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1.
Phys Rev Lett ; 125(14): 146801, 2020 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-33064521

RESUMO

Graphene nanoribbons (GNRs), low-dimensional platforms for carbon-based electronics, show the promising perspective to also incorporate spin polarization in their conjugated electron system. However, magnetism in GNRs is generally associated with localized states around zigzag edges, difficult to fabricate and with high reactivity. Here we demonstrate that magnetism can also be induced away from physical GNR zigzag edges through atomically precise engineering topological defects in its interior. A pair of substitutional boron atoms inserted in the carbon backbone breaks the conjugation of their topological bands and builds two spin-polarized boundary states around them. The spin state was detected in electrical transport measurements through boron-substituted GNRs suspended between the tip and the sample of a scanning tunneling microscope. First-principle simulations find that boron pairs induce a spin 1, which is modified by tuning the spacing between pairs. Our results demonstrate a route to embed spin chains in GNRs, turning them into basic elements of spintronic devices.

2.
Nat Commun ; 11(1): 4361, 2020 08 31.
Artigo em Inglês | MEDLINE | ID: mdl-32868773

RESUMO

The sensory responses of cortical neuronal populations following training have been extensively studied. However, the spike firing properties of individual cortical neurons following training remain unknown. Here, we have combined two-photon Ca2+ imaging and single-cell electrophysiology in awake behaving mice following auditory associative training. We find a sparse set (~5%) of layer 2/3 neurons in the primary auditory cortex, each of which reliably exhibits high-rate prolonged burst firing responses to the trained sound. Such bursts are largely absent in the auditory cortex of untrained mice. Strikingly, in mice trained with different multitone chords, we discover distinct subsets of neurons that exhibit bursting responses specifically to a chord but neither to any constituent tone nor to the other chord. Thus, our results demonstrate an integrated representation of learned complex sounds in a small subset of cortical neurons.


Assuntos
Córtex Auditivo/fisiologia , Percepção Auditiva/fisiologia , Neurônios/fisiologia , Estimulação Acústica/métodos , Córtex Auditivo/citologia , Sinalização do Cálcio , Eletrofisiologia/métodos , Aprendizagem/fisiologia , Microscopia de Fluorescência por Excitação Multifotônica/métodos , Neurônios/metabolismo , Análise de Célula Única/métodos
3.
Cell Calcium ; 91: 102265, 2020 11.
Artigo em Inglês | MEDLINE | ID: mdl-32814243

RESUMO

Fractalkine (FKN) and its specific receptor CX3CR1 play a critical role in the pathogenesis of atherosclerosis including recruitment of vascular cells and the development of inflammation. However, its contribution to regulating the development of atherosclerotic calcification has not been well documented. Osteogenic transformation of vascular smooth muscle cells (VSMCs) is critical in the development of calcification in atherosclerotic lesions. In this study, for the first time, we evaluated the effect of FKN/CX3CR1 on the progression of VSMCs calcification and defined molecular signaling that is operative in the FKN/CX3CR1-induced osteogenic transformation of VSMCs. We found that high-fat diet induced atherosclerotic calcification in vivo was markedly inhibited in the Apolipoprotein E (ApoE) and CX3CR1 deficient (ApoE-/-/CX3CR1-/-) mice compared with their control littermates. FKN and CX3CR1 were both expressed in VSMCs and up-regulated by oxidized low-density lipoprotein (ox-LDL). FKN/CX3CR1 promoted the expression of osteogenic markers, including osteopontin (OPN), bone morphogenetic protein (BMP)-2 and alkaline phosphatase (ALP) and decreased VSMCs markers, including smooth muscle (SM) α-actin and SM22-α in a dose-dependent manner. The essential role of FKN/CX3CR1 in VSMCs calcification was further confirmed by lentivirus-mediated knockdown or overexpression of CX3CR1 blocked or accelerated osteogenic transformation of VSMCs. This response was associated with reciprocal up- and down-regulation of osteogenic factor, runt-related transcription factor 2 (RUNX2), transcription factors in osteoclast differentiation, receptor activator of nuclear factor-κB (RANK), RANK ligand (RNAKL) and osteoprotegerin (OPG), respectively. Inhibition of FKN/CX3CR1-activated Jak2/Stat3 signaling by the Jak/Stat inhibitor AG490 blocked osteogenic transformation of VSMCs and RUNX2 induction concurrently. Taken together, our data uncovered novel roles of FKN/CX3CR1 in promoting VSMC osteogenic transformation and atherosclerotic calcification by activating RUNX2 through Jak2/Stat3 signaling pathway and suppressing OPG. Our findings suggest that targeting FKN/CX3CR1 may provide new strategies for the prevention and treatment of atherosclerotic calcification.

