arXiv subjects

Tim O. Wehling

Publications and source records attributed to Tim O. Wehling.

At least 19 recordsLinked to original sources

arXiv2025

Theory of intervalley-coherent AFM order and topological superconductivity in tWSe$_2$

The recent observation of superconductivity in the vicinity of Fermi surface reconstructed insulating or metallic states has established twisted bilayers of WSe\textsubscript{2} as an exciting platform to study the interplay of strong electron-electron interactions, broken symmetries and topology. In this work, we use a first-principles, material-specific theoretical treatment that is unbiased with respect to electronic instabilities to study the emergence of electronic ordering in twisted WSe\textsubscript{2} driven by gate-screened Coulomb interactions. We construct exponentially localized moiré Wannier orbitals that faithfully capture the bandstructure and topology of the system, project the gate-screened Coulomb interaction onto them and use unbiased functional renormalization group techniques to resolve the momentum and orbital structure of the leading instabilities and the relevant energy scales. We find an interplay between intervalley-coherent antiferromagnetic (IVC-AFM) order and chiral, mixed-parity $d/p$-wave superconductivity for carrier concentrations near a displacement field and twist-angle-tunable van-Hove singularity. Our microscopic approach establishes incommensurate IVC-AFM spin fluctuations as the dominant electronic mechanism driving the formation of superconductivity in $θ= 5.08^{\circ}$ twisted WSe\textsubscript{2} and explains key aspects of recent experiments including the asymmetric density dependence of the spin ordering with respect to the van-Hove line, the single and double-peak structure of the DOS in the ordered (hole-doped) IVC-AFM phase, the emergence of superconductivity as the density is varied across the van-Hove line and the evolution of the displacement field-density phase diagram with twist angles between $3.7^{\circ} \dots 5^{\circ}$.

cond-mat.str-el↗

arXiv2025

Obtaining the Spectral Function of Moiré Graphene Heavy-Fermions Using Iterative Perturbation Theory

The spectral functions of twisted bilayer graphene (TBG) in the absence of strain have recently been investigated in both the symmetric and symmetry-broken phases using dynamical mean-field theory (DMFT). The theoretically predicted Mott-Hubbard bands and gapless semimetallic state at half-filling have since been confirmed experimentally. Here, we develop several second-order perturbation theory approaches to the topological heavy-fermion (THF) model of TBG and twisted symmetric trilayer graphene (TSTG). In the symmetric phase, we adapt, implement, and benchmark an iterative perturbation theory (IPT) impurity solver within DMFT, enabling computationally efficient yet accurate spectral function calculations. We present momentum- and energy-resolved spectra over a broad range of temperatures and fillings for both symmetric and symmetry-broken states. In addition, we derive analytic expressions for the spectral function within the ``Hubbard-I'' approximation of the THF model and, as expected, find that while it provides a tractable description of Mott physics, it does not capture the low-energy Kondo peak or the finite lifetime broadening of the bands. Our methodology can be extended to include strain, lattice relaxation, and parameter variations, thereby allowing systematic predictions of TBG and TSTG spectral properties across a wide range of physical regimes. Because our perturbative approaches are far less computationally intensive than DMFT with numerically exact impurity solvers, they can be used to efficiently benchmark and scan extensive phase diagrams of the THF parameters, paving the way for full DMFT analyses of the TBG spectral function in the presence of strain and relaxation.

cond-mat.str-el↗

arXiv2025

Flat band excitons in a three-dimensional supertwisted spiral transition metal dichalcogenide

A new frontier in van der Waals twistronics is the development of three-dimensional (3D) supertwisted materials, where each successive atomic layer rotates by the same angle. While two-dimensional (2D) moire systems have been extensively studied, the unique phenomena arising from 3D twistronics remain largely unexplored. In this work, we report the discovery of flat-band excitons in 3D supertwisted WS2, revealed by systematic photoluminescence (PL) experiments and electronic structure calculations. These excitons retain key features of 2D moire transition metal dichalcogenides (TMDs)-such as layer confinement, moire-driven localization, and strong Coulomb interactions-while also offering advantages in scalability and enhanced optical responses in three dimensions. Beyond the PL signatures reminiscent of 2D A excitons, we observe novel direct and indirect exciton emission uniquely tied to the supertwist geometry. Using generalized Bloch band theory and local density of states calculations that incorporate screw rotational symmetry, we uncovered the coexistence of 2D and 3D flatband gaps. These flat-band excitons serve as sensitive probes of the electronic properties of 3D supertwisted semiconductors and open new pathways for applications in quantum optoelectronics.

