Open-system Renner–Teller dynamics with quantum Brownian motion within a Markovian Caldeira–Leggett limit
An open-system, coordinate-resolved formulation of Renner-Teller (RT) rovibronic dynamics is developed by embedding a two-state RT Hamiltonian in a quantum Brownian motion environment within the high-temperature, Markovian Caldeira-Leggett (CL) master-equation limit. I derive channel-resolved local balance laws for RT wavepacket densities in Jacobi coordinates, in which the Hermitian kinetic operator yields a curvilinear probability-current divergence, the RT off-diagonal blocks generate antisymmetric interchannel source-sink exchange, and the CL dissipator supplies coordinate-wise friction and momentum-diffusion corrections. These contributions are evaluated on a parity-adapted ΩK,M,ΛJ,p basis and used to construct a grid-resolved dominance analysis of the intersurface transfer-layer density for near-linear N2O. Application to the near-linear RT manifold of N2O illustrates how electronically controlled RT driving (through the adiabatic splitting ΔV and mixing angle α12) and bath-mediated dissipation jointly regulate the emergence, transport, reactivation, and late-time spreading of an intersurface transfer-layer density, providing a grid-resolved diagnostic that directly links wavepacket motion to environment-induced relaxation and decoherence.
Authors
- Mohammad Noh Daud (ORCID: https://orcid.org/0000-0001-9380-9340)
Institutions
- University of Malaya (MY)
Publication Details
- Journal
- The Journal of Chemical Physics
- Published
- 2026-04-16
- DOI
- https://doi.org/10.1063/5.0325114
- Primary Topic
- Spectroscopy and Quantum Chemical Studies
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Universiti Malaya