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1.
Nature ; 2024 Jun 26.
Artículo en Inglés | MEDLINE | ID: mdl-38926586

RESUMEN

Chiral superconductors, a unique class of unconventional superconductors in which the complex superconducting order parameter winds clockwise or anticlockwise in the momentum space1, represent a topologically non-trivial system with intrinsic time-reversal symmetry breaking (TRSB) and direct implications for topological quantum computing2,3. Intrinsic chiral superconductors are extremely rare, with only a few arguable examples, including UTe2, UPt3 and Sr2RuO4 (refs. 4-7). It has been suggested that chiral superconductivity may exist in non-centrosymmetric superconductors8,9, although such non-centrosymmetry is uncommon in typical solid-state superconductors. Alternatively, chiral molecules with neither mirror nor inversion symmetry have been widely investigated. We suggest that an incorporation of chiral molecules into conventional superconductor lattices could introduce non-centrosymmetry and help realize chiral superconductivity10. Here we explore unconventional superconductivity in chiral molecule intercalated TaS2 hybrid superlattices. Our studies reveal an exceptionally large in-plane upper critical field Bc2,|| well beyond the Pauli paramagnetic limit, a robust π-phase shift in Little-Parks measurements and a field-free superconducting diode effect (SDE). These experimental signatures of unconventional superconductivity suggest that the intriguing interplay between crystalline atomic layers and the self-assembled chiral molecular layers may lead to exotic topological materials. Our study highlights that the hybrid superlattices could lay a versatile path to artificial quantum materials by combining a vast library of layered crystals of rich physical properties with the nearly infinite variations of molecules of designable structural motifs and functional groups11.

2.
Nature ; 606(7916): 902-908, 2022 06.
Artículo en Inglés | MEDLINE | ID: mdl-35768590

RESUMEN

The discovery of chiral-induced spin selectivity (CISS) opens up the possibility to manipulate spin orientation without external magnetic fields and enables new spintronic device designs1-4. Although many approaches have been explored for introducing CISS into solid-state materials and devices, the resulting systems so far are often plagued by high inhomogeneity, low spin selectivity or limited stability, and have difficulties in forming robust spintronic devices5-8. Here we report a new class of chiral molecular intercalation superlattices (CMIS) as a robust solid-state chiral material platform for exploring CISS. The CMIS were prepared by intercalating layered two-dimensional atomic crystals (2DACs) (such as TaS2 and TiS2) with selected chiral molecules (such as R-α-methylbenzylamine and S-α-methylbenzylamine). The X-ray diffraction and transmission electron microscopy studies demonstrate highly ordered superlattice structures with alternating crystalline atomic layers and self-assembled chiral molecular layers. Circular dichroism studies show clear chirality-dependent signals between right-handed (R-) and left-handed (S-) CMIS. Furthermore, by using the resulting CMIS as the spin-filtering layer, we create spin-selective tunnelling junctions with a distinct chirality-dependent tunnelling current, achieving a tunnelling magnetoresistance ratio of more than 300 per cent and a spin polarization ratio of more than 60 per cent. With a large family of 2DACs of widely tunable electronic properties and a vast selection of chiral molecules of designable structural motifs, the CMIS define a rich family of artificial chiral materials for investigating the CISS effect and capturing its potential for new spintronic devices.

