A new hybrid molecular-based ferromagnet of formula [(dmaph)PPh
3][MnCr(ox)
3], where[(dmaph)PPh
3]
+ stands for the (4-dimethylaminophenyl)triphenylphosphonium cation (ox
2-being the oxalate anion), has been synthesized. It crystallizes in the monoclinic
P2
1 spacegroup, with lattice parameters
a = 13.954(2) Å,
b = 16.297(2) Å,
c = 14.323(2) Å, and
![](/images/gifchars/beta2.gif)
=99.27(1)
![](/images/entities/deg.gif)
. Refinement based on
Fo2 yields
R = 0.072 and wR
2 = 0.156. The compound exhibitsa ferromagnetic interaction between Cr
3+ and Mn
2+, with a long-range magnetic orderingat
TC = 4.5 K. The hyperpolarizability (
![](/images/gifchars/beta2.gif)
) of the cation is calculated within the frameworkof the INDO/SOS-based method, which indicates a
![](/images/gifchars/beta2.gif)
value comparable to that of
p-nitroaniline for an absorption maximum at 306 nm (
max = 28 500 M
-1 cm
-1). This result isconsistent with the observation of a SHG efficiency 4 times that of urea for the parent[(dmaph)PPh
3]Br salt, at 1.907
![](/images/entities/mgr.gif)
m. The non-centrosymmetric [(dmaph)PPh
3][Mn
IICr
III(ox)
3]derivative is used as a model compound for an investigation of the potential effect of aferromagnetic ordering on the bulk NLO response of hybrid materials made of NLO cationsinserted between magnetic anionic layers.