 K and 1.9 x 10 -4 eV/atom K at 300 K, in excellent agreement with isobaric heat capacity values c p (T) between 4 and 300 K. We anticipate that the experimental approach developed here will be valuable for determining vibrational properties of heteroepitaxial thin films since the use of grazing-incidence (θ ≲ θ c where θ c is the density-dependent critical angle) allows selective tuning of x-ray penetration depths to ≲ 10 nm.« less

A comment on the thermal conductivity of (U,Pu)O 2 and (U,Th)O 2 by molecular dynamics with adjustment for phonon-spin scattering

DOE PAGES

Cooper, Michael William D.; Liu, Xiang -Yang; Stanek, Christopher Richard; ...

2016-07-15

In this study, a new approach for adjusting molecular dynamics results on UO 2 thermal conductivity to include phonon-spin scattering has been used to improve calculations on U x Pu 1–x O 2 and U xTh 1xO 2. We demonstrate that by including spin scattering a strong asymmetry as a function of uranium actinide fraction, x, is obtained. Greater degradation is shown for U xTh 1–xO 2 than U xPu 1-xO 2. Minimum thermal conductivities are predicted at U 0.97Pu 0.03O 2 and U 0.58Th 0.42O 2, although the degradation in U xPu 1–xO 2 is negligible relative to puremore » UO 2.« less

Mutual friction in a cold color-flavor-locked superfluid and r-mode instabilities in compact stars.

PubMed

Mannarelli, Massimo; Manuel, Cristina; Sa'd, Basil A

2008-12-12

Dissipative processes acting in rotating neutron stars are essential in preventing the growth of the r-mode instability. We estimate the damping time of r modes of a hypothetical compact quark star made up by color-flavor-locked quark matter at a temperature T < or approximately 0.01 MeV. The dissipation that we consider is due to the mutual friction force between the normal and the superfluid component arising from the elastic scattering of phonons with quantized vortices. This process is the dominant one for temperatures T < or approximately 0.01 MeV, where the mean free path of phonons due to their self-interactions is larger than the radius of the star. We find that r-mode oscillations are efficiently damped by this mechanism for pulsars rotating at frequencies of the order of 1 Hz at most. Our analysis rules out the possibility that cold pulsars rotating at higher frequencies are entirely made up by color-flavor-locked quark matter.

CMOS-Memristor Hybrid Nanoelectronics for AES Encryption

DTIC Science & Technology

2013-03-01

characterizing memristive materials can be associated with the Raman Effect. The Raman Effect or Raman Scattering results from inelastic scattering...of the incident excitation photons from the vibrational phonons in a sample material. Raman interaction is typically very weak, on the order of 1...in 10 7 incident photons being Raman shifted. Intensity of Raman scattering is very nonlinearly related to the incident wavelength just as Rayleigh

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

Phonon-defect scattering and thermal transport in semiconductors: developing guiding principles

NASA Astrophysics Data System (ADS)

Polanco, Carlos; Lindsay, Lucas

First principles calculations of thermal conductivity have shown remarkable agreement with measurements for high-quality crystals. Nevertheless, most materials contain defects that provide significant extrinsic resistance and lower the conductivity from that of a perfect sample. This effect is usually accounted for with simplified analytical models that neglect the atomistic details of the defect and the exact dynamical properties of the system, which limits prediction capabilities. Recently, a method based on Greens functions was developed to calculate the phonon-defect scattering rates from first principles. This method has shown the important role of point defects in determining thermal transport in diamond and boron arsenide, two competitors for the highest bulk thermal conductivity. Here, we study the role of point defects on other relatively high thermal conductivity semiconductors, e.g., BN, BeSe, SiC, GaN and Si. We compare their first principles defect-phonon scattering rates and effects on transport properties with those from simplified models and explore common principles that determine these. Efforts will focus on basic vibrational properties that vary from system to system, such as density of states, interatomic force constants and defect deformation. Research supported by the U.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division.

