Strong Polarization of a J=1/2 to 1/2 Transition Arising from Unexpectedly Large Quantum Interference.

We experimentally show that the 1s^{2}2s^{2}2p_{1/2}-1s2s^{2}2p_{1/2}^{2} transition in Pb^{77+} emitted in dielectronic recombination of Pb^{78+} is strongly polarized, although it is an intrinsically unpolarized J=1/2 to 1/2 transition. This unanticipated polarization is shown to be due to quantum interference with radiative recombination. The interference effect has been studied on an asymmetric resonance profile but has never been studied on polarization. In this Letter, we show that the effect on polarization can arise from a different cross term than that responsible for asymmetry, resulting in unexpectedly large polarization even for a nearly symmetric resonance suggesting a small interference.

Fisher Information Analysis of Depth-of-Interaction Estimation in Double-Sided Strip Detectors.

In very-high-spatial-resolution gamma-ray imaging applications, such as preclinical PET and SPECT, estimation of 3D interaction location inside the detector crystal can be used to minimize parallax error in the imaging system. In this work, we investigate the effect of bias voltage setting on depth-of-interaction (DOI) estimates for a semiconductor detector with a double-sided strip geometry. We first examine the statistical properties of the signals and develop expressions for likelihoods for given gamma-ray interaction positions. We use Fisher Information to quantify how well (in terms of variance) the measured signals can be used for DOI estimation with different bias-voltage settings. We performed measurements of detector response versus 3D position as a function of applied bias voltage by scanning with highly collimated synchrotron radiation at the Advanced Photon Source at Argonne National Laboratory. Experimental and theoretical results show that the optimum bias setting depends on whether or not the estimated event position will include the depth of interaction. We also found that for this detector geometry, the z-resolution changes with depth.

CdTe XG-Cam: A new high-resolution x-ray and gamma-ray camera for studies of the pharmacokinetics of radiopharmaceuticals in small animals.

BACKGROUND: The recent emergence of targeted radionuclide therapy has increased the demand for imagers capable of visualizing pharmacokinetics in developing radiopharmaceuticals in the preclinical phase. Some radionuclides emit hard x-rays and gamma-rays below 100 keV, in which energy range the performance of conventional NaI scintillators is poor. Multipinhole collimators are also used for small animal imaging with a good spatial resolution but have a limited field of view (FOV). PURPOSE: In this study, a new imager with high sensitivity over a wide FOV in the low-energy band ( < $<$ 100 keV) was developed for the pharmacokinetic study. METHODS: We developed an x-ray and gamma-ray camera for high-resolution spectroscopy, named "CdTe XG-Cam," equipped with a cadmium telluride semiconductor detector and a parallel-hole collimator using a metal 3D printer. To evaluate the camera-system performance, phantom measurements with single and dual nuclides ( 99 m Tc $^{\rm 99m}{\rm Tc}$ , 111 In $^{111}{\rm In}$ , and 125 I ) $^{125}{\rm I)}$ were performed. The performance for in vivo imaging was evaluated using tumor-bearing mice to which a nuclide ( 99 m Tc $^{\rm 99m}{\rm Tc}$ or 125 I ) $^{125}{\rm I)}$  administered. RESULTS: We simultaneously obtained information on 111 In $^{111}{\rm In}$ and 125 I $^{125}{\rm I}$ , which emit emission lines in the low-energy band with peak energies close to each other (23-26 keV for 111 In $^{111}{\rm In}$ and 27-31 keV for 125 I ) $^{125}{\rm I)}$ , and applied an analytical method based on spectral model fitting to determine the individual radioactivities accurately. In the small animal imaging, the distributions of the nuclide in tumors were accurately quantified and time-activity curves in tumors are obtained. CONCLUSIONS: The demonstrated capability of our system to perform in vivo imaging suggests that the camera can be used for applications of pharmacokinetics research.

Three-dimensional and multienergy gamma-ray simultaneous imaging by using a Si/CdTe Compton camera.

