arXiv subjects

Kai Rossnagel

Publications and source records attributed to Kai Rossnagel.

At least 19 recordsLinked to original sources

arXiv2026

Infrared evidence for strong $C_{3}$ symmetry breaking in 1$T$-TiSe$_{2}$

The interplay between lattice and electron degrees of freedom gives rise to competing ordered states in quantum materials, which can lead to a series of subsequent symmetry breaking transitions. While the differences are often subtle, these phases can be distinguished by their remaining point group symmetries. Here, we use infrared optical spectroscopy to probe symmetry breaking at the charge density wave transition of 1$T$-TiSe$_{2}$. We uncover a previously unobserved splitting of a doubly degenerate $E_u$ optical phonon at $T_{\mathrm{CDW}}\approx$ 190 K that constitutes direct evidence for the breaking of three-fold rotational symmetry. Our finding rules out proposals where the CDW transition to a low temperature chiral or nematic phase takes place through an intermediary state that preserves three-fold symmetry. The energy difference between the two former $E_{u}$ partners can only be explained by large $C_{3}$ breaking distortions of the same order of magnitude as previously observed changes in bond lengths, suggesting that $C_{3}$ symmetry breaking plays a dominant role in the CDW transition. The linewidth of the single phonon mode above $T_{\mathrm{CDW}}$ could be consistent with a fluctuating state where three-fold symmetry is also broken.

cond-mat.str-el↗

arXiv2026

Magnetically coupled charge-transport crossover and giant negative magnetoresistance in iodine-incorporated Cr$_2$Se$_3$

We report the synthesis and comprehensive investigation of iodine-incorporated $Cr_2Se_3$, a non-van der Waals quasi-two-dimensional magnetic material, using structural, magnetic, transport, spectroscopic, and first-principles methods. Magnetization and electron spin resonance measurements reveal an antiferromagnetically ordered state below $T_N \approx 52$ K. At higher temperatures, a second, broader anomaly emerges near $T^* \approx 150$ K, coinciding with a shallow minimum in the temperature-dependent resistivity that resembles a metal-to-insulator-like crossover. Hall measurements indicate predominantly hole-like conduction at high temperatures ($\geq$ 150 K), while the nonlinear Hall response below T*, together with an anomaly in the third-harmonic electrical signal, suggests the emergence of mobility-dependent multichannel and spatially inhomogeneous transport. A large, non-saturating negative magnetoresistance reaching approximately -78\% at 25 K and 12 T further demonstrates strong coupling between charge transport and the magnetic state. Temperature-dependent Raman spectroscopy reveals no symmetry-changing structural transition near T*, whereas angle resolved photoemission spectroscopy (ARPES) measurements show no major reconstruction of the electronic structure occupied across the crossover. Taken together, these results identify the high-temperature anomaly as a broad magnetically coupled transport crossover arising from the interplay of short-range magnetic correlations, chemical disorder, and redistribution among competing conduction channels. These findings demonstrate that anion incorporation provides an effective route to tuning the coupled electronic and magnetic properties of non-layered Cr$_2$Se$_3$, establishing this system as a promising platform for investigating correlated transport and emergent spintronic functionalities in transition-metal chalcogenides.

cond-mat.mtrl-sci↗

arXiv2026

Boosting self hybridized exciton polaritons with metal clad WS2 waveguides

The formation of Fabry Perot and guided wave self hybridized exciton polaritons in two dimensional materials results in long range exciton energy transfer and strong exciton exciton interactions. Here, we demonstrate that the coupling strength between photonic modes and excitons is significantly boosted by embedding the active excitonic layer in a metal clad WS2 waveguide. The photonic modes in this waveguide exhibit modified dispersion properties for both Fabry Perot type and guided wave exciton polaritons compared to pure WS2 flakes, and show an increased couplingr strength. Our results provide a robust approach for controlling exciton photon interactions and their coupling strength in hybrid heterostructures.

