An intrinsic issue of the LDA+DMFT approach is the so called double counting of interaction terms. How to choose the double-counting potential in a manner that is both physically sound and consistent is unknown. We have conducted an extensive study of the charge transfer system NiO in the LDA+DMFT framework using quantum Monte Carlo and exact diagonalization as impurity solvers. By explicitly treating the double-counting correction as an adjustable parameter we systematically investigated the effects of different choices for the double counting on the spectral function. Different methods for fixing the double counting can drive the result from Mott insulating to almost metallic. We propose a reasonable scheme for the determination of double-counting corrections for insulating systems.
Non-local Coulomb interactions and metal-insulator transition in Ti$_2$O$_3$: a cluster LDA+DMFT approach
我们提出了Ti $_2$ O $_3$金属-绝缘体转变的从头计算量子理论。采用最近发展起来的集团LDA+DMFT方案来描述该化合物的多体特征。对于任何合理的库仑相互作用值，传统的单点DMFT都不能再现低温绝缘相。结果表明，非定域库仑相互作用和Ti-Ti对间强的化学键是Ti $_2$ O $_3$小能隙绝缘基态的起源.
I present a critical overview of so-called "{\it ab initio}" DFT (density fuctional theory) based calculation schemes for the description of the electronic structure, energy spectrum, and optical response for strongly correlated 3$d$ oxides, in particular, crystal-field and charge transfer transitions as compared with an "old"\, cluster model that does generalize crystal-field and ligand-field theory. As a most instructive illustration of validity of numerous calculation techniques I address the prototypical 3$d$ insulator NiO predicted to be a metal in frames of a standard LDA (local density …
In this paper we provide theoretical LDA+DMFT support of recent ARPES experimental observation of the so called hidden hole like band and corresponding hidden Fermi surface sheet near $Γ$-point in the K$_{0.62}$Fe$_{1.7}$Se$_2$ compound. To some extent this is a solution to the long-standing riddle of Fermi surface absence around $Γ$-point in the K$_x$Fe$_{2-y}$Se$_2$ class of iron chalcogenide superconductors. In accordance with the experimental data Fermi surface was found near the $Γ$-point within LDA+DMFT calculations. Based on the LDA+DMFT analysis in this paper it is shown that the large…
We present a computational study of 2$p$ core-level X-ray photoemission spectra of transition metal monoxides MO (M=Ni, Co, Mn) and sesquioxides M$_2$O$_3$ (M=V, Cr, Fe) using a theoretical framework based on the local-density approximation (LDA) $+$ dynamical mean-field theory (DMFT). We find a very good description of the fine spectral features, which improves considerably over the conventional cluster model. We analyze the role of the non-local screening and its relationship to the long-range magnetic order and the lattice geometry. Our results reveal the potential of the present method for…
The emergence of angle-resolved photoemission spectroscopy (ARPES) made it possible to observe electronic dispersion directly as a spectral function map. On the other hand, a spectral function map can be obtained theoretically, for example, in the LDA+DMFT method. The electronic band on such a map is characterized not only by its energy position at a given $k$-point, but also by its width and intensity. To illustrate a way of quantitative comparison of theoretical spectral functions and ARPES data, spectral functions obtained by the LDA+DMFT method are chosen. It is shown that the theoretical …
We implemented combination of DMFT and $GW$ in its fully self-consistent way, one shot $GW$ approximation, and quasiparticle self-consistent scheme, and studied how well these combined methods perform on H$_2$ molecule as compared to more established methods such as LDA+DMFT. We found that most flavors of $GW$+DMFT break down in strongly correlated regime due to causality violation. Among $GW$+DMFT methods, only the self-consistent quasiparticle $GW$+DMFT with static double-counting, and a new method with causal double-counting, correctly recover the atomic limit at large H-atom separation. Wh…
