NSF-MRI 2013

Title

MRI: The Development of an Instrument for Isotope Production and Photon Activation Analysis (MRI Track 2)

Proj Summary

Each proposal must contain a summary of the proposed project not more than one page in length. The Project Summary consists of an overview, a statement on the intellectual merit of the proposed activity, and a statement on the broader impacts of the proposed activity.

\centerlineTemplate:\bf Project Summary: The Development of an Instrument for Isotope Production and Photon Activation Analysis (MRI Track 2)

%\centerline{{\bf PIs}: Tony Forest, Alan Hunt, Phil Cole, Valeriia Starovoitova

We propose to develop an instrument that will irradiate materials for the purpose of supplying isotopes and facilitating multidisciplinary research using Photon Activation Analysis (PAA). In June of 2012, the Idaho Accelerator Center (IAC) received a grant from the state of Idaho as part of the Idaho Global Entrepreneurial Mission (IGEM) program. One of the proposed objectives was to investigate the use of an electron accelerator to produce copper isotopes for use in medical diagnostic procedures. Based on the above research, we now propose to develop an instrument, that qualifies for the MRI category ``Track 2, to produce isotopes and perform Photon Activation Analysis (PAA) services. The equipment needed to construct this instrument will leverage State and Federal funds. The second year work under the IGEM grant will seek to install a transport system to remotely moves samples in and out of the high radiation area. We request MRI funds to supplement this investment allowing the procurement of a more advanced transports system as well as a set of detectors and beam steerers to improve the irradiation quality and reduce sample heating. Funds from the MRI and the IGEM grant will be pooled to pay for the procurement and installation of the transport system. The MRI will further support the procurement of CVD diamond detectors to measure the radiation field in situ as well as beam position monitors and steering coils to position the radiation at the optimal location to maximize irradiation of the sample and as a result isotope activity. A bending magnet will be used to sweep electrons away from the sample thereby reducing heating of the sample by at least 80\%.

Intellectual Merits

The development of an accelerator based Isotope production tool with the dual purpose of enabling research that utilizes Photon Activation Analysis represents the primary intellectual merits of this proposal. Nuclear reactors currently produce many of the isotopes used by industry and medical procedures. The Idaho Accelerator Center (IAC) has been funded by the Idaho Global Entrepreneurial Mission (IGEM) to investigate the production of medical isotopes using an electron accelerator. We propose to investigate the production of several isotopes to be used by both industry and medicine. The application of photo-nuclear reactions for the production of isotopes contains several challenges for optimizing production efficiency. The most notable, based on our previous work, has been the alignment of the sample with the photon flux. We propose installing a photon monitoring system that will use CVD diamond detectors to measure photon rates up to $10^{12}$ photons/cm$^2$/sec.

The above research in accelerator based isotope production has also enhanced the IAC's Photon Activation Analysis (PAA) capabilities. The high photon luminosity used to produce isotopes may be used to irradiate samples for the purpose of quantifying the concentration of chemical elements within the sample. Previous PAA measurements done a the IAC have demonstrated the ability to measure chemical species to the $\mu$ g per g (PPM) level, there is pressing need to improve the systematics related to sample irradiation. The ability to perform these measurements non-destructively impacts research in disciplines ranging from environmental research to Archeology.

Broader impacts

The proposed instrument serves is a training facility as well as provide a service to both industry and research. As part of Idaho State University's Idaho Accelerator Center, the proposed instrument will serve as an education and training platform for students. Students in the accelerator physics program at ISU can receive hands on training in accelerator operations as well as investigate ways to improve accelerator performance for irradiating materials to produce isotopes or perform photon activation analysis. The insturments ability to producte isotopes can help reduce the isotope shortage being reported by DOE's National Isotope Center. The production of Cu-67, a current research project, can be used as an antibody label for cancer therapy and imaging. PAA has an established record of its impact on several research areas including environmental studies, material science, forensic science, biochemistry, art, archaeology, and other areas which rely on using a non-destructive method to quantify the elements present in materials.

