Research done by the Infrared Photonics team at Pacific Northwest National Laboratory (PNNL) is focused on developing miniaturized integrated optics for mid-wave infrared (MWIR) and long-wave infrared (LWIR) sensing applications by exploiting the unique optical and material properties of chalcogenide glass. PNNL has developed thin-film deposition capabilities, direct laser writing techniques, infrared photonic device demonstration, holographic optical element design and fabrication, photonic device modeling, and advanced optical metrology—all specific to chalcogenide glass. Chalcogenide infrared photonics provides a pathway to quantum cascade laser (QCL) transmitter miniaturization. QCLs provide a viable infrared laser source for a new class of laser transmitters capable of meeting the performance requirements for a variety of national security sensing applications. The high output power, small size, and superb stability and modulation characteristics of QCLs make them amenable for integration as transmitters into ultra-sensitive, ultra-selective point sampling and remote short-range chemical sensors that are particularly useful for nuclear nonproliferation missions. During FY 2005, PNNL’s Infrared Photonics research team made measurable progress exploiting the extraordinary optical and material properties of chalcogenide glass to develop miniaturized integrated optics for mid-wave infrared (MWIR) and long-wave infrared (LWIR) sensing applications. We investigated sulfur purification methods that will eventually lead to routine production of optical quality chalcogenide glass. We also discovered a glass degradation phenomenon and our investigation uncovered the underlying surface chemistry mechanism and developed mitigation actions. Key research was performed to understand and control the photomodification properties. This research was then used to demonstrate several essential infrared photonic devices, including LWIR single-mode waveguide devices and waveguide couplers. Optical metrology tools were also developed to characterize optical waveguide structures and LWIR optical components.

Chalcogenide glasses are formed by combining chalcogen elements with IV-V elements. Among the family of glasses, As2S3, and As2Se3 are important infrared (IR) transparent materials for a variety of applications such as IR sensors, waveguides, and photonic crystals. With the promise of accessibility to any wavelengths between 3.5 and 16 mum using tunable quantum cascade lasers (QCL) and chalcogenides with IR properties that can be compositionally adjusted, ultrasensitive, solid-state, photonic-based chemical sensing in mid-wave IR region is now possible. Pacific Northwest National Laboratory (PNNL) has been developing quantum cascade lasers (QCLs), chalcogenides, and all other components for an integrated approach to chemical sensing. Significant progress has been made in glass formation and fabrication of different structures at PNNL. Three different glass-forming systems, As-S, As-S-Se, and As-S-Ag have been examined for this application. Purification of constituents from contaminants and thermal history are two major issues in obtaining defect-free glasses. We have shown how the optical proper-ties can be systematically modified by changing the chemistry in As-S-Se system. Different fabrication techniques need to be employed for different geometries and structures. We have successfully fabricated periodic arrays and straight waveguides using laser-writing and characterized the structures. Wet-chemical lithography has been extended to chalcogenides and challenges identified. We have also demonstrated holographic recording or diffraction gratings in chalcogenides.

The infrared sensors group at the Pacific Northwest National Laboratory (PNNL) is focused on the science and technology of remote and in-situ chemical sensors for detecting proliferation and countering terrorism. To support these vital missions, PNNL is developing frequency-modulation techniques for remote probing over long optical paths by means of differential-absorption light detecting and ranging (LIDAR). This technique can easily monitor large areas, or volumes, that could only be accomplished with a large network of point sensors. Recently, PNNL began development of a rugged frequency-modulation differential-absorption LIDAR (FM-DIAL) system to conduct field experiments. To provide environmental protection for the system and facilitate field deployments and operations, a large, well insulated, temperature controlled trailer was specified and acquired. The trailer was outfitted with a shock-mounted optical bench, an electronics rack, a liquid nitrogen Dewar, and a power generator. A computer-controlled gimbal-mounted mirror was added to allow the telescope beam to be accurately pointed in both the vertical and horizontal plane. This turned out to be the most complicated addition, and is described in detail. This paper provides an overview of the FM-DIAL system and illustrates innovative solutions developed to overcome several alignment and stability issues encountered in the field.

The small size, high power, promise of access to any wavelength between 3.5 and 16 microns, substantial tuning range about a chosen center wavelength, and general robustness of quantum cascade (QC) lasers provide opportunities for new approaches to ultra-sensitive chemical detection and other applications in the mid-wave infrared. PNNL is developing novel remote and sampling chemical sensing systems based on QC lasers, using QC lasers loaned by Lucent Technologies. In recent months laboratory cavity-enhanced sensing experiments have achieved absorption sensitivities of 8.5 x 10-11 cm-1 Hz-1/2, and the PNNL team has begun monostatic and bi-static frequency modulated, differential absorption lidar (FM DIAL) experiments at ranges of up to 2.5 kilometers. In related work, PNNL and UCLA are developing miniature QC laser transmitters with the multiplexed tunable wavelengths, frequency and amplitude stability, modulation characteristics, and power levels needed for chemical sensing and other applications. Current miniaturization concepts envision coupling QC oscillators, QC amplifiers, frequency references, and detectors with miniature waveguides and waveguide-based modulators, isolators, and other devices formed from chalcogenide or other types of glass. Significant progress has been made on QC laser stabilization and amplification, and on development and characterization of high-purity chalcogenide glasses, waveguide writing techniques, and waveguide metrology.

Chemical detection using infrared hyperspectral imaging systems often is limited by the effects of variability of the scene background emissivity spectra and temperature. Additionally, the atmospheric up-welling and down-welling radiance and transmittance are difficult to estimate from the hyperspectral image data, and may vary across the image. In combination, these background variability effects are referred to as "clutter." A study has been undertaken at Pacific Northwest National Laboratory to determine the relative impact of atmospheric variability and background variability on the detection of trace chemical vapors. This study has analyzed Atmospheric Emitted Radiance Interferometer data to estimate fluctuations in atmospheric constituents.To allow separation of the effects of background and atmospheric variability, hyperspectral data were synthesized using large sets of simulated atmospheric spectra, measured background emissivity spectra, and measured high-resolution gas absorbance spectra. The atmosphere was simulated using FASCODE in which the constituent gas concentrations and temperatures were varied. These spectral sets were combined synthetically using a physics model to realize a statistical synthetic scene with a plume present in a portion of the image. Noise was added to the image with the level determined by a numerical model of the hyperspectral imaging instrument. The chemical detection performance was determined by applying a matched-filter estimator to both the on-plume and off-plume regions. The detected levels in the off-plume region were then used to determine the noise equivalent concentration path length (NECL), a measure of the chemical detection sensitivity. The NECL was estimated for numerous gases and for a variety of background and atmospheric conditions to determine the relative impact of instrument noise, background variability, and atmospheric variability.

The tunability, small size, and flexibility in the center wavelength of quantum-cascade lasers make them well-suited for sensing applications in the infrared.

This update briefly reports new measurements and analysis that are used to determine the noise equivalent absorbance for the FM-DIAL (frequency modulation – differential absorption light detection and ranging) system. The modeling work that is performed in parallel with the LIDAR experiments provides a useful benchmark to predict the performance of an experimental setup, and a detection sensitivity to strive to realize. Often, the theoretical performance is difficult to obtain experimentally, but with careful design experiments can come close to being limited by fundamental noise sources.

Preliminary scoping exercises indicate that remote-sensing lidar can play a useful role in missions that involve determining regional weather patterns and atmospheric transport conditions. Both meteorological modeling and local atmospheric sensing should be employed. Satellite-based remote sensing systems, using an incoherent Doppler wind-sensor, seem feasible.