arXiv subjects

Malte Rösner

Publications and source records attributed to Malte Rösner.

At least 19 recordsLinked to original sources

arXiv2026

Quantum Monte Carlo assessment of embedding for for strongly correlated defects: interplay between mean-field starting point and interactions

Point defects are of interest for many applications, from quantum sensing to modifying bulk properties of materials. Because of their localized orbitals, the electronic states are often strongly correlated, which has led to a proliferation of quantum embedding techniques to treat this correlation. In these techniques, most of the one-body states are treated with a weakly correlated theory such as density functional theory, and certain one-body states are singled out as an active space to be treated using an effective interaction. We assess these techniques for iron and chromium defects in aluminum nitride using quantum Monte Carlo (QMC) calculations on identical Hamiltonians. For these systems, we find the dominant errors in the embedding arise from the one-body crystal-field splitting in the d orbitals inherited from density functional theory (DFT), rather than double counting corrections, with the screened interactions also affected by the DFT orbitals. Strikingly, the best double counting recipe is opposite in these two cases. Because excitation energies can agree while the underlying wave functions do not, diagnosing these errors requires detailed information about the many-body wave functions, which QMC provides.

cond-mat.str-el↗

arXiv2026

Visualization of Defect Electronic States in Layered Semiconductor CrSBr

Chromium sulfur bromide (CrSBr) is a layered magnetic semiconducting material combining a rich magnetic phase diagram with axis-dependent electronic and optical properties. While defects in CrSBr have been shown to affect magnetic order and excitonic responses, their microscopic nature, atomic structure, and electronic properties are not yet fully understood. In this work, we use scanning tunneling microscopy/spectroscopy (STM/STS) to explore the structure and electronic signatures of two prominent defects in bulk CrSBr. Their structure reflects the symmetries of the underlying lattice, with electronic features near the valence band edge. By comparing experimental data with ab initio simulated STM images, we infer that a common defect corresponds to a b-axis-aligned double sulfur vacancy, in line with findings from a recent growth analysis study. This result advances our understanding of the role of intrinsic defects in shaping the electronic structure of CrSBr.

cond-mat.mes-hall↗

arXiv2026

Growth-controlled suppression of electrically active defects in CrSBr

In CrSBr, as in many crystalline materials, the type and density of defects are expected to strongly influence material behavior. Identifying the underlying atomic defect configurations and controlling their populations during growth are therefore important steps toward understanding and ultimately tailoring its rich magneto-electrical properties. However, systematic control of defects in CrSBr during chemical vapor transport (CVT) growth has not yet been established. Here, we correlate CVT growth conditions with defect concentrations measured using conductive atomic force microscopy (CAFM). We focus on a characteristic defect with a strong electronic fingerprint, labeled D*, and decrease its concentration by up to an order of magnitude through optimized growth conditions. We show that defect densities can be tuned by adjusting precursor stoichiometry, where sulfur- and bromine-rich conditions suppress defect formation, and by lowering the absolute growth temperatures while maintaining the same temperature gradient. Thermodynamic modeling and density functional theory calculations suggest that D* is most consistent with a sulfur-related vacancy complex rather than an isolated point defect. These results provide practical strategies for growing high-quality CrSBr with controlled defect densities.

cond-mat.mtrl-sci↗

arXiv2026

Importance of effective Coulomb interactions for $T_c$ in cuprates

Cuprate superconductors exhibit the highest observed superconducting $T_c$ at atmospheric pressure. However, the magnitude of $T_c$ varies significantly between different cuprates. At present, it is unclear what properties of the crystal structure affect $T_c$ most strongly, yet such an understanding must underpin any efforts toward high-$T_c$ materials design. To address this issue, we perform a large scale systematic study, employing a combination of data collection, state-of-the-art numerical methods, and statistical analysis. We identify about 40 different cuprate compounds, and we compile detailed data about their $T_c$'s and crystal structures from literature and the available databases. Using a fully automated procedure, for each compound we compute the DFT bandstructure and downfold it to two of the most commonly studied low-energy lattice models, namely the single-band Hubbard and the three-band Emery models. The downfolding is based on the approach of MLWFs and cRPA. Finally, we apply a thorough and unbiased statistical analysis to investigate the correlations between the experimentally measured $T_c$'s and the computed parameters of our theoretical models. Our data indicates that more sophisticated models might be needed to describe all cuprates on the same footing. Nevertheless, we find that $T_c$ scales well with simple functions of model parameters. We confirm a previously observed trend that $t'$ in the single-band model correlates with the experimental $T_c$, and we find that $T_c$ appears to vanish below a finite value of $t'$, in agreement with recent ground-state calculations for the Hubbard model. However, we find that the coupling strength also plays a role: throughout our entire dataset, $T_c$ correlates the most with the Coulomb coupling on the $p$-orbitals in the 3-band model, highlighting the importance of the oxygen sites in the copper-oxide planes.

