arXiv subjects

Rupert Huber

Publications and source records attributed to Rupert Huber.

At least 19 recordsLinked to original sources

arXiv2026

Subcycle videography of lightwave-driven Landau-Zener-Majorana transitions in graphene

Strong light fields have unlocked previously unthinkable possibilities to tailor coherent electron trajectories, engineer band structures and shape emergent phases of matter all-optically. Unravelling the underlying quantum mechanisms requires a visualisation of the lightwave-driven electron motion directly in the band structure. While photoelectron momentum microscopy has imaged optically excited electrons averaged over many cycles of light, actual subcycle band-structure videography has been limited to small electron momenta. Yet lightwave-driven elementary processes in quantum materials often occur throughout momentum space. Here, we introduce attosecond-precision, subcycle band-structure videography covering the entire first Brillouin zone (BZ) and visualize one of the most fundamental but notoriously elusive strong-field processes: non-adiabatic Landau-Zener-Majorana (LZM) tunnelling. The interplay of field-driven acceleration within the Dirac-like band structure of graphene and periodic LZM interband tunnelling manifest in a coherent displacement and distortion of the momentum distribution at the BZ edge. The extremely non-thermal electron distributions also allow us to disentangle competing scattering processes and assess their impact on coherent electronic control through electron redistribution and thermalization. Our panoramic view of strong-field-driven electron motion in quantum materials lays the foundation for a microscopic understanding of some of the most discussed light-driven phenomena in condensed matter physics.

cond-mat.mes-hall↗

arXiv2026

Observation of an isolated flat band in the van der Waals crystal NbOCl$_2$

Dispersionless electronic bands lead to an extremely high density of states and suppressed kinetic energy, thereby increasing electronic correlations and instabilities that can shape emergent ordered states, such as excitonic, ferromagnetic, and superconducting phases. A flat band that extends over the entire momentum space and is well isolated from other dispersive bands is, therefore, particularly interesting. Here, the band structure of the van der Waals crystal NbOCl$_2$ is revealed by utilizing photoelectron momentum microscopy. We directly map out an electronic band that is flat throughout the entire Brillouin zone and features a width of only $\sim$100 meV. This band is well isolated from both the conduction and remote valence bands. Moreover, the quasiparticle band gap shows a high tunability upon the deposition of caesium atoms on the surface. By combining the single-particle band structure with the optical transmission spectrum, the optical gap is identified. The fully isolated flat band in a van der Waals crystal provides a qualitatively new testbed for exploring flat-band physics.

cond-mat.mes-hall↗

arXiv2025

All-optical band structure reconstruction and onset of Landau quantization of Dirac fermions

The nature of relativistic electrons in solids depends on the precise shape of the underlying band structure. Prominently, symmetry-related mechanisms, such as the breaking of time reversal symmetry in topological insulators, can lead to the emergence of band gaps on small energy scales. It is, thus, important to quantify potential gaps of the Dirac cone with meV precision. Yet established band structure measurements are often challenged by their strict surface sensitivity or limited energy resolution. In this work, we use broadband, time-resolved THz magneto-spectroscopy to access the band structure of Dirac electrons in a buried HgTe quantum well by contact-free, all-optical measurements. Optical doping allows us to control the Fermi level without applying any electrical gate voltages. The background-free measurement of the cyclotron resonance of the Dirac system over 2.5 optical octaves, a broad range of magnetic field strengths, and different Fermi energies allows us to reconstruct the band structure near the Dirac point with sub-meV precision, and to observe a crossover of Landau quantization from a quasi-classical to the relativistic regime.

