Two-photon photocurrent and voltage up-conversion in a quantum dot intermediate band solar cell

It has been proposed that the use of self-assembled quantum dot (QD) arrays can break the Shockley-Queisser efficiency limit by extending the absorption of solar cells into the low-energy photon range while preserving their output voltage. This would be possible if the infrared photons are absorbed in the two sub-bandgap QD transitions simultaneously and the energy of two photons is added up to produce one single electron-hole pair, as described by the intermediate band model. Here, we present an InAs/Al 0.25Ga 0.75As QD solar cell that exhibits such electrical up-conversion of low-energy photons. When the device is monochromatically illuminated with 1.32 eV photons, open-circuit voltages as high as 1.58 V are measured (for a total gap of 1.8 eV). Moreover, the photocurrent produced by illumination with photons exciting the valence band to intermediate band (VB-IB) and the intermediate band to conduction band (IB-CB) transitions can be both spectrally resolved. The first corresponds to the QD inter-band transition and is observable for photons of energy mayor que 1 eV, and the later corresponds to the QD intra-band transition and peaks around 0.5 eV. The voltage up-conversion process reported here for the first time is the key to the use of the low-energy end of the solar spectrum to increase the conversion efficiency, and not only the photocurrent, of single-junction photovoltaic devices. In spite of the low absorption threshold measured in our devices - 0.25 eV - we report open-circuit voltages at room temperature as high as 1.12 V under concentrated broadband illumination.

Pseudo-random single photon counting for space-borne atmospheric sensing applications

The ability to accurately observe the Earth's carbon cycles from space gives scientists an important tool to analyze climate change. Current space-borne Integrated-Path Differential Absorption (IPDA) Iidar concepts have the potential to meet this need. They are mainly based on the pulsed time-offlight principle, in which two high energy pulses of different wavelengths interrogate the atmosphere for its transmission properties and are backscattered by the ground. In this paper, feasibility study results of a Pseudo-Random Single Photon Counting (PRSPC) IPDA lidar are reported. The proposed approach replaces the high energy pulsed source (e.g. a solidstate laser), with a semiconductor laser in CW operation with a similar average power of a few Watts, benefiting from better efficiency and reliability. The auto-correlation property of Pseudo-Random Binary Sequence (PRBS) and temporal shifting of the codes can be utilized to transmit both wavelengths simultaneously, avoiding the beam misalignment problem experienced by pulsed techniques. The envelope signal to noise ratio has been analyzed, and various system parameters have been selected. By restricting the telescopes field-of-view, the dominant noise source of ambient light can be suppressed, and in addition with a low noise single photon counting detector, a retrieval precision of 1.5 ppm over 50 km along-track averaging could be attained. We also describe preliminary experimental results involving a negative feedback Indium Gallium Arsenide (InGaAs) single photon avalanche photodiode and a low power Distributed Feedback laser diode modulated with PRBS driven acoustic optical modulator. The results demonstrate that higher detector saturation count rates will be needed for use in future spacebourne missions but measurement linearity and precision should meet the stringent requirements set out by future Earthobserving missions.

Optically enhanced photon recycling in mechanically stacked multijunction solar cells

Multijunction solar cells can be fabricated by mechanically bonding together component cells that are grown separately. Here, we present four-junction four-terminal mechanical stacks composed of GaInP/GaAs tandems grown on GaAs substrates and GaInAsP/GaInAs tandems grown on InP substrates. The component cells were bonded together with a low-index transparent epoxy that acts as an angularly selective reflector to the GaAs bandedge luminescence, while simultaneously transmitting nearly all of the subbandgap light. As determined by electroluminescence measurements and optical modeling, the GaAs subcell demonstrates a higher internal radiative limit and, thus, higher subcell voltage, compared with GaAs subcells without the epoxy reflector. The best cells demonstrate 38.8 ± 1.0% efficiency under the global spectrum at 1000 W/m2 and ~ 42% under the direct spectrum at ~100 suns. Eliminating the series resistance is the key challenge for further improving the concentrator cells.

Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes

Two-dimensional infrared spectra of peptides are introduced that are the direct analogues of two- and three-pulse multiple quantum NMR. Phase matching and heterodyning are used to isolate the phase and amplitudes of the electric fields of vibrational photon echoes as a function of multiple pulse delays. Structural information is made available on the time scale of a few picoseconds. Line narrowed spectra of acyl-proline-NH2 and cross peaks implying the coupling between its amide-I modes are obtained, as are the phases of the various contributions to the signals. Solvent-sensitive structural differences are seen for the dipeptide. The methods show great promise to measure structure changes in biology on a wide range of time scales.

