The breaking of inversion
symmetry can enhance the multifunctional
properties of layered hybrid organic–inorganic perovskites.
However, the mechanisms by which inversion symmetry can be broken
are not well-understood. Here, we study a series of MnCl
4
-based 2D perovskites with arylamine cations, namely, (C
6
H
5
C
x
H
2
x
NH
3
)
2
MnCl
4
(
x
= 0, 1, 2, 3), for which the
x
= 0, 1,
and 3 members are reported for the first time. The compounds with
x
= 1, 2, and 3 adopt polar crystal structures to well above
room temperature. We argue that the inversion symmetry breaking in
these compounds is related to the rotational degree of freedom of
the organic cations, which determine the hydrogen bonding pattern
that links the organic and inorganic layers. We show that the tilting
of MnCl
6
octahedra is not the primary mechanism involved
in inversion symmetry breaking in these materials. All four compounds
show 2D Heisenberg antiferromagnetic behavior. A ferromagnetic component
develops in each case below the long-range magnetic ordering temperature
of ∼42–46 K due to spin canting.
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