arXiv subjects

H. Y. Hwang

Publications and source records attributed to H. Y. Hwang.

At least 19 recordsLinked to original sources

arXiv2023

Universal orbital and magnetic structures in infinite-layer nickelates

We conducted a comparative study of the rare-earth infinite-layer nickelates films, RNiO2 (R = La, Pr, and Nd) using resonant inelastic X-ray scattering (RIXS). We found that the gross features of the orbital configurations are essentially the same, with minor variations in the detailed hybridization. For low-energy excitations, we unambiguously confirm the presence of damped magnetic excitations in all three compounds. By fitting to a linear spin-wave theory, comparable spin exchange coupling strengths and damping coefficients are extracted, indicating a universal magnetic structure in the infinite-layer nickelates. Interestingly, while signatures of a charge order are observed in LaNiO2 in the quasi-elastic region of the RIXS spectrum, it is absent in NdNiO2 and PrNiO2. This prompts further investigation into the universality and the origins of charge order within the infinite-layer inickelates.

cond-mat.str-el↗

arXiv2021

Concomitant appearance of conductivity and superconductivity in (111)LaAlO3/SrTiO3 interface with metal capping

In polar-oxide interfaces, a certain number of monolayers (ML) is needed for conductivity to appear. This threshold for conductivity is explained by accumulating sufficient electric potential to initiate charge transfer to the interface. Here we study experimentally and theoretically the (111) SrTiO3/LaAlO3 interface where a critical thickness, tc, of nine epitaxial LaAlO3 ML is required to turn the interface from insulating to conducting and even superconducting. We show that tc decreases to 3ML when depositing a cobalt over-layer (capping) and 6ML for platinum capping. The latter result contrasts with the (100) interface, where platinum capping increases tc beyond the bare interface. The observed threshold for conductivity for the bare and the metal-capped interfaces is confirmed by our density functional theory calculations. Interestingly, for (111) SrTiO3/LaAlO3/Metal interfaces, conductivity appears concomitantly with superconductivity in contrast with the (100) SrTiO3/LaAlO3/Metal interfaces where tc is smaller than the critical thickness for superconductivity. We attribute this dissimilarity to the different orbital polarization of e'g for the (111) versus dxy for the (001) interface.

cond-mat.supr-con↗

arXiv2021

Magnetic excitations in infinite-layer nickelates

The discovery of superconductivity in infinite-layer nickelates brings us tantalizingly close to a new material class that mirrors the cuprate superconductors. Here, we report on magnetic excitations in these nickelates, measured using resonant inelastic x-ray scattering (RIXS) at the Ni L3-edge, to shed light on the material complexity and microscopic physics. Undoped NdNiO2 possesses a branch of dispersive excitations with a bandwidth of approximately 200 meV, reminiscent of strongly-coupled, antiferromagnetically aligned spins on a square lattice, despite a lack of evidence for long range magnetic order. The significant damping of these modes indicates the importance of coupling to rare-earth itinerant electrons. Upon doping, the spectral weight and energy decrease slightly, while the modes become overdamped. Our results highlight the role of Mottness in infinite-layer nickelates.

cond-mat.supr-con↗

arXiv2020

Orbital and Spin Character of Doped Carriers in Infinite-Layer Nickelates

The recent discovery of superconductivity in Nd$_{1-x}$Sr$_{x}$NiO$_2$ has drawn significant attention in the field. A key open question regards the evolution of the electronic structure with respect to hole doping. Here, we exploit x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) to probe the doping dependent electronic structure of the NiO$_2$ planes. Upon doping, a higher energy feature in Ni $L_3$ edge XAS develops in addition to the main absorption peak. By comparing our data to atomic multiplet calculations including $D_{4h}$ crystal field, the doping induced feature is consistent with a $d^8$ spin singlet state, in which doped holes reside in the $d_{x^2-y^2}$ orbitals, similar to doped single band Hubbard models. This is further supported by orbital excitations observed in RIXS spectra, which soften upon doping, corroborating with Fermi level shift associated with increasing holes in the $d_{x^2-y^2}$ orbital.

