arXiv subjects

Thomas Frauenheim

Publications and source records attributed to Thomas Frauenheim.

At least 19 recordsLinked to original sources

arXiv2025

Over One Order of Magnitude Enhancement in Hole Mobility of 2D III-V Semiconductors through Valence Band Edge Shift

Two-dimensional (2D) semiconductors show great potential to sustain Moore's law in the era of ultra-scaled electronics. However, their scalable applications are severely constrained by low hole mobility. In this work, we take 2D-GaAs as a prototype of III-V semiconductors to investigate the effects of quantum anharmonicity (QA) on hole transport, employing the stochastic self-consistent harmonic approximation assisted by the machine learning potential. It is found that the room-temperature hole mobility of 2D-GaAs is reduced by $\sim$44% as the QA effects are incorporated, which is attributed to the enhanced electron-phonon scattering from the out-of-plane acoustic polarization. The valence band edge shift (VBES) strategy is proposed to increase the hole mobility by $\sim$1600% at room temperature, which can be realized by 1% biaxial compressive strain. The electron-phonon scattering rate is dramatically decreased due to the full filtering of the original interband electron-phonon scattering channels that existed in the flat hole pocket. The VBES strategy can be further extended to other 2D III-V semiconductors to promote their hole mobilities.

cond-mat.mtrl-sci↗

arXiv2025

Electronic and optical and topological properties of defects in bismuthene

In this work we use first principles density-functional theory and Bethe-Salpeter equation together with tight-binding based maximally localized wannier functions (MLWF-TB) to investigate the electronic, optical and topological properties of two-dimensional bismuth (bismuthene) containing vacancy defects. We demonstrate that these properties depends on the shape and size of the nanopores. Furthermore, \textit{ab initio} molecular dynamics (AIMD) simulations shows that all pores are thermally stable at room temperature. Finally, adsorption of gas phase small molecules indicates that these pores can serve as sensors, opening the path for further applications in gas separation and sensing.

cond-mat.mtrl-sci↗

arXiv2024

Unlocking high hole mobility in diamond over a wide temperature range via efficient shear strain

As a wide bandgap semiconductor, diamond holds both excellent electrical and thermal properties, making it highly promising in the electrical industry. However, its hole mobility is relatively low and dramatically decreases with increasing temperature, which severely limits further applications. Herein, we proposed that the hole mobility can be efficiently enhanced via slight compressive shear strain along the [100] direction, while the improvement via shear strain along the [111] direction is marginal. This impressive distinction is attributed to the deformation potential and the elastic compliance matrix. The shear strain breaks the symmetry of the crystalline structure and lifts the band degeneracy near the valence band edge, resulting in a significant suppression of interband electron-phonon scattering. Moreover, the hole mobility becomes less temperature-dependent due to the decrease of electron scatterings from high-frequency acoustic phonons. Remarkably, the in-plane hole mobility of diamond is increased by approximately 800% at 800 K with a 2% compressive shear strain along the [100] direction. The efficient shear strain strategy can be further extended to other semiconductors with face-centered cubic geometry.

cond-mat.mtrl-sci↗

arXiv2024

Giant enhancement of hole mobility for 4H-silicon carbide through suppressing interband electron-phonon scattering

4H-Silicon Carbide (4H-SiC) possesses a high Baliga figure of merit, making it a promising material for power electronics. However, its applications are limited by its low hole mobility. Herein, we found that the hole mobility of 4H-SiC is mainly limited by the strong interband electron-phonon scattering using mode-level first-principles calculations. Our research indicates that applying compressive strain can reverse the sign of crystal-field splitting and change the ordering of electron bands close to the valence band maximum. Therefore, the interband electron-phonon scattering is severely suppressed, and the out-of-plane hole mobility of 4H-SiC can be enhanced by 200% with 2% uniaxial compressive strain applied. This work provides new insights into the electron transport mechanisms in semiconductors and suggests a strategy to improve hole mobility that could be applied to other semiconductors with hexagonal crystalline geometries.

