arXiv subjects

Martin Wolf

Publications and source records attributed to Martin Wolf.

At least 73 records · Page 4Linked to original sources

arXiv2023

Nonlinear THz Control of the Lead Halide Perovskite Lattice

Lead halide perovskites (LHPs) have emerged as an excellent class of semiconductors for next-generation solar cells and optoelectronic devices. Tailoring physical properties by fine-tuning the lattice structures has been explored in these materials by chemical composition or morphology. Nevertheless, its dynamic counterpart, phonon-driven ultrafast material control, as contemporarily harnessed for oxide perovskites, has not been established yet. Here we employ intense THz electric fields to obtain direct lattice control via nonlinear excitation of coherent octahedral twist modes in hybrid CH3NH3PbBr3 and all-inorganic CsPbBr3 perovskites. These Raman-active phonons at 0.9 - 1.3 THz are found to govern the ultrafast THz-induced Kerr effect in the low-temperature orthorhombic phase and thus dominate the phonon-modulated polarizability with potential implications for dynamic charge carrier screening beyond the Froehlich polaron. Our work opens the door to selective control of LHP's vibrational degrees of freedom governing phase transitions and dynamic disorder.

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

Colour-kinematics duality, double copy, and homotopy algebras

Colour-kinematics duality is a remarkable property of Yang-Mills theory. Its validity implies a relation between gauge theory and gravity scattering amplitudes, known as double copy. Albeit fully established at the tree level, its extension to the loop level is conjectural. Lifting the on-shell, scattering amplitudes-based description to the level of action functionals, we argue that a theory that exhibits tree-level colour-kinematics duality can be reformulated in a way such that its loop integrands manifest a generalised form of colour-kinematics duality. Moreover, we show how the structures of higher homotopy theory naturally describe this off-shell reformulation of colour-kinematics duality.

hep-th↗

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

Optical Rectification and Electro-Optic Sampling in Quartz

We report electro-optic sampling (EOS) response and terahertz (THz) optical rectification (OR) in z-cut alpha-quartz. Due to its small effective second-order nonlinearity, echo-free waveform of intense THz pulses with a few MV/cm electric-field strength can be measured faithfully with no saturation effect. Both its OR and EOS responses are broad with extension up to ~8 THz. Strikingly, the latter responses are independent of the crystal thickness, a plausible indication of strong surface contribution to the total second-order nonlinear susceptibility of quartz. Our study introduces thin quartz plates as the reliable THz electro-optic medium for echo-free, high field THz detection.

physics.optics↗

arXiv2022

Second Harmonic Generation from Grating-Coupled Hybrid Plasmon-Phonon Polaritons

Polaritons can provide strong optical field enhancement allowing to boost light-matter interaction. Here, we experimentally observe enhancement of mid-infrared second-harmonic generation (SHG) using grating-coupled surface phonon polaritons of the 6H-SiC surface. In our experiment, we measure the SHG along the polariton dispersion by changing the incidence angle of the excitation beam. We observe hybridization between the propagating surface phonon polaritons and localized plasmon resonances in the gold grating, evidenced by the modification of the polariton dispersion as we change the area ratio of grating and substrate. Design options for engineering the plasmon-phonon polariton hybridization are discussed. Overall, we find a rather low yield of polariton-enhanced SHG in this geometry compared to prism-coupling and nanostructures, and discuss possible origins.

physics.optics↗

arXiv2022

Terahertz spin-to-charge current conversion in stacks of ferromagnets and the transition-metal dichalcogenide NbSe$_2$

