arXiv subjects

Laurenz Rettig

Publications and source records attributed to Laurenz Rettig.

At least 19 recordsLinked to original sources

arXiv2026

Framework for an AI-Ready ARPES Community Database

Condensed matter stands to gain profoundly from widespread adoption of artificial intelligence (AI). However, its current means of data organization impedes this endeavor. As a premier measure of electronic structure underlying material properties, Angle-Resolved Photoemission Spectroscopy (ARPES) has accumulated over four decades of spectra, yet the community's publication-centered workflow preserves only a highly selected fraction of its experimental record. A shared data ecosystem could transform these fragmented measurements and their contexts into a persistent, collective scientific memory, creating immediate value for reproducibility and reuse while laying the foundation for AI-enabled discovery. In this Perspective, we report outcomes of a recent community workshop and propose a practical path toward such an ecosystem. Its benefits unfold along three timescales. In the near term, standardized, searchable, and citable datasets strengthen analysis pipelines independently of AI. In the intermediate future, community-validated tools operating across laboratories could enable broader reuse and increasingly closed-loop automated experiments. In the long term, a diverse corpus of measured electronic spectra could support foundation models for quantum matter. Looking forward, a diverse corpus of measured electronic spectra could support foundation models for quantum matter and new discoveries. We discuss lessons from existing scientific databases, the current state of AI in ARPES, as well as areas of community convergence on data organization, access, credit, governance, and a staged pilot program.

cond-mat.mtrl-sci↗

arXiv2026

Ultrafast Formation and Annihilation of Strongly Bound, Anisotropic Excitons

Van der Waals (vdW) layered materials with long-range magnetic order have the potential to enable novel optoelectronic and spintronic applications. Among these, CrSBr is an air-stable, direct band gap semiconductor that hosts interlayer antiferromagnetic order, a highly anisotropic electronic structure, and strongly bound excitons. In particular, excitons in CrSBr have been shown to inherit the quasi-one-dimensional nature of the material and also couple to the underlying spinorder. However, mechanisms of exciton formation, dissociation, and interaction with free carriers remain largely unexplored, despite being crucial for spintronic and optoelectronic applications. Here, we employ time- and angle-resolved photoemission spectroscopy to map the electronic structure and excited state dynamics in CrSBr. We directly resolve an exceptionally large exciton binding energy (~800 meV) and a highly anisotropic momentum space distribution of the exciton, revealing its quasi-1D real-space character. We observe an excitation-density-dependent interconversion between bound excitons and quasi-free carriers on sub- to few-picosecond timescales, indicating that many-body effects govern the excited-state dynamics and optical properties during the initial stages of relaxation. Our work highlights the strongly bound, anisotropic character of excitons in CrSBr, as well as the microscopic interactions steering relaxation pathways after photoexcitation in elevated density regimes relevant for future device applications.

cond-mat.mtrl-sci↗

arXiv2026

Orbital mixing and strong Hund's coupling stabilize spin order in van der Waals ferromagnet CrI3

Recent years have seen a vast increase in research into van der Waals magnetic materials. In many of these systems, magnetism is introduced via light 3d-transition metal elements, combined with chalcogenides or halogens. Despite the high technological promise in the field of spintronics, the connection between the d-orbital configuration and the occurrence of low-dimensional magnetic order is currently unclear. Here we address the prototypical two-dimensional ferromagnet CrI3, via complementary spectroscopies and density functional theory calculations. We reveal the electronic structure and orbital character of bulk CrI3 in the paramagnetic and ferromagnetic phases, describing the couplings underpinning its energy diagram, and providing a robust experimental demonstration that the stabilization of ferromagnetism is attributable to orbital mixing between I p and Cr eg states, and to the presence of strong Hund's coupling. These findings reveal the microscopic connection between orbital and spin degrees of freedom, providing fundamental insights into the behavior of low-dimensional magnetic materials.

