Chirality reversal with the carrier-envelope phase: A next generation QTAIM interpretation

• Published in: Chemical physics letters 2024-08, Vol.848, p.141391, Article 141391
• Main Authors: Zhou, Xinjie, He, Huan, Hong, Genwei, Peng Mi, Xiao, Xu, Tianlv, Früchtl, Herbert, van Mourik, Tanja, Paterson, Martin J., Kirk, Steven R., Jenkins, Samantha
• Format: Article
• Language: English
• ISSN: 0009-2614; 1873-4448
• DOI: 10.1016/j.cplett.2024.141391

Left. The ethane C1-C2 BCP Hessian of ρ(r) eigenvector-following trajectories TF(s) for the right-handed, clockwise (CW[+1]) and left-handed, counter-clockwise (CCW[-1]) circularly polarized laser pulses of duration 10 fs for the carrier-envelope phase (CEP) angle ϕ = 0.0° corresponding to the electric field E = 200.0 x 10−4 a.u., see the main text for further explanation. The start and end of each TF(s) are denoted by balls and cubes respectively and are surrounded by an ellipse. Inset. The corresponding variation of the ethane C1-C2 BCP ellipticity ε, notice the position of the green arrow on the x-axis. Right. The corresponding ethane C1-C2 BCP TF(s) for the CEP angle ϕ = 180.0°. Notice the changed position of the black ellipse relative to the left figure. Inset. The corresponding variation of the ethane C1-C2 BCP ellipticity ε, notice that the green arrow on the x-axis has moved leftwards relative to that of the left inset. [Display omitted] •Left and right circularly polarized ultrafast laser pulses are applied to ethane.•The carrier-envelope phase (CEP) angle ϕ controlled the wavefunction ψ(r) evolution.•NG-QTAIM is used to quantify the effect of variation of the CEP angle ϕ.•The NG-QTAIM chirality assignments were found to be reversed from S to R.•A one-to-one mapping between the CEP angle ϕ and NG-QTAIM trajectories was discovered. Simulated circularly-polarized 10 fs laser pulses that induce a mixture of excited states are applied to ethane. Additionally, the carrier-envelope phase (CEP) angle ϕ, that quantifies the relationship between the time-varying direction of electric (E)-field and the amplitude envelope was used to manipulate the mechanical and chiral properties of ethane using Next Generation Quantum Theory of Atoms in Molecules (NG-QTAIM). The chirality assignments were reversed from S to R as the CEP angle ϕ was increased from ϕ = 0.0° to ϕ = 180°. A one-to-one mapping between the CEP angle ϕ and NG-QTAIM trajectories was discovered.