arXiv subjects

Richard B. Wilson

Publications and source records attributed to Richard B. Wilson.

16 recordsLinked to original sources

arXiv2025

Strong Temperature Dependence of Thermal Conductivity in High-Purity Cubic Boron Arsenide

Materials with high thermal conductivity are needed to conduct heat away from hot spots in high power electronics and optoelectronic devices. Cubic boron arsenide (c-BAs) has a high thermal conductivity due to its special phonon dispersion relation. Previous experimental studies of c-BAs report a room-temperature thermal conductivity between 1000 and 1300 W m-1 K-1. We synthesized high purity isotopically enriched c-BAs single crystals with room-temperature thermal conductivity of around 1500 W m-1 K-1. Using time-domain thermoreflectance (TDTR), we measured thermal conductivity and found a 1/T2 temperature dependence between 300 K and 600 K - slightly stronger than predictions from state-of-the-art theoretical models. Brillouin and Raman scattering revealed minimal changes in phonon frequencies over the same temperature range, suggesting that the observed 1/T2 dependence is not caused by temperature dependent changes in phonon dispersion. To probe defect densities in the BAs crystals we studied, we conducted transient reflectivity microscopy (TRM) measurements of absorption at sub-bandgap photon energies. We observe a correlation between TRM signal intensity and thermal conductivity. Notably, samples with thermal conductivity near 1500 W m-1 K-1 still exhibited nonzero TRM signals, suggesting the presence of defects despite the high thermal conductivity.

cond-mat.mtrl-sci↗

arXiv2025

Acoustic Phonon Characteristics of Gallium Oxide Single Crystals Investigated with Brillouin-Mandelstam Light Scattering Spectroscopy

We report an investigation of the bulk and surface acoustic phonons in gallium oxide ultra-wide bandgap single crystals along various crystallographic directions using Brillouin-Mandelstam spectroscopy. Pronounced anisotropy in the acoustic phonon dispersion and velocities was observed across different crystal orientations. The measured average acoustic phonon velocities for the crystallographic directions of interest are 5,250 m/s and 4,990 m/s. The surface acoustic phonons propagate approximately twice as slowly as the bulk acoustic phonons. Our results suggest that the anisotropy of heat conduction in gallium oxide results from the difference in phonon velocities rather than the phonon lifetime. The obtained information for bulk and surface acoustic phonons can be used for developing accurate theoretical models of phonon scattering and optimization of thermal and electrical transport in this technologically important ultra-wide bandgap semiconductor.

cond-mat.mtrl-sci↗

arXiv2025

Large spin accumulation signals in ultrafast magneto-optical experiments

Magneto-optical techniques have become essential tools in spintronics, enabling the investigation of spin dynamics in the ultrafast regime. A key challenge in this field has been to accurately isolate the contributions to magneto-optical signals of spin transport phenomena from the local magnetization dynamics. The contribution of transported and accumulated spins was long believed to be orders of magnitude smaller than that of the magnetization and thus previous approaches to disentangle these signals have relied on specific experimental designs, usually including thick metal layers. Here, we present experimental evidence demonstrating that the magneto-optical signal from ultrafast spin accumulations can, under certain conditions, be comparable to or even exceed that of the magnetic layer in a standard ultrafast demagnetization experiment. Our findings provide a new framework for accessing and isolating these spin accumulations, allowing for time and depth dependent probing of transported spin and/or orbital angular momentum.

cond-mat.mes-hall↗

arXiv2024

Ultrafast relaxation dynamics of excited carriers in metals: Simplifying the intertwined dependencies upon scattering strengths, phonon temperature, photon energy, and excitation level

