Design of Bioinspired Ordered Materials for Spectral Modulation

Conspectus Spectral modulation, the precise control over light reflection, transmission, absorption, and scattering, has become a transformative approach in areas such as smart windows, adaptive camouflage, radiative cooling, anticounterfeiting, and photovoltaics. Typical strategies primarily rely on tuning the intrinsic properties of electrochromic, thermochromic, or photochromic materials. Yet, these material-driven approaches still suffer from limited color purity, narrow tunability, slow response, and poor multifunction integration. An emerging alternative is to treat structural order as an independent physical design dimension. By organizing nanoscale building blocks into periodic, hierarchical, or reconfigurable architectures, one can manipulate light through Bragg diffraction, Mie scattering, plasmonic resonance, and graded-index effects. These mechanisms are difficult to access by chemical composition alone. Nature provides a rich library of such ordered designs. Photonic crystals, multilayers, porous networks, and graded-index arrays in organisms achieve efficient reflection, absorption, and transmission under ambient conditions. These biological systems show that precise control over orientation, periodicity, layer spacing, and refractive-index contrast can produce optical functions far beyond those of homogeneous materials. Translating these biological blueprints into synthetic stimuli-responsive systems offers a route from static structural control to dynamic and intelligent spectral regulation. In this Account, we describe our efforts along a three-stage trajectory. First, we show that ordered assembly of nanomaterials significantly improves the conductivity-transmittance trade-off, switching kinetics, and cycling stability of electrochromic materials, illustrating the performance gain achievable by moving from disorder to order. Second, by replicating natural static designs such as silver ant hairs for radiative cooling, butterfly scale porous networks for absorption, and moth-eye graded-index arrays for antireflection, performance levels that are difficult to achieve with conventional materials are reached. Third, inspired by cephalopods, chameleons, and other organisms, dynamic systems with mechanochromic, electrochromic, and thermochromic responses are designed for smart windows, pressure visualization, and fire warning. The progression from ordered assembly to static bioinspiration and then to dynamic intelligence reveals that order is not merely a passive geometrical feature. It is a functional variable that can be programmed across length scales. It allows conflicting optical requirements, such as high transparency and high conductivity, strong reflection and low haze, or visible and near-infrared (NIR) modulation, to be balanced through structural rather than compositional design. We also discuss unresolved challenges, including angular dependence, haze, actuation requirements, long-term environmental durability, and scalable fabrication. Throughout, we emphasize a unifying principle that structural order itself is an active, designable, and dynamically tunable parameter for spectral control. We close with perspectives on AI-assisted inverse design, cross-scale order integration, and multifunctional smart systems.