arXiv subjects

Mona Zebarjadi

Publications and source records attributed to Mona Zebarjadi.

At least 19 recordsLinked to original sources

arXiv2025

Spin-lattice entanglement in $\mathbf{CoPS}_3$

Complex chalcogenides in the $M$PS$_3$ family of materials ($M$ = Mn, Fe, Co, and Ni) display remarkably different phase progressions depending upon the metal center orbital filling, character of the P-P linkage, and size of the van der Waals gap. There is also a stacking pattern and spin state difference between the lighter and heavier transition metal-containing systems that places CoPS$_3$ at the nexus of these activities. Despite these unique properties, this compound is under-explored. Here, we bring together Raman scattering spectroscopy and infrared absorption spectroscopy with X-ray techniques to identify a structural component to the 119 K magnetic ordering transition as well as a remarkable lower temperature set of magnon-phonon pairs that engage in avoided crossings along with a magnetic scattering continuum that correlates with phonon lifetime effects. These findings point to strong spin-phonon entanglement as well as opportunities to control these effects under external stimuli.

cond-mat.str-el↗

arXiv2025

High thermoelectric power factor in Ni-Fe alloy for active cooling applications

Metallic thermoelectric materials are promising candidates for active cooling applications, where high thermal conductivity and a high thermoelectric power factor are essential to maximize effective thermal conductivity. While metals inherently possess high thermal and electrical conductivities, they typically exhibit low Seebeck coefficients. In this work, we create a database and apply machine learning techniques to identify metallic binary alloys with large Seebeck coefficients. Specifically, we identify Ni-Fe as a promising candidate for active cooling. We then fabricate Ni-Fe ingots and demonstrate thermoelectric power factor values as high as 120 μW/{cm.K^2} at 200 K for these stable alloys, which are composed of cost-effective and abundant elements. Furthermore, we show that the effective thermal conductivity of these alloys, under small temperature differences, can exceed that of pure copper at temperatures above 250 K.

cond-mat.mtrl-sci↗

arXiv2022

Conventional Half-Heusler Alloys Advance State-of-the-Art Thermoelectric Properties

Half-Heusler (HH) phases have garnered much attention as thermally stable and non-toxic thermoelectric materials for power conversion. The most studied alloys to date utilize Hf, Zr, and Ti as the base components. These alloys can achieve a moderate dimensionless figure of merit, ZT, near 1. Recent studies have advanced the thermoelectric performance of HH alloys by employing nanostructures and novel compositions to achieve larger ZT, reaching as high as 1.5. Herein, we report that traditional alloying techniques applied to the conventional HfZr-based half-Heusler alloys can also lead to exceptional ZT. Specifically, we present the well-studied p-type Hf0.3Zr0.7CoSn0.3Sb0.7, previously reported to have a ZT~0.8, resonantly doped with less than 1 at. % metallic Al on the Sn/Sb site, touting a remarkable ZT near 1.5 at 980 K. This is achieved through a significant increase in power factor, by ~65%, and a notable but smaller decrease in thermal conductivity, by ~13%, at high temperatures. These favorable thermoelectric properties are discussed in terms of a local anomaly in the density of states near the Fermi energy designed to enhance the Seebeck coefficient, as revealed by first-principles calculations, as well as the emergence of a highly heterogeneous grain structure that can scatter phonons across different length scales, effectively suppressing the thermal conductivity. Consequently, the effective mass is significantly enhanced from ~ 7 to 10me within a single parabolic band model, consistent with the result from first-principles calculations. The discovery of high ZT in a commonly studied half-Heusler alloy through a conventional and non-complex approach opens a new path for further discoveries in similar types of alloys. Furthermore, it is reasonable to believe that the study will reinvigorate effort in exploring high thermoelectric performance in conventional alloy systems.

cond-mat.mtrl-sci↗

arXiv2022

Effect of Electron-Phonon Interaction and Ionized Impurity Scattering on the Room Temperature Thermoelectric Properties of Bulk $MoSe_2$

We study the thermoelectric properties of bulk $MoSe_2$ within relaxation time approximation including electron-phonon and ionized impurity interactions using first-principles calculations at room temperatures. The anisotropy of this two-dimensional layered metal dichalcogenide is studied by calculations of electron mobility in the cross-plane and the in-plane directions. We show that the cross-plane mobility is two orders of magnitude smaller than the in-plane one. The inclusion of van der Waals interactions further lowers the carrier mobility in the cross-plane direction but minimally affects the in-plane one. The results for in-plane electrical mobility and conductivity are in close agreement with experimentally reported values indicating the accuracy of the calculations. The Seebeck coefficient calculations show that this coefficient is primarily dictated by the band structure. The details of relaxation times and inclusion of van der Waals interactions only slightly change the Seebeck coefficient. The in-plane thermoelectric power factor reaches a maximum value of 20 $μWcm^{-1}K^{-2}$ at a carrier concentration of $1.5x10^{20}$ $cm^{-3}$ at 300K.

