In this paper, we explore the effect of H and its bonding configurations on the defect state density and orbital localization of hydrogenated amorphous Si (a-Si:H)/crystalline Si (c-Si) heterostructures using density functional theory (DFT) studies of model interfaces between amorphous silicon (a- Si)/a-Si:H and c-Si. To model the atomic configuration of a-Si on c-Si, melting and quenching simulations were performed using classical molecular dynamics (MD). Different hydrogen contents were inserted into the a-Si in different bonding configurations followed by DFT relaxation to create the stable structures of a-Si:H representative of hydrogenated a-Si on crystalline Si surfaces. In contrast to crystalline heterojunctions (where the interface density is a maximum at the interface), we find that, in the most energetically stable configurations of H atoms, the defect state density is relatively low at the interface and maximum at the middle of a-Si layer. Our structural analysis shows that in these configurations, H atoms do not necessarily bond to dangling bonds or to interface atoms. However, they are able to significantly change the atomic structure of the heterostructure and consequently decrease the density of defect states and orbital localization at the a-Si layer and more significantly at the interface of a-Si/c-Si. The general form of the modeled defect state distribution demonstrates the passivating role of a-Si:H on c-Si substrates.
The changes of defect characteristics induced by accelerated lifetime tests on the heterostructure n-ZnO/i-ZnO/CdS/Cu(In, Ga)(S, Se)$_2$/Mo relevant for photovoltaic energy conversion are investigated. We subject heterojunction and Schottky devices to extended damp heat exposure at 85$^{\circ}$C ambient temperature and 85% relative humidity for various time periods. In order to understand the origin of the pronounced changes of the devices, we apply current--voltage and capacitance--voltage measurements, admittance spectroscopy, and deep-level transient spectroscopy. The fill factor and open-c…
Electronic devices are extremely sensitive to defects in their constituent semiconductors, but locating electronic point defects in bulk semiconductors has previously been impossible. Here we apply scanning transmission electron microscopy (STEM) electron beam-induced current (EBIC) imaging to map electronic defects in a GaAs nanowire Schottky diode. Imaging with a non-damaging 80 or 200 kV STEM acceleration potential reveals a minority-carrier diffusion length that decreases near the surface of the hexagonal nanowire, thereby demonstrating that the device's charge collection efficiency (CCE) …
Heterojunction Si solar cells exhibit notable performance degradation. We developed the SolDeg platform to model this degradation as electronic defects getting generated by thermal activation across energy barriers over time. First, molecular dynamics simulations were performed to create a-Si/c-Si stacks, using a machine-learning-based Gaussian approximation potential. Second, we created shocked clusters by a cluster blaster. Third, the shocked clusters were analyzed to identify which of them supported electronic defects. Fourth, the distribution of energy barriers that control the generation …
We have employed admittance spectroscopy and deep-level transient spectroscopy in order to investigate the electronic properties of ZnO/CdS/Cu(In,Ga)(S,Se)$_2$ heterojunctions and Cr/Cu(In,Ga)(S,Se)$_2$ Schottky contacts. Our work concentrates on the origin of an energy-distributed defect state commonly found in these systems. The activation energy of the defect state addressed continuously shifts upon air annealing or damp-heat treatment and is a valuable measure of the degree of band bending in Cu(In,Ga)(S,Se)$_2$-based junctions. We demonstrate that the band bending within the Cu(In,Ga)(S,S…
Using first-principles density-functional calculations, we address the magnetic properties of the ferromagnet/antiferromagnet La(0.67)Sr(0.33)MnO3/BiFeO3(001) heterojunctions, and investigate possible driving mechanisms for a ferromagnetic (FM) interfacial ordering of the Fe spins recently observed experimentally. We find that the chemically abrupt defect-free La(0.67)Sr(0.33)MnO3/BiFeO3(001) heterojunction displays, as ground state, an ordering with compensated Fe spins. Cation Fe/Mn intermixing at the interface tends to favour, instead, a FM interfacial order of the Fe spins, coupled antifer…
Using DFT calculations, we investigate the effects of the type, location, and density of point defects in monolayer MoS2 on electronic structures and Schottky barrier heights (SBH) of Au/MoS2 heterojunction. Three types of point defects in monolayer MoS2, that is, S monovacancy, S divacancy and MoS (Mo substitution at S site) antisite defects, are considered. The following findings are revealed: (1) The SBH for the monolayer MoS2 with defects is universally higher than that for its defect-free counterpart. (2) S divacancy and MoS antisite defects increase the SBH to a larger extent than S mono…
Localization due to disorder has been one of the most intriguing theoretical concepts evolved in condensed matter. Here, we expand the theory of localization by considering two types of disorder at the same time, namely the original Anderson's disorder and the structural defect disorder, which has been suggested to be a key component in recently discovered two-dimensional amorphous materials. While increasing the degree of both disorders could induce localization of wavefunction in real space, we find that a small degree of structural defect disorder can significantly enhance the localization.…
