Laser-Driven Anharmonic Oscillator: Ground-State Dissociation of the Helium Hydride Molecular Ion by Midinfrared Pulses.

The vibrational motion of molecules represents a fundamental example of an anharmonic oscillator. Using a prototype molecular system, HeH^{+}, we demonstrate that appropriate laser pulses make it possible to drive the nuclear motion in the anharmonic potential of the electronic ground state, increasing its energy above the potential barrier and facilitating dissociation by purely vibrational excitation. We find excellent agreement between the frequency-dependent response of the helium hydride molecular cation to both classical and quantum mechanical simulations, thus removing any ambiguities through electronic excitation.

Observing the Importance of the Phase-Volume Effect for Few-Cycle Light-Matter Interactions.

The spatially dependent phase distribution of focused few-cycle pulses, i.e., the focal phase, is much more complex than the well-known Gouy phase of monochromatic beams.

Carrier-envelope-phase measurement of few-cycle mid-infrared laser pulses using high harmonic generation in ZnO.

High-harmonic generation (HHG) in crystals offers a simple, affordable and easily accessible route to carrier-envelope phase (CEP) measurements, which scales favorably towards longer wavelengths. We present measurements of HHG in ZnO using few-cycle pulses at 3.1µm.

Heteronuclear Limit of Strong-Field Ionization: Fragmentation of HeH^{+} by Intense Ultrashort Laser Pulses.

The laser-induced fragmentation dynamics of this most fundamental polar molecule HeH^{+} are measured using an ion beam of helium hydride and an isotopologue at various wavelengths and intensities. In contrast to the prevailing interpretation of strong-field fragmentation, in which stretching of the molecule results primarily from laser-induced electronic excitation, experiment and theory for nonionizing dissociation, single ionization, and double ionization both show that the direct vibrational excitation plays the decisive role here. We are able to reconstruct fragmentation pathways and determine the times at which each ionization step occurs as well as the bond length evolution before the electron removal.

Single-shot, real-time carrier-envelope phase measurement and tagging based on stereographic above-threshold ionization at short-wave infrared wavelengths.

A high-precision, single-shot, and real-time carrier-envelope phase (CEP) measurement at 1.8 μm laser wavelength based on stereographic photoelectron spectroscopy is presented. A precision of the CEP measurement of 120 mrad for each and every individual laser shot for a 1 kHz pulse train with randomly varying CEP is demonstrated.