arXiv subjects

U. Keller

Publications and source records attributed to U. Keller.

17 recordsLinked to original sources

arXiv2023

Coherently averaged dual-comb spectroscopy with a low-noise and high-power free-running gigahertz dual-comb laser

We present a new type of dual optical frequency comb source capable of scaling applications to high measurement speeds while combining high average power, ultra-low noise operation, and a compact setup. Our approach is based on a diode-pumped solid-state laser cavity which includes an intracavity biprism operated at Brewster angle to generate two spatially-separated modes with highly correlated properties. The 15-cm-long cavity uses an Yb:CALGO crystal and a SESAM as an end mirror to generate more than 3 W average power per comb, below 80 fs pulse duration, a repetition rate of 1.03 GHz, and a continuously tunable repetition rate difference up to 27 kHz. We carefully investigate the coherence properties of the dual-comb by a series of heterodyne measurements, revealing several important features: (1) ultra-low jitter on the uncorrelated part of the timing noise; (2) the radio frequency comb lines of the interferograms are fully resolved in free-running operation; (3) we validate that through a simple measurement of the interferograms we can determine the fluctuations of the phase of all the radio frequency comb lines; (4) this phase information is used in a post-processing routine to perform coherently averaged dual-comb spectroscopy of acetylene (C2H2) over long timescales. Our results represent a powerful and general approach to dual-comb applications by combining low noise and high power operation directly from a highly compact laser oscillator.

physics.optics↗

arXiv2022

Ultrafast electron localization and screening in a transition metal dichalcogenide

The coupling of light to electrical charge carriers in semiconductors is the foundation of many technological applications. Attosecond transient absorption spectroscopy measures simultaneously how excited electrons and the vacancies they leave behind dynamically react to the applied optical fields. In compound semiconductors, these dynamics can be probed via any of their atomic constituents. Often, the atomic species forming the compound contribute comparably to the relevant electronic properties of the material. One therefore expects to observe similar dynamics, irrespective of the choice of atomic species via which it is probed. Here, we show in the two-dimensional transition metal dichalcogenide semiconductor $MoSe_2$, that through a selenium-based transition we observe charge carriers acting independently from each other, while when probed through molybdenum, the collective, many-body motion of the carriers dominates. Such unexpectedly contrasting behavior can be traced back to a strong localization of electrons around molybdenum atoms following absorption of light, which modifies the local fields acting on the carriers. We show that similar behavior in elemental titanium metal carries over to transition metal-containing compounds and is expected to play an essential role for a wide range of such materials. Knowledge of independent particle and collective response is essential for fully understanding these materials.

cond-mat.mtrl-sci↗

arXiv2022

Spatially multiplexed single-cavity dual-comb laser

Single-cavity dual-comb lasers are a new class of ultrafast lasers which have a wide possible application space including pump-probe sampling, optical ranging, and gas absorption spectroscopy. However, to this date laser cavity multiplexing usually came to the trade-off in laser performance or relative timing noise suppression. We present a new method for multiplexing a single laser cavity to support a pair of noise-correlated modes. These modes share all intracavity components and take a near-common path, but do not overlap on any active elements. We implement the method with an 80-MHz laser delivering more than 2.4 Watts of average power per comb with sub-140 fs pulses. We reach sub-cycle relative timing jitter of 2.2 fs [20 Hz, 100 kHz]. With this new multiplexing technique, we could implement slow feedback on the repetition rate difference Δfrep, enabling this quantity to be drift-free, low-jitter, and adjustable - a key combination for practical applications that was lacking in prior single-cavity dual-comb systems.

physics.optics↗

arXiv2019

Attoclock revisited on electron tunnelling time

The last decade has seen an intense renewed debate on tunnelling time, both from a theoretical and an experimental perspective. Here, we review recent developments and new insights in the field of strong-field tunnel ionization related to tunnelling time, and apply these findings to the interpretation of the attoclock experiment [Landsman et al., Optica 1, 343 (2014)]. We conclude that models including finite tunnelling time are consistent with recent experimental measurements.

