arXiv subjects

Cord L. Arnold

Publications and source records attributed to Cord L. Arnold.

31 records · Page 2Linked to original sources

arXiv2020

Attosecond electron-spin dynamics in Xe 4d photoionization

The photoionization of xenon atoms in the 70-100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe$^+$ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide new insight into the complex electron-spin dynamics of photo-induced phenomena.

physics.atom-ph↗

arXiv2020

Single-shot d-scan technique for ultrashort laser pulse characterization using transverse second-harmonic generation in random nonlinear crystals

We demonstrate a novel dispersion-scan (d-scan) scheme for single-shot temporal characterization of ultrashort laser pulses. The novelty of this method relies on the use of a highly dispersive crystal featuring antiparallel nonlinear domains with a random distribution and size. This crystal, capable of generating a transverse second-harmonic signal, acts simultaneously as the dispersive element and the nonlinear medium of the d-scan device. The resulting in-line architecture makes the technique very simple and robust, allowing the acquisition of single-shot d-scan traces in real time. In addition, the technique can be further simplified by avoiding the need of dispersion pre-compensation. The retrieved pulses are in very good agreement with independent FROG measurements. We also apply the new single-shot d-scan to a TW-class laser equipped with a programmable pulse shaper, obtaining an excellent agreement between the applied and the d-scan retrieved dispersions.

physics.optics↗

arXiv2020

Post-compression of picosecond pulses into the few-cycle regime

In this work, we demonstrate post-compression of 1.2 picosecond laser pulses to 13 fs via gas-based multi-pass spectral broadening. Our results yield a single-stage compression factor of about 40 at 200 W in-burst average power and a total compression factor >90 at reduced power. The employed scheme represents a route towards compact few-cycle sources driven by industrial-grade Yb:YAG lasers at high average power.

physics.optics↗

arXiv2020

Few-cycle lightwave-driven currents in a semiconductor at high repetition rate

When an intense, few-cycle light pulse impinges on a dielectric or semiconductor material, the electric field will interact nonlinearly with the solid, driving a coherent current. An asymmetry of the ultrashort, carrier-envelope-phase-stable waveform results in a net transfer of charge, which can be measured by macroscopic electric contact leads. This effect has been pioneered with extremely short, single-cycle laser pulses at low repetition rate, thus limiting the applicability of its potential for ultrafast electronics. We investigate lightwave-driven currents in gallium nitride using few-cycle laser pulses of nearly twice the duration and at a repetition rate two orders of magnitude higher than in previous work. We successfully simulate our experimental data with a theoretical model based on interfering multiphoton transitions, using the exact laser pulse shape retrieved from dispersion-scan measurements. Substantially increasing the repetition rate and relaxing the constraint on the pulse duration marks an important step forward towards applications of lightwave-driven electronics.

physics.optics↗

arXiv2019

Controlling the Photoelectric Effect in the Time Domain

When an atom or molecule absorbs a high-energy photon, an electron is emitted with a well-defined energy and a highly-symmetric angular distribution, ruled by energy quantization and parity conservation. These rules seemingly break down when small quantum systems are exposed to short and intense light pulses, which raise the question of their universality for the simplest case of the photoelectric effect. Here we investigate the photoionization of helium by a sequence of attosecond pulses in the presence of a weak infrared dressing field. We continuously control the energy and introduce an asymmetry in the emission direction of the photoelectrons, thus contradicting well established quantum-mechanical predictions. This control is possible due to an extreme temporal confinement of the light-matter interaction. Our work extends time-domain coherent control schemes to one of the fastest processes in nature, the photoelectric effect.

physics.atom-ph↗

arXiv2019

Spatial Control of Multiphoton Electron Excitations in InAs Nanowires by Varying Crystal Phase and Light Polarization

We demonstrate the control of multiphoton electron excitations in InAs nanowires (NWs) by altering the crystal structure and the light polarization. Using few-cycle, near-infrared laser pulses from an optical parametric chirped-pulse amplification system, we induce multiphoton electron excitations in InAs nanowires with controlled wurtzite (WZ) and zincblende (ZB) segments. With a photoemission electron microscope, we show that we can selectively induce multiphoton electron emission from WZ or ZB segments of the same wire by varying the light polarization. Developing \textit{ab-initio GW} calculations of 1st to 3rd order multiphoton excitations and using finite-difference time-domain simulations, we explain the experimental findings: While the electric-field enhancement due to the semiconductor/vacuum interface has a similar effect for all NW segments, the 2nd and 3rd order multiphoton transitions in the band structure of WZ InAs are highly anisotropic, in contrast to ZB InAs. As the crystal phase of NWs can be precisely and reliably tailored, our findings opens up for new semiconductor optoelectronics with controllable nanoscale emission of electrons through vacuum or dielectric barriers.

physics.optics↗

arXiv2019

Phase Control of Attosecond Pulses in a Train

Ultrafast processes in matter can be captured and even controlled by using sequences of few-cycle optical pulses, which need to be well characterized, both in amplitude and phase. The same degree of control has not yet been achieved for few-cycle extreme ultraviolet pulses generated by high-order harmonic generation in gases, with duration in the attosecond range. Here, we show that by varying the spectral phase and carrier-envelope phase (CEP) of a high-repetition rate laser, using dispersion in glass, we achieve a high degree of control of the relative phase and CEP between consecutive attosecond pulses. The experimental results are supported by a detailed theoretical analysis based upon the semiclassical three-step model for high-order harmonic generation.

