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At least 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

On the calculation of internal forces in mechanically stressed polyatomic molecules

We discuss how to define and to compute internal forces in a molecule subjected to mechanical stress. Because of the inherently many-body character of intramolecular interactions, internal forces cannot be uniquely defined without specifying a set of internal coordinates used to describe the molecular structure. When such a set is comprised of 3N − 6 interactomic distances (N being the number of atoms) and includes the bond lengths of interest, we show that the associated forces, while satisfying the equation F = ∂V/∂R (where R is the bond length, F is the internal force in this bond, and V is the potential energy of the molecule), can be determined from the molecular geometry alone. We illustrate these ideas using several toy models ranging from small molecules to a graphene sheet and show that the magnitude of the internal force in a bond is not necessarily a good predictor of its strength in response to mechanical loading. At the same time, analysis of internal forces reveals interesting phenomena such as the force multiplication effect, where weak external forces may, e.g., be used to break strong bonds, and offers insight into the catch-bond phenomenon where chemical reactivity is suppressed through application of a force.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Configurational forces in electronic structure calculations using Kohn-Sham density functional theory

Here we derive the expressions for configurational forces in Kohn-Sham density functional theory, which correspond to the generalized variational force computed as the derivative of the Kohn-Sham energy functional with respect to the position of a material point x. These configurational forces that result from the inner variations of the Kohn-Sham energy functional provide a unified framework to compute atomic forces as well as stress tensor for geometry optimization. Importantly, owing to the variational nature of the formulation, these configurational forces inherently account for the Pulay corrections. The formulation presented in this work treats both pseudopotential and all-electron calculations in a single framework, and employs a local variational real-space formulation of Kohn-Sham density functional theory (DFT) expressed in terms of the nonorthogonal wave functions that is amenable to reduced-order scaling techniques. We demonstrate the accuracy and performance of the proposed configurational force approach on benchmark all-electron and pseudopotential calculations conducted using higher-order finite-element discretization. To this end, we examine the rates of convergence of the finite-element discretization in the computed forces and stresses for various materials systems, and, further, verify the accuracy from finite differencing the energy. Wherever applicable, we also compare the forces and stresses with those obtained from Kohn-Sham DFT calculations employing plane-wave basis (pseudopotential calculations) and Gaussian basis (all-electron calculations). Finally, we verify the accuracy of the forces on large materials systems involving a metallic aluminum nanocluster containing 666 atoms and an alkane chain containing 902 atoms, where the Kohn-Sham electronic ground state is computed using a reduced-order scaling subspace projection technique

36 MATERIALS SCIENCE↗
DOE OSTI2024

Neural Networks to Find the Optimal Forcing for Offsetting the Anthropogenic Climate Change Effects

Abstract Of great relevance to climate engineering is the systematic relationship between the radiative forcing to the climate system and the response of the system, a relationship often represented by the linear response function (LRF) of the system. However, estimating the LRF often becomes an ill-posed inverse problem due to high-dimensionality and nonunique relationships between the forcing and response. Recent advances in machine learning make it possible to address the ill-posed inverse problem through regularization and sparse system fitting. Here, we develop a convolutional neural network (CNN) for regularized inversion. The CNN is trained using the surface temperature responses from a set of Green’s function perturbation experiments as imagery input data together with data sample densification. The resulting CNN model can infer the forcing pattern responsible for the temperature response from out-of-sample forcing scenarios. This promising proof of concept suggests a possible strategy for estimating the optimal forcing to negate certain undesirable effects of climate change. The limited success of this effort underscores the challenges of solving an inverse problem for a climate system with inherent nonlinearity. Significance Statement Predicting the climate response for a given climate forcing is a direct problem, while inferring the forcing for a given desired climate response is often an inverse, ill-posed, problem, posing a new challenge to the climate community. This study makes the first attempt to infer the radiative forcing for a given target pattern of global surface temperature response using a deep learning approach. The resulting deeply trained convolutional neural network inversion model shows promise in capturing the forcing pattern corresponding to a given surface temperature response, with a significant implication on the design of an optimal solar radiation management strategy for curbing global warming. This study also highlights the technical challenges that future research should prioritize in seeking feasible solutions to the inverse climate problem.

