Qucosa – Hemholtz-Zentrum Dresden-Rossendorf
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All-Metal water target with spherical window
Full text linkIntroduction
The use of a prefabricated target window assembly greatly simplifies the window installation. The window module is sealed by metal knife-edges, thus eliminating any elestomers in the target construction.
Spherical Havar window offers high strength at reduced thickness and does not require helium cooling.
The target body is of platinum-plated silver.
The target assembly includes an integral beam collimator and a four-sector mask
Experimental yields of PET radioisotopes from a prototype 7.8 MeV cyclotron
Full text linkIntroduction
The worldwide use of PET has proven beyond dispute the importance for both routine diagnosis and physiological, oncological and pharmacological research. In many ways the present success of PET relies on the mature technology of PET compact medical cyclotrons. As long time developers of new targets, isotopes and com-pounds, we have been inclined to look for new block-buster applications, high power targets and sustainable ways of embracing the GMP and regional distribution, but recent pioneering development [1] around very small cyclotrons and “embedded synthesis and qc” has pointed out an old, but important nuclear physics lesson now halfway forgotten: that many PET isotopes can be made in high yields with proton energies far below 10 MeV [2]. This has opened a new interest in small cyclotrons and their targets.
We have been testing the first GE Healthcare Prototype for a 7.8 MeV negative ion, internal ion source cyclotron with 3 production targets mounted on a short beamline. Here we present the first experimental yields of some of the important PET radionuclides.
Materials and methods
The prototype cyclotron (FIG. 1) has been in-stalled and tested without self-shield in designated experimental area in order to establish the neutron field around accelerator and targets in order to qualify design calculations for a future integrated shield.
The cyclotron energy is fixed by the radial position of the extraction foil, while the azimuth determines which of the 3 targets are being irradiated. The beam energy at front of target foil was determined on several occasions: 7.8 ± 0.1 MeV by a 2 copper-foil sandwich method (adopted from [3]). The available beam inside the cyclotron at extractor position is > 50 μA, and 35 μA are easily and long term reliably extracted (> 90 %) on to any of the 3 target positions. The prototype is capable of delivering more than 40 μA to target, but target current was limited to 35 μA under present unshielded conditions.
Results 18F
We have tested the prototype gridded (> 80 % transmission) niobium body target with 10μm Havar foil using 95 % 18O water and 35 μA on target + grid with yields given in TABLE 1. The observed yields corrected for stopping in foil, grid loss and water enrichment are 75 % of theoretical. One Fastlab FDG run using 2 h irradiation yielded 16 GBq FDG EOS, confirming the “usual” 18F activity.
Results 11C
Using gridded target and a 10μm foil with 99% N2 + 1 % O2 at 10 bar followed by trapping into ascarite gave EOB activity as shown in TABLE 2.
Results 13N
We know that the 16O(p,alpha)13N cross section is a very steep function of energy around 7.8 MeV. In the hope of using the simple water target route to 13N NH3 we have measured the 13N yields (corrected for 18F contribution). It is still unclear if these yields can be improved to make useful single doses of ammonia.
Results for other isotopes
We have used solid targets to make 45Ti, 64Cu, 68Ga and 89Zr. The development of these solid targets is still in progress, but especially the 68Ga yield looks promising (3 GBq EOB after 1 h on natural Zn will give > 15 GBq on enriched 68Zn)
Automated stopcock actuator
Full text linkIntroduction
We have developed a low-cost stopcock valve actuator for radiochemistry automation built using a stepper motor and an Arduino, an open-source single-board microcontroller. The con-troller hardware can be programmed to run by serial communication or via two 5–24 V digital lines for simple integration into any automation control system. This valve actuator allows for automated use of a single, disposable stopcock, providing a number of advantages over stopcock manifold systems available on many commercial radiochemistry rigs or over using solenoid valves. This actuator allows for the use a wide variety of stopcocks, ranging in size, shape and material, giving flexibility to be used in a large variety of applications.
