arXiv subjects

Yang-Hao Chan

Publications and source records attributed to Yang-Hao Chan.

At least 19 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

Anisotropic hot carrier relaxation mediated by electron phonon scattering in TiN thin films

Crystal orientations can shape the ultrafast energy relaxations of transition-metal nitride thin films. Here, we investigate the orientation-dependent electron-phonon (e-ph) mediated relaxation in titanium nitride (TiN) thin films along the [100], [110], and [111] directions by combining first-principles calculations with ultrafast pump-probe transient absorption spectroscopy. Using maximally localized Wannier functions, we evaluate e-ph quasiparticle scattering lifetimes near the Fermi level and identify a clear anisotropy: The TiN [111] orientation exhibits a longer e-ph scattering lifetime (15.96 fs) than [100] (13.69 fs) and [110] (11.12 fs), indicating reduced intrinsic e-ph scattering strength. Furthermore, we grew quasi-epitaxial, orientation-controlled TiN thin films on MgO substrates. Pump-probe measurements reveals that the population-level relaxation (hot-electron cooling) time also depends on orientations, with [111] films showing a significantly slower decay (110 fs) than [100] (90 fs) and [110] (80 fs). We emphasize that the calculated few-femtosecond scattering lifetimes and the measured few-hundred-femtosecond cooling time respectively represent single-event scattering and collective cooling, yet they exhibit consistent trends. These results demonstrate that crystallographic orientation provides a practical and powerful route to tune e-ph-governed relaxation in TiN thin films, offering essential design guidelines for refractory plasmonic and energy-conversion platforms.

cond-mat.mtrl-sci↗

arXiv2025

Observation of charge density wave excitonic order parameter in topological insulator monolayer WTe2

Strong electron-hole interactions in a semimetal or narrow-gap semiconductor may drive a ground state of condensed excitons. Monolayer WTe2 has been proposed as a host material for such an exciton condensate, but the order parameter - the key signature of a macroscopic quantum-coherent condensate - has not been observed. Here we use Fourier-transform scanning tunnelling spectroscopy (FT-STS) to study quasi-particle interference (QPI) and periodic modulations of the local density of states (LDOS) in monolayer WTe2. In WTe2 on graphene, in which the carrier density can be varied via back-gating, FT-STS shows QPI features in the 2D bulk bands, confirming the interacting nature of the bandgap in neutral WTe2 and the semi-metallic nature of highly n- and p-doped WTe2. We observe additional non-dispersive spatial modulations in the LDOS imprinted on the topological edge mode of neutral WTe2 on metallic substrates (graphene and graphite), which we interpret as the interaction of the topological edge mode with the expected charge density wave order parameter of the excitonic condensate in WTe2 at low interaction strength due to screening by the metallic substrates.

cond-mat.str-el↗

arXiv2024

Excitonic effects on infrared vibrational and Raman spectroscopy from first principles

We develop a first-principles approach to compute infrared (IR) vibrational absorption and Raman scattering spectra with excitonic effects included. Our method is based on a perturbative expansion of electron-phonon and electron-light couplings in the time-dependent adiabatic GW (TD-aGW) theory. We show that excitonic effects in the IR absorption spectrum can be included by replacing the free electron-hole propagators in the perturbative expression for independent particles with their interacting counterparts, which are readily available from standard GW-Bethe-Salpeter equation calculations. For Raman spectrum, our derived expression agrees with the single and double resonance terms from a diagrammatic approach. We show significant excitonic enhancement in both the IR and resonance Raman scattering intensity for monolayer MoS2, WS2, and WSe2. Moreover, the exciton-phonon coupling strength and exciton energy landscape can be accessed by analyzing resonance Raman spectrum of these materials.

cond-mat.mtrl-sci↗

arXiv2024

Driving non-trivial quantum phases in conventional semiconductors with intense excitonic fields

