Electronic energy loss and ion velocity correlation effects in track production in swift-ion-irradiated LiNbO_(3):A quantitative assessment between structural damage morphology and energy deposition

The primary motivation for studying how irradiation modifies the structures and properties of solid materials involves the understanding of undesirable phenomena,including irradiation-induced degradation of components in nuclear reactors and space exploration,and beneficial applications,including material performance tailoring through ion beam modification and defect engineering.In this work,the formation mechanism of latent tracks with different damage morphologies in LiNbO_(3)crystals under 0.09-6.17 Me V/u ion irradiation with an electronic energy loss from 2.6-13.2 ke V/nm is analyzed by experimental characterizations and numerical calculations.Irradiation-induced damage is preliminarily evaluated via the prism coupling technique to analyze the correlation between the dark-mode spectra and energy loss profiles of irradiated regions.Under the irradiation conditions of different ion velocities and electronic energy losses,different damage morphologies,from individual spherical defects to discontinuous and continuous tracks,are experimentally characterized.During ion penetration process,the ion velocity determines the spatiotemporal distribution of deposited irradiation energy induced by electronic energy loss,meaning that the two essential factors including electronic energy loss and ion velocity coaffect the track damage.The inelastic thermal spike model is used to numerically calculate the spatiotemporal evolutions of energy deposition and the corresponding atomic temperature under different irradiation conditions,and a quantitative relationship is proposed by comparison with corresponding experimentally observed track damage morphologies.The obtained quantitative relationship between irradiation conditions and track damage provides deep insight and guidance for understanding the damage behavior of crystal materials in extreme radiation environments and selecting irradiation parameters,including ion species and energies,for ion beam technique application in atomic-level defect manipulation,material modification,and micro/nanofabrication.

ENERGY-LOSS FUNCTIONS DERIVED FROM REELS SPECTRA FOR ALUMINUM

The effective energy loss functions for Al have been derived from differential i nverse inelastic mean free path based on the extended Landau approach. It has be en revealed that the effective energy loss function is very close in value to th e theoretical surface energy loss function in the lower energy loss region but g radually approaches the theoretical bulk energy loss function in the higher ener gy loss region. Moreover, the intensity corresponding to surface excitation in e ffective energy loss functions decreases with the increase of primary electron e nergy. These facts show that the present effective energy loss function describe s not only surface excitation but also bulk excitation. At last, REELS spectra s imulated by Monte Carlo method based on use of the effective energy loss functio ns has reproduced the experimental REELS spectra with considerable success.

Non-ionizing energy loss calculations for modeling electron-induced degradation of Cu(In,Ga)Se_2 thin-film solar cells

The lowest energies which make Cu,In,Ga,and Se atoms composing Cu（In,Ga）Se_2（CIGS） material displaced from their lattice sites are evaluated,respectively.The non-ionizing energy loss（NIEL） for electron in CIGS material is calculated analytically using the Mott differential cross section.The relation of the introduction rate（k） of the recombination centers to NIEL is modified,then the values of k at different electron energies are calculated.Degradation modeling of CIGS thin-film solar cells irradiated with various-energy electrons is performed according to the characterization of solar cells and the recombination centers.The validity of the modeling approach is verified by comparison with the experimental data.

A double toroidal analyzer for scanning probe electron energy spectrometer

An ultra-high vacuum （UHV） compatible electron spectrometer employing a double toroidal analyzer has been de- veloped. It is designed to be combined with a custom-made scanning tunneling microscope （STM） to study the spatially localized electron energy spectrum on a surface. A tip-sample system composed of a piezo-driven field-emission tungsten tip and a sample of highly ordered pyrolytic graphite （HOPG） is employed to test the performance of the spectrometer. Two-dimensional images of the energy-resolved and angle-dispersed electrons backscattered from the surface of HOPG are obtained, the performance is optimized and the spectrometer is calibrated. A complete electron energy loss spectrum covering the elastic peak to the secondary electron peaks for the HOPG surface, acquired at a tip voltage of -140 V and a sample current of 0.5 pA, is presented, demonstrating the viability of the spectrometer.

Three-dimensional size and orientation of the precipitates in AZ91 magnesium alloys measured by TEM techniques

Knowledge of the microscopic structure, including three-dimensional （3-D） size and orientation of the precipitates, is essential to fully understand the mechanical properties of the magnesium alloys and designing the alloys with better performance. Analytical TEM with high spatial resolution offers the simultaneous measurements of 3-D size, structure, orientation, composition of the precipitates from one typical sample along an established crystallographic axis. Besides popular Burgers orientation relationship （OR）, other ORs such as Pitsch-Schrader OR, Crawley OR, Potter OR and a new OR with the form of [0001]α 1.0° from [311]γ and （1120）α 2.0° from （033）γ between the magnesium matrix and the precipitate γ-MglTAl 12 are identified by TEM imaging and diffraction techniques. As a case study, the thicknesses of the individual precipitates with Burgers OR are further measured to be 100 200 nm through both electron energy-loss spectroscopy and x-ray energy dispersive spectroscopy combining differential x-ray absorption and extrapolation, which are in agreement with the overall 3-D size statistic distribution results obtained through analysing various samples along various directions. Furthermore, the fabricated wedge-shape structure provides a platform on which to study the dependence of the interfacial strain on the variation of the thickness.

