Dual-comb Spectroscopy Research Articles

Absolute angular position measurement by dual-comb spectroscopy of an autocollimation diffracted beam.

The dual-comb technique is a powerful tool in industrial inspection and scientific research and is capable of realizing ultrahigh-resolution and fast broadband spectral measurements. We propose an absolute angular-position measurement method based on dual-comb spectroscopy. With a simple layout, the absolute angular position can be naturally determined through the traceable and wide-amplitude spectra of the autocollimation diffracted beams of the target grating. We experimentally demonstrate that a precision of 0.12 arcsec in the dynamic range of approximately 6660 arcsec, along with a 1 kHz repetition rate difference, is achieved. Compared with a commercial autocollimator, over 1000 arcsec, the comparison residuals are kept within ±0.3 arcsec.

Measurement of 24-h continuous human CH4 release in a whole room indirect calorimeter.

We describe the technology and validation of a new whole room indirect calorimeter (WRIC) methodology to quantify volume of methane (VCH4) released from the human body over 24 h concurrently with the assessment of energy expenditure and substrate utilization. The new system extends the assessment of energy metabolism by adding CH4, a downstream product of microbiome fermentation that could contribute to energy balance. Our new system consists of an established WRIC combined with the addition of off-axis integrated-cavity output spectroscopy (OA-ICOS) to measure CH4 concentration ([CH4]). Development, validation, and reliability of the system included environmental experiments to measure the stability of the atmospheric [CH4], infusing CH4 into the WRIC and human cross-validation studies comparing [CH4] quantified by OA-ICOS and mid-infrared dual-comb spectroscopy (MIR DCS).Our infusion data indicated that the system measured 24-h [CH4] and VCH4 with high sensitivity, reliability, and validity. Cross-validation studies showed good agreement between OA-ICOS and MIR DCS technologies (r = 0.979, P < 0.0001). Human data revealed 24-h VCH4 was highly variable between subjects and within/between days. Finally, our method to quantify VCH4 released by breath or colon suggested that over 50% of the CH4 was eliminated through the breath. The method allows, for the first time, measurement of 24-h VCH4 (in kcal) and therefore the measurement of the proportion of human energy intake fermented to CH4 by the gut microbiome and released via breath or from the intestine; also, it allows us to track the effects of dietary, probiotic, bacterial, and fecal microbiota transplantation on VCH4.NEW & NOTEWORTHY This is the first time that continuous assessment of CH4 is reported in parallel with measurements of O2 consumption and CO2 production inside a whole room indirect calorimeter in humans and over 24 h. We provide a detailed description of the whole system and its parts. We carried out studies of reliability and validity of the whole system and its parts. CH4 is released in humans during daily activities.

Precision dual-comb spectroscopy using wavelength-converted frequency combs with low repetition rates

Precision spectroscopy contributed significantly to the development of quantum mechanics in its early stages. In the twenty-first century, precision spectroscopy has played an important role in several fields, including fundamental physics, precision measurement, environmental monitoring, and medical diagnostics. An optical frequency comb is indispensable in determining the frequency axis in precision spectroscopy and it is useful as a light source for spectroscopy. Dual-comb spectroscopy uses two frequency combs with slightly different repetition rates and has the potential to surpass conventional Fourier-transform infrared spectrometers. The resolution of dual-comb spectroscopy is limited by the frequency spacing of the comb components, that is, the repetition rate of the comb. We demonstrate dual-comb spectroscopy in the visible-wavelength region using wavelength-converted frequency combs from Er-doped fiber combs. The repetition rates of the combs are relatively low at 19.8 MHz, resulting in relatively high resolution in the dual-comb spectroscopy. The observed spectral shape in dual-comb spectroscopy agrees well with the fitting result based on the hyperfine structure of molecular iodine. The realized dual-comb spectroscopy using wavelength-converted Er-doped fiber combs is reliable (maintenance free) and applicable in other experiments at visible wavelengths.

Coherently averaged dual-comb spectroscopy with a low-noise and high-power free-running gigahertz dual-comb laser.

We present a new type of dual optical frequency comb source capable of scaling applications to high measurement speeds while combining high average power, ultra-low noise operation, and a compact setup. Our approach is based on a diode-pumped solid-state laser cavity which includes an intracavity biprism operated at Brewster angle to generate two spatially-separated modes with highly correlated properties. The 15-cm-long cavity uses an Yb:CALGO crystal and a semiconductor saturable absorber mirror as an end mirror to generate more than 3 W average power per comb, below 80 fs pulse duration, a repetition rate of 1.03 GHz, and a continuously tunable repetition rate difference up to 27 kHz. We carefully investigate the coherence properties of the dual-comb by a series of heterodyne measurements, revealing several important features: (1) ultra-low jitter on the uncorrelated part of the timing noise; (2) the radio frequency comb lines of the interferograms are fully resolved in free-running operation; (3) we validate that through a simple measurement of the interferograms we can determine the fluctuations of the phase of all the radio frequency comb lines; (4) this phase information is used in a post-processing routine to perform coherently averaged dual-comb spectroscopy of acetylene (C2H2) over long timescales. Our results represent a powerful and general approach to dual-comb applications by combining low noise and high power operation directly from a highly compact laser oscillator.