cond-mat.str-el↗

arXiv2026

Change in charge density wave order beyond the Lifshitz transition in 2H-Ta\textsubscript{1$\pmδ$}S\textsubscript{2}

We investigate electronic instabilities in 2H-TaS\textsubscript{2} and a self-intercalated variant, 2H$^\dagger$-Ta\textsubscript{1+$δ$}S\textsubscript{2}. In conventional samples, which we determine to be slightly hole-doped, spectral gaps and backfolded features are found as fingerprints of the $3\times3$ charge density wave (CDW). Notably, the backfolded features emerge only at a temperatures below $T\approx$~65~K, substantially lower than the established CDW temperature of 78~K, suggesting an incommensurate-commensurate lock-in transition analogous to the phenomenology of the 2H-TaSe\textsubscript{2}. In contrast, the self-intercalated 2H$^\dagger$ sample exhibits substantial electron doping and signatures of a novel \tworootthree CDW. Using \textit{ab initio} calculations of the phonon spectrum, we demonstrate that the \threebythree instability ($\mathbf{q}=\sfrac{2}{3}\mathbf{ΓM}$) is highly sensitive to band filling. Furthermore, with increased interlayer spacing, a competing soft phonon mode emerges near $\mathbf{q}=\sfrac{1}{2}\mathbf{ΓK}$, corresponding to the superstructure observed in the 2H$^\dagger$ phase, although in our calculations this instability arises under hole doping rather than the electron doping inferred experimentally. These results establish band filling and interlayer spacing as key control parameters for CDW ordering vectors in 2H-TaS\textsubscript{2}, and highlight a route to engineering electronic instabilities in a prototypical layered material.

cond-mat.str-el↗

arXiv2026

Exact downfolding and its perturbative approximation

Solving the many-electron problem, even approximately, is one of the most challenging and simultaneously most important problems in contemporary condensed matter physics with various connections to other fields. The standard approach is to follow a divide and conquer strategy that combines various numerical and analytical techniques. A crucial step in this strategy is the derivation of an effective model for a subset of degrees of freedom by a procedure called downfolding, which often corresponds to integrating out energy scales far away from the Fermi level. In this work we present a rigorous formulation of this downfolding procedure, which complements the renormalization group picture put forward by Honerkamp [PRB 85, 195129 (2012)}]. We derive an exact effective model in an arbitrarily chosen target space (e.g. low-energy degrees of freedom) by explicitly integrating out the the rest space (e.g. high-energy degrees of freedom). Within this formalism we state conditions that justify a perturbative truncation of the downfolded effective interactions to just a few low-order terms. Furthermore, we utilize the exact formalism to formally derive the widely used constrained random phase approximation (cRPA), uncovering underlying approximations and highlighting relevant corrections in the process. Lastly, we detail different contributions in the material examples of fcc Nickel and the infinite-layer cuprate SrCuO$_2$. Our results open up a new pathway to obtain effective models in a controlled fashion and to judge whether a chosen target space is suitable.

cond-mat.str-el↗

arXiv2025

Static treatment of dynamic interactions in the single-orbital Anderson impurity model

Correlated electron physics is intrinsically a multiscale problem, since high-energy electronic states screen the interactions between the correlated electrons close to the Fermi level, thereby reducing the magnitude of the interaction strength and dramatically shortening its range. Thus, the handling of screening is an essential ingredient in the first-principles modelling of correlated electron systems. Screening is an intrinsically dynamic process and the corresponding downfolding methods such as the constrained Random Phase Approximation indeed produce a dynamic interaction. However, many low-energy methods require an instantaneous interaction as input, which makes it necessary to map the fully dynamic interaction to an effective instantaneous interaction strength. It is a priori not clear if and when such an effective model can capture the physics of the one with dynamic interaction and how to best perform the mapping. Here, we provide a systematic benchmark relevant to correlated materials, in the form of the Anderson impurity model. Overall, we find that a static approximation can be valid and that the moment-based approach recently proposed by Scott and Booth can be a good tool to find the value of the static interaction. We also identify physical regimes, especially under doping, where an instantaneous interaction cannot capture all of the relevant physics.