quant-ph↗

arXiv2026

Phonon-induced pseudogap phase in TiSe$_2$

To comprehend quantum ordered states, such as charge density waves (CDW), in layered transition metal dichalcogenides (TMDCs), it is essential to uncover their underlying normal states. Here, we use time- and angle-resolved extreme ultraviolet photoemission spectroscopy and ab initio electron-phonon calculations to perform excited state band mapping of three prototypical 1T TMDCs, i.e., TiSe$_2$, HfTe$_2$, and ZrTe$_2$, at room temperature. The results reveal the profound impact of strong electron-phonon-induced thermal fluctuations on the normal-phase electronic structure. Specifically, in the moderate electron-phonon coupling regime, as in HfTe$_2$ and ZrTe$_2$, thermal fluctuations only lead to small spectral broadening and band renormalization. In the strongly coupled case, exemplified by TiSe$_2$, we observe soft-phonon-induced, momentum-dependent suppression of spectral weight, i.e., pseudogaps - extending up to 1 eV above the Fermi level. Our work establishes the normal phase of TiSe$_2$ as a phonon-induced pseudogap phase governed by strong CDW fluctuations, thereby uncovering previously missing aspects of the TiSe$_2$ phase diagram, with broader implications for other TMDCs in the strong electron-phonon coupling regime.

cond-mat.str-el↗

arXiv2026

Electronic Structure and Resonant Circular Dichroism of La$_{0.7}$Sr$_{0.3}$MnO$_3$ from Soft X-ray Angle-Resolved Photoemission

Coupling between spin, orbital, charge, and lattice degrees of freedom in transition-metal oxides produces a variety of electronic and magnetic phenomena of importance for future technologies. Here, we explore the electronic band structure of a (111)-oriented La0.7Sr0.3MnO3 thin film through soft X-ray angle-resolved photoemission spectroscopy (ARPES). The measurements agree with the electronic band structure calculated with density functional theory using Hubbard U correction. Furthermore, we probe the circular dichroism in ARPES, and observe a pronounced momentum- resolved magnetic circular dichroism in resonant photoemission from the Mn L-edge. The approach combines the momentum- and spin-selectivity of ARPES and X-ray magnetic circular dichroism, respectively, which could provide a useful approach for the study of unconventional magnetism.

cond-mat.str-el↗

arXiv2026

Percolative Instabilities and Sparse-Limit Fractality in 1T-TaS$_2$

The low-temperature metallic phase of 1T-TaS2 may originate from current- and voltage-driven destabilization of the commensurate charge density wave (CDW) in a strongly correlated Mott insulator, alongside the robust yet rarely realized influence of intrinsic electronic distortions. Electrical pulse-driven transport, combined with second harmonic response, reveals abrupt switching, negative differential resistance (NDR), and multiscale domain-wall reorganization. The free energy analysis identifies a critical order parameter threshold for the Mott-metal transition, with scaling exponents (β approx 1.3) consistent with 2D percolation. The sparse limit fractal dimension D_{f} approx 0.3 at 10 K, rising to approx 0.9 at 300 K, reflects the hierarchical evolution of the conductive pathways throughout the temperature. These findings establish a direct connection between fractal percolation, pulse-induced instabilities, and correlated electron transport, offering a framework for controlled access to non-equilibrium phase transitions in low-dimensional quantum materials.

cond-mat.mes-hall↗

arXiv2026

Ultrafast Band-Gap Renormalization in Bilayer Graphene

We demonstrate, by femtosecond time- and angle-resolved photoemission spectroscopy, that photoinduced interlayer charge transfer in a heterostructure consisting of Bernal-stacked bilayer graphene and a single atomic layer of silver on 6H-SiC(0001) transiently modulates the intrinsic potential landscape across the silver-graphene interface. This acts as an ultrafast optoelectronic gate that drives momentum-dependent band renormalizations, resulting in a transient band-gap opening on femtosecond timescales. Simultaneously, the photogenerated hot-carrier population enhances electronic screening, leading to subsequent closing of the band-gap beyond the thermal equilibrium value. These findings reveal two different mechanisms for photoinduced, reversible control of the electronic band structure in bilayer graphene -- interlayer charge transfer and hot-carrier-enhanced screening -- providing a general framework for the ultrafast control of electronic properties in graphene-based heterostructures. This opens up novel pathways for the realization of ultrafast optoelectronic devices and the exploration of correlated quantum phases in bilayer graphene under non-equilibrium conditions.

