Surface Circular Photogalvanic Effect in Tl-Pb Monolayer Alloys on Si(111) with Giant Rashba Splitting.

Taniuchi, Ibuki; Akiyama, Ryota; Hobara, Rei; Hasegawa, Shuji · ACS Nano · 2025

basic_science · Level V

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Abstract

We have found that surface superstructures made of "monolayer alloys" of Tl and Pb on Si(111), having giant Rashba effect, produce nonreciprocal spin-polarized photocurrent via circular photogalvanic effect (CPGE) by obliquely shining circularly polarized near-infrared (IR) light. CPGE is here caused by the injection of in-plane spin into spin-split surface-state bands, which is observed only on Tl-Pb alloy layers but not on single-element Tl nor Pb layers. In the Tl-Pb monolayer alloys, despite their monatomic thickness, the magnitude of CPGE is comparable to or even larger than the cases of many other spin-split thin-film materials. A model analysis has provided the relative permittivity <i>ε</i>* of the monolayer alloys to be ∼1.0, which is because the monolayer exists at a transition region between vacuum and the substrate. The present result opens the possibility that we can optically manipulate the spins of electrons even on monolayer materials.