arXiv subjects

Michael Schüler

Publications and source records attributed to Michael Schüler.

At least 37 records · Page 2Linked to original sources

arXiv2024

First-principle tight-binding approach to angle-resolved photoemission spectroscopy simulations: importance of light-matter gauge and ubiquitous interference effects

Angle-resolved photoemission spectroscopy (ARPES) is one of the most powerful techniques to study the electronic structure of materials. To go beyond the paradigm of band mapping and extract aspects of the Bloch wave-functions, the intricate interplay of experimental geometry, crystal structure, and photon polarization needs to be understood. In this work we discuss several model approaches to computing ARPES signals in a unified fashion. While we represent the Bloch wave-functions by first-principle Wannier functions, we introduce different approximations to the final states and discuss the implications for the predictive power. We also introduce various light-matter gauges and explain the role of the inevitable breaking of gauge invariance.Finally, we benchmark the different models for the two-dimensional semiconductor WSe$_2$, known for its strong Berry curvature, orbital angular momentum (OAM), and nontrivial orbital texture. The models are compared based on their ability to simulate photoemission intensity and interpret circular dichroism in ARPES (CD-ARPES). We show that interference effects are crucial to understanding the circular dichroism, and explain their photon-energy dependence. Our in-depth analysis provides insights into the advantages and limitations of various model approaches in clarifying the complex interplay between experimental observables and underlying orbital texture in materials.

cond-mat.mtrl-sci↗

arXiv2023

Controllable orbital angular momentum monopoles in chiral topological semimetals

The emerging field of orbitronics aims at generating and controlling currents of electronic orbital angular momentum (OAM) for information processing. Structurally chiral topological crystals could be particularly suitable orbitronic materials because they have been predicted to host topological band degeneracies in reciprocal space that are monopoles of OAM. Around such a monopole, the OAM is locked isotopically parallel or antiparallel to the direction of the electron's momentum, which could be used to generate large and controllable OAM currents. However, OAM monopoles have not yet been directly observed in chiral crystals, and no handle to control their polarity has been discovered. Here, we use circular dichroism in angle-resolved photoelectron spectroscopy (CD-ARPES) to image OAM monopoles in the chiral topological semimetals PtGa and PdGa. Moreover, we also demonstrate that the polarity of the monopole can be controlled via the structural handedness of the host crystal by imaging OAM monopoles and anti-monopoles in the two enantiomers of PdGa, respectively. For most photon energies used in our study, we observe a sign change in the CD-ARPES spectrum when comparing positive and negative momenta along the light direction near the topological degeneracy. This is consistent with the conventional view that CD-ARPES measures the projection of the OAM monopole along the photon momentum. For some photon energies, however, this sign change disappears, which can be understood from our numerical simulations as the interference of polar atomic OAM contributions, consistent with the presence of OAM monopoles. Our results highlight the potential of chiral crystals for orbitronic device applications, and our methodology could enable the discovery of even more complicated nodal OAM textures that could be exploited for orbitronics.

cond-mat.str-el↗

arXiv2023

Spin-orbit interaction driven terahertz nonlinear dynamics in transition metals

The interplay of electric charge, spin, and orbital polarizations, coherently driven by picosecond long oscillations of light fields in spin-orbit coupled systems, is the foundation of emerging terahertz spintronics and orbitronics. The essential rules for how terahertz light interacts with these systems in a nonlinear way are still not understood. In this work, we demonstrate a universally applicable electronic nonlinearity originating from spin-orbit interactions in conducting materials, wherein the interplay of light-induced spin and orbital textures manifests. We utilized terahertz harmonic generation spectroscopy to investigate the nonlinear dynamics over picosecond timescales in various transition metal films. We found that the terahertz harmonic generation efficiency scales with the spin Hall conductivity in the studied films, while the phase takes two possible values (shifted by π), depending on the d-shell filling. These findings elucidate the fundamental mechanisms governing non-equilibrium spin and orbital polarization dynamics at terahertz frequencies, which is relevant for potential applications of terahertz spin- and orbital-based devices.

