scholarly journals High efficiency excitation energy transfer in biohybrid quantum dot–bacterial reaction center nanoconjugates

2021 ◽  
Author(s):  
Giordano Amoruso ◽  
Juntai Liu ◽  
Daniel W Polak ◽  
Kavita Tiwari ◽  
Michael R Jones ◽  
...  

Reaction centers (RCs) are the pivotal component of natural photosystems, converting solar energy into the potential difference between separated electrons and holes that is used to power much of biology. RCs from anoxygenic purple photosynthetic bacteria such as Rhodobacter sphaeroides only weakly absorb much of the visible region of the solar spectrum which limits their overall light-harvesting capacity. For in vitro applications such as bio-hybrid photodevices this deficiency can be addressed by effectively coupling RCs with synthetic light-harvesting materials. Here, we studied the time scale and efficiency of Förster resonance energy transfer (FRET) in a nanoconjugate assembled from a synthetic quantum dot (QD) antenna and a tailored RC engineered to be fluorescent. Time-correlated single photon counting spectroscopy of biohybrid conjugates enabled the direct determination of FRET from QDs to attached RCs on a time scale of 26.6 ± 0.1 ns and with a high efficiency of 0.75 ± 0.01.

2020 ◽  
Author(s):  
Andreas Albrecht ◽  
Julia Nowak ◽  
Peter Walla

Nature provides evidence that there is no fundamental limit for harvesting and funneling nearly all scattered sun-photons onto smaller conversion centers by ultra-fast emergy transfer processes. Recently, a proof-of-principle study showed that this can also be achieved by artificial systems containing light-harvesting pools of randomly oriented molecules that funnel energy to individual, aligned light-redirecting molecules.<br>However, capturing the entire solar spectrum requires engineering of complex multi-element structures considering macroscopic refraction and wave guiding of different spectral ranges of multijunction photovoltaics as well as ultrafast, nanoscopic light-harvesting, energy transfer and funneling, anisotropic absorption and emission and the spectra of a multitude of pigments of different orientations and concentrations. So far, no tool excited that allowed model such structures in one system.<br>Here we present a ray tracing tool allowing to model and analyze such multi-scale structures, including molecular, ultrafast energy transfer and funneling as well as anisotropic absorption and emission as well as micro-and macroscopic waveguiding and raytracing in one tool. We present first results of solar concentrator architectures with the highest theoretical energy conversion efficiency reported so far.<br>A novel tool is provided that allows to construct, model and analyze any desired complex ultrafast light-harvesting/photovoltaic architecture with the highest efficiencies by considering molecular, nanometric energy transfer and funneling as well as microscopic waveguiding and raytracing.


2020 ◽  
Author(s):  
Andreas Albrecht ◽  
Julia Nowak ◽  
Peter Walla

Nature provides evidence that there is no fundamental limit for harvesting and funneling nearly all scattered sun-photons onto smaller conversion centers by ultra-fast emergy transfer processes. Recently, a proof-of-principle study showed that this can also be achieved by artificial systems containing light-harvesting pools of randomly oriented molecules that funnel energy to individual, aligned light-redirecting molecules.<br>However, capturing the entire solar spectrum requires engineering of complex multi-element structures considering macroscopic refraction and wave guiding of different spectral ranges of multijunction photovoltaics as well as ultrafast, nanoscopic light-harvesting, energy transfer and funneling, anisotropic absorption and emission and the spectra of a multitude of pigments of different orientations and concentrations. So far, no tool excited that allowed model such structures in one system.<br>Here we present a ray tracing tool allowing to model and analyze such multi-scale structures, including molecular, ultrafast energy transfer and funneling as well as anisotropic absorption and emission as well as micro-and macroscopic waveguiding and raytracing in one tool. We present first results of solar concentrator architectures with the highest theoretical energy conversion efficiency reported so far.<br>A novel tool is provided that allows to construct, model and analyze any desired complex ultrafast light-harvesting/photovoltaic architecture with the highest efficiencies by considering molecular, nanometric energy transfer and funneling as well as microscopic waveguiding and raytracing.


