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1.
Small ; : e2403651, 2024 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-38934537

RESUMO

Conjugated polymer sorting is recognized as an efficient and scalable method for the selective extraction of semiconducting single-walled carbon nanotubes (s-SWCNTs). However, this process typically requires the use of nonpolar and aromatic solvents as the dispersion medium, which are petroleum-based and carry significant production hazards. Moreover, there is still potential for improving the efficiency of batch purification. Here, this study presents fluorene-based conjugated polymer that integrates diamines containing ethylene glycol chains (ODA) as linkers within the main chain, to effectively extract s-SWCNTs in bio-renewable solvents. The introduction of ODA segments enhances the solubility in bio-renewable solvents, facilitating effective wrapping of s-SWCNTs in polar environments. Additionally, the ODA within the main chain enhances affinity to s-SWCNTs, thereby contributing to increased yields and purity. The polymer achieves a high sorting yield of 55% and a purity of 99.6% in dispersion of s-SWCNTs in 2-Methyltetrahydrofuran. Thin-film transistor arrays fabricated with sorted s-SWCNTs solution through slot-die coating exhibit average charge carrier mobilities of 20-23 cm2 V⁻¹ s⁻¹ and high on/off current ratios exceeding 105 together with high spatial uniformity. This study highlights the viability of bio-renewable solvents in the sorting process, paving the way for the eco-friendly approach to the purification of SWCNTs.

2.
Antioxidants (Basel) ; 13(6)2024 Jun 17.
Artigo em Inglês | MEDLINE | ID: mdl-38929174

RESUMO

Ten-eleven translocation 1 (TET1) is a methylcytosine dioxygenase involved in active DNA demethylation. In our previous study, we demonstrated that TET1 reprogrammed the ovarian cancer epigenome, increased stem properties, and activated various regulatory networks, including metabolic networks. However, the role of TET1 in cancer metabolism remains poorly understood. Herein, we uncovered a demethylated metabolic gene network, especially oxidative phosphorylation (OXPHOS). Contrary to the concept of the Warburg effect in cancer cells, TET1 increased energy production mainly using OXPHOS rather than using glycolysis. Notably, TET1 increased the mitochondrial mass and DNA copy number. TET1 also activated mitochondrial biogenesis genes and adenosine triphosphate production. However, the reactive oxygen species levels were surprisingly decreased. In addition, TET1 increased the basal and maximal respiratory capacities. In an analysis of tricarboxylic acid cycle metabolites, TET1 increased the levels of α-ketoglutarate, which is a coenzyme of TET1 dioxygenase and may provide a positive feedback loop to modify the epigenomic landscape. TET1 also increased the mitochondrial complex I activity. Moreover, the mitochondrial complex I inhibitor, which had synergistic effects with the casein kinase 2 inhibitor, affected ovarian cancer growth. Altogether, TET1-reprogrammed ovarian cancer stem cells shifted the energy source to OXPHOS, which suggested that metabolic intervention might be a novel strategy for ovarian cancer treatment.

3.
Psychol Res Behav Manag ; 17: 1451-1461, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38590759

RESUMO

Background: Diabetes distress (DD) is a negative emotion related to diabetes management and a predictor of depression; it affects diabetic retinopathy (DR) patients' quality of life and disease outcomes. The prevalence of DD was higher in patients undergoing surgery for DR. However, few studies have been conducted on DD in DR surgery patients. The present study aims to investigate the status of DD in DR surgery patients and identify factors associated with DD. Methods: Using a convenience sampling method, 210 DR surgery patients who were admitted to 2 tertiary-level hospitals in Wenzhou City (Zhejiang Province) and Zhengzhou City (Henan Province) from February to June 2023 were selected as research subjects. A questionnaire collecting demographic and disease-related information, the Diabetes Distress Scale, the Summary of Diabetes Self-Management Activities, the Family Care Index Scale, and the Social Support Rating Scale were used to collect data. Statistical analyses included descriptive statistics, t tests, ANOVAs, Pearson's correlation analyses and stepwise multiple linear regression. This study is reported according to the STROBE guidelines. Results: In total, 156 out of 210 (74.29%) DR surgery patients experienced DD, with an average score of 2.13±0.63. The results of the stepwise multiple regression analysis showed that residential location, employment status, self-management level, family support, and social support were significantly associated with DD. These variables accounted for 30.6% of the total variation in DD. Conclusions: DR surgery patients exhibit moderate levels of distress. Health care professionals should pay attention to DD in DR surgery patients and develop targeted interventions to improve the self-management ability of these patients, increase their family support and social support to reduce their DD levels.

