Ramez Cheaito

Crossover from incoherent to coherent phonon scattering in epitaxial oxide superlattices

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.

A frequency-domain thermoreflectance method for the characterization of thermal properties

A frequency-domain thermoreflectance method for measuring the thermal properties of homogenous materials and submicron thin films is described. The method can simultaneously determine the thermal conductivity and heat capacity of a sample, provided the thermal diffusivity is greater, similar3x10(-6) m(2)/s, and can also simultaneously measure in-plane and cross-plane thermal conductivities, as well the thermal boundary conductance between material layers. Two implementations are discussed, one based on an ultrafast pulsed laser system and one based on continuous-wave lasers. The theory of the method and an analysis of its sensitivity to various thermal properties are given, along with results from measurements of several standard materials over a wide range of thermal diffusivities. We obtain specific heats and thermal conductivities in good agreement with literature values, and also obtain the in-plane and cross-plane thermal conductivities for crystalline quartz.

Extreme tunability in aluminum doped Zinc Oxide plasmonic materials for near-infrared applications

Plasmonic materials (PMs), featuring large static or dynamic tunability, have significant impact on the optical properties due to their potential for applications in transformation optics, telecommunications, energy, and biomedical areas. Among PMs, the carrier concentration and mobility are two tunable parameters, which control the plasma frequency of a metal. Here, we report on large static and dynamic tunability in wavelengths up to 640 nm in Al-doped ZnO based transparent conducting degenerate semiconductors by controlling both thickness and applied voltages. This extreme tunability is ascribed to an increase in carrier concentration with increasing thickness as well as voltage-induced thermal effects that eventually diminish the carrier concentration and mobility due to complex chemical transformations in the multilayer growth process. These observations could pave the way for optical manipulation of this class of materials for potential transformative applications.

Characterization of thin metal films via frequency-domain thermoreflectance

Frequency-domain thermoreflectance is extended to the characterization of thin metals films on low thermal diffusivity substrates. We show how a single noncontact measurement can yield both the thickness and thermal conductivity of a thin metal film with high accuracy. Results are presented from measurements of gold and aluminum films 20–100 nm thick on fused silica substrate. The thickness measurements are verified independently with atomic force microscope cross sections, and the thermal conductivity measurements are verified through electrical conductivity measurements via the Wiedemann–Franz law. The thermoreflectance thermal conductivity values are in good agreement with the Wiedemann–Franz results for all the films at least 30 nm thick, indicating that our method can be used to estimate electrical conductivity along with thermal conductivity for sufficiently thick films.

Thermal conductivity of nano-grained SrTiO3 thin films

We measure the thermal conductivities of nano-grained strontium titanate (ng-SrTiO3) films deposited on sapphire substrates via time-domain thermoreflectance. The 170 nm thick oxide films of varying grain-size were prepared from a chemical solution deposition process. We find that the thermal conductivity of ng-SrTiO3 decreases with decreasing average grain size and attribute this to increased phonon scattering at grain boundaries. Our data are well described by a model that accounts for the spectral nature of anharmonic Umklapp scattering along with grain boundary scattering and scattering due to the film thickness.

Influence of interfacial properties on thermal transport at gold:silicon contacts

We measure the Kapitza conductances at Au:Si contacts from 100 to 296 K via time-domain thermoreflectance. Contacts are fabricated by evaporating Au films onto Si substrates. Prior to Au deposition, the Si substrates receive pretreatments in order to modify interfacial properties, i.e., bonding and structural disorder. Through the inclusion of a Ti adhesion layer and the removal of the native oxide, Kapitza conductance can be enhanced by a factor of four at 296 K. Furthermore, interfacial roughness is found to have a negligible effect, which we attribute to the already low conductances of poorly bonded Au:Si contacts.

