The
thin-film synthesis of high-pressure phases in inorganic compounds
remains a challenge. The synthesis of high-pressure phases in thin-film
form opens potential opportunities for creating unique optoelectronic
devices because high-pressure phases often exhibit intriguing characteristics
that cannot be accessed in ambient phases. We investigated a high-pressure
phase of MgSnN2 with the rocksalt structure (rs-MTN) which
has only been identified in recent years. rs-MTN is a direct-gap compound,
and its (111) plane matches perfectly with GaN(001), which implies
that rs-MTN is a promising candidate for optoelectronic materials
for light-emitting diodes and tandem solar cells. However, single-phase
rs-MTN has never been synthesized in either thin-film or single-crystalline
forms. Herein, single-phase rs-MTN thin films were successfully synthesized
via two routes. One was the high-pressure heat treatment of wurtzite-type
MTN precursor layers, and the other was direct growth onto isostructural
MgO(111) substrates using reactive co-sputtering. The former route
exploited the pressure-induced wurtzite-to-rocksalt transition and
was designed based on first-principles calculations that predicted
a transition pressure of ∼8 GPa. The latter route utilized
epitaxial stabilization on the (111) plane of MgO. The direct growth
of the rs-MTN films with smooth surfaces enabled the investigation
into their optoelectronic properties. Consequently, the rs-MTN films
were found to be n-type semiconductors with electron densities of
an order of 1017 cm–3 and a band gap
of 2.3 eV. These findings provide a platform for developing rs-MTN
as an optoelectronic semiconductor.