Tim Rathje

Attosecond tracing of correlated electron-emission in non-sequential double ionization

Despite their broad implications for phenomena such as molecular bonding or chemical reactions, our knowledge of multi-electron dynamics is limited and their theoretical modelling remains a most difficult task. From the experimental side, it is highly desirable to study the dynamical evolution and interaction of the electrons over the relevant timescales, which extend into the attosecond regime. Here we use near-single-cycle laser pulses with well-defined electric field evolution to confine the double ionization of argon atoms to a single laser cycle. The measured two-electron momentum spectra, which substantially differ from spectra recorded in all previous experiments using longer pulses, allow us to trace the correlated emission of the two electrons on sub-femtosecond timescales. The experimental results, which are discussed in terms of a semiclassical model, provide strong constraints for the development of theories and lead us to revise common assumptions about the mechanism that governs double ionization.

Attosecond-recollision-controlled selective fragmentation of polyatomic molecules.

Control over various fragmentation reactions of a series of polyatomic molecules (acetylene, ethylene, 1,3-butadiene) by the optical waveform of intense few-cycle laser pulses is demonstrated experimentally. We show both experimentally and theoretically that the responsible mechanism is inelastic ionization from inner-valence molecular orbitals by recolliding electron wave packets, whose recollision energy in few-cycle ionizing laser pulses strongly depends on the optical waveform. Our work demonstrates an efficient and selective way of predetermining fragmentation and isomerization reactions in polyatomic molecules on subfemtosecond time scales.

Precise, real-time, every-single-shot, carrier-envelope phase measurement of ultrashort laser pulses

In this Letter we demonstrate a method for real-time determination of the carrier-envelope phase of each and every single ultrashort laser pulse at kilohertz repetition rates. The technique expands upon the recent work of Wittmann and incorporates a stereographic above-threshold laser-induced ionization measurement and electronics optimized to produce a signal corresponding to the carrier-envelope phase within microseconds of the laser interaction, thereby facilitating data-tagging and feedback applications. We achieve a precision of 113 mrad (6.5°) over the entire 2π range.

Review of attosecond resolved measurement and control via carrier–envelope phase tagging with above-threshold ionization

A precise, real-time, single-shot carrier–envelope phase (CEP) tagging technique for few-cycle pulses was developed and combined with cold-target recoil-ion momentum spectroscopy and velocity-map imaging to investigate and control CEP-dependent processes with attosecond resolution. The stability and precision of these new techniques have allowed for the study of intense, few-cycle, laser-matter dynamics with unprecedented detail. Moreover, the same stereo above-threshold ionization (ATI) measurement was expanded to multi-cycle pulses and allows for CEP locking and pulse-length determination. Here we review these techniques and their first applications to waveform characterization and control, non-sequential double ionization of argon, ATI of xenon and electron emission from SiO2 nanospheres.

Real-time pulse length measurement of few-cycle laser pulses using above-threshold ionization

The pulse lengths of intense few-cycle (4-10 fs) laser pulses at 790 nm are determined in real-time using a stereographic above-threshold ionization (ATI) measurement of Xe, i.e. the same apparatus recently shown to provide a precise, real-time, every-single-shot, carrier-envelope phase measurement of ultrashort laser pulses. The pulse length is calibrated using spectral-phase interferometry for direct electric-field reconstruction (SPIDER) and roughly agrees with calculations done using quantitative rescattering theory (QRS). This stereo-ATI technique provides the information necessary to characterize the waveform of every pulse in a kHz pulse train, within the Gaussian pulse approximation, and relies upon no theoretical assumptions. Moreover, the real-time display is a highly effective tool for tuning and monitoring ultrashort pulse characteristics.

Precise, real-time, single-shot carrier-envelope phase measurement in the multi-cycle regime

Polarization gating is used to extend a real-time, single-shot, carrier-envelope phase (CEP) measurement, based on high-energy above-threshold ionization in xenon, to the multi-cycle regime. The single-shot CEP precisions achieved are better than 175 and 350 mrad for pulse durations up to 10 fs and 12.5 fs, respectively, while only 130 μJ of pulse energy are required. This opens the door to study and control of CEP-dependent phenomena in ultra-intense laser-matter interaction using optical parametric chirped pulse amplifier based tera- and petawatt class lasers.

Improved carrier-envelope phase locking of intense few-cycle laser pulses using above-threshold ionization

A robust nonoptical carrier-envelope phase (CEP) locking feedback loop, which utilizes a measurement of the left-right asymmetry in the above-threshold ionization (ATI) of Xe, is implemented, resulting in a significant improvement over the standard slow-loop f-to-2f technique. This technique utilizes the floating average of a real-time, every-single-shot CEP measurement to stabilize the CEP of few-cycle laser pulses generated by a standard Ti:sapphire chirped-pulse amplified laser system using a hollow-core fiber and chirped mirror compression scheme. With this typical commercially available laser system and the stereographic ATI method, we are able to improve short-term (minutes) CEP stability after a hollow-core fiber from 450 to 290 mrad rms and long-term (hours) stability from 480 to 370 mrad rms.

Momentum-resolved study of the saturation intensity in multiple ionization

(Received 25 September 2014; published 16 March 2015)We present a momentum-resolved study of strong field multiple ionization of ionic targets. Using adeconvolution method we are able to reconstruct the electron momenta from the ion momentum distributionsafter multiple ionization up to four sequential ionization steps. This technique allows an accurate determinationof the saturation intensity as well as of the electron release times during the laser pulse. The measured results arediscussed in comparison to typically used models of over-the-barrier ionization and tunnel ionization.DOI: 10.1103/PhysRevA.91.031401 PACS number(s): 32

CEP-stable tunable THz-emission originating from laser-waveform-controlled sub-cycle plasma-electron bursts

We study THz-emission from a plasma driven by an incommensurate-frequency two-colour laser field. A semi-classical transient electron current model is derived from a fully quantum-mechanical description of the emission process in terms of sub-cycle field-ionization followed by continuum-continuum electron transitions. For the experiment, a CEP-locked laser and a near-degenerate optical parametric amplifier are used to produce two-colour pulses that consist of the fundamental and its near-half frequency. By choosing two incommensurate frequencies, the frequency of the CEP-stable THz-emission can be continuously tuned into the mid-IR range. This measured frequency dependence of the THz-emission is found to be consistent with the semi-classical transient electron current model, similar to the Brunel mechanism of harmonic generation.

Accurate determination of absolute carrier-envelope phase dependence using photo-ionization.

The carrier-envelope phase (CEP) dependence of few-cycle above-threshold ionization (ATI) of Xe is calibrated for use as a reference measurement for determining and controlling the absolute CEP in other interactions. This is achieved by referencing the CEP-dependent ATI measurements of Xe to measurements of atomic H, which are in turn referenced to ab initio calculations for atomic H. This allows for the accurate determination of the absolute CEP dependence of Xe ATI, which enables relatively easy determination of the offset between the relative CEP measured and/or controlled by typical devices and the absolute CEP in the interaction.