cond-mat.mtrl-sci↗

arXiv2024

Coherent Phonon Control of Ultrafast Magnetization Dynamics in Fe$_\text{3}$GeTe$_\text{2}$ from Time-Dependent Ab Initio Theory

Exploring ultrafast magnetization control in two-dimensional (2D) magnets through optically driven coherent phonons has been well-established. Yet, the microscopic interplay between spin dynamics and lattice degrees of freedom remains less explored. Employing real-time time-dependent density functional theory (rt-TDDFT) coupled with Ehrenfest dynamics, we systematically investigate laser-induced spin-nuclei dynamics with coherent phonon excitation in the 2D ferromagnet Fe3GeTe2. We found that selectively pre-exciting three typical coherent phonon modes results in up to a 53% additional spin moment loss in an out-of-plane A2 1g mode within ~50 fs. Coherent phonon control of spin dynamics is closely linked to laser pulse parameters. The underlying microscopic mechanism of this phenomenon is primarily governed by coherent phonon-induced asymmetric spin-resolved charge transfer following the disappearance of the laser pulse, thereby enabling effective control of the spin moment loss. Our findings offer a novel insight into the coupling of coherent phonons with spin systems in 2D limits on femtosecond timescales.

physics.comp-ph↗

arXiv2024

Phonon-induced band gap renormalization by dielectric dependent global hybrid density functional tight-binding

Accurate electronic bandstructures of solids are indispensable for a wide variety of applications and should provide a sound prediction of phonon-induced band gap renormalization at finite temperatures. We employ our previously introduced formalism of general hybrid functionals within the approximate density functional method, DFTB, to present first insights into the accuracy of temperature dependent band gaps obtained by a dielectric-dependent global hybrid functional. The work targets the prototypical group-IV semiconductors diamond and silicon. Following Zacharias et al. [Phys. Rev. Lett. 115, 177401 (2015)], we sample the nuclear wave function by stochastic Monte-Carlo integration as well as the deterministic one-shot procedure [Phys. Rev. B 94, 075125 (2016)] derived from it. The computational efficiency of DFTB enables us to further compare these approaches, which fully take nuclear quantum effects into account, with classical Born-Oppenheimer molecular dynamic (BOMD) simulations. While the quantum mechanical treatments of Zacharias et al. yield band gaps in good agreement with experiment, calculations based on BOMD snapshots inadequately describe the renormalization effect at low temperatures. We demonstrate the importance of properly incorporating nuclear quantum effects by adapting the stochastic approach to normal amplitudes that arise from the classical equipartition principle. For low temperatures the results thus obtained closely resemble the BOMD predictions, while anharmonic effects become important beyond $500\,\mathrm{K}$. Comparisons between DFTB parametrized from semi-local DFT, and global hybrid DFTB, suggest that Fock-type exchange systematically yields a slightly more pronounced electron-phonon interaction, hence stronger gap renormalization and zero-point corrections.

physics.comp-ph↗

arXiv2024

Optically Helicity-Dependent Orbital and Spin Dynamics in Two-Dimensional Ferromagnets

Disentangling orbital (OAM) and spin (SAM) angular momenta in the ultrafast spin dynamics of two-dimensional (2D) ferromagnets on subfemtoseconds is a challenge in the field of ultrafast magnetism. Herein, we employed non-collinear spin version of real-time time-dependent density functional theory to investigate the orbital and spin dynamics of 2D ferromagnets Fe3GeTe2 (FGT) induced by circularly polarized light. Our results show the demagnetization of Fe sublattice in FGT is accompanied by helicity-dependent precession of OAM and SAM excited by circularly polarized lasers. We further identify that precession of OAM and SAM in FGT is faster than the demagnetization within a few femtoseconds. Remarkably, circularly polarized lasers can significantly induce a periodically transverse response of OAM and SAM on very ultrafast timescales of ~250 attoseconds. Our finding suggests a powerful new route for attosecond regimes of the angular momentum manipulation to coherently control helicity-dependent orbital and spin dynamics in 2D limits.

