Light-harvesting Processes Research Articles

Fabrication of graphene-incorporated tin-niobate-doped zinc oxide for highly enhanced photocatalytic hydrogen evolution and degradation

This study focuses on designing, synthesizing, and characterizing an innovative graphene-based Sn2Nb2O7-ZnO. Ternary Sn2Nb2O7-ZnO with graphene is added to a catalyst, enhancing the efficiency of visible-light photocatalytic hydrogen (H2) evolution and ciprofloxacin (CIP) degradation in an aqueous solution. It also facilitates easier charge transfer and control over electron-hole recombination between light-harvesting processes. Additionally, the UV–vis shows that rGO doping can be used to tune significant visible light absorption in addition to the effective charge transmission channel of Sn2Nb2O7-rGO-ZnO nanorods. Under visible light, Sn2Nb2O7-rGO-ZnO nanorods demonstrate expected photocatalytic hydrogen evolution and CIP degradation of 1240 μmol·h−1·g−1, a 96% increase over pure catalysts. Photocatalytic H2 production over Sn2Nb2O7-rGO-ZnO is assessed using transient photocurrent response, suggesting a possible mechanism. Owing to the type II process ability, more electrons can participate in the H2 evolution reduction and CIP degradation. Furthermore, it has the potential to completely replace the present base metal as an incredibly powerful and long-standing light radiation-based photocatalyst. In this study, we prepared catalysts that are more stable and highly efficient up to a six-cycle test, non-toxic, low-cost catalysts for H2 production and CIP degradation.

A Vision for the Future of Multiscale Modeling.

The rise of modern computer science enabled physical chemistry to make enormous progresses in understanding and harnessing natural and artificial phenomena. Nevertheless, despite the advances achieved over past decades, computational resources are still insufficient to thoroughly simulate extended systems from first principles. Indeed, countless biological, catalytic and photophysical processes require ab initio treatments to be properly described, but the breadth of length and time scales involved makes it practically unfeasible. A way to address these issues is to couple theories and algorithms working at different scales by dividing the system into domains treated at different levels of approximation, ranging from quantum mechanics to classical molecular dynamics, even including continuum electrodynamics. This approach is known as multiscale modeling and its use over the past 60 years has led to remarkable results. Considering the rapid advances in theory, algorithm design, and computing power, we believe multiscale modeling will massively grow into a dominant research methodology in the forthcoming years. Hereby we describe the main approaches developed within its realm, highlighting their achievements and current drawbacks, eventually proposing a plausible direction for future developments considering also the emergence of new computational techniques such as machine learning and quantum computing. We then discuss how advanced multiscale modeling methods could be exploited to address critical scientific challenges, focusing on the simulation of complex light-harvesting processes, such as natural photosynthesis. While doing so, we suggest a cutting-edge computational paradigm consisting in performing simultaneous multiscale calculations on a system allowing the various domains, treated with appropriate accuracy, to move and extend while they properly interact with each other. Although this vision is very ambitious, we believe the quick development of computer science will lead to both massive improvements and widespread use of these techniques, resulting in enormous progresses in physical chemistry and, eventually, in our society.

Transcriptomic meta-analysis and functional validation identify genes linked to adaptation and involved in high-light acclimation in Synechocystis sp. PCC 6803

Several mechanisms of high light (HL) acclimation have been identified in Synechocystis sp. PCC 6803. However, there are still gaps in understanding of the complex regulatory networks and molecular interactions involved. This study aims to investigate the molecular mechanisms underlying HL acclimation in Synechocystis by performing a meta-analysis of transcriptomic data. A total of 411 differentially expressed genes (DEGs) were identified in the meta-analysis, of which 179 were unique to the meta-analysis. These findings indicate a coordinated response of the Synechocystis transcriptome to HL, with specific genes being activated or suppressed to cope with the challenging conditions. Of all the DEGs, 307 were related to primary metabolism, 52 were involved in photosynthesis and light-harvesting processes, and 52 genes had no known function or were not properly annotated. Gene ontology and KEGG pathway enrichment analyses revealed the involvement of DEGs in various biological processes and pathways, including photosynthesis, energy metabolism and oxidative stress response. Comparison with previous HL adaptive laboratory evolution (ALE) experiments revealed 17 DEGs that had acquired adaptive mutations after HL ALE. Three of these adaptive mutations which lead to amino acid exchanges in the corresponding proteins (sll0267L1189P, sll0355F254S, and slr1855D200G) were selected to test their impact on HL acclimation in Synechocystis. The laboratory validation of strains carrying these three mutations, showed that each mutation had a positive effect on HL acclimation when reconstructed in the Synechocystis laboratory type (LT) background. The three mutants reached higher cell densities at the end of cultivation, showed comparable levels of chlorophyll fluorescence when exposed to incremental red-orange light, and at least one of the three mutations may alter gene function rather than suppress it. These findings offer valuable insight into the HL acclimation and adaptation of Synechocystis and contribute to a more comprehensive understanding of the molecular mechanisms that underlie its adaptation to HL. These results may direct future studies seeking to enhance the adaptability of cyanobacteria and related species to HL.

