Application of the weak-field asymptotic theory to tunneling ionization of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:math>

Madsen, Lars Bojer; Jensen, Frank; Tolstikhin, Oleg I.; Morishita, Tōru

doi:10.1103/physreva.89.033412

Cited by 28 publications

(18 citation statements)

References 39 publications

(70 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…These latter results form benchmark data for tunneling ionization with which other results in the literature [48] can be compared. Since in high-harmonic spectroscopy applications of the WFAT the phase of the structure factor is important [22][23][24], we emphasize that we show the structure factor and not its norm squared as in previous publications [26,30,39,49].…”

Section: Resultsmentioning

confidence: 72%

Structure factors for tunneling ionization rates of molecules: General Hartree-Fock-based integral representation

et al. 2017

Self Cite

View full text Add to dashboard Cite

In the leading-order approximation of the weak-field asymptotic theory (WFAT), the dependence of the tunneling ionization rate of a molecule in an electric field on its orientation with respect to the field is determined by the structure factor of the ionizing molecular orbital. The WFAT yields an expression for the structure factor in terms of a local property of the orbital in the asymptotic region. However, in general quantum chemistry approaches molecular orbitals are expanded in a Gaussian basis which does not reproduce their asymptotic behavior correctly. This hinders the application of the WFAT to polyatomic molecules, which are attracting increasing interest in strong-field physics. Recently, an integral-equation approach to the WFAT for tunneling ionization of one electron from an arbitrary potential has been developed. The structure factor is expressed in an integral form as a matrix element involving the ionizing orbital. The integral is not sensitive to the asymptotic behavior of the orbital, which resolves the difficulty mentioned above. Here, we extend the integral representation for the structure factor to many-electron systems treated within the Hartree-Fock method and show how it can be implemented on the basis of standard quantum chemistry software packages. We validate the methodology by considering noble-gas atoms and the CO molecule, for which accurate structure factors exist in the literature. We also present benchmark results for CO 2 and for NH 3 in the pyramidal and planar geometries.

show abstract

Section: Resultsmentioning

confidence: 72%

Structure factors for tunneling ionization rates of molecules: General Hartree-Fock-based integral representation

et al. 2017

Self Cite

View full text Add to dashboard Cite

show abstract

“…The dominant ionization channel for both states is ν = (0,0). According to the WFAT, the ionization rate in the limit F → 0 is given by the leading-order asymptotic formula (30). For the present system and states we have m = 0 and μ z = 0.…”

Section: Comparison With Time-dependent Calculationsmentioning

confidence: 95%

“…The techniques to extract the asymptotic coefficients g ν [Eq. (25a)] from an unperturbed molecular orbital were developed for linear [28,29] and nonlinear [30] molecules. To obtain the coefficients a ν [Eq.…”

Section: B Weak-field Asymptotic Theorymentioning

confidence: 99%

See 1 more Smart Citation

Weak-field asymptotic theory of tunneling ionization including the first-order correction terms: Application to molecules

et al. 2015

Self Cite

View full text Add to dashboard Cite

The weak-field asymptotic theory (WFAT) of tunneling ionization including the first-order correction terms is validated for molecules by comparison with accurate calculations of molecular Siegert states in a static electric field. Both fundamental observables related to tunneling ionization, namely, the ionization rate and transverse momentum distribution of the ionized electrons, are considered. This complements our previous study of atoms [V. H. Trinh et al., Phys. Rev. A 87, 043426 (2013)]. Similarly to the atomic case, the first-order terms essentially improve the agreement between the WFAT and accurate results in a wide interval of fields up to the onset of over-the-barrier ionization. This establishes the WFAT including the first-order correction terms as an appealing alternative to accurate calculations in the tunneling regime. In addition to demonstrating the quantitative performance of the WFAT, the theory is shown to be helpful for understanding the field and orientation dependencies of the observables. In particular, we show that the first-order terms account for a deviation of the shape of the orientation dependence of the ionization rate of a molecule from that of the ionizing orbital as the field grows, which has important implications for strong-field molecular imaging techniques. This prediction of the WFAT is confirmed by comparison with time-dependent calculations.

show abstract

“…The calculation of the structure factor from the asymptotic form of the wave function in the ME-WFAT provides a challenge. 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].…”

Section: Introductionmentioning

confidence: 99%

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

Self Cite

View full text Add to dashboard Cite

show abstract

Application of the weak-field asymptotic theory to tunneling ionization ofH2O

Cited by 28 publications

References 39 publications

Structure factors for tunneling ionization rates of molecules: General Hartree-Fock-based integral representation

Structure factors for tunneling ionization rates of molecules: General Hartree-Fock-based integral representation

Weak-field asymptotic theory of tunneling ionization including the first-order correction terms: Application to molecules

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

Contact Info

Product

Resources

About