physics.app-ph↗

arXiv2025

Site-polarized Mott phases competing with a correlated metal in twisted WSe$_2$

Twisted WSe$_2$ hosts superconductivity, metal-insulator phase transitions, and field-controllable Fermi-liquid to non-Fermi-liquid transport properties. In this work, we use dynamical mean-field theory to provide a coherent understanding of the electronic correlations shaping the twisted WSe$_2$ phase diagram. We find a correlated metal competing with three distinct site-polarized correlated insulators; the competition is controlled by interlayer potential difference and interaction strength. The insulators are characterized by a strong differentiation between orbitals with respect to carrier concentration and effective correlation strength. Upon doping, a strong particle-hole asymmetry emerges, resulting from a Zaanen-Sawatzky-Allen-type charge-transfer mechanism. The associated charge-transfer physics and proximity to a van Hove singularity in the correlated metal sandwiched between two site-polarized insulators naturally explains the interlayer potential-driven metal-to-insulator transition, particle-hole asymmetry in transport, and the coherence-incoherence crossover in $3.65^\circ$ twisted WSe$_2$.

cond-mat.str-el↗

arXiv2025

Superconductivity governed by Janus-faced fermiology in strained bilayer nickelates

High-temperature superconductivity in pressurized and strained bilayer nickelates (La,Pr)$_3$Ni$_2$O$_7$ has emerged as a new frontier. One of the key unresolved issues concerns the fermiology that underlies superconductivity. On both theoretical and experimental sides, no general consensus has been reached, and conflicting results exist regarding whether the relevant Fermi surface involves a $\gamma$ pocket -- a hole pocket with $d_{z^2}$-orbital character centered at the Brillouin zone corner. Here, we address this issue by unveiling a Janus-faced role of the $\gamma$ pocket in spin-fluctuation-mediated superconductivity. We show that this pocket simultaneously induces dominant pair-breaking and pair-forming channels for the leading $s_\pm$-wave pairing. Consequently, an optimal superconducting transition temperature $T_\mathrm{c}$ is achieved when the $\gamma$ pocket surfaces at the Fermi level, placing the system near a Lifshitz transition. This suggests that superconductivity can emerge, provided the maximum energy level of the $\gamma$ pocket lies sufficiently close to the Fermi level, either from below or above. Our finding not only reconciles two opposing viewpoints on the fermiology, but also naturally explains recent experiments on (La,Pr)$_3$Ni$_2$O$_7$ thin films, including the superconductivity under compressive strain, two conflicting measurements on the Fermi surface, and the dome shape of $T_\mathrm{c}$ as a function of hole doping.

cond-mat.supr-con↗

arXiv2025

Phonon fluctuation diagnostics: Origin of charge order in AV$_3$Sb$_5$ kagome metals

The microsopic origin of the charge-density wave (CDW) in AV$_3$Sb$_5$ (A = K, Rb, Cs) kagome metals remains a longstanding question, often revolving around electron-phonon coupling and purely electronic mechanisms involving Van Hove scenarios, nesting, and sublattice interference. To reveal the processes driving the CDW transition, we combine ab-initio calculations analysis of the phonon self-energy and angle-resolved photoemission spectroscopy (ARPES). Our momentum-resolved study, supported by ARPES data, reveals that lattice instabilities in the V-135 family of kagome metals appear to also be driven by electronic states far from high-symmetry points, where these states exhibit the strongest coupling with the phonon modes responsible for the CDW distortion. Footing on an interpretation scheme based on phonon fluctuation diagnostics, our work challenges and revises theories that so far have exclusively attributed CDW formation to nesting effects close to the Fermi level.

cond-mat.str-el↗

arXiv2025

Real-Space Switching of Local Moments Driven by Quantum Geometry in Correlated Graphene Heterostructures