Ren, Huiying↗
DOE OSTI2025

The Relative Importance of Forced and Unforced Temperature Patterns in Driving the Time Variation of Low-Cloud Feedback

Abstract Atmospheric models forced with observed sea surface temperatures (SSTs) suggest a trend toward a more-stabilizing cloud feedback in recent decades, partly due to the surface cooling trend in the eastern Pacific (EP) and the warming trend in the western Pacific (WP). Here, we show model evidence that the low-cloud feedback has contributions from both forced and unforced feedback components and that its time variation arises in large part through changes in the relative importance of the two over time, rather than through variations in forced or unforced feedbacks themselves. Initial-condition large ensembles (LEs) suggest that the SST patterns are dominated by unforced variations for 30-yr windows ending prior to the 1980s. In general, unforced SSTs are representative of an ENSO-like pattern, which corresponds to weak low-level stability in the tropics and less-stabilizing low-cloud feedback. Since the 1980s, the forced signals have become stronger, outweighing the unforced signals for the 30-yr windows ending after the 2010s. Forced SSTs are characterized by relatively uniform warming with an enhancement in the WP, corresponding to a more-stabilizing low-cloud feedback in most cases. The time-evolving SST pattern due to this increasing importance of forced signals is the dominant contributor to the recent stabilizing shift of low-cloud feedback in the LEs. Using single-forcing LEs, we further find that if only greenhouse gases evolve with time, the transition to the domination of forced signals occurs 10–20 years earlier compared to the LEs with full forcings, which can be understood through the compensating effect between aerosols and greenhouse gases.

58 GEOSCIENCES↗
DOE OSTI2017

Status Report on Activities of the Systems Assessment Task Force, OECD-NEA Expert Group on Accident Tolerant Fuels for LWRs

The Organization for Economic Cooperation and Development /Nuclear Energy Agency (OECD/NEA) Nuclear Science Committee approved the formation of an Expert Group on Accident Tolerant Fuel (ATF) for LWRs (EGATFL) in 2014. Chaired by Kemal Pasamehmetoglu, INL Associate Laboratory Director for Nuclear Science and Technology, the mandate for the EGATFL defines work under three task forces: (1) Systems Assessment, (2) Cladding and Core Materials, and (3) Fuel Concepts. Scope for the Systems Assessment task force (TF1) includes definition of evaluation metrics for ATF, technology readiness level definition, definition of illustrative scenarios for ATF evaluation, and identification of fuel performance and system codes applicable to ATF evaluation. The identification of irradiation facilities around the world that are being used, or are planned to be used, for the irradiation testing of ATF cladding and fuel materials was later added to the TF1 scope (April 2017). The Cladding and Core Materials (TF2) and Fuel Concepts (TF3) task forces have worked to identify gaps and needs for modeling and experimental demonstration; define key properties of interest; identify the data necessary to perform concept evaluation under normal conditions and illustrative scenarios; identify available infrastructure (internationally) to support experimental needs; and make recommendations on priorities. Where possible, considering proprietary and other export restrictions (e.g., International Traffic in Arms Regulations), the Expert Group has facilitated the sharing of data and lessons learned across the international group membership. The Systems Assessment task force is chaired by Shannon Bragg-Sitton (Idaho National Laboratory [INL], U.S.), the Cladding Task Force is chaired by Marie Moatti (Electricite de France [EdF], France), and the Fuels Task Force is chaired by a Masaki Kurata (Japan Atomic Energy Agency [JAEA], Japan). The original Expert Group mandate was established for June 2014 to June 2016. In April 2016 the Expert Group voted to extend the mandate one additional year to June 2017 in order to complete the task force deliverables; this request was subsequently approved by the Nuclear Science Committee. All reports are currently in final draft and will be submitted to NEA for final formatting/editing in October 2017. A final EGATFL meeting will be held at NEA Headquarters in Paris, France on November 2-3, 2017 to resolve any final comments on the task force reports. This report provides brief summary of the Systems Assessment Task Force deliverable report.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Robust global detection of forced changes in mean and extreme precipitation despite observational disagreement on the magnitude of change