cond-mat.str-el↗

arXiv2019

Electronic structure of the parent compound of superconducting infinite-layer nickelates

The search for oxide materials with physical properties similar to the cuprate high Tc superconductors, but based on alternative transition metals such as nickel, has grown and evolved over time. The recent discovery of superconductivity in doped infinite-layer nickelates RNiO2 (R = rare-earth element) further strengthens these efforts.With a crystal structure similar to the infinite-layer cuprates - transition metal oxide layers separated by a rare-earth spacer layer - formal valence counting suggests that these materials have monovalent Ni1+ cations with the same 3d electron count as Cu2+ in the cuprates. Here, we use x-ray spectroscopy in concert with density functional theory to show that the electronic structure of RNiO2 (R = La, Nd), while similar to the cuprates, includes significant distinctions. Unlike cuprates with insulating spacer layers between the CuO2 planes, the rare-earth spacer layer in the infinite-layer nickelate supports a weakly-interacting three-dimensional 5d metallic state. This three-dimensional metallic state hybridizes with a quasi-two-dimensional, strongly correlated state with 3dx2-y2 symmetry in the NiO2 layers. Thus, the infinite-layer nickelate can be regarded as a sibling of the rare earth intermetallics, well-known for heavy Fermion behavior, where the NiO2 correlated layers play an analogous role to the 4f states in rare-earth heavy Fermion compounds. This unique Kondo- or Anderson-lattice-like "oxide-intermetallic" replaces the Mott insulator as the reference state from which superconductivity emerges upon doping.

cond-mat.supr-con↗

arXiv2016

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO$_3$

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply sub-picosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO$_3$ ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond timescales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables direct comparison with first-principles-based molecular dynamics simulations, with good agreement obtained.

cond-mat.mtrl-sci↗

arXiv2016

Ultrafast THz Field Control of Electronic and Structural Interactions in Vanadium Dioxide

Vanadium dioxide, an archetypal correlated-electron material, undergoes an insulator-metal transition near room temperature that exhibits electron-correlation-driven and structurally-driven physics. Using ultrafast optical spectroscopy and x-ray scattering we show that these processes can be disentangled in the time domain. Specifically, following intense sub-picosecond electric-field excitation, a partial collapse of the insulating gap occurs within the first ps. Subsequently, this electronic reconfiguration initiates a change in lattice symmetry taking place on a slower timescale. We identify the kinetic energy increase of electrons tunneling in the strong electric field as the driving force, illustrating a novel method to control electronic interactions in correlated materials on an ultrafast timescale.

cond-mat.str-el↗

arXiv2015

Photoinduced demagnetization and insulator-to-metal transition in ferromagnetic insulating BaFeO$_3$ thin films

We studied the electronic and magnetic dynamics of ferromagnetic insulating BaFeO3 thin films by using pump-probe time-resolved resonant x-ray reflectivity at the Fe 2p edge. By changing the excitation density, we found two distinctly different types of demagnetization with a clear threshold behavior. We assigned the demagnetization change from slow (~ 150 ps) to fast (< 70 ps) to a transition into a metallic state induced by laser excitation. These results provide a novel approach for locally tuning magnetic dynamics. In analogy to heat assisted magnetic recording, metallization can locally tune the susceptibility for magnetic manipulation, allowing to spatially encode magnetic information.

cond-mat.str-el↗

arXiv2014

X-ray spectroscopic study of BaFeO$_{3}$ thin films; an Fe$ ^{4+}$ ferromagnetic insulator

