TY - JOUR AB - Recombination via subgap trap states is considered a limiting factor in the development of organometal halide perovskite solar cells. Here, the impact of active layer crystallinity on the accumulated charge and opencircuit voltage (Voc) in solar cells based on methylammonium lead triiodide (CH3NH3PbI3, MAPI) is demonstrated. It is shown that MAPI crystallinity can be systematically tailored by modulating the stoichiometry of the precursor mix, where small quantities of excess methylammonium iodide (MAI) improve crystallinity, increasing device Voc by ≈200 mV. Using in situ differential charging and transient photovoltage measurements, charge density and charge carrier recombination lifetime are determined under operational conditions. Increased Voc is correlated to improved active layer crystallinity and a reduction in the density of trap states in MAPI. Photoluminescence spectroscopy shows that an increase in trap state density correlates with faster carrier trapping and more nonradiative recombination pathways. Fundamental insights into the origin of Voc in perovskite photovoltaics are provided and it is demonstrated why highly crystalline perovskite films are paramount for highperformance devices. AU - Du,T AU - Kim,J AU - Ngiam,J AU - Xu,S AU - Barnes,PRF AU - Durrant,JR AU - McLachlan,MA DO - 10.1002/adfm.201801808 EP - 11 PY - 2018/// SN - 1616-301X SP - 1 TI - Elucidating the origins of subgap tail states and open-circuit voltage in methylammonium lead triiodide perovskite solar cells T2 - Advanced Functional Materials UR - http://dx.doi.org/10.1002/adfm.201801808 UR - http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000440810500011&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202 UR - https://onlinelibrary.wiley.com/doi/full/10.1002/adfm.201801808 UR - http://hdl.handle.net/10044/1/64346 VL - 28 ER -