arXiv subjects
Publications and source records attributed to A. J. Millis.
We use a numerical solution of the deterministic TDGL equations to determine the response induced by a probe field in a material quenched into a superconducting state. We characterize differences in response according to whether the probe is applied before, during, or after the phase stiffness has built up to its final steady state value.
We show that charge ordering (more precisely, two-sublattice bond disproportionation) in the rare earth nickelate perovskites is intimately related to a negative charge transfer energy. By adding an additional potential on the Ni d states we are able to vary the charge tranfer energy and compute relaxed structures within an ab-initio framework. We show that the difference in Ni-O bond lengths and the value of the ordered state magnetic moment correlate with the charge transfer energy and that the transition to the bond-disproportionated state occurs when the effective charge transfer energy becomes negative.
The electronic structure of transition metal oxides featuring correlated electrons can be rationalized within the Zaanen-Sawatzky-Allen framework. Following a brief description of the present paradigms of electronic behavior, we focus on the physics of rare earth nickelates as an archetype of complexity emerging within the charge transfer regime. The intriguing prospect of realizing the physics of high $T_c$ cuprates through heterostructuring resulted in a massive endeavor to epitaxially stabilize these materials in ultra-thin form. A plethora of new phenomena unfolded in such artificial structures due to the effect of epitaxial strain, quantum confinement, and interfacial charge transfer. Here we review the present status of artificial rare-earth nickelates in an effort to uncover the interconnection between the electronic and magnetic behavior and the underlying crystal structure. We conclude by discussing future directions to disentangle the puzzle regarding the origin of the metal-insulator transition, the role of oxygen holes, and the true nature of the antiferromagnetic spin configuration in the ultra-thin limit.
We define the entropy operator as the negative of the logarithm of the density matrix, give a prescription for extracting its thermodynamically measurable part, and discuss its dynamics. For an isolated system we derive the first, second and third laws of thermodynamics. For weakly-coupled subsystems of an isolated system, an expression for the long time limit of the expectation value of the rate of change of the thermodynamically measurable part of the entropy operator is derived and interpreted in terms of entropy production and entropy transport terms. The interpretation is justified by comparison to the known expression for the entropy production in an aged classical Markovian system with Gaussian fluctuations and by a calculation of the current-induced entropy production in a conductor with electron-phonon scattering.
The electronic correlation strength is a basic quantity that characterizes the physical properties of materials such as transition metal oxides. Determining correlation strengths requires both precise definitions and a careful comparison between experiment and theory. In this paper we define the correlation strength via the magnitude of the electron self-energy near the Fermi level. For the case of LaNiO$_3$, we obtain both the experimental and theoretical mass enhancements $m^\star/m$ by considering high resolution angle-resolved photoemission spectroscopy (ARPES) measurements and density functional + dynamical mean field theory (DFT + DMFT) calculations. We use valence-band photoemission data to constrain the free parameters in the theory, and demonstrate a quantitative agreement between the experiment and theory when both the realistic crystal structure and strong electronic correlations are taken into account. These results provide a benchmark for the accuracy of the DFT+DMFT theoretical approach, and can serve as a test case when considering other complex materials. By establishing the level of accuracy of the theory, this work also will enable better quantitative predictions when engineering new emergent properties in nickelate heterostructures.
We present density functional plus dynamical mean field studies of cubic BaRuO$_3$ using interaction parameters previously found to be appropriate for the related materials CaRuO$_3$ and SrRuO$_3$. The calculated variation in transition temperature between the Ba and Sr compounds is consistent with experiment, confirming the assignment of the compounds to the Hund's metal family of materials, and also confirming the appropriateness of the values for the interaction parameters previously estimated and the appropriateness of the single-site dynamical mean field approximation for these materials. The results provide insights into the origin of magnetism and the role of the van Hove singularity in the physics of Hund's metals.
We give a detailed comparison of the hierarchical quantum master equation (HQME) method to a continuous-time quantum Monte Carlo (CT-QMC) approach, assessing the usability of these numerically exact schemes as impurity solvers in practical nonequilibrium calculations. We review the main characteristics of the methods and discuss the scaling of the associated numerical effort. We substantiate our discussion with explicit numerical results for the nonequilibrium transport properties of a single-site Anderson impurity. The numerical effort of the HQME scheme scales linearly with the simulation time but increases (at worst exponentially) with decreasing temperature. In contrast, CT-QMC is less restricted by temperature at short times, but in general the cost of going to longer times is also exponential. After establishing the numerical exactness of the HQME scheme, we use it to elucidate the influence of different ways to induce transport through the impurity on the initial dynamics, discuss the phenomenon of coherent current oscillations, known as current ringing, and explain the non-monotonic temperature dependence of the steady-state magnetization as a result of competing broadening effects. We also elucidate the pronounced non-linear magnetization dynamics, which appears on intermediate time scales in the presence of an asymmetric coupling to the electrodes.
