Inversion of multiwavelength Raman lidar data for retrieval of bimodal aerosol size distribution

We report on the feasibility of deriving microphysical parameters of bimodal particle size distributions from Mie-Raman lidar based on a triple Nd:YAG laser. Such an instrument provides backscatter coefficients at 355, 532, and 1064 nm and extinction coefficients at 355 and 532 nm. The inversion method employed is Tikhonov's inversion with regularization. Special attention has been paid to extend the particle size range for which this inversion scheme works to approximately 10 microm, which makes this algorithm applicable to large particles, e.g., investigations concerning the hygroscopic growth of aerosols. Simulations showed that surface area, volume concentration, and effective radius are derived to an accuracy of approximately 50% for a variety of bimodal particle size distributions. For particle size distributions with an effective radius of < 1 microm the real part of the complex refractive index was retrieved to an accuracy of +/- 0.05, the imaginary part was retrieved to 50% uncertainty. Simulations dealing with a mode-dependent complex refractive index showed that an average complex refractive index is derived that lies between the values for the two individual modes. Thus it becomes possible to investigate external mixtures of particle size distributions, which, for example, might be present along continental rims along which anthropogenic pollution mixes with marine aerosols. Measurement cases obtained from the Institute for Tropospheric Research six-wavelength aerosol lidar observations during the Indian Ocean Experiment were used to test the capabilities of the algorithm for experimental data sets. A benchmark test was attempted for the case representing anthropogenic aerosols between a broken cloud deck. A strong contribution of particle volume in the coarse mode of the particle size distribution was found.     

Iterative method for the inversion of multiwavelength lidar signals to determine aerosol size distribution

Two iterative methods of inverting lidar backscatter signals to determine altitude profiles of aerosol extinction and altitude-resolved aerosol size distribution (ASD) are presented. The first method is for inverting two-wavelength lidar signals in which the shape of the ASD is assumed to be of power-law type, and the second method is for inverting multiwavelength lidar signals without assuming any a priori analytical form of ASD. An arbitrary value of the aerosol extinction-to-backscatter ratio (S(1)) is assumed initially to invert the lidar signals, and the ASD determined by use of the spectral dependence of the retrieved aerosol extinction coefficients is used to improve the value of S(1) iteratively. The methods are tested for different forms of altitude-dependent ASD's by use of simulated lidar-backscatter-signal profiles. The effect of random noise on the lidar backscatter signals is also studied.     

Retrieval of stratospheric aerosol size distributions and integral properties from simulated lidar backscatter measurements

A new approach for retrieving aerosol properties from extinction spectra is extended to retrieve aerosol properties from lidar backscatter measurements. In this method it is assumed that aerosol properties are expressed as a linear combination of backscatters at three or fewer wavelengths commonly used in lidar measurements. The coefficients in the weighted linear combination are obtained by minimization of the retrieval error averaged for a set of testing size distributions. The formulas can be used easily by investigators to retrieve aerosol properties from lidar backscatter measurements such as the Lidar In-Space Technology Experiment and Pathfinder Instruments for Clouds and Aerosols Spaceborne Observations.     

Bayesian assessment of uncertainty in aerosol size distributions and index of refraction retrieved from multiwavelength lidar measurements

We investigate the assessment of uncertainty in the inference of aerosol size distributions from backscatter and extinction measurements that can be obtained from a modern elastic/Raman lidar system with a Nd:YAG laser transmitter. To calculate the uncertainty, an analytic formula for the correlated probability density function (PDF) describing the error for an optical coefficient ratio is derived based on a normally distributed fractional error in the optical coefficients. Assuming a monomodal lognormal particle size distribution of spherical, homogeneous particles with a known index of refraction, we compare the assessment of uncertainty using a more conventional forward Monte Carlo method with that obtained from a Bayesian posterior PDF assuming a uniform prior PDF and show that substantial differences between the two methods exist. In addition, we use the posterior PDF formalism, which was extended to include an unknown refractive index, to find credible sets for a variety of optical measurement scenarios. We find the uncertainty is greatly reduced with the addition of suitable extinction measurements in contrast to the inclusion of extra backscatter coefficients, which we show to have a minimal effect and strengthens similar observations based on numerical regularization methods.     