Transition-metal dichalcogenides (TMDCs) are an aspiring class of materials with unique electronic and optical properties and potential applications in spin-based electronics. Here, we use terahertz emission spectroscopy to study spin-to-charge current conversion (S2C) in the TMDC NbSe$_2$ in ultra-high-vacuum-grown F|NbSe$_2$ thin-film stacks, where F is a layer of ferromagnetic Fe or Ni. Ultrafast laser excitation triggers an ultrafast spin current that is converted into an in-plane charge current and, thus, a measurable THz electromagnetic pulse. The THz signal amplitude as a function of the NbSe$_2$ thickness shows that the measured signals are fully consistent with an ultrafast optically driven injection of an in-plane-polarized spin current into NbSe$_2$. Modeling of the spin-current dynamics reveals that a sizable fraction of the total S2C originates from the bulk of NbSe$_2$ with the same, negative, sign as the spin Hall angle of pure Nb. By quantitative comparison of the emitted THz radiation from F|NbSe$_2$ to F|Pt reference samples and the results of ab-initio calculations, we estimate that the spin Hall angle of NbSe$_2$ for an in-plane polarized spin current lies between -0.2% and -1.1%, while the THz spin-current relaxation length is of the order of a few nanometers.

cond-mat.mes-hall↗

arXiv2022

Super Non-Abelian T-Duality

We analyse super non-Abelian T-duality for principal chiral models, symmetric space sigma models, and semi-symmetric space sigma models for general Lie supergroups. This includes T-duality along both bosonic and fermionic directions. As an example, we perform the explicit dualisation of the OSp(1|2) principal chiral model, and, whilst the target superspace of this model is a three-dimensional supergravity background, we find that its super non-Abelian T-dual falls outside the class of such backgrounds.

hep-th↗

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↗

arXiv2022

Femtosecond Thermal and Nonthermal Hot Electron Tunneling inside a Photoexcited Tunnel Junction

Efficient operation of electronic nanodevices at ultrafast speeds requires understanding and control of the currents generated by femtosecond bursts of light. Ultrafast laser-induced currents in metallic nanojunctions can originate from photo-assisted hot electron tunneling or lightwave-induced tunneling. Both processes can drive localized photocurrents inside a scanning tunneling microscope (STM) on femto- to attosecond time scales, enabling ultrafast STM with atomic spatial resolution. Femtosecond laser excitation of a metallic nanojunction, however, also leads to the formation of a transient thermalized electron distribution, but the tunneling of thermalized hot electrons on time scales faster than electron-lattice equilibration is not well understood. Here, we investigate ultrafast electronic heating and transient thermionic tunneling inside a metallic photoexcited tunnel junction and its role in the generation of ultrafast photocurrents in STM. Phase-resolved sampling of broadband THz pulses via the THz-field-induced modulation of ultrafast photocurrents allows us to probe the electronic temperature evolution inside the STM tip, and to observe the competition between instantaneous and delayed tunneling due to nonthermal and thermal hot electron distributions in real time. Our results reveal the pronounced nonthermal character of photo-induced hot electron tunneling, and provide a detailed microscopic understanding of hot electron dynamics inside a laser-excited tunnel junction.

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↗

arXiv2021

Infrared super-resolution wide-field microscopy using sum-frequency generation

Super-resolution microscopy in the visible is an established powerful tool in several disciplines. In the infrared (IR) spectral range, however, no comparable schemes have been demonstrated to date. In this work, we experimentally demonstrate super-resolution microscopy in the IR range ($λ_{IR}\approx 10-12\,μ$m) using IR-visible sum-frequency generation. We operate our microscope in a wide-field scheme and image localized surface phonon polaritons in 4H-SiC nanostructures as a proof-of-concept. With this technique, we demonstrate an enhanced spatial resolution of $\simλ_{IR}/9$, enabling to resolve the polariton resonances in individual sub-diffractional nanostructures with sub-wavelength spacing. Furthermore we show, that this resolution allows to differentiate between spatial patterns associated with different polariton modes within individual nanostructures.

physics.optics↗

arXiv2021

Spin-voltage-driven efficient terahertz spin currents from the magnetic Weyl semimetals Co$_2$MnGa and Co$_2$MnAl

