High-resolution mid-infrared spectroscopy based on ultrafast Cr:ZnSe laser.

High-resolution broadband direct frequency comb spectroscopy in the mid-infrared spectral region is an extremely powerful and versatile experimental technique that allows study of the molecular structure of gaseous compounds with multiple applicative and scientific implications. Here we present the first implementation of an ultrafast Cr:ZnSe mode-locked laser covering more than 7 THz at around the emission wavelength of 2.4 µm, for direct frequency comb molecular spectroscopy with a frequency sampling of 220 MHz and a frequency resolution of ∼100 kHz. This technique is based on a scanning micro-cavity resonator with a Finesse of ∼12,000 and a diffraction reflecting grating. We demonstrate its application in high-precision spectroscopy of the acetylene molecule by retrieving line center frequencies of more than 68 roto-vibrational lines. Our technique paves the way for real time spectroscopic studies as well as for hyperspectral imaging techniques.

Fiber laser system for standoff coherent Raman spectroscopy.

A fiber laser system for standoff detection of chemical and biological species by coherent anti-Stokes Raman scattering is presented. The system is based on an ytterbium fiber laser and a hollow-core photonic crystal fiber for generation of broadband pump/Stokes pulses. High-resolution Raman spectra encompassing the fingerprint region (600-1600cm-1) are obtained for toluene, and two simulants of chemical and biological warfare agents, specifically dimethyl methylphosphonate and sodium dipicolinate. The system is operated at standoff distances of 2 m and integration times of 8 ms. The fiber technology makes the approach suitable for implementation as a compact standoff detection and identification system.

Absolute frequency stabilization of a QCL at 8.6 µm by modulation transfer spectroscopy.

Modulation transfer spectroscopy is used to demonstrate absolute frequency stabilization of an 8.6-µm-wavelength quantum cascade laser against a sub-Doppler absorption of the CHF3 molecule. The obtained spectral emission properties are thoroughly characterized through a self-referenced optical frequency comb, stabilized against either a GPS-disciplined Rb clock or a 1.54-µm Er-fiber laser locked to a high-finesse ultra-low-expansion optical cavity. Fractional long-term stability and accuracy at a level of 4×10-12 (at 100 s) and 3×10-10, respectively, are demonstrated, along with an emission linewidth as narrow as 10 kHz for observation times of 0.1 s.

Nonlinear pulse compression to 22 fs at 15.6 µJ by an all-solid-state multipass approach.

We demonstrate nonlinear compression of pulses at 1.03 µm and repetition rate of 200 kHz generated by a ytterbium fiber laser using two cascaded all-solid-state multipass cells. The pulse duration has been compressed from 460 to 22 fs, corresponding to a compression factor of ∼21. The compressed pulse energy is 15.6 µJ, corresponding to an average power of 3.1 W, and the overall transmission of the two compression stages is 76%. The output beam quality factor is M2 ∼1.2 and the excess intensity noise introduced by nonlinear broadening is below 0.05%. These results show that nonlinear pulse compression down to ultrashort durations can be achieved with an all-solid-state approach, at pulse energies much higher than previously reported, while preserving the spatial characteristics of the laser.

Coherent mid-infrared supercontinuum generation in tapered suspended-core As39Se61 fibers pumped by a few-optical-cycle Cr:ZnSe laser.

We report on efficient supercontinuum generation in tapered suspended-core $ {{\rm As}_{39}}{{\rm Se}_{61}} $As39Se61 fibers pumped by a femtosecond mode-locked Cr:ZnSe laser. The supercontinuum spectrum spans the mid-infrared spectral region from 1.4 to 4.2 µm, and its spectral coherence is proved by heterodyning with a single-frequency narrow-linewidth Er-fiber laser at 1.55 µm, measuring a beat note with 27-dB signal-to-noise ratio in a resolution bandwidth of 100 kHz. The intensity stability of the supercontinuum radiation is also characterized by relative intensity noise measurements.

Broadband Fourier-transform coherent Raman spectroscopy with an ytterbium fiber laser.