Designer Disordered Complex Media: Hyperuniform Photonic and Phononic Band Gap Materials

NASA Astrophysics Data System (ADS)

Amoah, Timothy

In this thesis we investigate designer disordered complex media for photonics and phononics applications. Initially we focus on the photonic properties and we analyse hyperuniform disordered structures (HUDS) using numerical simulations. Photonic HUDS are a new class of photonic solids, which display large, isotropic photonic band gaps (PBG) comparable in size to the ones found in photonic crystals (PC). We review their complex interference properties, including the origin of PBGs and potential applications. HUDS combine advantages of both isotropy due to disorder (absence of long-range order) and controlled scattering properties from uniform local topology due to hyperuniformity (constrained disorder). The existence of large band gaps in HUDS contradicts the longstanding intuition that Bragg scattering and long-range translational order is required in PBG formation, and demonstrates that interactions between Mie-like local resonances and multiple scattering can induce on their own PBGs. The discussion is extended to finite height effects of planar architectures such as pseudo-band-gaps in photonic slabs as well as the vertical confinement in the presence of disorder. The particular case of a silicon-on-insulator compatible hyperuniform disordered network structure is considered for TE polarised light. We address technologically realisable designs of HUDS including localisation of light in point-defect-like optical cavities and the guiding of light in freeform PC waveguide analogues. Using finite-difference time domain and band structure computer simulations, we show that it is possible to construct optical cavities in planar hyperuniform disordered solids with isotropic band gaps that effciently confine TE polarised radiation. We thus demonstrate that HUDS are a promising general-purpose design platform for integrated optical micro-circuitry. After analysing HUDS for photonic applications we investigate them in the context of elastic waves towards phononics applications. We demonstrate the first phononic band gaps (PnBG) for HUDS. We find that PnBGs in phononic HUDS can confine and guide elastic waves similar to photonic HUDS for EM radiation.

Phase stability and lattice thermal conductivity reduction in CoSb{sub 3} skutterudites, doped with chalcogen atoms

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

Battabyal, M., E-mail: manjusha.battabyal@project.arci.res.in; Priyadarshini, B.; Gopalan, R.

We report a significant reduction in the lattice thermal conductivity of the CoSb{sub 3} skuttertudites, doped with chalcogen atoms. Te/Se chalcogen atoms doped CoSb{sub 3} skutterudite samples (Te{sub 0.1}Co{sub 4}Sb{sub 12}, Se{sub 0.1}Co{sub 4}Sb{sub 12}, Te{sub 0.05}Se{sub 0.05}Co{sub 4}Sb{sub 12}) are processed by ball milling and spark plasma sintering. X-ray diffraction data combined with energy dispersive X-ray spectra indicate the doping of Te/Se chalcogen atoms in the skutterudite. The temperature dependent X-ray diffraction confirms the stability of the Te/Se doped CoSb{sub 3} skutterudite phase and absence of any secondary phase in the temperature range starting from 300 K to 773more » K. The Raman spectroscopy reveals that different chalcogen dopant atoms cause different resonant optical vibrational modes between the dopant atom and the host CoSb{sub 3} skutterudite lattice. These optical vibrational modes do scatter heat carrying acoustic phonons in a different spectral range. It was found that among the Te/Se chalcogen atoms, Te atoms alter the host CoSb{sub 3} skutterudite lattice vibrations to a larger extent than Se atoms, and can potentially scatter more Sb related acoustic phonons. The Debye model of lattice thermal conductivity confirms that the resonant phonon scattering has important contributions to the reduction of lattice thermal conductivity in CoSb{sub 3} skutterudites doped with Te/Se chalcogen atoms. Lattice thermal conductivity ∼ 0.9 W/mK at 773 K is achieved in Te{sub 0.1}Co{sub 4}Sb{sub 12} skutterudites, which is the lowest value reported so far in CoSb{sub 3} skutterudites, doped with single Te chalcogen atom.« less

Thermal conductivity of graphene mediated by strain and size

DOE PAGES

Kuang, Youdi; Shi, Sanqiang; Wang, Xinjiang; ...

2016-06-09

Based on first-principles calculations and full iterative solution of the linearized Boltzmann–Peierls transport equation for phonons, we systematically investigate effects of strain, size and temperature on the thermal conductivity k of suspended graphene. The calculated size-dependent and temperature-dependent k for finite samples agree well with experimental data. The results show that, contrast to the convergent room-temperature k = 5450 W/m-K of unstrained graphene at a sample size ~8 cm, k of strained graphene diverges with increasing the sample size even at high temperature. Out-of-plane acoustic phonons are responsible for the significant size effect in unstrained and strained graphene due tomore » their ultralong mean free path and acoustic phonons with wavelength smaller than 10 nm contribute 80% to the intrinsic room temperature k of unstrained graphene. Tensile strain hardens the flexural modes and increases their lifetimes, causing interesting dependence of k on sample size and strain due to the competition between boundary scattering and intrinsic phonon–phonon scattering. k of graphene can be tuned within a large range by strain for the size larger than 500 μm. These findings shed light on the nature of thermal transport in two-dimensional materials and may guide predicting and engineering k of graphene by varying strain and size.« less