Material and Methods
The actuated valve consists of two main parts, the actuator and the control electronics. The actuator consists of a stepper motor, an infrared ‘home position’ sensor, a stopcock backplate, and a coupler from the driveshaft to stopcock handle. The stepper motor is a NEMA-17 size that runs 200 steps/rotation with a 5mm drive shaft. The coupler is an interchangeable part, custom to each stopcock model, with each part drilled out to fit the motor drive shaft and milled out for a tight fit to the stopcock handle. The backplane consists of a plate offset from the motor body with 5 screws positioned to keep the stopcock body from rotating relative to the motor. A reflective optical sensor (Vishay TCRT1000) is used as a limit switch to determine a ‘home’ position for the stopcock. With a slight modification to most any stopcock in cutting off a tab that limits rotation, the handle can rotate 360°. This allows for opening all three ports to each other, which has been done to all stopcocks used with this actuator.
The control electronics consist of an Arduino Uno board and a motor shield (add-on board), connecting to the actuator by an Ethernet cable. The motor shield functions to interface the low-power Arduino circuitry with a high power H-bridge motor driver circuit. The Arduino runs two sets of code, initialization and its loop. The initialization routine runs when power is first powered up, and then continues to run the loop. The initialization routine rotates the valve until the IR limit switch is activated, and rotates an-other 45° from position home, sealing off all ports on the stopcock. Following initialization, the Arduino enters its loop, which repeatedly compares its current position to its target posi-tion. When the target position and current posi-tion do not match, the stepper motor turns in the shortest direction towards its target position. The hardware can be interfaced by either serial communication or by two 5–24V digital signals defining positions 1–4. The wide range of allowed input signal voltages is realized by using an optocoupler that accepts 5–24 V inputs but outputs TTL signals compatible with the Arduino’s hardware.
Results and Conclusion
A photo of the implementation of the actuator is shown in FIGURE 1. It has overall dimensions of 3.5×1.75×2.5”, excluding a mounting bracket. Control electronics are housed in a compact box built for an Arduino, giving the control electron-ics a clean, professional look. Challenges in de-sign included determining a maximum motor speed where the motor would provide enough torque but yet move fast enough to be useful, finding that rotational speed of 6 seconds/full rotation is best
Development and Validation of Advanced Theoretical Modeling for Churn-Turbulent Flows and Subsequent Transitions
Full text linkThe applicability of CFD codes for two-phase flows has always been limited to special cases due to the very complex nature of its interface. Due to its tremendous computational cost, methods based on direct resolution of the interface are not applicable to most problems of practical relevance. Instead, averaging procedures are commonly used for these applications, such as the Eulerian-Eulerian approach, which necessarily means losing detailed information on the interfacial structure. In order to allow widespread application of the two-fluid approach, closure models are required to reintroduce in the simulations the correct interfacial mass, momentum, and heat transfer.
It is evident that such closure models will strongly depend on the specific flow pattern. When considering vertical pipe flow with low gas volume flow rates, bubbly flow occurs. With increasing gas volume flow rates larger bubbles are generated by bubble coalescence, which further leads to transition to slug, churn-turbulent, and annular flow. Considering, as an example, a heated tube producing steam by evaporation, as in the case of a vertical steam generator, all these flow patterns including transitions are expected to occur in the system. Despite extensive attempts, robust and accurate simulations approaches for such conditions are still lacking.
The purpose of this dissertation is the development, testing, and validation of a multifield model for adiabatic gas-liquid flows at high gas volume fractions, for which a multiple-size bubble approach has been implemented by separating the gas structures into a specified number of groups, each of which represents a prescribed range of sizes. A fully-resolved continuous gas phase is also computed, and represents all the gas structures which are large enough to be resolved within the computational mesh. The concept, known as GENeralized TwO Phase flow or GENTOP, is formulated as an extension to the bubble population balance approach known as the inhomogeneous MUltiple SIze Group (iMUSIG). Within the polydispersed gas, bubble coalescence and breakup allow the transfer between different size structures, while the modeling of mass transfer between the polydispersed and continuous gas allows including transitions between different gas morphologies depending on the flow situations. The calculations were performed using the computational fluid dynamic code from ANSYS, CFX 14.5, with the support of STAR-CCM+ v8.06 and v9.02. A complete three-field and four-field model, including a continuous liquid field and two to three gas fields representing bubbles of different sizes, were first tested for numerical convergence and then validated against experimental data from the TOPFLOW and MT-Loop facilities
Development of [NH3] Ammonia target for Cyclone-30 at KFSH&RC
Full text linkIntroduction
Nitrogen [13N] NH3 is a liquid radioisotope, produced by medical cyclotrons for nuclear medicine application and widely applied for evaluation of myocardial perfusion in clinical assessments [1,2]. Owing to its short half-life (10 minutes), the unloading procedure of the radio-active solution of [13N]NH3 from the target is crucial in saving the activity produced for patient. Therefore, an efficient technique in un-loading the radioactive solution from the target body was developed using COMSOL Multiphysics. The new design of the target with improved unloading technique resulted in 30% increase of the available 13N activity. In our experiments, 13N was produced by the 16O(p,α)13N reaction. The energy of proton beam was 16.5 MeV.