Watching the Interplay between Photoinduced Ultrafast Charge Dynamics and Nuclear Vibrations.

Here is presented the ultrafast hole-electron dynamics of photoinduced metal to ligand charge-transfer (MLCT) states in a Ru(II) complex, [Ru(dcbpy)2(NCS)2]4- (dcbpy = 4,4'-dicarboxy-2,2'-bipyridine), a photoactive molecule employed in dye sensitized solar cells. Via cutting-edge computational techniques, a tailored computational protocol is here presented and developed to provide a detailed analysis of the electronic manifold coupled with nuclear vibrations to better understand the nonradiative pathways and the resulting overall dye performances in light-harvesting processes (electron injection). Thus, the effects of different vibrational modes were investigated on both the electronic levels and charge transfer dynamics through a theoretical-computational approach. First, the linear response time-dependent density functional (LR-TDDFT) formalism was employed to characterize excitation energies and spacing among electronic levels (the electronic layouts). Then, to understand the ultrafast (femtosecond) charge dynamics on the molecular scale, we relied on the nonperturbative mean-field quantum electronic dynamics via real-time (RT-) TDDFT. Three vibrational modes were selected, representative for collective nuclear movements that can have a significant influence on the electronic structure: two involving NCS- ligands and one involving dcbpy ligands. As main results, we observed that such MLCT states, under vibrational distortions, are strongly affected and a faster interligand electron transfer mechanism is observed along with an increasing MLCT character of the adiabatic electronic states approaching closer in energy due to the vibrations. Such findings can help both in providing a molecular picture of multidimensional vibro-electronic spectroscopic techniques, used to characterize ultrafast coherent and noncoherent dynamics of complex systems, and to improve dye performances with particular attention to the study of energy or charge transport processes and vibronic couplings.

Bio-templated energy transfer system for constructing artificial light-harvesting antennae, white light generation, and photonic nanowires

Developing environmentally friendly, sustainable, and biocompatible artificial light-harvesting systems has become an essential area of research to understand natural light-harvesting processes involving multistep resonance energy transfer and building efficient energy conversion systems related to energy and optoelectronic applications. In this direction, bio-scaffolded artificial energy transfer systems for panchromatic light collection and sequential energy transfer have fascinated the scientific community. In this review, we have discussed what the dynamic structure and intrinsic physical properties of biomolecules like deoxyribonucleic acid, proteins, and peptides can provide for the development of new optical devices, sustainable and environmentally friendly white emitting materials, and cascaded energy transfer systems for energy harvesting from light. In doing so, we have highlighted some of the recent advances in bio-scaffolds as a platform for the assembly of different types of donor–acceptor chromophores involved in fluorescence energy transfer.

Dopant-driven recombination delay and ROS enhancement in nanoporous Cd1-xCuxS heterogeneous photocatalyst for the degradation of DR-23 dye under visible light irradiation

