arXiv subjects

Hsiao-Yi Chen

Publications and source records attributed to Hsiao-Yi Chen.

At least 19 recordsLinked to original sources

arXiv2026

Bridging ambient- and high-pressure superconductivity in La$_2$LnNi$_2$O$_7$ films

The discovery of high critical-temperature $T_{\mathrm{c}}$ superconductivity near 80 K in bilayer nickelates under high pressure has sparked extensive studies. While superconductivity exceeding 40 K was subsequently discovered at ambient pressure in compressively strained films, the relationship between ambient- and high-pressure regimes remains an open question. Here we present a systematic investigation of superconductivity in compressively strained La$_2$LnNi$_2$O$_7$ films (Ln = lanthanides) at ambient and high pressures. The normal-state resistivity at ambient pressure, revealed by suppressing superconductivity with magnetic fields of 59 T, tends toward $T^2$ behaviour. Under high pressure in a cubic-anvil cell, $T_{\mathrm{c}}$ was enhanced from 41-42 K at ambient pressure to 67-73 K at 16 GPa. On the other hand, lattice compression induced by Ln substitution, which may mimic effects of pressure, lowers $T_{\mathrm{c}}$. In both cases, $T_{\mathrm{c}}$ correlates with the evolution of normal-state transport between $T^2$ and $T$-linear behaviour, offering insight into the interplay between lattice structure and superconductivity in bilayer nickelates.

cond-mat.supr-con↗

arXiv2026

Pressure-induced superconductivity in epitaxially-stabilized Pr$_3$Ni$_2$O$_7$ films

The discovery of high critical-temperature $T_{\mathrm{c}}$ superconductivity in La$_3$Ni$_2$O$_7$ under high pressure has led to a rapid expansion of the $T_{\mathrm{c}}$ range through lanthanide $Ln$ substitution, and to ambient-pressure superconductivity in strained thin films, yet the exploration of new bilayer nickelates remains strongly constrained by thermodynamic stability. Beyond the difficulty of synthesis of bulk single-crystals, here we report on the pressure-induced high-$T_{\mathrm{c}}$ superconductivity in epitaxially-stabilized Pr$_3$Ni$_2$O$_7$ thin films. While the Pr$_3$Ni$_2$O$_7$ films exhibit insulating behaviour at ambient pressure regardless of ozone-annealing treatment, they show $T$-linear metallic transport and superconductivity reaching an onset $T_{\mathrm{c}}$ of 66 K and zero-resistance at nearly 40 K at 22 GPa. Furthermore, Nd$_3$Ni$_2$O$_7$, with the smaller rare-earth ion Nd, can also be stabilized, however, superconductivity is not observed in the measured pressure range. Epitaxial stabilization enables us to examine the dependence of $T_{\mathrm{c}}$ and the critical pressure $P_{\mathrm{c}}$ for superconductivity on the $Ln$ ion in $Ln_3$Ni$_2$O$_7$ ($Ln$ = La, Pr, Nd). These results suggest that a higher $P_{\mathrm{c}}$ is required for smaller $Ln$ ions, consistent with trends observed in bulk studies of $Ln$ substitution. This study demonstrates that epitaxial stabilization is a powerful technique to further expand the family of superconducting bilayer nickelates.

