Demonstration of a uniform, high-pressure, high-temperature gas cell with a dual frequency comb absorption spectrometer

TL;DR

This paper introduces a novel high-pressure, high-temperature gas cell design for precise absorption spectroscopy, validated with a dual frequency comb spectrometer to improve models for combustion and planetary atmospheres.

Contribution

The paper presents a new uniform, high-pressure, high-temperature gas cell design and demonstrates its effectiveness with broadband spectroscopy, enabling better absorption models for extreme environments.

Findings

Achieved temperature uniformity up to 1000 K and pressure up to 50 bar.

Measured CO₂ spectra showing discrepancies with existing databases.

Validated the gas cell with high-resolution dual frequency comb spectroscopy.

Abstract

Accurate absorption models for gases at high pressure and temperature support advanced optical combustion diagnostics and aid in the study of harsh planetary atmospheres. Developing and validating absorption models for these applications requires recreating the extreme temperature and pressure conditions of these environments in static, uniform, well-known conditions in the laboratory. Here, we present the design of a new gas cell to enable reference-quality absorption spectroscopy at high pressure and temperature. The design centers on a carefully controlled quartz sample cell housed at the core of a pressurized ceramic furnace. The half-meter sample cell is relatively long compared to past high- pressure and temperature absorption cells, and is surrounded by a molybdenum heat spreader that enables high temperature uniformity over the full length of the absorbing gas. We measure the temperature distribution of the sample gas using in situ thermocouples, and fully characterize the temperature uniformity across a full matrix of conditions up to 1000 K and 50 bar. The results demonstrate that the new design enables highly uniform and precisely known conditions across the full absorbing path length. Uniquely, we test the new gas cell with a broadband, high-resolution dual frequency comb spectrometer that enables highly resolved absorption spectroscopy across a wide range of temperature and pressure conditions. With this system, we measure the spectrum of CO$_2$ between 6800 and 7000 cm$^{-1}$ at pressures between 0.2 and 20 bar, and temperatures up to 1000 K. The measurements reveal discrepancies from spectra predicted by the HITRAN2016 database with a Voigt line shape at both low- and high-pressure conditions. These results motivate future work to expand absorption models and databases to accurately model high-pressure and -temperature spectra in combustion and planetary science research.