Boundary scattering of thermal phonons in thin solid films is typically analyzed using Fuchs-Sondheimer theory, which provides a simple equation to calculate the reduction of thermal conductivity as a function of the film thickness. However, this widely-used equation is not applicable to highly anisotropic solids like graphite because it assumes the phonon dispersion is isotropic. Here, we derive a generalization of the Fuchs-Sondheimer equation for solids with arbitrary dispersion relations and examine its predictions for graphite. We find that the isotropic equation vastly overestimates the boundary scattering that occurs in thin graphite films due to the highly anisotropic group velocity, and that graphite can maintain its high in-plane thermal conductivity even in thin films with thicknesses as small as ten nanometers.
Raman measurements of a Fano-type surface phonon mode associated with Dirac surface states (SS) in Bi2Se3 topological insulator thin films allowed an unambiguous determination of the electron-phonon coupling strength in Dirac SS as a function of film thickness ranging from 2 to 40 nm. A non-monotonic enhancement of the electron-phonon coupling strength with maximum for the 8 - 10 nm thick films was observed. The non-monotonicity is suggested to originate from plasmon-phonon coupling which enhances electron-phonon coupling when free carrier density in Dirac SS increases with decreasing film thi…
Transient reflectivity traces measured for nanometer-sized films of the topological insulator Bi2Se3 revealed GHz-range oscillations driven within the relaxation of hot carriers photoexcited with ultrashort laser pulses of 1.51 eV photon energy. These oscillations have been suggested to result from acoustic phonon dynamics, including coherent longitudinal acoustic phonons in the form of standing acoustic waves. An increase of oscillation frequency from ~35 to ~70 GHz with decreasing film thickness from 40 to 15 nm was attributed to the interplay between two different regimes employing travelin…
We have studied the absorption of electromagnetic radiation of an anisotropic quantum dot taking into account the spin-flip processes that is associated with the interaction of the electrons with optical phonons. It is shown that these processes lead to the resonance absorption. Explicit formula is derived for the absorption coefficient. The positions of the resonances peaks are found.
This study shows that the dielectric function of crystalline Si quantum wells (c-Si QW) is influenced by both carrier confinement and electron-phonon interactions. The energy shifts and lifetime broadening of the excitonic E1 direct gap transition of c-Si QWs from 2 to 10 nm are found to have a significant dimensional and temperature dependence that can be traced to changes in the phonon dispersion of nanoscale films. The influence of electron-phonon interactions on the dielectric function was verified by altering the phonon dispersion using different dielectric layers above a 5 nm c-Si QW.
We report direct visualization of gigahertz-frequency acoustic waves in lithium niobate phononic circuits. Primary propagation parameters, such as the power flow angle (PFA) and propagation loss (PL), are measured by transmission-mode microwave impedance microscopy (TMIM). Using fast Fourier transform, we can separately analyze forward and backward propagating waves and quantitatively evaluate the propagation loss. Our work provides insightful information on the propagation, diffraction, and attenuation in piezoelectric thin films, which is highly desirable for designing and optimizing phononi…
The thermal properties of anisotropic crystals are of both fundamental and practical interest, but transport phenomena in anisotropic materials such as graphite remain poorly understood because solutions of the Boltzmann equation often assume isotropy. Here, we extend an analytical solution of the Boltzmann equation to highly anisotropic solids and examine its predictions for graphite. We show that the phonon mean free paths in the cross-plane direction can be comparable to those in the in-plane direction despite the low cross-plane thermal conductivity, which instead arises primarily from the…
Interfacial electron-phonon coupling in ultrathin films has attracted much interest; it can give rise to novel effects and phenomena, including enhanced superconductivity. Here we report an observation of strong kinks in the energy dispersions of quantum well states in ultrathin Yb films grown on graphite. These kinks, arising from interfacial electron-phonon coupling, are most prominent for films with a preferred ("magic") thickness of 4 monolayers, which are strained and hole doped by the substrate. The energy position of the kinks agrees well with the optical phonon energy of graphite, and …
We observe a crossover from electron-phonon (ep) coupling limited energy relaxation to that governed by thermal boundary resistance (pp) in copper films at sub-kelvin temperatures. Our measurement yields a quantitative picture of heat currents, in terms of temperature dependences and magnitudes, in both ep and pp limited regimes, respectively. We show that by adding a third layer in between the copper film and the substrate, the thermal boundary resistance is increased fourfold, consistent with an assumed series connection of thermal resistances.
