Stefanos Carlström

Noncollinear optical gating

We present a novel scheme for high-order harmonic generation, enabling the production of spatially separated isolated attosecond pulses. This can be achieved by driving the generation process with two identical, but temporally delayed laser pulses, which are noncollinearly overlapping in the generation medium. Our approach provides intense attosecond pulses directly separated from the fundamental field, which is left undistorted. The method is therefore ideally suited for pump-probe studies in the extreme ultraviolet regime and promises new advances for intra-cavity attosecond pulse generation. We present a theoretical description of noncollinear optical gating, with an analytical derivation and simulations using the strong field approximation.

High-order harmonic generation using a high-repetition-rate turnkey laser

We generate high-order harmonics at high pulse repetition rates using a turnkey laser. High-order harmonics at 400 kHz are observed when argon is used as target gas. In neon, we achieve generation of photons with energies exceeding 90 eV (∼13 nm) at 20 kHz. We measure a photon flux of up to 4.4 × 10(10) photons per second per harmonic in argon at 100 kHz. Many experiments employing high-order harmonics would benefit from higher repetition rates, and the user-friendly operation opens up for applications of coherent extreme ultra-violet pulses in new research areas.

Sub-cycle ionization dynamics revealed by trajectory resolved, elliptically-driven high-order harmonic generation

The sub-cycle dynamics of electrons driven by strong laser fields is central to the emerging field of attosecond science. We demonstrate how the dynamics can be probed through high-order harmonic generation, where different trajectories leading to the same harmonic order are initiated at different times, thereby probing different field strengths. We find large differences between the trajectories with respect to both their sensitivity to driving field ellipticity and resonant enhancement. To accurately describe the ellipticity dependence of the long trajectory harmonics we must include a sub-cycle change of the initial velocity distribution of the electron and its excursion time. The resonant enhancement is observed only for the long trajectory contribution of a particular harmonic when a window resonance in argon, which is off-resonant in the field-free case, is shifted into resonance due to a large dynamic Stark shift.

Spatially and spectrally resolved quantum path interference with chirped driving pulses

We measure spectrally and spatially resolved high-order harmonics generated in argon using chirped multi-cycle laser pulses. Using a stable, high-repetition rate laser we observe detailed interference structures in the far-field. The structures are of two kinds; off-axis interference from the long trajectory only and on-axis interference including the short and long trajectories. The former is readily visible in the far-field spectrum, modulating both the spectral and spatial profile. To access the latter, we vary the chirp of the fundamental, imparting different phases on the different trajectories, thereby changing their relative phase. Using this method together with an analytical model, we are able to explain the on-axis behaviour and access the dipole phase parameters for the short (\(\alpha_s\)) and long (\(\alpha_l\)) trajectories. The extracted results compare very well with phase parameters calculated by solving the time-dependent Schrodinger equation. Going beyond the analytical model, we are also able to successfully reproduce the off-axis interference structure.

Quantum coherence in photo-ionisation with tailored XUV pulses

Ionisation with ultrashort pulses in the extreme ultraviolet (XUV) regime can be used to prepare an ion in a superposition of spin-orbit substates. In this work, we study the coherence properties of such a superposition, created by ionising xenon atoms using two phase-locked XUV pulses at different frequencies. In general, if the duration of the driving pulse exceeds the quantum beat period, dephasing will occur. If however, the frequency difference of the two pulses matches the spin-orbit splitting, the coherence can be efficiently increased and dephasing does not occur.

Phase metrology with multi-cycle two-colour pulses

Strong-field phenomena driven by an intense infrared (IR) laser depend on during what part of the field cycle they are initiated. By changing the sub-cycle character of the laser electric field it is possible to control such phenomena. For long pulses, sub-cycle shaping of the field can be done by adding a relatively weak, second harmonic of the driving field to the pulse. Through constructive and destructive interference, the combination of strong and weak fields can be used to change the probability of a strong-field process being initiated at any given part of the cycle. In order to control sub-cycle phenomena with optimal accuracy, it is necessary to know the phase difference of the strong and the weak fields precisely. If the weaker field is an even harmonic of the driving field, electrons ionized by the field will be asymmetrically distributed between the positive and negative directions of the combined fields. Information about the asymmetry can yield information about the phase difference. A technique to measure asymmetry for few-cycle pulses, called Stereo-ATI (Above Threshold Ionization), has been developed by [Paulus G G, et al 2003 Phys. Rev. Lett. 91]. This paper outlines an extension of this method to measure the phase difference between a strong IR and its second harmonic.

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 (HHG) 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 semi-classical three-step model for HHG.

High-Order Harmonic Generation and Plasmonics

Attosecond pulses allow for imaging of very fast processes, like electron dynamics. Stockman et al. suggested to use these pulses in connection with a Photoemission electron microscope (PEEM) to study the ultrafast dynamics of plasmons (Stockman et al. Nat Photonics 1:539–544, 2007). For efficient plasmon studies, the repetition rate of the attosecond pulses used needs to be higher than a few kHz (Mikkelsen et al. Rev Sci Instrum 80:123703, 2009). Attosecond pulses are produced in a process called high-order harmonic generation (HHG) (Paul et al. Science 292(5522):1689–1692, 2001; Ferray et al. J Phys B At Mol Opt Phys 21:L31–L35, 1988). In HHG, a strong laser field allows an electron to tunnel out, get accelerated and recombine with a high kinetic energy resulting in extreme ultraviolet attosecond pulses. The large intensity needed to drive the process normally limits the repetition rate of the laser to a few kHz. Using a tight focusing scheme (Heyl et al. Phys Rev Lett 107:033903, 2011; Vernaleken et al. Opt Lett 36:3428–3430, 2011), we, however, generate harmonics at a repetition rate of 200 kHz, both with a commercial turn-key laser and with an advanced laser system. Suitable nanostructures for a strong field enhancement are produced in-house and the field enhancement is studied with PEEM in a non-time resolved manner. With high-order harmonics produced at a high repetition rate, we hope to be able to follow also the ultrafast dynamics of plasmons in these structures (Marsell et al. Ann der Phys 525:162–170, 2013).

Photoionization time delay measurement close to a Fano resonance using tunable attosecond pulses

We investigate the influence of a Fano resonance on the delays for electron emission in two-photon, near-resonant ionization of argon. The delays were measured using an interferometric method that employed an attosecond pulse train.