Remote chemical detection in the atmosphere or some specific space has always been of great interest in many applications for environmental protection and safety. Laser absorption spectroscopy (LAS) is a highly desirable technology, benefiting from high measurement sensitivity, improved spectral selectivity or resolution, fast response and capability of good spatial resolution, multi-species and standoff detection with a non-cooperative target. Numerous LAS-based standoff detection techniques have seen rapid development recently and are reviewed herein, including differential absorption LiDAR, tunable laser absorption spectroscopy, laser photoacoustic spectroscopy, dual comb spectroscopy, laser heterodyne radiometry and active coherent laser absorption spectroscopy. An update of the current status of these various methods is presented, covering their principles, system compositions, features, developments and applications for standoff chemical detection over the last decade. In addition, a performance comparison together with the challenges and opportunities analysis is presented that describes the broad LAS-based techniques within the framework of remote sensing research and their directions of development for meeting potential practical use.

Standoff Chemical Detection Using Laser Absorption Spectroscopy: A Review

A transportable laser heterodyne radiometer (LHR) based on an external cavity quantum cascade laser, operating in the mid-infrared (mid-IR) around 8 µm, was developed for ground-based remote sensing of multiple greenhouse gases. A newly available novel flexible mid-IR polycrystalline fiber was first exploited to couple solar radiation, real-time captured using a portable sun-tracker, to the LHR receiver. Compared to free space coupling of sunlight, the technique usually used nowadays in the mid-IR, such fiber coupling configuration makes the LHR system readily more stable, simpler, and robust. Operation of the LHR with quasi-shot-noise limited performance was analyzed and experimentally achieved by optimizing local oscillator power. To the best of our knowledge, no such performance approaching the fundamental limit has been reported for a transportable LHR operating at a long mid-IR wavelength around 8 µm. CH4 and N2O were simultaneously measured in the atmospheric column using the developed mid-IR LHR. The experimental LHR spectrum of CH4 and N2O was compared and is in good agreement with a referenced Fourier-transform infrared spectrum from the Total Carbon Column Observing Network observation site and with a simulation spectrum from atmospheric transmission modeling.

Transportable mid-infrared laser heterodyne radiometer operating in the shot-noise dominated regime.

We have developed a portable near-infrared laser heterodyne radiometer (LHR) for quasi-simultaneous measurements of atmospheric carbon dioxide (CO2), methane (CH4), water vapor (H2O) and oxygen (O2) column absorption by using three distributed-feedback diode lasers as the local oscillators of the heterodyne detection. The developed system shows good performance in terms of its high spectral resolution of 0.066 cm-1 and a low solar power detection noise which was about 2 times the theoretical quantum limit. Its measurement precision of the column-averaged mole fraction for CO2 and CH4 is within 1.1%, based on the standard deviation from the mean value of the retrieved results for a clean sky. The column abundance information of the O2 is used to correct for the variations and uncertainties of atmosphere pressure, the solar altitude angle, and the prior profiles of pressure and temperature. Comparison measurements of daily column-averaged atmospheric mole fractions of CO2, CH4 and H2O, between our developed LHR and a greenhouse gas observing satellite, show a good agreement, which proves the reliability of our developed system.

Development of a laser heterodyne spectroradiometer for high-resolution measurements of CO 2 , CH 4 , H 2 O and O 2 in the atmospheric column

The performance of a mid-infrared laser heterodyne radiometer (MIR-LHR) based on a micro-electro-mechanical system (MEMS) mirror is demonstrated in ground-based solar occultation mode. A MEMS mirror is employed as an alternative modulator to the traditional mechanical chopper. High-resolution (∼0.0024 cm−1) transmission spectrum near 3.93 μm was obtained for atmospheric observation of N2O absorption. Operation of the MIR-LHR with laser-induced shot-noise limited performance was analyzed and experimentally achieved. The laser heterodyne spectrum obtained is consistent with Fourier-transform infrared (FT-IR) spectrometer and atmospheric transmission modeling. Compared to the traditional chopper, the MEMS mirror is smaller, lighter and lower power consumption which makes the system more stable and compact. The reported MIR-LHR in this article has great potential in aircraft instruments and satellite payloads.

MEMS Modulator-Based Mid-Infrared Laser Heterodyne Radiometer for Atmospheric Remote Sensing

We present the project of a 2U CubeSat format spaceborne multichannel laser heterodyne spectroradiometer (MLHS) for studies of the Earth’s atmosphere upper layers in the near-infrared (NIR) spectral range (1258, 1528, and 1640 nm). A spaceborne MLHS operating in the solar occultation mode onboard CubeSat platform, is capable of simultaneous vertical profiling of CO2, H2O, CH4, and O2, as well as Doppler wind measurements, in the tangent heights range of 5–50 km. We considered the low Earth orbit for the MLHS deployment and analyzed the expected surface coverage and spatial resolution during one year of operations. A ground-based prototype of the MLHS for CO2 and CH4 molecular absorption measurements with an ultra-high spectral resolution of 0.0013 cm−1 is presented along with the detailed description of its analytical characteristics and capabilities. Implementation of a multichannel configuration of the heterodyne receiver (four receivers per one spectral channel) provides a significant improvement of the signal-to-noise ratio with the reasonable exposure time typical for observations in the solar occultation mode. Finally, the capability of building up a tomographic picture of sounded gas concentration distributions provided by high spectral resolution is discussed.

A Concept of 2U Spaceborne Multichannel Heterodyne Spectroradiometer for Greenhouse Gases Remote Sensing

We present the design of a portable version of our miniaturized laser heterodyne radiometer (mini-LHR) that simultaneously measures methane (CH4) and carbon dioxide (CO2) in the atmospheric column. The mini-LHR fits on a backpack frame, operates autonomously, and requires no infrastructure because it is powered by batteries charged by a folding 30 W solar panel. Similar to our earlier instruments, the mini-LHR is a passive laser heterodyne radiometer that operates by collecting sunlight that has undergone absorption by CH4 and CO2. Within the mini-LHR, sunlight is mixed with light from a distributive feedback (DFB) laser centered at approximately 1.64 μm where both gases have absorption features. The laser scans across these absorption features roughly every minute and the resulting beat signal is collected in the radio frequency (RF). Scans are averaged into half hour and hour data products and analyzed using the Planetary Spectrum Generator (PSG) retrieval to extract column mole fractions. Instrument performance is demonstrated through two deployments at significantly different sites in interior Alaska and Hawaii. The resolving power (λ/∆λ) is greater than 500,000 at 1.64 μm with precisions of better than 20 ppb and 1 ppm for CH4 and CO2, respectively. Because mini-LHR instruments are portable and can be co-located, they can be used to characterize bias between larger, stationary, column observing instruments. In addition, mini-LHRs can be deployed quickly to respond to transient events such as methane leaks or can be used for field studies targeting geographical regions.

Z. Souders

Papers

A portable miniaturized laser heterodyne radiometer (mini‑LHR) for remote measurements of column CH 4 and CO 2 .