Charge carrier recombination in the perovskite solar cells (PSCs) has a deep influence on the electrical performance, such as open circuit voltage, short circuit current, fill factor and ultimately power conversion efficiency. The impacts of injection barrier, recombination channels, doping properties of carrier transport layers and light intensity on the performance of PSCs are theoretically investigated by drift-diffusion model in this work. The results indicate that due to the injection barrier at the interfaces of perovskite and carrier transport layer, the accumulated carriers modify the electric field distribution throughout the PSCs. Thus, a zero electric field is generated at a specific applied voltage, with greatly increases the interfacial recombination, resulting in a local kink of current density-voltage (J-V) curve. This work provides an effective strategy to improve the efficiency of PSCs by pertinently reducing both the injection barrier and interfacial recombination.
Drift-diffusion model is an indispensable modeling tool to understand the carrier dynamics (transport, recombination, and collection) and simulate practical-efficiency of solar cells (SCs) through taking into account various carrier recombination losses existing in multilayered device structures. Exploring the way to predict and approach the SC efficiency limit by using the drift-diffusion model will enable us to gain more physical insights and design guidelines for emerging photovoltaics, particularly perovskite solar cells. Our work finds out that two procedures are the prerequisites for pre…
Interfacial charge separation and recombination at heterojunctions of monolayer transition metal dichalcogenides (TMDCs) are of interest to two dimensional optoelectronic technologies. These processes can involve large changes in parallel momentum vector due to the confinement of electrons and holes to the K-valleys in each layer. Since these high-momentum valleys are usually not aligned across the interface of two TMDC monolayers, how parallel momentum is conserved in the charge separation or recombination process becomes a key question. Here we probe this question using the model system of a…
Despite the exciting recent research on perovskite based solar cells, the design space for further optimization and the practical limits of efficiency are not well known in the community. In this manuscript, we address these aspects through theoretical calculations and detailed numerical simulations. Here, we first provide the detailed balance limit efficiency in the presence of radiative and Auger recombination. Then, using coupled optical and carrier transport simulations, we identify the physical mechanisms that contribute towards bias dependent carrier collection, and hence low fill factor…
Halide perovskite light absorbers have great advantages for photovoltaics such as efficient solar energy absorption, but charge accumulation and recombination at the interface with an electron transport layer (ETL) remains a major challenge in realizing their full potential. Here we report the experimental realization of a zipper-like interdigitated interface between a Pb-based halide perovskite light absorber and an oxide ETL by the PbO capping of the ETL surface, which produces an atomically thin two-dimensional metallic layer that can significantly enhance the perovskite/ETL charge extracti…
Understanding and quantifying the main loss factors affecting the power conversion efficiency of perovskite solar cells are urgently needed. In this work, based on semiconductor physics, the expressions of bulk and surface recombination currents are analytically derived. Then taking the optical loss, series and shunt resistance losses, and bulk and surface recombination losses into consideration, an equivalent circuit model is proposed to describe the current density-voltage characteristics of practical perovskite solar cells. Furthermore, by comparing to the drift-diffusion model, the pre-def…
A theoretical approach to photoconversion efficiency modeling in perovskite p-i-n structures is developed. The results of this modeling compare favorably with the experiment and indicate that the surfaces of the perovskite solar cells (SCs) are naturally textured. It is shown that photoconversion efficiency in the limiting case of negligible Shockley-Read-Hall and surface recombination and in the absence of optical losses reaches the value of 29%. In the realistic case, the current-voltage curve ideality factor equals 2. This value is not due to recombination in the space-charge region; rather…
A sacrificial film of polystyrene nanoparticles was utilized to introduce nano-cavities in mesoporous metal oxide layers. This enabled the growth of larger perovskite crystals inside the oxide scaffold with significantly suppressed non-radiative recombination and improving device performance. This work exemplifies potential applications of such nanoarchitectonic approaches in perovskite opto-electronic devices.
State-of-the-art metal halide perovskite-based photovoltaics often employ organic ammonium salts, AX, as a surface passivator, where A is a large organic cation and X is a halide. These surface treatments passivate the perovskite by forming layered perovskites (e.g., A2PbX4) or by AX itself serving as a surface passivation agent on the perovskite photoactive film. It remains unclear whether layered perovskites or AX is the ideal passivator due to an incomplete understanding of the interfacial impact and resulting photoexcited carrier dynamics of AX treatment. In the present study, we use TRPL …
We report a model describing the molecular orientation disorder in CH3NH3PbI3, solving a classical Hamiltonian parametrised with electronic structure calculations, with the nature of the motions informed by ab-initio molecular dynamics. We investigate the temperature and static electric field dependence of the equilibrium ferroelectric (molecular) domain structure and resulting polarisability. A rich domain structure of twinned molecular dipoles is observed, strongly varying as a function of temperature and applied electric field. We propose that the internal electrical fields associated with …
The basic processes of perovskite radiation resistance are discussed for photo- and high-energy electron irradiation. It is shown that ionization of iodine ions and a staged mechanism of elastic scattering (upon intermediate scattering on light ions of an organic molecule) lead to the formation of a recombination center Ii. The features of ionization degradation of interfaces with both planar and fractal structures are considered. A special type of fractality is identified, and its minimum possible level of photodegradation is predicted. By using the methodology of classical radiation physics,…
Nearly perfect photon recycling helped GaAs cells achieve the highest efficiency ever reported for a solar cell. Recent reports of photon recycling in perovskite solar cells suggest that, once optimized, it may as well achieve GaAs-like performance. In this paper, we show that GaAs and perovskite cells recycle photons in different ways. First, although bare-perovskite has been shown to have lifetimes (~1us) in the radiative limit, non-radiative recombination at the transport layers restricts the solar cell operation far below the "photon-recycling" regime. GaAs cells have no such limitation. S…
Using a combination of continuous wave and time-resolved spectroscopy, we study the effects of interfacial conditions on the radiative lifetimes and photoluminescence intensities of colloidal CdTe/CdS quantum dots (QDs) embedded in a three-dimensional nanostructured silicon (NSi) matrix. The NSi matrix was thermally oxidized under different conditions to change the interfacial oxide thickness. QDs embedded in a NSi matrix with ~0.5 nm of interfacial oxide exhibited reduced photoluminescence intensity and nearly five times shorter radiative lifetimes (~16 ns) compared to QDs immobilized within …
