Unusual persistence of superconductivity against high magnetic fields in the strongly-correlated iron-chalcogenide film FeTe:O-x
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75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
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Results for “strong correlation”
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Charge transfer in strongly correlated systems: An exact diagonalization approach to model Hamiltonians
We study charge transfer in bridged di- and triruthenium complexes from a theoretical and computational point of view. Ab initio computations are interpreted from the perspective of a simple empirical Hamiltonian, a chemically specific Mott-Hubbard model of the complexes' π electron systems. This Hamiltonian is coupled to classical harmonic oscillators mimicking a polarizable dielectric environment. The model can be solved without further approximations in a valence bond picture using the method of exact diagonalization and permits the computation of charge transfer reaction rates in the framework of Marcus' theory. In comparison to the exact solution, the Hartree-Fock mean field theory overestimates both the activation barrier and the magnitude of charge-transfer excitations significantly. For triruthenium complexes, we are able to directly access the interruthenium antiferromagnetic coupling strengths.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Large intrinsic inductance in strongly correlated GaAs two-dimensional holes in the integer quantum hall regime
Quantum Hall measurements are performed for a two-dimensional hole system (2DHS) confined to a 20 nm quantum well in 〈100〉 GaAs. Quantum oscillations reveal a density of 4 - 5×10{sup 10} cm{sup −2} with mobility μ = 1 × 10{sup 6} cm{sup 2}/V s. For temperatures less than ∼350 mK, anomalous insulating peaks are observed between integer fillings 1-2, 2-3, and 3-4. A large out-of-phase signal appears at these peaks, which indicates a substantial inductance inherent to the charge carriers.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Increasing spin-flips and decreasing cost: Perturbative corrections for external singles to the complete active space spin flip model for low-lying excited states and strong correlation
An approximation to the spin-flip extended configuration interaction singles method is developed using a second-order perturbation theory approach. In addition to providing significant efficiency advantages, the new framework is general for an arbitrary number of spin-flips, with the current implementation being applicable for up to around 4 spin-flips. Two new methods are introduced: one which is developed using non-degenerate perturbation theory, spin-flip complete active-space (SF-CAS(S)), and a second quasidegenerate perturbation theory method, SF-CAS(S){sub 1}. These two approaches take the SF-CAS wavefunction as the reference, and then perturbatively includes the effect of single excitations. For the quasidegenerate perturbation theory method, SF-CAS(S){sub 1}, the subscripted “1” in the acronym indicates that a truncated denominator expansion is used to obtain an energy-independent down-folded Hamiltonian. We also show how this can alternatively be formulated in terms of an extended Lagrangian, by introducing an orthonormality constraint on the first-order wavefunction. Several numerical examples are provided, which demonstrate the ability of SF-CAS(S) and SF-CAS(S){sub 1} to describe bond dissociations, singlet-triplet gaps of organic molecules, and exchange coupling parameters for binuclear transition metal complexes.
74 ATOMIC AND MOLECULAR PHYSICS↗
Theoretical studies of strongly correlated rare-earth intermetallics RIn₃ and RSn₃ (R=Sm, Eu, and Gd)
In this paper, the structural, elastic, and electronic properties of RIn₃ and RSn₃ (R = Sm, Eu, Gd) compounds have been investigated using the full potential linearized augmented plane wave plus local orbital method within the density functional theory. The structural properties are investigated using the LDA, GGA, and the band correlated LDA+U and GGA+U schemes. The lattice parameters are in good agreement with the available experimental results and the divalent state of Eu is also verified. The spin-orbit coupling is included in order to predict the correct electronic properties and splitting of 4f states of the rare earth elements is also incorporated. We calculated Bulk modulus, shear modulus, Young's modulus, anisotropic ratio, Kleinman parameters, Poisson's ratio, Lame's co-efficient, sound velocities for shear and longitudinal waves, and Debye temperature. We also predict the Cauchy pressure and B/G ratio in order to explore the ductile and brittle behaviors of these compounds.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Communication: Configuration interaction combined with spin-projection for strongly correlated molecular electronic structures
We present single and double particle-hole excitations in the recently revived spin-projected Hartree-Fock. Our motivation is to treat static correlation with spin-projection and recover the residual correlation, mostly dynamic in nature, with simple configuration interaction (CI). To this end, we introduce the Wick theorem for nonorthogonal determinants, which enables an efficient implementation in conjunction with the direct CI scheme. The proposed approach, termed spin-extended CI with singles and doubles, achieves a balanced treatment between dynamic and static correlations. To approximately account for the quadruple excitations, we also modify the well-known Davidson correction. We report that our approaches yield surprisingly accurate potential curves for HF, H{sub 2}O, N{sub 2}, and a hydrogen lattice, compared to traditional single reference wave function methods at the same computational scaling as regular CI.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Communication: An adaptive configuration interaction approach for strongly correlated electrons with tunable accuracy
