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Accessing High Order Modes From Populated Vibrational States of a Model System
Accessing High Order Modes From Populated Vibrational States of a Model System
Accessing High Order Modes From Populated Vibrational States of a Model System

상세정보

자료유형  
 학위논문 서양
최종처리일시  
20260202105118
ISBN  
9798291505021
DDC  
541
저자명  
Oram, Kelson J. H.
서명/저자  
Accessing High Order Modes From Populated Vibrational States of a Model System
발행사항  
[Sl] : The University of Wisconsin - Madison, 2025
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2025
형태사항  
144 p
주기사항  
Source: Dissertations Abstracts International, Volume: 87-02, Section: B.
주기사항  
Advisor: Wright, John C.
학위논문주기  
Thesis (Ph.D.)--The University of Wisconsin - Madison, 2025.
초록/해제  
요약Multiresonant coherent multidimensional spectroscopy (MR-CMDS) can combine vibrational and electronic resonances at ultrafast time scales to probe the fundamental interactions and dynamics of molecular systems. The nonlinear methods may be used to interrogate the potential energy surface of a system, which is of broad interest. In this dissertation, the high order vibrational modes of a rhodium dicarbonyl compound are accessed by vibrational ladder climbing. Successive populations are achieved by excitation from a single intense IR laser pulse which interacts with the sample multiple times. From the populated vibrational states, a coherent probe measures high order overtone and combination band coherences of the asymmetric and symmetric carbonyl stretches. The high order vibrational states are directly related to the potential energy surface. The proposed vibrational ladder climbing pathway is explored by varying the frequencies and time delays of the excitation pulses. An estimate of the nonlinear susceptibility constant χ(3) is determined and used to compare the relative intensities of spectral features linked to vibrational populations. This work was done with a newly developed mixed-domain multidimensional spectrometer. The new instrument has three independently tunable optical parametric amplifiers which can probe resonances from the mid-infrared to the ultraviolet. The multidimensional spectrometer can perform a variety of MR-CMDS experiments. This work demonstrates the capabilities of MR-CMDS experiments and applies them to a model compound.
일반주제명  
Physical chemistry
일반주제명  
Chemistry
일반주제명  
Analytical chemistry
키워드  
Anharmonicities
키워드  
Multiresonant Coherent multidimensional spectroscopy
키워드  
Ultrafast spectroscopy
키워드  
Vibrational ladder climbing
기타저자  
The University of Wisconsin - Madison Chemistry
기본자료저록  
Dissertations Abstracts International. 87-02B.
전자적 위치 및 접속  
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■035    ▼a(MiAaPQ)AAI32237886
■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a541
■1001  ▼aOram,  Kelson  J.  H.
■24510▼aAccessing  High  Order  Modes  From  Populated  Vibrational  States  of  a  Model  System
■260    ▼a[Sl]▼bThe  University  of  Wisconsin  -  Madison▼c2025
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2025
■300    ▼a144  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  87-02,  Section:  B.
■500    ▼aAdvisor:  Wright,  John  C.
■5021  ▼aThesis  (Ph.D.)--The  University  of  Wisconsin  -  Madison,  2025.
■520    ▼aMultiresonant  coherent  multidimensional  spectroscopy  (MR-CMDS)  can  combine  vibrational  and  electronic  resonances  at  ultrafast  time  scales  to  probe  the  fundamental  interactions  and  dynamics  of  molecular  systems.  The  nonlinear  methods  may  be  used  to  interrogate  the  potential  energy  surface  of  a  system,  which  is  of  broad  interest.  In  this  dissertation,  the  high  order  vibrational  modes  of  a  rhodium  dicarbonyl  compound  are  accessed  by  vibrational  ladder  climbing.  Successive  populations  are  achieved  by  excitation  from  a  single  intense  IR  laser  pulse  which  interacts  with  the  sample  multiple  times.  From  the  populated  vibrational  states,  a  coherent  probe  measures  high  order  overtone  and  combination  band  coherences  of  the  asymmetric  and  symmetric  carbonyl  stretches.  The  high  order  vibrational  states  are  directly  related  to  the  potential  energy  surface.  The  proposed  vibrational  ladder  climbing  pathway  is  explored  by  varying  the  frequencies  and  time  delays  of  the  excitation  pulses.  An  estimate  of  the  nonlinear  susceptibility  constant  χ(3)  is  determined  and  used  to  compare  the  relative  intensities  of  spectral  features  linked  to  vibrational  populations.  This  work  was  done  with  a  newly  developed  mixed-domain  multidimensional  spectrometer.  The  new  instrument  has  three  independently  tunable  optical  parametric  amplifiers  which  can  probe  resonances  from  the  mid-infrared  to  the  ultraviolet.  The  multidimensional  spectrometer  can  perform  a  variety  of  MR-CMDS  experiments.  This  work  demonstrates  the  capabilities  of  MR-CMDS  experiments  and  applies  them  to  a  model  compound.
■590    ▼aSchool  code:  0262.
■650  4▼aPhysical  chemistry
■650  4▼aChemistry
■650  4▼aAnalytical  chemistry
■653    ▼aAnharmonicities
■653    ▼aMultiresonant  Coherent  multidimensional  spectroscopy
■653    ▼aUltrafast  spectroscopy
■653    ▼aVibrational  ladder  climbing
■690    ▼a0494
■690    ▼a0485
■690    ▼a0486
■71020▼aThe  University  of  Wisconsin  -  Madison▼bChemistry.
■7730  ▼tDissertations  Abstracts  International▼g87-02B.
■790    ▼a0262
■791    ▼aPh.D.
■792    ▼a2025
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17359429▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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