arXiv subjects

Thomas P. Devereaux

Publications and source records attributed to Thomas P. Devereaux.

At least 73 records · Page 4Linked to original sources

arXiv2022

Charge order and superconductivity in a minimal two-band model for infinite-layer nickelates

The recent discovery of superconductivity in infinite-layer nickelates has drawn considerable attention; however, a consensus on the fundamental building blocks and common ingredients necessary to understand and describe their ground states and emergent properties is lacking. A series of experimental and theoretical studies have suggested that an effective two-band Hubbard model with Ni 3$d_{x^2-y^2}$ and rare-earth ($R$) 5$d$ character may describe the low-energy physics. Here, we study the ground state properties of this two-band model on four-leg cylinders using the density-matrix renormalization group (DMRG) technique to better grasp whether such a simple model can embody the essential physics. A key difference compared to single-band Hubbard materials is that the system is self-doped: even at overall half-filling, the $R$-band acts as an electron reservoir, hole-doping the Ni-layer and fundamentally altering the physics expected from an undoped antiferromagnet. On the four-leg cylinder, the ground state is consistent with a Luttinger liquid, with anti-phase modulations of the charge density in the Ni- and $R$-layers having corresponding wavevectors that lock together. Light hole doping away from 1/2 filling releases the locking between the Ni and the $R$ charge modulations, as the electron density in the $R$-band decreases and eventually becomes exhausted at a hole doping concentration that depends sensitively on the effective splitting between the Ni and the $R$ orbitals. The ground state of the doped system is consistent with a Luther-Emery liquid, possessing quasi-long-range superconducting correlations in the Ni layer, similar to the single-band Hubbard model. Our results are consistent with experimental observations and may help to reveal the microscopic mechanism for pairing and other emergent properties.

cond-mat.str-el↗

arXiv2022

Rare-Earth Control of the Superconducting Upper Critical Field in Infinite-Layer Nickelates

The consequences of varying the rare-earth element in the superconducting infinite-layer nickelates have been much debated. Here we show striking differences in the magnitude and anisotropy of the superconducting upper critical field across the La-, Pr-, and Nd-nickelates. These 5 distinctions originate from the 4f electron characteristics of the rare-earth ions in the lattice: they are absent for La3+, nonmagnetic for the Pr3+ singlet ground state, and magnetic for the Nd3+ Kramer's doublet. The unique polar and azimuthal angle-dependent magnetoresistance found in the Nd-nickelates can be understood to arise from the magnetic contribution of the Nd3+ 4f moments. In the absence of rare-earth effects, we find that the nickelates broadly violate the Pauli limit. Such robust and tunable superconductivity suggests potential in future high-field applications.

cond-mat.supr-con↗

arXiv2022

Spectra of a Gapped Quantum Spin Liquid with a Strong Chiral Excitation on the Triangular Lattice

While a quantum spin liquid (QSL) phase has been identified in the $J_1$-$J_2$ Heisenberg model on a triangular lattice via numerical calculations, debate persists about whether or not such a QSL is gapped or gapless, with contradictory conclusions from different techniques. Moreover, information about excitations and dynamics is crucial for the experimental detection of such a phase. In this work, we use exact diagonalization to characterize signatures of a QSL phase on the triangular lattice through the dynamical spin structure factor $\mathcal{S}(q,ω)$ and Raman susceptibility $\mathcalχ(ω)$. We find that spectra for the QSL phase show distinct features compared to those of neighboring phases; and both the Raman spectra and spin structure factor show gapped behaviour in the QSL phase. Interestingly, there is a prominent excitation mode in the Raman $A_2$ channel, indicating a strong subleading tendency toward a chiral spin liquid phase.

cond-mat.str-el↗

arXiv2022

Magnon heat transport in a two-dimensional Mott insulator

Whether or not anomalies in the thermal conductivity in insulating cuprates can be attributed to antiferromagnetic order and magnons in a 2D Mott insulator remains an intriguing open question. To shed light on this issue, we investigate the thermal conductivity $κ$ and its relationship with the specific heat $c_v$ in the half-filled 2D single-band Hubbard model, using the numerically exact determinant quantum Monte Carlo algorithm and maximum entropy analytic continuation. At low temperatures where the charge degrees of freedom are gapped-out and $c_v$ exhibits a clear magnon peak, we observe that thermal conductivity $κ$ also tends to form a peak at similar temperatures. Reducing temperature further produces a sharp upturn in $κ$, associated with an increasing mean-free path. We identify this as the high-temperature side of the anomalous peak in insulating cuprates, where the mean-free path eventually is cut-off by other scattering effects, including phonons, disorder, and physical size. Different scattering effects in our model are identified and analyzed in the thermal diffusivity.

