Structure factors for tunneling ionization rates of diatomic molecules

Saito, Ryoichi; Tolstikhin, Oleg I.; Madsen, Lars Bojer; Morishita, Tōru

doi:10.1016/j.adt.2015.02.001

Cited by 26 publications

(30 citation statements)

References 29 publications

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“…From a simulation standpoint, a variety of computational approaches have been applied to angle-dependent ionization rates in molecules [8,9,13,14,[16][17][18][19][20][21]. These range from orbital model-based approaches like molecular-orbital Ammosov-Delone-Krainov (MO-ADK) [22][23][24] and weak-field asymptotic theory [25][26][27][28], to first-principles methods such as time-dependent Hartree-Fock (TDHF) [29][30][31], timedependent density functional theory (TDDFT) [32][33][34][35][36][37][38][39][40][41][42][43][44], and time-dependent configuration-interaction singles (TD-CIS) [45][46][47].…”

Section: Introductionmentioning

confidence: 99%

Angle dependence of strong-field single and double ionization of carbonyl sulfide

et al. 2018

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We have studied, experimentally and theoretically, the ionization probability of carbonyl sulfide (OCS) molecules in intense linearly-polarized 800 nm laser pulses as a function of the angle between the molecular axis and the laser polarization. Experimentally, the molecules are exposed to two laser pulses with a relative time delay. The first, weaker pulse induces a nuclear rotational wave packet within each molecule such that the ensemble exhibits preferential alignment in the laboratory frame at specific times. The second, stronger pulse induces ionization, and the variation in single and double ionization yields is measured as a function of the delay between the two pulses. The angular-dependence of the ionization yield is extracted by fitting the delay-dependent yields to a sum of delay-dependent moments of the rotational wave packet's angular distribution. We compute these same angular-dependent strong-field ionization yields for OCS using time-dependent density functional theory (TDDFT). For the single ionization case, our measurements agree well with TDDFT calculations and with previous experiments. Furthermore, analysis of the simulated one-body density reveals that, when averaged over a laser cycle, the resulting hole is delocalized across the molecule for light polarized perpendicular to the molecular axis, and mostly localized on the sulfur for parallel polarization. This suggests that preferential molecular alignment is a key parameter for controlling charge migration dynamics initiated by strong-field ionization. For double ionization, the agreement between experiment and theory is less compelling, reflecting the substantial challenges of computing double ionization yields using TDDFT methods.

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Section: Introductionmentioning

confidence: 99%

Angle dependence of strong-field single and double ionization of carbonyl sulfide

et al. 2018

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“…First we notice that our HF result agrees very well with the previous result in Refs. [19,23], with maxima at β = 0 and β = π , i.e., when the molecule is aligned along the polarization direction of the electric field. As discussed in previous works (e.g., in [19]), this form of the structure factor and therefore the tunneling ionization rate is due to the HOMO being of σ symmetry, with the charge density elongated along the internuclear axis.…”

Section: A Structure Factors For Hmentioning

confidence: 99%

“…(15), we follow the approach employed in Refs. [20,23]. We consider g 000 (β; η) as a function of 1/η with N fit points in the interval [1/η max ,1/η min ] and fit it with a polynomial of degree N deg ,…”

Section: Evaluation Of Structure Factorsmentioning

confidence: 99%

“…As already demonstrated for the one-electron WFAT, usage of standard quantum chemistry Gaussian basis sets to obtain the structure factor is made difficult by the slow convergence of the tail of the wave function with the number of primitive basis functions [19][20][21]: The calculation of the ground-state energy, which is the main objective in quantum chemistry, does not require an accurate treatment of the long-range behavior of the wave function. For diatomics in the HF approximation, an existing grid-based method in a prolate spheroidal basis, X2DHF [22], was shown to produce accurate long-range behavior [20,23]. For polyatomic molecules, the usage of a polarization-consistent basis was able to obtain structure factors in the HF approximation [20].…”

Section: Introductionmentioning

confidence: 99%

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Electron correlation in tunneling ionization of diatomic molecules: An application of the many-electron weak-field asymptotic theory with a generalized-active-space partition scheme

2017

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“…[18][19][20][21]), molecular alignment and orientation (see, e.g, Refs. [22][23][24][25][26]), isotope effect [27,28], multielectron effects (see, e.g., Refs. [29][30][31][32]), and contribution from multiple orbitals (see, e.g., Ref.…”

Section: Introductionmentioning

confidence: 99%

Torsional effects in strong-field ionization of molecules

Dnestryan

Tolstikhin

Jensen

et al. 2019

Phys. Rev. Research

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We investigate how the ionization rate of molecules consisting of a pair of phenyl rings depends on the torsional dihedral angle between these two rings. We consider different orientations of the molecules with respect to the external field direction and find differences in the rates in biphenyl and substituted biphenyl. The evaluation of the rates is made possible by application of the integral representation of the weak-field asymptotic theory for tunneling ionization. We report a strong variation of the ionization rates with dihedral angle with contributions from several orbitals and a large difference between biphenyl and substituted biphenyl related to the permanent dipole of the latter system.

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Structure factors for tunneling ionization rates of diatomic molecules

Cited by 26 publications

References 29 publications

Angle dependence of strong-field single and double ionization of carbonyl sulfide

Angle dependence of strong-field single and double ionization of carbonyl sulfide

Electron correlation in tunneling ionization of diatomic molecules: An application of the many-electron weak-field asymptotic theory with a generalized-active-space partition scheme

Torsional effects in strong-field ionization of molecules

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