Bulk Rashba Effect Splitting and Suppression in Polymorphs of Metal Iodine Perovskites

Autor(es)

de Araujo, Luis Octavio ^[1] ; Sabino, Fernando P. ^[2] ; Rego, Celso R. C. ^[3] ; Guedes-Sobrinho, Diego ^[1]

Afiliação do(s) autor(es)

^[1] Univ Fed Parana, Chem Dept, BR-81531980 Curitiba, Parana - Brazil

^[2] Fed Univ ABC, BR-09210580 Santo Andre, SP - Brazil

^[3] Karlsruhe Inst Technol, Inst Nanotechnol Hermann von Helmholtz Pl, D-76021 Karlsruhe - Germany

• Tipo de documento: Artigo Científico
• Fonte: Journal of Physical Chemistry Letters; v. 12, n. 30, p. 7245-7251, AUG 5 2021.
• Citações Web of Science: 0

Resumo

We quantified the bulk Rashba splitting and suppression in polymorphs of MA(Pb, Sn, Ge, or Si)I-3 perovskites. The low-computational-cost DFT-1/2 quasiparticle correction was performed for all structures, combined with the inclusion of spin-orbit coupling (SOC) effects. The presence of SOC and symmetry breaking from the metal offcentering octahedral distortion are indispensable and essential conditions for Rashba splitting, whose magnitude emerges from the Pb -> Si sequence. Additionally, the quasiparticle correction provides energy bandgaps for MAPbI(3) (cubic, tetragonal, and orthorhombic), MASnI(3) (cubic and tetragonal), and MAGeI(3) (cubic) that are in outstanding agreement with experimental results. However, while gap energies are yielded collaboratively from the metal off-centering and relative octahedral tiltings, the bulk Rashba suppression is reached for metal on-centering (octahedral platonic-like) configurations that are thermodynamically stable even when the charge polarization is kept invariant among metal-I bonds in the polymorphs. (AU)

• Processo FAPESP: 19/21656-8 - Métodos de Big Data para ajustar perovskitas às propriedades alvo: ligas, defeitos e dopagem
• Beneficiário: Fernando Pereira Sabino
• Modalidade de apoio: Bolsas no Brasil - Pós-Doutorado