Observation of excitonic resonances in the second harmonic spectrum of MoS${}_2$

Abstract

We measure the second-harmonic (SH) response of MoS${}_2$ in a broad fundamental photon energy range between 0.85 and 1.7 eV, and present a continuous SH spectrum capturing signatures of both the fundamental A and B excitons in addition to the intense C resonance. Moreover, we interpret our results in terms of the first exciton simulation of the SH properties of multi-layered MoS${}_2$ samples, represented by a study of trilayer MoS${}_2$. The good agreement between theory and experiments allows us to establish a connection between the measured spectrum and the underlying electronic structure, in the process elucidating the non-linear excitation of electron-hole pairs.

References in corpus (10)

• Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
• Vertical Field Effect Transistor based on Graphene-WS2 Heterostructures for flexible and transparent electronics
• Optical Spectrum of MoS${}_2$: Many-body Effects and Diversity of Exciton States
• Direct observation of the transition from indirect to direct bandgap in atomically thin epitaxial MoSe2
• Measurement of the optical dielectric function of transition metal dichalcogenide monolayers: MoS2, MoSe2, WS2 and WSe2
• Non-linear Optical Spectroscopy of Excited Exciton States for Efficient Valley Coherence Generation in WSe2 Monolayers
• Field-effect transistors and intrinsic mobility in ultra-thin MoSe2 layers
• High Mobility WSe2 p- and n-Type Field Effect Transistors Contacted by Highly Doped Graphene for Low-Resistance Contacts
• Mono- and Bilayer WS2 Light-Emitting Transistors
• Nonlinear Optical Properties of Transition Metal Dichalcogenide MX${}_2$ (M = Mo, W; X = S, Se) Monolayers and Trilayers from First-principles Calculations

Cited by in corpus (15)

• Electric-field switchable second-harmonic generation in bilayer MoS${}_2$ by inversion symmetry breaking
• Interlayer excitons in van der Waals heterostructures: Binding energy, Stark shift, and field-induced dissociation
• Intrinsic exciton states mixing and non-linear optical properties in transition metal dichalcogenide monolayers
• Two-dimensional Materials with Giant Optical Nonlinearities Near the Theoretical Upper Limit
• Excitonic structure of the optical conductivity in MoS${}_2$ monolayers
• Nonlinear optical selection rules of excitons in monolayer transition metal dichalcogenides
• Second- and third-order optical susceptibilities in bidimensional semiconductors near excitons states
• Gauge invariance of excitonic linear and nonlinear optical response
• High-Resolution Second Harmonic Generation Spectroscopy with Femtosecond Laser Pulses on Excitons in Cu${}_2$O
• Nonlinear optical response of doped mono- and bilayer graphene: length gauge tight-binding model
• Expeditious computation of nonlinear optical properties of arbitrary order with native electronic interactions in the time domain
• Third harmonic generation on exciton-polaritons in bulk semiconductors subject to a magnetic field
• Optical second and third harmonic generation on excitons in ZnSe/BeTe quantum wells
• Dual-Polarization SHG Interferometry for Imaging Antiparallel Domains and Stacking Angles of 2D Heterocrystals
• Gauge-invariant optical selection rules for excitons