All Optical Frequency Domain Lifetime Determination for Halide Perovskites under Operating Conditions

Constantin Bach^a, Yitian Du^b^,^c, Yana Vaynzof^b^,^c, Carsten Deibel^a

^aInstitut für Physik, Technische Universität Chemnitz, 09126 Chemnitz, Germany

^bLeibniz Institute for Solid State and Materials Research Dresden (IFW), Helmholtzstraße 20, 01069 Dresden, Germany

^cChair for Emerging Electronic Technologies, Technical University of Dresden, Nöthnitzer Str. 61, 01187 Dresden, Germany

Proceedings of Perovskite Semiconductors: From Fundamental Properties to Devices (PerFunPro)

Konstanz, Germany, 2025 September 8th - 10th

Organizers: Lukas Schmidt-Mende, Vladimir Dyakonov and Selina Olthof

Oral, Constantin Bach, presentation 034
Publication date: 16th July 2025

Despite its critical importance for solar cell device efficiency, the determination of the charge carrier
lifetime under steady state operation in perovskites is still a challenge: commonly used methods such
as time-resolved photoluminescence (TRPL) or intensity-modulated photovoltage spectroscopy (IMVS),
open-circuit voltage decay or transient photovoltage have their drawbacks. While TRPL is applicable to
thin-films as well as full devices it requires a) a precise calibration to get a 1 sun equivalent lifetime and
b) results in a lifetime that might be influenced by the (partial) filling of shallow traps [1]. The voltage based
techniques require the presence of contacts and are therefore only applicable to devices.
In this work we demonstrate the application of intensity modulated photoluminescence spectroscopy
(IMPLS), also called modulated photoluminescence (mPL) [2] or Quasi-Steady-State Photoluminescence
(QSSPL) [3] to halide perovskites. Similarly to IMVS the illumination of the sample is sinusoidally modulated
around a working point. This results in a modulation of the charge carrier density and therefore
of the PL signal (and in full devices of the photovoltage). The evaluation of the frequency-dependent
PL response allows for the determination of the charge carrier lifetime. Although this approach is well
known its application to perovskites has been limited [4],[5]. We apply this method to both halide perovskite
thin films and devices and suggest the use of a simple theoretical model for its evaluation. Albeit their
striking resemblance, IMPLS and IMVS, to our knowledge, have never been compared directly. We address
this omission by performing the two methods back to back and demonstrating the consistency of
the corresponding results.

References:

[1] Marunchenko, A.; Kumar, J.; Tatarinov D.; Pushkarev, A. P.; Vaynzof, Y.; Scheblykin, I. G. Hidden Photoexcitations Probed by Multipulse Photoluminescence. ACS Energy Lett. 2024, 9, 12, 5898–5906.

[2] Brüggemann R.; Reynolds, S. Modulated Photoluminescence Studies for Lifetime Determination in Amorphous-Silicon Passivated Crystalline-Silicon Wafers. J. Non-Cryst. Solids 2006, 352, 1888-1891.

[3] Trupke, T.; Bardos, R.A. Photoluminescence: a Surprisingly Sensitive Lifetime Technique. Proc. 31st IEEE Photovoltaic Specialists Conf. 2005, 903-906

[4] Mahaffey, M.; Onno, A.; Reich, C.; Danielson, A.; Sampath W.; Holman, Z. C. Measuring the Absorber Doping Concentration of Si, CdSeTe, and Perovskite Solar Cells Using Injection-Dependent Quasi-Steady-State Photoluminescence. IEEE J PHOTOVOLT 2023, 13, 800-807.

[5] Gillespie, S. C.; Alvarez, A. O.; Thiesbrummel, J.; Gevaerts, V. S.; Geerligs, L. J.; Ehrler, B.; Coletti, G.; Garnett E. C. Intensity-Modulated Photoluminescence Spectroscopy for Revealing Ionic Processes in Halide Perovskites. ACS Energy Lett. 2025, 10, 3122–3131.

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