Validation of open-path dual-comb spectroscopy against an O2 background.

Dual-comb spectroscopy measures greenhouse gas concentrations over kilometers of open air with high precision. However, the accuracy of these outdoor spectra is challenging to disentangle from the absorption model and the fluctuating, heterogenous concentrations over these paths. Relative to greenhouse gases, O2 concentrations are well-known and evenly mixed throughout the atmosphere. Assuming a constant O2 background, we can use O2 concentration measurements to evaluate the consistency of open-path dual-comb spectroscopy with laboratory-derived absorption models. To this end, we construct a dual-comb spectrometer spanning 1240 nm to 1700nm, which measures O2 absorption features in addition to CO2 and CH4. O2 concentration measurements across a 560 m round-trip outdoor path reach 0.1% precision in 10 minutes. Over seven days of shifting meteorology and spectrometer conditions, the measured O2 has -0.07% mean bias, and 90% of the measurements are within 0.4% of the expected hemisphere-average concentration. The excursions of up to 0.4% seem to track outdoor temperature and humidity, suggesting that accuracy may be limited by the O2 absorption model or by water interference. This simultaneous O2, CO2, and CH4 spectrometer will be useful for measuring accurate CO2 mole fractions over vertical or many-kilometer open-air paths, where the air density varies.

Absolute frequency referencing for swept dual-comb spectroscopy with midinfrared quantum cascade lasers

A scheme to calibrate a frequency-swept frequency comb against a reference laser is developed. Its application to a dual-comb spectrometer based on midinfrared quantum cascade lasers results in molecular spectra with high-frequency accuracy at fast refresh rates.

Sub-100 fs watt-level Kerr-lens mode-locked Yb:CaYAlO4 laser with a gigahertz repetition rate

We report a 1.04 GHz high-power Kerr-lens mode-locked Yb:CaYAlO4 laser pumped by a single-mode fiber laser at 976 nm. Based on a bow-tie cavity, stable unidirectional mode-locked operation is obtained with an output coupler of 1.6%. The oscillator delivers pulses with an average power of 1.46 W and with the pulse duration of 99 fs, which, to the best of our knowledge, is the first gigahertz-level Kerr-lens mode-locked laser based on the Yb:CaYAlO4 gain medium. We believe that the watt-level solid-state femtosecond laser at GHz would be an excellent source for developing time-resolved broadband dual-comb spectroscopy.

An Investigation of All Fiber Free-Running Dual-Comb Spectroscopy.

A dual-comb spectroscopy (DCS) system uses two phase-locked optical frequency combs with a slight difference in the repetition frequency. The spectrum can be sampled in the optical frequency (OF) domain and reproduces the characteristics in the radio frequency (RF) domain through asynchronous optical sampling. Therefore, the DCS system shows great advantages in achieving precision spectral measurement. During application, the question of how to reserve the mutual coherence between the two combs is the key issue affecting the application of the DCS system. This paper focuses on a software algorithm used to realize the mutual coherence of the two combs. Therefore, a pair of free-running large anomalous dispersion fiber combs, with a center wavelength of approximately 1064 nm, was used. After the signal process, the absorption spectra of multiple species were simultaneously obtained (simulated using the reflective spectra of narrow-bandwidth fiber Bragg gratings, abbreviated as FBG). The signal-to-noise ratio (SNR) could reach 13.97 dB (25) during the 100 ms sampling time. In this study, the feasibility of the system was first verified through the simulation system; then, a principal demonstration experiment was successfully executed. The whole system was connected by the optical fiber without additional phase-locking equipment, showing promise as a potential solution for the low-cost and practical application of DCS systems.

Fast dual-comb spectroscopy based on a dual-wavelength all-fiber ring laser with high repetition rate

We demonstrate fast dual-comb spectroscopy based on a high-repetition-rate dual-wavelength erbium-doped fiber laser with a large repetition rate difference. It can operate in three different dual-wavelength states with repetition rate differences of 4.32, 2.74 and 3.635 kHz, respectively. To the best of our knowledge, the corresponding refresh time can be as low as 231 μs, which is the fastest in dual-comb spectroscopy using a single fundamentally mode-locked all-fiber laser. The high repetition rate of approximately 154.68 MHz provides a maximum optical frequency bandwidth of 4.37 THz. Dual-comb spectroscopy was used to measure the transmittance curve of the Fabry–Perot etalon.

