Nora G. Johnson

Field-Free Orientation of CO Molecules by Femtosecond Two-Color Laser Fields

We report the first experimental observation of nonadiabatic field-free orientation of a heteronuclear diatomic molecule (CO) induced by an intense two-color (800 and 400 nm) femtosecond laser field. We monitor orientation by measuring fragment ion angular distributions after Coulomb explosion with an 800 nm pulse. The orientation of the molecules is controlled by the relative phase of the two-color field. The results are compared to quantum mechanical rigid rotor calculations. The demonstrated method can be applied to study molecular frame dynamics under field-free conditions in conjunction with a variety of spectroscopy methods, such as high-harmonic generation, electron diffraction, and molecular frame photoelectron emission.

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.

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.

Single-shot velocity-map imaging of attosecond light-field control at kilohertz rate

High-speed, single-shot velocity-map imaging (VMI) is combined with carrier-envelope phase (CEP) tagging by a single-shot stereographic above-threshold ionization (ATI) phase-meter. The experimental setup provides a versatile tool for angle-resolved studies of the attosecond control of electrons in atoms, molecules, and nanostructures. Single-shot VMI at kHz repetition rate is realized with a highly sensitive megapixel complementary metal-oxide semiconductor camera omitting the need for additional image intensifiers. The developed camera software allows for efficient background suppression and the storage of up to 1024 events for each image in real time. The approach is demonstrated by measuring the CEP-dependence of the electron emission from ATI of Xe in strong (≈10(13)u2009W/cm(2)) near single-cycle (4 fs) laser fields. Efficient background signal suppression with the system is illustrated for the electron emission from SiO(2) nanospheres.

Carrier–envelope phase-tagged imaging of the controlled electron acceleration from SiO2 nanospheres in intense few-cycle laser fields

Waveform-controlled light fields offer the possibility of manipu- lating ultrafast electronic processes on sub-cycle timescales. The optical light- wave control of the collective electron motion in nanostructured materials is key to the design of electronic devices operating at up to petahertz frequencies. We have studied the directional control of the electron emission from 95nm 10 Authors to whom any correspondence should be addressed.

Carrier-envelope-phase tagging in measurements with long acquisition times

We present a detailed analysis of the systematic errors that affect single-shot carrier envelope phase (CEP) measurements in experiments with long acquisition times, for which only limited long-term laser stability can be achieved. After introducing a scheme for eliminating these systematic errors to a large extent, we apply our approach to investigate the CEP dependence of the yield of doubly charged ions produced via non-sequential double ionization of argon in strong near-single-cycle laser pulses. The experimental results are compared to predictions of semiclassical calculations.

Confining the double ionization dynamics of argon to half of a laser cycle

The sub-cycle dynamics in non-sequential double ionization of argon are studied by combining a reaction microscope with a single-shot carrier-envelope phase measurement technique.

Sub-cycle double ionization dynamics of argon and neon

Since its discovery in 1982 by LHuillier and coworkers [1], non-sequential double ionization (NSDI) of atoms in strong laser fields has been the subject of numerous experimental and theoretical studies. Yet, the mechanisms that govern this process are not fully understood. Advances in ultra-fast laser technology have permitted the generation of light pulses with durations close to a single optical cycle [2], which can be used to study quantum dynamics with attosecond time resolution. Using a reaction microscope (REMI) in combination with the recently developed single-shot carrier-envelope phase (CEP) measurement technique [3], we investigate the sub-cycle dynamics of the NSDI process in argon and neon atoms exposed to near single-cycle laser pulses.