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First-principles investigation of dynamical properties of molecular devices under a steplike pulse

We report a computationally tractable approach to first principles investigation of time-dependent current of molecular devices under a step-like pulse. For molecular devices, all the resonant states below Fermi level contribute to the time-dependent current. Hence calculation beyond wideband limit must be carried out for a quantitative analysis of transient dynamics of molecules devices. Based on the exact non-equilibrium Green's function (NEGF) formalism of calculating the transient current in Ref.\onlinecite{Maciejko}, we develop two approximate schemes going beyond the wideband limit, they are all suitable for first principles calculation using the NEGF combined with density functional theory. Benchmark test has been done by comparing with the exact solution of a single level quantum dot system. Good agreement has been reached for two approximate schemes. As an application, we calculate the transient current using the first approximated formula with opposite voltage $V_L(t)=-V_R(t)$ in two molecular structures: Al-${\rm C}_{5}$-Al and Al-${\rm C}_{60}$-Al. As illustrated in these examples, our formalism can be easily implemented for real molecular devices. Importantly, our new formula has captured the essential physics of dynamical properties of molecular devices and gives the correct steady state current at $t=0$ and $t\rightarrow \infty$.