arXiv subjects

Thomas Brumme

Publications and source records attributed to Thomas Brumme.

At least 19 recordsLinked to original sources

arXiv2026

Spectrally Programmable Spin-Polarized Photocurrents in WSe$_2$-NiPS$_3$ Magnetic van der Waals Heterostructures

Efficient generation and control of spin-polarized currents in semiconductors remain central challenges for spin-based electronics, particularly due to impedance mismatch and the reliance on magnetic fields or ferromagnetic contacts. Here, we introduce a materials platform for spectrally programmable spin transport based on a van der Waals heterostructure combining the antiferromagnetic semiconductor NiPS$_3$ with WSe$_2$. In a p-n diode architecture, circularly polarized excitation produces pronounced photoconductive resonances with spin polarization reaching 80% near the Neel temperature and persisting at 30% at room temperature. Remarkably, selected spectral bands retain their polarization sign across the magnetic phase transition, evidencing robust, spectrally protected spin-polarized current generation. Polarization-resolved photogalvanic measurements reveal a dominant circular injection-current mechanism, confirming spin-polarized carrier transport. First-principles calculations show that an applied electric field induces interfacial hybridization and spin-layer locking, giving rise to localized symmetry breaking and enhanced optical absorption while preserving global time-reversal symmetry. These results establish spectral tuning of excitation as a new control knob for spin transport, enabling spin-current generation without magnetic fields or polarization switching. Our findings position magnetic van der Waals heterostructures as a versatile platform for opto-spintronic functionality and spectrally programmable spintronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Designer metal-free altermagnetism in honeycomb two-dimensional frameworks

Altermagnetism combines momentum-dependent spin splitting of opposite-spin channels with zero net magnetization, enabling electric-field control of spin transport that is robust against external magnetic fields. Although widely explored in inorganic systems, metal-free altermagnets with pi-spin splitting, particularly in two-dimensional organic frameworks, have remained elusive. Here, we introduce a molecular design strategy that achieves designer metal-free altermagnetism in honeycomb 2D crystals. By reducing the monomer point-group symmetry from D3h to C2v in triangulene-derived radicals, inversion symmetry is selectively broken while the bipartite lattice is preserved. Spin-polarized density-functional-theory calculations reveal strong antiferromagnetic couplings of -130 meV, d-wave spin splitting of 17 meV at the M point, and Mott-Hubbard gaps of 1.26 eV, all fully consistent with Lieb's theorem. A minimal tight-binding model shows that anisotropic nearest-neighbor hopping arising from direction-dependent pi-orbital overlap is the microscopic origin of spin splitting and altermagnetism. Biaxial compressive strain further enhances the spin splitting to 27 meV. These results establish a general approach to room-temperature organic altermagnets and open a pathway toward carbon-based altermagnetism via engineered inversion-symmetry breaking.

cond-mat.mtrl-sci↗

arXiv2026

Localized Exciton Emission with Spontaneous Circular Polarization in NiPS3/WSe2 Heterostructures

Two-dimensional (2D) van der Waals (vdW) heterostructures (HSs) provide a versatile platform for tailoring electronic, optical, and magnetic properties via proximity effects at their interfaces. In this work, we explore the optical response of few-layer NiPS3/WSe2 HSs using low-temperature micro-photoluminescence ({\mu}-PL) and magneto-PL spectroscopy. The HSs exhibit multiple sharp excitonic peaks that do not appear in the individual constituent materials, indicating the emergence of localized intralayer WSe2 excitons confined by interface-induced potentials. Notably, these excitons exhibit spontaneous circular polarization even in the absence of an external magnetic field, suggesting a magnetic proximity effect induced by uncompensated spins at the NiPS3 interface. Magneto-PL measurements further reveal nonlinear Zeeman splitting, consistent with the presence of an interfacial exchange field that alters the valley exciton dynamics. Density functional theory (DFT) calculations confirm the intralayer origin of the PL and reveal interfacial hybridization and spin texture modifications, supporting the experimental findings. These results highlight how combining a 2D semiconductor with a layered antiferromagnet enables control over valley polarization and spin degrees of freedom, offering new opportunities for chiral light sources and magnetically tunable optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Crystal Anisotropy Implications on the Magneto-Optical Properties of van der Waals FePS3