cond-mat.str-el↗

arXiv2025

From strong to weak correlations in breathing-mode kagome van der Waals materials: Nb$_3$(F,Cl,Br,I)$_8$ as a robust and versatile platform for many-body engineering

By combining ab initio downfolding with cluster dynamical mean-field theory, we study the degree of correlations in monolayer, bilayer and bulk breathing-mode kagome van der Waals materials Nb$_3$(F,Cl,Br,I)$_8$. Our new material-specific many-body model library shows that in low-temperature bulk structures the Coulomb correlation strength steadily increases from I to F, allowing us to identify Nb$_3$I$_8$ as a weakly correlated insulator, Nb$_3$Br$_8$ and Nb$_3$Cl$_8$ as strongly correlated insulators, and Nb$_3$F$_8$ as a prototypical bulk Mott-insulator. Angle-resolved photoemission spectroscopy measurements comparing Nb$_3$Br$_8$ and Nb$_3$I$_8$ allow us to experimentally confirm these findings by revealing spectroscopic footprints of the degree of correlation. Our calculations uncover how the thickness and the stacking affect the degree of correlations and predict that the entire material family can be tuned into correlated charge-transfer or Mott-insulating phases upon doping. Our magnetic property analysis based on our model parameter library additionally confirms that inter-layer magnetic interactions drive the lattice phase transition to the low-temperature structures. The accompanying bilayer hybridization through inter-layer dimerization yields magnetic singlet-like ground states in the Cl, Br, and I compounds. We further prove that all low-temperature compounds are dynamically stable and that electron-phonon coupling to the low-energy subspace is suppressed. Our findings establish Nb$_3$X$_8$ as a robust, versatile, and tunable class for van der Waals-based Coulomb and Mott engineering with a rich phase diagram and allow us to speculate on the symmetry-breaking effects necessary for the recently observed Josephson diode effect in NbSe$_2$/Nb$_3$Br$_8$/NbSe$_2$ heterostructures.

cond-mat.str-el↗

arXiv2025

Enhancing Plasmonic Superconductivity in Layered Materials via Dynamical Coulomb Engineering

Conventional Coulomb engineering, through controlled manipulation of the environment, offers an effective route to tune the correlation properties of atomically thin van der Waals materials via static screening. Here we present tunable dynamical screening as a method for precisely tailoring bosonic modes to optimize many-body properties. We show that ``bosonic engineering'' of plasmon modes can be used to enhance plasmon-induced superconducting critical temperatures of layered superconductors in metallic environments by up to an order of magnitude, due to the formation of interlayer hybridized plasmon modes with enhanced superconducting pairing strength. We determine optimal properties of the screening environment to maximize critical temperatures. We show how bosonic engineering can aid the search for experimental verification of plasmon mediated superconductivity.

cond-mat.supr-con↗

arXiv2025

Quasiparticle gap renormalization driven by internal and external screening in a WS$_2$ device

The electronic band gap of a two-dimensional semiconductor within a device architecture is sensitive to variations in screening properties of adjacent materials in the device and to gate-controlled doping. Here, we employ micro-focused angle resolved photoemission spectroscopy to separate band gap renormalization effects stemming from environmental screening and electron-doping during \textit{in situ} gating of a single-layer WS$_{2}$ device. The WS$_{2}$ is supported on hBN and contains a section that is exposed to vacuum and another section that is encapsulated by a graphene contact. We directly observe the doping-induced semiconductor-metal transition and band gap renormalization in the two sections of WS$_2$. Surprisingly, a larger band gap renormalization is observed in the vacuum-exposed section than in the graphene-encapsulated - and thus ostensibly better screened - section of the WS$_2$. Using $GW$ calculations, we determine that intrinsic screening due to stronger doping in vacuum exposed WS$_2$ exceeds the external environmental screening in graphene-encapsulated WS$_2$.

