Band-gap and band-edge engineering of multicomponent garnet scintillators from first principles

Yadav, Satyesh K.; Uberuaga, Blas P.; Nikl, Martin; Jiang, Chao; Stanek, Christopher R.

doi:10.1103/PhysRevApplied.4.054012

Title: Band-gap and band-edge engineering of multicomponent garnet scintillators from first principles

Journal Article · Tue Nov 24 00:00:00 EST 2015 · Physical Review Applied

DOI:https://doi.org/10.1103/PhysRevApplied.4.054012· OSTI ID:1248741

Yadav, Satyesh K. ^[1]; Uberuaga, Blas P. ^[1]; Nikl, Martin ^[2]; Jiang, Chao ^[3]; Stanek, Christopher R. ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Academy of Sciences of the Czech Republic, Prague (Czech Republic)
Thermo-Calc Software Inc., Pittsburgh, PA (United States)

Complex doping schemes in R₃Al₅O₁₂ (where R is the rare-earth element) garnet compounds have recently led to pronounced improvements in scintillator performance. Specifically, by admixing lutetium and yttrium aluminate garnets with gallium and gadolinium, the band gap is altered in a manner that facilitates the removal of deleterious electron trapping associated with cation antisite defects. Here, we expand upon this initial work to systematically investigate the effect of substitutional admixing on the energy levels of band edges. Density-functional theory and hybrid density-functional theory (HDFT) are used to survey potential admixing candidates that modify either the conduction-band minimum (CBM) or valence-band maximum (VBM). We consider two sets of compositions based on Lu₃B₅O₁₂ where B is Al, Ga, In, As, and Sb, and R₃Al₅O₁₂, where R is Lu, Gd, Dy, and Er. We find that admixing with various R cations does not appreciably affect the band gap or band edges. In contrast, substituting Al with cations of dissimilar ionic radii has a profound impact on the band structure. We further show that certain dopants can be used to selectively modify only the CBM or the VBM. Specifically, Ga and In decrease the band gap by lowering the CBM, while As and Sb decrease the band gap by raising the VBM, the relative change in band gap is quantitatively validated by HDFT. These results demonstrate a powerful approach to quickly screen the impact of dopants on the electronic structure of scintillator compounds, identifying those dopants which alter the band edges in very specific ways to eliminate both electron and hole traps responsible for performance limitations. Furthermore, this approach should be broadly applicable for the optimization of electronic and optical performance for a wide range of compounds by tuning the VBM and CBM.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-06NA25396; P204/12/0805

OSTI ID:: 1248741

Alternate ID(s):: OSTI ID: 1227086

Report Number(s):: LA-UR-15-23403; PRAHB2

Journal Information:: Physical Review Applied, Vol. 4, Issue 5; ISSN 2331-7019

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 57 works

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References (52)

