Ab Initio Investigation of Nonlinear Mode Coupling in C60,The Journal of Physical Chemistry Letters

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Ab Initio Investigation of Nonlinear Mode Coupling in C60
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-11-01 00:00:00 , DOI: 10.1021/acs.jpclett.7b02573
Antonia Karamatskou _{1,

2} , Robin Santra _{1,

2,

3} , Oriol Vendrell ₄

Affiliation

Strong light fields may be used to control molecular structure, thus providing a route to new, light-induced phases of matter. In this context, we present an ab initio molecular dynamics investigation of nonlinear mode coupling in C₆₀ and show that, under suitable conditions, resonant infrared excitation induces significant structural changes in the system. Surprisingly, exciting the highest-frequency infrared mode at field strengths employed in a recent experiment [Nature 2016, 530, 461–464], we observe no significant structural change. However, when targeting the first two infrared modes using stronger fields, all Raman modes gain energy through nonlinear coupling to the infrared modes, leading to large-amplitude vibrational excitations. We find a strong response of the H_g(5) mode, which is symmetric with respect to the equilibrium structure. For sufficiently strong field, it is of the same order as the infrared modes’ excitation. This encourages further investigations into the light-induced superconducting properties of alkali-doped fullerenes.

中文翻译：

C ₆₀中非线性模式耦合的从头算研究

强光场可用于控制分子结构，从而提供通往新的光诱导物质相的途径。在这种情况下，我们对C _60中的非线性模式耦合进行从头算分子动力学研究，结果表明，在合适的条件下，共振红外激发会在系统中引起明显的结构变化。令人惊讶地，令人兴奋的最高频率在最近的试验[使用的场强红外模式自然 2016，530（461-464），我们没有观察到明显的结构变化。但是，当使用更强的场作为前两个红外模式的目标时，所有拉曼模式都会通过与红外模式的非线性耦合来获取能量，从而导致大振幅的振动激发。我们发现H _g（5）模式具有很强的响应性，它相对于平衡结构是对称的。对于足够强的场，它与红外模式的激发具有相同的数量级。这鼓励了对掺杂碱的富勒烯的光诱导超导性质的进一步研究。

更新日期：2017-11-02

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