Optical and dielectric properties of MoO$_3$ nanosheets for van der Waals heterostructures

TL;DR

This study explores MoO$_3$ nanosheets as a transparent, birefringent 2D insulator with potential for use in van der Waals heterostructures, offering an alternative to hBN with optical anisotropy and encapsulation benefits.

Contribution

It provides the first detailed measurement of MoO$_3$'s anisotropic optical properties and demonstrates its suitability for polarization control and encapsulation in 2D heterostructures.

Findings

MoO$_3$ exhibits strong birefringence comparable to other 2D materials.

MoO$_3$ nanosheets are transparent in the visible spectrum.

Encapsulation with MoO$_3$ improves exciton linewidth and quantum emitter stability.

Abstract

Two-dimensional (2D) insulators are a key element in the design and fabrication of van der Waals heterostructures. They are vital as transparent dielectric spacers whose thickness can influence both the photonic, electronic, and optoelectronic properties of 2D devices. Simultaneously, they provide protection of the active layers in the heterostructure. For these critical roles, hexagonal Boron Nitride (hBN) is the dominant choice due to its large bandgap, atomic flatness, low defect density, and encapsulation properties. However, the broad catalogue of 2D insulators offers exciting opportunities to replace hBN in certain applications that require transparent thin layers with additional optical degrees of freedom. Here we investigate the potential of single-crystalline Molybdenum Oxide (MoO$_3$) as an alternative 2D insulator for the design of nanodevices that require precise adjustment of the light polarization at the nanometer scale. First, we measure the wavelength-dependent refractive indices of MoO$_3$ along its three main crystal axes and determine the in-plane and out-of-plane anisotropy of its optical properties. We find the birefringence in MoO$_3$ nanosheets compares favorably with other 2D materials that exhibit strong birefringence, such as black phosphorus, ReS$_2$, or ReSe$_2$, in particular in the visible spectral range where MoO$_3$ has the unique advantage of transparency. Finally, we demonstrate the suitability of MoO$_3$ for dielectric encapsulation by reporting linewidth narrowing and reduced inhomogeneous broadening of 2D excitons and optically active quantum emitters, respectively, in a prototypical monolayer transition-metal dichalcogenide semiconductor. These results show the potential of MoO$_3$ as a 2D dielectric layer for manipulation of the light polarization in vertical 2D heterostructures.