3.
Genomics ; 116(3): 110799, 2024 05.
Artículo en Inglés | MEDLINE | ID: mdl-38286348

RESUMEN

Malignant gliomas, characterized by pronounced heterogeneity, a complex microenvironment, and a propensity for relapse and drug resistaniguree, pose significant challenges in oncology. This study aimed to investigate the prognostic value of Ligand and Receptor related genes (LRRGs) within the glioma microenvironment. An intersection of 71 ligand-related genes (LRGs) and 2628 receptor-related genes (RRGs) yielded a total of 69 LRRGs. Utilizing the least absolute shrinkage and selection operator (LASSO) regression analysis, a prognostic RiskScore model comprising 28 LRRGs was constructed. The model demonstrated robust prognostic value, further validated in the TCGA-GBMLGG dataset. Subsequent analyses included differential gene expression, Gene Ontology (GO), Kyoto Encyclopedia of Genes and Genomes (KEGG), gene set enrichment (GSEA), and gene set variation (GSVA) within RiskScore groups. Additionally, evaluations of PPI, mRNA-RBP, mRNA-TF, and mRNA-drug interaction networks were conducted. Four hub genes were identified through differential expression analysis of the 28 LRRGs across various GSE datasets. A multivariate Cox prognostic model was constructed for nomogram analysis, gene mutation analysis, and related expression distribution. This study underscores the role of LRRGs in intercellular communication within the glioma microenvironment and identifies four hub genes crucial for prognostic assessment in clinical glioma patients. These findings offer a potential evaluation framework for glioma patients, enhancing our understanding of the disease and informing future therapeutic strategies.


Asunto(s)
Glioma , Microambiente Tumoral , Humanos , Biomarcadores de Tumor/genética , Biomarcadores de Tumor/metabolismo , Neoplasias Encefálicas/genética , Neoplasias Encefálicas/metabolismo , Neoplasias Encefálicas/patología , Regulación Neoplásica de la Expresión Génica , Glioma/genética , Glioma/metabolismo , Glioma/patología , Pronóstico , Transcriptoma , Microambiente Tumoral/genética
4.
Nano Lett ; 21(6): 2382-2389, 2021 Mar 24.
Artículo en Inglés | MEDLINE | ID: mdl-33689358

RESUMEN

Artificial spin ices are periodic arrangements of interacting nanomagnets which allow investigating emergent phenomena in the presence of geometric frustration. Recently, it has been shown that artificial spin ices can be used as building blocks for creating functional materials, such as magnonic crystals. We investigate the magnetization dynamics in a system exhibiting anisotropic magnetostatic interactions owing to locally broken structural inversion symmetry. We find a rich spin-wave spectrum and investigate its evolution in an external magnetic field. We determine the evolution of individual modes, from building blocks up to larger arrays, highlighting the role of symmetry breaking in defining the mode profiles. Moreover, we demonstrate that the mode spectra exhibit signatures of long-range interactions in the system. These results contribute to the understanding of magnetization dynamics in spin ices beyond the kagome and square ice geometries and are relevant for the realization of reconfigurable magnonic crystals based on spin ices.

5.
Wound Repair Regen ; 29(6): 1006-1016, 2021 11.
Artículo en Inglés | MEDLINE | ID: mdl-34448508

RESUMEN

Prolonged skin exposure to ultraviolet radiation can lead to development of several acute and chronic diseases, with UVA exposure considered a primary cause of dermal photodamage. We prepared a wild ginseng adventitious root extract (ARE) that could alleviate UVA irradiation-induced NIH-3T3 cell viability decline. After employing a series of purification methods to isolate main active components of ARE, adventitious root protein mixture (ARP) was identified then tested for protective effects against UVA irradiation-induced NIH-3T3 cell damage. The results showed that ARP treatment significantly reduced UVA-induced cell viability decline and confirmed that the active constituent of ARP was the protein, since proteolytic hydrolysis and heat treatment each eliminated ARP protective activity. Moreover, ARP treatment markedly inhibited UVA-induced apoptosis, cell cycle arrest and DNA fragmentation, while also significantly reversing UVA effects (elevated Bax levels, reduced Bcl-2 expression) by reducing Bax levels and increasing Bcl-2 expression. Mechanistically, ARP promoted Akt phosphorylation regardless of UVA exposure, thus confirming ARP resistance to inactivation by UVA light. Notably, in the presence of Akt inhibitor SC0227, ARP could no longer counteract UVA-induced cell viability decline and DNA fragmentation. Additionally, our results demonstrated that ARP treatment protected UVA-irradiated NIH-3T3 cells by preventing UVA-induced reduction of collagen-I expression. Taken together, these results suggest that ARP treatment of NIH-3T3 cells effectively mitigated UVA-induced cell viability decline by activating intracellular Akt to reduce UVA-induced DNA damage, leading to reduced rates of apoptosis and cell cycle arrest after UVA exposure and restoring collagen expression to normal levels.


