Spatially controlled nano-structuring of silicon with femtosecond vortex pulses.

Engineering material properties is key for development of smart materials and next generation nanodevices. This requires nanoscale spatial precision and control to fabricate structures/defects. Lithographic techniques are widely used for nanostructuring in which a geometric pattern on a mask is transferred to a resist by photons or charged particles and subsequently engraved on the substrate. However, direct mask-less fabrication has only been possible with electron and ion beams. That is because light has an inherent disadvantage; the diffraction limit makes it difficult to interact with matter on dimensions smaller than the wavelength of light. Here we demonstrate spatially controlled formation of nanocones on a silicon surface with a positional precision of 50 nm using femtosecond laser ablation comprising a superposition of optical vector vortex and Gaussian beams. Such control and precision opens new opportunities for nano-printing of materials using techniques such as laser-induced forward transfer and in general broadens the scope of laser processing of materials.

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.

Selective cell adhesion on femtosecond laser-microstructured polydimethylsiloxane.

We show that femtosecond laser irradiation of polydimethylsiloxane (PDMS) enables selective and patterned cell growth by altering the wetting properties of the surface associated with chemical and/or topographical changes. In the low pulse energy regime, the surface becomes less hydrophobic and exhibits a low water contact angle compared to the pristine material. X-ray photoelectron spectroscopy (XPS) also reveals an increased oxygen content in the irradiated regions, to which the C2C12 cells and rabbit anti-mouse protein were found to attach preferentially. In the high pulse energy regime, the laser-modified regions exhibit superhydrophobicity and were found to inhibit cell adhesion, whereas cells were found to attach to the surrounding regions due to the presence of nanoscale debris generated by the ablation process.

High harmonic spectroscopy of the Cooper minimum in molecules.

The Cooper minimum (CM) has been studied using high harmonic generation solely in atoms. Here, we present detailed experimental and theoretical studies on the CM in molecules probed by high harmonic generation using a range of near-infrared light pulses from λ=1.3 to 1.8 µm. We demonstrate the CM to occur in CS(2) and CCl(4) at ~42 and ~40 eV, respectively, by comparing the high harmonic spectra with the known partial photoionization cross sections of different molecular orbitals, confirmed by theoretical calculations of harmonic spectra. We use CM to probe electron localization in Cl-containing molecules (CCl(4), CH(2)Cl(2), and trans-C(2)H(2)Cl(2)) and show that the position of the minimum is influenced by the molecular environment.

Multi-µJ coherent extreme ultraviolet source generated from carbon using the plasma harmonic method.

We demonstrate intense high-order harmonic generation from plasma that is created from different carbon targets. We obtain high-order harmonic energy in the multi-microjoule range for each harmonic order from the 11th to the 17th harmonic. By analyzing the target morphology and the plasma composition, we conclude that the intense harmonics from the bulk carbon targets originate from nanoparticles target.

High-harmonic generation in H2O.

We demonstrate high-harmonic generation in H(2)O using 800 and 1300 nm laser pulses up to a maximum intensity of 5x10(14) W/cm(2). Under optimal phase-matching conditions, photon energies up to approximately 60 and approximately 87 eV are produced by using 800 and 1300 nm light, respectively. The harmonic spectra in H(2)O, when compared with Xe with a similar ionization potential, exhibit significant extension of the cutoff region, indicating suppression of ionization arising from molecular orbital symmetry.

Higher-order harmonic generation from fullerene by means of the plasma harmonic method.

We demonstrate, for the first time, high-order harmonic generation from C60 by an intense femtosecond Ti:sapphire laser. Laser-produced plasmas from C60-rich epoxy and C60 films were used as the nonlinear media. Harmonics up to the 19th order were observed. The harmonic yield from fullerene-rich plasma is about 25 times larger compared with those produced from a bulk carbon target. Structural studies of plasma debris confirm the presence and integrity of fullerenes within the plasma plume, indicating fullerenes as the source of high-order harmonics.

Optically produced arrays of planar nanostructures inside fused silica.

Linearly polarized femtosecond light pulses, focused inside fused silica to an intensity that leads to multiphoton ionization, produce arrayed planes of modified material having their normal parallel to the laser polarization. The planes are < or = 10 nm thick and are spaced at approximately lambda/2 in the medium for free space wavelengths of both 800 and 400 nm. By slowly scanning the sample under a fixed laser focus, order is maintained over macroscopic distances for all angles between the polarization and scan direction. With the laser polarization parallel to the scan direction we produce long-range Bragg-like gratings. We discuss how local field enhancement influences dielectric ionization, describe how this leads to nanoplane growth, why the planes are arrayed, and how long-range order is maintained.

Memory in nonlinear ionization of transparent solids.

We demonstrate a shot-to-shot reduction in the threshold laser intensity for ionization of bulk glasses illuminated by intense femtosecond pulses. For SiO2 the threshold change serves as positive feedback reenforcing the process that produced it. This constitutes a memory in nonlinear ionization of the material. The threshold change saturates with the number of pulses incident at a given spot. Irrespective of the pulse energy, the magnitude of the saturated threshold change is constant (approximately 20%). However, the number of shots required to reach saturation does depend on the pulse energy. Recognition of a memory in ionization is vital to understand multishot optical or electrical breakdown phenomena in dielectrics.