cond-mat.mtrl-sci↗

arXiv2020

Ultra-high lattice thermal conductivity and the effect of pressure in superhard hexagonal BC2N

Hexagonal BC$_{2}$N is a superhard material recently identified to be comparable to or even harder than cubic boron nitride (c-BN) due the full $sp^3$ bonding character and the higher number of C-C and B-N bonds compared to C-N and B-C.Using a first-principles approach to calculate force constants and an exact numerical solution to the phonon Boltzmann equation, we show that BC$_{2}$N has a high lattice thermal conductivity exceeding that of c-BN owing to the strong C-C and B-N bonds, which produce high phonon frequencies as well as high acoustic velocities. The existence of large group velocities in the optical branches is responsible for its large thermal conductivity. Its coefficient of thermal expansion (CTE) is found to vary from 2.6$\times$10$^{-6}$/K at room temperature to almost 5$\times$ 10$^{-6}$/K at 1000K. The combination of large thermal conductivity and a good CTE match with that of Si, makes BC$_2$N a promising material for use in thermal management and high-power electronics applications. We show that the application of compressive strain increases the thermal conductivity significantly. This enhancement results from the overall increased frequency scale with pressure, which makes acoustic and optic velocities higher, and weaker phonon-phonon scattering rates.

cond-mat.mtrl-sci↗

arXiv2020

The physical and mechanical properties of hafnium orthosilicate: experiments and first-principles calculations

Hafnium orthosilicate (HfSiO4: hafnon) has been proposed as an environmental barrier coating (EBC) material to protect silicon coated, silicon-based ceramic materials at high temperatures and as a candidate dielectric material in microelectronic devices. It can naturally form at the interface between silicon dioxide (SiO2) and hafnia (HfO2). When used in these applications, its coefficient of thermal expansion (CTE) should match that of silicon and SiC composites to reduce the stored elastic strain energy, and thus risk of failure of these systems. The physical, mechanical, thermodynamic and thermal transport properties of hafnon have been investigated using a combination of both density functional theory (DFT) calculations and experimental assessments. The average linear coefficient of thermal expansion (CTE) calculated using the quasi-harmonic approximation increase from 3.06 10-6 K-1 to 6.36 10-6 K-1, as the temperature increases from 300 to 1500 K, in agreement with both X-ray diffraction lattice parameter and dilatometry measurements. The predicted thermal conductivity from Boltzmann transport theory was approximately 18 W/m.K at 300K. Both hot disk and laser flash measurements gave a thermal conductivity of 13.3 W/m.K. This slightly lower value is indicative of residual disorder in the experimental samples that was absent in the theoretical analysis. First-principles calculations and nanoindentation techniques were used to assess the ambient temperature elastic constants and bulk modulus respectively. The elastic properties obtained by both approaches agreed to within 5% validating the computational approach and its future use for study of the thermomechanical properties of other oxides or silicates.

cond-mat.mtrl-sci↗

arXiv2019

Thermoelectric properties of semimetals

Heavily doped semiconductors are by far the most studied class of materials for thermoelectric applications in the past several decades. They have Seebeck coefficient values which are 2-3 orders of magnitude higher than metals, making them attractive for thermoelectric applications. Semimetals generally demonstrate smaller Seebeck coefficient values due to lack of an energy bandgap. However, when there is a large asymmetry in their electron and hole effective masses, semimetals could have large Seebeck coefficient values. In this work, we study the band structure of a class of 18 semimetals using first principles calculations and calculate their Seebeck coefficient using the linearized Boltzmann equation within the constant relaxation time approximation. We conclude, despite the absence of the band gap, that some semimetals are good thermoelectrics with Seebeck coefficient values reaching up to 200 $μ$V/K. We analyze the metrics often used to describe thermoelectric properties of materials, and show that the effective mass ratio is a key parameter resulting in high Seebeck coefficient values in semimetals.

