| Autor: |
Diego Guedes-Sobrinho, Danilo Neves Silveira, Luis O. de Araujo, Jônatas Favotto Dalmedico, W. Wenzel, Y. Pramudya, Maurício J. Piotrowski, Celso R. C. Rêgo |
| Jazyk: |
angličtina |
| Rok vydání: |
2023 |
| Předmět: |
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| Zdroj: |
Scientific Reports, Vol 13, Iss 1, Pp 1-11 (2023) |
| Druh dokumentu: |
article |
| ISSN: |
2045-2322 |
| DOI: |
10.1038/s41598-023-31220-8 |
| Popis: |
Abstract Two-dimensional hybrid lead iodide perovskites based on methylammonium (MA) cation and butylammonium (BA) organic spacer—such as $${\hbox {BA}_{2}\hbox {MA}_{n-1}\hbox {Pb}_{n}\hbox {I}_{3n+1}}$$ BA 2 MA n - 1 Pb n I 3 n + 1 —are one of the most explored 2D hybrid perovskites in recent years. Correlating the atomistic profile of these systems with their optoelectronic properties is a challenge for theoretical approaches. Here, we employed first-principles calculations via density functional theory to show how the cation partially canceled dipole moments through the $${{\hbox {NH}_{3}}^{+}}$$ NH 3 + terminal impact the structural/electronic properties of the $${\hbox {Pb}_{n}\hbox {I}_{3n+1}}$$ Pb n I 3 n + 1 sublattices. Even though it is known that at high temperatures, the organic cation assumes a spherical-like configuration due to the rotation of the cations inside the cage, our results discuss the correct relative orientation according to the dipole moments for ab initio simulations at 0 K, correlating well structural and electronic properties with experiments. Based on the combination of relativistic quasiparticle correction and spin-orbit coupling, we found that the MA horizontal-like configuration concerning the inorganic sublattice surface leads to the best relationship between calculated and experimental gap energy throughout n = 1, 2, 3, 4, and 5 number of layers. Conversely, the dipole moments cancellation (as in BA-MA aligned-like configuration) promotes the closing of the gap energies through an electron depletion mechanism. We found that the anisotropy $$\rightarrow$$ → isotropy optical absorption conversion (as a bulk convergence) is achieved only for the MA horizontal-like configuration, which suggests that this configuration contribution is the majority in a scenario under temperature effects. |
| Databáze: |
Directory of Open Access Journals |
| Externí odkaz: |
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