Antisite defect-free Lu3(GaxAl1−x)5O12:Pr scintillator Nikl, M.; Pejchal, J.; Mihokova, E. Applied Physics Letters, Vol. 88, Issue 14 https://doi.org/10.1063/1.2191741	journal	April 2006
Composition Engineering in Cerium-Doped (Lu,Gd) ₃ (Ga,Al) ₅ O ₁₂ Single-Crystal Scintillators Kamada, Kei; Endo, Takanori; Tsutumi, Kousuke Crystal Growth & Design, Vol. 11, Issue 10 https://doi.org/10.1021/cg200694a	journal	October 2011
Transparent ceramic scintillators for gamma spectroscopy and radiography Cherepy, N. J.; Kuntz, J. D.; Seeley, Z. M. SPIE Optical Engineering + Applications, SPIE Proceedings https://doi.org/10.1117/12.862503	conference	August 2010
Nonradiative decay from 5d states of rare earths in crystals Weber, M. J. Solid State Communications, Vol. 12, Issue 7 https://doi.org/10.1016/0038-1098(73)90326-8	journal	April 1973
Atomistic computer simulations of yttrium iron garnet (YIG) as an approach to materials defect chemistry. I. Intrinsic defects Donnerberg, H.; Catlow, C. R. A. Journal of Physics: Condensed Matter, Vol. 5, Issue 18 https://doi.org/10.1088/0953-8984/5/18/017	journal	May 1993
A grid-based Bader analysis algorithm without lattice bias Tang, W.; Sanville, E.; Henkelman, G. Journal of Physics: Condensed Matter, Vol. 21, Issue 8 https://doi.org/10.1088/0953-8984/21/8/084204	journal	January 2009
Effect of codoping on scintillation and optical properties of a Ce-doped Gd ₃ Ga ₃ Al ₂ O ₁₂ scintillator Tyagi, Mohit; Meng, Fang; Koschan, Merry Journal of Physics D: Applied Physics, Vol. 46, Issue 47 https://doi.org/10.1088/0022-3727/46/47/475302	journal	October 2013
Luminescence and Luminescence Quenching in Gd ₃ (Ga,Al) ₅ O ₁₂ Scintillators Doped with Ce ³⁺ Ogiegło, Joanna M.; Katelnikovas, Arturas; Zych, Aleksander The Journal of Physical Chemistry A, Vol. 117, Issue 12 https://doi.org/10.1021/jp309572p	journal	March 2013
Controlling electronic structure through epitaxial strain in ZnSe/ZnTe nano-heterostructures Yadav, S. K.; Sharma, V.; Ramprasad, R. Journal of Applied Physics, Vol. 118, Issue 1 https://doi.org/10.1063/1.4923385	journal	July 2015
The effect of intrinsic defects on garnet scintillator performance Stanek, C. R.; McClellan, K. J.; Levy, M. R. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 579, Issue 1 https://doi.org/10.1016/j.nima.2007.04.006	journal	August 2007
LASER OSCILLATIONS IN Nd‐DOPED YTTRIUM ALUMINUM, YTTRIUM GALLIUM AND GADOLINIUM GARNETS Geusic, J. E.; Marcos, H. M.; Van Uitert, L. G. Applied Physics Letters, Vol. 4, Issue 10 https://doi.org/10.1063/1.1753928	journal	May 1964
X-ray and optical studies of ytterbium-doped gallium garnets Shirinyan, Grigory; Ovanesyan, Karine L.; Eganyan, Atom Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 537, Issue 1-2 https://doi.org/10.1016/j.nima.2004.07.252	journal	January 2005
Band offsets and optical bowings of chalcopyrites and Zn‐based II‐VI alloys Wei, Su‐Huai; Zunger, Alex Journal of Applied Physics, Vol. 78, Issue 6 https://doi.org/10.1063/1.359901	journal	September 1995
Theoretical calculations of heterojunction discontinuities in the Si/Ge system Van de Walle, Chris G.; Martin, Richard M. Physical Review B, Vol. 34, Issue 8 https://doi.org/10.1103/physrevb.34.5621	journal	October 1986
Single-crystalline films of Ce-doped YAG and LuAG phosphors: advantages over bulk crystals analogues Zorenko, Yu.; Gorbenko, V.; Konstankevych, I. Journal of Luminescence, Vol. 114, Issue 2 https://doi.org/10.1016/j.jlumin.2004.12.002	journal	August 2005
Properties of the YAG:Ce scintillator Moszyński, M.; Ludziejewski, T.; Wolski, D. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 345, Issue 3 https://doi.org/10.1016/0168-9002(94)90500-2	journal	July 1994
Development of LuAG-based scintillator crystals – A review Nikl, M.; Yoshikawa, A.; Kamada, K. Progress in Crystal Growth and Characterization of Materials, Vol. 59, Issue 2 https://doi.org/10.1016/j.pcrysgrow.2013.02.001	journal	June 2013
Energy transfer phenomena in the luminescence of wide band-gap scintillators Nikl, M. physica status solidi (a), Vol. 202, Issue 2 https://doi.org/10.1002/pssa.200460107	journal	January 2005
