arXiv subjects

Roland K. Kawakami

Publications and source records attributed to Roland K. Kawakami.

At least 19 recordsLinked to original sources

arXiv2026

Ultrafast Light-Induced Magnetoelectric Effect in van der Waals Magnetic Semiconductor Heterostructures

Atomic-scale heterostructures of van der Waals (vdW) magnets and semiconductors provide a unique environment for exploring magnetic dynamics. In contrast to typical photothermal excitation of precessional magnetization dynamics by a pump laser pulse, we find that ultrafast optical excitation of a WS$_2$/CrGeTe$_3$ (CGT) bilayer produces an opposite sign of magnetic torque compared to an isolated CGT film. Experimental observations by time-resolved magneto-optic Kerr effect (TR-MOKE) and theoretical analysis by density functional theory (DFT) and Landau-Lifshitz-Gilbert (LLG) simulations support a mechanism in which charge transfer of photoexcited carriers across the interface alters the perpendicular magnetic anisotropy, which in turn generates a torque on the magnetic layer to trigger precessional magnetization dynamics. These results provide new avenues for ultrafast manipulation of magnetization in vdW heterostructures with type-II band alignments. Lastly, we show that optically-generated spin currents from WS$_2$ into CGT can also trigger precessional dynamics via angular momentum transfer.

cond-mat.mes-hall↗

arXiv2026

Disentangling High Harmonic Generation from Surface and Bulk States of a Topological Insulator

The discovery of topological phases has introduced a new dimension to materials science. Three-dimensional (3D) topological insulators (TIs) are a remarkable class of matter that is insulating in the bulk while hosting conductive topological surface states (TSSs) with unique charge and spin properties. High-order harmonic generation (HHG) has emerged as a powerful tool to probe condensed matter systems by providing insights into their electronic structure and dynamic behavior. Here, we investigate HHG in the prototype 3D-TI Bi$_2$Se$_3$. We demonstrate that the contributions of bulk and surface states to the harmonic emission can be controlled by tuning the thickness of thin film samples. An ultrathin (6 nm) film substantially enhances HHG from the surface states, while the bulk states dominate HHG in a thicker (50 nm) film. By applying a quasi-static terahertz perturbing field, we disentangle the bulk and surface responses and reveal the significant impact of the surface states' shift vector and Berry curvature on HHG. Our study provides effective methods for isolating the optical responses of TSSs from those of the bulk, which opens the door to resolving an ongoing debate regarding whether it is possible to reliably extract topological signatures in HHG.

cond-mat.mes-hall↗

arXiv2025

Electrical Side-Gate Control of Anisotropic Magnetoresistance and Magnetic Anisotropy in a Composite Multiferroic

Composite multiferroics consisting of a ferroelectric material interfaced with a ferromagnetic material can function above room temperature and exhibit improved magnetoelectric (ME) coupling compared to single-phase multiferroic materials, making them desirable for applications in energy efficient electronic devices. In this study, we demonstrate electrical side-gate control of magnetoresistance and magnetic anisotropy in single-crystalline ferromagnetic Fe$_{0.75}$Co$_{0.25}$ thin films grown on ferroelectric PMN-PT (001) substrates by molecular beam epitaxy. Fe$_{0.75}$Co$_{0.25}$ is selected due to its large magnetoelastic coupling and low magnetic damping. We find that the magnetoresistance curves of patterned Fe$_{0.75}$Co$_{0.25}$ films are controlled by voltages applied to electrostatic side gates. Angle-dependent magnetoresistance scans reveal that the origin of this effect is strain-mediated variation of the magnetic anisotropy due to piezoelectric effects in the PMN-PT. This electrical control of magnetic properties could serve as a building block for future magnetoelectronic and magnonic devices.

cond-mat.mtrl-sci↗

arXiv2025

Full-film dry transfer of MBE-grown van der Waals materials

Molecular beam epitaxy (MBE) has been used to create high-quality, large-scale two-dimensional van der Waals (2D vdW) materials. However, due to the strong adhesion between the substrate and deposited materials, the peel-off and dry transfer of MBE-grown vdW films onto other substrates has been challenging. This limits the study and use of MBE films for heterogeneous integration including stacked and twisted heterostructures. In this work, we develop a polymer-assisted dry transfer method and successfully perform full-film transfer of various MBE-grown 2D vdW materials including transition metal dichalcogenides (TMD), topological insulators (TI) and 2D magnets. In particular, we transfer air-sensitive 2D magnets, characterize their magnetic properties, and compare them with as-grown materials. The results show that the transfer technique does not degrade the magnetic properties, with the Curie temperature and hysteresis loops exhibiting similar behaviors after the transfer. Our results enable further development of heterogeneous integration of 2D vdW materials based on MBE growth.