cond-mat.supr-con↗

arXiv2025

First-Principles Approach to Spin Excitations in Noncollinear Magnetic Systems

We present a first-principles method based on density functional theory and many-body perturbation theory for computing spin excitations in magnetic systems with noncollinear spin textures. Traditionally, the study of magnetic excitations has relied on spin models that assume magnetic moments to be localized. Beyond this restriction, recent $ab~initio$ methods based on Green's functions within the local spin-density approximation have emerged as a general framework for calculating magnetic susceptibilities. However, their application has so far been largely limited to collinear ferromagnetic and antiferromagnetic systems. In this work, we extend this framework and enable the treatment of large-scale noncollinear magnetic systems by leveraging a Wannier-basis representation and implementing an ansatz potential method to reduce computational cost. We apply our method to the spin-spiral state of LiCu$_2$O$_2$, successfully capturing its steady-state spin-rotation pitch in agreement with the experimental measurement and resolving the characteristic magnon dispersion. We further analyze the interplay between the spiral spin structure and the on-site spin-exchange splitting, and elucidate the crucial role of magnetic dipoles on ligand ions in mediating effective ferromagnetic interaction among the primary spins on Cu$^{2+}$ ions. Finally, we provide a theoretical prediction of the magnon dispersion on top of the helical spin background in high agreement with the experimental measurement. Overall, this work establishes a general and computationally efficient framework for simulating collective spin dynamics in noncollinear magnetic systems from first principles, exemplified by -- but not limited to -- spin-spiral states.

cond-mat.mtrl-sci↗

arXiv2025

Magnon-phonon interactions from first principles

Modeling spin-wave (magnon) dynamics in novel materials is important to advance spintronics and spin-based quantum technologies. The interactions between magnons and lattice vibrations (phonons) limit the length scale for magnon transport. However, quantifying these interactions remains challenging. Here we show many-body calculations of magnon-phonon (mag-ph) coupling based on the ab initio Bethe-Salpeter equation. We derive expressions for mag-ph coupling matrices and compute them in 2D ferromagnets, focusing on hydrogenated graphene and monolayer CrI3. Our analysis shows that electron-phonon (e-ph) and mag-ph interactions differ significantly, where modes with weak e-ph coupling can exhibit strong mag-ph coupling (and vice versa), and reveals which phonon modes couple more strongly with magnons. In both materials studied here, the inelastic magnon relaxation time is found to decrease abruptly above the threshold for emission of strongly coupled phonons, thereby defining a low-energy window for efficient magnon transport. By averaging in this window, we compute the temperature-dependent magnon mean-free path, a key figure of merit for spintronics, entirely from first principles. The theory and computational tools shown in this work enable studies of magnon interactions, scattering, and dynamics in generic materials, advancing the design of magnetic systems and magnon- and spin-based devices.

cond-mat.mtrl-sci↗

arXiv2025

Strain-tuning for superconductivity in La$_3$Ni$_2$O$_7$ thin films

The recent discovery of high-transition temperature ($T_\mathrm{c}$) superconductivity in pressurized La$_{3}$Ni$_{2}$O$_{7}$ bulk crystals has attracted keen attention due to its characteristic energy diagram of $e_{g}$ orbitals, containing nearly half-filled $d_{3z^2 - r^2}$ and quarter-filled $d_{x^2 - y^2}$ orbitals. This finding provides valuable insights into the orbital contributions and interlayer interactions in double NiO$_{6}$ octahedra, offering opportunities to control the electronic structure via ligand field variations. Here, we demonstrate strain-tuning of $T_\mathrm{c}$ over a range of 50 K in La$_{3}$Ni$_{2}$O$_{7}$ films grown on different oxide substrates under 20 GPa. As the $c/a$ ratio increases, the onset $T_\mathrm{c}$ systematically rises from 10 K in the tensile-strained film on SrTiO$_{3}$ to a maximum of about 60 K in the compressively strained film on LaAlO$_{3}$. These systematic variations suggest that strain engineering is a promising strategy for expanding superconductivity in bilayer nickelates by tuning the orbital energy landscape toward high-$T_\mathrm{c}$ superconductivity.

cond-mat.supr-con↗

arXiv2025

DiracBilinears.jl: A package for computing Dirac bilinears in solids

DiracBilinears.jl is a Julia package for computing Dirac bilinears, which are fundamental physical quantities of electrons in relativistic quantum theory, using first-principles calculations for solids. In relativistic quantum theory, 16 independent bilinears can be defined using the four-component Dirac field. We take the non-relativistic limit for the bilinears, which corresponds to the $1/m$ expansion, and focus on the low-energy physics typically considered in condensed matter physics. This package can evaluate the spatial distributions and Wannier matrix elements of the Dirac bilinears in solids quantitatively by connecting to the external first-principles calculation packages, including Quantum ESPRESSO, Wannier90, and wan2respack.