We theoretically investigate the full time evolution of a nonequilibrium double quantum dot structure from initial conditions corresponding to different product states (no entanglement between dot and lead) to a nonequilibrium steady state. The structure is described by a two-level spinless Anderson model where the levels are coupled to two leads held at different chemical potentials. The problem is solved by a numerically exact hierarchical master equation technique and the results are compared to approximate ones obtained from Born-Markov theory. The methods allow us to study the time evolution up to times of order $10^4$ of the bare hybridization time, enabling eludication of the role of the initial state on the transient dynamics, coherent charge oscillations and an interaction-induced renormalization of energy levels. We find that when the system carries a single electron on average the formation of the steady state is strongly influenced by the coherence between the dots. The latter can be sizeable and indeed larger in the presence of a bias voltage than it is in equilibrium. Moreover, the interdot coherence is shown to lead to a pronounced difference in the population of the dots.
We show that a small number of intentionally introduced defects can be used as a spectroscopic tool to amplify quasiparticle interference in 2H-NbSe$_{2}$, that we measure by scanning tunneling spectroscopic imaging. We show from the momentum and energy dependence of the quasiparticle interference that Fermi surface nesting is inconsequential to charge density wave formation in 2H-NbSe$_{2}$. We demonstrate that by combining quasiparticle interference data with additional knowledge of the quasiparticle band structure from angle resolved photoemission measurements, one can extract the wavevector and energy dependence of the important electronic scattering processes thereby obtaining direct information both about the fermiology and the interactions. In 2H-NbSe$_{2}$, we use this combination to show that the important near-Fermi-surface electronic physics is dominated by the coupling of the quasiparticles to soft mode phonons at a wave vector different from the CDW ordering wave vector.
The interplay between interference effects and electron-electron interactions in electron transport through an interacting double quantum dot system is investigated using a hierarchical quantum master equation approach which becomes exact if carried to infinite order and converges well if the temperature is not too low. Decoherence due to electron-electron interactions is found to give rise to pronounced negative differential resistance, enhanced broadening of structures in current-voltage characteristics and an inversion of the electronic population. Dependence on gate voltage is shown to be a useful method of distinguishing decoherence-induced phenomena from effects induced by other mechanisms such as the presence of a blocking state. Comparison of results obtained by the hierarchical quantum master equation approach to those obtained from the Born-Markov approximation to the Nakajima-Zwanzig equation and from the non-crossing approximation to the nonequilibrium Green's function reveals the importance of an inter-dot coupling that originates from the energy dependence of the conduction bands in the leads and the need for a systematic perturbative expansion.
The driving forces behind electronic nematicity in the iron pnictides remain hotly debated. We use atomic-resolution variable-temperature scanning tunneling spectroscopy to provide the first direct visual evidence that local electronic nematicity and unidirectional antiferroic (stripe) fluctuations persist to temperatures almost twice the nominal structural ordering temperature in the parent pnictide NaFeAs. Low-temperature spectroscopic imaging of nematically-ordered NaFeAs shows anisotropic electronic features that are not observed for isostructural, non-nematic LiFeAs. The local electronic features are shown to arise from scattering interference around crystalline defects in NaFeAs, and their spatial anisotropy is a direct consequence of the structural and stripe-magnetic order present at low temperature. We show that the anisotropic features persist up to high temperatures in the nominally tetragonal phase of the crystal. The spatial distribution and energy dependence of the anisotropy at high temperatures is explained by the persistence of large amplitude, short-range, unidirectional, antiferroic (stripe) fluctuations, indicating that strong density wave fluctuations exist and couple to near-Fermi surface electrons even far from the structural and density wave phase boundaries.
