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CaOFeS is a semiconducting oxysulfide with polar layered triangularstructure. Here a comprehensive theoretical study has been performed to revealits physical properties, including magnetism, electronic structure, phasetransition, magnetodielectric effect, as well as optical absorption. Ourcalculations confirm the Ising-like G-type antiferromagnetic ground statedriven by the next-nearest neighbor exchanges, which breaks the trigonalsymmetry and is responsible for the magnetodielectric effect driven by exchangestriction. In addition, a large coefficient of visible light absorption ispredicted, which leads to promising photovoltaic effect with the maximumlight-to-electricity energy conversion efficiency up to 24.2%.

Exchange striction driven magnetodielectric effect and potential photovoltaic effect in polar CaOFeS