Abstract

The nonlinear photoacoustic response of indium phosphide nanocrystals on silicon nanotip arrays is investigated using time-resolved optical pump-probe spectroscopy and synchrotron-based X-ray diffraction. Femtosecond laser excitation triggers low-frequency and high-frequency radial breathing modes of the nanocrystals at 8 GHz and 10.3 GHz, respectively. At excitation fluences above 3 mJ/cm2, nonlinear frequency mixing occurs, including sum- and difference-frequency generation, indicative of strain-induced nonlinear elasticity. A higher-order extension of Hooke’s law models the fluence-dependent spectral response and yields a physically valid elastic energy potential. Ex-situ energy-dispersive X-ray spectroscopy reveals a correlation between nanocrystal oxidation and the emergence of nonlinear acoustic modes. Time-resolved X-ray diffraction confirms the nanocrystals as the origin of the low-frequency modes and supports the hypothesis of acoustic decoupling from the substrate.

Abstract

The nonlinear photoacoustic response of indium phosphide nanocrystals on silicon nanotip arrays is investigated using time-resolved optical pump-probe spectroscopy and synchrotron-based X-ray diffraction. Femtosecond laser excitation triggers low-frequency and high-frequency radial breathing modes of the nanocrystals at 8 GHz and 10.3 GHz, respectively. At excitation fluences above 3 mJ/cm2, nonlinear frequency mixing occurs, including sum- and difference-frequency generation, indicative of strain-induced nonlinear elasticity. A higher-order extension of Hooke’s law models the fluence-dependent spectral response and yields a physically valid elastic energy potential. Ex-situ energy-dispersive X-ray spectroscopy reveals a correlation between nanocrystal oxidation and the emergence of nonlinear acoustic modes. Time-resolved X-ray diffraction confirms the nanocrystals as the origin of the low-frequency modes and supports the hypothesis of acoustic decoupling from the substrate.

Abstract

The nonlinear photoacoustic response of indium phosphide nanocrystals on silicon nanotip arrays is investigated using time-resolved optical pump-probe spectroscopy and synchrotron-based X-ray diffraction. Femtosecond laser excitation triggers low-frequency and high-frequency radial breathing modes of the nanocrystals at 8 GHz and 10.3 GHz, respectively. At excitation fluences above 3 mJ/cm2, nonlinear frequency mixing occurs, including sum- and difference-frequency generation, indicative of strain-induced nonlinear elasticity. A higher-order extension of Hooke’s law models the fluence-dependent spectral response and yields a physically valid elastic energy potential. Ex-situ energy-dispersive X-ray spectroscopy reveals a correlation between nanocrystal oxidation and the emergence of nonlinear acoustic modes. Time-resolved X-ray diffraction confirms the nanocrystals as the origin of the low-frequency modes and supports the hypothesis of acoustic decoupling from the substrate.

Abstract

The nonlinear photoacoustic response of indium phosphide nanocrystals on silicon nanotip arrays is investigated using time-resolved optical pump-probe spectroscopy and synchrotron-based X-ray diffraction. Femtosecond laser excitation triggers low-frequency and high-frequency radial breathing modes of the nanocrystals at 8 GHz and 10.3 GHz, respectively. At excitation fluences above 3 mJ/cm2, nonlinear frequency mixing occurs, including sum- and difference-frequency generation, indicative of strain-induced nonlinear elasticity. A higher-order extension of Hooke’s law models the fluence-dependent spectral response and yields a physically valid elastic energy potential. Ex-situ energy-dispersive X-ray spectroscopy reveals a correlation between nanocrystal oxidation and the emergence of nonlinear acoustic modes. Time-resolved X-ray diffraction confirms the nanocrystals as the origin of the low-frequency modes and supports the hypothesis of acoustic decoupling from the substrate.