Aleksandra Foltynowicz

Mid-infrared Fourier transform spectroscopy with a broadband frequency comb

Optical frequency-comb-based-high-resolution spectrometers offer enormous potential for spectroscopic applications. Although various implementations have been demonstrated, the lack of suitable mid-infrared comb sources has impeded explorations of molecular fingerprinting. Here we present for the first time a frequency-comb Fourier transform spectrometer operating in the 2100-to-3700-cm-1 spectral region that allows fast and simultaneous acquisitions of broadband absorption spectra with up to 0.0056 cm-1 resolution. We demonstrate part-per-billion detection limits in 30 seconds of integration time for various important molecules including methane, ethane, isoprene, and nitrous oxide. Our system enables precise concentration measurements even in gas mixtures that exhibit continuous absorption bands, and it allows detection of molecules at levels below the noise floor via simultaneous analysis of multiple spectral features. This system represents a near real-time, high-resolution, high-bandwidth mid-infrared spectrometer which is ready to replace traditional Fourier transform spectrometers for many applications in trace gas detection, atmospheric science, and medical diagnostics.We present a first implementation of optical-frequency-comb-based rapid trace gas detection in the molecular fingerprint region in the mid-infrared. Near-real-time acquisition of broadband absorption spectra with 0.0056 cm(-1) maximum resolution is demonstrated using a frequency comb Fourier transform spectrometer which operates in the 2100-to-3700-cm(-1) spectral region. We achieve part-per-billion detection limits in 30 seconds of integration time for several important molecules including methane, ethane, isoprene, and nitrous oxide. Our system enables precise concentration measurements even in gas mixtures that exhibit continuous absorption bands, and it allows detection of molecules at levels below the noise floor via simultaneous analysis of multiple spectral features.

Quantum-noise-limited optical frequency comb spectroscopy.

We achieve a quantum-noise-limited absorption sensitivity of 1.7×10(-12) cm(-1) per spectral element at 400 s of acquisition time with cavity-enhanced frequency comb spectroscopy, the highest demonstrated for a comb-based technique. The system comprises a frequency comb locked to a high-finesse cavity and a fast-scanning Fourier transform spectrometer with an ultralow-noise autobalancing detector. Spectra with a signal-to-noise ratio above 1000 and a resolution of 380 MHz are acquired within a few seconds. The measured absorption line shapes are in excellent agreement with theoretical predictions.

Fiber-laser-based noise-immune cavity-enhanced optical heterodyne molecular spectrometry for Doppler-broadened detection of C2H2 in the parts per trillion range

Noise-immune cavity-enhanced optical heterodyne molecular spectro-metry (NICE-OHMS) is one of the most sensitive laser-based absorption techniques. The high sensitivity of NICE-OHMS is obtained by ...

Theoretical description of Doppler-broadened noise-immune cavity-enhanced optical heterodyne molecular spectroscopy under optically saturated conditions

A theoretical description of Doppler-broadened noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) under optically saturated conditions is presented. Expressions for ...

Optical frequency comb spectroscopy.

Optical frequency combs offer enormous potential in the detection and control of atoms and molecules by combining their vast spectral coverage with the extremely high spectral resolution of each individual comb component. Sensitive and multiplexed trace gas detection via cavity-enhanced direct frequency comb spectroscopy has been demonstrated for various molecules and applications; however, previous demonstrations have been confined to the visible and near-infrared wavelength range. Future spectroscopic capabilities are created by developing comb sources and spectrometers for the deep ultraviolet and mid-infrared spectral regions. Here we present a broadband high resolution mid-infrared frequency comb-based Fourier transform spectrometer operating in the important molecular fingerprint spectral region of 2100-3600 cm(-1) (2.8-4.8 microm). The spectrometer, employing a multipass cell, allows simultaneous acquisition of broadband, high resolution spectra (down to 0.0035 cm(-1) of many molecular species at concentrations in the part-per-billion range in less than 1 min acquisition time. The system enables precise measurements of concentration even in gas mixtures that exhibit continuous absorption bands. The current sensitivity, 2 x 10(-8) cm(-1) Hz-1/2 per spectral element, is expected to improve by two orders of magnitude with an external enhancement cavity. We have demonstrated this sensitivity increase by combining cavity-enhanced frequency comb spectroscopy with a scanning Fourier transform spectrometer in the near-infrared region and achieving a sensitivity of 4.7 x 10(-10) cm(-1) Hz(-1/2). A cavity-enhanced mid-infrared comb spectrometer will provide a near real-time, high sensitivity, high resolution, precisely frequency calibrated, broad bandwidth system for many applications.

Characterization of fiber-laser-based sub-Doppler NICE-OHMS for quantitative trace gas detection.

The potential of fiber-laser-based sub-Doppler noise-immune cavity-enhanced optical heterodyne molecular spectrometry for trace gas detection is scrutinized. The non-linear dependence of the on-resonance sub-Doppler dispersion signal on the intracavity pressure and power is investigated and the optimum conditions with respect to these are determined. The linearity of the signal strength with concentration is demonstrated and the dynamic range of the technique is discussed. Measurements were performed on C(2)H(2) at 1531 nm up to degrees of saturation of 100. The minimum detectable sub-Doppler optical phase shift was 5 x 10(-11) cm(-1) Hz(-1/2), corresponding to a partial pressure of C(2)H(2) of 1 x 10(-12) atm for an intracavity pressure of 20 mTorr, and a concentration of 10 ppb at 400 mTorr.

Sub-Doppler dispersion and noise-immune cavity-enhanced optical heterodyne molecular spectroscopy revised

An expression for the peak-to-peak sub-Doppler optical phase shift of two counter-propagating modes of light, to which the noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NI ...

Doppler-broadened fiber-laser-based NICE-OHMS — Improved detectability

The performance of fiber-laser-based noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) has been improved by elimination of the technical constraints that limited its first demonstration. Doppler-broadened detection of C(2)H(2) and CO(2) at ~1531 nm is demonstrated using a cavity with a finesse of 4800. Frequency and wavelength modulated detection at absorption and dispersion phase are compared and the optimum mode of detection is discussed. A minimum detectable absorption of 8 x 10-(11) cm(-1), which corresponds to a detection limit of 4.5 ppt (2 ppt.m) for C(2)H(2), was obtained for an acquisition time of 0.7 s by lineshape fitting. The linearity of the pressure dependence of the signal strengths is investigated for both C(2)H(2) and CO(2).

Surpassing the path-limited resolution of Fourier-transform spectrometry with frequency combs

We overcome the resolution limit of Fourier-transform spectrometry and measure instrumental line-shape-free broadband molecular spectra with lines narrower than the optical path-limited resolution. ...

Doppler-broadened noise-immune cavity-enhanced optical heterodyne molecular spectrometry signals from optically saturated transitions under low pressure conditions

The influence of optical saturation on noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) signals from purely Doppler-broadened transitions is investigated experimen ...