An overview of geoengineering of climate using stratospheric sulphate aerosols

We provide an overview of geoengineering by stratospheric sulphate aerosols. The state of understanding about this topic as of early 2008 is reviewed, summarizing the past 30 years of work in the area, highlighting some very recent studies using climate models, and discussing methods used to deliver sulphur species to the stratosphere. The studies reviewed here suggest that sulphate aerosols can counteract the globally averaged temperature increase associated with increasing greenhouse gases, and reduce changes to some other components of the Earth system. There are likely to be remaining regional climate changes after geoengineering, with some regions experiencing significant changes in temperature or precipitation. The aerosols also serve as surfaces for heterogeneous chemistry resulting in increased ozone depletion. The delivery of sulphur species to the stratosphere in a way that will produce particles of the right size is shown to be a complex and potentially very difficult task. Two simple delivery scenarios are explored, but similar exercises will be needed for other suggested delivery mechanisms. While the introduction of the geoengineering source of sulphate aerosol will perturb the sulphur cycle of the stratosphere signicantly, it is a small perturbation to the total (stratosphere and troposphere) sulphur cycle. The geoengineering source would thus be a small contributor to the total global source of 'acid rain' that could be compensated for through improved pollution control of anthropogenic tropospheric sources. Some areas of research remain unexplored. Although ozone may be depleted, with a consequent increase to solar ultraviolet-B (UVB) energy reaching the surface and a potential impact on health and biological populations, the aerosols will also scatter and attenuate this part of the energy spectrum, and this may compensate the UVB enhancement associated with ozone depletion. The aerosol will also change the ratio of diffuse to direct energy reaching the surface, and this may influence ecosystems. The impact of geoengineering on these components of the Earth system has not yet been studied. Representations for the formation, evolution and removal of aerosol and distribution of particle size are still very crude, and more work will be needed to gain confidence in our understanding of the deliberate production of this class of aerosols and their role in the climate system.     

Influence of lower stratospheric aerosol variations on guidestar performance

The probability distribution function for the logarithm of the mixing scatter ratio, based on long-term measurements of lower-stratospheric aerosol loading, is derived to model variations in total backscatter coefficient and extinction profiles in the visible and the near infrared (NIR). The profiles are used to estimate signal-to-noise ratio, laser-pulse energy, and wave-front measurement error with respect to backscatter strength, guidestar pulse length and altitude, and pixel noise. The results show that for a given wave-front measurement phase error (1) visible guidestars require less pulse energy for aerosol concentrations near background, where molecular backscatter dominates, and (2) for high aerosol loading following a major volcanic event, a NIR guidestar can reduce the energy requirement below that for visible sensing.     

Validation of the Lidar In-Space Technology Experiment: stratospheric temperature and aerosol measurements

The Lidar In-Space Technology Experiment (LITE) was flown on STS-64 in September 1994. The LITE employed a Nd:YAG laser operating at 1064, 532, and 355 nm to study the Earth's lower atmosphere. In this paper we investigate the nighttime stratospheric aerosol and temperature measurements derived from the 532- and 355-nm channels. The observations are compared with lidar observations obtained at Arecibo Observatory, Puerto Rico, and Starfire Optical Range, New Mexico, and with balloonsondes launched from the San Juan and Albuquerque airports. The backscatter ratios derived from the LITE and Arecibo data between 15 and 30 km differ by less than 5%. The Angstrom coefficients of the stratospheric aerosols derived from the 532- and 355-nm LITE channels exhibited only slight variation in altitude. The mean value between 15 and 30 km derived from three different orbital segments at approximately 20 degrees N and 35 degrees N was 1.7. The mean standard deviation was approximately 0.3. Temperature profiles were derived from the LITE data by correcting the 355-nm channel for aerosol scattering with the 532-nm signal and an assumed Angstrom coefficient. The rms differences between the corrected profiles and the balloonsonde data were as low as 2 K in the 15-30-km height range. The results were not particularly sensitive to the choice of the Angstrom coefficient and suggest that accurate temperature profiles can be derived from the LITE data in the upper troposphere and lower stratosphere provided that the aerosol loading is light.     