Graphene-based multilayer systems serve as versatile platforms for exploring the interplay between electron correlation and topology, thanks to distinctive low-energy bands marked by significant quantum metric and Berry curvature from graphene's Dirac bands. Here, we investigate Mott physics and local spin moments in Dirac bands hybridized with a flat band of localized orbitals in functionalized graphene. Via hybridization control, a topological transition is realized between two symmetry-distinct site-selective Mott states featuring local moments in different Wyckoff positions, with a geometrically enforced metallic state emerging in between. We find that this geometrically controlled real-space switching of local moments and associated metal-insulator physics may be realized through proximity coupling of epitaxial graphene on SiC(0001) with group IV intercalants, where the Mott state faces geometrical obstruction in the large-hybridization limit. Our work shows that chemically functionalized graphene provides a correlated electron platform, very similar to the topological heavy fermions in graphene moir\'e systems but at significantly enhanced characteristic energy scales.

cond-mat.str-el↗

arXiv2024

Ultrafast pseudomagnetic fields from electron-nuclear quantum geometry

Recent experiments demonstrate precise control over coherently excited circular phonon modes using high-intensity terahertz lasers, opening new pathways towards dynamical, ultrafast design of magnetism in functional materials. While the phonon Zeeman effect enables a theoretical description of phonon-induced magnetism, it lacks efficient angular momentum transfer from the phonon to the electron sector. In this work, we put forward a coupling mechanism based on electron-nuclear quantum geometry, with the inverse Faraday effect as a limiting case. This effect is rooted in the phase accumulation of the electronic wavefunction under a circular evolution of nuclear coordinates. An excitation pulse then induces a transient level splitting between electronic orbitals that carry angular momentum. First-principle simulations on SrTiO$_3$ demonstrate that in parts of the Brillouin zone, this splitting between orbitals carrying angular momentum can easily reach 50 meV.

cond-mat.mtrl-sci↗

arXiv2024

Bypassing the lattice BCS-BEC crossover in strongly correlated superconductors: resilient coherence from multiorbital physics

Superconductivity emerges from the spatial coherence of a macroscopic condensate of Cooper pairs. Increasingly strong binding and localization of electrons into these pairs compromises the condensate's phase stiffness, thereby limiting critical temperatures -- a phenomenon known as the BCS-BEC crossover in lattice systems. In this study, we demonstrate enhanced superconductivity in a multiorbital model of alkali-doped fullerides (A$_3$C$_{60}$) that goes beyond the limits of the lattice BCS-BEC crossover. We identify that the interplay of strong correlations and multiorbital effects results in a localized superconducting state characterized by a short coherence length but robust stiffness and a domeless rise in critical temperature with increasing pairing interaction. To derive these insights, we introduce a new theoretical framework allowing us to calculate the fundamental length scales of superconductors, namely the coherence length ($ξ_0$) and the London penetration depth ($λ_{\mathrm{L}}$), even in presence of strong electron correlations.

cond-mat.str-el↗

arXiv2024

k-resolved ultrafast light-induced band renormalization in monolayer WS$_2$ on graphene

Understanding and controlling the electronic properties of two-dimensional materials is crucial for their potential applications in nano- and optoelectronics. Monolayer transition metal dichalcogenides such as WS$_2$ have garnered significant interest due to their strong light-matter interaction and extreme sensitivity of the band structure to the presence of photogenerated electron-hole pairs. In this study, we investigate the transient electronic structure of monolayer WS$_2$ on a graphene substrate after resonant excitation of the A-exciton using time- and angle-resolved photoemission spectroscopy. We observe a pronounced band structure renormalization including a substantial reduction of the transient band gap that is in good quantitative agreement with our {\it ab initio} theory that reveals the importance of both intrinsic WS$_2$ and extrinsic substrate contributions to the transient band structure of monolayer WS$_2$. Our findings not only deepen the fundamental understanding of band structure dynamics in two-dimensional materials but also offer valuable insights for the development of novel electronic and optoelectronic devices based on monolayer TMDs and their heterostructures with graphene.

