arXiv subjects

Neophytos Neophytou

Publications and source records attributed to Neophytos Neophytou.

At least 19 recordsLinked to original sources

arXiv2026

Carrier scattering considerations and thermoelectric power factors of half-Heuslers

The electronic and thermoelectric (TE) transport properties of 13 n-type and p-type half-Heusler alloys are computationally examined using Boltzmann transport. The electronic scattering times resulting from all relevant phonon interactions and ionized impurity scattering (IIS) are fully accounted for using ab initio extracted parameters. We find that at room temperature the average peak TE power factors (PF) of all materials we examine reside between 5 and 10 mW/mK$^2$. We also find that IIS in combination with the long range polar optical phonon (POP) scattering are more influential in determining the electronic transport and PF over all other non-polar phonon interactions (acoustic and optical phonon transport). In fact, the combination of POP and IIS determines the thermoelectric power factor of the half-Heuslers examined on average by about 65\%. The results highlight the crucial impact of Coulombic scattering process (POP and IIS) on the TE properties of half-Heusler alloys and provide profound insight for understanding transport, which can be applied widely in other complex bandstructure materials. In terms of computation expense, the computationally cheaper POP and IIS provide an acceptable first-order estimate of the power factor of these materials, while the non-polar contributions, which require more expensive ab initio calculations, could be of secondary importance.

cond-mat.mtrl-sci↗

arXiv2025

Thermoelectric transport and the role of different scattering processes in the half-Heusler NbFeSb

We perform an ab initio computational investigation of the electronic and thermoelectric transport properties of one of the best performance half-Heusler (HH) alloys, NbFeSb. We use Boltzmann Transport equation while taking into account the full energy/momentum/band dependence of all relevant electronic scattering rates, i.e. with acoustic phonons, non-polar optical phonons (intra- and inter-valley), polar optical phonons (POP), and ionized impurity scattering (IIS). We use a highly efficient and accurate computational approach, where the scattering rates are derived using only a few ab initio extracted matrix elements, while we account fully for intra-/inter valley/band transitions, screening from both electrons and holes, and bipolar transport effects. Our computed thermoelectric power-factor (PF) values show good agreement with experiments across densities and temperatures, while they indicate the upper limit of PF performance for this material. We show that the polar optical phonon and ionized impurity scattering (importantly including screening), influence significantly the transport properties, whereas the computationally expensive non-polar phonon scattering part (acoustic and non-polar optical) is somewhat weaker, especially for electrons, and at lower to intermediate temperatures. This insight is relevant in the study of half-Heusler and other polar thermoelectric materials in general. Although we use NbFeSb as an example, the method we employ is material agnostic and can be broadly applied efficiently for electronic and thermoelectric materials in general, with more than 10x reduction in computational cost compared to fully ab initio methods, while retaining ab-initio accuracy.

cond-mat.mtrl-sci↗

arXiv2025

Off-resonant light-induced topological phase transition and thermoelectric transport in semi-Dirac materials

We show that a semi-Dirac (SD) system with an inversion symmetry breaking mass exhibits a topological phase transition when irradiated with off-resonant light. Using Floquet theory, we derive the band structure, Chern numbers, phase diagram, and we show that as the light intensity is swept at fixed mass, the SD system undergoes normal-Chern-normal insulator transition. Along the phase boundaries we observe single semi-Dirac-cone (SSDC) semimetal states in which one SD cone is gapless and the other gapped. The nontrivial Berry curvature distribution $\Omega(\mathbf{k}) \neq -\Omega ( - \mathbf{k} )$ generates an orbital magnetization $M$ and anomalous Nernst ($\alpha_{xy}$) and thermal Hall ($\kappa_{xy}$) conductivities. We show that $M$ remains constant as the Fermi level $E_F$ scans the insulating gap, but it changes linearly with it in the Chern insulator (CI) phase, as expected. In the normal insulator phase, we find that $\alpha_{xy}$ exhibits a dip-peak profile which is reversed in the CI phase. We also find that switching the light's circular polarization from left to right induces a sign change in $M$, $\alpha_{xy}$, and $\kappa_{xy}$, regardless of the topological phase, thereby allowing us to reverse the direction of flow of the transverse charge and heat currents. Further, we evaluate the components of the charge ($\sigma_{aa}$), thermoelectric ($\alpha_{aa}$), and thermal ($\kappa_{aa}$) conductivity tensors ($a=x, y$) and examine the effect of light on them. With a linear dispersion along the $y$-direction, we find that $\alpha_{yy}$ and $\kappa_{yy}$ are significantly larger than $\alpha_{xx}$ and $\kappa_{xx}$, respectively, due to the much larger squared Dirac velocity $v_y^2$ compared to $v_x^2$.

