This overview covers progress in the following areas in which Pacific Northwest Laboratory contributes to the CALIOPE Program: (1) Fabrication of electro-optic modulators to generate FM-coding on IR lasers in the 8-12 and 3-5 {mu}m regions. (2) IR spectroscopy of signature species, abnormal isotopic distributions, hydrolysis and kinetics of effluents interacting with the atmosphere, and reflectance measurements of natural surfaces. (3) Systems analysis of FM-DIAL concepts, including lateral phase coherence and MTF measurements, and laboratory tests of detector technology and demodulation methods. (4) Field tests of FM-DIAL, covering field validation of portable diode laser concepts, FM-CO{sub 2} interrogation of Hanford sites, and signal returns from natural specular surfaces. (5) Ancillary matters: ground-truthing at Hanford (and RSTR?), countermeasures, and new laser design concepts