Strong Electron Correlations Research Articles

Electronic Band Structure of a Superconducting Nickelate Probed by the Seebeck Coefficient in the Disordered Limit

Superconducting nickelates are a new family of strongly correlated electron materials with a phase diagram closely resembling that of superconducting cuprates. While analogy with the cuprates is natural, very little is known about the metallic state of the nickelates, making these comparisons difficult. We probe the electronic dispersion of thin-film superconducting five-layer (n=5) and metallic three-layer (n=3) nickelates by measuring the Seebeck coefficient S. We find a temperature-independent and negative S/T for both n=5 and n=3 nickelates. These results are in stark contrast to the strongly temperature-dependent S/T measured at similar electron filling in the cuprate La1.36Nd0.4Sr0.24CuO4. The electronic structure calculated from density-functional theory can reproduce the temperature dependence, sign, and amplitude of S/T in the nickelates using Boltzmann transport theory. This demonstrates that the electronic structure obtained from first-principles calculations provides a reliable description of the fermiology of superconducting nickelates and suggests that, despite indications of strong electronic correlations, there are well-defined quasiparticles in the metallic state. Finally, we explain the differences in the Seebeck coefficient between nickelates and cuprates as originating in strong dissimilarities in impurity concentrations. Our study demonstrates that the high elastic scattering limit of the Seebeck coefficient reflects only the underlying band structure of a metal, analogous to the high magnetic field limit of the Hall coefficient. This opens a new avenue for Seebeck measurements to probe the electronic band structures of relatively disordered quantum materials. Published by the American Physical Society 2024

Polaritonic Chemistry Using the Density Matrix Renormalization Group Method.

The emerging field of polaritonic chemistry explores the behavior of molecules under strong coupling with cavity modes. Despite recent developments in ab initio polaritonic methods for simulating polaritonic chemistry under electronic strong coupling, their capabilities are limited, especially in cases where the molecule also features strong electronic correlation. To bridge this gap, we have developed a novel method for cavity QED calculations utilizing the Density Matrix Renormalization Group (DMRG) algorithm in conjunction with the Pauli-Fierz Hamiltonian. Our approach is applied to investigate the effect of the cavity on the S0-S1 transition of n-oligoacenes, with n ranging from 2 to 5, encompassing 22 fully correlated π orbitals in the largest pentacene molecule. Our findings indicate that the influence of the cavity intensifies with larger acenes. Additionally, we demonstrate that, unlike the full determinantal representation, DMRG efficiently optimizes and eliminates excess photonic degrees of freedom, resulting in an asymptotically constant computational cost as the photonic basis increases.

Elucidating correlation-driven insulating state in an effective spin—½ antiferromagnet NdVO4

TheJeff= ½ state: a result of interplay of strong electronic correlations (U) with spin-orbit coupling (SOC) and crystal field splitting, offers a platform in the research of quantum materials. In this context, 4frare-earth based materials offer a fertile playground. Here, strong experimental and theoretical evidences for aJeff= ½ state is established in a three-dimensional spin system NdVO4. Magnetic measurements show the signatures of a SOC drivenJeff= ½ state along with the presence of antiferromagnetic (AFM) interaction between Nd3+moments, whereas, heat capacity reveals the presence of an AFM ordering around 0.8 K, within this state. An entropy of Rln2 (equivalent toJ= ½) is released around 4 K which implies the presence ofJeff= ½ state at low temperatures. Total energy calculations within the density functional theory (DFT) framework reflect the central role of SOC in driving the Nd3+ions to host such a state with AFM correlations between them, which is in agreement with experimental results. Further, DFT + SOC calculations with and without the inclusion ofU, points that electron-electron correlations give rise to the insulating state making NdVO4a potential candidate forU-driven correlated Mott insulator.

Superconductivity and Mott Physics in Organic Charge Transfer Materials.