4.
Rev Sci Instrum ; 95(3)2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38517256

RESUMO

Parametric superfluorescence (PSF), which originated from the optical amplification of vacuum quantum noise, is the primary noise source of femtosecond fluorescence non-collinear optical parametric amplification spectroscopy (FNOPAS). It severely affects the detection limit of FNOPAS to collect the femtosecond time-resolved spectra of extremely weak fluorescence. Here, we report the development of femtosecond fluorescence conical optical parametric amplification spectroscopy (FCOPAS), aimed at effectively suppressing the noise fluctuation from the PSF background. In contrast to traditional FNOPAS configurations utilizing lateral fluorescence collection and dot-like parametric amplification, FCOPAS employs an innovative conical fluorescence collection and ring-like amplification setup. This design enables effective cancellation of noise fluctuation across the entire PSF ring, resulting in an approximate order of magnitude reduction in PSF noise compared to prior FNOPAS outcomes. This advancement enables the resolution of transient fluorescence spectra of 4-dicyanomethylene-2-methyl-6-p-dimethylaminostyryl-4H-pyran (DCM) dye molecules in ethanol, even at an optically dilute concentration of 10-6 mol/l, with significantly enhanced signal-to-noise ratios. This improvement will be significant for extremely weak fluorescence detection on the femtosecond time scale.

5.
Head Neck ; 46(6): E61-E66, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38469981

RESUMO

BACKGROUND: Extrathyroid implantation or dissemination of thyroid tissue secondary to a thyroid procedure is rare. Most of these belonged to thyroid carcinoma with metastatic potential and uncommon for benign pathologies. METHODS: We report the case of a 31-year-old female who was identified to have multiple subcutaneous implantation of thyroid tissue 5 years after transoral endoscopic thyroidectomy vestibular approach. A comprehensive literature search on implantation of thyroid tissue secondary to thyroid procedures was performed. RESULTS: Accidental tearing of the capsule during previous surgery may lead to the subcutaneous implantation. Through literature review, a total 29 articles with 47 patients were identified. 33.3% were benign lesions, and implantation was mostly secondary to fine needle aspiration biopsy (46.5%). CONCLUSIONS: Subcutaneous or port site implantation after endoscopic thyroid surgery may occur in benign thyroid pathologies and therefore, oncologic principles must be strictly followed during surgery regardless of its histopathological nature.


Assuntos
Bócio Nodular , Tireoidectomia , Humanos , Feminino , Tireoidectomia/métodos , Tireoidectomia/efeitos adversos , Adulto , Bócio Nodular/cirurgia , Bócio Nodular/patologia , Cirurgia Endoscópica por Orifício Natural/métodos , Cirurgia Endoscópica por Orifício Natural/efeitos adversos , Endoscopia/métodos
6.
Sci Rep ; 14(1): 5707, 2024 03 08.
Artigo em Inglês | MEDLINE | ID: mdl-38459197

RESUMO

Biliary tract infection (BTI), a commonly occurring abdominal disease, despite being extensively studied for its initiation and underlying mechanisms, continues to pose a challenge in the quest for identifying specific diagnostic biomarkers. Extracellular vesicles (EVs), which emanate from diverse cell types, serve as minute biological entities that mirror unique physiological or pathological conditions. Despite their potential, there has been a relatively restricted exploration of EV-oriented methodologies for diagnosing BTI. To uncover potent protein biomarkers for BTI patients, we applied a label-free quantitative proteomic method known for its unbiased and high-throughput nature. Furthermore, 192 differentially expressed proteins surfaced within EVs isolated from individuals afflicted with BTI. Subsequent GO and KEGG analyses pinpointed Carcinoembryonic antigen-related cell adhesion molecule 1 (CEACAM1) and Crumbs homolog 3 (CRB3) as noteworthy biomarkers. Validation via data analysis of plasma-derived EV samples confirmed their specificity to BTI. Our study leveraged an unbiased proteomic tool to unveil CEACAM1 and CRB3 as promising protein biomarkers in serum EVs, presenting potential avenues for the advancement of diagnostic systems for BTI detection.


