arXiv subjects

Anderson Janotti

Publications and source records attributed to Anderson Janotti.

At least 37 records · Page 2Linked to original sources

arXiv2024

Magnetic proximity coupling to defects in a two-dimensional semiconductor

The ultrathin structure and efficient spin dynamics of two-dimensional (2D) antiferromagnetic (AFM) materials hold unprecedented opportunities for ultrafast memory devices, artificial intelligence circuits, and novel computing technology. For example, chromium thiophosphate (CrPS4) is one of the most promising 2D A-type AFM materials due to its robust stability in diverse environmental conditions and net out-of-plane magnetic moment in each layer, attributed to anisotropy in crystal axes (a and b). However, their net zero magnetic moment poses a challenge for detecting the Neel state that is used to encode information. In this study, we demonstrate the detection of the Neel vector by detecting the magnetic order of the surface layer by employing defects in tungsten diselenide (WSe2). These defects are ideal candidates for optically active transducers to probe the magnetic order due to their narrow linewidth and high susceptibility to magnetic fields. We observed spin-polarized charge transfer in the heterostructure of bulk CrPS4 and single-layer WSe2 indicating type-II band alignment as supported by density functional theory (DFT) calculations. In the A-type AFM regime, the intensity of both right-handed and left-handed circularly polarized light emanating from the sample remains constant as a function of the applied magnetic field, indicating a constant polarized transition behavior. Our results showcase a new approach to optically characterizing the magnetic states of 2D bulk AFM material, highlighting avenues for future research and technological applications.

cond-mat.mtrl-sci↗

arXiv2024

Role of chalcogen vacancies and hydrogen in the optical and electrical properties of bulk transition-metal dichalcogenides

Like in any other semiconductor, point defects in transition-metal dichalcogenides (TMDs) are expected to strongly impact their electronic and optical properties. However, identifying defects in these layered two-dimensional materials has been quite challenging with controversial conclusions despite the extensive literature in the past decade. Using first-principles calculations, we revisit the role of chalcogen vacancies and hydrogen impurity in bulk TMDs, reporting formation energies and thermodynamic and optical transition levels. We show that the S vacancy can explain recently observed cathodoluminescence spectra of MoS$_2$ flakes and predict similar optical levels in the other TMDs. In the case of the H impurity, we find it more stable sitting on an interstitial site in the Mo plane, acting as a shallow donor, and possibly explaining the often observed n-type conductivity in some TMDs. We also predict the frequencies of the local vibration modes for the H impurity, aiding its identification through Raman or infrared spectroscopy.

cond-mat.mtrl-sci↗

arXiv2023

Fermi-level pinning in ErAs nanoparticles embedded in III-V semiconductors

Embedding rare-earth pnictide (RE-V) nanoparticles into III-V semiconductors enables unique optical, electrical, and thermal properties, with applications in THz photoconductive switches, tunnel junctions, and thermoelectric devices. Despite the high structural quality and control over growth, particle size, and density, the underlying electronic structure of these nanocomposite materials has only been hypothesized. Basic questions about the metallic or semiconducting nature of the nanoparticles (that are typically < 3 nm in diameter) have remained unanswered. Using first-principles calculations, we investigated the structural and electronic properties of ErAs nanoparticles in AlAs, GaAs, InAs, and their alloys. Formation energies of the ErAs nanoparticles with different shapes and sizes (i.e., from cubic to spherical, with 1.14 nm, 1.71 nm, and 2.28 nm diameters) show that spherical nanoparticles are the most energetically favorable. As the diameter increases, the Fermi level is lowered from near the conduction band to the middle of the gap. For the lowest energy nanoparticles, the Fermi level is pinned near the mid-gap, at about 0.8 eV above the valence band in GaAs and about 1.2 eV in AlAs, and it is resonant in the conduction band in InAs. Our results show that the Fermi level is pinned on an absolute energy scale once the band alignment at AlAs/GaAs/InAs interfaces is considered, offering insights into the rational design of these nanocomposite materials.