Material and Methods
A 2D model was developed using COMSOL Multiphysics to simulate the inner geometry of [13N] Ammonia target. In the 2D model, water and aluminum were used as materials for the inner body and outer boundary (walls), respectively. The physical equations used to solve the problem of allocating proper place for the loading/unloading opening is turbulent, k-ε Module being extracted from fluid flow module. FIGURE 1 shows the result of simulating water flow on the target water channels. The entrance of the pushing solution (for unloading) was designed to create a turbulent flow inside the target body and, hence, to collect most of the activity inside the target.
FIGURE 2 shows the setup for 13N production. A peristaltic pump is used to push the solution after irradiation to the hotcell at 6 ml/min flowrate. The distance from the target to the hotcell is approximately 30 meters.
Results and Conclusion
FIGURE 3 presents activity produced in milicurie (mCi) for several patient runs. The activity obtained in some experiments reached up to 330 mCi when we irradiated the target with 25 μA for 15 min. This was satisfactory for delivery to the patient at the nuclear medicine department. Moreover, purity of [13N] purity was above 95 % what meets the standard regulation for administration to a patient
Symmetric solid target transport system
Full text linkIntroduction
The expansion of our PET isotope production with a new TR-19 cyclotron necessitated a suitable solid target transport system. None of the known existing and proposed solid target transport systems (STTS) was able to meet the technical and budget requirements of the MIR cyclotron facility [5].
A unique carrier design allowed us to develop a fully automated 50.8 mm inner diameter pneumatic tube STTS with an in-hot-cell compact form factor receiving station. The cyclotron or vault side loading station is a mere vertically symmetric version of the in-hot-cell station. The carrier is able to accommodate any of our inhouse developed 86Y, 64Cu, 76Br, 89Zr and 99mTc target holders without further modifications.
Material and Methods
Technical constraints were imposed by the dimensions of the target holders (FIG. 1) and the overall station size (FIG. 3). A receiving station would be inside a hot cell and, up to three sending stations would be located in the confined vault space under the solid target irradiation units. In addition, safety and budget requirements demanded a fully automated, easy to maintain STTS.
The target holders are of various geometries with the 99mTc having the maximum dimension of 46.65 mm along its diagonal.
Pseudo carriers with diameters ranging from 41 to 49.5 mm (no wear band) and lengths from 50.8 to 102 mm were tested on 50.8 mm inner diameter Kuriyama Tigerflex™ and Goodyear Nutriflex™ tubing. Smaller diameter and length test samples became wobbly, slow, and were getting stuck on occasion. Lengths in the upper limits became stuck in turns with radii close to the minimum radius of the tubing. The necessary negative pressure was achieved by employing a 2.5pHP Ridgid WD06250 blower. The transparent Goodyear Nutriflex™ tubing was chosen for the further STTS development.
A carrier capable of loading and unloading regardless of its axial orientation was constructed.
This novel design allows for a relatively compact station W 112 × H 220 × L 300, which reduce the dependence on the location of the tube openings in the walls of the hot cell (BqSv, Taiwan). As a result the station can be conveniently placed in areas not typically occupied by processing modules or used by chemists, e.g. close to the upper left corner. To avoid reliance on expensive proprietary parts, all components were designed or chosen to insure reliability with minimal maintenance. The enclosure and opening mechanism are 3D-printable using ABS plastic, and can be made in-house on demand. “Platform sharing” between hot cell and vault stations further simplifies support and maintenance.
As with the mechanical hardware, the electronic components and boards were selected to minimize the dependency on a single supplier. The main controller board is based on Atmel\'s AVR series of microcontrollers, which are known to be largely backward compatible, well documented and have an extensive user support base. A single “brick” controls up to three stations. Bricks can be daisy chained with one functioning as a master.
