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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Spin-Controllable Dynamics in Defect-Engineered Carbon Nanotubes as Single Photon Emitters: Data-Driven Modeling and Computations

Quantum technologies, such as quantum computing and sensing, require efficient single-photon emission (SPE) sources that operate at room temperature in telecom wavelengths. While several materials can serve as SPE sources, no single platform meets all the criteria for efficiency, ambient operation, and scalability. Single-walled carbon nanotubes (SWCNTs) with covalently attached molecules offer a promising solution. Their SPE can be easily tuned via modifications of the SWCNT's diameter, chirality, and bonded molecules, enabling emission across near-IR to telecom wavelengths at ambient conditions. However, to fully realize the potential of SWCNTs and unlock their quantum capabilities, a deeper understanding of how structural defects from molecular adducts affect their emission and competing photoexcited processes is essential. To address this gap in our knowledge, this project combined quantum chemistry calculations with data-driven methods of cheminformatics (QSAR) and machine learning (ML). The developed computational approaches have provided several design strategies for covalent functionalization of SWCNTs to improve their optical response. The collaboration with Los Alamos National Lab (LANL) enabled direct comparison of computational and experimental data, facilitating method validation. This partnership was enhanced through access to LANL's Center for Integrated Nanotechnologies (CINT) utilizing User Facility Program and summer internships, which provided three NDSU graduate students with hands-on experience at LANL. The outcomes of this project included (1) Advancing the current stage of computational methods in accurate modeling of non-adiabatic spin-dependent photoexcited dynamics and its applicability to nanosystems consisting of thousands of atoms, realized as open-access codes linked to existing DFT-based software; (2) Establishing the relationship between the structure of adducts and SWCNTs and intrinsic excitonic and spin properties of defect states for guiding novel synthetic strategies and experimental probes of chemically functionalized SWCNTs as near-IR emitting materials; (3) Generating virtual libraries of hypothetical functionalized SWCNTs for virtual screening of their chemical structures and optical properties, leveraging new functionalities of SWCNTs; (4) Offering a unique experience for NDSU graduate students that prepared them for future scientific careers related to materials modeling and big data processing. These results were summarized in 12 published journal papers and 3 recently submitted papers. One of a key finding is that the position of defect sites on the SWCNT surface primarily drives the emission redshift (up to 100 meV), while the polarity of the defect-inducing molecules has a much smaller effect (~10 meV). However, the electron-donating or withdrawing properties of a molecule influence selecting reactivity of defect sites. These insights important for optimizing synthetic protocols for desired emissions in SWCNTs. We also revealed that the interaction between two defects at various positions on the SWCNT enhances the redshift and optical activity of states, favoring strong near-IR emission. This suggests that manipulations in defect concentrations is a promising strategy for controlling efficient emission. Mostly important, the defect position was found controllable by the spin states of photoexcited intermediates: Excited aromatic molecules form ortho defects with SWCNTs at their singlet states in the presence of oxygen, while oxygen-free conditions favor para defects via the triplet-state mechanism. Additionally, a heat-activated [2+2] cycloaddition reaction facilitates divalent defect formation with fewer bonding positions that narrows emission bands. These groundbreaking findings have been experimentally validated and significantly advance our understanding of defect chemistry in SWCNTs. Using a novel encoding technique and 3D-MoRSE descriptors, we developed highly accurate ML/QSAR models to predict both the 3D structure and optical properties of SWCNTs with chemical defects. This model enabled the creation of a virtual library of 125,556 structures, providing new insights into the relationship between SWCNT-defect structure and emission.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Fabrication of single color centers in sub-50 nm nanodiamonds using ion implantation

Diamond color centers have been widely studied in the field of quantum optics. The negatively charged silicon vacancy (SiV – ) center exhibits a narrow emission linewidth at the wavelength of 738 nm, a high Debye–Waller factor, and unique spin properties, making it a promising emitter for quantum information technologies, biological imaging, and sensing. In particular, nanodiamond (ND)-based SiV – centers can be heterogeneously integrated with plasmonic and photonic nanostructures and serve as in vivo biomarkers and intracellular thermometers. Out of all methods to produce NDs with SiV – centers, ion implantation offers the unique potential to create controllable numbers of color centers in preselected individual NDs. However, the formation of single color centers in NDs with this technique has not been realized. We report the creation of single SiV– centers featuring stable high-purity single-photon emission through Si implantation into NDs with an average size of ~20 nm. We observe room temperature emission, with zero-phonon line wavelengths in the range of 730–800 nm and linewidths below 10 nm. Our results offer new opportunities for the controlled production of group-IV diamond color centers with applications in quantum photonics, sensing, and biomedicine.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Towards non-blinking and photostable perovskite quantum dots

