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Inversion symmetry breaking could lead to the creation of a Rashba–Dresselhauls magnetic field, which plays the key role in spintronic devices. In this work, we propose and develop a composition gradient engineering approach that breaks inversion symmetry into inorganic halide perovskites with strong spin–orbit coupling. We synthesize epitaxial CsPbBr x Cl (3− x ) with Br/Cl composition gradient by a two-step chemical vapor deposition approach. Through optoelectronic measurements, we show the presence of circular photogalvanic effects (CPGEs), evidencing a Rashba-like spin polarized band structure. By spatially resolved photoluminescence spectra, we find that the observed CPGE is likely a cumulative result of inversion symmetry-broken interfaces featured by abrupt and stepwise composition gradient between the pristine and separated daughter phases. Our work suggests an avenue in engineering the spintronic property of halide perovskites for information processing.
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Circular photogalvanic spectroscopy of Rashba splitting in 2D hybrid organic–inorganic perovskite multiple quantum wells
Abstract The two-dimensional (2D) Ruddlesden−Popper organic-inorganic halide perovskites such as (2D)-phenethylammonium lead iodide (2D-PEPI) have layered structure that resembles multiple quantum wells (MQW). The heavy atoms in 2D-PEPI contribute a large spin-orbit coupling that influences the electronic band structure. Upon breaking the inversion symmetry, a spin splitting (‘Rashba splitting’) occurs in the electronic bands. We have studied the spin splitting in 2D-PEPI single crystals using the circular photogalvanic effect (CPGE). We confirm the existence of Rashba splitting at the electronic band extrema of 35±10 meV, and identify the main inversion symmetry breaking direction perpendicular to the MQW planes. The CPGE action spectrum above the bandgap reveals spin-polarized photocurrent generated by ultrafast relaxation of excited photocarriers separated in momentum space. Whereas the helicity dependent photocurrent with below-gap excitation is due to spin-galvanic effect of the ionized spin-polarized excitons, where spin polarization occurs in the spin-split bands due to asymmetric spin-flip.
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- Award ID(s):
- 1810096
- PAR ID:
- 10154271
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 11
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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