Layered Semiconductors Integrated with Polyimide Thin Films for High‐Quality Valleytronic and Quantum‐Photonic Systems

Abstract Dielectric encapsulation/isolation of layered semiconductors is a prerequisite for fabricating high‐quality optoelectronic, valleytronic, and quantum‐photonic devices. While hexagonal boron nitride (hBN) is the current benchmark dielectric, exploration of the most suitable dielectric materials covering the complete substrates continues to expand. This work demonstrates the formation of high optical‐quality excitons in two widely explored layered semiconductors, WSe 2 and WS 2 , integrated into polyimide (PI) thin films of thicknesses ≈500 nm. The photoluminescence (PL) studies at T = 296 K show the formation of neutral excitons ( X 0 ) and trions in fully‐PI‐encapsulated 1L‐WSe 2 with 2‐sigma (2σ) spatial‐inhomogeneity of 4.5 (3.4) meV in X 0 emission energy (linewidth), which is ≈1/3rd (1/5th), respectively, that of inhomogeneity measured in fully‐hBN‐encapsulated 1L‐WSe 2 . A smaller 2σ of 2.1 (2.3) meV in X 0 emission energy (linewidth) is shown for fully‐PI‐encapsulated 1L‐WS 2 . Polarization‐resolved and excitation power‐dependent PL measurements of PI‐isolated 1L‐TMDs at T = 4 K further reveal formations of high‐quality neutral‐biexcitons and negatively‐charged biexcitons, with degrees of valley‐polarization up to 21% under non‐resonant excitation. Furthermore, the fully‐PI‐encapsulated 1L‐WSe 2 also hosts single quantum emitters with narrow linewidths and high‐spectral stability. This work indicates that PI thin films may serve the purpose of high‐quality dielectric material for integrating the layered materials on a wafer scale.