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Register a new userDeducing the key physical properties of a perovskite solar cell from its impedance response: insights from drift-diffusion modelling
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Interpreting the impedance response of perovskite solar cells (PSC) is significantly more challenging than for most other photovoltaics. This is for a variety of reasons, of which the most significant are the mixed ionic-electronic conduction properties of metal halide perovskites and the difficulty in fabricating stable, and reproducible, devices. Experimental studies, conducted on a variety of PSCs, produce a variety of impedance spectra shapes. However, they all possess common features, the most noteworthy of which is that they have at least two signals, at high and low frequency, with different characteristic responses to temperature, illumination and electrical bias. It is shown, by a combination of experiment and drift-diffusion modelling of the ion and charge carrier transport and recombination within the cell, that these common features are well reproduced by the simulation. In addition, we show that the high frequency response contains all the key information relating to the steady-state performance of a PSC, i.e. it is a signature of the recombination mechanisms and provides a measure of charge collection efficiency. Moreover, steady-state performance is significantly affected by the distribution of mobile ionic charge within the perovskite layer. Comparison between the electrical properties of different devices should therefore be made using high frequency impedance measurements performed in the steady-state voltage regime in which the cell is expected to operate.
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In this perspective, we explore the insights into the device physics of perovskite solar cells gained from modeling and simulation of these devices. We discuss a range of factors that influence the modeling of perovskite solar cells, including the role of ions, dielectric constant, density of states, and spatial distribution of recombination losses. By focusing on the effect of non-ideal energetic alignment in perovskite photovoltaic devices, we demonstrate a unique feature in low recombination perovskite materials - the formation of an interfacial, primarily electronic, self-induced dipole that results in a significant increase in the built-in potential and device open-circuit voltage. Finally, we discuss the future directions of device modeling in the field of perovskite photovoltaics, describing some of the outstanding open questions in which device simulations can serve as a particularly powerful tool for future advancements in the field.
Intrinsic and extrinsic ion migration is a very large threat to the operational stability of perovskite solar cells and is difficult to completely eliminate due to the low activation energy of ion migration and the existence of internal electric field. We propose a heterojunction route to help suppress ion migration, thus improving the operational stability of the cell from the perspective of eliminating the electric field response in the perovskite absorber. A heavily doped p-type (p+) thin layer semiconductor is introduced between the electron transporting layer (ETL) and perovskite absorber. The heterojunction charge depletion and electric field are limited to the ETL and p+ layers, while the perovskite absorber and hole transporting layer remain neutral. The p+ layer has a variety of candidate materials and is tolerant of defect density and carrier mobility, which makes this heterojunction route highly feasible and promising for use in practical applications.
Perovskite solar cells are notorious for exhibiting transient behaviour not seen in conventional inorganic semiconductor devices. Significant inroads have been made into understanding this fact in terms of rapid ion migration, now a well-established property of the prototype photovoltaic perovskite MAPbI$_3$ and strongly implicated in the newer mixed compositions. Here we study the manifestations of ion migration in frequency-domain small-signal measurements, focusing on the popular technique of Electrical Impedance Spectroscopy (EIS). We provide new interpretations for a variety of previously puzzling features, including giant photo-induced low-frequency capacitance and negative capacitance in a variety of forms. We show that these apparently strange measurements can be rationalized by the splitting of AC current into two components, one associated with charge-storage, and the other with the quasi-steady-state recombination current of electrons and holes. The latter contribution to the capacitance can take either a positive or a negative sign, and is potentially very large when slow, voltage-sensitive processes such as ion migration are at play. Using numerical drift-diffusion semiconductor models, we show that giant photo-induced capacitance, inductive loop features, and low-frequency negative capacitance all emerge naturally as consequences of ion migration via its coupling to quasi-steady-state electron and hole currents. In doing so, we unify the understanding of EIS measurements with the comparably well-developed theory of rate dependent current-voltage (I-V) measurements in perovskite cells. Comparing the two techniques, we argue that EIS is more suitable for quantifying I-V hysteresis than conventional methods based on I-V sweeps, and demonstrate this application on a variety of cell types.
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