Optical detection of acoustic waves with surface plasmons.

For broadband and sensitive detection of acoustic waves, the surface plasmon resonance (SPR) can be used, which responds to variations of dielectric properties in close proximity to a metal film supporting surface plasmon waves. When an acoustic wave is incident onto a receiving plate positioned within the penetration depth of the surface plasmons, it creates displacements of the surface of the plate and thus modulates the dielectric properties, affecting the SPR and the reflection of the incident light. Here we study characteristics and determine the optimal configuration of such an acousto-optical transducer with surface plasmons for efficient conversion of an acoustic signal into an optical one. We simulate the properties of this transducer and present estimates showing that it can have a large frequency bandwidth and high sensitivity.

Time slicing in 3D momentum imaging of the hydrogen molecular ion photo-fragmentation.

Photo-fragmentation of the hydrogen molecular ion was investigated with 800 nm, 50 fs laser pulses by employing a time slicing 3D imaging technique that enables the simultaneous measurement of all three momentum components which are linearly related with the pixel position and slicing time. This is done for each individual product particle arriving at the detector. This mode of detection allows us to directly measure the three-dimensional fragment momentum vector distribution without having to rely on mathematical reconstruction methods, which additionally require the investigated system to be cylindrically symmetric. We experimentally reconstruct the laser-induced photo-fragmentation of the hydrogen molecular ion. In previous experiments, neutral molecules were used as a target, but in this work, performed with molecular ions, the initial vibrational level populations are well-defined after electron bombardment, which facilitates the interpretation. We show that the employed time-slicing technique allows us to register the fragment momentum distribution that reflects the initial molecular states with greater detail, revealing features that were concealed in the full time-integrated distribution on the detector.

Probing nonadiabatic molecular alignment by spectral modulation.

We investigated molecular alignment wakes of femtosecond laser pulses. Evolution of nonadiabatic molecular alignment in nitrogen gas has been measured via its nonlinear interaction effects with a variably delayed probe pulse. The induced rotational wave packet was mapped as a function of the angular difference between polarization directions of femtosecond pump and probe pulses as well as their relative delay and the plot of the variations of the rotational wave packet, i.e. "quantum carpet", was found to be in good agreement with the calculated angular and temporal dependencies of molecular alignment parameter.

White-light generation control with crossing beams of femtosecond laser pulses.

We investigated the variations in generated white-light when crossing two femtosecond laser beams in a Kerr medium. By changing the relative delay of two interacting intense femtosecond laser pulses, we show that white-light generation can be enhanced or suppressed. With a decrease of the relative delay an enhancement of the white-light output was observed, which at even smaller delays was reverted to a suppression of white-light generation. Under choosen conditions, the level of suppression resulted in a white-light output lower than the initial level corresponding to large delays, when the pulses do not overlap in time. The enhancement of the white-light generation takes place in the pulse that is lagging. We found that the effect of the interaction of the beams depends on their relative orientation of polarization and increases when the polarizations are changed from perpendicular to parallel. The observed effects are explained by noting that at intermediate delays, the perturbations introduced in the path of the lagging beam lead to a shortening of the length of filament formation and enhancement of the white-light generation, whereas at small delays the stronger interaction and mutual rescattering reduces the intensity in the central part of the beams, suppressing filamentation and white-light generation.

Cascade Raman sideband generation and orbital angular momentum relations for paraxial beam modes.

In this work, the nonlinear parametric interaction of optical radiation in various transverse modes in a Raman-active medium is investigated both experimentally and theoretically. Verification of the orbital angular momentum algebra (OAM-algebra) [Strohaber et al.,Opt. Lett.37,3411 (2012)] was performed for high-order Laguerre Gaussian modes ℓ>1. It was found that this same algebra also describes the coherent transfer of OAM when Ince-Gaussian modes were used. New theoretical considerations extend the OAM-algebra to even and odd Laguerre Gaussian, and Hermite Gaussian beam modes through a change of basis. The results of this work provide details in the spatiotemporal synthesis of custom broadband pulses of radiation from Raman sideband generation.

