Influence of Nanoarchitecture on Charge Donation and
the Electrical-Transport Properties in [(SnSe)1+δ][TiSe2]q Heterostructures
Posted on 2020-06-16 - 15:13
A series
of [(SnSe)1+δ][TiSe2]q heterostructures with systematic changes
in the number of TiSe2 layers in the repeating unit were
synthesized, and both the structure and electronic-transport properties
were characterized. The c-axis lattice parameter
increased linearly as q increased, and the slope
was consistent with the thickness of a TiSe2 layer. In-plane
lattice constants for SnSe and TiSe2 were independent of q. Temperature-dependent resistivity and Hall coefficient
data varied systematically as q was increased. The
low-temperature electrical data was modeled assuming that only electrons
were involved, and the data was fit to a variable range hopping mechanism.
The number of carriers involved in this low-temperature transport
decreased as q increased, indicating that approximately
1/10th of an electron per SnSe bilayer was transferred to the TiSe2. Calculations also indicated that there was charge donation
from the SnSe layer to the TiSe2 layer, resulting in an
ionic bond between the layers, which aided in stabilizing the heterostructures.
The charge donation created a TiSe2–SnSe–TiSe2 block with the properties distinct from the constituent bulk
properties. At high temperatures in large q samples,
the transport data required holes to be activated across a band gap
to be successfully modeled. This high-temperature transport scales
with the number of TiSe2 layers that are not adjacent to
SnSe. Using a consistent model across all of the samples significantly
constrained the adjustable parameters. The charge transfer between
the two constituents results in the stabilization of the heterostructure
by an ionic interaction and the formation of a conducting TiSe2–SnSe–TiSe2 block. This is consistent
with prior reports, where interactions between two-dimensional (2D)
layers and their surroundings (i.e., adjacent layers, substrate, or
atmosphere) have been shown to strongly influence the properties.
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Hamann, Danielle
M.; Bardgett, Dylan; Bauers, Sage R.; Kasel, Thomas W.; Mroz, Austin M.; Hendon, Christopher H.; et al. (2020). Influence of Nanoarchitecture on Charge Donation and
the Electrical-Transport Properties in [(SnSe)1+δ][TiSe2]q Heterostructures. ACS Publications. Collection. https://doi.org/10.1021/acs.chemmater.0c01691