PURPOSE: To develop a silicon (Si) and cadmium telluride (CdTe) imaging Compton camera for biomedical application on the basis of technologies used for astrophysical observation and to test its capacity to perform three-dimensional (3D) imaging. MATERIALS AND METHODS: All animal experiments were performed according to the Animal Care and Experimentation Committee (Gunma University, Maebashi, Japan). Flourine 18 fluorodeoxyglucose (FDG), iodine 131 ((131)I) methylnorcholestenol, and gallium 67 ((67)Ga) citrate, separately compacted into micro tubes, were inserted subcutaneously into a Wistar rat, and the distribution of the radioisotope compounds was determined with 3D imaging by using the Compton camera after the rat was sacrificed (ex vivo model). In a separate experiment, indium 111((111)In) chloride and (131)I-methylnorcholestenol were injected into a rat intravenously, and copper 64 ((64)Cu) chloride was administered into the stomach orally just before imaging. The isotope distributions were determined with 3D imaging after sacrifice by means of the list-mode-expectation-maximizing-maximum-likelihood method. RESULTS: The Si/CdTe Compton camera demonstrated its 3D multinuclear imaging capability by separating out the distributions of FDG, (131)I-methylnorcholestenol, and (67)Ga-citrate clearly in a test-tube-implanted ex vivo model. In the more physiologic model with tail vein injection prior to sacrifice, the distributions of (131)I-methylnorcholestenol and (64)Cu-chloride were demonstrated with 3D imaging, and the difference in distribution of the two isotopes was successfully imaged although the accumulation on the image of (111)In-chloride was difficult to visualize because of blurring at the low-energy region. CONCLUSION: The Si/CdTe Compton camera clearly resolved the distribution of multiple isotopes in 3D imaging and simultaneously in the ex vivo model.

Extremely fast acceleration of cosmic rays in a supernova remnant.

Galactic cosmic rays (CRs) are widely believed to be accelerated by shock waves associated with the expansion of supernova ejecta into the interstellar medium. A key issue in this long-standing conjecture is a theoretical prediction that the interstellar magnetic field can be substantially amplified at the shock of a young supernova remnant (SNR) through magnetohydrodynamic waves generated by cosmic rays. Here we report a discovery of the brightening and decay of X-ray hot spots in the shell of the SNR RX J1713.7-3946 on a one-year timescale. This rapid variability shows that the X-rays are produced by ultrarelativistic electrons through a synchrotron process and that electron acceleration does indeed take place in a strongly magnetized environment, indicating amplification of the magnetic field by a factor of more than 100. The X-ray variability also implies that we have witnessed the ongoing shock-acceleration of electrons in real time. Independently, broadband X-ray spectrometric measurements of RX J1713.7-3946 indicate that electron acceleration proceeds in the most effective ('Bohm-diffusion') regime. Taken together, these two results provide a strong argument for acceleration of protons and nuclei to energies of 1 PeV (10(15) eV) and beyond in young supernova remnants.

Dual-radionuclide in vivo imaging of micro-metastasis and lymph tract with submillimetre resolution.

Multi-radionuclide in vivo imaging with submillimetre resolution can be a potent tool for biomedical research. While high-resolution radionuclide imaging faces challenges in sensitivity, multi-radionuclide imaging encounters difficulty due to radiation contamination, stemming from crosstalk between radionuclides and Compton scattering. Addressing these challenges simultaneously is imperative for multi-radionuclide high-resolution imaging. To tackle this, we developed a high-spatial-resolution and high-energy-resolution small animal single-photon emission computed tomography (SPECT) scanner, named CdTe-DSD SPECT-I. We first assessed the feasibility of multi-tracer SPECT imaging of submillimetre targets. Using the CdTe-DSD SPECT-I, we performed SPECT imaging of submillimetre zeolite spheres absorbed with 125I- and subsequently imaged 125I-accumulated spheroids of 200-400 µm in size within an hour, achieving clear and quantitative images. Furthermore, dual-radionuclide phantom imaging revealed a distinct image of the submillimetre sphere absorbed with 125I- immersed in a 99mTc-pertechnetate solution, and provided a fair quantification of each radionuclide. Lastly, in vivo imaging was conducted on a cancer-bearing mouse with lymph node micro-metastasis using dual-tracers. The results displayed dual-tracer images of lymph tract by 99mTc-phytic acid and the submillimetre metastatic lesion by 125I-, shown to align with the immunofluorescence image.

New liposome-radionuclide-chelate combination for tumor targeting and rapid healthy tissue clearance.

Radionuclide imaging and therapy are promising methods for controlling systemic cancers; however, their clinical application has been limited by excessive radionuclide accumulation in healthy tissues. To minimize radionuclide accumulation in non-cancerous tissues while ensuring sufficient build up in tumors, we aimed to develop a method that controlled the in vivo dynamics of radionuclides post-administration. To this end, we describe a novel strategy that combines liposomes, a potent carrier system for drug delivery, with unique radionuclide-ligand complexes based on 111In-ethylenedicysteine. Conventional 111In-ligand-complexes-carrying liposomes delivered substantial amounts of radionuclides to tumors; however, they also accumulated in the liver and spleen. In contrast, 111In-ethylenedicysteine-carrying liposomes greatly reduced non-specific accumulation, while being retained selectively at high doses within tumors. Liposomes were rapidly broken down in the liver, releasing encapsulated 111In-ligand complexes. Among the chelates used, only 111In-ethylenedicysteine could escape from the liver and be excreted in the urine. Instead, most liposomes remained intact in tumors, retaining the radionuclide-ligand complexes within them. Therefore, high tumor accumulation was obtained regardless of the type of 111In-ligand complexes in the liposomes. In vivo single photon emission computed tomography/computed tomography imaging with 111In-ethylenedicysteine-carrying liposomes accurately revealed tumor-selective radionuclide retention with little background. Hence, our new strategy could greatly enhance tumor-to-healthy tissue ratios, improve diagnostic imaging, boost therapeutic efficacy, reduce toxicity to healthy tissues, and facilitate radionuclide imaging and therapy.