The control software takes advantage of the rapid development capabilities of National Instrument\'s LabView graphical language. It is intended to work on Unix-like and Windows operating systems as well as to allow control from hand-held devices. Password security, interlocks and traceability follow the accepted safety standards for radioisotope handling.
Results and Conclusion
The Symmetric STTS has proven characteristics of reliability, ease of use and safety over hundreds of runs. Given that no convenient carting path exists, it is the ideal means for bringing solid target holders from the underground cyclotron vault to the chemistry processing hot cells at ground level. Transported activities are less than 37.0 GBq (1.0 Ci) for 64Cu and 3.7 GBq (100 mCi) for 89Zr. Carrier velocity is about 4.7m/s minimizing the time activity is present between cyclotron and hot cell. No human interaction with the irradiated target is needed during transport. The carrier does not need to be taken out of the STTS. Even though the BqSv hot cells are equipped with teletongs, they are not needed to recover the target when it arrives at the hot cell; the target is directly dropped into the processing module, e.g. the dissolution vessel for 64Cu processing.
The software is engineered in a manner that gives the operator full control of the states of the sending and receiving stations. At the same time, it avoids graphically dense and overloaded GUI in order to reduce the probability of human error. Currently the control program runs on a PC/Laptop and communicates with the controller over USB. LabView provides add-ons that allow control with a tablet or other hand-held (under development).
The fully automated symmetric STTS is ideal for isotope production facilities that are being envisioned, conceptualized or are in their planning stage. Its versatility, low initial and operating costs might even justify deployment in facilities which already employ a less optimal solid target transport.
Invention application for the Symmetric STTS was filed with the Office of Technology Management of Washington University in Saint Louis, Missouri, USA
Simplified targetry and separation chemistry for 68Ge production
Full text linkIntroduction
68Ge (t½ = 270.8 d, 100% EC) is an important radionuclide for two reasons: 1) once in equilib-rium with its daughter nuclide 68Ga (t½ = 68 min, 89 % β+, 3 % 1077 keV γ), it can be used as a positron source for attenuation correction and calibration of PET/MRI scanners; and 2) it can be employed as a generator of 68Ga for radiophar-maceutical preparation. Most isotope production facilities produce it using natural gallium (60.1% 69Ga, 39.9% 71Ga, melting point: 39 °C) as target material for proton bombardment at energies > 11.5 MeV, the threshold energy for 69Ga(p,2n)68Ge [1]. A maximum cross section of ~330 mb for natGa(p,x)68Ge occurs at ~20 MeV [1], hence proton energies in this neighborhood are mandatory for large scale production. Galli-um targetry is challenging due to its low melting point and corrosivity, hence compounds such as Ga2O3 (melting point: 1900 °C) or GaxNiy alloys (melting points > 800 °C) [2], have been used as target compounds [3,4,5]. The separation chem-istry technique employed by large-scale produc-tion facilities is liquid-liquid extraction using CCl4 [6,7]. In this work, two simple methods for GaxNiy alloy preparation are presented as well as a simple germanium separation procedure using a commercially available extraction resin.
Material and Methods
GaxNiy alloys were prepared by two methods (A,B). A) electrodeposition over 1.3 cm2 of a gold disk substrate. Ga2O3 and NiSO4.6H2O were dis-solved in a mixture of (27%) H2SO4 and NH4OH at pH 1.5 in a 3:2 mass ratio so that the Ga:Ni molar ratio was 4:1. The solution was then transferred to a 15 mL plating cell, in which a current of 29 mA/cm2 was applied with a platinum anode at 1 cm from the gold surface. B) Ga pellets were fused together with Ni powder at different Ga:Ni molar ratios using an induction furnace (EIA Power Cube 45/900). The resulting alloy pellets were then rolled to foils using a jeweler’s mill pressed between Nb foils to avoid contamination.
Target irradiations were performed on a GE PETtrace at 16 MeV protons. The electroplated alloys were mounted on a custom-made solid target irradiation system with direct water-jet cooling applied to the backside of the gold disk. The alloy foils were placed on top of in a 1.2 cm diameter, 406 μm deep pocket made of Nb and sealed against a 51 μm Nb foil using a teflon O-ring. The alloys were in direct contact with the Nb foil to allow thermal conduction. At the rear of the Nb pocket is a water-cooling stream to transfer heat convectively during irradiation.