Retrieval of aerosol properties from combined multiwavelength lidar and sunphotometer measurements

Simulation studies were carried out with regard to the feasibility of using combined observations from sunphotometer (SPM) and lidar for microphysical characterization of aerosol particles, i.e., the retrieval of effective radius, volume, and surface-area concentrations. It was shown that for single, homogeneous aerosol layers, the aerosol parameters can be retrieved with an average accuracy of 30% for a wide range of particle size distributions. Based on the simulations, an instrument combination consisting of a lidar that measures particle backscattering at 355 and 1574 nm, and a SPM that measures at three to four channels in the range from 340 to 1020 nm is a promising tool for aerosol characterization. The inversion algorithm has been tested for a set of experimental data. The comparison with the particle size distribution parameters, measured with in situ instrumentation at the lidar site, showed good agreement.     

Hybrid regularization method for the ill-posed inversion of multiwavelength lidar data in the retrieval of aerosol size distributions

A specially developed method is proposed to retrieve the particle volume distribution, the mean refractive index, and other important physical parameters, e.g., the effective radius, volume, surface area, and number concentrations of tropospheric and stratospheric aerosols, from optical data by use of multiple wavelengths. This algorithm requires neither a priori knowledge of the analytical shape of the distribution nor an initial guess of the distribution. As a result, even bimodal and multimodal distributions can be retrieved without any advance knowledge of the number of modes. The nonlinear ill-posed inversion is achieved by means of a hybrid method combining regularization by discretization, variable higher-order B-spline functions and a truncated singular-value decomposition. The method can be used to handle different lidar devices that work with various values and numbers of wavelengths. It is shown, to my knowledge for the first time, that only one extinction and three backscatter coefficients are sufficient for the solution. Moreover, measurement errors up to 20% are allowed. This result could be achieved by a judicious fusion of different properties of three suitable regularization parameters. Finally, numerical results with an additional unknown refractive index show the possibility of successfully recovering both unknowns simultaneously from the lidar data: the aerosol volume distribution and the refractive index.     

Inversion with regularization for the retrieval of tropospheric aerosol parameters from multiwavelength lidar sounding

We present an inversion algorithm for the retrieval of particle size distribution parameters, i.e., mean (effective) radius, number, surface area, and volume concentration, and complex refractive index from multiwavelength lidar data. In contrast to the classical Tikhonov method, which accepts only that solution for which the discrepancy reaches its global minimum, in our algorithm we perform the averaging of solutions in the vicinity of this minimum. This averaging stabilizes the underlying ill-posed inverse problem, particularly with respect to the retrieval of number concentration. Results show that, for typical tropospheric particles and 10% error in the optical data, the mean radius could be retrieved to better than 20% from a lidar on the basis of a Nd:YAG laser, which provides a combination of backscatter coefficients at 355, 532, and 1064 nm and extinction coefficients at 355 and 532 nm. The accuracy is improved if the lidar is also equipped with a hydrogen Raman shifter. In this case two additional backscatter coefficients at 416 and 683 nm are available. The combination of two extinction coefficients and five backscatter coefficients then allows one to retrieve not only averaged aerosol parameters but also the size distribution function. There was acceptable agreement between physical particle properties obtained from the evaluation of multiwavelength lidar data taken during the Lindenberg Aerosol Characterization Experiment in 1998 (LACE 98) and in situ data, which were taken aboard aircraft.     

Determination of stratospheric aerosol microphysical properties from independent extinction and backscattering measurements with a Raman lidar

An algorithm that permits the retrieval of profiles of particle mass and surface-area concentrations in the stratospheric aerosol layer from independently measured aerosol (particle and Rayleigh) and molecule (Raman or Rayleigh) backscatter signals is developed. The determination is based on simultaneously obtained particle extinction and backscatter profiles and on relations between optical and microphysical properties found from Mie-scattering calculations for realistic stratospheric particle size distributions. The size distributions were measured with particle counters released on balloons from Laramie, Wyoming, between June 1991 and April 1994. Mass and surface-area concentrations can be retrieved with relative errors of 10-20% and 20-40%, respectively, with a laser wavelength of 355 nm and with errors of 20-30% and 30-60%, respectively, with a laser wavelength of 308 nm. Lidar measurements taken within the first three years after the eruption of Mt. Pinatubo in June 1991 are shown. Surface-area concentrations around 20 μm(2) cm(-3) and mass concentrations of 3 to 6 μg m(-3) were found until spring 1993.     

