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Light Controlled In Vitro Gene Delivery Using Polymer-Tethered Spiropyran as a Photoswitchable Photosensitizer
摘要： A gene delivery system using spiropyran as a photoswitchable photosensitizer for controlled photochemical internalization effect was developed by engineering the outer coating of polyethylenimine/DNA complex with a small amount of spiropyran-containing cationic copolymers. The successful binding of cationic polymers by the polyethylenimine coating was detected by the distance-sensitive fluorescence resonance energy transfer technique that evidenced occurrence of energy transfer between fluorescein-labeled cationic copolymers and polyethylenimine-condensed rhodamine-labeled DNA. The ternary polyplexes feature reversible controllability of singlet oxygen generation based on the dual effect of spiropyrans in photochromism and aggregation-induced enhanced photosensitization, allowing significant light-induced amplification of bPEI-mediated in vitro transgene efficiency (from original 15% to final 91%) at a low DNA dose, with the integrity of supercoiled DNA structure unaffected. The use of spiropyran without the need of other photosensitizers circumvents the issue of uncontrolled long-lasting photocytotoxicity in gene delivery.
关键词： gene delivery,spiropyran,photoswitching,singlet oxygen,fluorescence resonance energy transfer
更新于2025-11-21 11:08:12
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Rational design of a visible-light photochromic diarylethene: a simple strategy by extending conjugation with electron donating groups
摘要： Photochromic diarylethenes have been widely used in many fields. However, their cyclization process must be induced by UV light. In this article, a simple strategy is developed by extending π-conjugation with electron donating groups. The modified dirylethene derivative can photocyclolize under 405-nm light with a good photochromic efficiency. Meanwhile, its absorption and moderate fluorescence can be switched effectively in both directions by visible lights (405 and 520 nm, respectively) in different solutions and in living cells. We believe that this simple method will become a versatile strategy for developing various dirylethylenes with visible-light photochromism.
关键词： fluorescence photoswitching,diarylethylenes,photoreaction quantum yield,visible-light photochromism
更新于2025-11-19 16:56:35
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A unimolecular platform based on diarylethene with multiple stimuli-gated photochromism
摘要： The gated photochromic systems have attracted great interest in scientific researches due to their merits in the opto-electronic fields, whereas the multi-stimuli gating function in a unimolecular platform has rarely been addressed. Herein, a new strategy to realize multi-stimuli gated photochromic function was devised relying on a simple Schiff-based diarylethene derivative. The compound shows no photoswitching properties in solution under irradiation with any wavelength of light. It is noteworthy that mecury(II) ions, water and protons can trigger its photo-reactivity independently with different absorption changes, respectively. Therefore, a molecular logic circuit with four inputs, including mecury(II) ions, water, protons and UV light, was fabricated on the basis of the unimolecular platform, suggesting promise for application in multi-controlled photoswitchings. These results could be valuable for the further development of photoswitchings with multiple stimuli responses.
关键词： Diarylethenes,photoswitching,molecular logic circuit,multiple stimuli responses,gated photochromism
更新于2025-09-23 15:23:52
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Manipulating Living Systems by Light; 生命現象の光操作技術の創出;
摘要： Complex gene networks are essential for diverse biological phenomena, such as cellular programming, metabolism, homeostasis, memory formation, and circadian rhythm. To understand these biological phenomena, including diseases, and to utilize or modify them, approaches that enable optical control of the genome are required. We developed new tools for targeted gene manipulation based on optical control of the CRISPR-Cas9 system and Cre-loxP system. These tools could greatly facilitate understanding of a variety of gene functions and prove useful in biomedical applications. Genome engineering technology and optogenetics technology have emerged as different technologies from each other so far. Our studies merge these emerging research fields together.
关键词： optogenetics,photoswitching protein,cell differentiation,Cre-loxP system,genome editing,CRISPR-Cas9 system
更新于2025-09-23 15:22:29
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Synthesis of a Novel Fluorescent Cyanide Chemosensor Based on Photoswitching Poly(pyrene-1-ylmethyl-methacrylate-random-methyl methacrylate-random-methacrylate spirooxazine)
摘要： The photoswitching poly(pyrene-1-ylmethyl-methacrylate-random-methyl methacrylate-random-methacrylate spirooxazine) was synthesized via atom transfer radical polymerization and characterized by proton nuclear magnetic resonance (1H NMR), gel permeation chromatography (GPC), Fourier transform infrared (FTIR) spectroscopy, UV-visible spectroscopy, and differential scanning calorimetry (DSC). The obtained copolymer exhibited the capability of erasable and rewritable photo-imaging, making it a potential candidate for optical data storage materials. Moreover, the copolymer also showed the sensing ability for cyanide anions effect in aqueous solutions.
