标题： 从头计算的长寿命电子相干性 显示英文标题

标题： Long-Lived Electronic Coherences from First Principles

摘要： 电子相干性可以用于控制分子动力学，但这种控制受到由电子激发与分子振动之间耦合引起的超快退相干的限制。 以理解和控制分子中的电子相干性为目标，我们引入了一种从头算的方法，该方法能够直接模拟分子中电子相干性的产生和衰减。 对多光子激发噻吩后观察到的长寿命相干性的模拟显示，在密堆积的里德伯态能级结构中，由于其相对平行的势能面，实现了相干的电子运动。 显示英文摘要

摘要： Electronic coherences can be leveraged to control molecular dynamics, but such control is limited by ultrafast decoherence driven by coupling between electronic excitations and molecular vibrations. With the goal of understanding and controlling electronic coherence in molecules, we introduce a first-principles approach that enables direct simulation of the creation and decay of electronic coherences in molecules. Simulations of long-lived experimentally-observed coherences created upon multiphoton excitation of thiophene reveal coherent electronic motions within a dense manifold of Rydberg states, enabled by their relatively parallel potential energy surfaces.