Predicting lattice thermal conductivity with help from ab initio methods

NASA Astrophysics Data System (ADS)

Broido, David

2015-03-01

The lattice thermal conductivity is a fundamental transport parameter that determines the utility a material for specific thermal management applications. Materials with low thermal conductivity find applicability in thermoelectric cooling and energy harvesting. High thermal conductivity materials are urgently needed to help address the ever-growing heat dissipation problem in microelectronic devices. Predictive computational approaches can provide critical guidance in the search and development of new materials for such applications. Ab initio methods for calculating lattice thermal conductivity have demonstrated predictive capability, but while they are becoming increasingly efficient, they are still computationally expensive particularly for complex crystals with large unit cells . In this talk, I will review our work on first principles phonon transport for which the intrinsic lattice thermal conductivity is limited only by phonon-phonon scattering arising from anharmonicity. I will examine use of the phase space for anharmonic phonon scattering and the Grüneisen parameters as measures of the thermal conductivities for a range of materials and compare these to the widely used guidelines stemming from the theory of Liebfried and Schölmann. This research was supported primarily by the NSF under Grant CBET-1402949, and by the S3TEC, an Energy Frontier Research Center funded by the US DOE, office of Basic Energy Sciences under Award No. DE-SC0001299.

Anharmonic phonons and magnons in BiFeO3

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

Delaire, Olivier A; Ma, Jie; Stone, Matthew B

2012-01-01

The phonon density of states (DOS) and magnetic excitation spectrum of polycrystalline BiFeO3 were measured for temperatures 200 < T < 750K , using inelastic neutron scattering (INS). Our results indicate that the magnetic spectrum of BiFeO3 closely resembles that of similar Fe perovskites, such as LaFeO3, despite the cycloid modulation in BiFeO3. We do not find any evidence for a spin gap. A strong T-dependence of the phonon DOS was found, with a marked broadening of the whole spectrum, providing evidence of strong anharmonicity. This anharmonicity is corroborated by large amplitude motions of Bi and O ions observed withmore » neutron diffraction. These results highlight the importance of spin-phonon coupling in this material.« less

Structure of the Kπ = 4+ bands in 186,188Os

NASA Astrophysics Data System (ADS)

Phillips, A. A.; Garrett, P. E.; Bettermann, L.; Braun, N.; Burke, D. G.; Demand, G. A.; Faestermann, T.; Finlay, P.; Green, K. L.; Hertenberger, R.; Krü; cken, R.; Leach, K. G.; Schumaker, M. A.; Svensson, C. E.; Wirth, H.-F.; Wong, J.

2009-01-01

The structures of 3+ states in Os have been debated over several decades. Based on measured B(E2) values they were interpreted in 186-192Os as Kπ = 4+ two-phonon vibrations, whereas inelastic scattering, and (t,α) work imply a hexadecapole phonon description. To clarify the nature of these Kπ = 4+ bands in 186,188Os, we performed a (3He,d) reaction on 185,187Re targets using 30 MeV 3He beams and a Q3D spectrograph. Absolute cross sections were obtained for excited states up to 3 MeV at 9 angles from 5° to 50°. Results indicate a significant 5/2+[402]π+3/2+[402]π component in agreement with quasiparticle phonon model predictions for a single hexadecapole phonon structure.

Phonons around a soliton in a continuum model of t-(CH)x

NASA Astrophysics Data System (ADS)

Ono, Y.; Terai, A.; Wada, Y.

1986-05-01

The eigenvalue problem for phonons around a soliton in a continuum model of trans-polyacetylene t-(CH)x, the so-called TLM model (Takayama et al, 1980), is reinvestigated using a kernel which satisfies the correct boundary condition. The three localized modes are reproduced, two with even parity and one with odd parity. The phase-shift analysis of the extended modes confirms their existence if the one-dimensional version of Levinson's theorem is applicable to the present problem. It is found that the phase shifts of even and odd modes differ from each other in the long-wavelength limit. The conclusion of Ito et al. (1984), that the scattering of phonons by the soliton is reflectionless, has to be modified in this limit, where phonons suffer reflection from the soliton.

Substrate-induced reduction of graphene thermal conductivity

NASA Astrophysics Data System (ADS)

Koniakhin, S. V.; Utesov, O. I.; Terterov, I. N.; Nalitov, A. V.

