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Circular photogalvanic spectroscopy of Rashba splitting in 2D hybrid organic–inorganic perovskite multiple quantum wells

Journal Article · · Nature Communications
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.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE); Univ. of Utah, Salt Lake City, UT (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC)
Grant/Contract Number:
SC0014579
OSTI ID:
1619767
Alternate ID(s):
OSTI ID: 1624238
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United Kingdom
Language:
English

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