Magnetic Weyl semimetals are an emerging material class that combines magnetic order and a topologically non-trivial band structure. Here, we study ultrafast optically driven spin injection from thin films of the magnetic Weyl semimetals Co$_2$MnGa and Co$_2$MnAl into an adjacent Pt layer by means of terahertz emission spectroscopy. We find that (i) Co$_2$MnGa and Co$_2$MnAl are efficient terahertz spin-current generators reaching efficiencies of typical 3d-transition-metal ferromagnets such as Fe. (ii) The relaxation of the spin current provides an estimate of the electron-spin relaxation time of Co$_2$MnGa (165 fs) and Co$_2$MnAl (102 fs), which is comparable to Fe (92 fs). Both observations are consistent with a simple analytical model and highlight the large potential of magnetic Weyl semimetals as spin-current sources in terahertz spintronic devices. Finally, our results provide a strategy to identify magnetic materials that provide maximum spin current amplitudes for a given deposited optical energy density.

cond-mat.mes-hall↗

arXiv2021

Transition of laser-induced terahertz spin currents from torque- to conduction-electron-mediated transport

Spin transport is crucial for future spintronic devices operating at bandwidths up to the terahertz (THz) range. In F|N thin-film stacks made of a ferro/ferrimagnetic layer F and a normal-metal layer N, spin transport is mediated by (1) spin-polarized conduction electrons and/or (2) torque between electron spins. To identify a cross-over from (1) to (2), we study laser-driven spin currents in F|Pt stacks where F consists of model materials with different degrees of electrical conductivity. For the magnetic insulators YIG, GIG and maghemite, identical dynamics is observed. It arises from the THz interfacial spin Seebeck effect (SSE), is fully determined by the relaxation of the electrons in the metal layer and provides an estimate of the spin-mixing conductance of the GIG/Pt interface. Remarkably, in the half-metallic ferrimagnet Fe3O4 (magnetite), our measurements reveal two spin-current components with opposite direction. The slower, positive component exhibits SSE dynamics and is assigned to torque-type magnon excitation of the A- and B-spin sublattices of Fe3O4. The faster, negative component arises from the pyro-spintronic effect and can consistently be assigned to ultrafast demagnetization of e-sublattice minority-spin hopping electrons. This observation supports the magneto-electronic model of Fe3O4. In general, our results provide a new route to the contact-free separation of torque- and conduction-electron-mediated spin currents.

cond-mat.mes-hall↗

arXiv2021

A New Search for Neutrino Point Sources with IceCube

The IceCube Neutrino Observatory, deployed inside the deep glacial ice at the South Pole, is the largest neutrino telescope in the world. While eight years have passed since IceCube discovered a diffuse flux of high-energy astrophysical neutrinos, the sources of the vast majority of these neutrinos remain unknown. Here, we present a new search for neutrino point sources that improves the accuracy of the statistical analysis, especially in the low energy regime. We replaced the usual Gaussian approximations of IceCube's point spread function with precise numerical representations, obtained from simulations, and combined them with new machine learning-based estimates of event energies and angular errors. Depending on the source properties, the new analysis provides improved source localization, flux characterization and thereby discovery potential (by up to 30%) over previous works. The analysis will be applied to IceCube data that has been recorded with the full 86-string detector configuration from 2011 to 2020 and includes improved detector calibration.

astro-ph.HE↗

arXiv2021

Double Copy from Homotopy Algebras

We show that the BRST Lagrangian double copy construction of $\mathcal{N}=0$ supergravity as the `square' of Yang-Mills theory finds a natural interpretation in terms of homotopy algebras. We significantly expand on our previous work arguing the validity of the double copy at the loop level, and we give a detailed derivation of the double copied Lagrangian and BRST operator. Our constructions are very general and can be applied to a vast set of examples.

hep-th↗

arXiv2021

The SkyLLH framework for IceCube point-source search

Hypothesis tests based on unbinned log-likelihood (LLH) functions are a common technique used in multi-messenger astronomy, including IceCube's neutrino point-source searches. We present the general Python-based tool "SkyLLH", which provides a modular framework for implementing and executing log-likelihood functions to perform data analyses with multi-messenger astronomy data. Specific SkyLLH framework features for a new and improved time-integrated IceCube point-source analysis are highlighted, including the support for kernel density estimation (KDE) based probability density functions. In addition, the support for a variety of point-source analysis types, such as stacked and time-variable searches, will be presented.

astro-ph.IM↗