Detection and attribution (D&A) of forced precipitation change are challenging due to internal variability, limited spatial, and temporal coverage of observational records and model uncertainty. These factors result in a low signal-to-noise ratio of potential regional and even global trends. Here, we use a statistical method – ridge regression – to create physically interpretable fingerprints for the detection of forced changes in mean and extreme precipitation with a high signal-to-noise ratio. The fingerprints are constructed using Coupled Model Intercomparison Project phase 6 (CMIP6) multi-model output masked to match coverage of three gridded precipitation observational datasets – GHCNDEX, HadEX3, and GPCC – and are then applied to these observational datasets to assess the degree of forced change detectable in the real-world climate in the period 1951–2020. We show that the signature of forced change is detected in all three observational datasets for global metrics of mean and extreme precipitation. Forced changes are still detectable from changes in the spatial patterns of precipitation even if the global mean trend is removed from the data. This shows the detection of forced change in mean and extreme precipitation beyond a global mean trend is robust and increases confidence in the detection method's power as well as in climate models' ability to capture the relevant processes that contribute to large-scale patterns of change. We also find, however, that detectability depends on the observational dataset used. Not only coverage differences but also observational uncertainty contribute to dataset disagreement, exemplified by the times of emergence of forced change from internal variability ranging from 1998 to 2004 among datasets. Furthermore, different choices for the period over which the forced trend is computed result in different levels of agreement between observations and model projections. These sensitivities may explain apparent contradictions in recent studies on whether models under- or overestimate the observed forced increase in mean and extreme precipitation. Lastly, the detection fingerprints are found to rely primarily on the signal in the extratropical Northern Hemisphere, which is at least partly due to observational coverage but potentially also due to the presence of a more robust signal in the Northern Hemisphere in general.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

The Radiative Forcing Model Intercomparison Project (RFMIP): Experimental protocol for CMIP6

The phrasing of the first of three questions motivating CMIP6 – “How does the Earth system respond to forcing?” – suggests that forcing is always well-known, yet the radiative forcing to which this question refers has historically been uncertain in coordinated experiments even as understanding of how best to infer radiative forcing has evolved. The Radiative Forcing Model Intercomparison Project (RFMIP) endorsed by CMIP6 seeks to provide a foundation for answering the question through three related activities: (i) accurate characterization of the effective radiative forcing relative to a near-preindustrial baseline and careful diagnosis of the components of this forcing; (ii) assessment of the absolute accuracy of clear-sky radiative transfer parameterizations against reference models on the global scales relevant for climate modeling; and (iii) identification of robust model responses to tightly specified aerosol radiative forcing from 1850 to present. Complete characterization of effective radiative forcing can be accomplished with 180 years (Tier 1) of atmosphere-only simulation using a sea-surface temperature and sea ice concentration climatology derived from the host model's preindustrial control simulation. Assessment of parameterization error requires trivial amounts of computation but the development of small amounts of infrastructure: new, spectrally detailed diagnostic output requested as two snapshots at present-day and preindustrial conditions, and results from the model's radiation code applied to specified atmospheric conditions. In conclusion, the search for robust responses to aerosol changes relies on the CMIP6 specification of anthropogenic aerosol properties; models using this specification can contribute to RFMIP with no additional simulation, while those using a full aerosol model are requested to perform at least one and up to four 165-year coupled ocean–atmosphere simulations at Tier 1.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1987