Ge separation was achieved based on the difference in distribution coefficients between Ge, Ga, Zn, Cu, Ni and Co at different HNO3 molarities in DGA resin (Triskem International). Initial tests on the resin were performed after two pilot irradiations on natural gallium (a,b). a) 16 MeV protons were directed downward on an external beam-line (−30 °) onto 640 mg of molten elemental natGa pooled on a water-cooled niobium support. b) 330 mg natGa pellet was melted in the same Nb pocket well used with the alloys and was also sealed against a 51 μm Nb foil. The irradiated gallium was left to decay for 2 weeks and then was dissolved in 6 mL of concentrated HNO3. The solution was then passed through 200 mg of DGA resin packed in a 5 mm diameter column at a flow rate of 1.1 mL/min. A separation profile for Ge, Ga and Zn was obtained by collecting 0.2–1.0 mL fractions, which were analyzed by gamma ray spectroscopy on a HPGe detector.
Two thick NiGa4 foils have been irradiated, one for 69Ge production and for radiocobalt, from 58Ni(p,α), separation quantification; and the other one for 68Ge production with the idea of preparing a mini-generator (< 13 MBq) of 68Ga for local use in phantom imaging work and animal studies.
Results and Conclusion
A) Each electroplating batch consisted of 66.5 ± 2.9 mg of Ga2O3 mixed with 44.9 ± 3.6 mg of NiSO4.6H2O (n = 9) in the 15 mL plating cell. Higher concentrations resulted in inefficient electroplating yields due to precipitation. 66 ±
6 % of the total Ga+Ni mass in solution, that is 39.5 ± 3.3 mg of Ga-Ni was deposited after 3 d. Three plating batches over one disk resulted in a maximum target thickness of 86.7 mg/cm2. A fourth batch did not add any significant amount of alloy and salt precipitation became a problem. The electroplated surface looked homogeneous at 10× magnification on a microscope and the targets were able to withstand up to 30 μA without presenting any dark spots.
B) Alloys with Ga:Ni molar ratios of 1.0, 2.0, 2.9, 3.7 and 5.2 were fused by induction heating. TABLE 1 summarizes the results from manipulating these foils. These alloys were analyzed by X-ray fluorescence using a 109Cd excitation source quantifying the x-rays peaks: 9.26 keV for Ga and 7.48 keV for Ni. A linear relationship between the ratio of count rates of these two peaks to the alloy Ga:Ni molar ratio was found and employed for the characterization of the electroplated Ga-Ni layers.
Results from the irradiations over natGa on Nb supports are presented in TABLE 2.
TABLE 3 presents the results from irradiating two thick NiGa4 foils made by induction heating.
Figure 1 contains the separation profile with DGA. 91% of the 68Ge is eluted in 2 mL of de-ionized water.
We developed two simple methods for NiGa4 alloy manufacture. With a melting point > 800 °C and 80% presence of natGa, it is a more convenient target for 68Ge production compared to Ga encapsulated in Nb. The separation method based on the extraction resin DGA yields similar results as the liquid-liquid extraction method mentioned in [6,7], but we believe this is a more convenient method since it only requires a single trap-and-release step and not many extraction steps
Relaxation dynamics in photoexcited semiconductor quantum wells studied by time-resolved photoluminiscence
Full text linkGegenstand der vorliegenden Arbeit ist die Untersuchung der Photolumineszenzdynamik von Halbleiter-Quantentöpfen (Quantum Wells), die durch Anregung von Intraband-Übergängen mittels resonanter Laserpulse im mittleren Infrarot- und Terahertz-Spektralbereich verändert wird. Diese Zweifarbenexperimente wurden mit Hilfe eines optischen Aufbaus für zeitaufgelöste Photolumineszenzspektroskopie am Großgerät Freie-Elektronen Laser FELBE am Helmholtz-Zentrum Dresden-Rossendorf realisiert. Zeitlich verzögert zur gepulsten optischen Anregung über die Bandlücke wurden Intersubband- oder Intraexziton-Übergange in den Quantum Wells resonant angeregt. Die dadurch erreichte Ladungsträgerumverteilung zeigt sich in einer deutlichen Verringerung der Photolumineszenzintensität zum Zeitpunkt des zweiten Anregepulses, die im Folgenden als Photolumineszenz-Quenching bezeichnet wird.