cond-mat.mes-hall↗

arXiv2025

Conditions for thermoelectric power factor improvements upon band alignment in complex bandstructure materials

Band alignment (or band convergence) is a strategy suggested to provide improvements in the thermoelectric power factor (PF) of materials with complex bandstructures. The addition of more bands at the energy region that contributes to transport, can provide more conducting paths and could improve the electrical conductivity and PF of a material. However, this can lead to increased inter-valley scattering, which will tend to degrade the conductivity. Using the Boltzmann Transport Equation (BTE) and a multi-band model, we theoretically investigate the conditions under which band alignment can improve the PF. We show that PF improvements are realized when intra-band scattering between the aligned bands dominates over inter-band scattering, with larger improvements reached when a light-band is brought into alignment. In the more realistic scenario of intra-and inter-band scattering co-existence, we show that in the light band alignment case, possibilities of PF improvement are present even down to the level where the intra- and inter-band scattering are of similar strength. For heavy band alignment this tolerance is weaker, and weaker inter-band scattering is necessary to realize PF improvements. On the other hand, when inter-band scattering dominates, it is not possible to realize any PF improvements upon band alignment, irrespective of bringing a light or a heavy band into alignment. Overall, to realize PF improvements upon band alignment, the valleys that are brought into alignment need to be as electrically conducting as possible compared to the lower energy base valleys and interact as little as possible with those.

cond-mat.mtrl-sci↗

arXiv2025

Asymmetric Electronic Band Alignment and Potentially Enhanced Thermoelectric Properties in Phase-Separated Mg2X (X=Si,Ge,Sn) Alloys

The Mg2X (X=Si, Ge, Sn) based alloy is an eco-friendly thermoelectric material for mid-temperature applications. The Mg2Si1-xSnx and Mg2Ge1-xSnx alloys can be phase-separated into Si(Ge)- and Sn-rich phases during material synthesis, leading to a nanocomposite with locally varying electronic band structure. First-principles calculations reveal that the valence band offset is eight-times larger than the conduction band offset at the interface between Si- and Sn-rich phases for x=0.6, showing type-I and asymmetric band alignment (0.092 eV versus 0.013 eV). Using Boltzmann transport theory and thermionic emission calculations, we show that the large valence band energy discontinuity could allow for energy filtering effects to take place that can potentially increase the power factor substantially in the p-type material system if designed appropriately.

cond-mat.mtrl-sci↗

arXiv2025

Theory of Quasi-Statically Screened Electron-Polar Optical Phonon Scattering

The scattering of electrons with polar optical phonons (POP) is an important mechanism that limits electronic transport and determines electron mobility in polar materials. This is typically a stronger mechanism compared to non-polar acoustic and optical phonon scattering, and of similar strength to the Coulomb ionized impurity scattering. At high densities, on the other hand, the cloud of charge carriers screens the dipoles that are responsible for POP scattering, and weakens the electron-POP scattering strength. However, in contrast to ionized impurity scattering, for which the well-known Brooks-Herring equation provides the scattering rates with the effect of screening included, for scattering with POP there is no such closed-form mathematical expression. In this work, we derive such an expression based on Fermi's Golden Rule, which would prove particularly useful in understanding electronic transport in complex crystal and complex band structure materials, in which electron-POP scattering could dominate electronic transport.

cond-mat.mtrl-sci↗

arXiv2025

Materials design criteria for ultra-high thermoelectric power factors in metals

Metals have high electronic conductivities, but very low Seebeck coefficients, which traditionally make them unsuitable for thermoelectric materials. Recent studies, however, showed that metals can deliver ultra-high thermoelectric power factors (PFs) under certain conditions. In this work, we theoretically examine the electronic structure and electronic transport specifications which allow for such high PFs. Using Boltzmann transport (BTE) simulations and a multi-band electronic structure model, we show that metals with: i) high degree of transport asymmetry between their bands, ii) strong inter-band scattering, and iii) a large degree of band overlap, can provide ultra-high power factors. We show that each of these characteristics adds to the steepness of the transport distribution function of the BTE, which allows for an increase of the Seebeck coefficient to sizable values, simultaneously with an increase in the electrical conductivity. This work generalizes the concept that transport asymmetry (i.e., mixture of energy regions of high and low contributions to the electrical conductivity), through a combination of different band masses, scattering strengths, or energy filtering scenarios, etc., can indeed result in very high thermoelectric power factors, even in the absence of a material bandgap. Under certain conditions, transport asymmetry can over-compensate any performance degradation to the PF due to bipolar conduction and the naturally low Seebeck coefficients that otherwise exist in this class of materials.

