arXiv subjects

David G. Cahill

Publications and source records attributed to David G. Cahill.

At least 37 records · Page 2Linked to original sources

arXiv2021

Thermal Visualization of Buried Interfaces by Transient and Steady-State Responses of Time-Domain Thermoreflectance

Thermal resistances from interfaces impede heat dissipation in micro/nanoscale electronics, especially for high-power electronics. Despite the growing importance of understanding interfacial thermal transport, advanced thermal characterization techniques which can visualize thermal conductance across buried interfaces, especially for nonmetal-nonmetal interfaces, are still under development. This work reports a dual-modulation-frequency TDTR mapping technique to visualize the thermal conduction across buried semiconductor interfaces for beta-Ga2O3-SiC samples. Both the beta-Ga2O3 thermal conductivity and the buried beta-Ga2O3-SiC thermal boundary conductance (TBC) are visualized for an area of 200 um x 200 um. Areas with low TBC values ( smaller than 20 MW/m2-K) are successfully identified on the TBC map, which correspond to weakly bonded interfaces caused by high-temperature annealing. The steady-state temperature rise (detector voltage), usually ignored in TDTR measurements, is found to be able to probe TBC variations of the buried interfaces without the limit of thermal penetration depth. This technique can be applied to detect defects/voids in deeply buried heterogeneous interfaces non-destructively, and also opens a door for the visualization of thermal conductance in nanoscale nonhomogeneous structures.

cond-mat.mtrl-sci↗

arXiv2021

Good Solid-State Electrolytes Have Low, Glass-like Thermal Conductivity

Management of heat during charging and discharging of Li-ion batteries is critical for their safety, reliability, and performance. Understanding the thermal conductivity of the materials comprising batteries is crucial for controlling the temperature and temperature distribution in batteries. This work provides systemic quantitative measurements of the thermal conductivity of three important classes of solid electrolytes (oxides, sulfides, and halides) over the temperature range 150-350 K. Studies include the oxides Li1.5Al0.5Ge1.5(PO4)3 and Li6.4La3Zr1.4Ta0.6O12, sulfides Li2S-P2S5, Li6PS5Cl, and Na3PS4, and halides Li3InCl6 and Li3YCl6. Thermal conductivities of sulfide and halide solid electrolytes are in the range 0.45-0.70 W m-1 K-1; thermal conductivities of Li6.4La3Zr1.4Ta0.6O12 and Li1.5Al0.5Ge1.5(PO4)3 are 1.4 W m-1 K-1 and 2.2 W m-1 K-1, respectively. For most of the solid electrolytes studied in this work, the thermal conductivity increases with increasing temperature; i.e., the thermal conductivity has a glass-like temperature dependence. The measured room-temperature thermal conductivities agree well with the calculated minimum thermal conductivities indicating the phonon mean-free-paths in these solid electrolytes are close to an atomic spacing. We attribute the low, glass-like thermal conductivity of the solid electrolytes investigated to the combination of their complex crystal structures and the atomic-scale disorder induced by the materials processing methods that are typically needed to produce high ionic conductivities.

cond-mat.mtrl-sci↗

arXiv2021

Thermal Conductivity Mapping of Oxidized SiC SiC Composites by Time Domain Thermoreflectance with Heterodyne Detection

Silicon carbide silicon carbide (SiC SiC) composites are often used in oxidizing environments at high temperatures. Measurements of the thermal conductance of the oxide layer provide a way to better understand the oxidation process with high spatial resolution. We use time domain thermoreflectance (TDTR) to map the thermal conductance of the oxide layer and the thermal conductivity of the SiC SiC composite with a spatial resolution of 3 μm. Heterodyne detection using a 50 kHz modulated probe beam and a 10 MHz modulated pump suppresses the coherent pick-up and enables faster data acquisition than what has previously been possible using sequential demodulation. By analyzing the noise of the measured signals, we find that in the limit of small integration time constants or low laser powers, the dominant source of noise is the input noise of the preamplifier. The thermal conductance of the oxide that forms on the fiber region is lower than the oxide on the matrix due to small differences in thickness and thermal conductivity.

cond-mat.mtrl-sci↗

arXiv2020

Polar magneto-optical Kerr effect in antiferromagnetic M$_2$As (M=Cr, Mn, Fe) under an external magnetic field