Asunto(s)
Panax , Rayos Ultravioleta , Animales , Apoptosis , Ratones , Células 3T3 NIH , Proteínas Proto-Oncogénicas c-akt , Rayos Ultravioleta/efectos adversos , Cicatrización de Heridas
6.
Rev Esp Enferm Dig ; 112(8): 649-658, 2020 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-32686455

RESUMEN

BACKGROUND AND AIMS: novel endoscopic techniques including narrowband imaging (NBI) and blue laser imaging (BLI) have led to the improved detection of early stage gastric cancer and precancerous lesions. However, these techniques are not generally thought to be equivalent at present and BLI is generally considered as superior to NBI. Therefore, this comprehensive meta-analysis aimed to definitively compare the diagnostic efficacy of NBI and BLI for the diagnosis of gastric cancer and precancerous lesions. METHODS: relevant articles were identified via searches of the PubMed, Web of Science, Embase and Cochrane Library databases from their inception until October 2019. In total, 28 relevant studies were identified and incorporated into the meta-analysis. RevMan5.3 was used to assess the relative diagnostic efficacy of these two imaging modalities in these studies. The threshold was assessed using Meta-DiSc 1.4 and STATA 14.0 for bivariate regression modeling of pooled studies. RESULTS: the pooled sensitivity of BLI for gastric cancer was 0.89 (0.80, 0.95) and the specificity was 0.92 (0.76, 0.98). The pooled sensitivity of NBI for gastric cancer was 0.83 (0.75, 0.89) and the specificity was 0.95 (0.91, 0.97). The pooled sensitivity of BLI for precancerous lesions was 0.81 (0.71, 0.87) and the specificity was 0.90 (0.80, 0.96). The pooled sensitivity of NBI for precancerous lesions was 0.80 (0.75, 0.85) and the specificity was 0.88 (0.77, 0.94). CONCLUSIONS: this study showed that both BLI and NBI have a very high diagnostic efficacy for the detection of gastric cancer and precancerous lesions, the sensitivity and specificity of these two approaches were similar.


Asunto(s)
Lesiones Precancerosas , Neoplasias Gástricas , Detección Precoz del Cáncer , Humanos , Rayos Láser , Imagen de Banda Estrecha , Lesiones Precancerosas/diagnóstico por imagen , Sensibilidad y Especificidad , Neoplasias Gástricas/diagnóstico por imagen
7.
Bioorg Med Chem ; 26(11): 2921-2927, 2018 07 15.
Artículo en Inglés | MEDLINE | ID: mdl-29784271

RESUMEN

The rapid rise of antimicrobial resistance is one of the greatest challenges currently facing medical science. The most common cause of resistance to ß-lactam antibiotics is the expression of ß-lactamase enzymes, such as KPC-2. As such the development of novel inhibitors of KPC-2 and related enzymes is of the upmost importance. We report the design and synthesis of novel boronic acid transition state analogs containing a 1,4-substituted 1,2,3-triazole linker based on the known inhibitor 3-nitrophenyl boronic acid and demonstrate that they are promising scaffolds for the development inhibitors of KPC-2 with the ability to recover sensitivity to the antibiotic cefotaxime.


