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Coral-Like Perovskite Nanostructures for Enhanced Light-Harvesting and Accelerated Charge Extraction in Perovskite Solar Cells
摘要： A novel coral-like perovskite nanostructured layer was grown on a compact perovskite foundation layer by the facile surface modification with dimethylformamide/isopropanol (DMF/IPA) as co-solvent. Surface morphological characterizations with SEM and XRD analyses revealed a growing mechanism of the new morphology, which was composed of the perovskite decomposition and recrystallization, excessive-PbI2 extraction, and sequential formation of coral-like nanostructured perovskite layer. The coral-like perovskite nanostructures resulted in significant light scattering, enhancing the light harvesting efficiency, and thus augmenting the photocurrent density. Moreover, the geometric configuration of the perovksite solar cells was changed from planar to bulk heterojunction, which results in the acceleration of charge separation and extraction due to the high surface area at the interface between the obtained perovskite and hole-transport layers. The optimal perovskite solar cell exhibited an impressive power conversion efficiency (PCE) of 19.47%, as compared to that of the pristine cell (17.19%).
关键词： solar cells,Bulk heterojunction,light-harvesting,coral-like nanostructures,surface modification,perovskite
更新于2025-11-21 11:01:37
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Excitation energy transfer in the far-red absorbing violaxanthin/vaucheriaxanthin chlorophyll a complex from the eustigmatophyte alga FP5
摘要： This work highlights spectroscopic investigations on a new representative of photosynthetic antenna complexes in the LHC family, a putative violaxanthin/vaucheriaxanthin chlorophyll a (VCP) antenna complex from a freshwater Eustigmatophyte alga FP5. A representative VCP-like complex, named as VCP-B3 was studied with both static and time-resolved spectroscopies with the aim of obtaining a deeper understanding of excitation energy migration within the pigment array of the complex. Compared to other VCP representatives, the absorption spectrum of the VCP-B3 is strongly altered in the range of the chlorophyll a Qy band, and is substantially red-shifted with the longest wavelength absorption band at 707 nm at 77 K. VCP-B3 shows a moderate xanthophyll-to-chlorophyll a efficiency of excitation energy transfer in the 50–60% range, 20–30% lower from comparable VCP complexes from other organisms. Transient absorption studies accompanied by detailed data fitting and simulations support the idea that the xanthophylls that occupy the central part of the complex, complementary to luteins in the LHCII, are violaxanthins. Target analysis suggests that the primary route of xanthophyll-to-chlorophyll a energy transfer occurs via the xanthophyll S1 state.
关键词： Chlorophyll a,Light-harvesting complex,Transient absorption,Violaxanthin,Photosynthesis,Vaucheriaxanthin
更新于2025-11-19 16:46:39
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Directed Nanoscale Self-assembly of Natural Photosystems on Nitrogen-doped Carbon Nanotubes for Solar Energy Harvesting
摘要： Natural photosystems (PSs) have received much attention as a biological solar energy harvester because of their high quantum efficiency for energy transfer. However, the PSs hybridized with solid electrodes exhibit low light-harvesting efficiencies because of poor interface properties and random orientations of PSs, all of which interfere with efficient charge extraction and transfer. Herein, we report the linker-free, oriented self-assembly of natural PSs with nitrogen-doped carbon nanotubes (NCNTs) via electrostatic interaction. Protonated nitrogen-doped sites on the NCNTs facilitate spontaneous immobilization of the negatively charged stroma side of PSs, which provides a favorable orientation for electron transfer without electrically insulating polymer linkers. The resulting PS/NCNT hybrids exhibit a photocurrent density of 1.25 ± 0.08 μA cm-2, which is much higher than that of PS/CNT hybrids stabilized with polyethylenimine (0.60 ± 0.01 μA cm-2) and sodium dodecyl sulfate (0.14 ± 0.01 μA cm-2), respectively. This work emphasizes the importance of the linker-free assembly of PSs into well-oriented hybrid structures to construct an efficient light-harvesting electrode.
