We present a system based on a high-energy femtosecond ytterbium laser seeding an optical parametric amplifier and a photonic crystal hollow core fiber (PCHCF) compressor for coherent anti-Stokes Raman scattering (CARS) spectroscopy. The PCHCF provides spectral broadening of the Stokes pulse which is then compressed to a duration matched to that of the pump pulse. In these conditions, the excitation efficiency of vibrational levels in the target molecules is largely improved, as the time gating effect due to the mismatch between the durations of the pump and Stokes pulses is avoided. Experiments are presented along with a theoretical model to quantify expected improvement of sensitivity. The system is used to detect bacterial spores deposited on a surface with a single laser shot at unprecedented signal-to-noise ratio.
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 â¼100 kHz. This technique is based on a scanning micro-cavity resonator with a Finesse of â¼12,000 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.
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.
Spectrum Analysis, Raman , Spores, Bacterial , Spectrum Analysis, Raman/methods , Lasers , Vibration
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.
Spectrum Analysis, Raman , Ytterbium , Fructose , Glucose , Lasers , Spectrum Analysis, Raman/methods , Toluene
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.
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.
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.
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 â¼21. 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 â¼1.2 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.
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.
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.
We report on a Yb-pumped optical parametric oscillator (OPO) that delivers 30 fs pulses with spectral coverage from 680 to 910 nm and an average output power of up to 1.1 W. The resulting peak power is â¼0.5 MW, which is, to the best of our knowledge, the highest ever demonstrated in a femtosecond OPO. The intensity noise remains at a level of 0.2% rms, and rapid wavelength tuning is obtained by simply scanning the resonator length. The performances of the OPO are promising for a variety of applications in nonlinear microscopy and ultrafast spectroscopy.
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.
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.
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.
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.
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.
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.
An integrated single-sideband modulator is used as the sole wide-bandwidth frequency actuator in a Pound-Drever-Hall locking loop. Thanks to the large modulation bandwidth, the device enables a locking range of ±75 MHz and a control bandwidth of 5 MHz without the need for a second feedback loop. As applied to the coupling of an extended-cavity diode laser at 1.55 µm to a high-finesse optical cavity, the in-loop frequency noise spectral density reaches a minimum of 1 mHz/Hz(1/2) at 1 kHz.
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 â¼30 dB signal-to-noise ratio of the detected beat-note together with the achieved closed-loop locking bandwidth of â¼500 kHz allows for a residual integrated phase noise of 0.78 rad (1 Hz-5 MHz), for an ultimate resolution of â¼21 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).
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.
