P. T. Woods

Pulse averaging methods for a laser remote monitoring system using atmospheric backscatter

Three methods for averaging differential absorption lidar (DIAL) measurements are discussed. They are compared using experimental data acquired with a dual-laser direct-detection DIAL system operating in the near UV using atmospheric backscatter. The data set was acquired with the two lasers tuned to the same wavelength to eliminate any spectral variations and fluctuations of differential absorbers from the measurement. The results are compared by evaluating both the standard deviations and the means of the integrated columns. The results suggest that shot noise on the backscattered signals dominates the measurement statistics and considerably reduces the necessity for short interpulse delay times.

Frequency determination of visible laser light by interferometric comparison with upconverted CO 2 laser radiation

A servocontrolled 1-m plane-parallel Fabry-Perot interferometer has been developed at NPL for the precise intercomparison of laser wavelengths. This instrument has been used to measure the wavelength ratio of a 679-nm radiation and that from a 633-nm iodine-stabilized He-Ne laser, achieving an accuracy of 2.9 parts in 10(11). The 679-nm light was derived from a stabilized CO(2) laser radiation by upconversion, and the wavelength of this 9.3-microm laser radiation can be calculated from the visible wavelength result. Frequency measurements on the same CO(2) laser radiation have already been made in this laboratory, so that the experiment reported here leads to a precise value for the speed of light in vacuum and to the value of 473, 612, 380.5 +/- 0.3 MHz for the absolute frequency of the visible radiation from a He-Ne laser stabilized to component d of (127)I(2).

Measurements of toluene and other aromatic hydrocarbons by differential-absorption LIDAR in the near-ultraviolet

The first measurements of toluene by differential-absorption LIDAR in the near-ultraviolet spectral region are reported. A pulse energy of 4.5 mJ was used for the measurement, generated by frequency-doubling the output from a tunable dye laser in beta-barium borate. The magnitude of spectral interference from other pollutant species has been calculated and the extension of the system to measure other aromatic hydrocarbons in the same spectral region is discussed.

INJECTION SEEDING OF AN INFRARED OPTICAL PARAMETRIC OSCILLATOR WITH A TUNABLE DIODE LASER

A lithium niobate optical parametric oscillator pumped by a Nd:YAG laser has been injection seeded with a continous-wave diode laser. Injection seeding was achieved over signal wavelengths ranging from 1.526 to 1.578 microm, with a corresponding range for the idler of 3.26 to 3.51 microm At a signal wavelength of 1.535 microm, 7.6 mJ of signal radiation was generated from a pump energy of 75 mJ, with a measured bandwidth of 0.18 GHz.

Column measurements of stratospheric trace species over Are, Sweden in the winter of 1991-1992

Total vertical column amounts of stratospheric HCl, HF, ClONO2 and HNO3 are reported from high resolution infrared solar absorption spectra taken during the European Arctic Stratospheric Ozone Experiment (EASOE) in the winter of 1991-1992. These ground based measurements were made near Are in North Sweden (63.4 deg N, 13.1 deg E) at an altitude of 800 m using a Fourier transform spectrometer and tunable diode laser heterodyne spectrometer. On 9th January 1992 the HCl vertical column dropped to 1.2 x 10(exp 15) molecules/sq cm from a November average of 3.6 x 10(exp 15) molecules/sq cm. The HCl drop occurred at a time when Are was below the polar vortex and the lower stratospheric ClO column above Are was elevated to approximately 2 x 10(exp 15) molecules/sq cm as measured by the Microwave Limb Sounder experiment on the Upper Atmosphere Research Satellite. These measurements indicate conversion of lower stratospheric chlorine from reservoir to chemically active forms.

Errors in spectroscopic measurements of SO2 due to nonexponential absorption of laser radiation, with application to the remote monitoring of atmospheric pollutants.

Methods of measuring the concentration of atmospheric pollutants by laser absorption spectroscopy, such as differential absorption lidar (DIAL) and integrated long-path techniques, all rely on the validity of Beer’s exponential absorption law. It is shown here that departures from this law occur if the probing laser has a bandwidth larger than the wavelength scale of structure in the absorption spectrum of the pollutant. A comprehensive experimental and theoretical treatment of the errors resulting from these departures is presented for the particular case of SO2 monitoring at ~300 nm. It is shown that the largest error occurs where the initial calibration measurement of absorption cross section is made at low pressure, in which case errors in excess of 5% in the cross section could occur for laser bandwidths >0.01 nm. Atmospheric measurements by DIAL or long-path methods are in most cases affected less, because pressure broadening smears the spectral structure, but when measuring high concentrations errors can exceed 5%.

