Blister formation in dynamic release mirror structures using femtosecond laser pulses.

Blister formation occurs when a laser pulse interacts with the underside of a polymer film on a glass substrate and is fundamental in Laser-Induced Forward Transfer (LIFT). We present a novel method of controlling blister formation using a thin metal film situated between two thin polymer films. This enables a wide range of laser pulse energies by limiting the laser penetration in the film, which allows us to exploit nonlinear interactions without transmitting high intensities that may destroy a transfer material. We study blisters using a helium ion microscope, which images their interiors, and find that laser energy deposition is primarily in the metal layer and the top polymer layer remains intact. Blister expansion is driven by laser-induced spallation of the gold film. Our work shows that this technique could be a viable platform for contaminant-free LIFT using nonlinear absorption beyond the diffraction limit.

Few-cycle Yb laser source at 20 kHz using multidimensional solitary states in hollow-core fibers.

We demonstrate ultrashort pulse compression from 300 fs down to 17 fs at a repetition rate of 20 kHz and 160-µJ output pulse energy (3.2 W of average power) using multidimensional solitary states (MDSS) in a 1-meter hollow-core fiber (HCF) filled with N2O. Under static pressure, thermal limitations at this repetition rate annihilate the MDSS with suppression of spectral broadening. The results obtained in differential pressure configuration mitigate thermal effects and significantly increase the range of repetition rate over which MDSS can be used to compress sub-picosecond laser pulses.

Single-shot dispersion sampling for optical pulse reconstruction.

We present a novel approach to single-shot characterization of the spectral phase of broadband laser pulses. Our method is inexpensive, insensitive to alignment and combines the simplicity and robustness of the dispersion scan technique, that does not require spatio-temporal pulse overlap, with the advantages of single-shot pulse characterization methods such as single-shot frequency-resolved optical gating at a real-time reconstruction rate of several Hz.

Generation of structured coherent extreme ultraviolet beams from an MgO crystal.

Short wavelength high-harmonic sources are undergoing intense development for applications in spectroscopy and microscopy. Despite recent progress in peak and average power, spatial control over coherent extreme ultraviolet (XUV) beams remains a formidable challenge due to the lack of suitable optical elements for beam shaping and control. Here we demonstrate a robust and precise approach that structures XUV high-order harmonics in space as they are emitted from a nanostructured MgO crystal. Our demonstration paves the way for bridging the numerous applications of shaped light beams from the visible to the short wavelengths, with potential uses for applications in microscopy and nanoscale machining.

Linking high harmonics from gases and solids.

When intense light interacts with an atomic gas, recollision between an ionizing electron and its parent ion creates high-order harmonics of the fundamental laser frequency. This sub-cycle effect generates coherent soft X-rays and attosecond pulses, and provides a means to image molecular orbitals. Recently, high harmonics have been generated from bulk crystals, but what mechanism dominates the emission remains uncertain. To resolve this issue, we adapt measurement methods from gas-phase research to solid zinc oxide driven by mid-infrared laser fields of 0.25 volts per ångström. We find that when we alter the generation process with a second-harmonic beam, the modified harmonic spectrum bears the signature of a generalized recollision between an electron and its associated hole. In addition, we find that solid-state high harmonics are perturbed by fields so weak that they are present in conventional electronic circuits, thus opening a route to integrate electronics with attosecond and high-harmonic technology. Future experiments will permit the band structure of a solid to be tomographically reconstructed.

Multiphoton laser-induced confined chemical changes in polymer films.

We report ultrafast-laser-induced photochemical, structural, and morphological changes in a polyimide film irradiated at the polymer-glass interface in back-incident geometry. Back-illumination creates locally hot material at the interface leading to a confined photochemical change at the interface and a morphological change through a blister formation. The laser-induced photochemical changes in polyimide resulted in new absorption and luminescence properties in the visible region. The laser-treated polyimide exhibited photoluminescence anisotropy resulting from formation of ordered polymer upon irradiation by linearly polarized ultrashort laser pulses. Confocal fluorescence microscopy resulted in similar observations to the bulk. Reflection-absorption infrared spectroscopy and X-ray photoelectron spectroscopy together indicated confinement of laser-induced chemical changes at the interface.

Clocking Enhanced Ionization of Hydrogen Molecules with Rotational Wave Packets.

Laser-induced rotational wave packets of H_{2} and D_{2} molecules were experimentally measured in real time by using two sequential 25-fs laser pulses and a reaction microscope. By measuring the time-dependent yields of the above-threshold dissociation and the enhanced ionization of the molecule, we observed a few-femtosecond time delay between the two dissociation channels for both H_{2} and D_{2}. The delay was interpreted and reproduced by a classical model that considers enhanced ionization and thus additional interaction within the laser pulse. We demonstrate that by accurately measuring the phase of the rotational wave packet in hydrogen molecules we can resolve dissociation dynamics which is occurring within a fraction of a molecular rotation. Such a rotational clock is a general concept applicable to sequential fragmentation processes in other molecules.