cond-mat.str-el↗

arXiv2022

Evidences for the exciton gas phase and its condensation in monolayer 1T-ZrTe2

The excitonic insulator (EI) is a Bose-Einstein condensation (BEC) of excitons bound by electron-hole interaction in a solid, which could support high-temperature BEC transition. The material realization of EI has been elusive, which is further challenged by the difficulty of distinguishing it from a conventional charge density wave (CDW) state. In the BEC limit, the pre-condensation exciton gas phase is a hallmark to distinguish EI from conventional CDW, yet direct experimental evidence has been lacking. Here we report a distinct correlated phase beyond the $2\times2$ CDW ground state emerging in epitaxially grown monolayer 1T-ZrTe2 and its investigation by angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM). The results show novel band- and energy-dependent folding behavior in a two-step process, evidenced by an exciton gas phase prior to its condensation into the final CDW state. The excellent agreement between experiments and theoretical predictions on the recovery of the pristine band structure by carrier-density-dependent suppression of the CDW state further corroborates the monolayer 1T-ZrTe2 as an EI. Our findings provide a versatile two-dimensional platform that allows tuning of the excitonic effect.

cond-mat.mtrl-sci↗

arXiv2022

Fluctuating intertwined stripes in the strange metal regime of the Hubbard model

Strongly correlated electron systems host a variety of poorly understood correlations in their high temperature normal state. Unlike ordered phases defined by order parameters, these normal state phases are often defined through unconventional properties such as strange metallic transport or spectroscopic pseudogaps. Characterizing the microscopic correlations in the normal state is necessary to elucidate mechanisms that lead to these properties and their connection to ground state orders. Here we establish the presence of intertwined charge and spin stripes in the strange metal normal state of the Hubbard model using determinant quantum Monte Carlo calculations. The charge and spin density waves constituting the stripes are fluctuating and short-ranged, yet they obey a mutual commensurability relation and remain microscopically interlocked, as evidenced through measurements of three-point spin-spin-hole correlation functions. Our findings demonstrate the ability of many-body numerical simulations to unravel the microscopic correlations that define quantum states of matter.

cond-mat.str-el↗

arXiv2022

Electronic structure of superconducting nickelates probed by resonant photoemission spectroscopy

The discovery of infinite-layer nickelate superconductors has spurred enormous interest. While the Ni$^{1+}$ cations possess nominally the same 3$d^9$ configuration as Cu$^{2+}$ in cuprates, the electronic structure variances remain elusive. Here, we present a soft x-ray photoemission spectroscopy study on parent and doped infinite-layer Pr-nickelate thin films with a doped perovskite reference. By identifying the Ni character with resonant photoemission and comparison to density functional theory + U (on-site Coulomb repulsion energy) calculations, we estimate U ~5 eV, smaller than the charge transfer energy $Δ$ ~8 eV, confirming the Mott-Hubbard electronic structure in contrast to charge-transfer cuprates. Near the Fermi level ($E_F$), we observe a signature of occupied rare-earth states in the parent compound, which is consistent with a self-doping picture. Our results demonstrate a correlation between the superconducting transition temperature and the oxygen 2$p$ hybridization near $E_F$ when comparing hole-doped nickelates and cuprates.

cond-mat.supr-con↗

arXiv2022

Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Towards Circular Dichroism without Circular Photons and Bloch Wavefunction Reconstruction

