Time-resolved photoluminescence (PL) is employed to characterize optical quality of ZnO tetrapods. PL decay of free excitons (FE) is concluded to contain two components with time constants of 1 and 14 ns at room temperature. The fast PL decay is attributed to nonradiative recombination whereas the slow decay is suggested to mainly represent FE radiative lifetime, based on correlation between thermally induced increases in the PL linewidth and FE lifetimes. The results underline superior optical quality of the tetrapods as the decay time of the slow PL component is comparable to the longest lifetimes reported to date for ZnO.

Comprehensive time-resolved photoluminescence measurements are performed on shallow neutral donor bound excitons (D⁰Xs) in bulk ZnO. It is found that transients of the no-phonon D⁰X transitions (I₆-I₉ lines) are largely affected by excitation conditions and change from a bi-exponential decay with characteristic fast (τ_f) and slow (τ_s) time constants under above-bandgap excitation to a single exponential one, determined by τ_s, under two-photon excitation. The slow decay also dominates transients of longitudinal optical phonon-assisted and two-electron-satellite D⁰X transitions, and is attributed to “bulk” D⁰X lifetime. The fast component is tentatively suggested to represent effects of surface recombination.

Temperature dependent photoluminescence and cathodoluminescence (CL) spectroscopies are employed to investigate free exciton (FX) emissions in ZnO tetrapods. The intensity of the no-phonon line is found to be largely suppressed as compared with longitudinal optical phonon assisted transitions, in sharp contrast to bulk ZnO. From spatially resolved CL studies, this suppression is shown to strongly depend on structural morphology of the ZnO tetrapods and becomes most significant within areas with faceted surfaces. A model based on reabsorption due to multiple internal reflections in the vicinity of the FX resonance is suggested to account for the observed effect.

By employing time-of-flight spectroscopy, the group velocity of light propagating through bulk ZnO is demonstrated to dramatically decrease down to 2044 km/s when photon energy approaches the absorption edge of the material. The magnitude of this decrease is found to depend on light polarization. It is concluded that even though the slowdown is observed in the vicinity of donor bound exciton (BX) resonances, the effect is chiefly governed by dispersion of free exciton (FX) polaritons that propagate coherently via ballistic transport. Based on the experimentally determined spectral dependence of the polariton group velocity, the polariton dispersion is accurately determined.

We study the propagation of exciton-polaritons through bulk ZnO using time-resolved photoluminescence (PL) complemented by time-of-flight measurements of laser pulses. When the photon energy approaches donor bound exciton resonances, substantial time delays in PL light propagation are observed which reach up to 210 ps for a 0.55 mm thick crystal. By comparing results from time-of-flight measurements performed using PL light and laser pulses, the observed delay is shown to be due to the formation of exciton-polaritons and their spectral dispersion. It is also shown that the main contribution to the slow-down effect arises from free exciton-polaritons, whereas bound exciton-polaritons become important only in close vicinity to the corresponding resonances.

Time-resolved and magneto-photoluminescence (PL) studies are performed for the so-called I(6)(B) and I(7)(B) excitonic transitions, previously attributed to neutral donor bound excitons involving a hole from the B valence band (VB), D(0)X(B). It is shown that PL decays of these emissions at 2 K are faster than that of their I(6) and I(7) counterparts involving an A VB hole, which is interpreted as being due to energy relaxation of the hole assisted by acoustic phonons. From the magneto-PL measurements, values of effective Lande g factors for conduction electrons and B VB holes are determined as g(e) = 1.91, g(h)(parallel to) = 1.79, and g(h)(perpendicular to) = 0, respectively.

Comprehensive time-resolved photoluminescence and magneto-optical measurements are performed on a bound exciton (BX) line peaking at 3.3621 eV (labeled as I*). Though the energy position of I* lies within the same energy range as that for donor bound exciton (DX) transitions, its behavior in an applied magnetic field is found to be distinctly different from that observed for DXs bound to either ionized or neutral donors. An exciton bound to an isoelectronic center with a hole-attractive local potential is shown to provide a satisfactory model that can account for all experimental results of the I* transition. DOI: 10.1103/PhysRevB.86.235205

Efficient upconversion of photoluminescence from donor-bound excitons is revealed in bulk and nanorod ZnO. Based on excitation power-dependent PL measurements performed with different energies of excitation photons, two-photon absorption (TPA) and two-step TPA (TS-TPA) processes are concluded to be responsible for the upconversion. The TS-TPA process is found to occur via a defect/impurity (or defects/impurities) with an energy level (or levels) lying within 1.14–1.56 eV from one of the band edges, without involving photon recycling. One of the possible defect candidates could be V_Zn. A sharp energy threshold, different from that for the corresponding one-photon absorption, is observed for the TPA process and is explained in terms of selection rules for the involved optical transitions.