Radiative cooling materials have gained prominence as a zero-energy solution for mitigating global warming.However,a comprehensive understanding of the atomic-scale optical properties and macroscopic optical performan...Radiative cooling materials have gained prominence as a zero-energy solution for mitigating global warming.However,a comprehensive understanding of the atomic-scale optical properties and macroscopic optical performance of radiative cooling materials remains elusive,limiting insight into the underlying physics of their optical response and cooling efficacy.La_(2)O_(3)and HfO_(2),which represent rare earth and third/fourth subgroup inorganic oxides,respectively,show promise for radiative cooling applications.In this study,we used multiscale simulations to investigate the optical properties of La_(2)O_(3)and HfO_(2)across a broad spectrum.First-principles calculations revealed their dielectric functions and intrinsic refractive indices,and the results indicated that the slightly smaller bandgap of La_(2)O_(3)compared to HfO_(2)induces a higher refractive index in the solar band.Additionally,three-phonon scattering was found to provide more accurate infrared optical properties than two-phonon scattering,which enhanced the emissivity in the sky window.Monte Carlo simulations were also used to determine the macroscopic optical properties of La_(2)O_(3)and HfO_(2)coatings.Based on the simulated results,we identified that the particle size and particle volume fraction play a dominant role in the optical properties.Our findings underscore the potential of La_(2)O_(3)and HfO_(2)nanocomposites for environment-friendly cooling and offer a new approach for high-throughput screening of optical materials through multiscale simulations.展开更多
基金the National Natural Science Foundation of China(Grant Nos.U23A20565,52301194,and 52101178)the Shanghai Science and Technology Commission(Grant No.22511100400)+1 种基金the startup funding from Shanghai Jiao Tong University(Grant No.WH220405009)Innovation Program of Shanghai Municipal Education Commission(Grant No.2023ZKZD15)for providing funding support for this research。
文摘Radiative cooling materials have gained prominence as a zero-energy solution for mitigating global warming.However,a comprehensive understanding of the atomic-scale optical properties and macroscopic optical performance of radiative cooling materials remains elusive,limiting insight into the underlying physics of their optical response and cooling efficacy.La_(2)O_(3)and HfO_(2),which represent rare earth and third/fourth subgroup inorganic oxides,respectively,show promise for radiative cooling applications.In this study,we used multiscale simulations to investigate the optical properties of La_(2)O_(3)and HfO_(2)across a broad spectrum.First-principles calculations revealed their dielectric functions and intrinsic refractive indices,and the results indicated that the slightly smaller bandgap of La_(2)O_(3)compared to HfO_(2)induces a higher refractive index in the solar band.Additionally,three-phonon scattering was found to provide more accurate infrared optical properties than two-phonon scattering,which enhanced the emissivity in the sky window.Monte Carlo simulations were also used to determine the macroscopic optical properties of La_(2)O_(3)and HfO_(2)coatings.Based on the simulated results,we identified that the particle size and particle volume fraction play a dominant role in the optical properties.Our findings underscore the potential of La_(2)O_(3)and HfO_(2)nanocomposites for environment-friendly cooling and offer a new approach for high-throughput screening of optical materials through multiscale simulations.