We report first-principles investigation of time-dependent current of molecular devices under a steplike pulse. Our results show that although the switch-on time of the molecular device is comparable to the transit time, much longer time is needed to reach the steady state. In reaching the steady state the current is dominated by resonant states below Fermi level. The contribution of each resonant state to the current shows the damped oscillatory behavior with frequency approximately equal to half of the bias of steplike pulse and decay rate determined by the life time of the corresponding resonant state. We found that all the resonant states below Fermi level have to be included for accurate results. This indicates that going beyond wideband limit is essential for a quantitative analysis of transient dynamics of molecular devices.

• Received 19 January 2010

DOI:https://doi.org/10.1103/PhysRevB.81.121103