cond-mat.mtrl-sci↗

arXiv2023

Mott transition and abnormal instability of electronic structure in FeSe

FeSe has been extensively explored as a quantum material, primarily due to the observed highest superconducting transition temperature among Fe-based unconventional superconductors. Nonetheless, the electronic structure and the electron correlations responsible for the remarkable diversity of physical properties in FeSe remain elusive. We undertook a comprehensive investigation of the electronic structure of FeSe, known as a Hund metal, and found that it is not uniquely defined. Through accounting for all two-particle irreducible diagrams constructed from electron Green's function $G$ and screened Coulomb interaction $W$ in a self-consistent manner, a Mott-insulator phase of FeSe is unveiled. The metal-insulator transition is driven by the strong on-site Coulomb interaction in its paramagnetic phase, accompanied by the weakening of both local and non-local screening effects on the Fe-3$d$ orbitals. Our results suggest that Mott physics may play a pivotal role in shaping the electronic, optical, and superconducting properties of monolayer or nanostructured FeSe.

cond-mat.str-el↗

arXiv2023

Large Rashba splittings in bulk and monolayer of BiAs

Two-dimensional materials with Rashba split bands near the Fermi level are key to developing upcoming next-generation spintronics. They enable generating, detecting, and manipulating spin currents without an external magnetic field. Here, we propose BiAs as a novel layered semiconductor with large Rashba splitting in bulk and monolayer forms. Using first-principles calculations, we determined the lowest energy structure of BiAs and its basic electronic properties. Bulk BiAs has a layered crystal structure with two atoms in a rhombohedral primitive cell, similar to the parent Bi and As elemental phases. It is a semiconductor with a narrow and indirect band gap. The spin-orbit coupling leads to Rashba-Dresselhaus spin splitting and characteristic spin texture around the L-point in the Brillouin zone of the hexagonal conventional unit cell, with Rashba energy and Rashba coupling constant for valence (conduction) band of $E_R$= 137 meV (93 meV) and $α_R$= 6.05 eVÅ~(4.6 eVÅ). In monolayer form (i.e., composed of a BiAs bilayer), BiAs has a much larger and direct band gap at $Γ$, with a circular spin texture characteristic of a pure Rashba effect. The Rashba energy $E_R$= 18 meV and Rashba coupling constant $α_R$= 1.67 eVÅ of monolayer BiAs are quite large compared to other known 2D materials, and these values are shown to increase under tensile biaxial strain.

cond-mat.mtrl-sci↗

arXiv2023

The deep-acceptor nature of the chalcogen vacancies in 2D transition-metal dichalcogenides

Chalcogen vacancies in the semiconducting monolayer transition-metal dichalcogenides (TMDs) have frequently been invoked to explain a wide range of phenomena, including both unintentional p-type and n-type conductivity, as well as sub-band gap defect levels measured via tunneling or optical spectroscopy. These conflicting interpretations of the deep versus shallow nature of the chalcogen vacancies are due in part to shortcomings in prior first-principles calculations of defects in the semiconducting two-dimensional (2D) TMDs that have been used to explain experimental observations. Here we report results of hybrid density functional calculations for the chalcogen vacancy in a series of monolayer TMDs, correctly referencing the thermodynamic charge transition levels to the fundamental band gap (as opposed to the optical band gap). We find that the chalcogen vacancies are deep acceptors and cannot lead to n-type or p-type conductivity. Both the (0/$-1$) and ($-$1/$-$2) transition levels occur in the gap, leading to paramagnetic charge states S=1/2 and S=1, respectively, in a collinear-spin representation. We discuss trends in terms of the band alignments between the TMDs, which can serve as a guide to future experimental studies of vacancy behavior.

