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1.
Sci Rep ; 14(1): 14412, 2024 06 22.
Artigo em Inglês | MEDLINE | ID: mdl-38909025

RESUMO

Access to individual-level health data is essential for gaining new insights and advancing science. In particular, modern methods based on artificial intelligence rely on the availability of and access to large datasets. In the health sector, access to individual-level data is often challenging due to privacy concerns. A promising alternative is the generation of fully synthetic data, i.e., data generated through a randomised process that have similar statistical properties as the original data, but do not have a one-to-one correspondence with the original individual-level records. In this study, we use a state-of-the-art synthetic data generation method and perform in-depth quality analyses of the generated data for a specific use case in the field of nutrition. We demonstrate the need for careful analyses of synthetic data that go beyond descriptive statistics and provide valuable insights into how to realise the full potential of synthetic datasets. By extending the methods, but also by thoroughly analysing the effects of sampling from a trained model, we are able to largely reproduce significant real-world analysis results in the chosen use case.


Assuntos
Análise de Dados , Humanos , Estudos Longitudinais , Inteligência Artificial
2.
Cells ; 13(6)2024 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-38534379

RESUMO

Disulfiram (DSF), an anti-alcoholism medicine, exerts treatment effects in patients suffering from persistent Borreliosis and also exhibits anti-cancer effects through its copper chelating derivatives and induction of oxidative stress in mitochondria. Since chronic/persistent borreliosis is characterized by increased amounts of pro-inflammatory macrophages, this study investigated opsonin-independent phagocytosis, migration, and surface marker expression of in vivo activated and in vitro cultured human monocyte-derived phagocytes (macrophages and dendritic cells) with and without DSF treatment. Phagocytosis of non-opsonized Dynabeads® M-450 and migration of macrophages and dendritic cells were monitored using live cell analyzer Juli™ Br for 24 h, imaging every 3.5 min. To simultaneously monitor phagocyte function, results were analyzed by a newly developed software based on the differential phase contrast images of cells before and after ingestion of Dynabeads. DSF decreased the phagocytic capacities exhibited by in vitro enriched and long-lived phagocytes. Although no chemotactic gradient was applied to the test system, vigorous spontaneous migration was observed. We therefore set up an algorithm to monitor and quantify both phagocytosis and migration simultaneously. DSF not only reduced phagocytosis in a majority of these long-lived phagocytes but also impaired their migration. Despite these selective effects by DSF, we found that DSF reduced the expression densities of surface antigens CD45 and CD14 in all of our long-lived phagocytes. In cells with a high metabolic activity and high mitochondrial contents, DSF led to cell death corresponding to mitochondrial oxidative stress, whereas metabolically inactive phagocytes survived our DSF treatment protocol. In conclusion, DSF affects the viability of metabolically active phagocytes by inducing mitochondrial stress and secondly attenuates phagocytosis and migration in some long-lived phagocytes.


Assuntos
Dissulfiram , Proteínas Opsonizantes , Humanos , Dissulfiram/farmacologia , Fagocitose , Fagócitos , Macrófagos
3.
Bioengineering (Basel) ; 10(5)2023 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-37237593

RESUMO

BACKGROUND: Endoscopic retrograde cholangiopancreatography (ERCP) is crucial to the treatment of biliopancreatic diseases with iatrogenic perforation as a potential complication. As of yet, the wall load during ERCP is unknown, as it is not directly measurable during an ERCP in patients. METHODS: In a life-like, animal-free model, a sensor system consisting of five load cells was attached to the artificial intestines (sensors 1 + 2: pyloric canal-pyloric antrum, sensor 3: duodenal bulb, sensor 4: descending part of the duodenum, sensor 5: distal to the papilla). Measurements were made with five duodenoscopes (n = 4 reusable and n = 1 single use). RESULTS: Fifteen standardized duodenoscopies were performed. Peak stresses were found at the antrum during the gastrointestinal transit (sensor 1 max. 8.95 N, sensor 2 max. 2.79 N). The load reduced from the proximal to the distal duodenum and the greatest load in the duodenum was discovered at the level of the papilla in 80.0% (sensor 3 max. 2.06 N). CONCLUSIONS: For the first time, intraprocedural load measurements and exerting forces obtained during a duodenoscopy for ERCP in an artificial model were recorded. None of the tested duodenoscopes were classified as dangerous for patient safety.