Mean fields induced by local gravity-wave forcing in the middle atmosphere

The role of geostrophic adjustment in the middle atmosphere for given wave packet forcing by a three-dimensional hydrostatic model is examined. It is shown that the induced fields consist of two different kinds of modes. One, produced by forcing vorticity only, is steady quasi-geostrophic flow; this is restricted to the forcing region. The other, produced by both forcing vorticity and forcing divergence, is oscillatory, and is in the form of gravity waves propagating out of the forcing region plus inertial oscillations in the forcing region. The scales and amplitudes of the induced gravity waves are determined by the forcing. For a typical example, a 200 km x 200 km gravity wave packet of momentum flux 0.5 N/sq m absorbed in a layer of 5 km thickness centered near 18 km altitude, the gravity waves spread to a larger region about 1000 km x 1000 km at a level 7 km above the forcing region. At that level, the horizontal and vertical wavelengths of the induced waves are about 300 km and 7 km respectively, and the momentum flux is substantially reduced to 0.0004 N/sq m. The results suggest that geostrophic adjustment processes may play an important role in specifying the gravity wave spectrum in the middle atmosphere.

Zhu, Xun↗
NASA NTRS1989

Influence of impeller shroud forces on turbopump rotor dynamics

The shrouded-impeller leakage path forces calculated by Childs (1987) have been analyzed to answer two questions. First, because of certain characteristics of the results of Childs, the forces could not be modeled with traditional approaches. Therefore, an approach has been devised to include the forces in conventional rotordynamic analyses. The forces were approximated by traditional stiffness, damping and inertia coefficients with the addition of whirl-frequency-dependent direct and cross-coupled stiffness terms. The forces were found to be well-modeled with this approach. Finally, the effect these forces had on a simple rotor-bearing system was analyzed, and, therefore, they, in addition to seal forces, were applied to a Jeffcott rotor. The traditional methods of dynamic system analysis were modified to incorporate the impeller forces and yielded results for the eigenproblem, frequency response, critical speed, transient response and an iterative technique for finding the frequency of free vibration as well as system stability. All results lead to the conclusion that the forces have little influence on natural frequency but can have appreciable effects on system stability. Specifically, at higher values of fluid swirl at the leakage path entrance, relative stability is reduced. The only unexpected response characteristics that occurred are attributed to the nonlinearity of the model.

Williams, Jim P.↗
NASA NTRS1992

A comparison of force control algorithms for robots in contact with flexible environments

In order to perform useful tasks, the robot end-effector must come into contact with its environment. For such tasks, force feedback is frequently used to control the interaction forces. Control of these forces is complicated by the fact that the flexibility of the environment affects the stability of the force control algorithm. Because of the wide variety of different materials present in everyday environments, it is necessary to gain an understanding of how environmental flexibility affects the stability of force control algorithms. This report presents the theory and experimental results of two force control algorithms: Position Accommodation Control and Direct Force Servoing. The implementation of each of these algorithms on a two-arm robotic test bed located in the Center for Intelligent Robotic Systems for Space Exploration (CIRSSE) is discussed in detail. The behavior of each algorithm when contacting materials of different flexibility is experimentally determined. In addition, several robustness improvements to the Direct Force Servoing algorithm are suggested and experimentally verified. Finally, a qualitative comparison of the force control algorithms is provided, along with a description of a general tuning process for each control method.

Wilfinger, Lee S.↗
NASA NTRS1993

Force reflection with compliance control

Two types of systems for force-reflecting control, which enables high force-reflection gain, are presented: position-error-based force reflection and low-pass-filtered force reflection. Both of the systems are combined with shared compliance control. In the position-error-based class, the position error between the commanded and the actual position of a compliantly controlled robot is used to provide force reflection. In the low-pass-filtered force reflection class, the low-pass-filtered output of the compliance control is used to provide force reflection. The increase in force reflection gain can be more than 10-fold as compared to a conventional high-bandwidth pure force reflection system, when high compliance values are used for the compliance control.

