Tuning the g-factor of neutral and charged excitons confined to self-assembled (Al,Ga)As shell quantum dots

We study the neutral exciton (X) and charged exciton (CX) transitions from (Al,Ga) As shell quantum dots located in core-shell nanowires, in the presence of a magnetic field. The g-factors and the diamagnetic coefficients of both the X and the CX depend on the orientation of the field with respect to the nanowire axis. The aspect ratio of the X wavefunction is quantified based on the anisotropy of the diamagnetic coefficient. For specific orientations of the magnetic field, it is possible to cancel the g-factor of the bright states of the X and the CX by means of an inversion of the sign of the hole's g-factor, which is promising for quantum information processing applications. (C) 2014 AIP Publishing LLC.

Nanoparticle sensitisation of solid-state nanocrystalline solar cell

Robert Plass

Over the past fifteen years dye-sensitised nanocrystalline solar cells have been the subject of intense research and development efforts. These systems provide a technically and economically credible alternative to classical p-n junction solar cells, reaching over 10 % certified efficiency under standard solar illumination conditions (AM 1.5, 1000 W/m2). Recently, the liquid electrolyte, commonly used in these dye-sensitised solar cells, could successfully be replaced by a novel solid hole-conducting material (spiro-OMeTAD). The absence of volatile solvents and corrosive components like iodine presents a clear advantage of these solid-state devices over their photoelectrochemical counterparts. Yet, their maximum overall efficiency of about 3 % clearly lacks behind the performance features of classical dye-sensitized solar cells. The objective of this work is the replacement of the usually used sensitiser (transition metal complexes and organic dyes) by quantum-dots. It was motivated by the possibility to achieve panchromatic light absorption due to the size-dependent properties of the quantum-dots. Some studies have been published using quantum-dots of inorganic low-bandgap semiconductors as sensitisers for mesoporous wide bandgap semiconductor electrodes in conjunction with liquid electrolytes. These systems often suffer from corrosion and photo-corrosion mainly due to the aggressive nature of the electrolyte employed. Solid-state organic-inorganic heterojunctions might provide the desired environment for quantum-dot sensitisation, as the environment is much less aggressive. A large variety of inorganic quantum-dot materials like PbS, CdS, PbSe and CdSe were scrutinized for their use as sensitisers. All particles were synthesised in situ on the TiO2 surface using two different techniques: dip-coating and chemical bath deposition. Lead sulphide was the most investigated due to its superior photovoltaic characteristics. High Resolution Transmission Electron Microscopy (HRTEM) of PbS sensitised TiO2 electrodes fabricated via dip-coating clearly showed the distinct particles on the surface of the semiconductor. The electron transfer dynamics following optical excitation of quantum-dot sensitized TiO2/spiro-OMeTAD heterojunctions were thoroughly studied. Fluorescence spectroscopy was used to prove the possible electron injection from the PbS into the TiO2. Nanosecond laser spectroscopy was applied to monitor the interfacial recombination of the injected electron and the oxidised hole-conductor. Femtosecond laser spectroscopy allowed measuring the ultra-fast kinetics in the system, including electron trapping, exciton recombination and PbS regeneration. An overall efficiency of 0.5 % at 0.1 sun (AM 1.5) has been reached with such systems. Chemical bath deposition (CBD) of PbS leads to the formation of a layer rather than distinct particles on the TiO2. Solar cells fabricated via CBD exhibited open-circuit voltages which were generally 100 mV higher then those of comparable devices made via dip-coating. The PbS layer acts as blocking layer, hindering the contact between TiO2 and the hole-conductor. This technique allowed achieving devices highly linear with respect to the illumination power. Different strategies were pursued to impede interfacial recombination, among which the introduction of self-assembled monolayers at the interface between the organic and inorganic phases was proven to be the most efficient. Nanosecond laser spectroscopy showed a strong decrease of the interfacial recombination kinetic rates in the presence of hexadecylmalonic acid or decylphosphonic acid monolayers. Short-circuit currents could be raised by a factor two to four using such type of molecules. The overall efficiency of the device could be strongly increased, reaching 1 % at 0.1 Sun (AM 1.5). CBD was also used to deposit PbSe and CdSe layers at the surface of TiO2. Fluorescence spectroscopy was used to probe electron injection from CdSe quantum dots to TiO2. Generally it was observed that metal sulfides were more efficient in sensitizing TiO2/OMeTAD heterojunctions then the respective selenides.

EPFL2004

Bandgap engineering in a nanowire: self-assembled 0, 1 and 2D quantum structures

Inherent to the nanowire morphology is the exciting possibility of fabricating materials organized at the nanoscale in three dimensions. Composition and structure can be varied along and across the nanowire, as well as within coaxial shells. This opens up a manifold of possibilities in nanoscale materials science and engineering which is only possible with a nanowire as a starting structure. As the variation in composition and structure is accompanied by a change in the band structure, it is possible to confine carriers within the nanowire. Interestingly, this results in the formation of local two, one and zero-dimensional structures from an electronic point of view within the nanowire. This novel palette of nanostructures paves the way toward novel applications in many engineering domains such as lasers, high-mobility transistors, quantum information and energy harvesting. In the present review we summarize and give an overview on recent achievements in the design and growth of advanced quantum structures starting from nanowire templates. The quantum structures presented have been grown by molecular beam epitaxy and correspond to different confinement approaches: quantum wells (2D), quantum wires (1D) and quantum dots (0D).

Elsevier2013

Self-assembled quantum dots in a nanowire system for quantum photonics

Marco Cantoni, Sonia Conesa Boj, Yannik Fontana, Martin Heiss, Bernt Ketterer, Nicola Marzari, Eleonora Russo

Quantum dots embedded within nanowires represent one of the most promising technologies for applications in quantum photonics. Whereas the top-down fabrication of such structures remains a technological challenge, their bottom-up fabrication through self-assembly is a potentially more powerful strategy. However, present approaches often yield quantum dots with large optical linewidths, making reproducibility of their physical properties difficult. We present a versatile quantum-dot-innanowire system that reproducibly self-assembles in core-shell GaAs/AlGaAs nanowires. The quantum dots form at the apex of a GaAs/AlGaAs interface, are highly stable, and can be positioned with nanometre precision relative to the nanowire centre. Unusually, their emission is blue-shifted relative to the lowest energy continuum states of the GaAs core. Large-scale electronic structure calculations show that the origin of the optical transitions lies in quantum confinement due to Al-rich barriers. By emitting in the red and self-assembling on silicon substrates, these quantum dots could therefore become building blocks for solid-state lighting devices and third-generation solar cells.

Nature Publishing Group2013

Nanoparticle sensitisation of solid-state nanocrystalline solar cell

Robert Plass

EPFL2004