cond-mat.mtrl-sci↗

arXiv2026

Nanoscale Confinement Enhances Ultrafast Demagnetization

Nanoscale miniaturization has revolutionized the field of spintronics by enabling exponential growth in areal bit density. A similar leap is also expected in device speeds through successfully harnessing femtosecond magnetization dynamics. However, combining this with the miniaturization of realistic devices is challenging. To address this, we studied the effect of dimensional confinement on the femtosecond demagnetization of Fe. By gradually increasing the level of confinement while keeping excitation conditions constant, we found that Fe layers thinner than 10 nm exhibit enlarged demagnetization amplitudes, reaching a $\sim75\%$ increase at 2 nm. By combining ultrafast experiments sensitive to the spins, the charge carriers, and the phonons, we establish that this finite$\text{-}$size effect is magnetic in origin and is not phonon$\text{-}$driven. With the support of ab$\text{-}$initio calculations and atomistic spin dynamics simulations, we identify the enhancement effect as due to local weakening of spin order at the Fe$\text{'}$s interface, which becomes significant upon increased confinement.

cond-mat.mes-hall↗

arXiv2026

Ultrafast nonlinear Hall effect in black phosphorus

The nonlinear Hall effect (NHE) is a recently discovered member of the Hall effect family in which the Hall voltage shows a nonlinear behavior when a transverse electric field is applied. While the NHE does not require broken time-reversal symmetry, such as that induced by a magnetic field, it requires broken inversion symmetry, which limits the range of suitable systems and potential applications. Here, we demonstrate an ultrafast NHE in centrosymmetric black phosphorus through dynamical symmetry breaking using femtosecond light pulses. We provide a detailed microscopic picture of excited carrier dynamics and induced fields using momentum-resolved photoemission spectroscopy combined with \textit{ab-initio} calculations. The ultrafast NHE is observed exclusively for the light polarization aligned with the armchair high-symmetry direction and persists over 300 fs, which opens new possibilities for selective and ultrafast light-to-current conversions.

cond-mat.mtrl-sci↗

arXiv2025

pynxtools: A Python framework for generating and validating NeXus files in experimental data workflows

Scientific data across physics, materials science, and materials engineering often lacks adherence to FAIR principles (Barker et al., 2022; Jacobsen et al., 2020; M. D. Wilkinson et al., 2016; S. R. Wilkinson et al., 2025) due to incompatible instrument-specific formats and diverse standardization practices. pynxtools is a Python software development framework with a command line interface (CLI) that standardizes data conversion for scientific experiments in materials science to the NeXus format (Klosowski et al., 1997; Könnecke, 2006; Könnecke et al., 2015) across diverse scientific domains. NeXus defines data storage specifications for different experimental techniques through application definitions. pynxtools provides a fixed, versioned set of NeXus application definitions that ensures convergence and alignment in data specifications across, among others, atom probe tomography, electron microscopy, optical spectroscopy, photoemission spectroscopy, scanning probe microscopy, and X-ray diffraction. Through its modular plugin architecture pynxtools provides conversion of data and metadata from instruments and electronic lab notebooks to these unified definitions, while performing validation to ensure data correctness and NeXus compliance. pynxtools can be integrated directly into Research Data Management Systems (RDMS) to facilitate parsing and normalization. We detail one example for the RDM system NOMAD. By simplifying the adoption of NeXus, the framework enables true data interoperability and FAIR data management across multiple experimental techniques.

cond-mat.mtrl-sci↗

arXiv2025

Conduction Band Structure and Ultrafast Dynamics of Ferroelectric $α$-GeTe(111)

$α$-GeTe(111) is a non-centrosymmetric ferroelectric (FE) material for which a significative lattice distortion combined with a strong spin-orbit interaction gives rise to giant Rashba split states in the bulk and at the surface, which have been intensively probed in the occupied valence states using static angle-resolved photoemission spectroscopy (ARPES). Nevertheless, its unoccupied conduction band structure remains unexplored, in particular the experimental determination of its electronic band gap across momentum space. Using time-resolved ARPES based on high-repetition rate and extreme ultraviolet femtosecond (fs) laser, we unveil the band structure of $α$-GeTe(111) in the full Brillouin zone, both in the valence and conduction states, as well as the exploration of its out-of-equilibrium dynamics. Our work confirms the semiconducting nature of $α$-GeTe(111) with a 0.85 eV indirect band gap, which provides an upper limit for comparison to density functional theory calculations. We finally reveal the dominant scattering mechanisms of photoexcited carriers during the out-of-equilibrium dynamics under fs light pulses.

