Coherence revival during the attosecond electronic and nuclear quantum photodynamics of the ozone molecule

A coherent superposition of two electronic states of ozone (ground and Hartley $B$) is prepared with a UV pump pulse. Using the multiconfiguration time-dependent Hartree approach, we calculate the subsequent time evolution of the two corresponding nuclear wave packets and the coherence between them. The resulting wave packet shows an oscillation between the two chemical bonds. Even more interesting, the coherence between the two electronics states reappears after the laser pulse is switched off, which could be observed experimentally with an attosecond probe pulse.

Figure 1

Potential energy surfaces of ozone as functions of the dissociation coordinate: ground state ($X$; solid line) and Hartley state ($B$; dashed line). The arrow denotes excitation of the $B$ state. The other two coordinates are fixed at $R_2=2.43$ a.u. and the bond angle is $\theta ={117}^{\circ }$.

Figure 2

Top: Applied electric field. Bottom: Time evolution of the diabatic populations in the ground ($X$) and diabatic excited ($B$) states.

Figure 3

Relative electronic coherence as a function of time. The real part, the imaginary part, and the absolute value of the relative electronic coherence between the ground ($X$) and the Hartley ($B$) states.

Figure 4

Snapshots of the time evolution of the nuclear wave-packet density along both O-O bonds (a.u.).

Figure 5

Local population density for state $B$ [solid (black) curve] and real part of the interference (last) term in Eq. (15) [dashed (green) curve] at the FC point as functions of time.

Figure 6

Time evolution of the excited differential electronic charge density, Eq. (15), at the FC geometry (side view). Dark (blue) area, hole; light (yellow) area, electron.