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Complexation and Photophysical Phenomena in Multi-Component Organic Semiconductor Materials Systems
Complexation and Photophysical Phenomena in Multi-Component Organic Semiconductor Material...
Complexation and Photophysical Phenomena in Multi-Component Organic Semiconductor Materials Systems

상세정보

자료유형  
 학위논문 서양
최종처리일시  
20250211152034
ISBN  
9798384463849
DDC  
539
저자명  
Ivancevic, Marko R.
서명/저자  
Complexation and Photophysical Phenomena in Multi-Component Organic Semiconductor Materials Systems
발행사항  
[Sl] : Princeton University, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
185 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-04, Section: B.
주기사항  
Advisor: Loo, Yueh-Lin.
학위논문주기  
Thesis (Ph.D.)--Princeton University, 2024.
초록/해제  
요약Organic semiconductors are promising materials due to their tunable optical properties, facile processing, and mechanical flexibility. Advancing their applications requires a deeper understanding of organic semiconductors, particularly how intermolecular interactions can be manipulated to achieve selective complexation. Improving our understanding of organic semiconductor phosphorescence, an uncommon photophysical process of organic semiconductors, is also essential. Multi-component organic semiconductor systems are useful for such investigations. In exploring fullerene-buckybowl solution complexation, we identify extending buckybowl π-surfaces strengthens buckybowl-fullerene complexation. We find stronger complexation with fullerenes when the buckybowl dipole moment is increased through heteroatom inclusion.We investigate second-scale room temperature phosphorescence of organic semiconductors, a phenomenon known as ultralong room temperature phosphorescence (URTP). URTP is generally rare due to quenching by nonradiative recombination processes. We enable URTP in various organic semiconductors by embedding them in rigid polymer hosts and thermally annealing to induce sub-micron aggregation. We deduce sub-micron organic semiconductor aggregates suppress nonradiative recombination and reduce diffusional exciton quenching, and we propose URTP is more ubiquitous than previously thought.We find contorted hexabenzocoronene (cHBC) exhibits uniquely efficient red URTP. This stems from the proximity of a higher-lying triplet to the lowest-lying singlet enhancing intersystem crossing, and comparatively slow fluorescence decay. Eliminating C-H stretching modes, which disproportionately contribute to nonradiative recombination, by perdeuterating cHBC significantly prolongs its URTP lifetime, generating the longest-lived organic red-emitter to our knowledge. We developed a melt-processable perdeuterated cHBC and rubbery polymer composite that is compatible with 3D printing, enabling the development of customizable phosphorescent objects.We demonstrate ubiquitous access to URTP in nanoparticles comprising an organic semiconductor, homopolymer, and surfactant stabilizer made by flash nanoprecipitation (FNP). FNP offers precise control over nanoparticle size and composition. The URTP lifetime of the nanoparticle dispersions is stable to drying and redispersion. Moreover, this nanoparticle form factor is extendable to formulating anti-counterfeiting inks, or bioimaging.This thesis highlights the use of multi-component organic semiconductor systems to better understand the intermolecular interactions and photophysical phenomena governing their behavior. Using this insight, we realize unique properties of organic semiconductors that contribute to generating materials that can fit new applications.
일반주제명  
Molecular physics
일반주제명  
Organic chemistry
일반주제명  
Molecular chemistry
키워드  
Aggregation
키워드  
Buckybowls
키워드  
Nanoparticles
키워드  
Organic semiconductors
키워드  
Photophysics
기타저자  
Princeton University Chemical and Biological Engineering
기본자료저록  
Dissertations Abstracts International. 86-04B.
전자적 위치 및 접속  
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MARC

