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

Xiaojie Liu, Ashish Chanana, Uyen Huynh, Fei Xue, Paul Haney, Steve Blair, Xiaomei Jiang () and Z. V. Vardeny ()
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Xiaojie Liu: University of Utah
Ashish Chanana: University of Utah
Uyen Huynh: University of Utah
Fei Xue: National Institute of Standards and Technology
Paul Haney: National Institute of Standards and Technology
Steve Blair: University of Utah
Xiaomei Jiang: University of South Florida
Z. V. Vardeny: University of Utah

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-019-14073-6

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