cond-mat.mtrl-sci↗

arXiv2018

Semi-metals as potential thermoelectric materials: case of HgTe

The best thermoelectric materials are believed to be heavily doped semiconductors. The presence of a bandgap is assumed to be essential to achieve large thermoelectric power factor and figure of merit. In this work, we study HgTe as an example semimetal with competitive thermoelectric properties. We employ ab initio calculations with hybrid exchange-correlation functional to accurately describe the electronic band structure in conjunction with the Boltzmann Transport theory to investigate the electronic transport properties. We show that intrinsic HgTe, a semimetal with large disparity in its electron and hole masses, has a high thermoelectric power factor that is comparable to the best known thermoelectric materials. We also calculate the lattice thermal conductivity using first principles calculations and evaluate the overall figure of merit. Finally, we prepare semi-metallic HgTe samples and we characterize their transport properties. We show that our theoretical calculations agree well with the experimental data

cond-mat.mtrl-sci↗

arXiv2017

Experimental determination of phonon thermal conductivity and Lorenz ratio of single crystal bismuth telluride

We use a magnetothermal resistance method to measure the lattice thermal conductivity of a single crystal of Bi$_2$Te$_3$ from 5 to 60 K. We apply a large transverse magnetic field to suppress the electronic thermal conduction while measuring thermal conductivity and electrical resistivity. The lattice thermal conductivity is then calculated by extrapolating the thermal conductivity versus electrical conductivity curve to a zero electrical conductivity value. Our results show that the measured phonon thermal conductivity follows the $e^{(Δ_{min}/T)}$ temperature dependence and the Lorenz ratio corresponds to the modified Sommerfeld value in the intermediate temperature range. Our low-temperature experimental data and analysis on Bi$_2$Te$_3$ are an important compliment to previous measurements of Goldsmid [14] and theoretical calculations by Broido $\textit{et al.}$ [21] at higher temperature 100 - 300 K.

cond-mat.mtrl-sci↗

arXiv2017

Experimental determination of phonon thermal conductivity and Lorenz ratio of single crystal metals: Al, Cu and Zn

We use a magnetothermal resistance method to measure lattice thermal conductivity of pure single crystal metals over a wide range of temperatures. Large transverse magnetic fields are applied to suppress electronic thermal conduction. The total thermal conductivity and the electrical conductivity are measured as functions of applied magnetic field. The lattice thermal conductivity is then extracted by extrapolating the thermal conductivity versus electrical conductivity curve at zero electrical conductivity. We used this method to experimentally measure the lattice thermal conductivity and Lorenz number in single crystal Al (100), Cu (100) and Zn (001) in a temperature range of 5 to 60 K. Our results show that the measured phonon thermal conductivity versus temperature plot has a peak around one tenth of the Debye Temperature, and the Lorenz number is found to deviate from the Sommerfeld value in the intermediate temperature range.

cond-mat.mtrl-sci↗

arXiv2017

Solid State Thermionic Power Generators: an analytical analysis in the nonlinear regime

Solid-state thermionic power generators are an alternative to thermoelectric modules. In this manuscript, we develop an analytical model to investigate the performance of these generators in the non-linear regime. We identify dimensionless parameters determining their performance and provide measures to estimate acceptable range of thermal and electrical resistances of thermionic generators. We find the relation between the optimum load resistance and the internal resistance and suggest guide lines for the design of thermionic power generators. Finally, we show that in the nonlinear regime, thermionic power generators can have efficiency values higher than the state of the art thermoelectric modules.

cond-mat.other↗

arXiv2016

Charge transfer at hybrid inorganic-organic interfaces

Organic dopants are frequently used to surface-dope inorganic semiconductors. The resulted hybrid inorganic-organic materials have a crucial role in advanced functional materials and semiconductor devices. In this article, we study charge transfer at hybrid silicon-molecule interfaces theoretically. The idea is to filter out the best molecular acceptors to dope silicon with hole densities as high as 1013 cm-2. Here, we use a combinatorial algorithm merging chemical hardness method and first-principles DFT and GW calculations. We start by using the chemical hardness method which is simple and fast to narrow down our search for molecular dopants. Then, for the most optimistic candidates, we perform first-principles DFT calculations and discuss the necessity of GW corrections. This screening approach is quite general and applicable to other hybrid interfaces.

cond-mat.mtrl-sci↗

arXiv2016

High Thermoelectric Power Factor in Graphene/hBN Devices

Fast and controllable cooling at nanoscales requires a combination of highly efficient passive cooling and active cooling. While passive cooling in graphene-based devices is quite effective due to graphene's extraordinary heat-conduction, active cooling has not been considered feasible due to graphene's low thermoelectric power factor. Here we show that the thermoelectric performance of graphene can be significantly improved by using hBN substrates instead of SiO2. We find the room temperature efficiency of active cooling, as gauged by the power factor times temperature, reaches values as high as 10.35 W/mK, corresponding to more than doubling the highest reported room temperature bulk power factors, 5 W/mK in YbAl3, and quadrupling the best 2D power factor, 2.5 W/mK, in MoS2. We further show that in these devices the electron-hole puddles region is significantly reduced. This enables fast gate-controlled switching of the Seebeck coefficient polarity for application in n- and p-type integrated active cooling devices.

