Traditional antibacterial procedures are getting inefficient due to the emergence of antimicrobial resistance, which makes alternative treatments in urgent demand. However, the selectivity toward ...infectious bacteria is still challenging. Herein, by taking advantage of the self-directed capture of infectious bacteria by macrophages, we developed a strategy to realize precise in vivo antibacterial photodynamic therapy (APDT) through adoptive photosensitizer-loaded macrophage transfer. TTD with strong reactive oxygen species (ROS) production and bright fluorescence was first synthesized and was subsequently formulated into TTD nanoparticles for lysosome targeting. TTD-loaded macrophages (TLMs) were constructed by direct incubation of TTD nanoparticles with macrophages, in which the TTD was localized in the lysosomes to meet the captured bacteria in the phagolysosomes. The TLMs could precisely capture and eradicate bacteria while being activated toward the proinflammatory and antibacterial M1 phenotype upon light illumination. More importantly, after subcutaneous injection, TLMs could effectively inhibit bacteria in the infected tissue through APDT, leading to good tissue recovery from severe bacterial infection. Overall, the engineered cell-based therapeutic approach shows great potential in the treatment of severe bacterial infectious diseases.
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IJS, KILJ, NUK, PNG, UL, UM
Chemical modification of phenothiazine‐benzophenone derivatives tunes the emission behavior from triplet states by selecting the geometry of the intramolecular charge transfer (ICT) state. A ...fundamental principle of planar ICT (PICT) and twisted ICT (TICT) is demonstrated to obtain selectively either room temperature phosphorescence (RTP) or thermally activated delayed fluorescence (TADF), respectively. Time‐resolved spectroscopy and time‐dependent density functional theory (TD‐DFT) investigations on polymorphic single crystals demonstrate the roles of PICT and TICT states in the underlying photophysics. This has resulted in a RTP molecule OPM, where the triplet states contribute with 89 % of the luminescence, and an isomeric TADF molecule OMP, where the triplet states contribute with 95 % of the luminescence.
Strukturmodifikationen, die zur Bildung einer planaren bzw. verdrehten intramolekularen Ladungstransfergeometrie (PICT oder TICT) führen, ermöglichen die schnelle und effiziente Nutzung von Triplettzuständen zur Erzeugung von Raumtemperaturphosphoreszenz (RTP) bzw. hocheffizienter thermisch aktivierter verzögerter Fluoreszenz (TADF).
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Fluorescent probes capable of in vivo lipids labeling are highly desirable for studying lipid‐accumulation‐related metabolic diseases, such as nonalcoholic fatty liver disease, type‐2 diabetes, and ...atherosclerosis. However, most of the current lipid‐specific fluorophores cannot be used for in vivo labeling due to their strong hydrophobicity. Herein, organic dots from bright luminogens with aggregation‐induced emission (AIEgen) are developed for in vivo labeling and three‐photon fluorescence imaging of lipid‐rich tissues, such as fatty liver, atherosclerotic plaques in brain vasculatures, and carotid arteries. The organic dots show excellent stability in an aqueous medium with high targeting specificity to lipids and strong three‐photon fluorescence in the far‐red/near‐infrared (NIR) region under NIR‐II laser excitation, which enables efficient in vivo labeling and imaging of lipids in deep tissues. The study will inspire the development of lipid‐targeting fluorophores for in vivo applications.
Stable aggregation‐induced‐emission (AIE) dots in an aqueous medium are synthesized for in vivo labeling of lipids. The ultrabright fluorescence in the far‐red/near‐infrared (NIR) region (quantum yield of 26%) enables intravital three‐photon fluorescence imaging of lipids in fatty liver and atherosclerotic plaques in brain vasculatures and carotid arteries under NIR‐II laser excitation.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
The precise treatment of cancer requires maximized lesion to cancer cells and minimized damage to normal cells; however, the current theranostic nanomaterials have limited generic theranostic ...specificity to cancer cells. Herein, as a proof of concept, a small-molecular system simultaneously possessing on-site fluorescence light-up feature, universal cancer cell selectivity, controllable subcellular localization, and activated therapeutic function is developed for cancer theranostics. These molecular probes are composed of photosensitizers (PSs) with the aggregation-induced emission (AIE) feature as the core and aliphatic chains containing lipophilic cations as the arms, which show fluorescence light-up upon entering cancer cells. The charges and lipophilicity of these light-up probes are fine-tuned by the number of lipophilic cations, which modulate their cancer cell selectivity and subcellular localization, where the synthesized AIE PS with four positive charges (TPETM-4+) shows the highest differentiation toward all tested cancer cells over normal ones; neutrally charged TPETM-2 with two arms stains the cytoplasm, TPETM-2+ with two positive charges stains the mitochondria, while TPETM-4+ labels the lysosome. Moreover, under light irradiation, TPETM-4+ exhibits specific photodynamic ablation toward cancer cells over normal ones. This study proposes a new approach to design delivery systems for generic cancer cell selectivity with subcellular localization control, which opens up new opportunities for precise cancer therapy.
