Award Abstract # 1806279
New Lanthanide-Containing Silicate Fluoride Scintillators for Radiation Detection

NSF Org: DMR
Division Of Materials Research
Recipient: UNIVERSITY OF SOUTH CAROLINA
Initial Amendment Date: April 11, 2018
Latest Amendment Date: April 11, 2018
Award Number: 1806279
Award Instrument: Standard Grant
Program Manager: Robert Meulenberg
rmeulenb@nsf.gov
 (703)292-2499
DMR
 Division Of Materials Research
MPS
 Directorate for Mathematical and Physical Sciences
Start Date: June 1, 2018
End Date: May 31, 2022 (Estimated)
Total Intended Award Amount: $499,773.00
Total Awarded Amount to Date: $499,773.00
Funds Obligated to Date: FY 2018 = $499,773.00
History of Investigator:
  • Hans-Conrad zur Loye (Principal Investigator)
    zurloye@mailbox.sc.edu
Recipient Sponsored Research Office: University of South Carolina at Columbia
1600 HAMPTON ST
COLUMBIA
SC  US  29208-3403
(803)777-7093
Sponsor Congressional District: 06
Primary Place of Performance: University of South Carolina at Columbia
1600 Hampton Street
Columbia
SC  US  29208-0001
Primary Place of Performance
Congressional District:
06
Unique Entity Identifier (UEI): J22LNTMEDP73
Parent UEI: Q93ZDA59ZAR5
NSF Program(s): SOLID STATE & MATERIALS CHEMIS
Primary Program Source: 01001819DB NSF RESEARCH & RELATED ACTIVIT
Program Reference Code(s): 9150
Program Element Code(s): 176200
Award Agency Code: 4900
Fund Agency Code: 4900
Assistance Listing Number(s): 47.049

ABSTRACT

Non-Technical

Border protection agencies, such as Homeland Security, must be able to detect rogue radiation sources, for example dirty bombs, before they are transported into the country. A pressing need exists for large quantities of materials know as scintillators, which are used in portable detection devices. Scintillators are materials that emit visible light when exposed to radiation, and the better the scintillator, the brighter the light and the smaller the amount of radioactive material that can be detected. This research, funded by the Solid State and Materials Chemistry Program in the Division of Materials Research at NSF, involves the fundamental aspects of crystal growth of improved scintillating materials and thereby advances the field of radiation detection. In addition, this research project provides a valuable educational experience for graduate and undergraduate students. Conducting this research trains students in the art of crystal growth and teaches them the concept of experimental design and methods optimization. Overall, this research contributes to the education and training of a wide range of individuals, including those from underrepresented groups, in the area of solid state and materials chemistry.

Technical

One area where the development of new functional materials can have a tremendous impact is homeland security. There exists a pressing need for large quantities of efficient scintillating materials for improved radiation detection. This research focuses on the synthesis of new neutron, X-ray, and gamma-ray activated scintillating oxides. Fluorine in mixed anion phases has been identified as one element that plays a crucial role in the intensity of fluorescence, and it has been demonstrated that fluorine can also increase the scintillation efficiency of rare earth silicates. Specifically, it is known that luminescent oxyfluorides in which the fluorine anions are located in LnOxFy polyhedra, such as in Cs3LnSi4O10F2 (Ln = Eu, Tb), a recently discovered brightly scintillating material, can exhibit scintillation as bright as Lu2SiO5:Ce3+. The targeted crystal growth of fluorine containing mixed-anion phases takes advantage of a recently developed enhanced flux growth technique that is known to yield crystals of oxyfluorides and salt-inclusion silicates. To better understand the processes involved in the formation of mixed anion phases in the various flux environments that are used for synthesis of complex oxide single crystals, in-situ neutron diffraction experiments are carried out to identify the optimal growth conditions for preparing new scintillators in the laboratory as well as to transform crystal growth from an empirical to a deliberate process. Additionally, this research contributes to the education and training of a wide range of individuals, including those from underrepresented groups, in the area of solid state and materials chemistry, for example through collaboration with Claflin University, an HBCU institution.

