Charged Dots Research Articles

Decoherence in a crystal-phase defined double quantum dot charge qubit strongly coupled to a high-impedance resonator

Decoherence in a crystal-phase defined double quantum dot charge qubit strongly coupled to a high-impedance resonator

An Aged Tree with a New Bloom: A Simple Spatiotemporal Programming Strategy Enables Carbon Dot Photosensitizers to Regulate Cell Pyroptosis for Enhanced Tumor Photodynamic-Immunotherapy.

Pyroptosis induced by photodynamic therapy (PDT) is a promising field in both PDT and immunotherapy for tumors. However, effectively inducing tumor cell pyroptosis while triggering a strong immune response using current photosensitizers remains challenging. Herein, the developed positively charged carbon dots (PCDs) nanoPSs were utilized to modulate tumor cell pyroptosis for the first time through a simple spatiotemporal programming strategy. Briefly, PCDs enabled precisely time-dependent targeting of the cell membrane or lysosome. Upon light irradiation, in vitro studies revealed that lysosome-targeted PDT primarily induced apoptosis, while membrane-targeted PDT triggered pyroptosis, resulting in enhanced PDT efficacy and robust activation of the immune response. Conclusively, in vivo studies demonstrated that PCDs could serve as a novel pyroptosis nanotuner for enhanced photodynamic-immunotherapy, thereby simultaneously eliminating primary tumors and inhibiting distant tumor growth and metastases. This spatiotemporal programming strategy unprecedentedly offers a rejuvenation of aged PSs and expands the biomedical use of CDs in immunotherapy.

Multimodal applications of green carbon dots derived from Potentilla indica (mock strawberry): Antioxidant, antimicrobial, and quenching based quercetin sensor

This study utilized a simple hydrothermal technique to synthesize negatively charged carbon dots from Potentilla indica fruit (MSTCDs) with antioxidant and broad-spectrum antimicrobial properties, as well as a specific capacity to detect quercetin. The characterization of MSTCDs was performed using spectrophotometry (UV–vis, fluorescence, X-ray photoelectron, and Fourier-transform infrared), zeta potential, and transmission electron microscopy. The prepared MSTCDs had an average size of 8 ± 0.22 nm and zeta potential of −21 mV. The prepared MSTCDs showed negligible cytotoxicity and were found to be biocompatible with human microglial cells. MSTCDs used the static quenching and inner filter effect as their two sensing mechanisms to detect quercetin. The fluorescence intensity of the MSTCDs decreased as the dose of quercetin increased, showing a linear correlation within the dose range of 0.01–70 μM (R2 = 0.9980) and the lowest detection limit of 2 nM. The prepared MSTCDs were applied to detect quercetin in the orange and grape juice, yielding values of 3.27 and 7.04 μM, respectively. Further, the MSTCDs displayed antioxidant activity by scavenging 2,2′-azino-bis (3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), 2,2-diphenyl-1-picrylhydrazyl, and hydroxyl radicals, with an EC50 value of 9.3, 140.82, and 187.91 µg/mL, respectively. The antiradical activity of MSTCDs was slightly lower than the ascorbic acid except for ABTS radicals, where MSTCDs showed superior scavenging ability (EC50 = 9.3 µg/mL) compared to the control (EC50 = 33.7 µg/mL). MSTCDs exhibited dose-dependent antimicrobial activity against fungi, Gram-negative bacteria, and Gram-positive bacteria. Thus, the developed CDs showed potential as antioxidant, antimicrobial, and quenching-based quercetin sensor.

Nanogel-Carbon Dot Conjugates: A Synergistic Approach for Enhanced Cancer Treatment through Combination Therapy.

