Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 152, Issue 22, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/5.0006429
Keywords
-
Funding
- Air Force Office of Scientific Research [FA9550-18-1-0058]
- National Science Foundation CAREER program [CHE-1848369]
Ask authors/readers for more resources
We use excited-state quantum chemistry techniques to investigate the intraband absorption of doped semiconductor nanoparticles as a function of doping density, nanoparticle radius, and material properties. Modeling the excess electrons as interacting electrons confined to a sphere, we find that the excitation evolves from single-particle to plasmonic with increasing number of electrons at fixed density, and the threshold number of electrons to produce a plasmon increases with density due to quantum confinement and electron-hole attraction. In addition, the excitation passes through an intermediate regime where it is best characterized as an intraband exciton. We compare equation-of-motion coupled-cluster theory with those of more affordable single-excitation theories and identify the inclusion of electron-hole interactions as essential to describing the evolution of the excitation. Despite the simplicity of our model, the results are in reasonable agreement with the experimental spectra of doped ZnO nanoparticles at a doping density of 1.4 x 10(20) cm(-3). Based on our quantum chemistry calculations, we develop a schematic model that captures the dependence of the excitation energy on nanoparticle radius and electron density.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available