2017-01-01

We develop a theory of heat conductivity in supported graphene, accounting for coherent phonon scattering on disorder induced by an amorphous substrate. We derive spectra for in-plane and out-of-plane phonons in the framework of Green's function approach. The energy parameters of the theory are obtained using molecular dynamics simulations for graphene on a SiO2 substrate. The heat conductivity is calculated by the Boltzmann transport equation. We find that the interaction with the substrate drastically reduces the phonon lifetime and completely suppresses the contribution of flexural (ZA) phonons to the heat conductivity. As a result, the total heat conductivity is reduced by several times, which matches with the tendency observed in the available experimental data. The considered effect is important for managing the thermal properties of graphene-based electronic devices.

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.

Theoretical Studies of Relaxation and Optical Properties of Polymers

NASA Astrophysics Data System (ADS)

Jin, Bih-Yaw

1993-01-01

This thesis is composed of two parts. In the part one, the empirical correlation between the logarithm of tunneling splittings and the temperature at which the spin-lattice relaxation time is minimum for methyl groups in different molecular crystals is explained successfully by taking multiphonon processes into account. We show that one phonon transitions dominate in the low barrier limit. However, in the intermediate barrier range and high barrier limit, it is necessary to include multiphonon processes. We also show that the empirical correlation depends only logarithmically on the details of the phonon bath. In the part two, we have investigated the optical and relaxation properties of conjugated polymers. The connection between the vibronic picture of Raman scattering and the third order perturbation approach in solid state physics is clarified in chapter 2. Starting from the Kramers -Heissenberg-Dirac formula for Raman scattering, we derive expressions for the Condon and Herzberg-Teller terms from a simple two-level system to a two-band system, i.e. polyacetylene, by using traditional vibronic picture. Both the Condon and Herzberg-Teller terms contribute to two-band processes, while three-band processes consist only of Herzberg-Teller terms in the solid state limit. Close to resonance the Condon term dominates and converges to the usual solid state result. In the off-resonance region the Herzberg -Teller term is comparable to Condon term for both small molecule and solid state system. In chapter 3, we will concentrate on the lattice relaxation of the lowest optically allowed 1B_ {u} state, especially, the effect of electron correlation on the excited state geometric relaxation for finite polyenes. We have examined the competition between electron-electron interaction and electron-phonon coupling on the formation of localized lattice distortion in the 1B_{u} state for finite polyene with chain length up to 30 double bonds. The chain length dependence of the lattice relaxation in 1B _{u} state has been studied thoroughly within singly excited configuration interaction for short range Hubbard, extended Hubbard model and long-range Pariser -Parr-Pople model. We have found that local distortion is not favored until a critical chain length is reached. Beyond this critical length, which is a function of electron-electron interaction and electron-phonon coupling strength, a self -trapped exciton is formed rather than the separated soliton -antisoliton configuration as expected in the independent electron theory. (Copies available exclusively from MIT Libraries, Rm. 14-0551, Cambridge, MA 02139-4307. Ph. 617 -253-5668; Fax 617-253-1690.).

Preface: Phonons 2007

NASA Astrophysics Data System (ADS)