Zunächst wird die Stärke des Photolumineszenz-Quenchings in Abhängigkeit der Polarisationsrichtung des midinfraroten Laserstrahls ausgewertet. Während die Absorption durch freie Ladungsträger für beide Polarisationsrichtungen nachweisbar ist, wird experimentell gezeigt, dass Intersubbandabsorption nur möglich ist, wenn ein Anteil der anregenden Strahlung senkrecht zur Quantum-Well-Ebene polarisiert ist.
Das Photolumineszenzsignal ist überwiegend an der energetischen Position der 1s-Exzitonresonanz unterhalb der Bandkante messbar. Die intraexzitonischen Übergangsenergien in Quantum Wells liegen typischerweise im Terahertzbereich. Unter intraexzitonischer 1s-2p Anregung erscheint auch auf dieser Energieskala ein abrupter Intensitätsverlust in der langsam abklingenden Photolumineszenztransiente. Erstmalig wurde im Photolumineszenzspektrum bei höheren Energien im Abstand der Terahertz-Photonenenergie ein zusätzliches 2s-Photolumineszenzsignal detektiert. Eine detaillierte theoretische Beschreibung dieses Problems durch unsere Kooperationspartner Koch et al. von der Phillips-Universität Marburg zeigt, dass unter intraexzitonischer 1s-2p Anregung eine effiziente Coulombstreuung zwischen den nahezu entarteten exzitonischen 2p- und 2s-Zustanden stattfindet. Während der 2p-Zustand optisch dunkel ist, kann die 2s-Population strahlend rekombinieren, was zu dem besagten 2s-Photolumineszenzsignal führt. Die Zeitkonstanten der untersuchten Ladungsträgerdynamik werden durch ein phänomenologisches Modell bestimmt, das die experimentellen Kurven sehr gut abbildet. Es wird ein Ratengleichungsmodell eingeführt, bei dem die involvierten Zustände auf optisch helle und optisch dunkle Besetzungsdichten reduziert werden.
Darüber hinaus werden mit einem modifizierten Versuchsaufbau die Terahertz-induzierten Photolumineszenzsignaturen von Magnetoexzitonen untersucht. Die Stärke des 1s-Photolumineszenz-Quenchings ändert sich dabei entsprechend der magnetoexzitonischen Übergänge, die im betrachteten Feldstärkebereich zwischen 0T und 7T liegen. Für Magnetfelder größer als 3T sind keine 2s-Photolumineszenzsignale mehr messbar, da durch das externe magnetische Feld die Entartung der 2p- und 2s-Zustände aufgehoben wird
Routine production of 18F‾ with a beam current of 200 µA on a GE PETtrace cyclotron: Experience over > 18 Months
Full text linkIntroduction
The increasing demand for [18F]FDG for clinical PET-CT and the efficiencies associated with large production runs have encouraged endeavors to increase the amount of 18F− produced by cyclotrons in a single run. The amount of 18F− is determined by the saturation yield of the nuclear reaction, the irradiation time and the beam current striking the target. The saturation yield is a function of beam energy (typically fixed for PET cyclotrons), the enrichment of the H218O (typically > 97 %) and the efficiency of the target design. Target design has already been optimized on current systems. Diminishing gains in activity are achieved by extending the irradiation time much beyond 3 hrs, so the main focus has been to increase beam current onto the targets. Increasing the beam current requires:
i) a cyclotron capable of producing the increased beam current;
ii) targets that tolerate the beam current without appreciable loss in saturation yield;
iii) sufficient shielding of the cyclotron and hot cells to accommodate the proportionally larger radiation dose rates during higher current irradiation and from the larger activities delivered to the hot cells.
We reported [1] that the self-shielded targets fitted to our cyclotron can accommodate 100 µA currents without appreciable loss in saturation yield. We also identified the potential of routine production at 200 A (100 A per target in dual target irradiation mode), but had not establish its long-term viability in routine use. We present our experience in using 200 µA for routine production of 18F- since September 2012.