Antiferromagnetic metals attract tremendous interest for memory applications due to their expected fast response dynamics in the terahertz frequency regime. Reading from and writing information into these materials is not easily achievable using magnetic fields, due to weak high-order magneto-optical signals and robustness of the magnetic structure against external magnetic fields. Polarized electromagnetic radiation is a promising alternative for probing their response, however, when ideal antiferromagnetic symmetry is present, this response vanishes. Hence, in this work we combine first-principles simulations with measurements of the polar magneto-optical Kerr effect under external magnetic fields, to study magneto-optical response of antiferromagnetic M$_2$As (M=Cr, Mn, and Fe). We devise a computational scheme to compute the magnetic susceptibility from total-energy changes using constraints on magnetic-moment tilting. Our predictions of the spectral dependence of polar magneto-optical Kerr rotation and ellipticity allow us to attribute these effects to breaking of the magnetic symmetry. We show that tilting affects the exchange interaction, while the spin-orbit interaction remains unaffected as the tilting angle changes. Our work provides understanding of the polar magneto-optical Kerr effect on a band structure level and underscores the importance of the magnetic susceptibility when searching for materials with large magneto-optical response.

cond-mat.mtrl-sci↗

arXiv2020

Effect of isotope disorder on the Raman spectra of cubic boron arsenide

Boron arsenide (c-BAs) is at the forefront of research on ultrahigh thermal conductivity materials. We present a Raman scattering study of isotopically tailored cubic boron arsenide single crystals for 11 isotopic compositions spanning the range from nearly pure c-$^{10}$BAs to nearly pure c-$^{11}$BAs. Our results provide insights on the effects of strong mass disorder on optical phonons and the appearance of two-mode behavior in the Raman spectra of mixed crystals. Strong isotope disorder also relaxes the one-phonon Raman selection rules, resulting in disorder-activated Raman scattering by acoustic phonons.

cond-mat.mtrl-sci↗

arXiv2020

Magnetocrystalline anisotropy of the easy-plane metallic antiferromagnet Fe$_2$As

Magnetocrystalline anisotropy is a fundamental property of magnetic materials that determines the dynamics of magnetic precession, the frequency of spin waves, the thermal stability of magnetic domains, and the efficiency of spintronic devices. We combine torque magnetometry and density functional theory calculations to determine the magnetocrystalline anisotropy of the metallic antiferromagnet Fe$_2$As. Fe$_2$As has a tetragonal crystal structure with the Néel vector lying in the (001) plane. We report that the four-fold magnetocrystalline anisotropy in the (001)-plane of Fe$_2$As is extremely small, ${K_{22}} = - 150~{\rm{ J/}}{\rm{m}^{\rm{3}}}$ at T = 4 K, much smaller than perpendicular magnetic anisotropy of ferromagnetic structure widely used in spintronics device. ${K_{22}}$ is strongly temperature dependent and close to zero at T > 150 K. The anisotropy ${K_1}$ in the (010) plane is too large to be measured by torque magnetometry and we determine ${K_1} = -830~{\rm{ kJ/}}{\rm{m}^{\rm{3}}}$ using first-principles density functional theory. Our simulations show that the contribution to the anisotropy from classical magnetic dipole-dipole interactions is comparable to the contribution from spin-orbit coupling. The calculated four-fold anisotropy in the (001) plane ${K_{22}}$ ranges from $- 292~{\rm{ J/}}{\rm{m}^{\rm{3}}}$ to $280~{\rm{ J/}}{\rm{m}^{\rm{3}}}$, the same order of magnitude as the measured value. We use ${K_1}$ from theory to predict the frequency and polarization of the lowest frequency antiferromagnetic resonance mode and find that the mode is linearly polarized in the (001)-plane with $f = $ 670 GHz.

cond-mat.mtrl-sci↗

arXiv2019

Non-Equilibrium Heat Transport in Pt and Ru Probed by an Ultrathin Co Thermometer