Project Description

\section{Introduction}

We propose to develop an instrument that will irradiate materials for the purpose of supplying isotopes and facilitate multidisciplinary research using Photon Activation Analysis (PAA).. In June of 2012, the Idaho Accelerator Center (IAC) received a grant from the state of Idaho as part of the Idaho Global Entrepreneurial Mission (IGEM) program. One of the proposed objectives was to investigate the use of an electron accelerator to produce copper isotopes for use in medical diagnostic procedures. Preliminary results of the work sponsored by this research have indicated that the production of copper isotopes, and isotopes in general, strongly depends on the alignment of incident radiation to the sample. While a sample size of 2 cm is predicted to produce the highest number of isotopes per volume, a misalignment of more than a centimeter may reduce the amount of isotopes produced by a factor of at least two. The results of this work illustrates the need for a system to monitor the spatial distribution of the photons used to irradiate the samples as well as a system to transport samples into and out of the high radiation area.

Based on the above research, we propose to develop an instrument, that qualifies for the MRI category ``Track 2, to produce isotopes and perform Photon Activation Analysis (PAA) services. The equipment needed to construct this instrument will leverage State and Federal funds. The second year work under the IGEM grant will seek to install a transport system to remotely moves samples in and out of the high radiation area. We request MRI funds to supplement this investment allowing the procurement of a more advanced transports system as well as a set of detectors and beam steerers to improve the irradiation quality and reduce sample heating. Funds from the MRI and the IGEM grant will be pooled to pay for the procurement and installation of the transport system. The MRI will further support the procurement of CVD diamond detectors to measure the radiation field in situ as well as beam position monitors and steering coils to position the radiation at the optimal location to maximize irradiation of the sample and as a result isotope activity. A bending magnet will be used to sweep electrons away from the sample thereby reducing heating of the sample by at least 80\%.

a.) Information

\section{Information about the Proposal (a)}

\subsubsection{Instrument Location and Type (a.1)}

Physical location: Idaho Accelerator Center, Pocatello, ID

Instrument type: MRI-61

\subsubsection{Justification for Submission as a Development (Track 2) Proposal (a.2)} (1 page)

The proposed instrument will be developed by combining several instruments from different vendors with an electron accelerator currently in operation at the Idaho Accelerator Center. A substantial amount of effort will be undertaken to transform the electron accelerator into a tool for isotope production and PAA. Preliminary results indicate that the electron accelerator can be developed into an instrument that is more efficient, stable, and effective at providing the service of isotope production and photon activation analysis. A key ingredient to the instrument will be a transport system (Rabbit) to remotely position samples at the optimum location for irradiation and then remove them from the high radiation area. The Idaho Accelerator Center's on staff engineers will install the system developed in conjunction with IntelliTrack, Inc. The second key component is a beam control and feedback system that will allow operators to deliver a constant flux of photons to the specified sample location. The implementation of CVD diamond photon detectors capable of measuring the high photon flux of $10^{12}$ photons/sec/cm$^2$ will be a challenge. The remote transport system and the photon flux monitor each represent the development of an instrument. An instrument for Isotope production and PAA can be developed by combining each of the two instruments above with an electron accelerator. The development of this instrument will require the design and fabrication talents of engineers as well as the quality control and measurement expertise of scientists.

b.) Research Activities

\section{Research Activities to be Enabled (b)} ( 4 pages) The research activities to be enabled by the proposed instrument can be grouped into two categories; Isotope production and Photon Activation Analysis.

\subsection{current isotope crisis}

The consumption of man made isotopes by industry and medicine continues to grow unabated. In fiscal year 2011, the Department of Energy's Isotope program had a budget of \$48.5 million that was used to send about 450 shipments of isotopes to over 150 industrial users and 100 researchers~\cite{FY2013CongBudgetOff}. The Isotope Production Facility (IPF) at Los Alamos National Laboratory, the Brookhaven Linac Isotope Producer (BLIP) at Brookhaven National Laboratory, and processing facilities at Oak Ridge National Laboratory (ORL) are the three primary facilities for isotope production. The increase in isotope demand has, in the case of medical isotopes, resulted in an isotope supply crisis. A world's supply of technetium 99, an isotope used in 85\% of the diagnostic imaging procedures, is becoming difficult to procure due to the shutdown of Canada's Chalk River facility and the reliability of the aging reactors like the Petten reactor in the Netherlands. The Chalk River and Patten reactors were producing about 60 \% of the world's techetium supply. As a result, alternative ways of producing isotopes are being pursued.