cond-mat.mtrl-sci↗

arXiv2025

Moiré-Tunable Localization of Simultaneous Type I and Type II Band Alignment in a MoSe2/WS2 Heterobilayer

Moiré heterobilayers exhibiting spatially varying band alignment and electron and hole localization that can be precisely controlled through the twist angle have emerged as exciting platforms for studying complex quantum phenomena. While most heterobilayers of transition metal dichalcogenides (TMDs) have a type II band alignment, the introduction of type I band alignment could enable stronger light-matter coupling and enhanced radiative emission. Here, we show through a combination of first-principles GW plus Bethe Salpeter equation (GW-BSE) calculations and time- and angle-resolved photoemission spectroscopy (tr-ARPES) measurements that contrary to previous understanding, the MoSe2/WS2 heterobilayer has a type I band alignment at large twist angles and simultaneous regions of type I and type II band alignment due to the structural reconstruction in different high symmetry regions at small twist angles. In tr-ARPES, consistent with our calculations, a long-lived electron population is only observed in MoSe2 for samples with large twist angles, while in samples with small twist angles, signals from two distinct long-lived excitons are observed. Moreover, despite the near degeneracy of the conduction bands of the two layers, no excitonic hybridization occurs, suggesting that previously observed absorption peaks in this material arise from lattice reconstruction. Our findings clarify the complex energy landscape in MoSe2/WS2 heterostructures, where the coexistence of type I and type II band alignment opens the door to moiré-tunable optoelectronic devices with intrinsic lateral heterojunctions.

cond-mat.mtrl-sci↗

arXiv2024

Large spin-orbit torque in a-plane $α$-Fe$_{2}$O$_{3}$/Pt bilayers

Realization of efficient spin-orbit torque switching of the Néel vector in insulating antiferromagnets is a challenge, often complicated by spurious effects. Quantifying the spin-orbit torques in antiferromagnet/heavy metal heterostructures is an important first step towards this goal. Here, we employ magneto-optic techniques to study damping-like spin-orbit torque (DL-SOT) in a-plane $α$-Fe$_2$O$_3$ (hematite) with a Pt spin-orbit overlayer. We find that the DL-SOT efficiency is two orders of magnitude larger than reported in c- and r-plane hematite/Pt using harmonic Hall techniques. The large magnitude of DL-SOT is supported by direct imaging of current-induced motion of antiferromagnetic domains that happens at moderate current densities. Our study introduces a new method for quantifying spin-orbit torque in antiferromagnets with a small canted moment and identifies a-plane $α$-Fe$_2$O$_3$ as a promising candidate to realize efficient SOT switching.

cond-mat.mtrl-sci↗

arXiv2024

Interface transparency to orbital current

The transport of spin currents across interfaces is relatively well studied, while the transport properties of orbital currents are just starting to be examined. In Cr/Ni bilayers, the spin-orbit torque (SOT) due to the orbital current generated in the Cr layer is believed to dominate over torques of other origins. In this work, we study SOT in Cr/X/Ni trilayers, where X is an ultra-thin spacer of a different material. Using the SOT as a proxy for the orbital current transferred from the Cr to the Ni layer, we compare Cr/X/Ni results to Pt/X/Ni, the system in which spin current generated in the Pt layer plays a dominant role. We find that across 12 different spacers the apparent interface transparency to the orbital current is comparable or larger than to the spin current.

cond-mat.mes-hall↗

arXiv2024

Antiferromagnetic order in a layered magnetic topological insulator MnBi$_2$Se$_4$ probed by resonant soft x-ray scattering