We present a theoretical study of electron-phonon scattering effects in thin films made of a strong topological insulator. Phonons are modelled by isotropic elastic continuum theory with stress-free boundary conditions, and the interaction with the helical surface Dirac fermions is mediated by the deformation potential. We determine the temperature-dependent electrical resistivity $ρ(T)$ and the quasiparticle decay rate $Γ(T)$ observable in photoemission. The low- and high-temperature power laws for both quantities are obtained analytically. Detailed estimates covering the full temperature ran…
We consider the deformation potential mechanism of the electron-phonon coupling in metal films and investigate the intensity of the associated heat transfer between the electron and phonon subsystems. The focus is on the temperature region below dimensional crossover $T<T^{\ast}$ where the thermally relevant vibrations are described in terms of a quasi-two-dimensional elastic medium, while electron excitations behave as a three-dimensional Fermi gas. We derive an explicit expression for the power $P\left( T\right) $ of the electron-phonon heat transfer which explains the behavior observed in s…
We report on a >100-fold enhancement of Raman responses from Bi2Se3 thin films if laser photon energy switches from 2.33 eV (532 nm) to 1.58 eV (785 nm), which is due to direct optical coupling to Dirac surface states (SS) at the resonance energy of ~1.5 eV (a thickness-independent enhancement) and due to nonlinearly excited Dirac plasmon (a thickness-dependent enhancement). Owing to the direct optical coupling, we observed an in-plane phonon mode of hexagonally arranged Se-atoms associated with a continuous network of Dirac SS. This mode revealed a Fano lineshape for films <15 nm thick, resul…
We study the anisotropic orbital effect in the electric field tunability of the phonon induced spin-flip rate in quantum dots (QDs). Our study shows that anisotropic gate potential enhances the spin-flip rate and reduces the level crossing point to a lower quantum dot radius due to the suppression of the Land$\acute{e}$ g-factor towards bulk crystal. In the range of $10^4-10^6$ V/cm, the electric field tunability of the phonon induced spin-flip rate can be manipulated through strong Dresselhaus spin-orbit coupling. These results might assist the development of a spin based solid state quantum …
In this paper, a detailed analysis of anisotropic effects on the phonon induced spin relaxation rate in III-V semiconductor quantum dots (QDs) is carried out. We show that the accidental degeneracy due to level crossing between the first and second excited states of opposite electron spin states in both isotropic and anisotropic QDs can be manipulated with the application of externally applied gate potentials. In particular, anisotropic gate potentials enhance the phonon mediated spin-flip rate and reduce the cusp-like structure to lower magnetic fields, in addition to the lower QDs radii in I…
We combine femtosecond electron diffuse scattering experiments and first-principles calculations of the coupled electron-phonon dynamics to provide a detailed momentum-resolved picture of the ultrafast lattice thermalization in a thin film of black phosphorus. The measurements reveal the emergence of highly anisotropic non-thermal phonon populations which persist for several picoseconds following excitation of the electrons with a light pulse. Combining ultrafast dynamics simulations based on the time-dependent Boltzmann formalism and calculations of the structure factor, we reproduce the expe…
Thermal transport by phonons in films with thicknesses of less than 10 nm is investigated in a soft system (Lennard-Jones argon) and a stiff system (Tersoff silicon) using two-dimensional lattice dynamics calculations and the Boltzmann transport equation. This approach uses a unit cell that spans the film thickness, which removes approximations related to the finite cross-plane dimension required in typical three-dimensional-based approaches. Molecular dynamics simulations are performed to obtain finite-temperature structures for the lattice dynamics calculations and to predict thermal conduct…
Ultrahigh-frequency acoustic-phonon resonators usually require atomically flat interfaces to avoid phonon scattering and dephasing, leading to expensive fabrication processes, such as molecular beam epitaxy. In contrast, mesoporous thin films are based on inexpensive wet chemical fabrication techniques. Here, we report mesoporous titanium dioxide-based acoustic resonators with resonances up to 90 GHz, and quality factors from 3 to 7. Numerical simulations show a good agreement with the picosecond ultrasonics experiments. We also numerically study the effect of changes in the speed of sound on …
We present the results of Monte-Carlo studies of the non-equilibrium properties of ferromagnetic Heisenberg films. Aging effects were observed in non-equilibrium critical behavior. The calculations were carried out for both high-temperature and low-temperature initial states. The characteristic correlation time, which diverges at the transition temperature in the thermodynamic limit, was obtained as a function of system size and waiting time.