Measurements of stratospheric chlorine monoxide (ClO) from groudbased FTIR observations

Infrared absorption features due to ClO in the lower stratosphere have been identified from groundbased solar absorption spectra taken from Aberdeen, U.K. (57° N, 2° W) on 20 January 1995. A vertical column abundance of 3.42 (±0.47)×1015 molec cm-2 has been derived from 13 independent absorption features in the P and R branches of the (0–1) vibration-rotation band of 35ClO, spanning the spectral region 817–855 cm-1. The observed absorption features are consistent with very high levels of ClO (approximately 2.6 parts per billion by volume (ppbv)) in the altitude range 16–22 km. A comparison of this profile with a 3D chemical transport model profile indicates the observation was made inside the polar vortex and shows good qualitative agreement but the model underestimates the concentrations of ClO. Simultaneous measurements of other species were made including HCl, HF and ClONO2. These columns yield a value for HCl+ClONO2+ClO of 7.02±0.65×1015 molec cm-2. This is lower than the total inorganic chlorine (ClOy) column of 10.7±1.6×1015 molec cm-2 estimated from mean measured (HCl+ClONO2)/HF ratios together with in-vortex HF measurements. The discrepancy is probably due to significant amounts of the ClO dimer (Cl2O2) in the lower part of the stratosphere. The measurements of highly elevated levels of ClO are used to estimate O3 loss rates at the 400, 475 and 550 K levels making assumptions about the probable distribution of ClO and Cl2O2. These are compared with loss rates derived from ozone sonde data.

The exploitation of ground-based Fourier transform infrared observations for the evaluation of tropospheric trends of greenhouse gases over Europe

Abstract Solar absorption measurements using Fourier transform infrared (FTIR) spectrometry carry information about the atmospheric abundances of many constituents, including non-CO2 greenhouse gases. Such observations have regularly been made for many years as a contribution to the Network for the Detection of Stratospheric Change (NDSC). They are the only ground-based remote sensing observations available nowadays that carry information about a number of greenhouse gases in the free troposphere. This work focuses on the discussion of the information content of FTIR long-term monitoring data of some direct and indirect greenhouse gases (CH4, N2O, O3 and CO and C2H6, respectively), at six NDSC stations in Western Europe. This European FTIR network covers the polar to subtropical regions. At several stations of the network, the observations span more than a decade. Existing spectral time series have been reanalyzed according to a common optimized retrieval strategy, in order to derive distinct tropospheric and stratospheric abundances for the above-mentioned target gases. A bootstrap resampling method has been implemented to evaluate trends of the tropospheric burdens of the target gases, including their uncertainties. In parallel, simulations of the target time series are being made with the Oslo CTM2 model: comparisons between the model results and the observations provide valuable information to improve the model and, in particular, to optimize emission estimates that are used as inputs to the model simulations. The work is being performed within the EC project UFTIR. The paper focuses on N2O for which the first trend results have been obtained.

A dynamic gravimetric standard for trace water

A system for generating traceable reference standards of water vapor at trace levels between 5 and 2000 nmol/mol has been developed. It can provide different amount fractions of trace water vapor by using continuous accurate measurements of mass loss from a permeation device coupled with a dilution system based on an array of critical flow orifices. An estimated relative expanded uncertainty of ±2% has been achieved for most amount fractions generated. The system has been used in an international comparison and demonstrates excellent comparability with National Metrology Institutes maintaining standards of water vapor in this range using other methods.

DIAL measurements for air pollution and fugitive-loss monitoring

This paper describes a mobile differential absorption LIDAR system, which operates in the UV, visible, and IR spectral regions. This system can measure a range of important air pollutants emitted by industry, including SO2, NO2, NO, HCl, benzene, toluene, and a large range of other VOCs. These species can be monitored at fugitive and flammable levels at ranges of up to 1 km (for IR measurements) and 3 km (for UV measurements). Examples of measurements of fluxes emitted from large scale industrial sties are presented and discussed. Comparisons are given between measured fluxes and those calculated using the US Environmental Protection Agencys and American Petroleum Institutes standard procedures for estimating industrial emissions. The fluxes measured by DIAL are higher than the values derived from the API procedures. Possible reasons for discrepancies between the measured results and the EPA/API estimation procedures will be discussed.