Structure and energetics of carbon-related defects in SiC (0001)/SiO2_{\rm 2} systems revealed by first-principles calculations: Defects in SiC, SiO2_{\rm 2}, and just at their interface

We report first-principles calculations that reveal the atomic forms, stability, and energy levels of carbon-related defects in SiC (0001)/SiO$_{\rm 2}$ systems. We clarify the stable position (SiC side, SiO$_{\rm 2}$ side, or just at the SiC/SiO$_{\rm 2}$ interface) of defects depending on the oxidation environment. Under an O-rich condition, the di-carbon antisite ((C$_{\rm 2}$)$_{\rm Si}$) in the SiC side is stable and critical for $n$-channel MOSFETs, whereas the di-carbon defect (Si-C-C-Si) at the interface becomes critical under an O-poor condition. Our results suggest that the oxidation of SiC under a high-temperature O-poor condition is favorable in reducing the defects, in consistent with recent experimental reports.Comment: 17 pages, 10 figure

Structural stability and energy levels of carbon-related defects in amorphous SiO2_2 and its interface with SiC

We report the density-functional calculations that systematically clarify the stable forms of carbon-related defects and their energy levels in amorphous SiO$_2$ using the melt-quench technique in molecular dynamics. Considering the position dependence of the O chemical potential near and far from the SiC/SiO$_2$ interface, we determine the most abundant forms of carbon-related defects: Far from the interface, the CO$_2$ or CO in the internal space in SiO$_2$ is abundant and they are electronically inactive; near the interface, the carbon clustering is likely and a particular mono-carbon defect and a di-carbon defect induce energy levels near the SiC conduction-band bottom, thus being candidates for the carrier traps.Comment: 8 figures, to be published in Japanese Journal of Applied Physic

Analysis of single and composite structural defects in pure amorphous silicon: a first-principles study

The structural and electronic properties of amorphous silicon ($a$-Si) are investigated by first-principles calculations based on the density-functional theory (DFT), focusing on the intrinsic structural defects. By simulated melting and quenching of a crystalline silicon model through the Car-Parrinello molecular dynamics (CPMD), we generate several different $a$-Si samples, in which three-fold ($T_3$), five-fold ($T_5$), and anomalous four-fold ($T_{4a}$) defects are contained. Using the samples, we clarify how the disordered structure of $a$-Si affects the characters of its density of states (DOS). We subsequently study the properties of defect complexes found in the obtained samples, including one that comprises three $T_5$ defects, and we show the conditions for the defect complexes to be energetically stable. Finally, we investigate the hydrogen passivation process of the $T_5$ defects in $a$-Si and show that the hydrogenation of $T_5$ is an exothermic reaction and that the activation energy for a H$_2$ molecule to passivate two $T_5$ sites is calculated to be 1.05 eV

Interstitial Channels that Control Band Gaps and Effective Masses in Tetrahedrally Bonded Semiconductors

We find that electron states at the bottom of the conduction bands of covalent semiconductors are distributed mainly in the interstitial channels and that this floating nature leads to the band-gap variation and the anisotropic effective masses in various polytypes of SiC. We find that the channel length, rather than the hexagonality prevailed in the past, is the decisive factor for the band-gap variation in the polytypes. We also find that the floating nature causes two-dimensional electron and hole systems at the interface of different SiC polytypes and even one-dimensional channels near the inclined SiC surface.Comment: 5 pages, 6 figure

Quantum Singwi-Tosi-Land-Sjoelander approach for interacting inhomogeneous systems under electromagnetic fields: Comparison with exact results

For inhomogeneous interacting electronic systems under a time-dependent electromagnetic perturbation, we derive the linear equation for response functions in a quantum mechanical manner. It is a natural extension of the original semi-classical Singwi-Tosi-Land-Sjoelander (STLS) approach for an electron gas. The factorization ansatz for the two-particle distribution is an indispensable ingredient in the STLS approaches for determination of the response function and the pair correlation function. In this study, we choose an analytically solvable interacting two-electron system as the target for which we examine the validity of the approximation. It is demonstrated that the STLS response function reproduces well the exact one for low-energy excitations. The interaction energy contributed from the STLS response function is also discussed.Comment: 5 figure

A novel intrinsic interface state controlled by atomic stacking sequence at interfaces of SiC/SiO2_2

On the basis of ab-initio total-energy electronic-structure calculations, we find that interface localized electron states at the SiC/SiO$_2$ interface emerge in the energy region between 0.3 eV below and 1.2 eV above the bulk conduction-band minimum (CBM) of SiC, being sensitive to the sequence of atomic bilayers in SiC near the interface. These new interface states unrecognized in the past are due to the peculiar characteristics of the CBM states which are distributed along the crystallographic channels. We also find that the electron doping modifies the energetics among the different stacking structures. Implication for performance of electron devices fabricated on different SiC surfaces are discussed.Comment: 5 pages, 4 figure