The electronic and structural properties of Janus MoSSe/MoX$_2$ (X=S,Se) in-plane heterojunctions, endowed with single-atom vacancies, were studied using density functional theory calculations. The stability of these structures was verified from cohesion energy calculations. Results showed that single-atom vacancies induce the appearance of flat midgap states, and a substantial amount of charge is localized in the vicinity of these defects. As a consequence, these heterojunctions presented an intrinsic dipole moment. No bond reconstructions were noted by removing an atom from the lattice, rega…
Mixed-dimensional van der Waals heterojunctions comprising polymer and twodimensional (2D) semiconductors have many characteristics of an ideal charge separation interface for optoelectronic and photonic applications. However, the photoelectron dynamics at polymer- 2D semiconductor heterojunction interfaces are currently not sufficiently understood to guide the optimization of devices for these applications. This manuscript is a report of a systematic exploration of the time-dependent photophysical processes that occur upon photoexcitation of a type-II heterojunction between the polymer PTB7 a…
The coexistence of semiconducting (2H) and metallic (1T) phases of MoS$_{2}$ monolayers have further pushed their strong potential for applications in the next generation of electronic devices based on the two-dimensional lateral heterojunctions. Structural defects have considerable effects on the properties of these 2D devices. In particular, the interfaces of two phases are often imperfect and may contain numerous vacancies created by phase engineering techniques, e.g. under the electron beam. Here, the transport behaviors of the heterojunctions in the existence of point defects are explored…
We have successfully demonstrated Si/GaAs p-n heterostructures using Al2O3 ultra-thin oxide interfacial layers. The band diagram and band offsets were investigated using X-ray photoelectron spectroscopy and confirm a small discontinuity in the conduction band (0.03 eV) at the interface. The interface defect density (Dit) values of the heterointerface with different ultra-thin oxide (UO) thicknesses ranged from 0.35 nm to 3.5 nm and were also characterized based on a metal-oxide-semiconductor capacitor (MOSCAP) structure using a capacitance-voltage measurement. The results revealed that a thin …
Gapless boundary modes at the interface between topologically distinct regions are one of the most salient manifestations of topology in physics. Metallic boundary states of time-reversal-invariant topological insulators (TIs), a realization of topological order in condensed matter, have been of much interest not only due to such a fundamental nature, but also due to their practical significance. These boundary states are immune to backscattering and localization owing to their topological origin, thereby opening up the possibility to tailor them for potential uses in spintronics and quantum c…
Modifications of spin-splitting dispersion relations and density of states for electrons in non-symmetric heterostructures under in-plane magnetic field are studied within the envelope function formalism. Spin-orbit interactions, caused by both a slow potential and the heterojunction potentials (which are described by the boundary conditions) are taken into account. The interplay between these contributions and the magnetic field contribution to the spin-splitting term in the Hamiltonian is essential when energy amount resulting from the Zeeman and spin-orbit coupling are of the same order. Su…
We investigate the electronic structure of gap and band tail states in amorphous silicon. Starting with two 216-atom models of amorphous silicon with defect concentration close to the experiments, we systematically study the dependence of electron localization on basis set, density functional and spin polarization using the first principles density functional code Siesta. We briefly compare three different schemes for characterizing localization: information entropy, inverse participation ratio and spatial variance. Our results show that to accurately describe defect structures within self con…
Carrier Localization in Pnictogen-Based Chalcohalides from Defect-Bound Hot Polarons
University of Oxford（牛津大学）；South China University of Technology（华南理工大学）；Universitat Politècnica de Catalunya（加泰罗尼亚理工大学）；Institució Catalana de Recerca i Estudis Avançats (ICREA)（加泰罗尼亚研究与高级研究学院）；Helmholtz-Zentrum Dresden – Rossendorf（德累斯顿-罗斯多夫亥姆霍兹中心）；Delft University of Technology（代尔夫特理工大学）；National Taiwan University（台湾大学）；University of Cambridge（剑桥大学）；Harvard University Center for the Environment（哈佛大学环境中心）
Novel 2D material CrI3 reveals unique combination of 2D ferromagnetism and robust excitonic response. We demonstrate that the possibility of the formation of magnetic topological defects, such as Neel skyrmions, together with large excitonic Zeeman splitting, leads to giant scattering asymmetry, which is the necessary prerequisite for the excitonic anomalous Hall effect. In addition, the diamagnetic effect breaks the inversion symmetry, and in certain cases can result in exciton localization on the skyrmion. This enables the formation of magnetoexcitonic quantum dots with tunable parameters.
