Terahertz Birefringent Biomimetic Aerogels Based on Cellulose Nanofibers and Conductive Nanomaterials

Biomimetic, lamellar, and highly porous transition-metal carbide (MXene) embedded cellulose nanofiber (CNF) aerogels are assembled by a facile bidirectional freeze-drying approach. The biopolymer aerogels have large-scale, parallel-oriented micrometer-sized pores and show excellent mechanical strength and flexibility, tunable electrical properties, and low densities (2.7-20 mg/cm³). The CNF, MXene, and lamellar pores are efficiently utilized to endow the aerogels with exceptionally high birefringence in the terahertz (THz) regime. Birefringence values as high as 0.09-0.27 at 0.4 THz are achieved, which is comparable to most commercial THz birefringent materials such as liquid crystals, which suffer from fast disintegration, high cost, and complicated preparation processes. Empirical modeling for different MXene contents and an experimental comparison with silver nanowire or carbon nanotube embedded CNF aerogels suggest that the intrinsic conductivity and content of embedded nanomaterials, the aerogel porosity, and the lamellar cell walls can affect the optical properties such as the THz birefringence and absorption. The determination of optical anisotropy in the biopolymer aerogels lays a foundation for further exploration of ultralight, freestanding, and low-cost biomimetic porous architecture-based THz devices.