Nanomaterials ◽  
2021 ◽  
Vol 11 (5) ◽  
pp. 1201
Author(s):  
Dan Dalacu ◽  
Philip J. Poole ◽  
Robin L. Williams

For nanowire-based sources of non-classical light, the rate at which photons are generated and the ability to efficiently collect them are determined by the nanowire geometry. Using selective-area vapour-liquid-solid epitaxy, we show how it is possible to control the nanowire geometry and tailor it to optimise device performance. High efficiency single photon generation with negligible multi-photon emission is demonstrated using a quantum dot embedded in a nanowire having a geometry tailored to optimise both collection efficiency and emission rate.


Materials ◽  
2021 ◽  
Vol 14 (11) ◽  
pp. 2753
Author(s):  
Bartosz Fetliński ◽  
Sebastian Turczyński ◽  
Michał Malinowski ◽  
Paweł Szczepański

In this work, we investigate Ce3+ to Yb3+ energy transfer in Y4Al2O9 (YAM) for potential application in solar spectrum down-converting layers for photovoltaic devices. Photoluminescence properties set, of 10 samples, of the YAM host activated with Ce3+ and Yb3+ with varying concentrations are presented, and the Ce3+ to Yb3+ energy transfer is proven. Measurement of highly non-exponential luminescence decays of Ce3+ 5d band allowed for the calculation of maximal theoretical quantum efficiency, of the expected down-conversion process, equal to 123%. Measurements of Yb3+ emission intensity, in the function of excitation power, confirmed the predominantly single-photon downshifting character of Ce3+ to Yb3+ energy transfer. Favorable location of the Ce3+ 5d bands in YAM makes this system a great candidate for down-converting, and down-shifting, luminescent layers for photovoltaics.


Author(s):  
Marcelo Davanco ◽  
C. Stephen Hellberg ◽  
Serkan Ates ◽  
Antonio Badolato ◽  
Kartik Srinivasan

2015 ◽  
Vol 2 (1) ◽  
pp. 60-67 ◽  
Author(s):  
Simanta Kundu ◽  
Santanu Bhattacharyya ◽  
Amitava Patra

The efficient resonance energy transfer from CdTe quantum dots (donors) to Nile Red dye (acceptor) encapsulated PMMA nanoparticles for light harvesting is described.


2021 ◽  
Author(s):  
Kaipeng Zhong ◽  
Siyu Lu ◽  
Wenting Guo ◽  
Junxia Su ◽  
Shihao Sun ◽  
...  

An efficient perovskite-quantum-dot light-harvesting system with NIR emission was fabricated based on passivation CH3NH3PbBr3 QDs in the supramolecular self-assembly of Zn(II) carboxyl functionalized-pillar[5]arene coordination polymer and two different fluorescence dyes,...


2010 ◽  
Vol 14 (01) ◽  
pp. 55-63 ◽  
Author(s):  
Pierre D. Harvey ◽  
Christine Stern ◽  
Claude P. Gros ◽  
Roger Guilard

Recent discoveries from our research groups on the photophysics of a few cofacial bisporphyrin dyads for through space singlet and triplet energy transfers raised several important investigations about the mechanism of energy transfers and energy migration in light-harvesting devices, notably LH II, in the heavily investigated purple photosynthetic bacteria. The key feature is that for face-to-face and slipped dyads with controlled structure using rigid spacers or spacers with limited flexibilities, our fastest rates for singlet energy transfer are in the 10 × 109 s -1 (i.e. 100 ps time scale) for donor-acceptor distances of ~3.5–3.6 Å. The time scale for energy transfers between different bacteriochlorophylls, notably B800*→B850, is in the ps despite the long Mg ⋯ Mg separation (~18 Å). This short rate drastically contrasts with the well-accepted Förster theory. This review focuses on the photophysical processes and dynamics in LH II and compares these parameters with our investigated model dyads build upon octa-etio-porphyrin chromophores and rigid and semi-rigid spacers. The recently discovered role of the rhodopin glucoside (carotenoid) will be analyzed as possible relay for energy transfers, including the possibility of uphill processes at room temperature. In this context the concept of energy migration may be complemented by parallel relays and uphill processes. It is also becoming more obvious that the irreversible electron transfer at the reaction center (electron transfer from the special pair to the phaeophytin) renders the rates for energy transfer and migration faster precluding all possibility of back transfers.


2014 ◽  
Vol 89 (15) ◽  
Author(s):  
Marcelo Davanço ◽  
C. Stephen Hellberg ◽  
Serkan Ates ◽  
Antonio Badolato ◽  
Kartik Srinivasan

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