We introduce a new procedure for iterative selection of determinant spaces capable of describing highly correlated systems. This adaptive configuration interaction (ACI) determines an optimal basis by an iterative procedure in which the determinant space is expanded and coarse grained until self-consistency. Two importance criteria control the selection process and tune the ACI to a user-defined level of accuracy. The ACI is shown to yield potential energy curves of N{sub 2} with nearly constant errors, and it predicts singlet-triplet splittings of acenes up to decacene that are in good agreement with the density matrix renormalization group.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Cost-effective description of strong correlation: Efficient implementations of the perfect quadruples and perfect hextuples models
Novel implementations based on dense tensor storage are presented here for the singlet-reference perfect quadruples (PQ) [J. A. Parkhill et al., J. Chem. Phys. 130, 084101 (2009)] and perfect hextuples (PH) [J. A. Parkhill and M. Head-Gordon, J. Chem. Phys. 133, 024103 (2010)] models. The methods are obtained as block decompositions of conventional coupled-cluster theory that are exact for four electrons in four orbitals (PQ) and six electrons in six orbitals (PH), but that can also be applied to much larger systems. PQ and PH have storage requirements that scale as the square, and as the cube of the number of active electrons, respectively, and exhibit quartic scaling of the computational effort for large systems. Applications of the new implementations are presented for full-valence calculations on linear polyenes (C n H n+2 ), which highlight the excellent computational scaling of the present implementations that can routinely handle active spaces of hundreds of electrons. The accuracy of the models is studied in the π space of the polyenes, in hydrogen chains (H 50 ), and in the π space of polyacene molecules. In all cases, the results compare favorably to density matrix renormalization group values. With the novel implementation of PQ, active spaces of 140 electrons in 140 orbitals can be solved in a matter of minutes on a single core workstation, and the relatively low polynomial scaling means that very large systems are also accessible using parallel computing.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Self-consistent implementation of ensemble density functional theory method for multiple strongly correlated electron pairs
Here, the spin-restricted ensemble-referenced Kohn-Sham (REKS) method is based on an ensemble representation of the density and is capable of correctly describing the non-dynamic electron correlation stemming from (near-)degeneracy of several electronic configurations. The existing REKS methodology describes systems with two electrons in two fractionally occupied orbitals. In this work, the REKS methodology is extended to treat systems with four fractionally occupied orbitals accommodating four electrons and self-consistent implementation of the REKS(4,4) method with simultaneous optimization of the orbitals and their fractional occupation numbers is reported. The new method is applied to a number of molecular systems where simultaneous dissociation of several chemical bonds takes place, as well as to the singlet ground states of organic tetraradicals 2,4-didehydrometaxylylene and 1,4,6,9-spiro[4.4]nonatetrayl.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Cluster decomposition of full configuration interaction wave functions: A tool for chemical interpretation of systems with strong correlation
Approximate full configuration interaction (FCI) calculations have recently become tractable for systems of unforeseen size, thanks to stochastic and adaptive approximations to the exponentially scaling FCI problem. The result of an FCI calculation is a weighted set of electronic configurations, which can also be expressed in terms of excitations from a reference configuration. The excitation amplitudes contain information on the complexity of the electronic wave function, but this information is contaminated by contributions from disconnected excitations, i.e., those excitations that are just products of independent lower-level excitations. The unwanted contributions can be removed via a cluster decomposition procedure, making it possible to examine the importance of connected excitations in complicated multireference molecules which are outside the reach of conventional algorithms. We present an implementation of the cluster decomposition analysis and apply it to both true FCI wave functions, as well as wave functions generated from the adaptive sampling CI algorithm. Furthermore, the cluster decomposition is useful for interpreting calculations in chemical studies, as a diagnostic for the convergence of various excitation manifolds, as well as as a guidepost for polynomially scaling electronic structure models. Applications are presented for (i) the double dissociation of water, (ii) the carbon dimer, (iii) the π space of polyacenes, and (iv) the chromium dimer. While the cluster amplitudes exhibit rapid decay with an increasing rank for the first three systems, even connected octuple excitations still appear important in Cr 2 , suggesting that spin-restricted single-reference coupled-cluster approaches may not be tractable for some problems in transition metal chemistry.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Exploring Hilbert space on a budget: Novel benchmark set and performance metric for testing electronic structure methods in the regime of strong correlation
