Wave Packets
Wave Packets
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波包
DOI：
10.1017/9781108584401.004
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发表时间：
2020
期刊：
影响因子：
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通讯作者：
R. Minns
中科院分区：
文献类型：
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作者：
R. Minns
提出了有助于理解分子里德伯波包动力学和控制的新实验和理论。通过实验证明了控制里德伯分子旋转量子态的直观方案。我们确定分子电子波包的各个分量之间的累积相位差，然后采用一系列锁相光脉冲来选择性地增强或减少特定的旋转状态。所产生的波包的角动量组成以及控制方案的效率是通过计算与时间相关的里德堡布居的多脉冲响应来确定的。使用光学拉姆齐方法观察预解离里德伯电子波包的动力学。时间分辨光谱是氢的，并且通过假设只有一个 p 里德伯级数对动力学有贡献，可以很好地建模。这与之前对自电离里德伯电子波包的观察形成鲜明对比，后者显示出与高于 Bom-Oppenheimer 极限的氢行为相当显着的偏差。这些偏差的根源在于电子相和分子相之间的相互作用。通过利用这些相，我们能够控制预解离与自电离的比率。对 NO 的里德堡态进行多通道量子缺陷理论分析。该分析考虑了所有具有 / < 3 的可访问系列以及所有记录的系列间相互作用。该分析是迄今为止对 NO 最完整的描述，将有助于设计未来的相干控制实验。本论文基于以下出版物：第3章分子里德伯波包旋转角动量的光学控制。 R.S.明斯，R.帕特尔，J.R.R.维莱和 H.H.菲尔丁。物理。莱特牧师。 91, 243601 (2003) 第4章自电离和预离解里德堡电子波包的观测与控制。 R.S.明斯，J.R.R. Verlet、L.J.沃特金斯和 H.H.菲尔丁。 J.化学。物理。 119 (12), 5842 (2003) 第 5 章 NO 分子的全局 MQDT 表示。 R.S.明斯，J.W.赫本、H.H.菲尔丁和 Ch.容根。 J.莫尔。规格正在准备其他出版物控制里德伯电子波包的角动量组成。 J.R.R.韦尔莱特，V.G.斯塔夫罗斯，R.S.明斯和 H.H.菲尔丁。物理。莱特牧师。 89（26），263004（2002）。使用锁相光脉冲控制 Xe 中里德伯波包的径向动力学。 J.R.R.韦尔莱特，V.G.斯塔夫罗斯，R.S.明斯和 H.H.菲尔丁。 J. Phys。蝙蝠。摩尔。选择。物理。 36（17），3683（2003）。 Na 中的干扰里德伯波包。关于。卡利，E.D.博利特，R.S. Minns、R. Patel 和 H.H. Fielding J. Phys。蝙蝠。摩尔。选择。物理。准备中
New experiments and theory contributing to the understanding of the dynamics and control of molecular Rydberg wave packets are presented. An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence of phase-locked optical pulses to selectively enhance or depopulate specific rotational states. The angular momentum composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multipulse response of the time dependent Rydberg populations. The dynamics of predissociating Rydberg electron wavepackets are observed using the optical Ramsey method. The time-resolved spectra are hydrogenic and are very well modeled by assuming that only one p Rydberg series contributes to the dynamics. This is in contrast with previous observations of autoionising Rydberg electron wave packets which show quite dramatic deviations from hydrogenic behaviour above the Bom-Oppenheimer limit. The origin of these deviations lies in the interplay between electronic and molecular phase. By exploiting these phases we are able to control the ratio of predissociaton to autoionisation A multichannel quantum defect theory analysis of the Rydberg state of NO is undertaken. The analysis takes into account all the accessible series with / < 3 and all documented interseries interactions. This analysis is the most complete description of NO to date and will aid in the design of future coherent control experiments. This thesis is based on the following publications Chapter 3 Optical control o f the rotational angular momentum o f a molecular Rydberg wave packet. R.S. Minns, R. Patel, J.R.R. Verlet and H.H. Fielding. Phys. Rev. Lett. 91, 243601 (2003) Chapter 4 Observation and control o f autoionising and predissociating Rydberg electron wave packets in NO. R.S. Minns, J.R.R. Verlet, L.J. Watkins and H.H. Fielding. J. Chem. Phys. 119 (12), 5842 (2003) Chapter 5 Global MQDT representation o f the NO molecule. R.S. Minns, J.W. Hepburn, H.H. Fielding and Ch. Jungen. J. Mol. Spec. In preparation Additional publications Controlling the angular momentum composition o f a Rydberg electron wave packet. J.R.R. Verlet, V.G. Stavros, R.S. Minns and H.H. Fielding. Phys. Rev. Lett. 89 (26), 263004 (2002). Controlling the radial dynamics o f Rydberg wave packets in Xe using phase-locked optical pulses. J.R.R. Verlet, V.G. Stavros, R.S. Minns and H.H. Fielding. J. Phys. B-At. Mol. Opt. Phys. 36 (17), 3683 (2003). Interfering Rydberg wave packets in Na. R.E. Carley, E.D. Boleat, R.S. Minns, R. Patel and H.H. Fielding J. Phys. B-At. Mol. Opt. Phys. In preparation