physics.atom-ph↗

arXiv2018

Attosecond screening dynamics mediated by electron-localization

Transition metals with their densely confined and strongly coupled valence electrons are key constituents of many materials with unconventional properties, such as high-Tc superconductors, Mott insulators and transition-metal dichalcogenides. Strong electron interaction offers a fast and efficient lever to manipulate their properties with light, creating promising potential for next-generation electronics. However, the underlying dynamics is a fast and intricate interplay of polarization and screening effects, which is poorly understood. It is hidden below the femtosecond timescale of electronic thermalization, which follows the light-induced excitation. Here, we investigate the many-body electron dynamics in transition metals before thermalization sets in. We combine the sensitivity of intra-shell transitions to screening effects with attosecond time resolution to uncover the interplay of photo-absorption and screening. First-principles time-dependent calculations allow us to assign our experimental observations to ultrafast electronic localization on d-orbitals. The latter modifies the whole electronic structure as well as the collective dynamic response of the system on a timescale much faster than the light-field cycle. Our results demonstrate a possibility for steering the electronic properties of solids prior to electron thermalization, suggesting that the ultimate speed of electronic phase transitions is limited only by the duration of the controlling laser pulse. Furthermore, external control of the local electronic density serves as a fine tool for testing state-of-the art models of electron-electron interactions. We anticipate our study to facilitate further investigations of electronic phase transitions, laser-metal interactions and photo-absorption in correlated electron systems on its natural timescale.

physics.atom-ph↗

arXiv2017

Interplay between Coulomb-focusing and non-dipole effects in strong-field ionization with elliptical polarization

Strong-field ionization and rescattering beyond the long-wavelength limit of the dipole approximation is studied with elliptically polarized mid-IR pulses. We have measured the full three-dimensional photoelectron momentum distributions (3D PMDs) with velocity map imaging and tomographic reconstruction. The ellipticity-dependent 3D-PMD measurements revealed an unexpected sharp, thin line-shaped ridge structure in the polarization plane for low momentum photoelectrons. With classical trajectory Monte Carlo (CTMC) simulations and analytical methods we identified the associated ionization dynamics for this sharp ridge to be due to Coulomb focusing of slow recollisions of electrons with a momentum approaching zero. This ridge is another example of the many different ways how the Coulomb field of the parent ion influences the different parts of the momentum space of the ionized electron wave packet. Building on this new understanding of the PMD, we extend our studies on the role played by the magnetic field component of the laser beam when operating beyond the long-wavelength limit of the dipole approximation. In this regime, we find that the PMD exhibits an ellipticity-dependent asymmetry along the beam propagation direction: the peak of the projection of the PMD onto the beam propagation axis is shifted from negative to positive values with increasing ellipticity. This turnover occurs rapidly once the ellipticity exceeds $\sim$0.1. We identify the sharp, thin line-shaped ridge structure in the polarization plane as the origin of the ellipticity-dependent PMD asymmetry in the beam propagation direction. These results yield fundamental insights into strong-field ionization processes, and should increase the precision of the emerging applications relying on this technique, including time-resolved holography and molecular imaging.

physics.atom-ph↗

arXiv2015

Ptychographic reconstruction of attosecond pulses

We demonstrate a new attosecond pulse reconstruction modality which uses an algorithm that is derived from ptychography. In contrast to other methods, energy and delay sampling are not correlated, and as a result, the number of electron spectra to record is considerably smaller. Together with the robust algorithm, this leads to a more precise and fast convergence of the reconstruction.

physics.optics↗

arXiv2015

Frequency-domain nonlinear optics in two-dimensionally patterned quasi-phase-matching media