cond-mat.mtrl-sci↗

arXiv2023

Elemental Ferroelectric Topological Insulator in $ψ$-bismuthene

Ferroelectric quantum spin Hall insulator (FEQSHI) exhibits coexisting ferroelectricity and time-reversal symmetry protected edge states, holding fascinating prospects for inviting both scientific and application advances, especially in two dimensions. However, all of the previously demonstrated FEQSHIs consist two or more constituent elements. We herein propose the $ψ$-bismuthene, an uncharted allotrope of bilayer Bi (110), to be the first example of 2D elemental FEQSHI. It is demonstrated that $ψ$-bismuthene harbors measurable ferroelectric polarization and nontrivial band gap with moderate switching barrier, which are highly beneficial for the detection and observation of the ferroelectric topologically insulating states. In addition, all-angle auxetic behavior with giant negative Poisson's ratio and ferroelectric controllable persistent spin helix in $ψ$-bismuthene are also discussed. The emergent elemental FEQSHI represents a novel domain for both fundamental physics and technological innovation.

cond-mat.mtrl-sci↗

arXiv2023

Ultrafast nonadiabatic electron dynamics in photoexcited C60: A comparative study among DFT exchange-correlation functionals

The non-radiative electron-relaxation dynamics in C$_{60}$ molecule is studied after selective initial photoexcitations. The methodology includes nonadibabtic molecular simulation combined with time-dependent density functional theory (DFT) and semi-classical surface hopping approach. Results of treating the DFT exchange-correlation (xc) interaction by the non-empirical Perdew-Burke-Ernzerhof (PBE), hybrid PBE0, and hybrid Becke 3-parameter Lee-Yang-Parr (B3LYP) functional are compared. Even though some differences in the details are found, all three functionals produce qualitatively similar unoccupied band structures in the ground state. The model-dependent differences in the ultrafast population dynamics, including the occurrences of transient entrapment of population, are studied systematically. The trend of the results demonstrates a universal dependence on the structure of unoccupied band offering a spectroscopic route to probe this structure. Results can be verified, as well as the best xc model for quantitative accuracy can be determined, by comparing with ultrafast transient absorption or time-resolved photoelectron spectroscopy measurements. From the computational standpoint, the study facilitates method optimization to simulate nonadiabatic relaxation dynamics in technologically important fullerene derivatives.

physics.atm-clus↗

arXiv2023

Hybrid functionals for periodic systems in the density functional tight-binding method

Screened range-separated hybrid (SRSH) functionals within generalized Kohn-Sham density functional theory (GKS-DFT) have been shown to restore a general $1/(r\varepsilon)$ asymptotic decay of the electrostatic interaction in dielectric environments. Major achievements of SRSH include an improved description of optical properties of solids and correct prediction of polarization-induced fundamental gap renormalization in molecular crystals. The density functional tight-binding method (DFTB) is an approximate DFT that bridges the gap between first principles methods and empirical electronic structure schemes. While purely long-range corrected RSH are already accessible within DFTB for molecular systems, this work generalizes the theoretical foundation to also include screened range-separated hybrids, with conventional pure hybrid functionals as a special case. The presented formulation and implementation is also valid for periodic boundary conditions (PBC) beyond the $Γ$-point. To treat periodic Fock exchange and its integrable singularity in reciprocal space, we resort to techniques successfully employed by DFT, in particular a truncated Coulomb operator and the minimum image convention. Starting from the first principles Hartree-Fock operator, we derive suitable expressions for the DFTB method, using standard integral approximations and their efficient implementation in the DFTB+ software package. Convergence behavior is investigated and demonstrated for the polyacene series as well as two- and three-dimensional materials. Benzene and pentacene molecular and crystalline systems show the correct polarization-induced gap renormalization by SRSH-DFTB at heavily reduced computational cost compared to first principles methods.

physics.comp-ph↗

arXiv2023

Ferroelectric Antiferromagnetic Quantum Anomalous Hall Insulator in TwoDimensional van der Waals Materials