Surface defect-induced photoluminescence blinking and photodarkening are ubiquitous in lead halide perovskite quantum dots. Despite efforts to stabilize the surface by chemically engineering ligand binding moieties, blinking accompanied by photodegradation still poses barriers to implementing perovskite quantum dots in quantum emitters. To date, ligand tail engineering in the solid state has rarely been explored for perovskite quantum dots. We posit that attractive intermolecular interactions between low-steric ligand tails, such as π-π stacking, can promote the formation of a nearly epitaxial ligand layer that significantly reduces the quantum dot surface energy. Here, we show that single CsPbBr 3 quantum dots covered by stacked phenethylammonium ligands exhibit nearly non-blinking single photon emission with high purity (~98%) and extraordinary photostability (12 hours continuous operation and saturated excitations), allowing the determination of size-dependent exciton radiative rates and emission line widths of CsPbBr 3 quantum dots at the single particle level.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Programmable quantum emitter formation in silicon

Abstract Silicon-based quantum emitters are candidates for large-scale qubit integration due to their single-photon emission properties and potential for spin-photon interfaces with long spin coherence times. Here, we demonstrate local writing and erasing of selected light-emitting defects using femtosecond laser pulses in combination with hydrogen-based defect activation and passivation at a single center level. By choosing forming gas (N 2 /H 2 ) during thermal annealing of carbon-implanted silicon, we can select the formation of a series of hydrogen and carbon-related quantum emitters, including T and C i centers while passivating the more common G-centers. The C i center is a telecom S-band emitter with promising optical and spin properties that consists of a single interstitial carbon atom in the silicon lattice. Density functional theory calculations show that the C i center brightness is enhanced by several orders of magnitude in the presence of hydrogen. Fs-laser pulses locally affect the passivation or activation of quantum emitters with hydrogen for programmable formation of selected quantum emitters.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Optical Properties of Low‐Defect Large‐Area Hexagonal Boron Nitride for Quantum Applications

Intrinsic defects and their concentrations in hexagonal boron nitride (h-BN) play a key role in single-photon emission. In this study, the optical properties of large-area multilayer h-BN-on-sapphire grown by metal-organic chemical vapor deposition are explored. Based on the detailed spectroscopic characterization using both cathodoluminescence (CL) and photoluminescence (PL) measurements, the material is devoid of random single-point defects instead of a few clustered complex defects. The emission spectra of the measurements confirm a record-low-defect concentration of ≈10 4 cm −2 . Post-annealing, no significant changes are observed in the measured spectra and the defect concentrations remain unaltered. Through CL and PL spectroscopy, an optically active boron vacancy spin defect is identified and a novel complex defect combination arising from carbon impurities is revealed. This complex defect, previously unreported, signifies a unique aspect of the material. In these findings, the understanding of defect-induced optical properties in h-BN films is contributed, providing insights for potential applications in quantum information science.

42 ENGINEERING↗
DOE OSTI2023

Discretized hexagonal boron nitride quantum emitters and their chemical interconversion

Quantum emitters in two-dimensional hexagonal boron nitride (hBN) are of significant interest because of their unique photophysical properties, such as single-photon emission at room temperature, and promising applications in quantum computing and communications. The photoemission from hBN defects covers a wide range of emission energies but identifying and modulating the properties of specific emitters remain challenging due to uncontrolled formation of hBN defects. In this study, more than 2000 spectra are collected consisting of single, isolated zero-phonon lines (ZPLs) between 1.59 and 2.25 eV from diverse sample types. Most of ZPLs are organized into seven discretized emission energies. All emitters exhibit a range of lifetimes from 1 to 6 ns, and phonon sidebands offset by the dominant lattice phonon in hBN near 1370 cm -1 . Two chemical processing schemes are developed based on water and boric acid etching that generate or preferentially interconvert specific emitters, respectively. The identification and chemical interconversion of these discretized emitters should significantly advance the understanding of solid-state chemistry and photophysics of hBN quantum emission.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Tuning spin–orbit coupling in (6,5) single-walled carbon nanotube doped with sp 3 defects