cond-mat.mes-hall↗

arXiv2025

Defect complexes in CrSBr revealed through electron microscopy and deep learning

Atomic defects underpin the properties of van der Waals materials, and their understanding is essential for advancing quantum and energy technologies. Scanning transmission electron microscopy is a powerful tool for defect identification in atomically thin materials, and extending it to multilayer and beam-sensitive materials would accelerate their exploration. Here we establish a comprehensive defect library in a bilayer of the magnetic quasi-1D semiconductor CrSBr by combining atomic-resolution imaging, deep learning, and ab-initio calculations. We apply a custom-developed machine learning work flow to detect, classify and average point vacancy defects. This classification enables us to uncover several distinct Cr interstitial defect complexes, combined Cr and Br vacancy defect complexes and lines of vacancy defects that extend over many unit cells. We show that their occurrence is in agreement with our computed structures and binding energy densities, reflecting the intriguing layer interlocked crystal structure of CrSBr. Our ab-initio calculations show that the interstitial defect complexes give rise to highly localized electronic states. These states are of particular interest due to the reduced electronic dimensionality and magnetic properties of CrSBr and are furthermore predicted to be optically active. Our results broaden the scope of defect studies in challenging materials and reveal new defect types in bilayer CrSBr that can be extrapolated to the bulk and to over 20 materials belonging to the same FeOCl structural family.

cond-mat.mtrl-sci↗

arXiv2025

Influence of surface relaxations on scanning probe microscopy images of the charge density wave material 2H-NbSe$_2$

Scanning tunneling microscopy is the method of choice for characterizing charge density waves by imaging the variation in atomic-scale contrast of the surface. Due to the measurement principle of scanning tunneling microscopy, the electronic and lattice degrees of freedom are convoluted, making it difficult to disentangle a structural displacement from spatial variations in the electronic structure. In this work, we characterize the influence of the displacement of the surface-terminating Se atoms on the 3 x 3 charge density wave contrast in scanning probe microscopy images of 2H-NbSe$_2$. In scanning tunneling microscopy images, we observe the 3 x 3 charge density wave superstructure and atomic lattice at all probed tip-sample distances. In contrast, non-contact atomic force microscopy images show both periodicities only at small tip-sample distances while, unexpectedly, a 3 x 3 superstructure is present at larger tip-sample distances. Using density functional theory calculations, we qualitatively reproduce the experimental findings and indicate that the 3 x 3 superstructure at different tip-sample distances in non-contact atomic force microscopy images is a result from different underlying interactions. In addition, we show that the displacement of the surface-terminating Se atoms has a negligible influence to the contrast in scanning tunneling microscopy images. Our combined experimental and theoretic work presents a method on how to discriminate the influence of the surface corrugation from the variation of the charge density to the charge density wave contrast in scanning probe microscopy images, which can provide insights into the influence of structural disorder to a charge density wave ground state.

cond-mat.mes-hall↗

arXiv2024

Roadmap on Quantum Magnetic Materials

Fundamental research on two-dimensional (2D) magnetic systems based on van der Waals materials has been gaining traction rapidly since their recent discovery. With the increase of recent knowledge, it has become clear that such materials have also a strong potential for applications in devices that combine magnetism with electronics, optics, and nanomechanics. Nonetheless, many challenges still lay ahead. Several fundamental aspects of 2D magnetic materials are still unknown or poorly understood, such as their often-complicated electronic structure, optical properties, and magnetization dynamics, and their magnon spectrum. To elucidate their properties and facilitate integration in devices, advanced characterization techniques and theoretical frameworks need to be developed or adapted. Moreover, developing synthesis methods which increase critical temperatures and achieve large-scale, high-quality homogeneous thin films is crucial before these materials can be used for real-world applications. Therefore, the field of 2D magnetic materials provides many challenges and opportunities for the discovery and exploration of new phenomena, as well as the development of new applications. This Roadmap presents the background, challenges, and potential research directions for various relevant topics in the field on the fundamentals, synthesis, characterization, and applications. We hope that this work can provide a strong starting point for young researchers in the field and provide a general overview of the key challenges for more experienced researchers.

cond-mat.mtrl-sci↗

arXiv2024

Giant exchange splitting in the electronic structure of A-type 2D antiferromagnet CrSBr