High-efficiency aerosol scatterometer that uses an integrating sphere for the calibration of multiwavelength lidar data

For the purpose of calibrating multiwavelength lidar data, we developed a scatterometer to measure the aerosol scattering coefficient at the ground level. The system is based on an integrating sphere, cw lasers (532 and 633 nm), and a controlled flow of the ambient air, including aerosol particles. The simulation study and experimental results indicate that the detection efficiency of this instrument is approximately 10%-40% better than that of an integrating nephelometer, because of the wider acceptance angle of the scattered light. The scattering coefficients measured at the two wavelengths, as well as the resulting value of the angstrom exponent, show good correlation with the results simultaneously measured with an integrating nephelometer and an optical particle counter.     

Derivation of the aerosol size distribution from a bistatic system of a muitiwavelength laser with the singular value decomposition method

Estimation of aerosol size distributions from measurements of scattered light intensity by the use of a bistatic system with a multiwavelength laser is presented. We investigated the effects of inversion of the scattered intensity on calculated aerosol size distribution in a numerical experiment. Two model aerosol size distributions were used, one a Junge type widely known as a typical example of the size distribution of suspended particles in the atmosphere and the other a log-normal type as an example of the monodisperse distribution. A singular value decomposition was applied to the inversion to infer the size distribution from the kernel function and the scattered light intensity. In the physical experiment, the size distributions were successfully inferred from analysis of the scattered light intensity from an artificial polystyrene latex aerosol.     

Measurements of stratospheric aerosols with a combined elastic-Raman-backscatter lidar

Improvements made to the NASA Goddard Space Flight Center Stratospheric Ozone Lidar system have extended its atmospheric-aerosol-measuring capabilities. The methods by which aerosol-scattering ratio, aerosol backscatter, and aerosol extinction are simultaneously derived from lidar data are reported, and results obtained during several intercomparison campaigns at worldwide locations are shown. The results track the evolution of the Mt. Pinatubo aerosol cloud from 1991 to 1994 and report wavelength-dependence information for aerosol backscatter between 308 and 351 nm. Two analysis techniques, a more common inversion method and a combined elastic-Raman-backscatter approach, are also compared.     

Retrieval of stratospheric aerosol size and composition information from solar infrared transmission spectra

Infrared transmission spectra were recorded by the Jet Propulsion Laboratory MkIV interferometer during flights aboard the NASA DC-8 aircraft as part of the Airborne Arctic Stratospheric Expedition II (AASE II) mission in the early months of 1992. In our research, we infer the properties of the stratospheric aerosols from these spectra. The instrument employs two different detectors, a HgCdTe photoconductor for 650-1850 cm(-1) and an InSb photodiode for 1850-5650 cm(-1), to simultaneously record the solar intensity throughout the mid-infrared. These spectra have been used to retrieve the concentrations of a large number of gases, including chlorofluorocarbons, NOy species, O3, and ozone-depleting gases. We demonstrate how the residual continua spectra, obtained after accounting for the absorbing gases, can be used to obtain information about the stratospheric aerosols. Infrared extinction spectra are calculated for a range of modeled aerosol size distributions and compositions with Mie theory and fitted to the measured residual spectra. By varying the size distribution parameters and sulfate weight percent, we obtain the microphysical properties of the aerosols that best fit the observations. The effective radius of the aerosols is found to be between 0.4 and 0.6 microm, consistent with that derived from a large number of instruments in this post-Pinatubo period. We demonstrate how different parts of the spectral range can be used to constrain the range of possible values of this size parameter and show how the broad spectral bandpass of the MkIV instrument presents a great advantage for retrieval ofboth aerosol size a nd composition over instruments with a more limited spectral range. The aerosol composition that provides the best fit to the measured spectra is a 70-75% sulfuric acid solution, in good agreement with that obtained from thermodynamic considerations.     

Development of a multiwavelength aerosol and water-vapor lidar at the Jungfraujoch Alpine Station (3580 m above sea level) in Switzerland

The Jungfraujoch Research Station (46.55 degrees N, 7.98 degrees E, 3580 m above sea level) for decades has contributed in a significant manner to the systematic observation of the Earth's atmosphere both with in situ measurements and with trace gas column detection. We report on the development of a lidar system that improves the measurement potential of highly resolved atmospheric parameters in both time and space, with the goal of achieving long-term monitoring of atmospheric aerosol optical properties and water-vapor content. From the simultaneously detected elastic-backscatter signals at 355, 532, and 1064 nm, Raman signals from nitrogen at 387 and 607 nm, and water vapor at 408 nm, the aerosol extinction and backscatter coefficients at three wavelengths and a water-vapor mixing ratio are derived. Additional information about particle shape is obtained by depolarization measurements at 532 nm. Water-vapor measurements by use of both nitrogen and water-vapor Raman returns from the 355-nm laser beam are demonstrated with a vertical range resolution of 75 m and an integration time of 2 h. The comparison to the water-vapor profile derived from balloon measurements (Snow White technique) showed excellent agreement. The system design and the results obtained by its operation are reported.     