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IJS, KILJ, NUK, PNG, UL, UM
We report an in-depth photophysical investigation of an asymmetric donor–acceptor–donor′ (D–A–D′) thermally activated delayed fluorescence (TADF) molecule ...(4-(9H-carbazol-9-yl)phenyl)(4-(10H-phenothiazin-10-yl)phenyl)sulfone and compare its photophysical properties to the parent symmetric D–A–D and D′–A–D′ molecules. These D–A–D type small molecules all show strong TADF. The work reveals how the relative orientations of D–A (D′–A) moieties favor reverse intersystem crossing (rISC) by forming stable charge transfer (CT) states. The key requirement for the efficient TADF emitters is to achieve a very small CT-local triplet state energy splitting, which is shown to be complex in the asymmetric molecule. Throughout the investigations, we show that in the asymmetric D–A–D′ system, even though E CT (D–A) > E CT (D′–A), no evidence of energy transfer from D–A to A–D′ is observed, nor from excited D to D′. This is ascribed to the near orthogonality of the D and D′ units and the very strong decoupling of the electrons on the D and A in the CT state. In addition, the possibility of aggregation-induced TADF (AI-TADF) is examined and shown to be a manifestation of solvatochromism in these particular molecules.
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Isomerization is an essential chemical process that often evokes dramatic change of chemical, physical, or biological properties. For a long time, isomerization has been known as a transformation ...that is induced by certain external energy such as light, heat, or mechanical force. Herein, a new isomerization phenomenon is described, which does not require external energy but simply occurs during molecular packing. The proposed isomerization is demonstrated by a series of symmetric donor–acceptor–donor (D–A–D) molecules, the donor of which may adopt two different stereoisomeric forms. Based on the evidence of the asymmetric isomers in crystals, the occurrence of isomerization during molecular packing is proved. Moreover, the unique asymmetric geometry in the solid state favors the restriction of intramolecular motion, resulting in highly efficient organic solids with quantum yields approaching unity.
A new isomerization phenomenon occurring during molecular packing is reported. Such a new type of isomerization tends to offer tight molecular packing with fewer voids in stacking, resulting in unique packing with abundant CH…π interactions. The unique packing in the solid state favors the restriction of intramolecular motion, resulting in highly efficient organic solids with quantum yields approaching unity.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
•A developed 6-dye, 29-plex Y-STR kit, for improved Y-STR genotyping ability.•Validation of the Microreader™ 29Y Prime ID System, following SWGDAM guidelines.•Sufficiently sensitive to detect DNA as ...low as 0.0625ng.•High stability against PCR inhibitors that commonly exist forensic samples.•High concordance between Yfiler® Plus Kit and Microreader™ 29Y Prime ID System.
Currently, Y-short tandem repeat loci (Y-STRs) have been increasingly used in the forensic field, particularly in investigations of sexual assault, determination of paternity and male lineage studies because of the characteristics of male-only and paternal inheritance. The Microreader™ 29Y Prime ID system is a 29-plex Y-STR genotyping system that amplifies 17 widely used commercial loci (DYS570, DYS546, DYS460, DYS458, DYS635, DYS533, DYS448, DYS627, DYS456, DYS576, DYS449, DYS437, DYS643, DYS518, DYF387S1 a/b, and a sexual locus Y GATA H4), European recommended 7 single-copy “minimal haplotypes” (DYS19, DYS389I, DYS389II, DYS390, DYS391, DYS392, DYS393, and DYS385a/b) and 2 additional loci (DYS438 and DYS439) recommended by The Scientific Working Group on DNA Analysis Methods (SWGDAM).