Using the Boltzmann transport equation (BTE), we study the evolution of nonequilibrium carrier distributions in simple ($sp$) metals, assumed to have been instantaneously excited by an ultrafast laser pulse with photon energy $h ν$. The mathematical structure of the BTE scattering integrals reveals that $h ν$ is a natural energy scale for describing the dynamics. Normalizing all energy quantities by $h ν$ leads to a set of three unitless parameters -- $β/ δ$, $γ$, and $α$ -- that control the relaxation dynamics: $β/ δ$ is the normalized ratio of electron-phonon to electron-electron scattering strengths, $γ$ is the normalized phonon (lattice) temperature, and $α$ is the normalized absorbed energy density. Using this theory, we systematically investigate relaxation times for the high-energy part of the distribution ($τ_H$), energy transfer to the phonon subsystem ($τ_E$), and intracarrier thermalization ($τ_{th}$). In the linear region of response (valid when $α$ is sufficiently small), we offer heuristic descriptions of each of these relaxation times as functions of $β/ δ$ and $γ$. Our results as a function of excitation level $α$ show that many ultrafast experimental investigations lie in a transition region between low excitation (where the relaxation times are independent of $α$) and high excitation (where the two-temperature model of carrier dynamics is valid). Approximate boundaries that separate these three regions are described by simple expressions involving the normalized parameters of our model.

cond-mat.mtrl-sci↗

arXiv2023

Specular Inverse Faraday Effect in Transition Metals

The inverse Faraday effect is an opto-magnetic phenomenon that describes the ability of circularly polarized light to induce magnetism in solids. The capability of light to control magnetic order in solid state materials and devices is of interest for a variety of applications, such as magnetic recording, quantum computation and spintronic technologies. However, significant gaps in understanding about the effect persist, such as what material properties govern the magnitude of the effect in metals. In this work, we report time-resolved measurements of the specular inverse Faraday effect in non-magnetic metals, i.e., the magneto-optic Kerr effect induced by circularly polarized light. We measure this specular inverse Faraday effect in Cu, Pd, Pt, W, Ta, and Au at a laser wavelength of 783 nm. For Ta and W, we investigate both α and \{beta} phases. We observe that excitation of these metals with circularly polarized light induces significant circular dichroism. This nonlinear magneto-optical response to circularly polarized light is an order of magnitude larger in α-W than other metals, e.g., Pt, Au, and is greater than nearly all other reported values for IFE in other materials. Our results benchmark the range of IFE that can be observed in non-magnetic metals and provide insight into what material properties govern the inverse Faraday effect in metals.

cond-mat.mtrl-sci↗

arXiv2023

Optical and Acoustic Phonons in Turbostratic and Cubic Boron Nitride Thin Films on Diamond Substrates

We report an investigation of the bulk optical, bulk acoustic, and surface acoustic phonons in thin films of turbostratic boron nitride (t-BN) and cubic boron nitride (c-BN) grown on B-doped polycrystalline and single-crystalline diamond (001) and (111) substrates. The characteristics of different types of phonons were determined using Raman and Brillouin-Mandelstam light scattering spectroscopies. The atomic structure of the films was determined using high-resolution transmission electron microscopy (HRTEM) and correlated with the Raman and Brillouin-Mandelstam spectroscopy data. The HRTEM analysis revealed that the cubic boron nitride thin films consisted of a mixture of c-BN and t-BN phases, with c-BN being the dominant phase. It was found that while visible Raman spectroscopy provided information for characterizing the t-BN phase, it faced challenges in differentiating the c-BN phase either due to the presence of high-density defects or the overlapping of the Raman features with those from the B-doped diamond substrates. In contrast, Brillouin-Mandelstam spectroscopy clearly distinguishes the bulk longitudinal and surface acoustic phonons of the c-BN thin films grown on diamond substrates. Additionally, the angle-dependent surface Brillouin-Mandelstam scattering data show the peaks associated with the Rayleigh surface acoustic waves, which have higher phase velocities in c-BN films on diamond (111) substrates. These findings provide valuable insights into the phonon characteristics of the c-BN and diamond interfaces and have important implications for the thermal management of electronic devices based on ultra-wide-band-gap materials.

