YMnO3 (YMO) thin film is one of the highly studied multiferroic
materials due to its tunable crystalline structure via misfit strain
from the substrate. This tunability involves intriguing physical phenomena
that encourage further explorations for fundamental research and practical
applications. The configuration of the initial atomic layers during
the growth of YMO thin films plays a key role in determining their
physical properties. In the present research, the correlation between
the substrate’s polarity and the misfit strain of the YMO films
is studied comprehensively. The results showed that despite the YMO
films grown on MgO (100) and MgO (111) being under the same growth
conditions and having resulted in the same hexagonal crystal structure
(h-YMO), the films do exhibit distinctly different
microstructures, electronic structures, and magnetic properties. We
suggest that the extent of charge accumulation induced by the surface
polarity of the substrates may have resulted in a substantially different
intermixing feature at the h-YMO/substrate interfaces,
which, in turn, alters the structure and thus the physical properties
of the films. Our results open up the possibility of manipulating
the h-YMO thin film’s magnetic properties
by interfacial engineering without significantly altering the structure
of the films which could benefit the fabrication efficiency for various
next-generation electronics.