Reference-free dual-comb spectroscopy with inbuilt coherence.

We demonstrate a simple system for dual-comb spectroscopy based on two inherently coherent optical frequency combs generated via seeded parametric downconversion. The inbuilt coherence is established by making the two combs share a common comb line. We show that the inbuilt coherence makes it possible to use a simple numerical post-processing procedure to compensate for small drifts of the dual-comb interferogram arrival time and phase. This enables long-time coherent averaging of the interferograms.

Versatile optical frequency combs based on multi-seeded femtosecond optical parametric generation.

This study proposes and demonstrates a versatile method for near- and mid-infrared optical frequency comb generation using multi-seeded femtosecond optical parametric generation. The method allows one to divide the repetition rate by an arbitrarily large integer factor, freely tune the offset frequency, and adjust the common phase offset of the comb modes. Since all possible degrees of freedom are adjustable, the proposed method manifests itself as versatile optical frequency synthesis.

Terahertz radiation detection with a cantilever-based photoacoustic sensor.

We report the photoacoustic (PA) response in the terahertz (THz) range by employing a detection process actuated with a silicon cantilever pressure sensor and a carbon-based radiation absorber. The detection relies on the mechanical response of the cantilever, when the volume of the carrier gas inside the PA cell expands with the heat produced by the radiation absorber. The detector interferometrically monitors the movement of the cantilever sensor to generate the PA signal. We selected the absorber material with the highest THz responsivity for detailed studies at 1.4 THz (214 µm wavelength). The observed responsivities of two different radiation absorbers are nearly the same at 1.4 THz and agree within 10% with responsivity values at 0.633 µm wavelength. The results demonstrate the potential of covering with a single PA detector a broad spectral range with approximately constant responsivity, large dynamic range, and high damage threshold.

Optical power detector with broad spectral coverage, high detectivity, and large dynamic range.

Optical power measurements are needed in practically all technologies based on light. Here, we report a general-purpose optical power detector based on the photoacoustic effect. Optical power incident on the detector's black absorber produces an acoustic signal, which is further converted into an electrical signal using a silicon-cantilever pressure transducer. We demonstrate an exceptionally large spectral coverage from ultraviolet to far infrared, with the possibility for further extension to the terahertz region. The linear dynamic range of the detector reaches 80 dB, ranging from a noise-equivalent power of 6 n W/H z to 600 mW (independent of signal averaging time).

Mid-infrared frequency comb with 25 pJ threshold via CW-seeded optical parametric generation in nonlinear waveguide.

We demonstrate efficient generation of mid-infrared frequency combs based on continuous-wave-seeded femtosecond optical parametric generation in nonlinear waveguides. Conversion of the near-infrared pump to signal and idler light takes place with very high efficiency (74%), and the threshold (25 pJ for 100 fs pulses) is over 300 times lower than in bulk analogs. Relative intensity noise of the mid-infrared comb is exceptionally low, below 5×10-5 (integrated from 10 Hz to 2 MHz). Furthermore, the mid-infrared bandwidth can be increased by driving the process with a broadband pump obtained via supercontinuum generation.

Radiocarbon dioxide detection using cantilever-enhanced photoacoustic spectroscopy.

In this Letter, we report on the sub-parts-per-billion-level radiocarbon dioxide detection using cantilever-enhanced photoacoustic spectroscopy. The 14C/C ratio of samples is measured by targeting a 14CO2 absorption line with minimal interference from other CO2 isotopes. Using a quantum cascade laser as a light source allows for a compact experimental setup. In addition, measurements of sample gases with 14CO2 concentrations as low as 100 parts-per-trillion (ppt) are presented. The Allan deviation demonstrates a noise equivalent concentration of 30 ppt at an averaging time of 9 min. The achieved sensitivity validates this method as a suitable alternative to more complex optical detection methods for radiocarbon dioxide detection used so far, and it can be envisioned for future in situ radiocarbon detection.

Broadband Laser-Based Infrared Detector for Gas Chromatography.

Cantilever-enhanced photoacoustic spectroscopy coupled with gas chromatography is used to quantitatively analyze a mixture of alcohols in a quasi-online manner. A full identification and quantification of all analytes are achieved based on their spectral fingerprints using a widely tunable continuous-wave laser as a light source. This can be done even in the case of interfering column/septum bleed or simultaneously eluted peaks. The combination of photoacoustic spectroscopy and gas chromatography offers a viable solution for compact and portable instruments in applications that require straightforward analyses with no consumables.

Broadband photoacoustic spectroscopy of CH414 with a high-power mid-infrared optical frequency comb.

We report a photoacoustic spectroscopy setup with a high-power mid-infrared frequency comb as the light source. The setup is used in broadband spectroscopy of radiocarbon methane. Owing to the high sensitivity of a cantilever-enhanced photoacoustic cell and the high-power light source, we can reach a detection limit below 100 ppb in a broadband measurement with a sample volume of only a few milliliters. The first infrared spectrum of CH414 is reported and given a preliminary assignment. The results lay a foundation for the development of optical detection systems for radiocarbon methane.