Non-equilibrium of electrons, phonons, and magnons in metals is a fundamental phenomenon in condensed matter physics and serves as an important driver in the field of ultrafast magnetism. In this work, we demonstrate that the magnetization of a sub-nm-thick Co layer with perpendicular magnetic anisotropy can effectively serve as a thermometer to monitor non-equilibrium dynamics in adjacent metals, Pt and Ru, via time-resolved magneto-optic Kerr effect. The temperature evolutions of the Co thermometer embedded in Pt layers of different thicknesses, 6-46 nm, are adequately described by a phenomenological three temperature model with a consistent set of materials parameters. We do not observe any systematic deviations between the model and the data that can be caused by a non-thermal distribution of electronic excitations. We attribute the consistently good agreement between the model and the data to strong electron-electron interaction in Pt. By using Pt/Co/Pt and Pt/Co/Pt/Ru structures, we determine the electron-phonon coupling parameters of Pt and Ru, g_ep(Pt)=(6+/-1)x10^17 W m-3 K-1 and g_ep(Ru)=(9+/-2)x10^17 W m-3 K-1. We also find that the length scales of non-equilibrium between electrons and phonons are l_ep=(Λ_e/g_ep)^1/2 =9 nm for Pt and 7 nm for Ru, shorter than their optical absorption depths, 11 and 13 nm, respectively. Therefore, the optically thick Pt and Ru layers show two steps of temperature rise: The initial jump of electron temperature that occurs within 1 ps is caused by direct optical excitation and electronic heat transport within a distance l_ep for the Co layer. The second temperature rise is caused by heat transport by electrons and phonons that are near thermal equilibrium. We contrast two-temperature modeling of heat transport in Pt an Ru films to calculations for Cu, which has a much longer non-equilibrium length scale, l_ep=63 nm.

cond-mat.mtrl-sci↗

arXiv2019

Thermal Conductivity of Oxide Tunnel Barriers in Magnetic Tunnel Junctions Measured by Ultrafast Thermoreflectance and Magneto-optic Kerr Effect Thermometry

Spin-dependent charge transport in magnetic tunnel junctions (MTJs) can be manipulated by a temperature gradient, which can be utilized for spintronic and spin caloritronic applications. Evaluation of the thermally induced phenomena requires knowledge of the temperature differences across the oxide tunnel barrier adjacent to the ferromagnetic (FM) leads. However, it is challenging to accurately measure thermal properties of an oxide tunnel barrier consisting of only a few atomic layers. In this work, we experimentally interrogate the temperature evolutions in Ru/oxide/FM/seed/MgO (oxide=MgO, MgAl2O4; FM=Co, CoFeB; seed=Pt, Ta) structures having perpendicular magnetic anisotropy using ultrafast thermometry. The Ru layer is optically thick and heated by ultrafast laser pulses; the subsequent temperature changes are monitored using thermoreflectance of Ru and magneto-optic Kerr effect (MOKE) of the FM layers. We independently measure the response times of Co and CoFeB magnetism using quadratic MOKE and obtain τem=0.2 ps for Co and 2 ps for CoFeB. These time scales are much shorter than the time scale of heat transport through the oxide tunnel barrier, which occurs at 10-3000 ps. We determine effective thermal conductivities of MgO and MgAl2O4 tunnel barriers in the range of 0.4-0.6 W m-1 K-1, comparable to an estimate of the series conductance of the Ru/oxide and oxide/FM interfaces and an order of magnitude smaller than the thermal conductivity of MgO thin films. We find that the electron-phonon thermal conductance near the tunnel barrier is only a factor of 5-12 larger than the thermal conductance of the oxide tunnel barrier. Therefore, the drop in the electronic temperature is approximately 20-30% larger than the drop in the phonon temperature across the tunnel barrier.

cond-mat.mtrl-sci↗

arXiv2019

Magneto-optic Response of the Metallic Antiferromagnet Fe$_{2}$As to Ultrafast Temperature Excursions

The linear magneto-optical Kerr effect (MOKE) is often used to probe magnetism of ferromagnetic materials, but MOKE cannot be applied to collinear antiferromagnets (AFs) due to the cancellation of sub-lattice magnetization. Magneto-optical constants that are quadratic in magnetization, however, provide an approach for studying AFs on picosecond time scales. Here, we combine transient measurements of optical reflectivity and birefringence to study the linear optical response of Fe$_{2}$As to small ultrafast temperature excursions. We performed temperature dependent pump-probe measurements on crystallographically isotropic (001) and anisotropic (010) faces of Fe$_{2}$As bulk crystals. We find the largest optical signals arise from changes in the index of refraction along the $z$-axis, i.e. perpendicular to the Néel vector. Both real and imaginary parts of the time-resolved optical birefringence rotation signal approximately follow the temperature dependence of the magnetic heat capacity, as expected if the changes in dielectric constants are dominated by contributions of exchange interactions to the dielectric constant. We conclude that under our experimental conditions, changes in the exchange interaction contribute more strongly to the temperature dependence of the magneto-optic constants than the Voigt effect.

