Theoretical chemists have been actively engaged for some time in processes such as ozone photodissociation, overtone photodissociation in nitric acid, pernitric acid, sulphuric acid, clusters and in small organic acids. The last of these have shown very different behaviours in the gas phase, liquid phase and importantly at the air–water interface in aqueous aerosols. The founder of molecular dynamics, B J Alder, pointed out long ago that hydrodynamic behaviour emerged when the symmetry of a random, thermalised population of hard spheres—billiard balls—was broken by a flux of energetic molecules. Despite this, efforts over two centuries to solve turbulence by finding top-down solutions to the Navier–Stokes equation have failed. It is time for theoretical chemistry to try a bottom-up solution. Gibbs free energy that drives the circulation arises from the entropy difference between the incoming low-entropy beam of visible and ultraviolet photons and the outgoing higher-entropy flux of infrared photons over the whole 4π solid angle. The role of the most energetic molecules with the highest velocities will affect the rovibrational line shapes of water, carbon dioxide and ozone in the far wings, where there is the largest effect on radiative transfer and hence on calculations of atmospheric temperature. The atmospheric state is determined by the interaction of radiation, chemistry and fluid dynamics on the microscopic scale, with propagation through the mesoscale to the macroscale. It will take theoretical chemistry to simulate that accurately. A challenging programme of research for theoretical chemistry is proposed, involving ab initio simulation by molecular dynamics of an air volume, starting in the upper stratosphere. The aim is to obtain scaling exponents for turbulence, providing a physical method for upscaling in numerical models. Turbulence affects chemistry, radiation and fluid dynamics at a fundamental, molecular level and is thus of basic concern to theoretical chemistry as it applies to the atmosphere, which consists of molecules in motion.