Quantification of spread of cerebellar long-term depression with chemical two-photon uncaging of glutamate

Localized, chemical two-photon photolysis of caged glutamate was used to map the changes in α-amino-3-hydroxy-5-methyl-4-isoxazolepropionic acid-type glutamate receptors caused by long-term synaptic depression (LTD) in cerebellar Purkinje cells. LTD produced by pairing parallel fiber activity with depolarization was accompanied by a decline in the response of Purkinje cells to uncaged glutamate that accounted for both the time course and magnitude of LTD. This depression of glutamate responses was observed not only at the site of parallel fiber stimulation but also at more distant sites. The amount of LTD decreased with distance and was half-maximal 50 μm away from the site of parallel fiber activity. Estimation of the number of parallel fibers active during LTD induction indicates that LTD modified glutamate receptors not only at active synapses but also at 600 times as many inactive synapses on a single Purkinje cell. Therefore, both active and inactive parallel fiber synapses can undergo changes at a postsynaptic locus as a result of associative pre- and postsynaptic activity.

Simultaneous two-photon excitation of distinct labels for dual-color fluorescence crosscorrelation analysis

Confocal fluorescence correlation spectroscopy as a time-averaging fluctuation analysis combining maximum sensitivity with high statistical confidence has proved to be a very versatile and powerful tool for detection and temporal investigation of biomolecules at ultralow concentrations on surfaces, in solutions, and in living cells. To probe the interaction of different molecular species for a detailed understanding of biologically relevant mechanisms, crosscorrelation studies on dual or multiple fluorophore assays with spectrally distinct excitation and emission are particularly promising. Despite the considerable improvement of detection specificity provided by fluorescence crosscorrelation analysis, few applications have so far been reported, presumably because of the practical challenges of properly aligning and controlling the stability of the experimental setup. In this work, we demonstrate that two-photon excitation combined with dual-color fluorescence correlation spectroscopy can be the key to simplifying simultaneous investigations of multiple fluorescent species significantly on a single-molecule scale. Two-photon excitation allows accession of common fluorophores of largely distinct emission by the same excitation wavelength, because differences in selection rules and vibronic coupling can induce considerable shifts between the one-photon and two-photon excitation spectra. The concept of dual-color two-photon fluorescence crosscorrelation analysis is introduced and experimentally demonstrated with an established assay probing the selective cleavage of dual-labeled DNA substrates by restriction endonuclease EcoRI.

Femtosecond dynamics of the forbidden carotenoid S1 state in light-harvesting complexes of purple bacteria observed after two-photon excitation

Time-resolved excited-state absorption intensities after direct two-photon excitation of the carotenoid S1 state are reported for light-harvesting complexes of purple bacteria. Direct excitation of the carotenoid S1 state enables the measurement of subsequent dynamics on a fs time scale without interference from higher excited states, such as the optically allowed S2 state or the recently discovered dark state situated between S1 and S2. The lifetimes of the carotenoid S1 states in the B800-B850 complex and B800-B820 complex of Rhodopseudomonas acidophila are 7 ± 0.5 ps and 6 ± 0.5 ps, respectively, and in the light-harvesting complex 2 of Rhodobacter sphaeroides ≈1.9 ± 0.5 ps. These results explain the differences in the carotenoid to bacteriochlorophyll energy transfer efficiency after S2 excitation. In Rps. acidophila the carotenoid S1 to bacteriochlorophyll energy transfer is found to be quite inefficient (φET1 <28%) whereas in Rb. sphaeroides this energy transfer is very efficient (φET1 ≈80%). The results are rationalized by calculations of the ensemble averaged time constants. We find that the Car S1 → B800 electronic energy transfer (EET) pathway (≈85%) dominates over Car S1 → B850 EET (≈15%) in Rb. sphaeroides, whereas in Rps. acidophila the Car S1 → B850 EET (≈60%) is more efficient than the Car S1 → B800 EET (≈40%). The individual electronic couplings for the Car S1 → BChl energy transfer are estimated to be approximately 5–26 cm−1. A major contribution to the difference between the energy transfer efficiencies can be explained by different Car S1 energy gaps in the two species.

Single photon emission computerized tomography imaging of amphetamine-induced dopamine release in drug-free schizophrenic subjects.

