High harmonic generation from axial chiral molecules

Abstract

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.

Investigation of Resonance-Enhanced High-Order Harmonics by Two-Component Laser-Produced Plasmas

“…High-order harmonic generation (HHG) is an extreme nonlinear optical process that promises important applications for generating coherent extreme ultraviolet (XUV) radiation [1][2][3][4][5] and detecting ultrafast dynamics of atomic, molecular, and solid systems [6,7]. However, a major shortcoming, which limits the applicability of HHG, is the low conversion efficiency.…”

Imaging charge-migration in chiral molecules using time-resolved x-ray diffraction

“…X-ray crystallography is the one of the most reliable methods to determine the absolute configuration [16]. In recent years, other methods such as microwave spectroscopy [17,18], coulomb-explosion imaging [19,20], high-harmonic generation [21][22][23][24], vibrational circular dichroism [25,26], and photoelectron circular dichroism [27][28][29][30][31][32][33] were employed to discern enantiomers. Here, we demonstrate that TRXD within pump-probe configuration provides an alternative to probe the handedness of chiral molecules.…”

Optimal Basis Set for Electron Dynamics in Strong Laser Fields: The case of Molecular Ion H2+

“… 22 Within these approaches, schemes have been proposed to compute ATI spectra in molecules 23 and to study the different molecular orbital contributions to HHG spectra. 24 , 25 Grid-based basis sets have demonstrated to be very accurate to describe nonlinear optical phenomena. However, the computational cost can be very high and strategies involving multilevel parallelization schemes have had to be developed.…”