cond-mat.mtrl-sci↗

arXiv2024

Non-equilibrium carrier dynamics and band structure of graphene on 2D tin

Intercalation of epitaxial graphene on SiC(0001) with Sn results in a well-ordered Sn $(1\times1)$ structure on the SiC surface with quasi-freestanding graphene on top. While the electronic properties of the individual layers have been studied in the past, emerging phenomena arising from possible inter-layer interactions between the 2D\,Sn layer and graphene remain unexplored. We use time- and angle-resolved photoemission spectroscopy to reveal a surprisingly short-lived non-equilibrium carrier distribution inside the Dirac cone of Sn-intercalated graphene. Further, we find that the graphene $π$-band exhibits a transient increase in binding energy that we attribute to charging of the graphene layer with holes. We interpret our results with support from density functional theory calculations of the graphene - 2D\,Sn heterostructure that reveal a substantial hybridization between the graphene $π$-bands and Sn states, providing a channel for efficient ultrafast charge transfer between the layers. Our results on the graphene - 2D\,Sn model system are expected to trigger similar investigations on related heterostructures obtained by intercalation of epitaxial graphene. Regarding the huge choice of materials that have been successfully intercalated in the past, we believe that the interlayer interactions revealed in the present work only represent the tip of the iceberg with many fascinating emerging phenomena to be discovered in the near future.

cond-mat.mes-hall↗

arXiv2024

Electronic correlations in epitaxial graphene: Mott states proximitized to a relativistic electron gas

Graphene, renowned for its exceptional electronic and optical properties as a robust 2D material, traditionally lacks electronic correlation effects. Proximity coupling offers a promising method to endow quantum materials with novel properties. In this study, we achieve such a proximity coupling by intercalating Sn between the buffer layer of graphene on SiC(0001), allowing us to explore the coupling between a correlated 2D electron gas and a Dirac metal. This results in the stabilization of Sn-$\sqrt{3}$ superlattice structures at the interface, which reveal Mott-Hubbard bands, in excellent agreement with both experimental observations and theoretical predictions. Additionally, we found signatures of quasiparticle peaks close to the Fermi energy, in detail depending on the hybridization strength and doping level.

cond-mat.str-el↗

arXiv2024

Supercell Wannier functions and a faithful low-energy model for Bernal bilayer graphene

We derive a minimal low-energy model for Bernal bilayer graphene and related rhombohedral graphene multilayers at low electronic densities by constructing Wannier orbitals defined in real-space supercells of the original primitive cell. Starting from an ab-initio electronic structure theory comprising the atomic carbon $p_z$-orbitals, momentum locality of the Fermi surface pockets around $K,K'$ is circumvented by backfolding the $π$-bands to the concomitant mini-Brillouin zone of the supercell, reminiscent of their (twisted) moiré counterparts. The supercell Wannier functions reproduce the spectral weight and Berry curvature of the microscopic model and offer an intuitive real-space picture of the emergent physics at low electronic densities being shaped by flavor-polarized wave packets with mesoscopic extent. By projecting an orbital-resolved, dual-gated Coulomb interaction to the effective Wannier basis, we find that the low-energy physics of Bernal bilayer graphene is governed by weak electron-electron interactions. Our study bridges between existing continuum theories and ab-initio studies of small Fermi pocket systems like rhombohedral graphene stacks by providing a symmetric lattice description of their low-energy physics.

cond-mat.mes-hall↗

arXiv2024

Charge correlation, doublon-holon binding and screening in the doped Hubbard model

Electronic correlations arise from the competition between the electrons' kinetic and Coulomb interaction energy and give rise to a rich phase diagram and many emergent quasiparticles. The binding of doubly-occupied and empty sites into a doublon-holon exciton is an example of this in the Hubbard model. Unlike traditional excitons in semiconductors, in the Hubbard model it is the kinetic energy which provides the binding energy. Upon doping, we find the emergence of exciton complexes, such as a holon-doublon-holon trion. The appearance of these low-lying collective excitations make screening more effective in the doped system. As a result, Hubbard-based modelling of correlated materials should use different values of $U$ for the doped system and the insulating parent compound, which we illustrate using the cuprates as an example.

cond-mat.str-el↗

arXiv2024

Quenched pair breaking by interlayer correlations as a key to superconductivity in La$_3$Ni$_2$O$_7$

