No Arabic abstract
We report measurements of the attenuation of a beam of orthoexciton-polaritons by a photoionizing optical probe. Excitons were prepared in a narrow resonance by two photon absorption of a 1.016 eV, 54 ps pulsed light source in cuprous oxide (Cu2O) at 1.4 K. A collinear, 1.165 eV, 54 ps probe delayed by 119 ps was used to measure the photoionization cross section of the excitons. Two photon absorption is quadratic with respect to the intensity of the pump and leads to polariton formation. Ionization is linear with respect to the intensity of the probe. Subsequent carrier recombination is quadratic with respect to the intenisty of the probe, and is distinguished because it shifts the exciton momentum away from the polariton anticrossing; the photoionizing probe leads to a rise in phonon-linked luminescence in addition to the attenuation of polaritons. The evolution of the exciton density was determined by variably delaying the probe pulse. Using the probe irradiance and the reduction in the transmitted polariton light, a cross section of 3.9*10^(-22) m^2 was deduced for the probe frequency.
High-lying Rydberg states of Mott-Wannier excitons are receiving considerable interest due to the possibility of adding long-range interactions to the physics of exciton-polaritons. Here, we study Rydberg excitation in bulk synthetic cuprous oxide grown by the optical float zone technique and compare the result with natural samples. X-ray characterization confirms both materials are mostly single crystal, and mid-infrared transmission spectroscopy revealed little difference between synthetic and natural material. The synthetic samples show principal quantum numbers up to $n=10$, exhibit additional absorption lines, plus enhanced spatial broadening and spatial inhomogeneity. Room temperature and cryogenic photoluminescence measurements reveal a significant excess of copper vacancies in the synthetic material. These measurements provide a route towards achieving mbox{high-$n$} excitons in synthetic crystals, opening a route to scalable quantum devices.
The various decay mechanisms of excitons in cuprous oxide (Cu2O) are highly sensitive to defects which can relax selection rules. Here we report cryogenic hyperspectral imaging of exciton luminescence from cuprous oxide crystals grown via the floating zone method showing the samples have few defects. Some locations, however, show strain splitting of the 1s orthoexciton triplet polariton luminescence. Strain is reduced by annealing. In addition, annealing causes annihilation of oxygen and copper vacancies, which leads to a negative correlation between luminescence of unlike vacancies.
Excitons with a radius of a few lattice constants can be affected by strong central-cell corrections, leading to significant deviations of the optical spectrum from the hydrogen-like Rydberg series, and also to an enhancement of the exciton mass. We present an approach to this situation based on a lattice model that incorporates the effects of a non-parabolic band structure, short distance corrections to the Coulomb interaction between electrons and holes, spin-orbit and exchange coupling. The lattice model allows for observation of the crossover from large radius Wannier to small radius Frenkel excitons without invoking a continuum approximation. We apply the lattice model approach especially to the yellow exciton series in the cuprous oxide, for which the optical spectrum and exciton mass enhancement are obtained through adaptation of only a few model parameters to material-specific values. Our results predict a strongly anisotropic ortho-exciton mass.
The electronic transport through Au-(Cu$_{2}$O)$_n$-Au junctions is investigated using first-principles calculations and the nonequilibrium Greens function method. The effect of varying the thickness (i.e., $n$) is studied as well as that of point defects and anion substitution. For all Cu$_{2}$O thicknesses the conductance is more enhanced by bulk-like (in contrast to near-interface) defects, with the exception of O vacancies and Cl substitutional defects. A similar transmission behavior results from Cu deficiency and N substitution, as well as from Cl substitution and N interstitials for thick Cu$_{2}$O junctions. In agreement with recent experimental observations, it is found that N and Cl doping enhances the conductance. A Frenkel defect, i.e., a superposition of an O interstitial and O substitutional defect, leads to a remarkably high conductance. From the analysis of the defect formation energies, Cu vacancies are found to be particularly stable, in agreement with earlier experimental and theoretical work.
Phonons are produced when an excited vacancy in cuprous oxide (Cu$_2$O) relaxes. Time resolved luminescence was used to find the excited copper vacancy (acceptor) and oxygen vacancy (donor) trap levels and lifetimes. It was also used to determine the typical energy and number of phonons in the phonon pulses emitted by vacancies. The vacancy properties of cuprous oxide are controlled by several synthesis parameters and by the temperature. We directly demonstrate the absorption of light by oxygen vacancies with transient absorption. Copper and oxygen vacancies behave differently, in part because the two kinds of traps capture carriers from different states. For example, the copper vacancy luminescence lifetime is around 25 times greater at low temperature. However, both kinds of vacancy luminescence are consistent with a Poissonian multiple phonon emission model.