Efficient luminescent solar concentrators based on self-absorption free, Tm2+ doped halides

The optical and luminescence properties of CaI2 and NaCl doped with divalent thulium are reported for solar energy applications. These halides strongly absorb solar light from the UV up to 900 nm due to the intense Tm2+ 4f13→4f125d1 electronic transitions. Absorption is followed by emission of 1140 nm light due to the 2F5/2→2F7/2 transition of the 4f13 configuration that can be efficiently converted to electric power by thin film CuInSe2 (CIS) solar cells. Because of a negligible spectral overlap between absorption and emission spectra, a luminescent solar concentrator (LSC) based on these black luminescent materials would not suffer from self-absorption losses. The Tm2+ doped halides may therefore lead to efficient semi-transparent power generating windows that absorb solar light over the whole visible spectrum. It will be shown that the power efficiency of the Tm2+ based LSCs can be up to four times higher compared to LSCs based on organic dyes or quantum dots.

Room temperature absorption in laterally biased Quantum Infrared Detectors fabricated by MBE regrowth

In this paper, we show room temperature operation of a quantum well infrared photodetector (QWIP) using lateral conduction through ohmic contacts deposited at both sides of two n-doped quantum wells. To reduce the dark current due to direct conduction in the wells, we apply an electric field between the quantum wells and two pinch-off Schottky gates, in a fashion similar to a field effect device. Since the normal incidence absorption is strongly reduced in intersubband transitions in quantum wells, we first analyze the response of a detector based on quantum dots (QD). This QD device shows photocurrent signal up to 150 K when it is processed in conventional vertical detector. However, it is possible to observe room temperature signal when it is processed in a lateral structure. Finally, the room temperature photoresponse of the QWIP is demonstrated, and compared with theory. An excellent agreement between the estimated and measured characteristics of the device is found

Integrated luminescent chemical microsensors based on GaN LEDs for security applications using smartphones

Development of PCB-integrateable microsensors for monitoring chemical species is a goal in areas such as lab-on-a-chip analytical devices, diagnostics medicine and electronics for hand-held instruments where the device size is a major issue. Cellular phones have pervaded the world inhabitants and their usefulness has dramatically increased with the introduction of smartphones due to a combination of amazing processing power in a confined space, geolocalization and manifold telecommunication features. Therefore, a number of physical and chemical sensors that add value to the terminal for health monitoring, personal safety (at home, at work) and, eventually, national security have started to be developed, capitalizing also on the huge number of circulating cell phones. The chemical sensor-enabled “super” smartphone provides a unique (bio)sensing platform for monitoring airborne or waterborne hazardous chemicals or microorganisms for both single user and crowdsourcing security applications. Some of the latest ones are illustrated by a few examples. Moreover, we have recently achieved for the first time (covalent) functionalization of p- and n-GaN semiconductor surfaces with tuneable luminescent indicator dyes of the Ru-polypyridyl family, as a key step in the development of innovative microsensors for smartphone applications. Chemical “sensoring” of GaN-based blue LED chips with those indicators has also been achieved by plasma treatment of their surface, and the micrometer-sized devices have been tested to monitor O2 in the gas phase to show their full functionality. Novel strategies to enhance the sensor sensitivity such as changing the length and nature of the siloxane buffer layer are discussed in this paper.

InAs/AlGaAs quantum dot intermediate band solar cells with enlarged sub-bandgaps

In the last decade several prototypes of intermediate band solar cells (IBSCs) have been manufactured. So far, most of these prototypes have been based on InAs/GaAs quantum dots (QDs) in order to implement the IB material. The key operation principles of the IB theory are two photon sub-bandgap (SBG) photocurrent, and output voltage preservation, and both have been experimentally demonstrated at low temperature. At room temperature (RT), however, thermal escape/relaxation between the conduction band (CB) and the IB prevents voltage preservation. To improve this situation, we have produced and characterized the first reported InAs/AlGaAs QD-based IBSCs. For an Al content of 25% in the host material, we have measured an activation energy of 361 meV for the thermal carrier escape. This energy is about 250 meV higher than the energies found in the literature for InAs/GaAs QD, and almost 140 meV higher than the activation energy obtained in our previous InAs/GaAs QD-IBSC prototypes including a specifically designed QD capping layer. This high value is responsible for the suppression of the SBG quantum efficiency under monochromatic illumination at around 220 K. We suggest that, if the energy split between the CB and the IB is large enough, activation energies as high as to suppress thermal carrier escape at room temperature (RT) can be achieved. In this respect, the InAs/AlGaAs system offers new possibilities to overcome some of the problems encountered in InAs/GaAs and opens the path for QD-IBSC devices capable of achieving high efficiency at RT.