Optical systems design for a stratospheric lidar system

The optical systems for the transmitter and receiver of a high-power lidar for stratospheric measurements have been designed and analyzed. The system requirements and design results are presented and explained. An important and driving factor of this design was the requirement for a small image diameter in the plane of an optical chopper to allow the high-intensity lidar returns from the lower atmosphere to be shielded from the detection system. Some results relevant to the optical performance of the system are presented. The resulting system has been constructed and is now in operation at the Mauna Loa Observatory, Hawaii, and is making regular measurements of stratospheric ozone, temperature, and aerosol profiles.     

Calibration method for the lidar-observed stratospheric depolarization ratio in the presence of liquid aerosol particles

A fine calibration of the depolarization ratio is required for a detailed interpretation of lidar-observed polar stratospheric clouds. We propose a procedure for analyzing data by using atmospheric depolarization lidar. The method is based on a plot of deltaT versus (1 - RT(-1)), where deltaT is the total depolarization ratio and RT is the total backscattering ratio. Assuming that there are only spherical particles in some altitude ranges of the lidar data, the characteristics of the plot of deltaT versus (1 - RT(-1)) lead to a simple but effective calibration method for deltaT. Additionally, the depolarization of air molecules deltam can be determined in the process of deltaT calibration. We compared determined values with theoretically calculated values for the depolarization of air to test the proposed method. The deltam value was calculated from the lidar data acquired at Ny-Alesund (79 degrees N, 12 degrees E), Svalbard in winter 1994-1995. When only sulfate aerosols were present on 24 December 1994, deltam was 0.46 +/- 0.35%. When the particles consisted of sulfate aerosols and spherical particles of polar stratospheric clouds on 4 January 1995, deltam was 0.45 +/- 0.07%. Both deltam values were in good agreement with the theoretically calculated value, 0.50 +/- 0.03%.     

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.     

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.     

Derivation of Mount Pinatubo stratospheric aerosol mean size distribution by means of a multiwavelength lidar

A multiwavelength lidar operated in Sodankyla, Finland, during the European Arctic Stratospheric Ozone Experiment (December 1991-March 1992). It produced vertical profiles of stratospheric aerosols at four wavelengths. The determination of aerosol mean size distribution has been performed by use of extinction/backscattering ratios as obtained from lidar data processing at 355, 352, and 750 nm. Lognormal distributions of sulfuric particles with mode radius of r(m) = 0.12-0.25 μm and corresponding widths of s = 2-1.6 have been retrieved as best fits of experimental data, in good agreement with in situ measurements. A successful attempt to derive bimodal log-normal distributions is also described, together with the experimental and theoretical problems involved.     

Relative equilibria of tethered satellite systems and their stability for very stiff tethers

We study the existence and stability of the relative equilibria of systems of two satellites joined by a tether. Since tethers used in practice are very stiff we consider a stiff tether as a perturbation of an inextensible tether. We show that the equations for relative equilibria and the stability conditions are continuous as stiffness approaches infinity and limit on the equations and conditions relevant to an inextensible tether. We obtain a numerical bifurcation diagram for a class of relative equilibria in the case of an inextensible tether.     

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.     

Optical and physical properties of stratospheric aerosols from balloon measurements in the visible and near-infrared domains. 1. Analysis of aerosol extinction spectra from the AMON and SALOMON balloonborne spectrometers

Aerosol extinction coefficients have been derived in the 375-700-nm spectral domain from measurement in the stratosphere since 1992, at night, at mid- and high latitudes from 15 to 40 km, by two balloonborne spectrometers, Absorption par les Minoritaires Ozone et NO(chi) (AMON) and Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NO(chi) (SALOMON). Log-normal size distributions associated with the Mie-computed extinction spectra that best fit the measurements permit calculation of integrated properties of the distributions. Although measured extinction spectra that correspond to background aerosols can be reproduced by the Mie scattering model by use of monomodal log-normal size distributions, each flight reveals some large discrepancies between measurement and theory at several altitudes. The agreement between measured and Mie-calculated extinction spectra is significantly improved by use of bimodal log-normal distributions. Nevertheless, neither monomodal nor bimodal distributions permit correct reproduction of some of the measured extinction shapes, especially for the 26 February 1997 AMON flight, which exhibited spectral behavior attributed to particles from a polar stratospheric cloud event.     

