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1.
Chemistry ; 30(23): e202304174, 2024 Apr 22.
Artículo en Inglés | MEDLINE | ID: mdl-38267371

RESUMEN

Photochemical action plots are a powerful tool for mapping photochemical reaction outcomes wavelength-by-wavelength. Typically, they map either the depletion of a reactant or the formation of a specific product as a function of wavelength. Herein, we exploit action plots to simultaneously map the formation of several photochemical products from a single chromophore. We demonstrate that the wavelength-resolved mapping of two reaction products formed during the irradiation of a chalcone species not only shows wavelength dependence - exhibiting the typical strong red-shift of the photochemical reactivity compared to the absorbance spectrum of the chromophore - but also a strong wavelength selectivity with remarkably different product distributions resulting from different irradiation wavelengths.

2.
Nano Converg ; 10(1): 31, 2023 Jul 04.
Artículo en Inglés | MEDLINE | ID: mdl-37402935

RESUMEN

A tradeoff between light absorption and charge transport is a well-known issue in PbS colloidal quantum dot (CQD) solar cells because the carrier diffusion length in PbS CQD films is comparable to the thickness of CQD film. We reduce the tradeoff between light absorption and charge transport by combining a Fabry-Perot (FP) resonator and a distributed Bragg reflector (DBR). A FP resonance is formed between the DBR and a dielectric-metal-dielectric film as a top transparent electrode. A SiO2-TiO2 multilayer is used to form a DBR. The FP resonance enhances light absorption near the resonant wavelength of the DBR without changing the CQD film thickness. The light absorption near the FP resonance wavelength is further boosted by coupling the FP resonance with the high reflectivity of the Ag-coated DBR. When the FP resonance and DBR are combined, the power conversion efficiency (PCE) of PbS CQD solar cells increases by 54%. Moreover, the DBR assisted FP resonance enables a very thin PbS layer to absorb near infrared light four times more. The overall PCE of the thin PbS CQD solar cell increases by 24% without sacrificing the average visible transmittance (AVT). Our results show how to overcome the inherence problem of the CQD and develop a semi-transparent solar cell where the wavelength-selective absorption and the transparency for visible light are important.

3.
Proc Natl Acad Sci U S A ; 120(25): e2220132120, 2023 06 20.
Artículo en Inglés | MEDLINE | ID: mdl-37307476

RESUMEN

Understanding and predicting the outcome of the interaction of light with DNA has a significant impact on the study of DNA repair and radiotherapy. We report on a combination of femtosecond pulsed laser microirradiation at different wavelengths, quantitative imaging, and numerical modeling that yields a comprehensive picture of photon-mediated and free-electron-mediated DNA damage pathways in live cells. Laser irradiation was performed under highly standardized conditions at four wavelengths between 515 nm and 1,030 nm, enabling to study two-photon photochemical and free-electron-mediated DNA damage in situ. We quantitatively assessed cyclobutane pyrimidine dimer (CPD) and γH2AX-specific immunofluorescence signals to calibrate the damage threshold dose at these wavelengths and performed a comparative analysis of the recruitment of DNA repair factors xeroderma pigmentosum complementation group C (XPC) and Nijmegen breakage syndrome 1 (Nbs1). Our results show that two-photon-induced photochemical CPD generation dominates at 515 nm, while electron-mediated damage dominates at wavelengths ≥620 nm. The recruitment analysis revealed a cross talk between nucleotide excision and homologous recombination DNA repair pathways at 515 nm. Numerical simulations predicted electron densities and electron energy spectra, which govern the yield functions of a variety of direct electron-mediated DNA damage pathways and of indirect damage by •OH radicals resulting from laser and electron interactions with water. Combining these data with information on free electron-DNA interactions gained in artificial systems, we provide a conceptual framework for the interpretation of the wavelength dependence of laser-induced DNA damage that may guide the selection of irradiation parameters in studies and applications that require the selective induction of DNA lesions.


