Deep- to near-ultraviolet Raman frequency conversion pumped by femtosecond pulses in a hollow-core waveguide.

Broadband vibrational/rotational Raman generation ranging from deep ultraviolet (DUV) to blue wavelengths is demonstrated by using molecular hydrogen in a hollow-core waveguide as a Raman-active medium pumped by a femtosecond DUV laser. We find the high-order transient stimulated Raman scattering is drastically enhanced for input beams including a circularly polarized component; a circularly polarized input beam achieves the highest conversion efficiency. Coherent vibrational anti-Stokes Raman emission is observed only for a circularly polarized pump beam, indicating that the waveguide effect also contributes to the upconversion of a DUV pulse via transient stimulated Raman scattering.

A Molecularly Modulated Mode-Locked Laser.

A mode-locked laser operating at a frequency over 10 THz is reported, which is three orders of magnitude greater than a standard mode-locked laser. The system used molecules with a Raman gain as an amplifier, while coherent molecular motions were used for optical modulation. Molecules in a high-finesse optical cavity modulated a continuous-wave beam to produce a train of ultrashort optical pulses at a repetition rate corresponding to the frequency of molecular motion. Phase-locking was achieved by an appropriate compensation of the total dispersion of the optical cavity. Thus, the oscillating multiple longitudinal modes were all coupled under phase-matching conditions of parametric four-wave mixing.

Continuous-wave phase-matched molecular optical modulator.

In optical modulation, the highest available modulation rate is basically limited to the GHz frequency range at best. This is because optical modulation is often performed using electro-optic or acousto-optic effects that require application of an external signal to solid-state nonlinear optical materials. Here we describe optical modulation of continuous-wave radiation at frequencies exceeding 10 THz based on ultrafast variation of molecule polarizability arising from coherent molecular motion. The optical modulation efficiency is extensively enhanced by fulfilling phase-matching conditions with the help of dispersion control of the optical cavity, generating sidebands with a highest ratio of 7.3 × 10(-3). These results will pave the way for development of versatile optical modulation-based techniques in a wide range of research fields in optical sciences, such as mode-locked lasers operating in the THz range.

Continuous-wave anti-Stokes Raman laser based on phase-matched nondegenerate four-wave mixing.

We demonstrate phase-matched nondegenerate four-wave mixing (FWM) in a high-finesse optical cavity using a gaseous Raman-active medium pumped by two independent continuous-wave lasers. Efficient upconversion is achieved for pump beams at different wavelengths under phase-matched conditions by optimizing the total dispersion of the hydrogen-filled optical cavity. The independent control of the pump-beam polarizations leads to further enhancement of the upconversion efficiency arising from a larger Raman gain than that in degenerate FWM. This approach offers a promising alternative for a narrow-linewidth tunable light source for highly precise laser spectroscopy.

Intracavity phase-matched coherent anti-Stokes Raman spectroscopy for trace gas detection.

We present a novel, cavity-enhanced spectroscopic technique based on a phase-matched Raman process to detect trace quantities of gas. The essence of this technique is the careful control of cavity dispersion to satisfy the phase-matching condition of coherent anti-Stokes Raman scattering (CARS) enhanced in a high-finesse optical cavity. A 6000-fold improvement of the CARS signal is observed under optimized conditions, indicating that this is a promising tool to quantify Raman-active molecules with an extremely low detection limit.

Ionization of pesticides using a far-ultraviolet femtosecond laser in gas chromatography/time-of-flight mass spectrometry.

The fourth harmonic emission (200 nm) of a femtosecond Ti:sapphire laser (35 fs) was generated and used in the multiphoton ionization of 49 pesticides in gas chromatography/time-of-flight mass spectrometry. The limit of detection was improved when the ionization source from the third harmonic emission (267 nm) was replaced with the fourth harmonic emission for several pesticide molecules that contained no conjugated double bonds since their absorption bands are located in the far-ultraviolet region. This analytical instrument was used in the analysis of a series of real samples including potatoes, carrots, and cabbage, and a signal suspected to arise from di-allate was observed for the potato sample. ᅟ

Control of quantum pathways for the generation of continuous-wave Raman sidebands.

The generation of a multifrequency continuous-wave laser through stimulated Raman scattering and phase-matched four-wave mixing in a medium-filled optical cavity is demonstrated. Three different quantum pathways for the four-wave mixing, two of them degenerate and one of them nondegenerate, can be excited independently by tuning the intracavity dispersion. The results suggest that phase-matched Raman sidebands were generated on the longer wavelength side as well as on the shorter wavelength side, which can be used for the Fourier synthesis of a train of ultrashort optical pulses.

Enhancement of molecular ions in mass spectrometry using an ultrashort optical pulse in multiphoton ionization.

