RESUMO
We study the nanoscale patterns that form on the surface of a rotating sample of an elemental material that is bombarded with a broad noble gas ion beam for angles of incidence θ just above the critical angle for pattern formation θ_{c}. The pattern formation depends crucially on the ion energy E. In simulations carried out in the low-energy regime in which sputtering is negligible, we find disordered arrays of nanoscale mounds (nanodots) that coarsen in time. Disordered arrays of nanodots also form in the high-energy regime in which there is substantial sputtering, but no coarsening occurs close to the threshold angle. Finally, for values of E just above the sputter yield threshold, nanodot arrays with an extraordinary degree of hexagonal order emerge for a range of parameter values, even though there is a broad band of linearly unstable wavelengths. This finding might prove to be useful in applications in which highly ordered nanoscale patterns are needed.
RESUMO
It is critical to understand the laws of quantum mechanics in transformative technologies for computation and quantum information science applications to enable the ongoing second quantum revolution calls. Recently, spin qubits based on point defects have gained great attention, since these qubits can be initiated, selectively controlled, and read out with high precision at ambient temperature. The major challenge in these systems is controllably generating multiqubit systems while properly coupling the defects. To address this issue, we began by tackling the engineering challenges these systems present and understanding the fundamentals of defects. In this regard, we controllably generate defects in MoS2 and WS2 monolayers and tune their physicochemical properties via proton irradiation. We quantitatively discovered that the proton energy could modulate the defects' density and nature; higher defect densities were seen with lower proton irradiation energies. Three distinct defect types were observed: vacancies, antisites, and adatoms. In particular, the creation and manipulation of antisite defects provides an alternative way to create and pattern spin qubits based on point defects. Our results demonstrate that altering the particle irradiation energy can regulate the formation of defects, which can be utilized to modify the properties of 2D materials and create reliable electronic devices.
RESUMO
Somatostatin derivative peptides previously designed for radiodiagnostic purposes (99mTc P829 or 99mTc depreotide) were reoptimized for radiotherapy of tumors with rhenium radioisotopes. An optimized pharmacophore peptide P1839 was derived by in vitro binding affinity assay to AR42J rat pancreatic tumor cell membranes. Peptides with chelating domains and their oxorhenium(V) complexes were tested in vitro for binding to NCI H69 human SCLC tumor membranes. Further optimization entailed radiolabeling with 99mTc and biodistribution in an AR42J xenograft mouse model. Kidney uptake was decreased substantially by removing positively charged residues. Neutral N3S diamide amine thiol chelators with no adjacent positive charges had the best overall properties. Substituting an aromatic amino acid into the chelator approximately doubled the tumor uptake. The final optimized peptide P2045 (39) radiolabeled with 99mTc exhibited increased tumor uptake ( approximately 25 %ID/g at 1.5 h), lower kidney uptake ( approximately 4.8 %ID/g at 1.5 h), and extensive urinary excretion (59 %ID at 1.5 h). Finally, comparison biodistribution studies between 99mTc and 188Re (39) showed a good correlation between the two metal complexes and demonstrated prolonged tumor retention (> or =24 h).
Assuntos
Quelantes/síntese química , Compostos Organometálicos/síntese química , Peptídeos/síntese química , Radioisótopos , Compostos Radiofarmacêuticos/síntese química , Receptores de Somatostatina/metabolismo , Rênio , Animais , Linhagem Celular Tumoral , Quelantes/química , Feminino , Humanos , Marcação por Isótopo , Camundongos , Camundongos Nus , Transplante de Neoplasias , Compostos Organometálicos/química , Compostos Organometálicos/farmacocinética , Peptídeos/química , Ensaio Radioligante , Compostos Radiofarmacêuticos/química , Compostos Radiofarmacêuticos/farmacocinética , Ratos , Relação Estrutura-Atividade , Tecnécio , Distribuição Tecidual , Transplante HeterólogoRESUMO
The early and later eluting [(99m)TcO]depreotide products on RP-HPLC were confirmed to be the anti and syn diastereomers, respectively, based on proton NMR and circular dichroism spectroscopy. NMR provided evidence of a folded, conformationally constrained structure for the syn diastereomer. The syn diastereomer is predominant (anti/syn approximately 10:90) in the [(99m)TcO]depreotide preparation and shows a slightly higher affinity (IC50 = 0.15 nM) for the somatostatin receptor than the anti diastereomer (IC50 = 0.89 nM). Both diastereomers showed higher binding affinities than the free peptide (IC(50) = 7.4 nM). Biodistribution studies in AR42J tumor xenograft nude mice also showed higher tumor uptake for syn [(99m)TcO]depreotide (6.58% ID/g) than for the anti [(99m)TcO]depreotide (3.38% ID/g). Despite the differences in biological efficacy, the favorable binding affinity, tumor uptake, and tumor-to-background ratio results for both diastereomeric species predict that both are effective for imaging somatostatin receptor-positive tumors in vivo.