This work reports on the first-time study of the temperature-dependent behavior of the Lorenz number of bio-supported average 3.2 nm-thin Ir film down to 10 K. Due to the strong imperfection-electron scattering, a very large residual resistivity is observed for the film that dominates the overall electron transport. The Debye temperature (221 K)of the film is found much smaller than that of bulk (308 K). This phonon softening strongly confirms the extensive surface and grain boundary electron scatterings. More than one order of magnitude reduction is observed for the thermal conductivity of th…
The two-temperature model (2TM) introduced by Kaganov, Lifshitz, and Tanatarov is widely used to describe the energy relaxation in the electron-phonon system of a metallic film. At the same time, the accuracy of the description of the electron-phonon system in terms of 2TM, i.e. on the basis of the electron and phonon temperatures, has not been considered in detail until now. In this paper we present a microscopic theory of cooling of instantly heated electrons in metallic films. In framework of this theory the main features of electron cooling in thick and thin films were found, and an analys…
Quasiparticle theory gives a local relation between heat current and temperature gradient, provided the quasiparticle mean free path is smaller than the scale of variation of temperature. When mean free paths are comparable to sample size, the relation becomes non-local. This non-local relation is formulated for phonon carriers; an explicit form is found in the approximation where current relaxation rates are replaced by quasiparticle relaxation rates. A quasiparticle definition of local temperature is offered. To extract the spatial variation of the temperature gradient requires inverting the…
We theoretically investigate pumping of phonons by the dynamics of a magnetic film into a non-magnetic contact. The enhanced damping due to the loss of energy and angular momentum shows interference patterns as a function of resonance frequency and magnetic film thickness that cannot be described by viscous ("Gilbert") damping. The phonon pumping depends on magnetization direction as well as geometrical and material parameters and is observable, e.g., in thin films of yttrium iron garnet on a thick dielectric substrate.
For a ultrathin NiO(001) film of 4 monolayers (ML) thickness grown on Ag(001), the vibrational properties have been determined by high-resolution electron energy loss spectroscopy (HREELS). For the well-ordered pseudomorphically grown film, nine phonon modes have been identified and their dispersions have been revealed along the Gamma-X high-symmetry direction. The comparison with phonon data for a 25 ML thick NiO(001) film shows that the NiO (001) phonon properties are already fully developed at 4 ML. Significant differences are found for the surface-localized phonon S6 which has an increased…
At micro- to nano-scales, classical size effects in heat conduction play an important role in suppressing the thermal transport process. Such effects occur when the characteristic lengths become commensurate to the mean free paths (MFPs) of heat carriers that are mainly phonons for nonmetallic crystals. Beyond existing experimental efforts on thin films using laser-induced thermal gratings, this work provides the complete theoretical analysis for a new approach to extract the effective phonon MFP distribution for the in-plane heat conduction within a thin film or flake-like sample. In this app…
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 [J. M. 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 valida…
We present a study of the structural and electronic properties of ultra-nanocrystalline diamond films that were modified by adding nitrogen to the gas mixture during chemical vapour deposition growth. Hall bar devices were fabricated from the resulting films to investigate their electrical conduction as a function of both temperature and magnetic field. Through low-temperature magnetoresistance measurements, we present strong evidence that the dominant conduction mechanism in these films can be explained by a combination of 3D weak localization (3DWL) and thermally activated hopping at higher …
We investigate spin-charge conversion phenomena in hybrid structures of topological insulator (TI) thin films and magnetic insulators. We find an anisotropic inverse spin-galvanic effect (ISGE) that yields a highly tunable spin-orbit torque (SOT). Concentrating on the quasiballistic limit, we also predict a giant anisotropic magnetoresistance (AMR) at low dopings. These effects, which have no counterparts in thick TIs, depend on the simultaneous presence of the hybridization between the surface states and the in-plane magnetization. Both the ISGE and AMR exhibit a strong dependence on the magn…