The present study reports the development of a novel nanoconjugate, NG-FACD, comprising a positively charged self-assembled nanogel (NG) derived from a peptide amphiphilic hydrogelator and a negatively charged folic acid-functionalized blue-emitting carbon dot (FACD), bound via electrostatic interactions. NG-FACD was developed to combine the advantages of the individual nanocarriers and overcome their drawbacks. The presence of folic acid enables NG-FACD to be successfully used in selective bioimaging and targeted combination therapy against folate receptor-positive (FR+) B16F10 over FR- cells. NG-FACD demonstrated improved riboflavin (RbF) and paclitaxel (PTX) loading compared to individual nanocarriers that made it ∼1.8- and 1.5-fold more cytotoxic toward FR+ B16F10 cells over RbF- and PTX-loaded individual nanocarriers. The concurrent presence of RbF and PTX on NG-FACD displayed ∼1.9-2.8-fold higher cytotoxicity than single drug-loaded individual nanocarriers and ∼3-4.5-fold higher cytotoxicity through RbF-mediated photodynamic therapy and PTX-induced chemotherapy in synergy compared to free drugs against FR+ B16F10 cells.

Carbon-Dots-Mediated Improvement of Antimicrobial Activity of Natural Products.

The development of new microbicidal compounds has become a top priority due to the emergence and spread of drug-resistant pathogenic microbes. In this study, blue-emitting and positively charged carbon dots (CDs), called Du-CDs, were fabricated for the first time utilizing the natural product extract of endophyte Diaporthe unshiuensis YSP3 as raw material through a one-step solvothermal method, which possessed varied functional groups including amino, carboxyl, hydroxyl, and sulfite groups. Interestingly, Du-CDs exhibited notably enhanced antimicrobial activities toward both bacteria and fungi as compared to the natural product extract of YSP3, with low minimum inhibitory concentrations. Moreover, Du-CDs significantly inhibited the formation of biofilms. Du-CDs bound with the microbial cell surface via electronic interaction or hydrophobic interaction entered the microbial cells and were distributed fully inside the cells. Du-CDs caused cell membrane damage and/or cell division cycle interruption, resulting in microbial cell death. Moreover, Du-CDs exhibited an improved antimicrobial effect and accelerated wound healing ability with good biocompatibility in the mouse model. Overall, we demonstrate that the formation of CDs from fungal natural products presents a promising and potential means to develop novel antimicrobial agents with great fluorescence, improved microbiocidal effect and wound healing capacity, and good biosafety for combating microbial infections.

Construction of a one-stop N-doped negatively charged carbon dot nanoplatform with antibacterial and anti-inflammatory dual activities for wound infection based on biocompatibility

The development of bacterial resistance significantly contributes to the persistence of infections. Although previous studies have highlighted the benefits of metal-doped positive carbon nanodots in managing bacterial wound infections, their mechanism of action is relatively simple and they may pose potential hazards to human cells. Therefore, it is essential to develop a one-stop carbon dot nanoplatform that offers high biocompatibility, antibacterial properties, and anti-inflammatory activities for wound infection management. This study explores the antibacterial efficacy, without detectable resistance, and wound-healing potential of nitrogen-doped (N-doped) negatively charged carbon dots (TPP-CDs). These carbon dots are synthesized using tannic acid (TA), polyethylene polyamine, and polyethylene glycol (PEG) as precursors, with a focus on their biocompatibility. Numerous systematic studies have shown that TPP-CDs can effectively destroy bacterial biofilms and deoxyribonucleic acid (DNA), while also inducing oxidative stress, leading to a potent antimicrobial effect. TPP-CDs also demonstrate the ability to scavenge excess free radicals, promote cellular proliferation, and inhibit inflammatory factors, all of which contribute to improved wound healing. TPP-CDs also demonstrate favorable cell imaging capabilities. These findings suggest that N-doped negatively charged TPP-CDs hold significant potential for treating bacterial infections and offer practical insights for their application in the medical field.

Nanodroplets Engineered with Folate Carbon Dots for Enhanced Cancer Cell Uptake toward Theranostic Application.