Development and Utility of an Imaging System for Internal Dosimetry of Astatine-211 in Mice.

In targeted radionuclide therapy, determining the absorbed dose of the ligand distributed to the whole body is vital due to its direct influence on therapeutic and adverse effects. However, many targeted alpha therapy drugs present challenges for in vivo quantitative imaging. To address this issue, we developed a planar imaging system equipped with a cadmium telluride semiconductor detector that offers high energy resolution. This system also comprised a 3D-printed tungsten collimator optimized for high sensitivity to astatine-211, an alpha-emitting radionuclide, and adequate spatial resolution for mouse imaging. The imager revealed a spectrum with a distinct peak for X-rays from astatine-211 owing to the high energy resolution, clearly distinguishing these X-rays from the fluorescent X-rays of tungsten. High collimator efficiency (4.5 × 10-4) was achieved, with the maintenance of the spatial resolution required for discerning mouse tissues. Using this system, the activity of astatine-211 in thyroid cancer tumors with and without the expression of the sodium iodide symporter (K1-NIS/K1, respectively) was evaluated through in vivo imaging. The K1-NIS tumors had significantly higher astatine-211 activity (sign test, p = 0.031, n = 6) and significantly decreased post-treatment tumor volume (Student's t-test, p = 0.005, n = 6). The concurrent examination of intratumor drug distribution and treatment outcome could be performed with the same mice.

Extraction behavior of a novel functionalized ionic liquid for separation of platinum group metals from aqueous nitric acid solution.

A novel ionic liquid (IL) functionalized with thiodiglycol amic acid containing a soft S donor was synthesized for the effective and efficient extraction of platinum group metals (Ru, Rh, and Pd) from aqueous nitric acid solutions, such as high-level radioactive liquid waste (HLLW). The IL enabled rapid extraction of Pd(II) with an extraction ratio of approximately 100%. The extractions of Ru(III) and Rh(III) by the IL were slower than that of Pd(II), but the rates were accelerated by temperature elevation. The extractions of Ru(III) and Rh(III) at 50 °C reached equilibrium within 4 and 8 h, respectively, with the extraction ratios of over 90% without assisting agents or other methods for the extraction system. Furthermore, the IL could extract more than 90% of Ru(III), Rh(III), and Pd(II) from the simulated HLLW within 2 h at 50 °C.

Non-destructive 3D imaging method using muonic X-rays and a CdTe double-sided strip detector.

Elemental analysis based on muonic X-rays resulting from muon irradiation provides information about bulk material composition without causing damage, which is essential in the case of precious or otherwise unreachable samples, such as in archeology and planetary science. We developed a three-dimensional (3D) elemental analysis technique by combining the elemental analysis method based on negative muons with an imaging cadmium telluride double-sided strip detector (CdTe-DSD) designed for the hard X-ray and soft [Formula: see text]-ray observation. A muon irradiation experiment using spherical plastic samples was conducted at the Japan Proton Accelerator Research Complex (J-PARC); a set of projection images was taken by the CdTe-DSD, equipped with a pinhole collimator, for different sample rotation angles. The projection images measured by the CdTe-DSD were utilized to obtain a 3D volumetric phantom by using the maximum likelihood expectation maximization algorithm. The reconstructed phantom successfully revealed the 3D distribution of carbon in the bulk samples and the stopping depth of the muons. This result demonstrated the feasibility of the proposed non-destructive 3D elemental analysis method for bulk material analysis based on muonic X-rays.

Simultaneous visualization of multiple radionuclides in vivo.

The insufficient energy and spatial resolutions of radionuclide imaging with conventional scintillation detectors restrict the visualization of multiple radionuclides and of microstructures in tissue. Here we report the development and performance of an imaging system equipped with a cadmium telluride diode detector that achieves an energy resolution of 1.7% at 140 keV and a spatial resolution of 250 µm. The combination of high-resolution spectra fitted to an X-ray analysis model of the emission lines of the radionuclides in a chosen energy band allowed us to accurately determine individual radiation activities from three radionuclides to simultaneously visualize thyroid tissue (via intravenously administered iodine-125), mandibular lymph nodes (via the intramuscular injection of indium-111) and parotid lymph nodes (via a subcutaneous injection of technetium-99m) in mice. Multi-radionuclide imaging may find advantageous applications in biomedical imaging.

An application of a Si/CdTe Compton camera for the polarization measurement of hard x rays from highly charged heavy ions.

