%0 Journal Article %T Benefiting from Spontaneously Generated 2D/3D Bulk©\Heterojunctions in Ruddlesden£¿Popper Perovskite by Incorporation of S©\Bearing Spacer Cation %A Alireza Honarfar %A Kaibo Zheng %A Shuang Yu %A T£¿nu Pullerits %A Yajie Yan %J Archive of "Advanced Science". %D 2019 %R 10.1002/advs.201900548 %X 2D Ruddlesden¨CPopper (RP) perovskite solar cells have manifested superior operation durability yet inferior charge transport compared to their 3D counterparts. Integrating 3D phases with 2D RP perovskites presents a compromise to maintain respective advantages of both components. Here, the spontaneous generation of 3D phases embedded in 2D perovskite matrix is demonstrated at room temperature via introducing S©\bearing thiophene£¿2£¿ethylamine (TEA) as both spacer and stabilizer of inorganic lattices. The resulting 2D/3D bulk heterojunction structures are believed to arise from the compression©\induced epitaxial growth of the 3D phase at the grain boundaries of the 2D phase through the Pb£¿S interaction. The as©\prepared 2D TEA perovskites exhibit longer exciton diffusion length and extended charge carrier lifetime than the paradigm 2D phenylethylamine (PEA)©\based analogues and hence demonstrate an outstanding power conversion efficiency of 7.20% with significantly increased photocurrent. Dual treatments by NH4Cl and dimethyl sulfoxide are further applied to ameliorate the crystallinity and crystal orientation of 2D perovskites. Consequently, TEA©\based devices exhibit a stabilized efficiency over 11% with negligible hysteresis and display excellent ambient stability without encapsulation by preserving 80% efficiency after 270 h storage in air with 60 ¡À 5% relative humidity at 25 ¡ãC %K 2D Ruddlesdden¨CPopper perovskites %K 3D phase %K air stability %K low©\temperature fabrication %K planar solar cells %U https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6661945/