Mechanisms of Electronic - Nuclear Energy Exchange in Molecular Rydberg States: A Time-Domain Study Focussed by Frequency-Domain Ideas

麻省理工学院的罗伯特·菲尔德教授在实验物理化学计划的支持下，对分子里德堡态中的能量转移动力学进行了一项新的研究。一个纳秒脉冲将被用来准备一个精心设计的初始态，一对扫描延迟相位相干红外飞秒脉冲将被用来研究初始局域激发的动力学。具体地说，第一脉冲用于在一组明确定义的里德堡状态之间准备相干叠加，而第二脉冲询问递归或重新相移。探测将通过场电离电压斜坡进行。我们将研究电子和核能流动的机制细节，改变相互作用状态之间的共振程度。在分子束中制备的碱土一卤化物，如CaF、CaCl和BaF，以前由PI在频域中研究，将被用作模型体系。里德堡态的研究加深了我们对小分子中能量流动和存储的理解。随着方法的改进，它可能会应用于越来越复杂的分子，对光化学和量子信息存储等领域有潜在的影响。

Professor Robert Field of MIT is supported by the Experimental Physical Chemistry Program for a novel study of the dynamics of energy transfer in molecular Rydberg states. A nanosecond pulse will be used to prepare a carefully designed initial state, and a pair of scanned-delay phase-coherent IR femtosecond pulses will be used to study the dynamics of the initially localized excitation. In particular, the first pulse is used to prepare a coherent superposition among a well defined set of Rydberg states, and the second pulse interrogates the recurrences or rephasing. Detection will be by a field ionization voltage ramp. The mechanistic details of electronic and nuclear energy flow will be studied, varying the extent of resonance between interacting states. Alkaline earth monohalides such as CaF, CaCl and BaF prepared in molecular beams, previously studied by the PI in the frequency domain, will be utilized as model systems. The study of Rydberg states enhances our understanding of energy flow and storage in small molecules. As the method is improved, it may be applied to increasingly complicated molecules, with potential impacts on fields such as photochemistry and quantum information storage.