We report complex band structure (CBS) calculations for the four late transition metal monoxides, MnO, FeO, CoO and NiO, in their paramagnetic phase. The CBS is obtained from density functional theory plus dynamical mean field theory (DMFT) calculations to take into account correlation effects. The so-called $β$ parameters, governing the exponential decay of the transmission probability in the non-resonant tunneling regime of these oxides, are extracted from the CBS. Different model constructions are examined in the DMFT part of the calculation. The calculated $β$ parameters provide theoretica…
We show that evolution of magnetic properties in FeS under pressure cannot be explained only in terms of a spin state transition. While uniform compression does show substantial suppression of the local magnetic moment and increase of the weights of configurations with low spin, analysis of the local spin-spin correlation function demonstrates increase of the spin itinerancy. This is related to a strong modification of the electronic structure under pressure: in the high-pressure phase FeS is in the Fermi-liquid state, while decrease of the pressure moves the system to an orbital-selective reg…
Calculation of photoemission spectra of the doped Mott insulator La_{1-x}Sr_xTiO_3 using LDA+DMFT(QMC)
采用量子化学从头计算方法LDA+DMFT（QMC）计算了具有强库仑关联的掺杂莫特绝缘体$_{1-x}$ $_{x}$ $_{3}$的光谱性质.它从局域密度近似（LDA）计算的非相互作用电子能带结构出发，引入动力学平均场论（DMFT）的丢失关联，采用数值精确量子Monte-Carlo（QMC）技术求解由此产生的自洽多带单杂质问题。用LDA+DMFT（QMC）方法计算了La $_{1-x}$ Sr $_{x}$ TiO $_{3}$的光电子能谱，计算结果与实验符合得很好，并且在定性和定量上都比标准LDA方法有了很大的改进.
Recent experimental observations of magnetization plateau in metallic tetraboride $\textrm{TmB}_{4}$ have created a lot of interest in these class of materials. Hysteretic longitudinal resistance and anomalous Hall Effect are other remarkable features in the rare-earth tetraborides which represent experimental realizations of Archimedean Shastry-Sutherland (SSL) lattice. Electronic band structures, calculated under GGA and GGA+SO approximations, show that $\textrm{TmB}_{4}$ is a narrow band system with considerable correlation in its f-level. Strong correlation effects in this system are studi…
Dynamical mean field theory (DMFT) combined with the local density approximation (LDA) is widely used in solids to predict properties of correlated systems. In this paper, its application to one of the simplest strongly correlated systems, the hydrogen molecule H$_2$, is demonstrated to develop a parameter-free LDA+DMFT framework. We propose a method to calculate the exact intersection of LDA and DMFT that leads to highly accurate subtraction of the doubly counted correlation in both methods. When the exact double-counting treatment and a good projector to the correlated subspace are used, LDA…
Doping Dependence of Correlation Effects in K{1-x}Fe{2-y}Se2 Superconductor: LDA'+DMFT Investigation
本文详细研究了新型K{1-x}Fe{2-y} Se_2超导体中相关效应与掺杂的关系。在四个不同的空穴掺杂水平进行计算，从假设的化学计量组成的电子总数等于29每单位电池通过28和27.2电子对26.52的情况下，这对应于最近的ARPES实验中研究的化学组成K{0.76}Fe{1.72} Se 2。在一般情况下，空穴掺杂的增加导致费米能级附近的宽能量窗口+/-2eV的准粒子带由于寿命效应而变得更宽，而相关诱导的Fe-3d LDA带宽压缩几乎保持不变，并且对于所有空穴浓度都在~1.3的数量级。然而接近费米能级的情况就比较复杂了。在这里，在从-1.0 eV到0.4 eV的能量区间中，裸Fe-3d LDA’带随着空穴掺杂的增加被显著更大的重整化因子压缩到5，而库仑相互作用的值保持不变。这一事实表明，在K{1-x}Fe{2-y} Se 2体系中，空穴掺杂增强了相关效应。与典型的磷属元素化合物相比，K{1-x}Fe{2-y} Se 2在费米能级上没有明确的准粒子带，而是赝能隙状的“暗”区。我们还发现，随着空穴掺杂的增长，不同对称性的Fe-3d轨道在布里渊区的不同部分以不同的方式受到关联的影响。为了说明这一点，我们确定准粒子质量重整化因子和能量位移，这将裸Fe-3d LDA'带的各种对称性的LDA'+ DMFT准粒子带。这些重整化因子有效地模拟了更复杂的能量依赖自能效应，并可用于分析现有的ARPE…