This work explores the ability of classical electronic structure methods to efficiently represent (compress) the information content of full configuration interaction (FCI) wave functions. We introduce a benchmark set of four hydrogen model systems of different dimensionalities and distinctive electronic structures: a 1D chain, a 1D ring, a 2D triangular lattice, and a 3D close-packed pyramid. To assess the ability of a computational method to produce accurate and compact wave functions, we introduce the accuracy volume, a metric that measures the number of variational parameters necessary to achieve a target energy error. Using this metric and the hydrogen models, we examine the performance of three classical deterministic methods: (i) selected configuration interaction (sCI) realized both via an a posteriori (ap-sCI) and variational selection of the most important determinants, (ii) an a posteriori singular value decomposition (SVD) of the FCI tensor (SVD-FCI), and (iii) the matrix product state representation obtained via the density matrix renormalization group (DMRG). We find that the DMRG generally gives the most efficient wave function representation for all systems, particularly in the 1D chain with a localized basis. For the 2D and 3D systems, all methods (except DMRG) perform best with a delocalized basis, and the efficiency of sCI and SVD-FCI is closer to that of DMRG. For larger analogs of the models, the DMRG consistently requires the fewest parameters but still scales exponentially in 2D and 3D systems, and the performance of SVD-FCI is essentially equivalent to that of ap-sCI.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Manipulating electronic phase separation in strongly correlated oxides with an ordered array of antidots
The interesting transport and magnetic properties in manganites depend sensitively on the nucleation and growth of electronic phase-separated domains. In this paper, by fabricating antidot arrays in La 0.325 Pr 0.3 Ca 0.375 MnO 3 (LPCMO) epitaxial thin films, we create ordered arrays of micrometer-sized ferromagnetic metallic (FMM) rings in the LPCMO films that lead to dramatically increased metal–insulator transition temperatures and reduced resistances. The FMM rings emerge from the edges of the antidots where the lattice symmetry is broken. Based on our Monte Carlo simulation, these FMM rings assist the nucleation and growth of FMM phase domains increasing the metal–insulator transition with decreasing temperature or increasing magnetic field. Finally, this study points to a way in which electronic phase separation in manganites can be artificially controlled without changing chemical composition or applying external field.
36 MATERIALS SCIENCE↗
Strongly correlated perovskite lithium ion shuttles
Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and biomimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO 3 (Li-SNO) contains a large amount of mobile Li + located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li + conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na + . The results highlight the potential of quantum materials and emergent physics in design of ion conductors.
36 MATERIALS SCIENCE↗
Pseudogap in electron-doped cuprates: Strong correlation leading to band splitting
The pseudogap phenomena have been a long-standing mystery of the cuprate high-temperature superconductors. The pseudogap in the electron-doped cuprates has been attributed to band folding due to antiferromagnetic (AFM) long-range order or short-range correlation. We performed an angle-resolved photoemission spectroscopy study of the electron-doped cuprates Pr 1.3−x La 0.7 Ce x CuO 4 showing spin-glass, disordered AFM behaviors, and superconductivity at low temperatures and, by measurements with fine momentum cuts, found that the gap opens on the unfolded Fermi surface rather than the AFM Brillouin zone boundary. The gap did not show a node, following the full symmetry of the Brillouin zone, and its magnitude decreased from the zone-diagonal to (π,0) directions, opposite to the hole-doped case. These observations were reproduced by cluster dynamical-mean-field-theory calculation, which took into account electron correlation precisely within a (CuO 2 ) 4 cluster. In conclusion, the present experimental and theoretical results are consistent with the mechanism that electron or hole doping into a Mott insulator creates an in-gap band that is separated from the upper or lower Hubbard band by the pseudogap.
74 ATOMIC AND MOLECULAR PHYSICS↗
Characterizing Hidden Structures at NSLS-II: Strongly Correlated Electron Systems, Functional Ceramics, Batteries, and Beyond
Brookhaven National Laboratory (New York) launched its highenergy X-ray science program at the inception of the National Synchrotron Light Source (NSLS), a U.S. Department of Energy (DOE) Office of Science User Facility. Built in the 1980s, the NSLS X17 beamline was the world’s first super-conducting wiggler facility and remained in service for more than 30 years. The NSLS facility was decommissioned in October 2014 and a third-generation synchrotron machine, DOE’s National Synchrotron Light Source II (NSLS-II), took over. Six years after completing construction, NSLS-II has a portfolio of 29 beamlines that includes two operating high-energy powder diffraction beamlines (XPD and PDF) and one high-energy imaging and diffraction beamline under construction (HEX).
36 MATERIALS SCIENCE↗
Entropy of Strongly Correlated Electrons in a Partially Filled Landau Level
We use high-resolution chemical potential measurements to extract the entropy of monolayer and bilayer graphene in the quantum Hall regime via the Maxwell relation [(𝑑𝜇)/(𝑑𝑇)]| 𝑁 =−[(𝑑𝑆)/(𝑑𝑁)]| 𝑇 . Measuring the entropy from 𝑇 = 300 K down to 𝑇 = 200 mK, we identify the sequential emergence of quantum Hall ferromagnetism, fractional quantum Hall states, and various charge orders by comparing the measured entropy in different temperature regimes with theoretical models. At the lowest temperature of 𝑇 ≈ 200 mK we perform a detailed study of the entropy near even-denominator fractional quantum Hall states in bilayer graphene, and comment on the possible topological origin of the observed excess entropy.
Assouline, Alexandre [University of California, Sa↗