Keith E. Grant

SUNDIALS: Suite of nonlinear and differential/algebraic equation solvers

SUNDIALS is a suite of advanced computational codes for solving large-scale problems that can be modeled as a system of nonlinear algebraic equations, or as initial-value problems in ordinary differential or differential-algebraic equations. The basic versions of these codes are called KINSOL, CVODE, and IDA, respectively. The codes are written in ANSI standard C and are suitable for either serial or parallel machine environments. Common and notable features of these codes include inexact Newton-Krylov methods for solving large-scale nonlinear systems; linear multistep methods for time-dependent problems; a highly modular structure to allow incorporation of different preconditioning and/or linear solver methods; and clear interfaces allowing for users to provide their own data structures underneath the solvers. We describe the current capabilities of the codes, along with some of the algorithms and heuristics used to achieve efficiency and robustness. We also describe how the codes stem from previous and widely used Fortran 77 solvers, and how the codes have been augmented with forward and adjoint methods for carrying out first-order sensitivity analysis with respect to model parameters or initial conditions.

Cloud susceptibility and the first aerosol indirect forcing: Sensitivity to black carbon and aerosol concentrations

[1] Present-day global anthropogenic emissions contribute more than half of the mass in submicron particles primarily due to sulfate and carbonaceous aerosol components derived from fossil fuel combustion and biomass burning. These anthropogenic aerosols increase cloud drop number concentration and cloud albedo. Here, we use an improved version of the fully coupled climate/chemistry models to investigate cloud susceptibility and the first indirect effect of anthropogenic aerosols (the Twomey effect). We examine the correspondence between the model simulation of cloud susceptibility and that inferred from satellite measurements to test whether our simulated aerosol concentrations and aerosol/cloud interactions give a faithful representation of these features. This comparison provides an overall measure of the adequacy of cloud cover and drop concentrations. We also address the impact of black carbon absorption in clouds on the first indirect forcing and examine the sensitivity of the forcing to different representations of natural aerosols. We find that including this absorption does not change the global forcing by more than 0.07 W m � 2 , but that locally it could decrease the forcing by as much as 0.7 W m � 2 in regions where black carbon emissions are pronounced. Because of the nonlinear relationship between cloud drop number and aerosol number concentrations, the total forcing does not equal the sum of the forcing from each individual source. Our estimated total first indirect forcing is � 1.85 W m � 2 , with � 0.30 W m � 2 associated with anthropogenic sulfate, � 1.16 W m � 2 associated with carbonaceous aerosols from biomass burning, and � 0.52 W m � 2 associated with carbonaceous aerosols from fossil fuel combustion. Estimates of forcing by sulfate and total carbonaceous aerosols increase to � 0.31 and � 1.67 W m � 2 , respectively, if natural emissions of organic aerosols are only 8.4 Tg yr � 1 , but decrease to � 0.26 and � 1.27 W m � 2 if they are as large as 42 Tg yr � 1 . Even larger estimates of forcing are derived if dust and sea-salt emissions are not included. The effect of aerosol abundance on cloud life cycle may be important but is not treated in this study. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0320 Atmospheric Composition and Structure: Cloud physics and chemistry; 1610 Global Change: Atmosphere (0315, 0325)