The phase diagrams of quasi two-dimensional organic superconductors display a plethora of fundamental phenomena associated with strong electron correlations, such as unconventional superconductivity, metal-insulator transitions, frustrated magnetism and spin liquid behavior. We analyze a minimal model for these compounds, the Hubbard model on an anisotropic triangular lattice, using cutting-edge quantum embedding methods respecting the lattice symmetry. We demonstrate the existence of unconventional superconductivity by directly entering the symmetry-broken phase. We show that the crossover from the Fermi liquid metal to the Mott insulator is associated with the formation of a pseudogap. The predicted momentum-selective destruction of the Fermi surface into hot and cold regions provides motivation for further spectroscopic studies. Our theoretical results agree with experimental phase diagrams of κ-BEDT organics.

First-principles investigation of the metal-insulator transition in the high-temperature phase of VO2 (A) at 473 K

The structure, electronic and magnetic properties of the high-temperature phase of VO2 (A) [HT-VO2 (A)] are extensively investigated by employing first-principles electronic structure calculations. Structural distortion is observed due to the alternative formation of V-V square wells and V-V rectangular four-chain columns in the ab plane and extending along the c-direction. The system is found to be a ferrimagnetic metal due to sharing of the available single V-3d electron by the V-dxy, dyz, dxz states in the spin majority channel and exclusively by the V-dxy states in the spin minority channel. This material encounters metal-to-half-metal transition for an effective Coulomb interaction of Ueff = 2 eV, exhibiting ferromagnetism. The sharing of the single V-3d electron by the V-dxy, dyz and dxz states in the spin majority channel results in the half-metallic behaviour of HT-VO2 (A). The system eventually encounters metal-insulator transition (MIT) upon the application of Ueff = 2.5 eV. Strong electron correlation triggered by U completely breaks both the V-dxy and dyz states into occupied and unoccupied components and hence sets up complete orbital ordering that is responsible for the observed MIT in HT-VO2 (A). The cooperative effect of p-d hybridization and V-O antiferromagnetic coupling gives rise to ferromagnetism in both the half-metallic and insulating phases of HT-VO2 (A).

Anomalous Hall effect and electronic correlation in a spin-reoriented kagome antiferromagnet LuFe6Sn6

Abstract The kagome lattice system has been identified as a fertile ground for the emergence of a number of new quantum states, including superconductivity, quantum spin liquids, and topological electronic states. This has attracted significant interest within the field of condensed matter physics. Here, we present the observation of an anomalous Hall effect in an iron-based kagome antiferromagnet LuFe6Sn6, which implies a non-zero Berry curvature in this compound. By means of extensive magnetic measurements, a high Neel temperature, T N = 552 K, and a spin reorientation behavior were identified and a simple temperature-field phase diagram was constructed. Furthermore, this compound was found to exhibit a large Sommerfeld coefficient of γ = 87 mJ⋅mol−1⋅K−2, suggesting the presence of a strong electronic correlation effect. Our research indicates that LuFe6Sn6 is an intriguing compound that may exhibit magnetism, strong correlation, and topological states.

Electronic correlations and partial gap in the bilayer nickelate La3Ni2O7

The discovery of superconductivity with a critical temperature of about 80 K in La3Ni2O7 single crystals under pressure has received enormous attention. La3Ni2O7 is not superconducting under ambient pressure but exhibits a transition at T ∗ ≃ 115 K. Understanding the electronic correlations and charge dynamics is an important step towards the origin of superconductivity and other instabilities. Here, our optical study shows that La3Ni2O7 features strong electronic correlations which significantly reduce the electron’s kinetic energy and place this system in the proximity of the Mott phase. The low-frequency optical conductivity reveals two Drude components arising from multiple bands at the Fermi level. The transition at T ∗ removes the Drude component exhibiting non-Fermi liquid behavior, whereas the one with Fermi-liquid behavior is barely affected. These observations in combination with theoretical results suggest that the Fermi surface dominated by the Ni-d3z2−r2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${d}_{3{z}^{2}-{r}^{2}}$$\\end{document} orbital is removed due to the transition at T ∗. Our experimental results provide pivotal information for understanding the transition at T ∗ and superconductivity in La3Ni2O7.