physics.app-ph↗

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

Suppression of Heating by Multi-color Driving Protocols in Floquet Engineered Strongly Correlated Systems

Heating effects in Floquet engineered system are detrimental to the control of physical properties. In this work, we show that the heating of periodically driven strongly correlated systems can be suppressed by multi-color driving, i.e., by applying auxiliary excitations which interfere with the absorption processes from the main drive. We focus on the Mott insulating single-band Hubbard model and study the effects of multi-color driving with nonequilibrium dynamical mean-field theory. The main excitation is a periodic electric field with frequency $Ω$ smaller than the Mott gap, while for the auxiliary excitations, we consider additional electric fields and/or hopping modulations with a higher harmonic of $Ω$. To suppress the 3-photon absorption of the main excitation, which is a parity-odd process, we consider auxiliary electric-field excitations and a combination of electric-field excitations and hopping modulations. On the other hand, to suppress the 2-photon absorption, which is a parity-even process, we consider hopping modulations. The conditions for an efficient suppression of heating are well captured by the Floquet effective Hamiltonian derived with the high-frequency expansion in a rotating frame. As an application, we focus on the exchange couplings of the spins (pseudo-spins) in the repulsive (attractive) model, and demonstrate that the suppression of heating allows to realize and clearly observe a significant Floquet-induced change of the low energy physics.

cond-mat.str-el↗

arXiv2023

Quantum optics measurement scheme for quantum geometry and topological invariants

We show how a quantum optical measurement scheme based on heterodyne detection can be used to explore geometrical and topological properties of condensed matter systems. Considering a 2D material placed in a cavity with a coupling to the environment, we compute correlation functions of the photons exiting the cavity and relate them to the hybrid light-matter state within the cavity. Different polarizations of the intracavity field give access to all components of the quantum geometric tensor on contours in the Brillouin zone defined by the transition energy. Combining recent results based on the metric-curvature correspondence with the measured quantum metric allows us to characterize the topological phase of the material. Moreover, in systems where $S_z$ is a good quantum number, the procedure also allows us to extract the spin Chern number. As an interesting application, we consider a minimal model for twisted bilayer graphene at the magic angle, and discuss the feasibility of extracting the Euler number.

cond-mat.mes-hall↗

arXiv2022

Probing magnetic orbitals and Berry curvature with circular dichroism in resonant inelastic X-ray scattering

Resonant inelastic X-ray scattering (RIXS) can probe localized excitations at selected atoms in materials, including particle-hole transitions between the valence and conduction bands. These transitions are governed by fundamental properties of the corresponding Bloch wave-functions, including orbital and magnetic degrees of freedom, and quantum geometric properties such as the Berry curvature. In particular, orbital angular momentum (OAM), which is closely linked to the Berry curvature, can exhibit a nontrivial momentum dependence. We demonstrate how information on such OAM textures can be extracted from the circular dichroism in RIXS. Based on accurate modeling with first-principles treatment of the key ingredient -- the light-matter interaction -- we simulate dichroic RIXS spectra for the prototypical transition metal dichalcogenide MoSe$_2$ and the two-dimensional topological insulator 1T$^\prime$-MoS$_2$. Guided by an intuitive picture for the optical selection rules, we discuss how the momentum-dependent OAM manifests itself in the dichroic RIXS signal if one controls the momentum transfer. Our calculations are performed for typical experimental geometries and parameter regimes, and demonstrate the possibility of observing the predicted circular dichroism in forthcoming experiments. Thus, our work establishes a new avenue to observing Berry curvature and topological states in quantum materials.

cond-mat.mtrl-sci↗

arXiv2022

Doping and gap-size dependence of high-harmonic generation in graphene : Importance of consistent formulation of light-matter coupling