The chemical and radiative effects of the Mount Pinatubo eruption

The eruption of Mount Pinatubo introduced large amounts of sulfur-containing particles into the stratosphere. Stratospheric ozone measured by ozonesondes and satellites is significantly lower following the June 1991 eruption and throughout 1992 and 1993. To clarify the mechanisms leading to effects on stratospheric ozone, time-dependent stratospheric aerosol and gas experiment II (SAGE II) and cryogenic limb array elaton spectrometer (CLAES) aerosol optical extinction data and SAGE II surface area density are used as parameters in a two-dimensional (2-D) zonally averaged chemical radiative transport model. The model was integrated with time from before the eruption through December 1993. The modeled impact on global ozone results from increased rates of heterogeneous reactions on sulfate aerosols and from the increased radiative heating and scattering caused by these aerosols. The models dynamical response to changes in forcing (from changes in radiatively active trace gas concentrations and from aerosol heating) is treated in one of three ways: (1) the stratospheric temperature is perturbed, with fixed seasonal circulation, (2) the circulation is perturbed, with fixed seasonal temperature, or (3) both circulation and temperature are unperturbed, when investigating only the impact of Mount Pinatubo increased aerosol surface area density (SAD) and aerosol scattering of actinic solar radiation, When the aerosol heating is allowed to modify the temperature distribution, the maximum change calculated in equatorial column ozone is −1.6%. The calculated equatorial temperature change and peak local ozone change in October 1991 are +6 K and −4%, respectively. When aerosol heating perturbs the circulation in the model, the maximum change in equatorial column ozone is −6%. Increased heterogeneous processing on sulfate aerosols is calculated to have changed equatorial column ozone in late 1991 by −1.5%. Global column ozone in the model in 1992 and 1993 changed by −2.8% and −2.4%, respectively. The relationship of ozone-controlling processes in the lower stratosphere is altered as well; HOx becomes the most important catalytic cycle, followed by ClOx and NOx. This is driven by significant changes in trace gas concentrations. In October 1991, lower stratospheric, equatorial NOx decreased by 40%, ClOx increased by 60%, and HOx increased by 25%. When the effect of heterogeneous chemical processing on sulfate aerosols is combined with aerosol heating, modifying either circulation or temperature, dramatically different ozone fingerprints with time and latitude are predicted. Model-derived changes in the equatorial region in column ozone best represented the observed data when perturbed circulation was combined with heterogeneous chemical effects. However, at high latitudes, the increased ozone production from the strengthening of the mean circulation tends to cancel the heterogeneous reduction of ozone. This is not in good agreement with observed data, especially in 1992 and 1993. When the circulation is held fixed and the temperature allowed to change, and heterogeneous chemical effects are included, the equatorial ozone decrease predicted was too small for 1991. However, the mid- to high-latitude decrease in 1992 and 1993 is in better agreement with observed data.

Modeling the spectral optical properties of ammonium sulfate and biomass burning aerosols: parameterization of relative humidity effects and model results

The importance of including the global and regional radiative effects of aerosols in climate models has increasingly been realized. Accurate modeling of solar radiative forcing due to aerosols from anthropogenic sulfate and biomass burning emissions requires adequate spectral resolution and treatment of spatial and temporal variability. The variation of aerosol spectral optical properties with local relative humidity and dry aerosol composition must be considered. Because the cost of directly including Mie calculations within a climate model is prohibitive, parameterizations from offline calculations must be used. Starting from a log-normal size distribution of dry ammonium sulfate, we developed optical properties for tropospheric sulfate aerosol at 15 relative humidities up to 99 percent. The resulting aerosol size distributions were then used to calculate bulk optical properties at wavelengths between 0.175 {micro}m and 4 {micro}m. Finally, functional fits of optical properties were made for each of 12 wavelength bands as a function of relative humidity. Significant variations in optical properties occurred across the total solar spectrum. Relative increases in specific extinction and asymmetry factor with increasing relative humidity became larger at longer wavelengths. Significant variation in single-scattering albedo was found only in the longest near-IR band. This is also the band with the lowest albedo. A similar treatment was done for aerosols from biomass burning. In this case, size distributions were taken as having two carbonaceous size modes and a larger dust mode. The two carbonaceous modes were considered to be humidity dependent. Equilibrium size distributions and compositions were calculated for 15 relative humidities and five black carbon fractions. Mie calculations and Chandrasekhar averages of optical properties were done for each of the resulting 75 cases. Finally, fits were made for each of 12 spectral bands as functions of relative humidity and black carbon fraction.

The Role of Atmospheric Chemistry in Climate Change

Surface emissions and concentrations of globally important trace gases are increasing. Climate models indicate significant temperature increases could occur in the next century due to increasing CO...

Comparisons of observed ozone and temperature trends in the lower stratosphere

One result of the Ozone Assessment [WMO, 1989] is that there is a significant negative ozone trend in the lower stratosphere and upper troposphere from 1970 through 1986. In this paper we examine the relationship of this trend in ozone to that of temperature in the same altitude region utilizing a 62 station set of rawinsonde data, and compare the results to the changes in temperature determined from a radiative equilibrium model calculation. The calculated and observed trends in lower stratospheric temperature indicate substantive agreement in shape and magnitude of the vertical profiles.