Assuntos
Sistema Biliar , Vesículas Extracelulares , Humanos , Proteômica/métodos , Biomarcadores , Vesículas Extracelulares/metabolismo
7.
J Sci Food Agric ; 104(7): 3982-3991, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38252712

RESUMO

BACKGROUND: Many diseases may be caused by pathogens and oxidative stress resulting from carcinogens. Earlier studies have highlighted the antimicrobial and antioxidant effects of plant essential oils (EO). It is crucial to effectively utilize agricultural waste to achieve a sustainable agricultural economy and protect the environment. The present study aimed to evaluate the potential benefits of EO extracted from the discarded peels of Citrus depressa Hayata (CD) and Citrus microcarpa Bunge (CM), synonyms of Citrus deliciosa Ten and Citrus japonica Thunb, respectively. RESULTS: Gas chromatography-mass spectrometry analysis revealed that the main compounds in CD-EO were (R)-(+)-limonene (38.97%), γ-terpinene (24.39%) and linalool (6.22%), whereas, in CM-EO, the main compounds were (R)-(+)-limonene (48.00%), ß-pinene (13.60%) and γ-terpinene (12.07%). CD-EO exhibited inhibitory effects on the growth of common microorganisms, including Candida albicans, Escherichia coli, Pseudomonas aeruginosa and Staphylococcus aureus. However, CM-EO showed only inhibitory effects on E. coli. Furthermore, CD-EO exhibited superior antioxidant potential, as demonstrated by its ability to eliminate 1,1-diphenyl-2-picrylhydrazyl and 2,2'-azinobis-3-ethylbenzthiazoline-6-sulfonate free radicals. Furthermore, CD-EO at a concentration of 100 µg mL-1 significantly inhibited 12-O-tetradecanoylphorbol-13-acetate-induced cancer transformation in mouse epidermal JB6 P+ cells (P < 0.05), possibly by up-regulating protein expression of nuclear factor erythroid 2-related factor 2 and its downstream antioxidant enzymes, such as NAD(P)H:quinone oxidoreductase 1, heme oxygenase-1 and UGT1A. CONCLUSION: These findings suggest that CD-EO exhibits inhibitory effects on pathogenic microorganisms, possesses antioxidant properties and has cancer chemopreventive potential. © 2024 Society of Chemical Industry.


Assuntos
Anti-Infecciosos , Citrus , Monoterpenos Cicloexânicos , Neoplasias , Óleos Voláteis , Animais , Camundongos , Óleos Voláteis/química , Antioxidantes/farmacologia , Antioxidantes/química , Limoneno/farmacologia , Citrus/química , Escherichia coli , Anti-Infecciosos/farmacologia , Anti-Infecciosos/química , Óleos de Plantas/química
8.
Adv Mater ; 36(19): e2312676, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38290714

RESUMO

Broad-spectrum-driven high-performance artificial photosynthesis is quite challenging. Herein, atomically ultrathin bismuthene with semimetallic properties is designed and demonstrated for broad-spectrum (ultraviolet-visible-near infrared light) (UV-vis-NIR)-driven photocatalytic CO2 hydrogenation. The trap states in the bandgap produced by edge dangling bonds prolong the lifetime of the photogenerated electrons from 90 ps in bulk Bi to 1650 ps in bismuthine, and excited-state electrons are enriched at the edge of bismuthine. The edge dangling bonds of bismuthene as the active sites for adsorption/activation of CO2 increase the hybridization ability of the Bi 6p orbital and O 2p orbital to significantly reduce the catalytic reaction energy barrier and promote the formation of C─H bonds until the generation of CH4. Under λ ≥ 400 nm and λ ≥ 550 nm irradiation, the utilization ratios of photogenerated electron reduction CO2 hydrogenation to CO and CH4 for bismuthene are 58.24 and 300.50 times higher than those of bulk Bi, respectively. Moreover, bismuthene can extend the CO2 hydrogenation reaction to the near-infrared region (λ ≥ 700 nm). This pioneering work employs the single semimetal element as an artificial photosynthetic catalyst to produce a broad spectral response.