High-harmonic generation in solids driven by counter-propagating pulses.

We used two 800 nm laser pulses propagating in the opposite directions, to drive the emission of high-order vacuum ultra-violet harmonics off of the surface of an MgO (100) single crystal. We demonstrated the advantages that our approach provides compared to a single beam geometry, in both forward and backward emission.

Threshold photodissociation dynamics of NO2 studied by time-resolved cold target recoil ion momentum spectroscopy.

We study the near-threshold photodissociation dynamics of NO2 by a kinematically complete femtosecond pump-probe scheme using a cold target recoil ion momentum spectrometer. We excite NO2 to the optically bright Ã2B2 state with a 400 nm pulse and probe the ensuing dynamics via strong field single and double ionization with a 25 fs, 800 nm pulse. The pump spectrum spans the NO(X2Π) + O(3P) dissociation channel threshold, and therefore, following internal conversion, excited NO2 is energetically prepared both "above threshold" (dissociating) and "below threshold" (nondissociating). Experimentally, we can clearly discriminate a weak two-photon pump channel from the dominant single-photon data. In the single ionization channel, we observe NO+ fragments with nonzero momentum at 200 fs delay and an increasing yield of NO+ fragments with near-zero momentum at 3.0 ps delay. For double ionization events, we observe a time-varying Coulombic kinetic energy release between the NO+ and O+ fragments impulsively created from the evolving "hot" neutral ground state. Supported by classical trajectory calculations, we assign the decreasing Coulombic kinetic energy release at longer time delays to the increasing average NO-O distances in the ground electronic state during its large amplitude phase space evolution toward free products. The time-resolved kinetic energy release in the double ionization channel probes the large amplitude ground state evolution from a strongly coupled "inner region" to a loosely coupled "outer region" where one O atom is on average much further away from the NO. Both the time evolution of the kinetic energy release and the NO+ angular distributions support our assignments.

Mapping complex polarization states of light on a solid.

Polarization states of light, represented by different points on a Poincaré sphere, can be readily analyzed for a Gaussian beam by a combination of wave plates and polarizers. However, this method cannot be extended to higher-order Poincaré spheres and complex polarization patterns produced by coherent superpositions of vector vortex (VV) beams. We demonstrate the visualization of complex polarization patterns by imprinting them onto a solid surface in the form of periodic nano-gratings oriented parallel to the local structure of the electric field of light. We design unconventional surface structures by controlling the superposition of VV beams. Our method is of potential interest to the production of sub-wavelength nano-structures.

Testing the Role of Recollision in N_{2}

It has been known for many years that during filamentation of femtosecond light pulses in air, gain is observed on the B to X transition in N_{2}^{+}. While the gain mechanism remains unclear, it has been proposed that recollision, a process that is fundamental to much of strong field science, is critical for establishing gain. We probe this hypothesis by directly comparing the influence of the ellipticity of the pump light on gain in air filaments. Then, we decouple filamentation from gain by measuring the gain in a thin gas jet that we also use for high harmonic generation. The latter allows us to compare the dependence of the gain on the ellipticity of the pump with the dependence of the high harmonic signal on the ellipticity of the fundamental. We find that gain and harmonic generation have very different behavior in both filaments and in the jet. In fact, in a jet we even measure gain with circular polarization. Thus, we establish that recollision does not play a significant role in creating the inversion.

2.5 TW, two-cycle IR laser pulses via frequency domain optical parametric amplification.

Broadband optical parametric amplification in the IR region has reached a new milestone through the use of a non-collinear Frequency domain Optical Parametric Amplification system. We report a laser source delivering 11.6 fs pulses with 30 mJ of energy at a central wavelength of 1.8 µm at 10 Hz repetition rate corresponding to a peak power of 2.5 TW. The peak power scaling is accompanied by a pulse shortening of about 20% upon amplification due to the spectral reshaping with higher gain in the spectral wings. This source paves the way for high flux soft X-ray pulses and IR-driven laser wakefield acceleration.

Harmonic generation in solids with direct fiber laser pumping.

High harmonic generation in solids presents the possibility for bringing attosecond techniques to semiconductors and a simple source for frequency comb spectroscopy in the vacuum ultraviolet. We generate up to the seventh harmonic of a Tm fiber laser by focusing in silicon or zinc oxide. The harmonics are strong and stable, with no indication of material damage. Calculations show the potential for generating nineteenth harmonic photons at 12 eV photons of energy.

Intense-Laser Solid State Physics: Unraveling the Difference between Semiconductors and Dielectrics.