cond-mat.mtrl-sci↗

arXiv2023

Excitation and Relaxation of Nonthermal Electron Energy Distributions in Metals with Application to Gold

A semiempirical theory for the excitation and subsequent relaxation of nonthermal electrons is described. The theory, which is applicable to ultrafast-laser excited metals, is based on the Boltzmann transport equation for the carrier distribution function $f(ε,t)$ and includes electron-phonon, electron-electron, and electron-photon scattering integrals in forms that explicitly depend on the electronic density of states. Electron-phonon coupling is treated by extending the theory of Allen [Phys. Rev. Lett. 59, 1460 (1987)] to include highly-excited nonthermal electron distributions, and is used to determine the energy transfer rate between a nonthermal electron subsystem and a thermal phonon subsystem. Electron-electron scattering is treated with a simple energy-conserving electron-electron scattering integral. The electron-photon integral assumes photon absorption is phonon assisted. We apply the theory to analyze prior ultrafast thermionic emission, two-color photoemission, and electronic inelastic light (Raman) scattering experiments on Au. These analyses show that getting the details of $f(ε,t)$ is necessary for proper interpretation of each experiment. Together, the photoemission and Raman-scattering analyses indicate an electron excited 1 eV above the Fermi level has an electron-electron scattering time in the range of 25 to 55 fs.

cond-mat.mtrl-sci↗

arXiv2022

The Effects of Boron Doping on the Bulk and Surface Acoustic Phonons in Single-Crystal Diamond

We report the results of the investigation of bulk and surface acoustic phonons in the undoped and boron-doped single-crystal diamond films using the Brillouin-Mandelstam light scattering spectroscopy. The evolution of the optical phonons in the same set of samples was monitored with Raman spectroscopy. It was found that the frequency and the group velocity of acoustic phonons decrease non-monotonically with the increasing boron doping concentration, revealing pronounced phonon softening. The change in the velocity of the shear horizontal and the high-frequency pseudo-longitudinal acoustic phonons in the degenerately doped diamond, as compared to the undoped diamond, was as large as ~15% and ~12%, respectively. As a result of boron doping, the velocity of the bulk longitudinal and transverse acoustic phonons decreased correspondingly. The frequency of the optical phonons was unaffected at low boron concentration but experienced a strong decrease at the high doping level. The density-functional-theory calculations of the phonon band structure for the pristine and highly-doped sample confirm the phonon softening as a result of boron doping in diamond. The obtained results have important implications for thermal transport in heavily doped diamond, which is a promising material for ultra-wide-band-gap electronics.

cond-mat.mtrl-sci↗

arXiv2022

Magneto-optical Kerr spectra of gold induced by spin accumulation

We report the magneto optic Kerr effect (MOKE) angle of Au magnetically excited by spin accumulation. We perform time resolved polar MOKE measurements on Au/Co heterostructures. In our experiment, the ultrafast optical excitation of the Co drives spin accumulation into an adjacent Au layer. The spin accumulation, together with spin-orbit coupling, leads to non-zero terms in the off-diagonal conductivity tensor of Au, which we measure by recording the polarization and ellipticity of light reflected from the Au surface for photon energies between 1.3 and 3.1 eV. At energies near the interband transition threshold of Au, the Kerr rotation per A/m exceeds 1 urad. Typical values for Kerr rotation per moment in transition ferromagnetic metals like Ni are < 10 nrad per A/m, while predicted values for heavy metals like Pt or W are < 13 nrad per A/m. The exceptional sensitivity of the optical properties of Au to spin magnetic moments make Au to be an exceptionally sensitive optical magnetometer, with potential applications in the development of optospintronic technologies.

cond-mat.mtrl-sci↗

arXiv2021

Differentiating Contributions of Electrons and Phonons to the Thermoreflectance Spectra of Gold

