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Janotti, Anderson

Publications and source records attributed to Janotti, Anderson.

13 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Reducing Dark Conductivity of Cesium Tin Halide Perovskites with Donor Doping

The inorganic tin halide perovskites (such as Cs Sn Br 3 and Cs Sn I 3 ) exhibit high hole concentrations, which have been attributed to the presence of intrinsic defects such as cation vacancies. Despite their promise as photovoltaic materials, this high intrinsic conductivity limits deployment. Using hybrid density functional theory, we examine the impact of these intrinsic defects on the electronic properties of Cs Sn Br 3 and Cs Sn I 3 . We find that tin and cesium vacancies have low formation energies, especially under Sn -poor conditions, in agreement with prior work, and that the presence of these native acceptor defects can lead to high hole concentrations. However, effective donor doping of these systems can be obtained via Sc or Y incorporation. These impurities substitute on the Sn site, where they act as single donors. By examining the formation energy of these dopants versus the native defects, we show that Sc or Y doping should lead to a strong compensation, reducing hole concentrations under Sn -rich conditions. Published by the American Physical Society 2025

Lyons, John L. (ORCID:0000000180233055)↗
DOE OSTI2024

Electronic properties of corundum-like Ir 2 O 3 and Ir 2 O 3 -Ga 2 O 3 alloys

In the hexagonal, corundum-like structure, α-Ga 2 O 3 has a bandgap of ~5.1 eV, which, combined with its relatively small electron effective mass, high Baliga's figure of merit, and high breakdown field, makes it a promising candidate for power electronics. Ga 2 O 3 is easy to dope n-type, but impossible to dope p-type, impeding the realization of some electronic device designs. Developing a lattice-matched p-type material that forms a high-quality heterojunction with n-type Ga 2 O 3 would open new opportunities in electronics and perhaps optoelectronic devices. In this work, we studied Ir 2 O 3 as a candidate for that purpose. Using hybrid density functional theory calculations we predict the electronic band structure of α-Ir 2 O 3 and compare that to α-Ga 2 O 3 , and study the stability and electronic properties of α-(Ir x Ga 1–x ) 2 O 3 alloys. We discuss the band offset between the two materials and compare it with recently available experimental data. We find that the Ir d bands that compose the top of the valence band in α-Ir 2 O 3 are much higher in energy than O p bands in α-Ga 2 O 3 , possibly enabling effective p-type doping. Finally, our results provide an insight into using the Ir 2 O 3 or Ir 2 O 3 -Ga 2 O 3 alloys as p-type material lattice-matched to α-Ga 2 O 3 for the realization of p–n heterojunctions.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Self-compensation of group-V acceptors in CdTe

Cadmium Telluride is at the core of an important thin-film technology for photovoltaics that is already commercially available, yet the CdTe-based solar cell efficiency remains limited at 22%, well below the theoretical limit of ~30%. Increasing the hole concentration is crucial for higher efficiency, and group-V elements such as As, P, and Sb are potential dopants as they are shallow acceptors. Nevertheless, group-V doped p-type CdTe often exhibits low doping activation, and the compensation source remains debated. Here, we performed hybrid density functional calculations with spin-orbit coupling to investigate possible sources of hole compensation in group-V doped CdTe. First, regarding possible self-compensation of the group-V dopants, we find that the formation of AX centers is unlikely since they are found to be unstable relative to the shallow acceptor forms. However, if the group-V dopants come in during growth (such as dimer molecules As2, P2, and Sb2), we find that the impurity atoms, which would occupy nearest neighbor sites, maintain the V-V bonds, limiting the hole density. For the native defects, our study reveals that Cd interstitial is the lowest energy donor defect in p-type CdTe. Still, it has a small migration barrier of 0.5 eV, making it highly mobile and unstable at room temperature. The Te vacancy is the next lowest formation energy donor. The migration barrier of 1.4 eV indicates that the Te vacancy is stable at room temperature. The antisite CdTe is also a donor, with low formation energy and stable at room temperature, potentially limiting the hole concentration. Our results, therefore, shed light on possible compensation centers and some guidance on how to avoid them.

14 SOLAR ENERGY↗
DOE OSTI2024

Large Rashba spin splittings in bulk and monolayer of BiAs

There is great interest in developing new materials with Rashba split bands near the Fermi level for spintronics. Here, using first-principles calculations, we predict BiAs as a semiconductor with large Rashba splitting in bulk and monolayer forms. Bulk BiAs has a layered crystal structure with two atoms in a rhombohedral primitive cell, derived from the structure of the parent Bi and As elemental phases. It is a narrow band gap semiconductor, and it shows a combination of Rashba and Dresselhaus spin splitting with a characteristic spin texture around the L point in the Brillouin zone of the hexagonal conventional unit cell. It has sizable Rashba energies and Rashba coupling constants in the valence and conduction bands at the band edges. The 2D monolayer of BiAs has a much larger band gap at Γ, with a circular spin texture characteristic of a pure Rashba effect. The Rashba energy and Rashba coupling constant of monolayer BiAs are large compared to other known 2D materials and rapidly increase under biaxial tensile strain.

