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[Display omitted] • Jahn–Teller effects increase charge carriers and boosts photon harvesting. • Strong absorption over full sun light for (Mn 2 O 3) 3 CuSiO 3 with Jahn–Teller defects. • Direct light absorption and heat storage of Cu-braunite–coated Mg(OH) 2. • Photo-dehydration conversion of Cu-braunite–Mg(OH)2 increases by 10 fold.. To improve photon harvesting, we demonstrated that Jahn–Teller defects can efficiently reduce the band gap and increase the carrier density, which significantly intensify light harvesting and widen the absorption band. This may be an effective method for designing solar materials. The substitution of Mn2+ with Jahn–Teller active Cu2+ leads to quasi-metallic (Mn 2 O 3) 3 CuSiO 3 nanoparticles with a high concentration of charge carriers, displaying intense absorption in entire solar spectrum. Silicates may represent a new type of photon harvesting material. Mg(OH) 2 powder coated by Cu-braunite shows a 150 % increase in photothermal temperature, a tenfold improvement in photothermal-dehydration conversion and a 15.8-fold increase in the reversibility of 30 cycles of heat storage and release. This material may be practicable for directly harvesting solar energy and storing thermoenergy. Jahn–Teller effects are effective for tuning photon harvesting. [ABSTRACT FROM AUTHOR]

[Display omitted] • A redox system has high density of delocalized charge carrier. • Metal-like CeO 2 –Co 3 O 4 absorbs light strongly in full solar spectrum. • CeO 2 –Co 3 O 4 can catalyze Ca(OH) 2 dehydration. • Ca(OH) 2 –CeO 2 –Co 3 O 4 composite can efficiently absorb sun light. • Ca(OH) 2 –CeO 2 –Co 3 O 4 is promising for direct photothermal storage. Thermal energy storage technology is an effective means for expanding the use of solar energy. Light harvesting across the full solar wavelength is essential for ensuring photothermal efficiency. Lattice defect engineering has been widely used to narrow the band gap and induce surface plasmon resonance absorption. In this study, we present an alternate method for intensifying light absorption. The CeO 2 –Co 3 O 4 redox system possesses highly delocalised electrons and numerous oxygen vacancies, allowing considerable light harvesting over the full solar spectrum. By incorporating CeO 2 –Co 3 O 4 as an absorber, the photothermal temperature, photothermal dehydration conversion and reversibility of the thermal storage and release cycles of Ca(OH) 2 can be drastically enhanced. The dehydration kinetics of Ca(OH) 2 are also substantially increased by reducing the dehydration activation energy using CeO 2 –Co 3 O 4. The Ca(OH) 2 –CeO 2 –Co 3 O 4 composite is a promising candidate for one-step photothermal conversion and thermal energy storage. Herein, we develop a light–material design for the very first time using a redox system. [ABSTRACT FROM AUTHOR]