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Spectral Reshaping of Single Dye Molecules Coupled to Single Plasmonic Nanoparticles
摘要： Fluorescent molecules are highly susceptible to their local environment. Thus, a fluorescent molecule near a plasmonic nanoparticle can experience changes in local electric field and local density of states that reshape its intrinsic emission spectrum. By avoiding ensemble averaging while simultaneously measuring the super-resolved position of the fluorophore and its emission spectrum, single-molecule hyperspectral imaging is uniquely suited to differentiate changes in spectrum from heterogeneous ensemble effects. Thus, we uncover for the first time single-molecule fluorescence emission spectrum reshaping upon near-field coupling to individual gold nanoparticles using hyperspectral super-resolution fluorescence imaging, and we resolve this spectral reshaping as a function of the nanoparticle/dye spectral overlap and separation distance. We find dyes bluer than the plasmon resonance maximum are red-shifted and redder dyes are blue-shifted. The primary vibronic peak transition probabilities shift to favor secondary vibronic peaks, leading to effective emission maxima shifts in excess of 50 nm, and we understand these light-matter interactions by combining super-resolution hyperspectral imaging and full-field electromagnetic simulations.
关键词： Plasmonic nanoparticles,Single-molecule hyperspectral imaging,Optoelectronics,Energy Conversion and Storage,Fluorescence emission spectrum reshaping,Plasmonics
更新于2025-09-11 14:15:04
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A comprehensive experimental characterisation of a novel porous media combustion-based thermophotovoltaic system with controlled emission
摘要： The high temperatures of combustion systems make them suitable for coupling with thermophotovoltaic systems. In practice, it is quite challenging to reduce heat losses and the spectral mismatch between the emission of the combustion source and the spectral response of photovoltaic (PV) cells. In an effort to pull these disparate energy-focussed research fields together, this paper explores the use of a low-cost erbia (Er2O3) coating on a novel porous media combustion-based thermophotovoltaic (PMC-TPV) reactor for continuous combined heat and power generation. In this work, three different configurations were analysed, including a non-coated porous foam, a coated porous foam, and a coated quartz container. As such, this study provides the first in-depth analysis and characterisation of all salient components of a PMC-TPV system. It includes a detailed characterisation of a 24-cell gallium antimonide (GaSb) array, which was attached to a heat sink and used to harvest the radiant emission from a hot (> 1200 °C), yttria-stabilised zirconia/alumina composite (YZA) ceramic foam. Since the ceramic foam does not have an ideal emissivity curve for these cells, the ability of the erbia coating to control the spectral emission was measured. The results show that by applying the erbia coating to the outer surface of the YZA foam (e.g. using a simple 2-step process of dip coating followed by curing/calcination), it is possible to increase performance, achieving a maximum in-band emission fraction of 25.4% at a firing rate of 1300 kW/m2 (i.e. around 10% of increase than that for non-coated configuration), which provides a temperature of 1285 °C. Additionally, a maximum power output of 1 W was achieved by using erbia coating on YZA foam. For the third configuration, the use of the erbia coating on the quartz tube (instead of the YZA foam) leads to an increase in the maximum core temperature of the reactor up to 1443 °C; however, this also leads to a decrease in electrical performance due to a lower in-band fraction. These findings show that applying an erbia coating on an industrial radiant emitter could enable a combined heat and power processes to gain around 30% increase of electrical output. Finally, since the PV fill factor was lower than expected, and electroluminescence measurements indicated cell damage, these findings also reveal the importance of continuously monitoring PV parameters in PMC-TPV systems.
关键词： Thermophotovoltaic systems,Direct energy conversion,Porous media combustion
更新于2025-09-11 14:15:04
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Thermal‐Emission Enhanced and Optically Modulated Radioisotope Thermophotovoltaic Generators
摘要： Infrared radiation generated by high energy density radioisotope decay can be converted to electrical energy in a radioisotope thermophotovoltaic (RTPV) generator. Thermal emission intensity and spectral properties have substantial implications in this thermal energy conversion process. To improve the performance of the RTPV generator, a silicone coating material was used as a thermal emission enhancer, and SiO2 was used as a filter. The silicone coating has excellent thermal emissivity at high temperatures. The SiO2 filter can optical modulation during the thermal energy conversion process. The heat transfer optimization problem caused by the internal temperature distribution of the system is discussed. Compared with the experimental model before optimization, the output power of the RTPV generator increased by 126%, obtained an open-circuit voltage of 2.64 V, an electric power of 89.88 mW, and an energy conversion efficiency of 5.62%. The RTPV generator is expected to be a potential candidate for energy supply in extreme environments.
