arXiv subjects

Shu-Shen Li

Publications and source records attributed to Shu-Shen Li.

At least 37 records · Page 2Linked to original sources

arXiv2021

s-d coupling enhanced phonon anharmonicity in copper-based compounds

Materials with ultralow thermal conductivity are of great interest for efficient energy conversion and thermal barrier coating. Copper-based semiconductors such as copper chalcogenides and copper halides are known to possess extreme low thermal conductivity, whereas the fundamental origin of the low thermal conductivity observed in the copper-based materials remains elusive. Here, we reveal that s-d coupling induced giant phonon anharmonicity is the fundamental mechanism responsible for the ultralow thermal conductivity of copper compounds. The symmetry controlled strong coupling of high-lying occupied copper 3d orbital with the unoccupied 4s state under thermal vibration remarkably lowers the lattice potential barrier, which enhances anharmonic scattering between phonons. This understanding is confirmed by temperature-dependent Raman spectra measurements. Our study offers an insight at atomic level connecting electronic structures with phonon vibration modes, and thus sheds light on materials properties that rely on electron-phonon coupling, such as thermoelectricity and superconductivity.

cond-mat.mtrl-sci↗

arXiv2020

Image charge interaction correction in charged-defect calculation

Charged-defect calculation using a periodic supercell is a significant class of problems in solid state physics. However, the finite supercell size induces an undesirable long-range image charge Coulomb interaction. Although a variety of methods have been proposed to eliminate such image Coulomb interaction, most of the previous schemes are based on a rough approximation of the defect charge screening. In this work, we present a rigorous derivation of the image charge interaction with a new defect screening model where the use of bulk macroscopic dielectric constant can be avoided. We have verified this approach in comparison with a widely used approach for 12 different defects. Our correction scheme offers a much faster convergence concerning the supercell size for cases with considerable image charge interactions. In those cases, we also found that the nonlinear dielectric screening might play an important role. The proposed new defect screening model will also shed new light on understanding the defect screening properties and can be applied to other defect systems.

cond-mat.mtrl-sci↗

arXiv2020

Emergence of the strong tunable linear Rashba spin-orbit coupling of two-dimensional hole gases in semiconductor quantum

Two-dimensional hole gases in semiconductor quantum wells are promising platforms for spintronics and quantum computation but suffer from the lack of the $\bf{k}$-linear term in the Rashba spin-orbit coupling (SOC), which is essential for spin manipulations without magnetism and commonly believed to be a $\bf{k}$-cubic term as the lowest order. Here, contrary to conventional wisdom, we uncover a strong and tunable $\bf{k}$-linear Rashba SOC in two-dimensional hole gases (2DHG) of semiconductor quantum wells by performing atomistic pseudopotential calculations combined with an effective Hamiltonian for a model system of Ge/Si quantum wells. Its maximal strength exceeds 120 meVÅ, comparable to the highest values reported in narrow bandgap III-V semiconductor 2D electron gases, which suffers from short spin lifetime due to the presence of nuclear spin. We also illustrate that this emergent $\bf{k}$-linear Rashba SOC is a first-order direct Rashba effect, originating from a combination of heavy-hole-light-hole mixing and direct dipolar intersubband coupling to the external electric field. These findings confirm Ge-based 2DHG to be an excellent platform towards large-scale quantum computation.

cond-mat.mes-hall↗

arXiv2020

Chebyshev Polynomial Method to Landauer-Büttiker Formula of Quantum Transport in Nanostructures

Landauer-Büttiker formula describes the electronic quantum transports in nanostructures and molecules. It will be numerically demanding for simulations of complex or large size systems due to, for example, matrix inversion calculations. Recently, Chebyshev polynomial method has attracted intense interests in numerical simulations of quantum systems due to the high efficiency in parallelization, because the only matrix operation it involves is just the product of sparse matrices and vectors. Many progresses have been made on the Chebyshev polynomial representations of physical quantities for isolated or bulk quantum structures. Here we present the Chebyshev polynomial method to the typical electronic scattering problem, the Landauer-Büttiker formula for the conductance of quantum transports in nanostructures. We first describe the full algorithm based on the standard bath kernel polynomial method (KPM). Then, we present two simple butefficient improvements. One of them has a time consumption remarkably less than the direct matrix calculation without KPM. Some typical examples are also presented to illustrate the numerical effectiveness.