Ferroelectricity, anti-ferromagnetism (AFM) and quantum anomalous Hall effect (QAHE) are three fundamental phenomena in the field of condensed matter physics, which could enable the realization of novel devices and thus attracts great attention. Here, we show theoretical evidence that twodimensional (2D) even-layer MnBi2Te4 allows for the simultaneous presence of intercorrelated ferroelectricity, AFM, and QAHE. Importantly, through rational van der Waals sliding, these exotic properties are strongly coupled. Such coupling could demonstrate many distinctive physics, for example, ferroelectric control of itinerant AFM phase and the sign of quantized anomalous Hall plateau.The explored phenomena and mechanism would not only enrich the research in 2D ferroelectricity and topological magnets, but also guide the design of low-consumption high-speed quantum devices.

physics.comp-ph↗

arXiv2022

Plasmonic Resonant Intercluster Coulombic Decay

Light-induced energy confinement in nanoclusters via plasmon excitations influences applications in nanophotonics, photocatalysis, and the design of controlled slow electron sources. The resonant decay of these excitations through the cluster's ionization continuum provides a unique probe of the collective electronic behavior. However, the transfer of a part of this decay amplitude to the continuum of a second conjugated cluster may offer control and efficacy in sharing the energy nonlocally to instigate remote collective events. With the example of a spherically nested dimer Na20@C240 of two plasmonic systems we find that such a transfer is possible through the resonant intercluster Coulomb decay (RICD) as a fundamental process. This plasmonic RICD signal can be experimentally detected by the photoelectron velocity map imaging technique.

physics.atm-clus↗

arXiv2022

Molecular Dynamics Study of Plasmon-Mediated Chemical Transformations

Heterogeneous catalysis of adsorbates on metallic surfaces mediated by plasmon has potential high photoelectric conversion efficiency and controllable reaction selectivity. Theoretical modeling of dynamical reaction processes provides in-depth analyses complementing experimental investigations. Especially for plasmon-mediated chemical transformations, light absorption, photoelectric conversion, electron-electron scattering, and electron-phonon coupling occur simultaneously at different timescales, rendering it very challenging to delineate the complex interplay of different factors. In this work, a trajectory surface hopping non-adiabatic molecular dynamics method is used to investigate the dynamics of plasmon excitation in an Au$_{20}$-CO system, including hot carrier generation, plasmon energy relaxation, and CO activation induced by electron-vibration coupling. The electronic properties indicate that when Au$_{20}$-CO is excited, a partial charge transfer takes place from Au$_{20}$ to CO. On the other hand, the dynamical simulations show that hot carriers generated after plasmon excitation transfer back and forth between Au$_{20}$ and CO. Meanwhile, the C-O stretching mode is activated due to the non-adiabatic couplings. The efficiency of plasmon-mediated transformation ($\sim$40\%) is obtained based on the ensemble average of these quantities. Our simulations provide important dynamical and atomistic insights into plasmon-mediated chemical transformation from the perspective of non-adiabatic simulations.

physics.chem-ph↗

arXiv2022

Ultrafast optically induced magnetic state transition in 2D antiferromagnets

Manipulating spin in antiferromagnetic (AFM) materials has great potential in AFM opto-spintronics. Laser pulses can induce a transient ferromagnetic (FM) state in AFM metallic systems, but have never been proven in two-dimensional (2D) AFM semiconductors and related van der Waals (vdW) heterostructures. Here, using 2D vdW heterostructures of FM MnS2 and AFM MXenes as prototypes, we investigated optically induced interlayer spin transfer dynamics based on the real-time time-dependent density functional theory (rt-TDDFT). We observed that laser pulses induce significant spin injection and the interfacial atom-mediated spin transfer from MnS2 to Cr2CCl2. In particular, we first demonstrated the transient FM state in semiconducting AFM/FM heterostructures during photoexcited processes. Because the proximity magnetism breaks the magnetic symmetry of Cr2CCl2 in heterostructures. Our results provide the microscopic understanding for optically controlled interlayer spin dynamics in 2D magnetic heterostructures and open a new way to manipulate magnetic orders in ultrafast opto-spintronics.