Single-walled carbon nanotubes (SWCNTs) containing sp 3 defects are a promising class of optoelectronic materials with bright photoluminescence and demonstrated single-photon emission. Using density functional theory simulations, complemented by measurements, we investigate the electronic structure of a series of quantum defects attached to (6,5) SWCNT with the goal of tuning the spin–orbit coupling by introduction of a heavy atom in the defect structure. We characterize the ground state electronic and spin properties of four synthesized and three potential defects on the tube and find that all of the synthesized defects considered introduce a localized midgap defect-centered state containing a single electron, ≈0.2–0.3 eV above the valence band. The spin density is located at the sp 3 defect site with negligible spin–orbit coupling even with the presence of a Pd atom. Three additional functional groups were tested via computation to increase spin localization near the metal, thereby increasing spin–orbit coupling. We predict that only the chlorodiphosphanepalladium(II)– [Cl(PH 3 ) 2 Pd(II)–] defect results in increased spin–orbit splitting of the defect state and the conduction band associated with the pristine-like SWCNT, a measure of the spin–orbit coupling of excited state transitions. This study suggests that for unpassivated sp 3 defects in (6,5) SWCNT, forming a direct bond between a heavy atom and the sp 3 carbon allows for tuning of spin–orbit coupling.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

The role of chalcogen vacancies for atomic defect emission in MoS 2

For two-dimensional (2D) layered semiconductors, control over atomic defects and understanding of their electronic and optical functionality represent major challenges towards developing a mature semiconductor technology using such materials. Here, we correlate generation, optical spectroscopy, atomic resolution imaging, and ab initio theory of chalcogen vacancies in monolayer MoS 2 . Chalcogen vacancies are selectively generated by in-vacuo annealing, but also focused ion beam exposure. The defect generation rate, atomic imaging and the optical signatures support this claim. We discriminate the narrow linewidth photoluminescence signatures of vacancies, resulting predominantly from localized defect orbitals, from broad luminescence features in the same spectral range, resulting from adsorbates. Vacancies can be patterned with a precision below 10 nm by ion beams, show single photon emission, and open the possibility for advanced defect engineering of 2D semiconductors at the ultimate scale.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ligand Controls Excited Charge Carrier Dynamics in Metal-Rich CdSe Quantum Dots: Computational Insights

Small metal-rich semiconducting quantum dots (QDs) are promising for solid-state lighting and single-photon emission due to their highly tunable yet narrow emission line widths. Nonetheless, the anionic ligands commonly employed to passivate these QDs exert a substantial influence on the optoelectronic characteristics, primarily owing to strong electron–phonon interactions. In this work, we combine time-domain density functional theory and nonadiabatic molecular dynamics to investigate the excited charge carrier dynamics of Cd 28 Se 17 X 22 QDs (X = HCOO – , OH – , Cl – , and SH – ) at ambient conditions. These chemically distinct but regularly used molecular groups influence the dynamic surface-ligand interfacial interactions in Cd-rich QDs, drastically modifying their vibrational characteristics. The strong electron–phonon coupling leads to substantial transient variations at the band edge states. The strength of these interactions closely depends on the physicochemical characteristics of passivating ligands. Consequently, the ligands largely control the nonradiative recombination rates and emission characteristics in these QDs. Our simulations indicate that Cd 28 Se 17 (OH) 22 has the fastest nonradiative recombination rate due to the strongest electron–phonon interactions. Conversely, QDs passivated with thiolate or chloride exhibit considerably longer carrier lifetimes and suppressed nonradiative processes. The ligand-controlled electron–phonon interactions further give rise to the broadest and narrowest intrinsic optical line widths for OH and Cl-passivated single QDs, respectively. Finally, obtained computational insights lay the groundwork for designing appropriate passivating ligands on metal-rich QDs, making them suitable for a wide range of applications, from blue LEDs to quantum emitters.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Towards the Stable Chelation of Radioantimony(V) for Targeted Auger Theranostics