The electronic spectral function of BaNi$_2$As$_2$ is investigated using both the angle-resolved photoemission spectroscopy (ARPES) and a combined computational scheme of local density approximation together with dynamical mean-field theory (LDA+DMFT). In contrast to well studied isostructural iron arsenide high temperature superconductors, the BaNi$_2$As$_2$ demonstrate weak correlation effects although Ni-3d elections have even lager on-site interaction than Fe-3d ones. LDA+DMFT effective mass enhancement for bands crossing the Fermi level is found to be only about $1.2$ which agrees well wi…
We present a computational study of resonant inelastic x-ray scattering (RIXS) and x-ray absorption in a representative rare-earth nickelate LuNiO$_3$. We study the changes in the spectra across the metal-insulator/site-disproportionation transition. In particular, we address the question of site-selectivity of the two methods in the disproportionated insulating phase and the signature of metal-insulator transition in the fluorescence-like feature of the RIXS spectra. To this end we use the local density approximation + dynamical mean-field theory (LDA+DMFT) approach combined with configuratio…
The LDA+DMFT method is a very powerful tool for gaining insight into the physics of strongly correlated materials. It combines traditional ab-initio density-functional techniques with the dynamical mean-field theory. The core aspects of the method are (i) building material-specific Hubbard-like many-body models and (ii) solving them in the dynamical mean-field approximation. Step (i) requires the construction of a localized one-electron basis, typically a set of Wannier functions. It also involves a number of approximations, such as the choice of the degrees of freedom for which many-body effe…
The electronic structure of the Cr(001) surface with its sharp resonance at the Fermi level is a subject of controversial debate of many experimental and theoretical works. To date, it is unclear whether the origin of this resonance is an orbital Kondo or an electron-phonon coupling effect. We have combined ab initio density functional calculations with dynamical mean-field simulations to calculate the orbitally resolved spectral function of the Cr(001) surface. The calculated orbital character and shape of the spectrum is in agreement with data from (inverse) photoemission experiments. We fin…
We present a computational study of $L$-edge resonant inelastic x-ray scattering (RIXS) in correlated 3$d$ transition-metal oxides using an $ab$ $initio$ method based on local density approximation + dynamical mean-field theory (DMFT). The present method, building on Anderson impurity model with an optimized continuum bath within DMFT, is an extension of the cluster model to include unbound electron-hole pair excitations as well as material-specific charge-transfer excitations with less empirical parameters. We find a good agreement with available experimental data. The relationship between co…
We have revisited the valence band electronic structure of NiO by means of hard x-ray photoemission spectroscopy (HAXPES) together with theoretical calculations using both the GW method and the local density approximation + dynamical mean-field theory (LDA+DMFT) approaches. The effective impurity problem in DMFT is solved through the exact diagonalization (ED) method. We show that the LDA+DMFT method alone cannot explain all the observed structures in the HAXPES spectra. GW corrections are required for the O bands and Ni-s and p derived states to properly position their binding energies. Our r…