4.
Eur Radiol ; 33(4): 2461-2468, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36477938

RESUMO

OBJECTIVES: Photon-counting computed tomography has lately found its way into clinical routine. The new technique could offer substantial improvements regarding general image quality, image noise, and radiation dose reduction. This study evaluated the first abdominal examinations in clinical routine and compared the results to conventional computed tomography. METHODS: In this single-center retrospective study, 66 patients underwent photon-counting and conventional abdominal CT. Four radiologists assessed general image quality, image noise, and image artifacts. Signal-to-noise ratio and dose properties of both techniques within the clinical application were compared. An ex vivo phantom study revealed the radiobiological impact by means of DNA double-strand break foci in peripheral blood cells by enumerating γ-H2AX+53BP1 foci. RESULTS: General image quality in accordance with the Likert scale was found superior for photon-counting CT (4.74 ± 0.46 vs. 4.25 ± 0.54; p < 0.001). Signal-to-noise ratio (p < 0.001) and also dose exposure were higher for photon-counting CT (DLP: 419.2 ± 162.2 vs. 372.3 ± 236.6 mGy*cm; p = 0.0435). CT exposure resulted in significantly increased DNA damage in comparison to sham control (p < 0.001). Investigation of the average foci per cell and radiation-induced foci numbers revealed significantly elevated numbers (p = 0.004 and p < 0.0001, respectively) after photon-counting CT. CONCLUSION: Photon-counting CT in abdominal examinations showed superior results regarding general image quality and signal-to-noise ratio in clinical routine. However, this seems to be traded for a significantly higher dose exposure and corresponding double-strand break frequency. Optimization of standard protocols in further clinical applications is required to find a compromise regarding picture quality and dose exposure. KEY POINTS: • Photon-counting computed tomography promises to enhance the diagnostic potential of medical imaging in clinical routine. • Retrospective single-center study showed superior general image quality accompanied by higher dose exposure in initial abdominal PCCT protocols compared to state-of-the-art conventional CT. • A simultaneous ex vivo phantom study revealed correspondingly increased frequencies of DNA double-strand breaks after PCCT.


Assuntos
DNA , Tomografia Computadorizada por Raios X , Humanos , Estudos Retrospectivos , Doses de Radiação , Tomografia Computadorizada por Raios X/métodos , Razão Sinal-Ruído , Imagens de Fantasmas
5.
ACS Appl Mater Interfaces ; 14(51): 56963-56974, 2022 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-36515688

RESUMO

Chalcogenide alloys are key materials for selector and memory elements used in next-generation nonvolatile memory cells. However, the high electric fields and Joule heating experienced during operation can promote interdiffusion at the interfaces that degrade device performance over time. A clear atomic scale understanding of how chalcogenide alloys interact with electrodes could aid in identifying ways to improve long-term device endurance. In this work, we develop a robust set of moment tensor potentials (MTPs) to examine interactions between Ge-Se alloys and Ti electrodes. Previous works have shown evidence of strong interactions between Ti and chalcogenide alloys. This system offers an important first test in the use of ML empirical potentials to understand the role of interfaces in endurance in memory elements and broader nanoscale devices. The empirical potentials are constructed using an active learning moment tensor potential framework that leverages a broad data set of first-principles calculations for Ti, Ge, and Se compounds. Long-term simulations (>1 ns) show significant interdiffusion at the Ti|Ge-Se interface with Ti and Se both actively moving across the original interface. The strong chemical affinity of Ti and Se leads to a well-defined Ti-Se region and a severely Se-depleted central Ge-Se region with unfavorable selector characteristics. The evolution of the Ti-Se layer can be described using a self-limited growth model. By comparing effective Ti-Se diffusion constants for simulations at different temperatures, we find a low activation energy of 0.1 eV for Ti-Se layer interdiffusion.

