posted on 2021-08-02, 12:10authored byRobynne
L. Paldi
<p>Vertically-aligned nanocomposite
thin films have recently emerged as a platform to combine multifunctionalities.
These materials are made up of two co-grown immiscible phases where one phase
grows as anisotropic vertical pillars in the matrix of the second phase. Many
of the classic systems of VAN consist of oxide-oxide nanocomposites but more
recently the oxide-metal combinations have been realized with great promise of
combining metal and oxide functionalities. In particular for streamlined
processing of hybrid plasmonic metamaterials with nanoscale light matter
manipulation. The work presented in this dissertation is towards realizing
oxide-metal VAN with ZnO as the matrix. ZnO is particularly interesting for
composite design due to its breadth of properties including piezoelectricity,
semiconductivity, relative non-toxicity, and wide-spread availability making it
applicable for sustainable and compact device designs. In the first part of
this dissertation, ZnO is combined with plasmonic Au to form ZnO-Au VAN. The
ZnO-Au design demonstrates highly ordered and tunable in-plane periodicity
which results in strong hyperbolic dispersion and plasmonic response, making it
desirable for hybrid plasmonic hyperbolic metamaterials. The resultant
morphology has spontaneous and controllable quasi-hexagonal in-plane order and
a tailorable microstructure through deposition parameter control.</p>
<p> In the second part of this work, a new
oxide-nanoalloy VAN system of ZnO-Au<sub>x</sub>Au<sub>1-x</sub> is designed to
reduce the optical losses of Au in hyperbolic metamaterials application. Ag is
combined with Au to reduce losses and overcome particle-in matrix morphology of
ZnO-Ag, with the result being reduced losses as compared to ZnO-Au. The third
part investigated the tunability of the new oxide-nanoalloy VAN ZnO-Au<sub>x</sub>Ag<sub>1-x</sub>
through the oxygen background pressure. Both optical properties and morphology
were shown to be strongly correlated with the background pressure. </p>
<p>In the final part,
ZnO is combined with ferromagnetic metals of Co, Ni, and their alloy Co<sub>x</sub>Ni<sub>1-x</sub>
for ferromagnetic/piezoelectric coupling. Oxidation was found to occur due to
the high reactivity of Ni and Co to oxygen ambient, with ZnO-Co growing as an oxide-oxide
VAN of ZnO-CoO. ZnO-Ni and ZnO-Co<sub>x</sub>Ni<sub>1-x</sub> demonstrated
anisotropic ferromagnetic and optical response. The work presented in the body
of this thesis serve to demonstrate ZnO-based nanocomposite towards future
device and heterostructure integrations in both optical and acoustic
applications.</p>
Funding
U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award DE-SC0020077
Purdue Doctoral Fellowship
Laboratory Directed Research and Development program at Sandia National Laboratories under award DE-NA-003525