In 2012, the Canadian nuclear and particle physics laboratory, TRIUMF, began developing Advanced Rare IsotopE Laboratory (ARIEL) to house a 50 MeV super conducting linac capable of generating 10 mA electron currents (500 kW). The primary mission of the facility is the production of rare isotopes with a secondary mission of anticipating the future uses of e-linac technologies for the production of medical isotopes. One goal of the rare isotope research it to develop next generation cancer treatment.

The Idaho Accelerator Center has, for the past year, been researching the production of Isotopes that may be used in medicine. The current research project, funded by the Idaho Global Entrepreneurial Mission (IGEM), involves an investigation into the production of Cu-67 using an electron accelerator. The reaction, ${68 \atop\; }Zn (\gamma,p){67 \atop \; }Cu$, uses the bremstrahlung photons, produced when an electron interacts with a tungsten target, to eject a proton from the zinc target thereby producing copper-67.

\subsection{accelerator based isotope production}

A common method used to artificially produced isotopes bombards materials with the neutron flux from a nuclear reactor. We propose to produce isotopes using the bremsstrahlung photons produced by the interaction of an accelerated electron beam with a Tungsten converter in order to remove a proton or neutron from a nucleus. In most cases, the isotope will be produced from naturally occurring material.

For example, Irridium-192, used by industry to test flaws in metals via gamma radiography, can be produced when a photon has sufficient energy to remove on of the neutrons in Irridium-193. Sixty three percents of naturally occurring Irridium is in the form of Irridium-163 while the remaining fraction of Irridium is in the form of Irridium-191. Nuclear reactors can produce Irridium-192 using the less dominant natural isotope Irricium-191. The cross section for the photo-production of Irridium -192 from Ir-193 peaks around 0.5 barns for 13 MeV photons(http://cdfe.sinp.msu.ru/services/exfor/m0049.exf). The thermal neutron capture cross section for Ir-191 is about 400 barns, eight hundred times larger than photo-production of Ir-192 from Ir-193. The photoprodction of Ir-192 can theoretically become competitive with the produciton of Ir-192 from nuclear reactors if the photon flux is more than four hundred times higher than the available neutron flux (10$^{15}$ neutrons/s/cm$^2$. Although this fundamental calculation provides a quick estimate, there are several application specific areas that need to be evaluated in order to determine how competitive accelerator based isotope production can be compared to reactor based production.

\subsection{interdisciplinary research enabled by the device}

Photon Activation Analysis (PAA) has been deployed as a research tool at the Idaho Accelerator Center for the past several years thanks mostly to visiting scientist Christian Segabade, one of the developers and leading experts in the field of PAA . The method has been used to quantify the content of materials based on the energy of photons emitted from nucleii that are transitioning from excited states after being pushed there as a result of their exposure to an intense photon beam produced through bremsstrahlung using the IAC's electron accelerators. PAA's most useful attribute is that it requires little to no sample preparation to non-destructively make an accurate measurement of a material's elemental composition.

Since PAA determines the chemical content of a samples under study relative to a calibrated sample with a well known chemical composition. A spectroscopic measurement of the calibrated and unknown samples is performed after each is irradiated by the same photon flux. The resulting element spectra are compared using methods similar to those used by inductively coupled plasma (ICP) mass spectroscopy or atomic absorption spectroscopy (AAS). Some advantages of PAA are that measurements can be made non-destructively, on samples that are a few milligrams or many kilograms, over the entire sample volume and not just on the sample surface, and with little risk of sample contamination. As a result, PAA has been applied to a wide range of research activities such as environmental studies, material science, archaeology, and forensic science. Two specific examples of PAA performed at the IAC are given below.

