RYDBERG WAVEPACKETS IN MOLECULES: From Observation to Control

Fielding, HH

doi:10.1146/annurev.physchem.55.091602.094428

Cited by 36 publications

(19 citation statements)

References 121 publications

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“…Rydberg wavepackets, formed by coherent superposition of highly excited Rydberg states, exhibit dynamics on a variety of time scales depending on the (effective) principle quantum number ( n ) 49 . Since the classical orbiting period of a Rydberg electron scales with n 3 , 50 the time scale of electron dynamics rapidly increases as n increases and reaches the femto- to pico-second range at n ∼ 10, which is comparable with those of vibrational and rotational degrees of freedom in a molecule.…”

Section: Application To Ultrafast Photoelectron Spectroscopymentioning

confidence: 99%

Single-order laser high harmonics in XUV for ultrafast photoelectron spectroscopy of molecular wavepacket dynamics

Fushitani

Hishikawa

2016

Structural Dynamics

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We present applications of extreme ultraviolet (XUV) single-order laser harmonics to gas-phase ultrafast photoelectron spectroscopy. Ultrashort XUV pulses at 80 nm are obtained as the 5th order harmonics of the fundamental laser at 400 nm by using Xe or Kr as the nonlinear medium and separated from other harmonic orders by using an indium foil. The single-order laser harmonics is applied for real-time probing of vibrational wavepacket dynamics of I2 molecules in the bound and dissociating low-lying electronic states and electronic-vibrational wavepacket dynamics of highly excited Rydberg N2 molecules.

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Section: Application To Ultrafast Photoelectron Spectroscopymentioning

confidence: 99%

Single-order laser high harmonics in XUV for ultrafast photoelectron spectroscopy of molecular wavepacket dynamics

Fushitani

Hishikawa

2016

Structural Dynamics

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“…The number of non-trivial solutions to equation (4) equals the number of open channels. Each ρth solution vector must be normalized…”

Section: Time-dependent Mqdtmentioning

confidence: 99%

“…The ability to control the dynamics of quantum mechanical systems is a fascinating development in modern physics, and includes selective population transfer in atoms and molecules, and the steering of the dynamics of bound and free electrons (see e.g. [3] and references in [4]). …”

Section: Introductionmentioning

confidence: 99%

Coherent control in the continuum: autoionization of Xe

Kirrander¹,

Fielding²

2007

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

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We explore, by time-dependent MQDT calculations, the potential for coherent control of autoionization using phase-shaped optical pulses. We investigate the effect of step-like spectral phase modulation on the autoionization dynamics of Rydberg wave packets in the Xe atom. It is found that a single step in the spectral phase has a substantial effect on the branching ratio, if the position of the step corresponds to a resonance in the Rydberg system. These effects are enhanced if the optical pulse is engineered to have multiple steps that reflect the periodicity inherent in Rydberg systems. Further calculations indicate that, to a large extent, the effects of phase manipulations are additive and independent. We also compare this new approach with approaches based on sequences of identical coherent optical pulses. The two methods are complementary, and we suggest that in the future they may be combined.

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“…The dynamics of competing ionisation and dissociation decay paths in Rydberg states of diatomic molecules attract considerable interest, not only as model systems for the investigation of competing non-radiative processes in larger molecules, but also as prototypes for coherent control [1][2][3][4]. Despite possessing only a single molecular bond, diatomic Rydberg molecules possess many of the characteristics of complex molecular systems, such as strong non-adiabatic couplings between electronic and nuclear motion, energy flow between different degrees of freedom (electronic, vibrational and rotational), delicately balanced interference effects between competing non-radiative decay pathways, complex resonances and internal time-scales spanning orders of magnitude.…”

Section: Introductionmentioning

confidence: 99%

A spectroscopic investigation of the ionisation and dissociation decay dynamics of Rydberg states of NO

et al. 2014

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Double-resonance spectroscopy has been employed to characterise the autoionising and predissociating Rydberg states of NO converging to the υ + = 0 and υ + = 1 levels of the X 1 + ground state of NO + . Below the lowest ionisation limit, we monitor the formation of the N( 2 D) predissociation product and observe a spectrum dominated by the p(N + = 0) series, with smaller contributions from the p(2) and f(2) series. Many of the lineshapes can be fit to a simple Fano line profile. Upon vibrational excitation, a competing autoionisation channel is opened and we monitor the products of both the dissociation and ionisation channels. The υ + = 1 predissociation spectrum appears much more complex than the υ + = 0 predissociation spectrum, with significant contributions from the p(0), f(2), p(2), s (1) and d(1) series. In contrast, the υ + = 1 ionisation spectrum is dominated by the p(0) and f(2) Rydberg series, with much weaker contributions from s(1), d(1) and p(2) series. The lineshapes in the υ + = 1 predissociation and autoionisation spectra are perturbed and cannot be fit to simple Fano line profiles. In some extreme cases, these perturbations result in the complete disappearance of peaks from either the autoionisation or predissociation spectrum.

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RYDBERG WAVEPACKETS IN MOLECULES: From Observation to Control

Cited by 36 publications

References 121 publications

Single-order laser high harmonics in XUV for ultrafast photoelectron spectroscopy of molecular wavepacket dynamics

Single-order laser high harmonics in XUV for ultrafast photoelectron spectroscopy of molecular wavepacket dynamics

Coherent control in the continuum: autoionization of Xe

A spectroscopic investigation of the ionisation and dissociation decay dynamics of Rydberg states of NO

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