Submillimeter-Wave Permittivity Measurements of Bound Water in Collagen Hydrogels via Frequency Domain Spectroscopy

This article presents measurements of the permittivity of gelatin hydrogels between 220 and 330 GHz. Hydrated gelatin was treated as a binary mixture of free water and a compound consisting of water bound to collagen. Submillimeter-wave reflectometry was used to estimate the hydrated gelatin permittivity, hydrated gelatin density, and free-water volume fraction in phantoms composed of 62, 67, 72, and 77% water by weight. A hydrated dry/wet density ratio of 0.335 was validated with optical-coherence tomography. A constant nonfreezing bound-water mass of 0.6 g/g was observed and confirmed with differential-scanning calorimetry. Good agreement between results from different modalities supports the dielectric spectroscopy methods and data analysis. Depending on the hydrodynamics at the sample/air interface, measurements indicate a bound-water compound permittivity of 3.77-j2.52 to 3.95-j2.49-contrasting the pure-water average permittivity of 5.16-j5.63. The loss related to bound water was much higher than anticipated and characterization will help reduce uncertainty in measurements of gelatin hydrogel-based tissue phantoms; particularly corneal phantoms where adjacent free water creates complex hydration gradients. This is the first known, submillimeter-wave, frequency domain measurement of complex permittivity of the bound-water component in solid, proteinaceous matter.