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David Maximilian Janas

Publications and source records attributed to David Maximilian Janas.

4 recordsLinked to original sources

Excitonic optical interface for GHz-THz collective excitations in a van der Waals magnet

Collective spin and lattice excitations in quantum materials span energy scales from GHz to THz, yet establishing a unified optical interface for these modes remains a central challenge. Here we show that excitonic resonances in the van der Waals antiferromagnet CrSBr provide a broadband optical interface for such excitations. Using femtosecond broadband transient reflectivity, we resolve coherent GHz magnon and THz phonon modes that modulate the dielectric response over a wide spectral range. Despite their distinct microscopic origin and frequency scales, both excitations give rise to the same emergent optical signature: a resonance at 1.46 eV that is absent in steady-state spectra and exhibits a characteristic π-phase inversion, identifying it as a discrete excitonic transition. We attribute this behaviour to boson-driven modulation of the dielectric response, which transiently transfers spectral weight from a nominally dark exciton into an observable channel without requiring a finite equilibrium oscillator strength. Supported by many-body calculations, we assign this feature to a higher-energy exciton with distinct momentum and orbital character and strongly suppressed optical matrix elements. These results establish excitonic resonances in van der Waals magnets as a platform for interfacing collective excitations across GHz, THz and optical frequency scales.

cond-mat.mtrl-sci↗

Momentum-Resolved Electronic Structure and Orbital Hybridization in the Layered Antiferromagnet CrPS$_4$

Chromium thiophosphate (CrPS$_4$) is a layered two-dimensional antiferromagnetic semiconductor exhibiting intriguing spintronic and magneto-optical properties, yet its electronic band structure has remained experimentally uncharacterized. Here, we employ momentum-resolved photoemission spectroscopy above and below the Néel temperature, complemented by density functional theory with Hubbard U corrections (DFT+U), to reveal a valence band dominated by Cr $3d$ and S $3p$ states with a ligand-to-metal charge-transfer band gap. We identify weakly hybridized t$_{2g}$ orbitals responsible for magnetic ordering and strongly hybridized e$_{g}$ orbitals that relax dipole selection rules, enabling optically active orbital transitions. These findings establish a foundational understanding of CrPS$_4$'s electronic structure, providing a benchmark for theoretical models and informing future investigations into its orbital physics and potential device applications.

cond-mat.mtrl-sci↗

Metalloporphyrins on Oxygen-Passivated Iron: Conformation and Order Beyond the First Layer

On-surface metal porphyrins can undergo electronic and conformational changes that play a crucial role in determining the chemical reactivity of the molecular layer. Therefore, understanding those properties is pivotal for the design and implementation of organic-based devices. Here, by means of photoemission orbital tomography supported by density functional theory calculations, we investigate the electronic and geometrical structure of two metallated tetraphenyl porphyrins (MTPPs), namely ZnTPP and NiTPP, adsorbed on the oxygen-passivated Fe(100)-p(1x1)O surface. Both molecules weakly interact with the surface as no charge transfer is observed. In the case of ZnTPP our data correspond to those of moderately distorted molecules, while NiTPP exhibits a severe saddle-shape deformation. From additional experiments on NiTPP multilayer films, we conclude that this distortion is a consequence of the interaction with the substrate, as the NiTPP macrocycle of the second layer turns out to be flat. We further find that distortions in the MTPP macrocycle are accompanied by an increasing energy gap between the highest occupied molecular orbitals (HOMO and HOMO-1). Our results demonstrate that photoemission orbital tomography can simultaneously probe the energy level alignment, the azimuthal orientation, and the adsorption geometry of complex aromatic molecules even in the multilayer regime.

cond-mat.mtrl-sci↗

Dirac bands in the topological insulator Bi2Se3 mapped by time-resolved momentum microscopy

We have studied the energy dispersion of the Dirac bands of the topological insulator Bi2Se3 at large parallel momenta using a setup for laser-based time-resolved momentum microscopy with 6 eV probe-photons. Using this setup, we can probe the manifold of unoccupied states up to higher intermediate-state energies in a wide momentum window. We observe a strongly momentum-dependent evolution of the topologically protected Dirac states into a conduction band resonance, highlighting the anisotropy dictated by the surface symmetry. Our results are in remarkable agreement with the theoretical surface spectrum obtained from a GW-corrected tight-binding model, suggesting the validity of the approach in the prediction of the quasiparticle excitation spectrum of large systems with non-trivial topology. After photoexcitation with 0.97 eV photons, assigned to a bulk valence band-conduction band transition, the out-of-equilibrium population of the surface state evolves on a multi-picosecond time scale, in agreement with a simple thermodynamical model with a fixed number of particles, suggesting a significant decoupling between bulk and surface states.

cond-mat.mtrl-sci↗