Cavity-enhanced cantilever-enhanced photo-acoustic spectroscopy.

We have improved the sensitivity of a state-of-the-art cantilever-enhanced photo-acoustic trace gas sensor by combining it with an optical power build-up cavity. The build-up cavity enhances the photo-acoustic signal by a factor of ∼100, resulting in an exceptionally good normalised noise equivalent absorption (NNEA) value of 1.75 × 10-12 W cm-1 Hz-1/2. We demonstrate the sensor platform in the 1530 nm wavelength range with a simple distributed feedback diode laser, achieving 75 ppt sensitivity for C2H2 with a 10 s integration time.

Step-modulated decay cavity ring-down detection for double resonance spectroscopy.

A method of measuring double resonant two-photon signal and background from a single cavity ring-down decay is introduced. This is achieved by modulating the double resonance loss via one of the light sources exciting the transition. The noise performance of the method is characterized theoretically and experimentally. The addition of a new parameter to the fitting function introduces a minor noise increase due to parameter correlation. However, the concurrent recording of the background can extend the stable measurement time. Alternatively, the method allows a faster measurement speed, while still recording the background, which is often advantageous in double resonance measurements. Finally, the method is insensitive to changes in the cavity decay rate at short timescales and can lead to improved performance if they have significant contribution to the final noise level compared to the detector noise.

Optical frequency comb photoacoustic spectroscopy.

We report the first photoacoustic detection scheme using an optical frequency comb-optical frequency comb photoacoustic spectroscopy (OFC-PAS). OFC-PAS combines the broad spectral coverage and the high resolution of OFCs with the small sample volume of cantilever-enhanced PA detection. In OFC-PAS, a Fourier transform spectrometer (FTS) is used to modulate the intensity of the exciting comb source at a frequency determined by its scanning speed. One of the FTS outputs is directed to the PA cell and the other is measured simultaneously with a photodiode and used to normalize the PA signal. The cantilever-enhanced PA detector operates in a non-resonant mode, enabling detection of a broadband frequency response. The broadband and the high-resolution capabilities of OFC-PAS are demonstrated by measuring the rovibrational spectra of the fundamental C-H stretch band of CH4, with no instrumental line shape distortions, at total pressures of 1000 mbar, 650 mbar, and 400 mbar. In this first demonstration, a spectral resolution two orders of magnitude better than previously reported with broadband PAS is obtained, limited by the pressure broadening. A limit of detection of 0.8 ppm of methane in N2 is accomplished in a single interferogram measurement (200 s measurement time, 1000 MHz spectral resolution, 1000 mbar total pressure) for an exciting power spectral density of 42 µW/cm-1. A normalized noise equivalent absorption of 8 × 10-10 W cm-1 Hz-1/2 is obtained, which is only a factor of three higher than the best reported with PAS based on continuous wave lasers. A wide dynamic range of up to four orders of magnitude and a very good linearity (limited by the Beer-Lambert law) over two orders of magnitude are realized. OFC-PAS extends the capability of optical sensors for multispecies trace gas analysis in small sample volumes with high resolution and selectivity.

Fully stabilized mid-infrared frequency comb for high-precision molecular spectroscopy.

A fully stabilized mid-infrared optical frequency comb spanning from 2.9 to 3.4 µm is described in this article. The comb is based on half-harmonic generation in a femtosecond optical parametric oscillator, which transfers the high phase coherence of a fully stabilized near-infrared Er-doped fiber laser comb to the mid-infrared region. The method is simple, as no phase-locked loops or reference lasers are needed. Precise locking of optical frequencies of the mid-infrared comb to the pump comb is experimentally verified at sub-20 mHz level, which corresponds to a fractional statistical uncertainty of 2 × 10-16 at the center frequency of the mid-infrared comb. The fully stabilized mid-infrared comb is an ideal tool for high-precision molecular spectroscopy, as well as for optical frequency metrology in the mid-infrared region, which is difficult to access with other stabilized frequency comb techniques.

Frequency comb assisted two-photon vibrational spectroscopy.

We report a setup for high-resolution two-photon spectroscopy using a mid-infrared continuous wave optical parametric oscillator (CW-OPO) and a near-infrared diode laser as the excitation sources, both of which are locked to fully stabilized optical frequency combs. The diode laser is directly locked to a commercial near-infrared optical frequency comb using an optical phase-locked loop. The near-infrared frequency comb is also used to synchronously pump a degenerate femtosecond optical parametric oscillator to produce a fully stabilized mid-infrared frequency comb. The beat frequency between the mid-infrared comb and the CW-OPO is then stabilized through frequency locking. We used the setup to measure a double resonant two-photon transition to a symmetric vibrational state of acetylene with a sub-Doppler resolution and high signal-to-noise ratio.

