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.

Versatile OSCAT time-domain THz spectrometer.

We report on a compact and versatile time-domain spectrometer operating in the THz spectral region from 0.2 to 2.5 THz based on ultrafast Yb:CALGO laser and photo-conductive antennas. The spectrometer operates with the optical sampling by cavity tuning (OSCAT) method based on laser repetition rate tuning, which allows at the same time the implementation of a delay-time modulation scheme. The whole characterization of the instrument is presented and compared to the classical THz time-domain spectroscopy implementation. THz spectroscopic measurements on a 520-µm thick GaAs wafer substrate together with water vapor absorption measurements are also reported to further validate the instrument capabilities.

Standoff detection of bacterial spores by field deployable coherent Raman spectroscopy.

Vibrational spectroscopies offer great potential for standoff detection of chemical and biological warfare agents, avoiding contamination to the operator and equipment. Among them, particularly promising is Coherent anti-Stokes Raman scattering (CARS) spectroscopy, using synchronized pump/Stokes laser pulses to set up a vibrational coherence of target molecules at a laser focus, which is read by further interaction with a probe pulse, resulting in the emission of a coherent beam detectable at a distance. CARS has previously demonstrated the capability to detect bacterial spores based on the Raman spectrum of the characteristic molecule calcium dipicolinate (CaDPA); however, a complex and bulky laser technology, which is only suitable for a laboratory environment, was employed. Here we develop a broadband CARS setup based on a compact, industrial grade ytterbium laser system. We demonstrate high signal-to-noise ratio detection of Bacillus atrophaeus spores at a concentration of 105 cfu/mm2, at a standoff distance of 1 m, and an acquisition time of 1 s. Our system, which combines chemical specificity and sensitivity along with improved ruggedness and portability, paves the way to a new generation of instruments for real-world standoff detection of chemical and biological threats.

Standoff CARS spectroscopy and imaging using an ytterbium-based laser system.

A laser system for standoff coherent anti-Stokes Raman scattering (CARS) spectroscopy of various materials under ambient light conditions is presented. The system is based on an ytterbium laser and an ultrafast optical parametric amplifier for the generation of a broadband pump tunable from 880 to 930 nm, a Stokes at 1025 nm, and a narrowband probe at 512.5 nm. High-resolution Raman spectra encompassing the fingerprint region (400-1800 cm-1) are obtained in 5 ms for toluene, and 100 ms for two types of sugars, glucose and fructose, at a distance of 1 m. As a demonstration of the potential of the setup, hyperspectral images of a 2×2-cm2 target area are collected for a toluene cuvette and a glucose/fructose pressed disk. Our approach is suitable for implementation of a portable system for standoff CARS imaging of chemical and biological materials.

Low-noise Yb:CALGO optical frequency comb.

We report on a compact optical frequency comb, operating in the wavelength range from 670 to 1500 nm, based on diode-pumped low-noise femtosecond Yb:CALGO amplified laser system. Both the carrier-envelope offset and repetition rate are phase-locked to reference synthesizers. A full characterization of the frequency comb, in terms of frequency stability, phase noise analysis, and optical beating against a single-frequency non-planar ring oscillator Nd:YAG laser, is presented, showing the excellent properties of the Yb:CALGO comb.

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.

Few-optical-cycle pulse generation based on a non-linear fiber compressor pumped by a low-energy Yb:CALGO ultrafast laser.

Pulse compression in a short, normal dispersion photonic-crystal fiber is investigated with a Yb:CaGdAlO4 laser pumped by a low-power fiber-coupled single-mode diode that delivers 70-fs pulses at 1050 nm central wavelength, with 45-mW average power at 60 MHz repetition rate. A simple and power-efficient compressor based on a ∼15-cm long, low-cost commercial nonlinear fiber, with normal dispersion at the laser wavelength, produces pulses as short as 14.9 fs, corresponding to ∼4.25 optical cycles, with 29 mW average power after a prism-pair compressor in double pass configuration. Pulse quality was investigated with frequency resolved optical gating (FROG) analysis. Furthermore, a comparative analysis of noise properties of the oscillator, pump laser and compressed pulses has been performed.

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.

Ultrafast Dy3+:fluoride fiber laser beyond 3 µm.

We report a passively mode-locked Dy3+:fluoride fiber laser emitting around 3.1 µm based on the nonlinear polarization evolution technique in a ring configuration, using in-band pumping at 2.8 µm. Transform-limited and self-starting mode-locked pulses as short as 828 fs with a center wavelength around 3.1 µm and repetition rates up to 60 MHz are obtained. In the single-pulse regime, a maximum average output power of 204 mW is measured, corresponding to a peak power of 4.2 kW and a pulse energy of 4.8 nJ. This first demonstration, to the best of our knowledge, of a femtosecond mode-locked fiber laser emitting directly beyond 3 µm paves the way for frequency comb synthesis in the molecular fingerprint region.

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.

The optical frequency comb fibre spectrometer.

Optical frequency comb sources provide thousands of precise and accurate optical lines in a single device enabling the broadband and high-speed detection required in many applications. A main challenge is to parallelize the detection over the widest possible band while bringing the resolution to the single comb-line level. Here we propose a solution based on the combination of a frequency comb source and a fibre spectrometer, exploiting all-fibre technology. Our system allows for simultaneous measurement of 500 isolated comb lines over a span of 0.12 THz in a single acquisition; arbitrarily larger span are demonstrated (3,500 comb lines over 0.85 THz) by doing sequential acquisitions. The potential for precision measurements is proved by spectroscopy of acetylene at 1.53 µm. Being based on all-fibre technology, our system is inherently low-cost, lightweight and may lead to the development of a new class of broadband high-resolution spectrometers.

Diamond photonics platform enabled by femtosecond laser writing.

Diamond is a promising platform for sensing and quantum processing owing to the remarkable properties of the nitrogen-vacancy (NV) impurity. The electrons of the NV center, largely localized at the vacancy site, combine to form a spin triplet, which can be polarized with 532 nm laser light, even at room temperature. The NV's states are isolated from environmental perturbations making their spin coherence comparable to trapped ions. An important breakthrough would be in connecting, using waveguides, multiple diamond NVs together optically. However, still lacking is an efficient photonic fabrication method for diamond akin to the photolithographic methods that have revolutionized silicon photonics. Here, we report the first demonstration of three dimensional buried optical waveguides in diamond, inscribed by focused femtosecond high repetition rate laser pulses. Within the waveguides, high quality NV properties are observed, making them promising for integrated magnetometer or quantum information systems on a diamond chip.

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.