We present a first-principles study of the cross-plane thermal conductivity $κ_{\perp}$ in a wide variety of semiconductor thin films. We introduce a simple suppression model that matches variance-reduced Monte Carlo simulations with ab-initio phonon dispersions and scattering rates within $\leq 5\%$ even for anisotropic compounds. This, in turn, enables accurate $κ_{\perp}$ reconstruction from tabulated cumulative conductivity curves $κ_Σ(Λ_{\perp})$. We furthermore reveal, and explain, a distinct quasiballistic regime characterised by a fractional thickness dependence $κ_{\perp} \sim L^{2-α}…
We developed the model of the internal phonon bottleneck to describe the energy exchange between the acoustically soft ultrathin metal film and acoustically rigid substrate. Discriminating phonons in the film into two groups, escaping and nonescaping, we show that electrons and nonescaping phonons may form a unified subsystem, which is cooled down only due to interactions with escaping phonons, either due to direct phonon conversion or indirect sequential interaction with an electronic system. Using an amplitude-modulated absorption of the sub-THz radiation technique, we studied electron-phono…
Anisotropic phonon transport along different lattice directions of two-dimensional (2D) materials has been observed, however, the effect decreases with increasing the thickness beyond a few atomic layers. Here we establish a novel mechanism to induce anisotropic phonon transport in quasi-2D materials with isotropic symmetry. The phonon propagation is guided by resonance hybridization with surface nanostructures. We demonstrate that the thermal conductivity of 3 nm-thick silicon membrane with surface nanofins is greater by $\sim50\%$ parallel to the fins than that perpendicular to the fins.
Ultrathin FeSe films grown on SrTiO$_{3}$ substrates are a recent milestone in atomic material engineering due to their important role in understanding unconventional superconductivity in Fe-based materials. Using femtosecond time- and angle-resolved photoelectron spectroscopy, we study phonon frequencies in ultrathin FeSe/SrTiO$_{3}$ films grown by molecular beam epitaxy. After optical excitation, we observe periodic modulations of the photoelectron spectrum as a function of pump-probe delay for 1 unit cell, 3 unit cell, and 60 unit cell thick FeSe films. The frequencies of the coherent inten…
NiO thin films with various strains were grown on SrTiO3 (STO) and MgO substrates using a pulsed laser deposition technique. The films were characterized using an x-ray diffractometer, atomic force microscopy, and infrared reflectance spectroscopy. The films grown on STO (001) substrate show a compressive in-plane strain which increases as the film thickness is reduced, resulting in an increase of the NiO phonon frequency. On the other hand, a tensile strain was detected in the NiO film grown on MgO (001) substrate which induces a softening of the phonon frequency. Overall, the variation of in…
Acoustic and Optical Phonon Frequencies and Acoustic Phonon Velocities in Silicon-Doped Aluminum Nitride Thin Films
University of California, Los Angeles（加州大学洛杉矶分校）；California NanoSystems Institute, University of California, Los Angeles（加州大学洛杉矶分校加利福尼亚纳米系统研究所）；Arizona State University（亚利桑那州立大学）；Auburn University（奥本大学）
We have measured directly the thermal conductance between electrons and phonons in ultra-thin Hf and Ti films at millikelvin temperatures. The experimental data indicate that electron-phonon coupling in these films is significantly suppressed by disorder. The electron cooling time $τ_ε$ follows the $T^{-4}$-dependence with a record-long value $τ_ε=25ms$ at $T=0.04K$. The hot-electron detectors of far-infrared radiation, fabricated from such films, are expected to have a very high sensitivity. The noise equivalent power of a detector with the area $1\mum^2$ would be $(2-3)10^{-20}W/Hz^{1/2}$, w…
We use the time-resolved magneto-optical Kerr effect (TRMOKE) to measure the local temperature and heat flow dynamics in ferromagnetic SrRuO3 thin films. After heating by a pump pulse, the film temperature decays exponentially, indicating that the heat flow out of the film is limited by the film/substrate interface. We show that this behavior is consistent with an effective boundary resistance resulting from disequilibrium between the spin and phonon temperatures in the film.