4.
Nat Commun ; 11(1): 2566, 2020 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-32444665

RESUMO

Adsorption of magnetic transition metal atoms on a metal surface leads to the formation of Kondo states at the atom/metal interfaces. However, the significant influence of surrounding environment presents challenges for potential applications. In this work, we realize a novel strategy to regularize the Kondo states by moving a CoPc molecular mold on an Au(111) surface to capture the dispersed Co adatoms. The symmetric and ordered structures of the atom-mold complexes, as well as the strong dπ-π bonding between the Co adatoms and conjugated isoindole units, result in highly robust and uniform Kondo states at the Co/Au(111) interfaces. Even more remarkably, the CoPc further enables a fine tuning of Kondo states through the molecular-mold-mediated superexchange interactions between Co adatoms separated by more than 12 Å. Being highly precise, efficient and reproducible, the proposed molecular mold strategy may open a new horizon for the construction and control of nano-sized quantum devices.

5.
Phys Rev Lett ; 124(17): 177201, 2020 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-32412280

RESUMO

Graphene can develop large magnetic moments in custom-crafted open-shell nanostructures such as triangulene, a triangular piece of graphene with zigzag edges. Current methods of engineering graphene nanosystems on surfaces succeeded in producing atomically precise open-shell structures, but demonstration of their net spin remains elusive to date. Here, we fabricate triangulenelike graphene systems and demonstrate that they possess a spin S=1 ground state. Scanning tunneling spectroscopy identifies the fingerprint of an underscreened S=1 Kondo state on these flakes at low temperatures, signaling the dominant ferromagnetic interactions between two spins. Combined with simulations based on the meanfield Hubbard model, we show that this S=1 π paramagnetism is robust and can be turned into an S=1/2 state by additional H atoms attached to the radical sites. Our results demonstrate that π paramagnetism of high-spin graphene flakes can survive on surfaces, opening the door to study the quantum behavior of interacting π spins in graphene systems.

6.
ACS Nano ; 14(2): 1895-1901, 2020 Feb 25.
Artigo em Inglês | MEDLINE | ID: mdl-31999431

RESUMO

The electronic properties of graphene nanoribbons (GNRs) can be precisely tuned by chemical doping. Here we demonstrate that amino (NH2) functional groups attached at the edges of chiral GNRs (chGNRs) can efficiently gate the chGNRs and lead to the valence band (VB) depopulation on a metallic surface. The NH2-doped chGNRs are grown by on-surface synthesis on Au(111) using functionalized bianthracene precursors. Scanning tunneling spectroscopy resolves that the NH2 groups significantly upshift the bands of chGNRs, causing the Fermi level crossing of the VB onset of chGNRs. Through density functional theory simulations we confirm that the hole-doping behavior is due to an upward shift of the bands induced by the edge NH2 groups.

7.
ACS Nano ; 13(9): 9936-9943, 2019 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-31381315

RESUMO

Controlling the spin of metal atoms embedded in molecular systems is a key step toward the realization of molecular electronics and spintronics. Many efforts have been devoted to explore the influencing factors dictating the survival or quenching of a magnetic moment in a metal-organic molecule, and among others, the spin control by axial ligand attachments is the most promising. Herein, from the interplay of high-resolution scanning tunneling microscopy imaging/manipulation and scanning tunneling spectroscopy measurements together with density functional theory calculations, we successfully demonstrate that a Ni trimer within a metal-organic motif acquires a net spin promoted by the adsorption of an on-top Br atom. The spin localization in the trimetal centers bonded to Br was monitored via the Kondo effect. The removal of the Br ligand resulted in the switch from a Kondo ON to a Kondo OFF state. The magnetic state induced by the Br ligand is theoretically attributed to the enhanced Br 4pz and Ni 3dz2 states due to the charge redistribution. The manipulation strategy reported here provides the possibility to explore potential applications of spin-tunable structures in spintronic devices.

