论文标题
通过超快等离子体衰减启用的分子光解离
Molecular photodissociation enabled by ultrafast plasmon decay
论文作者
论文摘要
我们提出了一种通过耦合到纳米颗粒等离子体的策略来实现正常光稳定分子的光解离。单分子水平上的大型耦合结合了等离激元模式的高度有损性质，其寿命在飞秒的阶段，为分子开放了一个超快衰变通道。对于分子垂直光激发能的等离子模式频率，激发能和发射能之间的差异在分子基态在拉曼样过程中转化为振动能。在正确的条件下，这种能量可以足够高，以在电子基态上实现有效的光解离。我们使用铝纳米颗粒附近的氢分子的Lindblad Master方程的数值模拟演示了该概念，并探索了与各种系统参数的函数探索光解异位效率。
We propose a strategy for enabling photodissociation of a normally photostable molecule through coupling to a nanoparticle plasmon. The large possible coupling on the single-molecule level combined with the highly lossy nature of plasmonic modes, with lifetimes on the order of femtoseconds, opens an ultrafast decay channel for the molecule. For plasmon mode frequencies below the vertical photoexcitation energy of the molecule, the difference between excitation and emission energy is converted into vibrational energy on the molecular ground state in a Raman-like process. Under the correct conditions, this energy can be high enough to enable efficient photodissociation on the electronic ground state. We demonstrate the concept using numerical simulations of the Lindblad master equation for the hydrogen molecule in the vicinity of an aluminum nanoparticle, and explore the photodissociation efficiency as a function of various system parameters.
