arXiv subjects

Chih-En Hsu

Publications and source records attributed to Chih-En Hsu.

11 recordsLinked to original sources

arXiv2026

Ab initio time-dependent GW approach for nonequilibrium exciton-phonon coupled dynamics across momentum space

The dynamics of optical excitations in materials generally involves intertwined electron-hole (e-h) and electron-phonon (e-ph) interactions out of equilibrium. However, a full theoretical description of such nonequilibrium dynamics requires a systematic treatment of the coherent excitonic excitations and exciton-phonon interactions across the entire crystal momentum space in real time, which remains a major challenge and out of reach for first-principles approaches. Here, we present a new ab initio time-dependent adiabatic GW methodology that incorporates full finite-momentum e-h and e-ph couplings, enabling real-time simulations of the coherently coupled exciton-phonon dynamics. The excitonic excitations are naturally described by the equation of motion of the interacting single-particle density matrix, whereas their couplings to phonons are formulated within a linear-response framework, hence the simulations can be efficiently carried out within a primitive unit cell. We demonstrate the capabilities of this new approach by investigating the direct-to-indirect exciton transitions in monolayer WSe2 in a pump-probe setup of time-resolved and angle-resolved photoemission spectroscopy. Our results reveal that the phonon-mediated ultrafast intervalley dynamics of excitons of this system is within ~0.5 ps, manifested as in-gap photoemission intensity transfer from the K-valley to the Q-valley. This work establishes a comprehensive and practical nonequilibrium Green's function framework for accurately simulating nonequilibrium and coherent excitations involving coupled excitons and phonons from first principles.

cond-mat.mtrl-sci↗

arXiv2026

Layer-tunable Hubbard bands probed via moir\'e excitons in MoSe$_2$/WS$_2$ heterostructures

Moir\'e superlattices in transition metal dichalcogenide heterostructures provide a highly tunable platform for engineering strongly interacting states at the nanoscale. However, quantitatively determining and in-situ tuning of the underlying Hubbard parameters remains experimentally challenging. Here, we report electric-field-driven reordering of layer-specific Hubbard bands by performing optical spectroscopy on a dual-gated, 60{\deg}-aligned MoSe$_2$/WS$_2$ heterobilayer. Using two spatially distinct moir\'e excitons as local optical probes and tracking them as a function of carrier filling and vertical electric field, we quantitatively extract the layer-dependent on-site Coulomb repulsions, U$_M$~60 meV in MoSe$_2$ and U$_W$~30 meV in WS$_2$. Furthermore, we stabilize generalized Wigner crystal and stripe phases by electrostatically tuning the system to a type-II band alignment, shifting the ground state into the WS$_2$ layer where reduced on-site repulsion allows inter-site Coulomb interactions to dominate. Our results establish vertical electric fields as a deterministic tuning knob for layer-selective Hubbard physics, enabling device-level control of complex many-body phases.

cond-mat.mes-hall↗

arXiv2025

Many-Body Correlation Effects in Fr\"ohlich Electron-Phonon Coupling

In compound semiconductors and insulators, the polar electron-phonon coupling diverges at long range, known as the Fr\"ohlich interaction. Modern first-principles electron-phonon calculations treat the Fr\"ohlich interaction in a semiclassical electrostatic formalism based on density-functional perturbation theory. Here, using many-body $GW$ perturbation theory, we reveal important electron correlation effects in the Fr\"ohlich-type electron-phonon coupling, which are missed by the prevailing approaches and rooted in the fundamentally distinct behavior between quasiparticle self-energy and semi-local exchange-correlation functionals in the long-range limit. Going beyond the electrostatic treatment, we derive and implement the $GW$ self-energy contribution to the long-range polar electron-phonon coupling, and demonstrate its critical role and nontrivial behaviors in properties such as electron linewidth and polaron formation in several prototype semiconductors. Remarkably, calculations on photoemission kink in electron-doped TiO$_2$ achieve excellent agreement with experiment. Our work establishes the many-body generalization of the Fr\"ohlich interaction that is essential for accurate electron-phonon calculations at the full $GW$ level combined with Wannier interpolation techniques.