\subsubsection{environmental science}

The extent of the introduction of air borne pollutants, either natural or manmade, has been quantified using PAA. On June 4, 2011, Chile's Puyehue volcano erupted throwing ash more than 6 miles into the atmosphere. The volcano is located in the Puyehue-Cordon Caulle chain of south-central Chile. Four dust samples were collected over a two week period in the area of Puyehue National Park, very near the center of the eruption. Drs Jeronimo Blostein and Romina Daga of the Centro Atomico Bariloche - Instituto Balseiro provided the ash samples that were used to perform a PAA. Figure ~\ref{fig:Puyehue2011} illustrates the concentration of Calcium in the air immediately following the Puyehue eruption. The concentration of Calcium increase about 50% just two days after the eruption and remained high for about two weeks.

\begin{figure}[htbp] \begin{center} \mbox{\includegraphics*[width=9cm]{Graphs/Sample_HpGeSpectrum4PAA.jpg}} \mbox{\includegraphics*[width=9cm]{Graphs/Puyehue2011.png}} \caption{\small A sample PAA spectrum using a HpGe detector. The concentration change of Calcium of a two week period after the Puyehue eruption on June 4, 20\ 11. \label{fig:Puyehue2011} \end{center} \end{figure}

\subsubsection{Moon Dust Characterization}

PAA was used to determine the trace elements present in the Minnessota Lunar Simulant 1 (MLS-1) material synthesized to approximate soil sample 10084 from the Apollo 11 mare material. The work was done in collaboration with the University of Colorado, who provided the simulant for the test. Synthesized materials, like MLS-1, were produced to aide in the development of next generation lunar technologies for future lunar missions. Figure XXX quantifies PAA's ability to measure the trace elements of this material. The results of this work indicate that PAA was able to reproduce previous measurements of the simulant's chemical composition using a different technique known as differential thermal analysis. PAA also seems to be as precise if not more precise than the previous measurements by Tucker and Setzer.

\begin{figure}[htbp] \begin{center} \mbox{\includegraphics*[width=9cm]{Graphs/MLS-1_PAAresults_Land.png}} \caption{\small The concentrations of several chemical elements in the Minnessota Lunar Simulant 1 (MLS-1) material. The uncertainty from measurements using PAA are given by the risers is the image and compare with the uncertainties reported by Tucker \& Setzer using a differential Thermal Analysis.} \label{fig:DeltaDoverD} \end{center} \end{figure}

Table of different research areas using PAA.

River sediment research http://link.springer.com/article/10.1007%2FBF02518904?LI=true

Lanthanum research http://www.sciencedirect.com/science/article/pii/096980439500196K

http://www.springerlink.com/index/Y771268781K46270.pdf

Recent PAA talk about iac work http://proceedings.aip.org/resource/2/apcpcs/1265/1/379_1?isAuthorized=no

c.) Description

\section{Description of Research Instrumentation and Needs (c)} (6 pages)

The Idaho Accelerator Center is currently operating a 40 MeV electron linac for the purpose of evaluating the viability of producing copper-67 as a medical isotope. Figure ~\ref{fig:JackPlusPhotonFlux} shows the exit window of the linac. Electrons impinging the tungsten target produce copious amounts of photons via Brehmsstrahlung. Figure~\ref{fig:JackPlusPhotonFlux} shows the flux of photons immediately downstream of the tungsten radiator. Samples with cross-sectional area of one square cm will be irradiated by at least 10$^{15}$ photons/sec/cm$^2$. A flux of similar magnitude as the neutrons from reactors used to produce isotopes. This flux is attenuated to about 10$^{12}$ photons/sec/cm$^2$ after passing through the zinc used for copper-67 production.