cond-mat.mtrl-sci↗

arXiv2025

Ultrafast demagnetization dynamics of 4f antiferromagnets

We study the ultrafast demagnetization dynamics of LnRh$_2$Si$_2$ (Ln $=$ Pr, Nd, Sm, Gd, Tb, Dy, Ho) antiferromagnets (AFM) after excitation by a laser pulse, using a combination of density functional theory and atomistic spin and spin-lattice dynamics simulations. First, we calculate the Heisenberg interactions using the magnetic force theorem and compare two approaches, where the $4f$ states of the rare earths are treated as frozen core states or as valence states with added correlation corrections. We find marked quantitative differences in terms of predicted Curie temperature for most of the systems, especially for those with large orbital moment of the rare earth cations. This can be attributed to the importance of indirect interactions of the $4f$ states through the Si states, which depend on the binding energy of the $4f$ states and coexists with RKKY-type interactions mediated by the conduction states. However, qualitatively, both approaches agree in terms of the predicted AFM ordering at low temperatures. In the second step, the atomistic dynamics simulations are combined with a heat-conserving two-temperature model, allowing for the calculation of spin and electronic temperatures during the magnetization dynamics simulations. Despite quite different demagnetization times, magnetization dynamics of all studied LnRh$_2$Si$_2$ AFM exhibit similar two-step behavior, in particular, the first fast drop followed by slower demagnetization. We observe that the demagnetization amplitude depends linearly on laser fluence for low fluences, which is in agreement with experimental observations. We also investigate the impact of lattice dynamics on ultrafast demagnetization using coupled atomistic spin-lattice dynamics simulations and a heat-conserving three-temperature model, which confirm linear dependence of magnetisation on laser fluence.

cond-mat.mtrl-sci↗

arXiv2025

The 2025 Roadmap to Ultrafast Dynamics: Frontiers of Theoretical and Computational Modelling

The exploration of ultrafast phenomena is a frontier of condensed matter research, where the interplay of theory, computation, and experiment is unveiling new opportunities for understanding and engineering quantum materials. With the advent of advanced experimental techniques and computational tools, it has become possible to probe and manipulate nonequilibrium processes at unprecedented temporal and spatial resolutions, providing insights into the dynamical behavior of matter under extreme conditions. These capabilities have the potential to revolutionize fields ranging from optoelectronics and quantum information to catalysis and energy storage. This Roadmap captures the collective progress and vision of leading researchers, addressing challenges and opportunities across key areas of ultrafast science. Contributions in this Roadmap span the development of ab initio methods for time-resolved spectroscopy, the dynamics of driven correlated systems, the engineering of materials in optical cavities, and the adoption of FAIR principles for data sharing and analysis. Together, these efforts highlight the interdisciplinary nature of ultrafast research and its reliance on cutting-edge methodologies, including quantum electrodynamical density-functional theory, correlated electronic structure methods, nonequilibrium Green's function approaches, quantum and ab initio simulations.

cond-mat.mtrl-sci↗

arXiv2024

Frontier orbitals control dynamical disorder in molecular semiconductors

Charge transport in organic semiconductors is limited by dynamical disorder. Design rules for new high-mobility materials have therefore focused on limiting its two foundations: structural fluctuations and the transfer integral gradient. However, it has remained unclear how these goals should be translated into molecular structures. Here we show that a specific shape of the frontier orbital, with a lack of nodes along the long molecular axis, reduces the transfer integral gradient and therefore the dynamical disorder. We investigated single crystals of the prototypical molecular semiconductors pentacene and picene by angle-resolved photoemission spectroscopy and dynamical disorder calculations. We found that picene exhibits a remarkably low dynamical disorder. By separating in- and out-of-plane components of dynamical disorder, we identify the reason as a reduced out-of-plane disorder from a small transfer integral derivative. Our results demonstrate that molecules with an armchair $π$-electron topology and same-phase frontier orbitals like picene are promising molecular building blocks for the next generation of organic semiconductors.

cond-mat.mtrl-sci↗

arXiv2024

Controlling 4f antiferromagnetic dynamics via itinerant electronic susceptibility

