Electronic structure descriptor for the discovery of narrow-band red-emitting phosphors

Wang, Zhenbin; Chu, Iek -Heng; Zhou, Fei; Ong, Shyue Ping

doi:10.1021/acs.chemmater.6b01496

Title: Electronic structure descriptor for the discovery of narrow-band red-emitting phosphors

Journal Article · Mon May 09 00:00:00 EDT 2016 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.6b01496· OSTI ID:1259764

Wang, Zhenbin ^[1]; Chu, Iek -Heng ^[1]; Zhou, Fei ^[2]; Ong, Shyue Ping ^[1]

Univ. of California San Diego, La Jolla, CA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Narrow-band red-emitting phosphors are a critical component of phosphor-converted light-emitting diodes for highly efficient illumination-grade lighting. In this work, we report the discovery of a quantitative descriptor for narrow-band Eu²⁺-activated emission identified through a comparison of the electronic structures of known narrow-band and broad-band phosphors. We find that a narrow emission bandwidth is characterized by a large splitting of more than 0.1 eV between the two highest Eu²⁺ 4f⁷ bands. By incorporating this descriptor in a high-throughput first-principles screening of 2259 nitride compounds, we identify five promising new nitride hosts for Eu²⁺-activated red-emitting phosphors that are predicted to exhibit good chemical stability, thermal quenching resistance, and quantum efficiency, as well as narrow-band emission. Lastly, our findings provide important insights into the emission characteristics of rare-earth activators in phosphor hosts and a general strategy to the discovery of phosphors with a desired emission peak and bandwidth.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1259764

Report Number(s):: LLNL-JRNL-692398

Journal Information:: Chemistry of Materials, Vol. 28, Issue 11; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 68 works

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References (41)