cond-mat.mtrl-sci↗

arXiv2024

Giant Hall effect in a highly conductive frustrated magnet GdCu$_2$

The Hall effect is one of the most fundamental but elusive phenomena in condensed matter physics due to the rich variety of underlying mechanisms. Here we report an exceptionally large Hall effect in a frustrated magnet GdCu$_2$ with high conductivity. The Hall conductivity at the base temperature is as high as 4 x 10$^4$ $Ω^{-1}$cm$^{-1}$ and shows abrupt sign changes under magnetic fields. Remarkably, the giant Hall effect is rapidly suppressed as the longitudinal conductivity is lowered upon increasing temperature or introducing tiny amount of quenched disorder. Our systematic transport measurements together with neutron scattering measurements and ab initio band calculations indicate that the unusual Hall effect can be understood in terms of spin-splitting induced emergence/disappearance of Fermi pockets as well as skew scattering from spin-chiral cluster fluctuations in a field-polarized state. The present study demonstrates complex interplay among magnetization, spin-dependent electronic structure, and spin fluctuations in producing the giant Hall effect in highly conductive frustrated magnets.

cond-mat.str-el↗

arXiv2024

Topological Hall effect of Skyrmions from First Principles

We formulate a first-principles approach for calculating the topological Hall effect (THE) in magnets with noncollinear nanoscale spin textures. We employ a modeling method to determine the effective magnetic field induced by the spin texture, thereby circumventing the computational challenges associated with superlattice calculations. Based on these results, we construct a Wannier tight-binding Hamiltonian to characterize the electronic states and calculate the Hall conductivity. Applying this approach to the skyrmion material $\rm Gd_2PdSi_3$ shows good agreement with experimental data. Our analysis in momentum space further reveals that the dominant contribution to the THE arises from the crossing points between the folded bands along high-symmetry lines in the Brillouin zone. This work advances numerical techniques for simulating general magnetic system, examplified by but not restricted to skyrmion lattice, and its result offering insights into the complex interplay between spin textures and electronic transport.

cond-mat.mes-hall↗

arXiv2022

First-Principles Ultrafast Exciton Dynamics and Time-Domain Spectroscopies: Dark-Exciton Mediated Valley Depolarization in Monolayer WSe$_2$

Calculations combining first-principles electron-phonon ($e$-ph) interactions with the Boltzmann equation enable studies of ultrafast carrier and phonon dynamics. However, in materials with weak Coulomb screening, electrons and holes form bound excitons and their scattering processes become correlated, posing additional challenges for modeling nonequilibrium physics. Here we show calculations of ultrafast exciton dynamics and related time-domain spectroscopies using $ab~initio$ exciton-phonon (ex-ph) interactions together with an excitonic Boltzmann equation. Starting from the nonequilibrium exciton populations, we develop simulations of time-domain absorption and photoemission spectra that take into account electron-hole correlations. We use this method to study monolayer WSe$_2$, where our calculations predict sub-picosecond timescales for exciton relaxation and valley depolarization and reveal the key role of intermediate dark excitons. The approach introduced in this work enables a quantitative description of nonequilibrium dynamics and ultrafast spectroscopies in materials with strongly bound excitons.

cond-mat.mtrl-sci↗

arXiv2022

Development of $ab ~initio$ method for exciton condensation and its application to $\bf TiSe_2$