cond-mat.mes-hall↗

arXiv2025

Attosecond charge transfer in atomic-resolution scanning tunnelling microscopy

Electrons in atoms and molecules move on attosecond time scales. Deciphering their quantum dynamics in space and time calls for high-resolution microscopy at this speed. While scanning tunnelling microscopy (STM) driven with terahertz pulses has visualized sub-picosecond motion of single atoms, the advent of attosecond light pulses has provided access to the much faster electron dynamics. Yet, combining direct atomic spatial and attosecond temporal resolution remained challenging. Here, we reveal atomic-scale quantum motion of single electrons in attosecond lightwave-driven STM. Near-infrared single-cycle waveforms from phase-controlled optical pulse synthesis steer and clock electron tunnelling. By keeping the thermal load of the tip-sample junction stable, thereby eliminating thermal artifacts, we detect waveform-dependent currents on sub-cycle time scales. Our joint theory-experiment campaign shows that single-cycle near-infrared pulses can drive isolated electronic wave packets shorter than 1 fs. The angstrom-scale decay of the tunnelling current earmarks a fascinating interplay of multi-photon and field-driven dynamics. By balancing these effects, we sharply image a single copper adatom on a silver surface with lightwave-driven currents. This long-awaited fusion of attosecond science with atomic-scale STM makes elementary dynamics of electrons inside atoms, molecules and solids accessible to direct spatio-temporal videography and atom-scale petahertz electronics.

physics.optics↗

arXiv2025

Magnetic control of an exciton-polariton condensate in a van der Waals magnet

Quasiparticle condensates are among the most spectacular solid-state manifestations of quantum physics. Coupling macroscopic real-space wavefunctions to additional degrees of freedom, such as the electron spin, would add valuable control knobs for quantum applications. While creating spin-carrying superconducting condensates has attracted enormous attention, man-made condensates of light-matter hybrids known as exciton-polaritons have lacked an analogous spin-based perspective. Here we open a new door by demonstrating magnetically tunable exciton-polariton condensation in the van der Waals magnet CrSBr. Under photoexcitation, CrSBr microwires embedded in an optical cavity show the hallmarks of polariton condensation: a dramatic increase of the emission intensity from an excited laterally confined polariton state by multiple orders of magnitude, spectral narrowing of the emission line, and a continuous shift of the peak energy. Interferometry evidences an increase in spatial and temporal coherence. Owing to the strong coupling between the spin order and excitonic correlation, the energy of the condensate can be tuned by up to 10.5 meV by an external magnetic field of only 2 Tesla. Our results establish CrSBr microcavities as a powerful platform for exploring magnetic control of polariton condensates and mark a significant step toward spin-controlled coherent quantum light sources.

cond-mat.mtrl-sci↗

arXiv2025

The 2D Materials Roadmap

Over the past two decades, 2D materials have rapidly evolved into a diverse and expanding family of material platforms. Many members of this materials class have demonstrated their potential to deliver transformative impact on fundamental research and technological applications across different fields. In this roadmap, we provide an overview of the key aspects of 2D material research and development, spanning synthesis, properties and commercial applications. We specifically present roadmaps for high impact 2D materials, including graphene and its derivatives, transition metal dichalcogenides, MXenes as well as their heterostructures and moir\'e systems. The discussions are organized into thematic sections covering emerging research areas (e.g., twisted electronics, moir\'e nano-optoelectronics, polaritronics, quantum photonics, and neuromorphic computing), breakthrough applications in key technologies (e.g., 2D transistors, energy storage, electrocatalysis, filtration and separation, thermal management, flexible electronics, sensing, electromagnetic interference shielding, and composites) and other important topics (computational discovery of novel materials, commercialization and standardization). This roadmap focuses on the current research landscape, future challenges and scientific and technological advances required to address, with the intent to provide useful references for promoting the development of 2D materials.

cond-mat.mtrl-sci↗

arXiv2023

Sculpting ultrastrong light-matter coupling through spatial matter structuring

The central theme of cavity quantum electrodynamics is the coupling of a single optical mode with a single matter excitation, leading to a doublet of cavity polaritons which govern the optical properties of the coupled structure. Especially in the ultrastrong coupling regime, where the ratio of the vacuum Rabi frequency and the quasi-resonant carrier frequency of light, $\Omega_{\mathrm R}/\omega_{\mathrm c}$, approaches unity, the polariton doublet bridges a large spectral bandwidth $2\Omega_{\mathrm R}$, and further interactions with off-resonant light and matter modes may occur. The resulting multi-mode coupling has recently attracted attention owing to the additional degrees of freedom for designing light-matter coupled resonances, despite added complexity. Here, we experimentally implement a novel strategy to sculpt ultrastrong multi-mode coupling by tailoring the spatial overlap of multiple modes of planar metallic THz resonators and the cyclotron resonances of Landau-quantized two-dimensional electrons, on subwavelength scales. We show that similarly to the selection rules of classical optics, this allows us to suppress or enhance certain coupling pathways and to control the number of light-matter coupled modes, their octave-spanning frequency spectra, and their response to magnetic tuning. This offers novel pathways for controlling dissipation, tailoring quantum light sources, nonlinearities, correlations as well as entanglement in quantum information processing.

