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Our expanding understanding of the brain at the level of neurons and synapses, and the level of cognitive phenomena such as language, leaves a formidable gap between these two scales. Here we introduce a computational system which promises to bridge this gap: the Assembly Calculus. It encompasses operations on assemblies of neurons, such as project, associate, and merge, which appear to be implicated in cognitive phenomena, and can be shown, analytically as well as through simulations, to be plausibly realizable at the level of neurons and synapses. We demonstrate the reach of this system by proposing a brain architecture for syntactic processing in the production of language, compatible with recent experimental results. Abstract Assemblies are large populations of neurons believed to imprint memories, concepts, words, and other cognitive information. We identify a repertoire of operations on assemblies. These operations correspond to properties of assemblies observed in experiments, and can be shown, analytically and through simulations, to be realizable by generic, randomly connected populations of neurons with Hebbian plasticity and inhibition. Assemblies and their operations constitute a computational model of the brain which we call the Assembly Calculus, occupying a level of detail intermediate between the level of spiking neurons and synapses and that of the whole brain. The resulting computational system can be shown, under assumptions, to be, in principle, capable of carrying out arbitrary computations. We hypothesize that something like it may underlie higher human cognitive functions such as reasoning, planning, and language. In particular, we propose a plausible brain architecture based on assemblies for implementing the syntactic processing of language in cortex, which is consistent with recent experimental results.