关键词： Radioisotope thermophotovoltaic,Nuclear battery,Thermal energy conversion,Gallium antimonide,Silicone coating
更新于2025-09-11 14:15:04
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Self-Healing of Photocurrent Degradation in Perovskite Solar Cells: The Role of Defect-Trapped Excitons
摘要： Solution-processed lead halide perovskites have emerged as one of the most promising materials in optoelectronic applications. However, the perovskites are not stable over prolonged solar illumination. A recent experimental study has revealed light-activated photocurrent degradation and self-healing in the lead halide perovskites, which has important implications in tackling the photostability problems of the perovskites. Unfortunately, the physical origin of the experimental observations is unclear. In this work, we propose a first-principles theory which can elucidate all key experimental observations. By focusing on defect-trapped excitons, the theory can rationalize both fast and slow timescales of self-healing, contrasting dynamics of the photocurrent degradation and its recovery, and steep temperature dependence of the two competing processes. We further predict that the same phenomenon of self-healing could also be observed in other lead halide perovskites with even faster timescales of recovery. The work provides a general framework to elucidate defect-controlled excitation dynamics in perovskites.
关键词： Energy Conversion and Storage,Plasmonics and Optoelectronics
更新于2025-09-11 14:15:04
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Kinetic Monte Carlo Study of the Role of the Energetic Disorder on the Open-circuit Voltage in Polymer:Fullerene Solar Cells
摘要： One major factors limiting the e?ciency in organic solar cells (OSCs) is the low open-circuit voltage (Voc). Existing theoretical studies link the Voc with the charge transfer (CT) state and non-radiative recombination. However, also morphology and energetic disorder can have a strong impact on the Voc within realistic bulk-heterojunction OSCs. In this work, we present a kinetic Monte Carlo study on the role of the energetic disorder on the maximum Voc. We compute the quasi-Fermi level splitting for di?erent energetic disorder and analyze the impact of the energetic disorder at the donor-acceptor interface as well as correlations in the site energies on the Voc. Our results show that the interface strongly controls the maximum Voc. For a higher interface disorder, charge densities and non-geminate recombination increases, and the Voc is reduced. Furthermore, the correlated morphologies show an increase in the maximum Voc and a reduced impact of the energetic disorder.
关键词： Open-circuit Voltage,Kinetic Monte Carlo,Energy Conversion and Storage,Plasmonics and Optoelectronics,Polymer:Fullerene Solar Cells
更新于2025-09-11 14:15:04
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Ultrathin 2D Conjugated Polymer Nanosheets for Solar Fuel Generation
摘要： Two-dimensional (2D) polymers are fascinating as they exhibit unique physical, chemical, mechanical, and electronic properties that are completely different from those of traditional linear or branched polymers. They are very promising for applications in catalysis, separation, optoelectronics, energy storage, and nanomedicine. Recently, ultrathin 2D conjugated polymers have emerged as advanced materials for converting solar energy into chemical energy. The inherent 2D planar structure with in-plane periodicity offers many features that are highly desirable for photon-involved catalytic energy conversion processes, including high absorption coefficients, large surface areas, abundant surface active sites, and efficient charge separation. Moreover, the possibility of finely tuning the optoelectronic and structural properties through precise molecular engineering has opened up new opportunities for design and synthesis of novel 2D polymer nanosheets with unprecedented applications. Herein, we highlight recent advances in developing ultrathin 2D conjugated polymer nanosheets for solar-to-chemical energy conversion. Specifically, we discuss emerging applications of ultrathin 2D conjugated polymer nanosheets for solar-driven water splitting and CO2 reduction. Meanwhile, future challenges and prospects for design and synthesis of ultrathin 2D conjugated polymer nanosheets for solar fuel generation are also included.
关键词： Energy conversion,2D polymers,Nanosheets,Conjugated polymers,Photocatalysis
更新于2025-09-10 09:29:36
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Drought-induced changes in photosynthetic electron transport in maize probed by prompt fluorescence, delayed fluorescence, P700 and cyclic electron flow signals
摘要： The effect of drought on the prompt chlorophyll a fluorescence (PF) transient (OJIP), delayed chlorophyll a fluorescence (DF), modulated 820-nm reflection (MR), energy conversion efficiencies in photosystems (PS) I and II, and cyclic electron flow (CEF) activity in two maize hybrids with contrasting drought tolerance was investigated. Our aim was to identify the target site of drought stress on the photosynthetic electron transport chain and investigate the relevance of the CEF pathway to the drought tolerance of maize plants. The OJIP analysis showed that drought stress, depending on its duration, decreased FP, increased FJ, and induced a pronounced K-band and a positive L-band. Moreover, OJIP parameters, including PIABS, RC/CSO, TRO/ABS, and ETO/TRO, were significantly reduced. The DF analysis showed that the values of I1 and I2 in the induction curve and L1 and L2 derived from the decay curve decreased progressively with the duration of drought stress. The MR analysis showed that drought stress inactivated both the fast decrease and slow increase phases of the MR transient, resulting in a gradual decrease in both VPSI and VPSII-PSI. The energy conversion analysis showed that drought stress decreased the PSI photochemical quantum yield Y(I) and PSII photochemical quantum yield Y(II). Compared to the tolerant hybrid, the drought-induced changes in the sensitive hybrid were stronger and appeared at an earlier treatment stage. The CEF activity analysis showed that the CEF pathway under drought stress operated for a longer time in the tolerant hybrid than that in the sensitive hybrid. The above results indicate that drought stress damaged the donor and acceptor sides of PSII, the PSII reaction center and the acceptor side of PSI and decreased the efficiency of both PSI and PSII and the capacity of electron transfer. The CEF pathway might play an important role in the tolerance of the maize photosynthetic electron transport chain to drought stress.
