NO2 jet cooled visible excitation spectrum: Vibronic chaos induced by the X̃ 2A1–Ã 2B2 interaction

Delon, Antoine; Jost, R.; Lombardi, M.

doi:10.1063/1.461620

Cited by 140 publications

(121 citation statements)

References 35 publications

(1 reference statement)

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“…The CI between the first two 2 AЈ states of the NO 2 molecule is known to lead to an extremely complex absorption spectra [13][14][15] and has been the subject of numerous studies of nonadiabatic dynamics. [16][17][18][19][20][21][22] For C 2v geometries the two surfaces ͑ 2 A 1 and 2 B 2 ͒ intersect at a bond angle that depends on the bond length and form a one-dimensional CI seam.…”

Section: Introductionmentioning

confidence: 99%

Time-resolved photoelectron spectroscopy of wavepackets through a conical intersection in NO2

Arasaki

Takatsuka²,

Wang³

et al. 2010

The Journal of Chemical Physics

105

111

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We report the results of theoretical studies of the time-resolved femtosecond photoelectron spectroscopy of quantum wavepackets through the conical intersection between the first two 2 AЈ states of NO 2 . The Hamiltonian explicitly includes the pump-pulse interaction, the nonadiabatic coupling due to the conical intersection between the neutral states, and the probe interaction between the neutral states and discretized photoelectron continua. Geometry-and energy-dependent photoionization matrix elements are explicitly incorporated in these studies. Photoelectron angular distributions are seen to provide a clearer picture of the ionization channels and underlying wavepacket dynamics around the conical intersection than energy-resolved spectra. Time-resolved photoelectron velocity map images are also presented.

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Section: Introductionmentioning

confidence: 99%

Time-resolved photoelectron spectroscopy of wavepackets through a conical intersection in NO2

Arasaki

Takatsuka²,

Wang³

et al. 2010

The Journal of Chemical Physics

105

111

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“…The CI between the first two 2 A 0 states of the NO 2 molecule is known to lead to an extremely complex absorption spectra, [35][36][37] and has been the subject of numerous studies of nonadiabatic dynamics. [38][39][40][41][42][43][44] For C 2v geometries the two surfaces ( 2 A 1 and 2 B 2 ) intersect at a bond angle that depends on the bond length and form a one-dimensional CI seam.…”

Section: Introductionmentioning

confidence: 99%

Monitoring the effect of a control pulse on a conical intersection by time-resolved photoelectron spectroscopy

Arasaki

Wang

McKoy

et al. 2011

Phys. Chem. Chem. Phys.

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We have previously shown how femtosecond angle-and energy-resolved photoelectron spectroscopy can be used to monitor quantum wavepacket bifurcation at an avoided crossing or conical intersection and also how a symmetry-allowed conical intersection can be effectively morphed into an avoided crossing by photo-induced symmetry breaking. The latter result suggests that varying the parameters of a laser to modify a conical intersection might control the rate of passage of wavepackets through such regions, providing a gating process for different chemical products. In this paper, we show with full quantum mechanical calculations that such optical control of conical intersections can actually be monitored in real time with femtosecond angle-and energy-resolved photoelectron spectroscopy. In turn, this suggests that one can optimally control the gating process at a conical intersection by monitoring the photoelectron velocity map images, which should provide far more efficient and rapid optimal control than measuring the ratio of products. To demonstrate the sensitivity of time-resolved photoelectron spectra for detecting the consequences of such optical control, as well as for monitoring how the wavepacket bifurcation is affected by the control, we report results for quantum wavepackets going through the region of the symmetry-allowed conical intersection between the first two 2 A 0 states of NO 2 that is transformed to an avoided crossing. Geometry-and energy-dependent photoionization matrix elements are explicitly incorporated in these studies. Time-resolved photoelectron angular distributions and photoelectron images are seen to systematically reflect the effects of the control pulse.

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“…There is an upper limit L max of L that one must be aware of: The spectral fluctuations of levels from billiards agree with those of random matrices -i.e. they are universal -within intervals of a maximum length which is inversely proportional to the length of the shortest periodic orbit in the billiard [34,35]. This requires L max = 5 here.…”

Section: The Distribution Of the Datamentioning

confidence: 99%

Analyzing symmetry breaking within a chaotic quantum system via Bayesian inference

Barbosa

Harney

2000

Phys. Rev. E

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Bayesian inference is applied to the level fluctuations of two coupled microwave billiards in order to extract the coupling strength. The coupled resonators provide a model of a chaotic quantum system containing two coupled symmetry classes of levels. The number variance is used to quantify the level fluctuations as a function of the coupling and to construct the conditional probability distribution of the data. The prior distribution of the coupling parameter is obtained from an invariance argument on the entropy of the posterior distribution.

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NO2 jet cooled visible excitation spectrum: Vibronic chaos induced by the X̃ 2A1–Ã 2B2 interaction

Cited by 140 publications

References 35 publications

Time-resolved photoelectron spectroscopy of wavepackets through a conical intersection in NO2

Time-resolved photoelectron spectroscopy of wavepackets through a conical intersection in NO2

Monitoring the effect of a control pulse on a conical intersection by time-resolved photoelectron spectroscopy

Analyzing symmetry breaking within a chaotic quantum system via Bayesian inference

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