The research in nanotherapeutics is rapidly advancing, particularly in the realm of nanoconstructs for drug delivery. This study introduces folate-based carbon dot-decorated nanodroplets (f-Dnm), synthesized from a binary mixture of negatively charged folic acid carbon dots (f-CDs) and cationic-branched polyethylenimine (PEI). The uniformly spherical nanodroplets with an average diameter of 115 ± 15 nm exhibit notable photoluminescence. Surface potential analysis reveals a significant change upon coacervation, attributed to strong electrostatic interactions between f-CD and PEI. The engineered nanodroplets show excellent colloidal and photostability even after 6 months of storage at room temperature. The pH-dependent self-assembly and disassembly properties of f-Dnm are explored for drug loading and release studies using doxorubicin (DOX) as a model anticancer drug. Moreover, the f-Dnm nanocarrier demonstrates significantly higher drug loading capabilities (∼90%). In vitro release studies of doxorubicin-loaded f-Dnm [f-Dnm(DOX)] reveal 5 times higher drug release at lysosomal pH 5.4 compared to that at physiological blood pH 7.4. Cytocompatibility assessments using the MTT assay on HeLa, A549, and NIH-3T3 cells confirm the nontoxic nature of f-Dnm, even at high concentrations. Additionally, f-Dnm(DOX) exhibits higher cytotoxicity in HeLa cells compared to f-CD(DOX) at similar DOX concentrations. Cellular uptake studies show an increased uptake of f-Dnm in folate receptor-positive HeLa and MDA-MB 231 cells. Hemolysis assay validated the biocompatibility of the developed formulation. Overall, these engineered nanodroplets represent a class of nontoxic nanocarriers that offer promising potential as nanotherapeutics for folate receptor-positive cells.

Electropositive Citric Acid-Polyethyleneimine Carbon Dots Carrying the PINK1 Gene Regulate ATP-Related Metabolic Dysfunction in APP/PS1-N2a Cells.

(1) Background: Alzheimer's disease (AD) is characterized by β-amyloid (Aβ) peptide accumulation and mitochondrial dysfunction during the early stage of disease. PINK1 regulates the balance between mitochondrial homeostasis and bioenergy supply and demand via the PINK1/Parkin pathway, Na+/Ca2+ exchange, and other pathways. (2) Methods: In this study, we synthesized positively charged carbon dots (CA-PEI CDs) using citric acid (CA) and polyethyleneimine (PEI) and used them as vectors to express PINK1 genes in the APP/PS1-N2a cell line to determine mitochondrial function, electron transport chain (ETC) activity, and ATP-related metabolomics. (3) Results: Our findings showed that the CA-PEI CDs exhibit the characteristics of photoluminescence, low toxicity, and concentrated DNA. They are ideal biological carriers for gene delivery. PINK1 overexpression significantly increased the mitochondrial membrane potential in APP/PS1-N2a cells and reduced reactive-oxygen-species generation and Aβ1-40 and Aβ1-42 levels. An increase in the activity of NADH ubiquinone oxidoreductase (complex I, CI) and cytochrome C oxidase (complex IV, CIV) induces the oxidative phosphorylation of mitochondria, increasing ATP generation. (4) Conclusions: These findings indicate that the PINK gene can alleviate AD by increasing bioenergetic metabolism, reducing Aβ1-40 and Aβ1-42, and increasing ATP production.

Multilayer pH-responsive hollow mesoporous silica nanoparticles with charge reversal for drug delivery and real-time monitoring by fluorescence

Drug delivery systems (DDSs) with charge reversal could simultaneously achieve long circulation time and enhanced cellular internalization efficiency. Here, hollow mesoporous silica nanoparticles (HMSNs) were used as the basic stuff for encapsulating doxorubicin (DOX), positive-charged chitosan (CS) was grafted on the surface of HMSNs, and negatively charged carboxyl-rich carbon dots (CDs) were coated on the outer layer of CS through non-covalent bonds. The new drug delivery vehicles with 56.6 % drug-loading content were prepared, named as CDs-CS/HMSNs@DOX. Tumor environment with a slightly acidic state could trigger the disruption of the non-covalent bonds, followed by the detachment of CDs, making the negatively charged CDs-CS/HMSNs@DOX change into positively charged CS/HMSNs@DOX. CS swelling reaction also happened in slightly acidic conditions. Both the CS swelling and the detachment of CDs resulted in the exposure of mesopore and drug release. Fluorescence recovery of detached CDs could be used to monitor the release of DOX in real-time. The multilayer pH-responsive nano carries with charge reversal and real-time monitoring demonstrated broad application prospects.

Biophilic Positive Carbon Dot Exerts Antifungal Activity and Augments Corneal Permeation for Fungal Keratitis.