cond-mat.mes-hall↗

arXiv2026

Electron-phonon-dominated charge-density-wave fluctuations in TiSe$_2$ accessed by ultrafast nonequilibrium dynamics

The complex phase diagram of 1T-TiSe2 consists of a charge density wave (CDW) below 200 K, and CDW fluctuations of still unknown origin at higher temperatures. Here, we use time-resolved extreme ultraviolet momentum microscopy and density functional perturbation theory to uncover the formation mechanism of CDW fluctuations and their spectral features at 295 K. We investigated the transient dynamics of fluctuations upon nonresonant ultrafast photoexcitation, and directly correlate it with the CDW soft-phonon hardening. Surprisingly, our results show that the coherent amplitude mode modulating ultrafast CDW recovery persists above TCDW, and reveal that CDW fluctuations are dominated by the electron-phonon interaction rather than excitonic correlations as commonly believed. Our findings on these microscopic CDW fluctuations clarify the complex interplay between electronic and lattice degrees of freedom at elevated temperatures and, therefore, could be useful in understanding the nature of the CDW phase transition in 1T-TiSe2 and similar quantum materials.

cond-mat.str-el↗

arXiv2026

Femtosecond concerted rotation of molecules on a 2D material interface

Interfaces between molecules and 2D materials exhibit energy-driven functionalities, wherein charge transfer directs molecular motion. Unlike equilibrium systems, where molecular assemblies settle into static configurations, continuous energy input can drive transient, collective molecular rearrangements. Here, we reveal ultrafast spectroscopic fingerprints of a collective rotational response of molecules on a 2D material following photoexcitation. Our results suggest that photoinduced charge transfer reshapes the interfacial energy potential, giving rise to macroscopic, unidirectional molecular rotation and the formation of a homochiral molecular arrangement. Using a multiplexed ultrafast photoemission spectroscopy approach, we simultaneously track, electronic states, atomic positions, and orbital wavefunctions with femtosecond and sub-ångström resolution. Multimodal valence and core electron emission analysis disentangles the intertwined electronic-structural dynamics of the molecule and the 2D material, revealing the dynamic modulation of charge distribution and intermolecular forces that drive collective molecular motion. Our findings open a pathway for designing energy-driven molecular systems with tunable interfacial dynamics, with potential applications in chiral engineering and active matter systems.

cond-mat.mtrl-sci↗

arXiv2025

Optical switching of ferro-rotational charge-density wave states

Tailored optical excitations can steer a system along non-equilibrium pathways to metastable states with specific structural or electronic properties. The light-induced hidden state of 1T-TaS$_{2}$, with its strongly enhanced conductivity and exceptionally long lifetime, represents a unique model system for studying the ultrafast switching of correlated electronic states. We use surface-sensitive electron diffraction in combination with a femtosecond optical quench to reveal the coexistence of both charge-density-wave (CDW) 2D chiralities as a structural characteristic of the hidden state, corresponding to coexisting ferro-rotational CDW states. Density functional theory (DFT) simulations of interfaces between opposite CDW 2D chiralities predict a higher-level, fractal-type moir'{e} superstructure with a kagome band structure near the Fermi energy. More broadly, these findings suggest that heterochiral interfaces in CDW systems provide an additional structural degree of freedom, expanding the possibilities for electronic control via twist-angle engineering.

cond-mat.mes-hall↗

arXiv2025

Direct signatures of $d$-level hybridization and dimerization in magnetic adatom chains on a superconductor

