Agradecimentos: L.S. gratefully acknowledges support from São Paulo Research Foundation (FAPESP; grant numbers 2017/11631-2 and 2018/21401-7), Shell, and the strategic importance of the support given by Brazil’s National Oil, Natural Gas, and Biofuels Agency (ANP) through the RD levy regulation. L.S. acknowledges FAPESP (grants 2020/04406-5 and 2021/12104-1). C.C.O. acknowledges FAPESP (grants 2018/01669-5 and 2014/25770-6). We also thank the National Council for Scientific and Technological Development (CNPq) and the Center for Innovation on New Energies (CINE). Y.V. thanks the Deutsche Forschungsgemeinschaft (DFG) for funding in the framework of the Special Priority Program (SPP 2196) project PERFECT PVs (#424216076). Author contributions Conceptualization, L.S., Y.V., and C.C.O.; writing – original draft, L.S.; writing – review editing, L.S., Y.V., A.F.N., and C.C.O.; supervision, Y.V., A.F.N., and C.C.O. Declaration of interests The authors declare no competing interests Ver menos

Abstract: Perovskite solar cells are a leading contender in the race to become the next commercially viable photovoltaic technology. Over the past decade, significant advancements have been made in the development and understanding of fundamental device physics principles, deposition techniques, compositional engineering, and passivation strategies. These advancements have resulted in improvements to the photovoltaic performance and stability of the devices. In particular, the integration of organic molecules in different layers of the device has played a key role in driving this progress. Organic molecules have been employed in electron and hole extraction layers, as well as in bulk and surface passivation layers. In this perspective, we provide an overview of the opportunities and potential associated with the use of organic molecules in perovskite solar cells. We propose strategies for the design of highly specific molecules with functionalities tailored to the desired application. Additionally, we highlight the use of chiral organic molecules to introduce asymmetry in the perovskite structure, thereby inducing chiroptical activity in the materials. These properties can be particularly appealing for the interface engineering of perovskite solar cells Ver menos