13C-NMR study of the phase transition in the layered antiferroelectric squaric acid

The temperature dependence of the¹³C-NMR spectra of undoped crystals of the layered antiferroelectric squaric acid (C₄H₂O₄; H₂SQ was measured at a resonance frequency of about 75 MHz by means of the¹H–¹³C double resonance technique. The relation between the order parameter and the chemical shift tensors at the¹³C nuclei is discussed in detail. The line splitting in the ordered phase belowT _c100°C is shown to be proportional to the order parameter. The phase transition is of first order and can be well described by a Landau expansion of the free energy. The results are compared to previous determinations of the temperature dependence of the order parameter. The spin lattice relaxation time of the¹³C system is estimated to be 5000–7500 s at 5°C and the given magnetic field.