  Efficient optical pumping is an important tool for state initialization in
quantum technologies, such as optical quantum memories. In crystals doped with
Kramers rare-earth ions, such as erbium and neodymium, efficient optical
pumping is challenging due to the relatively short population lifetimes of the
electronic Zeeman levels, of the order of 100 ms at around 4 K. In this article
we show that optical pumping of the hyperfine levels in isotopically enriched
$^{145}$Nd$^{3+}$:Y$_2$SiO$_5$ crystals is more efficient, owing to the longer
population relaxation times of hyperfine levels. By optically cycling the
population many times through the excited state a nuclear-spin flip can be
forced in the ground-state hyperfine manifold, in which case the population is
trapped for several seconds before relaxing back to the pumped hyperfine level.
To demonstrate the effectiveness of this approach in applications we perform an
atomic frequency comb memory experiment with 33% storage efficiency in
$^{145}$Nd$^{3+}$:Y$_2$SiO$_5$, which is on a par with results obtained in
non-Kramers ions, e.g. europium and praseodymium, where optical pumping is
generally efficient due to the quenched electronic spin. Efficient optical
pumping in neodymium-doped crystals is also of interest for spectral filtering
in biomedical imaging, as neodymium has an absorption wavelength compatible
with tissue imaging. In addition to these applications, our study is of
interest for understanding spin dynamics in Kramers ions with nuclear spin.
