Nuclear-wave-packet quantum interference in the intense laser dissociation of the D<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mrow /><mml:mn>2</mml:mn></mml:msub></mml:math><mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msup><mml:mrow /><mml:mo>+</mml:mo></mml:msup></mml:math>molecule

Halász, Gábor J.; Vibók, Ágnes; Moiseyev, Nimrod; Cederbaum, Lorenz S.

doi:10.1103/physreva.88.043413

Cited by 51 publications

(55 citation statements)

References 33 publications

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“…A wealth of nuclear-wave-packet quantum interferences show up in intense laser dissociation due to the nonadiabatic involvement of the rotation [8,9]. A robust effect in the angular distribution of the photofragments has been found that serves as a direct signature of the LICI and should be amenable to observations [10].…”

Section: Introductionmentioning

confidence: 99%

Towards controlling the dissociation probability by light-induced conical intersections

et al. 2016

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Light-induced conical intersections (LICIs) can be formed both by standing or by running laser waves. The position of a LICI is determined by the laser frequency while the laser intensity controls the strength of the nonadiabatic coupling. Recently, it was shown within the LICI framework that linearly chirped laser pulses have an impact on the dissociation dynamics of the D + 2 molecule (J. Chem. Phys. 143, 014305, (2015); ibid 144, 074309, (2016)). In this work we exploit this finding and perform calculations using chirped laser pulses in which the time dependence of the laser frequency is designed so as to force the LICI to move together with the field-free vibrational wave packet as much as possible. Since nonadiabaticity is strongest in the vicinity of the conical intersection, this is the first step towards controlling the dissociation process via the LICI. Our showcase example is again the D + 2 molecular ion. To demonstrate the impact of the LICIs on the dynamical properties of diatomics, the total dissociation probabilities and the population of the different vibrational levels after the dissociation process are studied and discussed.

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Section: Introductionmentioning

confidence: 99%

Towards controlling the dissociation probability by light-induced conical intersections

et al. 2016

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“…A signature of LICI's is quantum interference in strong-field laser-induced dissociation of the hydrogen or deuterium molecular ion [18,19]. Calculations predict that the interference produces modulations of the angular distributions of the dissociated fragments.…”

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Observation of Quantum Interferences via Light-Induced Conical Intersections in Diatomic Molecules

et al. 2016

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We observe energy-dependent angle-resolved diffraction patterns in protons from strong-field dissociation of the molecular hydrogen ion H + 2 . The interference is a characteristic of dissociation around a laser-induced conical intersection (LICI), which is a point of contact between two surfaces in the dressed 2-dimensional Born-Oppenheimer potential energy landscape of a diatomic molecule in a strong laser field. The interference magnitude and angular period depend strongly on the energy difference between the initial state and the LICI, consistent with coherent diffraction around a cone-shaped potential barrier whose width and thickness depend on the relative energy of the initial state and the cone apex. These findings are supported by numerical solutions of the time-dependent Schrödinger equation for similar experimental conditions.The Born-Oppenheimer approximation (BOA) represents intramolecular dynamics as the motion of nuclear wave packets on potential energy surfaces (PES) of electronic eigenvalues embedded in the space of nuclear geometries. A molecule on a single PES remains there so long as the adiabatic condition is obeyed, i.e. so long as nuclear kinetic energies are small compared to electronic state separations. This assumption must break down, however, if two or more PESs approach each other [1][2][3]. When this happens non-adiabatic couplings between the nearly-degenerate surfaces become important. The true eigenvalues can then be calculated by diagonalizing the Hamiltonian in the reduced space of the near degeneracy.According to simple geometrical arguments, molecules with at least two dimensions of internal nuclear motion (i.e. three or more atoms) must have some points where two or more PESs become degenerate, a condition known as a conical intersection (CI) [4]. These CIs play a key role in the relaxation dynamics of most polyatomic molecules including important biochemical processes such as the photostability of DNA [5], and the preliminary process of vision [6]. The dimension of the CI manifold is two less than the internal nuclear geometry. Thus for the simplest case of a tri-atomic molecule, the CI manifold has dimensionality of 3N − 8 = 1. The topological nature of CIs allows the nonadiabatic couplings to diverge and thus display related phenomena such as a geometric or Berry's phase [4,7] in wavepackets that circumnavigate the CI.Naturally occurring CIs cannot exist for a free diatomic molecule because the internuclear separation vector R is the only internal nuclear degree of freedom, and this is insufficient to fulfil the crossing condition. The nonadiabatic terms in the full Hamiltonian cause the BOA states to repel according to the so-called "no-crossing" rule. A diatomic molecule in a strong laser field, however, has a second degree of freedom defined by the laser polarization ε. When viewed in a Floquet basis of laserdressed electronic states, a molecule coupled by this field can exhibit a point of degeneracy called a light-induced conical intersection (LICI) in the 2−dimension...

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“…In the framework of this model, we have followed the nuclear motion on electronic potential energy surfaces which have an important role in the dynamics. We have extended an existing approach [10][11][12][13][14][15][16][17] which considered only bound electronic states in the dynamics by including the potential energy surfaces corresponding to ionized states. This way, beside the dissociation we were also able to study the ionization.…”

Section: Discussionmentioning

confidence: 99%

“…A few years ago, we have started a systematic study of the nonadiabatic effect induced by laser fields in molecular systems and demonstrated that the light-induced conical intersections have a significant impact on several dynamical properties (like the molecular spectra, the molecular alignment etc.) of diatomic molecules [10][11][12][13][14][15][16][17].…”

Section: Introductionmentioning

confidence: 99%

Toward the Full Quantum Dynamical Description of Photon Induced Processes in D₂⁺

et al. 2016

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The dissociative ionization (multiphoton regime) of the D ion by ultrashort laser pulses has been studied theoretically using ab initio calculations. The combined ionization and dissociation spectrum was explored for fixed molecular axis orientations. In accordance with previous investigations, the dominant features in the obtained joint energy spectrum were multiphoton peaks. In addition to this, in the present work, photoelectron angular distributions were analyzed as well. By performing a partial wave analysis for each multiphoton peak, we have identified the number of absorbed photons. Moreover, we also found that the angular distribution can significantly change inside a multiphoton peak as a function of electron and nuclear kinetic energy.

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Nuclear-wave-packet quantum interference in the intense laser dissociation of the D2+molecule

Cited by 51 publications

References 33 publications

Towards controlling the dissociation probability by light-induced conical intersections

Towards controlling the dissociation probability by light-induced conical intersections

Observation of Quantum Interferences via Light-Induced Conical Intersections in Diatomic Molecules

Toward the Full Quantum Dynamical Description of Photon Induced Processes in D₂⁺

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Nuclear-wave-packet quantum interference in the intense laser dissociation of the D2+molecule

Cited by 51 publications

References 33 publications

Towards controlling the dissociation probability by light-induced conical intersections

Towards controlling the dissociation probability by light-induced conical intersections

Observation of Quantum Interferences via Light-Induced Conical Intersections in Diatomic Molecules

Toward the Full Quantum Dynamical Description of Photon Induced Processes in D2+

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Toward the Full Quantum Dynamical Description of Photon Induced Processes in D₂⁺