The runaway greenhouse: implications for future climate change, geoengineering and planetary atmospheres

The ultimate climate emergency is a 'runaway greenhouse': a hot and water-vapour-rich atmosphere limits the emission of thermal radiation to space, causing runaway warming. Warming ceases only after the surface reaches approximately 1400 K and emits radiation in the near-infrared, where water is not a good greenhouse gas. This would evaporate the entire ocean and exterminate all planetary life. Venus experienced a runaway greenhouse in the past, and we expect that the Earth will in around 2 billion years as solar luminosity increases. But could we bring on such a catastrophe prematurely, by our current climate-altering activities? Here, we review what is known about the runaway greenhouse to answer this question, describing the various limits on outgoing radiation and how climate will evolve between these. The good news is that almost all lines of evidence lead us to believe that is unlikely to be possible, even in principle, to trigger full a runaway greenhouse by addition of non-condensible greenhouse gases such as carbon dioxide to the atmosphere. However, our understanding of the dynamics, thermodynamics, radiative transfer and cloud physics of hot and steamy atmospheres is weak. We cannot therefore completely rule out the possibility that human actions might cause a transition, if not to full runaway, then at least to a much warmer climate state than the present one. High climate sensitivity might provide a warning. If we, or more likely our remote descendants, are threatened with a runaway greenhouse, then geoengineering to reflect sunlight might be life's only hope. Injecting reflective aerosols into the stratosphere would be too short-lived, and even sunshades in space might require excessive maintenance. In the distant future, modifying Earth's orbit might provide a sustainable solution. The runaway greenhouse also remains relevant in planetary sciences and astrobiology: as extrasolar planets smaller and nearer to their stars are detected, some will be in a runaway greenhouse state.     

Contrasting approaches to the generation of environmental improvement options for production systems

This article reviews two common types of improvement tools presently used in industry to identify opportunities to prevent or at least to reduce the environmental impacts of production systems and processes. Despite their proven ability to result in appropriate environmental improvement options in different industry sectors, their successful application is hampered by the fact that these tools do not take the specific causes of the environmental impacts of the production process into account, i.e. the question of which process features cause the environmental impacts of the production process is not raised nor is the flexibility for change of the production system taken into consideration. This paper sets the stage for a new generation of improvement tools, based on an environmental diagnosis of the production system. The diagnosis aims to result in a thorough understanding of the production system to guide and drive the identification of environmental improvement options that specifically target process-, product-, and site-specific environmental conditions. Alternative ways to develop such a diagnostic approach on the basis of presently used tools are being explored, and a synthesis thereof is proposed to achieve synergy between these contrasting approaches. Received: 7 August 2000 / Accepted: 8 November 2000     

An evaluation of options for replacing HCFC-22 in medium temperature refrigeration systems

Due to the ongoing global phase-out of R-22, which is still the most widely used refrigerant around the world, there is a need to replace this refrigerant in many different applications. This paper focuses on a thorough evaluation of the R-22 replacement options for medium-temperature refrigeration applications. It includes a thermodynamic analysis, comparison of heat transfer and pressure drop characteristics, system performance comparisons using a validated detailed system model, safety issues, and determination of the environmental impact of refrigerant selection. Three potential alternatives to the R-22 were studied: two HFCs (404A and R-410A) and one HC (R-290). An HFC refrigerant, R-410A, is shown to be an efficient and environmentally acceptable option to replace R-22 in medium temperature applications.     

Optical modeling of stratospheric aerosols: present status

A stratospheric aerosol optical model is developed which is based on a size distribution conforming to direct measurements. Additional constraints are consistent with large data sets of independently measured macroscopic aerosol properties such as mass and backscatter. The period under study covers background as well as highly disturbed volcanic conditions and an altitude interval ranging from the tropopause to approximately 30 km. The predictions of the model are used to form a basis for interpreting and intercomparing several diverse types of stratospheric aerosol measurement.     