We have studied the electron-phonon (e-p) interaction in thin Cu and Au films at sub-Kelvin temperatures with the help of the hot electron effect, using symmetric normal metal-insulator-superconductor tunnel junction pairs as thermometers. By Joule heating the electron gas and measuring the electron and the lattice temperatures simultaneously, we show that the electron-phonon scattering rate follows a $T^{4}$ temperature dependence in both metals. The result is in accordance with the theory of e-p scattering in disordered films with vibrating boudaries and impurities, in contrast to the $T^{3}…
We explore the phonon dynamics of thin films of the topological insulator material Bi2Se2Te using ultrafast pump-probe spectroscopy. The time resolved differential reflectivity of the films exhibit fast and slow oscillations. We have given a careful analysis of variation of phonon frequency as a function of film thickness attributing this to existence of standing acoustic modes. However, no variation in the frequency of the optical phonon modes was found with film thickness. This indicates that the optical phonons intrinsically belong to the surface of the topological insulators. The fact that…
We report on the phonon and thermal properties of thin films of tantalum diselenide (2H-TaSe2) obtained via the graphene-like mechanical exfoliation of crystals grown by chemical vapor transport. The ratio of the intensities of the Raman peak from the Si substrate and the E2g peak of TaSe2 presents a convenient metric for quantifying film thickness. The temperature coefficients for two main Raman peaks, A1g and E2g, are -0.013 and -0.0097 cm-1/oC, respectively. The Raman optothermal measurements indicate that the room temperature thermal conductivity in these films decreases from its bulk valu…
Although extensive experimental and theoretical works have been conducted to understand the ballistic and diffusive phonon transport in nanomaterials recently, direct observation of temperature and thermal nonequilibrium of different phonon modes has not been realized. Herein, we have developed a method within the framework of molecular dynamics to calculate the temperatures of phonon in both real and phase spaces. Taking silicon thin film and graphene as examples, we directly obtained the spectral phonon temperature (SPT) and observed the local thermal nonequilibrium between the ballistic and…
We present a comparative investigation of the influence of crystallinity and film thickness on the acoustic and thermal properties of 2D layered PtSe2 thin films of varying thickness (0.6-24 nm) by combining a set of experimental techniques, namely, frequency domain thermo-reflectance, low-frequency Raman and pump-probe coherent phonon spectroscopy. We find a 35% reduction in the cross-plane thermal conductivity of polycrystalline films with thickness larger than 12 nm compared to the crystalline films of the same thickness due to phonon grain boundary scattering. Density functional theory cal…
We present the observation of strain induced sign reversal of anisotropic magnetoresistance (AMR) in LCMO (LCMO) ultrathin films (thickness 4 nm) deposited on STO (001) substrate (STO). We have also observed unusually large AMR in LCMO/STO thin films with thickness of 6 nm below but close to its Curie temperature (TC) which decrease as the film thickness increases. The sign reversal of AMR (with a maximum value of - 6) with magnetic field or temperature for the 4 nm thin film may be attributed to the increase in tensile strain in the plane of the thin film which in turn facilitates the rotatio…
Quantum wells made of simple polyvalent metals represent a novel family of doped 2D Mott-Hubbard insulators. As scanning tunneling microscopy experiments show, these systems exhibit an anisotropic form of metal-insulator transition. Their elementary excitations possess coherent wave-like properties along the normal axis, and show an incoherent behavior in-plane. The development of such an anisotropic coherence is most likely related to Coulomb interaction between localized and delocalized thin film electronic states - 2D Kondo screening.
