Chiral Hybrid Perovskites (R-/S-CLPEA)4Bi2I10 with Enhanced Chirality and Spin-Orbit Coupling Splitting for Strong Nonlinear Optical Circular Dichroism and Spin Selectivity Effects

Chiralhybrid halide perovskites have attracted considerable attentionin optoelectronics and spintronics owing to their unique optical,electric, and spin-orbit coupling (SOC) properties. In thisarticle, with focus on the design scheme to increase the nonlinearoptical (NLO) circular dichroism (CD) and spin selectivity effectsby assembling chlorine-modified chiral R-/S-CLPEA [CLPEA = 1-(4-chlorophenyl)-ethylamine] into bismuth-basedperovskites, a pair of chiral hybrid perovskites (R-/S-CLPEA)(4)Bi2I10 were synthesized and characterized experimentally. A large NLO CDeffect and strong spin-dependent charge transport were confirmed bythe experimental measurements. The unique chirality-induced spin textureswere illustrated in the SOC band structures from first-principlessimulations. The combined theoretical and experimental results demonstratethat it is the synergic effect of large chirality of CLPEA and strongSOC effect of the Bi2I10 dimer that endows theseperovskites with unique chiral spin textures, strong NLO CD effect,and remarkable spin-dependent charge transport properties, which areof importance for the functional design of chiral perovskites in nonlinearoptics and spintronics.

Automated summary

In this article, chiral hybrid halide perovskites (R-/S-CLPEA)(4)Bi2I10 were synthesized and characterized, and their unique optical and spin properties were investigated. The experimental measurements confirmed the large nonlinear optical circular dichroism effect and strong spin-dependent charge transport. Theoretical simulations demonstrated the chirality-induced spin textures in the band structures. These perovskites showed potential for application in nonlinear optics and spintronics.