Direct in situ observation of the electron-driven synthesis of Ag filaments on α-Ag2 WO4 crystals

In this letter, we report, for the first time, the real-time in situ nucleation and growth of Ag filaments on α-Ag2 WO4 crystals driven by an accelerated electron beam from an electronic microscope under high vacuum. We employed several techniques to characterise the material in depth. By using these techniques combined with first-principles modelling based on density functional theory, a mechanism for the Ag filament formation followed by a subsequent growth process from the nano-to micro-scale was proposed. In general, we have shown that an accelerated electron beam from an electronic microscope under high vacuum enables in situ visualisation of Ag filaments with subnanometer resolution and offers great potential for addressing many fundamental issues in materials science, chemistry, physics and other fields of science.

Structural and electronic analysis of the atomic scale nucleation of Ag on alpha-Ag2WO4 induced by electron irradiation

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Potentiated Electron Transference in alpha-Ag2WO4 Microcrystals with Ag Nanofilaments as Microbial Agent

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)

A combined experimental and theoretical study on the formation of ag filaments on beta-Ag2MoO4 induced by electron irradiation

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Optical transition radiation used in the diagnostic of low energy and low current electron beams in particle accelerators

Optical transition radiation (OTR) plays an important role in beam diagnostics for high energy particle accelerators. Its linear intensity with beam current is a great advantage as compared to fluorescent screens, which are subject to saturation. Moreover, the measurement of the angular distribution of the emitted radiation enables the determination of many beam parameters in a single observation point. However, few works deals with the application of OTR to monitor low energy beams. In this work we describe the design of an OTR based beam monitor used to measure the transverse beam charge distribution of the 1.9-MeV electron beam of the linac injector of the IFUSP microtron using a standard vision machine camera. The average beam current in pulsed operation mode is of the order of tens of nano-Amps. Low energy and low beam current make OTR observation difficult. To improve sensitivity, the beam incidence angle on the target was chosen to maximize the photon flux in the camera field-of-view. Measurements that assess OTR observation (linearity with beam current, polarization, and spectrum shape) are presented, as well as a typical 1.9-MeV electron beam charge distribution obtained from OTR. Some aspects of emittance measurement using this device are also discussed. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4748519]

Point defects in carbon nanostructures studied by in-situ electron microscopy

In the present work, the formation and migration of point defects induced by electron irradiation in carbon nanostructures, including carbon onions, nanotubes and graphene layers, were investigated by in-situ TEM. The mobility of carbon atoms normal to the layers in graphitic nanoparticles, the mobility of carbon interstitials inside SWCNTs, and the migration of foreign atoms in graphene layers or in layers of carbon nanotubes were studied. The diffusion of carbon atoms in carbon onions was investigated by annealing carbon onions and observing the relaxation of the compressed clusters in the temperature range of 1200 – 2000oC. An activation energy of 5.0±0.3 eV was obtained. This rather high activation energy for atom exchange between the layers not only prevents the exchange of carbon atoms between the layers at lower temperature but also explains the high morphological and mechanical stability of graphite nanostructures. The migration of carbon atoms in SWCNTs was investigated quantitatively by cutting SWCNT bundles repeatedly with a focused electron beam at different temperatures. A migration barrier of about 0.25 eV was obtained for the diffusion of carbon atoms inside SWCNTs. This is an experimental confirmation of the high mobility of interstitial atoms inside carbon nanotubes, which corroborates previously developed theoretical models of interstitial diffusivity. Individual Au and Pt atoms in one- or two-layered graphene planes and MWCNTs were monitored in real time at high temperatures by high-resolution TEM. The direct observation of the behavior of Au and Pt atoms in graphenic structures in a temperature range of 600 – 700°C allows us to determine the sites occupied by the metal atoms in the graphene layer and the diffusivities of the metal atoms. It was found that metal atoms were located in single or multiple carbon vacancies, not in off-plane positions, and diffused by site exchange with carbon atoms. Metal atoms showed a tendency to form clusters those were stable for a few seconds. An activation energy of around 2.5 eV was obtained for the in-plane migration of both Au and Pt atoms in graphene (two-dimensional diffusion). The rather high activation energy indicates covalent bonding between metal and carbon atoms. Metal atoms were also observed to diffuse along the open edge of graphene layers (one-dimensional diffusion) with a slightly lower activation energy of about 2.3 eV. It is also found that the diffusion of metal atoms in curved graphenic layers of MWCNTs is slightly faster than in planar graphene.