Studies of light yield as a function of temperature and low temperature thermoluminescence of Gd3Al2Ga3O12:Ce scintillator crystals Drozdowski, W.; Brylew, K.; Witkowski, M. E. Optical Materials, Vol. 36, Issue 10 https://doi.org/10.1016/j.optmat.2013.12.044	journal	August 2014
Characterization of GAGG:Ce scintillators with various Al-to-Ga ratio Sibczynski, Pawel; Iwanowska-Hanke, Joanna; Moszyński, Marek Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 772 https://doi.org/10.1016/j.nima.2014.10.041	journal	February 2015
The effect of Ga-doping on the defect chemistry of RE ₃ Al ₅ O ₁₂ garnets Stanek, C. R.; Jiang, C.; Yadav, S. K. physica status solidi (b), Vol. 250, Issue 2 https://doi.org/10.1002/pssb.201200524	journal	January 2013
Nanocrystalline lanthanide-doped Lu ₃ Ga ₅ O ₁₂ garnets: interesting materials for light-emitting devices Venkatramu, V.; Giarola, M.; Mariotto, G. Nanotechnology, Vol. 21, Issue 17 https://doi.org/10.1088/0957-4484/21/17/175703	journal	April 2010
Defects in yttrium aluminium perovskite and garnet crystals: atomistic study Kuklja, Maija M. Journal of Physics: Condensed Matter, Vol. 12, Issue 13 https://doi.org/10.1088/0953-8984/12/13/307	journal	March 2000
Bright White Upconversion Emission from Tm ³⁺ /Yb ³⁺ /Er ³⁺ -Doped Lu ₃ Ga ₅ O ₁₂ Nanocrystals Mahalingam, Venkataramanan; Mangiarini, Francesca; Vetrone, Fiorenzo The Journal of Physical Chemistry C, Vol. 112, Issue 46 https://doi.org/10.1021/jp8076479	journal	October 2008
Influence of the exchange screening parameter on the performance of screened hybrid functionals Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F. The Journal of Chemical Physics, Vol. 125, Issue 22 https://doi.org/10.1063/1.2404663	journal	December 2006
A NEW PHOSPHOR FOR FLYING‐SPOT CATHODE‐RAY TUBES FOR COLOR TELEVISION: YELLOW‐EMITTING Y ₃ Al ₅ O ₁₂ –Ce ³⁺ Blasse, G.; Bril, A. Applied Physics Letters, Vol. 11, Issue 2 https://doi.org/10.1063/1.1755025	journal	July 1967
Heterojunction band offset engineering Franciosi, A. Surface Science Reports, Vol. 25, Issue 1-4 https://doi.org/10.1016/0167-5729(95)00008-9	journal	January 1996
Characteristics of a Nonstoichiometric Gd _3+δ (Al,Ga) _5−δ O ₁₂ :Ce Garnet Scintillator Kanai, Tsuneyuki; Satoh, Makoto; Miura, Ichiro Journal of the American Ceramic Society, Vol. 91, Issue 2 https://doi.org/10.1111/j.1551-2916.2007.02123.x	journal	February 2008
Nuclear Quadrupole Resonance of Antimony in Ln3Sb5O12 Crystals Raevsky, A. M.; Gukalova, A. G.; Semin, G. K. Zeitschrift für Naturforschung A, Vol. 49, Issue 6 https://doi.org/10.1515/zna-1994-0605	journal	January 1994
Scintillation: mechanisms and new crystals Weber, M. J. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 527, Issue 1-2 https://doi.org/10.1016/j.nima.2004.03.009	journal	July 2004
Cathodoluminescent properties of nanocrystalline Lu3Ga5O12:Tb3+ phosphor for field emission display application Xu, X. G.; Chen, Jun; Deng, S. Z. Journal of Vacuum Science & Technology B, Nanotechnology and Microelectronics: Materials, Processing, Measurement, and Phenomena, Vol. 28, Issue 3 https://doi.org/10.1116/1.3392039	journal	May 2010
Band bowing and band alignment in InGaN alloys Moses, Poul Georg; Van de Walle, Chris G. Applied Physics Letters, Vol. 96, Issue 2 https://doi.org/10.1063/1.3291055	journal	January 2010
Disorder and Nonstoichiometry in Synthetic Garnets A ₃ B ₅ O ₁₂ (A = Y, Lu−La, B = Al, Fe, Ga). A Simulation Study Milanese, Chiara; Buscaglia, Vincenzo; Maglia, Filippo Chemistry of Materials, Vol. 16, Issue 7 https://doi.org/10.1021/cm031138u	journal	April 2004
Strain-assisted bandgap modulation in Zn based II-VI semiconductors Yadav, S. K.; Ramprasad, R. Applied Physics Letters, Vol. 100, Issue 24 https://doi.org/10.1063/1.4729153	journal	June 2012
The antisite LuAl defect-related trap in Lu3Al5O12:Ce single crystal Nikl, M.; Mihokova, E.; Pejchal, J. physica status solidi (b), Vol. 242, Issue 14 https://doi.org/10.1002/pssb.200541225	journal	November 2005
