Publisher’s Note: Probing Orbital Structure of Polyatomic Molecules by High-Order Harmonic Generation [Phys. Rev. Lett.<b>98</b>, 203007 (2007)]

Torres, Ricardo; Kajumba, N.; Underwood, Jonathan G.; Robinson, J.; Baker, Sarah; Tisch, J. W. G.; Nalda, R. de; Bryan, William A.; Velotta, R.; Altucci, C.; Turcu, I. C. E.; Marangos, J. P.

doi:10.1103/physrevlett.98.239903

Cited by 40 publications

(55 citation statements)

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“…It has been observed so far that the HHG from aligned molecules depends on the angle between the molecular axis and the laser field direction 5,6,8,9,[10][11][12][13] . This indicates that the nonlinear optical response of a molecule is strongly affected by the angular distribution of the highest occupied molecular orbital (HOMO) and/or the electron distribution in a molecule.…”

Section: Introductionmentioning

confidence: 99%

“…4,5) This demonstrated that one can control the HHG process with aligned molecules and also examine the molecular structure by observing the nonlinear optical response of aligned molecules. Then much attention was focused on the HHG in the experimental studies [6][7][8][9][10] as well as the theoretical [11][12][13][14][15][16] in a variety of fields of molecular science.…”

Section: Introductionmentioning

confidence: 99%

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Angular Dependence of High-order Harmonic Generation from Nonadiabatically Aligned Molecules

Yoshii

Miyaji

Miyazaki

2008

The Review of Laser Engineering

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We measured the dependence of high-order harmonic generation (HHG) on the angle α between polarization directions of high-intensity femtosecond laser pulses in the pump and probe experiment. The experimental results of N 2 and O 2 are compared with the calculated ones using the theory developed recently to illustrate the characteristic properties of HHG from aligned N 2 and O 2 , and then the excellent agreement is obtained. It is also shown that the observed α-dependent harmonic signal is strongly influenced by the degree of alignment of molecules and is not identical to the harmonic distribution calculated as a function of the angle between the field direction and the molecular axis.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Angular Dependence of High-order Harmonic Generation from Nonadiabatically Aligned Molecules

Yoshii

Miyaji

Miyazaki

2008

The Review of Laser Engineering

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“…While SAE based approaches have been successful in describing the interaction of inert gases with strong fields, more and more work on molecules reveals the involvement of orbitals lower in energy than the highest occupied orbital [5,6], suggesting the importance of many-electron mechanisms. Such involvement is usually related to the polarization direction of laser field in the molecular frame [7].…”

Section: Introductionmentioning

confidence: 99%

Tunneling ionization of the F4 and D6 states of vanadium: Exchange blockade

Chu

Groenenboom

2017

Phys. Rev. A

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Using TDDFT calculations we compare tunneling ionization of the a 4 F ground state and the a 6 D first excited state of vanadium in laser fields of intensities between 1.4 and 4.0×10 13 W/cm 2 .The calculated ionization yields of the ground state of vanadium were already shown to agree well with experimental results [Chu and Groenenboom, Phys. Rev. A 94, 053417 (2016)]. We find that the tunneling ionization rate of the sextet state is lower than that of the quartet state. This is surprising, since the ionization potential of the sextet is lower than that of the quartet state.This finding, however, is consistent with the experimental observation that niobium, whose ground state is a 6 D 1/2 , has a much smaller ionization yield than vanadium (a 4 F 3/2 ), even though their ionization potentials are extremely close [Smits et al., Phys. Rev. Lett. 93, 213003 (2004)]. Our calculations demonstrate the existence of exchange blockade for the higher spin state. It arises from a strong field dynamic effect that the highest and second highest electrons mixing in the same set of unoccupied spin orbitals, which causes an isotropic attractive potential that confines the electrons close to the core.