A scanning electron microscope for ultracold quantum gases

This thesis presents a new imaging technique for ultracold quantum gases. Since the first observation of Bose-Einstein condensation, ultracold atoms have proven to be an interesting system to study fundamental quantum effects in many-body systems. Most of the experiments use optical imaging rnmethods to extract the information from the system and are therefore restricted to the fundamental limitation of this technique: the best achievable spatial resolution that can be achieved is comparable to the wavelength of the employed light field. Since the average atomic distance and the length scale of characteristic spatial structures in Bose-Einstein condensates such as vortices and solitons is between 100 nm and 500 nm, an imaging technique with an adequate spatial resolution is needed. This is achieved in this work by extending the method of scanning electron microscopy to ultracold quantum gases. A focused electron beam is scanned over the atom cloud and locally produces ions which are subsequently detected. The new imaging technique allows for the precise measurement of the density distribution of a trapped Bose-Einstein condensate. Furthermore, the spatial resolution is determined by imaging the atomic distribution in one-dimensional and two-dimensional optical lattices. Finally, the variety of the imaging method is demonstrated by the selective removal of single lattice site. rn

The APSEL4D Monolithic Active Pixel Sensor and its Usage in a Single Electron Interference Experiment

We have realized a Data Acquisition chain for the use and characterization of APSEL4D, a 32 x 128 Monolithic Active Pixel Sensor, developed as a prototype for frontier experiments in high energy particle physics. In particular a transition board was realized for the conversion between the chip and the FPGA voltage levels and for the signal quality enhancing. A Xilinx Spartan-3 FPGA was used for real time data processing, for the chip control and the communication with a Personal Computer through a 2.0 USB port. For this purpose a firmware code, developed in VHDL language, was written. Finally a Graphical User Interface for the online system monitoring, hit display and chip control, based on windows and widgets, was realized developing a C++ code and using Qt and Qwt dedicated libraries. APSEL4D and the full acquisition chain were characterized for the first time with the electron beam of the transmission electron microscope and with 55Fe and 90Sr radioactive sources. In addition, a beam test was performed at the T9 station of the CERN PS, where hadrons of momentum of 12 GeV/c are available. The very high time resolution of APSEL4D (up to 2.5 Mfps, but used at 6 kfps) was fundamental in realizing a single electron Young experiment using nanometric double slits obtained by a FIB technique. On high statistical samples, it was possible to observe the interference and diffractions of single isolated electrons traveling inside a transmission electron microscope. For the first time, the information on the distribution of the arrival time of the single electrons has been extracted.

Structural characterization of intermediate and metastable phases by electron microscopy

Structure characterization of nanocrystalline intermediates and metastable phases is of primary importance for a deep understanding of synthetic processes undergoing solid-to-solid state phase transitions. Understanding the evolution from the first nucleation stage to the final synthetic product supports not only the optimization of existing processes, but might assist in tailoring new synthetic paths. A systematic investigation of intermediates and metastable phases is hampered because it is impossible to produce large crystals and only in few cases a pure synthetic product can be obtained. Structure investigation by X-ray powder diffraction methods is still challenging on nanoscale, especially when the sample is polyphasic. Electron diffraction has the advantage to collect data from single nanoscopic crystals, but is limited by data incompleteness, dynamical effects and fast deterioration of the sample under the electron beam. Automated diffraction tomography (ADT), a recently developed technique, making possible to collect more complete three-dimensional electron diffraction data and to reduce at the same time dynamical scattering and beam damage, thus allowing to investigate even beam sensitive materials (f.e. hydrated phases and organics). At present, ADT is the only technique able to deliver complete three-dimensional structural information from single nanoscopic grains, independently from other surrounding phases. Thus, ADT is an ideal technique for the study of on-going processes where different phases exist at the same time and undergo several structural transitions. In this study ADT was used as the main technique for structural characterization for three different systems and combined subsequently with other techniques, among which high-resolution transmission electron microscopy (HRTEM), cryo-TEM imaging, X-ray powder diffraction (XRPD) and energy disperse X-ray spectroscopy (EDX).rnAs possible laser host materials, i.e. materials with a broad band emission in the near-infrared region, two unknown phases were investigated in the ternary oxide system M2O-Al2O3-WO3 (M = K, Na). Both phases exhibit low purity as well as non-homogeneous size distribution and particle morphology. The structures solved by ADT are also affected by pseudo-symmetry. rnSodium titanate nanotubes and nanowires are both intermediate products in the synthesis of TiO2 nanorods which are used as additives to colloidal TiO2 film for improving efficiency of dye-sensitized solar cells (DSSC). The structural transition from nantubes to nanowires was investigated in a step by step time-resolved study. Nanowires were discovered to consist of a hitherto unknown phase of sodium titanate. This new phase, typically affected by pervasive defects like mutual layer shift, was structurally determined ab-initio on the basis of ADT data. rnThe third system is related with calcium carbonate nucleation and early crystallization. The first part of this study is dedicated to the extensive investigations of calcium carbonate formation in a step by step analysis, up to the appearance of crystalline individua. The second part is dedicated to the structure determination by ADT of the first-to-form anhydrated phase of CaCO3: vaterite. An exhaustive structure analysis of vaterite had previously been hampered by diffuse scattering, extra periodicities and fast deterioration of the material under electron irradiation. rn

