Disturbing interference patterns in femtosecond stimulated Raman microscopy

Femtosecond stimulated Raman microscopy (FSRM) is an upcoming technique in nonlinear microscopy which facilitates rapid chemical mapping. It employs femtosecond white‐light pulses as probe pulses and intense picosecond pulses as pump pulses. Stimulated Raman scattering (SRS) occurs at the focus of a scanning microscope. Chemical constituents in the sample are identified via their Raman signatures. In this article, disturbing interference patterns in FSRM are reported. They are caused by a broadening of the pump pulse due to nonlinear interactions in the focal region of the microscope and reduce the signal‐to‐noise ratio. The properties of these modulations are explored, and the methods to suppress them are presented. Copyright © 2009 John Wiley & Sons, Ltd.     

Microstructure fibers as frequency-tunable sources of ultrashort chirped pulses for coherent nonlinear spectroscopy

Microstructure fibers are shown to allow the creation of new tunable sources for femtosecond nonlinear spectroscopy. These fibers provide a high efficiency of frequency upconversion of regeneratively amplified femtosecond pulses of a Cr:forsterite laser, permitting the generation of subpicosecond anti-Stokes pulses with a smooth temporal envelope and a linear positive chirp. These pulses from a microstructure fiber were used to measure the spectra of coherent anti-Stokes Raman scattering (CARS) of toluene solution by cross-correlating these pulses with the femtosecond second-harmonic output of the Cr:forsterite laser in boxcars geometry (XFROG CARS). PACS 42.65.Wi; 42.81.Qb     

High-contrast chemical imaging with gated heterodyne coherent anti-Stokes Raman scattering microscopy

A novel method is presented which substantially improves the signal-to-background ratio for coherent anti-Stokes Raman scattering (CARS) microscopy. It exploits the fixed phase relation between pump, Stokes and CARS fields together with the strong phase coherence in supercontinua generated by femtosecond lasers. Three phase-locked optical parametric amplifiers are used for the realisation of heterodyne signal detection. Proper pulse timing yields a gating mechanism which nearly completely suppresses solvent background signals. PACS 42.65.Dr; 42.65.Hw; 42.65.Yj     

Carrier-envelope phase fluctuations of amplified femtosecond pulses: characterization with a simple spatial interference setup

We demonstrate a direct and versatile scheme to determine the carrier-envelope phase fluctuations of tunable ultrashort optical pulses. The spatial interferogram between the high frequency components and the parametrically amplified and frequency doubled low frequency components of an octave broad white light continuum is measured for every single pulse. It directly reveals the carrier-envelope phase fluctuations of the pump pulses from the regenerative amplifier, as well as of the white light and the tunable pulses generated from it. PACS 42.25.Kb; 42.65.Yj; 42.65.Re     

Origin of spectral interferences in femtosecond stimulated Raman microscopy

In femtosecond stimulated Raman microscopy (FSRM), a spectrally narrow (Raman pump) pulse and a broad (Raman probe) laser pulse are employed to generate the Raman spectra of microscopic objects. The resulting spectra exhibit, in addition to the Raman bands, spectral modulations of comparable amplitude. Here a model is devised that attributes these modulations to a four‐wave mixing (FWM) process. Two light fields of the probe pulse and one field of the pump pulse serve as input fields. The resulting FWM field experiences a heterodyne amplification by the probe field. Simulations based on this model reproduce the appearance of the spectral modulations. Furthermore, the amplitude of the modulations exhibits dependences on the energies of pump and probe pulses as well as on the nonlinear refractive index n₂, which are in line with the model. Copyright © 2011 John Wiley & Sons, Ltd.     

Generation of shaped ultraviolet pulses at the third harmonic of titanium-sapphire femtosecond laser radiation

We experimentally demonstrate a method to generate shaped femtosecond laser pulses in the ultraviolet at a central wavelength of 267 nm, the third harmonic of conventional titanium-sapphire femtosecond laser systems. Employing a 128-pixel liquid-crystal spatial light modulator, we impose variable spectral phase modulations upon the near-infrared laser pulses. By this, complex laser pulses can be shaped whose overall spectrum is still conserved. Our experiments show that it is possible to easily transfer these pulses into the ultraviolet at 267 nm via sum-frequency mixing in nonlinear crystals and to predictably generate multistructured ultraviolet femtosecond laser pulses. We analyze the temporal and spectral composition of these pulses after frequency conversion into the ultraviolet using difference-frequency cross-correlation and XFROG (cross-correlation frequency-resolved optical gating) techniques with an unmodulated fundamental laser pulse. The method can be employed to facilitate adaptive quantum control experiments in the ultraviolet wavelength regime, where the major absorption bands of many organic molecular systems are located. PACS 42.65.Re; 42.72.Bj; 32.80.Qk     

Systematic study of highly efficient white light generation in transparent materials using intense femtosecond laser pulses

