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Machine learning force field (ML-FF) has emerged as a potential promising approach to simulate various material phenomena for large systems with ab initio accuracy. However, most ML-FFs have been used to study the phenomena relatively close to the equilibrium ground states. In this work, we have studied a far from equilibrium system of liquid to crystal Si growth using ML-FF. We found that our ML-FF based on ab initio decomposed atomic energy can reproduce all the aspects of ab initio simulated growth, from local energy fluctuations to transition temperatures, to diffusion constant, and growth rates. We have also compared the growth simulation with the Stillinger–Weber classical force field and found significant differences. A procedure is also provided to correct a systematic fitting bias in the ML-FF training process, which exists in all training models, otherwise critical results like transition temperature will be wrong. [ABSTRACT FROM AUTHOR]

We present a new empirical pseudopotential (EPM) calculation approach to simulate the million atom nanostructured semiconductor devices under potential bias using periodic boundary conditions. To treat the nonequilibrium condition, instead of directly calculating the scattering states from the source and drain, we calculate the stationary states by the linear combination of bulk band method and then decompose the stationary wave function into source and drain injecting scattering states according to an approximated top of the barrier splitting (TBS) scheme based on physical insight of ballistic and tunneling transports. The decomposed electronic scattering states are then occupied according to the source/drain Fermi-Levels to yield the occupied electron density which is then used to solve the potential, forming a self-consistent loop. The TBS is tested in a one-dimensional effective mass model by comparing with the direct scattering state calculation results. It is also tested in a three-dimensional 22 nm double gate ultra-thin-body field-effect transistor study, by comparing the TBS-EPM result with the nonequilibrium Green's function tight-binding result. We expected the TBS scheme will work whenever the potential in the barrier region is smoother than the wave function oscillations and it does not have local minimum, thus there is no multiple scattering as in a resonant tunneling diode, and when a three-dimensional problem can be represented as a quasi-one-dimensional problem, e.g., in a variable separation approximation. Using our approach, a million atom nonequilibrium nanostructure device can be simulated with EPM on a single processor computer. [ABSTRACT FROM AUTHOR]

The development of the charge patching method for the calculation of the electronic structure of organic systems containing a large number of atoms was presented. The method was tested on a range of systems including alkane and alkene chains, polyacenes, polythiophenes, polypyrroles, polyfuranes, polyphenylene vinylene, and poly(amidoamine) dendrimers. The results obtained by the method are in very good agreement with direct calculations based on density functional theory, since the eigenstate errors are typically of the order of a few tens of meV. [ABSTRACT FROM AUTHOR]

The mechanical and electrical properties of CdTe tetrapod-shaped nanocrystals have been studied with atomic force microscopy. Tapping mode images of tetrapods deposited on silicon wafers revealed that they contact the surface with three of its arms. The length of these arms was found to be 130±10 nm. A large fraction of the tetrapods had a shortened vertical arm as a result of fracture during sample preparation. Fracture also occurs when the applied load is a few nanonewtons. Compression experiments with the atomic force microscope tip indicate that tetrapods with the shortened vertical arm deform elastically when the applied force was less than 50 nN. Above 90 nN additional fracture events occurred that further shortened the vertical arm. Loads above 130 nN produced irreversible damage to the other arms as well. Current-voltage characteristics of tetrapods deposited on gold revealed a semiconducting behavior with a current gap of ∼2 eV at low loads (<50 nN) and a narrowing to about 1 eV at loads between 60 and 110 nN. Atomistic force field calculations of the deformation suggest that the ends of the tetrapod arms are stuck during compression so that the deformations are due to bending modes. Empirical pseudopotential calculation of the electron states indicates that the reduction of the current gap is due to electrostatic effects, rather than strain deformation effects inside the tetrapod. [ABSTRACT FROM AUTHOR]