cond-mat.mtrl-sci↗

arXiv2023

Tuning the Band Topology of GdSb by Epitaxial Strain

Rare-earth monopnictide (RE-V) semimetal crystals subjected to hydrostatic pressure have shown interesting trends in magnetoresistance, magnetic ordering, and superconductivity, with theory predicting pressure-induced band inversion. Yet, thus far, there have been no direct experimental reports of interchanged band order in RE-Vs due to strain. This work studies the evolution of band topology in biaxially strained GdSb (001) epitaxial films using angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT). We find that biaxial strain continuously tunes the electronic structure from topologically trivial to nontrivial, reducing the gap between the hole and the electron bands dispersing along the [001] direction. The conduction and valence band shifts seen in DFT and ARPES measurements are explained by a tight-binding model that accounts for the orbital symmetry of each band. Finally, we discuss the effect of biaxial strain on carrier compensation and magnetic ordering temperature.

cond-mat.mtrl-sci↗

arXiv2023

Dramatic enhancement of visible-light absorption in TiO2 by adding Bi

TiO2 is a wide band-gap semiconductor that has been intensively investigated for photocatalysis and water-spiting. However, weak light absorption in the visible region of the spectrum poses stringent limitation to its practical application. Doping of TiO2 with N or transition-metal impurities has been explored to shift the onset of optical absorption to the visible region, yet with limited success. Based on hybrid density functional calculations, we propose adding Bi to TiO2, in the form of dilute Ti_(1-x)Bi_(x)O2 alloys, to efficiently shift the optical absorption to the visible region. Compared to N, Bi introduces an intermediate valence band that is significantly higher in the band gap, and leaves the conduction band almost unchanged, leading to a remarkable redshift in the absorption coefficient to cover almost all the visible-light spectrum. Comparing formation enthalpies, our results show that adding Bi costs significantly less energy than N in oxidizing conditions, and that Ti_(1-x)Bi_(x)O2 might make a much more efficient photocatalyst than TiO_(2-y)N_(y) for water splitting.

cond-mat.mtrl-sci↗

arXiv2023

Non-trivial topology in rare-earth monopnictides from dimensionality reduction

Thin films of rare-earth monopnictide semimetals are expected to turn into semiconductors due to quantum confinement effect, which lifts the overlap between electron pockets at Brillouin zone edges and hole pockets at the zone center. Instead, taking non-magnetic LaSb as an example, we find the emergence of a quantum spin Hall insulator phase in LaSb(001) films as the thickness is reduced to 7, 5, or 3 monolayers. This is attributed to a strong quantum confinement effect on the in-plane electron pockets, and the lack of quantum confinement on the out-of-plane pocket in reciprocal space projected onto zone center, leading to a band inversion. Spin-orbit coupling opens a sizeable non-trivial gap in the band structure of the thin films. Such effect is shown to be general in rare-earth monopnictides and may lead to interesting phenomena when coupled with the 4f magnetic moments present in other members of this family of materials.

cond-mat.mtrl-sci↗

arXiv2022

Phonon-mediated strong coupling between a three-dimensional topological insulator and a two-dimensional antiferromagnetic material

Van der Waals antiferromagnetic and topological insulator materials provide powerful platforms for modern optical, electronic, and spintronic devices applications. The interaction between an antiferromagnet (AFM) and a topological insulator (TI), if sufficiently strong, could offer emergent hybrid material properties that enable new functionality exceeding what is possible in any individual material constituent. In this work, we study strong coupling between THz excitations in a three dimensional (3D) topological insulator and a quasi-two dimensional (2D) antiferromagnetic material resulting in a new hybridized mode, namely a surface Dirac plasmon-phonon-magnon polariton. We find that the interaction between a surface Dirac plasmon polariton in the 3D TI and a magnon polariton in the 2D AFM is mediated by the phonon coupling in the 3D TI material. The coupling of phonons with an electromagnetic wave propagating in the 3D TI enhances the permittivity of the TI thin film in a way that results in a strong correlation between the dispersion of Dirac plasmon polaritons on the surfaces of the TI with the thickness of the TI. As a result, the dispersion of surface Dirac plasmon polaritons in the TI can be tuned toward resonance with the magnon polariton in the AFM material by varying the TI's thickness, thereby enhancing the strength of the coupling between the excitations in the two materials. The strength of this coupling, which results in the surface Dirac plasmon-phonon-magnon polariton, can be parameterized by the amplitude of the avoided-crossing splitting between the two polariton branches at the magnon resonance frequency...

