Correlated variational treatment of ionization coupled to nuclear motion: Ultrafast pump and ionizing probe of electronic and nuclear dynamics in LiH

Bello, Roger Y.; Lucchese, Robert R.; Rescigno, T. N.; McCurdy, C. William

doi:10.1103/physrevresearch.3.013228

Cited by 8 publications

(13 citation statements)

References 46 publications

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“…Our earlier study [30] found that indeed the changing character, from covalent to ionic, of the A 1 Σ + state is visible in the photoelectron energies and angular distributions as well as in the kinetic energies of the dissociating Li + and H fragments. However, in the case of the A 1 Σ + state the nuclear dynamics on the intermediate state and the changing character of the electronic state are probed differently at different geometries by the probe pulse, because the photoionization amplitudes change rapidly with internuclear distance.…”

Section: Introductionmentioning

confidence: 78%

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Pump and ionizing-probe dynamics in a simultaneous treatment of electronic and nuclear motion in LiH

Bello,

Lucchese,

McCurdy

2023

Phys. Rev. A

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The dissociative single ionization of the LiH molecule using a two-color UV-UV pump-probe scheme is simulated in ab initio calculations demonstrating how the dynamics initiated on intermediate Rydberg states of diatomic molecules can be imaged by such experiments. The theoretical treatment combines nuclear motion with highly correlated descriptions of electronic continua and bound electronic states. Nuclear dynamics on Rydberg states are only weakly reflected by changes in photoelectron energies ejected by time delayed ionizing pulses if the Rydberg potential curves parallel those of the ion states being produced. However, coincidence measurements guided by knowledge of the photoionization amplitudes as a function of internuclear distance can still reveal intermediate state dynamics in pump-probe experiments.

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Section: Introductionmentioning

confidence: 78%

“…We recently applied this methodology [30] to investigate how a correlated treatment of the ionization problem describes the dynamics of the LiH molecule in pump and probe processes that populate and then dissociatively ionize the intermediate A 1 Σ + first excited state of the molecule, shown in Fig. 1(d).…”

Section: Introductionmentioning

confidence: 99%

Pump and ionizing-probe dynamics in a simultaneous treatment of electronic and nuclear motion in LiH

Bello,

Lucchese,

McCurdy

2023

Phys. Rev. A

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“…The state population as a function of delay between separate XUV and NIR pulsed fields were calculated by solving the Time-Dependent Schödinger-Equation (TDSE). The time-dependent wave function was expanded in a basis of Born-Oppenheimer vibrational states [27], which were found by diagonalizing the nuclear Hamiltonian using the PECs discussed above. In order to simulate the different paths probed by the experiment two separated calculations were performed.…”

Section: Theoretical Methodsmentioning

confidence: 99%

Non-Equilibrium Dynamics in Two-Color, Few-Photon Dissociative Excitation and Ionization of D$_2$

Slaughter,

Sturm,

Bello

et al. 2021

Preprint

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D2 molecules, excited by linearly cross-polarized femtosecond extreme ultraviolet (XUV) and near-infrared (NIR) light pulses, reveal highly structured D + ion fragment momenta and angular distributions that originate from two different 4-step dissociative ionization pathways after four photon absorption (1 XUV + 3 NIR). We show that, even for very low dissociation kinetic energy release ≤ 240 meV, specific electronic excitation pathways can be identified and isolated in the final ion momentum distributions. With the aid of ab initio electronic structure and time-dependent Schrödinger equation calculations, angular momentum, energy, and parity conservation are used to identify the excited neutral molecular states and molecular orientations relative to the polarization vectors in these different photoexcitation and dissociation sequences of the neutral D2 molecule and its D + 2 cation. In one sequential photodissociation pathway, molecules aligned along either of the two light polarization vectors are excluded, while another pathway selects molecules aligned parallel to the light propagation direction. The evolution of the nuclear wave packet on the intermediate B 1 Σ + u electronic state of the neutral D2 molecule is also probed in real time.

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“…LiH as a prototype diatomic molecule in molecular reaction dynamics has attracted considerable attention, leading to widespread investigations in recent years [1][2][3][4][5][6]. The ground state structure and potential energy function of LiH have been provided [7][8][9], and dedicated efforts have been devoted to manipulate both orientation and photodissociation process [10][11][12].…”

Section: Introductionmentioning

confidence: 99%

Influence of molecular orientation on the photodissociation process of LiH molecules

Yan,

Liu,

Sheng

et al. 2024

Int J of Quantum Chemistry

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Regulation of photodissociation dynamics of oriented LiH molecules in different dissociation channels is proposed based on time dependent quantum wave packet theory. The enhancement of molecular orientation on the photodissociation of LiH is obvious with our theoretical scheme. The results show that the molecular orientation in the ground state has a great effect on the angular distributions of wave packets. By using the proper laser pulses and controlling the polarization direction of the laser pulses, the enhancement of the photodissociation could be realized. After the molecular orientation, an optimal dissociation channel is observed with an improved dissociation probability. Compared with the results without molecular orientation, the maximal dissociation probability is increased by 8.1% in the indirect dissociation channel and 30.7% in the direct dissociation channel. The enhancement effect is more obvious in the direct dissociation channel, which provides a possible method to manipulate the dissociation of LiH molecules experimentally. Additionally, the photodissociation process of LiH also relies on the electric intensity and delay time of two pump pulses.

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Correlated variational treatment of ionization coupled to nuclear motion: Ultrafast pump and ionizing probe of electronic and nuclear dynamics in LiH

Cited by 8 publications

References 46 publications

Pump and ionizing-probe dynamics in a simultaneous treatment of electronic and nuclear motion in LiH

Pump and ionizing-probe dynamics in a simultaneous treatment of electronic and nuclear motion in LiH

Non-Equilibrium Dynamics in Two-Color, Few-Photon Dissociative Excitation and Ionization of D$_2$

Influence of molecular orientation on the photodissociation process of LiH molecules

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