Realistic detailed balance study of the quantum efficiency of quantum dot solar cells

An attractive but challenging technology for high efficiency solar energy conversion is the intermediate band solar cell (IBSC), whose theoretical efficiency limit is 63%, yet which has so far failed to yield high efficiencies in practice. The most advanced IBSC technology is that based on quantum dots (QDs): the QD-IBSC. In this paper, k·p calculations of photon absorption in the QDs are combined with a multi-level detailed balance model. The model has been used to reproduce the measured quantum efficiency of a real QD-IBSC and its temperature dependence. This allows the analysis of individual sub-bandgap transition currents, which has as yet not been possible experimentally, yielding a deeper understanding of the failure of current QD-IBSCs. Based on the agreement with experimental data, the model is believed to be realistic enough to evaluate future QD-IBSC proposals.

Entangled two-photon source using biexciton emission of an asymmetric quantum dot in a cavity

A semiconductor based scheme has been proposed for generating entangled photon pairs from the radiative decay of an electrically pumped biexciton in a quantum dot. Symmetric dots produce polarization entanglement, but experimentally realized asymmetric dots produce photons entangled in both polarization and frequency. In this work, we investigate the possibility of erasing the “which-path” information contained in the frequencies of the photons produced by asymmetric quantum dots to recover polarization-entangled photons. We consider a biexciton with nondegenerate intermediate excitonic states in a leaky optical cavity with pairs of degenerate cavity modes close to the nondegenerate exciton transition frequencies. An open quantum system approach is used to compute the polarization entanglement of the two-photon state after it escapes from the cavity, measured by the visibility of two-photon interference fringes. We explicitly relate the two-photon visibility to the degree of the Bell-inequality violation, deriving a threshold at which Bell-inequality violations will be observed. Our results show that an ideal cavity will produce maximally polarization-entangled photon pairs, and even a nonideal cavity will produce partially entangled photon pairs capable of violating a Bell-inequality.

Foundations of quantum technology

Recent progress in fabrication and control of single quantum systems presage a nascent technology based on quantum principles. We review these principles in the context of specific examples including: quantum dots, quantum electromechanical systems, quantum communication and quantum computation.

Synthesis and evaluation of novel ligands for quantum dot stabilisation and polymerisation studies

This thesis describes the design and synthesis of a variety of functionalised phosphine oxides and sulfides, based on the structure of trioctylphosphine oxide, synthesised for the purpose of surface modification of quantum dots. The ability of the ligands to modify the surface chemistry via displacement of the original hexadecylamine capping layer of quantum dots was evaluated. Finally the surface modified quantum dots were investigated for enhancement in their inherent properties and improved compatibility with the various applications for which they were initially designed. Upon the commencement of research involving quantum dots it became apparent that more information on their behaviour and interaction with the environment was required. The limits of the inherent stability of hexadecylamine capped quantum dots were investigated by exposure to a number of different environments. The effect upon the stability of the quantum dots was monitored by changes in the photoluminescence ability of their cores. Subtle differences between different batches of quantum dots were observed and the necessity to account for these in future applications noted. Lastly the displacement of the original hexadecylamine coating with the "designer" functionalised ligands was evaluated to produce a set of conditions that would result in the best possible surface modification. A general procedure was elucidated however it was discovered that each displacement still required slight adjustment by consideration of the other factors such as the difference in ligand structure and the individuality of the various batches of quantum dots. This thesis also describes a procedure for the addition of a protective layer to the surface of quantum dots by cross-linking the functionalised ligands bound to the surface via an acyclic diene metathesis polymerisation. A detailed description of the problems encountered in the analysis of these materials combined with the use of novel techniques such as diffusion ordered spectroscopy is provided as a means to overcome the limitations encountered. Finally a demonstration of the superior stability, upon exposure to a range of aggressive environments of these protected materials compared with those before cross-linking provided physical proof of the cross-linking process and the advantages of the cross-linking modification. Finally this thesis includes the presentation of initial work into the production of luminescent nanocrystal encoded resin beads for the specific use in solid phase combinatorial chemistry. Demonstration of the successful covalent incorporation of quantum dots into the polymeric matrices of non-functionalised and functionalised resin beads is described. Finally by preliminary work to address and overcome the possible limitations that may be encountered in the production and general employment of these materials in combinatorial techniques is given.

