Bulk and interfacial ion dynamics in quasi-2D and 3D perovskite LEDs.

Shyantan Dasgupta^a, Liutauras Vaiciulis^a, Ignas Ledzinskas^a, Łukasz Gelczuk^b, Niansheng Xu^c, Tomas Murauskas^a, Adrianna Piejko^d, Eros Radicchi^e, Edoardo Mosconi^f, Marius Franckevicius^a, Feng Gao^c, Vidmantas Gulbinas^a

^aCenter for Physical Sciences and Technology (FTMC), Saulėtekio al. 3, LT-10257 Vilnius, Lithuania

^bDepartment of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, Poland

^cDepartment of Physics Chemistry and Biology (IFM) Linköping University, Linköping 58183, Sweden

^dWroclaw University of Science and Technology, Dept. of Semiconductor Materials Engineering, Wroclaw, Poland

^eUniversity of Verona, Strada Le Grazie 15, 37134 Verona

^fComputational Laboratory for Hybrid and Organic Photovoltaics - Istituto CNR di Scienze e Tecnologie Chimiche (SCITEC-CNR) c/o Department of Chemistry, Biology and Biotechnologies, University of Perugia Via Elce di Sotto 8, 06123 Perugia, Italy

Proceedings of MATSUS Fall 2026 Conference (MATSUSFall26)

B2 Ionic Dynamics and Transport Phenomena in Metal Halide Perovskites

Palma, Spain, 2026 October 26th - 30th

Organizers: Silvia Colella, Sofia Masi and Pablo P. Boix

Oral, Shyantan Dasgupta, presentation 250
Publication date: 22nd July 2026

The optimal performance of both photovoltaic and electroluminescent devices necessitates minimal nonradiative recombination losses. In perovskites, such losses are significantly influenced by carrier traps associated with mobile ions and vacancies, resulting in I–V hysteresis in solar cells and affecting the performance of perovskite-based optoelectronic devices, including photodetectors and LEDs.[1][2] Ideally in a perovskite LED (PeLED) operation, there are cations at the hole injection layer (HIL)/perovskite interface and anions at the electron injection layer (EIL)/perovskite interface, and upon the application of a forward bias, there is a redistribution of the ions at opposite interfaces under sufficient time scales. This consequently alters the energy landscape in a manner that promotes increased radiative recombination in the bulk.[3] In this work, we study ion dynamics at both the HIL and EIL interfaces along with the bulk of quasi-2D and 3D PeLEDs with time-resolved electroluminescence (TrEL) measurements, where we observed that with shorter pulse periods and longer pulse durations, the electroluminescence of quasi-2D PeLEDs underwent significant degradation compared to their 3D counterpart, which showed an opposite trend under similar conditions. We attribute this to the screening of the field at the HIL and EIL interfaces in the quasi-2D PeLEDs due to the presence of bulky spacer cations of the 2D perovskite lattice, which hamper the ionic redistribution at interfaces [4], thus mitigating the radiative recombination in the bulk. The presence of a large number of grain boundaries in quasi-2D PeLEDs is another factor contributing to strong ionic migration pathways under pulsed operations in their bulk. [5] In this work we corroborate the TrEL results with cross-section Kelvin probe force microscopy (KPFM) analysis and conductive atomic force microscopy (cAFM) studies performed under similar pulsed operations to study the ionic dynamics at the interface and the bulk. We also plan to investigate qualitatively the ionic species, mainly uncoordinated lead (Pb_i) and lead vacancies (V_Pb) formed under such pulsed operations through Deep Level Transient Spectroscopy (DLTS) under similar pulsed conditions implemented in TrEL measurements. Finally, to mitigate these field-induced traps, targeted bulk and interface passivation strategies will be deployed, incorporating novel charged dopants to passivate ionic species, suppress non-radiative recombination centers, and stabilize the quasi-2D PeLED lattice.

References:

[1] [1] R. Gegevičius, M. Franckevičius, J. Chmeliov, W. Tress, V. Gulbinas, “Electroluminescence Dynamics in Perovskite Solar Cells Reveals Giant Overshoot Effect” J. Phys. Chem. Lett. 2019, 10, 1779–1783.

[2] [1] S. Dasgupta, W. Żuraw, T. Ahmad, L. A. Castriotta, E. Radicchi, W. Mróz, M. Ścigaj, Ł. Pawlaczyk, M. Tamulewicz-Szwajkowska, M. Trzciński, J. Serafińczuk, E. Mosconi, A. Di Carlo, F. De Angelis, A. Dudkowiak, K. Wojciechowski, “Modification of a Buried Interface with Bulky Organic Cations for Highly Stable Flexible Perovskite Solar Cells” ACS Appl. Energy Mater. 2022, 5, 15114–15124.

[3] [1] M. A. Torre Cachafeiro, N. K. Kumawat, F. Gao, W. Tress, “Pulsed operation of perovskite LEDs: a study on the role of mobile ions” Natl. Sci. Rev. 2025, 12, DOI 10.1093/nsr/nwae128.

[4] [1] M. Pegu, S. Kazim, T. Bu, D. M. Bassani, S. Ahmad, “Deciphering the Orientation of the Aromatic Spacer Cation in Bilayer Perovskite Solar Cells through Spectroscopic Techniques” 2021,

[5] [1] W. Bai, T. Xuan, H. Zhao, H. Dong, X. Cheng, L. Wang, R. J. Xie, “Perovskite Light-Emitting Diodes with an External Quantum Efficiency Exceeding 30%” Adv. Mater. 2023, 35, 1–8.

Acknowledgements:

The presenting author acknowledges funding from the Research Council of Lithuania LMT project (2400- PL 789).

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