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Polarization-Resolved Plasmon-Enhanced Single-Molecule Microscopy
Polarization-Resolved Plasmon-Enhanced Single-Molecule Microscopy
Polarization-Resolved Plasmon-Enhanced Single-Molecule Microscopy

상세정보

자료유형  
 학위논문 서양
최종처리일시  
20250211153015
ISBN  
9798384045731
DDC  
620
저자명  
Chattopadhyay, Saaj.
서명/저자  
Polarization-Resolved Plasmon-Enhanced Single-Molecule Microscopy
발행사항  
[Sl] : University of Michigan, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
109 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-03, Section: B.
주기사항  
Advisor: Biteen, Julie.
학위논문주기  
Thesis (Ph.D.)--University of Michigan, 2024.
초록/해제  
요약Polarization-resolved microscopy adds a new control variable in single-molecule imaging and analysis, enabling the study of chiral light-matter interactions. I built the optics and experimental workflow to incorporate polarization control in the excitation and emission pathways of a wide-field epifluorescence microscope. I implemented the Jones formalism of optics and incorporated polarization optics elements. In this thesis, I present my workflow and the results of single-molecule and single-particle imaging under polarized plane-wave excitation.There were broadly two motivations for introducing polarization-resolved excitation: (1) To measure differential absorption of circularly polarized light at a single-particle and single-molecule level to uncover any heterogeneities that could be hidden in an ensemble measurement and, (2) To study the coupling of Au nanoantennas with circularly polarized light to understand the potential for plasmon-coupled fluorescence-detected circular dichroism of single molecules.After implementing polarization-resolved microscopy, I tested and disproved two proposed theories for unusual observations in the bulk measurement of Au nanorods mixed with insulin fibrils and thioflavin T, a dye that intercalates into the insulin fibrils.In addition to instrumentation that gives control over the polarization of the far-field electromagnetic field, I relied on numerical simulations to visualize the near-field electromagnetic field of the nanoantennas. The near-field of the antennas is changed drastically by changing the incident polarization. I also calculated the optical chirality, or the local twist of the field, to predict where absorption dissymmetry would be enhanced for chiral molecules. Simulations of the radiated power explain how the detected emission from linear emitters near chiral antennas is mis-handed: detected as circularly polarized instead of linearly polarized.Results from my single-molecule experiments using DNA-bound chiral fluorophores indicate that to compare the number and intensity of localizations, we need to first ensure that the adsorption characteristics are the same. The only significant indicator of molecular chirality was the increased detectability of right-handed J-dimers of Cy5 near achiral Au NP dimers under right circularly polarized illumination.
일반주제명  
Engineering
일반주제명  
Physical chemistry
일반주제명  
Optics
일반주제명  
Applied physics
키워드  
Plasmonics
키워드  
Single-molecule fluorescence imaging
키워드  
Photonics
키워드  
Polarization optics
키워드  
Optical chirality
기타저자  
University of Michigan Applied Physics
기본자료저록  
Dissertations Abstracts International. 86-03B.
전자적 위치 및 접속  
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MARC

 008250123s2024        us                              c    eng  d
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■020    ▼a9798384045731
■035    ▼a(MiAaPQ)AAI31631513
■035    ▼a(MiAaPQ)umichrackham005803
■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a620
■1001  ▼aChattopadhyay,  Saaj.
■24510▼aPolarization-Resolved  Plasmon-Enhanced  Single-Molecule  Microscopy
■260    ▼a[Sl]▼bUniversity  of  Michigan▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a109  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-03,  Section:  B.
■500    ▼aAdvisor:  Biteen,  Julie.
■5021  ▼aThesis  (Ph.D.)--University  of  Michigan,  2024.
■520    ▼aPolarization-resolved  microscopy  adds  a  new  control  variable  in  single-molecule  imaging  and  analysis,  enabling  the  study  of  chiral  light-matter  interactions.  I  built  the  optics  and  experimental  workflow  to  incorporate  polarization  control  in  the  excitation  and  emission  pathways  of  a  wide-field  epifluorescence  microscope.  I  implemented  the  Jones  formalism  of  optics  and  incorporated  polarization  optics  elements.  In  this  thesis,  I  present  my  workflow  and  the  results  of  single-molecule  and  single-particle  imaging  under  polarized  plane-wave  excitation.There  were  broadly  two  motivations  for  introducing  polarization-resolved  excitation:  (1)  To  measure  differential  absorption  of  circularly  polarized  light  at  a  single-particle  and  single-molecule  level  to  uncover  any  heterogeneities  that  could  be  hidden  in  an  ensemble  measurement  and,  (2)  To  study  the  coupling  of  Au  nanoantennas  with  circularly  polarized  light  to  understand  the  potential  for  plasmon-coupled  fluorescence-detected  circular  dichroism  of  single  molecules.After  implementing  polarization-resolved  microscopy,  I  tested  and  disproved  two  proposed  theories  for  unusual  observations  in  the  bulk  measurement  of  Au  nanorods  mixed  with  insulin  fibrils  and  thioflavin  T,  a  dye  that  intercalates  into  the  insulin  fibrils.In  addition  to  instrumentation  that  gives  control  over  the  polarization  of  the  far-field  electromagnetic  field,  I  relied  on  numerical  simulations  to  visualize  the  near-field  electromagnetic  field  of  the  nanoantennas.  The  near-field  of  the  antennas  is  changed  drastically  by  changing  the  incident  polarization.  I  also  calculated  the  optical  chirality,  or  the  local  twist  of  the  field,  to  predict  where  absorption  dissymmetry  would  be  enhanced  for  chiral  molecules.  Simulations  of  the  radiated  power  explain  how  the  detected  emission  from  linear  emitters  near  chiral  antennas  is  mis-handed:  detected  as  circularly  polarized  instead  of  linearly  polarized.Results  from  my  single-molecule  experiments  using  DNA-bound  chiral  fluorophores  indicate  that  to  compare  the  number  and  intensity  of  localizations,  we  need  to  first  ensure  that  the  adsorption  characteristics  are  the  same.  The  only  significant  indicator  of  molecular  chirality  was  the  increased  detectability  of  right-handed  J-dimers  of  Cy5  near  achiral  Au  NP  dimers  under  right  circularly  polarized  illumination.
■590    ▼aSchool  code:  0127.
■650  4▼aEngineering
■650  4▼aPhysical  chemistry
■650  4▼aOptics
■650  4▼aApplied  physics
■653    ▼aPlasmonics
■653    ▼aSingle-molecule  fluorescence  imaging
■653    ▼aPhotonics
■653    ▼aPolarization  optics
■653    ▼aOptical  chirality
■690    ▼a0752
■690    ▼a0494
■690    ▼a0537
■690    ▼a0215
■71020▼aUniversity  of  Michigan▼bApplied  Physics.
■7730  ▼tDissertations  Abstracts  International▼g86-03B.
■790    ▼a0127
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17164545▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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