Generalized eMC implementation for Monte Carlo dose calculation of electron beams from different machine types

The electron Monte Carlo (eMC) dose calculation algorithm available in the Eclipse treatment planning system (Varian Medical Systems) is based on the macro MC method and uses a beam model applicable to Varian linear accelerators. This leads to limitations in accuracy if eMC is applied to non-Varian machines. In this work eMC is generalized to also allow accurate dose calculations for electron beams from Elekta and Siemens accelerators. First, changes made in the previous study to use eMC for low electron beam energies of Varian accelerators are applied. Then, a generalized beam model is developed using a main electron source and a main photon source representing electrons and photons from the scattering foil, respectively, an edge source of electrons, a transmission source of photons and a line source of electrons and photons representing the particles from the scrapers or inserts and head scatter radiation. Regarding the macro MC dose calculation algorithm, the transport code of the secondary particles is improved. The macro MC dose calculations are validated with corresponding dose calculations using EGSnrc in homogeneous and inhomogeneous phantoms. The validation of the generalized eMC is carried out by comparing calculated and measured dose distributions in water for Varian, Elekta and Siemens machines for a variety of beam energies, applicator sizes and SSDs. The comparisons are performed in units of cGy per MU. Overall, a general agreement between calculated and measured dose distributions for all machine types and all combinations of parameters investigated is found to be within 2% or 2 mm. The results of the dose comparisons suggest that the generalized eMC is now suitable to calculate dose distributions for Varian, Elekta and Siemens linear accelerators with sufficient accuracy in the range of the investigated combinations of beam energies, applicator sizes and SSDs.

Dosimetric properties of an amorphous silicon EPID for verification of modulated electron radiotherapy

Purpose: To investigate the dosimetric properties of an electronic portal imaging device (EPID) for electron beam detection and to evaluate its potential for quality assurance (QA) of modulated electron radiotherapy (MERT). Methods: A commercially available EPID was used to detect electron beams shaped by a photon multileaf collimator (MLC) at a source-surface distance of 70 cm. The fundamental dosimetric properties such as reproducibility, dose linearity, field size response, energy response, and saturation were investigated for electron beams. A new method to acquire the flood-field for the EPID calibration was tested. For validation purpose, profiles of open fields and various MLC fields (square and irregular) were measured with a diode in water and compared to the EPID measurements. Finally, in order to use the EPID for QA of MERT delivery, a method was developed to reconstruct EPID two-dimensional (2D) dose distributions in a water-equivalent depth of 1.5 cm. Comparisons were performed with film measurement for static and dynamic monoenergy fields as well as for multienergy fields composed by several segments of different electron energies. Results: The advantageous EPID dosimetric properties already known for photons as reproducibility, linearity with dose, and dose rate were found to be identical for electron detection. The flood-field calibration method was proven to be effective and the EPID was capable to accurately reproduce the dose measured in water at 1.0 cm depth for 6 MeV, 1.3 cm for 9 MeV, and 1.5 cm for 12, 15, and 18 MeV. The deviations between the output factors measured with EPID and in water at these depths were within ±1.2% for all the energies with a mean deviation of 0.1%. The average gamma pass rate (criteria: 1.5%, 1.5 mm) for profile comparison between EPID and measurements in water was better than 99% for all the energies considered in this study. When comparing the reconstructed EPID 2D dose distributions at 1.5 cm depth to film measurements, the gamma pass rate (criteria: 2%, 2 mm) was better than 97% for all the tested cases. Conclusions: This study demonstrates the high potential of the EPID for electron dosimetry, and in particular, confirms the possibility to use it as an efficient verification tool for MERT delivery.

