The computational
discovery of novel materials has been one of
the main motivations behind research in theoretical chemistry for
several decades. Despite much effort, this is far from a solved problem,
however. Among other reasons, this is due to the enormous space of
possible structures and compositions that could potentially be of
interest. In the case of inorganic materials, this is exacerbated
by the combinatorics of the periodic table since even a single-crystal
structure can in principle display millions of compositions. Consequently,
there is a need for tools that enable a more guided exploration of
the materials design space. Here, generative machine learning models
have recently emerged as a promising technology. In this work, we
assess the performance of a range of deep generative models based
on reinforcement learning, variational autoencoders, and generative
adversarial networks for the prototypical case of designing Elpasolite
compositions with low formation energies. By relying on the fully
enumerated space of 2 million main-group Elpasolites, the precision,
coverage, and diversity of the generated materials are rigorously
assessed. Additionally, a hyperparameter selection scheme for generative
models in chemical composition space is developed.