We report the results of a systematic study of white light generation in different high band-gap optical media (BaF₂, acrylic, water and BK-7 glass) using ultrashort (45 fs) laser pulses. We have investigated the influence of different parameters, such as focal position of the incident laser light within the medium, the polarization state of the incident laser radiation and the pulse duration of the incident laser beam on the white light generation. Our results indicate that for intense, ultrashort pulses, the position of physical focus inside the media is crucial in the generation, with high efficiency, of white light spectra over the wavelength range 400–1100 nm. Linearly polarized incident laser light generates white light with higher intensity in the blue region than circularly polarized light. Ultrashort (45 fs) pulses generate a flatter spectrum with higher white light conversion efficiency than longer (300 fs) pulses of the same laser power. We believe that a flat response over a wide range of wavelengths in the continuum may be efficiently compressed for generation of sub-10 fs pulses. PACS 52.38.Hb; 42.65.Jx; 42.65.Tg; 33.80.Wz; 52.35.Mw     

Tunable mid-infrared,high-energy femtosecond laser source for glyco-protein structure analysis

We have developed a 6–12 μm mid-infrared (MIR) femtosecond laser source for glyco-protein structure analysis. The MIR femtosecond laser pulses are generated by a differential frequency generation (DFG) configuration with a combination of Ti:sapphire based regeneratively amplified femtosecond laser pulses (780 nm, 160 fs, 1 mJ) and a β-BaB₂O₄ (BBO) based optical parametric amplifier (OPA). The MIR pulse energy exceeds 4.5 μJ, where a glyco-protein molecule has resonant absorption lines due to the vibrational–rotational transitions. The pulse width is estimated to be less than 1 ps according to the cross correlation measurement between the two OPA output pulses. Using the MIR femtosecond laser pulses, we demonstrated photo-dissociation of the sialyl Lewis X (sLeX) proton added ion, which is the first time to the best of our knowledge. PACS 42.65.Re; 42.62.-b; 42.60.-b; 42.65.-k; 87.50     

A femtosecond stimulated raman spectrograph for the near ultraviolet

The design of a femtosecond stimulated Raman spectrograph (FSRS) optimized for measurements in the near UV is presented. It features a 387.5 nm Raman pump pulse causing a (pre-)resonance enhancement for molecular absorbing in the UV. As many photoreactive molecules absorb there, the set-up is particularly suited to study photochemical reactions. The 387.5 nm pulses are generated by frequency adding two femtosecond laser pulses with linear chirps, equal in magnitude but opposite in sign. This results in intense and spectrally narrow (∼10 cm^-1) Raman pump pulses which allow recording of Raman spectra with a good spectral resolution. The power of the spectrograph to trace ultrafast photoreactions is illustrated by measurements on the photochemistry of o-nitrobenzaldehyde. PACS 33.20.Fb; 39.30.+w     

Long-range self-channeling of infrared laser pulses in air: a new propagation regime without ionization

We report long-range self-channeling in air of multiterawatt femtosecond laser pulses with large negative initial chirps. The peak intensity in the light channels is at least one order of magnitude lower than required for multiphoton ionization of air molecules. A detailed comparison is made between experiments and realistic 3+1-dimensional numerical simulations. It reveals that the mechanism limiting the growth of intensity by filamentation is connected with broken revolution symmetry in the transverse diffraction plane. PACS 42.65.Sf; 42.25.Bs; 42.65.Jx; 52.38.Hb     

Stimulated Raman rotational photoacoustic spectroscopy using a quartz tuning fork and femtosecond excitation

Molecular alignment of linear molecules (O₂, N₂, CO₂ and CO) is measured photoacoustically in the gas phase. The rotational excitation is accomplished using a simple femtosecond stimulated Raman excitation scheme, employing two femtosecond pulses with variable delay between the pulses. Molecular alignment is determined directly by measuring the energy dumped into the gas by quartz-enhanced photoacoustic spectroscopy (QEPAS), utilizing a quartz tuning fork as a sensitive photoacoustic transducer. The experimental results demonstrate for the first time the use of a tuning fork for resonant photoacoustic detection of Raman spectra excited by femtosecond double pulses and match both simulation and literature values.     

Enhanced compression of femtosecond pulse in hollow-core photonic bandgap fibers

Compression of chirped free femtosecond pulses in hollow-core photonic bandgap fibers is investigated numerically. The results show that intrapulse stimulated Raman scattering can improve the quality of the compressed pulse. Positive third-order dispersion is the main limitation on the compression of the femtosecond pulse. However, the combined effect of the intrapulse stimulated Raman scattering and the negative third-order dispersion can form still shorter pulses than is possible with intrapulse stimulated Raman scattering alone. We also investigate the influence of width and peak power of input pulse on pulse compression.     

The influence of phase-modulation on femtosecond time-resolved coherent Raman spectroscopy

The influence of phase-modulation on femtosecond time-resolved coherent Raman scattering is investigated theoretically and experimentally. The coherent Raman signal taken as a function of the spectral position shows unexpected temporal oscillations close to time zero. A theoretical analysis of the coherent Raman scattering process indicates that the femtosecond light pulses are amplitude and phase modulated. The pulses are asymmetric in time with more slowly decaying trailing wings. The phase of the pulse amplitude contains quadratic and higher-order contributions.     

