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Luminescence in metal-organic frameworks: mechanisms and applications as phosphors and sensors

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TitleInfo
Title
Luminescence in metal-organic frameworks: mechanisms and applications as phosphors and sensors
Name (type = personal)
NamePart (type = family)
Lustig
NamePart (type = given)
William P.
NamePart (type = date)
1987-
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William P. Lustig
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RoleTerm (authority = RULIB)
author
Name (type = personal)
NamePart (type = family)
Li
NamePart (type = given)
Jing
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Jing Li
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Advisory Committee
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chair
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NamePart (type = family)
O'Carroll
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Deirdre
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Deirdre O'Carroll
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Advisory Committee
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internal member
Name (type = personal)
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Warmuth
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Ralf
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Ralf Warmuth
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Advisory Committee
Role
RoleTerm (authority = RULIB)
internal member
Name (type = personal)
NamePart (type = family)
Hu
NamePart (type = given)
Zhichao
DisplayForm
Zhichao Hu
Affiliation
Advisory Committee
Role
RoleTerm (authority = RULIB)
outside member
Name (type = corporate)
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Rutgers University
Role
RoleTerm (authority = RULIB)
degree grantor
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School of Graduate Studies
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school
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Text
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theses
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2019
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2019-10
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2019
Language
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English
Abstract (type = abstract)
Luminescent metal‐organic frameworks (LMOFs) are a class of supramolecular material composed of metal ions connected by organic ligands to form crystalline frameworks that emit light when excited. In these organic‐inorganic frameworks, single metal ions or metal ion clusters serve as ‘nodes’, with rigid multidentate ligand molecules linking these nodes into an ordered three‐dimensional lattice. Luminescence can arise from the metal nodes, organic ligands, or interactions between these components. Because the properties of an LMOF depend on both the characteristics of the building blocks used to construct it and how these building blocks interact with each other, altering these building blocks can impart an incredible degree of tunability to an LMOF’s properties. However, the complex interactions that are possible between framework components render the rational design of LMOFs with specific luminescent properties challenging.

This work used a combination of spectroscopic, crystallographic, and theoretical methods to understand the chemical and optoelectronic processes that take place within LMOFs. This understanding was then used to develop broadly‐applicable strategies for the rational design of LMOFs for commercial applications, which were in turn used to design and synthesize several new LMOFs with record‐breaking performance as optical sensors and phosphor materials. LMOF‐241 was designed for the detection of common food‐contaminating mycotoxins using a photoinduced electron transfer mechanism. It was used to optically detect mycotoxins with unprecedented speed and sensitivity, with detection limits on the ppb‐scale. A chromophoric‐ligand strategy was previously used to design LMOF‐231 for use as a blue‐excitable, yellow‐emitting phosphor material in white LED bulbs, and it demonstrated the highest quantum yield for any yellow‐emitting LMOF reported (76%). This exceptional quantum yield was improved to 88% in LMOF‐231‐F0.2, which was designed using a bandgap–modulation strategy. Finally, the effect of post‐synthetic structural rigidification on LMOF quantum yield was studied using the isostructural LMOFs‐263 and 301. This work demonstrated that rigidification via structural packing is an effective strategy for increasing luminescence efficiency, with LMOF‐263 demonstrating a nearly five‐fold increase in quantum yield.
Subject (authority = RUETD)
Topic
Chemistry and Chemical Biology
Subject (authority = local)
Topic
Metal-organic framework
Subject (authority = LCSH)
Topic
Organometallic compounds
Subject (authority = LCSH)
Topic
Electroluminescence
RelatedItem (type = host)
TitleInfo
Title
Rutgers University Electronic Theses and Dissertations
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ETD_10383
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application/pdf
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text/xml
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1 online resource (xv, 89 pages) : illustrations
Note (type = degree)
Ph.D.
Note (type = bibliography)
Includes bibliographical references
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School of Graduate Studies Electronic Theses and Dissertations
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rucore10001600001
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Identifier (type = doi)
doi:10.7282/t3-mazg-4579
Genre (authority = ExL-Esploro)
ETD doctoral
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Rights

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The author owns the copyright to this work.
RightsHolder (type = personal)
Name
FamilyName
Lustig
GivenName
William
Role
Copyright Holder
RightsEvent
Type
Permission or license
DateTime (encoding = w3cdtf); (qualifier = exact); (point = start)
2019-09-30 21:13:11
AssociatedEntity
Name
William Lustig
Role
Copyright holder
Affiliation
Rutgers University. School of Graduate Studies
AssociatedObject
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License
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Author Agreement License
Detail
I hereby grant to the Rutgers University Libraries and to my school the non-exclusive right to archive, reproduce and distribute my thesis or dissertation, in whole or in part, and/or my abstract, in whole or in part, in and from an electronic format, subject to the release date subsequently stipulated in this submittal form and approved by my school. I represent and stipulate that the thesis or dissertation and its abstract are my original work, that they do not infringe or violate any rights of others, and that I make these grants as the sole owner of the rights to my thesis or dissertation and its abstract. I represent that I have obtained written permissions, when necessary, from the owner(s) of each third party copyrighted matter to be included in my thesis or dissertation and will supply copies of such upon request by my school. I acknowledge that RU ETD and my school will not distribute my thesis or dissertation or its abstract if, in their reasonable judgment, they believe all such rights have not been secured. I acknowledge that I retain ownership rights to the copyright of my work. I also retain the right to use all or part of this thesis or dissertation in future works, such as articles or books.
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Type
Embargo
DateTime (encoding = w3cdtf); (qualifier = exact); (point = start)
2019-10-31
DateTime (encoding = w3cdtf); (qualifier = exact); (point = end)
2020-05-01
Detail
Access to this PDF has been restricted at the author's request. It will be publicly available after May 1st, 2020.
Copyright
Status
Copyright protected
Availability
Status
Open
Reason
Permission or license
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2019-10-01T13:58:55
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2019-10-01T13:58:55
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