Feasibility of dual comb spectroscopy in the UV range using a free-running, bidirectional ring titanium sapphire laser

We show that our developed free-running, bidirectional ring Ti:Sa laser cavity meets the requirements for Dual Comb Spectroscopy in the UV range (UV-DCS). Two counter-propagative frequency combs with slightly different repetition rate are generated in such a cavity and we show quantitatively that this repetition rate difference can be explained by the self-steepening effect. Molecular absorption lines of the O2 A-band centered around 760~nm are measured with a 1,5 GHz spectral resolution, demonstrating that the mutual coherence of the two combs allows GHz-resolution DCS measurements. Moreover, we demonstrate that the generated output peak power allows for efficient second harmonic generation (SHG), in the scope of developing laboratory and open-path UV-DCS experiments.

L-band dual-comb based on gain-switched lasers for CO2 monitoring

This paper reports the development of a dual-comb spectroscopy system based on gain-switched single-mode laser diodes emitting at 1572 nm. The switching is performed by a train of short electrical pulses at a repetition rate of 100 MHz while the lasers are subjected to external optical injection. Under these conditions, broad and Hat optical frequency combs (OFC) are generated, showing 500 tones within 10 dB and a line spacing fix ed by the repetition rate of the swi tching pulses. The dual-comb gene rated by th e interference of two such combs with slightly different line spacing, is used for measuring the absorption line of CO2 at 1572.02 nm. The transmission spectrum is analyzed and fitted to a Voigt profile. A deviation of 3% in the residuals of the fitting is obtained, denoting the high spectral performance of the spectroscopy system.

Dual-comb spectrometer in the two-micron region using a new design of dispersion-controlled highly nonlinear fibre

We present here an experimental demonstration of dual-comb spectroscopy performed around 2 µm, with the use of a new design of dispersion-controlled highly nonlinear fibre. The latter allows us to efficiently convert light via a four-wave mixing process from 1.55 µm to 2 µm, which is a spectral region suited for the detection of pollutants such as CO2 or N2O. Experimental measurements have been performed with these two molecules and show an excellent agreement with the HITRAN database.

Quantum cascade laser frequency comb locked with 200 mrad residual phase noise

Using near-infrared light, we tightly-lock a mid-infrared quantum cascade laser frequency comb to another laser, achieving a residual integrated phase noise of 200 mrad. This high coherence is pertinent for highly-sensitive dual-comb spectroscopy and metrology.

1 GHz electro-optical silicon-germanium modulator in the 5-9 µm wavelength range.

Spectroscopy in the mid-infrared (mid-IR) wavelength range is a key technique to detect and identify chemical and biological substances. In this context, the development of integrated optics systems paves the way for the realization of compact and cost-effective sensing systems. Among the required devices, an integrated electro-optical modulator (EOM) is a key element for advanced sensing circuits exploiting dual comb spectroscopy. In this paper, we have experimentally demonstrated an integrated EOM operating in a wide wavelength range, i.e. from 5 to 9 µm at radio frequency (RF) as high as 1 GHz. The modulator exploits the variation of free carrier absorption in a Schottky diode embedded in a graded silicon germanium (SiGe) photonic waveguide.

Flat Top Optical Frequency Combs Based on a Single-Core Quantum Cascade Laser at Wavelength of ∼ 8.7 μm

We present optical frequency combs with a spectral emission of 48 cm−1 and an output power of 420 mW based on a single-core quantum cascade laser at λ ∼ 8.7 μm. A flat top spectrum sustains up to 130 comb modes delivering ∼ 3.2 mW of optical power per mode, making it a valuable tool for dual comb spectroscopy. The homogeneous gain medium, relying on a slightly diagonal bound-to-continuum structure, promises to provide a broad and stable gain for comb operating. Remarkably, the dispersion of this device is measured within 300 fs2/mm to ensure stable comb operation over 90% of the total current range. The comb is observed with a narrow beatnote linewidth around 2 kHz and has weak dependence on the applied current for stable comb operation.

Flat top optical frequency combs based on a single-core quantum cascade laser at the wavelength of ~8.7 μm

Abstract We present optical frequency combs with a spectral emission of 48 cm-1 and an output power of 420 mW based on a single-core quantum cascade laser at λ~8.7 μm. A flat top spectrum sustains up to 130 comb modes delivering ~3.2 mW of optical power per mode, making it a valuable tool for dual comb spectroscopy. The homogeneous gain medium, relying on a slightly-diagonal bound-to-continuum structure, promises to provide broad and stable gain for comb operating. Remarkably, the dispersion of this device is measured within 300 fs2/mm to ensure stable comb operation over 90% of the total current range. The comb is observed with a narrow beatnote linewidth around 2 kHz and has weak dependence on the applied current for stable comb operation.