To better understand the many effects of temperature on the optical properties of metals, we experimentally and theoretically quantify the electron vs. phonon contributions to the thermoreflectance spectra of gold. We perform a series of pump/probe measurements on nanoscale Pt/Au bilayers at wavelengths between 400 and 1000 nm. At all wavelengths, we find that changes in phonon temperature, not electron temperature, are the primary contributor to the thermoreflectance of Au. The thermoreflectance is most sensitive to the electron temperature at wavelength of ~480 nm due to interband transitions between d-states and the Fermi-level. In the near infrared, the electron temperature is responsible for only ~2% of the total thermoreflectance. We also compute the thermoreflectance spectra of Au from first principles. Our calculations further confirm that phonon temperature dominates thermoreflectance of Au. Most of Au's thermoreflectance is due to the effect of the phonon population on electron lifetime.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast Measurements of the Interfacial Spin Seebeck Effect in Au and Rare-Earth Iron Garnet Bilayers

We investigate picosecond spin-currents across Au/iron-garnet interfaces in response to ultrafast laser heating of the electrons in the Au film. In the picoseconds after optical heating, interfacial spin currents occur due to an interfacial temperature difference between electrons in the metal and magnons in the insulator. We report measurements of this interfacial longitudinal spin Seebeck effect between Au and rare-earth iron-garnet insulators, i.e. RE$_3$ Fe$_5$O$_{12}$, where RE is Y, Eu, Tb, Tm. We use time domain thermoreflectance (TDTR) measurements to characterize the thermal response of the bilayer to ultrafast optical heating. We use time-resolved magneto-optic Kerr effect (TR-MOKE) measurements of the Au layer to measure the time-evolution of spin accumulation in the Au film. We observe a spin Seebeck effect between Au/TmIG that is three times larger than for an Au/YIG bilayer. The interfacial thermal conductance between electrons in the Au and magnons in the TmIG layer is ~ 3 $\frac{MW}{m^2 K}$.

cond-mat.mtrl-sci↗

arXiv2021

Electron-Phonon Scattering governs both Ultrafast and Precessional Magnetization Dynamics in Co-Fe Alloys

Recent investigations have advanced the understanding of how structure-property relationships in ferromagnetic metal alloys affect the magnetization dynamics on nanosecond time-scales. A similar understanding for magnetization dynamics on femto- to pico-second time-scales does not yet exist. To address this, we perform time-resolved magneto optic Kerr effect (TRMOKE) measurements of magnetization dynamics in Co-Fe alloys on femto- to nano-second regimes. We show that Co-Fe compositions that exhibit low Gilbert damping parameters also feature prolonged ultrafast demagnetization upon photoexcitation. We analyze our experimental TR-MOKE data with the three-temperature-model (3TM) and the Landau-Lifshitz-Gilbert equation. These analyses reveal a strong compositional dependence of the dynamics across all time-scales on the strength of electron-phonon interactions. Our findings are beneficial to the spintronics and magnonics community, and will aid in the quest for energy-efficient magnetic storage applications.

cond-mat.mtrl-sci↗

arXiv2020

Picosecond Spin Orbit Torque Switching

Reducing energy dissipation while increasing speed in computation and memory is a long-standing challenge for spintronics research. In the last 20 years, femtosecond lasers have emerged as a tool to control the magnetization in specific magnetic materials at the picosecond timescale. However, the use of ultrafast optics in integrated circuits and memories would require a major paradigm shift. An ultrafast electrical control of the magnetization is far preferable for integrated systems. Here we demonstrate reliable and deterministic control of the out-of-plane magnetization of a 1 nm-thick Co layer with single 6 ps-wide electrical pulses that induce spin-orbit torques on the magnetization. We can monitor the ultrafast magnetization dynamics due to the spin-orbit torques on sub-picosecond timescales, thus far accessible only by numerical simulations. Due to the short duration of our pulses, we enter a counter-intuitive regime of switching where heat dissipation assists the reversal. Moreover, we estimate a low energy cost to switch the magnetization, projecting to below 1fJ for a (20 nm)^3 cell. These experiments prove that spintronic phenomena can be exploited on picosecond time-scales for full magnetic control and should launch a new regime of ultrafast spin torque studies and applications.

