Owing to deep activation in biotissues and enhanced targeting efficiency, developing photoresponsive polymer-upconversion nanoparticles (PP-UCNPs) nanovectors has witnessed rapid growth in the past decade. However, up to date, all developed nanovectors require high-order photon processes to initiate the release of cargos. The photodamage caused by high-power near-infrared laser light may be a critical obstacle to their clinical application. Here, for the first time, by leveraging absorption-emission spectral matching between donor-acceptor Stenhouse adducts (DASA) PP and UCNPs (λ , 808 nm) in the green region (≈530 nm), the designed nanovector is capable of releasing cargos at a low-power 808 nm excitation (0.2 W). Considering the high molar absorptivity, biobenign, and synthetic tunability of DASA, DASA PP can be utilized as an up-and-coming candidate to design and synthesize the next generation of upconversion nanovectors without photodamage.
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http://dx.doi.org/10.1002/marc.202100318 | DOI Listing |
Chemistry
March 2025
Instituto de Química, Universidad Nacional Autónoma de México, Ciudad de México, México.
Non-linear optical reactive systems have important applications which require highly localized effects. Recently, we reported for the first time that donor-acceptor Stenhouse adducts (DASAs) have important two-photon switching properties. Here, we report on the nature of the non-linear excitation event and the resulting dynamics through femtosecond-resolved measurements.
View Article and Find Full Text PDFJ Phys Chem B
February 2025
Department of Chemistry, Stanford University, Stanford, California 94305, United States.
Simulating excited-state dynamics or computing spectra for molecules in condensed phases requires sampling the ground state to generate initial conditions. Initial conditions (or snapshots for spectra) are typically produced by QM/MM Boltzmann sampling following MM equilibration or optimization. Given the switch from a MM to a QM/MM potential energy surface, one should discard a set period of time (which we call the "healing time") from the beginning of the QM/MM trajectory.
View Article and Find Full Text PDFLangmuir
January 2025
Polymer Science and Engineering Division, CSIR-National Chemical Laboratory, Dr. Homi Bhabha Road, Pune 411008, India.
2,2-Bis-(methylol)propionic acid-based second-generation polyester dendron amphiphile (T-D) containing visible light-responsive donor-acceptor Stenhouse adduct (DASA) as hydrophobic tails is synthesized. Micelles of T-D amphiphile and its mixed micelles of varying compositions with nonresponsive dendron amphiphile containing lauryl groups are prepared in aqueous solution. In transmission electron microscopy and atomic force microscopy analyses, T-D amphiphiles show rice grain-like ellipsoidal micelles as the predominant morphology.
View Article and Find Full Text PDFACS Macro Lett
February 2025
Department of Chemical Engineering, Key Laboratory of Advanced Materials (MOE), Tsinghua University, Beijing 100084, China.
The microcapsule-containing self-reporting system has attracted attention for its excellent characteristics in visualizing microdamage. In this study, we developed self-reporting materials based on the formation of donor-acceptor Stenhouse adducts (DASA) from microcapsules containing Meldrum's acid furfural conjugate (MAFC). Under mechanical force, MAFC is released from broken microcapsules and forms highly colored DASA with secondary amines in the matrix to indicate the small cracks or deformations.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry, Loker Hydrocarbon Research Institute, University of Southern California, Los Angeles, California 90089, United States.
The development of photoswitches that absorb low energy light is of notable interest due to the growing demand for smart materials and therapeutics necessitating benign stimuli. Donor-acceptor Stenhouse adducts (DASAs) are molecular photoswitches that respond to light in the visible to near-infrared spectrum. As a result of their modular assembly, DASAs can be modified at the donor, acceptor, triene, and backbone heteroatom molecular compartments for the tuning of optical and photoswitching properties.
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