Fungal keratitis (FK) is an infectious eye disease that poses a significant risk of blindness. However, the effectiveness of conventional antifungal drugs is limited due to the intrinsic ocular barrier that impedes drug absorption. There is an urgent need to develop new therapeutic strategies to effectively combat FK. Herein, we synthesized an ultrasmall positively charged carbon dot using a simple stage-melting method. The carbon dot can penetrate the corneal barrier by opening the tight junctions, allowing them to reach the lesion site and effectively kill the fungi. The results both in vitro and in vivo demonstrated that it exhibited good biocompatibility and antifungal activity, significantly improving the therapeutic effect in a mouse model of FK. Therefore, this biophilic ultrasmall size and positive carbon dot, characterized by its ability to penetrate the corneal barrier and its antifungal properties, may offer valuable insights into the design of effective ocular nanomedicines.

Rapid targeting and imaging of mitochondria via carbon dots using an amino acid-based amphiphile as a carrier.

Green-fluorescent biocompatible carbon dots with a quantum yield of 40% were successfully synthesized through a solvothermal process and then they are comprehensively characterized. The carbon dots showed a negatively charged surface owing to the presence of carboxylic groups. This negative surface charge hinders the effective targeting and imaging of mitochondria. To address this limitation, a new approach is developed in this study. An amphiphile containing phenylalanine, with a positively charged polar head consisting of triphenylphosphine and a hydrophobic aliphatic tail, was designed, synthesized, purified, and characterized. This amphiphile formed spherical micelle-type nanostructures in an aqueous medium in the aggregated state. Although these nanoprobes lack inherent fluorescence, they exhibited the capability to image mitochondria when their spherical micelle-type nanostructures were decorated with negatively charged fluorescent nanocarbon dots in both cancerous (KB cells) and non-cancerous (CHO cells) cell lines. Notably, carbon dots without the amphiphile failed to penetrate the cell membrane as they exhibited significantly low emission inside the cell. This study extensively explored the cell entry mechanism of the hybrid nanoprobes. The photophysical changes and the interaction between the negatively charged carbon dots and the positively charged nanospheres of the amphiphile were also analyzed in this study.

A Nanoinhibitor Targeting cGAS-STING Pathway to Reverse the Homeostatic Imbalance of Inflammation in Psoriasis.

Psoriasis is a chronic skin inflammation characterized by dysregulated crosstalk between immune cells and keratinocytes. Here we show that the cyclic GMP-AMP synthase (cGAS)-stimulator of interferon genes (STING) pathway is a key regulator of psoriatic inflammation in a mouse model. Platinum-doped positively charged carbon dots (Pt-CDs) were designed to inhibit the cGAS-STING pathway. By inhibiting the cGAS-STING pathway with Pt-CDs, the secretion of proinflammatory cytokines in macrophages was reduced, and the proinflammatory cytokines-induced breakdown of immunological tolerance and overexpression of chemokines in keratinocytes was restored, which reversed the homeostatic imbalance through breaking these cytokines-mediated intercellular positive feedback loop. Topical Pt-CDs treatment exhibited therapeutic effects in imiquimod-induced psoriasis mice without noticeable toxicity. The reversal of elevated expression of STING, phosphorylated STING, and downstream genes within psoriatic lesions indicates that Pt-CDs effectively inhibit the cGAS-STING pathway. This work suggests a promising strategy for psoriasis treatment by targeting the cGAS-STING pathway with Pt-CDs nanoinhibitor to restore skin homeostatic balance.

Chitosan-PEI passivated carbon dots for plasmid DNA and miRNA-153 delivery in cancer cells

