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Ursula Keller

Publications and source records attributed to Ursula Keller.

30 records · Page 2Linked to original sources

Time delay anisotropy in photoelectron emission from the isotropic ground state of helium

Time delays of electrons emitted from an isotropic initial state and leaving behind an isotropic ion are assumed to be angle-independent. Using an interferometric method involving XUV attosecond pulse trains and an IR probe field in combination with a detection scheme, which allows for full 3D momentum resolution, we show that measured time delays between electrons liberated from the $1s^2$ spherically symmetric ground state of helium depend on the emission direction of the electrons relative to the linear polarization axis of the ionizing XUV light. Such time-delay anisotropy, for which we measure values as large as 60 attoseconds, is caused by the interplay between final quantum states with different symmetry and arises naturally whenever the photoionization process involves the exchange of more than one photon in the field of the parent-ion. With the support of accurate theoretical models, the angular dependence of the time delay is attributed to small phase differences that are induced in the laser-driven continuum transitions to the final states. Since most measurement techniques tracing attosecond electron dynamics involve the exchange of at least two photons, this is a general, significant, and initially unexpected effect that must be taken into account in all such photoionization measurements.

physics.atom-ph↗

Efficient Spectral Broadening in the 100-W Average Power Regime Using Gas Filled Kagome HC-PCF and Pulse Compression

We present nonlinear pulse compression of a high-power SESAM-modelocked thin-disk laser (TDL) using an Ar-filled hypocycloid-core Kagome Hollow-Core Photonic Crystal Fiber (HC-PCF). The output of the modelocked Yb:YAG TDL with 127 W average power, a pulse repetition rate of 7 MHz, and a pulse duration of 740 fs was spectrally broadened 16-fold while propagating in a Kagome HC-PCF containing 13 bar of static Argon gas. Subsequent compression tests performed using 8.4% of the full available power resulted in a pulse duration as short as 88 fs using the spectrally broadened output from the fiber. Compressing the full transmitted power through the fiber (118 W) could lead to a compressed output of >100 W of average power and >100 MW of peak power with an average power compression efficiency of 88%. This simple laser system with only one ultrafast laser oscillator and a simple single-pass fiber pulse compressor, generating both high peak power >100 MW and sub-100-fs pulses at megahertz repetition rate, is very interesting for many applications such as high harmonic generation and attosecond science with improved signal-to-noise performance.

physics.optics↗

Mid-infrared pulse generation via achromatic quasi-phase-matched OPCPA

We demonstrate a new regime for mid-infrared optical parametric chirped pulse amplification (OPCPA) based on achromatic quasi-phase-matching. Our mid-infrared OPCPA system is based on collinear aperiodically poled lithium niobate (APPLN) pre-amplifiers and a non-collinear PPLN power amplifier. The idler output has a bandwidth of 800 nm centered at 3.4 $μ$m. After compression, we obtain a pulse duration of 44.2 fs and a pulse energy of 21.8 $μ$J at a repetition rate of 50 kHz. We explain the wide applicability of the non-collinear QPM amplification scheme we used, including how it can enable octave-spanning OPCPA in a single device when combined with an aperiodic QPM grating.

physics.optics↗

Multiphoton transitions for delay-zero calibration in attosecond spectroscopy

The exact delay-zero calibration in an attosecond pump-probe experiment is important for the correct interpretation of experimental data. In attosecond transient absorption spectroscopy the determination of the delay-zero exclusively from the experimental results is not straightforward and may introduce significant errors. Here, we report the observation of quarter-laser-cycle (4ω) oscillations in a transient absorption experiment in helium using an attosecond pulse train overlapped with a precisely synchronized, moderately strong infrared pulse. We demonstrate how to extract and calibrate the delay-zero with the help of the highly nonlinear 4ω signal. A comparison with the solution of the time-dependent Schrödinger equation is used to confirm the accuracy and validity of the approach. Moreover, we study the mechanisms behind the quarter-laser-cycle and the better-known half-laser-cycle oscillations as a function of experimental parameters. This investigation yields an indication of the robustness of our delay-zero calibration approach.

physics.atom-ph↗

Gigahertz Self-referenceable Frequency Comb from a Semiconductor Disk Laser

We present a 1.75-GHz self-referenceable frequency comb from a vertical external-cavity surface-emitting laser (VECSEL) passively modelocked with a semiconductor saturable absorber mirror (SESAM). The VECSEL delivers 231-fs pulses with an average power of 100 mW and is optimized for stable and reliable operation. The optical spectrum was centered around 1038 nm and nearly transform-limited with a full width half maximum (FWHM) bandwidth of 5.5 nm. The pulses were first amplified to an average power of 5.5 W using a backward-pumped Yb-doped double-clad large mode area (LMA) fiber and then compressed to 85 fs with 2.2 W of average power with a passive LMA fiber and transmission gratings. Subsequently, we launched the pulses into a highly nonlinear photonic crystal fiber (PCF) and generated a coherent octave-spanning supercontinuum (SC). We then detected the carrier-envelope offset (CEO) frequency (fCEO) beat note using a standard f-to-2f-interferometer. The fCEO exhibits a signal-to-noise ratio of 17 dB in a 100-kHz resolution bandwidth and a FWHM of 10 MHz. To our knowledge, this is the first report on the detection of the fCEO from a semiconductor laser, opening the door to fully stabilized compact frequency combs based on modelocked semiconductor disk lasers.

