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Aerosols and clouds play central roles in atmospheric chemistry and physics,climate, air pollution, and public health. The mechanistic understanding andpredictability of aerosol and cloud properties, interactions,transformations, and effects are, however, still very limited. This is duenot only to the limited availability of measurement data, but also to thelimited applicability and compatibility of model formalisms used for theanalysis, interpretation, and description of heterogeneous and multiphaseprocesses. To support the investigation and elucidation of atmosphericaerosol and cloud surface chemistry and gas-particle interactions, wepresent a comprehensive kinetic model framework with consistent andunambiguous terminology and universally applicable rate equations andparameters. It enables a detailed description of mass transport and chemical reactions atthe gas-particle interface, and it allows linking aerosol and cloud surface processeswith gas phase and particle bulk processes in systems with multiple chemicalcomponents and competing physicochemical processes.  The key elements and essential aspects of the presented framework are: asimple and descriptive double-layer surface model (sorption layer andquasi-static layer); straightforward flux-based mass balance and rateequations; clear separation of mass transport and chemical reactions;well-defined and consistent rate parameters (uptake and accommodation coefficients,reaction and transport rate coefficients); clear distinction between gasphase, gas-surface, and surface-bulk transport (gas phase diffusion, surface and bulk accommodation); clear distinction betweengas-surface, surface layer, and surface-bulk reactions (Langmuir-Hinshelwoodand Eley-Rideal mechanisms); mechanistic description of concentration andtime dependences (transient and steady-state conditions); flexible addition of unlimited numbers of chemical species andphysicochemical processes; optional aggregation or resolution of intermediatespecies, sequential processes, and surface layers; and full compatibility with traditional resistor model formulations.The outlined double-layer surface concept and formalisms represent a minimumof model complexity required for a consistent description of the non-linearconcentration and time dependences observed in experimental studies ofatmospheric multiphase processes (competitive co-adsorption and surfacesaturation effects, etc.). Exemplary practical applications and modelcalculations illustrating the relevance of the above aspects are presented ina companion paper (Ammann and Pöschl, 2007).We expect that the presented model framework will serve as a useful tool andbasis for experimental and theoretical studies investigating and describingatmospheric aerosol and cloud surface chemistry and gas-particleinteractions. It shall help to end the "Babylonian confusion" that seems toinhibit scientific progress in the understanding of heterogeneous chemicalreactions and other multiphase processes in aerosols and clouds. Inparticular, it shall support the planning and design of laboratoryexperiments for the elucidation and determination of fundamental kineticparameters; the establishment, evaluation, and quality assurance ofcomprehensive and self-consistent collections of rate parameters; and thedevelopment of detailed master mechanisms for process models and derivationof simplified but yet realistic parameterizations for atmospheric and climatemodels

Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions – Part 1: General equations, parameters, and terminology