Assuntos
Neoplasias/diagnóstico por imagem , Compostos de Organotecnécio/isolamento & purificação , Compostos Radiofarmacêuticos/isolamento & purificação , Receptores de Somatostatina/metabolismo , Somatostatina/análogos & derivados , Animais , Linhagem Celular Tumoral , Dicroísmo Circular , Feminino , Marcação por Isótopo , Espectroscopia de Ressonância Magnética , Camundongos , Camundongos Nus , Transplante de Neoplasias , Neoplasias/metabolismo , Compostos de Organotecnécio/química , Compostos de Organotecnécio/farmacocinética , Neoplasias Pancreáticas , Ensaio Radioligante , Cintilografia , Compostos Radiofarmacêuticos/química , Compostos Radiofarmacêuticos/farmacocinética , Ratos , Somatostatina/química , Somatostatina/isolamento & purificação , Somatostatina/farmacocinética , Estereoisomerismo , Distribuição TecidualRESUMO
We study the nanoscale terraced topographies that arise when a solid surface is bombarded with a broad ion beam that has a relatively high angle of incidence θ. We find that the surface is not completely flat between the regions in which the surface slope changes rapidly with position: Instead, small-amplitude ripples propagate along the surface. Our analytical work on these ripples yields their propagation velocity as well as the scaling behavior of their amplitude. Our simulations establish that the surfaces exhibit interrupted coarsening, i.e., the characteristic width and height of the surface disturbance grow for a time but ultimately asymptote to finite values as the fully terraced state develops. In addition, as θ is reduced, the surface can undergo a transition from a terraced morphology that changes little with time as it propagates over the surface to an unterraced state that appears to exhibit spatiotemporal chaos. For different ranges of the parameters, our equation of motion produces unterraced topographies that are remarkably similar to those seen in various experiments, including pyramidal structures that are elongated along the projected beam direction and isolated lenticular depressions.
RESUMO
When a solid surface is bombarded with a broad ion beam at a relatively large angle of incidence, the surface often develops a terraced form. We introduce a model that includes an improved approximation to the sputter yield and that produces a terraced surface morphology at long times for a wide range of parameter values. Numerical integrations of our equation of motion reveal that the terraces coarsen as time passes, just as observed experimentally. We also show that the terrace propagation direction can reverse as the amplitude of the surface disturbance grows. This highlights the important role higher order nonlinearities play in determining the propagation velocity at high fluences.
RESUMO
When the surface of a nominally flat binary material is bombarded with a broad, normally incident ion beam, disordered hexagonal arrays of nanodots can form. Shipman and Bradley have derived equations of motion that govern the coupled dynamics of the height and composition of such a surface [Shipman and Bradley, Phys. Rev. B 84, 085420 (2011)]. We investigate the influence of initial conditions on the hexagonal order yielded by integration of those equations of motion. The initial conditions studied are hexagonal and sinusoidal templates, straight scratches, and nominally flat surfaces. Our simulations indicate that both kinds of templates lead to marked improvements in the hexagonal order if the initial wavelength is approximately equal to or double the linearly selected wavelength. Scratches enhance the hexagonal order in their vicinity if their width is close to or less than the linearly selected wavelength. Our results suggest that prepatterning a binary material can dramatically increase the hexagonal order achieved at large ion fluences.