Phonon-Dressed Third-Harmonic Generation in Diamond

Kavli Affiliate: Jeffrey Moses

| First 5 Authors: Jiaoyang Zheng, Guru Khalsa, Jeffrey Moses, ,

| Summary:

We demonstrate a strong, elastic, frequency-upshifting optical polarizability
that accompanies sum-frequency driving of Raman phonons and two-photon
absorption, extending the duality of structural and optical property
modification recently observed in light-driven phononics. The effect,
phonon-dressed third-harmonic generation (THG), is a degenerate low-frequency
analog of coherent anti-Stokes Raman scattering. In diamond, it has a cubic
electric susceptibility at least 58 times larger than purely electronic THG,
with polarization and frequency dependence reflecting strong coupling to Raman
phonon degrees of freedom.

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