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Hyun Ho Kim

Publications and source records attributed to Hyun Ho Kim.

12 recordsLinked to original sources

Structural Monoclinicity and Its Coupling to Layered Magnetism in Few-Layer $\mathrm{CrI_{3}}$

Using polarization-resolved Raman spectroscopy, we investigate layer number, temperature, and magnetic field dependence of Raman spectra in one- to four-layer $\mathrm{CrI_{3}}$. Layer-number-dependent Raman spectra show that in the paramagnetic phase a doubly degenerated $E_{g}$ mode of monolayer $\mathrm{CrI_{3}}$ splits into one $A_{g}$ and one $B_{g}$ mode in N-layer (N > 1) $\mathrm{CrI_{3}}$ due to the monoclinic stacking. Their energy separation increases in thicker samples until an eventual saturation. Temperature-dependent measurements further show that the split modes tend to merge upon cooling but remain separated until 10 K, indicating a failed attempt of the monoclinic-to-rhombohedral structural phase transition that is present in the bulk crystal. Magnetic-field-dependent measurements reveal an additional monoclinic distortion across the magnetic-field-induced layered antiferromagnetism-to-ferromagnetism phase transition. We propose a structural change that consists of both a lateral sliding toward the rhombohedral stacking and a decrease in the interlayer distance to explain our experimental observations.

cond-mat.mes-hall

Roadmap for gallium arsenide spin qubits

Gate-defined quantum dots in gallium arsenide (GaAs) have been used extensively for pioneering spin qubit devices due to the relative simplicity of fabrication and favourable electronic properties such as a single conduction band valley, a small effective mass, and stable dopants. GaAs spin qubits are readily produced in many labs and are currently studied for various applications, including entanglement, quantum non-demolition measurements, automatic tuning, multi-dot arrays, coherent exchange coupling, and teleportation. Even while much attention is shifting to other materials, GaAs devices will likely remain a workhorse for proof-of-concept quantum information processing and solid-state experiments.

cond-mat.mes-hall

Tunable layered-magnetism-assisted magneto-Raman effect in a two-dimensional magnet $\mathrm{CrI_3}$

We use a combination of polarized Raman spectroscopy experiment and model magnetism-phonon coupling calculations to study the rich magneto-Raman effect in the two-dimensional (2D) magnet $\mathrm{CrI_3}$. We reveal a novel layered-magnetism-assisted phonon scattering mechanism below the magnetic onset temperature, whose Raman excitation breaks time-reversal symmetry, has an antisymmetric Raman tensor, and follows the magnetic phase transitions across critical magnetic fields, on top of the presence of the conventional phonon scattering with symmetric Raman tensors in $N$-layer $\mathrm{CrI_3}$. We resolve in data and by calculations that the 1st-order $A_g$ phonon of monolayer splits into a $N$-fold multiplet in $N$-layer $\mathrm{CrI_3}$ due to the interlayer coupling ($N$>=2) and that the phonons with the multiple show distinct magnetic field dependence because of their different layered-magnetism-phonon coupling. We further find that such a layered-magnetism-phonon coupled Raman scattering mechanism extends beyond 1st-order to higher-order multi-phonon scattering processes. Our results on magneto-Raman effect of the 1st-order phonons in the multiplet and the higher-order multi-phonons in $N$-layer $\mathrm{CrI_3}$ demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underlines the unique opportunities of new spin-phonon physics in van der Waals layered magnets.

cond-mat.mtrl-sci

Observation of the polaronic character of excitons in a two-dimensional semiconducting magnet $\mathrm{CrI_3}$