We demonstrate a Fourier transform (FT) coherent anti-Stokes Raman scattering (CARS) spectroscopy system based on fiber technology with ultra-broad spectral coverage and high-sensitivity. A femtosecond ytterbium fiber oscillator is amplified and spectrally broadened in a photonic crystal fiber to synthesize pulses with energy of 14 nJ at 1040 nm, that are compressed to durations below 20 fs. The resulting pulse train is coupled to a FT-CARS interferometer enabling measurement of high-quality CARS spectra with Raman shifts of ~3000 cm-1 and signal to noise ratio up to 240 and 690 with acetonitrile and polystyrene samples, respectively, for observation times of 160 µs; a detection limit of one part per thousand is demonstrated with a cyanide/water solution. The system has the potential to detect trace contaminants in water as well as other broadband high-sensitivity CARS spectroscopy applications.

Fiber-format dual-comb coherent Raman spectrometer.

We demonstrate a fiber-format system for dual-comb coherent anti-Stokes Raman scattering spectroscopy. The system is based on two ytterbium fiber (Yb) femtosecond lasers at repetition frequencies of 94 MHz, a Yb amplifier, and a photonic crystal fiber for spectral broadening and generation of pulses with a central wavelength of 1040 nm and durations in the sub-20-fs regime. We observed Raman spectra of acetonitrile and ethyl acetate with spectral coverage from 100 to 1300 cm-1, resolution of 8 cm-1, and a signal-to-noise ratio of around 100, when averaging over 10 acquisitions. The design is suitable for implementing portable dual-comb coherent Raman spectrometers.

47-fs Kerr-lens mode-locked Cr:ZnSe laser with high spectral purity.

We report on a room-temperature Kerr-lens mode-locked Cr:ZnSe femtosecond laser operating at around 2.4 µm emission wavelength. Self-starting nearly transform-limited pulse trains with a minimum duration of 47 fs, corresponding to six optical cycles, and average output power of 0.25 W are obtained with repetition frequencies in the range from 140 to 300 MHz. The femtosecond pulse train is characterized by high-spectral purity and low time jitter.

Absolute frequency measurements of CHF3 Doppler-free ro-vibrational transitions at 8.6 µm.

We report on absolute measurements of saturated-absorption line-center frequencies of room-temperature trifluoromethane using a quantum cascade laser at 8.6 µm and the frequency modulation spectroscopy method. Absolute calibration of the laser frequency is obtained by direct comparison with a mid-infrared optical frequency comb synthesizer referenced to a radio-frequency Rb standard. Several sub-Doppler transitions falling in the υ5 vibrational band are investigated at around 1158.9 cm-1 with a fractional frequency precision of 8.6·10-12 at 1-s integration time, limited by the Rb-clock stability. The demonstrated frequency uncertainty of 6.6·10-11 is mainly limited by the reproducibility of the frequency measurements.

Double-Wall Carbon Nanotube Hybrid Mode-Locker in Tm-doped Fibre Laser: A Novel Mechanism for Robust Bound-State Solitons Generation.

The complex nonlinear dynamics of mode-locked fibre lasers, including a broad variety of dissipative structures and self-organization effects, have drawn significant research interest. Around the 2 µm band, conventional saturable absorbers (SAs) possess small modulation depth and slow relaxation time and, therefore, are incapable of ensuring complex inter-pulse dynamics and bound-state soliton generation. We present observation of multi-soliton complex generation in mode-locked thulium (Tm)-doped fibre laser, using double-wall carbon nanotubes (DWNT-SA) and nonlinear polarisation evolution (NPE). The rigid structure of DWNTs ensures high modulation depth (64%), fast relaxation (1.25 ps) and high thermal damage threshold. This enables formation of 560-fs soliton pulses; two-soliton bound-state with 560 fs pulse duration and 1.37 ps separation; and singlet+doublet soliton structures with 1.8 ps duration and 6 ps separation. Numerical simulations based on the vectorial nonlinear Schr¨odinger equation demonstrate a transition from single-pulse to two-soliton bound-states generation. The results imply that DWNTs are an excellent SA for the formation of steady single- and multi-soliton structures around 2 µm region, which could not be supported by single-wall carbon nanotubes (SWNTs). The combination of the potential bandwidth resource around 2 µm with the soliton molecule concept for encoding two bits of data per clock period opens exciting opportunities for data-carrying capacity enhancement.