Asunto(s)
Ácidos Borónicos/química , Inhibidores Enzimáticos/síntesis química , beta-Lactamasas/efectos de los fármacos , Ácidos Borónicos/farmacología , Cristalografía por Rayos X , Inhibidores Enzimáticos/química , Inhibidores Enzimáticos/farmacología , Escherichia coli/efectos de los fármacos , Pruebas de Sensibilidad Microbiana , Simulación del Acoplamiento Molecular , Estructura Molecular
8.
J Am Chem Soc ; 137(24): 7596-9, 2015 Jun 24.
Artículo en Inglés | MEDLINE | ID: mdl-26046480

RESUMEN

Synthesizing graphdiyne with a well-defined structure is a great challenge. We reported herein a rational approach to synthesize graphdiyne nanowalls using a modified Glaser-Hay coupling reaction. Hexaethynylbenzene and copper plate were selected as monomer and substrate, respectively. By adjusting the ratio of added organic alkali along with the amount of monomer, the proper amount of copper ions was dissolved into the solution, thus forming catalytic reaction sites. With a rapid reaction rate of Glaser-Hay coupling, graphdiyne grew vertically at these sites first, and then with more copper ions dissolved, uniform graphdiyne nanowalls formed on the surface of copper substrate. Raman spectra, UV-vis spectra, and HRTEM results confirmed the features of graphdiyne. These graphdiyne nanowalls also exhibited excellent and stable field-emission properties.

9.
Phys Chem Chem Phys ; 16(23): 11303-9, 2014 Jun 21.
Artículo en Inglés | MEDLINE | ID: mdl-24789090

RESUMEN

Two-dimensional (2D) materials composed of sp and sp(2) carbon atoms (e.g., graphyne and graphdiyne) show many interesting properties. These materials can be constructed through alkyne homocoupling; however, the occurrence of various side reactions increases the difficulty of their synthesis and structural characterization. Here, we investigate the thermodynamic properties and vibrational spectra of several aryl-alkynes. Both homocoupling and side reactions are found to occur spontaneously at room temperature in terms of thermodynamics. The calculated Raman spectra of the homocoupling products show regular changes with increasing polymerization degree. By rationalizing the vibrational modes of various oligomers, the Raman spectrum of a 2D sp-sp(2) carbon sheet is predicted; it exhibits three sharp peaks at 2241, 1560, and 1444 cm(-1). Although the target and byproducts display similar vibrational modes, a combination of Raman and infrared spectroscopies can be used to differentiate them. The theoretical results are then used to analyze the structure of a synthesized sample and provide useful information.

10.
Materials (Basel) ; 17(9)2024 May 06.
Artículo en Inglés | MEDLINE | ID: mdl-38730969

RESUMEN

In the field of lithium-ion batteries, the challenges posed by the low melting point and inadequate wettability of conventional polyolefin separators have increased the focus on ceramic-coated separators. This study introduces a highly efficient and stable boehmite/polydopamine/polyethylene (AlOOH-PDA-PE) separator. It is crafted by covalently attaching functionalized nanosized boehmite (γ-AlOOH) whiskers onto polyethylene (PE) surfaces. The presence of a covalent bond increases the stability at the interface, while amino groups on the surface of the separator enhance the infiltration of the electrolyte and facilitate the diffusion of lithium ions. The PE-PDA-AlOOH separator, when used in lithium-ion batteries, achieves a discharge capacity of 126 mAh g-1 at 5 C and retains 97.1% capacity after 400 cycles, indicating superior cycling stability due to its covalently bonded ceramic surface. Thus, covalent interface modification is a promising strategy to prevent delamination of ceramic coatings in separators.

11.
Database (Oxford) ; 20232023 Dec 27.
Artículo en Inglés | MEDLINE | ID: mdl-38150626

RESUMEN

De novo molecular generation is a promising approach to drug discovery, building novel molecules from the scratch that can bind the target proteins specifically. With the increasing availability of machine learning algorithms and computational power, artificial intelligence (AI) has emerged as a valuable tool for this purpose. Here, we have developed a database of 3D ligands that collects six AI models for de novo molecular generation based on target proteins, including 20 disease-associated targets. Our database currently includes 1767 protein targets and up to 164 107 de novo-designed molecules. The primary goal is to provide an easily accessible and user-friendly molecular database for professionals in the fields of bioinformatics, pharmacology and related areas, enabling them to efficiently screen for potential lead compounds with biological activity. Additionally, our database provides a comprehensive resource for computational scientists to explore and compare different AI models in terms of their performance in generating novel molecules with desirable properties. All the resources and services are publicly accessible at https://cmach.sjtu.edu.cn/drug/. Database URL: https://cmach.sjtu.edu.cn/drug/.


