Soft Mesocrystal Enabled Multi‐Degree Light Modulation

Abstract Mesocrystals introduce high‐level orders, such as chirality, topology, and hierarchy to the crystallography, and thus bring collective and emergent properties beyond traditional crystals. Orthogonally modulating the multiple degrees of light is highly pursued to fully explore the intrinsic multidimensional and large‐scale parallel processing capability of photon informatics. Unfortunately, it is unachievable with traditional light–matter interaction systems. Here, the multi‐degree light modulation is realized based on the hierarchical architecture of a soft mesocrystal. High‐quality monodomains of both blue phase I and blue phase II are formed via regulating the assembly of liquid crystals by photoalignment anchoring and electricity. The mapping relationship between optical freedoms (the spin, wavelength, and geometric phase of light) and hierarchical structures (the chirality of helix, lattice constant, and the azimuthal orientation of cubic lattices) is established. Omnidirectional spatial phase modulation with spin and full color selectivity is demonstrated. Based on the multi‐degree light modulation, 3D and wavelength‐selective orbital angular momentum generation as well as multichannel color holographic display are presented. This work extends the fundamental understanding of blue phase mesocrystals and provides a promising strategy for large‐scale parallel and multi‐degree light modulation that may be utilized in vital fields, such as supercomputing, optical communications, and virtual/augmented realities.