Advancing perovskite solar cell technologies toward their theoretical power conversion efficiency (PCE) requires delicate control over the carrier dynamics throughout the entire device. By controlling the formation of the perovskite layer and careful choices of other materials, we suppressed carrier recombination in the absorber, facilitated carrier injection into the carrier transport layers, and maintained good carrier extraction at the electrodes. When measured via reverse bias scan, cell PCE is typically boosted to 16.6% on average, with the highest efficiency of ~19.3% in a planar geometry without antireflective coating. The fabrication of our perovskite solar cells was conducted in air and from solution at low temperatures, which should simplify manufacturing of large-area perovskite devices that are inexpensive and perform at high levels.

http://science.sciencemag.org/content/sci/345/6196/542.full.pdf

Interface engineering of highly efficient perovskite solar cells

Within the space of a few years, hybrid organic–inorganic perovskite solar cells have emerged as one of the most exciting material platforms in the photovoltaic sector. This review describes the rapid progress that has been made in this area.

The emergence of perovskite solar cells

Metal-halide perovskites are crystalline materials originally developed out of scientific curiosity. Unexpectedly, solar cells incorporating these perovskites are rapidly emerging as serious contenders to rival the leading photovoltaic technologies. Power conversion efficiencies have jumped from 3% to over 20% in just four years of academic research. Here, we review the rapid progress in perovskite solar cells, as well as their promising use in light-emitting devices. In particular, we describe the broad tunability and fabrication methods of these materials, the current understanding of the operation of state-of-the-art solar cells and we highlight the properties that have delivered light-emitting diodes and lasers. We discuss key thermal and operational stability challenges facing perovskites, and give an outlook of future research avenues that might bring perovskite technology to commercialization.

Metal-halide perovskites for photovoltaic and light-emitting devices

Solar cells based on organometallic halide perovskite absorber layers are emerging as a high-performance photovoltaic technology. Using highly sensitive photothermal deflection and photocurrent spectroscopy, we measure the absorption spectrum of CH3NH3PbI3 perovskite thin films at room temperature. We find a high absorption coefficient with particularly sharp onset. Below the bandgap, the absorption is exponential over more than four decades with an Urbach energy as small as 15 meV, which suggests a well-ordered microstructure. No deep states are found down to the detection limit of ∼1 cm–1. These results confirm the excellent electronic properties of perovskite thin films, enabling the very high open-circuit voltages reported for perovskite solar cells. Following intentional moisture ingress, we find that the absorption at photon energies below 2.4 eV is strongly reduced, pointing to a compositional change of the material.

Organometallic Halide Perovskites: Sharp Optical Absorption Edge and Its Relation to Photovoltaic Performance

Organic–inorganic hybrid perovskite materials are attracting great interest for their applications in photovoltaics where they have demonstrated excellent efficiency. Here, Dou et al. demonstrate room temperature, solution-processed hybrid perovskite photodetectors with fast response and high detectivity.

/pdf/solution-processed-hybrid-perovskite-photodetectors-with-1cx3sj2i3d.pdf

Solution-processed hybrid perovskite photodetectors with high detectivity

The use of a thin layer of zinc oxide nanoparticles as an electron-transport layer allows flexible perovskite solar cells to be fabricated with a power conversion efficiency as high as 15.7%.

Perovskite solar cells with a planar heterojunction structure prepared using room-temperature solution processing techniques

Perovskite solar cells have rapidly advanced to the forefront of solution-processable photovoltaic devices, but the CH3NH3PbI3 semiconductor decomposes rapidly in moist air, limiting their commercial utility. In this work, we report a quantitative and systematic investigation of perovskite degradation processes. By carefully controlling the relative humidity of an environmental chamber and using in situ absorption spectroscopy and in situ grazing incidence X-ray diffraction to monitor phase changes in perovskite degradation process, we demonstrate the formation of a hydrated intermediate containing isolated PbI64– octahedra as the first step of the degradation mechanism. We also show that the identity of the hole transport layer can have a dramatic impact on the stability of the underlying perovskite film, suggesting a route toward perovskite solar cells with long device lifetimes and a resistance to humidity.