The Microreader™ 29Y Prime ID system was validated according to the guidelines of “Validation Guidelines for DNA Analysis Methods (2016)” described by the Scientific Working Group on DNA Analysis Methods (SWGDAM), including PCR-based, sensitivity, precision and accuracy evaluation, stutter percentage and peak height ratio, inhibitors, species specificity and DNA mixture studies. This study indicates that the Microreader™ 29Y Prime ID system is a useful tool for forensic cases and Y-STR genotyping.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Nanocrystals (NCs) are widely used in optoelectronics, photocatalysis, and bioimaging. As the surface area to volume ratio increases with a decrease in the size of NCs, strategies to control the size ...of NCs are highly valuable for many applications. Given the importance of photoluminescent dyes, especially those with aggregation‐induced emission, the transformation from an amorphous to a crystalline state can yield a drastic enhancement in their optical properties, which is of significance for biomedical applications. Till now, there is no general method available for the synthesis of small NCs with accurate control over the size and uniformity. Herein, a simple and general approach of ouzo nanocrystallization is presented for the synthesis of small (<100 nm) and highly uniform (polydispersity index~0.1) NCs with good control over the size. The process of nanoprecipitation is used to synthesize uniform nanoparticles (NPs) with different size, which is followed by solvent addition to form swollen NPs. Further, the amorphous core of swollen NPs is converted into NCs within polymer shell under Ouzo zone, which restricts NCs to grow above certain size. To demonstrate the general applicability of ouzo nanocrystallization, two different classes of luminescent materials are used as examples to fabricate small and highly uniform NCs.
Nanocrystals have shown tremendous progress and great promises in biomedical, photocatalytic, and optoelectronic applications. Till now, methods available for the synthesis of polymer encapsulated nanocrystals are slow, lack controllability, and are not generic. In this study, we present the method of ouzo crystallization for fast, systematic, and controlled synthesis of small organic NCs (<100 nm) with high uniformity (PDI~0.1).
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The biodegradation characteristic and potential metabolic pathway for removal of environmental N,N-dimethylacetamide （DMAC） by Rhodococcus sp. strain B83 was studied. Rhodococcus sp. strain B83 was ...isolated from the rhizosphere of a pagoda tree and proved capable of utilizing DMAC as sole source of carbon and nitrogen. Batch culture studies showed that strain B83 could tolerate up to 25 g/L DMAC and showed distinct growth on possible catabolic intermediates except for acetate. The nitrogen balance analysis revealed that approximately 71% of the initial nitrogen was converted to organic nitrogen. DMAC degradation has led to accumulation of acetate and organic nitrogen, meanwhile traces of nitrate and ammonia was build-up but without nitrite. The growth of strain B83 could be inhibited by adding exogenous acetate. By means of the assay of enzymatic degradation of DMAC, several catabolic intermediates at different intervals were observed and identified. Based on the results obtained from culture solution and enzymatic degradation assay, a detailed pathway is proposed for DMAC biodegradation.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
•A 6-dye, 38-plex Y-STR kit for improved power of discrimination.•Highly sensitive to detect DNA as low as 0.0625 ng.•Stable performance against various PCR inhibitors.
Y-STR is widely used in sexual ...assaults and familial searches of suspects. Here, we reported a novel 38-plex STR genotyping system designed for forensic applications. Microreader™ Y Prime Plus ID System (YPP) amplifies 38 loci in one reaction, including 29 loci from commonly used Yfiler® Plus PCR Amplification Kit & PowerPlex® Y23 System (DYS393, DYS570, DYS19, DYS392, DYS549, Y GATA H4, DYS460, DYS458, DYS481, DYS635, DYS448, DYS533, DYS449, DYS456, DYS389I, DYS390, DYS389Ⅱ, DYS438, DYS391, DYS439, DYS437, DYS385a/b, DYS643, DYS518, DYS576, DYF387S1a/b, and DYS627), 6 commonly used loci for the Y-STR database (DYS444, DYS447, DYS596, DYF404a/b, DYS527a/b, DYS557) and one Y-indel specific for the Chinese population. YPP is designed for different types of samples, such as blood card and swabs. In this work, YPP was validated following SWGDAM guidelines (2016) and guidelines from Ministry of Public Security of the People’s Republic of China, including PCR-based, sensitivity, accuracy and precision, mixture, stability and inhibitor, and species specificity. The results indicate that the Microreader™ Y Prime Plus ID System is a powerful identification kit designed for forensic databases.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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