Michael E. Turk

We use time-integrated and time-resolved photoluminescence and absorption to characterize the low-temperature optical properties of CdSe quantum dot solids after exchanging native aliphatic ligands for thiocyanate and subsequent thermal annealing. In contrast to trends established at room temperature, our data show that at low temperature the band-edge absorptive bleach is dominated by 1S_3/2h hole occupation in the quantum dot interior. We find that our ligand treatments, which bring enhanced interparticle coupling, lead to faster surface state electron trapping, a greater proportion of surface-related photoluminescence, and decreased band-edge photoluminescence lifetimes.

We study gate-controlled, low-temperature resistance and magnetotransport in indium-doped CdSe quantum dot field effect transistors. We show that using the gate to accumulate electrons in the quantum dot channel increases the “localization product” (localization length times dielectric constant) describing transport at the Fermi level, as expected for Fermi level changes near a mobility edge. Our measurements suggest that the localization length increases to significantly greater than the quantum dot diameter.

We use subpicosecond time-resolved photoluminescence measurements to study the nature of photoluminescence in graphene oxide and reduced graphene oxide. Our data indicate that, in contrast to prior suggestions, the photoluminescence spectra of graphene oxide and reduced graphene oxide are inhomogeneously broadened. We observe substantial energy redistribution and relaxation among the emitting states within the first few picoseconds, leading to a progressive red shift of the emission spectrum. Blue shifts that arise in time-integrated spectra upon photothermal reduction are easily understood within this dynamical context without invoking a modified distribution of dipole-coupled states. Rather, reduction increases the nonradiative electron-hole recombination rate and curtails the red-shifting process, which is consistent with an increase in quenching through the introduction of larger and/or more numerous sp(2) clusters. Polarization memory measurements show energetic signatures of electron-hole correlations, established on a subpicosecond time scale and developing little thereafter.

The manipulation of radiative properties of light emitters coupledwith surface plasmons is important for engineering new nanoscale optoelectronic devices, including lasers, detectorsand single photon emitters^{1,2,3,4,5,6,7,8}. However, so far the radiative rates of excited states in semiconductors and molecular systems have been enhanced only moderately, typically by a factor of 10–50, producing emission mostly from thermalizedexcitons^2,6,9,10,11. Here, we show the generation of dominant hot-exciton emission, that is, luminescence from non-thermalized excitons that are enhanced by the highly concentrated electromagnetic fields supported by the resonant whispering-gallery plasmonic nanocavities of CdS–SiO₂–Ag core–shell nanowire devices. By tuning the plasmonic cavity size to match the whispering-gallery resonances, an almost complete transition from thermalized exciton to hot-exciton emission can be achieved, which reflects exceptionally high radiative rate enhancement of >10³ and sub-picosecond lifetimes. Core–shell plasmonic nanowires are an ideal test bed for studying and controlling strong plasmon–exciton interaction at the nanoscale and opens new avenues for applications in ultrafast nanophotonic devices.