Computed tomographic (CT) reconstructions of air contaminant concentration fields were conducted in a roomsized chamber employing a single open-path Fourier transform infrared (OP-FTIR) instrument and a combination of 52 flat mirrors and 4 retroreflectors. A total of 56 beam path data were repeatedly collected for around 1 hr while maintaining a stable concentration gradient. The plane of the room was divided into 195 pixels (13 Ă— 15) for reconstruction.The algebraic reconstruction technique (ART) failed to reconstruct the original concentration gradient patterns for most cases. These poor results were caused by the "highly underdetermined condition" in which the IMPLICATIONS Gas concentration mapping in a room-sized chamber with the use of CT techniques, coupled with OP-FTIR, demonstrates that this system and reconstruction method could be directly applied in many environmental and industrial settings. The experimental beam configuration was in the highly underdetermined condition, which is commonly encountered in most conceivable fields. A new CT algorithm, the PWLS, was applied to remedy this unfavorable condition, since the standard ART algorithm results in poor CT reconstructions. Generally, concentration gradient patterns and peak locations were successfully reproduced. This system is the first experimental verification for the practical application of a CT system for real air pollutant mapping.number of unknown values (156 pixels) exceeds that of known data (56 path integral concentrations) in the experimental setting. A new CT algorithm, called the penalized weighted least-squares (PWLS), was applied to remedy this condition. The peak locations were correctly positioned in the PWLS-CT reconstructions. A notable feature of the PWLS-CT reconstructions was a significant reduction of highly irregular noise peaks found in the ART-CT reconstructions. However, the peak heights were slightly reduced in the PWLS-CT reconstructions due to the nature of the PWLS algorithm. PWLS could converge on the original concentration gradient even when a fairly high error was embedded into some experimentally measured path integral concentrations.It was also found in the simulation tests that the PWLS algorithm was very robust with respect to random errors in the path integral concentrations. This beam geometry and the use of a single OP-FTIR scanning system, in combination with the PWLS algorithm, is a system applicable to both environmental and industrial settings.