Exciton condensation indicating the spontaneous formation of electron-hole pair can cause the phase transition from a semimetal to an excitonic insulator by gap opening at the Fermi surface. While the idea of this excitonic insulator has been proposed for decades, current theoretical approaches can only provide qualitative descriptions, and a quantitative predicting tool is still missing. To shed insight on this problem, we developed an $ab~initio$ method based on the finite-temperature density functional theory and many-body perturbation theory to compute the exciton condensation critical behavior. Applying our approach to the monolayer $\rm TiSe_2$, we find a lattice distortion accompanied by the formation of the excitonic gap via electron-phonon coupling without phonon softening, proving that the exciton condensation is the origin of the charge-density-wave state observed in this compound. Overall, the methodology introduced in this work is general and paves the way to searching for candidate excitonic insulators in natural material systems.

cond-mat.mtrl-sci↗

arXiv2022

Dark Matter Direct Detection in Materials with Spin-Orbit Coupling

Semiconductors with $\mathcal{O}(\text{meV})$ band gaps have been shown to be promising targets to search for sub-MeV mass dark matter (DM). In this paper we focus on a class of materials where such narrow band gaps arise naturally as a consequence of spin-orbit coupling (SOC). Specifically, we are interested in computing DM-electron scattering and absorption rates in these materials using state-of-the-art density functional theory (DFT) techniques. To do this, we extend the DM interaction rate calculation to include SOC effects which necessitates a generalization to spin-dependent wave functions. We apply our new formalism to calculate limits for several DM benchmark models using an example ZrTe$_{5}$ target and show that the inclusion of SOC can substantially alter projected constraints.

hep-ph↗

arXiv2020

Radiative properties of quantum emitters in boron nitride from excited state calculations and Bayesian analysis

Point defects in hexagonal boron nitride (hBN) have attracted growing attention as bright single-photon emitters. However, understanding of their atomic structure and radiative properties remains incomplete. Here we study the excited states and radiative lifetimes of over 20 native defects and carbon or oxygen impurities in hBN using ab initio density functional theory and GW plus Bethe-Salpeter equation calculations, generating a large data set of their emission energy, polarization and lifetime. We find a wide variability across quantum emitters, with exciton energies ranging from 0.3 to 4 eV and radiative lifetimes from ns to ms for different defect structures. Through a Bayesian statistical analysis, we identify various high-likelihood defect emitters, among which the native $\mathrm{V_NN_B}$ defect is predicted to possess emission energy and radiative lifetime in agreement with experiments. Our work advances the microscopic understanding of hBN single-photon emitters and introduces a computational framework to characterize and identify quantum emitters in 2D materials.

cond-mat.mtrl-sci↗

arXiv2020

Facile ab initio approach for self-localized polarons from canonical transformations

Electronic states in a crystal can localize due to strong electron-phonon (e-ph) interactions, forming so-called small polarons. Methods to predict the formation and energetics of small polarons are either computationally costly or not geared toward quantitative predictions. Here we show a formalism based on canonical transformations to compute the polaron formation energy and wavefunction using ab initio e-ph interactions. Comparison of the calculated polaron and band edge energies allows us to determine whether charge carriers in a material favor a localized small polaron over a delocalized Bloch state. Due to its low computational cost, our approach enables efficient studies of the formation and energetics of small polarons, as we demonstrate by investigating electron and hole polaron formation in alkali halides and metal oxides and peroxides. We outline refinements of our scheme and extensions to compute transport in the polaron hopping regime.

cond-mat.mtrl-sci↗

arXiv2020

Precise Radiative Lifetimes in Bulk Crystals from First Principles: The Case of Wurtzite GaN

Gallium nitride (GaN) is a key semiconductor for solid-state lighting, but its radiative processes are not fully understood. Here we show a first-principles approach to accurately compute the radiative lifetimes in bulk uniaxial crystals, focusing on wurtzite GaN. Our computed radiative lifetimes are in very good agreement with experiment up to 100 K. We show that taking into account excitons (through the Bethe-Salpeter equation) and spin-orbit coupling to include the exciton fine structure is essential for computing accurate radiative lifetimes. A model for exciton dissociation into free carriers allows us to compute the radiative lifetimes up to room temperature. Our work enables precise radiative lifetime calculations in III-nitrides and other anisotropic solid-state emitters.