cond-mat.mtrl-sci↗

arXiv2025

Advancing Quantum Many-Body GW Calculations on Exascale Supercomputing Platforms

Advanced ab initio materials simulations face growing challenges as increasing systems and phenomena complexity requires higher accuracy, driving up computational demands. Quantum many-body GW methods are state-of-the-art for treating electronic excited states and couplings but often hindered due to the costly numerical complexity. Here, we present innovative implementations of advanced GW methods within the BerkeleyGW package, enabling large-scale simulations on Frontier and Aurora exascale platforms. Our approach demonstrates exceptional versatility for complex heterogeneous systems with up to 17,574 atoms, along with achieving true performance portability across GPU architectures. We demonstrate excellent strong and weak scaling to thousands of nodes, reaching double-precision core-kernel performance of 1.069 ExaFLOP/s on Frontier (9,408 nodes) and 707.52 PetaFLOP/s on Aurora (9,600 nodes), corresponding to 59.45% and 48.79% of peak, respectively. Our work demonstrates a breakthrough in utilizing exascale computing for quantum materials simulations, delivering unprecedented predictive capabilities for rational designs of future quantum technologies.

cond-mat.mtrl-sci↗

arXiv2025

Moir\'e excitons in generalized Wigner crystals

Moir\'e superlattices of transition-metal dichalcogenide bilayers host strong Coulomb interactions residing in narrow electron bands, leading to correlated insulating states at fractional carrier doping densities, known as generalized Wigner crystals. In excited states, the formation of moir\'e excitons is expected to be fundamentally shaped by the Wigner-crystal ground states, manifesting an intricate interplay between electronic and excitonic correlations. However, the microscopic description of these Wigner crystalline excitons (WCEs) remains elusive, largely subject to speculations, and is further needed for the understanding of exotic excitonic phases (e.g., exciton insulators and exciton density waves) and their unique properties (e.g., anomalous exciton diffusion). Here, using first-principles many-body GW-Bethe-Salpeter-equation calculations, we directly reveal the internal structures of WCEs in angle-aligned MoSe2/MoS2 moir\'e heterostructure at hole fillings of 1/3 and 2/3. Our results unveil the propagation of correlation effects from the ground state to excited states, shaping the real-space characteristics of WCEs. The strong two-particle excitonic correlations dominate over the kinetic energy of free electron-hole pairs, in analog to the strong single-particle correlations of flat bands. We propose that such unusual excited-state correlation effects of WCEs can be experimentally probed by photocurrent tunneling microscopy. Our work provides a microscopic understanding of strongly correlated WCEs, suggesting them as a highly tunable mixed boson-fermion platform to study many-body interactions and phenomena.

cond-mat.mtrl-sci↗

arXiv2025

High-Throughput GW Calculations via Machine Learning

We present a machine learning (ML) framework that predicts $G_0W_0$ quasiparticle energies across molecular dynamics (MD) trajectories with high accuracy and efficiency. Using only DFT-derived mean-field eigenvalues and exchange-correlation potentials, the model is trained on 25\% of MD snapshots and achieves RMSEs below 0.1 eV. It accurately reproduces k-resolved quasiparticle band structures and density of states, even for BN polymorphs excluded from the training data. This approach bypasses the computational bottlenecks of $G_0W_0$ simulations over dynamic configurations, offering a scalable route to excited-state electronic structure simulations with many-body accuracy.

cond-mat.mtrl-sci↗

arXiv2025

Correlated insulating states in slow Dirac fermions on a honeycomb moir{\'e} superlattice

Strong Coulomb repulsion is predicted to open a many-body charge gap at the Dirac point of graphene, transforming the semimetal into a Mott insulator. However, this correlated insulating phase has remained inaccessible in pristine graphene, where a large Fermi velocity dominates the interaction effects. To overcome this limitation, we realize a honeycomb moir{\'e} superlattice in a twisted MoSe$_2$ homobilayer, where a graphene-like band structure forms with a Fermi velocity reduced by nearly two orders of magnitude. These slow moir{\'e} bands are folded from the valence band maximum at the $\Gamma$ valley of the extended Brillouin zone with negligible spin-orbital coupling, and can therefore simulate massless Dirac fermions in the strongly correlated regime with full SU(2) symmetry. By correlating Rydberg exciton sensing with moir{\'e} trions of different spatial characters, we detect a Mott gap at the Dirac point that persists up to 110 K. We further identify correlated insulating states at $\nu=-1$ with a weak ferromagnetic coupling as well as at several fractional fillings. Our results highlight the potential of studying a wide range of quantum many-body phenomena in twisted two-dimensional materials.