Advances in the amplification and manipulation of ultrashort laser pulses has led to revolutions in several areas. Examples include chirped pulse amplification for generating high peak-power lasers, power-scalable amplification techniques, pulse shaping via modulation of spatially-dispersed laser pulses, and efficient frequency-mixing in quasi-phase-matched nonlinear crystals to access new spectral regions. In this work, we introduce and demonstrate a new platform for nonlinear optics which has the potential to combine all of these separate functionalities (pulse amplification, frequency transfer, and pulse shaping) into a single monolithic device. Moreover, our approach simultaneously offers solutions to the performance-limiting issues in the conventionally-used techniques, and supports scaling in power and bandwidth of the laser source. The approach is based on two-dimensional patterning of quasi-phase-matching gratings combined with optical parametric interactions involving spatially dispersed laser pulses. Our proof of principle experiment demonstrates this new paradigm via mid-infrared optical parametric chirped pulse amplification of few-cycle pulses.

physics.optics↗

arXiv2015

Gravitational slopes, geomorphology, and material strengths of the nucleus of comet 67P/Churyumov-Gerasimenko from OSIRIS observations

We study the link between gravitational slopes and the surface morphology on the nucleus of comet 67P/Churyumov-Gerasimenko and provide constraints on the mechanical properties of the cometary material. We computed the gravitational slopes for five regions on the nucleus that are representative of the different morphologies observed on the surface, using two shape models computed from OSIRIS images by the stereo-photoclinometry (SPC) and stereo-photogrammetry (SPG) techniques. We estimated the tensile, shear, and compressive strengths using different surface morphologies and mechanical considerations. The different regions show a similar general pattern in terms of the relation between gravitational slopes and terrain morphology: i) low-slope terrains (0-20 deg) are covered by a fine material and contain a few large ($>$10 m) and isolated boulders, ii) intermediate-slope terrains (20-45 deg) are mainly fallen consolidated materials and debris fields, with numerous intermediate-size boulders from $<$1 m to 10 m for the majority of them, and iii) high-slope terrains (45-90 deg) are cliffs that expose a consolidated material and do not show boulders or fine materials. The best range for the tensile strength of overhangs is 3-15 Pa (upper limit of 150 Pa), 4-30 Pa for the shear strength of fine surface materials and boulders, and 30-150 Pa for the compressive strength of overhangs (upper limit of 1500 Pa). The strength-to-gravity ratio is similar for 67P and weak rocks on Earth. As a result of the low compressive strength, the interior of the nucleus may have been compressed sufficiently to initiate diagenesis, which could have contributed to the formation of layers. Our value for the tensile strength is comparable to that of dust aggregates formed by gravitational instability and tends to favor a formation of comets by the accrection of pebbles at low velocities.

astro-ph.EP↗

arXiv2015

The effect of electron-electron correlation on the attoclock experiment

We investigate multi-electron effects in strong-field ionization of Helium using a semi-classical model that, unlike other commonly used theoretical approaches, takes into account electron-electron correlation. Our approach has an additional advantage of allowing to selectively switch off different contributions from the parent ion (such as the remaining electron or the nuclear charge) and thereby investigate in detail how the final electron angle in the attoclock experiment is influenced by these contributions. We find that the bound electron exerts a significant effect on the final electron momenta distribution that can, however, be accounted for by an appropriately selected mean field. Our results show excellent agreement with other widely used theoretical models done within a single active electron approximation.

physics.atom-ph↗

arXiv2015

Energy-dependent photoemission delays from noble metal surfaces by attosecond interferometry

How quanta of energy and charge are transported on both atomic spatial and ultrafast time scales is at the heart of modern technology. Recent progress in ultrafast spectroscopy has allowed us to directly study the dynamical response of an electronic system to interaction with an electromagnetic field. Here, we present energy-dependent photoemission delays from the noble metal surfaces Ag(111) and Au(111). An interferometric technique based on attosecond pulse trains is applied simultaneously in a gas phase and a solid state target to derive surface-specific photoemission delays. Experimental delays on the order of 100 as are in the same time range as those obtained from simulations. The strong variation of measured delays with excitation energy in Ag(111), which cannot be consistently explained invoking solely electron transport or initial state localization as supposed in previous work, indicates that final state effects play a key role in photoemission from solids.

