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Register a new userBand Alignment in Quantum Wells from Automatically Tuned DFT+$U$
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Band alignment between two materials is of fundamental importance for multitude of applications. However, density functional theory (DFT) either underestimates the bandgap - as is the case with local density approximation (LDA) or generalized gradient approximation (GGA) - or is highly computationally demanding, as is the case with hybrid-functional methods. The latter can become prohibitive in electronic-structure calculations of supercells which describe quantum wells. We propose to apply the DFT$+U$ method, with $U$ for each atomic shell being treated as set of tuning parameters, to automatically fit the bulk bandgap and the lattice constant, and then use thus obtained $U$ parameters in large supercell calculations to determine the band alignment. We apply this procedure to InP/In$_{0.5}$Ga$_{0.5}$As, In$_{0.5}$Ga$_{0.5}$As/In$_{0.5}$Al$_{0.5}$As and InP/In$_{0.5}$Al$_{0.5}$As quantum wells, and obtain good agreement with experimental results. Although this procedure requires some experimental input, it provides both meaningful valence and conduction band offsets while, crucially, lattice relaxation is taken into account. The computational cost of this procedure is comparable to that of LDA. We believe that this is a practical procedure that can be useful for providing accurate estimate of band alignments between more complicated alloys.
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Accurate computational predictions of band gaps are of practical importance to the modeling and development of semiconductor technologies, such as (opto)electronic devices and photoelectrochemical cells. Among available electronic-structure methods, density-functional theory (DFT) with the Hubbard U correction (DFT+U) applied to band edge states is a computationally tractable approach to improve the accuracy of band gap predictions beyond that of DFT calculations based on (semi)local functionals. At variance with DFT approximations, which are not intended to describe optical band gaps and other excited-state properties, DFT+U can be interpreted as an approximate spectral-potential method when U is determined by imposing the piecewise linearity of the total energy with respect to electronic occupations in the Hubbard manifold (thus removing self-interaction errors in this subspace), thereby providing a (heuristic) justification for using DFT+U to predict band gaps. However, it is still frequent in the literature to determine the Hubbard U parameters semiempirically by tuning their values to reproduce experimental band gaps, which ultimately alters the description of other total-energy characteristics. Here, we present an extensive assessment of DFT+U band gaps computed using self-consistent ab initio U parameters obtained from density-functional perturbation theory to impose the aforementioned piecewise linearity of the total energy. The study is carried out on 20 compounds containing transition-metal or p-block (group III-IV) elements, including oxides, nitrides, sulfides, oxynitrides, and oxysulfides...
The energy spectrum of the valence band in HgTe/Cd$_x$Hg$_{1-x}$Te quantum wells with a width $(8-20)$~nm has been studied experimentally by magnetotransport effects and theoretically in framework $4$-bands $kP$-method. Comparison of the Hall density with the density found from period of the Shubnikov-de Haas (SdH) oscillations clearly shows that the degeneracy of states of the top of the valence band is equal to 2 at the hole density $p< 5.5times 10^{11}$~cm$^{-2}$. Such degeneracy does not agree with the calculations of the spectrum performed within the framework of the $4$-bands $kP$-method for symmetric quantum wells. These calculations show that the top of the valence band consists of four spin-degenerate extremes located at $k eq 0$ (valleys) which gives the total degeneracy $K=8$. It is shown that taking into account the mixing of states at the interfaces leads to the removal of the spin degeneracy that reduces the degeneracy to $K=4$. Accounting for any additional asymmetry, for example, due to the difference in the mixing parameters at the interfaces, the different broadening of the boundaries of the well, etc, leads to reduction of the valleys degeneracy, making $K=2$. It is noteworthy that for our case two-fold degeneracy occurs due to degeneracy of two single-spin valleys. The hole effective mass ($m_h$) determined from analysis of the temperature dependence of the amplitude of the SdH oscillations show that $m_h$ is equal to $(0.25pm0.02),m_0$ and weakly increases with the hole density. Such a value of $m_h$ and its dependence on the hole density are in a good agreement with the calculated effective mass.
The energy spectrum of the conduction band in HgTe/Cd$_x$Hg$_{1-x}$Te quantum wells of a width $d=(4.6-20.2)$ nm has been experimentally studied in a wide range of electron density. For this purpose, the electron density dependence of the effective mass was measured by two methods: by analyzing the temperature dependence of the Shubnikov-de Haas oscillations and by means of the quantum capacitance measurements. There was shown that the effective mass obtained for the structures with $d<d_c$, where $d_csimeq6.3$ nm is a critical width of quantum well corresponding to the Dirac-like energy spectrum, is close to the calculated values over the whole electron density range; with increasing width, at $d>(7-8)$ nm, the experimental effective mass becomes noticeably less than the calculated ones. This difference increases with the electron density decrease, i.e., with lowering the Fermi energy; the maximal difference between the theory and experiment is achieved at $d = (15-18)$ nm, where the ratio between the calculated and experimental masses reaches the value of two and begins to decrease with a further $d$ increase. We assume that observed behavior of the electron effective mass results from the spectrum renormalization due to electron-electron interaction.
Contradictory theoretical results for oxygen vacancies in SrTiO$_3$ (STO) were often related to the peculiar properties of STO, which is a $d^0$ transition metal oxide with mixed ionic-covalent bonding. Here, we apply, for the first time, density functional theory (DFT) within the extended Hubbard DFT+$U$+$V$ approach, including on-site as well as inter-site electronic interactions, to study oxygen-deficient STO with Hubbard $U$ and $V$ parameters computed self-consistently via density-functional perturbation theory. Our results demonstrate that the extended Hubbard functional is a promising approach to study defects in materials with electronic properties similar to STO. Indeed, DFT+$U$+$V$ provides a better description of stoichiometric STO compared to standard DFT or DFT+$U$, the band gap and crystal field splitting being in good agreement with experiments. In turn, also the description of the electronic properties of oxygen vacancies in STO is improved, with formation energies in excellent agreement with experiments as well as results obtained with the most frequently used hybrid functionals, however at a fraction of the computational cost. While our results do not fully resolve the contradictory findings reported in literature, our systematic approach leads to a deeper understanding of their origin, which stems from different cell sizes, STO phases, the exchange-correlation functional, and the treatment of structural relaxations and spin-polarization.
Spin-orbit splitting of conduction band in HgTe quantum wells was studied experimentally. In order to recognize the role of different mechanisms, we carried out detailed measurements of the Shubnikov-de Haas oscillations in gated structures with a quantum well widths from $8$ to $18$ nm over a wide range of electron density. With increasing electron density controlled by the gate voltage, splitting of the maximum of the Fourier spectrum $f_0$ into two components $f_1$ and $f_2$ and the appearance of the low-frequency component $f_3$ was observed. Analysis of these results shows that the components $f_1$ and $f_2$ give the electron densities $n_1$ and $n_2$ in spin-orbit split subbands while the $f_3$ component results from magneto-intersubband oscillations so that $f_3=f_1 - f_2$. Comparison of these data with results of self-consistent calculations carried out within the framework of four-band emph{kP}-model shows that a main contribution to spin-orbit splitting comes from the Bychkov-Rashba effect. Contribution of the interface inversion asymmetry to the splitting of the conduction band turns out to be four-to-five times less than that for the valence band in the same structures.
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