Second Harmonic Excitation of Acetylene by the Optical Near Field Generated in a Porous Material
Second Harmonic Excitation of Acetylene by the Optical Near Field Generated in a Porous Material
复制标题
多孔材料中产生的光学近场对乙炔的二次谐波激发
DOI：
10.1021/acs.jpcc.7b02744
复制
发表时间：
2017
期刊：
影响因子：
3.7
通讯作者：
Nobusada Katsuyuki
中科院分区：
文献类型：
--
作者：
Noda Masashi;Yamaguchi Maiku;Nobusada Katsuyuki
我们进行第一性原理计算的乙炔分子在金属有机框架，IRMOF-10的光激发动力学。IRMOF-10的共振激光激发在两个苯环周围产生光学近场（ONF），所述两个苯环构成IRMOF-10的主框架。有趣的是，沿着与IRMOF-10的谐振频率相同的频率ω的ONF，产生ONF的二次谐波（=2ω）分量。尽管入射激光场与ω调谐，但二次谐波分量以2ω的频率有效地激发乙炔分子。值得注意的是，二次谐波激发是由ONF相互作用的空间非均匀性引起的。它完全不同于传统的双光子激发，比双光子激发的效率高出几个数量级。
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.