cond-mat.mtrl-sci↗

arXiv2022

Fortnet, a software package for training Behler-Parrinello neural networks

A new, open source, parallel, stand-alone software package (Fortnet) has been developed, which implements Behler-Parrinello neural networks. It covers the entire workflow from feature generation to the evaluation of generated potentials, coupled with higher-level analysis such as the analytic calculation of atomic forces. The functionality of the software package is demonstrated by driving the training for the fitted correction functions of the density functional tight binding (DFTB) method, which are commonly used to compensate the inaccuracies resulting from the DFTB approximations to the Kohn-Sham Hamiltonian. The usual two-body form of those correction functions limits the transferability of the parameterizations between very different structural environments. The recently introduced DFTB+ANN approach strives to lift these limitations by combining DFTB with a near-sighted artificial neural network (ANN). After investigating various approaches, we have found the combination of DFTB with an ANN acting on-top of some baseline correction functions (delta learning) the most promising one. It allowed to introduce many-body corrections on top of two-body parametrizations, while excellent transferability to chemical environments with deviating energetics could be demonstrated.

physics.chem-ph↗

arXiv2022

Dynamical evolution of the Schottky barrier as a determinant contribution to electron-hole pair stabilization and photocatalysis of plasmon-induced hot carriers

The harnessing of plasmon-induced hot carriers promises to open new avenues for the development of clean energies and chemical catalysis. The extraction of carriers before thermalization and recombination is of primordial importance to obtain appealing conversion yields. Here, hot carrier injection in the paradigmatic Au-TiO$_{2}$ system is studied by means of electronic and electron-ion dynamics. Our results show that pure electronic features (without considering many-body interactions or dissipation to the environment) contribute to the electron-hole separation stability. These results reveal the existence of a dynamic contribution to the interfacial potential barrier (Schottky barrier) that arises at the charge injection pace, impeding electronic back transfer. Furthermore, we show that this charge separation stabilization provides the time needed for the charge to leak to capping molecules placed over the TiO$_{2}$ surface triggering a coherent bond oscillation that will lead to a photocatalytic dissociation. We expect that our results will add new perspectives to the interpretation of the already detected long-lived hot carrier lifetimes, their catalytical effect, and concomitantly to their technological applications.

cond-mat.mes-hall↗

arXiv2022

Fano resonance and incoherent interlayer excitons in molecular van der Waals heterostructures

Complex van der Waals heterostructures from layered molecular stacks are promising optoelectronic materials offering means to efficient, modular charge separation and collection layers. The effect of stacking in the electrodynamics of such hybrid organic-inorganic two-dimensional materials remains largely unexplored, whereby molecular scale engineering could lead to advanced optical phenomena. For instance, tunable Fano engineering could make possible on-demand transparent conducting layers or photoactive elements, and passive cooling. We employ an adapted Gersten-Nitzan model and real time time-dependent density functional tight-binding to study the optoelectronics of self-assembled monolayers on graphene nanoribbons. We find Fano resonances that cause electromagnetic induced opacity and transparency, and reveal an additional incoherent process leading to interlayer exciton formation with a characteristic charge transfer rate. These results showcase hybrid van der Waals heterostructures as paradigmatic 2D optoelectronic stacks, featuring tunable Fano optics and unconventional charge transfer channels.

cond-mat.mes-hall↗

arXiv2021

Magnetoelastic Coupling in Hole-doped Two-dimensional \b{eta}-PbO

The realization of intertwined ferroelasticity and ferromagnetism in two-dimensional (2D) lattices is of great interest for broad nanoscale applications, but still remains a remarkable challenge. Here, we propose an alternative approach to realize the strongly coupled ferromagnetism and ferroelasticity by carrier doping. We demonstrate that prototypical 2D \b{eta}-PbO is dynamically, thermally and mechanically stable. Under hole doping, 2D \b{eta}-PbO possesses ferromagnetism and ferroelasticity simultaneously. Moreover, the robustness of ferromagnetic and ferroelastic orders are doping tunable. In particular, 2D \b{eta}-PbO features in-plane easy magnetization axis that is coupled with lattice direction, enabling ferroelastic manipulation of spin direction. Our work highlights a new direction for 2D magnetoelastic research and enables the possibility for multifunctional devices.

cond-mat.mtrl-sci↗