cond-mat.mtrl-sci↗

arXiv2019

Anomalous Spin-Orbit Torques in Magnetic Single-Layer Films

Spin-orbit interaction (SOI) couples charge and spin transport, enabling electrical control of magnetization. A quintessential example of SOI-induced transport is the anomalous Hall effect (AHE), first observed in 1880, in which an electric current perpendicular to the magnetization in a magnetic film generates charge accumulation on the surfaces. Here we report the observation of a counterpart of the AHE that we term the anomalous spin-orbit torque (ASOT), wherein an electric current parallel to the magnetization generates opposite spin-orbit torques on the surfaces of the magnetic film. We interpret the ASOT as due to a spin-Hall-like current generated with an efficiency of 0.053+/-0.003 in Ni80Fe20, comparable to the spin Hall angle of Pt. Similar effects are also observed in other common ferromagnetic metals, including Co, Ni, and Fe. First principles calculations corroborate the order of magnitude of the measured values. This work suggests that a strong spin current with spin polarization transverse to magnetization can exist in a ferromagnet, despite spin dephasing. It challenges the current understanding of spin-orbit torque in magnetic/nonmagnetic bilayers, in which the charge-spin conversion in the magnetic layer has been largely neglected.

cond-mat.mes-hall↗

arXiv2018

Impact of thermal fluctuations on transport in antiferromagnetic semimetals

Recent demonstrations on manipulating antiferromagnetic (AF) order have triggered a growing interest in antiferromagnetic metal (AFM), and potential high-density spintronic applications demand further improvements in the anisotropic magnetoresistance (AMR). The antiferromagnetic semimetals (AFS) are newly discovered materials that possess massless Dirac fermions that are protected by the crystalline symmetries. In this material, a reorientation of the AF order may break the underlying symmetries and induce a finite energy gap. As such, the possible phase transition from the semimetallic to insulating phase gives us a choice for a wide range of resistance ensuring a large AMR. To further understand the robustness of the phase transition, we study thermal fluctuations of the AF order in AFS at a finite temperature. For macroscopic samples, we find that the thermal fluctuations effectively decrease the magnitude of the AF order by renormalizing the effective Hamiltonian. Our finding suggests that the insulating phase exhibits a gap narrowing at elevated temperatures, which leads to a substantial decrease in AMR. We also examine spatially correlated thermal fluctuations for microscopic samples by solving the microscopic Landau-Lifshitz-Gilbert equation finding a qualitative difference of the gap narrowing in the insulating phase. For both cases, the semimetallic phase shows a minimal change in its transmission spectrum illustrating the robustness of the symmetry protected states in AFS. Our finding may serve as a guideline for estimating and maximizing AMR of the AFS samples at elevated temperatures.

cond-mat.mes-hall↗

arXiv2016

Role of remote interfacial phonon (RIP) scattering in heat transport across graphene/SiO2 interfaces

Heat transfer across interfaces of graphene and polar dielectrics (e.g. SiO2) could be mediated by direct phonon coupling, as well as electronic coupling with remote interfacial phonons (RIPs). To understand the relative contribution of each component, we develop a new pump-probe technique, called voltage-modulated thermoreflectance (VMTR), to accurately measure the change of interfacial thermal conductance under an electrostatic field. We employed VMTR on top gates of graphene field-effect transistors and find that the thermal conductance of SiO2/graphene/SiO2 interfaces increases by up to ΔG=0.8 MW m-2 K-1 under electrostatic fields of <0.2 V nm-1 . We propose two possible explanations for the observed ΔG. First, since the applied electrostatic field induces charge carriers in graphene, our VMTR measurements could originate from heat transfer between the charge carriers in graphene and RIPs in SiO2. Second, the increase in heat conduction could be caused by better conformity of graphene interfaces un-der electrostatic pressure exerted by the induced charge carriers. Regardless of the origins of the observed ΔG, our VMTR measurements establish an upper limit for heat transfer from unbiased graphene to SiO2 substrates via RIP scattering; i.e., only <2 % of the interfacial heat transport is facilitated by RIP scattering even at a carrier concentration of 4x10^12 cm-2.

