Terahertz driven intraband dynamics of excitons in nanorods

Abstract

Quantum dots and nanorods are becoming increasingly important structures due to their potential applications that range from photovoltaic devices to medicine. The majority of the research on carrier dynamics in these structures has been in the optical regime, with little work performed at Terahertz frequencies where excitonic dynamics can be more directly probed. In this work, we examine theoretically the interaction of Terahertz radiation with colloidal CdSe nanorods to determine the dynamics of excitons generated via a short optical pulse. We calculate the energies and wavefunctions for the excitons within the envelope function approximation in the low density limit where there is at most one exciton per nanorod. The linear Terahertz transmittance and absorbance is found for nanorods that are approximately 70 nm in length and 7 nm in diameter and are compared with experimental results that have shown the first observation of intra-excitonic transitions in nanorods. We find absorbance peaks at 8.5 THz and 11 THz that result from polarizations in the longitudinal (rod axis) and transverse directions respectively. Our theoretical results show that the 8.5 THz and 11 Thz peaks are due to 1s-2pz and 1s-2px transitions respectively. The theoretical absorbance spectra is in good agreement with the experimental one and show that only the ground state is significantly populated 1 ps after optical excitation. This provides strong evidence of rapid trapping of excited holes into the ligand used to passivate the nanorods. A full set of dynamical equations were then constructed from Heisenberg's equation of motion, and were used to model the excitonic correlations as a function of time. Transmittance and absorbance were calculated for different nanorod orientations and electric field strengths in both the linear and nonlinear regime. These results were then averaged over nanorod orientation in order to more accurately reflect experimental conditions. Nonlinearity was found to become significant at peak pulse field strengths of 7 kV/cm and greater. Due to two-photon processes, we predict the 2pz-3dz transition that is not observed in the linear regime will be clearly seen in the nonlinear absorbance spectrum.