cond-mat.mtrl-sci↗

arXiv2020

Exciton-Phonon Interaction and Relaxation Times from First Principles

Electron-phonon ($e$-ph) interactions are key to understanding the dynamics of electrons in materials, and can be modeled accurately from first-principles. However, when electrons and holes form Coulomb-bound states (excitons), quantifying their interactions and scattering processes with phonons remains an open challenge. Here we show a rigorous approach for computing exciton-phonon (ex-ph) interactions and the associated exciton dynamical processes from first principles. Starting from the ab initio Bethe-Salpeter equation, we derive expressions for the ex-ph matrix elements and relaxation times. We apply our method to bulk hexagonal boron nitride, for which we map the ex-ph relaxation times as a function of exciton momentum and energy, analyze the temperature and phonon-mode dependence of the ex-ph scattering processes, and accurately predict the phonon-assisted photoluminescence. The approach introduced in this work is general and provides a framework for investigating exciton dynamics in a wide range of materials.

cond-mat.mtrl-sci↗

arXiv2019

Ab Initio Calculations of Exciton Radiative Lifetimes in Bulk Crystals, Nanostructures and Molecules

Excitons are bound electron-hole pairs that dominate the optical response of semiconductors and insulators, especially in materials where the Coulomb interaction is weakly screened. Light absorption (including excitonic effects) has been studied extensively using first-principles calculations, but methods for computing radiative recombination and light emission are still being developed. Here we show a unified ab initio approach to compute exciton radiative recombination in materials ranging from bulk crystals to nanostructures and molecules. We derive the rate of exciton radiative recombination in bulk crystals, isolated systems, and in one- and two-dimensional materials, using Fermi's golden rule within the Bethe-Salpeter equation approach. We present benchmark calculations of radiative lifetimes in a GaAs crystal and in gas-phase organic molecules. Our work provides a general method for studying exciton recombination and light emission in bulk, nanostructured and molecular materials from first principles.

cond-mat.mtrl-sci↗

arXiv2019

Next-to-Leading Order Ab Initio Electron-Phonon Scattering

Electron-phonon (e-ph) interactions are usually treated in the lowest order of perturbation theory. Here we derive next-to-leading order e-ph interactions, and compute from first principles the associated two-phonon e-ph scattering rates. The derivation involves Matsubara sums of the relevant two-loop Feynman diagrams, and the numerical calculations are challenging since they involve Brillouin zone integrals over two crystal momenta and depend critically on the intermediate state lifetimes. Using random grids and Monte Carlo integration, together with a self-consistent update of the intermediate state lifetimes, we compute and converge the two-phonon scattering rates, using GaAs as a case study. For the longitudinal optical phonon in GaAs, we find that the two-phonon scattering rates are as large as nearly half the value of the leading-order rates. The energy and temperature dependence of the two-phonon processes are analyzed. We show that including the two-phonon processes is important to accurately predicting the electron mobility in GaAs.

cond-mat.mes-hall↗

arXiv2018

Theory and Ab Initio Computation of the Anisotropic Light Emission in Monolayer Transition Metal Dichalcogenides

Monolayer transition metal dichalcogenides (TMDCs) are direct gap semiconductors with unique potential for ultrathin light emitters. Yet, their photoluminescence (PL) is not completely understood. We compute the radiative recombination rate in monolayer TMDCs as a function of photon emission direction and polarization, and obtain polar plots of the PL for different excitation scenarios using the ab initio Bethe-Salpeter equation. We show that excitons in a quantum superposition state of the K and K' inequivalent valleys emit light anisotropically upon recombination. Our results can explain the PL anisotropy and polarization dependence measured in recent experiments, and predict new light emission regimes. When averaged over emission angle and exciton momentum, our new treatment recovers the temperature dependent radiative lifetimes we previously derived. Our work provides a first-principles approach to study light emission in two-dimensional materials.

cond-mat.mtrl-sci↗