Exploration of a New Class p-type Conducting Oxide Based on the Strong Correlation Effect

Transparent conducting oxides (TCOs) have been researched for several decades thus utilizing in many technology advances especially on display area. While such an advance p-type TCO entry is still rare compared to the n-type one as hindering the next generation oxide-based electronics. This article briefly introduces materials design concepts on typical TCOs, and a new approach to realize a high-performance p-type TCO based on strong electron correlation effect.

Superconductivity under pressure in a chromium-based kagome metal.

Superconductivity in a highly correlated kagome system has been theoretically proposed for years (refs. 1-5), yet the experimental realization is hard to achieve6,7. The recently discovered vanadium-based kagome materials8, which exhibit both superconductivity9-11 and charge-density-wave orders12-14, are nonmagnetic8,9 and weakly correlated15,16. Thus these materials are unlikely to host the exotic superconductivity theoretically proposed. Here we report the discovery of a chromium-based kagome metal, CsCr3Sb5, which is contrastingly featured with strong electron correlations, frustrated magnetism and characteristic flat bands close to the Fermi level. Under ambient pressure, this kagome metal undergoes a concurrent structural and magnetic phase transition at 55 K, with a stripe-like 4a0 structural modulation. At high pressure, the phase transition evolves into two transitions, possibly associated with charge-density-wave and antiferromagnetic spin-density-wave orderings. These density-wave-like orders are gradually suppressed with pressure and, remarkably, a superconducting dome emerges at 3.65-8.0 GPa. The maximum of the superconducting transition temperature, Tcmax = 6.4 K, appears when the density-wave-like orders are completely suppressed at 4.2 GPa, and the normal state exhibits a non-Fermi-liquid behaviour, reminiscent of unconventional superconductivity and quantum criticality in iron-based superconductors17,18. Our work offers an unprecedented platform for investigating superconductivity in correlated kagome systems.

Effects of electronic correlation on topological properties of Kagome semimetal Ni3In2S2.

Kagome metals gain attention as they manifest a spectrum of quantum phenomena such as superconductivity, charge order, frustrated magnetism, and allied correlated states of condensed matter. With regard to electronic band structure, several of them exhibit non-trivial topological characteristics. Here, we present a thorough investigation on the growth and the physical properties of single crystals of Ni3In2S2 which is established to be a Dirac nodal line Kagome semimetal. Extensive characterization is attained through temperature and field-dependent resistivity, angle-dependent magnetoresistance and specific heat measurements. The central question we seek to address is the effect of electronic correlations in suppressing the manifestation of topological characteristics. In most metals, the Fermi liquid behaviour is restricted to a narrow range of temperatures. Here we show that Ni3In2S2 follows the Fermi-liquid behaviour up to 86K. This phenomenon is further supported by a high Kadowaki-Woods ratio obtained through specific heat analysis. Different interpretations of the magneto-transport study reveal that magnetoresistance exhibits linear behavior, suggesting the presence of Dirac semi-metallic signatures at lower temperatures. The angle-dependent magneto-transport study obeys the Voigt-Thomson formula. This, on the contrary, implies the classical origin of magnetoresistance. Thus, the effect of strong electron correlation in Ni3In2S2 manifests itself in the anisotropic magneto-transport. Furthermore, the magnetization measurement shows the presence of de-Haas van Alphen oscillations. Calculations of Berry phase provide insights into the topological features in the Kagome semimetal Ni3In2S2.&#xD.

