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In-Situ Observation of Coulomb Fission of Individual Plasmonic Nanoparticles
摘要: Reshaping plasmonic nanoparticles with laser pulses has been extensively researched as a tool for tuning their properties. However, in the absence of direct observations of the processes involved, important mechanistic details have remained elusive. Here, we present an in-situ electron microscopy study of one such process that involves Coulomb fission of plasmonic nanoparticles under femtosecond laser irradiation. We observe that gold nanoparticles encapsulated in a silica shell fission by emitting progeny droplets comprised of about 10-500 atoms, with ejection preferentially occurring along the laser polarization direction. Under continued irradiation, the emitted droplets coalesce into a second core within the silica shell, and the system evolves into a dual-core particle. Our findings are consistent with a mechanism in which electrons are preferentially emitted from the gold core along the laser polarization direction. The resulting anisotropic charge distribution in the silica shell then determines the direction in which progeny droplets are ejected. In addition to yielding insights into the mechanism of Coulomb fission in plasmonic nanoparticles, our experiments point towards a facile method for forming surfaces decorated with aligned dual-gold-core silica shell particles.
关键词: single-particle observation,gold-core silica shell particles,plasmonic nanoparticles,in-situ,nanoparticle reshaping,Coulomb fission,transmission electron microscopy
更新于2025-09-11 14:15:04
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Determination of Sulfite in Botanical Medicine Using Headspace Thin-Film Microextraction and Surface Enhanced Raman Spectrometry
摘要: A facile method using headspace thin-film microextraction (HS-TFME) coupled with surface enhanced Raman spectrometry (SERS) has been developed for the determination of sulfite in traditional Chinese herbal medicine. The extraction substrate was synthesized by depositing urchin-like ZnO micron particles on glass sheets using chemical liquid phase deposition. Under the optimal conditions, the intensity of the SERS signal at 630–640 cm?1 provided a good linear relationship with the concentration of sulfite from 25 to 400 mg/kg, and the linear correlation coefficient (R) was 0.996 with a detection limit of 6 mg/kg. The method was employed for the determination of sulfite in herbal medicines, and the results were confirmed by a traditional distillation-titration method. Therefore, this developed HS-TFME-SERS method may play an important role in the rapid, simple, and selective determination of sulfite residues in Chinese herbal medicine and become a potentially universal method for this analyte in various solid samples.
关键词: Headspace thin-film microextraction (HS-TFME),scanning electron microscopy (SEM),X-ray diffraction (XRD),surface enhanced Raman spectrometry (SERS),transmission electron microscopy (TEM)
更新于2025-09-10 09:29:36
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Atomic Structure and Electrical Activity of Grain Boundaries and Ruddlesden-Popper Faults in Cesium Lead Bromide Perovskite
摘要: To evaluate the role of planar defects in lead-halide perovskites—cheap, versatile semiconducting materials—it is critical to examine their structure, including defects, at the atomic scale and develop a detailed understanding of their impact on electronic properties. In this study, postsynthesis nanocrystal fusion, aberration-corrected scanning transmission electron microscopy, and first-principles calculations are combined to study the nature of different planar defects formed in CsPbBr3 nanocrystals. Two types of prevalent planar defects from atomic resolution imaging are observed: previously unreported Br-rich [001](210)∑5 grain boundaries (GBs) and Ruddlesden–Popper (RP) planar faults. The first-principles calculations reveal that neither of these planar faults induce deep defect levels, but their Br-deficient counterparts do. It is found that the ∑5 GB repels electrons and attracts holes, similar to an n–p–n junction, and the RP planar defects repel both electrons and holes, similar to a semiconductor–insulator–semiconductor junction. Finally, the potential applications of these findings and their implications to understand the planar defects in organic–inorganic lead-halide perovskites that have led to solar cells with extremely high photoconversion efficiencies are discussed.
