Abstract
We theoretically study the nonadiabatic relaxation dynamics of low-lying singlet excited-states of semisaturated planar tetracoordinated carbon molecule, C7H4. This molecule possesses a stable C2v ground-state equilibrium geometry. The three low-lying singlet states, S1, S2 and S3, lie in the energy gap of about 1.2 eV. The potential energy surfaces constructed within the quadratic vibronic coupling formalism reveal multiple conical intersections in the Franck-Condon region. Upon photoexcitation to S3, the wavepacket decays rapidly to lower states via these conical intersections. We also observe the wavepacket transfer to S3 during the initial wavepacket evolution on lower states, suggesting the nonadiabatic behavior of photoexcited planar C7H4.
Highlights
The ongoing research in planar tetracoordinated carbon for over five decades has opened a new era in the chemistry of carbon
We focus on elucidating the excited-state dynamics of the semisaturated planar tetracoordinated carbon (ptC), C7H4, using combined electronic structure computations and quantum dynamics simulations
As these states lie within this energy gap, one would expect the molecule to follow nonadiabatic behavior upon photoexcitation
Summary
The ongoing research in planar tetracoordinated carbon (ptC) for over five decades has opened a new era in the chemistry of carbon. Molecules containing ptC or even higher coordination have been successfully suggested and synthesized. The deviation from the long-established concept of tetrahedral tetracoordinate carbon by van’t Hoff [1] and Le Bel [2] has raised the curiosity of researchers. Designing systems containing a planar tetracoordinated carbon center has remained a challenging task. The concept of ptC was first introduced by Monkhorst in 1968 [3]. Using a planar methane model, Hoffmann and coworkers proposed strategies for stabilizing planar tetracoordinated carbon arrangements by electronic effects as well as steric effects [4,5]
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