Perrin, Bernard

2007-06-01

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 phonons can help tracking dark matter. These 328 presentations gave rise to 185 articles published in the present proceedings. The traditional topics of this conference series (phonons in superconductors and new materials, lattice dynamics, phonons in glasses and disordered materials, phase transitions, light, neutrons and x-ray inelastic scattering) were still very important in the scientific program but an increasing number of contributions occurred in the fields of coherent phonon generation, phonons in nanoscaled structures and nano/micro thermal phonon transport, expressing the growing involvement of condensed matter physicists in nanosciences. Areas like acoustic solitons and phononic crystals are now well established. Two noteworthy contributions have been brought in the long term quest for an operational SASER : one by Harold De Wijn's group from Utrecht in the classical ruby system and another one by Anthony Kent's group from Nottingham, who used semiconductor nanodevices to realize both an amplifying medium and a cavity. With these semiconductor devices the possibility for engineering, generation and detection of THz acoustic phonons are now imminent. By tradition, a prize is awarded every three years at the International Conference on Phonon Scattering in Condensed Matter to honour a scientist for his outstanding contributions to the field of phonon physics. For this twelfth edition, Humphrey Maris has been honoured for his numerous breakthroughs in the physics of phonons and quantum fluids. According to the words of James Wolfe 'Humphrey Maris has delighted and innovated the members of our phonon community with an entertaining style and challenging wit'. Prizes were also awarded for the best presentations during the poster sessions. The two winners were Peter van Capel from Utrecht, Netherlands, ('Simulations of acoustic soliton-induced chirping of exciton resonances') and Patrick Emery from Lille, France, ('Acoustic attenuation in silica in the 100-250 GHz range using coloured picosecond ultrasonics). Both prizes were offered by C'Nano IdF (Centre de Compétence NanoSciences Ile-de-France/Paris District Competence Center in Nanosciences). I want also to point out the strong support given by three institutions: CNRS (Centre National de la Recherche Scientifique), INSP (Institut des NanoSciences de Paris) and SFA (Socitété Française d'Acoustique). Finally, I would like to thank the members of the different committees who helped for the organization of this conference. I am particularly indebted to Bernard Bonello, Arnaud Devos, Jean-Yves Duquesne, Jean-Yves Prieur and Clément Rossignol for their invaluable help. I appreciated the kindness and efficiency of Armelle Guilloux ('Ellipse & Co'). I want also to express my thanks to close collaborators: Catherine Dematteis, Agnès Huynh and Emmanuel Péronne. During the conference, I appreciated the valuable assistance of Sandrine Guit, Béatrice Desoudin and of the student team. The edition of these proceedings could not have been possible without the tremendous amount of work performed by Jean-Yves Duquesne and the valuable help of Jean-Yves Prieur. I hope that the delegates of PHONONS 2007 enjoyed the program and will be willing to attend the 13th conference which will be chaired by Professor Chi Kuang Sun in Taiwan in 2010. Bernard Perrin, Chairman of PHONONS 2007 Institut des NanoSciences de Paris, Paris, November 2007 Copyright: CNRS Photo - Nicole TIGET. The PDF contains the lists of committee members, sponsors and participants.

Is localized infrared spectroscopy now possible in the electron microscope?

PubMed

Rez, Peter

2014-06-01

The recently developed in-column monochromators make it possible to record energy-c spectra with resolutions better than 30 meV from nanometer-sized regions. It should therefore in principle be possible to detect localized vibrational excitations. The scattering geometry in the electron microscope means that bond stretching in the specimen plane or longitudinal optic phonons dominate the scattering. Most promising for initial studies are vibrations with energies between 300 and 400 meV from hydrogen bonded to other atoms. Estimates of the scattering cross-sections on the basis of a simple model show that they are about the same as inner shell scattering cross-sections. Cross-sections also increase with charge transfer between the atoms, and theory incorporating realistic charge distributions shows that signal/noise is the only limitation to high-resolution imaging. Given the magnitude of the scattering cross-sections, minimizing the tail of the zero-loss peak is just as important as achieving a small-width at half-maximum. Improvements in both resolution and controlling the zero-loss tail will be necessary before it is practical to detect optic phonons in solids between 40 and 60 meV.

First-principles studies of electron transport in Ga2O3

NASA Astrophysics Data System (ADS)

Kang, Youngho; Krishnaswamy, Karthik; Peelaers, Hartwin; van de Walle, Chris G.

Ga2O3 is a wide-gap semiconductor with a monoclinic crystal structure and a band gap of 4.8 eV. Its high carrier mobility and large band gap have attracted a lot of attention for use in high power electronics and transparent conductors. Despite its potential for adoption in these applications, an understanding of its carrier transport properties is still lacking. In this study we use first-principles calculations to analyze and compute the electron scattering rates in Ga2O3. Scattering due to ionized impurities and polar longitudinal-optical (LO) phonon is taken into account. We find that the electron mobility is nearly isotropic, despite the low-symmetry monoclinic structure of Ga2O3. At low carrier densities ( 1017 cm-3), the mobility is limited by LO phonon scattering. Scattering by ionized impurities becomes increasingly important at higher carrier densities. This type of scattering is enhanced when compensating native point defects are present; in particular, gallium vacancies, which are triply negatively charged, can have a strong effect on mobility. These effects explain the downturn in mobility observed in experiments at high carrier densities. This work was supported by ARO and NSF.

Lattice Vibrations Boost Demagnetization Entropy in Shape Memory Alloy

DOE PAGES

Stonaha, Paul J.; Manley, Michael E.; Bruno, Nick; ...

