Reversible Excitonic Charge State Conversion and High Quasiparticle Densities in PVA-doped Monolayer WS$_2$ on 2D Microsphere Array

TL;DR

This paper demonstrates reversible excitonic charge state conversion and high quasiparticle densities in monolayer WS$_2$ via PVA doping and strain engineering, enabling stable, high-density excitonic states without electrostatic gating.

Contribution

It introduces a novel PVA-based doping method combined with strain application to achieve reversible excitonic charge conversion and enhanced quasiparticle densities in 2D WS$_2$, avoiding traditional doping drawbacks.

Findings

Achieved nearly 100% reversible trion-to-exciton conversion.

Enhanced quasiparticle density with high stability at room temperature.

Boosted trion emission by 41% through strain-induced electron funneling.

Abstract

Controllable quasiparticle radiation in two-dimensional (2D) semiconductors is essential for efficient carrier recombination, tunable emission, and modulation of valley polarization which are strongly determined by both the density and nature of underlying excitonic species. Conventional chemical doping techniques, however, often hinder the reversibility and density of excitonic charge states (exciton and trion) due to unfavorable interactions between dopant and 2D materials. In this work, efficient excitonic charge state conversion is achieved by doping monolayer WS$_2$ using water rinsed PVA and the quasiparticle densities are further enhanced by applying high periodic biaxial strain (up to 2.3%) through a 2D silica microsphere array. The method presented here enables nearly 100% reversible trion-to-exciton conversion without the need of electrostatic gating, while delivering thermally stable trions with a large binding energy of ~56 meV and a high free electron density of ~3$\times$10$^{13}$ cm$^{-2}$ at room temperature. Strain-induced funneling of the PVA-injected free electrons substantially increases the excitonic quasiparticle densities and boosts the trion emission by 41%. Overall, this approach establishes a versatile platform for excitonic charge state conversion and enhanced quasiparticle density in 2D materials, offering promising opportunities for future optical data storage, quantum-light and display technologies.