Antiferromagnetic FePS3 has recently gained significant interest in its potential applications in spin-related devices. Here, we show that in-plane structural anisotropy has a major impact in shaping the optical responses of FePS3 single-crystals from the bulk form down to the monolayer limit. X-ray diffraction on a bulk FePS3 crystal confirms a distorted FeS6 octahedron causing inequivalent Fe-Fe distances and consequently resulting in a higher a/b lattice parameter ratio. Micro-photoluminescence observations on bulk and monolayer FePS3 reveal four emissions: one intra-atomic d-d transition (band A, centered at ~1.24 eV) and three p-d charge transfer transitions (bands B, C, and D, centered around ~1.79 eV, ~2.3 eV, and ~2.56 eV, respectively). These bands exhibit different polarization behaviors, which persist down to the monolayer limit. Density functional theory calculations from bulk to monolayer FePS3 reveal the underlying electronic structure, assign the observed emissions, and indicate why these peaks have contrasting linear and circular polarization responses. These results establish a direct structure-optics relation in FePS3, highlighting the strong coupling between lattice anisotropy, electronic transitions, and symmetry-selective optical selection rules.

cond-mat.mtrl-sci↗

arXiv2025

Spin injection and emission helicity switching in a 2D perovskite/WSe2 heterostructure

The initialization and control of a long-lived spin population in lead halide perovskites are prerequisites for their use in spintronic applications. Here, we demonstrate circular polarization of the interlayer exciton emission in a (BA)2PbI4/WSe2 monolayer heterostructure. The helicity of this emission is controlled by tuning the energy of the excitation laser through the manifold of exciton resonances of the WSe2 monolayer, together with an emerging interlayer absorption feature of the heterostructure. Theoretical calculations show that this resonance arises from hybridized (BA)2PbI4/WSe2 states in the valence band. This hybrid character enables its observation in both linear absorption and ultrafast pump-probe spectroscopies, and plays a key role in controlling the sign of the helicity of the interlayer exciton emission. The tunable spin polarization demonstrated here, with the WSe2 monolayer effectively acting as a tunable spin filter, represents an important step toward the use of 2D perovskites in opto-spintronic applications.

cond-mat.mtrl-sci↗

arXiv2025

Edge-state competition in a 2D topological insulator-semiconductor heterostructure

Quantum spin Hall edge transport in two-dimensional transition-metal dichalcogenides depends on whether their one-dimensional edge channels are preserved under realistic substrates and device boundaries. Here we implement spin-orbit coupling in DFTB and GFN-xTB within the Amsterdam Modeling Suite, and apply it to 1T$'$/2H WSe$_2$ heterostructures. Edge-projected spectra reveal robust edge states in 1T$'$ ribbons; and these states remain robust against a laterally infinite 2H substrate, which only shifts the Dirac point via long-wavelength corrugation without introducing additional in-gap states. By contrast, terminated 2H edges generate trivial dispersion branches in the same energy window that hybridize only weakly with the topological edge modes. In the bulk, Fermi-level states are 1T$'$-derived; at the small twist angle, lattice-relaxation-induced strain drives miniband reconstruction, whereas at the large twist angle, the layers become electronically decoupled. These findings suggest the conditions -- controlled twist angle and avoidance of terminated 2H edges -- for achieving quantized conductance and unambiguous spectroscopic

cond-mat.mes-hall↗

arXiv2025

Hybrid d/p-wave altermagnetism in Ca$_{3}$Ru$_{2}$O$_{7}$ and strain-controlled spin splitting