cond-mat.mtrl-sci↗

arXiv2024

Energy Filtering in Doping Modulated Nanoengineered Thermoelectric Materials: A Monte Carlo Simulation Approach

Using Monte Carlo electronic transport simulations, coupled self-consistently with the Poisson equation for electrostatics, we explore the thermoelectric power factor of nanoengineered materials. These materials consist of alternating highly doped and intrinsic regions on the scale of several nanometers. This structure enables the creation of potential wells and barriers, implementing a mechanism for filtering carrier energy. Our study demonstrates that by carefully designing the nanostructure, we can significantly enhance its thermoelectric power factor compared to the original pristine material. Importantly, these enhancements stem not only from the energy filtering effect that boosts the Seebeck coefficient but also from the utilization of high-energy carriers within the wells and intrinsic barrier regions to maintain relatively high electronic conductivity. These findings can offer guidance for the design and optimization of new-generation thermoelectric materials through improvements in the power factor.

cond-mat.mtrl-sci↗

arXiv2024

Super-suppression of long wavelength phonons in constricted nanoporous geometries

In a typical semiconductor material, the majority of heat is carried by long wavelength, long mean-free-path phonons. Nanostructuring strategies to reduce thermal conductivity, a promising direction in the field of thermoelectrics, place scattering centers of size and spatial separation comparable to the mean-free-paths of the dominant phonons to selectively scatter them. The resultant thermal conductivity is in most cases well predicted using Matthiessens rule. In general, however, long wavelength phonons are not as effectively scattered as the rest of the phonon spectrum. In this work, using large-scale Molecular Dynamics simulations, Non-Equilibrium Greens Function simulations, and Monte Carlo simulations, we show that specific nanoporous geometries, which create narrow constrictions in the passage of phonons, lead to anticorrelated heat currents in the phonon spectrum. This results in super-suppression of long-wavelength phonons due to heat trapping, and reductions in the thermal conductivity well below what is predicted by Matthiessens rule.

cond-mat.mes-hall↗

arXiv2023

The role of electronic bandstructure shape in improving the thermoelectric power factor of complex materials

The large variety of complex electronic structure materials and their alloys, offer highly promising directions for improvements in thermoelectric (TE) power factors (PF). Their electronic structure contains rich features, referred to as 'surface complexity', one of them being the highly anisotropic warped energy surface shapes with elongated features and threads in some cases. In this work we use Boltzmann transport simulations to quantify the influence that the shape of the electronic structure energy surfaces has on the PF. Using both analytical ellipsoidal bands, as well as realistic bands from the group of half-Heuslers, we show that band shape complexity alone can offer an advantage to the PF of ~3x in realistic cases. The presence of anisotropic scattering mechanisms such as ionized impurity or polar optical phonon scattering, however, can reduce these improvements by up to ~50%. We show that expressions based on the simple ratio of the density-of-states to the conductivity effective masses, mDOS/mC, together with the number of valleys, can capture the anisotropy shape with a moderate to high degree of correlation. For this, we use a convenient way to extract these masses by mapping the complex bandstructures of materials to parabolic electronic structures, without the need for Boltzmann transport codes. Despite the fact that the PF depends on many parameters, information about the benefits of the band shape alone, would be very useful for identifying and understanding the performance of novel thermoelectric materials.

cond-mat.mtrl-sci↗

arXiv2023

ElecTra Code: Full-Band Electronic Transport Properties of Materials

This paper introduces ElecTra, an open-source code which solves the linearized Boltzmann transport equation in the relaxation time approximation for charge carriers in a full-band electronic structure of arbitrary complexity, including their energy, momentum, and band-index dependence. ElecTra stands for 'ELECtronic TRAnsport' and computes the electronic and thermoelectric transport coefficients electrical conductivity, Seebeck coefficient, electronic thermal conductivity, and mobility, for semiconductor materials, for both unipolar and bipolar (small bandgap) materials. The code uses computed full-bands and relevant scattering parameters as inputs and considers single crystal materials in 3D and 2D. The present version of the code (v1) considers: i) elastic scattering with acoustic phonons and inelastic scattering with non-polar optical phonons in the deformation potential approximation, ii) inelastic scattering with polar phonons, iii) scattering with ionized dopants, and iv) alloy scattering. The user is given the option of intra- and inter-valley scattering considerations. The simulation output also includes relevant relaxation times and mean-free-paths. The transport quantities are computed as a function of Fermi level position, doping density, and temperature. ElecTra can interface with any DFT code which saves the electronic structure in the '.bxsf' format. In this paper ElecTra is validated against ideal electronic transport situations of known analytical solutions, existing codes employing the constant relaxation time approximation, as well as experimentally well-assessed materials such as Si, Ge, SiGe, and GaAs.

