Pengyu Sun

The optoelectronic role of chlorine in CH3NH3PbI3(Cl)-based perovskite solar cells.

Perovskite photovoltaics offer a compelling combination of extremely low-cost, ease of processing and high device performance. The optoelectronic properties of the prototypical CH3NH3PbI3 can be further adjusted by introducing other extrinsic ions. Specifically, chlorine incorporation has been shown to affect the morphological development of perovksite films, which results in improved optoelectronic characteristics for high efficiency. However, it requires a deep understanding to the role of extrinsic halide, especially in the absence of unpredictable morphological influence during film growth. Here we report an effective strategy to investigate the role of the extrinsic ion in the context of optoelectronic properties, in which the morphological factors that closely correlate to device performance are mostly decoupled. The chlorine incorporation is found to mainly improve the carrier transport across the heterojunction interfaces, rather than within the perovskite crystals. Further optimization according this protocol leads to solar cells achieving power conversion efficiency of 17.91%.

Single Crystal Formamidinium Lead Iodide (FAPbI3): Insight into the Structural, Optical, and Electrical Properties

5 mm-scale large FAPbI 3 single crystals and corresponding photoconductive properties are shown. The phase transition of FAPbI3 between the α-phase and δ-phase is studied. The carrier mobility is 4.4 cm(2) V(-1) s(-1) with a lifetime of 484 ns in the bulk of the single crystal. Finally, photodetectors based on single-crystal FAPbI3 are demonstrated.

Guanidinium: A Route to Enhanced Carrier Lifetime and Open-Circuit Voltage in Hybrid Perovskite Solar Cells

Hybrid perovskites have shown astonishing power conversion efficiencies owed to their remarkable absorber characteristics including long carrier lifetimes, and a relatively substantial defect tolerance for solution-processed polycrystalline films. However, nonradiative charge carrier recombination at grain boundaries limits open circuit voltages and consequent performance improvements of perovskite solar cells. Here we address such recombination pathways and demonstrate a passivation effect through guanidinium-based additives to achieve extraordinarily enhanced carrier lifetimes and higher obtainable open circuit voltages. Time-resolved photoluminescence measurements yield carrier lifetimes in guanidinium-based films an order of magnitude greater than pure-methylammonium counterparts, giving rise to higher device open circuit voltages and power conversion efficiencies exceeding 17%. A reduction in defect activation energy of over 30% calculated via admittance spectroscopy and confocal fluorescence intensity mapping indicates successful passivation of recombination/trap centers at grain boundaries. We speculate that guanidinium ions serve to suppress formation of iodide vacancies and passivate under-coordinated iodine species at grain boundaries and within the bulk through their hydrogen bonding capability. These results present a simple method for suppressing nonradiative carrier loss in hybrid perovskites to further improve performances toward highly efficient solar cells.

Improving the TiO2 electron transport layer in perovskite solar cells using acetylacetonate-based additives

We developed a facile and quantitative method to improve the electron transport properties and resulting device performances of perovskite solar cells based on post-incorporation of various acetylacetonate additives. Previous studies rely on synthesis or soaking processes with limited additive control. Here, our acetylacetonated-based additives are used as effective intermediate gels to interact with TiO2 nanocrystals using a simple approach. The incorporation process can be controlled effectively and quantitatively using a range of additives from divalent (II), trivalent (III), and tetravalent (IV) to hexavalent (VI) acetylacetonate. Electronic parameters of solar cell devices, such as short circuit current (Jsc) and fill factor (FF), are enhanced, regardless of the different valencies of the additives. Zirconium(IV) acetylacetonate was found to be the most effective additive, with average PCE improved from 15.0% to 15.8%. Detailed characterization experiments including transient photoluminescence spectra, ultra-violet photoelectron spectroscopy, photovoltage decay, and photocurrent decay indicate an improved interface with improved carrier extraction originating from the TiO2 modification.

Tailoring the Interfacial Chemical Interaction for High-Efficiency Perovskite Solar Cells

The ionic nature of perovskite photovoltaic materials makes it easy to form various chemical interactions with different functional groups. Here, we demonstrate that interfacial chemical interactions are a critical factor in determining the optoelectronic properties of perovskite solar cells. By depositing different self-assembled monolayers (SAMs), we introduce different functional groups onto the SnO2 surface to form various chemical interactions with the perovskite layer. It is observed that the perovskite solar cell device performance shows an opposite trend to that of the energy level alignment theory, which shows that chemical interactions are the predominant factor governing the interfacial optoelectronic properties. Further analysis verifies that proper interfacial interactions can significantly reduce trap state density and facilitate the interfacial charge transfer. Through use of the 4-pyridinecarboxylic acid SAM, the resulting perovskite solar cell exhibits striking improvements to the reach the highest efficiency of 18.8%, which constitutes an ∼10% enhancement compared to those without SAMs. Our work highlights the importance of chemical interactions at perovskite/electrode interfaces and paves the way for further optimizing performances of perovskite solar cells.