cond-mat.mes-hall↗

arXiv2022

Epitaxial growth, magnetoresistance, and electronic band structure of GdSb magnetic semimetal films

Motivated by observations of extreme magnetoresistance (XMR) in bulk crystals of rare-earth monopnictide (RE-V) compounds and emerging applications in novel spintronic and plasmonic devices based on thin-film semimetals, we have investigated the electronic band structure and transport behavior of epitaxial GdSb thin films grown on III-V semiconductor surfaces. The Gd3+ ion in GdSb has a high spin S=7/2 and no orbital angular momentum, serving as a model system for studying the effects of antiferromagnetic order and strong exchange coupling on the resulting Fermi surface and magnetotransport properties of RE-Vs. We present a surface and structural characterization study mapping the optimal synthesis window of thin epitaxial GdSb films grown on III-V lattice-matched buffer layers via molecular beam epitaxy. To determine the factors limiting XMR in RE-V thin films and provide a benchmark for band structure predictions of topological phases of RE-Vs, the electronic band structure of GdSb thin films is studied, comparing carrier densities extracted from magnetotransport, angle-resolved photoemission spectroscopy (ARPES), and density functional theory (DFT) calculations. ARPES shows hole-carrier rich topologically-trivial semi-metallic band structure close to complete electron-hole compensation, with quantum confinement effects in the thin films observed through the presence of quantum well states. DFT predicted Fermi wavevectors are in excellent agreement with values obtained from quantum oscillations observed in magnetic field-dependent resistivity measurements. An electron-rich Hall coefficient is measured despite the higher hole carrier density, attributed to the higher electron Hall mobility. The carrier mobilities are limited by surface and interface scattering, resulting in lower magnetoresistance than that measured for bulk crystals.

cond-mat.mtrl-sci↗

arXiv2022

Predicting band gaps and band-edge positions of oxide perovskites using DFT and machine learning

Density functional theory within the local or semilocal density approximations (DFT-LDA/GGA) has become a workhorse in electronic structure theory of solids, being extremely fast and reliable for energetics and structural properties, yet remaining highly inaccurate for predicting band gaps of semiconductors and insulators. Accurate prediction of band gaps using firstprinciples methods is time consuming, requiring hybrid functionals, quasi-particle GW, or quantum Monte Carlo methods. Efficiently correcting DFT-LDA/GGA band gaps and unveiling the main chemical and structural factors involved in this correction is desirable for discovering novel materials in high-throughput calculations. In this direction, we use DFT and machine learning techniques to correct band gaps and band-edge positions of a representative subset of ABO3 perovskite oxides. Relying on results of HSE06 hybrid functional calculations as target values of band gaps, we find a systematic band gap correction of ~1.5 eV for this class of materials, where ~1 eV comes from downward shifting the valence band and ~0.5 eV from uplifting the conduction band. The main chemical and structural factors determining the band gap correction are determined through a feature selection procedure.