Angle-resolved photoemission spectroscopy (ARPES) is the most powerful technique to investigate the electronic band structure of crystalline solids. To completely characterize the electronic structure of topological materials, one needs to go beyond band structure mapping and access information about the momentum-resolved Bloch wavefunction, namely orbitals, Berry curvature, and topological invariants. However, because phase information is lost in the process of measuring photoemission intensities, retrieving the complex-valued Bloch wavefunction from photoemission data has yet remained elusive. We introduce a novel measurement methodology and associated observable in extreme ultraviolet angle-resolved photoemission spectroscopy, based on continuous modulation of the ionizing radiation polarization axis. Tracking the energy- and momentum-resolved amplitude and phase of the photoemission intensity modulation upon polarization axis rotation allows us to retrieve the circular dichroism in photoelectron angular distributions (CDAD) without using circular photons, providing direct insights into the phase of photoemission matrix elements. In case of two relevant bands, it is possible to reconstruct the orbital pseudospin (and thus the Bloch wavefunction) with moderate theory input, as demonstrated for the prototypical layered semiconducting transition metal dichalcogenide 2H-WSe$_2$. This novel measurement methodology in ARPES, which is articulated around the manipulation of the photoionization transition dipole matrix element, in combination with a simple tight-binding theory, is general and adds a new dimension to obtaining insights into the orbital pseudospin, Berry curvature, and Bloch wavefunctions of many relevant crystalline solids.

cond-mat.mtrl-sci↗

arXiv2021

On the nature of valence charge and spin excitations via multi-orbital Hubbard models for infinite-layer nickelates

Building upon the recent progress on the intriguing underlying physics for the newly discovered infinite-layer nickelates, in this article we review an examination of valence charge and spin excitations via multi-orbital Hubbard models as way to determine the fundamental building blocks for Hamiltonians that can describe the low energy properties of infinite-layer nickelates. We summarize key results from density-functional approaches, and apply them to the study of x-ray absorption to determine the valence ground states of infinite-layer nickelates in their parent form, and show that a fundamental $d^9$ configuration as in the cuprates is incompatible with a self-doped ground state having holes in both $d_{x^2-y^2}$ and a rare-earth-derived axial orbital. When doped, we determine that the rare-earth-derived orbitals empty and additional holes form low spin $(S=0)$ $d^8$ Ni states, which can be well-described as a doped single-band Hubbard model. Using exact diagonalization for a 2-orbital model involving Ni and rare earth orbitals, we find clear magnons at 1/2 filling that persist when doped, albeit with larger damping, and with a dependence on the precise orbital energy separation between the Ni- and rare-earth-derived orbitals. Taken together, a full two-band model for infinite-layer nickelates can well describe the valence charge and spin excitations observed experimentally.

cond-mat.supr-con↗

arXiv2021

Sign-Free Determinant Quantum Monte Carlo Study of Excitonic Density Orders in a Two-Orbital Hubbard-Kanamori Model

While excitonic instabilities in multiorbital systems recently have come under scrutiny in a variety of transition-metal compounds, understanding emergence of these instabilities from strong electronic interactions has remained a challenge. Here, we present a sign-problem-free determinant quantum Monte Carlo study of excitonic density orders in a half-filled two-orbital Hubbard-Kanamori model with broken orbital degeneracy, which accounts for the role of Hund's coupling in transition-metal compounds. For strong inverted (negative) Hund's exchange, we find numerical evidence for the emergence of excitonic density order, with competition between anti-ferro-orbital order and $\mathbf{Q} = (π,π)$ excitonic density order as a function of orbital splitting and Hund's coupling. While inverted Hund's coupling stabilizes a spin-singlet excitonic density phase for weak orbital splitting, positive Hund's coupling favors a spin-triplet excitonic density phase.

cond-mat.str-el↗

arXiv2021

A Broken Translational Symmetry State in an Infinite-Layer Nickelate

A defining signature of strongly correlated electronic systems is the existence of competing phases with similar ground state energies, resulting in a rich phase diagram. While in the recently discovered nickelate superconductors, a high antiferromagnetic exchange energy has been reported, which implies the existence of strong electronic correlations, signatures of competing phases have not yet been observed. Here, we uncover a charge order (CO) in infinite-layer nickelates La1-xSrxNiO2 using resonant x-ray scattering across the Ni L-edge. In the parent compound, the CO arranges along the Ni-O bond direction with an incommensurate wave vector (0.344+/-0.002, 0) r.l.u., distinct from the stripe order in other nickelates which propagates along a direction 45 degree to the Ni-O bond. The CO resonance profile indicates that CO originates from the Ni 3d states and induces a parasitic charge modulation of La electrons. Upon doping, the CO diminishes and the ordering wave vector shifts toward a commensurate value of 1/3 r.l.u., indicating that the CO likely arises from strong correlation effects and not from Fermi surface nesting.