Asunto(s)
Inteligencia Artificial , Proteínas , Algoritmos , Descubrimiento de Drogas , Bases de Datos Factuales , Diseño de Fármacos
12.
Front Psychiatry ; 14: 1219592, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-37492064

RESUMEN

Background: Reversible splenial lesion syndrome (RESLES) is a rare neurological condition characterized by temporary abnormalities in the splenium of the corpus callosum, which has been reported in mental disorders. Previous studies on bipolar disorder (BD) primarily focused on aspects such as brain structure and function, neurochemical changes, and genetics. However, there have been no studies reporting the occurrence of this syndrome during hypomanic episodes and its disappearance during the remission phase in bipolar disorder type 2 (BD-II). Case presentation: We present a case report of a 30 years-old female patient with BD-II who exhibited symptoms of RESLES during a hypomanic episode. The patient, with a 12 years psychiatric history, has experienced recurrent depressive episodes initially, with the first hypomanic episode occurring 8 years ago. During this period, this patient made several visits to the outpatient clinic to have her medications adjusted due to repeated suicide attempts. This time, she was admitted to our hospital with a second hypomanic episode due to drug withdrawal during pregnancy. The RESLES was observed on her brain magnetic resonance image, and it was alleviated after treatment with lithium carbonate and quetiapine until achieving remission. Conclusion: We present the first report of identifying RESLES in BD-II with hypomanic episodes, which subsequently disappears during the remission phase. Our case report highlights a potential association between BD and RESLES, emphasizing the need for future studies to explore the underlying mechanisms connecting these two conditions in greater depth.

13.
Int J Numer Method Biomed Eng ; 39(10): e3737, 2023 10.
Artículo en Inglés | MEDLINE | ID: mdl-37269226

RESUMEN

Central venous disease (CVD) with stenosis or occlusion is a severe and prevalent complication for chronic hemodialysis (HD) patients, resulting in dialysis access dysfunction. Percutaneous transluminal angioplasty with stent placement (PTS) has become one of the first-line treatments for CVD. In clinical practice, the extra stents would be used if the curative efficacy of a single stent were unsatisfactory. Aiming to evaluate the therapeutic effect of different PTS schemes, computational fluid dynamics (CFD) simulations on four patients were performed to compare the hemodynamic characteristics of real-life HD patients after stent placement. The three-dimensional central vein's models of each patient were built using computational tomography angiography (CTA) images, and idealized models were constructed as contrast. Two inlet velocity modes were imposed to imitate the blood flow rate of healthy and HD patients. The hemodynamic parameters for different patients were investigated, including wall shear stress (WSS), velocity, and helicity. The results showed that the implantation of double stents is able to improve flexibility. When subjected to external force, the double stents have better radial stiffness. This paper evaluated the therapeutic efficacy of stent placement and provided a theoretical basis for CVD intervention in hemodialysis patients.


Asunto(s)
Enfermedades Cardiovasculares , Stents , Humanos , Venas , Angioplastia/métodos , Hemodinámica
14.
J Funct Biomater ; 14(6)2023 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-37367273

RESUMEN

Polymeric heart valves (PHVs) are a promising and more affordable alternative to mechanical heart valves (MHVs) and bioprosthetic heart valves (BHVs). Materials with good durability and biocompatibility used for PHVs have always been the research focus in the field of prosthetic heart valves for many years, and leaflet thickness is a major design parameter for PHVs. The study aims to discuss the relationship between material properties and valve thickness, provided that the basic functions of PHVs are qualified. The fluid-structure interaction (FSI) approach was employed to obtain a more reliable solution of the effective orifice area (EOA), regurgitant fraction (RF), and stress and strain distribution of the valves with different thicknesses under three materials: Carbothane PC-3585A, xSIBS and SIBS-CNTs. This study demonstrates that the smaller elastic modulus of Carbothane PC-3585A allowed for a thicker valve (>0.3 mm) to be produced, while for materials with an elastic modulus higher than that of xSIBS (2.8 MPa), a thickness less than 0.2 mm would be a good attempt to meet the RF standard. What is more, when the elastic modulus is higher than 23.9 MPa, the thickness of the PHV is recommended to be 0.l-0.15 mm. Reducing the RF is one of the directions of PHV optimization in the future. Reducing the thickness and improving other design parameters are reliable means to reduce the RF for materials with high and low elastic modulus, respectively.

