ABSTRACT
Pump-dependent photoluminescence imaging and second-order photon correlation studies have been performed on individual single-walled carbon nanotubes (SWCNTs) at room temperature. These studies enable the extraction of both the exciton diffusion constant and the Auger recombination coefficient. A linear correlation between these parameters is attributed to the effect of environmental disorder in setting the exciton mean free path and capture-limited Auger recombination at this length scale. A suppression of photon antibunching is attributed to the creation of multiple spatially nonoverlapping excitons in SWCNTs, whose diffusion length is shorter than the laser spot size. We conclude that complete antibunching at room temperature requires an enhancement of the exciton-exciton annihilation rate that may become realizable in SWCNTs allowing for strong exciton localization.
ABSTRACT
Composite quasi-particles with emergent functionalities in spintronic and quantum information science can be realized in correlated materials due to entangled charge, spin, orbital, and lattice degrees of freedom. Here we show that by reducing the lateral dimension of correlated antiferromagnet NiPS3 flakes to tens of nanometers and thickness to less than ten nanometers, we can switch-off the bulk spin-orbit entangled exciton in the near-infrared (1.47 eV) and activate visible-range (1.8-2.2 eV) transitions. These ultra-sharp lines (<120 µeV at 4.2 K) share the spin-correlated nature of the bulk exciton by displaying a strong linear polarization below Néel temperature. Furthermore, exciton photoluminescence lineshape analysis indicates a polaronic character VIA coupling with at-least 3 phonon modes and a comb-like Stark effect through discretization of charges in each layer. These findings augment the knowledge on the many-body nature of excitonic quasi-particles in correlated antiferromagnets and also establish the nanoscale correlated antiferromagnets as a promising platform for integrated magneto-optic devices.
ABSTRACT
Nongeminate charge recombination occurs over a broad range of time scales in polymer solar cells and represents a serious loss channel for the performance and lifetime of devices. Multiple factors influence this process, including changes in morphology and formation of permanent defects, but individual contributions are often difficult to resolve from conventional experiments. We use intensity modulated photocurrent/photovoltage spectroscopy (IMPS/IMVS) to investigate nongeminate charge recombination in blends of poly[2,6-(4,4-bis-(2-ethylhexyl)-4 H-cyclopenta [2,1- b;3,4- b']dithiophene)- alt-4,7(2,1,3-benzothiadiazole)] (PCPDTBT) and [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) solar cells. PCPDTBT/PCBM devices are exposed to varying doses of UV light resonant with PCBM to induce small perturbations in the thin film morphology, namely local heating. IMPS/IMVS sweeps display signatures unique to degradation, that is, photocurrent and photovoltage leading the excitation light modulation appearing as positive phase shifts or 1st quadrant features in Bode and Nyquist representations, respectively. We assign this component to interface charging at purified PCPDTBT/PCBM phase boundaries that trap mobile charges and facilitate nongeminate recombination. Time- and frequency-domain drift-diffusion simulations are then used to model the perturbed photocurrent responses that show good agreement with experiments. Trap occupancies and their impact of photocurrent production are investigated using variable background (dc) excitation light intensities revealing increases of the 1st quadrant component in devices irradiated for longer times. No evidence of chemical degradation was observed from molecular spectroscopy and imaging experiments, and we conclude that morphological changes are chiefly responsible for larger nongeminate charge recombination yields as devices age. Lastly, we propose that the 1st quadrant IMPS/IMVS is a universal signature of morphology-related degradation, although its relative contribution may vary between material systems.
ABSTRACT
We report on a general theoretical approach to study exciton transport and emission in a single-walled carbon nanotube (SWNT) in the presence of a localized surface-plasmon (SP) mode within a metal nanoparticle interacting via near-field coupling. We derive a set of quantum mechanical equations of motion and approximate rate equations that account for the exciton, SP, and the environmental degrees of freedom. The material equations are complemented by an expression for the radiated power that depends on the exciton and SP populations and coherences, allowing for an examination of the angular distribution of the emitted radiation that would be measured in experiment. Numerical simulations for a (6,5) SWNT and cone-shaped Ag metal tip (MT) have been performed using this methodology. Comparison with physical parameters shows that the near-field interaction between the exciton-SP occurs in a weak coupling regime, with the diffusion processes being much faster than the exciton-SP population exchange. In such a case, the effect of the exciton population transfer to the MT with its subsequent dissipation (i.e., the Förster energy transfer) is to modify the exciton steady state distribution while reducing the equilibration time for excitons to reach a steady sate distribution. We find that the radiation distribution is dominated by SP emission for a SWNT-MT separation of a few tens of nanometers due to the fast SP emission rate, whereas the exciton-SP coherences can cause its rotation.