cond-mat.mtrl-sci↗

arXiv2022

Bi2Se3 Growth on (001) GaAs Substrates for Terahertz Integrated Systems

Terahertz (THz) technologies have been of interest for many years due to the variety of applications including gas sensing, nonionizing imaging of biological systems, security and defense, etc. To date, scientists have used different classes of materials to perform different THz functions. However, to assemble an on-chip THz integrated system, we must understand how to integrate these different materials. Here, we explore the growth of Bi2Se3, a topological insulator (TI) material that could serve as a plasmonic waveguide in THz integrated devices, on technologically-important GaAs (001) substrates. We explore surface treatments and find that atomically smooth GaAs surface is critical to achieving high-quality Bi2Se3 films despite the relatively weak film/substrate interaction. Calculations indicate that the Bi2Se3/GaAs interface is likely selenium-terminated and shows no evidence of chemical bonding between the Bi2Se3 and the substrate. These results are a guide for integrating van der Waals materials with conventional semiconductor substrates and serve as the first steps toward achieving an on-chip THz integrated system.

cond-mat.mtrl-sci↗

arXiv2022

Hybrid Molecular Beam Epitaxy of Ge-based Oxides

Germanium-based oxides such as rutile GeO2 are garnering attention owing to their wide band gaps and the prospects for ambipolar doping for application in high-power devices. Here, we present the use of germanium tetraisopropoxide (GTIP) (an organometallic chemical precursor) as a source of Ge for the demonstration of hybrid molecular beam epitaxy (MBE) for Ge-containing compounds. We use Sn1-xGexO2 and SrSn1-xGexO3 as model systems to demonstrate this new synthesis method. A combination of high-resolution X-ray diffraction, scanning transmission electron microscopy, and X-ray photoelectron spectroscopy confirms the successful growth of epitaxial rutile Sn1-xGexO2 on TiO2(001) substrates up to x = 0.54 and coherent perovskite SrSn1-xGexO3 on GdScO3(110) substrates up to x = 0.16. Characterization and first-principles calculations corroborate that Ge preferentially occupies the Sn site, as opposed to the Sr site. These findings confirm the viability of the GTIP precursor for the growth of germanium-containing oxides by hybrid MBE, and thus open the door to high-quality perovskite germanate films.

cond-mat.mtrl-sci↗

arXiv2022

Hole conductivity through a defect band in $\rm ZnGa_2O_4$

Semiconductors with wide band gap (3.0 eV), high dielectric constant (> 10), good thermal dissipation, and capable of $n$- and $p$-type doping are highly desirable for high-energy power electronic devices. Recent studies indicate that $\rm ZnGa_2O_4$ may be suitable for these applications, standing out as an alternative to $\rm Ga_2O_3$. The simple face centered cubic spinel structure of $\rm ZnGa_2O_4$ results in isotropic electronic and optical properties, in contrast to the large anisotropic properties of the $β$-monoclinic $\rm Ga_2O_3$. In addition, $\rm ZnGa_2O_4$ has shown, on average, better thermal dissipation and potential for $n$- and $p$-type conductivity. Here we use density functional theory and hybrid functional calculations to investigate the electronic, optical, and point defect properties of $\rm ZnGa_2O_4$, focusing on the possibility for $n$- and p-type conductivity. We find that the cation antisite $\rm Ga_{Zn}$ is the lowest energy donor defect that can lead to unintentional $n$-type conductivity. The stability of self-trapped holes (small hole polarons) and the high formation energy of acceptor defects make it difficult to achieve $p$-type conductivity. However, with excess of Zn, forming $\rm Zn_{(1+2x)}Ga_{2(1-x)}O_4$ alloys display an intermediate valence band, facilitating $p$-type conductivity. Due to the localized nature of this intermediate valence band, $p$-type conductivity by polaron hopping is expected, explaining the low mobility and low hole density observed in recent experiments.