Magnetic adatom chains on superconductors provide a platform to explore correlated spin states and emergent quantum phases. Using low-temperature scanning tunneling spectroscopy, we study the distance-dependent interaction between Fe atoms on 2H-NbSe$_2$. While single atoms exhibit four Yu-Shiba-Rusinov states and partially occupied $d$ levels consistent with a $S=2$ spin state, the spin is quenched when two Fe atoms reside in nearest neighbor lattice sites, where the $d$ levels of the atoms hybridize. The non-magnetic dimer configuration is stable in that dimerization persists in chains with weak interactions among the dimers. Thus, the spin-state quenching has important implications also for Fe chains. While even-numbered chains are stable and non-magnetic, odd-numbered chains host a single magnetic atom at one of the chain's ends, with its position being switchable by voltage pulses. Our findings emphasize the role of interatomic coupling in shaping quantum ground states and suggest that engineering alternating hopping amplitudes analogous to the Su-Schrieffer-Heeger model may offer a pathway to realizing topological systems.

cond-mat.mes-hall↗

arXiv2025

3D atomic structure determination with ultrashort-pulse MeV electron diffraction

Understanding structure at the atomic scale is fundamental for the development of materials with improved properties. Compared to other probes providing atomic resolution, electrons offer the strongest interaction in combination with minimal radiation damage. Here, we report the successful implementation of MeV electron diffraction for ab initio 3D structure determination at atomic resolution. Using ultrashort electron pulses from the REGAE accelerator, we obtained high-quality diffraction data from muscovite and $1T-TaS_2$, enabling structure refinements according to the dynamical scattering theory and the accurate determination of hydrogen atom positions. The increased penetration depth of MeV electrons allows for structure determination from samples significantly thicker than those typically applicable in electron diffraction. These findings establish MeV electron diffraction as a viable approach for investigating a broad range of materials, including nanostructures and radiation-sensitive compounds, and open up new opportunities for in-situ and time-resolved experiments.

cond-mat.mtrl-sci↗

arXiv2025

Zero-energy band observation in an interfacial chalcogen-organic network

Structurally-defined molecule-based lattices such as covalent organic or metal-organic networks on substrates, have emerged as highly tunable, modular platforms for two-dimensional band structure engineering. The ability to grow molecule-based lattices on diverse platforms, such as metal dichalcogenides, would further enable band structure tuning and alignment to the Fermi level, which is crucial for the exploration and design of quantum matter. In this work, we study the emergence of a zero-energy band in a triarylamine-based network on semiconducting 1T-TiSe2 at low temperatures, by means of scanning probe microscopy and photoemission spectroscopy, together with density-functional theory. Hybridization between the position-selective nitrogens and selenium p-states results in CN-Se interfacial coordination motifs, leading to a hybrid molecule-semiconductor band at the Fermi level. Our findings introduce chalcogen-organic networks and showcase an approach for the engineering of organic-inorganic quantum matter.

physics.chem-ph↗

arXiv2025

Photoemission electron microscopy of exciton-polaritons in thin WSe$_2$ waveguides

Exciton-polaritons emerging from the interaction of photons and excitons in the strong coupling regime are intriguing quasiparticles for the potential exchange of energy during light-matter interaction processes such as light harvesting. The coupling causes an energy anti-crossing in the photon dispersion centered around the exciton resonance, i.e., a Rabi splitting between a lower and upper energetic branch. The size of this splitting correlates with the coupling strength between the exciton and the photonic modes. In this work, we investigate this coupling between excitons and photonic waveguide modes excited simultaneously in thin-film flakes of the transition-metal dichalcogenide WSe$_2$. Using a Photoemission electron microscope, we are able to extract the dispersion of the transversal electric and magnetic modes propagating through these flakes as well as extract the energy splitting. Ultimately, our findings provide a basis for the investigation of the propagation of exciton-polaritons in the time-domain via time-resolved photoemission.

cond-mat.mtrl-sci↗

arXiv2025

Odd-parity ground state in dilute Yu-Shiba-Rusinov dimers and chains

Magnetic adatoms on superconductors induce Yu-Shiba-Rusinov (YSR) states, which are key to the design of low-dimensional correlated systems and topological superconductivity. Competing magnetic interactions and superconducting pairing lead to a rich phase diagram. Using a scanning tunneling microscope (STM), we position Fe atoms on 2H-NbSe$_2$ to build a dimer with an odd-parity ground state, i.e., a partially screened YSR channel with the hybridized states spanning the Fermi level. This ground state makes the dimer a promising precursor for a topological YSR chain. By adding one atom at a time, we track the formation of YSR bands. The lowest-energy band crosses the Fermi level and we find strong site-dependent spectral variations especially at the chain's terminations. We attribute these features to quantum spin effects and ferromagnetic coupling influenced by the local chemical environment, rather than topological superconductivity or Majorana modes.

