Exploring Transport Behavior in Hybrid Perovskites Solar Cells via Machine Learning Analysis of Environmental‐Dependent Impedance Spectroscopy

Abstract

Hybrid organic–inorganic perovskites are one of the promising candidates for the next‐generation semiconductors due to their superlative optoelectronic properties. However, one of the limiting factors for potential applications is their chemical and structural instability in different environments. Herein, the stability of (FAPbI3)0.85(MAPbBr3)0.15 perovskite solar cell is explored in different atmospheres using impedance spectroscopy. An equivalent circuit model and distribution of relaxation times (DRTs) are used to effectively analyze impedance spectra. DRT is further analyzed via machine learning workflow based on the non‐negative matrix factorization of reconstructed relaxation time spectra. This exploration provides the interplay of charge transport dynamics and recombination processes under environment stimuli and illumination. The results reveal that in the dark, oxygen atmosphere induces an increased hole concentration with less ionic character while ionic motion is dominant under ambient air. Under 1 Sun illumination, the environment‐dependent impedance responses show a more striking effect compared with dark conditions. In this case, the increased transport resistance observed under oxygen atmosphere in equivalent circuit analysis arises due to interruption of photogenerated hole carriers. The results not only shed light on elucidating transport mechanisms of perovskite solar cells in different environments but also offer an effective interpretation of impedance responses.

Light–ferroelectric interaction in two-dimensional lead iodide perovskites

“…The millisecond time scale under dark conditions could activate electronic charge carriers in MHPs and charge injection, rather than ion migration that occurs within either sub-or several seconds or minute time scale as demonstrated in many studies. [38][39][40][41][42][43] However, at high biases, the applied pulse duration could also drive ion migration. Therefore, during our measurements, it is expected that both electronic and ionic charge carriers transit in 2D MHPs.…”

Gaussian Processes for the Analysis of Electrochemical Impedance Spectroscopy Data: Prediction, Filtering, and Active Learning

“…The EIS spectrum was measured from 1 Hz to 5 MHz in a 1 atm atmosphere with a 100 mV voltage amplitude. The ECM was fitted against a model developed in [61], and the parameter values are given in Table S4. The impedance of this solar cell was regressed over the whole frequency range and was predicted below 1 Hz (Figure 7 (c)).…”

Operando Analysis of Losses in Commercial-Sized Solid Oxide Cells: Methodology Development and Validation

“…For instance, in SOCs, the evolution of the intensity and the relaxation time of the DRT peaks is commonly studied under different working temperatures, current load, and gas flow rates and compositions [7]. In the case of Li-ion batteries, the DRT profile is commonly studied at different state-of-charge values [8][9][10], while on solar cells, it is examined under different light irradiation levels [11,12].…”