The interplay of strong electronic correlations, sizable octahedral distortions, and pronounced spin-orbit coupling (SOC) makes perovskite oxides promising candidates for realizing altermagnetic phases. We study altermagnetic phases in Ca$_3$Ru$_2$O$_7$, a non-centrosymmetric layered perovskite whose ground state is a Kramers-degenerate antiferromagnet. We show that an alternative N\'eel-type spin arrangement hosts a P-2 d-wave altermagnetic state with orbital selectivity similar to Ca$_2$RuO$_4$. Including SOC generates a symmetry-allowed p-wave component and yields a hybrid d/p-wave altermagnetic order. We further demonstrate that biaxial strain tunes both magnetic stability and band splitting: compressive strain beyond 2 % favors the altermagnetic phase over the antiferromagnetic ground state, while tensile strain increases altermagnetic splittings by up to 9 %. To quantify these trends, we define an altermagnetic figure of merit and trace its strain dependence to changes in electronic localization and octahedral geometry in this polar metal.

cond-mat.mtrl-sci↗

arXiv2024

Interlayer Magnetic Coupling in FePS$_{3}$ and NiPS$_{3}$ Stacked Bilayers

Single layers of transition-metal thiophosphates (2D-TMPS$_{3}$) van der Waals magnets are an ideal platform for studying antiferromagnetic interactions in two dimensions. However, the magnetic coupling mechanism between two or more individual layers of these materials remains mostly unexplored. This study presents a density-functional based analysis and analytical models to describe the magnetic configurations of FePS$_{3}$ and NiPS$_{3}$ stacked bilayers. We explore the interplay between magnetic configurations and stacking shift, therefore identifying the mechanisms that result in either ferromagnetic or antiferromagnetic coupling between layers. Our findings indicate that the stacking with the lowest energy is metal-dependent, and the interlayer magnetic configuration (ferromagnetic or antiferromagnetic) varies based on the stacking type and the metal involved. Using an Ising-Hamiltonian model and a tight-binding model based on Wannier functions, we show that interlayer exchange interactions must be considered up to the third nearest neighbor and to elucidate the superexchange mechanism for the NiPS$_{3}$ system.

cond-mat.mtrl-sci↗

arXiv2024

Emergence of non-uniform strain induced exciton species in homo- and heterobilayer transition metal dichalcogenides

Full control of excitons in 2D materials is an important step to exploit them for applications. Straintronics is one method that can be used to effectively control the movement of excitons. Unfortunately, the effects of non-uniform strain in 2D materials are not yet well understood theoretically, although these strain fields can be present in experiments in the form of wrinkles, bubbles, and folds, or even explicitly applied to 2D materials through pre-patterned surfaces. The effects of these non-uniform strain fields on multilayers are even less studied due to the sheer size of these systems. In the present investigation, we study wrinkles that form in homo- and heterobilayers of 2D transition metal dichalcogenides using density functional theory. We show that the non-uniform strain leads to the formation of interlayer excitons in homobilayers of $ \mathrm WSe_2 $ and to exciton localization in heterobilayers of $ \mathrm WSe_2$-$ \mathrm MoSe_2$. Our results also reveal that the spin angular momentum is changed due to the mixing of in- and out-of-plane states which can explain the brightening of the formerly dark excitonic states under strain. Our results will pave the way towards a full understanding of the strain-control of excitons in 2D materials.

cond-mat.mtrl-sci↗

arXiv2023

Funneling and spin-orbit coupling in transition-metal dichalcogenide nanotubes and wrinkles

Strain engineering provides a powerful means to tune the properties of two-dimensional materials. Accordingly, numerous studies have investigated the effect of bi- and uniaxial strain. Yet, the strain fields in many systems such as nanotubes and nanoscale wrinkles are intrinsically inhomogeneous and the consequences of this symmetry breaking are much less studied. Understanding how this affects the electronic properties is crucial especially since wrinkling is a powerful method to apply strain to two-dimensional materials in a controlled manner. In this paper, we employ density functional theory to understand the correlation between the atomic and the electronic structure in nanoscale wrinkles and nanotubes of the prototypical transition metal dichalcogenide $\mathrm{WSe}_2$. Our research shows that the symmetry breaking in these structures leads to strong Rashba-like splitting of the bands at the $\Gamma$ point and they thus may be utilized in future tunable spintronic devices. The inhomogeneous strain reduces the band gap and leads to a localization of the band edges in the highest-curvature region, thus funneling excitons there. Moreover, we show how wrinkles can be modeled as nanotubes with the same curvature and when this comparison breaks down and further inhomogenities have to be taken into account.