Abstract Antimony‐119 ( 119 Sb) is one of the most attractive Auger‐electron emitters identified to date, but it remains practically unexplored for targeted radiotherapy because no chelators have been identified to stably bind this metalloid in vivo. In a departure from current studies focused on chelator development for Sb(III), we explore the chelation chemistry of Sb(V) using the tris‐catecholate ligand TREN‐CAM. Through a combination of radiolabeling, spectroscopic, solid‐state, and computational studies, the radiochemistry and structural chemistry of TREN‐CAM with 1XX/nat Sb(V) were established. The resulting [ 1XX Sb]Sb–TREN‐CAM complex remained intact for several days in human serum, signifying high stability under biological conditions. Finally, the first in vivo single photon emission computed tomography and positron emission tomography imaging studies were carried out using 117 Sb, the diagnostic analogue of 119 Sb. These studies revealed marked differences in the uptake and distribution of activity in mice administered unchelated [ 117 Sb]Sb(OH) 6 – versus [ 117 Sb]Sb–TREN‐CAM, suggesting that 117 Sb is largely retained by TREN‐CAM over the time course of the study. Collectively, these findings demonstrate the most physiologically stable complex of no‐carrier‐added 1XX Sb yet reported, offering new promise for the clinical implementation of radioantimony in nuclear medicine. Our results also establish the feasibility of 117 Sb as an elementally matched partner to 119 Sb for theranostic applications.

Olson, Aeli P. [Department of Medical Physics Univ↗
DOE OSTI2025

Towards the Stable Chelation of Radioantimony(V) for Targeted Auger Theranostics

Antimony-119 ( 119 Sb) is one of the most attractive Auger-electron emitters identified to date, but it remains practically unexplored for targeted radiotherapy because no chelators have been identified to stably bind this metalloid in vivo. In a departure from current studies focused on chelator development for Sb(III), we explore the chelation chemistry of Sb(V) using the tris-catecholate ligand TREN-CAM. Through a combination of radiolabeling, spectroscopic, solid-state, and computational studies, the radiochemistry and structural chemistry of TREN-CAM with 1XX/nat Sb(V) were established. The resulting [ 1XX Sb]Sb–TREN-CAM complex remained intact for several days in human serum, signifying high stability under biological conditions. Finally, the first in vivo single photon emission computed tomography and positron emission tomography imaging studies were carried out using 117 Sb, the diagnostic analogue of 119 Sb. These studies revealed marked differences in the uptake and distribution of activity in mice administered unchelated [ 117 Sb]Sb(OH) 6 – versus [ 117 Sb]Sb–TREN-CAM, suggesting that 117 Sb is largely retained by TREN-CAM over the time course of the study. Collectively, these findings demonstrate the most physiologically stable complex of no-carrier-added 1XX Sb yet reported, offering new promise for the clinical implementation of radioantimony in nuclear medicine. In conclusion, our results also establish the feasibility of 117 Sb as an elementally matched partner to 119 Sb for theranostic applications.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2021

Evaluation of a Variable-Aperture Full-Ring SPECT System using Large-Area Pixelated CZT Modules: A Simulation Study for Brain SPECT Applications

Single photon emission computed tomography (SPECT) scanner using cadmium zinc telluride (CZT) offers improved imaging capability over conventional NaI (Tl)-based SPECT scanner. We aim to demonstrate a full-ring SPECT system design with eight large-area CZT detectors that can be used for a broad spectrum of SPECT radiopharmaceuticals and provides higher sensitivity and better spatial resolution than those of conventional NaI (Tl)-based gamma cameras. A newly-designed full-ring SPECT system is composed of 8 large-area CZT cameras (128 mm × 179.2 mm effective area) that can be independently swiveled around their own axes of rotation independently and can have radial motion for varying aperture sizes that can be adapted to different sizes of imaging volume. Extended projection data were generated by conjoining projections of two adjacent detectors to overcome the limited field-of-view (FOV) by each CZT camera. Using Monte Carlo simulations, we evaluated this new system design with digital phantoms including a Derenzo hot-rod phantom and a Zubal brain phantom. Comparison of performance metrics such as spatial resolution, sensitivity, contrast-to-noise ratio (CNR), and contrast-recovery ratio were made between our design and a conventional SPECT scanner. The proposed scanner could result in up to about 3 times faster in acquisition time over conventional scan time at same acquisition time per step. The spatial resolution of our proposed scanner was similar or better to that of the conventional scanner, and there was significant performance improvement over the conventional scanner particularly in sensitivity (approximately 4 times). Overall, we successfully reconstructed the phantom image for both 99 mTc-based perfusion and 123 I-based dopamine transporter (DaT) brain studies simulated for our new design. In particular, the striatal/background contrast-recovery ratio in 3-to-1 reference ratio was over the 0.8 for the 123 I-based DaT study. In conclusion, we demonstrated the potential of our new full-ring CZT SPECT design, showing improved performance metrics such as improved system sensitivity and CNR while maintaining other important imaging parameters such as spatial resolution.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Simulation studies of a full-ring, CZT SPECT system for whole-body imaging of 99m Tc and 177 Lu