关键词: Ruddlesden–Popper faults,lead-halide perovskites,scanning transmission electron microscopy,density-functional theory,grain boundaries
更新于2025-09-10 09:29:36
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Inner Segment Remodeling and Mitochondrial Translocation in Cone Photoreceptors in Age-Related Macular Degeneration With Outer Retinal Tubulation
摘要: PURPOSE. To quantify impressions of mitochondrial translocation in degenerating cones and to determine the nature of accumulated material in the subretinal space with apparent inner segment (IS)-like features by examining cone IS ultrastructure. METHODS. Human donor eyes with advanced age-related macular degeneration (AMD) were screened for outer retinal tubulation (ORT) in macula-wide, high-resolution digital sections. Degenerating cones inside ORT (ORT cones) and outside ORT (non-ORT cones) from AMD eyes and unaffected cones in age-matched control eyes were imaged using transmission electron microscopy. The distances of mitochondria to the external limiting membrane (ELM), cone IS length, and cone IS width at the ELM were measured. RESULTS. Outer retinal tubulation and non-ORT cones lose outer segments (OS), followed by shortening of IS and mitochondria. In non-ORT cones, IS broaden. Outer retinal tubulation and non-ORT cone IS myoids become undetectable due to mitochondria redistribution toward the nucleus. Some ORT cones were found lacking IS and containing mitochondria in the outer fiber (between soma and ELM). Unlike long, thin IS mitochondria in control cones, ORT and non-ORT IS mitochondria are ovoid or reniform. Shed IS, some containing mitochondria, were found in the subretinal space. CONCLUSIONS. In AMD, macula cones exhibit loss of detectable myoid due to IS shortening in addition to OS loss, as described. Mitochondria shrink and translocate toward the nucleus. As reflectivity sources, translocating mitochondria may be detectable using in vivo imaging to monitor photoreceptor degeneration in retinal disorders. These results improve the knowledge basis for interpreting high-resolution clinical retinal imaging.
关键词: ellipsoid,outer retinal tubulation,age-related macular degeneration,histology,photoreceptors,cones,myoid,transmission electron microscopy,Müller cells
更新于2025-09-10 09:29:36
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Real-time observation of the temperature-induced phase transformation in GeTe and its thermal expansion properties
摘要: The GeTe-based system has long been considered as a promising candidate system for various functional applications; many of which are directly related to the polymorphic phase transformation in their crystalline forms. Consequently, the microstructure underlying their intriguing phase transition has been the subject of numerous studies. Here we provide real-time observation of the microstructural changes associated with the reversible pseudo-cubic (or rhombohedral) to cubic GeTe phase transition using high-voltage transmission electron microscopy (HV-TEM) operating at 1,250kV and complementary high-temperature X-ray diffraction (XRD). As a result of the phase transition, the pseudo-cubic GeTe domain’s configuration significantly changes from its original band-like to a spike-like morphology with a different orientation after a heating/cooling cycle. The coefficients of thermal expansion (CTE) properties as a function of temperature are also explored in relation to the GeTe phase transition.
关键词: CTE ellipsoids,in-situ high voltage transmission electron microscopy,GeTe,thermal expansion tensor,ferroelectric domains
更新于2025-09-10 09:29:36
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Monolithic axial and radial metal-semiconductor nanowire heterostructures
摘要: The electrical and optical properties of low dimensional nanostructures depend critically on size and geometry and may differ distinctly from those of their bulk counterparts. In particular, ultra-thin semiconducting layers as well as nanowires have already proven the feasibility to realize and study quantum size effects enabling novel ultra-scaled devices. Further, plasmonic metal nanostructures attracted recently a lot of attention because of appealing near-field mediated enhancement effects. Thus, combining metal and semiconducting constituents in quasi 1D heterostructures will pave the way for ultra-scaled systems and high-performance devices with exceptional electrical, optical and plasmonic functionality. This paper reports on the sophisticated fabrication and structural properties of axial and radial, Al-Ge and Al-Si nanowire heterostructures, synthesized by a thermally induced exchange reaction of single-crystalline Ge-Si core-shell nanowires and Al pads. This enables a self-aligned metallic contact formation to Ge segments beyond lithographic limitations as well as ultra-thin semiconducting layers wrapped around monocrystalline Al core nanowires. High-resolution transmission electron microscopy, energy dispersive X-ray spectroscopy and μ-Raman measurements proved the composition and perfect crystallinity of these metal-semiconductor nanowire heterostructures. This exemplary selective replacement of Ge by Al represents a general approach for the elaboration of radial and axial metal-semiconductor heterostructures in various Ge-semiconductor heterostructures.
关键词: metal-semiconductor heterostructure,germanium,aluminum,transmission electron microscopy,nanowire
更新于2025-09-10 09:29:36
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Heat-Treatment Induced Magnetic Anisotropy of GaMnSb Films
摘要: Conditions and mechanisms of controlled variation of the magnetic anisotropy of GaMnSb films containing magnetic MnSb nanoinclusions by means of heat treatment have been determined. For this purpose, the temperature and magnetic-field dependences of the magnetic moments of samples before and after thermal annealing were measured using a SQUID magnetometer. It is established that the heat treatment of GaMnSb films leads to a significant increase in the values of characteristics determined by the magnetic anisotropy, including the growth of blocking temperature (from 95 to 390 K) and the magnetic anisotropy field (from 330 to 630 Oe). Results of transmission electron microscopy investigation indicate that a change in the magnetic anisotropy of GaMnSb films as a result of their thermal annealing can be related to a transition of the crystalline structure of magnetic MnSb nanoinclusions from hexagonal (space group P62/mmc) to cubic (space group F-43m).