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“…In fact, rich information contained in HHG spectra from aligned molecules is mostly washed out if the molecules are not well aligned. Whereas earlier studies have focused mostly on simple molecules with the use of infrared lasers, more recent studies in HHG spectroscopy have now expanded to more complex targets and by using midinfrared lasers [14][15][16][17].As the geometric arrangement of atoms in stereoisomers differs, they can serve as interesting tests for HHG spectroscopy. In a recent paper by Wong et al [16], HHG spectra from stereoisomers of 1,2-dichloroethylene (1,2-DCE, C 2 H 2 Cl 2 ) and 2-butene (C 4 H 8 ) have been reported.…”

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confidence: 99%

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confidence: 99%

High-order-harmonic generation from molecular isomers with midinfrared intense laser pulses

Lucchese

Lin

2013

Phys. Rev. A

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We present theoretical calculations of high-order-harmonic generation (HHG) from stereoisomers of 1,2-dichloroethylene (C 2 H 2 Cl 2 ) and 2-butene (C 4 H 8 ) based on the quantitative rescattering theory. Our results show that the HHG spectra from these cis and trans isomers with intense midinfrared laser pulses are clearly distinguishable, even when the molecules are randomly oriented, in good agreement with the recent experiments by Wong et al. [Phys. Rev. A 84, 051403(R) (2011)]. We found that the angle-averaged tunneling ionization yields and photoionization cross sections from the cis and trans isomers for both molecules are nearly identical. The origin of the differences in HHG spectra is traced as due to the interplay in the angular dependence of the photoionization (or photorecombination) cross section and ionization rate. High-order-harmonic generation (HHG) has been shown both experimentally and theoretically to contain information about the target molecular structure and dynamics, which are encoded in the amplitude and phase of the emitted high-order harmonics [1][2][3][4][5][6][7][8][9][10][11][12]. HHG spectroscopy for simple molecules has been greatly benefited from the ability to align molecules [13]. In fact, rich information contained in HHG spectra from aligned molecules is mostly washed out if the molecules are not well aligned. Whereas earlier studies have focused mostly on simple molecules with the use of infrared lasers, more recent studies in HHG spectroscopy have now expanded to more complex targets and by using midinfrared lasers [14][15][16][17].As the geometric arrangement of atoms in stereoisomers differs, they can serve as interesting tests for HHG spectroscopy. In a recent paper by Wong et al. [16], HHG spectra from stereoisomers of 1,2-dichloroethylene (1,2-DCE, C 2 H 2 Cl 2 ) and 2-butene (C 4 H 8 ) have been reported. It was found that the spectra from these cis and trans isomers are quite distinguishable in a broad range of energy, even when the molecules are not aligned. The mechanism behind this was attributed as due to the differences in the strong-field ionization. The ability to distinguish nonaligned isomers by HHG spectroscopy is of great interest. In particular, it opens up the possibility to study fast structural changes during the isomerization process using HHG [18] even without the need of molecular alignment.In this Rapid Communication we employ the quantitative rescattering (QRS) theory [4,19,20] as extended to polyatomic targets [21] to calculate HHG spectra from cis and trans stereoisomers of 1,2-DCE and 2-butene under intense midinfrared laser pulses. Our calculation shows good agreements with experiment by Wong et al. [16]. However, we found that the angle-averaged ionization yields from cis and trans isomers are nearly indistinguishable. Here we provide an analysis of the nature of the differences in HHG spectra from these isomers.Within the QRS, the laser-induced dipole D(ω,θ,φ) for a molecule in a linearly polarized intense laser pulse can be written as a p...

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Publisher’s Note: Probing Orbital Structure of Polyatomic Molecules by High-Order Harmonic Generation [Phys. Rev. Lett.98, 203007 (2007)]

Cited by 40 publications

References 0 publications

Angular Dependence of High-order Harmonic Generation from Nonadiabatically Aligned Molecules

Angular Dependence of High-order Harmonic Generation from Nonadiabatically Aligned Molecules

Tunneling ionization of the F4 and D6 states of vanadium: Exchange blockade

High-order-harmonic generation from molecular isomers with midinfrared intense laser pulses

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