High-harmonic generation (HHG) in solids is a fundamental nonlinear phenomenon, which can be efficiently controlled by modifying system parameters such as doping-level and temperature. In order to correctly predict the dependence of HHG on these parameters, consistent theoretical formulation of the light-matter coupling is crucial. Recently, contributions to the current that are often missing in the HHG analysis based on the semiconductor Bloch equations have been pointed out [J. Wilhelm, et.al. PRB 103 125419 (2021)]. In this paper, by systematically analyzing the doping and gap-size dependence of HHG in gapped graphene, we discuss the practical impact of such terms. In particular, we focus on the role of the current $J_{\rm ra}^{(2)}$, which originates from the change of the intraband dipole via interband transition. When the gap is small and the system is close to half filling, intraband and interband currents mostly cancel, thus suppressing the HHG signal - an important property that is broken when neglecting $J_{\rm ra}^{(2)}$. Furthermore, without $J_{\rm ra}^{(2)}$, the doping and gap-size dependence of HHG becomes qualitatively different from the full evaluation. Our results demonstrate the importance of the consistent expression of the current to study the parameter dependence of HHG for the small gap systems.

cond-mat.mes-hall↗

arXiv2022

Polarization-Modulated Angle-Resolved Photoemission Spectroscopy: Towards Circular Dichroism without Circular Photons and Bloch Wavefunction Reconstruction

Angle-resolved photoemission spectroscopy (ARPES) is the most powerful technique to investigate the electronic band structure of crystalline solids. To completely characterize the electronic structure of topological materials, one needs to go beyond band structure mapping and access information about the momentum-resolved Bloch wavefunction, namely orbitals, Berry curvature, and topological invariants. However, because phase information is lost in the process of measuring photoemission intensities, retrieving the complex-valued Bloch wavefunction from photoemission data has yet remained elusive. We introduce a novel measurement methodology and associated observable in extreme ultraviolet angle-resolved photoemission spectroscopy, based on continuous modulation of the ionizing radiation polarization axis. Tracking the energy- and momentum-resolved amplitude and phase of the photoemission intensity modulation upon polarization axis rotation allows us to retrieve the circular dichroism in photoelectron angular distributions (CDAD) without using circular photons, providing direct insights into the phase of photoemission matrix elements. In case of two relevant bands, it is possible to reconstruct the orbital pseudospin (and thus the Bloch wavefunction) with moderate theory input, as demonstrated for the prototypical layered semiconducting transition metal dichalcogenide 2H-WSe$_2$. This novel measurement methodology in ARPES, which is articulated around the manipulation of the photoionization transition dipole matrix element, in combination with a simple tight-binding theory, is general and adds a new dimension to obtaining insights into the orbital pseudospin, Berry curvature, and Bloch wavefunctions of many relevant crystalline solids.

cond-mat.mtrl-sci↗

arXiv2022

Probing Topological Floquet States in WSe$_2$ using Circular Dichroism in Time- and Angle-Resolved Photoemission Spectroscopy

Observing signatures of light-induced Floquet topological states in materials has been shown to be very challenging. Angle-resolved photoemission spectroscopy (ARPES) is well suited for the investigation of Floquet physics, as it allows to directly probe the dressed electronic states of driven solids. Depending on the system, scattering and decoherence can play an important role, hampering the emergence of Floquet states. Another challenge is to disentangle Floquet side bands from laser-assisted photoemission (LAPE), since both lead to similar signatures in ARPES spectra. Here, we investigate the emergence of Floquet state in the transition metal dichalcogenide $2H$-WSe$_2$, one of the most promising systems for observing Floquet physics. We discuss how the Floquet topological state manifests in characteristic features in the circular dichroism in photoelectron angular distributions (CDAD) that is determined by the transient band structure modifications and the associated texture of the orbital angular momentum. Combining highly accurate modeling of the photoemission matrix elements with an \emph{ab initio} description of the light-matter interaction, we investigate regimes which can be realized in current state-of-the-art experimental setups. The predicted features are robust against scattering effects and are expected to be observed in forthcoming experiments.

cond-mat.mtrl-sci↗

arXiv2021

Unveiling the Orbital Texture of 1T-TiTe$_2$ using Intrinsic Linear Dichroism in Multidimensional Photoemission Spectroscopy