关键词： spirooxazine,chemosensor,photoswitching polymers,atom transfer radical polymerization
更新于2025-09-23 15:21:01
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On the impact of competing intra- and intermolecular triplet-state quenching on photobleaching and photoswitching kinetics of organic fluorophores
摘要： While buffer cocktails remain the most commonly used method for photostabilization and photoswitching of fluorescent markers, intramolecular triplet-state quenchers emerge as an alternative strategy to impart fluorophores with 'self-healing' or even functional properties such as photoswitching. In this contribution, we evaluated combinations of both approaches and show that inter- and intramolecular triplet-state quenching processes compete with each other. We find that although the rate of triplet-state quenching is additive, the photostability is limited by the faster pathway. Often intramolecular processes dominate the photophysical situation for combinations of covalently-linked and solution-based photostabilizers and photoswitching agents. Furthermore we show that intramolecular photostabilizers can protect fluorophores from reversible off-switching events caused by solution-additives, which was previously misinterpreted as photobleaching. Our studies also provide practical guidance for usage of photostabilizer–dye conjugates for STORM-type super-resolution microscopy permitting the exploitation of their improved photophysics for increased spatio-temporal resolution. Finally, we provide evidence that the biochemical environment, e.g., proximity of aromatic amino-acids such as tryptophan, reduces the photostabilization efficiency of commonly used buffer cocktails. Not only have our results important implications for a deeper mechanistic understanding of self-healing dyes, but they will provide a general framework to select label positions for optimal and reproducible photostability or photoswitching kinetics in different biochemical environments.
关键词： photoswitching,intramolecular quenching,self-healing dyes,super-resolution microscopy,intermolecular quenching,photostabilization,fluorophores,triplet-state quenching,STORM
更新于2025-09-19 17:15:36
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Second-order nonlinear optical properties of Stenhouse photoswitches: insights from density functional theory
摘要： We report the first investigation of the second-order nonlinear optical (NLO) properties of donor–acceptor Stenhouse adducts (DASAs), an emerging class of colored photochromes that undergo photoswitching with visible light to a colorless form. By using time-dependent density functional theory, we provide insights into the relationships linking the nature of the chemical substituents to the amplitude and contrasts of the NLO response. Solvent and frequency dispersion effects are also analyzed. The calculations predict that DASAs behave as high contrast NLO switches, a finding that extends their potential applications to photo-responsive NLO materials and devices.
关键词： photoswitching,Stenhouse photoswitches,nonlinear optical properties,density functional theory,second harmonic generation
更新于2025-09-19 17:15:36
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Photoswitching mechanism of a fluorescent protein revealed by time-resolved crystallography and transient absorption spectroscopy
摘要： Reversibly switchable fluorescent proteins (RSFPs) serve as markers in advanced fluorescence imaging. Photoswitching from a non-fluorescent off-state to a fluorescent on-state involves trans-to-cis chromophore isomerization and proton transfer. Whereas excited-state events on the ps timescale have been structurally characterized, conformational changes on slower timescales remain elusive. Here we describe the off-to-on photoswitching mechanism in the RSFP rsEGFP2 by using a combination of time-resolved serial crystallography at an X-ray free-electron laser and ns-resolved pump–probe UV-visible spectroscopy. Ten ns after photoexcitation, the crystal structure features a chromophore that isomerized from trans to cis but the surrounding pocket features conformational differences compared to the final on-state. Spectroscopy identifies the chromophore in this ground-state photo-intermediate as being protonated. Deprotonation then occurs on the μs timescale and correlates with a conformational change of the conserved neighbouring histidine. Together with a previous excited-state study, our data allow establishing a detailed mechanism of off-to-on photoswitching in rsEGFP2.
关键词： time-resolved crystallography,fluorescent proteins,transient absorption spectroscopy,photoswitching,rsEGFP2
更新于2025-09-19 17:13:59
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Ultrafast Terahertz Frequency and Phase Tuning by All‐Optical Molecularization of Metasurfaces
摘要： The integration of photoactive semiconductors exhibiting strong light–matter interactions into functional unit meta-atoms facilitates effective approaches to dynamically manipulate terahertz (THz) waves. Here, a new metaphotonic modulator is proposed and comprehensively studied, which demonstrates extensive tunability of the resonant frequency and phase with the merit of ultrafast photoswitching. Specifically, parallel silicon (Si) bridges are embedded in metasurfaces to reinforce the connection ability, achieving ultrafast optical molecularization from a magnetic quadrupole into an electric dipole. Under femtosecond pulse excitation, the demonstrated resonant frequency tuning range is as high as 40% (from 1.16 to 0.7 THz) and can be further promoted up to 48% (from 1.56 to 0.81 THz) by varying the Si bridge length. Meanwhile, the phase delay at given frequencies can be controlled up to 53.3° without significantly changing the high transmission. Furthermore, the transient frequency switching and phase shifting dynamics are systematically investigated for the first time, showing a full recovery time within 2 ns. By optically molecularizing metasurfaces, extended tuning ranges with regard to the resonant frequency and phase, as well as an ultrafast switching speed, are simultaneously acquired in the proposed metamodulator, which provides deeper insight into the multifunctional active-tuning systems.
关键词： silicon microstructures,ultrafast photoswitching,terahertz metamaterials,molecularization
更新于2025-09-11 14:15:04
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Temporal and reversible control of a DNAzyme by orthogonal photoswitching
摘要： The reversible switching of catalytic systems capable of performing complex DNA computing operations using the temporal control of light is described. Two distinct photoresponsive molecules have been separately incorporated into a split horseradish peroxidase mimicking DNAzyme. We show that its catalytic function can be turned on and off reversibly upon irradiation with specific wavelengths of light. The system responded orthogonally not only to a sophisticated selection of irradiation wavelengths but depended also on different durations of irradiation. Furthermore, the DNAzyme exhibits reversible switching and retains this ability throughout multiple switching cycles. We apply the DNAzyme to act as a light-controlled 4:2 multiplexer. Photoswitchable DNAzyme-based catalysts as introduced here have potential use for controlling complex logical operations and for future applications in DNA nanodevices.
关键词： orthogonal control,nanotechnology,DNAzyme,DNA computing,photoswitching
更新于2025-09-10 09:29:36