Simulations of the accuracy in retrieving stratospheric aerosol effective radius, composition, and loading from infrared spectral transmission measurements

We examine the extent to which three physical aerosol parameters--effective radius, composition (sulfate weight percent), and total volume-can be determined from infrared transmission spectra. Using simulated transmission data over the range 800-4750 cm(-1) (12.5-2.1 microm) and errors taken from the infrared spectral measurements of the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument, we use optimal estimation to recover these aerosol parameters. Uncertainties in these are examined as a function of the size, composition, and loading of stratospheric aerosols and of the spectral range employed. Using the entire spectral range above, we retrieve all three parameters with a precision to within 3% if the size distribution form is known. Additional errors result, however, from an uncertainty in the size distribution width. These are small (only a few percent) for composition and total volume but are substantial (as much as 50%) for effective radius. Errors also increase substantially when the spectral range is reduced. The retrieved effective radius can have an error of 100% or greater for typical stratospheric aerosol sizes when the spectral range is restricted to the lower wavenumber part of the range. For good accuracy in effective radius, the spectral range must extend beyond approximately 3000 cm(-1). Composition and total volume are less sensitive to the spectral range than effective radius. These simulations were carried out with modeled data to test the potential accuracy of stratospheric sulfate aerosol retrievals from the Atmospheric Chemistry Experiment (ACE). Because of the limitations that result from the use of simulated data, we have tested our retrieval algorithm using ATMOS spectra in different filter regions and present here the aerosol parameters obtained.     

Alternative statistical methods for spectral data processing: applications to laser-induced breakdown spectroscopy of gaseous and aerosol systems

A new spectral data processing scheme based on the standard deviation of collected spectra is compared with the traditional ensemble-averaging of laser-induced breakdown spectroscopy (LIBS)-based spectral data for homogenous (i.e., pure gas phase) systems and with a LIBS-based traditional conditional spectral analysis scheme for non-homogenous (e.g., aerosol system) analyte systems under discrete particle loadings. The range of conditions enables quantitative assessment of the analytical approaches under carefully controlled experimental conditions. In the homogeneous system with gaseous carbon dioxide producing the carbon atomic emission signal, the standard deviation method provided a suitable metric that is directly proportional to the analyte signal and compares favorably with a traditional ensemble averaging scheme. In contrast, the applicability of the standard deviation method for analysis of non-homogenous analyte systems (e.g., aerosol systems) must be carefully considered. It was shown both experimentally and via Monte Carlo simulations that the standard deviation approach can produce an analyte response that is monotonic with analyte concentration up to a point at which the analyte signal starts to transition from a non-homogeneous system to a homogeneous systems (i.e., around a 50% sampling point for aerosol particles). In addition, the standard deviation spectrum is capable of revealing spectral locations of non-homogeneously dispersed analyte species without a priori knowledge.     

In situ measurements of H2O from a stratospheric balloon by diode laser direct-differential absorption spectroscopy at 1.39 microm

A distributed-feedback InGaAs laser diode emitting near 1.393 mum is used in conjunction with an optical multipass cell that is open to the atmosphere to yield ambient water-vapor measurements by infrared absorption spectroscopy. To obtain the high dynamic range for the measurements that is required for continuous water-vapor monitoring in the upper troposphere and the lower stratosphere, we used a simple circuit that combined differential and direct detection. Furthermore, the laser emission wavelength was tuned to balance the steep decrease in H(2)O concentration with altitude by sweeping molecular transitions of stronger line strengths. The technique was implemented by use of the Spectromètre à Diodes Laser Accordables (SDLA), a tunable diode laser spectrometer operated from a stratospheric balloon. Absorption spectra of H(2)O in the 5-30-km altitude range obtained at 1-s intervals during recent balloon flights are reported. Water-vapor mixing ratios were retrieved from the absorption spectra by a fit to the full molecular line shape in conjunction with in situ pressure and temperature measurements, with a precision error ranging from 5% to 10%.