A Robust Routine to Analyse 1-D Transient Photoluminescence of Metal Halide Perovskites

Antonio Cabas Vidani^a, Simon Zeder^a^,^b, Urs Aeberhard^a^,^c, Daniele Braga^a, Sandra Jenatsch^a, Beat Ruhstaller^a^,^d

^aFluxim AG, 8400 Winterthur, Switzerland

^bEPFL – PV-LAB, Institute of Microengineering, 2002 Neuchâtel, Switzerland

^cETHZ – Integrated Systems Laboratory, 8092 Zürich, Switzerland

^dZHAW – Institute of Computational Physics, 8401 Winterthur, Switzerland

Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Spring Meeting 2022 (NSM22)

#PhotoPero22. Photophysics of Halide Perovskites and Related Materials - from Bulk to Nano

Online, Spain, 2022 March 7th - 11th

Organizers: Sascha Feldmann, Annamaria Petrozza and Ajay Ram Srimath Kandada

Contributed talk, Daniele Braga, presentation 088
DOI: https://doi.org/10.29363/nanoge.nsm.2022.088
Publication date: 7th February 2022

Transient photoluminescence (trPL) is a powerful technique to study charge carrier dynamics and identify carrier recombination channels in luminescent thin films and devices. It has been widely used to quantify carrier radiative and non-radiative lifetimes,^[1] to compute the charge extraction velocity ^[2], and to study the influence of the interfaces on the recombination mechanisms.^[3]

Data fitting helps you extract this information from experimental trPL decays, but considering the number and nature of involved variables, the set of extracted values is most of the time not unique. Indeed, the trPL decay is ruled by the radiative and non-radiative recombination processes which follow, respectively, a quadratic and a linear dependence on the photogenerated carriers. The concentration of these carriers depends on several parameters, such as the injection level, the doping of the emitting material, the radiative recombination coefficient, and the trap density. Because of this interdependence, it is easy to obtain comparable trPL decay fits by using different combinations of values and, hence, interpreting incorrectly the recombination events. To obtain reliable information, it is better to use a robust simulation approach where the parameters are distinctly assessed and recursively optimized according to experimental data from the literature.

We demonstrate how to simulate experimental trPL curves of a halide perovskite on glass by fitting the data with a fully-coupled 1D optoelectronic simulation. The validity of the simulated trPL curves is also verified by fitting the decay with a bi-exponential function, which allows estimating the lifetimes of the different recombination mechanisms. We will present a robust routine to ascertain the reliability of the obtained results. This routine is based on experimentally measured material properties and on the analysis of the band diagram evolution during the PL transient. Our approach is not limited to the analysis of bare perovskites. We will show also a first analysis of the influence of the absorber interfaces on the trPL. The mentioned routine for trPL simulation can be further extended with the inclusion of photon recycling.^[4]

References:

[1] Kirchartz, T., Márquez, J. A., Stolterfoht, M., Unold, T., Photoluminescence-Based Characterization of Halide Perovskites for Photovoltaics. Adv. Energy Mater. 2020, 10, 1904134

[2] Staub, F., Hempel, H., Hebig, J-C., Mock, J., Paetzold, U. W., Rau, U., Unold, T., Kirchartz, T., Beyond Bulk Lifetimes: Insights into Lead Halide Perovskite Films from Time-Resolved Photoluminescence. Phys. Rev. Applied 2016, 6, 044017

[3] Haddad J., Krogmeier B. Klingebiel B., Krückemeier L., Melhem, S., Liu Z, Hüpkes J., Mathur S., Kirchartz T., Analyzing Interface Recombination in Lead-Halide Perovskite Solar Cells with Organic and Inorganic Hole-Transport Layers, Adv. Mater. Interfaces 2020, 7, 2000366.

[4] Aeberhard, U., Zeder, S., Ruhstaller, B., Reconciliation of dipole emission with detailed balance rates for the simulation of luminescence and photon recycling in perovskite solar cells, Opt. Express 2021, 29, 14773.

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