2015-10-07

Magnetocaloric (MC) materials present an avenue for chemical-free, solid state refrigeration through cooling via adiabatic demagnetization. We have used inelastic neutron scattering to measure the lattice dynamics in the MC material Ni 45Co 5Mn 36.6In 13.4. Upon heating across TC, the material exhibits an anomalous increase in phonon entropy of 0.17 0.04 k_B/atom, which is nine times larger than expected from conventional thermal expansion. We find that the phonon softening is focused in a transverse optic phonon, and we present the results of first-principle calculations which predict a strong coupling between lattice distortions and magnetic excitations.

Quantitative scanning thermal microscopy of ErAs/GaAs superlattice structures grown by molecular beam epitaxy

NASA Astrophysics Data System (ADS)

Park, K. W.; Nair, H. P.; Crook, A. M.; Bank, S. R.; Yu, E. T.

2013-02-01

A proximal probe-based quantitative measurement of thermal conductivity with ˜100-150 nm lateral and vertical spatial resolution has been implemented. Measurements on an ErAs/GaAs superlattice structure grown by molecular beam epitaxy with 3% volumetric ErAs content yielded thermal conductivity at room temperature of 9 ± 2 W/m K, approximately five times lower than that for GaAs. Numerical modeling of phonon scattering by ErAs nanoparticles yielded thermal conductivities in reasonable agreement with those measured experimentally and provides insight into the potential influence of nanoparticle shape on phonon scattering. Measurements of wedge-shaped samples created by focused ion beam milling provide direct confirmation of depth resolution achieved.

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.

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.

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

Terahertz lasers and amplifiers based on resonant optical phonon scattering to achieve population inversion

NASA Technical Reports Server (NTRS)

Hu, Qing (Inventor); Williams, Benjamin S. (Inventor)

2007-01-01

The present invention provides quantum cascade lasers and amplifier that operate in a frequency range of about 1 Terahertz to about 10 Terahertz. In one aspect, a quantum cascade laser of the invention includes a semiconductor heterostructure that provides a plurality of lasing modules connected in series. Each lasing module includes a plurality of quantum well structure that collectively generate at least an upper lasing state, a lower lasing state, and a relaxation state such that the upper and the lower lasing states are separated by an energy corresponding to an optical frequency in a range of about 1 to about 10 Terahertz. The lower lasing state is selectively depopulated via resonant LO-phonon scattering of electrons into the relaxation state.

Terahertz lasers and amplifiers based on resonant optical phonon scattering to achieve population inversion

NASA Technical Reports Server (NTRS)

Williams, Benjamin S. (Inventor); Hu, Qing (Inventor)

2009-01-01

The present invention provides quantum cascade lasers and amplifier that operate in a frequency range of about 1 Terahertz to about 10 Terahertz. In one aspect, a quantum cascade laser of the invention includes a semiconductor heterostructure that provides a plurality of lasing modules connected in series. Each lasing module includes a plurality of quantum well structure that collectively generate at least an upper lasing state, a lower lasing state, and a relaxation state such that the upper and the lower lasing states are separated by an energy corresponding to an optical frequency in a range of about 1 to about 10 Terahertz. The lower lasing state is selectively depopulated via resonant LO-phonon scattering of electrons into the relaxation state.

Localization length and intraband scattering of excitons in linear aggregates

NASA Astrophysics Data System (ADS)

Lemaistre, J. P.

1999-07-01

A theoretical model to describe the intraband scattering of excitons in linear aggregates of finite size which exhibit strong intermolecular interactions is presented. From the calculation of the aggregate eigenstates, the localization length of excitons is evaluated for various configurations featuring physical situations like trapping, edge effects, inclusion of diagonal and/or orientational disorders. The intraband scattering is studied by considering the exciton-phonon stochastic coupling induced by the thermal bath. This coupling creates local dynamical fluctuations in the site energies which are characterized by their amplitude ( Δ) and their correlation time ( τc). Expressions of scattering rates are provided and used in a Pauli master equation to calculate the time dependence of the eigenstates populations after initial excitation of the quasi exciton-band. It is shown that the time evolution of the lowest state population as well as the Stokes shift strongly depend on τc. Comparison of the theoretical results to time-resolved experiments performed on triaryl pyrylium salts allows us to interpret the observed Stokes shift and to derive an average value of the exciton-phonon correlation time.

Thermal Properties and Phonon Spectral Characterization of Synthetic Boron Phosphide for High Thermal Conductivity Applications.

