Ba-rich compositions in the Ba
x
Sr1–x
MnO3 (BSMO)
cubic perovskite
(3C) system are magnetic ferroelectrics and are of interest for their
strong magnetoelectric coupling. Beyond x = 0.5,
they only form in hexagonal polymorphs. Here, the 3C phase boundary
is pushed to Ba0.6Sr0.4MnO3 for the
thin films. Using regular pulsed laser deposition (rPLD), 3C Ba0.6Sr0.4MnO3 could be epitaxially stabilized
on DyScO3 (101)o substrates by using a 0.1%
O2/99.9% N2 gas mixture. However, the 3C phase
was mixed with the 4H polymorph for films 24 nm thick and above, and
the films were relatively rough. To improve flatness and phase purity,
changes in growth kinetics were investigated and interval PLD (iPLD)
was especially effective. In iPLD, deposition is interrupted after
completion of approximately one monolayer, and the deposit is annealed
for a specific period of time before repeating. Both film flatness
and, more importantly, the volume of the 3C polymorph improved with
iPLD, resulting in 40 nm single-phase films. The results imply that
iPLD improves the persistent nucleation of highly metastable phases
and offers a new approach to epitaxial stabilization of novel materials,
including more Ba-rich BSMO compositions in the 3C structure.