Scanning micro-resonator direct-comb absolute spectroscopy.

Direct optical Frequency Comb Spectroscopy (DFCS) is proving to be a fundamental tool in many areas of science and technology thanks to its unique performance in terms of ultra-broadband, high-speed detection and frequency accuracy, allowing for high-fidelity mapping of atomic and molecular energy structure. Here we present a novel DFCS approach based on a scanning Fabry-Pérot micro-cavity resonator (SMART) providing a simple, compact and accurate method to resolve the mode structure of an optical frequency comb. The SMART approach, while drastically reducing system complexity, allows for a straightforward absolute calibration of the optical-frequency axis with an ultimate resolution limited by the micro-resonator resonance linewidth and can be used in any spectral region from UV to THz. We present an application to high-precision spectroscopy of acetylene at 1.54 µm, demonstrating performances comparable or even better than current state-of-the-art DFCS systems in terms of sensitivity, optical bandwidth and frequency-resolution.

Comb-locked Lamb-dip spectrometer.

Overcoming the Doppler broadening limit is a cornerstone of precision spectroscopy. Nevertheless, the achievement of a Doppler-free regime is severely hampered by the need of high field intensities to saturate absorption transitions and of a high signal-to-noise ratio to detect tiny Lamb-dip features. Here we present a novel comb-assisted spectrometer ensuring over a broad range from 1.5 to 1.63 µm intra-cavity field enhancement up to 1.5 kW/cm(2), which is suitable for saturation of transitions with extremely weak electric dipole moments. Referencing to an optical frequency comb allows the spectrometer to operate with kHz-level frequency accuracy, while an extremely tight locking of the probe laser to the enhancement cavity enables a 10(-11) cm(-1) absorption sensitivity to be reached over 200 s in a purely dc direct-detection-mode at the cavity output. The particularly simple and robust detection and operating scheme, together with the wide tunability available, makes the system suitable to explore thousands of lines of several molecules never observed so far in a Doppler-free regime. As a demonstration, Lamb-dip spectroscopy is performed on the P(15) line of the 01120-00000 band of acetylene, featuring a line-strength below 10(-23) cm/mol and an Einstein coefficient of 5 mHz, among the weakest ever observed.

Frequency-comb-assisted precision laser spectroscopy of CHF3 around 8.6 µm.

We report a high-precision spectroscopic study of room-temperature trifluoromethane around 8.6 µm, using a CW quantum cascade laser phase-locked to a mid-infrared optical frequency comb. This latter is generated by a nonlinear down-conversion process starting from a dual-branch Er:fiber laser and is stabilized against a GPS-disciplined rubidium clock. By tuning the comb repetition frequency, several transitions falling in the υ5 vibrational band are recorded with a frequency resolution of 20 kHz. Due to the very dense spectra, a special multiple-line fitting code, involving a Voigt profile, is developed for data analysis. The combination of the adopted experimental approach and survey procedure leads to fractional accuracy levels in the determination of line center frequencies, down to 2 × 10(-10). Line intensity factors, pressure broadening, and shifting parameters are also provided.

Frequency-noise measurements of optical frequency combs by multiple fringe-side discriminator.

The frequency noise of an optical frequency comb is routinely measured through the hetherodyne beat of one comb tooth against a stable continuous-wave laser. After frequency-to-voltage conversion, the beatnote is sent to a spectrum analyzer to retrive the power spectral density of the frequency noise. Because narrow-linewidth continuous-wave lasers are available only at certain wavelengths, heterodyning the comb tooth can be challenging. We present a new technique for direct characterization of the frequency noise of an optical frequency comb, requiring no supplementary reference lasers and easily applicable in all spectral regions from the terahertz to the ultraviolet. The technique is based on the combination of a low finesse Fabry-Perot resonator and the so-called "fringe-side locking" method, usually adopted to characterize the spectral purity of single-frequency lasers, here generalized to optical frequency combs. The effectiveness of this technique is demonstrated with an Er-fiber comb source across the wavelength range from 1 to 2 µm.