36 MATERIALS SCIENCE↗
DOE OSTI2023

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). As biaxial strain is tuned from tensile to compressive strain, the gap between the hole and the electron bands dispersed along [001] decreases. 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.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Synthesis and Observation of Emergent Phenomena in Epitaxial Heusler Compound Heterostructures

The proposal was on the synthesis and observation of emergent phenomena in epitaxial Heusler compound heterostructures. The large range of properties and number of Heusler compounds opens up a wide number of potential compounds that will exhibit emergent phenomena. The similarity, large range of relatively inexpensive, large area, high crystal quality, III-V bulk substrates, lattice parameters and the ability to tune the lattice parameters through ternary or quaternary III-V compound semiconductor epitaxial growth, makes III-V semiconductors an ideal choice for substrates for epitaxial growth of Heusler compounds. A number of half Heusler compounds have been predicted to exhibit band inversion, making them topological and are therefore expected to exhibit spin-momentum locked topological surface states with linear dispersion. Others are predicted to be semimetals with Weyl points and others semiconducting and magnetic. During the course of this grant, emphasis has been on investigating Heusler compounds with emergent phenomena and demonstrating the ability to tune their properties through alloying and strain. We have grown toplogical semimetal (PtLuSb, PtMnBi), Weyl (Co 2 MnAl, Co 2 TiGe), half metal (PtMnSb, Co 2 MnSi, Co 2 MnAl x Si 1-x , Co2FeAl), and semiconducting (CoTiSb, NiTiSn) and tuned their properties through alloying and epitaxial strain. We also investigated the closely related materials of rare-earth monopnictide, some of which have also been predicted to be topological. During the attempts to grow the PtMnBi, it was discovered that Bi, another predicted topological material when ultrathin, could be grown epitaxially on InSb, results for which are also reported here. The main focus for this effort has been on using variable photon energy and spin-dependent angle resolved photoemission (ARPES) to determine bulk band structure and surface states of pristine epitaxial films grown on III-V semiconductor and MgO substrates and correlate results with theory and transport measurements. Theory has been critical to interpretation of experimental results and has been essential in guiding experiments. The research benefited from several strong collaborations between the PIs and the beamline scientists at the Advanced Light Source at Lawrence Berkeley Laboratory, the Stanford Linear Accelerator Center (SLAC) at Stanford and at the Max Lab at Lund University in Sweden. The strong experiment - theory collaboration between the PI’s groups, the Palmstrøm group at UCSB and the Janotti group at the University of Delaware, has been critical for interpreting the experimental ARPES and magnetotransport measurements results and making predictions to guide experiments. Weekly interactive Zoom meetings made this work well. A collaboration between the Palmstrøm group and Dr. Alexei Fedorov at the Advanced Light Source (ALS) resulted in significant modifications to his end chamber to accommodate the vacuum suitcase that was designed and constructed in the Palmstrøm group at UCSB. In collaboration with beamline scientists, Drs. Makoto Hashimoto and Donghui Lu at SLAC, Palmstrøm made modifications to the vacuum suitcase and developed special sample holders that allowed samples to be grown in the Palmstrøm MBE systems at UCSB and transported in the UHV vacuum suitcase to SLAC for ARPES measurements. The development of the vacuum suitcase was essential for this grant as it has allowed variable photon energies to be used to identify surface versus bulk states on samples that could not be capped and decapped using As- or Sb-capping layers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Engineering metal oxidation using epitaxial strain

The oxides of platinum group metals are promising for future electronics and spintronics due to the delicate interplay of spin-orbit coupling and electron correlation energies. However, their synthesis as thin films remains challenging due to their low vapour pressures and low oxidation potentials. Here we show how epitaxial strain can be used as a control knob to enhance metal oxidation. Using Ir as an example, we demonstrate the use of epitaxial strain in engineering its oxidation chemistry, enabling phase-pure Ir or IrO 2 films despite using identical growth conditions. The observations are explained using a density-functional-theory-based modified formation enthalpy framework, which highlights the important role of metal-substrate epitaxial strain in governing the oxide formation enthalpy. We also validate the generality of this principle by demonstrating epitaxial strain effect on Ru oxidation. The IrO 2 films studied in our work further revealed quantum oscillations, attesting to the excellent film quality. The epitaxial strain approach we present could enable growth of oxide films of hard-to-oxidize elements using strain engineering.

36 MATERIALS SCIENCE↗