Kim, Won S.↗
NASA NTRS1991

Manual discrimination of force

Optimal design of human-machine interfaces for teleoperators and virtual-environment systems which involve the tactual and kinesthetic modalities requires knowledge of the human's resolving power in these modalities. The resolution of the interface should be appropriately matched to that of the human operator. We report some preliminary results on the ability of the human hand to distinguish small differences in force under a variety of conditions. Experiments were conducted on force discrimination with the thumb pushing an interface that exerts a constant force over the pushing distance and the index finger pressing against a fixed support. The dependence of the sensitivity index d' on force increment can be fit by a straight line through the origin and the just-noticeable difference (JND) in force can thus be described by the inverse of the slope of this line. The receiver operating characteristic (ROC) was measured by varying the a priori probabilities of the two alternatives, reference force and reference force plus an increment, in one-interval, two-alternative, forced-choice experiments. When plotted on normal deviate coordinates, the ROC's were roughly straight lines of unit slope, thus supporting the assumption of equal-variance normal distributions and the use of the conventional d' measure. The JND was roughly 6-8 percent for reference force ranging from 2.5 to 10 newtons, pushing distance from 5 to 30 mm, and initial finger-span from 45 to 125 mm. Also, the JND remained the same when the subjects were instructed to change the average speed of pushing from 23 to 153 mm/sec. The pushing was terminated by reaching either a wall or a well, and the JND's were essentially the same in both cases.

Pang, Xiao-Dong↗
NASA NTRS1993

Accurate Quartic Force Fields and Vibrational Frequencies for HCN and HNC

The quartic force fields of HCN and HNC are determined using atomic natural orbital one-particle basis sets of spdf/spd and spdfg/spdf quality in conjunction with the CCSD(T) electron correlation method (singles and doubles coupled-cluster theory plus a perturbational estimate of the effects of connected triple excitations). The HCN force field is in good agreement with a recent experimentally derived force field and also with the force field recently computed by Wong and Bacskay. On the basis of the good agreement obtained for HCN, it is argued that the ab initio quartic force field for HNC is superior to a prior force field derived from experiment. The harmonic frequencies of HNC are predicted to be 3822 +/- 10,472 +/- 5, and 2051 +/-10/cm for omega1, omega2, and omega3, respectively; the experimentally derived values are above these values and fall outside the estimated uncertainties. Using the quartic force field, spectroscopic constants are predicted for HNC based on a vibrational second-order perturbation theory analysis. It is also asserted that the gas-phase fundamental v(sub 3) for HNC is slightly lower than the matrix isolation value. The range of validity of the quartic force fields is investigated by comparison of variational vibrational energies computed with the quartic force fields to those obtained from our recently reported global HCN/HNC potential energy surface and also to experimental data.

Lee, Timothy J.↗
NASA NTRS1993

Accurate Quartic Force Fields and Vibrational Frequencies for HCN and HNC

The quartic force fields of HCN and HNC are determined using atomic natural orbital one-particle basis sets of spdf/spd and spdfg/spdf quality in conjunction with the CCSD(T) electron correlation method (singles and doubles coupled-cluster theory plus a perturbation estimate of the effects of connected triple excitations). The HCN force field is in good agreement with a recent experimentally derived force field and also with the force field recently computed by Wong and Bacskay. On the basis of the good agreement obtained for HCN, it is argued that the ab initio quartic force field for HNC is superior to a prior force field derived from experiment. The harmonic frequencies of HNC are predicted to be 3822 +/- 10, 472 +/- 5, and 2051 +/- 10 cm(exp -1) for omega(sub 1), omega(sub 2), and omega(sub 3), respectively; the experimentally derived values are above these values and fall outside the estimated uncertainties. Using the quartic force field, spectroscopic constants are predicted for HNC based on a vibrational second-order perturbation theory analysis. It is also asserted that the gas-phase fundamental nu(sub 3) for HNC is slightly lower than the matrix isolation value. The range of validity of the quartic force fields is investigated by comparison of variational vibrational energies computed with the quartic force fields to those obtained from our recently reported global HCN/HNC potential energy surface and also to experimental data.

