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020 ▼a 9781085611602
035 ▼a (MiAaPQ)AAI13899320
040 ▼a MiAaPQ ▼c MiAaPQ ▼d 247004
0820 ▼a 540
1001 ▼a Pun, Andrew B.
24510 ▼a Exciton Fission and Fusion.
260 ▼a [S.l.]: ▼b Columbia University., ▼c 2019.
260 1 ▼a Ann Arbor: ▼b ProQuest Dissertations & Theses, ▼c 2019.
300 ▼a 338 p.
500 ▼a Source: Dissertations Abstracts International, Volume: 81-02, Section: B.
500 ▼a Advisor: Campos, Luis M.
5021 ▼a Thesis (Ph.D.)--Columbia University, 2019.
506 ▼a This item must not be sold to any third party vendors.
520 ▼a The crux of all modern semiconductor technology is the exciton, the bound electron-hole pair that drives everything from photovoltaics to light emitting diodes to transistors. This dissertation explores how we can develop materials that are able to control the energetics of excitons, by splitting them and combining them. Also explored are the applications allowed by the control of exciton energetics.The topics covered in this thesis are singlet exciton fission, and triplet fusion upconversion. Chapter 1 will introduce these concepts, and provide an overview of these fields. Chapter 2 discusses the singlet fission properties of a fully conjugated tetracene polymer and its derivatives. This chapter includes the synthesis of these materials, their photophysical properties, as well as their incorporation into bilayer semiconducting devices and their properties under an applied magnetic field. Chapter 3 explores the study of an organic-inorganic hybrid singlet fission triplet acceptor complex. A singlet fission capable pentacene dimer was covalently linked to an iron-oxo cluster with an electron affinity appropriate to accept triplets generated from singlet fission. This chapter explores the synthesis and photophysical properties of this hybrid complex, as well as the nature of the triplet pair state generated from intramolecular singlet fission.In Chapter 4, a new design rule for intramolecular singlet fission is studied, the energy sink. A series of pentacene dimers spaced by tetracene bridges are synthesized, and their singlet fission properties are explored via transient absorption spectroscopy and time resolved electron spin resonance spectroscopy.Chapter 5 begins the portion of the thesis focused on triplet fusion upconversion. The lessons learned from previous work in intramolecular singlet fission are applied to synthesize more efficient annihilators for upconversion. A series of tetracene dimers are synthesized, and their upconversion properties are explored. The work demonstrates intramolecular triplet fusion as a method to enhance the performance of existing annihilators.Chapter 6 details the discovery that diketopyrrolopyrroles can be used as upconversion annihilators. The advantages of these materials relative to existing annihilators are explained. Energetic design rules for upconversion annihilators are also discussed.Finally, in Chapter 7 a new application of triplet fusion upconversion is explored: infrared light sensitized photoredox catalysis.
590 ▼a School code: 0054.
650 4 ▼a Chemistry.
690 ▼a 0485
71020 ▼a Columbia University. ▼b Chemistry.
7730 ▼t Dissertations Abstracts International ▼g 81-02B.
773 ▼t Dissertation Abstract International
790 ▼a 0054
791 ▼a Ph.D.
792 ▼a 2019
793 ▼a English
85640 ▼u http://www.riss.kr/pdu/ddodLink.do?id=T15492043 ▼n KERIS ▼z 이 자료의 원문은 한국교육학술정보원에서 제공합니다.
980 ▼a 202002 ▼f 2020
990 ▼a ***1008102
991 ▼a E-BOOK