Implementation of quantum imaginary-time evolution method on NISQ devices: Nonlocal approximation

The imaginary-time evolution method is widely known to be efficient for obtaining the ground state in quantum many-body problems on a classical computer. A recently proposed quantum imaginary-time evolution method (QITE) faces problems of deep circuit depth and difficulty in the implementation on noisy intermediate-scale quantum (NISQ) devices. In this study, a nonlocal approximation is developed to tackle this difficulty. We found that by removing the locality condition or local approximation (LA), which was imposed when the imaginary-time evolution operator is converted to a unitary operator, the quantum circuit depth is significantly reduced. We propose two-step approximation methods based on a nonlocality condition: extended LA (eLA) and nonlocal approximation (NLA). To confirm the validity of eLA and NLA, we apply them to the max-cut problem of an unweighted 3-regular graph and a weighted fully connected graph; we comparatively evaluate the performances of LA, eLA, and NLA. The eLA and NLA methods require far fewer circuit depths than LA to maintain the same level of computational accuracy. Further, we developed a ``compression'' method of the quantum circuit for the imaginary-time steps as a method to further reduce the circuit depth in the QITE method. The eLA, NLA, and the compression method introduced in this study allow us to reduce the circuit depth and the accumulation of error caused by the gate operation significantly and pave the way for implementing the QITE method on NISQ devices.Comment: 9 pages, 3figure

Periodicity-free unfolding method of electronic energy spectra: Application to twisted bilayer graphene

We propose a novel periodicity-free unfolding method of the electronic energy spectra. Our new method solves a serious problem that calculated electronic band structure strongly depends on the choice of the simulation cell, i.e., primitive-cell or supercell. The present method projects the electronic states onto the free-electron states, giving rise to the {\it plane-wave unfolded} spectra. Using the method, the energy spectra can be calculated as a completely independent quantity from the choice of the simulation cell. We have examined the unfolded energy spectra in detail for three models and clarified the validity of our method: One-dimensional interacting two chain model, monolayer graphene, and twisted bilayer graphene. Furthermore, we have discussed that our present method is directly related to the experimental ARPES (Angle-Resolved Photo-Emission Spectroscopy) spectra.Comment: 10 pages, 5 figure

Comparison of Green's functions for transition metal atoms using self-energy functional theory and coupled-cluster singles and doubles (CCSD)

We demonstrate in the present study that self-consistent calculations based on the self-energy functional theory (SFT) are possible for the electronic structure of realistic systems in the context of quantum chemistry. We describe the procedure of a self-consistent SFT calculation in detail and perform the calculations for isolated $3 d$ transition metal atoms from V to Cu as a preliminary study. We compare the one-particle Green's functions (GFs) obtained in this way and those obtained from the coupled-cluster singles and doubles (CCSD) method. Although the SFT calculation starts from the spin-unpolarized Hartree--Fock (HF) state for each of the target systems, the self-consistency loop correctly leads to degenerate spin-polarized ground states. We examine the spectral functions in detail to find their commonalities and differences among the atoms by paying attention to the characteristics of the two approaches. It is demonstrated via the two approaches that calculations based on the density functional theory (DFT) can fail in predicting the orbital energy spectra for spherically symmetric systems. It is found that the two methods are quite reliable and useful beyond DFT.Comment: 7 figure

Quasiparticle energy spectra of isolated atoms from coupled-cluster singles and doubles (CCSD): Comparison with exact CI calculations

In this study, we have calculated single-electron energy spectra via the Green's function based on the coupled-cluster singles and doubles (GFCCSD) method for isolated atoms from H to Ne. In order to check the accuracy of the GFCCSD method, we compared the results with the exact ones calculated from the full-configuration interaction (FCI). Consequently, we have found that the GFCCSD method reproduces not only the correct quasiparticle peaks but also satellite ones by comparing the exact spectra with the 6-31G basis set. It is also found that open-shell atoms such as C atom exhibit Mott gaps at the Fermi level, which the exact density-functional theory (DFT) fails to describe. The GFCCSD successfully reproduces the Mott HOMO-LUMO (highest-occupied molecular orbital and lowest-unoccupied molecular orbital) gaps even quantitatively. We also discussed the origin of satellite peaks as shake-up effects by checking the components of wave function of the satellite peaks. The GFCCSD is a novel cutting edge to investigate the electronic states in detail.Comment: 9 pages, 4 figure