Strongly Enhanced Electronic Bandstructure Renormalization by Light in Nanoscale Strained Regions of Monolayer MoS$_2$/Au(111) Heterostructures

Abstract

Understanding and controlling the photoexcited quasiparticle (QP) dynamics in monolayer transition metal dichalcogenides lays the foundation for exploring the strongly interacting, non-equilibrium 2D quasiparticle and polaritonic states in these quantum materials and for harnessing the properties emerging from these states for optoelectronic applications. In this study, scanning tunneling microscopy/spectroscopy with light illumination at the tunneling junction is performed to investigate the QP dynamics in monolayer MoS$_2$ on an Au(111) substrate with nanoscale corrugations. The corrugations on the surface of the substrate induce nanoscale local strain in the overlaying monolayer MoS$_2$ single crystal, which result in energetically favorable spatial regions where photoexcited QPs, including excitons, trions, and electron-hole plasmas, accumulate. These strained regions exhibit pronounced electronic bandstructure renormalization as a function of the photoexcitation wavelength and intensity as well as the strain gradient, implying strong interplay among nanoscale structures, strain, and photoexcited QPs. In conjunction with the experimental work, we construct a theoretical framework that integrates non-uniform nanoscale strain into the electronic bandstructure of a monolayer MoS$_2$ lattice using a tight-binding approach combined with first-principle calculations. This methodology enables better understanding of the experimental observation of photoexcited QP localization in the nanoscale strain-modulated electronic bandstructure landscape. Our findings illustrate the feasibility of utilizing nanoscale architectures and optical excitations to manipulate the local electronic bandstructure of monolayer TMDs and to enhance the many-body interactions of excitons, which is promising for the development of nanoscale energy-adjustable optoelectronic and photonic technologies.