Investigation of CH3NH3PbI3 Degradation Rates and Mechanisms in Controlled Humidity Environments Using in Situ Techniques

The rapid development of organometal halide perovskite solar cells has led to reports of power conversion efficiencies of over 20%. Despite this excellent performance, their instability remains the major challenge limiting their commercialization. In this report, we systematically investigate the origin of the thermal instability of perovskite solar cells fabricated using ZnO electron transport layers. Through in situ grazing incidence X-ray diffraction experiments and density functional theory calculations, we show that the basic nature of the ZnO surface leads to proton-transfer reactions at the ZnO/CH3NH3PbI3 interface, which results in decomposition of the perovskite film. The decomposition process is accelerated by the presence of surface hydroxyl groups and/or residual acetate ligands; calcination of the ZnO layer results in a more thermally stable ZnO/CH3NH3PbI3 interface, albeit at the cost of a small decrease in power conversion efficiency.

Origin of the Thermal Instability in CH3NH3PbI3 Thin Films Deposited on ZnO

The recent breakthrough of organometal halide perovskites as the light harvesting layer in photovoltaic devices has led to power conversion efficiencies of over 16%. To date, most perovskite solar cells have adopted a structure in which the perovskite light absorber is placed between carrier-selective electron- and hole-transport layers (ETLs and HTLs). Here we report a new type of compact layer free bilayer perovskite solar cell and conclusively demonstrate that the ETL is not a prerequisite for obtaining excellent device efficiencies. We obtained power conversion efficiencies of up to 11.6% and 13.5% when using poly(3-hexylthiophene) and 2,2′,7,7′-tetrakis(N,N-di(4-methoxyphenyl)amino)-9,9′-spirobifluorene, respectively, as the hole-transport material. This performance is very comparable to that obtained with the use of a ZnO ETL. Impedance spectroscopy suggests that while eliminating the ZnO leads to an increase in contact resistance, this is offset by a substantial decrease in surface recombination.

Compact Layer Free Perovskite Solar Cells with 13.5% Efficiency

Recent advances in the development of perovskite solar cells based on CH3NH3PbI3 have produced devices with power conversion efficiencies of >15%. While initial work in this area assumed that the perovskite-based cells required a mesoporous TiO2 support, many recent reports have instead focused on the development of planar heterojunction structures. A better understanding of how both cell architecture and various design parameters (e.g., perovskite thickness and morphology) affect cell performance is needed. Here, we report the fabrication of perovskite solar cells based on a ZnO nanoparticle electron transport layer, CH3NH3PbI3 light absorber, and poly(3-hexylthiophene) (P3HT) hole transport layer. We show that vapor-phase deposition of the PbI2 precursor film produces devices with performances equivalent to those prepared using entirely solution-based techniques, but with very precise control over the thickness and morphology of the CH3NH3PbI3 layer. Optimization of the layer thickness yielded devices with efficiencies of up to 11.3%. The results further demonstrate that a delicate balance between light absorption and carrier transport is required in these planar heterojunction devices, with the thickest perovskite films producing only very low power conversion efficiencies.

/pdf/effect-of-ch3nh3pbi3-thickness-on-device-efficiency-in-legpd2ob6f.pdf

Timothy L. Kelly

Papers

Perovskite solar cells with a planar heterojunction structure prepared using room-temperature solution processing techniques

Investigation of CH3NH3PbI3 Degradation Rates and Mechanisms in Controlled Humidity Environments Using in Situ Techniques

Origin of the Thermal Instability in CH3NH3PbI3 Thin Films Deposited on ZnO

Compact Layer Free Perovskite Solar Cells with 13.5% Efficiency

Effect of CH3NH3PbI3 thickness on device efficiency in planar heterojunction perovskite solar cells