The momentum-dependent orbital character in crystalline solids, referred to as orbital texture, is of capital importance in the emergence of symmetry-broken collective phases such as charge density waves as well as superconducting and topological states of matter. By performing extreme ultraviolet multidimensional angle-resolved photoemission spectroscopy for two different crystal orientations linked to each other by mirror symmetry, we isolate and identify the role of orbital texture in photoemission from the transition metal dichalcogenide 1T-TiTe$_2$. By comparing our experimental results with theoretical calculations based on both a quantitative one-step model of photoemission and an intuitive tight-binding model, we unambiguously demonstrate the link between the momentum-dependent orbital orientation and the emergence of strong intrinsic linear dichroism in the photoelectron angular distributions. Our results represent an important step towards going beyond band structure (eigenvalues) mapping and learn about electronic wavefunction and orbital texture of solids by exploiting matrix element effects in photoemission spectroscopy.

cond-mat.mtrl-sci↗

arXiv2021

Self-energy dynamics and mode-specific phonon threshold effect in a Kekulé-ordered graphene

Electron-phonon interaction and related self-energy are fundamental to both the equilibrium properties and non-equilibrium relaxation dynamics of solids. Although electron-phonon interaction has been suggested by various time-resolved measurements to be important for the relaxation dynamics of graphene, the lack of energy- and momentum-resolved self-energy dynamics prohibits direct identification of the role of specific phonon modes in the relaxation dynamics. Here by performing time- and angle-resolved photoemission spectroscopy measurements on a Kekulé-ordered graphene with folded Dirac cones at the $Γ$ point, we have succeeded in resolving the self-energy effect induced by coupling of electrons to two phonons at $Ω_1$ = 177 meV and $Ω_2$ = 54 meV and revealing its dynamical change in the time domain. Moreover, these strongly coupled phonons define energy thresholds, which separate the hierarchical relaxation dynamics from ultrafast, fast to slow, thereby providing direct experimental evidence for the dominant role of mode-specific phonons in the relaxation dynamics

cond-mat.mes-hall↗

arXiv2021

Theory of subcycle time-resolved photoemission: application to terahertz photodressing in graphene

Motivated by recent experimental progress we revisit the theory of pump-probe time- and angle-resolved photoemission spectroscopy (trARPES), which is one of the most powerful techniques to trace transient pump-driven modifications of the electronic properties. The pump-induced dynamics can be described in different gauges for the light-matter interaction. Standard minimal coupling leads to the velocity gauge, defined by linear coupling to the vector potential. In the context of tight-binding (TB) models, the Peierls substitution is the commonly employed scheme for single-band models. Multi-orbital extensions -- including the coupling of the dipole moments to the electric field -- have been introduced and tested recently. In this work, we derive the theory of time-resolved photoemission within both gauges from the perspective of nonequilibrium Green's functions. This approach naturally incorporates the photoelectron continuum, which allows for a direct calculation of the observable photocurrent. Following this route we introduce gauge-invariant expressions for the time-resolved photoemission signal. The theory is applied to graphene pumped with short terahertz pulses, which we treat within a first-principles TB model. We investigate the gauge invariance and discuss typical effects observed in subcycle time-resolved photoemission. Our formalism is an ideal starting point for realistic trARPES simulations including scattering effects.

cond-mat.mes-hall↗

arXiv2021

Dynamically Induced Exceptional Phases in Quenched Interacting Semimetals

We report on the dynamical formation of exceptional degeneracies in basic correlation functions of non-integrable one- and two-dimensional systems quenched to the vicinity of a critical point. Remarkably, fine-tuned semi-metallic points in the phase diagram of the considered systems are thereby promoted to topologically robust non-Hermitian (NH) nodal phases emerging in the coherent long-time evolution of a dynamically equilibrating system. In the framework of non-equilibrium Green's function methods within the conserving second Born approximation, we predict observable signatures of these novel NH nodal phases in simple spectral functions as well as in the time-evolution of momentum distribution functions.