Single photon emission computed tomography (SPECT) is an imaging modality that has demonstrated its utility in a number of clinical indications. Despite this progress, a high sensitivity, high spatial resolution, multi-tracer SPECT with a large field of view suitable for whole-body imaging of a broad range of radiotracers for theranostics is not available. With the goal of filling this technological gap, we have designed a cadmium zinc telluride (CZT) full-ring SPECT scanner instrumented with a broad-energy tungsten collimator. The final purpose is to provide a multi-tracer solution for brain and whole-body imaging. Our static SPECT does not rely on the dual- and the triple-head rotational SPECT standard paradigm, enabling a larger effective area in each scan to increase the sensitivity. We provide a demonstration of the performance of our design using a realistic model of our detector with simulated body-sized phantoms filled with 99m Tc and 177 Lu. Our SPECT design can resolve 7.9 mm rods for 99m Tc (140 keV) and 9.5 mm for 177 Lu (208 keV) in a hot-rod Derenzo phantom with a 3-min exposure and reach an image contrast of 78% for 99m Tc and 57% for 177 Lu using the NEMA IQ phantom with a 6-min exposure. Our modified scatter correction shows an improved contrast-recovery ratio compared to a standard correction. In this paper, we demonstrate the good performance of our design for whole-body imaging purposes. This adds to our previous demonstration of improved qualitative and quantitative 99m Tc imaging of brain perfusion and 123 I imaging of dopamine transport with respect to state-of-the-art NaI dual-head cameras. We show that our design provides similar IQ and contrast to the commercial full-ring SPECT VERITON for 99m Tc. Regarding 177 Lu imaging of the 208 keV emissions, our design provides similar contrast to that of other state-of-the-art SPECTs with a significant reduction in exposure. In conclusion, the high sensitivity and extended energy range up to 250 keV makes our SPECT design a promising alternative for clinical imaging and theranostics of emerging radionuclides.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

In Situ Ion Counting for Improved Implanted Ion Error Rate and Silicon Vacancy Yield Uncertainty

An in situ counted ion implantation experiment improving the error on the number of ions required to form a single optically active silicon vacancy (SiV) defect in diamond 7-fold compared to timed implantation is presented. Here, traditional timed implantation relies on a beam current measurement followed by implantation with a preset pulse duration. It is dominated by Poisson statistics, resulting in large errors for low ion numbers. Instead, our in situ detection, measuring the ion number arriving at the substrate, results in a 2-fold improvement of the error on the ion number required to generate a single SiV compared to timed implantation. Through postimplantation analysis, the error is improved 7-fold compared to timed implantation. SiVs are detected by photoluminescence spectroscopy, and the yield of 2.98% is calculated through the photoluminescence count rate. Hanbury–Brown–Twiss interferometry is performed on locations potentially hosting single-photon emitters, confirming that 82% of the locations exhibit single photon emission statistics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Strain-Induced Growth of Twisted Bilayers during the Coalescence of Monolayer MoS 2 Crystals