We present an unconventional scheme that is able to dramatically modify single-electron states as well as their couplings in semiconductor nanostructures. The approach consists in perturbing the wave-function core (rather than the insignificant tail) of nanostructure states. We demonstrate this approach using a structure of silicon quantum rings. Anomalous interstate mixing, large tunability of orbital energy, and uncommon s/p level crossing are predicted. [ABSTRACT FROM AUTHOR]

The separate effects of strain and film thickness on the antiferromagnetic-to-ferromagnetic phase transition temperature of FeRh thin films by both experiment and density functional calculations were determined. Strain was introduced by epitaxial growth onto MgO, SrTiO3, and KTaO3 substrates. Film thicknesses below 15 nm substantially suppress the transition temperature, T*, to below room temperature in unstrained films. For strained films, tensile/compressive strain decreases/increases T*, respectively. KTaO3 (001) substrates produce sufficient compressive strain to increase the transition temperature of 10 nm FeRh films above room temperature, which is useful for many proposed applications previously limited by the stabilization of the ferromagnetic state at small thicknesses. These results demonstrate that a judicious use of film thickness and substrate can be used to manipulate FeRh's transition temperature over a ∼200K range. [ABSTRACT FROM AUTHOR]

Correcting the band structure within the density functional theory (DFT) formalism is a long term goal for its development. Recently, we have proposed a Wannier Koopman method (WKM) to correct the DFT bandgap using the Kohn-Sham equation. Previous tests show that WKM works well for common semiconductors. Here, we test its accuracy in terms of predicting the bandgap of extreme ionic crystals: alkali halides. We found that the WKM can accurately reproduce the alkali halide bandgaps with accuracy in par with the GW method. On the other hand, the hybrid functional with common parameters, which work well for common semiconductors, significantly underestimate the alkali halides. [ABSTRACT FROM AUTHOR]

We apply a recently developed Wannier-Koopmans method (WKM), based on density functional theory (DFT), to calculate the electronic energy level alignment at an interface between a molecule and metal substrate. We consider two systems: benzenediamine on Au (111), and a bipyridine-Au molecular junction. The WKM calculated level alignment agrees well with the experimental measurements where available, as well as previous GW and DFT + Σ results. Our results suggest that the WKM is a general approach that can be used to correct DFT eigenvalue errors, not only in bulk semiconductors and isolated molecules, but also in hybrid interfaces. [ABSTRACT FROM AUTHOR]

BiVO4 is one of the most promising photoanodes for water-splitting applications. Similar to many d10 materials, where the full-shell d electrons are not directly involved in the bonding, the Bi 6s electrons form isolated low-energy bands in BiVO4. By systematically altering the energy of the Bi 6s states, we find direct evidences that the isolated s states, through the s-p coupling, affect the BiVO4 properties, including valence band maximum position, charge density, and atomic structural distortion. We find that many good properties of BiVO4 for water splitting are related to the s-p coupling due to the existence of Bi 6s states. Based on this understanding, we propose that alloying Bi with Sb can enhance these properties, and hence improve the water-splitting efficiency. [ABSTRACT FROM AUTHOR]

Heterojunction interfaces between metal oxides are often highly lattice mismatched. The atomic and electronic structures of such interfaces, however, are not well understood. We have synthesized Cu2O/TiO2 heterojunction thin films with 13% lattice mismatch and studied the interface via experimental methods and large-scale density function theory calculations of supercells containing ~1300 atoms. We find that an interface of epitaxial quality is formed via a coincidence site lattice of 8 Cu2O unit cells matching 9 TiO2 unit cells. Calculations reveal the existence of a dislocation core of the O sublattices at the interface and a random arrangement of one layer of interfacial Cu atoms. The interfacial electronic structure is found to be mostly determined by the interfacial Cu distribution, rather than by the O dislocation core. The conduction band minimum and valence band maximum states are spatially separated, and there is no strongly localized state near the core. [ABSTRACT FROM AUTHOR]