Exciton dynamics can be strongly affected by lattice vibrations through electron-phonon coupling. This is rarely explored in two-dimensional magnetic semiconductors. Focusing on bilayer CrI3, we first show the presence of strong electron-phonon coupling through temperature-dependent photoluminescence and absorption spectroscopy. We then report the observation of periodic broad modes up to the 8th order in Raman spectra, attributed to the polaronic character of excitons. We establish that this polaronic character is dominated by the coupling between the charge-transfer exciton at 1.96 eV and a longitudinal optical phonon at 120.6 cm-1. We further show that the emergence of long-range magnetic order enhances the electron-phonon coupling strength by about 50$\%$ and that the transition from layered antiferromagnetic to ferromagnetic order tunes the spectral intensity of the periodic broad modes, suggesting a strong coupling among the lattice, charge and spin in two-dimensional CrI3. Our study opens opportunities for tailoring light-matter interactions in two-dimensional magnetic semiconductors.

cond-mat.mes-hall

Magnetic field-induced quantum phase transitions in a van der Waals magnet

Exploring new parameter regimes to realize and control novel phases of matter has been a main theme in modern condensed matter physics research. The recent discovery of 2D magnetism in nearly freestanding monolayer atomic crystals has already led to observations of a number of novel magnetic phenomena absent in bulk counterparts. Such intricate interplays between magnetism and crystalline structures provide ample opportunities for exploring quantum phase transitions in this new 2D parameter regime. Here, using magnetic field and temperature dependent circularly polarized Raman spectroscopy of phonons and magnons, we map out the phase diagram of CrI3 that has been known to be a layered AFM in its 2D films and a FM in its 3D bulk. We, however, reveal a novel mixed state of layered AFM and FM in 3D CrI3 bulk crystals where the layered AFM survives in the surface layers and the FM appears in deeper bulk layers. We then show that the surface layered AFM transits into the FM at a critical magnetic field of 2 T, similar to what was found in the few layer case. Interestingly, concurrent with this magnetic phase transition, we discover a first-order structural phase transition that alters the crystallographic point group from C3i to C2h and thus, from a symmetry perspective, this monoclinic structural phase belongs to the 3D nematic order universality class. Our result not only unveils the complex single magnon behavior in 3D CrI3, but also settles down the puzzle of how CrI3 transits from a bulk FM to a thin layered AFM semiconductor, despite recent efforts in understanding the origin of layered AFM in CrI3 thin layer, and reveals the intimate relationship between the layered AFM-to-FM and the crystalline rhombohedral-to-monoclinic phase transitions. These findings further open up opportunities for future 2D magnet-based magneto-mechanical devices.

cond-mat.mtrl-sci

Magneto-memristive switching in a two-dimensional layer antiferromagnet

Memristive devices whose resistance can be hysteretically switched by electric field or current are intensely pursued both for fundamental interest as well as potential applications in neuromorphic computing and phase-change memory. When the underlying material exhibits additional charge or spin order, the resistive states can be directly coupled, further allowing for electrical control of the collective phases. Here, we report the observation of abrupt, memristive switching of tunneling current in nanoscale junctions of ultrathin CrI$_3$, a natural layer antiferromagnet. The coupling to spin order enables both tuning of the resistance hysteresis by magnetic field, and electric-field switching of magnetization even in multilayer samples.

cond-mat.mtrl-sci

Quantum tunneling devices incorporating two-dimensional magnetic semiconductors

Research in two-dimensional (2D) materials has experienced rapid growth in the past few years. In particular, various layered compounds exhibiting quantum phenomena, such as superconductivity and magnetism, have been isolated in atomically thin form, often in spite of their chemical instability. The nature of the 2D phases can be different than their bulk counterparts, making such systems attractive for fundamental studies. Owing to their high crystallinity and absence of dangling bonds, devices and heterostructures incorporating these materials may also show performance exceeding that of traditional films. In this roadmap article, we focus on a few recent developments in spin-based quantum devices utilizing the 2D magnetic semiconductor, CrI$_3$.

cond-mat.mtrl-sci

Tailored tunnel magnetoresistance response in three ultrathin chromium trihalides