High-density large-scale field emitter arrays for x-ray free electron laser cathodes

High brightness electron sources are of great importance for the operation of the hard X-ray free electron lasers. Field emission cathodes based on the double-gate metallic field emitter arrays (FEAs) can potentially offer higher brightness than the currently used ones. We report on the successful application of electron beam lithography for fabrication of the large-scale single-gate as well as double-gate FEAs. We demonstrate operational high-density single-gate FEAs with sub-micron pitch and total number of tips up to 106 as well as large-scale double-gate FEAs with large collimation gate apertures. The details of design, fabrication procedure and successful measurements of the emission current from the single- and double-gate cathodes are presented.

Forward treatment planning for modulated electron radiotherapy (MERT) employing Monte Carlo methods

PURPOSE This paper describes the development of a forward planning process for modulated electron radiotherapy (MERT). The approach is based on a previously developed electron beam model used to calculate dose distributions of electron beams shaped by a photon multi leaf collimator (pMLC). METHODS As the electron beam model has already been implemented into the Swiss Monte Carlo Plan environment, the Eclipse treatment planning system (Varian Medical Systems, Palo Alto, CA) can be included in the planning process for MERT. In a first step, CT data are imported into Eclipse and a pMLC shaped electron beam is set up. This initial electron beam is then divided into segments, with the electron energy in each segment chosen according to the distal depth of the planning target volume (PTV) in beam direction. In order to improve the homogeneity of the dose distribution in the PTV, a feathering process (Gaussian edge feathering) is launched, which results in a number of feathered segments. For each of these segments a dose calculation is performed employing the in-house developed electron beam model along with the macro Monte Carlo dose calculation algorithm. Finally, an automated weight optimization of all segments is carried out and the total dose distribution is read back into Eclipse for display and evaluation. One academic and two clinical situations are investigated for possible benefits of MERT treatment compared to standard treatments performed in our clinics and treatment with a bolus electron conformal (BolusECT) method. RESULTS The MERT treatment plan of the academic case was superior to the standard single segment electron treatment plan in terms of organs at risk (OAR) sparing. Further, a comparison between an unfeathered and a feathered MERT plan showed better PTV coverage and homogeneity for the feathered plan, with V95% increased from 90% to 96% and V107% decreased from 8% to nearly 0%. For a clinical breast boost irradiation, the MERT plan led to a similar homogeneity in the PTV compared to the standard treatment plan while the mean body dose was lower for the MERT plan. Regarding the second clinical case, a whole breast treatment, MERT resulted in a reduction of the lung volume receiving more than 45% of the prescribed dose when compared to the standard plan. On the other hand, the MERT plan leads to a larger low-dose lung volume and a degraded dose homogeneity in the PTV. For the clinical cases evaluated in this work, treatment plans using the BolusECT technique resulted in a more homogenous PTV and CTV coverage but higher doses to the OARs than the MERT plans. CONCLUSIONS MERT treatments were successfully planned for phantom and clinical cases, applying a newly developed intuitive and efficient forward planning strategy that employs a MC based electron beam model for pMLC shaped electron beams. It is shown that MERT can lead to a dose reduction in OARs compared to other methods. The process of feathering MERT segments results in an improvement of the dose homogeneity in the PTV.

The electron optical limits of performance of single-polepiece magnetic electron lenses