Experiments on intense laser driven dielectrics have revealed population transfer to the conduction band to be oscillatory in time. This is in stark contrast to ionization in semiconductors and is currently unexplained. Current ionization theories neglect coupling between the valence and conduction band and therewith, the dynamic Stark shift. Our single-particle analysis identifies this as a potential reason for the different ionization behavior. The dynamic Stark shift increases the band gap with increasing laser intensities, thus suppressing ionization to an extent where virtual population oscillations become dominant. The dynamic Stark shift plays a role dominantly in dielectrics which, due to the larger band gap, can be exposed to significantly higher laser intensities.

Perturbative High Harmonic Wave Front Control.

We pattern the wave front of a high harmonic beam by intersecting the intense driving laser pulse that generates the high harmonic with a weak control pulse. To illustrate the potential of wave-front control, we imprint a Fresnel zone plate pattern on a harmonic beam, causing the harmonics to focus and defocus. The quality of the focus that we achieve is measured using the spectral wave-front optical reconstruction by diffraction method. We will show that it is possible to enhance the peak intensity by orders of magnitude without a physical optical element in the path of the extreme ultraviolet (XUV) beam. Through perturbative wave-front control, XUV beams can be created with a flexibility approaching what technology allows for visible and infrared light.

Molecular Frame Reconstruction Using Time-Domain Photoionization Interferometry.

Photoionization of molecular species is, essentially, a multipath interferometer with both experimentally controllable and intrinsic molecular characteristics. In this work, XUV photoionization of impulsively aligned molecular targets (N_{2}) is used to provide a time-domain route to "complete" photoionization experiments, in which the rotational wave packet controls the geometric part of the photoionization interferometer. The data obtained is sufficient to determine the magnitudes and phases of the ionization matrix elements for all observed channels, and to reconstruct molecular frame interferograms from lab frame measurements. In principle, this methodology provides a time-domain route to complete photoionization experiments and the molecular frame, which is generally applicable to any molecule (no prerequisites), for all energies and ionization channels.

Ultrafast Dissociation of Metastable CO

We triply ionize the van der Waals bound carbon monoxide dimer with intense ultrashort pulses and study the breakup channel (CO)_{2}^{3+}→C^{+}+O^{+}+CO^{+}. The fragments are recorded in a cold target recoil ion momentum spectrometer. We observe a fast CO^{2+} dissociation channel in the dimer, which does not exist for the monomer. We found that a nearby charge breaks the symmetry of a X^{3}Π state of CO^{2+} and induces an avoided crossing that allows a fast dissociation. Calculation on the full dimer complex shows the coupling of different charge states, as predicted from excimer theory, gives rise to electronic state components not present in the monomer, thereby enabling fast dissociation with higher kinetic energy release. These results demonstrate that the electronic structure of molecular cluster complexes can give rise to dynamics that is qualitatively different from that observed in the component monomers.

Streak Camera for Strong-Field Ionization.

Ionization of an atom or molecule by a strong laser field produces suboptical cycle wave packets whose control has given rise to attosecond science. The final states of the wave packets depend on ionization and deflection by the laser field, which are convoluted in conventional experiments. Here, we demonstrate a technique enabling efficient electron deflection, separate from the field driving strong-field ionization. Using a midinfrared deflection field permits one to distinguish electron wave packets generated at different field maxima of an intense few-cycle visible laser pulse. We utilize this capability to trace the scattering of low-energy electrons driven by the midinfrared field. Our approach represents a general technique for studying and controlling strong-field ionization dynamics on the attosecond time scale.

Following a chemical reaction using high-harmonic interferometry.

The study of chemical reactions on the molecular (femtosecond) timescale typically uses pump laser pulses to excite molecules and subsequent probe pulses to interrogate them. The ultrashort pump pulse can excite only a small fraction of molecules, and the probe wavelength must be carefully chosen to discriminate between excited and unexcited molecules. The past decade has seen the emergence of new methods that are also aimed at imaging chemical reactions as they occur, based on X-ray diffraction, electron diffraction or laser-induced recollision--with spectral selection not available for any of these new methods. Here we show that in the case of high-harmonic spectroscopy based on recollision, this apparent limitation becomes a major advantage owing to the coherent nature of the attosecond high-harmonic pulse generation. The coherence allows the unexcited molecules to act as local oscillators against which the dynamics are observed, so a transient grating technique can be used to reconstruct the amplitude and phase of emission from the excited molecules. We then extract structural information from the amplitude, which encodes the internuclear separation, by quantum interference at short times and by scattering of the recollision electron at longer times. The phase records the attosecond dynamics of the electrons, giving access to the evolving ionization potentials and the electronic structure of the transient molecule. In our experiment, we are able to document a temporal shift of the high-harmonic field of less than an attosecond (1 as = 10(-18) s) between the stretched and compressed geometry of weakly vibrationally excited Br(2) in the electronic ground state. The ability to probe structural and electronic features, combined with high time resolution, make high-harmonic spectroscopy ideally suited to measuring coupled electronic and nuclear dynamics occurring in photochemical reactions and to characterizing the electronic structure of transition states.