Minimum Line Width of Surface Plasmon Resonance in Doped ZnO Nanocrystals

The optical response of ZnO nanocrystals (NCs) doped with Al (Ga) impurities is calculated using a model that incorporates the effects of quantum confinement, dielectric mismatch, surface, and ionized impurity scattering. For dopant concentrations of a few percent, the NC polarizability is dominated by a localized surface plasmon resonance (LSPR) in the infrared (IR) which follows the Drude-Lorentz law for NC diameter above ∼10 nm but is strongly blue-shifted for smaller diameters due to quantum confinement effects. The intrinsic width of the LSPR peak is calculated in order to characterize plasmon losses induced by ionized impurity scattering. Widths below 80 meV are found in the best cases, in agreement with the lowest values recently measured on single NCs. These results confirm that doped ZnO NCs are very promising for the development of IR plasmonics. The width of the LSPR peak strongly increases when dopants are placed near the surface of the NCs or when additional fixed charges are present

Effects of Strain on the Carrier Mobility in Silicon Nanowires

We investigate electron and hole mobilities in strained silicon nanowires (Si NWs) within an atomistic tight-binding framework. We show that the carrier mobilities in Si NWs are very responsive to strain and can be enhanced or reduced by a factor >2 (up to 5×) for moderate strains in the ±2% range. The effects of strain on the transport properties are, however, very dependent on the orientation of the nanowires. Stretched ⟨100⟩ Si NWs are found to be the best compromise for the transport of both electrons and holes in ≈10 nm diameter Si NWs. Our results demonstrate that strain engineering can be used as a very efficient booster for NW technologies and that due care must be given to process-induced strains in NW devices to achieve reproducible performances

Mercury Telluride Colloidal Quantum Dots: Electronic Structure, Size-Dependent Spectra, and Photocurrent Detection up to 12 μm

HgTe colloidal quantum dots are synthesized with high monodispersivity with sizes up to ∼15 nm corresponding to a room temperature absorption edge at ∼5 μm. The shape is tetrahedral for larger sizes and up to five peaks are seen in the absorption spectra with a clear size dependence. The size range of the HgTe quantum dots is extended to ∼20 nm using regrowth. The corresponding room temperature photoluminescence and absorption edge reach into the long-wave infrared, past 8 μm. Upon cooling to liquid nitrogen temperature, a photoconductive response is obtained in the long-wave infrared region up to 12 μm. Configuration-interaction tight-binding calculations successfully explain the spectra and the size dependence. The five optical features can be assigned to sets of single hole to single electron transitions whose strengths are strongly influenced by the multiband/multiorbital character of the quantum-dot electronic states

Size Dependence of the Exciton Transitions in Colloidal CdTe Quantum Dots

In this paper, we present a detailed investigation of the size dependence of the optical transitions of colloidal CdTe QDs ranging in diameter from 2.9 to 14.8 nm. The energy integrated absorption cross section per CdTe unit is investigated in detail for the lowest two exciton transitions (1S_3/2(h)–1S_(e) and 2S_3/2(h)–1S_(e)) and shown to increase with decreasing size, although the size dependence of the 2S_3/2(h)–1S_(e) is less pronounced. The experimental absorption spectra are compared to spectra calculated by using a tight-binding approach. The calculations were carried out with electron–hole configuration interaction (CI) and without (single-particle, SP). The optical absorption spectra calculated by using the CI approach are in excellent agreement with the experiment, as well as the evolution of the optical gap and the optical transitions with nanocrystal size

Nanoscale Carrier Multiplication Mapping in a Si Diode

Carrier multiplication (CM), the creation of electron–hole pairs from an excited electron, has been investigated in a silicon p–n junction by multiple probe scanning tunneling microscopy. The technique enables an unambiguous determination of the quantum yield based on the direct measurement of both electron and hole currents that are generated by hot tunneling electrons. The combined effect of impact ionization, carrier diffusion, and recombination is directly visualized from the spatial mapping of the CM efficiency. Atomically well-ordered areas of the p–n junction surface sustain the highest CM rate, demonstrating the key role of the surface in reaching high yield

