Organic–inorganic halide perovskites are promising photodetector materials due to their strong absorption, large carrier mobility, and easily tunable bandgap. Up to now, perovskite photodetectors are mainly based on polycrystalline thin films, which have some undesired properties such as large defective grain boundaries hindering the further improvement of the detector performance. Here, perovskite thin‐single‐crystal (TSC) photodetectors are fabricated with a vertical p–i–n structure. Due to the absence of grain‐boundaries, the trap densities of TSCs are 10–100 folds lower than that of polycrystalline thin films. The photodetectors based on CH3NH3PbBr3and CH3NH3PbI3TSCs show low noise of 1–2 fA Hz−1/2, yielding a high specific detectivity of 1.5 × 1013cm Hz1/2W−1. The absence of grain boundaries reduces charge recombination and enables a linear response under strong light, superior to polycrystalline photodetectors. The CH3NH3PbBr3photodetectors show a linear response to green light from 0.35 pW cm−2to 2.1 W cm−2, corresponding to a linear dynamic range of 256 dB.
Tri‐cation (Cs+/CH3NH3+/CH(NH2)2+) and dual‐anion (Br–/I–) perovskites are promising light absorbers for inexpensive infrared (IR) photodetectors but degrade under prolonged IR exposure. Here, stable IR photodetectors based on electrospun tri‐cation perovskite fibers infiltrated with hole‐transporting π‐conjugated small molecule 2,2′,7,7′‐tetrakis[
- NSF-PAR ID:
- 10378550
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Functional Materials
- Volume:
- 32
- Issue:
- 45
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Molecular I2can be produced from iodide‐based lead perovskites under thermal stress; triiodide, I3−, is formed from this I2and I−. Triiodide attacks protic cation MA+‐ or FA+‐based lead halide perovskites (MA+, methylammonium; FA+, formamidinium) as explicated through solution‐based nuclear magnetic resonance (NMR) studies: triiodide has strong hydrogen‐bonding affinity for MA+or FA+, which leads to their deprotonation and perovskite decomposition. Triiodide is a catalyst for this decomposition that can be obviated through perovskite surface treatment with thiol reducing agents. In contrast to methods using thiol incorporation into perovskite precursor solutions, no penetration of the thiol into the bulk perovskite is observed, yet its surface application stabilizes the perovskite against triiodide‐mediated thermal stress. Thiol applied to the interface between FAPbI3and Spiro‐OMeTAD (“Spiro”) prevents oxidized iodine species penetration into Spiro and thus preserves its hole‐transport efficacy. Surface‐applied thiol affects the perovskite work function; it ameliorates hole injection into the Spiro overlayer, thus improving device performance. It helps to increase interfacial adhesion (“wetting”): fewer voids are observed at the Spiro/perovskite interface if thiols are applied. Perovskite solar cells (PSCs) incorporating interfacial thiol treatment maintain over 80% of their initial power conversion efficiency (PCE) after 300 h of 85 °C thermal stress.
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Abstract Flexible perovskite solar cells (
f ‐PSCs) have attracted great attention due to their promising commercial prospects. However, the performance off ‐PSCs is generally worse than that of their rigid counterparts. Herein, it is found that the unsatisfactory performance of planar heterojunction (PHJ)f ‐PSCs can be attributed to the undesirable morphology of electron transport layer (ETL), which results from the rough surface of the flexible substrate. Precise control over the thickness and morphology of ETL tin dioxide (SnO2) not only reduces the reflectance of the indium tin oxide (ITO) on polyethylene 2,6‐naphthalate (PEN) substrate and enhances photon collection, but also decreases the trap‐state densities of perovskite films and the charge transfer resistance, leading to a great enhancement of device performance. Consequently, thef ‐PSCs, with a structure of PEN/ITO/SnO2/perovskite/Spiro‐OMeTAD/Ag, exhibit a power conversion efficiency (PCE) up to 19.51% and a steady output of 19.01%. Furthermore, thef ‐PSCs show a robust bending resistance and maintain about 95% of initial PCE after 6000 bending cycles at a bending radius of 8 mm, and they present an outstanding long‐term stability and retain about 90% of the initial performance after >1000 h storage in air (10% relative humidity) without encapsulation. -
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Abstract Semiconducting molecules have been employed to passivate traps extant in the perovskite film for enhancement of perovskite solar cells (PSCs) efficiency and stability. A molecular design strategy to passivate the defects both on the surface and interior of the CH3NH3PbI3perovskite layer, using two phthalocyanine (Pc) molecules (
NP ‐SC6‐ZnPc andNP ‐SC6‐TiOPc) is demonstrated. The presence of lone electron pairs on S, N, and O atoms of the Pc molecular structures provides the opportunity for Lewis acid–base interactions with under‐coordinated Pb2+sites, leading to efficient defect passivation of the perovskite layer. The tendency of bothNP ‐SC6‐ZnPc andNP ‐SC6‐TiOPc to relax on the PbI2terminated surface of the perovskite layer is also studied using density functional theory (DFT) calculations. The morphology of the perovskite layer is improved due to employing the Pc passivation strategy, resulting in high‐quality thin films with a dense and compact structure and lower surface roughness. UsingNP ‐SC6‐ZnPc andNP ‐SC6‐TiOPc as passivating agents, it is observed considerably enhanced power conversion efficiencies (PCEs), from 17.67% for the PSCs based on the pristine perovskite film to 19.39% forNP ‐SC6‐TiOPc passivated devices. Moreover, PSCs fabricated based on the Pc passivation method present a remarkable stability under conditions of high moisture and temperature levels. -
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Abstract Understanding interfacial reactions that occur between the active layer and charge‐transport layers can extend the stability of perovskite solar cells. In this study, the exposure of methylammonium lead iodide (CH3NH3PbI3) thin films prepared on poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)‐coated glass to 70% relative humidity (R.H.) leads to a perovskite crystal structure change from tetragonal to cubic within 2 days. Interface‐sensitive photoluminescence measurements indicate that the structural change originates at the PEDOT:PSS/perovskite interface. During exposure to 30% R.H., the same structural change occurs over a much longer time scale (>200 days), and a reflection consistent with the presence of (CH3)2NH2PbI3is detected to coexist with the cubic phase by X‐ray diffraction pattern. The authors propose that chemical interactions at the PEDOT:PSS/perovskite interface, facilitated by humidity, promote the formation of dimethylammonium, (CH3)2NH2+. The partial A‐site substitution of CH3NH3+for (CH3)2NH2+to produce a cubic (CH3NH3)1−
x [(CH3)2NH2]x PbI3phase explains the structural change from tetragonal to cubic during short‐term humidity exposure. When (CH3)2NH2+content exceeds its solubility limit in the perovskite during longer humidity exposures, a (CH3)2NH2+‐rich, hexagonal phase of (CH3NH3)1−x [(CH3)2NH2]x PbI3emerges. These interfacial interactions may have consequences for device stability and performance beyond CH3NH3PbI3model systems and merit close attention from the perovskite research community.
