Carrier-envelope phase on-chip scanner and control of laser beams.

The carrier-envelope phase (CEP) is an important property of few-cycle laser pulses, allowing for light field control of electronic processes during laser-matter interactions. Thus, the measurement and control of CEP is essential for applications of few-cycle lasers. Currently, there is no robust method for measuring the non-trivial spatial CEP distribution of few-cycle laser pulses. Here, we demonstrate a compact on-chip, ambient-air, CEP scanning probe with 0.1 µm3 resolution based on optical driving of CEP-sensitive ultrafast currents in a metal-dielectric heterostructure. We successfully apply the probe to obtain a 3D map of spatial changes of CEP in the vicinity of an oscillator beam focus with pulses as weak as 1 nJ. We also demonstrate CEP control in the focal volume with a spatial light modulator so that arbitrary spatial CEP sculpting could be realized.

Carrier envelope phase sensitivity of photoelectron circular dichroism.

We report on a combined experimental and numerical study of photoelectron circular dichroism (PECD) induced by intense few-cycle laser pulses, using methyloxirane as the molecular example. Our experiments reveal a remarkably pronounced sensitivity of the PECD strength of double-ionization on the carrier-envelope phase (CEP) of the laser pulses. By comparison to the simulations, which reproduce the measured CEP-dependence for specific orientations of the molecules in the lab frame, we attribute the origin of the observed CEP-dependence of PECD to the CEP-induced modulation of ionization from different areas of the wave functions of three dominant orbitals.

Laser-Induced Electron Transfer in the Dissociative Multiple Ionization of Argon Dimers.

We report on an experimental and theoretical study of the ionization-fragmentation dynamics of argon dimers in intense few-cycle laser pulses with a tagged carrier-envelope phase. We find that a field-driven electron transfer process from one argon atom across the system boundary to the other argon atom triggers subcycle electron-electron interaction dynamics in the neighboring atom. This attosecond electron-transfer process between distant entities and its implications manifests itself as a distinct phase-shift between the measured asymmetry of electron emission curves of the Ar^{+}+Ar^{2+} and Ar^{2+}+Ar^{2+} fragmentation channels. This letter discloses a strong-field route to controlling the dynamics in molecular compounds through the excitation of electronic dynamics on a distant molecule by driving intermolecular electron-transfer processes.

Generalized Phase Sensitivity of Directional Bond Breaking in the Laser-Molecule Interaction.

We establish a generalized picture of the phase sensitivity of laser-induced directional bond breaking using the H_{2} molecule as the example. We show that the well-known proton ejection anisotropy measured with few-cycle pulses as a function of their carrier-envelope phases arises as an amplitude modulation of an intrinsic anisotropy that is sensitive to the laser phase at the ionization time and determined by the molecule's electronic structure. Our work furthermore reveals a strong electron-proton correlation that may open up a new approach to experimentally accessing the laser-sub-cycle intramolecular electron dynamics also in larger molecules.

Experimental Separation of Subcycle Ionization Bursts in Strong-Field Double Ionization of H_{2}.

We report on the unambiguous observation of the subcycle ionization bursts in sequential strong-field double ionization of H_{2} and their disentanglement in molecular frame photoelectron angular distributions. This observation was made possible by the use of few-cycle laser pulses with a known carrier-envelope phase, in combination with multiparticle coincidence momentum imaging. The approach demonstrated here will allow sampling of the intramolecular electron dynamics and the investigation of charge-state-specific Coulomb distortions on emitted electrons in polyatomic molecules.

Subfemtosecond Tracing of Molecular Dynamics during Strong-Field Interaction.

We introduce and experimentally demonstrate a method where the two intrinsic timescales of a molecule, the slow nuclear motion and the fast electronic motion, are simultaneously measured in a photoelectron photoion coincidence experiment. In our experiment, elliptically polarized, 750 nm, 4.5 fs laser pulses were focused to an intensity of 9×10^{14} W/cm^{2} onto H_{2}. Using coincidence imaging, we directly observe the nuclear wave packet evolving on the 1sσ_{g} state of H_{2}^{+} during its first round-trip with attosecond temporal and picometer spatial resolution. The demonstrated method should enable insight into the first few femtoseconds of the vibronic dynamics of ionization-induced unimolecular reactions of larger molecules.