Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 46, Pages 19705-19714Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c09647
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Funding
- National Natural Science Foundation of China [11574248, 61505161]
- China Postdoctoral Science Foundation [2016M590947]
- Scientific Research Plan Projects of Shaanxi Education Department [17JK0700]
- Natural Science Basic Research Plan in Shaanxi Province of China [2019JQ-119]
- Fundamental Research Funds for the Central Universities [xjj2016031]
- Global Frontier R&D Program of the Center for Multiscale Energy System by the National Research Foundation under the Ministry of Education, Science and Technology, Korea [2012M3A6A7054855]
- ONR [N00014-20-1-2725]
- SHyNE Resource [NSF ECCS-1542205]
- IIN
- Northwestern's MRSEC program [NSF DMR-1720139]
- State of Illinois
- Northwestern University
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The halide perovskite Ruddlesden-Popper (RP) phases are a homologous layered subclass of solution-processable semiconductors that have aroused great attention, especially for developing long-term solar photovoltaics. They are defined as (A')(2)(A)(n-1)PbnX3n+1 (A' = spacer cation, A = cage cation, and X = halide anion). The orientation control of low-temperature self-assembled thin films is a fundamental issue associated with the ability to control the charge carrier transport perpendicular to the substrate. Here we report new chemical derivatives designed from a molecular perspective using a novel spacer cation 3-phenyl-2-propenammonium (PPA) with conjugated backbone as a low-temperature strategy to assemble more efficient solar cells. First, we solved and refined the crystal structures of single crystals with the general formula (PPA)(2)(FA(0.5)MA(0.5))(n-1)PbnI3n+1 (n = 2 and 3, space group C2) using X-ray diffraction and then used the mixed halide (PPA)(2)(Cs-0.05(FA(0.88)MA(0.12))(0.95))(n-1)Pb-n(I0.88Br0.12)(3n+1) analogues to achieve more efficient devices. While forming the RP phases, multiple hydrogen bonds between PPA and inorganic octahedra reinforce the layered structure. For films we observe that as the targeted layer thickness index increases from n = 2 to n = 4, a less horizontal preferred orientation of the inorganic layers is progressively realized along with an increased presence of high-n or 3D phases, with an improved flow of free charge carriers and vertical to substrate conductivity. Accordingly, we achieve an efficiency of 14.76% for planar p-i-n solar cells using PPA-RP perovskites, which retain 93.8 +/- 0.25% efficiency with encapsulation after 600 h at 85 degrees C and 85% humidity (ISOS-D-3).
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