15.
Front Pharmacol ; 14: 1106423, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-37006998

RESUMEN

Background: Lamotrigine may cause severe skin reactions. There is a known interaction between lamotrigine and valproic acid with an increase in lamotrigine levels and lamotrigine toxicity risk. Few cases of severe rash and systemic reactions in bipolar patients using lamotrigine and valproate have been reported. Here, we report a rare case of severe skin rash and lymphadenopathy associated with lamotrigine-valproic acid combination. Case presentation: An 18-year-old female adolescent with bipolar disorder type I was treated with lamotrigine, magnesium valproate, and perospirone for 12 days. After the last dose of lamotrigine, she abruptly developed generalized rash and swollen lymph nodes, which continued to progress over the next 3 days. This finally subsided after stopping valproate and with glucocorticoid treatment. Conclusion: This case suggests that lamotrigine-valproic acid combination may cause not only rash but also lymphadenopathy. Even though the aforementioned reactions appear after the last dose of lamotrigine, it cannot be ruled out as suspicious. We recommend caution during titration of lamotrigine and valproate and early withdrawal of both when signs of hypersensitivity appear.

16.
Polymers (Basel) ; 15(3)2023 Jan 25.
Artículo en Inglés | MEDLINE | ID: mdl-36771918

RESUMEN

With the improvement of protection technology, the damage power of conventional penetrators has become increasingly inferior. Reactive material is a new type of energetic material, which has strong energy release capabilities under high-velocity-impact conditions. In this paper, the reactive materials were put into the penetrator, and its penetration characteristics were studied. First, the penetrator with enhanced lateral effect (PELE) projectile structure with better penetration capability was obtained by numerical simulation. Then, based on the established polytetrafluoroethylene (PTFE)/Al reactive material reaction model, the numerical simulation and experimental research of the PELE projectile with a reactive inner core penetrating the target were carried out. The results show that the simulation results are in good agreement with the experimental results, which verifies the confidence of the numerical simulation. The PELE projectile had a significant increase in power with the use of a truncated conical head and reactive materials. The residual velocity of the truncated cone PELE projectile increases by 8.41-21% over conventional PELE projectiles. Its damage range is 43% higher than that of conventional penetrators. The simulation method and the conclusions obtained in this paper can provide support and reference for further research on reactive materials and on effectively improving the damage power of the penetrator.

17.
Exp Ther Med ; 26(6): 581, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-38023355

RESUMEN

[This retracts the article DOI: 10.3892/etm.2019.8270.].