9.
J Gastroenterol Hepatol ; 39(3): 544-551, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38059883

RESUMO

BACKGROUND AND AIM: Chromoendoscopy with the use of indigo carmine (IC) dye is a crucial endoscopic technique to identify gastrointestinal neoplasms. However, its performance is limited by the endoscopist's skill, and no standards are available for lesion identification. Thus, we developed an artificial intelligence (AI) model to replace chromoendoscopy. METHODS: This pilot study assessed the feasibility of our novel AI model in the conversion of white-light images (WLI) into virtual IC-dyed images based on a generative adversarial network. The predictions of our AI model were evaluated against the assessments of five endoscopic experts who were blinded to the purpose of this study with a staining quality rating from 1 (unacceptable) to 4 (excellent). RESULTS: The AI model successfully transformed the WLI of polyps with different morphologies and different types of lesions in the gastrointestinal tract into virtual IC-dyed images. The quality ratings of the real IC-dyed and AI images did not significantly differ concerning surface structure (AI vs IC: 3.08 vs 3.00), lesion border (3.04 vs 2.98), and overall contrast (3.14 vs 3.02) from 10 sets of images (10 AI images and 10 real IC-dyed images). Although the score depended significantly on the evaluator, the staining methods (AI or real IC) and evaluators had no significant interaction (P > 0.05) with each other. CONCLUSION: Our results demonstrated the feasibility of employing AI model's virtual IC staining, increasing the possibility of being employed in daily practice. This novel technology may facilitate gastrointestinal lesion identification in the future.


Assuntos
Inteligência Artificial , Lesões Pré-Cancerosas , Humanos , Projetos Piloto , Endoscopia/métodos , Índigo Carmim , Carmim , Lesões Pré-Cancerosas/diagnóstico por imagem
10.
ACS Appl Mater Interfaces ; 16(1): 425-434, 2024 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-38115766

RESUMO

Directional graphene aerogels (DGAs) are proposed as electrode materials to alleviate ionic and mass transport issues in organic redox flow batteries (ORFBs). DGAs with high pore directionality would provide low resistance channels for effective ionic charge and liquid electrolyte transport in these devices. DGAs' porous and directional characteristics can be controlled by the growth of ice crystals during freeze casting, which is influenced by the self-diffusivity of water, phase change driving forces, water-ice graphene interactions, and convection in the water-graphene media. It is found that mass transport-related properties of DGAs, including pore size and directionality, show a significant dependence on freezing temperature, graphene oxide (GO) loadings, and synthesis vessel diameter-to-height ratio (D/H). For the freezing temperature change from -20 to -115 °C, the average pore size progressively decreased from 120 to 20 µm, and the pore directionality transitioned from lamellar to ill-defined structures. When GO loadings were increased from 2 to 10 mg/mL at a fixed freezing temperature, pore size reduction was observed with less defined directionality. Furthermore, the pore directionality diminished with an increased width-to-height aspect ratio of DGA samples due to the buoyancy-driven convective circulation, which interfered with the directional ice/pore growth. Understanding the comprehensive effects of these mechanisms enables the controlled growth of ice crystals, leading to graphene aerogels with highly directional microstructures.

11.
J Med Syst ; 48(1): 4, 2023 Dec 18.
Artigo em Inglês | MEDLINE | ID: mdl-38105364

RESUMO

Adhesion is a critical quality attribute and performance characteristic for transdermal and topical delivery systems (TDS). Regulatory agencies recommend in vivo skin adhesion studies to support the approval of TDS in both new drug applications and abbreviated new drug applications. The current assessment approach in such studies is based on the visual observation of the percent adhesion, defined as the ratio of the area of TDS attached to the skin to the total area of the TDS. Visually estimated percent adhesion by trained clinicians or trial participants creates variability and bias. In addition, trial participants are typically confined to clinical centers during the entire product wear period, which may lead to challenges when translating adhesion performance to the real world setting. In this work we propose to use artificial intelligence and mobile technologies to aid and automate the collection of photographic evidence and estimation of percent adhesion. We trained state-of-art deep learning models with advanced techniques and in-house curated data. Results indicate good performance from the trained models and the potential use of such models in clinical practice is further explored.