cond-mat.mtrl-sci↗

arXiv2022

Light and microwave driven spin pumping across FeGaB-BiSb interface

3-D topological insulators (TI) with large spin Hall conductivity have emerged as potential candidates for spintronic applications. Here, we report spin to charge conversion in bilayers of amorphous ferromagnet (FM) Fe_{78}Ga_{13}B_{9} (FeGaB) and 3-D TI Bi_{85}Sb_{15} (BiSb) activated by two complementary techniques: spin pumping and ultrafast spin-current injection. DC magnetization measurements establish the soft magnetic character of FeGaB films, which remains unaltered in the heterostructures of FeGaB-BiSb. Broadband ferromagnetic resonance (FMR) studies reveal enhanced damping of precessing magnetization and large value of spin mixing conductance (5.03 x 10^{19} m^{-2}) as the spin angular momentum leaks into the TI layer. Magnetic field controlled bipolar dc voltage generated across the TI layer by inverse spin Hall effect is analyzed to extract the values of spin Hall angle and spin diffusion length of BiSb. The spin pumping parameters derived from the measurements of the femtosecond light-pulse-induced terahertz emission are consistent with the result of FMR. Kubo-Bastin formula and tight-binding model calculations shed light on the thickness-dependent spin-Hall conductivity of the TI films, with predictions that are in remarkable agreement with the experimental data. Our results suggest that room temperature deposited amorphous and polycrystalline heterostructures provide a promising platform for creating novel spin orbit torque devices.

cond-mat.mtrl-sci↗

arXiv2022

Strong coupling between a topological insulator and a III-V heterostructure at terahertz frequency

We probe theoretically the emergence of strong coupling in a system consisting of a topological insulator (TI) and a III-V heterostructure using a numerical approach based on the scattering matrix formalism. Specifically, we investigate the interactions between terahertz excitations in a structure composed of Bi$_{2}$Se$_{3}$ and GaAs materials. We find that the interaction between the Bi$_{2}$Se$_{3}$ layer and AlGaAs/GaAs quantum wells with intersubband transitions (ISBTs) in the terahertz frequency regime creates new hybrid modes, namely Dirac plasmon-phonon-ISBT polaritons. The formation of these hybrid modes results in anti-crossings (spectral mode splitting) whose magnitude is an indication of the strength of the coupling. By varying the structural parameters of the constituent materials, our numerical calculations reveal that the magnitude of splitting depends strongly on the doping level and the scattering rate in the AlGaAs/GaAs quantum wells, as well as on the thickness of the GaAs spacer layer that separates the quantum-well structure from the TI layer. Our results reveal the material and device parameters required to obtain experimentally-observable signatures of strong coupling. Our model includes the contribution of an extra two-dimensional hole gas (2DHG) that is predicted to arise at the Bi$_{2}$Se$_{3}$/GaAs interface, based on density functional theory (DFT) calculations that explicitly account for details of the atomic terminations at the interface. The presence of this massive 2DHG at the TI/III-V interface shifts the dispersion of the Dirac plasmon-ISBT polaritons to higher frequencies. The damping rate at this interface, in contrast, compensates the effect of the 2DHG. Finally, we observe that the phonon resonances in the TI layer are crucial to the coupling between the THz excitations in the TI and III-V materials.

cond-mat.mtrl-sci↗

arXiv2022

Controlling magnetoresistance by tuning semimetallicity through dimensional confinement and heteroepitaxy

Controlling the electronic properties via bandstructure engineering is at the heart of modern semiconductor devices. Here, we extend this concept to semimetals where, utilizing LuSb as a model system, we show that quantum confinement lifts carrier compensation and differentially affects the mobility of the electron and hole-like carriers resulting in a strong modification in its large, non-saturating magnetoresistance behavior. Bonding mismatch at the heteroepitaxial interface of a semimetal (LuSb) and a semiconductor (GaSb) leads to the emergence of a novel, two-dimensional, interfacial hole gas and is accompanied by a charge transfer across the interface that provides another avenue to modify the electronic structure and magnetotransport properties in the ultra-thin limit. Our work lays out a general strategy of utilizing confined thin film geometries and heteroepitaxial interfaces to engineer electronic structure in semimetallic systems, which allows control over their magnetoresistance behavior and simultaneously, provides insights into its origin.

cond-mat.mtrl-sci↗