8.
Chemphyschem ; 20(18): 2305-2310, 2019 09 17.
Artigo em Inglês | MEDLINE | ID: mdl-31328365

RESUMO

Within the collection of surface-supported reactions currently accessible for the production of extended molecular nanostructures under ultra-high vacuum, Ullmann coupling has been the most successful in the controlled formation of covalent single C-C bonds. Particularly advanced control of this synthetic tool has been obtained by means of hierarchical reactivity, commonly achieved by the use of different halogen atoms that consequently display distinct activation temperatures. Here we report on the site-selective reactivity of certain carbon-halogen bonds. We use precursor molecules halogenated with bromine atoms at two non-equivalent carbon atoms and found that the Ullmann coupling occurs on Au(111) with a remarkable predilection for one of the positions. Experimental evidence is provided by means of scanning tunneling microscopy and core level photoemission spectroscopy, and a rationalized understanding of the observed preference is obtained from density functional theory calculations.

9.
Nano Lett ; 19(5): 3288-3294, 2019 05 08.
Artigo em Inglês | MEDLINE | ID: mdl-30964303

RESUMO

We report on the fabrication and transport characterization of atomically precise single-molecule devices consisting of a magnetic porphyrin covalently wired by graphene nanoribbon electrodes. The tip of a scanning tunneling microscope was utilized to contact the end of a GNR-porphyrin-GNR hybrid system and create a molecular bridge between the tip and sample for transport measurements. Electrons tunneling through the suspended molecular heterostructure excited the spin multiplet of the magnetic porphyrin. The detachment of certain spin centers from the surface shifted their spin-carrying orbitals away from an on-surface mixed-valence configuration, recovering its original spin state. The existence of spin-polarized resonances in the free-standing systems and their electrical addressability is the fundamental step in the utilization of carbon-based materials as functional molecular spintronics systems.

10.
Nat Commun ; 10(1): 200, 2019 01 14.
Artigo em Inglês | MEDLINE | ID: mdl-30643120

RESUMO

Turning graphene magnetic is a promising challenge to make it an active material for spintronics. Predictions state that graphene structures with specific shapes can spontaneously develop magnetism driven by Coulomb repulsion of π-electrons, but its experimental verification is demanding. Here, we report on the observation and manipulation of individual magnetic moments in graphene open-shell nanostructures on a gold surface. Using scanning tunneling spectroscopy, we detect the presence of single electron spins localized around certain zigzag sites of the carbon backbone via the Kondo effect. We find near-by spins coupled into a singlet ground state and quantify their exchange interaction via singlet-triplet inelastic electron excitations. Theoretical simulations picture how electron correlations result in spin-polarized radical states with the experimentally observed spatial distributions. Extra hydrogen atoms bound to radical sites quench their magnetic moment and switch the spin of the nanostructure in half-integer amounts. Our work demonstrates the intrinsic π-paramagnetism of graphene nanostructures.

11.
Nat Neurosci ; 21(11): 1541-1550, 2018 11.
Artigo em Inglês | MEDLINE | ID: mdl-30361547

RESUMO

Urination (also called micturition) is thought to be regulated by a neural network that is distributed in both subcortical and cortical regions. Previously, urination-related neurons have been identified in subcortical structures such as the pontine micturition center (also known as Barrington's nucleus). However, the origin of the descending cortical pathway and how it interfaces with this subcortical circuit to permit voluntary initiation of urination remain elusive. Here we identified a small cluster of layer 5 neurons in the primary motor cortex whose activities tightly correlate with the onset of urination in freely behaving mice and increase dramatically during territorial marking. Optogenetically activating these neurons elicits contraction of the bladder and initiates urination, through their projections to the pontine micturition center, while silencing or ablating them impairs urination and causes retention of urine. Together these results reveal a novel cortical component upstream of the pontine micturition center that is critically involved in urination.