These days carbon dots have been developed for multiple biomedical applications. In the current study, the transfection potential of synthesized carbon dots from single biopolymers such as chitosan, PEI-2kDa, and PEI-25kDa (CS-CDs, PEI2-CDs, and PEI25-CDs) and by combining two biopolymers (CP2-CDs and CP25-CDs) through a bottom-up approach have been investigated. The characterization studies revealed successful synthesis of fluorescent, positively charged carbon dots <20 nm in size. Synthesized carbon dots formed a stable complex with plasmid DNA (EGFP-N1) and miRNA-153 that protected DNA/miRNA from serum-induced degradation. In-vitro cytotoxicity analysis revealed minimal cytotoxicity in cancer cell lines (A549 and MDA-MB-231). In-vitro transfection of EGFP-N1 plasmid DNA with PEI2-CDs, PEI25-CDs and CP25-CDs demonstrated that these CDs could strongly transfect A549 and MDA-MB-231 cells. The highest EGFP-N1 plasmid transfection efficiency was observed with PEI2-CDs at a weight ratio of 32:1. PEI25-CDs polyplex showed maximum transfection at a weight ratio of 8:1 in A549 at a weight ratio of 16:1 in MDA-MB-231 cells. CP25-CDs exhibited the highest transfection at a weight ratio of 16:1 in both cell lines. The in-vitro transfection of target miRNA, i.e., miR-153 in A549 and MDA-MB-231 cells with PEI2-CDs, PEI25-CDs, and CP25-CDs suggested successful transfer of miR-153 into cells which induced significant cell death in both cell lines. Importantly, CS-CDs and CP2-CDs could be tolerated by cells up to 200 μg/mL concentration, while PEI2-CDs, PEI25-CDs, and CP25-CDs showed non-cytotoxic behavior at low concentrations (25 μg/mL). Together, these results suggest that a combination of carbon dots synthesized from chitosan and PEI (CP25-CDs) could be a novel vector for transfection nucleic acids that can be utilized in cancer therapy.

Charge Oscillations in Bilayer Graphene Quantum Confinement Devices.

Quantum confinement structures are building blocks of quantum devices in fundamental physics exploration and technological applications. In this work, we fabricate dual-gated bilayer graphene Fabry-Pérot quantum Hall interferometers employing two different gating strategies and conduct finite element simulations to understand the electrostatics of the confinement structures and to guide device design and fabrication. We observe two types of resistance oscillations arising from the charging of quantum dots formed inside the interferometers. We obtain the size, location, and charging energy of the dots by measuring the dependence of the oscillations on the magnetic field, gate voltages, and dc bias. We analyze and discuss the origin of the quantum dots and their impact on quantum Hall edge state backscattering and interference. Insights gained in these studies shed light on the construction of van der Waals quantum confinement devices.

Tuning Arrays with Rays: Physics-Informed Tuning of Quantum Dot Charge States

Tuning Arrays with Rays: Physics-Informed Tuning of Quantum Dot Charge States

Polysaccharide/Carbon Quantum Dots Composite Film on Model Colloidal Particles-An Electro-Optical Study.

Negatively charged carbon dots (Cdots) were successfully impregnated into chitosan/alginate film formed on model colloidal particles as a result of the attractive interactions with the chitosan molecules. The electrical properties of the produced films were studied by electrokinetic spectroscopy. In this study, the electric light scattering method was applied for first the time for the investigation of suspensions of carbon-based structures. The electro-optical behavior for the suspension of polymer-coated particles showed that the electric polarizability of the particle-covered layer from alginate was significantly higher compared to that of the layer from chitosan due to the higher charge density of alginate. The presence of a low concentration of Cdots in the film results in partial charge screening. It was confirmed that the polarizability of counterions with lower mobility along the adsorbed polyion chains was responsible for the registered electro-optical effect from the suspension of polymer-coated particles and that the participation of diffuse H+ counterions of Cdots in the creation of the electro-optical effect was negligible. The observed oscillation behavior in the evolution of the film thickness was interpreted through the participation of compensatory effects due to the additional adsorption/desorption of polyelectrolyte complexes from the film surface. The concentration of Cdots in the film was determined, and the loaded amount was ca. 6.6 µg/mL per layer.

Using 19F NMR to Investigate Cationic Carbon Dot Association with Per- and Polyfluoroalkyl Substances (PFAS).

