Organic-to-inorganic structural chirality transfer in a 2D hybrid perovskite and impact on Rashba-Dresselhaus spin-orbit coupling

TLDR

Chirality and asymmetry transfer across structural motifs and length scales underpins unique functionalities in biological and synthetic systems. We introduce structural chirality transfer across the organic–inorganic interface in two‑dimensional hybrid perovskites using chiral organic cations. The chiral spacer cations R‑(+)‑ or S‑(−)‑1‑(1‑naphthyl)ethylammonium form asymmetric hydrogen bonds with lead bromide layers, inducing symmetry‑breaking helical distortions in the inorganic lattice that are absent with racemic spacers. First‑principles calculations reveal a substantial bulk Rashba‑Dresselhaus spin‑splitting in the conduction band with opposite spin textures for R‑ and S‑hybrids, establishing chirality transfer as a design route for spin‑polarized properties in hybrid perovskite spintronics.

Abstract

Abstract Translation of chirality and asymmetry across structural motifs and length scales plays a fundamental role in nature, enabling unique functionalities in contexts ranging from biological systems to synthetic materials. Here, we introduce a structural chirality transfer across the organic–inorganic interface in two-dimensional hybrid perovskites using appropriate chiral organic cations. The preferred molecular configuration of the chiral spacer cations, R -(+)- or S -(−)-1-(1-naphthyl)ethylammonium and their asymmetric hydrogen-bonding interactions with lead bromide-based layers cause symmetry-breaking helical distortions in the inorganic layers, otherwise absent when employing a racemic mixture of organic spacers. First-principles modeling predicts a substantial bulk Rashba-Dresselhaus spin-splitting in the inorganic-derived conduction band with opposite spin textures between R - and S -hybrids due to the broken inversion symmetry and strong spin-orbit coupling. The ability to break symmetry using chirality transfer from one structural unit to another provides a synthetic design paradigm for emergent properties, including Rashba-Dresselhaus spin-polarization for hybrid perovskite spintronics and related applications.