Asunto(s)
Daño del ADN , Electrones , Dímeros de Pirimidina , Reparación del ADN , Rayos Láser
4.
Nanomaterials (Basel) ; 12(19)2022 Sep 22.
Artículo en Inglés | MEDLINE | ID: mdl-36234425

RESUMEN

Perovskite materials offer high-efficiency low-cost solar cells and applications versatility. We report on cesium-based hybrid perovskite solar cells with wavelength-selective properties ranging from 500 nm (UV-VIS) to 800 nm (IR). The band gap tuning was achieved through composition changes of mainly lead(II) iodide PbI2 and lead(II) bromide PbBr2. The optical spectra of the developed materials were studied, including the photoluminescence (PL), optical transparency, X-ray diffraction and external quantum efficiency for samples prepared under different compositions. It was found that a high content of iodine displayed a photoluminescence (PL) peak at 790 nm, whereas a high content of bromine showed a PL peak at 548 nm. The combined composition mixture of PbI2 and PbBr2 can be fine-tuned to prepare materials that absorbed light in the visible range (640-660 nm) or other selective wavelengths in the range from 500 to 800 nm. The illuminated current-voltage characteristics of the solar cells were carried out under the AM 1.5 condition using an ABET solar simulator with a reference solar cell for comparison and control. The average efficiency of the fabricated solar cells ranged from 3.5% to 15.5%, depending on perovskite composition. Wavelength-selective solar cells have potential applications in smart windows, building of integrated PVs and solar-operated greenhouses.

5.
Macromol Rapid Commun ; 43(9): e2200055, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-35338541

RESUMEN

Light-tunable covalent chemistry is highly urgent in the fields of chemistry, biology, and materials science, especially for the smart materials and surface, due to the spatiotemporal control and feasible operation. Here, a new type of wavelength-selective photo-cycloaddition of styryl-anthracene carboxylic acid (SACA) is reported. Upon the irradiation of 450 nm visible light or 365 nm UV light, SACA can undergo [2+2] or [2+4] photocycloaddition, respectively. Furthermore, the [2+2] photocycloaddition induced by vis-light of 450 nm is reversible and can be disrupted by 365 nm UV light to form dimer-24 which cannot be photo-cleavable. Owing to the feasibility and spatiotemporal characteristics of UV-vis light-controlled photocycloaddition, the SACA possesses potential applications in various areas such as self-assembly, dynamic wrinkles, and fluorescence patterns, which are also explored and exhibited in this work.


Asunto(s)
Antracenos , Luz , Reacción de Cicloadición , Polímeros , Rayos Ultravioleta
6.
Adv Mater ; 34(5): e2105868, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-34652041

RESUMEN

Conventional optical diffusers, such as thick volume scatterers (Rayleigh scattering) or microstructured surface scatterers (geometric scattering), lack the potential for on-chip integration and are thus incompatible with next-generation photonic devices. Dielectric Huygens' metasurfaces, on the other hand, consist of 2D arrangements of resonant dielectric nanoparticles and therefore constitute a promising material platform for ultrathin and highly efficient photonic devices. When the nanoparticles are arranged in a random but statistically specific fashion, diffusers with exceptional properties are expected to come within reach. This work explores how dielectric Huygens' metasurfaces can implement wavelength-selective diffusers with negligible absorption losses and nearly Lambertian scattering profiles that are largely independent of the angle and polarization of incident waves. The combination of tailored positional disorder with a carefully balanced electric and magnetic response of the nanoparticles is shown to be an integral requirement for the operation as a diffuser. The proposed metasurfaces' directional scattering performance is characterized both experimentally and numerically, and their usability in wavefront-shaping applications is highlighted. Since the metasurfaces operate on the principles of Mie scattering and are embedded in a glassy environment, they may easily be incorporated in integrated photonic devices, fiber optics, or mechanically robust augmented reality displays.