Materials with correlated electrons often respond very strongly to external or internal influences, leading to instabilities and states of matter with broken symmetry. This behavior can be studied theoretically either by evaluating the linear response characteristics, or by simulating the ordered phases of the materials under investigation. We developed the necessary tools within the dynamical mean-field theory (DMFT) to search for electronic instabilities in materials close to spin-state crossovers and to analyze the properties of the corresponding ordered states. This investigation, motivate…
We study $1s$ and $2p$ hard x-ray photoemission spectra (XPS) in a series of late transition metal oxides: Fe$_2$O$_3$ (3$d^{5}$), FeTiO$_3$ (3$d^{6}$), CoO (3$d^{7}$) and NiO (3$d^{8}$). The experimental spectra are analyzed with two theoretical approaches: the MO$_6$ cluster model and the local density approximation (LDA) + dynamical mean-field theory (DMFT). Owing to the absence of the core-valence multiplets and spin-orbit coupling, 1$s$ XPS is found to be a sensitive probe of chemical bonding and nonlocal charge-transfer screening, providing complementary information to 2$p$ XPS. The 1$s$…
The LDA+DMFT Approach to Materials with Strong Electronic Correlations
LDA+DMFT是一种新型计算技术，用于具有强关联电子的真实材料（例如过渡金属及其氧化物）的从头算研究。它结合了局域密度近似（LDA）中传统能带结构理论与现代多体方法，动力学平均场理论（DMFT）的优势。在过去的几年中，LDA+DMFT已被证明是一个强大的工具，为现实的建模强相关的电子系统。本文讨论了LDA+DMFT（X）方法的基本思想和建立，其中X是求解DMFT方程的方法。给出了X=QMC（量子蒙特卡罗）和X=NCA（非交叉近似）的计算结果，并进行了比较。通过模型系统La $_{1-x}$ Sr $_{x}$ TiO $_{3}$，我们定性和定量地证明了方法X的重要性。此外，我们还讨论了过渡金属氧化物V $_2$ O $_3$中的Mott-Hubbard金属-绝缘体转变和4f电子系统Ce中的$α$ - $γ$转变的最新结果.
Motivated by recent core-level x-ray photoemission spectroscopy (XPS), x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) experiments for the newly-discovered superconducting infinite-layer nickelate, we investigate the core-level spectra of the parent compounds NdNiO$_2$ and LaNiO$_2$ using the combination of local density approximation and dynamical mean-field theory (LDA+DMFT). Adjusting a charge-transfer energy to match the experimental spectra, we determine the optimal model parameters and discuss the nature of the NdNiO$_2$ ground state. We find that self-…
The electronic structure and magnetic properties of a single Fe adatom on a CuN surface have been studied using density functional theory in the local spin density approximation (LSDA), the LSDA+U approach and the local density approximation plus dynamical mean-field theory (LDA+DMFT). The impurity problem in LDA+DMFT is solved through exact diagonalization and in the Hubbard-I approximation. The comparison of the one-particle spectral functions obtained from LSDA, LSDA+U and LDA+DMFT show the importance of dynamical correlations for the electronic structure of this system. Most importantly, w…
We present the results of extended theoretical LDA+DMFT calculations for a new iron-pnictide high temperature superconductor NaFeAs compared with the recent high quality angle-resolved photoemission (ARPES) experiments on this system [1]. The universal manifestation of correlation effects in iron-pnictides is narrowing of conducting bands near the Fermi level. Our calculations demonstrate that for NaFeAs the effective mass is renormalized on average by a factor of the order of 3, in good agreement with ARPES data. This is essentially due to correlation effects on Fe-3d orbitals only and no add…
Using local density approximation plus dynamical mean-field theory (LDA+DMFT), we have computed the valence band photoelectron spectra of highly popular multiferroic BiFeO$_{3}$. Within DMFT, the local impurity problem is tackled by exact diagonalization (ED) solver. For comparison, we also present result from LDA+U approach, which is commonly used to compute physical properties of this compound. Our LDA+DMFT derived spectra match adequately with the experimental hard X-ray photoelectron spectroscopy (HAXPES) and resonant photoelectron spectroscopy (RPES) for Fe 3$d$ states, whereas the other …