Material and Methods
Our PETtrace cyclotron was installed in 2002 and has been used for routine production of various 18F and 11C tracers since January 2003. It has been upgraded incrementally so that it is now equivalent to a current generation PETtrace 880 cyclotron, which is specified at a total beam current of 130 µA. The only components on our cyclotron currently not part of the standard PETtrace 880 cyclotron configuration are the self-shielded targets and a license which allows total target beam current of 200 µA. The self-shielded targets utilize a W/Cu alloy for the main body of the target surrounding the Havar foil to provide shielding from the Havar foil by a factor of about 10 and shielding of any remnant 18F- activity in the targets by a factor of about 100 [1]. The niobium target chamber is the same size as used in the standard GE Nb25 targets. However, it dispenses with the He cooling and the vacuum foil. Only the water foil is used, which is directly exposed to the vacuum in the chamber. Foil cooling is through the water in the target chamber. One of the issues that we previously identified [1] is beam stripping by gas molecules in the vacuum tank. The amount of beam that is stripped and which impacts on components in the cyclotron is proportional to the beam current. At high currents, this can result in a runaway condition, where the effects of the stripped beam deteriorate vacuum; this then results in more beam stripping and more severe effects. The effect of diffusion pump maintenance on vacuum system performance and on the reduction of beam stripping was investigated as part of this study. We have previously found that running the ion source gas at a low flow rate (2 sccm) when cyclotron is not used greatly reduces deterioration of ion source performance over time and with use [1]. This gas flow also appears to have a beneficial effect on the vacuum. Ion source gas flow when cyclotron is off has been employed throughout the evaluation period. [18F]FDG was produced with TRACERlab MXFDG modules or FASTlab modules using both Phosphate and Citrate cassettes. Stability studies of [18F]FDG were performed to ensure it met specifications over the specified expiry time. Our current stabilization regime did not have to be adjusted for the higher activities produced with the higher beam currents.
[18F]FDG yields were calculated using input activity estimates from saturation yield and beam time and current and the non-decay corrected [18F]FDG activity measured at the end of synthesis. Thus yield calculations include target yield variations and losses in the transfer lines and not just synthesis yield.
Results and Conclusion
The flip-in probe to extraction foil transmissions as a function of ion source gas flow are given in TABLE 1. Transmission decreases with increasing ion source gas flow, as expected for a system with an internal ion source. In addition, diffusion pump maintenance had a positive impact on the transmission and this is of particular benefit at the higher beam currents where minimising beam stripping becomes more critical. The ion source output, however, decreases with decreasing ion source gas flow; hence ion source gas flow is a compromise between ion source output and probe to foil transmission. We currently use a gas flow of 5.5 sccm for our 200 µA runs. Over the period from 1st September 2012 to end of March 2014, a total of 419 [18F]FDG produc-tions were performed at total target beam currents ranging from 160 µA to 200 µA, with 227 production runs being performed at 200 µA. Beam times were typically 90 to 120 min, with some productions up to 180 min. The [18F]FDG yields are summarized in TABLE 2. The yields for the FASTlab phosphate and citrate cassettes have been listed separately in TABLE 2 as they are known to be different [2,3]. The yields obtained with the TRACERlab MXFDG are also shown. The yields at 200 µA total target current are not appreciably different from those at 120 µAh, respectively. As more experience has been gained with the self-shielded targets, service interval is actually being extended from about 10,000 µAh to 20,000 µAh, despite the higher beam currents. Diffusion pump maintenance is currently recommended every 5 years, but a 2 year maintenance interval may be advantageous for 200 µA, given the observed deterioration over a 5 year period and the improvement in performance post service (Table 1). The more frequent service is associated with the additional costs of diffusion pump oil and an extra day of scheduled down-time. Typically, vacuum is sufficiently well established 24 h after opening of the vacuum tank to run 200 µA beams with the vacuum and beam conditioning that we employ.