6.
Molecules ; 27(12)2022 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-35744975

RESUMO

Adsorption of carbon dioxide (CO2), as well as many other kinds of small molecules, is of importance for industrial and sensing applications. Metal-organic framework (MOF)-based adsorbents are spotlighted for such applications. An essential for MOF adsorbent application is a simple and easy fabrication process, preferably from a cheap, sustainable, and environmentally friendly ligand. Herein, we fabricated a novel structural, thermally stable MOF with fluorescence properties, namely Zn [5-oxo-2,3-dihydro-5H-[1,3]-thiazolo [3,2-a]pyridine-3,7-dicarboxylic acid (TPDCA)] • dimethylformamide (DMF) •0.25 H2O (coded as QUF-001 MOF), in solvothermal conditions by using zinc nitrate as a source of metal ion and TPDCA as a ligand easy accessible from citric acid and cysteine. Single crystal X-ray diffraction analysis and microscopic examination revealed the two-dimensional character of the formed MOF. Upon treatment of QUF-001 with organic solvents (such as methanol, isopropanol, chloroform, dimethylformamide, tetrahydrofuran, hexane), interactions were observed and changes in fluorescence maxima as well as in the powder diffraction patterns were noticed, indicating the inclusion and intercalation of the solvents into the interlamellar space of the crystal structure of QUF-001. Furthermore, CO2 and CH4 molecule sorption properties for QUF-001 reached up to 1.6 mmol/g and 8.1 mmol/g, respectively, at 298 K and a pressure of 50 bars.

7.
Opt Lett ; 47(10): 2542-2545, 2022 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-35561396

RESUMO

A Tm3+:Ho3+-codoped free-space single-oscillator fiber laser is under investigation with special focus on the power scalability of emission wavelengths from 2.1 µm to 2.2 µm. Using a tunable diffraction grating, a 200-nm tunable laser source is built. Laser output powers above 10 W are delivered from 1990 nm up to 2190 nm, demonstrating the range for stable high-power laser operation. By replacing the diffraction grating by a highly reflective, narrow linewidth volume Bragg grating, power scaling is performed at 2.1 µm and is even enabled at a wavelength of 2.2 µm. Using a volume Bragg grating (VBG) at 2.1 µm, a slope efficiency of 49% is measured with an output power of 262 W. Using another VBG with a center wavelength of 2.2 µm, the fiber laser delivers a record power of 77 W with a slope efficiency of 29%.

8.
Pharmaceuticals (Basel) ; 15(3)2022 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-35337097

RESUMO

Affective (AF) and Schizophrenic (SZ) Spectrum disorders manifest with risk factors, involving inflammatory processes linked to infections and autoimmunity. This study searched for novel biomarkers in cerebrospinal fluid (CSF) and peripheral blood. A total of 29 AF and 39 SZ patients with treatment-resistant disease were included. In CSF, the chemokine IL-8 was significantly elevated in AF and SZ patients. IL-8 promotes chemotaxis by neutrophils and may originate from different tissues. S100B, a glia-derived brain damage marker, was higher in CSF from AF than SZ patients. Among the plasma-derived biomarkers, ferritin was elevated in AF and SZ. Soluble CD25, indicating Treg dysfunction, was higher in SZ than in AF patients. Interferon-γ, implying virus-specific immune activation, was positive in selective AF patients, only. Both groups showed elevated expression of immunosuppressive CD33 on monocytes, but higher amounts of CD123+ plasmacytoid dendritic cells were restricted to SZ. In conclusion, chemotactic IL-8 indicates neuronal stress and inflammation in the CSF of both groups. Novel plasma-derived biomarkers such as sCD25 and monocytic CD33 distinguish SZ from AF with an autoimmune phenotype.