We investigated the electronic and magnetic properties of fully oxidized BaFeO3 thin films, which show ferromagnetic-insulating properties with cubic crystal structure, by hard x-ray photoemission spectroscopy (HAXPES), x-ray absorption spectroscopy (XAS) and soft x-ray magnetic circular dichroism (XMCD). We analyzed the results with configuration-interaction (CI) cluster-model calculations for Fe4+, which showed good agreement with the experimental results. We also studied SrFeO3 thin films, which have an Fe4+ ion helical magnetism in cubic crystal structure, but are metallic at all temperatures. We found that BaFeO3 thin films are insulating with large magnetization (2.1muB/formula unit) under ~ 1 T, using valence-band HAXPES and Fe 2p XMCD, which is consistent with the previously reported resistivity and magnetization measurements. Although Fe 2p core-level HAXPES and Fe 2p XAS spectra of BaFeO3 and SrFeO3 thin films are quite similar, we compared the insulating BaFeO3 to metallic SrFeO3 thin films with valence-band HAXPES. The CI cluster-model analysis indicates that the ground state of BaFeO3 is dominated by d5L (L: ligand hole) configuration due to the negative charge transfer energy, and that the band gap has significant O 2p character. We revealed that the differences of the electronic and magnetic properties between BaFeO3 and SrFeO3 arise from the differences in their lattice constants, through affecting the strength of hybridization and bandwidth.

cond-mat.str-el↗

arXiv2014

Visible light enhanced field effect at LaAlO3/SrTiO3 interface

Electrical field and light-illumination have been two most widely used stimuli in tuning the conductivity of semiconductor devices. Via capacitive effect electrical field modifies the carrier density of the devices, while light-illumination generates extra carriers by exciting trapped electrons into conduction band1. Here, we report on an unexpected light illumination enhanced field effect in a quasi-two-dimensional electron gas (q2DEG) confined at the LaAlO3/SrTiO3 (LAO/STO) interface which has been the focus of emergent phenomenon exploration2-14. We found that light illumination greatly accelerates and amplifies the field effect, driving the field-induced resistance growth which originally lasts for thousands of seconds into an abrupt resistance jump more than two orders of magnitude. Also, the field-induced change in carrier density is much larger than that expected from the capacitive effect, and can even be opposite to the conventional photoelectric effect. This work expands the space for novel effect exploration and multifunctional device design at complex oxide interfaces.

cond-mat.mtrl-sci↗

arXiv2014

The potential profile at the LaAlO3/SrTiO3 (001) heterointerface in operando conditions

We report measurements of the gate-bias dependent band alignment, especially the confining potential profile, at the conducting LaAlO3/SrTiO3 (001) heterointerface using soft and hard x-ray photoemission spectroscopy. Depth-profiling analysis reveals that a significant potential drop on the SrTiO3 side of the interface occurs within ~2 nm of the interface under negative gate bias voltage. These results demonstrate gate control of the collapse of permittivity at the interface, and explain the dramatic loss of electron mobility with back-gate depletion.

cond-mat.mtrl-sci↗

arXiv2013

Transistor operation and mobility enhancement in top-gated LaAlO_3 / SrTiO_3 heterostructures

We report the operation of LaAlO_3 / SrTiO_3 depletion mode top-gated junction field-effect transistors using a range of LaAlO_3 thicknesses as the top gate insulator. Gated Hall bars show near ideal transistor characteristics at room temperature with on-off ratios greater than 1000. Lower temperature measurements demonstrate a systematic increase in the Hall mobility as the sheet carrier density in the channel is depleted via the top gate, providing a route to higher mobility, lower density electron gases in this system.

cond-mat.mtrl-sci↗

arXiv2013

Stoichiometry control of the electronic properties of the LaAlO_3/SrTiO_3 heterointerface

We investigate the effect of the laser parameters of pulsed laser deposition on the film stoichiometry and electronic properties of LaAlO_3/SrTiO_3 (001) heterostructures. The La/Al ratio in the LaAlO_3 films was varied over a wide range from 0.88 to 1.15, and was found to have a strong effect on the interface conductivity. In particular, the carrier density is modulated over more than two orders of magnitude. The film lattice expansion, caused by cation vacancies, is found to be the important functional parameter. These results can be understood to arise from the variations in the electrostatic boundary conditions, and their resolution, with stoichiometry.