This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

PUBLICATIONS PRODUCED AS A RESULT OF THIS RESEARCH

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Aslani, Ceren Kutahyali and Klepov, Vladislav V. and Aslani, Mahmoud A. and Loye, Hans-Conrad zur "Hydrothermal Synthesis of New Iodates Ln 2 (IO 3 ) 3 (IO 4 ) (Ln = La, Nd, Pr) Containing the Tetraoxoiodate(V) Anion: Creation of Luminescence Properties by Doping with Eu, Dy, and Tb" Crystal Growth & Design , v.21 , 2021 https://doi.org/10.1021/acs.cgd.1c00545 Citation Details
Aslani, Ceren Kutahyali and Klepov, Vladislav V. and zur Loye, Hans-Conrad "Hydrothermal synthesis of new mixed-oxoanion materials: Rare earth iodate sulfates Sm(IO3)(SO4) and Ln2(IO3)3(SO4)OH·3H2O (Ln = Sm, Eu, Dy)" Solid State Sciences , v.129 , 2022 https://doi.org/10.1016/j.solidstatesciences.2022.106918 Citation Details
Ayer, Gyanendra B. and Klepov, Vladislav V. and Pace, Kristen A. and zur Loye, Hans-Conrad "Quaternary cerium( iv ) containing fluorides exhibiting Ce 3 F 16 sheets and Ce 6 F 30 frameworks" Dalton Transactions , v.49 , 2020 https://doi.org/10.1039/d0dt00616e Citation Details
Ayer, Gyanendra B. and Klepov, Vladislav V. and Smith, Mark D. and Hu, Ming and Yang, Zhonghua and Martin, Corey R. and Morrison, Gregory and zur Loye, Hans-Conrad "BaWO 2 F 4 : a mixed anion X-ray scintillator with excellent photoluminescence quantum efficiency" Dalton Transactions , v.49 , 2020 https://doi.org/10.1039/D0DT02184A Citation Details
Ayer, Gyanendra B. and Klepov, Vladislav V. and Smith, Mark D. and zur Loye, Hans-Conrad "Mild Hydrothermal Synthesis of the Complex Hafnium-Containing Fluorides Cs 2 [M(H 2 O) 6 ][Hf 2 F 12 ] (M = Ni, Co, Zn), CuHfF 6 (H 2 O) 4 , and Cs 2 Hf Inorganic Chemistry , v.58 , 2019 10.1021/acs.inorgchem.9b01958 Citation Details
Ayer, Gyanendra B. and Morrison, Gregory and Smith, Mark D. and Jacobsohn, Luiz G. and zur Loye, Hans-Conrad "Luminescence and Scintillation of [Nb 2 O 2 F 9 ] 3 -Dimer-Containing OxideFluorides: Cs 10 (Nb 2 O 2 F 9 ) 3 F, Cs 9.4 K 0.6 (Nb Inorganic Chemistry , v.61 , 2022 https://doi.org/10.1021/acs.inorgchem.1c03787 Citation Details
Ayer, Gyanendra B. and Smith, Mark D. and Jacobsohn, Luiz G. and Morrison, Gregory and Tisdale, Hunter B. and Breton, Logan S. and Zhang, Weiguo and Halasyamani, P. Shiv and zur Loye, Hans-Conrad "Synthesis of Hydrated Ternary Lanthanide-Containing Chlorides Exhibiting X-ray Scintillation and Luminescence" Inorganic Chemistry , v.60 , 2021 https://doi.org/10.1021/acs.inorgchem.1c02004 Citation Details
Carone, Darren and Jacobsohn, Luiz G. and Breton, Logan S. and zur Loye, Hans-Conrad "Synthesis, structure, and scintillation of Rb4Ta2Si8O23" Solid State Sciences , v.127 , 2022 https://doi.org/10.1016/j.solidstatesciences.2022.106861 Citation Details
Carone, Darren and Klepov, Vladislav V. and Smith, Mark D. and zur Loye, Hans-Conrad "Flux Crystal Growth of Lanthanide Tungsten Oxychlorides, La 8.64 W 6 O 30.45 Cl, Ce 8.64 W 5.74 O 30 Cl, and Ln 8.33 W 6 O 30 Cl (Ln = Pr, Nd): Structural S" Inorganic Chemistry , v.58 , 2019 10.1021/acs.inorgchem.9b03015 Citation Details
Carone, Darren and Morrison, Gregory and Smith, Mark D. and zur Loye, Hans-Conrad "Crystal Growth of New Germanate Framework Structures: Impact of the Presence of Square Planar Copper Species and Mixed Ge/Mn Sites on the Overall Structures of Rb 2 Cu 3 Ge 5 O 14 , Cs 2 Cu 3 Crystal Growth & Design , v.22 , 2022 https://doi.org/10.1021/acs.cgd.2c00133 Citation Details
Carone, Darren and Usman, Mohammad and Klepov, Vladislav V. and Smith, Mark D. and Kocevski, Vancho and Besmann, Theodore M. and zur Loye, Hans-Conrad "New germanate and mixed cobalt germanate salt inclusion materials: [(Rb 6 F)(Rb 4 F)][Ge 14 O 32 ] and [(Rb 6 F)(Rb 3.1 Co 0.9 F 0.96 )][Co 3.8 Ge 10.2" CrystEngComm , v.22 , 2020 https://doi.org/10.1039/D0CE01099E Citation Details
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PROJECT OUTCOMES REPORT