cond-mat.mes-hall↗

arXiv2025

Resistively detected electron spin resonance and g-factor in few-layer exfoliated MoS2 devices

MoS2 has recently emerged as a promising material for enabling quantum devices and spintronic applications. In this context, an improved physical understanding of the g-factor of MoS2 depending on device geometry is of great importance. Resistively detected electron spin resonance (RD-ESR) could be employed to and the determine the g-factor in micron-scale devices However, its application and RD-ESR studies have been limited by Schottky or high-resistance contacts to MoS2. Here, we exploit naturally n-doped few-layer MoS2 devices with ohmic tin (Sn) contacts that allow the electrical study of spin phenomena. Resonant excitation of electron spins and resistive detection is a possible path to exploit the spin effects in MoS2 devices. Using RD-ESR, we determine the g-factor of few-layer MoS2 to be ~1.92 and observe that the g-factor value is independent of the charge carrier density within the limits of our measurements.

cond-mat.mes-hall↗

arXiv2025

Charge-density-wave quantum critical point under pressure in 2$H$-TaSe$_2$

Suppressing of an ordered state that competes with superconductivity is one route to enhance superconducting transition temperatures. Whereas the effect of suppressing magnetic states is still not fully understood, materials featuring charge-density waves and superconductivity offer a clearer scenario as both states can be associated with electron-phonon coupling. Metallic transition-metal dichalcogenides are prime examples for such intertwined electron-phonon-driven phases, yet, various compounds do not show the expected interrelation or feature additional mechanisms which makes an unambiguous interpretation difficult. Here, we report high-pressure X-ray diffraction and inelastic X-ray scattering measurements of the prototypical transition-metal dichalcogenide 2$H$-TaSe$_2$ and determine the evolution of the charge-density-wave state and its lattice dynamics up to and beyond its suppression at the critical pressure $p_c = 19.9(1)\,\rm{GPa}$ and at low temperatures. The high quality of our data allows the full refinement of the commensurate charge-density-wave superstructure at low pressure and we find the quantum critical point of the charge-density-wave to be in close vicinity to the reported maximum superconducting transition temperature $T_{sc} = 8.2\,\rm{K}$. $Ab-initio$ calculations corroborate that 2$H$-TaSe$_2$ is a reference example of order-suppressed enhanced superconductivity and can serve as a textbook case to investigate superconductivity near a charge-density-wave quantum critical point.

cond-mat.str-el↗

arXiv2024

Spin polarization of the two-dimensional electron gas at the EuO/SrTiO$_3$ interface

Spin-polarized two-dimensional electron gases (2DEGs) are of particular interest for functional oxide electronics applications. The redox-created 2DEG residing on the strontium titanate, SrTiO$_3$ (STO), side of a europium monoxide (EuO)/SrTiO$_3$ (001) interface is expected to be significantly spin-polarized due to the proximity to the strong ($7\,μ_B/f.u.$) Heisenberg ferromagnet EuO. We apply magnetic circular dichroism in the angular distribution (MCDAD) of photoemitted electrons to investigate whether and how the induced spin polarization of the 2DEG depends on the dimensionality of the overlaying EuO layer. The experimental data are complemented by density functional theory calculations with a Hubbard $U$ term (DFT+$U$). We show that the EuO/STO interfacial 2DEG is spin-polarized even for ultrathin EuO overlayers, starting at an EuO threshold thickness of only two monolayers. Additional EuO monolayers even increase the induced magnetic Ti moment and thus the spin polarization of the 2DEG. Our results and the potential to enhance the magnetic order of EuO by other proximity effects indicate that the EuO/STO (001) interface is an ideal template for creating (multi-)functional spin-polarized 2DEGs for application in oxide electronics.

cond-mat.mtrl-sci↗