PubMed

Kang, Joon Sang; Wu, Huan; Hu, Yongjie

2017-12-13

Heat dissipation is an increasingly critical technological challenge in modern electronics and photonics as devices continue to shrink to the nanoscale. To address this challenge, high thermal conductivity materials that can efficiently dissipate heat from hot spots and improve device performance are urgently needed. Boron phosphide is a unique high thermal conductivity and refractory material with exceptional chemical inertness, hardness, and high thermal stability, which holds high promises for many practical applications. So far, however, challenges with boron phosphide synthesis and characterization have hampered the understanding of its fundamental properties and potential applications. Here, we describe a systematic thermal transport study based on a synergistic synthesis-experimental-modeling approach: we have chemically synthesized high-quality boron phosphide single crystals and measured their thermal conductivity as a record-high 460 W/mK at room temperature. Through nanoscale ballistic transport, we have, for the first time, mapped the phonon spectra of boron phosphide and experimentally measured its phonon mean free-path spectra with consideration of both natural and isotope-pure abundances. We have also measured the temperature- and size-dependent thermal conductivity and performed corresponding calculations by solving the three-dimensional and spectral-dependent phonon Boltzmann transport equation using the variance-reduced Monte Carlo method. The experimental results are in good agreement with that predicted by multiscale simulations and density functional theory, which together quantify the heat conduction through the phonon mode dependent scattering process. Our finding underscores the promise of boron phosphide as a high thermal conductivity material for a wide range of applications, including thermal management and energy regulation, and provides a detailed, microscopic-level understanding of the phonon spectra and thermal transport mechanisms of boron phosphide. The present study paves the way toward the establishment of a new framework, based on the phonon spectra-material structure relationship, for the rational design of high thermal conductivity materials and nano- to multiscale devices.

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

Lower lattice thermal conductivity in SbAs than As or Sb monolayers: a first-principles study.

PubMed

Guo, San-Dong; Liu, Jiang-Tao

2017-12-06

Phonon transport in group-VA element (As, Sb and Bi) monolayer semiconductors has been widely investigated in theory, and, of them, monolayer Sb (antimonene) has recently been synthesized. In this work, phonon transport in monolayer SbAs is investigated with a combination of first-principles calculations and the linearized phonon Boltzmann equation. It is found that the lattice thermal conductivity of monolayer SbAs is lower than those of both monolayer As and Sb, and the corresponding sheet thermal conductance is 28.8 W K -1 at room temperature. To understand the lower lattice thermal conductivity in monolayer SbAs than those in monolayer As and Sb, the group velocities and phonon lifetimes of monolayer As, SbAs and Sb are calculated. The calculated results show that the group velocities of monolayer SbAs are between those of monolayer As and Sb, but that the phonon lifetimes of SbAs are smaller than those of both monolayer As and Sb. Hence, the low lattice thermal conductivity in monolayer SbAs is attributed to very small phonon lifetimes. Unexpectedly, the ZA branch has very little contribution to the total thermal conductivity, only 2.4%, which is obviously different from those of monolayer As and Sb with very large contributions. This can be explained by very small phonon lifetimes for the ZA branch of monolayer SbAs. The lower lattice thermal conductivity of monolayer SbAs compared to that of monolayer As or Sb can be understood by the alloying of As (Sb) with Sb (As), which should introduce phonon point defect scattering. We also consider the isotope and size effects on the lattice thermal conductivity. It is found that isotope scattering produces a neglectful effect, and the lattice thermal conductivity with a characteristic length smaller than 30 nm can reach a decrease of about 47%. These results may offer perspectives on tuning the lattice thermal conductivity by the mixture of multiple elements for applications of thermal management and thermoelectricity, and motivate further experimental efforts to synthesize monolayer SbAs.

Electron mobility limited by optical phonons in wurtzite InGaN/GaN core-shell nanowires

NASA Astrophysics Data System (ADS)

Liu, W. H.; Qu, Y.; Ban, S. L.

2017-09-01

Based on the force-balance and energy-balance equations, the optical phonon-limited electron mobility in InxGa1-xN/GaN core-shell nanowires (CSNWs) is discussed. It is found that the electrons tend to distribute in the core of the CSNWs due to the strong quantum confinement. Thus, the scattering from first kind of the quasi-confined optical (CO) phonons is more important than that from the interface (IF) and propagating (PR) optical phonons. Ternary mixed crystal and size effects on the electron mobility are also investigated. The results show that the PR phonons exist while the IF phonons disappear when the indium composition x < 0.047, and vice versa. Accordingly, the total electron mobility μ first increases and then decreases with indium composition x, and reaches a peak value of approximately 3700 cm2/(V.s) when x = 0.047. The results also show that the mobility μ increases as increasing the core radius of CSNWs due to the weakened interaction between the electrons and CO phonons. The total electron mobility limited by the optical phonons exhibits an obvious enhancement as decreasing temperature or increasing line electron density. Our theoretical results are expected to be helpful to develop electronic devices based on CSNWs.

