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For a class of 2D hybrid organic-inorganic perovskite semiconductors based on$\pi$-conjugated organic cations, we predict quantitatively how varying theorganic and inorganic component allows control over the nature, energy andlocalization of carrier states in a quantum-well-like fashion. Ourfirst-principles predictions, based on large-scale hybrid density-functionaltheory with spin-orbit coupling, show that the interface between the organicand inorganic parts within a single hybrid can be modulated systematically,enabling us to select between different type-I and type-II energy levelalignments. Energy levels, recombination properties and transport behavior ofelectrons and holes thus become tunable by choosing specific organicfunctionalizations and juxtaposing them with suitable inorganic components.

Tunable Semiconductors: Control over Carrier States and Excitations in Layered Hybrid Organic-Inorganic Perovskites