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We present a common-path optical device consisting of four optical components that produce a laser field consisting of two sub-beams with one radially polarized and the other linearly polarized. In the focus, the radially polarized sub-beam produces longitudinal polarization while the linearly polarized sub-beam produces polarization perpendicular to the propagation direction. By rotating the optical components, the orientation of the resulting electric field in the focus can be continuously varied in any direction. Estimates of the angular resolution of the device are given within the paraxial approximation.

We employed a midinfrared frequency comb source for methane detection in ambient air. The transmitted spectra over a bandwidth of about 500 nm were recorded with an optical spectrum analyzer under various experimental conditions of different path lengths. The normalized absorption spectra were compared and fitted with simulations, yielding quantitative values of concentrations of methane and water vapor in the ambient air. The 3σ detection limit was ∼6.6×10 -7   cm -1 in ambient air for a broad spectral range, achieved with a path length of ∼590  m. This approach provides a broad spectral range, a large dynamic range, high sensitivity, and accurate calibration. The performed analysis of the residuals shows that an excellent agreement between the measured and calculated spectral profiles was obtained.

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.

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.

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.

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.

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.

We present a femtosecond frequency comb vernier spectrometer in the near infrared with a femtosecond Er doped fiber laser, a scanning high-finesse cavity and an InGaAs camera. By utilizing the properties of a frequency comb and a scanning high-finesse cavity such a spectrometer provides broad spectral bandwidth, high spectral resolution, and high detection sensitivity on a short time scale. We achieved an absorption sensitivity of ~8 × 10(-8) cm(-1)Hz(-1/2), corresponding to a detection limit of ~70 ppbv for acetylene, with a resolution of ~1.1 GHz in single images taken in 0.5 seconds and covering a frequency range of ~5 THz. Such measurements have broad applications for sensing greenhouse gases in this fingerprint near infrared region with a simple apparatus.

We generate broadband light by focusing two femtosecond pulses into a Raman-active crystal. By reflecting Raman sideband beams together with the two driving beams back to the same crystal (with a slight spatial offset), we generate sidebands covering a broader spectral range, compared to a single pass. In this novel double-path configuration, multiple Raman sideband beams interact with each other since the phase-matching condition is automatically fulfilled. This scheme enables an enhanced cascaded coherent anti-Stokes scattering process and also doubles the interaction length, thus it allows one to use relatively weak energy pump pulses and thereby avoid optical damage.

We have generated multi-color optical vortices in a Raman-active crystal PbWO4 using two-color Fourier-transform limited femtosecond laser pulses. This setup overcomes some of the limitation of our previous research by allowing for the production of subcycle femtosecond optical vortices without the need for compensating for added chirp. In addition, the use of an OPA allows for greater flexibility in exciting different Raman modes. We verified the topological charges using two different methods. These diagnostic experiments verify not only theoretically predicted OAM algebra but demonstrated instabilities in high-order OVs. We have also studied factors which affect the high-order vortex sidebands such as the diameter and intensity of the input beams.

The dynamics of electronic excitations and their relaxation in a gold film is studied on the femtosecond time scale with a pump-probe technique. For the pump beam we use pulses with wavelengths centered at 800 nm, 400 nm or both. The surface plasmon resonance (SPR) in Kretschmann's configuration is used as a sensitive and fast-response probe of the dynamics of the dielectric properties of the gold film. The quantity that is monitored is the intensity of the reflected light at an incidence angle close to the SPR. With changes of the dielectric properties induced by the pump beam and during subsequent relaxation, the amount of the reflected light of the probe beam, sent with a variable delay, also changes, thus providing information on the temporal characteristics of the thermalization process. Special features of SPR probing with short pulses are also accounted for in this work. The thermalization of the electronic subsystem and energy transfer to the lattice are discussed in connection with the two-temperature relaxation model that takes into account temperature dependences of the electronic heat capacity and the electron-phonon coupling.

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.

We report on a high-power mid-infrared (MIR) frequency comb source based on a femtosecond (fs) Er:fiber oscillator with a stabilized repetition rate of 250 MHz. The MIR frequency comb is produced through difference frequency generation in a periodically poled MgO-doped lithium niobate crystal. The output power is about 120 mW, with a pulse duration of about 80 fs and spectrum coverage from 2.9 to 3.6 μm, and the single comb mode power is larger than 0.3 μW over the range of 700 nm. The coherence properties of the produced high-power broadband MIR frequency comb are maintained, which was verified by heterodyne measurements. As the first application, the spectrum of a ~200 ppm methane-air mixture in a short 20 cm glass cell at ambient atmospheric pressure and temperature was measured.

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.

A portable apparatus for the separation of krypton from environmental air samples was tested. The apparatus is based on the cryogenic trapping of gases at liquid nitrogen temperature followed by controlled releases at higher temperatures. The setup consists of a liquid nitrogen trap for the removal of H(2)O and CO(2), followed by charcoal-filled coils that sequentially collect and release krypton and other gases providing four stages of gas chromatography to achieve separation and purification of krypton from mainly N(2), O(2), and Ar. Residual reactive gases remaining after the final stage of chromatography are removed with a hot Ti sponge getter. A thermal conductivity detector is used to monitor the characteristic elution times of the various components of condensed gases in the traps during step-wise warming of the traps from liquid nitrogen temperatures to 0 °C, and then to 100 °C. This allows optimizing the switching times of the valves between the stages of gas chromatography so that mainly krypton is selected and loaded to the next stage while exhausting the other gases using a He carrier. A krypton separation efficiency of ~80 % was determined using a quadrupole mass spectrometer.

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.