cond-mat.supr-con↗

arXiv2021

Orbitally Selective Resonant Photodoping to Enhance Superconductivity

Signatures of superconductivity at elevated temperatures above $T_c$ in high temperature superconductors have been observed near 1/8 hole doping for photoexcitation with infrared or optical light polarized either in the CuO$_2$-plane or along the $c$-axis. While the use of in-plane polarization has been effective for incident energies aligned to specific phonons, $c$-axis laser excitation in a broad range between 5 $μ$m and 400 nm was found to affect the superconducting dynamics in striped La$_{1.885}$Ba$_{0.115}$CuO$_4$, with a maximum enhancement in the $1/ω$ dependence to the conductivity observed at 800 nm. This broad energy range, and specifically 800 nm, is not resonant with any phonon modes, yet induced electronic excitations appear to be connected to superconductivity at energy scales well above the typical gap energies in the cuprates. A critical question is what can be responsible for such an effect at 800 nm? Using time-dependent exact diagonalization, we demonstrate that the holes in the CuO$_2$ plane can be photoexcited into the charge reservoir layers at resonant wavelengths within a multi-band Hubbard model. This orbitally selective photoinduced charge transfer effectively changes the in-plane doping level, which can lead to an enhancement of $T_c$ near the 1/8 anomaly.

cond-mat.supr-con↗

arXiv2021

Phonon-Mediated Long-Range Attractive Interaction in One-Dimensional Cuprates

Establishing a minimal microscopic model for cuprates is a key step towards the elucidation of a high-$T_c$ mechanism. By a quantitative comparison with a recent \emph{in situ} angle-resolved photoemission spectroscopy measurement in doped 1D cuprate chains, our simulation identifies a crucial contribution from long-range electron-phonon coupling beyond standard Hubbard models. Using reasonable ranges of coupling strengths and phonon energies, we obtain a strong attractive interaction between neighboring electrons, whose strength is comparable to experimental observations. Nonlocal couplings play a significant role in the mediation of neighboring interactions. Considering the structural and chemical similarity between 1D and 2D cuprate materials, this minimal model with long-range electron-phonon coupling will provide important new insights on cuprate high-$T_C$ superconductivity and related quantum phases.

cond-mat.str-el↗

arXiv2021

X-Ray Scattering from Light-Driven Spin Fluctuations in a Doped Mott Insulator

Manipulating spin fluctuations with ultrafast laser pulses is a promising route to dynamically control collective phenomena in strongly correlated materials. However, understanding how photoexcited spin degrees of freedom evolve at a microscopic level requires a momentum- and energy-resolved characterization of their nonequilibrium dynamics. Here, we study the photoinduced dynamics of finite-momentum spin excitations in two-dimensional Mott insulators on a square lattice. By calculating the time-resolved resonant inelastic x-ray scattering cross-section, we show that an ultrafast pump above the Mott gap induces a prompt softening of the spin excitation energy, compatible with a transient renormalization of the exchange interaction. While spin fluctuations in a hole-doped system (paramagnons) are well described by Floquet theory, magnons at half filling are found to deviate from this picture. Furthermore, we show that the paramagnon softening is accompanied by an ultrafast suppression of $d$-wave pairing correlations, indicating a link between the transient spin excitation dynamics and superconducting pairing far from equilibrium.

cond-mat.str-el↗

arXiv2021

Numerical approaches for calculating the low-field dc Hall coefficient of the doped Hubbard model