Comparative Study on the Localized Surface Plasmon Resonance of Boron- and Phosphorus-Doped Silicon Nanocrystals

Localized surface plasmon resonance (LSPR) of doped Si nanocrystals (NCs) is critical to the development of Si-based plasmonics. We now experimentally show that LSPR can be obtained from both B- and P-doped Si NCs in the mid-infrared region. Both experiments and calculations demonstrate that the Drude model can be used to describe the LSPR of Si NCs if the dielectric screening and carrier effective mass of Si NCs are considered. When the doping levels of B and P are similar, the LSPR energy of B-doped Si NCs is higher than that of P-doped Si NCs because B is more efficiently activated to produce free carriers than P in Si NCs. We find that the plasmonic coupling between Si NCs is effectively blocked by oxide at the NC surface. The LSPR quality factors of B- and P-doped Si NCs approach those of traditional noble metal NCs. We demonstrate that LSPR is an effective means to gain physical insights on the electronic properties of doped Si NCs. The current work on the model semiconductor NCs, <i>i.e.</i>, Si NCs has important implication for the physical understanding and practical use of semiconductor NC plasmonics

Asymmetric Optical Transitions Determine the Onset of Carrier Multiplication in Lead Chalcogenide Quantum Confined and Bulk Crystals

Carrier multiplication is a process in which one absorbed photon excites two or more electrons. This is of great promise to increase the efficiency of photovoltaic devices. Until now, the factors that determine the onset energy of carrier multiplication have not been convincingly explained. We show experimentally that the onset of carrier multiplication in lead chalcogenide quantum confined and bulk crystals is due to asymmetric optical transitions. In such transitions most of the photon energy in excess of the band gap is given to either the hole or the electron. The results are confirmed and explained by theoretical tight-binding calculations of the competition between impact ionization and carrier cooling. These results are a large step forward in understanding carrier multiplication and allow for a screening of materials with an onset of carrier multiplication close to twice the band gap energy. Such materials are of great interest for development of highly efficient photovoltaic devices

Crystal Facet Engineering in Ga-Doped ZnO Nanowires for Mid-Infrared Plasmonics

The metal–organic chemical vapor deposition growth of various Ga-doped ZnO nanostructures for plasmonics is investigated, with a particular focus on the nanowire facet transformations induced by the addition of trimethylgallium in the gas phase. For nonintentionally doped spontaneous ZnO nanowires, the aspect ratio is strongly decreased due to residual Ga in the reactor, and the shape evolves rapidly toward Christmas-tree-like and hierarchical structures upon intentional Ga doping. Regarding ZnO/ZnO:Ga core–shell structures, a change of the smooth initial M-oriented facets occurs, with the development of {202̅1} surfaces, and further {101̅1} and {0001} surfaces. Interestingly, a similar evolution of the lateral roughness is observed in Au-catalyzed doped nanowires. High concentrations of Ga in the grown nanostructures are revealed by photoluminescence and confirmed by Rutherford backscattering spectrometry. First photoacoustic measurements show an optical absorption at 6 μm, evidencing that the degenerated material is suitable for plasmonics applications in the infrared range. The influence of Ga doping on the facet transformations and the occurrence of unexpected {0001} polar surfaces are discussed. The results can be mainly understood by a Ga surfactant effect (at least partial) responsible for the modification of the surface energies and kinetics. Density functional calculations support the floating behavior of the negatively charged Ga^– ion on the growing surface

Broadband and Picosecond Intraband Absorption in Lead-Based Colloidal Quantum Dots

Using femtosecond transient absorption spectroscopy, we demonstrate that lead chalcogenide nanocrystals show considerable photoinduced absorption (PA) in a broad wavelength range just below the band gap. The time-dependent decay of the PA signal correlates with the recovery of the band gap absorption, indicating that the same carriers are involved. On this basis, we assign this PA signal to intraband absorption, that is, the excitation of photogenerated carriers from the bottom of the conduction band or the top of the valence band to higher energy levels in the conduction and valence band continuum. We confirm our experiments with tight-binding calculations. This broadband response in the commercially interesting near- to mid-infrared range is very relevant for ultra-high-speed all-optical signal processing. We benchmark the performance with bulk Si and Si nanocrystals