关键词： Cyclic electron flow,Delayed fluorescence,Modulated 820 nm reflection,Energy conversion efficiencies in photosystems (PS) I and II,Prompt fluorescence OJIP,Maize,Drought stress
更新于2025-09-10 09:29:36
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Dopants Control of Electron-Hole Recombination in Cesium-Titanium Halide Double Perovskite by Time Domain Ab Initio Simulation: Co-Doping Supersedes Mono-Doping
摘要： Using nonadiabatic (NA) molecular dynamics combined with time-domain density functional theory, we simulate electron-hole recombination in pristine and doped inorganic Pb-free double perovskite Cs2TiBr6. We show that replacing the titanium and/or bromine with silicon and/or chlorine extends the charge carrier lifetime. Importantly, dopants avoid deep traps despite they do not change the fundamental bandgap of Cs2TiBr6, they decrease the NA electron-phonon coupling and accelerate decoherence, arising from the reduced overlap of electron and hole wave functions as well as fast phonon modes induced by light dopants respectively, suppressing electron-hole recombination. More importantly, co-doping can reduce the formation energy of silicon and achieve higher doping concentration, potentially increasing the lifetime further. Our study suggests a rational strategy to reduce energy losses by co-doping in design of high performance all-inorganic Pb-free perovskite solar cells.
关键词： Co-doping,Electron-Hole Recombination,Mono-doping,Energy Conversion and Storage,Cesium-Titanium Halide Double Perovskite,Plasmonics and Optoelectronics,Time Domain Ab Initio Simulation,Dopants Control
更新于2025-09-10 09:29:36
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Effects of Electron-Phonon Coupling on Electronic Properties of Methylammonium Lead Iodide Perovskites
摘要： Temperature can have a dramatic effect on the solar efficiency of methylammonium lead iodide (CH3NH3PbI3) absorbers due to changes in the electronic structure of the system even within the range of stability of a single phase. Herein using first principles density functional theory, we investigate the electron band structure of the tetragonal and orthorhombic phases of CH3NH3PbI3 as a function of temperature. The electron-phonon interactions are computed to all orders using a Monte Carlo approach, which is needed considering that the second-order Allen-Heine-Cardona theory in electron-phonon coupling is not adequate. Our results show that the band gap increases with temperature in excellent agreement with experimental results. We verified that anharmonic effects are only important near the tetragonal-cubic phase transition temperature. We also found that temperature has a significant effect on the effective masses and Rashba coupling. At room temperature, electron–phonon coupling is found to enhance the band effective mass by a factor of two, and to diminish the Rashba coupling by the same factor compared to T=0 K values. Our results underscore the significant impact of electron-phonon coupling on electronic properties of the hybrid perovskites.
关键词： Energy Conversion and Storage,Methylammonium Lead Iodide Perovskites,Plasmonics and Optoelectronics,Electron-Phonon Coupling,Electronic Properties
更新于2025-09-10 09:29:36
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Nanoscale Materials in Water Purification || Photocatalysis of Graphene and Carbon Nitride-Based Functional Carbon Quantum Dots
摘要： Day by day, global energy demands increase due to the rapid consumption of depleting fossil fuels and environmental pollution. This has led to the search for materials capable of both energy conversion and elimination of environmental pollutants through the aid of renewable solar energy. This is a promising approach for meeting future energy requirements and eliminating environmental pollutants. In this pursuit, semiconductor photocatalysts have immense potential for solving both energy and environmental issues. To date, numerous semiconductor materials have been explored, including those of metal oxides, chalcogenides, borates, titanates, tungstates, vanadates, zirconates, oxyhalides, and metal-based interstitial compounds. However, the majority of these suffer from limitations such as complex synthesis procedures, limited light absorption range due to their wide band gap, high cost, and toxicity-related issues. Over the past decade, carbon-based nanomaterials have gained attention in the field of photocatalysis. Many recent articles have placed emphasis upon metal-free carbon-based photocatalytic systems for degradation of organic pollutants and hydrogen production from water splitting. The prime merit of these nanomaterials is that they originate from naturally abundant constituent elements such as carbon, nitrogen, and oxygen, making them more economical than their metal-based counterparts. Most reported carbon-based photocatalysts have tunable band gap energies, enhancing their optical absorption range. Band gap energy can be tuned by varying synthesis conditions and precursors, resulting in the formation of nanomaterials with different morphologies. The preparation procedures for most carbon-based nanomaterials are less complex than those of metal-based materials.
关键词： water splitting,energy conversion,semiconductor photocatalysts,graphene,carbon nitride,quantum dots,carbon-based nanomaterials,hydrogen production,solar energy,environmental pollutants,photocatalysis
更新于2025-09-09 09:28:46