Enhancing multiphoton upconversion through energy clustering at sublattice level

Handle URI:
http://hdl.handle.net/10754/563100
Title:
Enhancing multiphoton upconversion through energy clustering at sublattice level
Authors:
Wang, Juan; Deng, Renren; Macdonald, Mark A B; Chen, Bolei; Yuan, Jikang; Wang, Feng; Chi, Dongzhi; Hor, Andy Sum Andy; Zhang, Peng; Liu, Guokui; Han, Yu ( 0000-0003-1462-1118 ) ; Liu, Xiaogang
Abstract:
The applications of lanthanide-doped upconversionnanocrystals in biological imaging, photonics, photovoltaics and therapeutics have fuelled a growing demand for rational control over the emission profiles of the nanocrystals. A common strategy for tuning upconversion luminescence is to control the doping concentration of lanthanide ions. However, the phenomenon of concentration quenching of the excited state at high doping levels poses a significant constraint. Thus, the lanthanide ions have to be stringently kept at relatively low concentrations to minimize luminescence quenching. Here we describe a new class of upconversion nanocrystals adopting an orthorhombic crystallographic structure in which the lanthanide ions are distributed in arrays of tetrad clusters. Importantly, this unique arrangement enables the preservation of excitation energy within the sublattice domain and effectively minimizes the migration of excitation energy to defects, even in stoichiometric compounds with a high Yb 3+ content (calculated as 98 mol%). This allows us to generate an unusual four-photon-promoted violet upconversion emission from Er 3+ with an intensity that is more than eight times higher than previously reported. Our results highlight that the approach to enhancing upconversion through energy clustering at the sublattice level may provide new opportunities for light-triggered biological reactions and photodynamic therapy. © 2014 Macmillan Publishers Limited. All rights reserved.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Nanostructured Functional Materials (NFM) laboratory
Publisher:
Springer Nature
Journal:
Nature Materials
Issue Date:
24-Nov-2013
DOI:
10.1038/nmat3804
Type:
Article
ISSN:
14761122
Sponsors:
The bulk of the work was supported by the Institute of Materials Research and Engineering (IMRE/12-8C0101) and the Singapore Ministry of Education (MOE2010-T2-1-083). Y.H. is grateful to KAUST Global Collaborative Research for the Academic Excellence Alliance (AEA) fund and P.Z. acknowledges the financial support from NSERC Canada. The PNC/XSD facilities at the Advanced Photon Source are supported by the US Department of Energy (DOE)-Basic Energy Sciences, a Major Resources Support grant from NSERC, the University of Washington, the Canadian Light Source, and the Advanced Photon Source. Use of the Advanced Photon Source was supported by the US DOE under contract no. DE-AC02-06CH11357. We thank PNC/XSD staff beamline scientist R. Gordon for synchrotron technical support. The authors thank H. Zhu, S. Animesh and R. Chen for technical assistance.
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Chemical Science Program

Full metadata record

DC FieldValue Language
dc.contributor.authorWang, Juanen
dc.contributor.authorDeng, Renrenen
dc.contributor.authorMacdonald, Mark A Ben
dc.contributor.authorChen, Boleien
dc.contributor.authorYuan, Jikangen
dc.contributor.authorWang, Fengen
dc.contributor.authorChi, Dongzhien
dc.contributor.authorHor, Andy Sum Andyen
dc.contributor.authorZhang, Pengen
dc.contributor.authorLiu, Guokuien
dc.contributor.authorHan, Yuen
dc.contributor.authorLiu, Xiaogangen
dc.date.accessioned2015-08-03T11:35:46Zen
dc.date.available2015-08-03T11:35:46Zen
dc.date.issued2013-11-24en
dc.identifier.issn14761122en
dc.identifier.doi10.1038/nmat3804en
dc.identifier.urihttp://hdl.handle.net/10754/563100en
dc.description.abstractThe applications of lanthanide-doped upconversionnanocrystals in biological imaging, photonics, photovoltaics and therapeutics have fuelled a growing demand for rational control over the emission profiles of the nanocrystals. A common strategy for tuning upconversion luminescence is to control the doping concentration of lanthanide ions. However, the phenomenon of concentration quenching of the excited state at high doping levels poses a significant constraint. Thus, the lanthanide ions have to be stringently kept at relatively low concentrations to minimize luminescence quenching. Here we describe a new class of upconversion nanocrystals adopting an orthorhombic crystallographic structure in which the lanthanide ions are distributed in arrays of tetrad clusters. Importantly, this unique arrangement enables the preservation of excitation energy within the sublattice domain and effectively minimizes the migration of excitation energy to defects, even in stoichiometric compounds with a high Yb 3+ content (calculated as 98 mol%). This allows us to generate an unusual four-photon-promoted violet upconversion emission from Er 3+ with an intensity that is more than eight times higher than previously reported. Our results highlight that the approach to enhancing upconversion through energy clustering at the sublattice level may provide new opportunities for light-triggered biological reactions and photodynamic therapy. © 2014 Macmillan Publishers Limited. All rights reserved.en
dc.description.sponsorshipThe bulk of the work was supported by the Institute of Materials Research and Engineering (IMRE/12-8C0101) and the Singapore Ministry of Education (MOE2010-T2-1-083). Y.H. is grateful to KAUST Global Collaborative Research for the Academic Excellence Alliance (AEA) fund and P.Z. acknowledges the financial support from NSERC Canada. The PNC/XSD facilities at the Advanced Photon Source are supported by the US Department of Energy (DOE)-Basic Energy Sciences, a Major Resources Support grant from NSERC, the University of Washington, the Canadian Light Source, and the Advanced Photon Source. Use of the Advanced Photon Source was supported by the US DOE under contract no. DE-AC02-06CH11357. We thank PNC/XSD staff beamline scientist R. Gordon for synchrotron technical support. The authors thank H. Zhu, S. Animesh and R. Chen for technical assistance.en
dc.publisherSpringer Natureen
dc.titleEnhancing multiphoton upconversion through energy clustering at sublattice levelen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentNanostructured Functional Materials (NFM) laboratoryen
dc.identifier.journalNature Materialsen
dc.contributor.institutionDepartment of Chemistry, National University of Singapore, Singapore 117543, Singaporeen
dc.contributor.institutionDepartment of Chemistry, Dalhousie University, Halifax, NS B3H 4J3, Canadaen
dc.contributor.institutionDepartment of Applied Physics, Hong Kong Polytechnic University, Kowloon, Hong Kongen
dc.contributor.institutionInstitute of Materials Research and Engineering, Agency for Science, Technology and Research, Singapore 117602, Singaporeen
dc.contributor.institutionArgonne National Laboratory, Chemical Sciences and Engineering Division, Argonne, IL 60439, United Statesen
kaust.authorHan, Yuen
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