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- W2022553993 abstract "Non-linear-optical properties in ${mathrm{C}}_{60}$ have attracted enormous attention for over two decades. The endohedral complex $mathrm{N}@{mathrm{C}}_{60}$, with its remarkable thermal stability and spin-quartet ground state, is a candidate for future room-temperature quantum computing, but there has been no investigation of its non-linear-optical properties. Here, a first-principles calculation shows that $mathrm{N}@{mathrm{C}}_{60}$ is a promising material for nanoscale and ultrafast modulations. Excitation by a pump laser pulse of the nitrogen-atom vibration inside the ${mathrm{C}}_{60}$ cage transiently breaks inversion symmetry and can enable second-harmonic generation (SHG) from a probe pulse. Unlike the SHG observed in ${mathrm{C}}_{60}$ thin films, this harmonic signal is switched on and off periodically every 345 fs. For an fcc crystal of $mathrm{N}@{mathrm{C}}_{60}$, the second-order susceptibility ${ensuremath{chi}}^{(2)}$ is on the order of ${10}^{ensuremath{-}8}phantom{rule{0.28em}{0ex}}mathrm{esu}$, similar to commercially used nonlinear materials." @default.
- W2022553993 created "2016-06-24" @default.
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- W2022553993 date "2011-08-19" @default.
- W2022553993 modified "2023-10-16" @default.
- W2022553993 title "First-principles prediction of optical second-order harmonic generation in the endohedralN@C60compound" @default.
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- W2022553993 doi "https://doi.org/10.1103/physreva.84.023837" @default.
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