More accurate representation of aerosol-cloud interactions in warm clouds, as mediated by turbulent fluid dynamical processes such as updraft rise and entrainment, is critical to improving the overall accuracy of global models of the atmosphere. Moreover, as horizontal resolutions of global models become more varied, parameterizations must consider the length- and timescale dependence of these interactions. Thus, there is need for coincident data on aerosol, cloud microphysical, thermodynamical, and dynamical quantities over sufficient spatial and temporal extents to inform development of modern parameterizations of aerosol-cloud interactions. Large eddy simulations using detailed microphysical schemes are well poised to supply large volumes of this much needed data. Here, we describe the design and contents of a library of large eddy simulations of liquid clouds performed with the PINACLES model coupled to the Hebrew University Fast Spectral bin scheme. The simulations are initialized and forced based on observed conditions within four key global cloud regions: the eastern North Atlantic, Northeastern Pacific, continental U.S., and the Southern Ocean. The library is augmented with aerosol perturbation experiments. We characterize the coverage of the library in terms of cloud controlling factors identified in the literature and, where appropriate, their LES-centric analogs.