Transition metal oxides: a new frontier in spintronics driven by novel quantum states and efficient charge-spin interconversion

Transition metal oxides (TMOs) have emerged as promising candidates for spintronic applications due to their unique electronic properties and novel quantum states. The intricate interplay between strong spin-orbit coupling and electronic correlations in TMOs gives rise to distinct spin and orbital textures, leading to enhanced spin-momentum locking and efficient charge-spin interconversion. Remarkably, recent researches have unveiled the significant and highly tunable nature of charge-spin interconversion efficiency in TMOs, which can be manipulated through strategies such as electric field gating, epitaxial strain, and heterostructure engineering. This review provides a comprehensive overview of the recent advances in understanding the electronic band structures of TMOs and their correlation with charge-spin interconversion mechanisms. We summarize the tunability of these properties through various experimental approaches and discuss the potential implications for spintronic device applications. The insights gained from this review can guide future research efforts towards the development of high-performance, energy-efficient spintronic devices based on TMOs.

Universality and the thermoelectric transport properties of a double quantum dot system: Seeking for conditions that improve the thermoelectric efficiency

Employing universal relations for the Onsager coefficients in the linear regime at the symmetric point of the single impurity Anderson model, we calculate the conditions under which the quantum scattering phase shift should satisfy to produce the asymptotic Carnot’s limit for the thermoelectric efficiency. We show that a single quantum dot connected by metallic leads at the Kondo regime cannot achieve the best thermoelectric efficiency. We study a serial double quantum dot system, with the quantum dots immersed in ballistic conduction channels. Each QD exhibits a strong but finite local electronic correlation UU. We show that maintaining one dot in the electron-hole symmetric point and allowing charge fluctuations in the other QD makes it possible to drive the system to the maximum thermoelectric efficiency. We also show that the bound states in the continuum (BICs) and quasi-BICs associated with the quantum scattering interference process drive the DQD to the maximum thermoelectric efficiency. We identify two types of quasi-BICs that occur at low and high temperatures: The first is associated with single Fano resonances, and the last is with several Fano processes. We also discussed possible temperature values and conditions that could be linked with the experimental realization of the results.

Exploring the effect of strong electronic correlations in Seebeck Coefficient of the NdCoO3 compound : Using experimental and DFT+U approach

The presence of complexity in the electronic structure of strongly correlated electron system NdCoO3 (NCO) have sparked interest in the investigation of its physical properties. Here, we study the Seebeck coefficient (α) of NCO by using the combined experimental and DFT+U based methods. The experimentally measured Seebeck coefficient is found to be ∼444 μ V/K at 300 K, which decreases to 109.8 μ V/K at 600 K. In order to understand the measured Seebeck coefficient, we have calculated the PDOS and band structure of the NCO. Furthermore, the calculated occupancy of 6.4 for Co 3d orbitals and presence of large unoccupied O 2p states indicate the covalent nature of the bonding. Apart from this, the maximum effective mass is found to be 36.75 (28.13) me for the spin-up (dn) channel in conduction band indicates the n-type behaviour of the compound in contrast to our experimentally observed p-type behaviour. While, the calculated Seebeck coefficient at the temperature-dependent chemical potential (μ) at 300 K shows the p-type behaviour of the compound. Fairly good agreement is seen between the calculated and measured values of α at U ff = 5.5 eV and U dd = 2.7 eV. The maximum power factor (PF) is found to be 47.6 (114.4)×1014 μW K −2cm−1 s −1 at 1100 K, which corresponds to p (n)-type doping of ∼1.4 (0.7)×1021 cm−3. This study suggests the importance of strong on-site electron correlation in understanding the thermoelectric property of the compound

Modulation of Kondo Behavior in a Two-Dimensional Epitaxial Bilayer Bi(111)/Fe3GeTe2 Moiré Heterostructure.

Artificial two-dimensional (2D) moiré superlattices provide a platform for generating exotic quantum matter or phenomena. Here, an epitaxial heterostructure composed of bilayer Bi(111) and an Fe3GeTe2 substrate with a zero-twist angle is acquired by molecular beam epitaxy. Scanning tunneling microscopy and spectroscopy studies reveal the spatially tailored Kondo resonance and interfacial magnetism within this moiré superlattice. Combined with first-principles calculations, it is found that the modulation effect of the moiré superlattice originates from the interfacial orbital hybridization between Bi and Fe atoms. Our work provides a tunable platform for strong electron correlation studies to explore 2D artificial heavy Fermion systems and interface magnetism.