The specific activity of isotopes produced is dependent on the sample's alignment with respect to the incident photon flux. Figure ~\ref{fig:JackPlusPhotonFlux} shows a rapid decrease of photon flux as you move half a centimeter away from the accelerator's central axis. This sharp decrease in flux reduces can result in a decrease in activity for samples that are not aligned with the photon flux at the mm level. Previous measurements at the IAC have observed reductions in copper-67 activities of more than 50% when the zinc sample is misaligned by 5 mm. A system to detect the photon flux distribution is needed to maximize the activity of isotope production.

\begin{figure}[htbp] \begin{center} \mbox{\includegraphics*[width=9cm]{Graphs/JackAccelPhoto_02072013.png}} \includegraphics*[width=9cm]{Graphs/frontZn.jpg} \caption{\small A picture of the Idaho Accelerator Center's 44 MeV linac to be used as the foundation for an Isotope production and PAA tool. The photon flux a\ fter the radiator is shown.} \label{fig:JackPlusPhotonFlux} \end{center} \end{figure}

\subsection{CVD detectors}

Journal: Nuclear Instruments & Methods in Physics Research Section A-accelerators Spectrometers Detectors and Associated Equipment - NUCL INSTRUM METH PHYS RES A , vol. 524, no. 1, pp. 115-123, 2004

Diamond detectors in particle physics, R J Tapper, Rep. Prog. Phys. 63 (2000) 1273–1316.

The chemical vapor deposition (CVD) of polycrystalline diamond onto films has become an industry that currently provides "off-the-shelf" detectors among other applications.

A set of photon detectors (CVD diamond film based) will be purchased and mounted on a movable platform that will sweep the detectors through the brehmmstrahlung beam measuring its profile. Figure~\ref{fig:CVDdiamondDetector} show the packages detector that is available from CIVIDEC Instrumentation. The manufacturer specifications indicate that a photon flux of 10^$9$ to 10$^{12} photons/cm2 should output voltages from 50 mV to 5 V in a 50Ω system if a 40dB amplifier is used. The amplifier is a RF broadband amplifier with 2 GHz analog bandwith. It has the advantage that you will see all single photon pulses which are extracted from the LINAC, possibly also the RF structure of the LINAC.

The chemical vapor deposition (CVD) of polycrystalline diamond onto films has become an industry that currently provides "off-the-shelf" detectors among other applications.

A set of beam position monitors (BPMs) will be installed along with steering coils in order to steer the incident electron beam. The photon flux can then be maximized in the region of the sample in order to optimize the sample activity. After measuring the photon distribution, the detectors will be parked behind the sample in order to directly measure the photon flux during irradiation. A measurement of the flux during irradiation will document its stability and quanitfy the amount of incident radiation. An online data acquition systtem will provide a feedback system between the BPMs and the diamond photon flux detectors.

The second component is a detector system with beam position feedback to measure the radiation field in the region of the sample and then monitor the photon flux during irradiation.

GSI shows a signal output of about 2 ns when hit with a 200 MeV/u C-12 atom.

\begin{figure}[htbp] \begin{center} \includegraphics*[width=9cm]{Graphs/B4_CVD_DiamondDetextor.png} \caption{\small A packaged CVD diamond high photon flux detector manufactured by Cividec. } \label{fig:CVDdiamondDetector} \end{center} \end{figure}

\subsection{Transport System}

\begin{figure}[htbp] \begin{center} \mbox{\includegraphics*[width=9cm]{Graphs/WhiteRoomEndStation_02072013.png}} \includegraphics*[width=9cm]{Graphs/500-DriveTube.jpg} \caption{\small An illustration of the drive system from IntelliTrack which will be used to construct a ``Rabbit conveyor system to remove samples from the high radiation area.} \label{fig:TransportSystem} \end{center} \end{figure}

\subsection{BPM monitors}

\subsection{permanent deflecting magnet}

The proposed instrument will be composed of two major hardware acquisitions. The first component is a system to remotely transport samples into the radiation area and then return them to a shielded area after being activated by a high intensity photon beam. The irradiation cell, as well as the sample itself, has the potential to have a high level of activity that prevents local manual access. The remote transport system will be required to bring the sample out of the high radiation area and deposit the sample into a lead shield, if necessary. The proposed design has the potential benefit of eliminating the need to turn off the accelerator in order to access the area. In addition to reducing the sample retrieval time, this will enhance accelerator operational stability since the electron beam will remain on. Systematic effects related to the irradiation will be reduced with this increased operational stability.

d.) Impact

\section{Impact on Research and Training Infrastructure (d)} ( 2 pages)

The proposed instrument will be a facility for performing isotope production research and training accelerator physicists. The research on copper isotopes is well underway and quickly approaching a point where production for consumption is likely. The production of other isotopes for industry and research will also be under investigation using this device. The goal will be for the instrument to be self sustaining and a means of training students.