cond-mat.mtrl-sci↗

arXiv2012

Strongly spin-orbit coupled two-dimensional electron gas emerging near the surface of polar semiconductors

We investigate the two-dimensional (2D) highly spin-polarized electron accumulation layers commonly appearing near the surface of n-type polar semiconductors BiTeX (X = I, Br, and Cl) by angular-resolved photoemission spectroscopy. Due to the polarity and the strong spin-orbit interaction built in the bulk atomic configurations, the quantized conduction-band subbands show giant Rashba-type spin-splitting. The characteristic 2D confinement effect is clearly observed also in the valence-bands down to the binding energy of 4 eV. The X-dependent Rashba spin-orbit coupling is directly estimated from the observed spin-split subbands, which roughly scales with the inverse of the band-gap size in BiTeX.

cond-mat.mtrl-sci↗

arXiv2012

Magnetotransport effects in polar versus non-polar SrTiO3 based heterostructures

Anisotropic magnetoresistance and negative magnetoresistance for in-plane fields are compared for the LaAlO3 /SrTiO3 interface and the symmetric Nb-doped SrTiO3 heterostructure. Both effects are exceptionally strong in LaAlO3 /SrTiO3 . We analyze their temperature, magnetic field and gate voltage dependencies and find them to arise from a Rashba type spin-orbit coupling with magnetic scatterers that have two contributions to their potential: spin exchange and Coulomb interaction. Atomic spin-orbit coupling is sufficient to explain the small effects observed in Nb-doped SrTiO3 . These results clarify contradicting transport interpretations in SrTiO3 -based heterostructures.

cond-mat.str-el↗

arXiv2012

Metal-to-insulator transition in anatase TiO2 thin films induced by growth rate modulation

We demonstrate control of the carrier density of single phase anatase TiO2 thin films by nearly two orders of magnitude by modulating the growth kinetics during pulsed laser deposition, under fixed thermodynamic conditions. The resistivity and the intensity of the photoluminescence spectra of these TiO2 samples, both of which correlate with the number of oxygen vacancies, are shown to depend strongly on the growth rate. A quantitative model is used to explain the carrier density changes.

cond-mat.mtrl-sci↗

arXiv2012

Coexistence of two- and three-dimensional Shubnikov-de Haas oscillations in Ar^+ -irradiated KTaO_3

We report the electron doping in the surface vicinity of KTaO_3 by inducing oxygen-vacancies via Ar^+ -irradiation. The doped electrons have high mobility (> 10^4 cm^2/Vs) at low temperatures, and exhibit Shubnikov-de Haas oscillations with both two- and three-dimensional components. A disparity of the extracted in-plane effective mass, compared to the bulk values, suggests mixing of the orbital characters. Our observations demonstrate that Ar^+ -irradiation serves as a flexible tool to study low dimensional quantum transport in 5d semiconducting oxides.

cond-mat.mes-hall↗

arXiv2012

Scanning SQUID Susceptometry of a paramagnetic superconductor

Scanning SQUID susceptometry images the local magnetization and susceptibility of a sample. By accurately modeling the SQUID signal we can determine the physical properties such as the penetration depth and permeability of superconducting samples. We calculate the scanning SQUID susceptometry signal for a superconducting slab of arbitrary thickness with isotropic London penetration depth, on a non-superconducting substrate, where both slab and substrate can have a paramagnetic response that is linear in the applied field. We derive analytical approximations to our general expression in a number of limits. Using our results, we fit experimental susceptibility data as a function of the sample-sensor spacing for three samples: 1) delta-doped SrTiO3, which has a predominantly diamagnetic response, 2) a thin film of LaNiO3, which has a predominantly paramagnetic response, and 3) a two-dimensional electron layer (2-DEL) at a SrTiO3/AlAlO3 interface, which exhibits both types of response. These formulas will allow the determination of the concentrations of paramagnetic spins and superconducting carriers from fits to scanning SQUID susceptibility measurements.

cond-mat.supr-con↗