In:
The Journal of Chemical Physics, AIP Publishing, Vol. 142, No. 5 ( 2015-02-07)
Abstract:
For an open, time-dependent quantum system, Lindblad derived the most general modification of the quantum Liouville equation in the Markovian approximation that models environmental effects while preserving the non-negativity of the system’s density matrix. While Lindblad’s modification is correct for N-electron density matrices, solution of the Liouville equation with a Lindblad operator causes the one-electron reduced density matrix (1-RDM) to violate the Pauli exclusion principle. Consequently, after a short time, the 1-RDM is not representable by an ensemble N-electron density matrix (not ensemble N-representable). In this communication, we derive the necessary and sufficient constraints on the Lindbladian matrix within the Lindblad operator to ensure that the 1-RDM remains N-representable for all time. The theory is illustrated by considering the relaxation of an excitation in several molecules F2, N2, CO, and BeH2 subject to environmental noise.
Type of Medium:
Online Resource
ISSN:
0021-9606
,
1089-7690
Language:
English
Publisher:
AIP Publishing
Publication Date:
2015
detail.hit.zdb_id:
3113-6
detail.hit.zdb_id:
1473050-9
Bookmarklink