Optical manipulation of magnetism holds promise for future ultrafast spintronics, especially with lanthanides and their huge, localized 4f magnetic moments. These moments interact indirectly via the conduction electrons (RKKY exchange), influenced by interatomic orbital overlap, and the conduction electron susceptibility. Here, we study this influence in a series of 4f antiferromagnets, GdT2Si2 (T=Co, Rh, Ir), using ultrafast resonant X-ray diffraction. We observe a twofold increase in ultrafast angular momentum transfer between the materials, originating from modifications in the conduction electron susceptibility, as confirmed by first-principles calculations.

cond-mat.mtrl-sci↗

arXiv2023

Berry Curvature Signatures in Chiroptical Excitonic Transitions

The topology of the electronic band structure of solids can be described by its Berry curvature distribution across the Brillouin zone. We theoretically introduce and experimentally demonstrate a general methodology based on the measurement of energy- and momentum-resolved optical transition rates, allowing to reveal signatures of Berry curvature texture in reciprocal space. By performing time- and angle-resolved photoemission spectroscopy of atomically thin WSe$_2$ using polarization-modulated excitations, we demonstrate that excitons become an asset in extracting the quantum geometrical properties of solids. We also investigate the resilience of our measurement protocol against ultrafast scattering processes following direct chiroptical transitions.

cond-mat.mtrl-sci↗

arXiv2023

Orbital-resolved Observation of Singlet Fission

Singlet fission may boost photovoltaic efficiency [by transforming a singlet exciton into two triplet excitons and thereby doubling the number of excited charge carriers. The primary step of singlet fission is the ultrafast creation of the correlated triplet pair. While several mechanisms have been proposed to explain this step, none has emerged as a consensus. The challenge lies in tracking the transient excitonic states. Here we use time- and angle-resolved photoemission spectroscopy to observe the primary step of singlet fission in crystalline pentacene. Our results suggest a charge-transfer mediated mechanism with a hybridization of Frenkel and charge-transfer states in the lowest bright singlet exciton. We gained intimate knowledge about the localization and the orbital character of the exciton wave functions recorded in momentum maps. This allowed us to directly compare the localization of singlet and bitriplet excitons and decompose energetically overlapping states based on their orbital character. Orbital- and localization- resolved many-body dynamics promise deep insights into the mechanics governing molecular systems and topological materials.

cond-mat.mtrl-sci↗

arXiv2022

Observation of multi-directional energy transfer in a hybrid plasmonic-excitonic nanostructure

Hybrid plasmonic devices involve a nanostructured metal supporting localized surface plasmons to amplify light-matter interaction, and a non-plasmonic material to functionalize charge excitations. Application-relevant epitaxial heterostructures, however, give rise to ballistic ultrafast dynamics that challenge the conventional semiclassical understanding of unidirectional nanometal-to-substrate energy transfer. We study epitaxial Au nanoislands on WSe$_2$ with time- and angle-resolved photoemission spectroscopy and femtosecond electron diffraction: this combination of techniques resolves material, energy and momentum of charge-carriers and phonons excited in the heterostructure. We observe a strong non-linear plasmon-exciton interaction that transfers the energy of sub-bandgap photons very efficiently to the semiconductor, leaving the metal cold until non-radiative exciton recombination heats the nanoparticles on hundreds of femtoseconds timescales. Our results resolve a multi-directional energy exchange on timescales shorter than the electronic thermalization of the nanometal. Electron-phonon coupling and diffusive charge-transfer determine the subsequent energy flow. This complex dynamics opens perspectives for optoelectronic and photocatalytic applications, while providing a constraining experimental testbed for state-of-the-art modelling.

cond-mat.mes-hall↗

arXiv2022

A machine learning route between band mapping and band structure

Electronic band structure (BS) and crystal structure are the two complementary identifiers of solid state materials. While convenient instruments and reconstruction algorithms have made large, empirical, crystal structure databases possible, extracting quasiparticle dispersion (closely related to BS) from photoemission band mapping data is currently limited by the available computational methods. To cope with the growing size and scale of photoemission data, we develop a pipeline including probabilistic machine learning and the associated data processing, optimization and evaluation methods for band structure reconstruction, leveraging theoretical calculations. The pipeline reconstructs all 14 valence bands of a semiconductor and shows excellent performance on benchmarks and other materials datasets. The reconstruction uncovers previously inaccessible momentum-space structural information on both global and local scales, while realizing a path towards integration with materials science databases. Our approach illustrates the potential of combining machine learning and domain knowledge for scalable feature extraction in multidimensional data.