Numerical simulations of pulsed and quasi-cw regimes of synchronously pumped Raman oscillators

Synchronously pumped Raman oscillators allow for an efficient frequency conversion of pump pulses whose power is well below the threshold for extracavity stimulated Raman scattering (SRS). Numerical simulations show that the cavity mismatch of pump laser and Raman oscillator is critical for maximum conversion efficiency and minimum pulse duration for transient and stationary SRS. At a certain mismatch the simulations predict a quasi-cw Raman oscillator output even at moderate cavity quality factors. Optimum operation conditions are discussed for pump pulse trains of finite lengths. The results of the numerical calculations are in qualitative agreement with a simple phenomenological model. PACS 42.55.Ye; 42.65.Dr; 42.55.Lt     

Talbot effect under illumination of double femtosecond laser pulses

The Talbot effect under illumination of double femtosecond laser pulses has been reported. Spectrums of double femtosecond laser pulses with phase differences are quite different from that of one single femtosecond laser pulse. Therefore, the Talbot images of the double femtosecond laser pulses with phase differences are different from that of one single femtosecond laser pulse. Specifically, for the phase difference corresponding to π, the Talbot image shows the largest difference from that of one single pulse. Experimental results are in good agreement with the theoretical analysis. The behaviors of Talbot images under double femtosecond laser pulses illumination cannot be obtained under one femtosecond laser pulse, monochromatic or polychromatic light illumination. Therefore, it is a new interesting optical phenomenon for the Talbot effect which should have potential applications.     

Generation of an ultrashort optical pulse by four-wave Raman mixing in deuterium cooled at 77 K

When a 100-fs Ti:sapphire laser is focused into molecular deuterium cooled at 77 K, rotational stimulated Raman emission is generated based on four-wave Raman mixing. By phase locking the emission lines, the laser pulsewidth was reduced to 40 fs, when a nearly transform-limited pulse was utilized as a fundamental laser. The pulsewidth was further reduced to 20 fs, when a positively chirped pulse was employed. Computer simulation suggests that the Raman emission is strongly chirped and a train of pulses with lower intensities are formed when a chirp pulse is used as a fundamental laser. PACS 42.65.Dr; 42.55.Ye; 42.50-p     

Enhanced harmonic conversion efficiency in the self-guided propagation of femtosecond ultraviolet laser pulses in argon

Harmonic generation during the self-guided propagation of femtosecond ultraviolet (UV) laser pulses (248-nm, 450-fs) in argon is investigated. The third (82.7-nm) and fifth (49.6-nm) harmonics are generated in the UV filament. The energy-conversion efficiencies for the harmonics are found to be at least two orders of magnitude higher than those reported in the literature for similar gas pressures. The enhancement is attributed to the quasi-phase matching of the harmonics due to the self-guiding of the driving pulse. PACS 42.25.Bs; 42.65.Jx; 42.65.Re; 42.65.Ky     

All-optical stabilization of carrier-envelope phase by use of difference frequency generation with seeded amplification of colored conical emission

We stabilized the carrier-envelope phase of pulses emitted by a femtosecond regenerative amplifier through difference frequency generation between pump and seeded amplification of colored conical emission. Seeded amplification of colored conical emission was induced by modulational instability in the second harmonic generation with a supercontinuum injected and amplified. As a consequence, it inherited the origin phase of the pump pulse. After difference frequency with the pump pulses, the generated tunable idler pulses were carrier-envelope phase stabilized, which was verified with a simple and robust spectral interference setup. PACS 42.65.Re; 42.65.Yj; 42.25.Kb     

Conical four-wave mixing in sodium vapour excited by femtosecond laser pulses

Broadband (sometimes exceeding 1500 cm^-1) red-shifted (with respect to the sodium 3S–3P transition frequency) conical emission has been observed with the pump wavelength tuned in the range between 540 and 589 nm. Such broadband emission was attributed to the generation and amplification of light at the Rabi sideband frequencies in the field of intense femtosecond laser pulses. It has been shown that the cone angle of the emitted radiation is determined by the process of four-wave mixing under the conditions of longitudinal (Cherenkov-type) phase matching. PACS 42.65.Ky; 42.65.Re; 42.50.Hz     

Dynamics of femtosecond laser interactions with dielectrics

Femtosecond laser pulses appear as an emerging and promising tool for processing wide bandgap dielectric materials for a variety of applications. This article aims to provide an overview of recent progress in understanding the fundamental physics of femtosecond laser interactions with dielectrics that may have the potential for innovative materials applications. The focus of the overview is the dynamics of femtosecond laser-excited carriers and the propagation of femtosecond laser pulses inside dielectric materials. PACS 61.80.Ba; 52.38.Mf; 42.65.Jx; 78.47.+p; 71.35.-y