Multiwavelength lidar observations of the decay phase of the stratospheric aerosol layer produced by the eruption of mount pinatubo in june 1991

A small three-wavelength (355-, 532-, and 1064-nm) lidar system at NASA Langley Research Center in Hampton, Virginia, has been used since 1992 to make measurements on stratospheric aerosols. The data have been processed to study the decay rate of the stratospheric aerosol layer formed after the eruption of Mount Pinatubo in 1991 and its modulation, the aerosol effective radius, and the column mass loading. The stratospheric aerosol decay curves show annual and biennial cycles as well as short-term changes. At 532 nm, the decay time constant was 302 days for the period from February 1992 to August 1994 and had increased to 645 days for the period from September 1994 to December 1997. By 1996 the integrated stratospheric aerosol backscatter had fallen to levels (7.7 x 10(-5) sr(-1) at 532 nm) close to those seen in 1979 and 1989-1991. This decreasing trend was still continuing in 1997, showing no evidence for any anthropogenic contribution to the stratospheric aerosol.     

Extension of the graphical technique for estimation of particle size distribution parameters for the consistent intercomparison of diverse sets of multiwavelength lidar derived optical coefficients

In applying the graphical technique to the estimation of the particle size distribution (PSD) parameters, determination of proper bounds surrounding the solution space for a particular confidence level is essential to the consistent intercomparison of diverse multiwavelength lidar optical data sets. The graphical technique utilizes ratios of backscatter and/or extinction coefficients, and it is shown that if the correlation between ratios is not taken into account in calculating the error bounds, the solution space will be overestimated, resulting in relatively larger discrepancies for a larger number of optical coefficients. A method for correcting the bounds, to account for the correlation is developed for various numbers of wavelengths. These improved bounds are then applied, for the case of a monomodal lognormal PSD, with an assumed refractive index, to assess the role additional Raman extinction channels play in improving retrieval capability of a typical three-channel backscatter lidar (1064, 532, and 355 nm) under varying noise levels. Applying the same formalism to underlying bimodal distributions of coarse and fine particles can result in false monomodal solutions. However, when both Raman optical extinction channels are available, no solution is obtained. This can potentially serve as a quick and simple method, prior to a more complex regularization analysis, to differentiate between cases in which the fine mode is dominant versus the cases in which the contribution from the coarse mode is significant.     

Design and performance of a multiwavelength airborne polarimetric lidar for vegetation remote sensing

The University of Nebraska has developed a multiwavelength airborne polarimetric lidar (MAPL) system to support its Airborne Remote Sensing Program for vegetation remote sensing. The MAPL design and instrumentation are described in detail. Characteristics of the MAPL system include lidar waveform capture and polarimetric measurement capabilities, which provide enhanced opportunities for vegetation remote sensing compared with current sensors. Field tests were conducted to calibrate the range measurement. Polarimetric calibration of the system is also discussed. Backscattered polarimetric returns, as well as the cross-polarization ratios, were obtained from a small forested area to validate the system's ability for vegetation canopy detection. The system has been packaged to fly abroad a Piper Saratoga aircraft for airborne vegetation remote sensing applications.     

Ratio of aerosol and gases of radioactive chlorine and particle size distribution of aerosol formed by high-energy proton irradiation

To estimate internal doses due to the inhalation of radionuclides produced by the nuclear spallation of the air nuclei in high-energy proton accelerator facilities, the physicochemical properties of radionuclides are very important. Thus, the ratio of aerosol and gases of 38Cl and 39Cl formed by irradiating argon gas-added air with a 48 MeV proton beam has been measured. Radionuclides of 38Cl and 39Cl exist as aerosol, acid gas and non-acid gas. The percentages of activity of 38Cl and 39Cl aerosols are about 80%. The number size distributions of non-radioactive aerosol were characterised by two peaks with diameters of 10-20 nm and larger than 20 nm. As a result predicted by a simple surface model, it was found that the activity size distribution of 38Cl aerosols can be regarded as that having a single peak at 120 nm.