physics.atom-ph↗

arXiv2019

Compact 200 kHz HHG source driven by a few-cycle OPCPA

We present efficient high-order harmonic generation (HHG) based on a high-repetition rate, few-cycle, near infrared (NIR), carrier-envelope phase stable, optical parametric chirped pulse amplifier (OPCPA), emitting 6fs pulses with 9μJ pulse energy at 200kHz repetition rate. In krypton, we reach conversion efficiencies from the NIR to the extreme ultraviolet (XUV) radiation pulse energy on the order of ~10^{-6} with less than 3μJ driving pulse energy. This is achieved by optimizing the OPCPA for a spatially and temporally clean pulse and by a specially designed high-pressure gas target. In the future, the high efficiency of the HHG source will be beneficial for high-repetition rate two-colour (NIR-XUV) pumpprobe experiments, where the available pulse energy from the laser has to be distributed economically between pump and probe pulses.

physics.atom-ph↗

arXiv2018

Spatio-temporal coupling of attosecond pulses

The shortest light pulses produced to date are of the order of a few tens of attoseconds, with central frequencies in the extreme ultraviolet range and bandwidths exceeding tens of eV. They are often produced as a train of pulses separated by half the driving laser period, leading in the frequency domain to a spectrum of high, odd-order harmonics. As light pulses become shorter and more spectrally wide, the widely-used approximation consisting in writing the optical waveform as a product of temporal and spatial amplitudes does not apply anymore. Here, we investigate the interplay of temporal and spatial properties of attosecond pulses. We show that the divergence and focus position of the generated harmonics often strongly depend on their frequency, leading to strong chromatic aberrations of the broadband attosecond pulses. Our argumentation uses a simple analytical model based on Gaussian optics, numerical propagation calculations and experimental harmonic divergence measurements. This effect needs to be considered for future applications requiring high quality focusing while retaining the broadband/ultrashort characteristics of the radiation.

physics.optics↗

arXiv2016

Controlled free-induction decay in the extreme ultraviolet

Coherent sources of attosecond extreme ultraviolet (XUV) radiation present many challenges if their full potential is to be realized. While many applications benefit from the broadband nature of these sources, it is also desirable to produce narrow band XUV pulses, or to study autoionizing resonances in a manner that is free of the broad ionization background that accompanies above-threshold XUV excitation. Here we demonstrate a method for controlling the coherent XUV free induction decay that results from using attosecond pulses to excite a gas, yielding a fully functional modulator for XUV wavelengths. We use an infrared (IR) control pulse to manipulate both the spatial and spectral phase of the XUV emission, sending the light in a direction of our choosing at a time of our choosing. This allows us to tailor the light using opto-optical modulation, similar to devices available in the IR and visible wavelength regions.

physics.atom-ph↗

arXiv2016

Generalized projection retrieval of dispersion scans for ultrashort pulse characterization

We present a retrieval algorithm based on generalized projections for ultrashort pulse characterization using dispersion scan (d-scan). The new algorithm is tested on several simulated cases and in two different experimental cases in the few-cycle regime. The proposed algorithm is much faster and leads to a drastic reduction of retrieval times, but performs less robust in the retrieval of noisy d-scan traces compared to the standard algorithm.

physics.optics↗

arXiv2015

Spatiotemporal characterization of ultrashort optical vortex pulses

Generation of few-cycle optical vortex pulses is challenging due to the large spectral bandwidths, as most vortex generation techniques are designed for monochromatic light. In this work, we use a spiral phase plate to generate few-cycle optical vortices from an ultrafast titanium:sapphire oscillator, and characterize them in the spatiotemporal domain using a recently introduced technique based on spatially resolved Fourier transform spectrometry. The performance of this simple approach to the generation of optical vortices is analyzed from a wavelength dependent perspective, as well as in the spatiotemporal domain, allowing us to completely characterize ultrashort vortex pulses in space, frequency, and time.

physics.optics↗

arXiv2015

Photoemission electron microscopy of localized surface plasmons in silver nanostructures at telecommunication wavelengths

We image the field enhancement at Ag nanostructures using femtosecond laser pulses with a center wavelength of 1.55 micrometer. Imaging is based on non-linear photoemission observed in a photoemission electron microscope (PEEM). The images are directly compared to ultra violet PEEM and scanning electron microscopy (SEM) imaging of the same structures. Further, we have carried out atomic scale scanning tunneling microscopy (STM) on the same type of Ag nanostructures and on the Au substrate. Measuring the photoelectron spectrum from individual Ag particles shows a larger contribution from higher order photoemission process above the work function threshold than would be predicted by a fully perturbative model, consistent with recent results using shorter wavelengths. Investigating a wide selection of both Ag nanoparticles and nanowires, field enhancement is observed from 30% of the Ag nanoparticles and from none of the nanowires. No laser-induced damage is observed of the nanostructures neither during the PEEM experiments nor in subsequent SEM analysis. By direct comparison of SEM and PEEM images of the same nanostructures, we can conclude that the field enhancement is independent of the average nanostructure size and shape. Instead, we propose that the variations in observed field enhancement could originate from the wedge interface between the substrate and particles electrically connected to the substrate.

cond-mat.mes-hall↗