The instrument will be an opportunity to train students in the operation of an electron accelerator as well as the techniques for isotope production and PAA. Graduate students, once trained, would operate the accelerator as a means of supporting their studies at ISU.

e.) Management

\section{Management Plan (e)} ( 2 pages)

The Idaho Accelerator Center has an established record of managing a facility serving the needs of interdisciplinary researchers that use beams of electrons or photons in their research. This proposal requests the procurement of two main pieces of equipment that, when combined, serve as an inegrated instrument for the production of Isotopes and Photon Activation Analysis. The components used to develop this instrument may be considered ``off the shelf. The accelerator expertise of the IAC and the detector development expertise of the PI will be relied upon to construct a working instrument. The track records of both entities are quite sound for this project. The long term operations and maintenance plan will rely on the instruments ability to attract users. The growth of demand for medical isotopes and the continued warning of an isotop production crisis by the Department of Energy is a strong indication that the instrument will be in demand should its ability to produce isotopes become well established.

Months after award | Activity | Phase |

References

\begin{thebibliography}{99} %--- Tony's ---- \bibitem{Zhang04}X.~Zheng {\it et al.}, Phys.~Rev.~Lett.~92 (2004) 012004.

\bibitem{FY2013CongBudgetOff} FY2013 Cngressionl Budget (http://science.energy.gov/~/media/budget/pdf/sc-budget-request-to-congress/fy-2013/Cong_Budget_2013_IsoptopeProductionandDistributionProgramFunding.pdf)

\end{thebibliography}

Budget

\section{Budget}

\begin{table}[h] \begin{center} \begin{tabular}{ccc} \multicolumn{1}{c}{Cost} & \multicolumn{1}{c}{Match} & \multicolumn{1}{c}{Description} \\ \hline\hline 50,000 & N & Conveyor system for isotope samples \\ 20,000 & N & 2 electron Beam Position Monitors, steering coils, and power supplies\\ 50,000 & N & CVD diamond detectors \\ 28,000 & N & Data Acquisition System \\ 22,000 & Y & end station \\ 50,000 & Y & Professional \& Technical Services \\ \hline \end{tabular} \caption{Budget: Total expenses = \$220,000, Available Match \$72,000 (33 \%)} \end{center} \label{table:Projects} \end{table}

Budget Justification.

OCS IntelliTrack, Inc has estimated that the transport system can be acquired for \$50,000. The system will be able to move up to a 100 lb mass from the user (low radiation) area to the end station (a high radiation area). A set of beam position monitors and associated readout electronics from Bergoz instrumentation can be purchased for 5,340 euros each. An amount of \$20,000 has been budgeted to include coil steerers, power supplies, and fluctuations of the US dollar with respect to the Euro. A quote from CIVIDEC instrumentation estimates the procurement cost of a single 3mm effective area CVD diamond detector at about 6,000 euros. I have budgeted \$50,000 for four of these CVD diamond detectors and the translation stages need to sweep them through the beam using a worm gear system that has analog position encoding. A modern VME based DAQ system with EPICs monitoring is estimated to cost \$28,000 and will include a 32 channel ADC ($6k), a readout controller($3k), a miniCrate($4k), a host server ($2k), a trigger supervisor ($3k) and a NIM Discriminator /Trigger/ECL output module ($10k).

The Idaho Accelerator Center will provide a shielded end station for the irradiation area at a cost of \$22,000 and the manpower to install the remote transport system from OCS IntelliTrack, Inc as well as the translation stages to position the CVD diamond detectors at an estimated cost of \$50,000. The original source of the funds is a grant from the state of Idaho that has already been awarded.