The promises of quantum computing is to enable faster and more powerful computation than would ever be possible with a classical processor based on binary logic. Quantum linear optics is one of many promising platforms to build a universal quantum computers by leveraging the interaction between indistinguishable photons.
A common technique to prepare such states is photon heralding, where many identical photons can be generated and used to encode and process information. Photon pairs are typically generated from a second-order nonlinear interaction known as spontaneous parametric downconversion (SPDC). In all existing platforms, materials are used as both a source of optical nonlinearity, and a phase-matching medium, often resulting in narrow-band and non-reconfigurable operation.
2D materials promise to change this, thanks to their high nonlinearity, inherent broadband phase-matching, and highly configurable electro-optical properties. To date SPDC has only been reported in structures with many millions of atoms, stimulating experimental efforts to validate its scaling laws in structures only a few atoms thick. In this thesis we investigate SPDC in group IV transition-metal dichalcogenides (TMDCs), and describe efforts towards the experimental observation of non-resonant SPDC from a diffraction-limited area. Because of the intimate connection between the classical second-harmonic generation (SHG) and the quantum SPDC, the efficiency of one process provides insights on the other. This guides the design of single-photon coincidence measurements required to demonstrate the strong temporal correlations of these entangled states. Measurements are hindered by the presence of a broadband, temporally uncorrelated background, attributed to photoluminescence. This work improves the understanding of the nonlinear quantum optical potential of these crystals, and provides a performance benchmark for these ultra-thin materials.