physics.optics↗

Transferring the attoclock technique to velocity map imaging

Attosecond angular streaking measurements have revealed deep insights into the timing of tunnel ionization processes of atoms in intense laser fields. So far experiments of this type have been performed only with a cold-target recoil-ion momentum spectrometer (COLTRIMS). Here, we present a way to apply attosecond angular streaking experiments to a velocity map imaging spectrometer (VMIS) with few-cycle pulses at a repetition rate of 10 kHz and a high ionization yield per pulse. Three-dimensional photoelectron momentum distributions from strong-field ionization of helium with an elliptically polarized, sub-10-fs pulse were retrieved by tomographic reconstruction from the momentum space electron images and used for the analysis in the polarization plane.

physics.atom-ph↗

Comparison of different approaches to the longitudinal momentum spread after tunnel ionization

We introduce a method to investigate the longitudinal momentum spread resulting from strong-field tunnel ionization of Helium which, unlike other methods, is valid for all ellipticities of laser pulse. Semiclassical models consisting of tunnel ionization followed by classical propagation in the combined ion and laser field reproduce the experimental results if an initial longitudinal spread at the tunnel exit is included. The values for this spread are found to be of the order of twice the transverse momentum spread.

physics.atom-ph↗

Virtual single-photon transition interrupted: time-gated optical gain and loss

The response of matter to an optical excitation consists essentially of absorption and emission. Traditional spectroscopy accesses the frequency-resolved and time-integrated response, while the temporal evolution stays concealed. However, we will demonstrate here that the temporal evolution of a virtual single-photon transition can be mapped out by a second pulsed electromagnetic field. The resulting optical signal shows previously unexpected optical gain and loss, which can be gated and controlled via the relative delay of the electromagnetic fields. The model presented here can be applied to any system that assumes a two-level character through near-resonant optical dipole excitation, whether they are of atomic, molecular or even solid-state nature. These theoretical observations are in excellent qualitative agreement with our transient absorption spectroscopy study in helium. The presented results can act as starting point for a new scheme for creating optical gain, which is a prerequisite for the operation of lasers. It may be possible to open the doors to spectral regions, which were difficult to access until now, e.g. in the extreme ultraviolet.

physics.atom-ph↗

Tunneling Time in Ultrafast Science is Real and Probabilistic

We compare the main competing theories of tunneling time against experimental measurements using the attoclock in strong laser field ionization of helium atoms. Refined attoclock measurements reveal a real and not instantaneous tunneling delay time over a large intensity regime, using two different experimental apparatus. Only two of the theoretical predictions are compatible within our experimental error: the Larmor time, and the probability distribution of tunneling times constructed using a Feynman Path Integral (FPI) formulation. The latter better matches the observed qualitative change in tunneling time over a wide intensity range, and predicts a broad tunneling time distribution with a long tail. The implication of such a probability distribution of tunneling times, as opposed to a distinct tunneling time, challenges how valence electron dynamics are currently reconstructed in attosecond science. It means that one must account for a significant uncertainty as to when the hole dynamics begin to evolve.

physics.atom-ph↗

Rydberg states and momentum bifurcation in tunnel ionization with elliptically polarized light

It is well-known from numerical and experimental results that the fraction of Rydberg states (excited neutral atoms) created by tunnel ionization declines dramatically with increasing ellipticity of laser light. We present a method to analyze this dependence on ellipticity, deriving a probability distribution of Rydberg states that agrees closely with recent experimental [1] and numerical results. In particular, contradicting the existing proposed mechanism [1] and general expectations, our results indicate that the dependence of Rydberg yield on laser ellipticity is not caused by a rescattering process. Rather, we show that most Rydberg electrons never come back to the vicinity of the exit point after ionization, and end up relatively far from the atom (compared to the exit point) after the laser pulse has passed. We also present experimental data revealing a bifurcation that corresponds to a cut-off in Rydberg generation, and present an analytic derivation with a perturbative inclusion of the Coloumb force. [1] T. Nubbemeyer, K. Gorling, A. Saenz, U. Eichmann, and W. Sandner, Phys. Rev. Lett. 101, 233001 (2008).

physics.atom-ph↗

Probing the longitudinal momentum spread of the electron wave packet at the tunnel exit

We present an ellipticity resolved study of momentum distributions arising from strong-field ionization of Helium at constant intensity. The influence of the ion potential on the departing electron is considered within a semi-classical model consisting of an initial tunneling step and subsequent classical propagation. We find that the momentum distribution can be explained by the presence of a longitudinal momentum spread of the electron at the exit from the tunnel. Our combined experimental and theoretical study provides an estimate of this momentum spread.

physics.atom-ph↗

Attoclock reveals geometry for laser-induced tunneling

Tunneling plays a central role in the interaction of matter with intense laser pulses, and also in time-resolved measurements on the attosecond timescale. A strong laser field influences the binding potential of an electron in an atom so strongly, that a potential barrier is created which enables the electron to be liberated through tunneling. An important aspect of the tunneling is the geometry of the tunneling current flow. Here we provide experimental access to the tunneling geometry and provide a full understanding of the laser induced tunnel process in space and time. We perform laser tunnel ionization experiments using the attoclock technique, and present a correct tunneling geometry for helium and argon. In addition for argon the potential barrier is significantly modified by all the electrons remaining in the ion, and furthermore from a quantum state whose energy is Stark-shifted by the external field. The resulting modified potential geometry influences the dynamics of the liberated electron, changes important physical parameters and affects the interpretation of attosecond measurements. These effects will become even more pronounced for molecules and surfaces, which are more polarizable.

physics.atom-ph↗