Direct observation of geometric-phase interference in dynamics around a conical intersection

On the Nature of Geometric and Topological Phases in the Presence of Conical Intersections

“…We believe that our findings are general and not restricted to the model system studied here. These findings can be seen as an indication, in addition to previous theoretical formulations 23,24 as well as recent experimental results, 13 that topological phases cannot be observed in molecular processes in the presence of CIs; only dynamics-induced geometric phases can.…”

“…It is important to notice that the observation of a non-negligible population along X > 0, Y = 0 is not an artifact of the initial condition we used, which is slightly different from those used in ref . To demonstrate this numerically, we report in Figure SI2 an analysis similar to that in Figure but for a system in which the dynamics is initialized from the minimum of the electronic ground state [centered at R 0 = (−1.5, 0)].…”

“…In the domain of physical chemistry, recent years have witnessed growing efforts devoted to demonstrating experimentally the effect of geometric phases on the behavior of molecules. − The concept of geometric phases is general and has emerged in many aspects of physical chemistry − and physics, , e.g., as a demonstration of the nonlocal nature of quantum mechanics, in molecular reactions, ,,− in condensed matter physics, − and in optics. , …”

“…The electron–nuclear dynamics of interest in this work is initiated in the ground state of a Jahn–Teller model, which has been extensively studied with respect to geometric phase effects in the past. − We use the E ⊗ e Jahn–Teller Hamiltonian recently explored by Valahu et al (details in section SI1 of the Supporting Information). The experimental setup of ref consists of a mixed-qudit-boson encoding in which both electronic and motional degrees of freedom are described. The physical system is a confined 171 Yb + ion where the vibrations are represented by the ion transverse vibrational modes while the electronic states are the two hyperfine levels of the 2 S 1/2 ground state.…”

“…The physical system is a confined 171 Yb + ion where the vibrations are represented by the ion transverse vibrational modes while the electronic states are the two hyperfine levels of the 2 S 1/2 ground state. Therefore, in the following, the nuclear coordinates R = ( X , Y ) will indicate the two dimensionless vibrational coordinates, and the dynamics will be observed on a time scale of 2 ms, as in ref . The PESs in the adiabatic representation, i.e., the eigenvalues of Ĥ el with R = ( X , Y ), are depicted in Figure .…”