Controlling vibrational excitations in C60 by laser pulse durations.
Two similar off-resonant ultrafast laser experiments in C60 have reported two different vibrational modes that dominate the relaxation process: one predicts the A(g) modes while the other the H(g) modes. A systematical simulation presented here reveals that this experimental discrepancy results from the laser pulse duration. The numerical results show that since each mode nu has a distinctive optimal duration tau(nu)(o), the A(g) modes are strongly suppressed for durations longer than 40 fs, while the H(g) modes start to grow. For the off-resonant and low-intensity excitations, the period Omega(o)(nu) of the dominant mode and tau(nu)(o) satisfy the relation Omega(o)(nu)/tau(nu)(o) approximately 3.4. By carefully scanning the laser frequencies and pulse durations, a comprehensive excitation diagram is constructed, which can be used to guide experiments to selectively excite the A(g) and H(g) modes in C60 by an ultrafast laser. Its potential impact is also discussed.
Zhang
G P
GP
Department of Physics, Indiana State University, Terre Haute, Indiana 47809, USA.
George
Thomas F
TF