The Micro-structural Studies of Ni-BaTiO_3 Nanocomposite Films by TEM and EELS

Epitaxial BaTiO3 films with embedded metallic Ni nanocrystal （Ni-BaTiO3） were successfully fabricated on SrTiO3 （001） single-crystalline substrate through the laser molecular beam epitaxial （L-MBE） technique.High resolution transmission electron microscopy （HRTEM） and electron energy loss spectrum （EELS） with Kramers-Kronig analysis methods were employed to characterize the microstructures,elementary distribution and the electron structure of these films.HRTEM results suggested that the structure of BaTiO3 was tetragonal with lattice parameters of a=0.399 nm and c=0.403 nm.Energy dispersive X-Ray spectroscopy （EDX） confirmed metallic Ni nanocrystal embedded successfully in BaTiO3 epitaxial films.The Ni-BaTiO3 composite films were compound of the epitaxial BaTiO3 （110） layers alternating with Ni NCs array （111） layers.Furthermore,the existence of the misfit dislocations induced by the embedding of Ni nanoparticles was also clearly demonstrated by the HRTEM images.The Ni L2,3 edges of EELS revealed that Ni NCs in their metallic state were embedded uniformly in the BaTiO3 matrix.A chemical shift of about 7 eV regarding L3 edges in the Ni EELS was also observed.The optical band gap of BaTiO3 in these films was about 3.84 eV,higher than 3.55 eV for pure BaTiO3 films at room temperature.

Collective excitations and quantum size effects on the surfaces of Pb(111)films:An experimental study

Pb(111)film is a special system that exhibits strong quantum size effects in many electronic properties.The collective excitations,i.e.,plasmons,in Pb(111)films are also expected to show signatures of the quantum size effect.Here,using high-resolution electron energy loss spectroscopy,we measured the plasmons on the surface of Pb(111)films with different film thicknesses and analyzed the plasmon dispersions.One surface plasmon branch exhibits prominent damping in the small momentum range,which can be attributed to the interaction between the top and bottom interfaces of the Pb(111)films.With the film thickness increasing,the critical momentum characterizing the damping in Pb(111)films decays not only much slower in Pb(111)films than in other metal films,and even in films with the thickness up to 40 monolayers the damping still exists.The slow decay of the surface plasmon damping,manifesting the strong quantum size effect in Pb(111)films,might be related to the strong nesting of the Fermi surface along the(111)direction.

Design of a novel correlative reflection electron microscope for in-situ real-time chemical analysis

A novel instrument that integrates reflection high energy electron diffraction(RHEED),electron energy loss spectroscopy(EELS),and imaging is designed and simulated.Since it can correlate the structural,elemental,and spatial information of the same surface region via the simultaneously acquired patterns of RHEED,EELS,and energy-filtered electron microscopy,it is named correlative reflection electron microscopy(c-REM).Our simulation demonstrates that the spatial resolution of this c-REM is lower than 50 nm,which meets the requirements for in-situ monitoring the structural and chemical evolution of surface in advanced material.

Spatially Resolved Analytical Electron Microscopy at Grain Boundaries of α-Al_2O_3

In this work the electronic structure and the impurity excess of the basal and rhombohedral twin grain boundaries are investigated, using electron energy loss spectroscopy (EELS) and energy dispersive X-ray spectroscopy (EDXS). The measurability of electronic structures of the twin grain boundaries are discussed by comparing theoretical density of states (DOS) from bulk material with interfacial DOS, obtained from local density functional theory (LDFT) calculations.

Fast-electron-impact study on excitations of 4d electron of xenon

The electron energy loss spectrum of the 4d excitations of xenon was measured at an incident electron energy of1500 eV and a scattering angle of 6°. Besides the optically allowed transitions of 4d5/2^-1np and 4d3/2^-1np, the optically forbidden transitions of 4d5/2^-1ns, 4d5/2^-1nd, 4d3/2^-1ns, and 4d3/2^-1nd were observed. The measured features are assigned with the help of the calculation by the Cowan Code. The line profile parameters of both optically allowed transitions and optically forbidden ones were determined and compared with the previous available data. It is found that the natural widths of both dipole-allowed and dipole-forbidden excitations are approximately identical, which means the spectator transitions dominate the resonant Auger effect for both dipole-allowed and dipole-forbidden transitions.