The spectral domain of an ultraviolet femtosecond laser was expanded by stimulated Raman scattering/four-wave Raman mixing, and the resulting laser pulse was compressed using a pair of gratings. The pulse width was then measured using an autocorrelator comprised of a Michelson interferometer equipped with a multiphoton ionization/mass spectrometer which was used as a two-photon detector. A gas chromatograph/mass spectrometer was employed to analyze triacetone triperoxide (TATP), and the molecular ion induced by multiphoton ionization was substantially enhanced by decreasing the laser pulse width.

Quantitative measurement of the phase locking of highly repetitive ultrashort optical pulses generated by a multifrequency continuous-wave Raman laser.

We proposed and demonstrated a novel method for the evaluation of optical pulse trains generated by a multifrequency continuous-wave Raman laser operating at a mode separation of 17.6 THz. This approach is based on the detection of a nonlinear signal arising from the intensity modulation of a pulse train, which should provide a useful means for measuring the deviation from phase locking of multifrequency lasers. Our results suggest that an optimization of intracavity dispersion allows the generation of phase-locked multifrequency emissions, which leads to optical pulse trains at a repetition rate in excess of 10 THz.

Near-ultraviolet femtosecond laser ionization of dioxins in gas chromatography/time-of-flight mass spectrometry.

Gas chromatography/multiphoton ionization/time-of-flight mass spectrometry (GC/MPI/TOF-MS) was applied to the trace analysis of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs). To determine the optimum wavelength for analysis of PCDD/Fs, the wavelength of the femtosecond laser utilized for multiphoton ionization was converted to near-ultraviolet status using stimulated Raman scattering. A femtosecond laser emitting at 300 nm completely eliminated the background signal arising from the bleeding compounds generated from a stationary phase of the capillary column in GC.

Generation of intense 11-fs ultraviolet pulses using phase modulation by two types of coherent molecular motions.

The use of two types of phase modulations arising from the coherent rotations of ortho-hydrogen and para-hydrogen to generate an intense ultrashort ultraviolet pulse without substantial generation of sub-pulses was demonstrated. This technique allows use of a high-energy long-probe pulse in the pump-probe regime for generating a high-energy compressed pulse. A 100-fs ultraviolet pulse was compressed to 11-fs by the phase modulation followed by dispersion compensation with chirped mirrors.

Phase-matched Raman-resonant four-wave mixing in a dispersion-compensated high-finesse optical cavity.

A highly efficient intracavity four-wave mixing in a Raman-active medium pumped by a continuous-wave laser is first demonstrated. Managing the intracavity dispersion to satisfy the phase matching in a high-finesse cavity substantially enhances the anti-Stokes emission. This process is observed in a region far beyond small signal approximation, indicating the generation of phase-locked sidebands arising from molecular modulation. This points to a novel approach of an optical modulator and mode-locked laser operating at a frequency of more than 10 THz.

Interferometric characterization of ultrashort deep ultraviolet pulses using a multiphoton ionization mass spectrometer.

The temporal characterization of a femtosecond laser pulse in the deep ultraviolet region using an interferometric autocorrelation scheme is demonstrated. Two-photon ionization of a molecule in a time-of-flight mass spectrometer was used as a nonlinear detector to obtain an autocorrelation trace. This setup proved useful in not only providing a temporal characterization of a pulse but also investigating the ultrafast dynamics of photochemical processes.

Efficient generation of a three-primary-color laser from the second-harmonic emission of a Nd:YAG laser.

Laser emission, consisting of three primary colors, is generated by frequency conversions of the second-harmonic emission of a picosecond (120 ps) Nd:YAG laser by means of stimulated Raman scattering and subsequent four-wave Raman mixing in molecular deuterium. In the double-pass configuration, the fundamental beam (532 nm, 14.16 mJ, 100%) is converted to blue (459 nm, 1.71 mJ, 12.1%), green (532 nm, 7.04 mJ, 49.7%), and red (632 nm, 4.90 mJ, 34.6%), resulting in a total conversion efficiency of 96.4%.

Pulse compression based on coherent molecular motion induced by transient stimulated Raman scattering.

A novel method for compressing a laser pulse, using a combination of transient stimulated Raman scattering and a pump-probe technique, is proposed. The approach does not require a short laser pulse, in contrast to a reported method based on impulsive stimulated Raman scattering. The observed spectrum was sufficiently broad to generate a sub-10 fs pulse. In fact, a 100-fs pulse in the near-ultraviolet region was compressed to the sub-30 fs. Further compression of the laser pulse would be achieved by compensating for phase distortion, as suggested from the observed data of the spectral phase.

Generation of a sub-20-fs single optical pulse by four-wave Raman mixing using two Raman cells filled with molecular hydrogen.

To attempt to expand the spectral domain for pulse shortening, we generated several emission lines by stimulated Raman scattering and subsequent four-wave Raman mixing. The efficiency of generation of the Raman emission was improved by passing the beam through two Raman cells that were connected in series. The group-velocity dispersion induced by a Raman cell window and hydrogen was compensated for by means of a pair of chirped mirrors for pulse compression. By a phase lock of the emission lines in the process of four-wave Raman mixing, the pulse width was reduced from 114 to 17 fs in the second Raman cell.