Assessment of gas molar density by gas modulation refractometry: A review of its basic operating principles and extraordinary performance

A technique for high-precision and high-accuracy assessment of both gas molar (and number) density and pressure, Gas Modulation Refractometry (GAMOR), is presented. The technique achieves its properties by assessing refractivity as a shift of a directly measurable beat frequency by use of Fabry-Perot cavity (FPC) based refractometry utilizing the Pound-Drever-Hall laser locking technique. Conventional FPC-based refractometry is, however, often limited by fluctuations and drifts of the FPC. GAMOR remedies this by an additional utilization of a gas modulation methodology, built upon a repeated filling and evacuation of the measurement cavity together with an interpolation of the empty cavity responses. The procedure has demonstrated an ability to reduce the influence of drifts in a non-temperature stabilized dual-FPC (DFPC)-based refractometry system, when assessing pressure, by more than three orders of magnitude. When applied to a DFPC system with active temperature stabilization, it has demonstrated, for assessment of pressure of N2 at 4304 Pa at room temperature, which corresponds to a gas molar density of 1.7 × 10−6 mol/cm3, a sub-0.1 ppm precision (i.e. a resolution of 0.34 mPa). It is claimed that the ability to assess gas molar density is at least as good as so far has been demonstrated for pressure (i.e. for the molar density addressed, a resolution of at least 1.2 × 10−13 mol/cm3). It has recently been argued that the methodology should be capable of providing an accuracy that is in the low ppm range. These levels of precision and accuracy are unprecedented among laser-based techniques for detection of atomic and molecular species. Since the molar polarizability of He can be calculated by ab initio quantum mechanical calculations with sub-ppm accuracy, it can also be used as a primary or semi-primary standard of both gas molar (and number) density and pressure