Proceedings of nanoGe September Meeting 2017 (NFM17)
Publication date: 20th June 2016
In this talk, I will discuss recent work from our group on characterizing, simulating, and engineering nanocrystal surfaces. First, I will present ab initio molecular dynamics (AIMD) on experimentally-relevant sized lead sulfide (PbS) NCs constructed with thiol or Cl, Br, and I anion surfaces. These simulations allow us to investigate the vibrational and dynamic electronic structure. We show that electron-phonon interactions can experimentally explain observed thermal broadening and carrier cooling rates in Pb-chalcogenide NCs. We demonstrate that electron-phonon interactions are suppressed in halide terminated NCs due reduction of both the thermal displacement of surface atoms and the spatial overlap of the charge carriers with these large vibrations. This work showing how surface engineering – guided by simulations – can be used to systematically control carrier dynamics emphasizes how important exact knowledge of NC shape and atomic structure it. A simple particle in a sphere is no longer sufficient. With the increasing complexity of multi-shell and graded core-shell structures, determining the exact shape and structure of NCs is challenging. Here, I will discuss how a combination of x-ray scattering and electron microscopy techniques can be used to obtain the detailed structures needed for simulation.