There is much concern about per- and polyfluoroalkyl substances (PFAS) based on their environmental persistence and toxicity, resulting in an urgent need for remediation technologies. This study focused on determining if nanoscale polymeric carbon dots are a viable sorbent material for PFAS and developing fluorine nuclear magnetic resonance spectroscopy (19F NMR) methods to probe interactions between carbon dots and PFAS at the molecular scale. Positively charged carbon dots (PEI-CDs) were synthesized using branched polyethyleneimine to target anionic PFAS by promoting electrostatic interactions. PEI-CDs were exposed to perfluorooctanoic acid (PFOA) to assess their potential as a PFAS sorbent material. After exposure to PFOA, the average size of the PEI-CDs increased (1.6 ± 0.5 to 7.8 ± 1.8 nm) and the surface charge decreased (+38.6 ± 1.1 to +26.4 ± 0.8 mV), both of which are consistent with contaminant sorption. 19F NMR methods were developed to gain further insight into PEI-CD affinity toward PFAS without any complex sample preparation. Changes in PFOA peak intensity and chemical shift were monitored at various PEI-CD concentrations to establish binding curves and determine the chemical exchange regime. 19F NMR spectral analysis indicates slow-intermediate chemical exchange between PFOA and CDs, demonstrating a high-affinity interaction. The α-fluorine had the greatest change in chemical shift and highest affinity, suggesting electrostatic interactions are the dominant sorption mechanism. PEI-CDs demonstrated affinity for a wide range of analytes when exposed to a mixture of 24-PFAS, with a slight preference toward perfluoroalkyl sulfonates. Overall, this study shows that PEI-CDs are an effective PFAS sorbent material and establishes 19F NMR as a suitable method to screen for novel sorbent materials and elucidate interaction mechanisms.

Positively Charged Carbon Dots with Antibacterial and Antioxidant Dual Activities for Promoting Infected Wound Healing.

Bacterial infection and excess reactive oxygen species are key factors that lead to slow or substantially delayed wound healing. It is crucial to design and develop new nanomaterials with antibacterial and antioxidative capabilities for wound healing. Here, positively charged carbon dots (CDs) are rationally designed and synthesized from p-phenylenediamine and polyethyleneimine by a facile one-pot solvothermal method, which show good biocompatibility in in vitro cytotoxicity, hemolysis assays, and in vivo toxicity evaluation. The positively charged CDs show superior antimicrobial effect against Staphylococcus aureus (S. aureus) at very low concentrations, reducing the risk of wound infection. At the same time, CDs with surface defects and unpaired electrons can effectively scavenge excess free radicals to reduce oxidative stress damage, accelerate wound inflammation-proliferation transition, and promote wound healing. The mouse model of skin infection demonstrates that CDs can effectively promote the wound healing of skin infection without obvious side effects by simply dropping or spraying onto the wound. We believe that the prepared CDs have satisfactory biocompatibility, antioxidant capacity, and excellent antibacterial activity and have great application potential in wound healing.

Multicomponent hydroxides supported Cu/Cu2O nanoparticles for high efficient photocatalytic ammonia synthesis

Environmentally friendly photocatalytic N2 fixation process has attracted considerable attention. Developing efficient photocatalysts with high electron-hole separation rates and gas adsorption capacities remains quite challenging. Herein, a facile fabrication strategy of Cu-Cu2O and multicomponent hydroxide S-scheme heterojunctions with carbon dot charge mediators is reported. The rational heterostructurebrings excellent N2 absorption ability and high photoinduced electron/hole separation efficiency, and the ammonia produced yield reach above 210 µmol·gcal-1·h−1 during the nitrogen photofixation process. More superoxide and hydroxyl radicals are generated simultaneously in the as-prepared samples under light illumination. This work offers a reasonable construction method to further develop suitable photocatalysts for ammonia synthesis.

Flopping-mode spin qubit in a Si-MOS quantum dot

Spin qubits based on silicon metal-oxide semiconductor (Si-MOS) quantum dots (QDs) are promising platforms for large-scale quantum computers. To control spin qubits in QDs, electric dipole spin resonance (EDSR) has been most commonly used in recent years. By delocalizing an electron across a double quantum dots charge state, “flopping-mode” EDSR has been realized in Si/SiGe QDs. Here, we demonstrate a flopping-mode spin qubit in a Si-MOS QD via Elzerman single-shot readout. When changing the detuning with a fixed drive power, we achieve s-shape spin resonance frequencies, an order of magnitude improvement in the spin Rabi frequencies, and virtually constant spin dephasing times. Our results offer a route to large-scale spin qubit systems with higher control fidelity in Si-MOS QDs.