cond-mat.mtrl-sci↗

arXiv2023

Edge conductivity in PtSe$_2$ nanostructures

PtSe$_2$ is a promising 2D material for nanoelectromechanical sensing and photodetection in the infrared regime. One of its most compelling features is the facile synthesis at temperatures below 500 {\deg}C, which is compatible with current back-end-of-line semiconductor processing. However, this process generates polycrystalline thin films with nanoflake-like domains of 5 to 100 nm size. To investigate the lateral quantum confinement effect in this size regime, we train a deep neural network to obtain an interatomic potential at DFT accuracy and use that to model ribbons, surfaces, nanoflakes, and nanoplatelets of PtSe$_2$ with lateral widths between 5 to 15 nm. We determine which edge terminations are the most stable and find evidence that the electrical conductivity is localized on the edges for lateral sizes below 10 nm. This suggests that the transport channels in thin films of PtSe$_2$ might be dominated by networks of edges, instead of transport through the layers themselves.

cond-mat.mtrl-sci↗

arXiv2022

Electron Holographic Mapping of Structural and Electronic Reconstruction at Mono- and Bilayer Steps of h-BN

Here, by making use of medium and high resolution autocorrected off-axis electron holography, we directly probe the electrostatic potential as well as in-plane and out-of-plane charge delocalization at edges and steps in multilayer hexagonal boron nitride. In combination with ab-initio calculations, the data allows to directly reveal the formation of out-of-plane covalent bonds at folded zig-zag edges and steps comprising two monolayers and the absence of which at monolayer steps. The technique paves the way for studying other charge (de)localization phenomena in 2D materials, e.g., at polar edges, topological edge states and defects.

cond-mat.mtrl-sci↗

arXiv2021

Stacking polymorphism in PtSe$_2$ drastically affects its electromechanical properties

PtSe$_2$ is one of the most promising materials for the next generation of piezoresistive sensors. However, the large-scale synthesis of homogeneous thin films with reproducible electromechanical properties is challenging due to polycrystallinity. We show that stacking phases other than the AA-stacking in the 1T phase become thermodynamically available at elevated temperatures. We show that these can make up a significant fraction in a polycrystalline thin film and discuss methods to characterize these stacking phases. Lastly, we estimate their gauge factors, which vary strongly and significantly impact the performance of a nanoelectromechanical device.

cond-mat.mtrl-sci↗

arXiv2021

Non-Equilibrium First-Order Exciton Mott Transition at Monolayer Lateral Heterojunctions Visualized by Ultrafast Microscopy

Atomically precise lateral heterojunctions based on transition metal dichalcogenides provide a new platform for exploring exciton Mott transition in one-dimension. To investigate the intrinsically non-equilibrium Mott transition, we employed ultrafast microscopy with ~ 200 fs temporal resolution to image the transport of different exciton phases in a type II WSe2-WS1.16Se0.84 lateral heterostructure. These measurements visualized the extremely rapid expansion of a highly non-equilibrium electron-hole (e-h) plasma phase with a Fermi velocity up to 3.2*10^6 cm*s-1. An abrupt first-order exciton Mott transition at a density of ~ 5*10^12 cm-2 at room temperature was revealed by ultrafast microscopy, which could be disguised as a continuous transition in conventional steady-state measurements. These results point to exciting new opportunities for designing atomically thin lateral heterojunctions as novel highways of excitons and collective e-h plasma for high-speed electronic applications.