Sensitivity of direct global warming potentials to key uncertainties

The concept of global warming potential was developed as a relative measure of the potential effects on climate of a greenhouse gas as compared to CO2. In this paper a series of sensitivity studies examines several uncertainties in determination of Global Warming Potentials (GWPs). For example, the original evaluation of GWPs for the Intergovernmental Panel on Climate Change (IPCC, 1990) did not attempt to account for the possible sinks of carbon dioxide (CO2) that could balance the carbon cycle and produce atmospheric concentrations of CO2 that match observations. In this study, a balanced carbon cycle model is applied in calculation of the radiative forcing from CO2. Use of the balanced model produces up to 21% enhancement of the GWPs for most trace gases compared with the IPCC (1990) values for time horizons up to 100 years, but a decreasing enhancement with longer time horizons. Uncertainty limits of the fertilization feedback parameter contribute a 20% range in GWP values. Another systematic uncertainty in GWPs is the assumption of an equilibrium atmosphere (one in which the concentration of trace gases remains constant) versus a disequilibrium atmosphere (one in which the concentration of trace gases varies with time). The latter gives GWPs that are 19 to 32% greater than the former for a 100 year time horizons, depending upon the carbon dioxide emission scenario chosen. Five scenarios are employed: constant-concentration, constant-emission past 1990 and the three IPCC (1992) emission scenarios. For the analysis of uncertainties in atmospheric lifetime (τ) the GWP changes in direct proportion toτ for short-lived gases, but to a lesser extent for gases withτ greater than the time horizontal for the GWP calculation.

The Livermore Regional Air Quality Model: I. Concept and Development

Abstract By using the Eulerian form of the mass conservation equation integrated vertically from the surface to the base of the inversion, two regional air quality models (LIRAQ-1 and LIRAQ-2) have been developed for use in the San Francisco Bay Area. The models consider the complex topography, changing meteorology and detailed source emission patterns in generating surface and vertical average pollutant concentrations with grid resolutions of 1, 2 or 5 km. The focus of LIRAQ-1 is the treatment of transport and dispersion of relatively nonreactive species, accomplished through use of a sophisticated transport prescription. The LIRAQ-2 model, employing a simpler transport scheme, treats photochemically active pollutants and incorporates a photochemical reaction set involving 19 species.

Applications of sensitivity analysis to uncertainty quantification in variably saturated flow

In this paper, we present results demonstrating the effectiveness of a sensitivity analysis approach to uncertainty quantification of a variably saturated flow model. The basis for our method is a software system which simultaneously solves for solutions of large-scale nonlinear systems of equations and the sensitivity of the solutions to selected parameters. We present test cases showing the effects on the relative uncertainty of pressure due to heterogeneity in the absolute permeability and to differences in parameterizing the Van Genuchten curve soil parameters, α and n .

Radiative forcing calculations for CH3Cl and CH3Br

Methyl chloride, CH 3 Cl, and methyl bromide, CH 3 Br, are particularly important in the global atmosphere as major natural sources of chlorine and bromine to the stratosphere. The production of these gases is dominated by natural sources, but smaller, important anthropogenic sources, such as agricultural fumigation and/or biomass burning, also exist. As absorbers of infrared radiation these gases are of interest for their potential effect on the tropospheric energy balance as well as for chemical interactions. In this study we estimate the radiative forcing and Global Warming Potentials (GWPs) of CH 3 Cl and CH 3 Br. Our calculations use an infrared radiative transfer model based on the correlated k -distribution algorithm for band absorption. Radiative forcing values of 0.0047 W/m 2 per part per billion by volume (ppbv) for CH 3 Cl in the troposphere and 0.0049 W/m 2 per ppbv for CH 3 Br in the troposphere were obtained. On a per molecule basis the radiative forcing values are about 2% of the forcing of CFC-11 and about 270 times the forcing of CO 2 . GWPs for these gases are about 8 for CH 3 Cl and about 4 for CH 3 Br (100 year time integration, CO 2 = 1). These results indicate that while CH 3 Cl and CH 3 Br have direct GWPs similar to that of CH 4 , the current emission rates are too low to contribute meaningfully to atmospheric greenhouse heating effects.