9.
Int J Radiat Biol ; 98(5): 865-872, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-34982640

RESUMO

PURPOSE: Advanced angiographic procedures in interventional radiology are becoming more important and are more frequently used, especially in the treatment of several acute life-threatening diseases like stroke or aortic injury. In recent years, technical advancement has led to a broader spectrum of interventions and complex procedures with longer fluoroscopy times. This involves the risk of higher dose exposures, which, in rare cases, may cause deterministic radiation effects, e.g. erythema in patients undergoing angiographic procedures. Against this background, these procedures recently also became subject to national and international regulations regarding radiation protection. At the same time, individual risk assessment of possible stochastic radiation effects for each patient must be weighed up against the anticipated benefits of the therapy itself. Harmful effects of the administered dose are not limited to the patient but can also affect the radiologist and the medical staff. In particular, the development of cataracts in interventionalists is a rising matter of concern. Furthermore, long-term effects of repeated and prolonged x-ray exposure have long been neglected by radiologists but have come into focus in the past years. CONCLUSIONS: With all this in mind, this review discusses different efforts to reduce radiation exposition levels for patients and medical staff by means of technical, personal as well as organizational measures.


Assuntos
Exposição Ocupacional , Exposição à Radiação , Lesões por Radiação , Proteção Radiológica , Fluoroscopia/efeitos adversos , Fluoroscopia/métodos , Humanos , Exposição Ocupacional/efeitos adversos , Doses de Radiação , Exposição à Radiação/efeitos adversos , Lesões por Radiação/etiologia , Lesões por Radiação/prevenção & controle , Proteção Radiológica/métodos , Radiologia Intervencionista
10.
Front Med (Lausanne) ; 9: 1026298, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36687421

RESUMO

Background: Sepsis causes a high rate of mortality and long-term morbidity, associated with an imbalance of innate immunity against infections and inflammation. Obesity and diabetes increase the risk for disease severity. Monocyte dysfunction plays a major role and justify further investigations. Objective: To investigate the distribution and inflammatory phenotypes in circulating monocyte subsets in patients manifesting with sepsis including septic shock with and without obesity and diabetes. Methods: A total of 235 blood samples were tested from critically ill adult patients registered at the intensive care unit (ICU). The cohorts were divided into non-diabetic groups with or without obesity and diabetic groups with or without obesity, suffering from sepsis or septic shock. We determined frequencies of total monocytes and of monocyte subsets in the circulation and density expression levels of functional markers, including CD14, CD16, HLA-DR, CD33, CD163, CD206, and arginase-1 by flow cytometric analysis. Results: When progressing to septic shock in non-diabetic and diabetic patients, the percentages of total monocytes among the leukocyte population and of CD33+ and CD14+ monocytes among the monocyte population were consistently down-regulated compared to non-sepsis in non-diabetic and diabetic patients, respectively. Non-diabetic sepsis patients further presented with decreased CD33 and up-regulated CD163 expression density, which was absent in diabetic patients. We subsequently addressed obesity-related changes of monocytes in non-diabetic and diabetic septic patients. Obese septic patients with diabetes were unique in displaying increased monocytic CD16 and CD163 expression. However, obese septic patients without diabetes solely presented with lower amounts of non-classical monocytes. Body mass index (BMI) dependent changes were restricted to diabetic septic patients, with a significantly higher diminution of the classical monocyte subset and concomitantly increased CD16 expression densities. Conclusion: Distribution and phenotypes of monocyte subsets were differentially modulated in critically ill patients with and without metabolic disease when progressing to sepsis or septic shock. Only diabetic septic patients displayed decline of classical monocytes and increase of CD16 expression densities. Therefore, diabetes but not obesity appears to promote the inflammatory phenotype of circulating monocytes in critically ill patients.

11.
Opt Lett ; 46(9): 2139-2142, 2021 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-33929438

RESUMO

A mid-infrared ${{\rm ZnGeP}_2}$ optical parametric oscillator pumped by a ${{\rm Tm}^{3 +}}$-doped fiber laser is reported, providing pulse energies of $230 \;\unicode{x00B5}{\rm J}$, pulse widths of 40 ns, and peak powers of ${\sim}6\;{\rm kW} $ with excellent efficiency and beam quality. The pump source is an actively $Q$-switched single oscillator optimized to generate high pulse energies.