cond-mat.mes-hall↗

arXiv2016

Design of efficient vdW thermionic heterostructures from first principles

This work is the first step towards understanding thermionic transport properties of graphene/phosphorene/graphene van der Waals heterostructures in contact with gold electrodes by using density functional theory based first principles calculations combined with real space Green's function formalism. We show that for monolayer phosphorene in the heterostructure, quantum tunneling dominates the transport. By adding more phosphorene layers, one can switch from tunneling dominated transport to thermionic dominated transport, resulting in transporting more heat per charge carrier, thus, enhancing the cooling coefficient of performance. The thermionic coefficient of performance for the proposed device is 18.5 at 600 K corresponding to an equivalent ZT of 0.13, which is significant for nanoscale devices.

cond-mat.mtrl-sci↗

arXiv2015

Heat Management in Thermoelectric Power Generators

Thermoelectric power generators are used to convert heat into electricity. Like any other heat engine, the performance of a thermoelectric generator increases as the temperature difference on the sides increases. It is generally assumed that as more heat is forced through the thermoelectric legs, their performance increases. Therefore, insulations are typically used to minimize the heat losses and to confine the heat transport through the thermoelectric legs. In this paper we show that to some extend it is beneficial to purposely open heat loss channels in order to establish a larger temperature gradient and therefore to increase the overall efficiency and achieve larger electric power output. We define a modified Biot number (Bi) as an indicator of requirements for sidewall insulation. We show that if Bi<1, cooling from sidewalls increases the efficiency, while for Bi>1, it lowers the conversion efficiency.

physics.class-ph↗

arXiv2015

Dimensionless Mapping: A Combinatorial Algorithm to Design Invisible Dopants

Electronic cloaking has been recently suggested to design invisible dopants with electronic scattering cross sections smaller than 1% of the physical cross section ( . Cloaking layers could be designed to coat nanoparticle dopants to minimally scatter conduction electrons and to enhance the electronic mobility. In some cases, such enhancements would result in larger thermoelectric power factors. The main difficulty is the fact that the created potential upon coating is not tunable and is determined by the band alignment of the chosen materials for the core, the shell and the host as well as the charge distribution in these layers. To find proper combinations of materials, one needs to probe a large class of materials combinations and layer sizes. This approach is time-consuming and impractical. Here we introduce a mapping method to identify possible combinations by comparing the dimensionless parameters of the chosen materials with the provided maps and without any transport calculations. Using this approach, we have identified several combinations of core, shell and host materials for which electronic cloaking is achievable. We have optimized the size and doping level of some of these materials combinations to maximize their thermoelectric power factor. Compared to traditional impurity-doped samples, up to 14.50 times improvement in the thermoelectric power factor was observed at T=77K.

cond-mat.mtrl-sci↗

arXiv2006

Monte Carlo Simulation of Electron Transport in Degenerate Semiconductors

A modified algorithm is proposed to include Pauli exclusion principle in Monte-Carlo simulations. This algorithm has significant advantages to implement in terms of simplicity, speed and memory storage. We show that even in moderately high applied fields, one can estimate electronic distribution with a shifted Fermi sphere without introducing significant errors. Furthermore, the free-flights must be coupled to state availability constraints; this leads to substantial decrease in carrier heating at high fields. We give the correct definition for electronic temperature and show that in high applied fields, the quasi Fermi level is valley dependent. The effect of including Pauli exclusion principle on the band profile; electronic temperature and quasi Fermi level for inhomogeneous case of a single barrier heterostructure is illustrated.

cond-mat.mtrl-sci↗

arXiv2006

Thermoelectric transport perpendicular to thin film heterostructures using Monte Carlo technique

The Monte Carlo technique is used to calculate electrical as well as thermoelectric transport properties across thin film heterostructures. We study a thin InGaAsP barrier layer sandwiched between two InGaAs contact layers, when the barrier thickness is in 50nm-2000nm range. We found that with decreasing size, the effective Seebeck coefficient is increased substantially. The transition between pure ballistic thermionic transport and fully diffusive thermoelectric transport is also described.

cond-mat.mtrl-sci↗