cond-mat.mtrl-sci↗

arXiv2023

Electronic transport computation in thermoelectric materials: From ab initio scattering rates to nanostructures

Over the last two decades a plethora of new thermoelectric materials, their alloys, and their nanostructures were synthesized. The ZT figure of merit, which quantifies the thermoelectric efficiency of these materials increased from values of unity to values consistently beyond two across material families. At the same time, the ability to identify and optimize such materials, has stressed the need for advanced numerical tools for computing electronic transport in materials with arbitrary bandstructure complexity, multiple scattering mechanisms, and a large degree of nanostructuring. Many computational methods have been developed, the majority of which utilize the Boltzmann transport equation (BTE) formalism, spanning from fully ab initio to empirical treatment, with varying degree of computational expense and accuracy. In this paper we describe a suitable computational process that we have recently developed specifically for thermoelectric materials. The method consists of three independent software packages that we have developed and: 1) begins from ab initio calculation of the electron-phonon scattering rates, 2) to then be used within a Boltzmann transport simulator, and 3) calculated quantities from BTE are then passed on to a Monte Carlo simulator to examine electronic transport in highly nanostructured material configurations. The method we describe is computationally significantly advantageous compared to current fully ab initio and existing Monte Carlo methods, but with a similar degree of accuracy, thus making it truly enabling in understanding and assessing thermoelectric transport in complex band, nanostructured materials.

cond-mat.mtrl-sci↗

arXiv2023

Computationally efficient Monte Carlo electron transport algorithm for nanostructured thermoelectric material configurations

Monte Carlo statistical ray-tracing methods are commonly employed to simulate carrier transport in nanostructured materials. In the case of a large degree of nanostructuring and under linear response (small driving fields), these simulations tend to be computationally overly expensive due to the difficulty in gathering the required flux statistics. Here, we present a novel MC ray-tracing algorithm with computational efficiency of at least an order of magnitude compared to existing algorithms. Our new method, which is a hybrid of analytical Boltzmann transport equation and Monte Carlo uses a reduced number of ray-tracing particles, avoids current statistical challenges such as the subtraction of two opposite going fluxes, the application of a driving force altogether, and the large simulation time required for low energy carriers. We demonstrate the algorithm's efficiency and power in accurate simulations in large domain nanostructures with multiple defects. We believe that the new method we present is indeed more robust and user friendly compared to common methods, and can enable the efficient study of transport in nanostructured materials under low-field steady-state conditions.

cond-mat.mes-hall↗

arXiv2022

Tunable topological phases in monolayer Pt$_2$HgSe$_3$ with exchange fields

We investigate topological phases of monolayer jacutingaite (Pt$_2$HgSe$_3$) that arise when considering the competing effects of spin-orbit coupling (SOC), magnetic exchange interactions, and staggered sublattice potential V. The interplay between the staggered potential and exchange field offers the possibility of attaining different topological phases. By analyzing the Berry curvatures and computing the Chern numbers and Hall conductivities, we demonstrate that the system is time-reversal-symmetry-broken quantum spin Hall insulator when $m_b<λ_{so}$, where $m_b$ is the exchange field operating on the bottom Hg sublattice and $λ_{so}$ is the intrinsic SOC. For $m_b > λ_{so}$ and in the presence of Rashba SOC, we find that the band gap at valley $K(K^{\prime})$ is topologically trivial (non-trivial) with Chern number $C=1$ and valley Chern number $C_v=-1$, indicating that the system is valley-polarized quantum anomalous Hall insulator. We show that the topology of each valley is swapped (the Chern number becomes $C=-1$) by reversing the sign of the exchange field. The system transitions to a valley-polarized metal and quantum valley Hall phase as V increases. Along the phase boundaries, we observe a single-Dirac cone semimetal states. These findings shed more light on the possibility of realizing and controlling topological phases in spintronics and valleytronics devices.

cond-mat.mes-hall↗

arXiv2022

Electron and Hole Mobility of SnO2 from Full-Band Electron-Phonon and Ionized Impurity Scattering Computations

