Not yet reviewed by Pith; the record is open.

Important properties of complex quantum many-body systems and their phase diagrams can often already be inferred from the impurity limit. The Bose polaron problem describing an impurity atom immersed in a Bose-Einstein condensate is a paradigmatic example. One of the most interesting features of this model is the competition between the emergent impurity-mediated attraction between the bosons and their intrinsic repulsion. The arising higher-order correlations make the physics rich and interesting, but also complex to describe theoretically. To tackle this challenge, we develop a quantum chemistry-inspired computational technique and compare two state-of-the-art variational methods that fully include both the boson-impurity and boson-boson interactions on a non-perturbative level. For a sweep of the boson-impurity interaction strength, we find two regimes of qualitatively different behaviour. If the impurity-mediated interactions overcome the repulsion between the bosons, the polaron becomes unstable due to the formation of large bound clusters. If instead the interboson interactions dominate, the impurity will experience a crossover from a polaron into a small molecule. We achieve a unified understanding incorporating both of these regimes and the transition between them. We show that both the instability and crossover regime can be studied in realistic cold-atom experiments. Moreover, we develop a simple analytical model that allows us to interpret these phenomena in the typical Landau framework of first-order phase transitions that turn second-order at a critical endpoint, revealing a deep connection of the Bose polaron model to both few- and many-body physics.