7.
ACS Appl Mater Interfaces ; 13(37): 44833-44843, 2021 Sep 22.
Artículo en Inglés | MEDLINE | ID: mdl-34499488

RESUMEN

Photoactuated liquid crystalline elastomer (LCE) materials are gaining much attention in many application fields, but challenges for the precise modulation of their photoresponses still exist. Researchers have explored various optical parameters, such as polarization, intensity, and wavelength, to obtain differential responses. The development of photoactuated LCE materials with wavelength-selective responsiveness is more versatile and has attracted more interest, but such LCE materials are commonly prepared by incorporating different molecular chromophores or dyes into the LCE matrices. When the surface plasmon resonance (SPR) characteristic of nanometals, which can generate strong photothermal conversion, and the difference of SPR absorption wavelength bands of different nanometals are considered, a strategy of constructing wavelength-selective actuation of LCE materials by using the SPR photothermal effect can be demonstrated, as done herein. The LCE nanocomposites doped by nanogold or nanosilver were fabricated and exhibited good SPR absorption but in different wavelength bands of the visible spectrum range. They had strong actuation under light irradiation with the wavelengths being inside their respective absorption band but could not be effectively actuated by the light beyond their respective absorption band. A smart electronic device, implementing a hierarchical structured LCE nanocomposite doped by nanogold and nanosilver in different domains as the two-switch actuator, was prepared and capable of outputting different signals in response to the different wavelength bands filtered from a light source, which released the actuator from the restriction of light scanning direction or position. Our work provides new insights for the convenient and precise photoactuation of the LCE actuators.

8.
Adv Mater ; 33(44): e2102967, 2021 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-34515381

RESUMEN

Spectroscopic photodetection plays a key role in many emerging applications such as context-aware optical sensing, wearable biometric monitoring, and biomedical imaging. Photodetectors based on organic semiconductors open many new possibilities in this field. However, ease of processing, tailorable optoelectronic properties, and sensitivity for faint light are still significant challenges. Here, the authors report a novel concept for a tunable spectral detector by combining an innovative transmission cavity structure with organic absorbers to yield narrowband organic photodetection in the wavelength range of 400-1100 nm, fabricated in a full-vacuum process. Benefiting from this strategy, one of the best performed narrowband organic photodetectors is achieved with a finely wavelength-selective photoresponse (full-width-at-half-maximum of ≈40 nm), ultrahigh specific detectivity above 1014 Jones, the maximum response speed of 555 kHz, and a large dynamic range up to 168 dB. Particularly, an array of transmission cavity organic photodetectors is monolithically integrated on a small substrate to showcase a miniaturized spectrometer application, and a true proof-of-concept transmission spectrum measurement is successfully demonstrated. The excellent performance, the simple device fabrication as well as the possibility of high integration of this new concept challenge state-of-the-art low-noise silicon photodetectors and will mature the spectroscopic photodetection into technological realities.

9.
Adv Healthc Mater ; 9(7): e1901553, 2020 04.
Artículo en Inglés | MEDLINE | ID: mdl-32100475

RESUMEN

Photoresponsive materials have been widely used in vitro for controlled therapeutic delivery and to direct 4D cell fate. Extension of the approaches into a bodily setting requires use of low-energy, long-wavelength light that penetrates deeper into and through complex tissue. This review details recent reports of photoactive small molecules and proteins that absorb visible and/or near-infrared light, opening the door to exciting new applications in multiplexed and in vivo regulation.


Asunto(s)
Hidrogeles , Rayos Infrarrojos , Proteínas
10.
ACS Nano ; 13(2): 2127-2135, 2019 Feb 26.
Artículo en Inglés | MEDLINE | ID: mdl-30706707

RESUMEN

Organic photodiodes (OPDs), based on organic semiconductors with high absorption coefficients for visible light, are emerging as potential candidates for replacing silicon photodiodes in image sensors, particularly due to the possibility of realizing a thin thickness and exclusion of color filters, both of which can contribute to a dramatically enhanced degree of integration for image sensors. Despite years of research, techniques have not yet been developed that allow the OPD itself to have color selectivity while maintaining a thin (<1 µm) OPD thickness, in combination with a sufficiently high detectivity (>1012 cm·Hz0.5/W). To solve this issue, we introduce a concept of "etalon-electrode", which can perform the function of electrode and simultaneously the function of selective wavelength transparency. A strategically designed OPD architecture consisting of an etalon-electrode, a panchromatic organic active layer, and a counter electrode displays well-defined narrowband R-/G-/B-selective detectivity spectra depending on precision-adjusted thickness composition of the etalon-electrode. While a thin thickness of OPD is preserved at less than 800 nm including electrodes, active layer, and other buffer layers for all R-/G-/B-selective OPDs, high average detectivity values over 1012 cm·Hz0.5/W are demonstrated. Furthermore, the characteristic of imparting color selectivity by the etalon-electrode enables a more facile full color patterning, such that a prototype of a 10 × 10 image sensor with a pixel pitch of 500 µm is realized, resulting in accurate picturing of a well-defined full color image.