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., (© 2012 Optical Society of America)

We report on the photoionization and photofragmentation of benzene (C(6)H(6)) and of the monohalobenzenes C(6)H(5)-X (X = F, Cl, Br, I) under intense-field, single-molecule conditions. We focus 50-fs, 804-nm pulses from a Ti:sapphire laser source, and record ion mass spectra as a function of intensity in the range ∼10(13) W/cm(2) to ∼10(15) W/cm(2). We count ions that were created in the central, most intense part of the focal area; ions from other regions are rejected. For all targets, stable parent ions (C(6)H(5)X(+)) are observed. Our data is consistent with resonance-enhanced multiphoton ionization (REMPI) involving the neutral (1)ππ* excited state (primarily a phenyl excitation): all of our plots of parent ion yield versus intensity display a kink when this excitation saturates. From the intensity dependence of the ion yield we infer that both the HOMO and the HOMO-1 contribute to ionization in C(6)H(5)F and C(6)H(5)Cl. The proportion of phenyl (C(6)H(5)) fragments in the mass spectra increases in the order X = F, Cl, Br, I. We ascribe these substituent-dependent observations to the different lifetimes of the C(6)H(5)X (1)ππ* states. In X = I the heavy-atom effect leads to ultrafast intersystem crossing to a dissociative (3)nσ* state. This breaks the C-I bond in an early stage of the ultrashort pulse, which explains the abundance of fragments that we find in the iodobenzene mass spectrum. For the lighter X = F, Cl, and Br this dissociation is much slower, which explains the lesser degree of fragmentation observed for these three molecules.

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.

The transmission of ultrashort (7 fs) broadband laser pulses through periodic gold nano-structures is studied. The distribution of the transmitted light intensity over wavelength and angle shows an efficient coupling of the incident p-polarized light to two counter-propagating surface plasmon (SP) modes. As a result of the mode interaction, the avoided crossing patterns exhibit energy and momentum gaps, which depend on the configuration of the nano-structure and the wavelength. Variations of the widths of the SP resonances and an abrupt change of the mode interaction in the vicinity of the avoided crossing region are observed. These features are explained by the model of two coupled modes and a coupling change due to switching from the higher frequency dark mode to the lower frequency bright mode for increasing wavelength of the excitation light.

We describe a method for retrieving spectral phase information from second harmonic interferometric autocorrelation measurements supplemented by the use of the observed spectral intensity. By applying a combination of graduated optimization and genetic algorithms, accurate phase retrieval of laser pulses as short as a few optical cycles was obtained from the measured autocorrelation and spectral intensity. The effectiveness of the combined algorithms is demonstrated on a set of significantly different femtosecond pulse shapes.

We study propagation of short laser pulses through water and use a spectral hole filling technique to essentially perform a sensitive balanced comparison of absorption coefficients for pulses of different duration. This study is motivated by an alleged violation of the Bouguer-Lambert-Beer law at low light intensities, where the pulse propagation is expected to be linear, and by a possible observation of femtosecond optical precursors in water. We find that at low intensities, absorption of laser light is determined solely by its spectrum and does not directly depend on the pulse duration, in agreement with our earlier work and in contradiction to some work of others. However, as the laser fluence is increased, interaction of light with water becomes nonlinear, causing energy exchange among the pulse's spectral components and resulting in peak-intensity dependent (and therefore pulse-duration dependent) transmission. For 30 fs pulses at 800 nm center wavelength, we determine the onset of nonlinear propagation effects to occur at a peak value of about 0.12 mJ/cm(2) of input laser energy fluence.

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.

We image spatial distributions of Xeq+ ions in the focus of a laser beam of ultrashort, intense pulses in all three dimensions, with a resolution of approximately 3 microm and approximately 12 microm in the two transverse directions. This allows for studying ionization processes without spatially averaging ion yields. Our in situ ion imaging is also useful to analyze focal intensity profiles and to investigate the transverse modal purity of tightly focused beams of complex light. As an example, the intensity profile of a Hermite-Gaussian beam mode HG1,0 recorded with ions is found to be in good agreement with optical images.

We introduce a simple and practical method to create ultrashort intense optical vortices for applications involving high-intensity lasers. Our method utilizes femtosecond laser pulses to laser etch grating lines into laser-quality gold mirrors. These grating lines holographically encode an optical vortex. We derive mathematical equations for each individual grating line to be etched, for any desired (integer) topological charge. We investigate the smoothness of the etched grooves. We show that they are smooth enough to produce optical vortices with an intensity that is only a few percent lower than in the ideal case. We demonstrate that the etched gratings can be used in a folded version of our 2f-2f setup [Opt. Express 19, 7599 (2005)] to compensate angular dispersion. Finally, we show that the etched gratings withstand intensities of up to 10(12) W/cm(2).

We experimentally demonstrate that small misalignments of the pulse stretcher or compressor of our chirped-pulse-amplification laser can precompensate for angular chirp when producing ultrashort paraxial beam modes with holographic gratings. Using this approach we can eliminate one of the two gratings needed in our 2f-2f setup [Mariyenko, Opt. Express 13, 7599 (2005)]. This allows for up to an order of magnitude more output power. We see our method as the next step in the production of intense exotic forms of ultrashort pulses, which can be used in the investigation of intense laser-matter interactions. In addition, we produce the first femtosecond (helical-)Ince-Gaussian beams.

We experimentally created a femtosecond optical vortex using a pair of computer-synthesized holographic gratings arranged in a 2f - 2f optical setup. We present measurements showing that the resulting donut mode is free of spatial chirp, and support this finding with an analysis of the optical wave propagation through our system based on the Kirchhoff-Fresnel diffraction integral. An interferogram confirms that our ultrashort vortex has topological charge 1, and a conservative experimental estimation of its duration is 280 fs. We used 25-fs radiation pulses (bandwidth approximately 40 nm) produced by a Ti:sapphire laser oscillator.