Tiled unitary product states for strongly correlated Hamiltonians.

Approximating the electronic wave function for strongly correlated systems remains a major theoretical challenge. Emerging quantum computers can enable new types of wave-function ansatz to be considered, with the potential to overcome the exponential memory storage for strong correlation. I have recently introduced the tiled Unitary Product States (tUPS) ansatz, which successfully combines the preservation of particle-number and spin symmetry with shallow quantum circuits and local qubit connectivity [H. G. A. Burton, Phys. Rev. Res., 2024, 6, 023300]. In this contribution, I investigate the accuracy of this tUPS hierarchy for strongly-correlated Hamiltonians. I consider the picket-fence pairing Hamiltonian and the two-dimensional Hubbard lattice, which collectively describe a range of strong correlation mechanisms found in molecules. Numerical results demonstrate that highly accurate energies can be achieved with a compact approximation for both weak and strong correlation in the Hubbard model, and the repulsive pairing regime. These data provide valuable insights into the applicability of the tUPS hierarchy for strong electron correlation.

Nonadiabatic Molecular Dynamics with Fermionic Subspace-Expansion Algorithms on Quantum Computers.

We introduce a novel computational framework for excited-state molecular quantum dynamics simulations driven by quantum-computing-based electronic-structure calculations. This framework leverages the fewest-switches surface-hopping method for simulating the nuclear dynamics and calculates the required excited-state transition properties with different flavors of the quantum subspace expansion and quantum equation-of-motion algorithms. We apply our method to simulate the collision reaction between a hydrogen atom and a hydrogen molecule. For this system, we critically compare the accuracy and efficiency of different quantum subspace expansion and equation-of-motion algorithms and show that only methods that can capture both weak and strong electron correlation effects can properly describe the nonadiabatic effects that tune the reactive event.

Multiferroicity and Topology in Twisted Transition Metal Dichalcogenides.

Van der Waals heterostructures have recently emerged as an exciting platform for investigating the effects of strong electronic correlations, including various forms of magnetic or electrical orders. Here, we perform an unbiased exact diagonalization study of the effects of interactions on topological flat bands of twisted transition metal dichalcogenides (TMDs) at odd integer fillings. For hole-filling ν_{h}=1, we find that the Chern insulator phase, expected from interaction-induced spin-valley polarization of the bare bands, is quite fragile, and gives way to spontaneous multiferroic order-coexisting ferroelectricity and ferromagnetism, in the presence of long-range Coulomb repulsion. We provide a simple real-space picture to understand the phase diagram as a function of interaction range and strength. Our findings establish twisted TMDs as a novel and highly tunable platform for multiferroicity, and we outline a potential route towards electrical control of magnetism in the multiferroic phase.

Competition between d-wave superconductivity and magnetism in uniaxially strained Sr2RuO4

The pairing symmetry of Sr2RuO4 is a long-standing fundamental question in the physics of superconducting materials with strong electronic correlations. We use the functional renormalization group to investigate the behavior of superconductivity under uniaxial strain in a two-dimensional realistic model of Sr2RuO4 obtained with density functional theory and incorporating the effect of spin-orbit coupling. We find a dominant dx2−y2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${d}_{{{{{\\rm{x}}}}}^{2}-{{{{\\rm{y}}}}}^{2}}$$\\end{document} superconductor mostly hosted by the dxy-orbital, with no other closely competing superconducting state. Within this framework, we reproduce the experimentally observed enhancement of the critical temperature under strain and propose a simple mechanism driven by the density of states to explain our findings. We also investigate the competition between superconductivity and spin-density wave ordering as a function of interaction strength. By comparing theory and experiment, we discuss constraints on a possible degenerate partner of the dx2−y2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${d}_{{{{{\\rm{x}}}}}^{2}-{{{{\\rm{y}}}}}^{2}}$$\\end{document} superconducting state.