Luminescence Properties of a Red Phosphor, CaAlSiN[sub 3]:Eu[sup 2+], for White Light-Emitting Diodes Uheda, Kyota; Hirosaki, Naoto; Yamamoto, Yoshinobu Electrochemical and Solid-State Letters, Vol. 9, Issue 4 https://doi.org/10.1149/1.2173192	journal	January 2006
Preparation of CaAlSiN ₃ :Eu ²⁺ Phosphors by the Self-Propagating High-Temperature Synthesis and Their Luminescent Properties Piao, Xianqing; Machida, Ken-ichi; Horikawa, Takashi Chemistry of Materials, Vol. 19, Issue 18 https://doi.org/10.1021/cm070623c	journal	September 2007
Yellow-Orange-Emitting CaAlSiN ₃ :Ce ³⁺ Phosphor: Structure, Photoluminescence, and Application in White LEDs Li, Y. Q.; Hirosaki, N.; Xie, R. J. Chemistry of Materials, Vol. 20, Issue 21 https://doi.org/10.1021/cm801669x	journal	October 2008
Low Temperature Precursor Route for Highly Efficient Spherically Shaped LED-Phosphors M ₂ Si ₅ N ₈ :Eu ²⁺ (M = Eu, Sr, Ba) Zeuner, Martin; Hintze, Frauke; Schnick, Wolfgang Chemistry of Materials, Vol. 21, Issue 2 https://doi.org/10.1021/cm8024796	journal	December 2008
Narrow-band red-emitting Sr[LiAl3N4]:Eu2+ as a next-generation LED-phosphor material Pust, Philipp; Weiler, Volker; Hecht, Cora Nature Materials, Vol. 13, Issue 9 https://doi.org/10.1038/nmat4012	journal	June 2014
Ca[LiAl ₃ N ₄ ]:Eu ²⁺ —A Narrow-Band Red-Emitting Nitridolithoaluminate Pust, Philipp; Wochnik, Angela S.; Baumann, Elen Chemistry of Materials, Vol. 26, Issue 11 https://doi.org/10.1021/cm501162n	journal	May 2014
Toward New Phosphors for Application in Illumination-Grade White pc-LEDs: The Nitridomagnesosilicates Ca[Mg ₃ SiN ₄ ]:Ce ³⁺ , Sr[Mg ₃ SiN ₄ ]:Eu ²⁺ , and Eu[Mg ₃ SiN ₄ ] Schmiechen, Sebastian; Schneider, Hajnalka; Wagatha, Peter Chemistry of Materials, Vol. 26, Issue 8 https://doi.org/10.1021/cm500610v	journal	April 2014
Rare-Earth Activated Nitride Phosphors: Synthesis, Luminescence and Applications Xie, Rong-Jun; Hirosaki, Naoto; Li, Yuanqiang Materials, Vol. 3, Issue 6 https://doi.org/10.3390/ma3063777	journal	June 2010
On the Performance Enhancement of Nitride Phosphors as Spectral Conversion Materials in Solid State Lighting Xie, Rong-Jun; Hirosaki, Naoto; Takeda, T. ECS Journal of Solid State Science and Technology, Vol. 2, Issue 2 https://doi.org/10.1149/2.002302jss	journal	November 2012
Optical Properties of (Oxy)Nitride Materials: A Review Xie, Rong-Jun; Bert Hintzen, Hubertus T. Journal of the American Ceramic Society, Vol. 96, Issue 3 https://doi.org/10.1111/jace.12197	journal	March 2013
Solid-State Lighting R&D Plan - 2015 Bardsley, Norman; Bland, Stephen; Hansen, Monica https://doi.org/10.2172/1220487	report	May 2015
Research challenges to ultra-efficient inorganic solid-state lighting Phillips, J. M.; Coltrin, M. E.; Crawford, M. H. Laser & Photonics Review, Vol. 1, Issue 4, p. 307-333 https://doi.org/10.1002/lpor.200710019	journal	December 2007
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
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
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis Ong, Shyue Ping; Richards, William Davidson; Jain, Anubhav Computational Materials Science, Vol. 68 https://doi.org/10.1016/j.commatsci.2012.10.028	journal	February 2013
Li−Fe−P−O ₂ Phase Diagram from First Principles Calculations Ong, Shyue Ping; Wang, Lei; Kang, Byoungwoo Chemistry of Materials, Vol. 20, Issue 5 https://doi.org/10.1021/cm702327g	journal	February 2008
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
The Materials Application Programming Interface (API): A simple, flexible and efficient API for materials data based on REpresentational State Transfer (REST) principles Ong, Shyue Ping; Cholia, Shreyas; Jain, Anubhav Computational Materials Science, Vol. 97 https://doi.org/10.1016/j.commatsci.2014.10.037	journal	February 2015
Hybrid functionals based on a screened Coulomb potential Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 118, Issue 18 https://doi.org/10.1063/1.1564060	journal	May 2003
Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)] Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 124, Issue 21 https://doi.org/10.1063/1.2204597	journal	June 2006
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y. Physical Review B, Vol. 57, Issue 3, p. 1505-1509 https://doi.org/10.1103/PhysRevB.57.1505	journal	January 1998
First-principles study of luminescence in Eu $^{2 +}$ -doped inorganic scintillators Chaudhry, A.; Boutchko, R.; Chourou, S. Physical Review B, Vol. 89, Issue 15 https://doi.org/10.1103/PhysRevB.89.155105	journal	April 2014