18.
J Ginseng Res ; 47(6): 714-725, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-38107393

RESUMEN

Background: Our previous investigation indicated that the preparation of Panax ginseng Meyer (P. ginseng) inhibited melanogenesis. It comprised salicylic acid (SA), protocatechuic acid (PA), p-coumaric acid (p-CA), vanillic acid (VA), and caffeic acid (CA). In this investigation, the regulatory effects of P. ginseng phenolic acid monomers on melanin production were assessed. Methods: In vitro and in vivo impact of phenolic acid monomers were assessed. Results: SA, PA, p-CA and VA inhibited tyrosinase (TYR) to reduce melanin production, whereas CA had the opposite effects. SA, PA, p-CA and VA significantly downregulated the melanocortin 1 receptor (MC1R), cycle AMP (cAMP), protein kinase A (PKA), cycle AMP-response element-binding protein (CREB), microphthalmia-associated transcription factor (MITF) pathway, reducing mRNA and protein levels of TYR, tyrosinase-related protein 1 (TYRP1), and TYRP2. Moreover, CA treatment enhanced the cAMP, PKA, and CREB pathways to promote MITF mRNA level and phosphorylation. It also alleviated MITF protein level in α-MSH-stimulated B16F10 cells, comparable to untreated B16F10, increasing the expression of phosphorylation glycogen synthase kinase 3ß (p-GSK3ß), ß-catenin, p-ERK/ERK, and p-p38/p38. Furthermore, the GSK3ß inhibitor promoted p-GSK3ß and p-MITF expression, as observed in CA-treated cells. Moreover, p38 and ERK inhibitors inhibited CA-stimulated p-p38/p38, p-ERK/ERK, and p-MITF increase, which had negative binding energies with MC1R, as depicted by molecular docking. Conclusion: P. ginseng roots' phenolic acid monomers can safely inhibit melanin production by bidirectionally regulating melanin synthase transcription. Furthermore, they reduced MITF expression via MC1R/cAMP/PKA signaling pathway and enhanced MITF post-translational modification via Wnt/mitogen-activated protein kinase signaling pathway.

19.
Nat Nanotechnol ; 18(4): 357-364, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36702955

RESUMEN

The success of the lead halide perovskites in diverse optoelectronics has motivated considerable interest in their fundamental photocarrier dynamics. Here we report the discovery of photocarrier-induced persistent structural polarization and local ferroelectricity in lead halide perovskites. Photoconductance studies of thin-film single-crystal CsPbBr3 at 10 K reveal long-lasting persistent photoconductance with an ultralong photocarrier lifetime beyond 106 s. X-ray diffraction studies reveal that photocarrier-induced structural polarization is present up to a critical freezing temperature. Photocapacitance studies at cryogenic temperatures further demonstrate a systematic local phase transition from linear dielectric to paraelectric and relaxor ferroelectric under increasing illumination. Our theoretical investigations highlight the critical role of photocarrier-phonon coupling and large polaron formation in driving the local relaxor ferroelectric phase transition. Our findings show that this photocarrier-induced persistent structural polarization enables the formation of ferroelectric nanodomains at low temperature, which suppress carrier recombination and offer the possibility of exploring intriguing carrier-phonon interplay and the rich polaron photophysics.

20.
Eur J Med Chem ; 240: 114571, 2022 Oct 05.
Artículo en Inglés | MEDLINE | ID: mdl-35792385

RESUMEN

Inhibition of ß-lactamases is a promising strategy to overcome antimicrobial resistance to commonly used ß-lactam antibiotics. Boronic acid derivatives have proven to be effective inhibitors of ß-lactamases due to their direct interaction with the catalytic site of these enzymes. We synthesized a series of phenylboronic acid derivatives and evaluated their structure-activity relationships as Klebsiella pneumoniae carbapenemase (KPC-2) inhibitors. We identified potent KPC-2 inhibitors 2e & 6c (Ki = 0.032 µM and 0.038 µM, respectively) that enhance the activity of cefotaxime in KPC-2 expressing Escherichia coli. The measured acid dissociation constants (pKa) of selected triazole-containing phenylboronic acids was broad (5.98-10.0), suggesting that this is an additional property of the compounds that could be tuned to optimize the target interaction and/or the physicochemical properties of the compounds. These findings will help to guide the future development of boronic acid compounds as inhibitors of KPC-2 and other target proteins.


Asunto(s)
Klebsiella pneumoniae , Triazoles , Antibacterianos/metabolismo , Antibacterianos/farmacología , Proteínas Bacterianas/metabolismo , Ácidos Borónicos/química , Farmacorresistencia Microbiana , Escherichia coli , Pruebas de Sensibilidad Microbiana , Triazoles/farmacología , Inhibidores de beta-Lactamasas/metabolismo , Inhibidores de beta-Lactamasas/farmacología , beta-Lactamasas/metabolismo
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