Structural damage response of lanthanum and yttrium aluminate crystals to nuclear collisions and electronic excitation:Threshold assessment of irradiation damage

A comparative analysis is performed on the structural damage response and associated mechanisms in lanthanum aluminate and yttrium aluminate crystals under various irradiation conditions by a combination of experimental and theoretical approaches.Under low-energy Au~+irradiation,the damage accumulation curve shows a higher damage rate for LaAlO_(3)crystals than YAlO_(3)crystals.The relatively low irradiation tolerance of LaAlO_(3)to the action of nuclear collisions is ascribed to the large amorphization cross-section and effective cross-section for defect-stimulated amorphization.Under swift Ar^(12+),Ni^(19+)and Kr^(17+)irradiation with different ion energies and velocities,the formed highly-disordered/amorphous latent tracks with different morphologies in pristine and predamaged crystals are discussed,and the corresponding electronic energy loss and lattice temperature thresholds are quantitatively determined.Compared to YAlO_(3),LaAlO_(3)exhibits lower sensitivity and higher damage tolerance to the electronic energy loss process,attributing to its relatively high recrystallization efficiency during the rapid quenching process.Furthermore,the introduction of lattice defects into LaAlO_(3)and YAlO_(3)crystals considerably enhances the sensitivity and intensity of thermal spike response to the electronic energy loss,and the induced effective modification of track morphologies demonstrates the synergistic effect between the electronic energy loss and pre-existing defects created by nuclear collisions.In this case,even under the action of electronic energy loss below the threshold,the lattice temperature in the nuclear-collision damaged crystalline system could still meet the criterion for track production.The irradiation energy deposited to atoms and induced lattice temperature evolution discussed in this work provide a deeper insight into the complex processes involved in irradiation-induced latent track behaviors.

Electron microscopy methods for space-, energy-, and time-resolved plasmonics

Nanoscale plasmonic systems combine the advantages of optical frequencies with those of small spatial scales, circumventing the limitations of conventional photonic systems by exploiting the strong field confinement of surface plasmons. As a result of this miniaturization to the nanoscale, electron microscopy techniques are the natural investigative methods of choice. Recent years have seen the development of a number of electron microscopy techniques that combine the use of electrons and photons to enable unprecedented views of surface plasmons in terms of combined spatial, energy, and time resolution. This review aims to provide a comparative survey of these different approaches from an experimental viewpoint by outlining their respective experimental domains of suitability and highlighting their complementary strengths and limitations as applied to plasmonics in particular.

Average kinetic energy of ions ejected from pure Coulomb explosions of methane clusters

We use an electrostatic model to study the average kinetic energy of ions ejected from the pure Coulomb explosions of methane clusters （CA4）n （light atom A=H and D）. It is found that the ratio of the average kinetic energy of the ions to their initial average electrostatic potential energy is irrelevant to the cluster size. This finding implies that as long as the ratio is given, the average kinetic energies of the ions can be simply estimated from their initial average electrostatic potential energies, rather than from the timeconsuming simulations. The ratios for the different charge states of carbon ions are presented.

Charged particles:Unique tools to study irradiation resistance of concentrated solid solution alloys

Many multicomponent concentrated solid solution alloys(CSAs),including high-entropy alloys(HEAs),exhibit improved radiation resistance and enhanced structural stability in harsh environments.To study and assess irradiation resistance of nuclear materials,energetic ion and electron beams are commonly used to create displacement damage.Moreover,charged particles of ions,electrons,and positrons are unique tools to create and characterize radiation effects.Ion beam analysis(e.g.,Rutherford backscattering spectrometry,nuclear reaction analysis,and time-of-flight elastic recoil detection analysis),electron microscopy techniques(e.g.,transmission or scanning electron microscopy,and electron diffraction),and positron annihilation spectroscopy have been applied to characterize irradiated CSAs or HEAs to understand defect formation and evolution together with chemical and microstructural information.Their distinctive analyzing power and some perspectives in these techniques are reviewed.In developing structural alloys desirable for applications in advanced reactors,neutron exposure is a critical test but the limitation in achievable high damage levels is,however,a bottleneck.Ion irradiation is often used as a surrogate for neutron irradiation,and the associated reduced transmutations and higher displacements per atom(dpa)rates are desirable for materials research.Nevertheless,cautions need to be taken when relying on ion irradiation results for reactor evaluations.Literature on differences between ions and neutrons is briefly reviewed.In addition,the links to bridge the current advances on fundamental understandings to reactor applications are discussed to lay the groundwork between neutrons and ions for radiation effects studies.