physics.app-ph↗

arXiv2020

Unifying femtosecond and picosecond single-pulse magnetic switching in GdFeCo

Many questions are still open regarding the physical mechanisms behind the magnetic switching in GdFeCo alloys by single optical pulses. Phenomenological models suggest a femtosecond scale exchange relaxation between sublattice magnetization as the driving mechanism for switching. The recent observation of thermally induced switching in GdFeCo by using both several picosecond optical laser pulse as well as electric current pulses has questioned this previous understanding. This has raised the question of whether or not the same switching mechanics are acting at the femo- and picosecond scales. In this work, we aim at filling this gap in the understanding of the switching mechanisms behind thermal single-pulse switching. To that end, we have studied experimentally thermal single-pulse switching in GdFeCo alloys, for a wide range of system parameters, such as composition, laser power and pulse duration. We provide a quantitative description of the switching dynamics using atomistic spin dynamics methods with excellent agreement between the model and our experiments across a wide range of parameters and timescales, ranging from femtoseconds to picoseconds. Furthermore, we find distinct element-specific damping parameters as a key ingredient for switching with long picosecond pulses and argue, that switching with pulse durations as long as 15 picoseconds is possible due to a low damping constant of Gd. Our findings can be easily extended to speed up dynamics in other contexts where ferrimagnetic GdFeCo alloys have been already demonstrated to show fast and energy-efficient processes, e.g. domain-wall motion in a track and spin-orbit torque switching in spintronics devices.

cond-mat.mtrl-sci↗

arXiv2017

Single shot ultrafast all optical magnetization switching of ferromagnetic Co/Pt multilayers

In a number of recent experiments, it has been shown that femtosecond laser pulses can control magnetization on picosecond timescales, which is at least an order of magnitude faster compared to conventional magnetization dynamics. Among these demonstrations, one material system (GdFeCo ferromagnetic films) is particularly interesting, as deterministic toggle-switching of the magnetic order has been achieved without the need of any symmetry breaking magnetic field. This phenomenon is often referred to as all optical switching (AOS). However, so far, GdFeCo remains the only material system where such deterministic switching has been observed. When extended to ferromagnetic systems, which are of greater interest in many technological applications, only a partial effect can be achieved, which in turn requires repeated laser pulses for full switching. However, such repeated pulsing is not only energy hungry, it also negates the speed advantage of AOS. Motivated by this problem, we have developed a general method for single-shot, picosecond timescale, complete all optical switching of ferromagnetic materials. We demonstrate that in exchange-coupled layers of Co/Pt and GdFeCo, single shot, switching of the ferromagnetic Co/Pt layer is achieved within 7 picoseconds after irradiation by a femtosecond laser pulse. We believe that this approach will greatly expand the range of materials and applications for ultrafast magnetic switching.

cond-mat.mes-hall↗

arXiv2016

The role of electron and phonon temperatures in the helicity-independent all-optical switching of GdFeCo

Ultrafast optical heating of the electrons in ferrimagnetic metals can result in all-optical switching (AOS) of the magnetization. Here we report quantitative measurements of the temperature rise of GdFeCo thin films during helicity-independent AOS. Critical switching fluences are obtained as a function of the initial temperature of the sample and for laser pulse durations from 55 fs to 15 ps. We conclude that non-equilibrium phenomena are necessary for helicity-independent AOS, although the peak electron temperature does not play a critical role. Pump-probe time-resolved experiments show that the switching time increases as the pulse duration increases, with 10 ps pulses resulting in switching times of ~sim 13 ps. These results raise new questions about the fundamental mechanism of helicity-independent AOS.

cond-mat.mes-hall↗