Analytical model for active metamaterials with quantum ingredients

We present an analytical model for describing complex dynamics of a hybrid system consisting of resonantly coupled classical resonator and quantum structures. Classical resonators in our model correspond to plasmonic metamaterials of various geometries, as well as other types of nano- and microstructure, the optical responses of which can be described classically. Quantum resonators are represented by atoms or molecules, or their aggregates (for example, quantum dots, carbon nanotubes, dye molecules, polymer or bio-molecules etc), which can be accurately modelled only with the use of the quantum mechanical approach. Our model is based on the set of equations that combines well established density matrix formalism appropriate for quantum systems, coupled with harmonic-oscillator equations ideal for modelling sub-wavelength plasmonic and optical resonators. As a particular example of application of our model, we show that the saturation nonlinearity of carbon nanotubes increases multifold in the resonantly enhanced near field of a metamaterial. In the framework of our model, we discuss the effect of inhomogeneity of the carbon-nanotube layer (bandgap value distribution) on the nonlinearity enhancement. © 2012 IOP Publishing Ltd.

Quantum dot materials for terahertz generation applications

Compact and tunable semiconductor terahertz sources providing direct electrical control, efficient operation at room temperatures and device integration opportunities are of great interest at the present time. One of the most well-established techniques for terahertz generation utilises photoconductive antennas driven by ultrafast pulsed or dual wavelength continuous wave laser systems, though some limitations, such as confined optical wavelength pumping range and thermal breakdown, still exist. The use of quantum dot-based semiconductor materials, having unique carrier dynamics and material properties, can help to overcome limitations and enable efficient optical-to-terahertz signal conversion at room temperatures. Here we discuss the construction of novel and versatile terahertz transceiver systems based on quantum dot semiconductor devices. Configurable, energy-dependent optical and electronic characteristics of quantum-dot-based semiconductors are described, and the resonant response to optical pump wavelength is revealed. Terahertz signal generation and detection at energies that resonantly excite only the implanted quantum dots opens the potential for using compact quantum dot-based semiconductor lasers as pump sources. Proof-of-concept experiments are demonstrated here that show quantum dot-based samples to have higher optical pump damage thresholds and reduced carrier lifetime with increasing pump power.

Self-Assembled InAs/GaAs Quantum Dot Solar Cells

Our work focuses on experimental and theoretical studies aimed at establishing a fundamental understanding of the principal electrical and optical processes governing the operation of quantum dot solar cells (QDSC) and their feasibility for the realization of intermediate band solar cell (IBSC). Uniform performance QD solar cells with high conversion efficiency have been fabricated using carefully calibrated process recipes as the basis of all reliable experimental characterization. The origin for the enhancement of the short circuit current density (Jsc) in QD solar cells was carefully investigated. External quantum efficiency (EQE) measurements were performed as a measure of the below bandgap distribution of transition states. In this work, we found that the incorporation of self-assembled quantum dots (QDs) interrupts the lattice periodicity and introduce a greatly broadened tailing density of states extending from the bandedge towards mid-gap. A below-bandgap density of states (DOS) model with an extended Urbach tail has been developed. In particular, the below-bandgap photocurrent generation has been attributed to transitions via confined energy states and background continuum tailing states. Photoluminescence measurement is used to measure the energy level of the lowest available state and the coupling effect between QD states and background tailing states because it results from a non-equilibrium process. A basic I-V measurement reveals a degradation of the open circuit voltage (Voc) of QD solar cells, which is related to a one sub-bandgap photon absorption process followed by a direct collection of the generated carriers by the external circuit. We have proposed a modified Shockley-Queisser (SQ) model that predicts the degradation of Voc compared with a reference bulk device. Whenever an energy state within the forbidden gap can facilitate additional absorption, it can facilitate recombination as well. If the recombination is non-radiative, it is detrimental to solar cell performance. We have also investigated the QD trapping effects as deep level energy states. Without an efficient carrier extraction pathway, the QDs can indeed function as mobile carriers traps. Since hole energy levels are mostly connected with hole collection under room temperature, the trapping effect is more severe for electrons. We have tried to electron-dope the QDs to exert a repulsive Coulomb force to help improve the carrier collection efficiency. We have experimentally observed a 30% improvement of Jsc for 4e/dot devices compared with 0e/dot devices. Electron-doping helps with better carrier collection efficiency, however, we have also measured a smaller transition probability from valance band to QD states as a direct manifestation of the Pauli Exclusion Principle. The non-linear performance is of particular interest. With the availability of laser with on-resonance and off-resonance excitation energy, we have explored the photocurrent enhancement by a sequential two-photon absorption (2PA) process via the intermediate states. For the first time, we are able to distinguish the nonlinearity effect by 1PA and 2PA process. The observed 2PA current under off-resonant and on-resonant excitation comes from a two-step transition via the tailing states instead of the QD states. However, given the existence of an extended Urbach tail and the small number of photons available for the intermediate states to conduction band transition, the experimental results suggest that with the current material system, the intensity requirement for an observable enhancement of photocurrent via a 2PA process is much higher than what is available from concentrated sun light. In order to realize the IBSC model, a matching transition strength needs to be achieved between valance band to QD states and QD states to conduction band. However, we have experimentally shown that only a negligible amount of signal can be observed at cryogenic temperature via the transition from QD states to conduction band under a broadband IR source excitation. Based on the understanding we have achieved, we found that the existence of the extended tailing density of states together with the large mismatch of the transition strength from VB to QD and from QD to CB, has systematically put into question the feasibility of the IBSC model with QDs.