The recent discovery of superconductivity in La$_3$Ni$_2$O$_7$ with $T_\mathrm{c} \simeq 80~\mathrm{K}$ under high pressure opens up a new route to high-$T_\mathrm{c}$ superconductivity. This material realizes a bilayer square lattice model featuring a strong interlayer hybridization unlike many unconventional superconductors. A key question in this regard concerns how electronic correlations driven by the interlayer hybridization affect the low-energy electronic structure and the concomitant superconductivity. Here, we demonstrate using a cluster dynamical mean-field theory that the interlayer electronic correlations (IECs) induce a Lifshitz transition resulting in a change of Fermi surface topology. By solving an appropriate gap equation, we further show that the leading pairing instability, $s \pm$-wave, is enhanced by the IECs. The underlying mechanism is the quenching of a strong ferromagnetic channel, resulting from the Lifshitz transition driven by the IECs. Based on this picture, we provide a possible reason of why superconductivity emerges only under high pressure.

cond-mat.supr-con↗

arXiv2024

Downfolding from Ab Initio to Interacting Model Hamiltonians: Comprehensive Analysis and Benchmarking of the DFT+cRPA Approach

Model Hamiltonians are regularly derived from first-principles data to describe correlated matter. However, the standard methods for this contain a number of largely unexplored approximations. For a strongly correlated impurity model system, here we carefully compare a standard downfolding technique with the best possible ground-truth estimates for charge-neutral excited state energies and wavefunctions using state-of-the-art first-principles many-body wave function approaches. To this end, we use the vanadocene molecule and analyze all downfolding aspects, including the Hamiltonian form, target basis, double counting correction, and Coulomb interaction screening models. We find that the choice of target-space basis functions emerges as a key factor for the quality of the downfolded results, while orbital-dependent double counting correction diminishes the quality. Background screening to the Coulomb interaction matrix elements primarily affects crystal-field excitations. Our benchmark uncovers the relative importance of each downfolding step and offers insights into the potential accuracy of minimal downfolded model Hamiltonians

cond-mat.str-el↗

arXiv2024

Collective charge excitations between moiré-minibands in twisted WSe2 bilayers from resonant inelastic light scattering

We establish low-temperature resonant inelastic light scattering (RILS) spectroscopy as a tool to probe the formation of a series of moiré-bands in twisted WSe_{2} bilayers by accessing collective intermoiré-band excitations (IMBE). We observe resonances in RILS spectra at energies in agreement with inter-moiré band transitions obtained from an ab-initio based continuum model. Transitions between the first and second inter-moiré band for a twist angle of about 8° are reported and between first and second, third and higher bands for a twist of about 3°. The signatures from IMBE for the latter highlight a strong departure from parabolic bands with flat minibands exhibiting very high density of states in accord with theory. These observations allow to quantify the transition energies at the K-point where the states relevant for correlation physics are hosted.

cond-mat.str-el↗

arXiv2024

Ab initio electron-lattice downfolding: potential energy landscapes, anharmonicity, and molecular dynamics in charge density wave materials

The interplay of electronic and nuclear degrees of freedom presents an outstanding problem in condensed matter physics and chemistry. Computational challenges arise especially for large systems, long time scales, in nonequilibrium, or in systems with strong correlations. In this work, we show how downfolding approaches facilitate complexity reduction on the electronic side and thereby boost the simulation of electronic properties and nuclear motion - in particular molecular dynamics (MD) simulations. Three different downfolding strategies based on constraining, unscreening, and combinations thereof are benchmarked against full density functional calculations for selected charge density wave (CDW) systems, namely 1H-TaS$_2$, 1T-TiSe$_2$, 1H-NbS$_2$, and a one-dimensional carbon chain. We find that the downfolded models can reproduce potential energy surfaces on supercells accurately and facilitate computational speedup in MD simulations by about five orders of magnitude in comparison to purely ab initio calculations. For monolayer 1H-TaS$_2$ we report classical replica exchange and quantum path integral MD simulations, revealing the impact of thermal and quantum fluctuations on the CDW transition.

cond-mat.str-el↗