Inducing novel quantum phases and topologies in materials using intense light fields is a key objective of modern condensed matter physics, but nonetheless faces significant experimental challenges. Alternately, theory predicts that in the dense limit, excitons - collective excitations composed of Coulomb-bound electron-hole pairs - could also drive exotic quantum phenomena. However, the direct observation of these phenomena requires the resolution of electronic structure in momentum space in the presence of excitons, which became possible only recently. Here, using time- and angle-resolved photoemission spectroscopy of an atomically thin semiconductor in the presence of a high-density of resonantly and coherently photoexcited excitons, we observe the Bardeen-Cooper-Schrieffer (BCS) excitonic state - analogous to the Cooper pairs of superconductivity. We see the valence band transform from a conventional paraboloid into a Mexican-hat like Bogoliubov dispersion - a hallmark of the excitonic insulator phase; and we observe the recently predicted giant exciton-driven Floquet effects. Our work realizes the promise that intense bosonic fields, other than photons, can also drive novel quantum phenomena and phases in materials.

cond-mat.mtrl-sci↗

arXiv2024

Engineering the strain and interlayer excitons of 2D materials via lithographically engraved hexagonal boron nitride

Strain engineering has quickly emerged as a viable option to modify the electronic, optical and magnetic properties of 2D materials. However, it remains challenging to arbitrarily control the strain. Here we show that by creating atomically-flat surface nanostructures in hexagonal boron nitride, we achieve an arbitrary on-chip control of both the strain distribution and magnitude on high-quality molybdenum disulfide. The phonon and exciton emissions are shown to vary in accordance with our strain field designs, enabling us to write and draw any photoluminescence color image in a single chip. Moreover, our strain engineering offers a powerful means to significantly and controllably alter the strengths and energies of interlayer excitons at room temperature. This method can be easily extended to other material systems and offers a promise for functional excitonic devices.

cond-mat.mes-hall↗

arXiv2023

Diagrammatic approach to excitonic effects on nonlinear optical response

Optical responses of atomically thin 2D materials are greatly influenced by electron-hole interactions. It is by far established that exciton signatures can be well-identified in the optical absorption spectrum of quasi-2D materials. However, the same level of understanding of excitonic effects on nonlinear optical responses and the ability to compute them accurately is still much desired. Based on the functional integral formalisms and working in the velocity gauge, we introduce a convenient Feynman diagram approach for calculating nonlinear responses including excitonic effects. By dressing electron-photon interactions with electron-hole ladder diagrams, we derive an expression for second-order optical responses and provide a comprehensive description of excitonic effects. We apply our approach to a monolayer h-BN model and show qualitative changes in the second harmonic generation spectrum when comparing with results assuming independent particles. Our approach can be readily extended to higher order optical responses and is feasible for first-principles calculations.

cond-mat.mes-hall↗

arXiv2023

A gate-tunable quantum phase transition in a topological excitonic insulator

Coulomb interactions among electrons and holes in two-dimensional (2D) semimetals with overlapping valence and conduction bands can give rise to a correlated insulating ground state via exciton formation and condensation. One candidate material in which such excitonic state uniquely combines with non-trivial band topology are atomic monolayers of tungsten ditelluride (WTe2), in which a 2D topological excitonic insulator (2D TEI) forms. However, the detailed mechanism of the 2D bulk gap formation in WTe2, in particular with regard to the role of Coulomb interactions, has remained a subject of ongoing debate. Here, we show that WTe2 is susceptible to a gate-tunable quantum phase transition, evident from an abrupt collapse of its 2D bulk energy gap upon ambipolar field-effect doping. Such gate tunability of a 2D TEI, into either n- and p-type semimetals, promises novel handles of control over non-trivial 2D superconductivity with excitonic pairing.

cond-mat.str-el↗

arXiv2023

Electron-phonon coupling from GW perturbation theory: Practical workflow combining BerkeleyGW, ABINIT, and EPW

We present a workflow of practical calculations of electron-phonon (e-ph) coupling with many-electron correlation effects included using the GW perturbation theory (GWPT). This workflow combines BerkeleyGW, ABINIT, and EPW software packages to enable accurate e-ph calculations at the GW self-energy level, going beyond standard calculations based on density functional theory (DFT) and density-functional perturbation theory (DFPT). This workflow begins with DFT and DFPT calculations (ABINIT) as starting point, followed by GW and GWPT calculations (BerkeleyGW) for the quasiparticle band structures and e-ph matrix elements on coarse electron k- and phonon q-grids, which are then interpolated to finer grids through Wannier interpolation (EPW) for computations of various e-ph coupling determined physical quantities such as the electron self-energies or solutions of anisotropic Eliashberg equations, among others. A gauge-recovering symmetry unfolding technique is developed to reduce the computational cost of GWPT (as well as DFPT) while fulfilling the gauge consistency requirement for Wannier interpolation.

