Abstract
We perform first-principles calculations of the photoexcitation dynamics of an acetylene molecule in a metal organic framework, IRMOF-10. Resonant laser excitation of the IRMOF-10 generates an optical near field (ONF) around the two benzene rings that comprise the main framework of the IRMOF-10. Interestingly, along with the ONF of frequency ω, which synchronizes with the resonant frequency of the IRMOF-10, a second harmonic (=2ω) component of the ONF is generated. The second harmonic component effectively excites the acetylene molecule at a frequency of 2ω, although the incident laser field is in tune with ω. It is noteworthy that the second harmonic excitation is caused by spatial nonuniformity of the ONF interaction. It is completely different from the conventional two-photon excitation and is much more efficient than the two-photon excitation by several orders of magnitude.
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