Pressure optimization of high harmonic generation in a differentially pumped Ar or H2 gas jet.

We experimentally studied the dependence of high harmonic generation in argon and molecular hydrogen on pressure changes in a gas jet that cause variations of the phase matching conditions and absorption. The study was performed at a peak laser intensity of ∼1.5 × 10(14) W/cm(2). To enable measurements over a wide range of pressures, we employed differential pumping with an additional cell (∼20 cm(3) volume) enclosing the gas jet. By increasing the pressure in the gas jet up to a maximum of 1.5 bars with argon or 0.5 bars with hydrogen, we observed an increase in the high harmonic (HH) yield until an optimum pressure of 0.2 bars was reached for Ar, beyond which the output began decreasing. For H2, we observed an increase of the HH output up to the maximum pressure of 0.5 bars. This pressure-dependence study allowed us to achieve a tenfold enhancement in the high harmonic yield at the optimum pressure.

Hyperfine structure constant of the neutron halo nucleus (11)Be(+).

The hyperfine splittings of ground state Be+11 have been measured precisely by laser-microwave double resonance spectroscopy for trapped and laser cooled beryllium ions. The ions were produced at relativistic energies and subsequently slowed down and trapped at mK temperatures. The magnetic hyperfine structure constant of Be+11 was determined to be A11=-2677.302 988(72) MHz from the measurements of the mF-mF'=0-0 field independent transition. This measurement provides essential data for the study of the distribution of the halo neutron in the single neutron halo nucleus Be11 through the Bohr-Weisskopf effect.

Multipass cell based on confocal mirrors for sensitive broadband laser spectroscopy in the near infrared.

We report on broadband absorption spectroscopy in the near IR using a multipass cell design based on highly reflecting mirrors in a confocal arrangement having the particular aim of achieving long optical paths. We demonstrate a path length of 314 m in a cell consisting of two sets of highly reflecting mirrors with identical focal length, spaced 0.5 m apart. The multipass cell covers this path length in a relatively small volume of 1.25 l with the light beam sampling the whole volume. In a first application, the absorption spectra of the greenhouse gases CO(2), CH(4), and CO were measured. In these measurements we used a femtosecond fiber laser with a broadband spectral range spanning the near IR from 1.5 to 1.7 µm. The absorption spectra show a high signal-to-noise ratio, from which we derive a sensitivity limit of 6 ppmv for methane observed in a mixture with air.

White-light generation using spatially-structured beams of femtosecond radiation.

We studied white-light generation in water using spatially- structured beams of femtosecond radiation. By changing the transverse spatial phase of an initial Gaussian beam with a 1D spatial light modulator to that of an Hermite-Gaussian (HGn,m) mode, we were able to generate beams exhibiting phase discontinuities and steeper intensity gradients. When the spatial phase of an initial Gaussian beam (showing no significant white-light generation) was changed to that of a HG01, or HG11 mode, significant amounts of white-light were produced. Because self-focusing is known to play an important role in white-light generation, the self-focusing lengths of the resulting transverse intensity profiles were used to qualitatively explain this production. Distributions of the laser intensity for beams having step-wise spatial phase variations were modeled using the Fresnel-Kirchhoff integral in the Fresnel approximation and found to be in good agreement with experiment.

Energy transfer between laser filaments in liquid methanol.

We demonstrate energy exchange between two filament-forming femtosecond laser beams in liquid methanol. Our results are consistent with those of previous works documenting coupling between filaments in air; in addition, we identify an unreported phenomenon in which the direction of energy exchange oscillates at increments in the relative pulse delay equal to an optical period (2.6 fs). Energy transfer from one filament to another may be used in remote sensing and spectroscopic applications utilizing femtosecond laser filaments in water and air.

Coherent transfer of optical orbital angular momentum in multi-order Raman sideband generation.