cond-mat.mes-hall↗

arXiv2020

Numerical Study of Disorder on the Orbital Magnetization in Two Dimensions

The modern theory of orbital magnetization (OM) was developed by using Wannier function method, which has a formalism similar with the Berry phase. In this manuscript, we perform a numerical study on the fate of the OM under disorder, by using this method on the Haldane model in two dimensions, which can be tuned between a normal insulator or a Chern insulator at half filling. The effects of increasing disorder on OM for both cases are simulated. Energy renormalization shifts are observed in the weak disorder regime and topologically trivial case, which was predicted by a self-consistent T-matrix approximation. Besides this, two other phenomena can be seen. One is the localization trend of the band orbital magnetization. The other is the remarkable contribution from topological chiral states arising from nonzero Chern number or large value of integrated Berry curvature. If the fermi energy is fixed at the gap center of the clean system, there is an enhancement of |M| at the intermediate disorder, for both cases of normal and Chern insulators, which can be attributed to the disorder induced topological metal state before localization.

cond-mat.mes-hall↗

arXiv2020

Emergence of an upper bound to the electric field controlled Rashba spin splitting in InAs nanowires

The experimental assessment of the strength ($α_R$) of the Rashba spin-orbit coupling is rather indirect and involves the measurement of the spin relaxation length from magnetotransport, together with a model of weak antilocalization. The analysis of the spin relaxation length in nanowires, however, clouds the experimental assessment of the $α_R$ and leads to the prevailing belief that it can be tuned freely with electric field--a central tenant of spintronics. Here, we report direct theory of $α_R$ leading to atomistic calculations of the spin band structure of InAs nanowires upon application of electric field-- a direct method that does not require a theory of spin relaxation. Surprisingly, we find an {\it upper bound} to the electric field tunable Rashba spin splitting and the ensuing $α_R$; for InAs nanowires, $α_R$ is pinned at about 170 meVÅ irrespective of the applied field strength. We find that this pinning is due to the quantum confined stark effect, that reduces continuously the nanowire band gap with applied electric field, leading eventually to band gap closure and a considerable increase in the density of free carriers. This results in turn in a strong screening that prevents the applied electric field inside the nanowire from increasing further beyond around 200 kV/cm for InAs nanowires. Therefore, further increase in the gate voltage will not increase $α_R$. This finding clarifies the physical trends to be expected in nanowire Rashba SOC and the roles played by the nano size and electric field.

cond-mat.mes-hall↗

arXiv2019

Anharmonic corrections to the multiphonon deep-level charge capture ab initio calculations for semiconductors

Nonradiative carrier recombination at semiconductor deep centers is of great importance to both fundamental physics and device engineering. In this letter, we provide a revised analysis of K. Huang's original nonradiative multi-phonon (NMP) theory with ab initio calculations. First, we identify at first-principle level that Huang's concise formula gives the same results as the matrix based formula, and Huang's high temperature formula provides an analytical expression for the coupling constant in Marcus theory. Secondly, the anharmonic effects are corrected by taking into account local phonon mode variation at different charge states of the defect. The corrected capture rates for defects in GaN and SiC agree well with experiments.

cond-mat.mtrl-sci↗

arXiv2019

A realistic dimension-independent approach for charged defect calculations in semiconductors

First-principles calculations of charged defects have become a cornerstone of research in semiconductors and insulators by providing insights into their fundamental physical properties. But current standard approach using the so-called jellium model has encountered both conceptual ambiguity and computational difficulty, especially for low-dimensional semiconducting materials. In this Communication, we propose a physical, straightforward, and dimension-independent universal model to calculate the formation energies of charged defects in both three-dimensional (3D) bulk and low-dimensional semiconductors. Within this model, the ionized electrons or holes are placed on the realistic host band-edge states instead of the virtual jellium state, therefore, rendering it not only naturally keeps the supercell charge neutral, but also has clear physical meaning. This realistic model reproduces the same accuracy as the traditional jellium model for most of the 3D semiconducting materials, and remarkably, for the low-dimensional structures, it is able to cure the divergence caused by the artificial long-range electrostatic energy introduced in the jellium model, and hence gives meaningful formation energies of defects in charged state and transition energy levels of the corresponding defects. Our realistic method, therefore, will have significant impact for the study of defect physics in all low-dimensional systems including quantum dots, nanowires, surfaces, interfaces, and 2D materials.

cond-mat.mtrl-sci↗

arXiv2019

A large-scale first-principles quantum transport simulation method using plane waves

As the characteristic lengths of advanced electronic devices are approaching the atomic scale, ab initio simulation method, with fully consideration of quantum mechanical effects, becomes essential to study the quantum transport phenomenon in them. However, current widely used non-equilibrium Green's function (NEGF) approach is based on atomic basis set, which usually can only study small system with less than 1000 atoms in practice. Here we present a large-scale quantum transport simulation method using plane waves basis, based on the previously developed plane wave approach (Phys. Rev. B 72, 045417). By applying several high-efficiency parallel algorithms, such as linear-scale ground-state density function theory (DFT) algorithm, folded spectrum method, and filtering technique, we demonstrate that our new method can simulate the system with several thousands of atoms. We also use this method to study several nanowires with about 4000 copper atoms, and show how the shape and point defect affect the transport properties of them. Such quantum simulation method will be useful to investigate and design nanoscale devices, especially the on-die interconnects.