Methods to measure the polarization of x rays from highly charged heavy ions with a significantly higher accuracy than that of the existing technology are needed to explore relativistic and quantum electrodynamics effects, including the Breit interaction. We developed an Electron Beam Ion Trap Compton Camera (EBIT-CC), a new Compton polarimeter with pixelated multi-layer silicon, and cadmium telluride counters. The EBIT-CC detects the three-dimensional position of Compton scattering and photoelectric absorption, and thus, the degree of polarization of incoming x rays can be evaluated. We attached the EBIT-CC on the Tokyo Electron Beam Ion Trap (Tokyo-EBIT) in the University of Electro-Communications. An experiment was performed to evaluate its polarimetric capability through an observation of radiative recombination x rays emitted from highly charged krypton ions, which were generated by the Tokyo-EBIT. The CC of the EBIT-CC was calibrated for the ∼75 keV x rays. We developed event reconstruction and selection procedures and applied them to every registered event. As a result, we successfully obtained the polarization degree with an absolute uncertainty of 0.02. This uncertainty is small enough to probe the difference between the zero-frequency approximation and full-frequency-dependent calculation for the Breit interaction, which is expected for dielectronic recombination x rays of highly charged heavy ions.

Imaging of 99mTc-DMSA and 18F-FDG in humans using a Si/CdTe Compton camera.

The Compton camera can simultaneously acquire images of multiple isotopes injected in a body; therefore, it has the potential to introduce a new subfield in the field of biomedical imaging applications. The objective of this study is to assess the ability of a prototype semiconductor-based silicon/cadmium telluride (Si/CdTe) Compton camera to simultaneously image the distributions of technetium (99mTc)-dimercaptosuccinic acid (DMSA) (141 keV emission) and 18F-fluorodeoxyglucose (FDG) (511 keV emission) injected into a human volunteer. 99mTc-DMSA and 18F-FDG were injected intravenously into a 25-year-old male volunteer. The distributions of 99mTc-DMSA and 18F-FDG were simultaneously made visible by setting a specified energy window for each radioisotope. The images of these radiopharmaceuticals acquired using the prototype Compton camera were superimposed onto computed tomography images for reference. The reconstructed image showed that 99mTc-DMSA had accumulated in both kidneys, which is consistent with the well-known diagnostic distribution determined by clinical imaging via single-photon emission computed tomography. In the 18F-FDG image, there is broad distribution around the liver and kidneys, which was expected based on routine clinical positron emission tomography imaging. The current study demonstrated for the first time that the Si/CdTe Compton camera was capable of simultaneously imaging the distributions of two radiopharmaceuticals, 99mTc-DMSA and 18F-FDG, in a human body. These results suggest that the Si/CdTe Compton camera has the potential to become a novel modality for nuclear medical diagnoses enabling multi-probe simultaneous tracking.

In vivo simultaneous imaging with 99mTc and 18F using a Compton camera.

We have been developing a medical imaging technique using a Compton camera. This study evaluates the feasibility of clear imaging with 99mTc and 18F simultaneously, and demonstrates in vivo imaging with 99mTc and/or 18F. We used a Compton camera with silicon and cadmium telluride (Si/CdTe) semiconductors. We estimated the imaging performance of the Compton camera for 141 keV and 511 keV gamma rays from 99mTc and 22Na, respectively. Next, we simultaneously imaged 99mTc and 18F point sources to evaluate the cross-talk artifacts produced by a higher energy gamma-ray background. Then, in the in vivo experiments, three rats were injected with 99mTc-dimercaptosuccinic acid and/or 18F-fluorodeoxyglucose and imaged. The Compton images were compared with PET images. The rats were euthanized, and the activities in their organs were measured using a well counter. The energy resolution and spatial resolution were measured for the sources. No apparent cross-talk artifacts were observed in the practical-activity ratio (99mTc:18F = 1:16). We succeeded in imaging the distributions of 99mTc and 18F simultaneously, and the results were consistent with the PET images and well counter measurements. Our Si/CdTe Compton camera can thus work as a multi-tracer imager, covering various SPECT and PET probes, with less cross-talk artifacts in comparison to the conventional Anger cameras using a collimator. Our findings suggest the possibility of human trials.

Beam range estimation by measuring bremsstrahlung.

We describe a new method for estimating the beam range in heavy-ion radiation therapy by measuring the ion beam bremsstrahlung. We experimentally confirm that the secondary electron bremsstrahlung process provides the dominant bremsstrahlung contribution. A Monte Carlo simulation shows that the number of background photons from annihilation gamma rays is about 1% of the bremsstrahlung strength in the low-energy region used in our estimation (63-68 keV). Agreement between the experimental results and the theoretical prediction for the characteristic shape of the bremsstrahlung spectrum validates the effectiveness of our new method in estimating the ion beam range.