Numerical Study of Carrier Multiplication Pathways in Nanocrystalline and Bulk Form of PbSe

Employing the interband exciton scattering model, we have performed a numerical study of the direct photogeneration and population relaxation processes contributing to carrier multiplication (CM) in nanocrystalline and bulk PbSe. We argue that in both cases the impact ionization is the main mechanisms of CM. This explains weak contribution of the direct photogeneration to the total quantum efficiency (QE). Investigated size scaling of QE in NCs and comparison to the bulk limit provide microscopic insight in the experimentally observed trends.Comment: 4 pages, 3 figures (revised version) Accepted for publication in Physical Review Letter

Degenerate parametric down-conversion facilitated by exciton-plasmon polariton states in nonlinear plasmonic cavity

We study the effect of degenerate parametric down-conversion (DPDC) in an ensemble of two-level quantum emitters (QEs) coupled via near-field interactions to a single surface plasmon (SP) mode of a nonlinear plasmonic cavity. For this purpose, we develop a quantum driven-dissipative model capturing non-equilibrium dynamics of the system in which incoherently pumped QEs have transition frequency tuned near the second-harmonic response of the SPs. Considering the strong coupling regime, i.e., the SP-QE interaction rate exceeds system dissipation rates, we find a critical SP-QE coupling attributed to the phase transition between normal and lasing steady states. Examining fluctuations above the system's steady states, we predict new elementary excitations, namely, the exciton-plasmon polaritons formed by the two-SP quanta and single-exciton states of QEs. The contribution of two-SP quanta results in the linear scaling of the SP-QE interaction rate with the number of QEs, ${\cal N}_o$, as opposed to the $\sqrt{{\cal N}_o}$-scaling known for the Dicke and Tavis-Cummings models. We further examine how SP-QE interaction scaling affects the polariton dispersions and power spectra in the vicinity of the critical coupling. For this purpose, we compare the calculation results assuming a finite ensemble of QEs and the model thermodynamic limit. The calculated power spectra predict an interplay of coherent photon emission by QEs near the second-harmonic frequency and correlated photon-pair emission at the fundamental frequency by the SPs (i.e., the photonic DPDC effect).Comment: 8 pages, 3 figure

Probing dynamical symmetry breaking using quantum-entangled photons

We present an input/output analysis of photon-correlation experiments whereby a quantum mechanically entangled bi-photon state interacts with a material sample placed in one arm of a Hong-Ou-Mandel (HOM) apparatus. We show that the output signal contains detailed information about subsequent entanglement with the microscopic quantum states in the sample. In particular, we apply the method to an ensemble of emitters interacting with a common photon mode within the open-system Dicke Model. Our results indicate considerable dynamical information concerning spontaneous symmetry breaking can be revealed with such an experimental system