The electronic and structural properties of pure and defective cerium oxide are investigated using a unified LDA+U approach which allows to treat the different valence states of Ce occurring for different stoichiometries on a same ground, without any {\it a priori} assumptions on the defect chemistry. The method correctly predicts the atomistic and electronic structures of the \4ce and \3ce bulk phases, as well as the subtle defect chemistry in reduced materials \xce, which controls the oxygen storage functionality of cerium-based oxides. The analysis of the energetics highlights the limits of…
We study the light transmission in two-dimensional photonic crystal waveguides with embedded nonlinear defects. First, we derive the effective discrete equations with long-range interaction for describing the waveguide modes, and demonstrate that they provide a highly accurate generalization of the familiar tight-binding models which are employed, e.g., for the study of the coupled-resonator optical waveguides. Using these equations, we investigate the properties of straight waveguides and waveguide bends with embedded nonlinear defects and demonstrate the possibility of the nonlinearity-induc…
We investigate the dynamical response of a mass defect in a one-dimensional non-loaded horizontal chain of identical spheres which interact via the nonlinear Hertz potential. Our experiments show that the interaction of a solitary wave with a light intruder excites localized mode. In agreement with dimensional analysis, we find that the frequency of localized oscillations exceeds the incident wave frequency spectrum and nonlinearly depends on the size of the intruder and on the incident wave strength. The absence of tensile stress between grains allows some gaps to open, which in turn induce a…
The 3D local atomic structures and crystal defects at the interfaces of heterostructures control their electronic, magnetic, optical, catalytic and topological quantum properties, but have thus far eluded any direct experimental determination. Here we determine the 3D local atomic positions at the interface of a MoS2-WSe2 heterojunction with picometer precision and correlate 3D atomic defects with localized vibrational properties at the epitaxial interface. We observe point defects, bond distortion, atomic-scale ripples and measure the full 3D strain tensor at the heterointerface. By using the…
We have performed accurate \emph{ab--initio} pseudopotential calculations for the structural and electronic properties of ZnSe/GaAs(001) heterostructures with interface configurations accounting for charge neutrality prescriptions. Beside the simplest configurations with atomic interdiffusion we consider also some configurations characterized by As depletion and cation vacancies, motivated by the recent successfull growth of ZnSe/GaAs pseudomorphic structures with minimum stacking fault density characterized by the presence of a defected (Zn,Ga)Se alloy in the interface region. We find that--u…
The role of irradiation induced defects and temperature in the conducting properties of single-walled (10,10) carbon nanotubes has been analyzed by means of a first-principles approach. We find that di-vacancies modify strongly the energy dependence of the differential conductance, reducing also the number of contributing channels from two (ideal) to one. A small number of di-vacancies (5-9) brings up strong Anderson localization effects and a seemly universal curve for the resistance as a function of the number of defects. It is also shown that low temperatures, around 15-65 K, are enough to …
Hetero-epitaxial crystalline films underlie many electronic and optical technologies but are prone to forming defects at their hetero-interfaces. Atomic-scale defects such as threading dislocations that propagate into a film impede the flow of charge carriers and light degrading electrical-optical performance of devices. Diagnosis of subsurface defects traditionally requires time consuming invasive techniques such as cross sectional transmission electron microscopy. Using III-V films grown on Si, we have demonstrated noninvasive, bench-top diagnosis of sub-surface defects by optical second-har…
We demonstrate locally coherent heteroepitaxial growth of silicon carbide (SiC) on diamond, a result contrary to current understanding of heterojunctions as the lattice mismatch exceeds $20\%$. High-resolution transmission electron microscopy (HRTEM) confirms the quality and atomic structure near the interface. Guided by molecular dynamics simulations, a theoretical model is proposed for the interface wherein the large lattice strain is alleviated via point dislocations in a two-dimensional plane without forming extended defects in three dimensions. The possibility of realising heterojunctions…
(In,Ga)N insertions embedded in self-assembled GaN nanowires are of current interest for applications in solid state light emitters. Such structures exhibit a notoriously broad emission band. We use cathodoluminescence spectral imaging in a scanning electron microscope and micro-photoluminescence spectroscopy on single nanowires to learn more about the mechanisms underlying this emission. We observe a shift of the emission energy along the stack of six insertions within single nanowires that may be explained by compositional pulling. Our results also corroborate reports that the localization o…
A novel bilayer is introduced, consisting of a stiff film adhered to a soft substrate with patterned holes beneath the film and substrate interface. To uncover the transition of surface patterns, two dimensional plane strain simulations are performed on the defected bilayer subjected to uniaxial compression. Although the substrate is considered as the linear elastic material, the presence of defects can directly trigger the formation of locally ridged and then folding configurations from flat surface with a relatively small compressive strain. It is followed by the coexisting phases of folds a…