cond-mat.mtrl-sci↗

arXiv2023

Excitonic interactions and mechanism for ultrafast interlayer photoexcited response in van der Waals heterostructures

Optical dynamics in van der Waals heterobilayers is of fundamental scientific and practical interest. Based on a time-dependent adiabatic GW approach, we discover a new many-electron (excitonic) channel for converting photoexcited intralayer to interlayer excitations and the associated ultrafast optical responses in heterobilayers, which is conceptually different from the conventional single-particle picture. We find strong electron-hole interactions drive the dynamics and enhance the pump-probe optical responses by an order of magnitude with a rise time of ~300 fs in MoSe$_2$/WSe$_2$ heterobilayers, in agreement with experiment.

cond-mat.mtrl-sci↗

arXiv2023

Large shift current via in-gap and charge-neutral exciton excitations in BN nanotubes and single BN layer

We perform {\it ab initio} many-body calculations to investigate the exciton shift current in small diameter zigzag BN nanotubes and also single BN sheet, using the GW plus Bethe-Salpeter equation (GW-BSE) method with the newly developed efficient algorithms. Our GW-BSE calculations reveal a giant in-gap peak in the shift current spectrum in all the studied BN systems due to the excitation of the A exciton. The peak value of the excitonic shift current is more than three times larger than that of the quasiparticle shift current, and is attributed to the gigantic enhancement of the optical dipole matrix element by the A exciton resonance. The effective exciton shift current conductivity is nearly ten times larger than the largest shift conductivity observed in ferroelectric semiconductors. Importantly, the direction of the shift current in the BN nanotubes is found to be independent of the tube chirality ($n,0$) (or diameter), contrary to the simple rule of $ sgn(J_\text{shift})=\text{mod}(n,3)$ predicted by previous model Hamiltonian studies. Finally, our {\it ab initio} calculations also show that the exciton excitation energies decrease significantly with the decreasing diameter due to the curvature-induced orbital rehybridization in small diameter zigzag BN nanotubes.

cond-mat.mes-hall↗

arXiv2021

Unmasking the Origin of Kinks in the Photoemission Spectra of Cuprate Superconductors

The origin of a ubiquitous bosonic coupling feature in the photoemission spectra of high-Tc cuprates, an energy-momentum dispersion 'kink' observed at ~70 meV binding energy, remains a two-decade-old mystery. Understanding this phenomenon requires an accurate description of the coupling between the electron and some collective modes. We report here ab initio calculations based on GW perturbation theory and show that correlation-enhanced electron-phonon interaction in cuprates gives rise to the strong kinks, which not only explains quantitatively the observations but provides new understanding of experiments. Our results reveal it is the electron density-of-states being the predominant factor in determining the doping-dependence of the kink size, manifesting the multi-band nature of the cuprates, as opposed to the prevalent belief of it being a measure of the mode-coupling strength.

cond-mat.supr-con↗

arXiv2020

Predominance of non-adiabatic effects in zero-point renormalization of the electronic band gap

Electronic and optical properties of materials are affected by atomic motion through the electron-phonon interaction: not only band gaps change with temperature, but even at absolute zero temperature, zero-point motion causes band-gap renormalization. We present a large-scale first-principles evaluation of the zero-point renormalization of band edges beyond the adiabatic approximation. For materials with light elements, the band gap renormalization is often larger than 0.3 eV, and up to 0.7 eV. This effect cannot be ignored if accurate band gaps are sought. For infrared-active materials, global agreement with available experimental data is obtained only when non-adiabatic effects are taken into account. They even dominate zero-point renormalization for many materials, as shown by a generalized Fröhlich model that includes multiple phonon branches, anisotropic and degenerate electronic extrema, whose range of validity is established by comparison with first-principles results.

