Energy-Efficient, High-Color-Rendering LED Lamps Using Oxyfluoride and Fluoride Phosphors

Setlur, Anant; Radkov, Emil; Henderson, Claire S.; Her, Jae‐Hyuk; Srivastava, A.M.; Karkada, Nagaveni; Kishore, M. Satya; Kumar, N. Prasanth; Aesram, Danny; Deshpande, Anirudha; Kolodin, Boris; Grigorov, L.; Happek, U.

doi:10.1021/cm100960g

Cited by 270 publications

(207 citation statements)

References 34 publications

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“…[1][2][3][4][5][6] Until now, most of the efforts to find new hosts relied on trial and error. An accurate and efficient methodology to design new materials would be a remarkable achievement.…”

mentioning

confidence: 99%

Assessment of First‐Principles and Semiempirical Methodologies for Absorption and Emission Energies of Ce³⁺‐Doped Luminescent Materials

Jia

Poncé

Miglio

et al. 2017

Advanced Optical Materials

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Abstract:In search of a reliable methodology for the prediction of light absorption and emission of Ce 3+ -doped luminescent materials, thirteen representative materials are studied with first-principles and semi-empirical approaches. In the first-principles approach, that combines constrained density-functional theory and ∆SCF, the atomic positions are obtained for both ground and excited states of the Ce 3+ ion. The structural information is fed into Dorenbos' semi-empirical model. Absorption and emission energies are calculated with both methods and compared with experiment. The first-principles approach matches experiment within 0.3 eV, with two exceptions at 0.5 eV. In contrast, the semi-empirical approach does not perform as well (usually more than 0.5 eV error). The general applicability of the present first-principles scheme, with an encouraging predictive power, opens a novel avenue for crystal site engineering and high-throughput search for new phosphors and scintillators. 2The 4f→5d transition of Ce 3+ ion has been widely used in the design of efficient luminescent systems such as white LED phosphors, scintillators and laser materials due to its spin-allowed character and its tunability as a function of the host material. [1-6] Until now, most of the efforts to find new hosts relied on trial and error. An accurate and efficient methodology to design new materials would be a remarkable achievement. With this idea in mind, a semi-empirical model has been proposed by Dorenbos, to describe Ce 3+ luminescence in inorganic compounds. [7] This semi-empirical model provides correct general trend for absorption.Unfortunately, it suffers from several drawbacks. First, its quantitative predictions rely on some fitting parameters, which have been determined only for oxide, nitride and fluoride materials at present.[6] Second, the semi-empirical model fails to predict the emission energy and Stokes shift. This limitation is due to missing experimental relaxed structure configurations in the excited state. These two shortcomings result in limited accuracy and scope of the semi-empirical approach.In a recent paper, we have explored a first-principles alternative to overcome the drawbacks of Dorenbos' semi-empirical model. [8] The successful quantitative description of the neutral excitation, emission energy and Stokes shift in two Ce 3+ -doped lanthanum silicate nitrides has been realized. Our approach is based on constrained density functional theory (CDFT) and the ∆SCF methods, following the early work by Marsman. [9] Recently, Canning and co-authors used CDFT to identify several promising hosts for efficient scintillators, but they did not study the emission and Stokes shifts. [10] In the present work, we assess the generality and accuracy of the proposed theoretical method, and compare it with Dorenbos' semi-empirical model. To do so, firstly we study from first principles the absorption, emission and Stokes shift of a set of thirteen representative Ce 3+ -doped materials that include oxides, nitrides and halid...

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mentioning

confidence: 99%

Assessment of First‐Principles and Semiempirical Methodologies for Absorption and Emission Energies of Ce³⁺‐Doped Luminescent Materials

Jia

Poncé

Miglio

et al. 2017

Advanced Optical Materials

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“…Upon laser excitation at 515 nm an external QE of about 40 % is obtained. Substitution of Ca with Mg or Sr, and of Si with Al, allows shifting the emission and excitation maxima, confirming the [136] potential of these phosphors in combination with a blue LED. The nitride SrAlSi 4 N 7 has been proposed as a host for the lanthanide ions Ce 3?…”

Section: Red Phosphors-other Hostsmentioning

confidence: 60%

“…In this case, the doping ion shows luminescence spectra due to 4f 14 $ 4f 13 5d 1 interconfigurational transitions [139]. The oxynitride [136] material is characterized by a single broad band centered at 549 nm (Fig. 22).…”

Section: Green Phosphors-other Hostsmentioning

confidence: 98%

“…Setlur et al [136] have proposed oxyfluoride and fluoride phosphors for energyefficient, high-color rendering LED lamps. Among them, it is worth mentioning the oxyfluoride (Sr,Ca) 3 (Al,Si)O 4 (F,O):Ce 3?…”

Section: Green Phosphors-other Hostsmentioning

confidence: 99%

“…Huang et al [17] Setlur et al [136] have proposed the development of a red phosphor for pcLEDs based on the ion Mn 4? as a dopant in octahedral coordination.…”

Section: Red Phosphors-other Hostsmentioning

confidence: 99%

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Inorganic Phosphor Materials for Lighting

2016

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This chapter addresses the development of inorganic phosphor materials capable of converting the near UV or blue radiation emitted by a light emitting diode to visible radiation that can be suitably combined to yield white light. These materials are at the core of the new generation of solid-state lighting devices that are emerging as a crucial clean and energy saving technology. The chapter introduces the problem of white light generation using inorganic phosphors and the structureproperty relationships in the broad class of phosphor materials, normally containing lanthanide or transition metal ions as dopants. Radiative and non-radiative relaxation mechanisms are briefly described. Phosphors emitting light of different colors (yellow, blue, green, and red) are described and reviewed, classifying them in different chemical families of the host (silicates, phosphates, aluminates, borates, and non-oxide hosts). This research field has grown rapidly and is still growing, but the discovery of new phosphor materials with optimized properties (in terms of emission efficiency, chemical and thermal stability, color, purity, and cost of fabrication) would still be of the utmost importance.

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Light Emitting Diode Materials and Devices

Krames¹

2016

Materials for Solid State Lighting and Displays

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Energy-Efficient, High-Color-Rendering LED Lamps Using Oxyfluoride and Fluoride Phosphors

Cited by 270 publications

References 34 publications

Assessment of First‐Principles and Semiempirical Methodologies for Absorption and Emission Energies of Ce³⁺‐Doped Luminescent Materials

Assessment of First‐Principles and Semiempirical Methodologies for Absorption and Emission Energies of Ce³⁺‐Doped Luminescent Materials

Inorganic Phosphor Materials for Lighting

Light Emitting Diode Materials and Devices

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Energy-Efficient, High-Color-Rendering LED Lamps Using Oxyfluoride and Fluoride Phosphors

Cited by 270 publications

References 34 publications

Assessment of First‐Principles and Semiempirical Methodologies for Absorption and Emission Energies of Ce3+‐Doped Luminescent Materials

Assessment of First‐Principles and Semiempirical Methodologies for Absorption and Emission Energies of Ce3+‐Doped Luminescent Materials

Inorganic Phosphor Materials for Lighting

Light Emitting Diode Materials and Devices

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Assessment of First‐Principles and Semiempirical Methodologies for Absorption and Emission Energies of Ce³⁺‐Doped Luminescent Materials

Assessment of First‐Principles and Semiempirical Methodologies for Absorption and Emission Energies of Ce³⁺‐Doped Luminescent Materials