Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.033
Publication date: 16th December 2024
The chemical and structural flexibility of layered (2D) hybrid organic–inorganic metal-halide perovskites (HOIPs) has been proposed as an ideal platform for the synthesis of novel circularly polarized light emitters through the incorporation of chiral organic molecules, showing potential application in optoelectronics and spintronics.[1,2] Furthermore, the weak forces between the organic layers in the case of Ruddlesden-Popper 2D HOIPs, allow mechanical exfoliation of bulk crystals to obtain flakes[3] making possible their integration in nanodevices. Most studies to date have focused on bulk compounds, specifically on the unstable and toxic Pb-based HOIPs,[1,2] although Mn-based HOIPs apart from lower toxicity can show not only chiroptical but also magnetic properties[4]. In this work, we report the chiroptical properties of R- and S-β-methylphenethylammonium Mn chloride HOIPs, which exhibit antiferromagnetic order,[5] in both bulk and mechanically exfoliated flakes. In these compounds, we observe the red photoluminescence (PL) emission originating from the octahedrally coordinated Mn2+, with a PL redshift as they transition from bulk to flake form. Circular dichroism (CD) and circularly polarized luminescence (CPL) mirrored signals confirm the chirality transfer from the organic cations to the inorganic lattice in bulk materials, presenting glum values (0.01) among the highest reported for chiral hybrid Mn halides. This chirality is preserved in the exfoliated flakes, reaching degrees of circularly polarized PL (P) of up to 17% at 80K, which systematically decrease with increasing temperature as previously observed in 2D Pb-based HOIPs[6]. Additionally, angle-resolved PL measurements show that the PL emission and P are isotropic. Therefore, our results demonstrate that these 2D Mn-based HOIPs are highly valuable, as they can compete with their Pb analogs and offer additional functionalities for spin-optoelectronic applications, thanks to the magnetic behavior associated with Mn2+.[7]
This work is supported under Projects PID2021-122511OB-I00, PID2021-128004NB-C21, PID2021-124484OB-I00 and PID2019-104772GB-I00 funded by Spanish MICIU/AEI/10.13039/501100011033 and by ERDF/EU; under the María de Maeztu Units of Excellence Programme (Grants CEX2020-001038-M, CEX2020-001067-M) and Spanish MICIU/AEI/10.13039/501100011033 and ESF+ for Y.A. PhD grant PRE2021-099999). This work was also supported by the FLAG-ERA grant MULTISPIN, by the Spanish MICIU/AEI/10.13039/501100011033, and the European Union NextGenerationEU/PRTR with grant number PCI2021-122038-2A; and European Union’s Horizon 2020 Research and Innovation Programme under the Marie Skłodowska–Curie grant agreement no. 101024823 (INFLED). Additionally, this work was carried out with support from the Basque Science Foundation for Science (IKERBASQUE) – HYMNOS project and the “Ramón y Cajal” Programme by the Spanish MICIU/AEI/10.13039/501100011033 and European Union NextGenerationEU/PRTR (grants no. RYC2021-034836-I and RYC2021-031705-I).
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