The dopamine hypothesis of schizophrenia proposes that hyperactivity of dopaminergic transmission is associated with this illness, but direct observation of abnormalities of dopamine function in schizophrenia has remained elusive. We used a newly developed single photon emission computerized tomography method to measure amphetamine-induced dopamine release in the striatum of fifteen patients with schizophrenia and fifteen healthy controls. Amphetamine-induced dopamine release was estimated by the amphetamine-induced reduction in dopamine D2 receptor availability, measured as the binding potential of the specific D2 receptor radiotracer [123I] (S)-(-)-3-iodo-2-hydroxy-6-methoxy-N-[(1-ethyl-2-pyrrolidinyl) methyl]benzamide ([123I]IBZM). The amphetamine-induced decrease in [123I]IBZM binding potential was significantly greater in the schizophrenic group (-19.5 +/- 4.1%) compared with the control group (-7.6 +/- 2.1%). In the schizophrenic group, elevated amphetamine effect on [123I]IBZM binding potential was associated with emergence or worsening of positive psychotic symptoms. This result suggests that psychotic symptoms elicited in this experimental setting in schizophrenic patients are associated with exaggerated stimulation of dopaminergic transmission. Such an observation would be compatible with an abnormal responsiveness of dopaminergic neurons in schizophrenia.

Neural-network-based classification of cognitively normal, demented, Alzheimer disease and vascular dementia from single photon emission with computed tomography image data from brain.

Single photon emission with computed tomography (SPECT) hexamethylphenylethyleneamineoxime technetium-99 images were analyzed by an optimal interpolative neural network (OINN) algorithm to determine whether the network could discriminate among clinically diagnosed groups of elderly normal, Alzheimer disease (AD), and vascular dementia (VD) subjects. After initial image preprocessing and registration, image features were obtained that were representative of the mean regional tissue uptake. These features were extracted from a given image by averaging the intensities over various regions defined by suitable masks. After training, the network classified independent trials of patients whose clinical diagnoses conformed to published criteria for probable AD or probable/possible VD. For the SPECT data used in the current tests, the OINN agreement was 80 and 86% for probable AD and probable/possible VD, respectively. These results suggest that artificial neural network methods offer potential in diagnoses from brain images and possibly in other areas of scientific research where complex patterns of data may have scientifically meaningful groupings that are not easily identifiable by the researcher.

The photoreceptor sensory rhodopsin I as a two-photon-driven proton pump.

Proton translocation experiments with intact cells of Halobacterium salinarium overproducing sensory rhodopsin I (SRI) revealed transport activity of SRI in a two-photon process. The vectoriality of proton translocation depends on pH, being outwardly directed above, and inwardly directed below, pH 5.7. Activation of the transport cycle requires excitation of the initial dark state of SRI, SRI590, to form the intermediate SRI380. Action spectra identify the photocycle intermediates SRI380 and SRI520 as the two photochemically reactive species in the outwardly directed transport process. As shown by flash photolysis experiments, SRI520 undergoes a so-far unknown photochemical reaction to SRI380 with a half-time of <200 micros. Mutation of SRI residue Asp-76, the residue which is equivalent to the proton acceptor Asp-85 in bacteriorhodopsin, to asparagine leads to inactivation of proton translocation. This demonstrates that the underlying mechanisms of proton transport in both retinal proteins share similar features. However, SRI is to our knowledge the first case where photochemical reactions between two thermally unstable photoproducts of a retinal protein constitute a catalytic ion transport cycle.

Anisotropic exchange interaction induced by a single photon in semiconductor microcavities

We investigate coupling of localized spins in a semiconductor quantum dot embedded in a microcavity. The lowest cavity mode and the quantum dot exciton are coupled and close in energy, forming a polariton. The fermions forming the exciton interact with localized spins via exchange. Exact diagonalization of a Hamiltonian in which photons, spins, and excitons are treated quantum mechanically shows that a single polariton induces a sizable indirect anisotropic exchange interaction between spins. At sufficiently low temperatures strong ferromagnetic correlations show up without an appreciable increase in exciton population. In the case of a (Cd,Mn)Te quantum dot, Mn-Mn ferromagnetic coupling is still significant at 1 K: spin-spin correlation around 3 for exciton occupation smaller than 0.3. We find that the interaction mediated by photon-polaritons is 10 times stronger than the one induced by a classical field for equal Rabi splitting.

Single photon emission mammography with convergent collimators

Tese de doutoramento, Engenharia Biomédica e Biofísica, Universidade de Lisboa, Faculdade de Ciências, 2016