Disclaimer

This Project Outcomes Report for the General Public is displayed verbatim as submitted by the Principal Investigator (PI) for this award. Any opinions, findings, and conclusions or recommendations expressed in this Report are those of the PI and do not necessarily reflect the views of the National Science Foundation; NSF has not approved or endorsed its content.

The discovery of optically active materials and the ability to grow them as single crystals is at the core of modern materials research and encompasses a broad range of both theoretical and experimental activities. One area in which optically active materials promise to play an integral role is homeland security, where there exists a pressing need for large quantities of efficient and inexpensive scintillator materials for improved radiation detection.  Scintillators, materials that can both absorb high energy radiation and convert this energy into excited states in active luminescence centers for light emission, have many uses ranging from X-ray photography, to X-ray phosphors, to PET and CT scanners, X-ray and neutron detectors, and, more recently, by homeland security for improved nuclear detection systems. The discovery of these materials will help make America a safer place. Meeting this need constitutes an important aspect of new materials development, where one ongoing challenge is the targeted discovery of new (or modified) strongly scintillating materials.  Numerous approaches were taken including 1) the preparation of single crystals of novel chemical compositions with specific structural motifs known to favor scintillation and 2) the modification of existing materials to enhance the desired scintillating properties via our extensive understanding of crystal chemistry, i.e., structure-composition-property relationships, as well as fine tuning of dopant concentration. This research created almost 50 new materials, many of which luminesced and scintillated.  We expect that the impact of this research will reach far beyond scintillation materials and potentially transform how we will approach crystal growth and new material discovery in the future.

 

The synthesis and characterization of new materials that resulted from this research is one important component of, and one driving force behind, solid-state chemistry research.  The use high temperature solutions and mild hydrothermal methods to grow crystals of the desired scintillating materials have resulted in new materials that can advance the field of radiation detection, while at the same time it provided a valuable educational experience for graduate and undergraduate students. Several graduate students were trained in the science of crystal growth and educated in experimental design and methods optimization. Most importantly, their involvement in this research project taught them fundamental concepts concerning oxide materials and crystal growth, crystal structure determination, and general physical property measurements, including luminescence and scintillation. This research has contributed to the education of a wide range of individuals, including those from underrepresented groups.

 

 


Last Modified: 06/02/2022
Modified by: Hans-Conrad Zur Loye

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