Developing an efficient heterogeneous photocatalyst for environmental remediation and treatment strategies using visible light harvesting processes is promising but challenging. Herein, Cd1-xCuxS materials have been synthesized and characterized by precise analytical tools. Cd1-xCuxS materials exhibited excellent photocatalytic activity for direct Red 23 (DR-23) dye degradation in visible light irradiation. The operational parameters, like dopant concentration, photocatalyst dose, pH, and initial concentration of dye were investigated during the process. The photocatalytic degradation process follows pseudo-first-order kinetics. As compared to other tested materials, 5% Cu doped CdS material revealed superior photocatalytic performance for the degradation of DR-23 (k = 13.96 × 10−3 min−1). Transient absorption spectroscopy, EIS, PL, and transient photocurrent indicated that adding copper to the CdS matrix improved the separation of photo-generated charge carriers by lowering the recombination rate. Spin-trapping experiments recognized the photodegradation primarily based on secondary redox products, i.e., hydroxyl and superoxide radicals. According to by Mott-Schottky curves, photocatalytic mechanism and photo-generated charge carrier density were elucidated regarding dopant-induced valence and conduction bands shifting. Thermodynamic probability of radical formation in line with the altered redox potentials by Cu doping has been discussed in the mechanism. The identification of intermediates by mass spectrometry study also showed a plausible breakdown mechanism for DR-23. Moreover, samples treated with nanophotocatalyst displayed excellent results when tested for water quality metrics such as DO, TDS, BOD, and COD. Developed nanophotocatalyst shows high recyclability with superior heterogeneous nature. 5% Cu-doped CdS also exhibit strong photocatalytic activity for the degradation of colourless pollutant bisphenol A (BPA) under visible light (k = 8.45 × 10−3 min−1). The results of this study offer exciting opportunities to alter semiconductors' electronic band structures for visible-light-induced photocatalytic activity for wastewater treatment.

The inhibition and recovery mechanisms of the diatom Phaeodactylum tricornutum in response to high light stress - A study combining physiological and transcriptional analysis.

By combining physiological/biochemical and transcriptional analysis, the inhibition and recovery mechanisms of Phaeodactylum tricornutum in response to extreme high light stress (1300 μmol photons · m-2 · s-1 ) were elucidated. The population growth was inhibited in the first 24 h and started to recover from 48 h. At 24 h, photoinhibition was exhibited as the changes of PSII photosynthetic parameters and decrease in cellular pigments, corresponding to the downregulation of genes encoding light-harvesting complex and pigments synthesis. Changes in those photosynthetic parameters and genes were kept until 96 h, indicating that the decrease of light absorption abilities might be one strategy for photoacclimation. In the meanwhile, we observed elevated cellular ROS levels, dead cells proportions, and upregulation of genes encoding antioxidant materials and proteasome pathway at 24 h. Those stress-related parameters and genes recovered to the controls at 96 h, indicating a stable intracellular environment after photoacclimation. Finally, genes involving carbon metabolisms were upregulated from 24 to 96 h, which ensured the energy supply for keeping high base and nucleotide excision repair abilities, leading to the recovery of cell cycle progression. We concluded that P. tricornutum could overcome photoinhibition by decreasing light-harvesting abilities, enhancing carbon metabolisms, activating anti-oxidative functions, and elevating repair abilities. The parameters of light harvesting, carbon metabolisms, and repair processes were responsible for the recovery phase, which could be considered long-term adaptive strategies for diatoms under high light stress.

Biomimetic Approach toward Visible Light-Driven Hydrogen Generation Based on a Porphyrin-Based Coordination Polymer Gel.

There has been a widespread interest in developing self-assembled porphyrin nanostructures to mimic nature's light-harvesting processes. Herein, porphyrin-based coordination polymer gel (CPG) has been developed as a "soft" photocatalyst material for hydrogen (H2) production from water under visible light. The CPG offers a hierarchical nanofibrous network structure obtained through self-assembly of a terpyridine alkyl-amide appended porphyrin (TPY-POR)-based low molecular weight gelator with ruthenium ions (RuII) and produces H2 with a rate of 5.7 mmol g-1 h-1 in the presence of triethylamine (TEA) as a sacrificial electron donor. Further, the [Fe2(bdt)(CO)6] (dbt = 1,2-benzenedithiol) cocatalyst, which can mimic the activity of iron hydrogenase, is coassembled in the CPG and shows remarkable improvement in H2 evolution (catalytic activity; rate ∼10.6 mmol g-1 h-1 and turnover number ∼1287). The significant enhancement in catalytic activity was supported by several controlled experiments, including femtosecond transient absorption (TA) spectroscopy and also DFT calculation. The TA study supported the cascade electron transfer process from porphyrin core to [Ru(TPY)2]2+ center, and subsequently, the electron transfers to the cocatalyst [Fe2(bdt)(CO)6] for H2 production.

Carotenoid responds to excess energy dissipation in the LH2 complex from Rhodoblastus acidophilus.

