Intense deep-red zero phonon line emission of Mn4+ in double perovskite La4Ti3O12

Ji, Haipeng; Ueda, Jumpei; Brik, Mikhail G.; Du, Mao-Hua; Chen, Deliang; Tanabe, Setsuhisa

doi:10.1039/c9cp04007b

Title: Intense deep-red zero phonon line emission of Mn⁴⁺ in double perovskite La₄Ti₃O₁₂

Abstract

Phosphors that emit in the deep-red spectral region are critical for plant cultivation light-emitting diodes. In this work, ultrabroadband deep-red luminescence of Mn⁴⁺ in La₄Ti₃O₁₂ was studied, which showed intense zero phonon line emission. The double-perovskite structural La₄Ti₃O₁₂ simultaneously contains two Ti⁴⁺ sites forming slightly- and highly-distorted TiO₆ octahedra, respectively. The influence of octahedral distortion on the Mn⁴⁺ emission energy in the two distinct Ti⁴⁺ sites was studied both experimentally and theoretically. The spectral measurements indicated that Mn⁴⁺ in La₄Ti₃O₁₂ showed intense zero phonon line emission (ZPL) at deep-red 710–740 nm under excitation of 400 nm charging the O^2- → Mn⁴⁺ charge transfer transition. The splitting of the ZPL of the Mn^{4+ 2}E_g → ⁴A_2g transition as well as the intensity of ZPL relative to the vibronic phonon sideband emissions were found to be greatly influenced by the degree of octahedral distortion. The crystal-field strength and Racah parameters of Mn4+ in each Ti4+ site were also estimated. The Mn^{4+ 2}E_g → ⁴A_2g luminescence exhibited severe thermal quenching, which was explained by the low-lying ⁴T_2g level and charge-transfer state.

Authors:

^[1];

^[2];

^[3];

^[4];

^[5];

^[2]

Zhengzhou Univ. (China); Kyoto Univ. (Japan)
Kyoto Univ. (Japan)
Chongqing Univ. of Posts and Telecommunications (China); Univ. of Tartu (Estonia)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Zhengzhou Univ. (China)

Publication Date:: 2019-10-22

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1607041

Alternate Identifier(s):: OSTI ID: 1573269

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Physical Chemistry Chemical Physics. PCCP

Additional Journal Information:: Journal Volume: 21; Journal Issue: 45; Journal ID: ISSN 1463-9076

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Mn4+; luminescence; double perovskite; titanate

Citation Formats


                    Ji, Haipeng, Ueda, Jumpei, Brik, Mikhail G., Du, Mao-Hua, Chen, Deliang, and Tanabe, Setsuhisa. Intense deep-red zero phonon line emission of Mn4+ in double perovskite La4Ti3O12.  United States: N. p., 2019. 
Web.  doi:10.1039/c9cp04007b.

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                    Ji, Haipeng, Ueda, Jumpei, Brik, Mikhail G., Du, Mao-Hua, Chen, Deliang, & Tanabe, Setsuhisa. Intense deep-red zero phonon line emission of Mn4+ in double perovskite La4Ti3O12.  United States.  https://doi.org/10.1039/c9cp04007b

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                    Ji, Haipeng, Ueda, Jumpei, Brik, Mikhail G., Du, Mao-Hua, Chen, Deliang, and Tanabe, Setsuhisa. Tue .  
"Intense deep-red zero phonon line emission of Mn4+ in double perovskite La4Ti3O12".  United States.  https://doi.org/10.1039/c9cp04007b.  https://www.osti.gov/servlets/purl/1607041.

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@article{osti_1607041,

  title        = {Intense deep-red zero phonon line emission of Mn4+ in double perovskite La4Ti3O12},

  author       = {Ji, Haipeng and Ueda, Jumpei and Brik, Mikhail G. and Du, Mao-Hua and Chen, Deliang and Tanabe, Setsuhisa},

  abstractNote = {Phosphors that emit in the deep-red spectral region are critical for plant cultivation light-emitting diodes. In this work, ultrabroadband deep-red luminescence of Mn4+ in La4Ti3O12 was studied, which showed intense zero phonon line emission. The double-perovskite structural La4Ti3O12 simultaneously contains two Ti4+ sites forming slightly- and highly-distorted TiO6 octahedra, respectively. The influence of octahedral distortion on the Mn4+ emission energy in the two distinct Ti4+ sites was studied both experimentally and theoretically. The spectral measurements indicated that Mn4+ in La4Ti3O12 showed intense zero phonon line emission (ZPL) at deep-red 710–740 nm under excitation of 400 nm charging the O2- → Mn4+ charge transfer transition. The splitting of the ZPL of the Mn4+ 2Eg → 4A2g transition as well as the intensity of ZPL relative to the vibronic phonon sideband emissions were found to be greatly influenced by the degree of octahedral distortion. The crystal-field strength and Racah parameters of Mn4+ in each Ti4+ site were also estimated. The Mn4+ 2Eg → 4A2g luminescence exhibited severe thermal quenching, which was explained by the low-lying 4T2g level and charge-transfer state.},

