We
report magnetic birefringence measurements up to high fields
(17.5 T) of dilute aqueous suspensions of rod-like cellulose nanocrystals
with well characterized distributions of lengths, widths and thicknesses.
We compare these data with three models, one with colinear (1), one
with perpendicular cylindrically symmetric tensors for diamagnetic
susceptibility and refractive index (2) and one with biaxial diamagnetic
anisotropy (3). We find that taking into account polydispersities
of length, width, and thickness is essential for accurate fitting
and that model 1 is the most appropriate, presumably because of the
twisting of the suspended nanocrystal along their long axis. The best-fitted
susceptibility anisotropy was Δχ
z(xy) = χ
zz
–(χ
xx
+χ
yy
)/2 = −2.44 × 10–6 when considering only the crystalline core of nanocrystals and,
more appropriately, Δχ
z(xy) = −0.95 × 10–6 when including crystalline core and skin. The latter value is slightly
higher than Δχ
z(xy) = −0.68(5) × 10–6 deduced from estimations using Pascal’s additivity law. The
specific birefringence of the nanocrystals in water was found to be δn
0 = +0.120(2), which is well accounted
for by the intrinsic birefringence of crystalline cellulose (δn
0
intr = n
∥–n
⊥ = +0.0744) and the birefringence arising
from the slender shape of nanocrystals.