Charge-induced dipole vs. relativistically enhanced covalent interactions in Ar-tagged Au-Ag tetramers and pentamers.

Vibrational spectra of Au(n)Ag(m)(+)⋅Ar(k) (n + m = 4, 5; k = 1-4) clusters are determined by far-infrared resonant multiple photon dissociation spectroscopy in the range ν̃=100-250 cm(-1). The experimental spectra are assigned using density functional theory for geometries obtained by the Birmingham cluster genetic algorithm. Putative global minimum candidates of the Ar complexes are generated by adding Ar atoms to the Au(n)Ag(m)(+) low energy isomers and subsequent local optimization. Differential Ar binding energies indicate exceptionally strong Au-Ar bonds in Au-rich clusters, leading to fundamental changes to the IR spectra. The stronger Ar binding is attributed to a relativistically enhanced covalent character of the Au-Ar bond, while in Au-rich species charge-induced dipole interactions overcompensate the relativistic affinity to Au. Moreover, not only the absolute composition but also the topologies are essential in the description of Ar binding to a certain cluster.

Field dependent avalanche ionization rates in dielectrics.

From the pulse length dependence of the absorption of intense ultrashort laser pulses focused inside fused silica, we reveal the role field-assisted collisional ionization plays in the multiphoton ionization process. This constitutes a cold avalanche ionization mechanism that persists at pulse lengths considered too short for a traditional avalanche.

Orientation-dependent multiphoton ionization in wide band gap crystals.

Using different crystalline dielectrics and intense femtosecond laser pulses, we show that nonlinear absorption depends on sample orientation. This arises primarily because of the direction dependence of the effective mass of the electron. The multiphoton nature of the interaction creates a local probe that can be used anywhere in the material. We show that the structure of crystal quartz is not changed by repeated illumination of the focal region with 45 fs pulses.

Femtosecond laser erasing and rewriting of self-organized planar nanocracks in fused silica glass.

Tightly focused, linearly polarized, femtosecond laser radiation can produce highly birefringent nanograting structures inside fused silica glass. Here we report that when the polarization direction of the femtosecond light is changed, old nanogratings are erased and simultaneously replaced with new ones whose orientation is solely determined by the polarization of the rewrite beam. We also show that these volume nanogratings can be rewritten 1000 times with little degradation in their quality.

Direct measurement of the angular dependence of ionization for N2, O2, and CO2 in intense laser fields.

We experimentally measure the ionization probability as a function of alignment angle of three molecules in intense laser fields: nitrogen, oxygen, and carbon dioxide. Unlike atoms, molecules have a rotational degree of freedom. By controlling the alignment of the molecule relative to the laser field, molecules offer additional ways to understand strong-field ionization. The angular dependence of ionization directly maps to the orbital symmetry of each molecule. Carbon dioxide is seen to have a very sharp preference for ionization when aligned at 45 degrees to the laser field, in significant disagreement with current theories.

Femtosecond laser writing of porous capillaries inside fused silica glass.

We demonstrate that within a restricted optical pulse duration-pulse energy parameter space tightly focused femtosecond laser radiation can be used to fabricate porous capillaries in bulk fused silica glass by simply moving the laser focus through the material. We show that the rate of penetration of liquids into the porous capillaries can be controlled by the laser polarization, which determines their morphology. The fluid propagation is measured using the form birefringence of nanocrack/nanovoid structures produced inside the capillaries. We also demonstrate the nanofiltration capabilities of the capillaries by separating the relatively small molecules of Rhodamine 6G dye from their solvent.

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.

Dynamic polarization in the strong-field ionization of small metal clusters.

We report on the strong field ionization of small transition metal clusters (nickel, Ni(n) n=1-36) within the quasistatic regime at an infrared wavelength of 1.5 microm and at intensities up to 2 x 10(14) W/cm(2). From ion yields in a constant axial intensity beam, we obtained saturation intensities for the individual Ni(n) clusters. As compared to quasistatic, single active electron calculations, a dramatic suppression of ionization was observed. Dynamic polarization in the laser field likely leads to strong multielectron screening of the "active" electron. Representing the metal clusters as classical conducting spheres, we obtained, via a barrier suppression calculation, the classical ionization rates. Agreement was obtained for larger clusters with n>10 when the dynamic polarization was taken into account, emphasizing the multielectron nature of the ionization suppression.

Absolute ionization rates of multielectron transition metal atoms in strong infrared laser fields.

We report on nonresonant strong field ionization of the multielectron transition metal atoms V, Nb, Ta, Ni, and Pd. Operating in the adiabatic regime (lambda = 1.5 microm), we quantitatively determined both (i) the first charge state saturation intensities and (ii) the absolute ionization rates for intensities ranging from threshold up to 3 x 10(14) W/cm2. We observed a dramatic suppression of ionization relative to single active electron approximation expectations. We suggest that this derives from dynamic polarization or screening effects within the multielectron atom, stressing a need for many-body theories of strong field ionization.

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.

Alignment-dependent strong field ionization of molecules.

We demonstrate a method to measure strong field laser ionization of aligned molecules. The method employs a macroscopic field-free dynamic alignment, which occurs during revivals of rotational wave packets produced by a femtosecond laser pulse. We investigate the dependence of strong field ionization of N2 on molecular orientation. We determine that N2 molecules are four times more likely to ionize when aligned parallel to the field than when aligned perpendicular to it.

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.

A simultaneous outbreak on a neonatal unit of two strains of multiply antibiotic resistant Klebsiella pneumoniae controllable only by ward closure.

Two aminoglycoside-resistant strains of Klebsiella pneumoniae caused an outbreak on the neonatal unit at St Thomas' Hospital. One, which affected 18 patients, was capsular type K18 and resistant to newer cephalosporins by the production of the extended-spectrum beta-lactamase SHV-2; the other, which colonized four patients, was capsular non-typeable and did not produce extended-spectrum beta-lactamase. Both strains were probably brought into the unit by carrier patients; the probable carrier of the non-typeable strain was transferred from another hospital but was negative on a single admission screen; the probable carrier of the K18 strain was not screened on admission because he had been born at St Thomas', but his mother had been transferred from another hospital. Despite intensive efforts to control the outbreak by standard methods of hand washing, screening, patient isolation and environmental cleaning, a total of 22 neonates on the unit eventually became colonized or infected. One of three patients with bacteraemia died. A small proportion of samples of expressed breast milk, electronic thermometers and oxygen saturation probes were contaminated by the K18 strain and may have contributed to some of the cross-infection, but this did not explain the extent of the outbreak. The outbreak was controlled only by opening a temporary ward for colonized neonates and another for newly born babies, which allowed the closure and cleaning of the main neonatal unit. Multiply antibiotic resistant klebsiellas may be highly epidemic and cause serious, difficult-to-control outbreaks on neonatal units. All patients, regardless of their admission history, should be screened on admission for carriage of multiply resistant enterobacteria by a sensitive method, and units should have plans for temporary ward closure should outbreaks occur.