  The dipole moment is a crucial molecular property linked to a molecular
system's bond polarity and overall electronic structure. To that end, the
electronic dipole moment, which results from the electron density of a system,
is often used to assess the accuracy and reliability of new electronic
structure methods. This work analyses electronic dipole moments computed with
the pair coupled cluster doubles (pCCD) ansatz and its linearized coupled
cluster (pCCD-LCC) corrections using the canonical Hartree--Fock and
pCCD-optimized (localized) orbital bases. The accuracy of pCCD-based dipole
moments is assessed against experimental and CCSD(T) reference values using
relaxed and unrelaxed density matrices and different basis set sizes. Our test
set comprises molecules of various bonding patterns and electronic structures,
exposing pCCD-based methods to a wide range of electron correlation effects.
Additionally, we investigate the performance of pCCD-in-DFT dipole moments of
some model complexes. Finally, our work indicates the importance of orbital
relaxation in the pCCD model and shows the limitations of the linearized couple
cluster corrections in predicting electronic dipole moments of multiple-bonded
systems. Most importantly, pCCD with a linearized CCD correction can reproduce
the dipole moment surfaces in singly-bonded molecules, which are comparable to
the multi-reference ones.