Experimental results from the generation of Raman sidebands using optical vortices are presented. By generating two sets of sidebands originating from different locations in a Raman-active crystal, one set containing optical orbital angular momentum and the other serving as a reference, Young's double slit experiment was simultaneously realized for each sideband. The interference between the two sets of sidebands was used to determine the helicity and topological charge in each order. Topological charges in all orders were found to be discrete and follow selection rules predicted by a cascaded Raman process.

In situ tomography of femtosecond optical beams with a holographic knife-edge.

We present an in situ beam characterization technique to analyze femtosecond optical beams in a folded version of a 2f-2f setup. This technique makes use of a two-dimensional spatial light modulator (SLM) to holographically redirect radiation between different diffraction orders. This manipulation of light between diffraction orders is carried out locally within the beam. Because SLMs can withstand intensities of up to I ∼ 10(11) W/cm2, this makes them suitable for amplified femtosecond radiation. The flexibility of the SLM was demonstrated by producing a diverse assortment of "soft apertures" that are mechanically difficult or impossible to reproduce. We test our method by holographically knife-edging and tomographically reconstructing both continuous wave and broadband radiation in transverse optical modes.

Single-snapshot and intensity-resolved two-photon fluorescence measurements.

We present a single-snapshot (SSS) method for obtaining intensity-resolved two-photon fluorescence (TPF). This simple method uses a digital camera to image the TPF spot on a liquid dye jet. By making a comparison between the local laser and TPF intensities, TPF probabilities are reconstructed. We compare our intensity-resolved TPF results with those obtained by the more common intensity scanning (IS) and z-scan methods. The dependence of the TPF probability on intensity obtained by the SSS method for coumarin-30 exhibits a clear maximum around I approximately 4 x 10(12) W/cm(2) and a postsaturation decrease, while no such effects were found in the data obtained by the other methods. Additionally, theoretical models are presented to extract the overall probability from within the volume integral. To our knowledge, we present the first reported measurements of such intensity-resolved TPF.

Precision measurement of the hyperfine structure of laser-cooled radioactive 7Be+ ions produced by projectile fragmentation.

The ground state hyperfine splitting of (7)Be+ has been measured by laser-microwave double-resonance spectroscopy in the online rf trap of RIKEN's slow RI-beam facility. Be ions produced by projectile fragmentation of 13C at approximately 1 GeV were thermalized in a rf ion guide gas cell and subsequently laser cooled in the ion trap to approximately 1 microeV. This 10(15)-fold reduction of the kinetic energy allows precision spectroscopy of these ions. A magnetic hfs constant of A=-742.772 28(43) MHz was measured for 7Be+, from which a nuclear magnetic moment of mu(I)=-1.399 28(2)mu(N) was deduced.

Focal transformation and the Gouy phase shift of converging one-cycle surface acoustic waves excited by femtosecond laser pulses.

We studied the changes of the pulse shape and the phase of the spectral components in converging-surface acoustic wave pulses. These pulses were excited with a femtosecond laser by a thermoelastic mechanism. To produce converging acoustic pulses, the laser beam was focused with an axicon in a circle on the surface of an aluminum sample. During propagation through the focus, the shape of the pulses of the normal surface velocity changed from two to three polar. The absolute value of the phase of the spectral components experienced a change close to pi/2 rad (Gouy phase shift) after passage of the focal region. These observations were confirmed by analytical and numerical calculations based on the two-dimensional wave equation for surface acoustic waves.

Raman spectra of dipicolinic acid in crystalline and liquid environments.

Raman spectra of dipicolinic acid (DPA) are important for detection of bacterial spores, since DPA and its salts present one of their major components. The implementation of a deeply cooled CCD camera in combination with pulsed excitation at 532 nm allowed measuring well-resolved Raman spectra of the DPA in different forms. Powder preparations, crystals grown from saturated solutions and aqueous solutions of the DPA were studied. The spectral features in different environments and comparison with the spectra obtained by other methods are discussed.