Mobility is a key parameter for SnO2, which is extensively studied as a practical transparent oxide n-type semiconductor. In experiments, the mobility of electrons in bulk SnO2 single crystals varies from 70 to 260 cm2V-1s-1 at room temperature. Here, we calculate the mobility as limited by electron-phonon and ionized impurity scattering by coupling the Boltzmann transport equation with density functional theory electronic structures. The linearized Boltzmann transport equation is solved numerically beyond the commonly employed constant relaxation-time approximation by taking into account all energy and momentum dependencies of the scattering rates. Acoustic deformation potential and polar optical phonons are considered for electron-phonon scattering, where polar optical phonon scattering is found to be the main factor which determines the mobility of both electrons and holes at room temperature. The calculated phonon-limited electron mobility is found to be 265 cm2V-1s-1, whereas that of holes is found to be 7.6 cm2V-1s-1. We present the mobility as a function of the carrier concentration, which shows the upper mobility limit. The large difference between the mobilities of n-type and p-type SnO2 is a result of the different effective masses between electrons and holes.

cond-mat.mtrl-sci↗

arXiv2022

Super-Suppression of Long Phonon Mean-Free-Paths in Nano-engineered Si due to Heat Current Anticorrelations

The ability to minimize the thermal conductivity of dielectrics with minimal structural intervention that could affect electrical properties is an important capability for engineering thermoelectric efficiency in low-cost materials such as Si. We recently reported the discovery of special arrangements for nanoscale pores in Si that produce a particularly large reduction in thermal conductivity accompanied by strongly anticorrelated heat current fluctuations, a phenomenon that is missed by the diffuse adiabatic boundary conditions conventionally used in numerical Boltzmann transport models. This manuscript presents the results of molecular dynamics simulations and a Monte Carlo ray tracing model that teases apart this phenomenon to reveal that special pore layouts elastically backscatter long-wavelength heat-carrying phonons. This means that heat carriage by a phonon before scattering is undone by the scattered phonon, resulting in an effective mean-free-path that is significantly shorter than the geometric line-of-sight to the pores. This effect is particularly noticeable for the long-wavelength, long mean-free-path phonons whose transport is impeded drastically more than is expected purely from the usual considerations of scattering defined by the distance between defects. This super-suppression of the mean-free-path below the characteristic length scale of the nanostructuring offers a route for minimizing thermal conductivity with minimal structural impact, while the stronger impact on long wavelengths offers possibilities for the design of band-pass phonon filtering. Moreover, the ray tracing model developed in this paper shows that different forms of correlated scattering imprint a unique signature in the heat current autocorrelation function that could be used as a diagnostic in other nanostructured systems.

cond-mat.mtrl-sci↗

arXiv2022

Bipolar conduction asymmetries lead to ultra-high thermoelectric power factor

Low band gap thermoelectric materials suffer from bipolar effects at high temperatures, with increased electronic thermal conductivity and reduced Seebeck coefficient, leading to reduced power factor and low ZT figure of merit. In this work we show that the presence of strong transport asymmetries between the conduction and valence bands can allow high phonon-limited electronic conductivity at finite Seebeck coefficient values, leading to largely enhanced power factors. The power factors that can be achieved can be significantly larger compared to their maximum unipolar counterparts, allowing for doubling of the ZT figure of merit. We identify this behavior in low band gap cases from the half-Heusler materials family. Using both, advanced electronic Boltzmann transport calculations for realistic material bandstructures, as well as model parabolic electronic bands, we elaborate on the parameters that determine this effect. We then develop a series of descriptors which can guide machine learning studies in identifying such classes of materials with extraordinary power factors at nearly pristine conditions. For this we test more than 3000 analytical bandstructures and their features, and more than 120 possible descriptors, to identify the most promising ones that contain: i) only band structure features for easy identification from material databases, and ii) band structure and transport parameters that provide much higher correlations, but for which parameter availability can be somewhat scarce.

cond-mat.mtrl-sci↗

arXiv2021

Deformation potential extraction and computationally efficient mobility calculations in silicon from first principles

We present a first-principles framework to extract deformation potentials in Silicon based on density-functional theory (DFT) and density-functional perturbation theory (DFPT). We compute the electronic band structures, phonon dispersion relations, and electron-phonon matrix elements to extract deformation potentials for acoustic and optical phonons for all possible processes. The matrix elements clearly show the separation between intra- and inter-valley scattering in the conduction band, and quantify the strength of the scattering events in the degenerate bands of the valence band. We then use an advanced numerical Boltzmann transport equation (BTE) simulator that couples DFT electronic structures and energy/momentum-dependent scattering rates to compute the transport properties for electrons and holes. By incorporating ionized impurity scattering as well, we calculate the n-type and p-type mobility versus carrier density and make comparisons to experiments, indicating excellent agreement. The fact that the method we present uses well-established theoretical tools and requires the extraction of only a limited number of matrix elements, makes it generally computationally very attractive, especially for semiconductors with a large unit cell and lower symmetry.

cond-mat.mtrl-sci↗