关键词： Light-harvesting,Electrostatic interaction,Photosystems,Nitrogen-doped carbon nanotubes,Self-assembly
更新于2025-11-14 15:29:11
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Complementary Chromophore Decoration in NU-1000 via Solvent-Assisted Ligands Incorporation: Efficient Energy Transfer within the Metal-Organic Frameworks
摘要： BODIPY-incorporated solvent-assisted ligand incorporation metal-organic frameworks (SALI-MOFs) were designed and synthesized using NU-1000 and carboxylic acid functionalized BODIPY moieties by the solvent-assisted ligand incorporation (SALI) approach. SALI-MOFs were characterized by various technique including powder X-ray diffraction, scanning electron microscope, N2 adsorption/desorption isotherms, Fourier transform infrared spectroscopy, and nuclear magnetic resonance spectroscopy. The SALI-MOFs were found to have cooperative light-harvesting properties and shown to possess efficient singlet oxygen (1O2) generation ability.
关键词： Light-harvesting properties,Singlet oxygen,Metal-organic frameworks,Solvent-assisted ligands incorporation,Energy transfer,BODIPY
更新于2025-11-14 15:14:40
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Ultraviolet patterns of flowers revealed in polymer replica – caused by surface architecture
摘要： Angiosperms and their pollinators are adapted in a close co-evolution. For both the plants and pollinators, the functioning of the visual signaling system is highly relevant for survival. As the frequency range of visual perception in many insects extends into the ultraviolet (UV) region, UV-patterns of plants play an important role in the flower–pollinator interaction. It is well known that many flowers contain UV-absorbing pigments in their petal cells, which are localized in vacuoles. However, the contribution of the petal surface microarchitecture to UV-reflection remains uncertain. The correlation between the surface structure and its reflective properties is also relevant for biomimetic applications, for example, in the field of photovoltaics. Based on previous work, we selected three model species with distinct UV-patterns to explore the possible contribution of the surface architecture to the UV-signaling. Using a replication technique, we transferred the petal surface structure onto a transparent polymer. Upon illumination with UV-light, we observed structural-based patterns in the replicas that were surprisingly comparable to those of the original petals. For the first time, this experiment has shown that the parameters of the surface structure lead to an enhancement in the amount of absorbed UV-radiation. Spectrophotometric measurements revealed up to 50% less reflection in the UV-absorbing regions than in the UV-reflecting areas. A comparative characterization of the micromorphology of the UV-reflecting and UV-absorbing areas showed that, in principle, a hierarchical surface structure results in more absorption. Therefore, the results of our experiments demonstrate the structural-based amplification of UV-reflection and provide a starting point for the design of bioinspired antireflective and respectively strongly absorbing surfaces.
关键词： hierarchical structures,biomimetics,light absorption,light harvesting,light reflection
更新于2025-10-22 19:40:53
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Maze-Like Halide Perovskite Films for Efficient Electron Transport Layer-Free Perovskite Solar Cells
摘要： Perovskite solar cells (PSCs) without an electron transport layer (ETL) exhibit fascinating advantages such as simplified configuration, low cost, and facile fabrication process. However, the performance of ETL-free PSCs has been hampered by severe charge carrier recombination induced either by current leakage (insufficient perovskite film coverage) or inferior charge extraction. Herein, an additive-assisted morphological engineering strategy is used to construct an intriguing bilayer perovskite film featuring a dense bottom layer and a maze-like top layer. Such maze-like perovskite films enable the construction of ETL-free PSCs with a PCE of 18.5% and negligible hysteresis, which can be attributed to the higher crystallinity and superior light-harvesting capability of the resultant perovskite film, as well as facilitated hole extraction at the hole transport layer (HTL)/perovskite interface. This work provides a simple approach to modify the perovskite film morphology and demonstrates the correlation between facilitated charge-carrier extraction and high-performance ETL-free perovskite photovoltaics.