关键词: magnetic anisotropy,GaMnSb films,SQUID magnetometer,transmission electron microscopy,MnSb nanoinclusions,heat treatment
更新于2025-09-10 09:29:36
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Characterization of grain boundary disconnections in SrTiO3 part I: the dislocation component of grain boundary disconnections
摘要: High-resolution transmission electron microscopy is often used to characterize grain boundaries, but it is usually limited to special high symmetry boundaries with a high density of coincident sites. For these ‘special’ boundaries, both crystals can be brought into a low-index zone-axis with the boundary plane parallel to the incident electron beam. In this case the atomistic structure of the boundary can be solved, which is not possible for other, more general grain boundaries. In the present study, general grain boundaries in SrTiO3 were analyzed using aberration-corrected transmission electron microscopy and scanning transmission electron microscopy. These boundaries included at least one type of disconnection (i.e., defects that can have a step and/or a dislocation component). Since the dislocation component of disconnections along general grain boundaries cannot be fully resolved using the methods currently available, a plane matching approach was used to compare disconnections at different boundaries. Using this approach, the dislocation component of the disconnections was partially characterized and was found to have an edge component mainly parallel to {100} and {110}, close to normal to the macroscopic grain boundary plane. The step component of the disconnections was found to be aligned mainly parallel to the same crystallographic planes ({100} and {110}).
关键词: scanning transmission electron microscopy,grain boundaries,transmission electron microscopy,SrTiO3,disconnections
更新于2025-09-09 09:28:46
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Dynamics of gold nanoparticle clusters observed with liquid-phase electron microscopy
摘要: The dynamics of processes of nanoparticles such as diffusion, attraction and repulsion, and self-assembly of structures of nanoparticles at the solid-liquid interfaces differ significantly from those occurring for bulk conditions and their fundamental physical rules are still unknown. Here, we used liquid phase scanning transmission electron microscopy (LP-STEM) to study several aspects of nanoparticle dynamics of colloidal chitosan coated gold nanoparticle (TCHIT-AuNP) clusters in a liquid layer enclosed between two SiN membranes. We found that upon beam irradiation using an electron flux of 0.9 e?/s?2, the AuNPs assembled in clusters that shifted and rotated with time. The newly formed clusters could join and form larger clusters via a mechanism of oriented attachment. By increasing the electron flux to 6.2 e?/s?2, we observed the fragmentation of some of the clusters and TCHIT-AuNPs were exchanged between clusters. At the highest electron flux studied 25 e?/s?2, we observed AuNPs moving at a very slow speed compared to Brownian motion in liquid even though they were not permanently attached or pinned to the liquid-enclosing membrane. Experiments using branched polyethylenimine (BPEI) coated AuNPs were carried out for comparison.
关键词: nanoparticle clustering,nanoparticle dynamics,solid-liquid interface,gold nanoparticles,scanning transmission electron microscopy,liquid-phase electron microscopy
更新于2025-09-09 09:28:46
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-II
摘要: The basic and the charge density wave (CDW) structures of the monoclinic NbS3-II polymorph were studied by synchrotron x-ray diffraction, ab initio calculations, simulation of electron diffraction patterns, and by atomic-resolution transmission electron and low-temperature scanning tunneling microscopies. It is con?rmed that the basic structure belongs to the space group P 21/m and is described with a unit cell, formed of four pairs of symmetry-related trigonal prismatic (TP) columns [a0 = 0.96509(8) nm, b0 = 0.33459(2) nm, c0 = 1.9850(1) nm, and β0 = 110.695(4)?]. The incommensurate components of the two CDWs, (cid:3)q1 = (0, 0.298, 0) and (cid:3)q2 = (0, 0.352, 0), are related as q1b + 2q2b ≈ 1. Both CDWs form their own modulation patterns with unit cells (am = 2a0, bm = b0/qjb, cm = c0, βm = β0) and are ordered along adjacent isosceles TP columns either pairwise or with both columns modulated by either the (cid:3)q1 or (cid:3)q2 CDW only. The CDWs are ordered according to one of the two possible modulation pattern space groups, Cm or C2/m. If considered as long-period commensurate, the entire modulated structure with both CDWs included is described within experimental error with an enlarged unit cell (a = 2a0, b = 37b0, c = c0, and β = β0) and with all atoms displaced from their average positions in accord with the speci?ed modulation pattern.
关键词: synchrotron x-ray diffraction,ab initio calculations,charge density wave,scanning tunneling microscopy,transmission electron microscopy,NbS3-II
更新于2025-09-09 09:28:46