Using determinant Quantum Monte Carlo, we compare three methods of evaluating the dc Hall coefficient $R_H$ of the Hubbard model: the direct measurement of the off-diagonal current-current correlator $χ_{xy}$ in a system coupled to a finite magnetic field (FF), $χ_{xy}^{\text{FF}}$; the three-current linear response to an infinitesimal field as measured in the zero-field (ZF) Hubbard Hamiltonian, $χ_{xy}^{\text{ZF}}$; and the leading order of the recurrent expansion $R_H^{(0)}$ in terms of thermodynamic susceptibilities. The two quantities $χ_{xy}^{\text{FF}}$ and $χ_{xy}^{\text{ZF}}$ can be compared directly in imaginary time. Proxies for $R_H$ constructed from the three-current correlator $χ_{xy}^{\text{ZF}}$ can be determined under different simplifying assumptions and compared with $R_H^{(0)}$. We find these different quantities to be consistent with one another, validating previous conclusions about the close correspondence between Fermi surface topology and the sign of $R_H$, even for strongly correlated systems. These various quantities also provide a useful set of numerical tools for testing theoretical predictions about the full behavior of the Hall conductivity for strong correlations.

cond-mat.str-el↗

arXiv2021

Anomalously Strong Near-Neighbor Attraction in Doped 1D Cuprate Chains

In the cuprates, one-dimensional chain compounds provide a unique opportunity to understand the microscopic physics due to the availability of reliable theories. However, progress has been limited by the inability to controllably dope these materials. Here, we report the synthesis and spectroscopic analysis of the one-dimensional cuprate Ba$_{2-x}$Sr$_x$CuO$_{3+δ}$ over a wide range of hole doping. Our angle-resolved photoemission experiments reveal the doping evolution of the holon and spinon branches. We identify a prominent folding branch whose intensity fails to match predictions of the simple Hubbard model. An additional strong near-neighbor attraction, which may arise from coupling to phonons, quantitatively explains experiments for all accessible doping levels. Considering structural and quantum chemistry similarities among cuprates, this attraction will play a similarly crucial role in the high-$T_C$ superconducting counterparts

cond-mat.str-el↗

arXiv2021

Evolution of the electronic structure in Ta$_2$NiSe$_5$ across the structural transition revealed by resonant inelastic x-ray scattering

We utilized high-energy-resolution resonant inelastic X-ray scattering (RIXS) at both the Ta and Ni $L_3$-edges to map out element-specific particle-hole excitations in Ta$_2$NiSe$_5$ across the phase transition. Our results reveal a momentum dependent gap-like feature in the low energy spectrum, which agrees well with the band gap in element-specific joint density of states calculations based on ab initio estimates of the electronic structure in both the low temperature monoclinic and the high temperature orthorhombic structure. Below $T_c$, the RIXS energy-momentum map shows a minimal gap at the Brillouin zone center ($\sim$ 0.16 eV), confirming that Ta$_2$NiSe$_5$ possesses a direct band gap in its low temperature ground state. However, inside the gap, no signature of anticipated collective modes with an energy scale comparable to the gap size can be identified. Upon increasing the temperature to above $T_c$, whereas the gap at the zone center closes, the RIXS map at finite momenta still possesses the gross features of the low temperature map, suggesting a substantial mixing between the Ta and Ni orbits in the conduction and valence bands, which does not change substantially across the phase transition. Our experimental observations and comparison to the theoretical calculations lend further support that the phase transition and the corresponding gap opening in Ta$_2$NiSe$_5$ is largely structural by nature with possible minor contribution from the putative exciton condensate.

cond-mat.str-el↗

arXiv2021

Self-energy dynamics and mode-specific phonon threshold effect in a Kekulé-ordered graphene

Electron-phonon interaction and related self-energy are fundamental to both the equilibrium properties and non-equilibrium relaxation dynamics of solids. Although electron-phonon interaction has been suggested by various time-resolved measurements to be important for the relaxation dynamics of graphene, the lack of energy- and momentum-resolved self-energy dynamics prohibits direct identification of the role of specific phonon modes in the relaxation dynamics. Here by performing time- and angle-resolved photoemission spectroscopy measurements on a Kekulé-ordered graphene with folded Dirac cones at the $Γ$ point, we have succeeded in resolving the self-energy effect induced by coupling of electrons to two phonons at $Ω_1$ = 177 meV and $Ω_2$ = 54 meV and revealing its dynamical change in the time domain. Moreover, these strongly coupled phonons define energy thresholds, which separate the hierarchical relaxation dynamics from ultrafast, fast to slow, thereby providing direct experimental evidence for the dominant role of mode-specific phonons in the relaxation dynamics

cond-mat.mes-hall↗