The Journal of Chemical Physics
T 2 can be greater than 2T1 even at finite temperature
Brian B. Laird, James L. Skinner
Abstract
The relaxation of a nondegenerate two-level quantum system linearly and off-diagonally coupled to a thermal bath of quantum-mechanical harmonic oscillators is studied. The population and phase relaxation times, T1 and T2, are calculated to fourth order in the system/bath interaction. Focus is on a specific model of the bath spectral density that is both Ohmic (proportional to frequency at low frequency) and Lorentzian, and which has the property that, in the semiclassical or high-temperature limit, it reproduces the stochastic model studied previously by Budimir and Skinner [J. Stat. Phys. 49, 1029 (1987)]. For this fully quantum-mechanical model, it is found that under certain conditions the standard inequality, T2≤2T1, is violated, demonstrating that this unusual result, which was originally derived from the (infinite-temperature) stochastic model, is valid at finite temperature as well.