Phase control of wavepacket dynamics using shaped femtosecond pulses
| Autor: | Radoslaw Uberna, Richard A. Loomis, Stephen R. Leone, Zohar Amitay |
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| Rok vydání: | 1999 |
| Předmět: | |
| Zdroj: | Faraday Discussions. 113:385-400 |
| ISSN: | 1364-5498 1359-6640 |
| Popis: | Coherent vibrational and rotational dynamics of the Li2 molecule is controlled by varying the relative phases, φn, of the rovibrational wavepacket components, ∣n〉 e-i(ωnt+φn). The coherent superposition is created by excitation of a set of ten rovibronic E 1Σg+(νE=12–16, JE=17, 19) states from an intermediate state, A 1Σu+(νA=14, JA=18), using ultrashort optical pulses with well defined spectral amplitudes and phases encoded into the pulse by a liquid crystal spatial light modulator. The wavepacket is probed by time-dependent photoionization and the quantum interference signal is measured as a total ionization yield. The phases of the wavepacket components are optimized to produce partial localization of the wavepacket at a given time t, in specific regions of three-dimensional space defined by the radial and angular coordinates. As a result, the ionization yield, I(t), is maximized or minimized at a time t. The degree of control achieved in the experiment (Imax-Imin)/Imax=64(±12%). The experimental data are interpreted in terms of time-dependent radial and angular probability distributions, calculated for different initial conditions that are determined by the phase relationships in the excitation pulse. |
| Databáze: | OpenAIRE |
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