cond-mat.mes-hall↗

arXiv2021

Dynamical signatures of symmetry protected topology following symmetry breaking

We investigate topological signatures in the short-time non-equilibrium dynamics of symmetry protected topological (SPT) systems starting from initial states which break the protecting symmetry. Naïvely, one might expect that topology loses meaning when a protecting symmetry is broken. Defying this intuition, we illustrate, in an interacting Su-Schrieffer-Heeger (SSH) model, how this combination of symmetry breaking and quench dynamics can give rise to both single-particle and many-body signatures of topology. From the dynamics of the symmetry broken state, we find that we are able to dynamically probe the equilibrium topological phase diagram of a symmetry respecting projection of the post-quench Hamiltonian. In the ensemble dynamics, we demonstrate how spontaneous symmetry breaking (SSB) of the protecting symmetry can result in a quantized many-body topological `invariant' which is not pinned under unitary time evolution. We dub this `dynamical many-body topology' (DMBT). We show numerically that both the pure state and ensemble signatures are remarkably robust, and argue that these non-equilibrium signatures should be quite generic in SPT systems, regardless of protecting symmetries or spatial dimension.

cond-mat.str-el↗

arXiv2021

Correlation-Assisted Quantized Charge Pumping

We investigate charge pumping in the vicinity of order-obstructed topological phases, i.e. symmetry protected topological phases masked by spontaneous symmetry breaking in the presence of strong correlations. To explore this, we study a prototypical Su-Schrieffer-Heeger model with finite-range interaction that gives rise to orbital charge density wave order, and characterize the impact of this order on the model's topological properties. In the ordered phase, where the many-body topological invariant loses quantization, we find that not only is quantized charge pumping still possible, but it is even assisted by the collective nature of the orbital charge density wave order. Remarkably, we show that the Thouless pump scenario may be used to uncover the underlying topology of order-obstructed phases.

cond-mat.str-el↗

arXiv2021

Gauge invariance of light-matter interactions in first-principle tight-binding models

We study the different ways of introducing light-matter interaction in first-principle tight-binding (TB) models. The standard way of describing optical properties is the velocity gauge, defined by linear coupling to the vector potential. In finite systems a transformation to represent the electromagnetic radiation by the electric field instead is possible, albeit subtleties arise in periodic systems. The resulting dipole gauge is a multi-orbital generalization of Peierl's substitution. In this work, we investigate accuracy of both pathways, with particular emphasis on gauge invariance, for TB models constructed from maximally localized Wannier functions. Focusing on paradigmatic two-dimensional materials, we construct first-principle models and calculate the response to electromagnetic fields in linear response and for strong excitations. Benchmarks against fully converged first-principle calculations allow for ascertaining the accuracy of the TB models. We find that the dipole gauge provides a more accurate description than the velocity gauge in all cases. The main deficiency of the velocity gauge is an imperfect cancellation of paramagnetic and diamagnetic current. Formulating a corresponding sum rule however provides a way to explicitly enforce this cancellation. This procedure corrects the TB models in the velocity gauge, yielding excellent agreement with dipole gauge and thus gauge invariance.

cond-mat.mtrl-sci↗

arXiv2020

Revealing Hidden Orbital Pseudospin Texture with Time-Reversal Dichroism in Photoelectron Angular Distributions

We performed angle-resolved photoemission spectroscopy (ARPES) of bulk 2H-WSe$_2$ for different crystal orientations linked to each other by time-reversal symmetry. We introduce a new observable called time-reversal dichroism in photoelectron angular distributions (TRDAD), which quantifies the modulation of the photoemission intensity upon effective time-reversal operation. We demonstrate that the hidden orbital pseudospin texture leaves its imprint onto TRDAD, due to multiple orbitals interference effects in photoemission. Our experimental results are in quantitative agreement with both tight-binding model and state-of-the-art fully relativistic calculations performed using the one-step model of photoemission. While spin-resolved ARPES probes the spin component of entangled spin-orbital texture in multiorbital systems, we unambiguously demonstrate that TRDAD reveals its orbital pseudospin texture counterpart.

cond-mat.mtrl-sci↗