cond-mat.mes-hall↗

arXiv2025

Theory of ab initio downfolding with arbitrary range electron-phonon coupling

Ab initio downfolding describes the electronic structure of materials within a low-energy subspace, often around the Fermi level. Typically starting from mean-field calculations, this framework allows for the calculation of one- and two-electron interactions, and the parametrization of a many-body Hamiltonian representing the active space of interest. The subsequent solution of such Hamiltonians can provide insights into the physics of strongly-correlated materials. While phonons can substantially screen electron-electron interactions, electron-phonon coupling has been commonly ignored within ab initio downfolding, and when considered this is done only for short-range interactions. Here we propose a theory of ab initio downfolding that accounts for all mechanisms of electron-phonon coupling on equal footing, regardless of the range of the interactions. Our practical computational implementation is readily compatible with current downfolding approaches. We apply our approach to polar materials MgO and GeTe, and we reveal the importance of both short-range and long-range electron-phonon coupling in determining the magnitude of electron-electron interactions. Our results show that in the static limit, phonons reduce the on-site repulsion between electrons by 40% for MgO, and by 79% for GeTe. Our framework also predicts that overall attractive nearest-neighbor interactions arise between electrons in GeTe, consistent with superconductivity in this material.

cond-mat.mtrl-sci↗

arXiv2025

Phonon-mediated electron attraction in SrTiO$_3$ via the generalized Fr\"ohlich and deformation potential mechanisms

Superconductivity in doped SrTiO$_3$ was discovered in 1964, the first superconducting transition observed in a doped semiconductor. However, the mechanism of electron pairing in SrTiO$_3$ remains a subject of debate. By developing a theoretical framework to incorporate dynamical lattice screening in the electronic Coulomb interactions of semiconductors and insulators, we demonstrate analytically that linear long-range coupling of electrons to multiple longitudinal optical phonons, described by a generalized Fr\"ohlich mechanism, can result in superconductivity in SrTiO$_3$. Moreover, by combining our theory with first-principles calculations, we reveal an additional attractive interaction between electrons in SrTiO$_3$ due to the deformation potential mechanism, arising from the mixed ionic-covalent character of the Ti-O bond. Our results may have implications for the emergence of phonon-mediated electron attraction and superconductivity in a broad range of materials.

cond-mat.supr-con↗

arXiv2024

Diverse Manifestations of Electron-Phonon Coupling in a Kagome Superconductor

Recent angle-resolved photoemission spectroscopy (ARPES) experiments on a kagome metal CsV$_3$Sb$_5$ revealed distinct multimodal dispersion kinks and nodeless superconducting gaps across multiple electron bands. The prominent photoemission kinks suggest a definitive coupling between electrons and certain collective modes, yet the precise nature of this interaction and its connection to superconductivity remain to be established. Here, employing the state-of-the-art \textit{ab initio} many-body perturbation theory computation, we present direct evidence that electron-phonon ($e$-ph) coupling induces the multimodal photoemission kinks in CsV$_3$Sb$_5$, and profoundly, drives the nodeless $s$-wave superconductivity, showcasing the diverse manifestations of the $e$-ph coupling. Our calculations well capture the experimentally measured kinks and their fine structures, and reveal that vibrations from different atomic species dictate the multimodal behavior. Results from anisotropic $GW$-Eliashberg equations predict a phonon-mediated superconductivity with nodeless $s$-wave gaps, in excellent agreement with various ARPES and scanning tunneling spectroscopy measurements. Despite of the universal origin from the $e$-ph coupling, the contributions of several characteristic phonon vibrations vary in different phenomena, highlighting a versatile role of $e$-ph coupling in shaping the low-energy excitations of kagome metals.

cond-mat.supr-con↗

arXiv2024

Efficient light upconversion via resonant exciton-exciton annihilation of dark excitons in few-layer transition metal dichalcogenides

In this work, we report a pronounced light upconversion in few-layer transition metal dichalcogenides. Our joint theory-experiment study attributes the upconversion photoluminescence to a resonant exciton-exciton annihilation involving a pair of dark excitons with opposite momenta, followed by the spontaneous emission of upconverted bright excitons, which can have a high upconversion efficiency. Additionally, the upconversion photoluminescence is generic in MoS2, MoSe2, WS2, and WSe2, showing a high tuneability from green to ultraviolet light.

cond-mat.mtrl-sci↗