The functions of both (bacterio) chlorophylls and carotenoids in light-harvesting complexes have been extensively studied during thepast decade, yet, the involvement of BChl a high-energy Soret band in the cascade of light-harvesting processes still remainsa relatively unexplored topic. Here, we present transient absorption data recorded after excitation of the Soret band in the LH2 complex from Rhodoblastus acidophilus. Comparison of obtained data to those recorded after excitation of rhodopin glucoside and B800 BChl a suggests that no Soret-to-Car energy transfer pathway is active in LH2 complex. Furthermore, a spectrally rich pattern observed in the spectral region of rhodopin glucoside ground state bleaching (420-550nm) has been assigned toanelectrochromic shift. The results of global fitting analysis demonstrate two more features. A 6ps component obtained exclusively after excitation of the Soret band has been assigned to the response of rhodopin glucoside to excess energy dissipation in LH2. Another time component, ~ 450ps, appearing independently of theexcitation wavelength was assigned to BChla-to-Car triplet-triplet transfer. Presented data demonstrate several new features of LH2 complex and its behavior following the excitation of the Soret band.

Plasmon enhanced fluorescence of photosynthetic complexes by conjugating with gold micro-plates and their single-particle sensing application

Fundamental investigating and understanding the light harvesting process of natural antenna complexes will inspire and encourage us for rational design more efficient artificial devices for applications. Here, gold micro-plates are covalently linked with photosynthetic complexes, and their linked sites can be varied through adjusting the concentration of photosynthetic complexes. Significantly strong fluorescent emission enhancement has been observed from single gold micro-plate. When excited at 480 nm, the intensity enhancement is over two times higher than that excited at 405 nm, as the peridinin-chlorophyll-protein complexes prefer to absorbing light at 480 nm and they possess different pathways of energy transfer at different excitation wavelength. The synergistic effect originated from gold microplates make the enhancement factor of single peridinin-chlorophyll-protein complex from single gold micro-plate reach to 3.68 × 107, which could be utilized in designing single particle fluorescent sensor such as detecting Hg2+. Our method not only provides an effective way for significantly enhancing the fluorescent emission intensity and efficiency of light-harvesting, but also presents a robust single-particle application.

Photoacclimation impacts the molecular features of photosystem supercomplexes in the centric diatom Thalassiosira pseudonana

In diatoms, light-harvesting processes take place in a specific group of proteins, called fucoxanthin chlorophyll a/c proteins (FCP). This group includes many members and represents the major characteristic of the diatom photosynthetic apparatus, with specific pigments bound (chlorophyll c, fucoxanthin, diadino- and diatoxanthin besides chlorophyll a). In thylakoids, FCP and photosystems (PS) form multimeric supercomplexes.In this study, we compared the biochemical properties of PS supercomplexes isolated from Thalassiosira pseudonana cells grown under low light or high light conditions, respectively. High light acclimation changed the molecular features of the PS and their ratio in thylakoids. In PSII, no obvious changes in polypeptide composition were observed, whereas for PSI changes in one specific group of FCP proteins were detected. As reported before, the amount of xanthophyll cycle pigments and their de-epoxidation ratio was increased in PSI under HL. In PSII, however, no additional xanthophyll cycle pigments occurred, but the de-epoxidation ratio was increased as well. This comparison suggests how mechanisms of photoprotection might take place within and in the proximity of the PS, which gives new insights into the capacity of diatoms to adapt to different conditions and in different environments.

One-Shot Trajectory Learning of Open Quantum Systems Dynamics.

Nonadiabatic quantum dynamics is important for understanding light-harvesting processes, but its propagation with traditional methods can be rather expensive. Here we present a one-shot trajectory learning approach that allows us to directly make an ultrafast prediction of the entire trajectory of the reduced density matrix for a new set of such simulation parameters as temperature and reorganization energy. The whole 10-ps-long propagation takes 70 ms as we demonstrate on the comparatively large quantum system, the Fenna-Matthews-Olsen (FMO) complex. Our approach also significantly reduces time and memory requirements for training.

