MULTICHARME: a modified Chernin-type multi-pass cell designed for IR and THz long-path absorption measurements in the CHARME atmospheric simulation chamber

Abstract

We have developed MULTICHARME, a modified Chernin-type multi-pass cell especially designed for IR and THz long-path absorption measurements in the CHamber for Atmospheric Reactivity and Metrology of the Environment (CHARME). By measuring the output power using a near-IR diode-laser and a THz amplified multiplication chain, we have established that the effective reflectivity of MULTICHARME is better than 94 % over approximately three decades of frequency. Absorption measurements of N2O have been performed by probing highly excited rovibrational transitions in the near-IR and ground state rotational transitions at submillimeter wavelengths. In each case the linearity of the absorbance with the path lengths was verified. Finally, we demonstrate that THz spectroscopy is able to study the isotopic composition of greenhouse polar gases such as N2O and to absolutely quantify stable (N2O) and reactive (O3) species at trace levels. At low pressure the ozone concentration was continuously monitored and its decay characterized. The deduced ozone lifetime of 3.4 ± 0.1 h is shorter compared with previous measurements performed in CHARME at atmospheric pressure. For the first time, the ability of THz rotational spectroscopy to monitor, with a very high degree of selectivity, stable and reactive polar compounds at trace level in an atmospheric simulation chamber is demonstrated. However, the sensitivity of the THz monitoring needs to be improved to reach atmospheric trace levels. For this purpose, it is necessary to fully understand the origin of the observed baseline variations caused by the complex multiple standing waves present in MULTICHARME.