12.
J Phys Condens Matter ; 32(1): 015901, 2020 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-31470430

RESUMO

QuantumATK is an integrated set of atomic-scale modelling tools developed since 2003 by professional software engineers in collaboration with academic researchers. While different aspects and individual modules of the platform have been previously presented, the purpose of this paper is to give a general overview of the platform. The QuantumATK simulation engines enable electronic-structure calculations using density functional theory or tight-binding model Hamiltonians, and also offers bonded or reactive empirical force fields in many different parametrizations. Density functional theory is implemented using either a plane-wave basis or expansion of electronic states in a linear combination of atomic orbitals. The platform includes a long list of advanced modules, including Green's-function methods for electron transport simulations and surface calculations, first-principles electron-phonon and electron-photon couplings, simulation of atomic-scale heat transport, ion dynamics, spintronics, optical properties of materials, static polarization, and more. Seamless integration of the different simulation engines into a common platform allows for easy combination of different simulation methods into complex workflows. Besides giving a general overview and presenting a number of implementation details not previously published, we also present four different application examples. These are calculations of the phonon-limited mobility of Cu, Ag and Au, electron transport in a gated 2D device, multi-model simulation of lithium ion drift through a battery cathode in an external electric field, and electronic-structure calculations of the composition-dependent band gap of SiGe alloys.

13.
Adv Sci (Weinh) ; 6(22): 1901345, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31763144

RESUMO

Herein, emerging applications of luminescent semiconductor nanocrystals are addressed, such as quantum dots and quantum rods as down-conversion materials used in liquid crystal displays (LCD). Their precisely tunable emission wavelengths and narrow emission bandwidths offer high color purity resulting in a wide color gamut with vivid colors for LCDs. Anisotropic materials, such as quantum rods, have the additional advantage of polarized emission, which can bring a significant improvement to the efficiency of LCD displays. The basic optical properties of these nanomaterials are considered, with a focus on quantum rods, and the challenges and progress in their assembly are discussed. Different techniques for quantum rod alignment are introduced such as shear-oriented, electric field and magnetic field assisted assembly, mechanical rubbing, stretching, and electrospinning. The photoalignment approach allows for an easy arrangement of quantum rods in-plane, and the implications of this method to patterning are considered. Different configurations of LCDs utilizing semiconductor quantum dots and quantum rods as down-conversion layers are also presented, and the potential applications that are enabled by the wide range of emerging materials are highlighted.

14.
Sci Rep ; 9(1): 14522, 2019 10 10.
Artigo em Inglês | MEDLINE | ID: mdl-31601835

RESUMO

Hemoadsorption devices are used to treat septic shock by adsorbing inflammatory cytokines and as yet incompletely defined danger and pathogen associated molecular patterns. In an ideal case, hemoadsorption results in immediate recovery of microvascular endothelial cells' (mEC) function and rapid recovery from catecholamine-dependency and septic shock. We here tested a single device, which consists of polystyrene-divinylbenzene core particles of 450 µm diameter with a high affinity for hydrophobic compounds. The current study aimed at the proof of concept that endothelial-specific damage mediators are adsorbed and can be recovered from hemoadsorption devices. Because of excellent clinical experience, we tested protein fractions released from a hemoadsorber in a novel endothelial bioassay. Video-based, long-term imaging of mEC proliferation and cell death were evaluated and combined with apoptosis and ATP measurements. Out of a total of 39 fractions recovered from column fractionation, we identified 3 fractions that caused i) inhibition of mEC proliferation, ii) increased cell death and iii) induction of apoptosis in mEC. When adding these 3 fractions to mEC, their ATP contents were reduced. These fractions contained proteins of approximately 15 kDa, and high amounts of nucleic acid, which was at least in part oxidized. The efficacy for endothelial cell damage prevention by hemoadsorption can be addressed by a novel endothelial bioassay and long-term video observation procedures. Protein fractionation of the hemoadsorption devices used is feasible to study and define endothelial damage ligands on a molecular level. The results suggest a significant effect by circulating nucleic acids - bound to an as yet undefined protein, which may constitute a major danger-associated molecular pattern (DAMP) in the exacerbation of inflammation when patients experience septic shock. Hemoadsorption devices may thus limit endothelial damage, through the binding of nucleic acid-bearing aggregates and thus contribute to improved endothelial barrier function.