We have presented a fully atomistic quantum mechanical simulation method on band-to-band tunneling (BTBT) field-effect transistors (FETs). Our simulation approach is based on the linear combination of bulk band method with empirical pseudopotentials, which is an atomist method beyond the effective-mass approximation or k.p perturbation method, and can be used to simulate real-size devices (~105 atoms) efficiently (~5 h on a few computational cores). Using this approach, we studied the InAs dual-gate BTBT FETs. The I-V characteristics from our approach agree very well with the tight-binding non-equilibrium Green's function results, yet our method costs much less computationally. In addition, we have studied ways to increase the tunneling current and analyzed the effects of different mechanisms for that purpose. [ABSTRACT FROM AUTHOR]

The band-to-band tunneling of monolayer transition metal dichalcogenides nano-junction is investigated using atomistic ab initio quantum transport simulations. From the simulation, it is found that the transition metal vacancy defect in the two-dimensional MX2 (M = Mo,W; X = S,Se) band-to-band tunneling diode can dramatically boost the on-state current up to 10 times while maintaining the device sub-threshold swing. The performance enhancement mechanism is discussed in detail by examining partial density of states of the system. It is found that the transition metal vacancy induces band-gap states, which reduce the effective length of the tunneling transition region. [ABSTRACT FROM AUTHOR]

We performed direct calculations of carrier hopping rates in strongly disordered conjugated polymers based on the atomic structure of the system, the corresponding electronic states and their coupling to all phonon modes. We found that the dependence of hopping rates on distance and the dependence of the mobility on temperature are significantly different than the ones stemming from the simple Miller–Abrahams model, regardless of the choice of the parameters in the model. A model that satisfactorily describes the hopping rates in the system and avoids the explicit calculation of electron–phonon coupling constants was then proposed and verified. Our results indicate that, in addition to electronic density of states, the phonon density of states and the spatial overlap of the wave functions are the quantities necessary to properly describe carrier hopping in disordered conjugated polymers. [ABSTRACT FROM AUTHOR]

The electronic structures of lattice highly mismatched ZnTe1-xOx alloys are calculated with the linear scaling three-dimensional fragment method. We found that the intermediate band states should be described as a result of the coupling between O impurity states rather than the coupling of the impurity state with the conduction band states. We also found that this system can be used for intermediate band state solar cell with a theoretical efficiency of 63%. [ABSTRACT FROM AUTHOR]

By comparing the results of some well-controlled calculation methods, we analyze the relative importance of bulk band structure, multi-bulk-band coupling, and boundary conditions in determining colloidal quantum dot conduction band eigenenergies. We find that while the bulk band structure and correct boundary conditions are important, the effects of multi-bulk-band coupling are small. [ABSTRACT FROM AUTHOR]

We present a theoretical study of crystal and electronic structures of CaB6 within a screened-exchange local density approximation (sX-LDA). Our ab initio total energy calculations show that CaB6 is a semiconductor with a gap of >1.2 eV, in agreement with recent experimental observations. We show a very sensitive band-gap dependence on the crystal internal parameter, which might partially explain the scatter of previous theoretical results. Our calculation demonstrates that it is essential to study this system simultaneously for both crystal structures and electronic properties, and that the sX-LDA provides an ideal method for this problem. [ABSTRACT FROM AUTHOR]

Compares the k.p and the direct diagonalization approaches for the electronic structure of quantum dots. Production of incorrect order of valence states in k.p approach; Contribution of s-like valence state from bulk light-hole band; Diagnosis of k.p errors in quantum dots via k.p errors in bulk solids.

Field emission properties of undoped chemical vapor deposited diamond and diamondlike carbon films have been measured for a variety of different deposition conditions. The nature and appearance of the damage site after testing, together with the mathematical form of the observed current–voltage relations, are correlated with the conductivity of the film. This is consistent with a model for the overall current which is a combination of conduction mechanisms through the bulk of the film with Fowler–Nordheim tunneling. © 1998 American Institute of Physics. [ABSTRACT FROM AUTHOR]