Direct phase-locking of a 8.6-µm quantum cascade laser to a mid-IR optical frequency comb: application to precision spectroscopy of N2O.

We developed a high-precision spectroscopic system at 8.6 µm based on direct heterodyne detection and phase-locking of a room-temperature quantum-cascade-laser against an harmonic, 250-MHz mid-IR frequency comb obtained by difference-frequency generation. The ∼30 dB signal-to-noise ratio of the detected beat-note together with the achieved closed-loop locking bandwidth of ∼500 kHz allows for a residual integrated phase noise of 0.78 rad (1 Hz-5 MHz), for an ultimate resolution of ∼21 kHz, limited by the measured linewidth of the mid-IR comb. The system was used to perform absolute measurement of line-center frequencies for the rotational components of the ν2 vibrational band of N2O, with a relative precision of 3×10(-10).

Narrow-linewidth quantum cascade laser at 8.6 µm.

We report on a narrow-linewidth distributed-feedback quantum cascade laser at 8.6 µm that is optical-feedback locked to a high-finesse V-shaped cavity. The spectral purity of the quantum cascade laser is fully characterized using a high-sensitivity optical frequency discriminator, leading to a 1 ms linewidth of less than 4 kHz and a minimum laser frequency noise spectral density as low as 0.01 Hz2/Hz for Fourier frequencies larger than 100 kHz. The cumulative standard deviation of the laser intensity is better than 0.1% over an integration bandwidth from 2 Hz to 100 MHz.

High-power frequency comb in the range of 2-2.15 µm based on a holmium fiber amplifier seeded by wavelength-shifted Raman solitons from an erbium-fiber laser.

We demonstrate a room-temperature high-power frequency comb source covering the spectral region from 2 to 2.15 µm. The source is based on a femtosecond erbium-fiber laser operating at 1.55 µm with a repetition rate of 250 MHz, wavelength-shifted up to 2.06 µm by the solitonic Raman effect, seeding a large-mode-area holmium (Ho) fiber amplifier pumped by a thulium (Tm) fiber laser emitting at 1.94 µm. The frequency comb has an integrated power of 2 W, with overall power fluctuations as low as 0.3%. The beatnote between the comb and a high-spectral-purity, single-frequency Tm-Ho laser has a linewidth of 32 kHz over 1 ms observation time, with a signal-to-noise ratio in excess of 30 dB.

Milliwatt-level frequency combs in the 8-14 µm range via difference frequency generation from an Er:fiber oscillator.

We report on the generation of mid-infrared (mid-IR) pulses with a maximum average optical power of 4 mW and wide tunability in the 8-14 µm range via difference frequency generation (DFG) in GaSe from an Er:fiber laser oscillator. The DFG process is seeded with self-frequency shifted Raman solitons that are shown to be phase coherent within the whole tuning range, from 1.76 to 1.93 µm. Interference measurements between adjacent pulses at the idler wavelengths attest coherence transfer to the mid-IR.

Frequency-stabilized 1 W optical comb at 2.2-2.6 µm by Cr2+:ZnSe multipass amplification.

We present a frequency comb source with power level up to 150 µW per comb mode, tunable in the 2.2-2.6 µm wavelength region, based on a Cr(2+):ZnSe multipass solid-state amplifier seeded by the output of an actively stabilized optical parametric oscillator, synchronously pumped by a commercial 250 MHz Er:fiber laser. Phase relationship between idler, signal, and pump waves is exploited to perform frequency comb stabilization in the whole 2.2-2.6 µm mid-infrared spectral region.

250-MHz synchronously pumped optical parametric oscillator at 2.25-2.6 µm and 4.1-4.9 µm.

A compact and versatile femtosecond mid-IR source is presented, based on an optical parametric oscillator (OPO) synchronously pumped by a commercial 250-MHz Er:fiber laser. The mid-IR spectrum can be tuned in the range 2.25-2.6 µm (signal) and 4.1-4.9 µm (idler), with average power from 20 to 60 mW. At 2.5 µm a minimum pulse duration of 110 fs and a power of 40 mW have been obtained. Active stabilization of the OPO cavity length has been achieved in the whole tuning range.