Enhanced room temperature electronic and thermoelectric properties of the dilute bismuthide InGaBiAs

We report room temperature electronic and thermoelectric properties of Si-doped In0.52Ga0.48BiyAs1−y with varying Bi concentrations. These films were grown epitaxially on a semi-insulating InP substrate by molecular beam epitaxy. We show that low Bi concentrations are optimal in improving the conductivity, Seebeck coefficient, and thermoelectric power factor, possibly due to the surfactant effects of bismuth. We observed a reduction in thermal conductivity with increasing Bi concentration, which is expected because of alloy scattering. We report a peak ZT of 0.23 at 300 K.

Protein Thermal Conductivity Measured in the Solid State Reveals Anharmonic Interactions of Vibrations in a Fractal Structure

Energy processes and vibrations in biological macromolecules such as proteins ultimately dictate biological, chemical, and physical functions in living materials. These energetic vibrations in the ribbon-like motifs of proteins interact on self-similar structures and fractal-like objects over a range of length scales of the protein (a few angstroms to the size of the protein itself, a few nanometers). In fact, the fractal geometries of protein molecules create a complex network of vibrations; therefore, proteins represent an ideal material system to study the underlying mechanisms driving vibrational thermal transport in a dense, fractal network. However, experimental studies of thermal energy transport in proteins have been limited to dispersive protein suspensions, which limits the knowledge that can be extracted about how vibrational energy is transferred in a pure protein solid. We overcome this by synthesizing solid, water-insoluble protein films for thermal conductivity measurements via time-domain thermoreflectance. We measure the thermal conductivity of bovine serum albumin and myoglobin solid films over a range of temperatures from 77 to 296 K. These temperature trends indicate that anharmonic coupling of vibrations in the protein is contributing to thermal conductivity. This first-ever observation of anharmonic-like trends in the thermal conductivity of a fully dense protein forms the basis of validation of seminal theories of vibrational energy-transfer processes in fractal objects.

Experimental evidence of excited electron number density and temperature effects on electron-phonon coupling in gold films

The electronic transport properties of metals with weak electron-phonon coupling can be influenced by non-thermal electrons. Relaxation processes involving non-thermal electrons competing with the thermalized electron system have led to inconsistencies in the understanding of how electrons scatter and relax with the less energetic lattice. Recent theoretical and computational works have shown that the rate of energy relaxation with the metallic lattice will change depending on the thermalization state of the electrons. Even though 20 years of experimental works have focused on understanding and isolating these electronic relaxation mechanisms with short pulsed irradiation, discrepancies between these existing works have not clearly answered the fundamental question of the competing effects between non-thermal and thermal electrons losing energy to the lattice. In this work, we demonstrate the ability to measure the electron relaxation for varying degrees of both electron-electron and electron-phonon thermalization. This series of measurements of electronic relaxation over a predicted effective electron temperature range up to ∼3500 K and minimum lattice temperatures of 77 K validate recent computational and theoretical works that theorize how a nonequilibrium distribution of electrons transfers energy to the lattice. Utilizing this wide temperature range during pump-probe measurements of electron-phonon relaxation, we explain discrepancies in the past two decades of literature of electronic relaxation rates. We experimentally demonstrate that the electron-phonon coupling factor in gold increases with increasing lattice temperature and laser fluences. Specifically, we show that at low laser fluences corresponding to small electron perturbations, energy relaxation between electrons and phonons is mainly governed by non-thermal electrons, while at higher laser fluences, non-thermal electron scattering with the lattice is less influential on the energy relaxation mechanisms.

Thermal boundary conductance across metal-gallium nitride interfaces from 80 to 450 K

Thermal boundary conductance is of critical importance to gallium nitride (GaN)-based device performance. While the GaN-substrate interface has been well studied, insufficient attention has been paid to the metal contacts in the device. In this work, we measure the thermal boundary conductance across interfaces of Au, Al, and Au-Ti contact layers and GaN. We show that in these basic systems, metal-GaN interfaces can impose a thermal resistance similar to that of GaN-substrate interfaces. We also show that these thermal resistances decrease with increasing operating temperature and can be greatly affected by inclusion of a thin adhesion layers.