Assuntos
Córtex Motor/fisiologia , Neurônios/fisiologia , Ponte/fisiologia , Bexiga Urinária , Micção/fisiologia , Animais , Camundongos , Vias Neurais/fisiologia , Medula Espinal/fisiologia , Bexiga Urinária/fisiologia
12.
Biochem Biophys Res Commun ; 503(3): 1356-1363, 2018 09 10.
Artigo em Inglês | MEDLINE | ID: mdl-30007438

RESUMO

High-fat diet (HFD) is known to promote atherosclerosis which accelerates the development of atherosclerotic cardiovascular diseases. Vascular dysfunction characterized by inflammation and lipid accumulation is common in atherosclerosis caused by HFD. The specific effects of HFD on blood vessels and the underlying mechanisms need to be further clarified. Toll-like receptor 4 (TLR4) is a key contributing factor in atherosclerosis and TLR4 deficiency protects vascular smooth muscle cells against inflammatory responses and lipid accumulation in vitro. However, the physiological significance of TLR4 signaling in HFD-induced changes is unknown. In this study, we observed that HFD feeding increased body weight, circulating inflammatory cytokines and lipid accumulation in the aorta of wild-type mice but apart from increasing body weight, did not affect the TLR4 knockout mice. TLR4 expression increased significantly in the arterial walls after receiving HFD treatment, while that of the co-localizing PPARγ and ABCG1 markedly decreased. TLR4 deficiency reversed the HFD-induced attenuation of PPARγ and ABCG1. In conclusion, TLR4 mediates HFD induced increase in body weight, inflammation and aortic lipid accumulation through, at least partly, the PPARγ/ABCG1 signaling pathway. Therefore, interfering with TLR4 signaling is a viable therapeutic option in diet induced atherosclerosis.


Assuntos
Membro 1 da Subfamília G de Transportadores de Cassetes de Ligação de ATP/metabolismo , Dieta Hiperlipídica/efeitos adversos , Inflamação/metabolismo , Músculo Liso Vascular/metabolismo , PPAR gama/metabolismo , Receptor 4 Toll-Like/metabolismo , Animais , Ensaio de Imunoadsorção Enzimática , Inflamação/patologia , Lipídeos/química , Masculino , Camundongos , Camundongos Endogâmicos C57BL , Camundongos Knockout , Músculo Liso Vascular/patologia , Transdução de Sinais , Receptor 4 Toll-Like/deficiência
13.
Sci Adv ; 4(2): eaaq0582, 2018 02.
Artigo em Inglês | MEDLINE | ID: mdl-29464209

RESUMO

We report on the construction and magnetic characterization of a fully functional hybrid molecular system composed of a single magnetic porphyrin molecule bonded to graphene nanoribbons with atomically precise contacts. We use on-surface synthesis to direct the hybrid creation by combining two molecular precursors on a gold surface. High-resolution imaging with a scanning tunneling microscope finds that the porphyrin core fuses into the graphene nanoribbons through the formation of new carbon rings at chemically predefined positions. These ensure the stability of the hybrid and the extension of the conjugated character of the ribbon into the molecule. By means of inelastic tunneling spectroscopy, we prove the survival of the magnetic functionality of the contacted porphyrin. The molecular spin appears unaffected by the graphenoid electrodes, and we simply observe that the magnetic anisotropy appears modified depending on the precise structure of the contacts.

14.
Sci Rep ; 8(1): 49, 2018 01 08.
Artigo em Inglês | MEDLINE | ID: mdl-29311673

RESUMO

In the primary auditory cortex (A1), neuronal ensembles are activated relative to anticipated sound events following rhythmic stimulation, but whether the echo responses of the neurons are related to their frequency selectivity remains unknown. Therefore, we used in vivo two-photon Ca2+ imaging to record the neuronal activities in the mouse A1 to elucidate the relationship between their echo responses and frequency selectivity. We confirmed the presence of echo responses in a subgroup of mouse Layer 2/3 A1 neurons following a train of rhythmic pure tone stimulation. After testing with a range of frequencies, we found that these echo responses occurred preferentially close to the best frequencies of the neurons. The local organization of the echo responses of the neurons was heterogeneous in the A1. Therefore, these results indicate that the observed echo responses of neurons within A1 are highly related to their frequency selectivity.