Assuntos
Inteligência Artificial , Sistemas de Liberação de Medicamentos , Humanos , Administração Cutânea , Sistemas de Liberação de Medicamentos/métodos , Pele , Tecnologia
12.
Pediatr Neonatol ; 2023 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-38012896

RESUMO

BACKGROUND: The clinical presentations of abusive head trauma can abruptly worsen, so the occurrence of seizures and changes of EEG can be variable according to patients' conditions. Since the changes of EEG background waves reflect the cortical function of children, we aimed to find out whether the timing of EEG background, epileptiform discharges and seizure patterns were associated with the outcomes of patients with AHT. MATERIAL AND METHODS: Using seizure type and acute stage electroencephalographic (EEG) characteristics to assess adverse neurological outcomes in children with seizures secondary to abusive head trauma (AHT). Children who were hospitalized with AHT at a tertiary referral hospital from October 2000 to April 2010 were evaluated retrospectively. A total of 50 children below 6 years of age admitted due to AHT were included. KOSCHI outcome scale was used to evaluate the primary outcome and neurological impairment was used as secondary outcome after 6 months discharge. RESULTS: Children with apnea, cardiac arrest, reverse blood flow and skull fracture in clinic had a higher mortality rate even in the no-seizure group (3/5 [60%] vs. 3/45 [6.7%], odds ratio [OR] = 11; 95% CI = 2.3-52; p = 0.025). Seizure occurrence reduced mostly at the second day after admission in seizure groups; but children with persistent seizures for 1 week showed poor neurological outcomes. The occurrence of initial seizure was frequency associated with younger age; focal seizure, diffuse cortical dysfunction in acute-stage EEG, and low Glasgow Coma Scale (GCS) score were significantly related to poor outcomes after 6 months. Diffuse cortical dysfunction was also associated with motor, speech, and cognitive dysfunction. CONCLUSIONS: Diffuse cortical dysfunction in acute-stage EEG combined with low GCS score and focal seizure may related to poor outcomes and neurological dysfunctions in children with AHT.

13.
Artigo em Inglês | MEDLINE | ID: mdl-37897812

RESUMO

The manipulation of the polymer backbone structure has a profound influence on the crystalline behavior and charge transport characteristics of polymers. These strategies are commonly employed to optimize the performance of stretchable polymer semiconductors. However, a universal method that can be applied to conjugated polymers with different donor-acceptor combinations is still lacking. In this study, we propose a universal strategy to boost the stretchability of polymers by incorporating the nonlinear conjugated linker (NCL) into the main chain. Specifically, we incorporate meta-dibromobenzene (MB), characterized by its asymmetric linkage sites, as the NCL into the backbone of diketopyrrolopyrrole-thiophene-based (DPP-based) polymers. Our research demonstrates that the introduction of MB prompts chain-kinking, thereby disrupting the linearity and central symmetry of the DPP conjugated backbone. This modification reshapes the polymer conformation, decreasing the radius of gyration and broadening the free volume, which consequently adjusts the level of crystallinity, leading to a considerable increase in the stretchability of the polymer. Importantly, this method increases stretchability without compromising mobility and exhibits broad applicability across a wide range of donor-acceptor pair polymers. Leveraging this strategy, fully stretchable transistors were fabricated using a DPP polymer that incorporates 10 mol % of MB. These transistors display a mobility of approximately 0.5 cm2 V-1 s-1 and prove remarkably durable, maintaining 90% of this mobility even after enduring 1000 cycles at 25% strain. Overall, we propose a method to systematically control the main-chain conformation, thereby enhancing the stretchability of conjugated polymers in a widely applicable manner.

14.
J Phys Chem Lett ; 14(43): 9640-9645, 2023 Nov 02.
Artigo em Inglês | MEDLINE | ID: mdl-37870497

RESUMO

Femtosecond helicity-resolved pump-probe spectroscopy is performed to study the spin and valley dynamics in monolayer (ML) MoS2. Both the bright to dark intravalley exciton transition (∼50 fs) and the reverse transition process (<50 fs) are directly monitored. It suggests that the bright exciton state of ML MoS2 is lower in energy than the dark one, which is also confirmed by observing the temperature-dependent co-polarized photobleaching dynamics of A and B excitons. Furthermore, the band splitting in the conduction band of ML MoS2 with a value of 15 ± 0.3 meV is determined by fitting the temperature-dependent ratios of the population in bright and dark states using the Boltzmann distribution law. Such minor band splitting allows the phonon-mediated intravalley spin-flip to even occur from the lower to the upper conduction band within tens of femtoseconds, which will have non-negligible effects on the performance of these ML MoS2-based optoelectronic and photonic devices.