Tailoring the grain boundaries (GBs) and twist angles between two-dimensional (2D) crystals are two crucial synthetic challenges to deterministically enable envisioned applications such as moiré excitons, emerging magnetism, or single-photon emission. Here, we reveal how twisted 2D bilayers can be synthesized from the collision and coalescence of two growing monolayer MoS 2 crystals during chemical vapor deposition. The twisted bilayer (TB) moiré angles are found to preserve the misorientation angle (θ) of the colliding crystals. The shapes of the TB regions are rationalized by a kink propagation model that predicts the GB formed by the coalescing crystals. Optical spectroscopy measurements reveal a θ-dependent long-range strain in crystals with stitched grain boundaries and a sharp (θ > 20°) threshold for the appearance of TBs, which relieves this strain. Reactive molecular dynamics simulations explain this strain from the continued growth of the crystals during coalescence due to the insertion of atoms at unsaturated defects along the GB, a process that self-terminates when the defects become saturated. The simulations also reproduce atomic-resolution electron microscopy observations of faceting along the GB, which is shown to arise from the growth-induced long-range strain. These facets align with the axes of the colliding crystals to provide favorable nucleation sites for second-layer growth of a TB with twist angles that preserve the misorientation angle θ. This interplay between strain generation and aligned nucleation provides a synthetic pathway for the growth of TBs with deterministic angles.

2D materials↗
DOE OSTI2025

Correlated Lattice Fluctuations in CsPbBr 3 Quantum Dots Give Rise to Long-Lived Electronic Coherence

Electronic coherence is central to numerous areas of science, from quantum biology to quantum materials. In quantum materials, lead-halide perovskite (LHP) quantum dots (QDs) have been shown to support electronic coherence through observation of coherent single-photon emission and superfluorescence arising from spatial coherence at low temperatures. In contrast, direct measurement of temporal coherence between exciton states has been lacking. Here, we employ coherent multi-dimensional spectroscopy to observe an electronic coherence between exciton states in CsPbBr 3 QDs that is long-lived at room temperature, surviving nearly three times longer than the electronic dephasing time. This observation of a long-lived electronic coherence at room temperature points to nearly perfectly correlated lattice fluctuations for each excitonic state in the superposition. In conclusion, these experiments reveal that the properties of LHP QDs extend to lattice dynamics that give rise to correlated fluctuations in the basis exciton states, a process that may next be optimized by design.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Quantum Emitters Induced by High Pressure and UV Laser Irradiation in Multilayer GaSe

In this work, we report on defect generation in multilayer GaSe through hydrostatic pressure quenching and UV laser irradiation. The Raman line width from the UV 266 nm irradiated sample is much wider than that in pressure-quenched GaSe, corresponding to a wider defect energy distribution range in the former sample than the latter. After quenching from 11.2 GPa, three photoluminescence (PL) peaks from defect states are observed at 657, 681, and 695 nm at a low temperature of 93 K. Defect-related peaks at 649, 694, 750, and 774 nm also appear in low-temperature PL spectra after UV laser irradiation, with a nonmonotonous intensity dependence on irradiation duration. There are common features in defects produced by these two methods: the PL peaks with the lowest energy are sharp, and their PL intensities increase linearly with the excitation laser power and saturate above a certain excitation laser power. These two features are similar to those in defects for single-photon emission (SPE) in other 2D materials at even lower temperatures. Fluorescence lifetime imaging shows distinguished short (2.3 ns) and long (75.6 nm) lifetimes of the 695 nm PL line in pressure-quenched GaSe. The density functional theory predicts defect energy levels related to Se vacancy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Production and Purification of Terbium-155 Using Natural Gadolinium Targets

Terbium-155 (t 1/2 = 5.32 days) is one of four medically relevant radioisotopes of terbium. It is of interest to the field as a suitable diagnostic counterpart for therapeutic radiolanthanides, as its decay scheme includes γ-rays that are suitable for single photon emission computed tomography (SPECT) imaging. Additionally, 155 Tb has an Auger electron (AE) yield that is viable for AE therapy. There are several direct and indirect production routes that can produce 155 Tb. Two possible direct routes include proton irradiation on gadolinium targets via 155 Gd(p,n) 155 Tb and 156 Gd(p,2n) 155 Tb. The 155 Gd(p,n) 155 Tb reaction is accessible at incident proton beam energies of ∼10 MeV, whereas the 156 Gd(p,2n) 155 Tb nuclear reaction requires ∼18 MeV. This study aims to investigate the production of 155 Tb from natGd through the nat Gd(p,x) nuclear reaction, wherein both (p,n) and (p,2n) reactions were leveraged, and the purification using a three-column ion chromatography method. Using this system, recoveries of radioterbium of up to 97% were achieved in addition to high recoveries of the Gd target material, illustrating the suitability of this technique for enriched targets.

36 MATERIALS SCIENCE↗