Correlated_phases_and_dynamics_of_excitons_in_van_der_Waals_heterostructures Public

Hadjri, Zacharia (Spring 2024)

Permanent URL: https://etd.library.emory.edu/concern/etds/q524jq237?locale=fr
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Abstract

Semiconducting transition metal dichalcogenides (TMDs) couple strongly to light via the excitation of electrons from the valence band to the conduction band, leaving a hole in the valence band. The excited electron binds to the hole forming an exciton, a hydrogenic quasiparticle. The interactions between excitons and between excitons and charge carriers can realize interesting phases of matter, especially in multi-layer stacks of TMDs. Heterostructures with type-II band structures can host interalyer excitons with a finite out-of-plane dipole moment. Furthermore, either a twist angle between layers or a large lattice mismatch can generate a moir\'{e} potential with a lattice constant orders of magnitude of larger than the underling lattices. This emergent long-wavelength potential is felt by both excitons and charge carriers. 

In this thesis, we report firstly on the observation of electric-field tunable quadrupolar excitons in a WS$_2$/WSe$_2$/WS$_2$ heterotrilayer and an interaction-driven quadrupolar-to-dipolar transition. Secondly, we describe the decay dynamics of interacting Moire excitons in a WS$_2$/WSe$_2$ heterobilayer where the exciton lifetime at short times increases with power up to hundreds of nanoseconds. 

Table of Contents

1 Introduction

2 Background

2.1 TMD vdW Superlattices

2.1.1 Dipolar interlayer excitons in heterobilayers

2.2 Moir´e superlattices

3 Methods

3.1 Exfoliation

3.2 Sample assembly

3.3 Optical measurements

3.3.1 Time-resolved PL measurements

4 Quadrupolar Excitons in a WSe2/WS2 Heterobilayer

4.1 Experimental Details

4.2 Evidence of Quadrupolar Excitons

4.2.1 Model

4.2.2 AB-stacked heterotrilayer

4.3 Control of excitonic lifetime with electric field

4.4 Interaction-driven quadrupolar-dipolar transition

4.5 Exchange splitting and signatures of anti-ferroelectric correlations

About this Honors Thesis

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