  doi          = {10.1039/c9cp04007b},

  journal      = {Physical Chemistry Chemical Physics. PCCP},

  number       = 45,

  volume       = 21,

  place        = {United States},

  year         = {2019},

  month        = {10}

}

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https://doi.org/10.1039/c9cp04007b

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Cited by: 16 works

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Figure 1: XRD pattern of the as-prepared La₄(Ti_2.998Mn_0.002)O₁₂ (the insert shows digital image of the sample). The reference pattern (No. 01-074-2661) of La₄Ti₃O₁₂was also given.

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Title: Intense deep-red zero phonon line emission of Mn4+ in double perovskite La4Ti3O12

Abstract

Citation Formats

Figures / Tables:

Generalized Gradient Approximation Made Simple journal, October 1996

Rare-earth-free red-emitting K 2 Ge 4 O 9 :Mn 4+ phosphor excited by blue light for warm white LEDs journal, January 2016

Composition dependent spectral shift of Mn4+ luminescence in silicate garnet hosts CaY2M2Al2SiO12 (M = Al, Ga, Sc) journal, June 2018

Understanding the quenching nature of Mn 4+ in wide band gap inorganic compounds: design principles for Mn 4+ phosphors with higher efficiency journal, January 2018

Mn 2+ and Mn 4+ red phosphors: synthesis, luminescence and applications in WLEDs. A review journal, January 2018

Excitation power dependent optical temperature behaviors in Mn 4+ doped oxyfluoride Na 2 WO 2 F 4 journal, January 2018

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal, July 1996

Luminescence of Mn 4+ in the orthorhombic perovskite, LaGaO 3 journal, March 2017

From ultrasoft pseudopotentials to the projector augmented-wave method journal, January 1999

Luminescence, energy transfer and optical thermometry of a novel narrow red emitting phosphor: Cs 2 WO 2 F 4 :Mn 4+ journal, January 2017

Local coordination, electronic structure, and thermal quenching of Ce 3+ in isostructural Sr 2 GdAlO 5 and Sr 3 AlO 4 F phosphors journal, August 2018

Highly efficient non-rare-earth red emitting phosphor for warm white light-emitting diodes journal, July 2014

Spin-Forbidden Transitions in the Spectra of Transition Metal Ions and Nephelauxetic Effect journal, September 2015

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Water splitting into H2 and O2 over niobate and titanate photocatalysts with (111) plane-type layered perovskite structure journal, January 2009

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data journal, October 2011

Efficient Mn(IV) Emission in Fluorine Coordination journal, January 1973

K_2SiF_6:Mn^4+ as a red phosphor for displays and warm-white LEDs: a review of properties and perspectives journal, January 2017

Quenching of the red Mn4+ luminescence in Mn4+-doped fluoride LED phosphors journal, May 2018

Synthesis and properties of Rb 2 GeF 6 :Mn 4+ red-emitting phosphors journal, January 2018

Neutron powder diffraction refinement of the crystal structure of La4Ti3O12 journal, March 2000

Cation-Deficient Perovskite-Related (Ba,La)nTin−δO3n (n≥4δ) Microphases in the La4Ti3O12–BaTiO3 System: An HRTEM Approach journal, July 1999

Crystal field studies of the Mn4+ energy levels in the perovskite, LaAlO3 journal, June 2013

Influence of Covalency on the Mn 4+ 2 E g → 4 A 2g Emission Energy in Crystals journal, December 2014

The dependence of 10 Dq crystal field parameter for Mn4+ (3d3 configuration) and the magnitude of 7F1 level splitting for Eu3+ (4f6 configuration) on pyrochlore compositions journal, December 2012

Spectroscopy of Mn 4+ in Double Perovskites, La 2 LiSbO 6 and La 2 MgTiO 6 : Deep Red Photon Generators for Agriculture LEDs journal, July 2017

A highly-distorted octahedron with a C 2v group symmetry inducing an ultra-intense zero phonon line in Mn 4+ -activated oxyfluoride Na 2 WO 2 F 4 journal, January 2017