Dual-comb spectroscopy using free-running mechanical sharing dual-comb fiber lasers

We demonstrate balanced-detection dual-comb spectroscopy using two free-running mechanical sharing dual-comb fiber lasers assisted by an all-computational digital phase correction algorithm. The mutual coherence between the combs allows us perform mode-resolved spectroscopy of gaseous hydrogen cyanide by digitally compensating residual timing and offset frequency fluctuations of the dual-comb signal. Setting the repetition rate difference between the combs to 500 Hz (1.5 kHz) yields more than 2000 resolved radio frequency comb lines after phase correction in a 3-dB bandwidth centered at 1560 nm of wavelength. Through coadding the corrected interferograms, we obtain a single time-domain trace with a signal-to-noise ratio (SNR) of 6378 (13 960) and 12.64 (13.77) bits of dynamic range in 1 s of averaging. The spectral SNR of the coadded trace reaches 529 (585), corresponding to a figure of merit of SNR of 1.3 × 106 (1.4 × 106). The measured absorption spectrum of hydrogen cyanide agrees well with the HITRAN database.

Black Arsenic-Phosphorus Nanosheets for Highly Responsive Photodetection and Dual-Wavelength Ultrafast Pulse Generation at Telecommunication Bands.

Black arsenic-phosphorus (b-AsP), an alloy containing black phosphorus and arsenic in the form of b-AsxP1-x, has a broadly tunable band gap changing with the chemical ratios of As and P. Although mid-infrared photodetectors and mode-locked or Q-switched pulse lasers based on b-AsP (mostly b-As0.83P0.17) are investigated, the potential of this family of materials for near-infrared photonic and optoelectronic applications at telecommunication bands is not fully explored. Here, we have verified a multifunctional fiber device based on b-As0.4P0.6 nanosheets for highly responsive photodetection and dual-wavelength ultrafast pulse generation at around 1550 nm. The fiber laser with a saturable absorber (SA) based on b-As0.4P0.6 nanosheets can output dual-wavelength mode-locking pulses with a larger bandwidth and spectral separation than those based on other two-dimensional (2D) materials. Remarkably, it is found that the b-As0.4P0.6-based photodetector can achieve a high responsivity of 10,200 A/W at 1550 nm and a peak responsivity of 2.29 × 105 A/W at 980 nm. Our work suggests that b-As0.4P0.6 shows great potential in ultrafast photonics, dual-comb spectroscopy, and infrared signal detection.

Hybrid integrated mode-locked laser using a GaAs-based 1064 nm gain chip and a SiN external cavity.

External cavity mode-locked lasers could be used as comb sources for high volume application such as LIDAR and dual comb spectroscopy. Currently demonstrated chip scale integrated mode-locked lasers all operate in the C-band. In this paper, a hybrid-integrated external cavity mode-locked laser working at 1064 nm is demonstrated, a wavelength beneficial for optical coherence tomography or Raman spectroscopy applications. Additionally, optical injection locking is demonstrated, showing an improvement in the optical linewidth, and an increased stability of the comb spectrum.

High-sensitivity frequency comb carrier-envelope-phase metrology in solid state high harmonic generation

Non-perturbative and phase-sensitive light–matter interactions have led to the generation of attosecond pulses of light and the control of electrical currents on the same time scale. Traditionally, probing these effects via high harmonic generation has involved complicated lasers and apparatuses to generate the few-cycle and high peak power pulses needed to obtain and measure spectra that are sensitive to the phase of the light wave. Instead, we show that nonlinear effects dependent on the carrier-envelope phase can be accessed in solid state crystals with simple, low pulse energy frequency combs that we combine with high-sensitivity demodulation techniques to measure harmonic spectral modulations. Central to this advance is the use of a scalable 100 MHz erbium-fiber frequency comb at 1550 nm to produce 12 nJ, 20 fs pulses that are focused to the T W / c m 2 level. In a single pass through a 500 µm ZnO crystal, this yields harmonic spectra extending down to 200 nm. With this system, we introduce a technique of carrier-envelope amplitude modulation spectroscopy (CAMS) and use it to characterize the phase-sensitive modulation of the ultraviolet harmonics with an 85 dB signal-to-noise ratio. We further verify the non-perturbative nature of the harmonic generation through polarization gating of the driving pulse to increase the effects of the carrier-envelope phase. This work demonstrates robust and ultra-sensitive methods for generating and characterizing harmonic generation at 100 MHz rates that should provide advantages in the study of attosecond nonlinear processes in solid state systems. Additionally, as a simple and low-noise frequency comb, this broadband source will be useful for precision dual-comb spectroscopy of a range of physical systems across the ultraviolet and visible spectral regions (200–650 nm).