The quasi-two-dimensional magnetic topological insulator MnBi$_2$Se$_4$, stabilized via non-equilibrium molecular beam epitaxy, is investigated by resonant soft x-ray scattering. Kiessig fringes are observed, confirming a high sample quality and a thin film thickness of 10 septuple layers ($\sim$13 nm). An antiferromagnetic Bragg peak is observed at the structurally forbidden reflection, whose magnetic nature is validated by studying its temperature, energy, and polarization dependence. Through a detailed analysis, an A-type antiferromagetic order with in-plane moments is implied. This alternative spin structure in MnBi$_2$Se$_4$, in contrast to the Ising antiferromagnetic states in other magnetic topological insulators, might be relevant for hosting new topological states.

cond-mat.str-el↗

arXiv2024

Atomic Layer Molecular Beam Epitaxy of Kagome Magnet RMn$_6$Sn$_6$ (R = Er, Tb) Thin Films

Kagome lattices have garnered substantial interest because their band structure consists of topological flat bands and Dirac cones. The RMn$_6$Sn$_6$ (R = rare earth) compounds are particularly interesting because of the existence of large intrinsic anomalous Hall effect (AHE) which originates from the gapped Dirac cones near the Fermi level. This makes RMn$_6$Sn$_6$ an outstanding candidate for realizing the high-temperature quantum anomalous Hall effect. The growth of RMn$_6$Sn$_6$ thin films is beneficial for both fundamental research and potential applications. However, most of the studies on RMn$_6$Sn$_6$ have focused on bulk crystals so far, and the synthesis of RMn$_6$Sn$_6$ thin films has not been reported so far. Here we report the atomic layer molecular beam epitaxy growth, structural and magnetic characterizations, and transport properties of ErMn$_6$Sn$_6$ and TbMn$_6$Sn$_6$ thin films. It is especially noteworthy that TbMn$_6$Sn$_6$ thin films have out-of-plane magnetic anisotropy, which is important for realizing the quantum anomalous Hall effect. Our work paves the avenue toward the control of the AHE using devices patterned from RMn$_6$Sn$_6$ thin films.

cond-mat.mtrl-sci↗

arXiv2023

Scanning Tunneling Microscopy Study of Epitaxial Fe3GeTe2 Monolayers on Bi2Te3

Introducing magnetism to the surface state of topological insulators, such as Bi2Te3, can lead to a variety of interesting phenomena. We use scanning tunneling microscopy (STM) to study a single quintuple layer (QL) of the van der Waals magnet Fe3GeTe2 (FGT) that is grown on Bi2Te3 via molecular beam epitaxy. STM topographic images show that the FGT grows as free-standing islands on Bi2Te3 and outwards from Bi2Te3 steps. Atomic resolution imaging shows atomic lattices of 390 +- 10 pm for FGT and 430 +- 10 pm for Bi2Te3, consistent with the respective bulk crystals. A moiré pattern is observed on FGT regions with a periodicity of 4.3 +- 0.4 nm that can be attributed solely to this lattice mismatch and thus indicates zero rotational misalignments. While most of the surface is covered by a single QL of the FGT, there are small double QL regions, as well as regions with distinct chemical terminations due to an incomplete QL. The most common partial QL surface termination is the FeGe layer, in which the top two atomic layers are missing. This termination has a distinctive electronic structure and a (sqrt3 x sqrt3)R30 reconstruction overlaid on the moiré pattern in STM images. Magnetic circular dichroism (MCD) measurements confirm these thin FGT films are ferromagnetic with TC ~190 K.

cond-mat.mtrl-sci↗

arXiv2023

Room-Temperature Magnetic Skyrmions in Pt/Co/Cu Multilayers

Magnetic skyrmions are promising for next-generation information storage and processing owing to their potential advantages in data storage density, robustness, and energy efficiency. The magnetic multilayers consisting of Pt, Co, and a third metal element $X$ provide an ideal platform to study the skyrmions due to their highly tunable magnetic properties. Here, we report the observation of room-temperature bubble-like Néel skyrmions in epitaxial Pt/Co/Cu multilayers in samples with multidomain states in zero field. The magneto-optic Kerr effect (MOKE) and superconducting quantum interference device (SQUID) magnetometry are applied to investigate the shapes of the hysteresis loops, the magnetic anisotropy, and the saturation magnetization. By tuning the Co thickness and the number of periods, we achieve perpendicular and in-plane magnetized states and multidomain states that are identified by a wasp-waisted hysteresis loop. Skyrmions are directly imaged by magnetic force microscopy (MFM) and Lorentz transmission electron microscopy (LTEM). The development of room-temperature skyrmions in Pt/Co/Cu multilayers may lead to advances in skyrmion-related research and applications.

