K. Zrost

Determination of the carrier-envelope phase of few-cycle laser pulses with terahertz-emission spectroscopy

The availability of few-cycle optical pulses opens a window to physical phenomena occurring on the attosecond timescale. To take full advantage of such pulses, it is crucial to measure1,2,3,4 and stabilize1,2 their carrier-envelope (CE) phase, that is, the phase difference between the carrier wave and the envelope function. We introduce an approach to determine the CE phase by down-conversion of the laser light to the terahertz (THz) frequency range by means of plasma generation in ambient air, an isotropic medium where optical rectification (down-conversion) in the forward direction is only possible if the inversion symmetry is broken by electrical or optical means5,6,7,8,9,10. We show that few-cycle pulses directly produce a spatial charge asymmetry in the plasma. The asymmetry, associated with THz emission, depends on the CE phase, which allows determination of the phase by measurement of the amplitude and polarity of the THz pulse.

Correlated Multielectron Dynamics in Ultrafast Laser Pulse Interactions with Atoms

We present the results of the detailed experimental study of multiple ionization of Ne and Ar by 25 and 7 fs laser pulses. Whereas in multiple ionization of Ar different mechanisms, involving field ionization steps and recollision-induced excitations, play a role, for Ne only one channel, where the highly correlated instantaneous emission of up to four electrons is triggered by a recollisional electron impact, is found to be important. Using few-cycle pulses we are able to suppress those processes that occur on time scales longer than one laser cycle.

Resonant structures in the low-energy electron continuum for single ionization of atoms in the tunnelling regime

We present high-resolution fully differential experimental data on single ionization of He, Ne and Ar by ultra-short (25 fs, 6 fs) 795 nm laser pulses at intensities 0.15–2.0 × 1015 W cm−2. We show that the ATI-like pattern can survive deep in the tunnelling regime and that the atomic structure plays an important role in the formation of the low-energy photoelectron spectra even at high intensities. The absence of ponderomotive shifts, the splitting of the peaks and their degeneration for few-cycle pulses indicate that the observed structures originate from a resonant process.

Atomic structure dependence of nonsequential double ionization of He, Ne and Ar in strong laser pulses

The ion momentum spectra for nonsequential double ionization of rare gases (He, Ne and Ar) in 23 fs 795 nm laser pulses were measured in the intensity range 0.075–1.25 PW cm−2. In the studies published, confusing differences in the shape of momentum distributions among different targets are consistently explained within a recollision scenario: excitation during recollision plus subsequent field ionization, not implemented in most theoretical approaches, evidently plays a decisive role for He and Ar nonsequential double ionization whereas it plays only a minor role for Ne.

Fragmentation dynamics of molecular hydrogen in strong ultrashort laser pulses

We present the results of a systematic experimental study of dissociation and Coulomb explosion of molecular hydrogen induced by intense ultrashort (7–25 fs) laser pulses. Using coincident recoil-ion momentum spectroscopy we can distinguish the contributions from dissociation and double ionization even if they result in the same kinetic energies of the fragments. The dynamics of all fragmentation channels drastically depends on the pulse duration, and for 7 fs pulses becomes extremely sensitive to the pulse shape.

EUV-photon-induced multiple ionization and fragmentation dynamics: from atoms to molecules

Multiple ionization (MI), induced by a few EUV photons at energies of 28.2 eV, 38 eV and 44 eV from FLASH (the free-electron laser at Hamburg), has been studied for atoms (He, Ne, Ar) and N2 molecules utilizing our multi-hit coincident technology?the reaction microscope. At comparably low intensities of I 1011?1013 W cm?2 we find the non-sequential (NS) MI mechanism dominating Ar3+ and Ar4+ production. Inspecting recoil ion and electron momentum distributions evidence is provided (i) for preferential back-to-back emission of electrons for NS double ionization of He and (ii) for angular entanglement between two outgoing electrons in sequential ionization (SI). In contrast to atoms, SI is observed to be most effective for MI of N2 molecules at an intensity of ~1013 W cm?2 leading, among others, to N2+2 ? N+ + N+, N3+2 ? N2+ + N+, N4+2 ? N2+ + N2+ Coulomb explosion channels. Fragment ion momentum distributions are investigated and are demonstrated to allow tracing SI pathways.

Ultrafast mapping of H2+ (D2+) nuclear wave packets using time-resolved Coulomb explosion imaging

The time evolution of H2+ (D2+) nuclear wave packets is studied exploiting a combination of coincident Coulomb explosion imaging and femtosecond pump–probe techniques. Using two 25 fs laser pulses, we map the motion of the dissociating molecular ion, observe an enhanced ionization rate at an internuclear separation of ~11 au and resolve trajectories due to the one- and two-photon Floquet channels. With two 7 fs pulses, we are able to visualize the vibrational motion of the bound part of the wave packet, which exhibits counterintuitive quantum behaviour and dephases within about 100 fs, in agreement with recent numerical simulations.

Sequential and direct two-photon double ionization of D2 at FLASH

Sequential and direct two-photon double ionization (DI) of D2 molecule is studied experimentally and theoretically at a photon energy of 38.8 eV. Experimental and theoretical kinetic energy releases of D++D+fragments, consisting of the contributions of sequential DI via the D2+(1sσg) state and direct DI via a virtual state, agree well with each other.

Sequential versus nonsequential two-photon double ionization of the D2 molecule at 38 eV

A simple theoretical model is used to interpret recent experimental results for two-photon double ionization (DI) of D2 at 38 eV. We show that the measured kinetic energy distribution associated with emission of two protons can be interpreted as a sum of two processes: a sequential and an instantaneous absorption of the two incident photons. These processes lead to peaks in different regions of the spaectrum.

Measurement of the Carrier-Envelope Phase of Few-Cycle Laser Pulses by THz-Emission Spectroscopy

THz-emission from laser-generated plasmas opens a way to measure the carrier-envelope phase of few-cycle optical pulses, a parameter of critical significance for numerous experiments with sub-10-fs light pulses.