Lee, Timothy J.↗
NASA NTRS1997

Infrared Radiative Forcing and Atmospheric Lifetimes of Trace Species Based on Observations from UARS

Observations from instruments on the Upper Atmosphere Research Satellite (UARS) have been used to constrain calculations of infrared radiative forcing by CH4, CCl2F2 and N2O, and to determine lifetimes Of CCl2F2 and N2O- Radiative forcing is calculated as a change in net infrared flux at the tropopause that results from an increase in trace gas amount from pre-industrial (1750) to contemporary (1992) times. Latitudinal and seasonal variations are considered explicitly, using distributions of trace gases and temperature in the stratosphere from UARS measurements and seasonally averaged cloud statistics from the International Satellite Cloud Climatology Project. Top-of-atmosphere fluxes calculated for the contemporary period are in good agreement with satellite measurements from the Earth Radiation Budget Experiment. Globally averaged values of the radiative forcing are 0.536, 0.125, and 0.108 W m-2 for CH4, CCl2F2, and N2O, respectively. The largest forcing occurs near subtropical latitudes during summer, predominantly as a result of the combination of cloud-free skies and a high, cold tropopause. Clouds are found to play a significant role in regulating infrared forcing, reducing the magnitude of the forcing by 30-40% compared to the case of clear skies. The vertical profile of CCl2F2 is important in determining its radiative forcing; use of a height-independent mixing ratio in the stratosphere leads to an over prediction of the forcing by 10%. The impact of stratospheric profiles on radiative forcing by CH4 and N2O is less than 2%. UARS-based distributions of CCl2F2 and N2O are used also to determine global destruction rates and instantaneous lifetimes of these gases. Rates of photolytic destruction in the stratosphere are calculated using solar ultraviolet irradiances measured on UARS and a line-by-line model of absorption in the oxygen Schumann-Runge bands. Lifetimes are 114 +/- 22 and 118 +/- 25 years for CCl2F2 and N2O, respectively.

Minschwaner, K.↗
NASA NTRS2003

Task III: Development of an Effective Computational Methodology for Body Force Representation of High-speed Rotor 37

A framework for an effective computational methodology for characterizing the stability and the impact of distortion in high-speed multi-stage compressor is being developed. The methodology consists of using a few isolated-blade row Navier-Stokes solutions for each blade row to construct a body force database. The purpose of the body force database is to replace each blade row in a multi-stage compressor by a body force distribution to produce same pressure rise and flow turning. To do this, each body force database is generated in such a way that it can respond to the changes in local flow conditions. Once the database is generated, no hrther Navier-Stokes computations are necessary. The process is repeated for every blade row in the multi-stage compressor. The body forces are then embedded as source terms in an Euler solver. The method is developed to have the capability to compute the performance in a flow that has radial as well as circumferential non-uniformity with a length scale larger than a blade pitch; thus it can potentially be used to characterize the stability of a compressor under design. It is these two latter features as well as the accompanying procedure to obtain the body force representation that distinguish the present methodology from the streamline curvature method. The overall computational procedures have been developed. A dimensional analysis was carried out to determine the local flow conditions for parameterizing the magnitudes of the local body force representation of blade rows. An Euler solver was modified to embed the body forces as source terms. The results from the dimensional analysis show that the body forces can be parameterized in terms of the two relative flow angles, the relative Mach number, and the Reynolds number. For flow in a high-speed transonic blade row, they can be parameterized in terms of the local relative Mach number alone.

