A dielectric medium containing noncentrosymmetric
domains can exhibit
piezoelectric and second-harmonic generation (SHG) responses when
an electric field is applied. Since many crystalline biopolymers have
noncentrosymmetric structures, there has been a great deal of interest
in exploiting their piezoelectric and SHG responses for electromechanical
and electro-optic devices, especially owing to their advantages such
as biocompatibility and low density. However, exact mechanisms or
origins of such polarization responses of crystalline biopolymers
remain elusive due to the convolution of responses from multiple domains
with varying degrees of structural disorder or difficulty of ensuring
the unidirectional alignment of noncentrosymmetric domains. In this
study, we investigate the polarization responses of a noncentrosymmetric
crystalline biopolymer, namely, unidirectionally aligned β-chitin
crystals interspersed in the amorphous protein matrix, which can be
obtained naturally from tubeworm Lamellibrachia satsuma (LS) tube. The mechanisms governing polarization responses in different
dynamic regimes covering optical (>1013 Hz), acoustic/ultrasonic
(103–105 Hz), and low (10–2–102 Hz) frequencies are explained. Relationships
between the polarization responses dominant in different frequencies
are addressed. Also, electromechanical coupling responses, including
piezoelectricity of the LS tube, are quantitatively discussed. The
findings of this study can be applicable to other noncentrosymmetric
crystalline biopolymers, elucidating their polarization responses.