Pure Formamidinium‐Based Perovskite Light‐Emitting Diodes with High Efficiency and Low Driving Voltage

A formamidinium(FA)-based perovskite showns superior optoelectronic properties including better stability than methylammonium-based counterparts. Pure FA-perovskite-based light-emitting diodes (LEDs) with high efficiency are reported. Interestingly, the LED clearly shows a sub-bandgap emission at 1.7 V (bandgap 2.3 eV). This important discovery provides further insights of the charge transport mechanism in perovskite-based optoelectronic devices.

Low-Temperature TiOx Compact Layer for Planar Heterojunction Perovskite Solar Cells

Here, we demonstrate an effective low-temperature approach to fabricate a uniform and pinhole-free compact TiO2 layer for enhancing photovoltaic performance of perovskite solar cells. TiCl4 was used to modify TiO2 for efficient charge generation and significantly reduced recombination loss. We found that a TiO2 layer with an appropriate TiCl4 treatment possesses a smooth surface with full coverage of the conductive electrode. Further studies on charge carrier dynamics confirmed that the TiCl4 treatment improves the contact of the TiO2/perovskite interface, facilitating charge extraction and suppressing charge recombination. On the basis of the treatment, we improved the open circuit voltage from 1.01 V of the reference cell to 1.08 V, and achieved a power conversion efficiency of 16.4%.

Working Mechanism for Flexible Perovskite Solar Cells with Simplified Architecture

In this communication, we report an efficient and flexible perovskite solar cell based on formamidinium lead trihalide (FAPbI3) with simplified configuration. The device achieved a champion efficiency of 12.70%, utilizing direct contact between metallic indium tin oxide (ITO) electrode and perovskite absorber. The underlying working mechanism is proposed subsequently, via a systematic investigation focusing on the heterojunction within this device. A significant charge storage has been observed in the perovskite, which is believed to generate photovoltage and serves as the driving force for charge transferring from the absorber to ITO electrode as well. More importantly, this simplified device structure on flexible substrates suggests its compatibility for scale-up fabrication, which paves the way for commercialization of perovskite photovoltaic technology.

High-Brightness Blue and White LEDs based on Inorganic Perovskite Nanocrystals and their Composites

Inorganic metal halide perovskite nanocrystals (NCs) have been employed universally in light-emitting applications during the past two years. Here, blue-emission (≈470 nm) Cs-based perovskite NCs are derived by directly mixing synthesized bromide and chloride nanocrystals with a weight ratio of 2:1. High-brightness blue perovskite light-emitting diodes (PeLEDs) are obtained by controlling the grain size of the perovskite films. Moreover, a white PeLED is demonstrated for the first time by blending orange polymer materials with the blue perovskite nanocrystals as the active layer. Exciton transfer from the blue nanocrystals to the orange polymers via Förster or Dexter energy transfer is analyzed through time resolved photoluminescence. By tuning the ratio between the perovskite nanocrystals and polymers, pure white light is achieved with the a CIE coordinate at (0.33,0.34).

Ternary System with Controlled Structure: A New Strategy toward Efficient Organic Photovoltaics

Recently, a new type of active layer with a ternary system has been developed to further enhance the performance of binary system organic photovoltaics (OPV). In the ternary OPV, almost all active layers are formed by simple ternary blend in solution, which eventually leads to the disordered bulk heterojunction (BHJ) structure after a spin-coating process. There are two main restrictions in this disordered BHJ structure to obtain higher performance OPV. One is the isolated second donor or acceptor domains. The other is the invalid metal-semiconductor contact. Herein, the concept and design of donor/acceptor/acceptor ternary OPV with more controlled structure (C-ternary) is reported. The C-ternary OPV is fabricated by a sequential solution process, in which the second acceptor and donor/acceptor binary blend are sequentially spin-coated. After the device optimization, the power conversion efficiencies (PCEs) of all OPV with C-ternary are enhanced by 14-21% relative to those with the simple ternary blend; the best PCEs are 10.7 and 11.0% for fullerene-based and fullerene-free solar cells, respectively. Moreover, the averaged PCE value of 10.4% for fullerene-free solar cell measured in this study is in great agreement with the certified one of 10.32% obtained from Newport Corporation.