cond-mat.mes-hall↗

arXiv2021

Electronic Structures of Two-Dimensional PC6-Type Materials

Two-dimensional (2D) materials may exhibit intriguing band structure features (e.g., Dirac points), that lay far away from the Fermi level. They are, thus, not usable in applications. The semiconducting 2D material PC6 has two Dirac cones above and below the Fermi level. Therefore, it is an ideal playground to demonstrate chemical functionalization methods for shifting the Fermi level in order to access interesting band structure features. PC6 is based on the sqrt(7) x sqrt(7)R19.1deg super cell of graphene with two carbon atoms per unit cell substituted by phosphorous. It is demonstrated how substitution with other heteroatoms that contain a different number of valence electrons, the Dirac points can be accessed. Alternatively, hydrogen atoms can be used as adatoms at the heteroatom sites. This increases electron filling and shifts the Fermi level upwards.

cond-mat.mtrl-sci↗

arXiv2021

Electrical control of orbital and vibrational interlayer coupling in bi- and trilayer 2H-MoS$_2$

Manipulating electronic interlayer coupling in layered van der Waals (vdW) materials is essential for designing opto-electronic devices. Here, we control vibrational and electronic interlayer coupling in bi- and trilayer 2H-MoS$_2$ using large external electric fields in a micro-capacitor device. The electric field lifts Raman selection rules and activates phonon modes in excellent agreement with ab-initio calculations. Through polarization resolved photoluminescence spectroscopy in the same device, we observe a strongly tunable valley dichroism with maximum circular polarization degree of $\sim 60\%$ in bilayer and $\sim 35\%$ in trilayer MoS$_2$ that are fully consistent with a rate equation model which includes input from electronic band structure calculations. We identify the highly delocalized electron wave function between the layers close to the high symmetry $Q$ points as the origin of the tunable circular dichroism. Our results demonstrate the possibility of electric field tunable interlayer coupling for controlling emergent spin-valley physics and hybridization driven effects in vdW materials and their heterostructures.

cond-mat.mes-hall↗

arXiv2020

Strong band-filling-dependence of the scattering lifetime in gated MoS2 nanolayers induced by the opening of intervalley scattering channels

Gated molybdenum disulphide (MoS2) exhibits a rich phase diagram upon increasing electron doping, including a superconducting phase, a polaronic reconstruction of the bandstructure, and structural transitions away from the 2H polytype. The average time between two charge-carrier scattering events - the scattering lifetime - is a key parameter to describe charge transport and obtain physical insight in the behavior of such a complex system. In this work, we combine the solution of the Boltzmann transport equation (based on ab-initio density functional theory calculations of the electronic bandstructure) with the experimental results concerning the charge-carrier mobility, in order to determine the scattering lifetime in gated MoS2 nanolayers as a function of electron doping and temperature. From these dependencies, we assess the major sources of charge-carrier scattering upon increasing band filling, and discover two narrow ranges of electron doping where the scattering lifetime is strongly suppressed. We indentify the opening of additional intervalley scattering channels connecting the simultaneously-filled K/K' and Q/Q' valleys in the Brillouin zone as the source of these reductions, which are triggered by the two Lifshitz transitions induced by the filling of the high-energy Q/Q' valleys upon increasing electron doping.

cond-mat.mes-hall↗

arXiv2020

Artificial Relativistic Molecules

We fabricate artificial molecules composed of heavy atom lead on a van der Waals crystal. Pb atoms templated on a honeycomb charge-order superstructure of IrTe2 form clusters ranging from dimers to heptamers including benzene-shaped ring hexamers. Tunneling spectroscopy and electronic structure calculations reveal the formation of unusual relativistic molecular orbitals within the clusters. The spin-orbit coupling is essential both in forming such Dirac electronic states and stabilizing the artificial molecules by reducing the adatom-substrate interaction. Lead atoms are found to be ideally suited for a maximized relativistic effect. This work initiates the use of novel two dimensional orderings to guide the fabrication of artificial molecules of unprecedented properties.

cond-mat.mtrl-sci↗