Stabilization of femtosecond optical parametric oscillators for infrared frequency comb generation.

A synchronously pumped optical parametric oscillator (SP-OPO) is one of the most common techniques to generate femtosecond frequency combs in the mid-infrared region. Stable long-term operation of an SP-OPO requires active locking of the OPO resonator round-trip time to the pump pulse interval. A simple modulation-free locking method based on stabilization of narrow-band frequency-doubled power of the SP-OPO output comb is demonstrated in this Letter. The method relies on the strong dependency of frequency-doubled power on spectral shape of the comb, leading to better stability of the comb envelope spectrum than the commonly used dither-and-lock method.

Parts-per-trillion-level detection of nitrogen dioxide by cantilever-enhanced photo-acoustic spectroscopy.

We present a simple and highly sensitive cantilever-enhanced photo-acoustic sensor for detection of nitrogen dioxide. A noise equivalent detection limit of 50 parts-per-trillion in 1 s is demonstrated. The limit was reached with an average optical power of 4.7 W using a continuous-wave laser at 532 nm. The achieved normalized noise equivalent absorption coefficient was 2.6×10(-10) W cm(-1) Hz(-1/2).

High-power mid-infrared frequency comb from a continuous-wave-pumped bulk optical parametric oscillator.

We demonstrate that it is possible to obtain a mid-infrared optical frequency comb (OFC) experimentally by using a continuous-wave-pumped optical parametric oscillator (OPO). The comb is generated without any active modulation. It is based on cascading quadratic nonlinearities that arise from intra-cavity phase mismatched second harmonic generation of the signal wave that resonates in the OPO. The generated OFC is transferred from the signal wavelength (near-infrared) to the idler wavelength (mid-infrared) by intracavity difference frequency generation between the OPO pump wave and the signal comb. We have produced a mid-infrared frequency comb which is tunable from 3.0 to 3.4 µm with an average output power of up to 3.1 W.

Frequency-comb-referenced mid-infrared source for high-precision spectroscopy.

We report on a tunable continuous-wave mid-infrared optical parametric oscillator (OPO), which is locked to a fully stabilized near-infrared optical frequency comb using a frequency doubling scheme. The OPO is used for 40 GHz mode-hop-free, frequency-comb-locked scans in the wavelength region between 2.7 and 3.4 µm. We demonstrate the applicability of the method to high-precision cavity-ring-down spectroscopy of nitrous oxide (N2O) and water (H2O) at 2.85 µm and of methane (CH4) at 3.2 µm.

Frequency-comb-referenced tunable diode laser spectroscopy and laser stabilization applied to laser cooling.

Laser cooling of trapped atoms and ions in optical clocks demands stable light sources with precisely known absolute frequencies. Since a frequency comb is a vital part of any optical clock, the comb lines can be used for stabilizing tunable, user-friendly diode lasers. Here, a light source for laser cooling of trapped strontium ions is described. The megahertz-level stability and absolute frequency required are realized by stabilizing a distributed-feedback semiconductor laser to a frequency comb. Simple electronics is used to lock and scan the laser across the comb lines, and comb mode number ambiguities are resolved by using a separate, saturated absorption cell that exhibits easily distinguishable hyperfine absorption lines with known frequencies. Due to the simplicity, speed, and wide tuning range it offers, the employed technique could find wider use in precision spectroscopy.

High sensitivity trace gas detection by cantilever-enhanced photoacoustic spectroscopy using a mid-infrared continuous-wave optical parametric oscillator.

Highly sensitive cantilever-enhanced photoacoustic detection of hydrogen cyanide and methane in the mid-infrared region is demonstrated. A mid-infrared continuous-wave frequency tunable optical parametric oscillator was used as a light source in the experimental setup. Noise equivalent detection limits of 190 ppt (1 s) and 65 ppt (30 s) were achieved for HCN and CH(4), respectively. The normalized noise equivalent absorption coefficient is 1.8 × 10(-9) W cm(-1) Hz(-1/2).

Frequency comb generation by a continuous-wave-pumped optical parametric oscillator based on cascading quadratic nonlinearities.

We report optical frequency comb generation by a continuous-wave pumped optical parametric oscillator (OPO) without any active modulation. The OPO is configured as singly resonant with an additional nonlinear crystal (periodically poled MgO:LiNbO3) placed inside the OPO for phase mismatched second harmonic generation (SHG) of the resonating signal beam. The phase mismatched SHG causes cascading χ(2) nonlinearities, which can substantially increase the effective χ(3) nonlinearity in MgO:LiNbO3, leading to spectral broadening of the OPO signal beam via self-phase modulation. The OPO generates a stable 4 THz wide (-30 dB) frequency comb centered at 1.56 µm.