Polydimethylsiloxane (PDMS) is a prominent material for radiative cooling due to its promising optical properties in the mid-infrared spectral region as well as its fabrication easiness. Even though several works have reported that the mid-infrared emissivity of a PDMS film can be increased by surface modification, there is still room for further enhancement through global optimization. Here, we designed and fabricated the thin PDMS film patterned with two-dimensional gratings to obtain the highest emissivity in the wavelength range from 8 to 13 μm. A surrogate-model-based optimization was performed, and the optimum structure exhibited the averaged emissivity value of 0.99 in the wavelength of 8–13 μm, which is the highest value reported to date among polymer-based radiative coolers. For real-world applications, we also developed the fabrication method that is repeatable and applicable for various surfaces using a flexible master mold.

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