Tan, Choon-Sooi↗
NASA NTRS2000

Influence of central set on anticipatory and triggered grip-force adjustments

The effects of predictability of load magnitude on anticipatory and triggered grip-force adjustments were studied as nine normal subjects used a precision grip to lift, hold, and replace an instrumented test object. Experience with a predictable stimulus has been shown to enhance magnitude scaling of triggered postural responses to different amplitudes of perturbations. However, this phenomenon, known as a central-set effect, has not been tested systematically for grip-force responses in the hand. In our study, predictability was manipulated by applying load perturbations of different magnitudes to the test object under conditions in which the upcoming load magnitude was presented repeatedly or under conditions in which the load magnitudes were presented randomly, each with two different pre-load grip conditions (unconstrained and constrained). In constrained conditions, initial grip forces were maintained near the minimum level necessary to prevent pre-loaded object slippage, while in unconstrained conditions, no initial grip force restrictions were imposed. The effect of predictable (blocked) and unpredictable (random) load presentations on scaling of anticipatory and triggered grip responses was tested by comparing the slopes of linear regressions between the imposed load and grip response magnitude. Anticipatory and triggered grip force responses were scaled to load magnitude in all conditions. However, regardless of pre-load grip force constraint, the gains (slopes) of grip responses relative to load magnitudes were greater when the magnitude of the upcoming load was predictable than when the load increase was unpredictable. In addition, a central-set effect was evidenced by the fewer number of drop trials in the predictable relative to unpredictable load conditions. Pre-load grip forces showed the greatest set effects. However, grip responses showed larger set effects, based on prediction, when pre-load grip force was constrained to lower levels. These results suggest that anticipatory processes pertaining to load magnitude permit the response gain of both voluntary and triggered rapid grip force adjustments to be set, at least partially, prior to perturbation onset. Comparison of anticipatory set effects for reactive torque and lower extremity EMG postural responses triggered by surface translation perturbations suggests a more general rule governing anticipatory processes.

Non-NASA Center↗
NASA NTRS2005

Global Impacts of Gas-Phase Chemistry-Aerosol Interactions on Direct Radiative Forcing by Anthropogenic Aerosols and Ozone

We present here a first global modeling study on the influence of gas-phase chemistry/aerosol interactions on estimates of anthropogenic forcing by tropospheric O3 and aerosols. Concentrations of gas-phase species and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols in the preindustrial, present-day, and year 2100 (IPCC SRES A2) atmospheres are simulated online in the Goddard Institute for Space Studies general circulation model II' (GISS GCM II'). With fully coupled chemistry and aerosols, the preindustrial, presentday, and year 2100 global burdens of tropospheric ozone are predicted to be 190, 319, and 519 Tg, respectively. The burdens of sulfate, nitrate, black carbon, and organic carbon are predicted respectively to be 0.32. 0.18, 0.01, 0.33 Tg in preindustrial time, 1.40, 0.48, 0.23, 1.60 Tg in presentday, and 1.37, 1.97, 0.54, 3.31 Tg in year 2100. Anthropogenic O3 is predicted to have a globally and annually averaged present-day forcing of +0.22 W m(sup -2) and year 2100 forcing of +0.57 W m(sup -2) at the top of the atmosphere (TOA). Net anthropogenic TOA forcing by internally mixed sulfate, nitrate, organic carbon, and black carbon aerosols is estimated to be virtually zero in the present-day and +0.34 W m(sup -2) in year 2100, whereas it is predicted to be -0.39 W m(sup -2) in present-day and -0.61 W m(sup -2) in year 2100 if the aerosols are externally mixed. Heterogeneous reactions are shown to be important in affecting anthropogenic forcing. When reactions of N2O5, NO3, NO2, and HO2 on aerosols are accounted for, TOA anthropogenic O3 forcing is less by 20-45% in present-day and by 20-32% in year 2100 at mid to high latitudes in the Northern Hemisphere, as compared with values predicted in the absence of heterogeneous gas aerosol reactions. Mineral dust uptake of HNO3 and O3 is shown to have practically no influence on anthropogenic O3 forcing. Heterogeneous reactions of N2Os, NO3, NO2, and HO2 are predicted to have noticeable impacts on anthropogenic aerosol forcing over industrialized areas, leading to 0-2 W m(sup -2) more anthropogenic aerosol cooling in present-day and 2-8 W m(sup -2) more cooling in year 2100 in these areas as compared with forcings calculated in the absence of heterogeneous reactions. Sea salt uptake of SO2 reduces the magnitude of TOA aerosol cooling by 0.5-1 W m(sup -2) over the oceans around 60 N in the present-day and year 2100 scenarios. Near dust sources, mineral dust uptake of SO2 and HNO3 leads to less anthropogenic aerosol cooling by 0.5-1 W m(sup -2) in the present day and 1-2 W m(sup -2) in year 2100.

Liao, Hong↗