We have used symmetric normal metal-insulator-superconductor (NIS) tunnel junction pairs, known as SINIS structures, for ultrasensitive thermometry in the temperature range 50 - 700 mK. By Joule heating the electron gas and measuring the electron temperature, we show that the electron-phonon (e-p) scattering rate in the simplest noble metal disordered thin films (Cu,Au) follows a $T^4$ temperature dependence, leading to a stronger decoupling of the electron gas from the lattice at the lowest temperatures. This power law is indicative e-p coupling mediated by vibrating disorder, in contrast to …
The influence of size effects on the thermoelectric properties of thin platinum films is investigated and compared to the bulk. Structural properties, like the film thickness and the grain size, are varied. We correlate the electron mean free path with the temperature dependence of the electrical conductivity and the absolute Seebeck coefficient $S_{\text{Pt}}$ of platinum. We use a measurement platform as a standardized method to determine $S_{\text{Pt}}$ and show that $S_{\text{Pt,film}}$ is reduced compared to $S_{\text{Pt,bulk}}$. Boundary and surface scattering reduce the thermodiffusion …
A femtosecond laser-irradiated crystallizing technique is tried to convert amorphous Sb2Te3 film into crystalline film. Sensitive coherent phonon spectroscopy (CPS) is used to monitor the crystallization of amorphous Sb2Te3 film at the original irradiation site. The CPS reveals that the vibration strength of two phonon modes that correspond to the characteristic phonon modes of crystalline Sb2Te3, enhances with increasing laser irradiation fluence (LIF), showing the rise of the degree of crystallization with LIF and that femtosecond laser irradiation is a good post-treatment technique. Time-re…
We investigate the transient photoexcited lattice dynamics in a layered perovskite Mott insulator Sr2IrO4 by femtosecond X-ray diffraction using a laser plasma-based X-ray source. Ultrafast structural dynamics of Sr2IrO4 thin films are determined by observing the shift and broadening of the (0012) Bragg diffraction after excitation by 1.5 eV and 3.0 eV pump photons for films with different thicknesses. The observed transient lattice response can be well interpreted as a distinct three-step dynamics due to the propagation of coherent acoustic phonons generated by the photoinduced quasiparticles…
The temperature and thickness dependencies of the in-plane anisotropic magnetoresistance (AMR) of SmB$_6$ thin films are reported. We find that the AMR changes sign from negative ($ρ_{||}<ρ_{\perp}$) at high temperatures to positive ($ρ_{||}>ρ_{\perp}$) at low temperatures. The temperature, T$_s$, at which this sign change occurs, decreases with increasing film thickness $t$ and T$_s$ vanishes for $t$ $>$ 30 nm. We interpret our results in the framework of a competition between two components: a negative bulk contribution and a positive surface AMR.
We report experimental evidence of charge density wave (CDW) transition in monolayer 1T-VTe$_2$ film. 4$\times$4 reconstruction peaks are observed by low energy electron diffraction below the transition temperature $T_{CDW}$ = 186 K. Angle-resolved photoemission spectroscopy measurements reveal arc-like pockets with anisotropic CDW gaps up to 50 meV. The anisotropic CDW gap is attributed to the imperfect nesting of the CDW wave vector, and first-principles calculations reveal phonon softening at the same vector, suggesting the important roles of Fermi surface nesting and electron-phonon intera…
Few-layer flakes of hexagonal boron nitride were prepared by ultrasonication of bulk crystals and agglomerated to form thin films. The transmission and reflection spectra of the thin films were measured. The spectral dependences of the linear and circular polarization revealed a hidden anisotropy of the films over the whole sample area which could not be explained by the anisotropy of the chaotically-oriented individual particles. Statistical analysis of optical microscopy images showed a macroscopic particle density distribution with ordering corresponding to the optical axis observed in the …
Observation of the Optical Phonons in α-MnTe films
University of Central Florida（中佛罗里达大学）；Nanoscience Technology Center, University of Central Florida（中佛罗里达大学纳米科学技术中心）；Department of Materials Science and Engineering, University of Central Florida（中佛罗里达大学材料科学与工程系）；Institute of Low Temperature and Structure Research, Polish Academy of Sciences（波兰科学院低温与结构研究所）；Institute of Nuclear Physics, Polish Academy of Sciences（波兰科学院核物理研究所）
We study the heat relaxation in current biased metallic films in the regime of strong electron-phonon coupling. A thermal gradient in the direction normal to the film is predicted, with a spatial temperature profile determined by the temperature-dependent heat conduction. In the case of strong phonon scattering the heat conduction occurs predominantly via the electronic system and the profile is parabolic. This regime leads to the linear dependence of the noise temperature as a function of voltage bias, in spite of the fact that all the dimensions of the film are large compared to the electron…