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■035    ▼a(MiAaPQ)AAI31335141
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■0820  ▼a539
■1001  ▼aIvancevic,  Marko  R.▼0(orcid)0000-0001-6308-5978
■24510▼aComplexation  and  Photophysical  Phenomena  in  Multi-Component  Organic  Semiconductor  Materials  Systems
■260    ▼a[Sl]▼bPrinceton  University▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a185  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-04,  Section:  B.
■500    ▼aAdvisor:  Loo,  Yueh-Lin.
■5021  ▼aThesis  (Ph.D.)--Princeton  University,  2024.
■520    ▼aOrganic  semiconductors  are  promising  materials  due  to  their  tunable  optical  properties,  facile  processing,  and  mechanical  flexibility.  Advancing  their  applications  requires  a  deeper  understanding  of  organic  semiconductors,  particularly  how  intermolecular  interactions  can  be  manipulated  to  achieve  selective  complexation.  Improving  our  understanding  of  organic  semiconductor  phosphorescence,  an  uncommon  photophysical  process  of  organic  semiconductors,  is  also  essential.  Multi-component  organic  semiconductor  systems  are  useful  for  such  investigations.  In  exploring  fullerene-buckybowl  solution  complexation,  we  identify  extending  buckybowl  π-surfaces  strengthens  buckybowl-fullerene  complexation.  We  find  stronger  complexation  with  fullerenes  when  the  buckybowl  dipole  moment  is  increased  through  heteroatom  inclusion.We  investigate  second-scale  room  temperature  phosphorescence  of  organic  semiconductors,  a  phenomenon  known  as  ultralong  room  temperature  phosphorescence  (URTP).  URTP  is  generally  rare  due  to  quenching  by  nonradiative  recombination  processes.  We  enable  URTP  in  various  organic  semiconductors  by  embedding  them  in  rigid  polymer  hosts  and  thermally  annealing  to  induce  sub-micron  aggregation.  We  deduce  sub-micron  organic  semiconductor  aggregates  suppress  nonradiative  recombination  and  reduce  diffusional  exciton  quenching,  and  we  propose  URTP  is  more  ubiquitous  than  previously  thought.We  find  contorted  hexabenzocoronene  (cHBC)  exhibits  uniquely  efficient  red  URTP.  This  stems  from  the  proximity  of  a  higher-lying  triplet  to  the  lowest-lying  singlet  enhancing  intersystem  crossing,  and  comparatively  slow  fluorescence  decay.  Eliminating  C-H  stretching  modes,  which  disproportionately  contribute  to  nonradiative  recombination,  by  perdeuterating  cHBC  significantly  prolongs  its  URTP  lifetime,  generating  the  longest-lived  organic  red-emitter  to  our  knowledge.  We  developed  a  melt-processable  perdeuterated  cHBC  and  rubbery  polymer  composite  that  is  compatible  with  3D  printing,  enabling  the  development  of  customizable  phosphorescent  objects.We  demonstrate  ubiquitous  access  to  URTP  in  nanoparticles  comprising  an  organic  semiconductor,  homopolymer,  and  surfactant  stabilizer  made  by  flash  nanoprecipitation  (FNP).  FNP  offers  precise  control  over  nanoparticle  size  and  composition.  The  URTP  lifetime  of  the  nanoparticle  dispersions  is  stable  to  drying  and  redispersion.  Moreover,  this  nanoparticle  form  factor  is  extendable  to  formulating  anti-counterfeiting  inks,  or  bioimaging.This  thesis  highlights  the  use  of  multi-component  organic  semiconductor  systems  to  better  understand  the  intermolecular  interactions  and  photophysical  phenomena  governing  their  behavior.  Using  this  insight,  we  realize  unique  properties  of  organic  semiconductors  that  contribute  to  generating  materials  that  can  fit  new  applications.
■590    ▼aSchool  code:  0181.
■650  4▼aMolecular  physics
■650  4▼aOrganic  chemistry
■650  4▼aMolecular  chemistry
■653    ▼aAggregation
■653    ▼aBuckybowls
■653    ▼aNanoparticles
■653    ▼aOrganic  semiconductors
■653    ▼aPhotophysics
■690    ▼a0609
■690    ▼a0490
■690    ▼a0431
■71020▼aPrinceton  University▼bChemical  and  Biological  Engineering.
■7730  ▼tDissertations  Abstracts  International▼g86-04B.
■790    ▼a0181
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17162626▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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