Mn2Mo3O8 simultaneously exhibits
ferroelectric polarization and unique magnetic properties, such as
strong magnetoelectric coupling and magnetic-field-induced collinear-to-noncollinear
spin structure transitions. However, practical applications of multiferroic
Mn2Mo3O8 are hindered by low spontaneous
magnetization (0.01 μ
B/f.u. at 2
K) owing to the collinear spin order. Herein, we report the emergence
of large spontaneous magnetization of 0.35 μ
B/f.u. by applying 0.5% tensile strain to c-axis-oriented Mn2Mo3O8 epitaxial
films. The Mn and Mo valence states were divalent and tetravalent,
respectively. The enhanced spontaneous magnetization was directed
in the in-plane direction, in contrast to that in the case of the
bulk. These results suggest that the film has a noncollinear spin
structure with tilted Mn2+ magnetic moments from the c-axis probably due to the tensile strain. We also performed
first-principles calculations and demonstrated that the direction
of the Mn2+ magnetic moment is sensitive to tensile strain.