Molecular high-order-harmonic generation due to the recollision mechanism by a circularly polarized laser pulse

Zhu, Xinxin; Liu, Xi; Yang, Li; Qin, Meiyan; Zhang, Qingbin; Lan, Pengfei; Lu, Peixiang

doi:10.1103/physreva.91.043418

Cited by 36 publications

(16 citation statements)

References 59 publications

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“…HHG has been intensively studied in experimental and theoretical investigations [3][4][5], because it promises both applications for generating attosecond pulses [6][7][8] and for probing the molecular structure [9][10][11][12] and ultrafast dynamics [13][14][15][16][17]. The HHG process can be nicely explained by the three-step model [18,19].…”

Section: Introductionmentioning

confidence: 99%

Helicity reversion in high-order-harmonic generation driven by bichromatic counter-rotating circularly polarized laser fields

Zhang

Zhu

et al. 2016

Phys. Rev. A

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We investigate the polarization properties of high harmonics generated with the bichromatic counterrotating circularly polarized (BCCP) laser fields by numerically solving time-dependent Schrödinger equation (TDSE). It is found that, the helicity of the elliptically polarized harmonic emission is reversed at particular harmonic orders. Based on the time-frequency analysis and the classical three-step model, the correspondence between the positions of helicity reversions and the classical trajectories of continuum electrons is established. It is shown that, the electrons ionized at one lobe of laser field can be divided into different groups based on the different lobes they recombine at, and the harmonics generated by adjacent groups have opposite helicities. Our study performs a detailed analysis of high harmonics in terms of electron trajectories and depicts a clear and intuitive physical picture of the HHG process in BCCP laser field.

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Section: Introductionmentioning

confidence: 99%

Helicity reversion in high-order-harmonic generation driven by bichromatic counter-rotating circularly polarized laser fields

Zhang

Zhu

et al. 2016

Phys. Rev. A

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“…Basically, the CD of HHG here results from the chiral structure of the molecule that the substituents on each side must be different. Due to the rescattering feature of HHG process, HHG driven by CP laser pulses has some problems, such as low efficiency [25,45] and low cutoff frequencies [46]. These shortages are adverse to its possible applications, like chiral discrimination.…”

Section: Resultsmentioning

confidence: 99%

High harmonic generation from axial chiral molecules

Wang¹,

Zhu²,

Liu³

et al. 2017

Opt. Express

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Axial chiral molecules, whose stereogenic element is an axis rather than a chiral center, have attracted widespread interest due to their important application, such as asymmetric synthesis and chirality transfer. We investigate high harmonic generation from axial chiral molecules with bichromatic counterrotating circularly polarized laser fields. High harmonic generation from three typical molecules: (Sa)-3-chloropropa-1,2-dien-1-ol, propadiene, and (Ra)-2,3-pentadiene is simulated with time-dependent density-functional theory and strong field approximation. We found that harmonic spectra for 3D oriented axial chiral molecules exhibit obvious circular dichroism. However, the circular dichroism of High harmonic generation from an achiral molecule is much trivial. Moreover, the dichroism of high harmonic generation still exists when axial chiral molecules are 1D oriented,such as (Sa) -3-chloropropa-1,2-dien-1-ol. For a special form of axial chiral molecules with the formula abC=C=Cab (a, b are different substituents), like (Ra)-2,3-pentadiene, the dichroism discriminations disappear when the molecules are only in 1D orientation. The circular dichroism of high harmonic generation from axial chiral molecules is well explained by the trajectory analysis based on the semiclassical three-step mechanism.

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“…Before the time evolution of the wave function, an initial state is prepared. For the symmetric diatomic molecules, the ground state (electronic 1 sσ state and υ = 0 state) is chosen to be the initial state of the system and is obtained by propagating the field-free Schrödinger equation in imaginary time 38 39 . For the asymmetric diatomic molecule, the lowest bound state is the first excited 2 pσ electronic state.…”

Section: Methodsmentioning

confidence: 99%

Correlated electron-nuclear dynamics in above-threshold multiphoton ionization of asymmetric molecule

Wang

Zhou

et al. 2017

Sci Rep

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The partition of the photon energy into the subsystems of molecules determines many photon-induced chemical and physical dynamics in laser-molecule interactions. The electron-nuclear energy sharing from multiphoton ionization of molecules has been used to uncover the correlated dynamics of the electron and fragments. However, most previous studies focus on symmetric molecules. Here we study the electron-nuclear energy sharing in strong-field photoionization of HeH2+ by solving the one-dimensional time-dependent Schrödinger equation (TDSE). Compared with symmetric molecules, the joint electron-nuclear energy spectrum (JES) of HeH2+ reveals an anomalous energy shift at certain nuclear energies, while it disappears at higher and lower nuclear energies. Through tracing the time evolution of the wavepacket of bound states, we identify that this energy shift originates from the joint effect of the Stark shift, associated with the permanent dipole, and the Autler-Townes effect due to the coupling of the 2pσ and 2sσ states in strong fields. The energy shift in the JES appears at certain nuclear distances only when both Stark effect and Autler-Townes effect play important roles. We further demonstrate that the electron-nuclei energy sharing can be controlled by varying laser intensity for asymmetric molecules, providing alternative approaches to manipulate photochemical reactions for more complex molecules.

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Molecular high-order-harmonic generation due to the recollision mechanism by a circularly polarized laser pulse

Cited by 36 publications

References 59 publications

Helicity reversion in high-order-harmonic generation driven by bichromatic counter-rotating circularly polarized laser fields

Helicity reversion in high-order-harmonic generation driven by bichromatic counter-rotating circularly polarized laser fields

High harmonic generation from axial chiral molecules

Correlated electron-nuclear dynamics in above-threshold multiphoton ionization of asymmetric molecule

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