关键词： light harvesting,morphological engineering,additives,perovskite solar cells,charge extraction
更新于2025-10-22 19:40:53
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Quantumness in light harvesting is determined by vibrational dynamics
摘要： We demonstrate for the multi-level spin-boson (MLSB) Hamiltonian, typically used to describe biological light-harvesting, that the distinction between quantum and classical dynamics is determined entirely by the thermal environment. In particular, any MLSB model featuring classical interactions with a classical bath is exactly equivalent in its absorption and energy transfer dynamics to a classical model involving coupled harmonic oscillators. This result holds in the linear response regime for both pulsed and incoherent excitation. In the biological context, this finding highlights the centrality of vibrational dynamics in determining the 'quantumness' of photosynthetic light-harvesting, particularly in the creation of the photosynthetic energy funnel where excitation energy concentrates near the reaction center via a series of downhill energy transfer events. These findings support the idea that this energy funnel is exclusively quantum-mechanical in origin, although it need not rely on entanglement.
关键词： vibrational dynamics,energy transfer,photosynthesis,quantumness,light harvesting,spin-boson model
更新于2025-09-23 15:23:52
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Electronic Structure of Chlorophyll a Solution Investigated by Photoelectron Yield Spectroscopy
摘要： Various bio-related processes are driven by electron transfer reactions. Therefore the electronic structures of bio-molecules in their living environment are keys of their functionalities. One significant example photosynthesis which has attracted much attention due to urgent necessity of clean energy source. In this study, we carried out photoelectron yield spectroscopy (PYS) measurements to demonstrate the electronic structures of oligomerizedChl-a molecules, which is known as an essential reaction center of the photosystem in general green plants, under the atmospheric environment. The ionization energies of the Chl-a aggregates are successfully derived.
关键词： Photoelectron Yield Spectroscopy,Polarization energy,Light harvesting antenna,Photosynthesis,Photosystem,Electronic structure,Ionization energy,Reaction center,Chlorophyll a
更新于2025-09-23 15:23:52
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Machine Learning of Two-Dimensional Spectroscopic Data
摘要： Two-dimensional electronic spectroscopy has become one of the main experimental tools for analyzing the dynamics of excitonic energy transfer in large molecular complexes. Simplified theoretical models are usually employed to extract model parameters from the experimental spectral data. Here we show that computationally expensive but exact theoretical methods encoded into a neural network can be used to extract model parameters and infer structural information such as dipole orientation from two dimensional electronic spectra (2DES) or reversely, to produce 2DES from model parameters. We propose to use machine learning as a tool to predict unknown parameters in the models underlying recorded spectra and as a way to encode computationally expensive numerical methods into efficient prediction tools. We showcase the use of a trained neural network to efficiently compute disordered averaged spectra and demonstrate that disorder averaging has non-trivial effects for polarization controlled 2DES.
关键词： Neural Networks,excitonic energy transfer,light-harvesting complexes,ML numerical methods
更新于2025-09-23 15:23:52
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Effective mass and optical properties of orthorhombic Al1?xInxFeO3 perovskite: An ab-initio study
摘要： Electronic and optical properties of AlFeO3 and Al1?xInxFeO3 (x = 0.25, 0.5, 0.75) are studied using ab-initio calculations. Electronic structure in the vicinity of the conduction band minimum (CBM) and valence band maximum (VBM), the effective masses of holes and electrons at the gamma point are calculated. The calculated effective masses of electrons is smaller than that of holes (mc1⊥, mc1‖ (me*) < mv1⊥, mv1‖, mv2⊥, mv2‖ (mh*)), for all values of x; this is expected to contribute to the desirable photocatalytic performance. Effective mass tensor for electrons is found to be isotropic (unlike holes). The optical constants such as static dielectric constant, refractive index, extinction coefficient and absorption coefficient are comparable with that Si. The maximum absorption exists in the visible light region for all the phases studied; making In-doped AlFeO3 suitable for energy harvesting applications. We noted from our previous work (Sudha Priyanga and Thomas, 2018) that the computed band gap values could be underestimated by as large as ～0.5 eV. Even so, the reported phases would be relevant for light harvesting.
关键词： AlFeO3,Optical properties,Ab-initio calculations,Effective masses,Light-harvesting
更新于2025-09-23 15:22:29