Proxies from Ab Initio Calculations for Screening Efficient Ce ³⁺ Phosphor Hosts Brgoch, Jakoah; DenBaars, Steven P.; Seshadri, Ram The Journal of Physical Chemistry C, Vol. 117, Issue 35 https://doi.org/10.1021/jp405858e	journal	August 2013
The Elastic Behaviour of a Crystalline Aggregate Hill, R. Proceedings of the Physical Society. Section A, Vol. 65, Issue 5 https://doi.org/10.1088/0370-1298/65/5/307	journal	May 1952
Narrow-Band Green Emitting Nitridolithoalumosilicate Ba[Li ₂ (Al ₂ Si ₂ )N ₆ ]:Eu ²⁺ with Framework Topology whj for LED/LCD-Backlighting Applications Strobel, Philipp; Schmiechen, Sebastian; Siegert, Markus Chemistry of Materials, Vol. 27, Issue 17 https://doi.org/10.1021/acs.chemmater.5b02702	journal	August 2015
Characterization and properties of green-emitting β-SiAlON:Eu2+ powder phosphors for white light-emitting diodes Hirosaki, Naoto; Xie, Rong-Jun; Kimoto, Koji Applied Physics Letters, Vol. 86, Issue 21 https://doi.org/10.1063/1.1935027	journal	May 2005
Luminescence properties of red-emitting M2Si5N8:Eu2+ (M=Ca, Sr, Ba) LED conversion phosphors Li, Y. Q.; van Steen, J. E. J.; van Krevel, J. W. H. Journal of Alloys and Compounds, Vol. 417, Issue 1-2 https://doi.org/10.1016/j.jallcom.2005.09.041	journal	June 2006
SrAlSi ₄ N ₇ :Eu ²⁺ − A Nitridoalumosilicate Phosphor for Warm White Light (pc)LEDs with Edge-Sharing Tetrahedra Hecht, Cora; Stadler, Florian; Schmidt, Peter J. Chemistry of Materials, Vol. 21, Issue 8 https://doi.org/10.1021/cm803231h	journal	March 2009
Thermal quenching of Eu ²⁺ 5d–4f luminescence in inorganic compounds Dorenbos, P. Journal of Physics: Condensed Matter, Vol. 17, Issue 50 https://doi.org/10.1088/0953-8984/17/50/027	journal	December 2005
Insights into Current Limitations of Density Functional Theory Cohen, A. J.; Mori-Sanchez, P.; Yang, W. Science, Vol. 321, Issue 5890 https://doi.org/10.1126/science.1158722	journal	August 2008
High-Throughput Combinatorial Database of Electronic Band Structures for Inorganic Scintillator Materials Setyawan, Wahyu; Gaume, Romain M.; Lam, Stephanie ACS Combinatorial Science, Vol. 13, Issue 4 https://doi.org/10.1021/co200012w	journal	June 2011
Synthesis and Structure of Alkaline Earth Silicon Nitrides: BaSiN ₂ , SrSiN ₂ , and CaSiN ₂ Gál, Zoltán A.; Mallinson, Phillip M.; Orchard, Heston J. Inorganic Chemistry, Vol. 43, Issue 13 https://doi.org/10.1021/ic049901p	journal	June 2004
Preparation, Electronic Structure, and Photoluminescence Properties of Eu ²⁺ - and Ce ³⁺ /Li ⁺ -Activated Alkaline Earth Silicon Nitride MSiN ₂ (M = Sr, Ba) Duan, C. J.; Wang, X. J.; Otten, W. M. Chemistry of Materials, Vol. 20, Issue 4 https://doi.org/10.1021/cm701875e	journal	January 2008
Phosphates as Lithium-Ion Battery Cathodes: An Evaluation Based on High-Throughput ab Initio Calculations Hautier, Geoffroy; Jain, Anubhav; Ong, Shyue Ping Chemistry of Materials, Vol. 23, Issue 15 https://doi.org/10.1021/cm200949v	journal	August 2011
Data Mined Ionic Substitutions for the Discovery of New Compounds Hautier, Geoffroy; Fischer, Chris; Ehrlacher, Virginie Inorganic Chemistry, Vol. 50, Issue 2 https://doi.org/10.1021/ic102031h	journal	January 2011
The inorganic crystal structure data base Bergerhoff, G.; Hundt, R.; Sievers, R. Journal of Chemical Information and Modeling, Vol. 23, Issue 2 https://doi.org/10.1021/ci00038a003	journal	May 1983
Das neue Orthotitanat CsNa3[TiO4] Wei�, C.; Hoppe, R. Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 622, Issue 10 https://doi.org/10.1002/zaac.19966221015	journal	October 1996
“Fragmentierung” und “Aggregation” bei Bleioxiden Über das Oligooxoplumbat(IV) K ₂ Li ₆ [Pb ₂ O ₈ ] Brazel, B.; Hoppe, R. Zeitschrift für anorganische und allgemeine Chemie, Vol. 497, Issue 2 https://doi.org/10.1002/zaac.19834970216	journal	February 1983
Highly efficient narrow-band green and red phosphors enabling wider color-gamut LED backlight for more brilliant displays Wang, Le; Wang, Xiaojun; Kohsei, Takahashi Optics Express, Vol. 23, Issue 22 https://doi.org/10.1364/OE.23.028707	journal	January 2015
Investigations of the Electronic Structure and Bandgap of the Next-Generation LED-Phosphor Sr[LiAl ₃ N ₄ ]:Eu ²⁺ -Experiment and Calculations Tolhurst, Thomas M.; Boyko, Teak D.; Pust, Philipp Advanced Optical Materials, Vol. 3, Issue 4 https://doi.org/10.1002/adom.201400558	journal	January 2015
Electronic structure of the alkaline-earth silicon nitrides M ₂ Si ₅ N ₈ (M = Ca and Sr) obtained from first-principles calculations and optical reflectance spectra Fang, C. M.; Hintzen, H. T.; With, G. de Journal of Physics: Condensed Matter, Vol. 13, Issue 1 https://doi.org/10.1088/0953-8984/13/1/307	journal	December 2000

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