cond-mat.mtrl-sci↗

arXiv2023

Tuning the Curie temperature of a 2D magnet/topological insulator heterostructure to above room temperature by epitaxial growth

Heterostructures of two-dimensional (2D) van der Waals (vdW) magnets and topological insulators (TI) are of substantial interest as candidate materials for efficient spin-torque switching, quantum anomalous Hall effect, and chiral spin textures. However, since many of the vdW magnets have Curie temperatures below room temperature, we want to understand how materials can be modified to stabilize their magnetic ordering to higher temperatures. In this work, we utilize molecular beam epitaxy to systematically tune the Curie temperature ($T_C$) in thin film Fe$_3$GeTe$_2$/Bi$_2$Te$_3$ from bulk-like values ($\sim$220 K) to above room temperature by increasing the growth temperature from 300 $^\circ$C to 375 $^\circ$C. For samples grown at 375 $^\circ$C, cross-sectional scanning transmission electron microscopy (STEM) reveals the spontaneous formation of different Fe$_m$Ge$_n$Te$_2$ compositions (e.g. Fe$_5$Ge$_2$Te$_2$ and Fe$_7$Ge$_6$Te$_2$) as well as intercalation in the vdW gaps, which are possible origins of the enhanced Curie temperature. This observation paves the way for developing various Fe$_m$Ge$_n$Te$_2$/TI heterostructures with novel properties.

cond-mat.mtrl-sci↗

arXiv2023

Magnon Diffusion Length and Longitudinal Spin Seebeck Effect in Vanadium Tetracyanoethylene (V[TCNE]$_x$, $x \sim 2$)

Spintronic, spin caloritronic, and magnonic phenomena arise from complex interactions between charge, spin, and structural degrees of freedom that are challenging to model and even more difficult to predict. This situation is compounded by the relative scarcity of magnetically-ordered materials with relevant functionality, leaving the field strongly constrained to work with a handful of well-studied systems that do not encompass the full phase space of phenomenology predicted by fundamental theory. Here we present an important advance in this coupled theory-experiment challenge, wherein we extend existing theories of the spin Seebeck effect (SSE) to explicitly include the temperature-dependence of magnon non-conserving processes. This expanded theory quantitatively describes the low-temperature behavior of SSE signals previously measured in the mainstay material yttrium iron garnet (YIG) and predicts a new regime for magnonic and spintronic materials that have low saturation magnetization, $M_S$, and ultra-low damping. Finally, we validate this prediction by directly observing the spin Seebeck resistance (SSR) in the molecule-based ferrimagnetic semiconductor vanadium tetracyanoethylene (V[TCNE]$_x$, $x \sim 2$). These results validate the expanded theory, yielding SSR signals comparable in magnitude to YIG and extracted magnon diffusion length ($λ_m>1$ $μ$ m) and magnon lifetime for V[TCNE]$_x$ ($τ_{th}\approx 1-10$ $μ$ s) exceeding YIG ($τ_{th}\sim 10$ ns). Surprisingly, these properties persist to room temperature despite relatively low spin wave stiffness (exchange). This identification of a new regime for highly efficient SSE-active materials opens the door to a new class of magnetic materials for spintronic and magnonic applications.

cond-mat.mtrl-sci↗

arXiv2023

Epitaxial Kagome Thin Films as a Platform for Topological Flat Bands

Systems with flat bands are ideal for studying strongly correlated electronic states and related phenomena. Among them, kagome-structured metals such as CoSn have been recognized as promising candidates due to the proximity between the flat bands and the Fermi level. A key next step will be to realize epitaxial kagome thin films with flat bands to enable tuning of the flat bands across the Fermi level via electrostatic gating or strain. Here we report the band structures of epitaxial CoSn thin films grown directly on insulating substrates. Flat bands are observed using synchrotron-based angle-resolved photoemission spectroscopy (ARPES). The band structure is consistent with density functional theory (DFT) calculations, and the transport properties are quantitatively explained by the band structure and semiclassical transport theory. Our work paves the way to realize flat band-induced phenomena through fine-tuning of flat bands in kagome materials.

