Time-resolved configuration interaction

Schumacher, Douglass; Duncan, D. I.; Jones, Robert R.; Gallagher, T. F.

doi:10.1088/0953-4075/29/11/002

Cited by 26 publications

(12 citation statements)

References 13 publications

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“…Unfortunately, further progress with this detection technique was hampered by the rather low signal intensities obtained due to the relatively small probability of photoionizing high Rydberg states (approximately 10 −4 ). To overcome this problem a more efficient experimental approach, based on the observation of Ramsey interference fringes, was proposed by Noordam et al (1992) and subsequently exploited widely (see, for example, Broers et al 1993;Christian et al 1993;Jones et al 1993;Wals et al 1994;Fielding et al 1995;Noel & Stroud 1995;Schumacher et al 1996). In these experiments, the return of an electron wavepacket to its initial state, at time t = 0, after a time t = τ (i.e.…”

Section: Detection Of Rydberg Electron Wavepacketsmentioning

confidence: 99%

“…to observe a time-resolved configuration interaction. In an interesting experiment, Schumacher et al (1996) created a radial wavepacket in atomic Ba in the presence of a degenerate doubly excited Rydberg state and observed a temporal oscillation between configurations. Other recent Rydberg electron wavepacket experiments have involved exciting superpositions of several angular momentum states to create electron wavepackets that evolve in the angular coordinates.…”

Section: Introductionmentioning

confidence: 99%

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Rydberg electron wavepacket dymanics in atoms and molecules

Ramswell

Stavros

Hong

et al. 1998

Philosophical Transactions of the Royal Society of London. Seri

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The generation and detection of Rydberg electron wavepackets using picosecond lasers is discussed with reference to the observation of the dynamics of spin-orbit autoionization in Xe. A multiphoton (nanosecond + picosecond) excitation scheme is employed with two-photon phase-sensitive detection, based on the observation of Ramsey interference fringes. To complement the experiment, time-dependent multichannel quantum-defect theory (TD-MQDT) calculations have been developed to investigate the dynamics of a spin-orbit autoionizing Rydberg wavepacket in Ar. The time-dependent partial photoionization cross-sections reveal interesting interference patterns in the recurrence spectra which are accounted for in terms of the quantum defects of the autoionizing channels. Finally, the rovibrational and rotational autoionization dynamics of a Rydberg wavepacket in H 2 are investigated using TD-MQDT. It is demonstrated that, in the time-domain, the configuration interaction between rotational channels can be described quantitatively in terms of an interaction time. In contrast to the rovibrational autoionization lifetime, which is determined by the classical orbit period (∝ n 3 ), the rotational autoionization lifetime is determined by the kinetic energy of the electron wavepacket following collision with the ion core.

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Section: Detection Of Rydberg Electron Wavepacketsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Rydberg electron wavepacket dymanics in atoms and molecules

Ramswell

Stavros

Hong

et al. 1998

Philosophical Transactions of the Royal Society of London. Seri

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show abstract

“…It is also possible to use wavepackets to investigate the interaction between different electronic configurations, i.e., to observe a time-resolved configuration interaction. In an interesting experiment, Schumacher et al 3 created a radial wavepacket in atomic Ba in the presence of a degenerate doubly excited Rydberg state and observed a temporal oscillation between configurations. Other recent Rydberg electron wavepacket experiments have involved excitating superpositions of several angular momentum states to create electron wavepackets that evolve in the angular coordinates.…”

Section: Introductionmentioning

confidence: 99%

Rovibrational and rotational autoionization dynamics of Rydberg electron wavepackets in H2: A time-dependent multichannel quantum-defect theory approach

Fielding

1997

The Journal of Chemical Physics

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Articles you may be interested inRovibrational spectroscopy using a kinetic energy operator in Eckart frame and the multi-configuration timedependent Hartree (MCTDH) approach Lifetime measurements and quantum-defect theory treatment of the k 3 Π u − state of hydrogen moleculeThe rovibrational and rotational autoionization dynamics of a Rydberg electron wavepacket in para-H 2 has been investigated using time-dependent multichannel quantum-defect theory ͑MQDT͒. In the case of rovibrational autoionization, rotational channel interactions are shown to introduce a phase shift to the electron wavepacket proportional to the strength of the configuration interaction. In the case of pure rotational autoionization, the electron wavepacket is observed to remain trapped in the Coulombic potential of the rotating molecule following rotational relaxation, thus increasing the autoionization lifetime.

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“…There have been a few steps in the next obvious direction in which two electrons participate in the wave packet motion in a nontrivial manner [1][2][3][4][5][6][7][8]. In the early studies, both electrons are excited above the ground state although at least one of the electrons has been restricted to a quite small distance, typically less than 5 Bohr radii.…”

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confidence: 99%

Propagation of double Rydberg wave packets

Robicheaux

Forrey

2005

J. Phys. B: At. Mol. Opt. Phys.

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Double Rydberg wave packets for He electronic states are propagated in time using fully quantum mechanical calculations. The wave packets are constructed so that the two electrons are simultaneously excited up to n Ryd ∼ 15 states and coupled to total orbital angular momentum equal to zero and to total spin equal to zero. We attempt to construct a wave packet to isolate symmetric stretch motion. Classical and quantum ideas are used to interpret several features of the time-dependent wave function. We briefly discuss some of the interesting problems that can be addressed.

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Time-resolved configuration interaction

Cited by 26 publications

References 13 publications

Rydberg electron wavepacket dymanics in atoms and molecules

Rydberg electron wavepacket dymanics in atoms and molecules

Rovibrational and rotational autoionization dynamics of Rydberg electron wavepackets in H2: A time-dependent multichannel quantum-defect theory approach

Propagation of double Rydberg wave packets

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