Characterization of Compositionally Complex Hydrides in a Metastable Refractory High-Entropy Alloy

Here,we study the hydride formation in a metastable Ti-33Zr-22Hf-11Ta(at.%)refractory high entropy alloy(RHEA).Deviating to non-equiatomic compositions of RHEAs promotes the formation of transformation-induced plasticity where the body-centered cubic phase transforms to hexagonal close-packed(HCP)phase.It is found that the phase transformation capability assists the hydride formation due to the low solubility of hydrogen within the HCP phase.In this study,hydrogen is charged via electrochemical polishing and the corresponding phase transformation is activated in the metastable RHEAs.The newly formed HCP phase interacts with hydrogen to form a face-centered cubic hydride verified by electron energy loss spectroscopy.This work provides a primary exploration of the formation of compositionally complex metal hydrides in the metastable RHEAs,which are potential candidates for future hydrogen storage material design.

Deviating from the nanorod shape： Shape-dependent plasmonic properties of silver nanorice and nanocarrot structures

Noble metallic nanostructures exhibit special optical properties resulting from excitation of surface plasmons. Among the various metallic nanostructures, nanorods have attracted particular attention because of their unique and intriguing shape-dependent plasmonic properties. Nanorods can sup- port transverse and longitudinal plasmon modes, the latter ones depending strongly on the aspect ratio of the nanorod. These modes can be routinely tuned from the visible to the near-infrared spectral regions. Although nanorods have been investigated extensively, there are few studies de- voted to nanostructures deviating from the nanorod shape. This review provides an overview of recent progress in the development of two kinds of novel quasi-one-dimensional silver nanostruc- tures, nanorice and nanocarrot, including their syntheses, crystalline characterizations, plasmonic property analyses, and performance in plasmonic sensing applications.

Surfactant-free synthesis of metallic bismuth spheres by microwave-assisted solvothermal approach as a function of the power level

In the present work, the synthesis of micro- and nano-sized spheres of metallic bismuth by microwave-assisted solvothermal method is reported. The synthesis method was carried out at different power levels and at a unique frequency of microwave irradiation. The sphere sizes were controlled by the microwave power level and the concentration of dissolved precursor. Structural and morphological characterization was performed by SEM, HRTEM, EELS and XRD. The results demonstrated that rhombohedral zero valent Bi spheres were synthesized after microwave radiation at 600 and 1200 W. However, if the power level is decreased to 120 W, a monoclinic phase of Bi203 is obtained with a flake-like morphology. In comparison with a conventional hydrothermal process, the microwave-assisted solvothermal approach provides many advantages such as shorter reaction time, optimum manipulation of morphologies and provides a specific chemical phase and avoids the mixture of structural phases and morphologies which is essential for further applications such as drug delivery or functionalization with organic materials, thanks to its biocompatibility.

Synthesis of yttrium iron garnet/bismuth quantum dot heterostructures with localized plasmon enhanced magneto-optical performance

Interactions between light and magnetic matter attracted great attention lately due to their potential applications in nanophotonics,spintronics,and high-accuracy sensing.Here,we grew bismuth quantum dots(Bi–QDs)with strong spin–orbit coupling on a magnetic insulator yttrium iron garnet(YIG)via molecular beam epitaxy.The YIG/Bi–QDs material shows an enhanced magneto-optical Kerr rotation up to 130%compared with that of a bare YIG film.The Bi–QDs were also introduced onto a lutetium–bismuth co-doped YIG film to form a hybrid system with remarkably enhanced Kerr rotation(from 1626 to 2341 mdeg).Ferromagnetic resonance measurements showed an increased effective magnetization as well as interfacial spin–orbit field in the YIG/Bi–QD heterostructures.Localized plasmons were mapped using electron energy loss spectroscopy with high spatial resolution,revealing enhanced plasmon intensity at both the Bi–QD surface and YIG/Bi–QD interface.Introducing Bi-QDs onto the YIG film enhanced Kerr rotation owing to the attenuated optical reflection and increased effective magnetization.The Bi–QDenhanced magneto-optical effect enables development of efficient nanoscale light switching,spintronics,and even plasmonic nano-antennas.

Advanced TEM Characterization for Single-atom Catalysts:from Ex-situ Towards In-situ

Clean energy innovation has triggered the development of single-atom catalysts(SACs)due to their excellent catalytic activity,high tunability and low cost.The success of SACs for many catalytic reactions has opened a new field,where the fundamentals of catalytic property-structure relationship at atomic level await exploration,and thus raises challenges for structural characterization.Among the characterization techniques for SACs,aberration-corrected transmission electron microscopy(TEM)has become an essential tool for direct visualization of single atoms.In this review,we briefly summarize recent studies on SACs using advanced TEM.We first introduce TEM methods,which are particularly important for SACs characterization,and then discuss the applications of advanced TEM for SAC characterization,where not only atomic dispersion of single atoms can be studied,but also the distribution of elements and the valence state with local coordination can be resolved.We further extend our review towards in-situ TEM,which has increasing importance for the fundamental understanding of catalytic mechanism.Perspectives of TEM for SACs are finally discussed.