Spin-Orbit Coupling in n-Type PbTe/PbEuTe Quantum Wells

Magnetoresistance measurements were performed on an n-type PbTe/PbEuTe quantum well and weak antilocalization effects were observed. This indicates the presence of spin orbit coupling phenomena and we showed that the Rashba effect is the main mechanism responsible for this spin orbit coupling. Using the model developed by Iordanskii et al., we fitted the experimental curves and obtained the inelastic and spin orbit scattering times. Thus we could compare the zero field energy spin-splitting predicted by the Rashba theory with the energy spin-splitting obtained from the analysis of the experimental curves. The final result confirms the theoretical prediction of strong Rashba effect on IV-VI based quantum wells.

Quantum Hall Effect near the Charge Neutrality Point in a Two-Dimensional Electron-Hole System

We study the transport properties of HgTe-based quantum wells containing simultaneously electrons and holes in a magnetic field B. At the charge neutrality point (CNP) with nearly equal electron and hole densities, the resistance is found to increase very strongly with B while the Hall resistivity turns to zero. This behavior results in a wide plateau in the Hall conductivity sigma(xy) approximate to 0 and in a minimum of diagonal conductivity sigma(xx) at nu = nu(p) - nu(n) = 0, where nu(n) and nu(p) are the electron and hole Landau level filling factors. We suggest that the transport at the CNP point is determined by electron-hole ""snake states'' propagating along the nu = 0 lines. Our observations are qualitatively similar to the quantum Hall effect in graphene as well as to the transport in a random magnetic field with a zero mean value.

Control of the persistent currents in two interacting quantum rings through the Coulomb interaction and interring tunneling

The persistent current in two vertically coupled quantum rings containing few electrons is studied. We find that the Coulomb interaction between the rings in the absence of tunneling affects the persistent current in each ring and the ground-state configurations. Quantum tunneling between the rings alters significantly the ground state and the persistent current in the system.

Universal zero-bias conductance through a quantum wire side-coupled to a quantum dot

A numerical renormalization-group study of the conductance through a quantum wire containing noninteracting electrons side-coupled to a quantum dot is reported. The temperature and the dot-energy dependence of the conductance are examined in the light of a recently derived linear mapping between the temperature-dependent conductance and the universal function describing the conductance for the symmetric Anderson model of a quantum wire with an embedded quantum dot. Two conduction paths, one traversing the wire, the other a bypass through the quantum dot, are identified. A gate potential applied to the quantum wire is shown to control the current through the bypass. When the potential favors transport through the wire, the conductance in the Kondo regime rises from nearly zero at low temperatures to nearly ballistic at high temperatures. When it favors the dot, the pattern is reversed: the conductance decays from nearly ballistic to nearly zero. When comparable currents flow through the two channels, the conductance is nearly temperature independent in the Kondo regime, and Fano antiresonances in the fixed-temperature plots of the conductance as a function of the dot-energy signal interference between them. Throughout the Kondo regime and, at low temperatures, even in the mixed-valence regime, the numerical data are in excellent agreement with the universal mapping.