cond-mat.mes-hall↗

arXiv2019

Localization Trajectory and Chern-Simons axion coupling for Bilayer Quantum Anomalous Hall Systems

Quantum anomalous Hall (QAH) multilayers provide a platform of topological materials with high Chern numbers. We investigate the localization routes of bilayer QAH systems with Chern number C = 2 under strong disorder, by numerical simulations on their quantum transport properties and the Chern-Simons axion coupling. Compared to the single layer counterpart with C = 2, the localization trajectories present much richer behaviors, for example, the existence of the stable intermediate state with C = 1 can be tuned by model parameters. This state was always unstable in the single layer case. Furthermore, the two parameter scaling trajectories also exhibit multiple patterns, some of which were not captured by the standard Pruisken picture. During the process towards localization, the Chern-Simons axion coupling shows a surprisingly remarkable peak which is even higher and sharper in the large size limit. Therefore the disordered bilayer QAH system can be a good candidate for this nontrivial magnetoelectric coupling mediated by orbital motions.

cond-mat.mes-hall↗

arXiv2018

Uncovering and tailoring hidden Rashba spin-orbit splitting in centrosymmetric crystals

Hidden Rashba and Dresselhaus spin-splittings in centrosymmetric crystals with subunits (sectors) having non-centrosymmetric symmetries (the R-2 and D-2 effects) have been predicted and observed experimentally, but the microscopic mechanism remains unclear. Here we demonstrate that the spin-splitting in R-2 is enforced by specific symmetries (such as the non-symmorphic in the present example) which ensures that the pertinent spin wavefunctions segregate spatially on just one of the two inversion-partner sectors and thus avoid compensation. This finding establishes a common fundamental source for the conventional Rashba (R-1) effect and the R-2 effect, both originating from the local sector symmetries, rather than from the global crystal asymmetry alone for R-1 per se. We further show that the effective Hamiltonian for the R-1 effect is also applicable for the R-2 effect, but applying a symmetry-breaking electric field to an R-2 compound produces different spin-splitting pattern than applying a field to a trivial (non-R-2) centrosymmetric compound.

cond-mat.mtrl-sci↗

arXiv2018

Unified theory of the direct or indirect bandgap nature of conventional semiconductors

Although the direct or indirect nature of the bandgap transition is an essential parameter of semiconductors for optoelectronic applications, the understanding why some of the conventional semiconductors have direct or indirect bandgaps remains ambiguous. In this Letter, we revealed that the existence of the occupied cation d bands is a prime element in determining the directness of the bandgap of semiconductors through the s-d and p-d couplings, which push the conduction band energy levels at the X- and L-valley up, but leaves the Γ-valley conduction state unchanged. This unified theory unambiguously explains why Diamond, Si, Ge, and Al-containing group III-V semiconductors, which do not have active occupied d bands, have indirect bandgaps and remaining common semiconductors, except GaP, have direct bandgaps. Besides s-d and p-d couplings, bond length and electronegativity of anions are two remaining factors regulating the energy ordering of the Γ-, X-, and L-valley of the conduction band, and are responsible for the anomalous bandgap behaviors in GaN, GaP, and GaAs that have direct, indirect, and direct bandgaps, respectively, despite the fact that N, P, and As are in ascending order of the atomic number. This understanding will shed light on the design of new direct bandgap light-emitting materials.

cond-mat.mtrl-sci↗

arXiv2018

Photocorrosion-limited maximum efficiency of solar photoelectrochemical water splitting

Photoelectrochemical (PEC) water splitting to generate hydrogen is one of the most studied methods for converting solar energy into clean fuel because of its simplicity and potentially low cost. Despite over 40 years of intensive research, PEC water splitting remains in its early stages with stable efficiencies far less than 10%, a benchmark for commercial applications. Here, we revealed that the desired photocorrosion stability sets a limit of 2.48 eV (relative to the normal hydrogen electrode (NHE)) for the highest possible potential of the valence band (VB) edge of a photocorrosion-resistant semiconducting photocatalyst. We further demonstrated that such limitation has a deep root in underlying physics after deducing the relation between energy position of the valence band edge and free-energy for a semiconductor. The disparity between the stability-limited VB potential at 2.48 V and the oxygen evolution reaction (OER) potential at 1.23 V vs NHE reduces the maximum STH conversion efficiency to approximately 8% for long-term stable single-bandgap PEC water splitting cells. Based on this understanding, we suggest that the most promising strategy to overcome this 8% efficiency limit is to decouple the requirements of efficient light harvesting and chemical stability by protecting the active semiconductor photocatalyst surface with a photocorrosion-resistant oxide coating layer.