A fast method for electronic couplings in embedded multichromophoric systems

Electronic couplings are key to understanding exciton delocalization and transport in natural and artificial light harvesting processes. We develop a method to compute couplings in multichromophoric aggregates embedded in complex environments without running expensive quantum chemical calculations. We use a transition charge approximation to represent the quantum mechanical transition densities of the chromophores and an atomistic and polarizable classical model to describe the environment atoms. We extend our framework to estimate transition charges directly from the chromophore geometry, i.e., bypassing completely the quantum mechanical calculations using a regression approach. The method allows to rapidly compute accurate couplings for a large number of geometries along molecular dynamics trajectories.

Exploring the Aggregation and Light-Harvesting Aptitude of Naphthalimide-Based Amphiphile and Non-amphiphile AIEgen.

Herein, we report a comparative study of two naphthalimide-tethered amphiphile and non-amphiphile with their aggregation-induced emission properties. A synthetic modulation of a hydrophobic tail on the framework repressed the ACQ-phoric fluorophore to an AIEgen. L1 and L2 remain in the dispersed form in DMF and exhibits aggregation and intense emission signal in aqueous media. Microscopy detailing of the aggregating process has been analyzed. Not only the AIEgens are emissive in water but also they are emissive in the solid state. The natural light-harvesting process is mimicked by the aggregated state, establishing an energy transfer process between L1 and commercial dye. Disaggregation of the AIEgen has also been utilized in the detection of nitroaromatics. Analytical utility of the AIE-gen is being demonstrated concerning the detection of explosives in aqueous media.

Ultrafast Plasmonics Beyond the Perturbative Regime: Breaking the Electronic-Optical Dynamics Correspondence.

The transient optical response of plasmonic nanostructures has recently been the focus of extensive research. Accurate prediction of the ultrafast dynamics following excitation of hot electrons by ultrashort laser pulses is of major relevance in a variety of contexts from the study of light harvesting and photocatalytic processes to nonlinear nanophotonics and the all-optical modulation of light. So far, all studies have assumed the correspondence between the temporal evolution of the dynamic optical signal, retrieved by transient absorption spectroscopy, and that of the photoexcited hot electrons, described in terms of their temperature. Here, we show both theoretically and experimentally that this correspondence does not hold under a nonperturbative excitation regime. Our results indicate that the main mechanism responsible for the breaking of the correspondence between electronic and optical dynamics is universal in plasmonics, being dominated by the nonlinear smearing of the Fermi–Dirac occupation probability at high hot-electron temperatures.

Organic Electronics from Nature: Computational Investigation of the Electronic and Optical Properties of the Isomers of Bixin and Norbixin Present in the Achiote Seeds.

Organic compounds have been employed in developing new green energy solutions with good cost-efficiency compromise, such as photovoltaics. The light-harvesting process in these applications is a crucial feature that still needs improvements. Here, we studied natural dyes to propose an alternative for enhancing the light-harvesting capability of photovoltaics. We performed density functional theory calculations to investigate the electronic and optical properties of the four natural dyes found in achiote seeds (Bixa orellana L.). Different DFT functionals, and basis sets, were used to calculate the electronic and optical properties of the bixin, norbixin, and their trans-isomers (molecules present in Bixa orellana L.). We observed that the planarity of the molecules and their similar extension for the conjugation pathways provide substantially delocalized wavefunctions of the frontier orbitals and similar values for their energies. Our findings also revealed a strong absorption peak in the blue region and an absorption band over the visible spectrum. These results indicate that Bixa orellana L. molecules can be good candidates for improving light-harvesting in photovoltaics.

Origin of layered perovskite device efficiencies revealed by multidimensional time-of-flight spectroscopy.

Mixtures of layered perovskite quantum wells with different sizes form prototypical light-harvesting antenna structures in solution-processed films. Gradients in the bandgaps and energy levels are established by concentrating the smallest and largest quantum wells near opposing electrodes in photovoltaic devices. Whereas short-range energy and charge carrier funneling behaviors have been observed in layered perovskites, our recent work suggests that such light-harvesting processes do not assist long-range charge transport due to carrier trapping at interfaces between quantum wells and interstitial organic spacer molecules. Here, we apply a two-pulse time-of-flight technique to a family of layered perovskite systems to explore the effects that interstitial organic molecules have on charge carrier dynamics. In these experiments, the first laser pulse initiates carrier drift within the active layer of a photovoltaic device, whereas the second pulse probes the transient concentrations of photoexcited carriers as they approach the electrodes. The instantaneous drift velocities determined with this method suggest that the rates of trap-induced carrier deceleration increase with the concentrations of organic spacer cations. Overall, our experimental results and model calculations suggest that the layered perovskite device efficiencies primarily reflect the dynamics of carrier trapping at interfaces between quantum wells and interstitial organic phases.