quant-ph↗

arXiv2022

Perspective on real-space nanophotonic field manipulation using non-perturbative light-matter coupling

The achievement of large values of the light-matter coupling in nanoengineered photonic structures can lead to multiple photonic resonances contributing to the final properties of the same hybrid polariton mode. We develop a general theory describing multi-mode light-matter coupling in systems of reduced dimensionality and we explore their novel phenomenology, validating the predictions of our theory against numerical electromagnetic simulations. On the one hand, we characterise the spectral features linked with the multi-mode nature of the polaritons. On the other hand, we show how the interference between different photonic resonances can modify the real-space shape of the electromagnetic field associated with each polariton mode. We argue that the possibility of engineering nanophotonic resonators to maximise the multi-mode mixing, and to alter the polariton modes via applied external fields, could allow for the dynamical real-space tailoring of subwavelength electromagnetic fields.

physics.optics↗

arXiv2022

Interferometric carrier-envelope phase stabilization for ultrashort pulses in the mid-infrared

We demonstrate an active carrier-envelope phase (CEP) stabilization scheme for optical waveforms generated by difference-frequency mixing of two spectrally detuned and phase-correlated pulses. By performing ellipsometry with spectrally overlapping parts of two co-propagating near-infrared generation pulse trains, we stabilize their relative timing to 18 as. Consequently, we can lock the CEP of the generated mid-infrared (MIR) pulses with a remaining phase jitter below 30 mrad. Employing these pulses for high-harmonic generation in a bulk semiconductor validates our technique. This experiment reveals that our method also stabilizes the energy of the MIR pulses, thereby approaching the intrinsic stability of the underlying laser system.

physics.optics↗

arXiv2021

Quantifying nanoscale electromagnetic fields in near-field microscopy by Fourier demodulation analysis

Confining light to sharp metal tips has become a versatile technique to study optical and electronic properties far below the diffraction limit. Particularly near-field microscopy in the mid-infrared spectral range has found a variety of applications in probing nanostructures and their dynamics. Yet, the ongoing quest for ultimately high spatial resolution down to the single-nanometer regime and quantitative three-dimensional nano-tomography depends vitally on a precise knowledge of the spatial distribution of the near fields emerging from the probe. Here, we perform finite element simulations of a tip with realistic geometry oscillating above a dielectric sample. By introducing a novel Fourier demodulation analysis of the electric field at each point in space, we reliably quantify the distribution of the near fields above and within the sample. Besides inferring the lateral field extension, which can be smaller than the tip radius of curvature, we also quantify the probing volume within the sample. Finally, we visualize the scattering process into the far field at a given demodulation order, for the first time, and shed light onto the nanoscale distribution of the near fields and its evolution as the tip-sample distance is varied. Our work represents a crucial step in understanding and tailoring the spatial distribution of evanescent fields in optical nanoscopy.

physics.optics↗

arXiv2020

Momentum-resolved observation of exciton formation dynamics in monolayer WS$_2$

The dynamics of exciton formation in transition metal dichalcogenides is difficult to measure experimentally, since many momentum-indirect exciton states are not accessible to optical interband spectroscopy. Here, we combine a tuneable pump, high-harmonic probe laser source with a 3D momentum imaging technique to map photoemitted electrons from monolayer WS$_2$. This provides momentum-, energy- and time-resolved access to excited states on an ultrafast timescale. The high temporal resolution of the setup allows us to trace the early-stage exciton dynamics on its intrinsic timescale and observe the formation of a momentum-forbidden dark K$\Sigma$ exciton a few tens of femtoseconds after optical excitation. By tuning the excitation energy we manipulate the temporal evolution of the coherent excitonic polarization and observe its influence on the dark exciton formation. The experimental results are in excellent agreement with a fully microscopic theory, resolving the temporal and spectral dynamics of bright and dark excitons in WS$_2$.