cond-mat.mtrl-sci↗

arXiv2018

In-situ strain tuning of the Dirac surface states in Bi2Se3 films

Elastic strain has the potential for a controlled manipulation of the band gap and spin-polarized Dirac states of topological materials, which can lead to pseudo-magnetic-field effects, helical flat bands and topological phase transitions. However, practical realization of these exotic phenomena is challenging and yet to be achieved. Here, we show that the Dirac surface states of the topological insulator Bi2Se3 can be reversibly tuned by an externally applied elastic strain. Performing in-situ x-ray diffraction and in-situ angle-resolved photoemission spectroscopy measurements during tensile testing of epitaxial Bi2Se3 films bonded onto a flexible substrate, we demonstrate elastic strains of up to 2.1% and quantify the resulting reversible changes in the topological surface state. Our study establishes the functional relationship between the lattice and electronic structures of Bi2Se3 and, more generally, demonstrates a new route toward momentum-resolved mapping of strain-induced band structure changes.

cond-mat.mtrl-sci↗

arXiv2018

Ising order in a magnetized Heisenberg chain subject to a uniform Dzyaloshinskii-Moriya interaction

We report a combined analytical and density matrix renormalized group study of the antiferromagnetic XXZ spin-1/2 Heisenberg chain subject to a uniform Dzyaloshinskii-Moriya (DM) interaction and a transverse magnetic field. The numerically determined phase diagram of this model, which features two ordered Ising phases and a critical Luttinger liquid one with fully broken spin-rotational symmetry, agrees well with the predictions of Garate and Affleck [Phys. Rev. B 81, 144419 (2010)]. We also confirm the prevalence of the N z Néel Ising order in the regime of comparable DM and magnetic field magnitudes.

cond-mat.str-el↗

arXiv2017

Gapped Electronic Structure of Epitaxial Stanene on InSb(111)

Stanene (single-layer grey tin), with an electronic structure akin to that of graphene but exhibiting a much larger spin-orbit gap, offers a promising platform for room-temperature electronics based on the quantum spin Hall (QSH) effect. This material has received much theoretical attention, but a suitable substrate for stanene growth that results in an overall gapped electronic structure has been elusive; a sizable gap is necessary for room-temperature applications. Here, we report a study of stanene epitaxially grown on the (111)B-face of indium antimonide (InSb). Angle-resolved photoemission spectroscopy (ARPES) measurements reveal a gap of 0.44 eV, in agreement with our first-principles calculations. The results indicate that stanene on InSb(111) is a strong contender for electronic QSH applications.

cond-mat.mtrl-sci↗

arXiv2017

Strain Engineering a $4a\times\sqrt{3}a$ Charge Density Wave Phase in Transition Metal Dichalcogenide 1T-VSe$_2$

We report a rectangular charge density wave (CDW) phase in strained 1T-VSe$_2$ thin films synthesized by molecular beam epitaxy on c-sapphire substrates. The observed CDW structure exhibits an unconventional rectangular 4a{\times}{\sqrt{3a}} periodicity, as opposed to the previously reported hexagonal $4a\times4a$ structure in bulk crystals and exfoliated thin layered samples. Tunneling spectroscopy shows a strong modulation of the local density of states of the same $4a\times\sqrt{3}a$ CDW periodicity and an energy gap of $2Δ_{CDW}=(9.1\pm0.1)$ meV. The CDW energy gap evolves into a full gap at temperatures below 500 mK, indicating a transition to an insulating phase at ultra-low temperatures. First-principles calculations confirm the stability of both $4a\times4a$ and $4a\times\sqrt{3}a$ structures arising from soft modes in the phonon dispersion. The unconventional structure becomes preferred in the presence of strain, in agreement with experimental findings.

cond-mat.mtrl-sci↗

arXiv2017

Elemental topological Dirac semimetal: α-Sn on InSb(111)

Three-dimensional (3D) topological Dirac semimetals (TDSs) are rare but important as a versatile platform for exploring exotic electronic properties and topological phase transitions. A quintessential feature of TDSs is 3D Dirac fermions associated with bulk electronic states near the Fermi level. Using angle-resolved photoemission spectroscopy (ARPES), we have observed such bulk Dirac cones in epitaxially-grown α-Sn films on InSb(111), the first such TDS system realized in an elemental form. First-principles calculations confirm that epitaxial strain is key to the formation of the TDS phase. A phase diagram is established that connects the 3D TDS phase through a singular point of a zero-gap semimetal phase to a topological insulator (TI) phase. The nature of the Dirac cone crosses over from 3D to 2D as the film thickness is reduced.

cond-mat.mtrl-sci↗