Scintillator-oriented combinatorial search in Ce-doped (Y,Gd)₃(Ga,Al)₅O₁₂ multicomponent garnet compounds Kamada, K.; Yanagida, T.; Pejchal, J. Journal of Physics D: Applied Physics, Vol. 44, Issue 50, Article No. 505104 https://doi.org/10.1088/0022-3727/44/50/505104	journal	December 2011
Understanding Photocatalytic Activity of S- and P-Doped TiO ₂ under Visible Light from First-Principles Yang, Kesong; Dai, Ying; Huang, Baibiao The Journal of Physical Chemistry C, Vol. 111, Issue 51 https://doi.org/10.1021/jp0756350	journal	December 2007
Scintillator Materials—Achievements, Opportunities, and Puzzles Nikl, M.; Mihokova, E.; Pejchal, J. IEEE Transactions on Nuclear Science, Vol. 55, Issue 3 https://doi.org/10.1109/TNS.2007.913480	journal	June 2008
Role of ${Ce}^{4 +}$ in the Scintillation Mechanism of Codoped ${Gd}_{3} {Ga}_{3} {Al}_{2} O_{12} ∶ Ce$ Wu, Yuntao; Meng, Fang; Li, Qi Physical Review Applied, Vol. 2, Issue 4 https://doi.org/10.1103/PhysRevApplied.2.044009	journal	October 2014
High-resolution optical spectroscopy of YAG:Nd: A test for structural and distribution models Lupei, V.; Lupei, A.; Tiseanu, C. Physical Review B, Vol. 51, Issue 1 https://doi.org/10.1103/PhysRevB.51.8	journal	January 1995
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides Shannon, R. D. Acta Crystallographica Section A, Vol. 32, Issue 5, p. 751-767 https://doi.org/10.1107/S0567739476001551	journal	September 1976
Band-gap engineering for removing shallow traps in rare-earth Lu $_{3}$ Al $_{5}$ O $_{12}$ garnet scintillators using Ga $^{3 +}$ doping Fasoli, M.; Vedda, A.; Nikl, M. Physical Review B, Vol. 84, Issue 8 https://doi.org/10.1103/PhysRevB.84.081102	journal	August 2011
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Special quasirandom structures Zunger, Alex; Wei, S.-H.; Ferreira, L. G. Physical Review Letters, Vol. 65, Issue 3, p. 353-356 https://doi.org/10.1103/PhysRevLett.65.353	journal	July 1990
Scintillation Efficiency Improvement by Mixed Crystal Use Gektin, Alexander V.; Belsky, Andrei N.; Vasil'ev, Andrey N. IEEE Transactions on Nuclear Science, Vol. 61, Issue 1 https://doi.org/10.1109/TNS.2013.2277883	journal	February 2014
Fundamental Limitations in the Performance of ${\rm Ce}^{3+}$–, ${\rm Pr}^{3+}$–, and ${\rm Eu}^{2+}$–Activated Scintillators Dorenbos, Pieter IEEE Transactions on Nuclear Science, Vol. 57, Issue 3 https://doi.org/10.1109/TNS.2009.2031140	journal	June 2010
The antisite LuAl defect-related trap in Lu3Al5O12:Ce single crystal Nikl, M.; Mihokova, E.; Pejchal, J. physica status solidi (b), Vol. 242, Issue 14 https://doi.org/10.1002/pssb.200590023	journal	November 2005
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect Tatemizo, Nobuyuki; Imada, Saki; Okahara, Kizuna Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-58835-5	journal	February 2020
An ultrasensitive molybdenum-based double-heterojunction phototransistor Zenodo https://doi.org/10.5281/zenodo.4835973	text	January 2021
Controlling Electronic Structure Through Epitaxial Strain in ZnSe/ZnTe Nano-heterostructures Yadav, Satyesh Kumar; Sharma, Vinit; Ramprasad, Rampi arXiv https://doi.org/10.48550/arxiv.1505.01217	text	January 2015

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Ultrafast Zn(Cd,Mg)O:Ga nanoscintillators with luminescence tunable by band gap modulation Procházková, Lenka; Čuba, Václav; Beitlerová, Alena Optics Express, Vol. 26, Issue 22 https://doi.org/10.1364/oe.26.029482	journal	January 2018
Evidence of Optically Stimulated Luminescence in Lu ₃ Al ₅ O ₁₂ :Ce Gallo, Salvatore; Veronese, Ivan; Vedda, Anna physica status solidi (a), Vol. 216, Issue 14 https://doi.org/10.1002/pssa.201900103	journal	April 2019
Excitation Transfer Engineering in Ce-Doped Oxide Crystalline Scintillators by Codoping with Alkali-Earth Ions Auffray, Etiennette; Augulis, Ramūnas; Fedorov, Andrei physica status solidi (a), Vol. 215, Issue 7 https://doi.org/10.1002/pssa.201700798	journal	February 2018
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