cond-mat.mtrl-sci↗

arXiv2019

Ultrafast transition between exciton phases in van der Waals heterostructures

Heterostructures of atomically thin van der Waals bonded monolayers have opened a unique platform to engineer Coulomb correlations, shaping excitonic, Mott insulating, or superconducting phases. In transition metal dichalcogenide heterostructures, electrons and holes residing in different monolayers can bind into spatially indirect excitons with a strong potential for optoelectronics, valleytronics, Bose condensation, superfluidity, and moir\'e-induced nanodot lattices. Yet these ideas require a microscopic understanding of the formation, dissociation, and thermalization dynamics of correlations including ultrafast phase transitions. Here we introduce a direct ultrafast access to Coulomb correlations between monolayers; phase-locked mid-infrared pulses allow us to measure the binding energy of interlayer excitons in WSe2/WS2 hetero-bilayers by revealing a novel 1s-2p resonance, explained by a fully quantum mechanical model. Furthermore, we trace, with subcycle time resolution, the transformation of an exciton gas photogenerated in the WSe2 layer directly into interlayer excitons. Depending on the stacking angle, intra- and interlayer species coexist on picosecond scales and the 1s-2p resonance becomes renormalized. Our work provides a direct measurement of the binding energy of interlayer excitons and opens the possibility to trace and control correlations in novel artificial materials.

cond-mat.mtrl-sci↗

arXiv2019

Ultrafast two-dimensional field spectroscopy of terahertz intersubband saturable absorbers

Intersubband (ISB) transitions in semiconductor multi-quantum well (MQW) structures are promising candidates for the development of saturable absorbers at terahertz (THz) frequencies. Here, we exploit amplitude and phase-resolved two-dimensional (2D) THz spectroscopy on the sub-cycle time scale to observe directly the saturation dynamics and coherent control of ISB transitions in a metal-insulator MQW structure. Clear signatures of incoherent pump-probe and coherent four-wave mixing signals are recorded as a function of the peak electric field of the single-cycle THz pulses. All nonlinear signals reach a pronounced maximum for a THz electric field amplitude of 11 kV/cm and decrease for higher fields. We demonstrate that this behavior is a fingerprint of THz-driven carrier-wave Rabi flopping. A numerical solution of the Maxwell-Bloch equations reproduces our experimental findings quantitatively and traces the trajectory of the Bloch vector. This microscopic model allows us to design tailored MQW structures with optimized dynamical properties for saturable absorbers that could be used in future compact semiconductor-based single-cycle THz sources.

physics.optics↗

arXiv2018

Rapid-scan acousto-optical delay line with 34 kHz scan rate and 15 attosecond precision

An optical fast-scan delay exploiting the near-collinear interaction between a train of ultrashort optical pulses and an acoustic wave propagating in a birefringent crystal is introduced. In combination with a femtosecond Er:fiber laser, the scheme is shown to delay few-fs pulses by up to 6 ps with a precision of 15 as. A resolution of 5 fs is obtained for a single sweep at a repetition rate of 34 kHz. This value can be improved to 39 as for multiple scans at a total rate of 0.3 kHz.

