Over the past 12 years since the groundbreaking work on graphene, the field of 2D layered materials has grown by leaps and bounds as more materials are theoretically predicted and experimentically verified. These materials and their unique electronic, optical, and mechanical properties have inspired the scientific community to explore and investigate novel, fundamental physical phenomena as well create and refine technological devices which leverage the host of unique benefits which these materials possess. In the past few years, this burgeoning field has heavily moved towards combining layers of various materials into novel heterostructures. These heterostructures are an exciting area of research because of the plethora of exciting possibilities and results which arise due to the large number of heterostructure combinations and configurations. Particularly, the research into the optical properties of these layered materials and their heterostructures under confinement provides another exciting avenue for developing optoelectric devices.;In this dissertation, I present work on the synthesis of Bi2Se 3 nanostructures via chemical vapor deposition (CVD) and the study of the optical properties of these nanostructures and their heterostructures with MoS2. The bulk of the current published work on Bi2Se 3 has focused on the exotic topological properties of its surface states, both interesting fundamental physics purposes as well as for studying avenues for spintronics. In contrast, the work presented here focuses on studying the optical properties of Bi2Se3 nanostructures and how these properties evolve when subjected to confinement. Specifically, the absorbance of singlecrystal Bi2Se3 with sizes tailored down to a few nanometers in diameter and a few quintuple layers (QLs) in thickness. We find a dramatically large bandgap, Eg ≥ 2.5 eV, in the smallest particles which is much higher than that seen in 1QL measurements taken with ARPES. Additionally, utilizing photoluminescence (PL) measurements of CVD-grown Bi 2Se3 nanoplates with few QL thickness and effective diameters in the tens of nanometers, Bi2Se3 nanoplatelets show a strong PL response with photon energies, Eph, in the ∼2.1-2.3 eV region. Annealing of these samples at 200?C for 4 hours increases the PL intensity by a factor of 2.4 to 3 for nanoscale Bi2Se3. Furthermore, this work investigates the synthesis of the novel Bi2Se3-MoS 2 heterocrystal that arises from epitaxial growth of Bi2Se 3 on MoS2 substrates. These heterocrystals consist of n layers of Bi2Se3 perfectly rotationally-aligned epitaxially with the monolayer MoS2 substrate. Investigation into these heterocystals produced results which include 100% PL-suppression of the MoS2 PL response, precisely tunable band-gap ranging from 1.1eV ? 0.75 eV, and a spectacular wide-band enhancement of photo-absorption over nearly the entire solar spectral wavelengths. Finally, a simple laser-treatment appears to dramatically reverse these changes, attributed to breakdown of the rotational congruency between the MoS2 and Bi2Se3 layers. These heterocrystals have immense potentials for novel physics and applications in nanoelectronics, optoelectronics and energy sciences at the atomically-thin scale.
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