We present the evolution of the electronic structure of CrSBr from its antiferromagnetic ground state to the paramagnetic phase above T_N=132 K, in both experiment and theory. Low temperature angle-resolved photoemission spectroscopy (ARPES) results are obtained using a novel method to overcome sample charging issues, revealing quasi-2D valence bands in the ground state. The results are very well reproduced by our QSGŴ calculations, which further identify certain bands at the X points to be exchange-split pairs of states with mainly Br and S character. By tracing band positions as a function of temperature, we show the splitting disappears above T_N. The energy splitting is interpreted as an effective exchange splitting in individual layers in which the Cr moments all align, within the so-called A-type antiferromagnetic arrangement. Our results lay firm foundations for the interpretation of the many other intriguing physical and optical properties of CrSBr.

cond-mat.str-el↗

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

Pressure-tuned many-body phases through $Γ$-K valleytronics in moiré bilayer WSe$_2$

Recent experiments in twisted bilayer transition-metal dichalcogenides have revealed a variety of strongly correlated phenomena. To theoretically explore their origin, we combine here ab initio calculations with correlated model approaches to describe and study many-body effects in twisted bilayer WSe$_2$ under pressure. We find that the interlayer distance is a key factor for the electronic structure, as it tunes the relative energetic positions between the K and the $Γ$ valleys of the valence band maximum of the untwisted bilayer. As a result, applying uniaxial pressure to a twisted bilayer induces a charge-transfer from the K valley to the flat bands in the $Γ$ valley. Upon Wannierizing moiré bands from both valleys, we establish the relevant tight-binding model parameters and calculate the effective interaction strengths using the constrained random phase approximation. With this, we approximate the interacting pressure-doping phase diagram of WSe$_2$ moiré bilayers using self-consistent mean field theory. Our results establish twisted bilayer WSe$_2$ as a platform that allows the direct pressure-tuning of different correlated phases, ranging from Mott insulators, charge-valley-transfer insulators to Kondo lattice-like systems.

cond-mat.str-el↗

arXiv2024

From orbital to paramagnetic pair breaking in layered superconductor 2H-NbS$_2$

The superconducting transition metal dichalcogenides 2H-NbSe$_2$ and 2H-NbS$_2$ are intensively studied on account of their unique electronic properties such as Ising superconductivity, found in multi- and monolayers, with upper critical fields beyond the Pauli limit. Even in bulk crystals, there are reports of multiband superconductivity and exotic states, such as the Fulde-Ferrell-Larkin-Ovchinnikov phase. In this work, we investigate the superconducting properties of 2H-NbS$_2$ through a detailed high-field mapping of the phase diagram by means of magnetotransport and magnetostriction experiments. We compare the phase diagram between bulk crystals and a 6~nm thick flake of 2H-NbS$_2$ and find a drastically enhanced Maki parameter in the flake, signifying a change of the relevant pair breaking mechanism from orbital to paramagnetic pair breaking, which we attribute to an effect of enhanced spin-orbit coupling.

cond-mat.supr-con↗

arXiv2023

Discovery of interlayer plasmon polaron in graphene/WS$_2$ heterostructures

Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials [1]. In situations where charge carriers induce a lattice distortion due to the electron-phonon interaction, the conducting states get "dressed". This leads to the formation of polaronic quasiparticles that dramatically impact charge transport, surface reactivity, thermoelectric and optical properties, as observed in a variety of crystals and interfaces composed of polar materials [2-6]. Similarly, when oscillations of the charge density couple to conduction electrons the more elusive plasmon polaron emerges [7], which has been detected in electron-doped semiconductors [8-10]. However, the exploration of polaronic effects on low energy excitations is still in its infancy in two-dimensional (2D) materials. Here, we present the discovery of an interlayer plasmon polaron in heterostructures composed of graphene on top of SL WS$_2$. By using micro-focused angle-resolved photoemission spectroscopy (microARPES) during in situ doping of the top graphene layer, we observe a strong quasiparticle peak accompanied by several carrier density-dependent shake-off replicas around the SL WS$_2$ conduction band minimum (CBM). Our results are explained by an effective many-body model in terms of a coupling between SL WS$_2$ conduction electrons and graphene plasmon modes. It is important to take into account the presence of such interlayer collective modes, as they have profound consequences for the electronic and optical properties of heterostructures that are routinely explored in many device architectures involving 2D transition metal dichalcogenides (TMDs) [11-15].

cond-mat.mes-hall↗