Assuntos
Alarminas/química , Bioensaio/métodos , Proteínas Sanguíneas/química , Células Endoteliais/patologia , Endotélio Vascular/patologia , Trifosfato de Adenosina/química , Adsorção , Idoso , Apoptose , Sobrevivência Celular , Citocinas/metabolismo , Feminino , Humanos , Inflamação , Ligantes , Microcirculação , Oxigênio/química , Poliestirenos/química , Choque Séptico/patologia , Compostos de Vinila/química
15.
ACS Nano ; 13(10): 12024-12031, 2019 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-31589022

RESUMO

We realized the synthesis of carbon nanorods-monodisperse colloidal particles with a length of 50 nm and a width of 20 nm-which can be considered an addition to the family of light-emitting carbon-based nanostructures. Their anisotropic shape is determined by the use of the surfactant aminopropylisobutyl polyhedral oligomeric silsesquioxane, and their optical properties originate from domains of polycyclic aromatic hydrocarbons incorporated within an inorganic framework. The nanorods show dual polarized emission with a quantum yield of 15-20% and emission anisotropy of ∼0.3, which changes from blue (460 nm) to yellow (565 nm) depending on the excitation wavelength. These carbon nanorods expand the range of light-emitting carbon nanomaterials available for optoelectronic and biolabeling applications.

16.
Small ; 14(20): e1800315, 2018 May.
Artigo em Inglês | MEDLINE | ID: mdl-29575504

RESUMO

A cellulose paper is used impregnated with light-emitting CdTe nanocrystals and carbon dots, and filled with a polyurethane to fabricate uniform transparent composite films with bright photoluminescence of red (R), green (G), and blue (B) (RGB) colors. A building brick-like assembly method is introduced to realize RGB multicolor emission patterns from this composite material. By sectioning out individual pixels from monochrome-emissive composite sheets, the advantage of the self-healing properties of polyurethane is taken to arrange and weld them into a RGB patterned fabric by brief exposure to ethanol. This provides an approach to form single layer RGB light-emitting pixels, such as potentially required in the display applications, without the use of any lithographic or etching processing. The method can utilize a wide range of different solution-based kinds of light-emitting materials.

17.
Arch Toxicol ; 92(1): 323-336, 2018 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-28924833

RESUMO

Bacterial protein toxins became valuable molecular tools for the targeted modulation of cell functions in experimental pharmacology and attractive therapeutics because of their potent and specific mode of action in human cells. C2IN-C3lim, a recombinant fusion toxin (~50 kDa) of the Rho-inhibiting C3lim from Clostridium (C.) limosum and a non-toxic portion of the C. botulinum C2 toxin (C2IN), is selectively internalized into the cytosol of monocytic cells where C3lim specifically ADP-ribosylates Rho A and -B, thereby inhibiting Rho-mediated signaling. Thus, we hypothesized that these unique features make C2IN-C3lim an attractive molecule for the targeted pharmacological down-regulation of Rho-mediated functions in monocytes. The analysis of the actin structure and the Rho ADP-ribosylation status implied that C2IN-C3lim entered the cytosol of primary human monocytes from healthy donors ex vivo within 1 h. Moreover, it inhibited the fMLP-induced chemotaxis of human monocytes in a Boyden chamber model ex vivo. Similarly, in a 3-dimensional ex vivo model of extravasation, single cell analysis revealed that C2IN-C3lim-treated cells were not able to move. In a clinically relevant mouse model of blunt chest trauma, the local application of C2IN-C3lim into the lungs after thorax trauma prevented the trauma-induced recruitment of monocytes into the lungs in vivo. Thus, C2IN-C3lim might be an attractive lead compound for novel pharmacological strategies to avoid the cellular damage response caused by monocytes in damaged tissue after trauma and during systemic inflammation. The results suggest that the pathophysiological role of clostridial C3 toxins might be a down-modulation of the innate immune system.


