RESUMO
The action to reduce anthropogenic greenhouse gas emissions is severely constrained by the difficulty of locating sources and quantifying their emission rates. Methane emissions by the energy sector are of particular concern. We report results achieved with a new area monitoring approach using laser dispersion spectroscopy to measure path-averaged concentrations along multiple beams. The method is generally applicable to greenhouse gases, but this work is focused on methane. Nineteen calibrated methane releases in four distinct configurations, including three separate blind trials, were made within a flat test area of 175 m by 175 m. Using a Gaussian plume gas dispersion model, driven by wind velocity data, we calculate the data anticipated for hundreds of automatically proposed candidate source configurations. The Markov-chain Monte Carlo analysis finds source locations and emission rates whose calculated path-averaged concentrations are consistent with those measured and associated uncertainties. This approach found the correct number of sources and located them to be within <9 m in more than 75% of the cases. The relative accuracy of the mass emission rate results was highly correlated to the localization accuracy and better than 30% in 70% of the cases. The discrepancies for mass emission rates were <2 kg/h for 95% of the cases.
RESUMO
A variant of cavity-enhanced Raman spectroscopy (CERS) is introduced, in which diode laser radiation at 635 nm is coupled into an external linear optical cavity composed of two highly reflective mirrors. Using optical feedback stabilisation, build-up of circulating laser power by 3 orders of magnitude occurs. Strong Raman signals are collected in forward scattering geometry. Gas phase CERS spectra of H(2), air, CH(4) and benzene are recorded to demonstrate the potential for analytical applications and fundamental molecular studies. Noise equivalent limits of detection in the ppm by volume range (1 bar sample) can be achieved with excellent linearity with a 10 mW excitation laser, with sensitivity increasing with laser power and integration time. The apparatus can be operated with battery powered components and can thus be very compact and portable. Possible applications include safety monitoring of hydrogen gas levels, isotope tracer studies (e.g., (14)N/(15)N ratios), observing isotopomers of hydrogen (e.g., radioactive tritium), and simultaneous multi-component gas analysis. CERS has the potential to become a standard method for sensitive gas phase Raman spectroscopy.
