TY - JOUR
T1 - Scoring molecular wires subject to an ultrafast laser pulse for molecular electronic devices
AU - Lu, Hui
AU - Azizi, Alireza
AU - Mi, Xiao Peng
AU - Wenjing, Yu
AU - Peng, Yuting
AU - Xu, Tianlv
AU - Früchtl, Herbert
AU - van Mourik, Tanja
AU - Kirk, Steven R
AU - Jenkins, Samantha
N1 - Funding: The Hunan Natural Science Foundation of China project gratefully acknowledged approval number: 2022JJ30029. The One Hundred Talents Foundation of Hunan Province is also gratefully acknowledged for the support of S.J. and S.R.K. H.F. and T.v.M. gratefully acknowledge computational support via the EaStCHEM Research Computing Facility.
PY - 2023/8/5
Y1 - 2023/8/5
N2 - A nonionizing ultrafast laser pulse of 20-fs duration with a peak amplitude electric-field ±E = 200 × 10−4
a.u. was simulated. It was applied to the ethene molecule to consider
its effect on the electron dynamics, both during the application of the
laser pulse and for up to 100 fs after the pulse was switched off. Four
laser pulse frequencies ω = 0.2692, 0.2808, 0.2830, and 0.2900 a.u. were chosen to correspond to excitation energies mid-way between the (S1,S2), (S2,S3), (S3,S4) and (S4,S5) electronic states, respectively. Scalar quantum theory of atoms in molecules (QTAIM) was used to quantify the shifts of the C1—C2 bond critical points (BCPs). Depending on the frequencies ω selected, the C1—C2 BCP shifts were up to 5.8 times higher after the pulse was switched off compared with a static E-field
with the same magnitude. Next generation QTAIM (NG-QTAIM) was used to
visualize and quantify the directional chemical character. In
particular, polarization effects and bond strengths, in the form of
bond-rigidity vs. bond-flexibility, were found, for some laser pulse
frequencies, to increase after the laser pulse was switched off. Our
analysis demonstrates that NG-QTAIM, in partnership with ultrafast laser
irradiation, is useful as a tool in the emerging field of ultrafast
electron dynamics, which will be essential for the design, and control
of molecular electronic devices.
AB - A nonionizing ultrafast laser pulse of 20-fs duration with a peak amplitude electric-field ±E = 200 × 10−4
a.u. was simulated. It was applied to the ethene molecule to consider
its effect on the electron dynamics, both during the application of the
laser pulse and for up to 100 fs after the pulse was switched off. Four
laser pulse frequencies ω = 0.2692, 0.2808, 0.2830, and 0.2900 a.u. were chosen to correspond to excitation energies mid-way between the (S1,S2), (S2,S3), (S3,S4) and (S4,S5) electronic states, respectively. Scalar quantum theory of atoms in molecules (QTAIM) was used to quantify the shifts of the C1—C2 bond critical points (BCPs). Depending on the frequencies ω selected, the C1—C2 BCP shifts were up to 5.8 times higher after the pulse was switched off compared with a static E-field
with the same magnitude. Next generation QTAIM (NG-QTAIM) was used to
visualize and quantify the directional chemical character. In
particular, polarization effects and bond strengths, in the form of
bond-rigidity vs. bond-flexibility, were found, for some laser pulse
frequencies, to increase after the laser pulse was switched off. Our
analysis demonstrates that NG-QTAIM, in partnership with ultrafast laser
irradiation, is useful as a tool in the emerging field of ultrafast
electron dynamics, which will be essential for the design, and control
of molecular electronic devices.
U2 - 10.1002/jcc.27126
DO - 10.1002/jcc.27126
M3 - Article
C2 - 37133985
SN - 0192-8651
VL - 44
SP - 1776
EP - 1785
JO - Journal of Computational Chemistry
JF - Journal of Computational Chemistry
IS - 21
ER -