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Molecular simulations can help us understand fundamental processes that take place in the atmosphere. Results of three projects will be presented addressing (a) the accommodation of water vapour into ice and liquid water surfaces and the free energy profiles across these interfaces, (b) water's structure on ionic crystal surfaces, i.e. depositional ice nucleation on silver iodide and the inhibition of ice nucleation on barium fluoride, and (c) how co-emitted organic compounds can influence the water uptake of black carbon particles.