11.
Adv Sci (Weinh) ; 5(8): 1800446, 2018 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-30128251

RESUMEN

Independent control over multiple cell-material interactions with high spatiotemporal resolution is a key for many biomedical applications and understanding cell biology, as different cell types can perform different tasks in a multicellular context. In this study, the binding of two different cell types to materials is orthogonally controlled with blue and red light providing independent regulation in space and time. Cells expressing the photoswitchable protein cryptochrome 2 (CRY2) on cell surface bind to N-truncated CRY-interacting basic helix-loop-helix protein 1 (CIBN)-immobilized substrates under blue light and cells expressing the photoswitchable protein phytochrome B (PhyB ) on cell surface bind to phytochrome interaction factor 6 (PIF6)-immobilized substrates under red light, respectively. These light-switchable cell interactions provide orthogonal and noninvasive control using two wavelengths of visible light. Moreover, both cell-material interactions are dynamically switched on under light and reversible in the dark. The specificity of the CRY2/CIBN and PhyB/PIF6 interactions and their response to different wavelengths of light allow selectively activating the binding of one cell type with blue and the other cell type with red light in the presence of the other cell type.

12.
Materials (Basel) ; 11(5)2018 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-29786650

RESUMEN

Radiative thermal transport of metamaterials has begun to play a significant role in thermal science and has great engineering applications. When the key features of structures become comparable to the thermal wavelength at a particular temperature, a narrowband or wideband of wavelengths can be created or shifted in both the emission and reflection spectrum of nanoscale metamaterials. Due to the near-field effect, the phenomena of radiative wavelength selectivity become significant. These effects show strong promise for applications in thermophotovoltaic energy harvesting, nanoscale biosensing, and increased energy efficiency through radiative cooling in the near future. This review paper summarizes the recent progress and outlook of both near-field and far-field radiative heat transfer, different design structures of metamaterials, applications of unique thermal and optical properties, and focuses especially on exploration of the tunable radiative wavelength selectivity of nano-metamaterials.

13.
Front Neural Circuits ; 12: 16, 2018.
Artículo en Inglés | MEDLINE | ID: mdl-29527156

RESUMEN

Many visual animals exploit spectral information for seeking food and mates, for identifying preys and predators, and for navigation. Animals use chromatic information in two ways. "True color vision," the ability to discriminate visual stimuli on the basis of their spectral content independent of brightness, is thought to play an important role in object identification. In contrast, "wavelength-specific behavior," which is strongly dependent on brightness, often associates with foraging, navigation, and other species-specific needs. Among animals capable of chromatic vision, insects, with their diverse habitats, stereotyped behaviors, well-characterized anatomy and powerful genetic tools, are attractive systems for studying chromatic information processing. In this review, we first discuss insect photoreceptors and the relationship between their spectral sensitivity and animals' color vision and ecology. Second, we review recent studies that dissect chromatic circuits and explore neural mechanisms of chromatic information processing. Finally, we review insect behaviors involving "true color vision" and "wavelength-specific behaviors," especially in bees, butterflies, and flies. We include examples of high-order color vision, such as color contrast and constancy, which are shared by vertebrates. We focus on Drosophila studies that identified neuronal correlates of color vision and innate spectral preferences. We also discuss the electrophysiological studies in bees that reveal color encoding. Despite structural differences between insects' and vertebrates' visual systems, their chromatic vision appears to employ the same processing principles, such as color opponency, suggesting convergent solutions of neural computation to common problems.


Asunto(s)
Visión de Colores/fisiología , Insectos/fisiología , Animales , Conducta Animal/fisiología , Percepción de Color/fisiología , Insectos/anatomía & histología , Células Fotorreceptoras de Invertebrados/citología , Células Fotorreceptoras de Invertebrados/fisiología
14.
Angew Chem Int Ed Engl ; 56(45): 14306-14309, 2017 11 06.
Artículo en Inglés | MEDLINE | ID: mdl-28857401

RESUMEN

Star-shaped polymers represent highly desired materials in nanotechnology and life sciences, including biomedical applications (e.g., diagnostic imaging, tissue engineering, and targeted drug delivery). Herein, we report a straightforward synthesis of wavelength-selective multifunctional photoinitiators (PIs) that contain a bisacylphosphane oxide (BAPO) group and an α-hydroxy ketone moiety within one molecule. By using three different wavelengths, these photoactive groups can be selectively addressed and activated, thereby allowing the synthesis of ABC-type miktoarm star polymers through a simple, highly selective, and robust free-radical polymerization method. The photochemistry of these new initiators and the feasibility of this concept were investigated in unprecedented detail by using various spectroscopic techniques.

