论文标题
通过非线性光谱揭示一个完整的量子梯子
Revealing a full quantum ladder by nonlinear spectroscopy
论文作者
论文摘要
IR或可见区域中的相干二维光谱对于研究相关性,能量弛豫/转移途径非常有效,在复杂的多人团或多模式系统中。但是,通常仅限于两Quanta激发及其特性。在本文中,提出了任意水平的激发水平,即扫描量子系统的非线性潜在表面的实用性,直至所需的激发程度。这可以通过简单的三脉冲激光光谱法实现。可以直接获得对高级非谐度和过渡幅度的准确评估。此外,可以通过研究绝对峰位置来解决有关探测系统量子性质的问题。
Coherent two-dimensional spectroscopy in IR or visible region is very effective for studying correlations, energy relaxation/transfer pathways in complex multi-chromophore or multi-mode systems. However it is usually restricted up to two-quanta excitations and their properties. In this paper an arbitrary level of excitation is suggested as the utility to scan nonlinear potential surfaces of quantum systems up to a desired excitation degree. This can be achieved by a simple three-pulse laser spectroscopy approach. Accurate evaluation of high-level anharmonicities as well as transition amplitudes can be directly obtained. Additionally, questions regarding the quantum nature of the probed system can be addressed by studying absolute peak positions.