Matthias F. Kling

Optical damage threshold of Au nanowires in strong femtosecond laser fields

Ultrashort, intense light pulses permit the study of nanomaterials in the optical non-linear regime. Non-linear regimes are often present just below the damage threshold thus requiring careful tuning of the laser parameters to avoid melting the materials. Detailed studies of the damage threshold of nanoscale materials are therefore needed. We present results on the damage threshold of gold (Au) nanowires when illuminated by intense femtosecond pulses. These nanowires were synthesized via the directed electrochemical nanowire assembly (DENA) process in two configurations: (1) free-standing Au nanowires on tungsten (W) electrodes and (2) Au nanowires attached to fused silica slides. In both cases the wires have a single-crystalline structure. For 790 nm laser pulses with durations of 108 fs and 32 fs at a repetition rate of 2 kHz, we find that the free-standing nanowires melt at intensities close to 3 TW/cm2 (194 mJ/cm2) and 7.5 TW/cm2 (144 mJ/cm2), respectively. The Au nanowires attached to silica slides melt at slightly higher intensities, just above 10 TW/cm2 (192 mJ/cm2) for 32 fs pulses. Our results can be explained with an electron-phonon interaction model that describes the absorbed laser energy and subsequent heat conduction across the wire.

Carrier-envelope-phase stabilized terawatt class laser at 1 kHz with a wavelength tunable option

We demonstrate a chirped-pulse-amplified Ti:Sapphire laser system operating at 1 kHz, with 20 mJ pulse energy, 26 femtosecond pulse duration (0.77 terawatt), and excellent long term carrier-envelope-phase (CEP) stability. A new vibrational damping technique is implemented to significantly reduce vibrational noise on both the laser stretcher and compressor, thus enabling a single-shot CEP noise value of 250 mrad RMS over 1 hour and 300 mrad RMS over 9 hours. This is, to the best of our knowledge, the best long term CEP noise ever reported for any terawatt class laser. This laser is also used to pump a white-light-seeded optical parametric amplifier, producing 6 mJ of total energy in the signal and idler with 18 mJ of pumping energy. Due to preservation of the CEP in the white-light generated signal and passive CEP stability in the idler, this laser system promises synthesized laser pulses spanning multi-octaves of bandwidth at an unprecedented energy scale.

Thick-lens velocity-map imaging spectrometer with high resolution for high-energy charged particles

A novel design for a velocity-map imaging (VMI) spectrometer with high resolution over a wide energy range surpassing a standard VMI design is reported. The main difference to a standard three-electrode VMI is the spatial extension of the applied field using 11 electrodes forming a thick-lens. This permits measurements of charged particles with higher energies while achieving excellent resolving power over a wide range of energies. Using SIMION simulations, the thick-lens VMI is compared to a standard design for up to 360 eV electrons. The simulations also show that the new spectrometer design is suited for charged-particle detection with up to 1 keV using a repeller-electrode voltage of -30 kV. The experimental performance is tested by laser-induced ionization of rare gases producing electrons up to about 70 eV. The thick-lens VMI is useful for a wide variety of studies on atoms, molecules and nanoparticles in intense laser fields and high-photon-energy fields from high-harmonic-generation or free-electron lasers.

Non-sequential double ionization of Ar: from the single-to the many-cycle regime

The transition from the near-single to the multi-cycle regime in non-sequential double ionization of argon is investigated experimentally. Argon atoms are exposed to intense laser pulses with a center wavelength around 790 nm and the momenta of electrons and ions generated in the double ionization process are measured in coincidence using a reaction microscope. The duration of the near transform-limited pulses is varied from 4 to 30 fs. We observe an abrupt collapse of the cross-shaped two-electron momentum distribution [17] in the few-cycle regime. The transition to longer pulses is further accompanied by a strong increase in the fraction of anti-correlated to correlated electrons.

The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields

Much of our intuition about strong-field processes is built upon studies of diatomic molecules, which typically have electronic states that are relatively well separated in energy. In polyatomic molecules, however, the electronic states are closer together, leading to more complex interactions. A combined experimental and theoretical investigation of strong-field ionization followed by hydrogen elimination in the hydrocarbon series C2D2, C2D4 and C2D6 reveals that the photofragment angular distributions can only be understood when the field-dressed orbitals rather than the field-free orbitals are considered. Our measured angular distributions and intensity dependence show that these field-dressed orbitals can have strong Rydberg character for certain orientations of the molecule relative to the laser polarization and that they may contribute significantly to the hydrogen elimination dissociative ionization yield. These findings suggest that Rydberg contributions to field-dressed orbitals should be routinely considered when studying polyatomic molecules in intense laser fields.

The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense few-cycle laser pulses

We demonstrate the importance of ionization from Rydberg orbitals via experimental and theoretical work focusing on the strong-field dissociative single ionization of small hydrocarbons. Our findings suggest that Rydberg states should be routinely considered when studying polyatomic molecules in intense laser fields.

Attosecond Transient Absorption Spectroscopy for Real-Time Observation of Valence Electron Motion

Combining attosecond technology and X-ray absorption spectroscopy further expands the horizon of attosecond science. In a proof-of-principle experiment we traced valence electron motion in real time and completely reconstructed the strong-field initiated spin-orbit wavepacket coherence.