15.
Adv Mater ; 29(33)2017 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-28675522

RESUMEN

Spectroscopic photodetection is a powerful tool in disciplines such as medical diagnosis, industrial process monitoring, or agriculture. However, its application in novel fields, including wearable and biointegrated electronics, is hampered by the use of bulky dispersive optics. Here, solution-processed organic donor-acceptor blends are employed in a resonant optical cavity device architecture for wavelength-tunable photodetection. While conventional photodetectors respond to above-gap excitation, the cavity device exploits weak subgap absorption of intermolecular charge-transfer states of the intercalating poly[2,5-bis(3-tetradecylthiophen-2-yl)thieno[3,2-b]thiophene] (PBTTT):[6,6]-phenyl-C61-butyric acid methyl ester (PCBM) bimolecular crystal. This enables a highly wavelength selective, near-infrared photoresponse with a spectral resolution down to 14 nm, as well as dark currents and detectivities comparable with commercial inorganic photodetectors. Based on this concept, a miniaturized spectrophotometer, comprising an array of narrowband cavity photodetectors, is fabricated by using a blade-coated PBTTT:PCBM thin film with a thickness gradient. As an application example, a measurement of the transmittance spectrum of water by this device is demonstrated.

16.
Sci Adv ; 3(4): e1602697, 2017 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-28439553

RESUMEN

The search for higher-performance photothermal microactuators has typically involved unavoidable trade-offs that hinder the demonstration of ubiquitous devices with high energy density, speed, flexibility, efficiency, sensitivity, and multifunctionality. Improving some of these parameters often implies deterioration of others. Photothermal actuators are driven by the conversion of absorbed optical energy into thermal energy, which, by different mechanisms, can produce mechanical displacement of a structure. We present a device that has been strategically designed to show high performance in every metric and respond to optical radiation of selected wavelength bands. The device combines the large energy densities and sensitivity of vanadium dioxide (VO2)-based actuators with the wavelength-selective absorption properties of single-walled carbon nanotube (SWNT) films of different chiralities. SWNT coatings increased the speed of VO2 actuators by a factor of 2 while decreasing the power consumption by approximately 50%. Devices coated with metallic SWNT were found to be 1.57 times more responsive to red light than to near-infrared, whereas semiconducting SWNT coatings resulted in 1.42 times higher responsivities to near-infrared light than to red light. The added functionality establishes a link between optical and mechanical domains of high-performance photoactuators and enables the future development of mechanical logic gates and electronic devices that are triggered by optical radiation from different frequency bands.

17.
Angew Chem Int Ed Engl ; 55(31): 8948-52, 2016 07 25.
Artículo en Inglés | MEDLINE | ID: mdl-27294300

RESUMEN

We successfully introduced two-photon-sensitive photolabile groups ([7-(diethylamino)coumarin-4-yl]methyl and p-dialkylaminonitrobiphenyl) into DNA strands and demonstrated their suitability for three-dimensional photorelease. To visualize the uncaging, we used a fluorescence readout based on double-strand displacement in a hydrogel and in neurons. Orthogonal two-photon uncaging of the two cages is possible, thus enabling complex scenarios of three-dimensional control of hybridization with light.


Asunto(s)
Color , ADN/química , Hibridación de Ácido Nucleico , Fotones
18.
Adv Mater ; 26(29): 5012-7, 2014 Aug 06.
Artículo en Inglés | MEDLINE | ID: mdl-24831417

RESUMEN

Polyurethane thin films that photopolymerize and photodegrade upon exposure to light of different wavelengths are presented. The chromic response is based on two caged monomers with the ability to be activated or photocleaved with different wavelengths under single and two-photon excitation. This material represents a dual photoresist with "positive" and "negative" tone contained in a single resist formulation and with the ability to generate complex 2D and 3D patterns.


Asunto(s)
Luz , Procesos Fotoquímicos , Polímeros/química , Nitrocompuestos/química , Polimerizacion
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