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.

Thermally triggered phononic gaps in liquids at THz scale

DOE PAGES

Bolmatov, Dima; Zhernenkov, Mikhail; Zavyalov, Dmitry; ...

2016-01-14

In this study we present inelastic X-ray scattering experiments in a diamond anvil cell and molecular dynamic simulations to investigate the behavior of phononic excitations in liquid Ar. The spectra calculated using molecular dynamics were found to be in a good agreement with the experimental data. Furthermore, we observe that, upon temperature increases, a low-frequency transverse phononic gap emerges while high-frequency propagating modes become evanescent at the THz scale. The effect of strong localization of a longitudinal phononic mode in the supercritical phase is observed for the first time. The evidence for the high-frequency transverse phononic gap due to themore » transition from an oscillatory to a ballistic dynamic regimes of motion is presented and supported by molecular dynamics simulations. This transition takes place across the Frenkel line thermodynamic limit which demarcates compressed liquid and non-compressed fluid domains on the phase diagram and is supported by calculations within the Green-Kubo phenomenological formalism. These results are crucial to advance the development of novel terahertz thermal devices, phononic lenses, mirrors, and other THz metamaterials.« less

Proton Transports in Pure Liquid Water Characterized by Melted Ice Lattice Model

NASA Astrophysics Data System (ADS)

Jie, Binbin; Sah, Chihtang

Basic water properties have not been understood for 200 years. Our Melted Ice Lattice model accounts for the 2 basic properties of pure water, the ion product (pH) and mobilities. It has HCP primitive unit cells, each with 4H2O, based on the 1933 Bernal-Fowler model, verified by 1935 Pauling residual entropy theory of 1928-1935 Giauque experimental low temperature specific heat measurements. Our 2 ion species are point-mass protons p + and p-, for mass and electricity transport. Three protonic thermal activation energies are obtained from pH and p + and p- mobilities vs T (0-100OC). Proton transport is analyzed in 3 proton-phonon collision steps: proton detrapping by protonic phonon absorption, proton scattering by oxygenic (water) phonons, and proton trapping with protonic phonon emission. Distinction between Potential and Kinetic Energy Bands of protons (Fermions) and phonons (Bosons) is noted. Experimental protonic activation energies are the phonon energies given by the spring-mass vibration frequencies of lattice, wn = (kn/mn)1/2 . n is the proton-mass unit of the synchronized vibrating particles in the primitive unit cells.

Real-Time Observation of Exciton-Phonon Coupling Dynamics in Self-Assembled Hybrid Perovskite Quantum Wells.

PubMed

Ni, Limeng; Huynh, Uyen; Cheminal, Alexandre; Thomas, Tudor H; Shivanna, Ravichandran; Hinrichsen, Ture F; Ahmad, Shahab; Sadhanala, Aditya; Rao, Akshay

2017-11-28

Self-assembled hybrid perovskite quantum wells have attracted attention due to their tunable emission properties, ease of fabrication, and device integration. However, the dynamics of excitons in these materials, especially how they couple to phonons, remains an open question. Here, we investigate two widely used materials, namely, butylammonium lead iodide (CH 3 (CH 2 ) 3 NH 3 ) 2 PbI 4 and hexylammonium lead iodide (CH 3 (CH 2 ) 5 NH 3 ) 2 PbI 4 , both of which exhibit broad photoluminescence tails at room temperature. We performed femtosecond vibrational spectroscopy to obtain a real-time picture of the exciton-phonon interaction and directly identified the vibrational modes that couple to excitons. We show that the choice of the organic cation controls which vibrational modes the exciton couples to. In butylammonium lead iodide, excitons dominantly couple to a 100 cm -1 phonon mode, whereas in hexylammonium lead iodide, excitons interact with phonons with frequencies of 88 and 137 cm -1 . Using the determined optical phonon energies, we analyzed photoluminescence broadening mechanisms. At low temperatures (<100 K), the broadening is due to acoustic phonon scattering, whereas at high temperatures, LO phonon-exciton coupling is the dominant mechanism. Our results help explain the broad photoluminescence line shape observed in hybrid perovskite quantum wells and provide insights into the mechanism of exciton-phonon coupling in these materials.