We report the direct observation in real space of the charge density wave (CDW) phase transition in pristine 2H-NbSe2 using atomic-resolution scanning tunneling microscopy (STM). We find that static CDW order is established in nanoscale regions in the vicinity of defects at temperatures that are several times the bulk transition temperature Tcdw. On lowering the temperature, the correlation length of these patches increases steadily until CDW order is established in all of space, demonstrating the crucial role played by defects in the physics of the transition region. The nanoscale CDW order has an energy and temperature-independent wavelength. Spectroscopic imaging measurements of the real-space phase of the CDW indicate that an energy gap in NbSe2 occurs at 0.7eV below the Fermi energy in the CDW phase, suggesting that strong electron-lattice interactions and not Fermi surface physics is the dominant cause for CDW formation in NbSe2.
We review our studies of the effect of transverse fields on the susceptibility and magnetization of single crystals of the prototype single molecule magnet (SMM), Mn$_{12}$-acetate, and of a new high-symmetry variant, Mn$_{12}$-acetate-MeOH. SMM single crystals can exhibit long range ferromagnetic order associated with intermolecular dipole interactions. Transverse fields increase quantum spin fluctuation and quantum tunneling of the magnetization suppressing long range order. However, we have found that suppression of the Curie temperature by a transverse field in Mn$_{12}$-acetate is far more rapid than predicted by the Transverse-Field Ising Ferromagnetic Model (TFIFM). It appears that solvent disorder in Mn$_{12}$-acetate that results in an intrinsic distribution of small discrete tilts of the molecular magnetic easy axis from the global easy axis of the crystal ($\approx \pm 1^\circ$) gives rise to a distribution of random-fields that further suppresses long-range order. Semiquantitative agreement with the predictions of a Random-Field Ising Ferromagnet Model is found. Subsequent susceptibility studies we have conducted of the high symmetry Mn$_{12}$ variant, Mn$_{12}$-acetate-MeOH, with the same spin structure and similar lattice constants but without the same solvent disorder as Mn$_{12}$-acetate, agrees with the TFIFM. An important implication of our studies is that long-range order in these two chemically very similar SMMs are described by distinct physical models.
Dynamical mean field methods are used to calculate the phase diagram, many-body density of states, relative orbital occupancy and Fermi surface shape for a realistic model of $LaNiO_3$-based superlattices. The model is derived from density functional band calculations and includes oxygen orbitals. The combination of the on-site Hunds interaction and charge-transfer between the transition metal and the oxygen orbitals is found to reduce the orbital polarization far below the levels predicted either by band structure calculations or by many-body analyses of Hubbard-type models which do not explicitly include the oxygen orbitals. The findings indicate that heterostructuring is unlikely to produce one band model physics and demonstrate the fundamental inadequacy of modeling the physics of late transition metal oxides with Hubbard-like models.
We provide a prescription for constructing Hamiltonians representing the low energy physics of correlated electron materials with dynamically screened Coulomb interactions. The key feature is a renormalization of the hopping and hybridization parameters by the processes that lead to the dynamical screening. The renormalization is shown to be non-negligible for various classes of correlated electron materials. The bandwidth reduction effect is necessary for connecting models to materials behavior and for making quantitative predictions for low-energy properties of solids.
We report measurements of the magnetic susceptibility of single crystals of Mn$_{12}$-acetate-MeOH, a new high-symmetry variant of the original single molecule magnet Mn$_{12}$-acetate. A comparison of these data to theory and to data for the Mn$_{12}$ acetate material shows that Mn$_{12}$-acetate-MeOH is a realization of a transverse-field Ising ferromagnet in contrast to the original Mn$_{12}$ acetate material, in which solvent disorder leads to effects attributed to random field Ising ferromagnetism.
We study the one-dimensional two-orbital Hubbard model with general local interactions including a pair-hopping term. The model might be realized in one-dimensional transition-metal nanowires. Phase diagrams at T=0 are obtained by numerical integration of renormalization group equations and bosonization. Particular attention is paid to the effects of orbital degeneracy (or near-degeneracy), interactions favoring locally high-spin configurations, and velocity differences. Dynamical symmetry enlargement and duality approaches are employed to determine ground states and to understand quantum phase transitions between them. An important result is that the pair-hopping term and associated orbital symmetry can lead to new insulating states. The ground state for spin-polarized case is also discussed.
We used the Hartree-Fock approximation to classify the electronic phases that might occur in a transition metal nanowire. The important features of this situation are orbital degeneracy (or near-degeneracy) and interactions favoring locally high-spin configurations. In this circumstance, spin density wave and triplet superconductivity states are favored. If the interactions favor locally low-spin configurations as in the previously studied spin ladder systems, orbital density wave and singlet superconductivity are observed.