Pulsed quantum-cascade-laser spectroscopy with intermediate-size pulses: application to NH3 in the 10 μm region

Abstract

Pulsed quantum-cascade-laser spectrometers are usually used to detect atmospheric gases with either the interpulse technique (short pulses, typically 5–20 ns) or the intrapulse technique (long pulses, typically 500–800 ns). Each of these techniques has its drawbacks. Particularly the gas absorption spectra are generally distorted. We have previously developed another technique called intermediate-size pulses (typically 50–100 ns) technique for gas detection using pulsed QCL spectrometers. In this paper, infrared spectra of ammonia recorded with this technique in the 10 μm region are presented. For the NH3 spectra recorded at low pressure (i.e. in the mbar range), the spectra show typical oscillations after the absorption. The Beer–Lambert law cannot explain these oscillations, termed the rapid-passage effect. Comparisons between experimental and calculated spectra will be realized. This phenomenon is not satisfactory from a spectroscopic point of view and spectra must be recorded at higher pressures. For the NH3 spectra recorded at higher pressure (i.e. in the 50 mbar range), the oscillations disappear and the Beer–Lambert law could be reused. This paper will demonstrate that the intermediate-size technique gives reliable measurements for NH3 detection. Moreover the typical apparatus function (0.003 cm−1 HWHM) is far lower from the typical apparatus function of the interpulse QCL spectrometers (0.015 cm−1 HWHM).