The thesis is concerned with the electron properties of single-polepiece magnetic electron lenses especially under conditions of extreme polepiece saturation. The electron optical properties are first analysed under conditions of high polepiece permeability. From this analysis, a general idea can be obtained of the important parameters that affect ultimate lens performance. In addition, useful information is obtained concerning the design of improved lenses operating under conditions of extreme polepiece saturation, for example at flux densities of the order of 10 Tesla. It is shown that in a single-polepiece lens , the position and shape of the lens exciting coil plays an important role. In particular, the maximum permissible current density in the windings,rather than the properties of the iron, can set a limit to lens performance. This factor was therefore investigated in some detail. The axial field distribution of a single-polepiece lens, unlike that of a conventional lens, is highly asymmetrical. There are therefore two possible physical arrangements of the lens with respect to the incoming electron beam. In general these two orientations will result in different aberration coefficients. This feature has also been investigated in some detail. Single-pole piece lenses are thus considerably more complicated electron- optically than conventional double polepiece lenses. In particular, the absence of the usual second polepiece causes most of the axial magnetic flux density distribution to lie outside the body of the lens. This can have many advantages in electron microscopy but it creates problems in calculating the magnetic field distribution. In particular, presently available computer programs are liable to be considerably in error when applied to such structures. It was therefore necessary to find independent ways of checking the field calculations. Furthermore, if the polepiece is allowed to saturate, much more calculation is involved since the field distribution becomes a non-linear function of the lens excitation. In searching for optimum lens designs, care was therefore taken to ensure that the coil was placed in the optimum position. If this condition is satisfied there seems to be no theoretical limit to the maximum flux density that can be attained at the polepiece tip. However , under iron saturation condition, some broadening of the axial field distribution will take place, thereby changing the lens aberrations . Extensive calculations were therefore made to find the minimum spherical and chromatic aberration coefficients . The focal properties of such lens designs are presented and compared with the best conventional double-polepiece lenses presently available.

Experimental Study of Storage Ring Free-Electron Laser with Novel Capabilities

The Duke Free-electron laser (FEL) system, driven by the Duke electron storage ring, has been at the forefront of developing new light source capabilities over the past two decades. In 1999, the Duke FEL demonstrated the first lasing of a storage ring FEL in the vacuum ultraviolet (VUV) region at $194$ nm using two planar OK-4 undulators. With two helical undulators added to the outboard sides of the planar undulators, in 2005 the highest FEL gain ($47.8\%$) of a storage ring FEL was achieved using the Duke FEL system with a four-undulator configuration. In addition, the Duke FEL has been used as the photon source to drive the High Intensity $\gamma$-ray Source (HIGS) via Compton scattering of the FEL beam and electron beam inside the FEL cavity. Taking advantage of FEL's wavelength tunability as well as the adjustability of the energy of the electron beam in the storage ring, the nearly monochromatic $\gamma$-ray beam has been produced in a wide energy range from $1$ to $100$ MeV at the HIGS. To further push the FEL short wavelength limit and enhance the FEL gain in the VUV regime for high energy $\gamma$-ray production, two additional helical undulators were installed in 2012 using an undulator switchyard system to allow switching between the two planar and two helical undulators in the middle section of the FEL system. Using different undulator configurations made possible by the switchyard, a number of novel capabilities of the storage ring FEL have been developed and exploited for a wide FEL wavelength range from infrared (IR) to VUV. These new capabilities will eventually be made available to the $\gamma$-ray operation, which will greatly enhance the $\gamma$-ray user research program, creating new opportunities for certain types of nuclear physics research.

With the wide wavelength tuning range, the FEL is an intrinsically well-suited device to produce lasing with multiple colors. Taking advantage of the availability of an undulator system with multiple undulators, we have demonstrated the first two-color lasing of a storage ring FEL. Using either a three- or four-undulator configuration with a pair of dual-band high reflectivity mirrors, we have achieved simultaneous lasing in the IR and UV spectral regions. With the low-gain feature of the storage ring FEL, the power generated at the two wavelengths can be equally built up and precisely balanced to reach FEL saturation. A systematic experimental program to characterize this two-color FEL has been carried out, including precise power control, a study of the power stability of two-color lasing, wavelength tuning, and the impact of the FEL mirror degradation. Using this two-color laser, we have started to develop a new two-color $\gamma$-ray beam for scientific research at the HIGS.

Using the undulator switchyard, four helical undulators installed in the beamline can be configured to not only enhance the FEL gain in the VUV regime, but also allow for the full polarization control of the FEL beams. For the accelerator operation, the use of helical undulators is essential to extend the FEL mirror lifetime by reducing radiation damage from harmonic undulator radiation. Using a pair of helical undulators with opposite helicities, we have realized (1) fast helicity switching between left- and right-circular polarizations, and (2) the generation of fully controllable linear polarization. In order to extend these new capabilities of polarization control to the $\gamma$-ray operation in a wide energy range at the HIGS, a set of FEL polarization diagnostic systems need to be developed to cover the entire FEL wavelength range. The preliminary development of the polarization diagnostics for the wavelength range from IR to UV has been carried out.