Assuntos
Córtex Auditivo/fisiologia , Percepção Auditiva , Estimulação Acústica , Animais , Mapeamento Encefálico , Cálcio/metabolismo , Fenômenos Eletrofisiológicos , Potenciais Evocados Auditivos , Masculino , Camundongos , Imagem Molecular/métodos , Neurônios/metabolismo , Tempo de Reação
15.
Prog Electromagn Res M Pier M ; 75: 193-203, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30595794

RESUMO

Magnetic proximity detection systems (PDSs) used in underground mines occasionally generate false alarms when the miner-wearable component (MWC) is close to nearby conductors such as power cables. This is because the signals from the generators (antennas) of the PDS wirelessly couple to nearby cables, travel along these cables, and then couple back from the cable to a distant MWC to cause a false alarm. In order to manage such a false alarm, it is necessary to understand the basic near-field coupling characteristics from a generator to a long wire. Researchers from the National Institute for Occupational Safety and Health (NIOSH) have developed a method to measure such coupling characteristics for a ferrite-cored antenna to a straight wire. The method is introduced in this paper along with the test results.

16.
Brain Struct Funct ; 223(1): 519-533, 2018 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-29124351

RESUMO

Two-photon Ca2+ imaging has become a popular approach for monitoring neuronal population activity with cellular or subcellular resolution in vivo. This approach allows for the recording of hundreds to thousands of neurons per animal and thus leads to a large amount of data to be processed. In particular, manually drawing regions of interest is the most time-consuming aspect of data analysis. However, the development of automated image analysis pipelines, which will be essential for dealing with the likely future deluge of imaging data, remains a major challenge. To address this issue, we developed NeuroSeg, an open-source MATLAB program that can facilitate the accurate and efficient segmentation of neurons in two-photon Ca2+ imaging data. We proposed an approach using a generalized Laplacian of Gaussian filter to detect cells and weighting-based segmentation to separate individual cells from the background. We tested this approach on an in vivo two-photon Ca2+ imaging dataset obtained from mouse cortical neurons with differently sized view fields. We show that this approach exhibits superior performance for cell detection and segmentation compared with the existing published tools. In addition, we integrated the previously reported, activity-based segmentation into our approach and found that this combined method was even more promising. The NeuroSeg software, including source code and graphical user interface, is freely available and will be a useful tool for in vivo brain activity mapping.


Assuntos
Cálcio/metabolismo , Processamento Eletrônico de Dados/métodos , Neurônios/citologia , Neurônios/fisiologia , Algoritmos , Animais , Mapeamento Encefálico , Tamanho Celular , Processamento Eletrônico de Dados/instrumentação , Processamento de Imagem Assistida por Computador , Masculino , Camundongos , Camundongos Endogâmicos C57BL , Distribuição Normal , Óptica e Fotônica , Software
17.
J Stroke Cerebrovasc Dis ; 27(2): 479-485, 2018 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-29056405

RESUMO

BACKGROUND: In the Stenting and Aggressive Medical Management for Preventing Recurrent Stroke in Intracranial Stenosis (SAMMPRIS) trial, 19.1% of ischemic strokes occurred out of the territory of previously symptomatic stenosis during the mean follow-up period of 23.4 months. However, it is unknown how many ischemic strokes were due to a previously asymptomatic intracranial atherosclerotic stenosis (ICAS). The objective of this study was to investigate whether the concomitant asymptomatic ICAS influences the outcome of patients undergoing symptomatic ICAS stenting. METHODS: We retrospectively reviewed 576 consecutive patients with nondisabling ischemic stroke (modified Rankin scale score of ≤3) who were treated with symptomatic ICAS (≥70% stenosis) stenting with or without concomitant asymptomatic ICAS. The baseline characteristics and the 30-day primary end points (stroke or death after stenting) were compared by bivariate and multivariable logistic analyses. RESULTS: The 30-day rate of primary end points was 5.2%, which was higher in patients with concomitant asymptomatic ICAS (≥50% stenosis) than in those without asymptomatic ICAS (no stenosis or <50% stenosis) (8.9% versus 3.8%, P = .014). In patients with concomitant asymptomatic ICAS, 25% of ischemic strokes occurred out of the territory of the stented artery, whereas in patients without asymptomatic ICAS, no ischemic stroke occurred out of the territory of the stented artery. Multivariable analysis showed that concomitant asymptomatic ICAS was an independent risk factor for 30-day stroke (odds ratio = 2.37, 95% confidence interval, 1.14-5.63; P = .023). CONCLUSIONS: Concomitant asymptomatic ICAS (≥50% stenosis) might increase the 30-day risk of stroke in patients undergoing symptomatic ICAS stenting.


