Dynamics of strongly degenerate electron-hole plasmas and excitons in single InP nanowires.

Low-temperature time-resolved photoluminescence spectroscopy is used to probe the dynamics of photoexcited carriers in single InP nanowires. At early times after pulsed excitation, the photoluminescence line shape displays a characteristic broadening, consistent with emission from a degenerate, high-density electron-hole plasma. As the electron-hole plasma cools and the carrier density decreases, the emission rapidly converges toward a relatively narrow band consistent with free exciton emission from the InP nanowire. The free excitons in these single InP nanowires exhibit recombination lifetimes closely approaching that measured in a high-quality epilayer, suggesting that in these InP nanowires, electrons and holes are relatively insensitive to surface states. This results in higher quantum efficiencies than other single-nanowire systems as well as significant state-filling and band gap renormalization, which is observed at high electron-hole carrier densities.

Enhanced down conversion of photons emitted by photoexcited Er xY2-xSi2O7 films grown on silicon

Photon cutting with efficiencies up to 400% is demonstrated in Erx Y2-x Si2 O7 films grown on Si and its concentration dependence is analyzed. The cutting is the result of cross-energy-transfer processes occurring within a single rare earth (Er3+) acting as both sensitizer and activator. Similarities with upconversion are revealed and possible applications in solar cells are discussed. © 2010 The American Physical Society.

Nonequilibrium dynamics of photoexcited electrons in graphene: Collinear scattering, Auger processes, and the impact of screening

We present a combined analytical and numerical study of the early stages (sub-100-fs) of the nonequilibrium dynamics of photoexcited electrons in graphene. We employ the semiclassical Boltzmann equation with a collision integral that includes contributions from electron-electron (e-e) and electron-optical phonon interactions. Taking advantage of circular symmetry and employing the massless Dirac fermion (MDF) Hamiltonian, we are able to perform an essentially analytical study of the e-e contribution to the collision integral. This allows us to take particular care of subtle collinear scattering processes - processes in which incoming and outgoing momenta of the scattering particles lie on the same line - including carrier multiplication (CM) and Auger recombination (AR). These processes have a vanishing phase space for two-dimensional MDF bare bands. However, we argue that electron-lifetime effects, seen in experiments based on angle-resolved photoemission spectroscopy, provide a natural pathway to regularize this pathology, yielding a finite contribution due to CM and AR to the Coulomb collision integral. Finally, we discuss in detail the role of physics beyond the Fermi golden rule by including screening in the matrix element of the Coulomb interaction at the level of the random phase approximation (RPA), focusing in particular on the consequences of various approximations including static RPA screening, which maximizes the impact of CM and AR processes, and dynamical RPA screening, which completely suppresses them. © 2013 American Physical Society.

Fabrication of excitonic luminescent inorganic-organic hybrid nano- and microcrystals

Inorganic-organic (IO) hybrid nano- and microcrystals are fabricated by a low-cost, environmentally friendly and easily scaled-up route. Lead(II) iodide (PbI 2) nano/microcrystals are obtained by solvothermal techniques and subsequent IO hybrid (C 12H 25NH 3) 2PbI 4 crystals are produced by intercalation of the organic moiety. The hexagonally shaped crystals obtained range in size from 20 nm to ∼7 μm. Sequential stacking of inorganic/organic layers in these IO hybrid crystals results in strong room-temperature exciton photoluminescence, wherein the excitons are confined within the inorganic sheets. © 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Ultrafast dynamics of exciton formation in semiconductor nanowires.

The dynamics of free electron-hole pairs and excitons in GaAs-AlGaAs-GaAs core-shell-skin nanowires is investigated using femtosecond transient photoluminescence spectroscopy at 10 K. Following nonresonant excitation, a bimolecular interconversion of the initially generated electron-hole plasma into an exciton population is observed. This conducting-to-insulating transition appears to occur gradually over electron-hole charge pair densities of 2-4 × 10(16) cm(-3) . The smoothness of the Mott transition is attributed to the slow carrier-cooling during the bimolecular interconversion of free charge carriers into excitons and to the presence of chemical-potential fluctuations leading to inhomogeneous spectral characteristics. These results demonstrate that high-quality nanowires are model systems for investigating fundamental scientific effects in 1D heterostructures.

Resonant excitation and imaging of nonequilibrium exciton spins in single core-shell GaAs-AlGaAs nanowires.

Nonequilibrium spin distributions in single GaAs/AlGaAs core-shell nanowires are excited using resonant polarized excitation at 10 K. At all excitation energies, we observe strong photoluminescence polarization due to suppressed radiative recombination of excitons with dipoles aligned perpendicular to the nanowire. Excitation resonances are observed at 1- or 2-LO phonon energies above the exciton ground states. Using rate equation modeling, we show that, at the lowest energies, strongly nonequilibrium spin distributions are present and we estimate their spin relaxation rate.

Transient reflectivity on vertically aligned single-wall carbon nanotubes

One-color transient reflectivity measurements are carried out on two different samples of vertically aligned single-wall carbon nanotube bundles and compared with the response recently published on unaligned bundles. The negative sign of the optical response for both samples indicates that the free electron character revealed on unaligned bundles is only due to the intertube interactions favored by the tube bending. Neither the presence of bundles nor the existence of structural defects in aligned bundles is able to induce a free-electron like behavior of the photoexcited carriers. This result is also confirmed by the presence of non-linear excitonic effects in the transient response of the aligned bundles. © 2013 Elsevier B.V.

Structural tunability and switchable exciton emission in inorganic-organic hybrids with mixed halides

Room-temperature tunable excitonic photoluminescence is demonstrated in alloy-tuned layered Inorganic-Organic (IO) hybrids, (C12H 25NH3)2PbI4(1-y)Br4y (y = 0 to 1). These perovskite IO hybrids adopt structures with alternating stacks of low-dimensional inorganic and organic layers, considered to be naturally self-assembled multiple quantum wells. These systems resemble stacked monolayer 2D semiconductors since no interlayer coupling exists. Thin films of IO hybrids exhibit sharp and strong photoluminescence (PL) at room-temperature due to stable excitons formed within the low-dimensional inorganic layers. Systematic variation in the observed exciton PL from 510 nm to 350 nm as the alloy composition is changed, is attributed to the structural readjustment of crystal packing upon increase of the Br content in the Pb-I inorganic network. The energy separation between exciton absorption and PL is attributed to the modified exciton density of states and diffusion of excitons from relatively higher energy states corresponding to bromine rich sites towards the lower energy iodine sites. Apart from compositional fluctuations, these excitons show remarkable reversible flips at temperature-induced phase transitions. All the results are successfully correlated with thermal and structural studies. Such structural engineering flexibility in these hybrids allows selective tuning of desirable exciton properties within suitable operating temperature ranges. Such wide-range PL tunability and reversible exciton switching in these novel IO hybrids paves the way to potential applications in new generation of optoelectronic devices. © 2013 AIP Publishing LLC.

Doping dependence of the Raman spectrum of defected graphene.

We investigate the evolution of the Raman spectrum of defected graphene as a function of doping. Polymer electrolyte gating allows us to move the Fermi level up to 0.7 eV, as directly monitored by in situ Hall-effect measurements. For a given number of defects, we find that the intensities of the D and D' peaks decrease with increasing doping. We assign this to an increased total scattering rate of the photoexcited electrons and holes, due to the doping-dependent strength of electron-electron scattering. We present a general relation between D peak intensity and defects valid for any doping level.