Excitation Energies of Localized Correlated Defects via Quantum Monte Carlo: A Case Study of Mn 4+ -Doped Phosphors journal, November 2018

On the Mn4+ R-line emission intensity and its tunability in solids journal, May 2019

Interpretation of the Spectroscopic Properties of α-LiAlO 2 : Mn 4+ journal, July 2017

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Title: Intense deep-red zero phonon line emission of Mn⁴⁺ in double perovskite La₄Ti₃O₁₂

Generalized Gradient Approximation Made Simple
journal, October 1996

Rare-earth-free red-emitting K ₂ Ge ₄ O ₉ :Mn ⁴⁺ phosphor excited by blue light for warm white LEDs
journal, January 2016

Composition dependent spectral shift of Mn4+ luminescence in silicate garnet hosts CaY2M2Al2SiO12 (M = Al, Ga, Sc)
journal, June 2018

Understanding the quenching nature of Mn ⁴⁺ in wide band gap inorganic compounds: design principles for Mn ⁴⁺ phosphors with higher efficiency
journal, January 2018

Mn ²⁺ and Mn ⁴⁺ red phosphors: synthesis, luminescence and applications in WLEDs. A review
journal, January 2018

Excitation power dependent optical temperature behaviors in Mn ⁴⁺ doped oxyfluoride Na ₂ WO ₂ F ₄
journal, January 2018

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Luminescence of Mn 4+ in the orthorhombic perovskite, LaGaO 3
journal, March 2017

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Luminescence, energy transfer and optical thermometry of a novel narrow red emitting phosphor: Cs ₂ WO ₂ F ₄ :Mn ⁴⁺
journal, January 2017

Local coordination, electronic structure, and thermal quenching of Ce ³⁺ in isostructural Sr ₂ GdAlO ₅ and Sr ₃ AlO ₄ F phosphors
journal, August 2018

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journal, July 2014

Spin-Forbidden Transitions in the Spectra of Transition Metal Ions and Nephelauxetic Effect
journal, September 2015

Temperature effect on the emission spectra of narrow band Mn ⁴⁺ phosphors for application in LEDs
journal, January 2017

Distortion parameters for coordination polyhedra
journal, March 1976

Water splitting into H2 and O2 over niobate and titanate photocatalysts with (111) plane-type layered perovskite structure
journal, January 2009

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011

Efficient Mn(IV) Emission in Fluorine Coordination
journal, January 1973

K_2SiF_6:Mn^4+ as a red phosphor for displays and warm-white LEDs: a review of properties and perspectives
journal, January 2017

Quenching of the red Mn4+ luminescence in Mn4+-doped fluoride LED phosphors
journal, May 2018

Synthesis and properties of Rb ₂ GeF ₆ :Mn ⁴⁺ red-emitting phosphors
journal, January 2018

Neutron powder diffraction refinement of the crystal structure of La4Ti3O12
journal, March 2000

Cation-Deficient Perovskite-Related (Ba,La)nTin−δO3n (n≥4δ) Microphases in the La4Ti3O12–BaTiO3 System: An HRTEM Approach
journal, July 1999

Crystal field studies of the Mn4+ energy levels in the perovskite, LaAlO3
journal, June 2013

Influence of Covalency on the Mn ^{4+ 2} E _g → ⁴ A _2g Emission Energy in Crystals
journal, December 2014

The dependence of 10 Dq crystal field parameter for Mn4+ (3d3 configuration) and the magnitude of 7F1 level splitting for Eu3+ (4f6 configuration) on pyrochlore compositions
journal, December 2012

Spectroscopy of Mn ⁴⁺ in Double Perovskites, La ₂ LiSbO ₆ and La ₂ MgTiO ₆ : Deep Red Photon Generators for Agriculture LEDs
journal, July 2017

A highly-distorted octahedron with a C _2v group symmetry inducing an ultra-intense zero phonon line in Mn ⁴⁺ -activated oxyfluoride Na ₂ WO ₂ F ₄
journal, January 2017

Excitation Energies of Localized Correlated Defects via Quantum Monte Carlo: A Case Study of Mn ⁴⁺ -Doped Phosphors
journal, November 2018

On the Mn4+ R-line emission intensity and its tunability in solids
journal, May 2019

Interpretation of the Spectroscopic Properties of α-LiAlO ₂ : Mn ⁴⁺
journal, July 2017

The nature of Mn 4+ luminescence in the orthorhombic perovskite, GdAlO 3
journal, January 2017

Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets
journal, May 2021

High-resolution X-ray luminescence extension imaging
journal, February 2021

Lead palladium titanate: A room temperature nanoscale multiferroic thin film
journal, February 2020