Tubulin dipole moment, dielectric constant and quantum behavior: computer simulations, experimental results and suggestions.

We used computer simulation to calculate the electric dipole moments of the alpha- and beta-tubulin monomers and dimer and found those to be |p(alpha)| = 552D, |p(beta)| = 1193D and |p(alphabeta)| = 1740D, respectively. Independent surface plasmon resonance (SPR) and refractometry measurements of the high-frequency dielectric constant and polarizability strongly corroborated our previous SPR-derived results, giving Deltan/Deltac approximately 1.800 x 10(-3)ml/mg. The refractive index of tubulin was measured to be n(tub) approximately 2.90 and the high-frequency tubulin dielectric constant k(tub) approximately 8.41, while the high-frequency polarizability was found to be alpha(tub) approximately 2.1 x 10(-33)C m(2)/V. Methods for the experimental determination of the low-frequency p are explored, as well as ways to test the often conjectured quantum coherence and entanglement properties of tubulin. Biobits, bioqubits and other applications to bioelectronics are discussed.

Measurements of the cross-bridge attachment/detachment process within intact sarcomeres by surface plasmon resonance.

We have developed a surface plasmon resonance (SPR) system to monitor the cross-bridge attachment/detachment process within intact sarcomeres from mouse heart muscle. SPR occurs when laser light energy is transferred to surface plasmons that are resonantly excited in a metal (gold) film. This resonance manifests itself as a minimum in the reflection of the incident laser light and occurs at a characteristic angle. The angle of the SPR occurrence depends on the dielectric permittivity of the sample medium adjacent to the gold film. Purified sarcomeric preparations are immobilized onto the gold film in the presence of a relaxing solution. Replacement of the relaxing solution with increasing Ca(2+) concentration solution activates the cross-bridge interaction and produces an increase in the SPR angle. These results imply that the interaction of myosin heads with actin within an intact sarcomere changes the dielectric permittivity of the sarcomeric structure. In addition, we further verify that SPR measurements can detect the changes in the population of the attached cross-bridges with altered concentrations of phosphate, 2,3-butanedione monoxime, or adenosine triphosphate at a fixed calcium concentration, which have been shown to reduce the force and increase the cross-bridge population in attached state. Thus, our data provide the first evidence that the SPR technique allows the monitoring of the cross-bridge attachment/detachment process within intact sarcomeres.

Surface-plasmon resonance spectrometry and characterization of absorbing liquids.

The effect of absorption of the sample medium on the surface-plasmon resonance (SPR) characteristics is analyzed by approximate analytical and exact numerical models. We show that absorption leads to specific changes in the value of reflectivity near the SPR angle and that these can be used for absorbance detection. The strongest absorption-induced change in reflectivity occurs at two values of metal film thickness (28 and 55 nm for a gold film and lambda = 632.8 nm). Using a sample solution of Rhodamine 700 in ethanol, we measured the characteristic changes in the SPR angle and in reflectivity over the wavelength interval encompassing the strong absorption band at 610-680 nm. The possibility of the simultaneous determination of the refractive index and absorption from SPR measurements is demonstrated and has the potential for substance-specific detection.

Excitation of capillary waves in strongly absorbing liquids by a modulated laser beam.

Several mechanisms for the excitation of capillary waves and for the development of the average deformation of a liquid surface under the action of a modulated laser beam are considered. The amplitude of the capillary wave in a strongly absorbing solution of the dye LDS 751 in ethylene glycol is experimentally studied as a function of laser intensity. Consecutive changes in the predominant mechanism of the excitation with increasing laser intensity are observed and described. At low laser intensities the mechanism connected with the creation of a surface tension gradient prevails. This mechanism becomes nonlinear with increasing influence of the convective motion. In addition, pressure pulsations of the convective flow start to contribute significantly to the generation process. The resonances of capillary waves in a cylindrical container are also investigated and used for determining the surface tension and viscosity of the liquid.