Assuntos
ADP Ribose Transferases/genética , Toxinas Botulínicas/genética , Quimiotaxia/efeitos dos fármacos , Monócitos/efeitos dos fármacos , Proteínas Recombinantes de Fusão/farmacologia , Proteínas rho de Ligação ao GTP/antagonistas & inibidores , Animais , Movimento Celular/efeitos dos fármacos , Células Cultivadas , Modelos Animais de Doenças , Humanos , Pulmão/efeitos dos fármacos , Pulmão/patologia , Macrófagos/efeitos dos fármacos , Masculino , Camundongos Endogâmicos C57BL , Monócitos/citologia , Proteínas Recombinantes de Fusão/genética , Traumatismos Torácicos/tratamento farmacológico , Ferimentos não Penetrantes/tratamento farmacológico , Proteínas rho de Ligação ao GTP/metabolismo
18.
Nano Lett ; 17(12): 7710-7716, 2017 12 13.
Artigo em Inglês | MEDLINE | ID: mdl-29188711

RESUMO

Carbon dots (CDs) are an intriguing fluorescent material; however, due to a plethora of synthesis techniques and precursor materials, there is still significant debate on their structure and the origin of their optical properties. The two most prevalent mechanisms to explain them are based on polycyclic aromatic hydrocarbon domains and small molecular fluorophores, for instance, citrazinic acid. Yet, how these form and whether they can exist simultaneously is still under study. To address this, we vary the hydrothermal synthesis time of CDs obtained from citric acid and ethylenediamine and show that in the initial phase molecular fluorophores, likely 2-pyridone derivatives, account for the blue luminescence of the dots. However, over time, while the overall size of the CDs does not change, aromatic domains form and grow, resulting in a second, faster decay channel at similar wavelengths and also creating additional lower energetic states. Electrophoresis provides further evidence that the ensemble of CDs consists of several subsets with different internal structure and surface charge. The understanding of the formation mechanism enables a control of the chemical origin of these emitters and the ensuing optical properties of the CDs through synthetic means.

19.
Nanoscale ; 9(32): 11730-11738, 2017 Aug 17.
Artigo em Inglês | MEDLINE | ID: mdl-28782778

RESUMO

Carbon Dots (CDs), fabricated by hydrothermal bottom-up synthesis, are complex materials, whose optical properties are influenced by multiple factors. The presence of domains of conjugated sp2 carbon, which are formed upon carbonization of precursors at high temperature; nitrogen doping; and as recently shown, the presence of molecular fluorophores, are contributing to the emission of such CDs. We conducted a series of syntheses, each designed with specific precursors and reaction conditions that reveal the contribution of the above-mentioned factors. Specifically, we enforced carbonization by using graphene oxide as a precursor material; favored the formation of molecular fluorophores by conducting the synthesis at lower temperature and ambient pressure; and employed two different nitrogen precursors, namely ethylenediamine and triethanolamine. We compared and analyzed the distinct optical properties of the resulting products; furthermore, to address the relationship of CDs and molecular fluorophores, we examined photobleaching characteristics of these materials, under exposure to UV irradiation. From the analysis of the emission lifetimes, we revealed the quenching of the molecular fluorophores, whereas species with a higher degree of carbonization offer protection through incorporation into a carbon matrix. Based on a detailed comparison of different carbon dot species, our study provides novel physical insights into the origin of the luminescence properties of carbon dot derived nanomaterials.

20.
Angew Chem Int Ed Engl ; 56(32): 9571-9576, 2017 08 01.
Artigo em Inglês | MEDLINE | ID: mdl-28612482

RESUMO

A top-down method is demonstrated for the fabrication of CH3 NH3 PbBr3 and CH3 NH3 PbI3 perovskite nanocrystals, employing a mixture of ligands oleic acid and oleylamine as coordinating solvents. This approach avoids the use of any polar solvents, skips multiple reaction steps by employing a simple ultrasonic treatment of the perovskite precursors, and yields rather monodisperse blue-, green-, and red-emitting methylammonium lead halide nanocrystals with a high photoluminescence quantum yield (up to 72 % for the green-emitting nanocrystals) and remarkably improved stability. After discussing all relevant reaction parameters, the green-emitting CH3 NH3 PbBr3 nanocrystals are employed as a component of down-conversion white-light-emitting devices.

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