Niobium-based Superconducting Radio Frequency (SRF) cavity performance is sensitive to localized defects that give rise to quenches at high accelerating gradients. In order to identify these material defects on bulk Nb surfaces at their operating frequency and temperature, it is important to develop a new kind of wide bandwidth microwave microscopy with localized and strong RF magnetic fields. By taking advantage of write head technology widely used in the magnetic recording industry, one can obtain ~200 mT RF magnetic fields, which is on the order of the thermodynamic critical field of Nb, on…
Damage accumulation induced metal-insulator transition through ion implantation of ScN thin films
PPRIME Institute, CNRS, Université de Poitiers–ENSMA（普雷米研究所，法国国家科学研究中心，普瓦捷大学-国立高等机械工程学院）；Inorganic Chemistry, Department of Chemistry - Ångström, Uppsala University（乌普萨拉大学Ångström化学系无机化学）；Thin Film Physics Division, Department of Physics, Chemistry and Biology (IFM), Linköping University（林雪平大学物理、化学和生物学学院薄膜物理分部）
Diamond nanocrystals that host room temperature narrowband single photon emitters are highly sought after for applications in nanophotonics and bio-imaging. However, current understanding of the origin of these emitters is extremely limited. In this work we demonstrate that the narrowband emitters are point defects localized at extended morphological defects in individual nanodiamonds. In particular, we show that nanocrystals with defects such as twin boundaries and secondary nucleation sites exhibit narrowband emission that is absent from pristine individual nanocrystals grown under the same …
A simple model to describe Mixed Ionic Electronic Conductors (MIEC) in terms of standard semiconductor physics is described. This model allows to understand defect equilibrium and charge transport at ideal heterojunctions between materials simultaneously conducting electronic and ionic point defects and to explore how rectifying effects on the electronic or ionic currents may affect the chemical diffusion and voltage at the interfaces under polarization. We found qualitatively good agreement with experimental measurements of the electrical conductivity relaxation of La2NiO4+d thin films epitax…
The study of defect centers in silicon has been recently reinvigorated by their potential applications in optical quantum information processing. A number of silicon defect centers emit single photons in the telecommunication $O$-band, making them promising building blocks for quantum networks between computing nodes. The two-carbon G-center, self-interstitial W-center, and spin-$1/2$ T-center are the most intensively studied silicon defect centers, yet despite this, there is no consensus on the precise configurations of defect atoms in these centers, and their electronic structures remain amb…
Cation site disorder provides a degree of freedom in the growth of ternary nitrides for tuning the technologically relevant properties of a material system. For example, the band gap of ZnGeN$_2$ changes when the ordering of the structure deviates from that of its ground state. By combining the perspectives of carrier localization and defect states, we analyze the impact of different degrees of disordering on electronic properties in ZnGeN$_2$, addressing a gap in current studies which focus on dilute or fully disordered systems. The present study demonstrates changes in the density of states …
Long-lived, pulse-induced absorption in $\mathrm{LiNb}_{1-x}\mathrm{Ta}_x\mathrm{O}_3$ solid solutions: the case of three intrinsic defect sites for electron localization with strong coupling
In energetic materials, the localization of energy into "hotspots" when a shock wave interacts with the material's microstructure is known to dictate the initiation of chemical reactions and detonation. Recent results have shown that, following the shock-induced collapse of pores with circular cross-sections, more energy is localized as internal potential energy (PE) than can be inferred from the kinetic energy (KE) distribution. This leads to a complex thermo-mechanical state that is typically overlooked. The mechanisms associated with pore collapse and hotspot formation and the resulting ene…
In order to optimize the optoelectronic properties of novel solar cell architectures, such as the amorphous-crystalline interface in silicon heterojunction devices, we calculate and analyze the local microscopic structure at this interface and in bulk a-Si:H, in particular with respect to the impact of material inhomogeneities. The microscopic information is used to extract macroscopic material properties, and to identify localized defect states, which govern the recombination properties encoded in quantities such as capture cross sections used in the Shockley-Read-Hall theory. To this end, at…
We combine infrared reflectivity and EXAFS (Extended X-ray Absorption Fine Structure) techniques to study the solid solution La0.67Ca0.33MnO3 prepared by different methods yielding samples with different insulator-metal transition temperatures (TIM). While the small polaron analysis of the optical conductivity provides a natural description for the higher frequency reflectivity tail of conducting samples, our structural results are in accord with two non-equivalent sites in the insulating phase of good-quality samples. Those sites, one for the Mn3+ Jahn-Teller distorted octahedra and another f…