physics.data-an↗

arXiv2022

Relaxation of photo-excited hot carriers beyond multi-temperature models: General theory description verified by experiments on Pb/Si(111)

The equilibration of electronic carriers in metals after excitation by an ultra-short laser pulse provides an important class of non-equilibrium phenomena in metals and allows measuring the effective electron-phonon coupling parameter. Since the observed decay of the electronic distribution is governed by the interplay of both electron-electron and electron-phonon scattering, the interpretation of experimental data must rely on models that ideally should be easy to handle, yet accurate. In this work, an extended rate-equation model is proposed that explicitly includes non-thermal electronic carriers while at the same time incorporating data from first-principles calculations of the electron-phonon coupling via Eliashberg-Migdal theory. The model is verified against experimental data for thin Pb films grown on Si(111). Improved agreement between theory and experiment at short times (<0.3ps) due to non-thermal electron contributions is found. Moreover, the rate equations allow for widely different coupling strength to different phonon subsystems. Consequently, an indirect, electron-mediated energy transfer between strongly and weakly coupled groups of phonons can be observed in the simulations that leads to a retarded equilibration of the subsystems only after several picoseconds.

cond-mat.mtrl-sci↗

arXiv2022

Robust magnetic order upon ultrafast excitation of an antiferromagnet

The ultrafast manipulation of magnetic order due to optical excitation is governed by the intricate flow of energy and momentum between the electron, lattice and spin subsystems. While various models are commonly employed to describe these dynamics, a prominent example being the microscopic three temperature model (M3TM), systematic, quantitative comparisons to both the dynamics of energy flow and magnetic order are scarce. Here, we apply a M3TM to the ultrafast magnetic order dynamics of the layered antiferromagnet GdRh$_2$Si$_2$. The femtosecond dynamics of electronic temperature, surface ferromagnetic order, and bulk antiferromagnetic order were explored at various pump fluences employing time- and angle-resolved photoemission spectroscopy and time-resolved resonant magnetic soft x-ray diffraction, respectively. After optical excitation, both the surface ferromagnetic order and the bulk antiferromagnetic order dynamics exhibit two-step demagnetization behaviors with two similar timescales (<1 ps, ~10 ps), indicating a strong exchange coupling between localized 4f and itinerant conduction electrons. Despite a good qualitative agreement, the M3TM predicts larger demagnetization than our experimental observation, which can be phenomenologically described by a transient, fluence-dependent increased Néel temperature. Our results indicate that effects beyond a mean-field description have to be considered for a quantitative description of ultrafast magnetic order dynamics.

cond-mat.str-el↗

arXiv2022

Observation of ultrafast interfacial Meitner-Auger energy transfer in a van der Waals heterostructure

Atomically thin layered van der Waals heterostructures feature exotic and emergent optoelectronic properties. With growing interest in these novel quantum materials, the microscopic understanding of fundamental interfacial coupling mechanisms is of capital importance. Here, using multidimensional photoemission spectroscopy, we provide a layer- and momentum-resolved view on ultrafast interlayer electron and energy transfer in a monolayer-WSe$_2$/graphene heterostructure. Depending on the nature of the optically prepared state, we find the different dominating transfer mechanisms: while electron injection from graphene to WSe$_2$ is observed after photoexcitation of quasi-free hot carriers in the graphene layer, we establish an interfacial Meitner-Auger energy transfer process following the excitation of excitons in WSe$_2$. By analysing the time-energy-momentum distributions of excited-state carriers with a rate-equation model, we distinguish these two types of interfacial dynamics and identify the ultrafast conversion of excitons in WSe$_2$ to valence band transitions in graphene. Microscopic calculations find interfacial dipole-monopole coupling underlying the Meitner-Auger energy transfer to dominate over conventional Förster- and Dexter-type interactions, in agreement with the experimental observations. The energy transfer mechanism revealed here might enable new hot-carrier-based device concepts with van der Waals heterostructures.

cond-mat.mtrl-sci↗