cond-mat.mes-hall↗

arXiv2016

Picosecond spin Seebeck effect

We report time-resolved magneto-optic Kerr effect measurements of the longitudinal spin Seebeck effect driven by an interfacial temperature difference between itinerant electrons and magnons. The measured time-evolution of spin accumulation induced by laser-excitation indicates transfer of angular momentum across Au/Y$_3$Fe$_5$O$_{12}$ and Cu/Y$_3$Fe$_5$O$_{12}$ interfaces on a picosecond time-scale. The product of spin-mixing conductance and interfacial spin Seebeck coefficient determined is of the order of $10^8$ A m$^{-2}$ K$^{-1}$.

cond-mat.mes-hall↗

arXiv2015

Anisotropic Thermal Conductivity of Exfoliated Black Phosphorus

We ascertain the anisotropic thermal conductivity of alumina passivated black phosphorus (BP), a reactive 2D nanomaterial with strong in-plane anisotropy. We measure the room temperature thermal conductivity by time-domain thermoreflectance for the three crystalline axes of exfoliated BP. The thermal conductivity along the zigzag direction (86 +/- 8 W/(m*K)) is ~2.5 times higher than that of the armchair direction (34 +/- 4 W/(m*K)).

cond-mat.mtrl-sci↗

arXiv2014

Micro- and Nano-scale Measurement Methods for Phase Change Heat Transfer on Planar and Structured Surfaces

In this opinion piece, we discuss recent advances in experimental methods for characterizing phase change heat transfer. We begin with a survey of techniques for high-resolution measurements of temperature and heat flux at the solid surface and in the working fluid. Next, we focus on diagnostic tools for boiling heat transfer and describe techniques for visualizing the temperature and velocity fields, as well as measurements at the single bubble level. Finally, we discuss techniques to probe the kinetics of vapor formation within a few molecular layers of the interface. We conclude with our outlook for future progress in experimental methods for phase change heat transfer.

cond-mat.mes-hall↗

arXiv2013

Compositionally-modulated Si1-xGex multilayers with cross-plane thermal conductivity below the thin-film alloy limit

We describe epitaxial Ge/Si multilayers with cross-plane thermal conductivities which can be systematically reduced to exceptionally low values, as compared both with bulk and thin-film SiGe alloys of the same average concentration, by simply changing the thicknesses of the constituent layers. Ab initio calculations reveal that partial interdiffusion of Ge into the Si spacers, which naturally results from Ge segregation during growth, plays a determinant role, lowering the thermal conductivity below what could be achieved without interdiffusion (perfect superlattice), or with total interdiffusion (alloy limit). This phenomenon is similar to the one previously observed in alloys with embedded nanoparticles, and it stresses the importance of combining alloy and nanosized scatterers simultaneously to minimize thermal conductivity. Our calculations thus suggest that superlattices with sharp interfaces, which are commonly sought but difficult to realize, are worse than compositionally-modulated Si1-xGex multilayers in the search for materials with ultralow thermal conductivities.

cond-mat.mtrl-sci↗

arXiv2010

High temperature thermoelectric response of double-doped SrTiO$_3$ epitaxial films

SrTiO$_3$ is a promising $n$-type oxide semiconductor for thermoelectric energy conversion. Epitaxial thin films of SrTiO$_3$ doped with both La and oxygen vacancies have been synthesized by pulsed laser deposition (PLD). The thermoelectric and galvanomagnetic properties of these films have been characterized at temperatures ranging from 300 K to 900 K and are typical of a doped semiconductor. Thermopower values of double-doped films are comparable to previous studies of La doped single crystals at similar carrier concentrations. The highest thermoelectric figure of merit ($ZT$) was measured to be 0.28 at 873 K at a carrier concentration of $2.5\times10^{21}$ cm$^{-3}$.

cond-mat.mtrl-sci↗

arXiv2010

Heat Conduction across Monolayer and Few-Layer Graphenes

We report the thermal conductance G of Au/Ti/graphene/SiO2 interfaces (graphene layers 1 < n < 10) typical of graphene transistor contacts. We find G ~ 25 MW m-2 K-1 at room temperature, four times smaller than the thermal conductance of a Au/Ti/SiO2 interface, even when n = 1. We attribute this reduction to the thermal resistance of Au/Ti/graphene and graphene/SiO2 interfaces acting in series. The temperature dependence of G from 50 < T < 500 K also indicates that heat is predominantly carried by phonons through these interfaces. Our findings indicate that metal contacts can limit not only electrical transport, but also thermal dissipation from sub-micron graphene devices.

cond-mat.mes-hall↗