15.
BMC Geriatr ; 23(1): 589, 2023 09 23.
Artigo em Inglês | MEDLINE | ID: mdl-37742002

RESUMO

BACKGROUND: Implant rupture is one of the complications of breast augmentation surgery. The rupture of silicone implants is often insidious, potentially causing problems at any time. This is a case report of the rupture of 145-cc breast implants manufactured by Dow Corning Corporation and their removal at 40 years after augmentation. CASE PRESENTATION: A 70-year-old female patient was admitted for the removal of a lump in the upper and inner quadrants of the right breast. After a detailed examination, a rupture of the bilateral breast implants was diagnosed. Explantation without replacement was performed; the entire procedure proceeded smoothly. Immunohistochemical staining revealed siliconoma with lymphoid hyperplasia and calcification in the bilateral breasts with no signs of malignancy. CONCLUSIONS: Silicone breast augmentation is one of the most popular aesthetic surgical procedures worldwide. Therefore, it is important to educate patients on the need for close monitoring of their implants after augmentation through magnetic resonance imaging or ultrasound to facilitate early detection of any changes before a rupture occurs. Early detection of the implant rupture, in turn, will facilitate early and effective management.


Assuntos
Implantes de Mama , Feminino , Humanos , Idoso , Implantes de Mama/efeitos adversos , Géis de Silicone/efeitos adversos , Hospitalização
16.
JGH Open ; 7(6): 419-423, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37359110

RESUMO

Background and Aim: A pyogenic liver abscess (PLA) is an infectious disease with high in-hospital mortality. It has no specific symptoms and is difficult to be diagnosed early in the emergency department. Ultrasound is commonly used to detect PLA lesions of PLA, but its sensitivity can be affected by lesion size, location, and clinician experience. Therefore, early diagnosis and prompt treatment (especially abscess drainage) are crucial for better patient outcomes and should be prioritized by clinical physicians. Methods: We conducted a retrospective study to compare the effect of early and late (i.e., receiving CT scanning within 48 h and >48 h after admission) adoption of nonenhanced computed tomography (CT) scanning regarding the hospitalization days and interval between admission and drainage of patients with PLA. Results: This study included 76 hospitalized patients with PLA in the Department of Digestive Disease of Xiamen Chang Gung Hospital in China who underwent CT examinations from 2014 to 2021. We conducted CT scans on 56 patients within 48 h of admission and on 20 patients more than 48 h after admission. The early CT group had a significantly shorter hospitalization length compared with the late CT group (15.0 days vs. 20.5 days; P = 0.035). Besides, the median time to initiate drainage after admission was also significantly shorter in the early CT group than in the late CT group (1.0 days vs. 4.5 days; P < 0.001). Conclusion: Early CT scanning within 48 h of admission may aid in early PLA diagnosis and benefit disease recovery, as revealed by our findings.

17.
J Phys Chem Lett ; 14(20): 4657-4665, 2023 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-37167104

RESUMO

Due to the strong Coulomb interaction, the optical and electrical properties of two-dimensional transition metal dichalcogenides (TMDCs) are greatly determined by the emergence of many-body complexes such as excitons or trions. To fully realize the potential functionalities of these atomically thin materials, a comprehensive understanding of their many-body interaction mechanism is essential. Here, using the advanced femtosecond two-dimensional electronic spectroscopy technique combined with broadband transient absorption spectroscopy, a strong electron-exciton coupling effect in monolayer WSe2 following the ultrafast photoexcitation is revealed. We demonstrate that such many-body complexes can be generated effectively through the band-edge optical excitation, with a ∼1.5 ps stabilization process. The coherent optical phonon plays a dominant role in this electron-exciton interaction, and the coherence of the electron (exciton)-phonon coupling can last for ∼4.5 ps. This finding offers new insight into the formation mechanism of photoinduced many-body complexes in TMDCs.