cond-mat.mtrl-sci↗

arXiv2018

Barrier tunneling of the Loop-Nodal Semimetal in the Hyperhoneycomb lattice

We theoretically investigate the barrier tunneling in the three-dimensional model of the hyperhoneycomb lattice, which is a nodal-line semimetal with a Dirac loop at zero energy. In the presence of a rectangular potential, the scattering amplitudes for different injecting states around the nodal loop are calculated, by using analytical treatments of the effective model, as well as numerical simulations of the tight binding model. In the low energy regime, states with remarkable transmissions are only concentrated in a small range around the loop plane. When the momentum of the injecting electron is coplanar with the nodal loop, nearly perfect transmissions can occur for a large range of injecting azimuthal angles if the potential is not high. For higher potential energies, the transmission shows a resonant oscillation with the potential, but still with peaks being perfect transmissions that do not decay with the potential width. These robust transports of the loop-nodal semimetal can be approximately explained by a momentum dependent Dirac Hamiltonian.

cond-mat.mes-hall↗

arXiv2017

Atomic-ordering-induced quantum phase transition between topological crystalline insulator and Z2 topological insulator

Topological phase transition in a single material usually refers to transitions between a trivial band insulator and a topological Dirac phase, but the transition may also occur between different classes of topological Dirac phases. However, it is a fundamental challenge to realize quantum transition between Z2 nontrivial topological insulator (TI) and topological crystalline insulator (TCI) in one material because Z2 TI and TCI are hardly both co-exist in a single material due to their contradictory requirement on the number of band inversions. The Z2 TIs must have an odd number of band inversions over all the time-reversal invariant momenta, whereas, the newly discovered TCIs, as a distinct class of the topological Dirac materials protected by the underlying crystalline symmetry, owns an even number of band inversions. Here, take PbSnTe2 alloy as an example, we show that at proper alloy composition the atomic-ordering is an effective way to tune the symmetry of the alloy so that we can electrically switch between TCI phase and Z2 TI phase when the alloy is ordered from a random phase into a stable CuPt phase. Our results suggest that atomic-ordering provides a new platform to switch between different topological phases.

cond-mat.mtrl-sci↗

arXiv2016

Resonant impurities states-driven topological transition in quantum well

We demonstrate theoretically that a new system quantum well can realize the topological transition based on the 16-band kp model. Utilizing the strain introduced by the doped impurities, the band anti crossing induced by the doped nitrogen and valence band anti crossing induced by the doped bismuth, the band gap of the quantum well is rapidly decreased and even becomes negative. As a result, the topological transitions arise. Furthermore, the band gap as a function of the concentration of nitrogen and bismuth is calculated, where the negative gap corresponds to the topological phase. Noting the cancel of strain resulting from the combination of tensile strain introduced by N and strain introduced by Bi, we can easily tune the ratio of the N and Bi to meet the requirement of strain in the crystal growth procedure. Our proposal provides a promising approach for topological insulator in traditional semiconductor system utilizing the semiconductor fabrication technologies.

cond-mat.mes-hall↗

arXiv2016

Atomic-scale positioning of single spins via multiple nitrogen-vacancy centers

We present a scheme of positioning a single electron spin with sub-nanometer resolution through multiple nitrogen-vacancy centers in diamond. With unwanted noise suppressed by dynamical decoupling, the spin coherence of each center develops characteristic oscillations due to a single electron spin located $4{\sim20}$ nm away from the centers. We can extract the position information from the characteristic electron spin-coherence oscillations of each center. This scheme is useful for high-resolution nanoscale magnetometry and spin-based quantum computing.

quant-ph↗

arXiv2015

Route towards Localization for Quantum Anomalous Hall Systems with Chern Number 2

The quantum anomalous Hall system with Chern number 2 can be destroyed by sufficiently strong disorder. During its process towards localization, it was found that the electronic states will be directly localized to an Anderson insulator (with Chern number 0), without an intermediate Hall plateau with Chern number 1. Here we investigate the topological origin of this phenomenon, by calculating the band structures and Chern numbers for disordered supercells. We find that on the route towards localization, there exists a hidden state with Chern number 1, but it is too short and too fluctuating to be practically observable. This intermediate state cannot be stabilized even after some "smart design" of the model and this should be a universal phenomena for insulators with high Chern numbers. By performing numerical scaling of conductances, we also plot the renormalization group flows for this transition, with Chern number 1 state as an unstable fixed point. This is distinct from known results, and can be tested by experiments and further theoretical analysis.

cond-mat.mes-hall↗