physics.ins-det↗

arXiv2018

Terahertz light-matter interaction beyond unity coupling strength

Achieving control over light-matter interaction in custom-tailored nanostructures is at the core of modern quantum electrodynamics [1-15]. In ultrastrongly coupled systems [5-15], excitation is repeatedly exchanged between a resonator and an electronic transition at a rate known as the vacuum Rabi frequency $\Omega_R$. For $\Omega_R$ approaching the resonance frequency $\omega_c$, novel quantum phenomena including squeezed states [16], Dicke superradiant phase transitions [17,18], the collapse of the Purcell effect [19], and a population of the ground state with virtual photon pairs [16,20] are predicted. Yet, the experimental realization of optical systems with $\Omega_R$/$\omega_c$ has remained elusive. Here, we introduce a paradigm change in the design of light-matter coupling by treating the electronic and the photonic components of the system as an entity instead of optimizing them separately. Using the electronic excitation to not only boost the oscillator strength but furthermore tailor the shape of the vacuum mode, we push $\Omega_R$/$\omega_c$ of cyclotron resonances ultrastrongly coupled to metamaterials far beyond unity. As one prominent illustration of the unfolding possibilities, we calculate a ground state population of 0.37 virtual photons for our best structure with $\Omega_R$/$\omega_c$ = 1.43, and suggest a realistic experimental scenario for measuring vacuum radiation by cutting-edge terahertz quantum detection [21,22].

cond-mat.mes-hall↗

arXiv2018

Direct observation of ultrafast exciton formation in monolayer WSe$_2$

Many of the fundamental optical and electronic properties of atomically thin transition metal dichalcogenides are dominated by strong Coulomb interactions between electrons and holes, forming tightly bound atom-like excitons. Here, we directly trace the ultrafast formation of excitons by monitoring the absolute densities of bound and unbound electron-hole pairs in monolayers of WSe$_2$ following femtosecond non-resonant optical excitation. To this end, phase-locked mid-infrared probe pulses and field-sensitive electro-optic sampling are used to map out the full complex-valued optical conductivity of the non-equilibrium system and to discern the hallmark low-energy responses of bound and unbound pairs. While free charge carriers strongly influence the infrared response immediately after above-bandgap injection, up to 60% of the electron-hole pairs are bound as excitons already on a sub-picosecond timescale, evidencing extremely fast and efficient exciton formation. During the subsequent recombination phase, we still find a large density of free carriers in addition to excitons, indicating a non-equilibrium state of the photoexcited electron-hole system.

cond-mat.mtrl-sci↗

arXiv2018

Dielectric Engineering of Electronic Correlations in a van der Waals Heterostructure

Heterostructures of van der Waals bonded layered materials offer unique means to tailor dielectric screening with atomic-layer precision, opening a fertile field of fundamental research. The optical analyses used so far have relied on interband spectroscopy. Here we demonstrate how a capping layer of hexagonal boron nitride (hBN) renormalizes the internal structure of excitons in a WSe$_2$ monolayer using intraband transitions. Ultrabroadband terahertz probes sensitively map out the full complex-valued mid-infrared conductivity of the heterostructure after optical injection of $1s$ A excitons. This approach allows us to trace the energies and linewidths of the atom-like $1s$-$2p$ transition of optically bright and dark excitons as well as the densities of these quasiparticles. The fundamental excitonic resonance red shifts and narrows in the WSe$_2$/hBN heterostructure compared to the bare monolayer. Furthermore, the ultrafast temporal evolution of the mid-infrared response function evidences the formation of optically dark excitons from an initial bright population. Our results provide key insight into the effect of non local screening on electron-hole correlations and open new possibilities of dielectric engineering of van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2018

Light emission from gold nanoparticles under ultrafast near-infrared excitation: thermal emission, inelastic light scattering or multiphoton luminescence?

Gold nanoparticles emit broad-band upconverted luminescence upon irradiation with pulsed infrared laser radiation. Although the phenomenon is widely observed, considerable disagreement still exists concerning the underlying physics - most notably over the applicability of concepts such as multiphoton absorption, inelastic scattering, and interband and intraband electronic transitions. Here, we study single particles and small clusters of particles by employing a spectrally resolved power-law analysis of the irradiation-dependent emission as a sensitive probe of these physical models. Two regimes of emission are identified: at low irradiance levels of kW/cm2, the emission follows a well-defined integer-exponent power law suggestive of a multiphoton process. However, at higher irradiance levels of several kW/cm2, the nonlinearity exponent itself depends on the photon energy detected, a tell-tale signature of a radiating heated electron gas. We show that in this regime, the experiments are incompatible with both interband transitions and inelastic light scattering as the cause the luminescence, while they are compatible with the notion of luminescence linked to intraband transitions.

cond-mat.mtrl-sci↗