Emission Polarization Anisotropy and Directionality of Phonon Modes in Two-Dimensional Metal Halide Perovskites

Roman Krahne^a, Mehrdad Faraji^a, Alexander Schleusener^a, Lin-Han Li^b, Miao-Ling Lin^b, Ping-Heng Tan^b, Martina Borreani^a

^aOptoelectronics Research Line, Istituto Italiano di Tecnologia, Via Morego 20, 16163 Genoa, Italy

^bInstitute of Semiconductors, Chinese Academy of Sciences, China

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2024 Conference (MATSUS24)

#2Dpero - 2D perovskites: chemical versatility, photophysics and applications

Barcelona, Spain, 2024 March 4th - 8th

Organizers: Claudio Quarti and Yana Vaynzof

Oral, Roman Krahne, presentation 315
DOI: https://doi.org/10.29363/nanoge.matsus.2024.315
Publication date: 18th December 2023

Metal-halide perovskite materials demonstrated extraordinary performance in solar cells and light emission in recent years, and their layered low-dimensional counterparts promise even greater tunability due to the huge variety of molecules available for the organic phase. [1, 2] Single octahedra-layer structures act as two-dimensional quantum wells, showing strong confinement and large exciton binding energies. Band gap and light emission can be designed by the choice of the organic cations.[3-5]

We investigate the emission from single plates of two-dimensional Ruddlesden-Popper metal-halide perovskites with different organic cations by angle-resolved polarized photoluminescence (PL) spectroscopy. The choice of the organic cation strongly influences the number of PL peaks that we observe in the band edge emission, and the different PL peaks manifest a strong angle dependence in their linear polarization, manifesting an angle-dependent intensity maximum along one of the principal axes of the octahedra lattice. Such a marked intensity maximum along one in-plane direction is surprising, since theory predicts isotropic in-plane exciton wave function distributions [6]. Therefore, electron-phonon coupling could be at the origin of the distinct anisotropy of the emission polarization, since a large number of phonon bands in such materials show strong directionality. [7, 8] We investigate the angle resolved phonon response together with the emission polarisation of the single plates with resonant and non-resonant Raman spectroscopy, which allows for a detailed correlation of the directionality of the emission with the phonons. The combined angle-resolved emission and Raman spectroscopy allows for a detailed investigation of the exciton fine structure and assignment of confined exciton states and phonon side bands.

References:

[1] A. Dey, et al.,“State of the Art and Prospects for Halide Perovskite Nanocrystals”. ACS Nano, 15, 10775-10981, (2021).

[2] X. Li, J.M. Hoffman, and M.G. Kanatzidis, “The 2D Halide Perovskite Rulebook: How the Spacer Influences Everything from the Structure to Optoelectronic Device Efficiency”. Chem. Rev., 121, 2230-2291, (2021).

[3] B. Dhanabalan, G. Biffi, A. Moliterni, V. Olieric, C. Giannini, G. Saleh, L. Ponet, M. Prato, M. Imran, L. Manna, R. Krahne, S. Artyukhin, and M.P. Arciniegas, “Engineering the Optical Emission and Robustness of Metal-Halide Layered Perovskites through Ligand Accommodation”. Adv. Mater., 33, 2008004, (2021).

[4] B. Dhanabalan, A. Castelli, M. Palei, D. Spirito, L. Manna, R. Krahne, and M. Arciniegas, “Simple fabrication of layered halide perovskite platelets and enhanced photoluminescence from mechanically exfoliated flakes”. Nanoscale, 11, 8334-8342, (2019).

[5] S. Kutkan, B. Dhanabalan, M.-L. Lin, P.-H. Tan, A. Schleusener, M.P. Arciniegas, and R. Krahne, “Impact of the organic cation on the band-edge emission of two-dimensional lead–bromide perovskites”. Nanoscale, 15, 12880-12888, (2023).

[6] C. Quarti, G. Giorgi, C. Katan, J. Even, and M. Palummo, “Exciton Ground State Fine Structure and Excited States Landscape in Layered Halide Perovskites from Combined BSE Simulations and Symmetry Analysis”. Adv. Opt. Mater., n/a, 2202801, (2023).

[7] M.-L. Lin, B. Dhanabalan, G. Biffi, Y.-C. Leng, S. Kutkan, M.P. Arciniegas, P.-H. Tan, and R. Krahne, “Correlating Symmetries of Low-Frequency Vibrations and Self-Trapped Excitons in Layered Perovskites for Light Emission with Different Colors”. Small, 18, 2106759, (2022).

[8] B. Dhanabalan, Y.-C. Leng, G. Biffi, M.-L. Lin, P.-H. Tan, I. Infante, L. Manna, M.P. Arciniegas, and R. Krahne, “Directional Anisotropy of the Vibrational Modes in 2D-Layered Perovskites”. ACS Nano, 14, 4689-4697, (2020)

Acknowledgements:

A.S. acknowledges the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Funding Program (Project Together, grant agreement No.101067869).

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