Self-Hybridized Exciton-Polaritons in Sub-10-nm-Thick WS₂ Flakes: Roles of Optical Phase Shifts at WS₂/Au Interfaces

Exciton–polaritons (EPs) can be formed in transition metal dichalcogenide (TMD) multilayers sustaining optical resonance modes without any external cavity. The self-hybridized EP modes are expected to depend on the TMD thickness, which directly determines the resonance wavelength. Exfoliated WS₂ flakes were prepared on SiO₂/Si substrates and template-stripped ultraflat Au layers, and the thickness dependence of their EP modes was compared. For WS₂ flakes on SiO₂/Si, the minimum flake thickness to exhibit exciton–photon anticrossing was larger than 40 nm. However, for WS₂ flakes on Au, EP mode splitting appeared in flakes thinner than 10 nm. Analytical and numerical calculations were performed to explain the distinct thickness-dependence. The phase shifts of light at the WS₂/Au interface, originating from the complex Fresnel coefficients, were as large as π/2 at visible wavelengths. Such exceptionally large phase shifts allowed the optical resonance and resulting EP modes in the sub-10-nm-thick WS₂ flakes. This work helps us to propose novel optoelectronic devices based on the intriguing exciton physics of TMDs.