cond-mat.mtrl-sci↗

arXiv2023

Magneto-Optical Detection of the Orbital Hall Effect in Chromium

The orbital Hall effect has been theoretically predicted but its direct observation is a challenge. Here, we report the magneto-optical detection of current-induced orbital accumulation at the surface of a light 3$d$ transition metal, Cr. The orbital polarization is in-plane, transverse to the current direction, and scales linearly with current density, consistent with the orbital Hall effect. Comparing the thickness-dependent magneto-optical measurements with $\textit{ab initio}$ calculations, we estimate an orbital diffusion length in Cr of $6.6\pm 0.6$ nm.

cond-mat.mes-hall↗

arXiv2023

Observation of Skyrmion Bubbles in Multilayer [Pt/Co/Cu]n using spin-polarized STM

Magnetic multilayers are a promising platform for storage and logic devices based on skyrmion spin textures, due to the large materials phase space for tuning properties. Epitaxial superlattice structures of [Pt/Co/Cu]n thin films were grown by molecular beam epitaxy at room temperature. Spin-polarized scanning tunneling microscopy (SP-STM) of these samples was used to probe the connection between surface structure and skyrmion morphology with nanoscale spatial resolution. Irregular-shaped skyrmion bubbles were observed, with effective diameters from 20-200 nm that are much larger than the nanoscale grain structure of the surface topography. Nucleation, annihilation, and motion of skyrmion bubbles could be driven using the stray field of the ferromagnetic tip in repeated imaging, and spin-polarized current/voltage pulses. Our detailed comparison of STM topography and differential conductance images shows that there are no surface defects or inhomogeneities at length scales that could account for the range in skyrmion bubble size or shape observed in the measurements.

cond-mat.mtrl-sci↗

arXiv2023

An Atomically Tailored Chiral Magnet with Small Skyrmions at Room Temperature

Creating materials that do not exist in nature can lead to breakthroughs in science and technology. Magnetic skyrmions are topological excitations that have attracted great attention recently for their potential applications in low power, ultrahigh density memory. A major challenge has been to find materials that meet the dual requirement of small skyrmions stable at room temperature. Here we meet both these goals by developing epitaxial FeGe films with excess Fe using atomic layer molecular beam epitaxy (MBE) far from thermal equilibrium. Our novel atomic layer design permits the incorporation of 20% excess Fe while maintaining a non-centrosymmetric crystal structure supported by theoretical calculations and necessary for stabilizing skyrmions. We show that the Curie temperature is well above room temperature, and that the skyrmions probed by topological Hall effect have sizes down to 15 nm as imaged by Lorentz transmission electron microscopy (LTEM) and magnetic force microscopy (MFM). Our results illustrate new avenues for creating artificial materials tailored at the atomic scale that can impact nanotechnology.

cond-mat.mtrl-sci↗

arXiv2022

Atomic Layer Epitaxy of Kagome Magnet Fe${_3}$Sn${_2}$ and Sn-modulated Heterostructures

Magnetic materials with kagome crystal structure exhibit rich physics such as frustrated magnetism, skyrmion formation, topological flat bands, and Dirac/Weyl points. Until recently, most studies on kagome magnets have been performed on bulk crystals or polycrystalline films. Here we report the atomic layer molecular beam epitaxy synthesis of high-quality thin films of topological kagome magnet Fe${_3}$Sn${_2}$. Structural and magnetic characterization of Fe${_3}$Sn${_2}$ on epitaxial Pt(111) identifies highly ordered films with c-plane orientation and an in-plane magnetic easy axis. Studies of the local magnetic structure by anomalous Nernst effect imaging reveals in-plane oriented micrometer size domains. Superlattice structures consisting of Fe${_3}$Sn${_2}$ and Fe${_3}$Sn are also synthesized by atomic layer molecular beam epitaxy, demonstrating the ability to modulate the sample structure at the atomic level. The realization of high-quality films by atomic layer molecular beam epitaxy opens the door to explore the rich physics of this system and investigate novel spintronic phenomena by interfacing Fe${_3}$Sn${_2}$ with other materials.

cond-mat.mtrl-sci↗