cond-mat.other↗

arXiv2015

Resonance effects in photoemission time delays

We present measurements of single-photon ionization time delays between valence electrons of argon and neon using a coincidence detection technique that allows for the simultaneous measurement of both species under identical conditions. Taking into account the chirp of the ionizing single attosecond pulse (attochirp) ensures that the clock of our measurement technique is started at the same time for both types of electrons, revealing with high accuracy and resolution energy-dependent time delays of a few tens of attoseconds. By comparing our results with theoretical predictions, we confirm that the so-called Wigner delay correctly describes single-photon ionization delays as long as atomic resonances can be neglected. Our data, however, also reveal that such resonances can greatly affect the measured delays beyond the simple Wigner picture.

physics.atom-ph↗

arXiv2014

Breakdown of the Dipole Approximation in Strong-Field Ionization

We report the breakdown of the electric dipole approximation in the long-wavelength limit in strong-field ionization with linearly polarized few-cycle mid-infrared laser pulses at intensities on the order of 10$^{13}$ W/cm$^2$. Photoelectron momentum distributions were recorded by velocity map imaging and projected onto the beam propagation axis. We observe an increasing shift of the peak of this projection opposite to the beam propagation direction with increasing laser intensities. From a comparison with semi-classical simulations, we identify the combined action of the magnetic field of the laser pulse and the Coulomb potential as origin of our observations.

physics.atom-ph↗

arXiv2013

Ultrafast and widely tuneable vertical-external-cavity surface-emitting laser, mode-locked by a graphene-integrated distributed Bragg reflector

We report a versatile and cost-effective way of controlling the unsaturated loss, modulation depth and saturation fluence of graphene-based saturable absorbers (GSAs), by changing the thickness of a spacer between SLG and a high-reflection mirror. This allows us to modulate the electric field intensity enhancement at the GSA from 0 up to 400%, due to the interference of incident and reflected light at the mirror. The unsaturated loss of the SLG-mirror-assembly can be reduced to$\sim$0. We use this to mode-lock a VECSEL from 935 to 981nm. This approach can be applied to integrate SLG into various optical components, such as output coupler mirrors, dispersive mirrors, dielectric coatings on gain materials. Conversely, it can also be used to increase absorption (up to 10%) in various graphene based photonics and optoelectronics devices, such as photodetectors.

cond-mat.mtrl-sci↗

arXiv2012

Sequential Tunneling vs. Electron Correlation in Multiple Photo-ionization

We take advantage of the information provided by use of elliptical polarization in a recent two-electron release time experiment [A.N. Pfeiffer et al., Nature Physics 7, 428 (2011)]. This allows a comparative test of the currently dominant conjectures regarding independent-electron tunneling theory vs. fully electron-correlated classical release theory to describe electron release in strong-field double ionization.

physics.atom-ph↗

arXiv2008

Spectral signature of short attosecond pulse trains

We report experimental measurements of high-order harmonic spectra generated in Ar using a carrier-envelope-offset (CEO) stabilized 12 fs, 800nm laser field and a fraction (less than 10%) of its second harmonic. Additional spectral peaks are observed between the harmonic peaks, which are due to interferences between multiple pulses in the train. The position of these peaks varies with the CEO and their number is directly related to the number of pulses in the train. An analytical model, as well as numerical simulations, support our interpretation.

physics.atom-ph↗

arXiv2004

Phase-preserving chirped-pulse optical parametric amplification to 17.3 fs directly from a Ti:Sapphire oscillator

Phase-stabilized 12-fs, 1-nJ pulses from a commercial Ti:sapphire oscillator are directly amplified in a chirped-pulse optical parametric amplifier and recompressed to yield near-transform-limited 17.3-fs pulses. The amplification process is demonstrated to be phase preserving and leads to 85-uJ, carrier-envelope-offset phase-locked pulses at 1 kHz for 0.9 mJ of pump, corresponding to a single-pass gain of 8.5 x 10^4.

physics.optics↗