Materials that demonstrate large magnetoresistance have attracted significant interest for many decades. Recently, extremely large tunnel magnetoresistance (TMR) has been reported by several groups across ultrathin CrI$_3$ by exploiting the weak antiferromagnetic coupling between adjacent layers. Here, we report a comparative study of TMR in all three chromium trihalides (CrX$_3$, X= Cl, Br, or I) in the two-dimensional limit. As the materials exhibit different transition temperatures and interlayer magnetic ordering in the ground state, tunneling measurements allow for an easy determination of the field-temperature phase diagram for the three systems. By changing sample thickness and biasing conditions, we then demonstrate how to maximize and further tailor the TMR response at different temperatures for each material. In particular, near the magnetic transition temperature, TMR is non-saturating up to the highest fields measured for all three compounds owing to the large, field-induced exchange coupling.

cond-mat.mtrl-sci

Evolution of interlayer and intralayer magnetism in three atomically thin chromium trihalides

We conduct a comprehensive study of three different magnetic semiconductors, CrI$_3$, CrBr$_3$, and CrCl$_3$, by incorporating both few- and bi-layer samples in van der Waals tunnel junctions. We find that the interlayer magnetic ordering, exchange gap, magnetic anisotropy, as well as magnon excitations evolve systematically with changing halogen atom. By fitting to a spin wave theory that accounts for nearest neighbor exchange interactions, we are able to further determine a simple spin Hamiltonian describing all three systems. These results extend the 2D magnetism platform to Ising, Heisenberg, and XY spin classes in a single material family. Using magneto-optical measurements, we additionally demonstrate that ferromagnetism can be stabilized down to monolayer in more isotropic CrBr$_3$, with transition temperature still close to that of the bulk.

cond-mat.mtrl-sci

Raman fingerprint of two terahertz spin wave branches in a two-dimensional honeycomb Ising ferromagnet

Two-dimensional (2D) magnetism has been long sought-after and only very recently realized in atomic crystals of magnetic van der Waals materials. So far, a comprehensive understanding of the magnetic excitations in such 2D magnets remains missing. Here we report polarized micro-Raman spectroscopy studies on a 2D honeycomb ferromagnet CrI3. We show the definitive evidence of two sets of zero-momentum spin waves at frequencies of 2.28 terahertz (THz) and 3.75 THz, respectively, that are three orders of magnitude higher than those of conventional ferromagnets. By tracking the thickness dependence of both spin waves, we reveal that both are surface spin waves with lifetimes an order of magnitude longer than their temporal periods. Our results of two branches of high-frequency, long-lived surface spin waves in 2D CrI3 demonstrate intriguing spin dynamics and intricate interplay with fluctuations in the 2D limit, thus opening up opportunities for ultrafast spintronics incorporating 2D magnets.

cond-mat.mes-hall

One million percent tunnel magnetoresistance in a magnetic van der Waals heterostructure

We report the observation of a very large negative magnetoresistance effect in a van der Waals tunnel junction incorporating a thin magnetic semiconductor, CrI3, as the active layer. At constant voltage bias, current increases by nearly one million percent upon application of a 2 Tesla field. The effect arises from a change between antiparallel to parallel alignment of spins across the different CrI3 layers. Our results elucidate the nature of the magnetic state in ultrathin CrI3 and present new opportunities for spintronics based on two-dimensional materials.

cond-mat.mtrl-sci

Dimensionality-driven orthorhombic MoTe2 at room temperature

We use a combination of Raman spectroscopy and transport measurements to study thin flakes of the type-II Weyl semimetal candidate MoTe2 protected from oxidation. In contrast to bulk crystals, which undergo a phase transition from monoclinic to the inversion symmetry breaking, orthorhombic phase below ~250 K, we find that in moderately thin samples below ~12 nm, a single orthorhombic phase exists up to and beyond room temperature. This could be due to the effect of c-axis confinement, which lowers the energy of an out-of-plane hole band and stabilizes the orthorhombic structure. Our results suggest that Weyl nodes, predicated upon inversion symmetry breaking, may be observed in thin MoTe2 at room temperature.

cond-mat.mtrl-sci