A partially linearized spin-mapping approach for simulating nonlinear optical spectra.

We present a partially linearized method based on spin-mapping for computing both linear and nonlinear optical spectra. As observables are obtained from ensembles of classical trajectories, the approach can be applied to the large condensed-phase systems that undergo photosynthetic light-harvesting processes. In particular, the recently derived spin partially linearized density matrix method has been shown to exhibit superior accuracy in computing population dynamics compared to other related classical-trajectory methods. Such a method should also be ideally suited to describing the quantum coherences generated by interaction with light. We demonstrate that this is, indeed, the case by calculating the nonlinear optical response functions relevant for the pump-probe and 2D photon-echo spectra for a Frenkel biexciton model and the Fenna-Matthews-Olsen light-harvesting complex. One especially desirable feature of our approach is that the full spectrum can be decomposed into its constituent components associated with the various Liouville-space pathways, offering a greater insight beyond what can be directly obtained from experiments.

Recent advances in single-molecule spectroscopy studies on light-harvesting processes in oxygenic photosynthesis

Photosynthetic light-harvesting complexes (LHCs) play a crucial role in concentrating the photon energy from the sun that otherwise excites a typical pigment molecule, such as chlorophyll-a, only several times a second. Densely packed pigments in the complexes ensure efficient energy transfer to the reaction center. At the same time, LHCs have the ability to switch to an energy-quenching state and thus play a photoprotective role under excessive light conditions. Photoprotection is especially important for oxygenic photosynthetic organisms because toxic reactive oxygen species can be generated through photochemistry under aerobic conditions. Because of the extreme complexity of the systems in which various types of pigment molecules strongly interact with each other and with the surrounding protein matrixes, there has been long-standing difficulty in understanding the molecular mechanisms underlying the flexible switching between the light-harvesting and quenching states. Single-molecule spectroscopy studies are suitable to reveal the conformational dynamics of LHCs reflected in the fluorescence properties that are obscured in ordinary ensemble measurements. Recent advanced single-molecule spectroscopy studies have revealed the dynamical fluctuations of LHCs in their fluorescence peak position, intensity, and lifetime. The observed dynamics seem relevant to the conformational plasticity required for the flexible activations of photoprotective energy quenching. In this review, we survey recent advances in the single-molecule spectroscopy study of the light-harvesting systems of oxygenic photosynthesis.

Supramolecular photoswitch with white-light emission based on bridged bis(pillar[5]arene)s

White light-emitting (WLE) switches have greatly promising and worthy applications in the field of controllable lighting, display, and sensing. Here, we unprecedentedly construct a photocontrollable light-harvesting supramolecular nanoassembly (G/H@NiR) with rarely switchable white light emission, which comprised oligo(phenylenevinylene)-bridged pillar[5]arenes (H), photochromic diarylethene (G), and Nile red (NiR), through host–guest complexation. In the nanosystem, color-tunable photoluminescence such as cyan, orange red, and especially white with chromaticity coordinates (0.33, 0.34) is achieved through altering the proportions of the energy donor (H in assembly G/H) and acceptor center (NiR). Importantly, G, acting as a modulator, can controllably change the energy-transfer (ET) pathway between H and NiR, when the G/H@NiR nanoassembly was exposed to distinct light, achieving reversible switching of multicolor photoluminescence including white-light emission. In addition, the designed intelligent supramolecular assembly G/H@NiR with captivating characteristics has extremely valuable application as erasable multicolor fluorescent inks to be filled in the groove of a three-dimensional model and further form a high-security-level chromatic anticounterfeiting quick response (QR) code, which can be completely hidden and revealed under stimulation of distinct light. Besides, the erasable fluorescent inks can also be used to record data information in mixed fiber film, which can be completely wiped off and rerecord by distinct light. The study provides a controllable supramolecular light-harvesting strategy (the photo-modulating ET pathway in the light-harvesting process) for developing photo-responsive intelligent photoluminescence materials, particularly photosensitive WLE materials, possessing potential applications in photosensitive lighting and display, multicolor imaging, light-manipulative data storage, and high-security-level anticounterfeiting.