Assuntos
Procedimentos Endovasculares/efeitos adversos , Procedimentos Endovasculares/instrumentação , Arteriosclerose Intracraniana/terapia , Stents , Acidente Vascular Cerebral/etiologia , Doenças Assintomáticas , Distribuição de Qui-Quadrado , China , Feminino , Humanos , Arteriosclerose Intracraniana/complicações , Arteriosclerose Intracraniana/diagnóstico por imagem , Modelos Logísticos , Masculino , Pessoa de Meia-Idade , Análise Multivariada , Razão de Chances , Estudos Retrospectivos , Medição de Risco , Fatores de Risco , Índice de Gravidade de Doença , Acidente Vascular Cerebral/diagnóstico , Fatores de Tempo , Resultado do Tratamento
18.
J Phys Chem Lett ; 9(1): 25-30, 2018 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-29220194

RESUMO

Recent advances in graphene-nanoribbon-based research have demonstrated the controlled synthesis of chiral graphene nanoribbons (chGNRs) with atomic precision using strategies of on-surface chemistry. However, their electronic characterization, including typical figures of merit like band gap or frontier band's effective mass, has not yet been reported. We provide a detailed characterization of (3,1)-chGNRs on Au(111). The structure and epitaxy, as well as the electronic band structure of the ribbons, are analyzed by means of scanning tunneling microscopy and spectroscopy, angle-resolved photoemission, and density functional theory.

19.
ACS Nano ; 11(11): 11661-11668, 2017 11 28.
Artigo em Inglês | MEDLINE | ID: mdl-29049879

RESUMO

We report the energy level alignment evolution of valence and conduction bands of armchair-oriented graphene nanoribbons (aGNR) as their band gap shrinks with increasing width. We use 4,4″-dibromo-para-terphenyl as the molecular precursor on Au(111) to form extended poly-para-phenylene nanowires, which can subsequently be fused sideways to form atomically precise aGNRs of varying widths. We measure the frontier bands by means of scanning tunneling spectroscopy, corroborating that the nanoribbon's band gap is inversely proportional to their width. Interestingly, valence bands are found to show Fermi level pinning as the band gap decreases below a threshold value around 1.7 eV. Such behavior is of critical importance to understand the properties of potential contacts in GNR-based devices. Our measurements further reveal a particularly interesting system for studying Fermi level pinning by modifying an adsorbate's band gap while maintaining an almost unchanged interface chemistry defined by substrate and adsorbate.

20.
Adv Mater ; 29(38)2017 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-28833592

RESUMO

Interference-free hyperbolic phonon polaritons (HPPs) excited by natural wrinkles in a hexagonal boron nitride (hBN) microcrystal are reported both experimentally and theoretically. Although their geometries are off-resonant with the excitation wavelength, the wrinkles compensate for the large momentum mismatch between photon and phonon polariton, and launch the HPPs without interference. The spatial feature of wrinkles is about 200 nm, which is an order of magnitude smaller than resonant metal antennas at the same excitation wavelength. Compared with phonon polaritons launched by an atomic force microscopy tip, the phonon polaritons launched by wrinkles are interference-free, independent of the launcher geometry, and exhibit a smaller damping rate (γ ≈ 0.028). On the same hBN microcrystal, in situ nanoinfrared imaging of HPPs launched by different mechanisms is performed. In addition, the dispersion of HPPs is modified by changing the dielectric environments of hBN crystals. The wavelength of HPPs is compressed twofold when the substrate is changed from SiO2 to gold. The findings provide insights into the intrinsic properties of hBN-HPPs and demonstrate a new way to launch and control polaritons in van der Waals materials.

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