Sb3+-doped 0D Cs3GdCl6 microcrystals with a near-unity photoluminescence quantum yield and high thermal quenching resistance for light-emitting application - Details

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All-inorganic　lead-free　luminescent　metal　halides　doped　with　main-group　ns2-electron　ions　have　attracted　considerable　interest　in　a　variety　of　optoelectronic　applications.　However,　they　normally　suffer　from　severe　thermal　quenching　of　photoluminescence　(PL)　due　to　aggravated　nonradiative　relaxation　at　high　temperatures.　Herein,　we　report　a　new　class　of　luminescent　materials　based　on　5s2-electron　Sb3+-doped　0D　Cs3GdCl6　microcrystals　(MCs),　which　exhibit　intense　yellowish　PL　at　540　nm　under　ultraviolet　(UV)　excitation,　in　parallel　with　a　broad　bandwidth　of　510　meV,　a　large　Stokes　shift　of　190　nm,　a　near-unity　PL　quantum　yield,　and　remarkable　resistance　against　thermal　quenching　(I150°C　=　82.4%).　Mechanistic　investigation　unravels　that　the　broadband　emission　originates　from　the　spin-orbital　allowed　3P1　→　1S0　transition　of　Sb3+　which　experiences　a　dynamic　Jahn-Teller　distortion　in　the　excited　state.　These　properties　facilitate　Cs3GdCl6:Sb3+　MCs　as　an　efficient　yellowish　phosphor　for　near-UV-converted　white　light-emitting　diodes,　demonstrating　a　high　color-rendering　index　of　96.4　and　excellent　operational　stability.　This　work　provides　not　only　fundamental　insights　into　the　excited-state　dynamics　of　Sb3+　in　Cs3GdCl6　MCs,　but　also　a　new　way　for　the　exploration　of　novel　and　highly　emissive　rare-earth　halides　through　ns2-electron　ion　doping　towards　various　light-emitting　applications.　©　2024　The　Royal　Society　of　Chemistry.

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[ 1 ] [Liang X.]Fujian Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry and CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 2 ] [Liang X.]College of Physics and Energy, Fujian Normal University, Fujian, Fuzhou, 350117, China
[ 3 ] [Zhang W.]Fujian Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry and CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 4 ] [Zhang W.]Key Laboratory of Advanced Materials Technologies and International (Hongkong, Macao and Taiwan) Joint Laboratory on Advanced Materials Technologies, College of Materials Science and Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 5 ] [Shi Y.]Fujian Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry and CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 6 ] [Shi Y.]College of Physics and Energy, Fujian Normal University, Fujian, Fuzhou, 350117, China
[ 7 ] [Zhang W.]Fujian Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry and CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 8 ] [Yang H.]Fujian Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry and CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 9 ] [Huang P.]Fujian Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry and CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 10 ] [Huang P.]College of Physics and Energy, Fujian Normal University, Fujian, Fuzhou, 350117, China
[ 11 ] [Li L.]Key Laboratory of Advanced Materials Technologies and International (Hongkong, Macao and Taiwan) Joint Laboratory on Advanced Materials Technologies, College of Materials Science and Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 12 ] [Zhang Q.]Key Laboratory of Advanced Materials Technologies and International (Hongkong, Macao and Taiwan) Joint Laboratory on Advanced Materials Technologies, College of Materials Science and Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 13 ] [Zheng W.]Fujian Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry and CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 14 ] [Zheng W.]College of Physics and Energy, Fujian Normal University, Fujian, Fuzhou, 350117, China
[ 15 ] [Chen X.]Fujian Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry and CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
[ 16 ] [Chen X.]College of Physics and Energy, Fujian Normal University, Fujian, Fuzhou, 350117, China

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Journal of Materials Chemistry C

ISSN： 2050-7526

Year： 2024

Issue： 15

Volume： 12

Page： 5538-5548

5 . 7 0 0

JCR@2023

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SCOPUS Cited Count： 3

ESI Highly Cited Papers on the List： 0 Unfold All

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