Polarization-selective etching in femtosecond laser-assisted microfluidic channel fabrication in fused silica.

We fabricate microchannels in fused silica by femtosecond laser irradiation followed by etching in diluted hydrofluoric acid. We show a dramatic dependence of the etch rate on the laser polarization, spanning 2 orders of magnitude. We establish the existence of an energy-per-pulse threshold at which etching of the laser-modified zones becomes highly polarization selective. The enhanced selective etching is due to long-range, periodic, polarization-dependent nanostructures formed in the laser-modified material.

Recollision during the High Laser Intensity Ionization of C60.

Through C60, we address the role of electron recollision in the nonresonant, femtosecond laser ionization of large, highly polarizable molecules. We show how the electron trajectories are influenced by the laser field, the laser induced dipole field, and the Coulomb field of the ion core. Working at long wavelengths we observe recollision in C60 through the ellipticity dependence of the fragmentation it produces. The ionizing electron emerges from C60z+ (z = 3, 4) with a lateral velocity of approximately 12 angstroms/fs, approximately half its Fermi velocity. Despite the large lateral velocity and competing forces on the electron, recollision remains relatively probable for this scale of molecule.

Stress in femtosecond-laser-written waveguides in fused silica.

We identify two states of stress induced in waveguides fabricated by femtosecond lasers in fused silica and show how they can be relieved by annealing. In-plane stress and stress concentration are revealed through birefringence and loss measurements. Another kind of laser-induced stress appears in the form of swelling of the glass surface when waveguides are written near the surface and is a manifestation of confined rapid material quenching. By annealing the sample we reduce the losses by approximately 30% (at 633 nm) and decrease the birefringence by a factor of 4 in fused silica.

Fully differential rates for femtosecond multiphoton double ionization of neon.

We have investigated the full three-dimensional momentum correlation between the electrons emitted from strong field double ionization of neon when the recollision energy of the first electron is on the order of the ionization potential. The momentum correlation in the direction perpendicular to the laser field depends on the time difference of the two electrons leaving the ion. Our results are consistent with double ionization proceeding through transient double excited states that field ionize.

Internal laser-induced dipole force at work in C60 molecule.

We show how the many electron response of a complex molecule to an intense laser field can be incorporated with the single active electron picture. This enables us to introduce an "over-the-barrier" model for Cz+60 ionization, valid for long wavelength light. Using infrared radiation, we confirm the model and also produce stable, highly charged C60 reaching C12+60, the highest charge state ever observed. At high intensities and high charge states the internal laser-induced dipole force and rapid charging lead to stress on the molecule. The interplay between the forces provides control and suggest strategies for reaching even higher charge states.

Electron-electron momentum exchange in strong field double ionization.

We have investigated the momentum balance between the two electrons from strong field double ionization of argon at 780 nm and 1.9 x 10(14) W/cm(2). Experimental data show that perpendicular to the laser polarization direction the electrons emerge preferentially in opposite directions. Results of model calculations are found to agree well with the data and reveal a dominant role of the Coulomb correlation between the two outgoing electrons in this kinematical geometry. Differences between the experimental observations and the theoretical results for the ion momentum distribution indicate the importance of the further effects during the three-body breakup.

Femtosecond laser fabrication of nanostructures in silica glass.

A femtosecond laser beam focused inside fused silica and other glasses can modify the refractive index of the glass. Chemical etching and atomic-force microscope studies show that the modified region can have a sharp-tipped cone-shaped structure with a tip diameter as small as 100 nm. Placing the structure near the bottom surface of a silica glass sample and applying a selective chemical etch to the bottom surface produces clean, circular, submicrometer-diameter holes. Holes spaced as close to one another as 1.4 microm are demonstrated.

Quantum interference in double ionization and fragmentation of C(6)H(6) in intense laser fields.

During tunnel ionization of atoms or molecules by strong laser fields, the electron acquires a transverse velocity which is characteristic of the ionization process. Ellipticity measurements identify nonsequential double ionization as due to recollision in C(6)H(6) and simultaneously measure the transverse velocity distribution of the electron wave packet. We observe signatures of quantum interference of different tunneling trajectories and find identical dependence of nonsequential double ionization and fragmentation of C(6)H(6) on the ellipticity of the laser polarization. This identifies electron recollision as the dominant source of fragmentation at 1.4 microm.

Few cycle dynamics of multiphoton double ionization.

In intense field ionization, an electron removed from the atomic core oscillates in the combined fields of the laser and the parent ion. This oscillation forces repeated revivals of its spatial correlation with the bound electrons. The total probability of double ionization depends on the number of returns and therefore on the number of optical periods in the laser pulse. We observed the yield of Ne(2+) relative to Ne(+) with 12 fs pulses to be clearly less compared to 50 fs pulses in qualitative agreement with our theoretical model.