Abstract

The ideality factor determined by measuring the open circuit voltage (VOC) as function of light intensity is often used as a means to identify the dominant recombination mechanism in solar cells. However, applying this Suns-VOC technique to perovskite cells is problematic since the VOC evolves with time in a way which depends on the previously applied bias (Vpre), the light intensity, and the device architecture/processing. Here we show that the dominant recombination mechanism in two structurally similar CH3NH3PbI3 devices containing either mesoporous Al2O3 or TiO2 layers can be identified from the signature of the transient ideality factor following application of a forward bias, Vpre, to the device in the dark. The transient ideality factor, is measured by monitoring the temporal evolution of VOC at different light intensities. The initial values of the transient ideality were consistent with corresponding photoluminescence vs intensity as well as electroluminescence vs current density measurements. Time-dependent simulations of the measurement on modelled devices, which include the effects of mobile ionic charge, show that Shockley Read Hall (SRH) recombination through deep traps at the charge collection interfaces is dominant in both devices. Using transient photovoltage measurements superimposed on the evolving VOC of bifacial devices we further show that the charge collection interface extends throughout the mesoporous TiO2 layer, consistent with a transient ideality signature corresponding to SRH recombination in the bulk of the film. This information could not be inferred from an ideality factor determined from only steady-state VOC values. The method we have developed will be useful for identifying performance bottlenecks in new variants of perovskite devices by comparison with the transient ideality signatures we have predicted for a range of possible recombination schemes.

Highlights

  • Identifying the dominant recombination mechanisms in hybrid perovskite solar cells is necessary to rationally optimize device architectures for performance and stability

  • We show that the dominant recombination mechanism in two structurally similar CH3NH3PbI3 devices containing either mesoporous Al2O3 or TiO2 layers can be identified from the signature of the transient ideality factor following application of a forward bias, Vpre, to the device in the dark

  • Using transient photovoltage measurements directly following illumination on bifacial devices, we further show that the perovskite–electron-transport-layer interface extends throughout the mesoporous TiO2 layer, consistent with a transient ideality signature corresponding to SRH recombination in the bulk of the film

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Summary

INTRODUCTION

Identifying the dominant recombination mechanisms in hybrid perovskite solar cells is necessary to rationally optimize device architectures for performance and stability. Solar cells [1,2,3] Applying this technique to perovskite devices is problematic, since mobile ions modulate recombination and injection of electronic carriers at interfaces [4,5,6,7], inducing slow transient changes in the VOC that depend on light and voltage-bias device preconditioning [8]. Following forward bias, the initial and final values of the nid(t) can be related to an established quasi-zero-dimensional model while steady-state values must be analyzed taking into account the homogeneity of carrier populations throughout the absorber layer These insights enable the dominant recombination mechanism to be inferred in the measured devices and resolve a long-standing contradiction whereby devices suspected of being dominated by surface recombination have shown stabilized ideality factors of approximately 2 [14,17,19,20]

Measuring ideality factors in solar cells
Ideality and recombination
Devices
Transient Suns-VOC measurement
J-EL measurement
Suns-PL measurement
Transient photovoltage measurements
Device simulation
The evolution of VOC with light intensity and preconditioning bias
Transient ideality factors
Interfacial
Assignment of recombination mechanisms to the measured devices
Recombination mechanism in the mesoporous Al2O3 cell
15 Initial EL 10
Recombination mechanism in the mesoporous TiO2 cell
CONCLUSIONS
Band-to-band recombination
Voltmeter
Full Text
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