A structurally and compositionally well-defined and spectrally tunable artificial light-harvesting system has been constructed in which multiple organic dyes attached to a three-arm-DNA nanostructure serve as an antenna conjugated to a photosynthetic reaction center isolated from Rhodobacter sphaeroides 2.4.1. The light energy absorbed by the dye molecules is transferred to the reaction center, where charge separation takes place. The average number of DNA three-arm junctions per reaction center was tuned from 0.75 to 2.35. This DNA-templated multichromophore system serves as a modular light-harvesting antenna that is capable of being optimized for its spectral properties, energy transfer efficiency, and photostability, allowing one to adjust both the size and spectrum of the resulting structures. This may serve as a useful test bed for developing nanostructured photonic systems.
A CdZnTe/MgCdTe double-heterostructure (DH) consisting of a 3 μm thick Cd0.9946 Zn0.0054Te middle layer that is lattice-matched to an InSb substrate has been grown using molecular beam epitaxy. A long carrier lifetime of 3.4 × 102 ns has been demonstrated at room temperature, which is approximately three times as long as that of a CdTe/MgCdTe DH with identical layer thickness. This substantial improvement is due to the reduction in misfit dislocation density in the CdZnTe alloy. In contrast, a CdTe/MgCdTe DH with 3 μm thick CdTe layer grown on an InSb substrate exhibits a strain relaxation of ∼30%, which leads to a wider x-ray diffraction peak, a weaker integrated photoluminescence intensity, and a shorter minority carrier lifetime of 1.0 × 102 ns. These findings indicate that CdZnTe lattice-matched to InSb has great potential as applied to high-efficiency solar cells as well as virtual substrates for high-performance large-area HgCdTe focal plane arrays.
Time-resolved fluorescence spectroscopy was used to explore the pathway and kinetics of energy transfer in photosynthetic membrane vesicles (chromatophores) isolated from Rhodobacter (Rba.) sphaeroides cells harvested 2, 4, 6 or 24 hours after a transition from growth in high to low level illumination. As previously observed, this light intensity transition initiates the remodeling of the photosynthetic apparatus and an increase in the number of light harvesting 2 (LH2) complexes relative to light harvesting 1 (LH1) and reaction center (RC) complexes. It has generally been thought that the increase in LH2 complexes served the purpose of increasing the overall energy transmission to the RC. However, fluorescence lifetime measurements and analysis in terms of energy transfer within LH2 and between LH2 and LH1 indicate that, during the remodeling time period measured, only a portion of the additional LH2 generated are well connected to LH1 and the reaction center. The majority of the additional LH2 fluorescence decays with a lifetime comparable to that of free, unconnected LH2 complexes. The presence of large LH2-only domains has been observed by atomic force microscopy in Rba. sphaeroides chromatophores (Bahatyrova et al., Nature, 2004, 430, 1058), providing structural support for the existence of pools of partially connected LH2 complexes. These LH2-only domains represent the light-responsive antenna complement formed after a switch in growth conditions from high to low illumination, while the remaining LH2 complexes occupy membrane regions containing mixtures of LH2 and LH1–RC core complexes. The current study utilized a multi-parameter approach to explore the fluorescence spectroscopic properties related to the remodeling process, shedding light on the structure-function relationship of the photosynthetic assembles. Possible reasons for the accumulation of these largely disconnected LH2-only pools are discussed.
Monocrystalline CdTe/MgCdTe double-heterostructures (DHs) grown on lattice-matched InSb substrates have demonstrated impressively long carrier lifetimes in both unintentionally doped and Indium-doped n-type CdTe samples. The non-radiative recombination inside of, and at the interfaces of the CdTe absorbers in CdTe/MgCdTe DH samples has been significantly reduced due to the use of lattice-matched InSb substrates, and the excellent passivation provided by the MgCdTe barrier layers. The external luminescent quantum efficiency (η_ext) of n-type CdTe/MgCdTe DHs is up to 3.1%, observed from a 1-µm-thick CdTe/MgCdTe DH doped at 1017 cm-3. The 3.1% η_ext corresponds to an internal luminescent quantum efficiency (η_int) of 91%. Such a high η_ext gives an implied Voc, or quasi-Fermi-level splitting, of 1.13 V.
To obtain actual Voc, the quasi-Fermi-level splitting should be extracted to outside the circuit using a hole-selective contact layer. However, CdTe is difficult to be doped p-type, making it challenging to make efficient PN junction CdTe solar cells. With the use of MgCdTe barrier layers, the hole-contact layer can be defective without affecting the voltage. P-type hydrogenated amorphous silicon is an effective hole-selective contact for CdTe solar cells, enabling monocrystalline CdTe/MgCdTe DH solar cells to achieve Voc over 1.1 V, and a maximum active area efficiency of 18.8% (Jsc = 23.3 mA/cm2, Voc = 1.114 V, and FF = 72.3%). The knowledge gained through making the record-efficiency monocrystalline CdTe cell, particularly the n-type doping and the double-heterostructure design, may be transferable to polycrystalline CdTe thin-film cells and improve their competitiveness in the PV industry.