论文标题

探索与被困Rydberg离子的圆锥交叉点附近的多体动力学

Exploring the many-body dynamics near a conical intersection with trapped Rydberg ions

论文作者

Gambetta, Filippo Maria, Zhang, Chi, Hennrich, Markus, Lesanovsky, Igor, Li, Weibin

论文摘要

电子势能表面之间的圆锥形相交是研究大分子激发态中非绝热过程的范式。但是,由于相应的动力学发生在飞秒时间尺度上,因此他们的研究仍然具有挑战性,需要超快光谱技术。我们证明,被困的rydberg离子是设计圆锥形交集的平台,并分别在纳米和微秒的较大长度和时间尺度上模拟其随之而来的动态。所有这些都在高度可控的系统中。在这里,由于高极化性与Rydberg离子的强极化性与强极度互换相互作用之间的相互作用,势能表面的形状和圆锥交叉的位置可以调节。我们研究圆锥形交集的存在如何影响核和电子动力学,特别是表明它如何导致核运动的抑制。这些效果可以通过直接的光谱测量在最先进的实验设置中实时监测。

Conical intersections between electronic potential energy surfaces are paradigmatic for the study of non-adiabatic processes in the excited states of large molecules. However, since the corresponding dynamics occurs on a femtosecond timescale, their investigation remains challenging and requires ultrafast spectroscopy techniques. We demonstrate that trapped Rydberg ions are a platform to engineer conical intersections and to simulate their ensuing dynamics on larger length and time scales of the order of nanometers and microseconds, respectively; all this in a highly controllable system. Here, the shape of the potential energy surfaces and the position of the conical intersection can be tuned thanks to the interplay between the high polarizability and the strong dipolar exchange interactions of Rydberg ions. We study how the presence of a conical intersection affects both the nuclear and electronic dynamics demonstrating, in particular, how it results in the inhibition of the nuclear motion. These effects can be monitored in real-time via a direct spectroscopic measurement of the electronic populations in a state-of-the-art experimental setup.

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