18.
Nanotechnology ; 34(23)2023 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-36877995

RESUMO

In this work, ultrafast carrier dynamics of mechanically exfoliated 1T-TiSe2flakes from the high-quality single crystals with self-intercalated Ti atoms are investigated by femtosecond transient absorption spectroscopy. The observed coherent acoustic and optical phonon oscillations after ultrafast photoexcitation reveal the strong electron-phonon coupling in 1T-TiSe2. The ultrafast carrier dynamics probed in both visible and mid-infrared regions indicate that some photogenerated carriers localize near the intercalated Ti atoms and form small polarons rapidly within several picoseconds after photoexcitation due to the strong and short-range electron-phonon coupling. The formation of polarons leads to a reduction of carrier mobility and a long-time relaxation process of photoexcited carriers for several nanoseconds. The formation and dissociation rates of the photoinduced polarons are dependent on both the pump fluence and the thickness of TiSe2sample. This work offers new insights into the photogenerated carrier dynamics of 1T-TiSe2, and emphasizes the effects of intercalated atoms on the electron and lattice dynamics after photoexcitation.

19.
J Am Chem Soc ; 145(10): 5769-5777, 2023 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-36863033

RESUMO

A series of novel surface Ru-H bipyridine complexes-grafted TiO2 nanohybrids were for the first time prepared by a combined procedure of surface organometallic chemistry with post-synthetic ligand exchange for photocatalytic conversion of CO2 to CH4 with H2 as electron and proton donors under visible light irradiation. The selectivity toward CH4 increased to 93.4% by the ligand exchange of 4,4'-dimethyl-2,2'-bipyridine (4,4'-bpy) with the surface cyclopentadienyl (Cp)-RuH complex and the CO2 methanation activity was enhanced by 4.4-fold. An impressive rate of 241.2 µL·g-1·h-1 for CH4 production was achieved over the optimal photocatalyst. The femtosecond transient IR absorption results demonstrated that the hot electrons were fast injected in 0.9 ps from the photoexcited surface 4,4'-bpy-RuH complex into the conduction band of TiO2 nanoparticles to form a charge-separated state with an average lifetime of ca. 50.0 ns responsible for the CO2 methanation. The spectral characterizations indicated clearly that the formation of CO2•- radicals by single electron reduction of CO2 molecules adsorbed on surface oxygen vacancies of TiO2 nanoparticles was the most critical step for the methanation. Such radical intermediates were inserted into the explored Ru-H bond to generate Ru-OOCH species and finally CH4 and H2O in the presence of H2.

20.
Int J Mol Sci ; 24(6)2023 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-36982674

RESUMO

Window of implantation (WOI) genes have been comprehensively identified at the single cell level. DNA methylation changes in cervical secretions are associated with in vitro fertilization embryo transfer (IVF-ET) outcomes. Using a machine learning (ML) approach, we aimed to determine which methylation changes in WOI genes from cervical secretions best predict ongoing pregnancy during embryo transfer. A total of 2708 promoter probes were extracted from mid-secretory phase cervical secretion methylomic profiles for 158 WOI genes, and 152 differentially methylated probes (DMPs) were selected. Fifteen DMPs in 14 genes (BMP2, CTSA, DEFB1, GRN, MTF1, SERPINE1, SERPINE2, SFRP1, STAT3, TAGLN2, TCF4, THBS1, ZBTB20, ZNF292) were identified as the most relevant to ongoing pregnancy status. These 15 DMPs yielded accuracy rates of 83.53%, 85.26%, 85.78%, and 76.44%, and areas under the receiver operating characteristic curves (AUCs) of 0.90, 0.91, 0.89, and 0.86 for prediction by random forest (RF), naïve Bayes (NB), support vector machine (SVM), and k-nearest neighbors (KNN), respectively. SERPINE1, SERPINE2, and TAGLN2 maintained their methylation difference trends in an independent set of cervical secretion samples, resulting in accuracy rates of 71.46%, 80.06%, 80.72%, and 80.68%, and AUCs of 0.79, 0.84, 0.83, and 0.82 for prediction by RF, NB, SVM, and KNN, respectively. Our findings demonstrate that methylation changes in WOI genes detected noninvasively from cervical secretions are potential markers for predicting IVF-ET outcomes. Further studies of cervical secretion of DNA methylation markers may provide a novel approach for precision embryo transfer.


Assuntos
Infertilidade Feminina , beta-Defensinas , Feminino , Gravidez , Humanos , Metilação de DNA , Teorema de Bayes , Serpina E2/genética , Infertilidade Feminina/metabolismo , Endométrio/metabolismo , Implantação do Embrião/genética , Marcadores Genéticos , Fertilização in vitro/métodos , beta-Defensinas/metabolismo , Proteínas de Transporte/metabolismo , Proteínas do Tecido Nervoso/metabolismo
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