Strain-induced changes of electronic and optical properties of Zr-based MXenes

Zr-based MXenes recently attracted attention because of its experimental preparation showing temperature stability, mechanical strength, and promising energy, sensoric, and electrochemistry applications. However, necessary theoretical predictions at a precise/predictive level are complicated due to essential excitonic features and strong electron correlation (i.e., a necessity to go beyond standard density functional theory, DFT). Contrary to the prevailing focus on oxygen-terminated MXenes and standard predictions of other Zr-based MXenes as conductors, based on the hybrid DFT and GW many-body perturbational theory, we were able to find seven different semiconductors (five of them for their equilibrium geometry and two others under slight tensile biaxial strain) in the case of two- and three-layered Zr2CT2 and Zr3C2T2 configurations with various terminations (T = O, F, S, Cl). We observed semiconductor-to-conductor transition induced by strain in the majority of such Zr-based MXenes at an experimentally achievable strain range. Furthermore, using the Bethe–Salpeter equation (BSE), we demonstrated that selected semiconducting Zr-based MXenes possess high optical absorption efficiency (20%–30%) in the visible light range, underscoring their potential in photonic applications. The high sensitivity of Zr-based MXenes to external conditions and functionalization combined with the thermal stability makes the materials promising for applications at operational temperatures in electronic and optical technologies.

Toward the Next Generation of Density Functionals: Escaping the Zero-Sum Game by Using the Exact-Exchange Energy Density.

ConspectusKohn-Sham density functional theory (KS DFT) is arguably the most widely applied electronic-structure method with tens of thousands of publications each year in a wide variety of fields. Its importance and usefulness can thus hardly be overstated. The central quantity that determines the accuracy of KS DFT calculations is the exchange-correlation functional. Its exact form is unknown, or better "unknowable", and therefore the derivation of ever more accurate yet efficiently applicable approximate functionals is the "holy grail" in the field. In this context, the simultaneous minimization of so-called delocalization errors and static correlation errors is the greatest challenge that needs to be overcome as we move toward more accurate yet computationally efficient methods. In many cases, an improvement on one of these two aspects (also often termed fractional-charge and fractional-spin errors, respectively) generates a deterioration in the other one. Here we report on recent notable progress in escaping this so-called "zero-sum-game" by constructing new functionals based on the exact-exchange energy density. In particular, local hybrid and range-separated local hybrid functionals are discussed that incorporate additional terms that deal with static correlation as well as with delocalization errors. Taking hints from other coordinate-space models of nondynamical and strong electron correlations (the B13 and KP16/B13 models), position-dependent functions that cover these aspects in real space have been devised and incorporated into the local-mixing functions determining the position-dependence of exact-exchange admixture of local hybrids as well as into the treatment of range separation in range-separated local hybrids. While initial functionals followed closely the B13 and KP16/B13 frameworks, meanwhile simpler real-space functions based on ratios of semilocal and exact-exchange energy densities have been found, providing a basis for relatively simple and numerically convenient functionals. Notably, the correction terms can either increase or decrease exact-exchange admixture locally in real space (and in interelectronic-distance space), leading even to regions with negative admixture in cases of particularly strong static correlations. Efficient implementations into a fast computer code (Turbomole) using seminumerical integration techniques make such local hybrid and range-separated local hybrid functionals promising new tools for complicated composite systems in many research areas, where simultaneously small delocalization errors and static correlation errors are crucial. First real-world application examples of the new functionals are provided, including stretched bonds, symmetry-breaking and hyperfine coupling in open-shell transition-metal complexes, as well as a reduction of static correlation errors in the computation of nuclear shieldings and magnetizabilities. The newest versions of range-separated local hybrids (e.g., ωLH23tdE) retain the excellent frontier-orbital energies and correct asymptotic exchange-correlation potential of the underlying ωLH22t functional while improving substantially on strong-correlation cases. The form of these functionals can be further linked to the performance of the recent impactful deep-neural-network "black-box" functional DM21, which itself may be viewed as a range-separated local hybrid.