The targets generally have coped well with the 100 µA per target current (200 µA total beam current for dual target irradiation) over this 18 month period. However, currents of 80 µA to µ100 A per target in dual target irradiation mode reduce the tolerance to sudden increases in one of the target currents. There were 4 occasions (2 test beams and 2 production beams) when there were sudden increases of target current from 90 µA and 100 µA to about 150 µA. The rapid increase in heat deposited on the foil and target chamber and the resultant rapid pressure rise in the target chamber could not be withstood by the foil and target foil rupture ensued. This compared to 1 target foil issue over a similar period of time (18 months) at lower beam currents on the standard Nb25 target. Three separate causes were identified for these overshoots in target current: 1) behavior of control system when beam is allowed to continue past the set time; 2) large changes of set current of one of the two targets irradiated during a dual irradiation test beam and 3) an issue with DEE voltage regulation caused by the mechanical flap controls. These issues have been addressed by procedural changes (issues 1 and 2) and by fitting an available upgrade of the mechanical flap control mechanism (issue 3). The two target foil ruptures during production did not cause cancellation or delays to patient scanning, as the demand could be met by multi-ple productions and deliveries from the unaf-fected target. No unscheduled down-days occurred during the evaluation period. We have been able to achieve routine operation at 200 µA beam current through careful optimization of the critical components and parameters and a maintenance regime that we have detailed previously [1]. This maintenance scheme has not changed for the routine 200 µA operation. The safety margin, however, is reduced and so careful monitoring of the system is required to ensure that issues in one of the subsystems do not cause major events such as target foil ruptures. Our [18F]FDG yields have been maintained at the higher current and 200 µA allows large quantities of [18F]FDG to be produced routinely in a single run with relatively short beam times
Carrier Relaxation Dynamics in Graphene
Full text linkGraphene, the two-dimensional lattice of sp2-hybridized carbon atoms, has a great potential for future electronics, in particular for opto-electronic devices. The carrier relaxation dynamics, which is of key importance for such applications, is in the main focus of this thesis. Besides a short introduction into the most prominent material properties of graphene and the experimental techniques, this thesis is divided into three main parts.
The investigation of the carrier relaxation dynamics in the absence of a magnetic field is presented in Chapter 3. In the first experiment, the anisotropy of the carrier excitation and relaxation in momentum space was investigated by pump-probe measurements in the near-infrared range.
While this anisotropy was not considered in all previous experiments, our measurements with a temporal resolution of less than 50 fs revealed the polarization dependence of the carrier excitation and the subsequent relaxation. About 150 fs after the electrons are excited, the carrier distribution in momentum space gets isotropic, caused by electron-phonon scattering. In a second set of two-color pump-probe experiments, the temperature of the hot carrier distribution, which was obtained within the duration of the pump pulse (about 200 fs), could be estimated. Furthermore, a change in sign of the pump-probe signal can be used as an indicator for the Fermi energy of different graphene layers.
Pump-probe experiments in the far-infrared range in reflection and transmission geometry were performed at high pump power. A strong saturation of the pump-induced transmission was found in previous experiments, which was attributed to the pump-induced change in absorption. Our investigation shows the strong influence of pump-induced reflection at long wavelengths, as well as a lot smaller influence of the saturation of the pump-induced change in absorption. At a high pump power, the increase of the reflection exceeds the change in absorption strongly, which leads to negative pump-probe signals in transmission geometry.
In Chapter 4, investigations of the carrier dynamics of graphene in magnetic fields of up to 7T are presented. Even though the optical properties of Landau-quantized graphene are very interesting, the carrier dynamics were nearly unexplored. A low photon energy of 14meV allows the investigation of the intraband Landau-level (LL) transitions. These experiments revealed two main findings: Firstly, the Landau quantization strongly suppresses the carrier relaxation via optical-phonon scattering, resulting in an increased relaxation time.
Secondly, a change in sign of the pump-probe signal can be observed when the magnetic field is varied. This change in sign indicates a hot carrier distribution shortly after the pump pulse, which means that carrier-carrier scattering remains very strong in magnetic fields. In a second set of pump-probe measurements, carried out at a photon energy of 75meV, the relaxation dynamics of interband LL transitions was investigated. In particular, experiments on the two energetically degenerate LL transitions LL(−1)->LL(0) and LL(0)->LL(1) showed the influence of extremely strong Auger processes.
An ultrafast and extremely broadband terahertz detector, based on a graphene flake, is presented in the last chapter of this thesis. To couple the radiation efficiently to the small flake, the inner part of a logarithmic periodic antenna is connected to it. With a rise time of about 50 ps in a wavelength range of 9 μm to 500 μm, this detector is very interesting to obtain the temporal overlap in two-color pump-probe experiments with the free-electron laser FELBE. Furthermore, the importance of the substrate material, in particular for the high-speed performance, is discussed