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% graduate school requirement: less than 350 words
\chapter*{Abstract}
\addcontentsline{toc}{chapter}{Abstract}
Coherent multidimensional spectroscopy (CMDS) encompasses a family of experimental strategies
involving the nonlinear interaction between electric fields and a material under investigation. %
This approach has several unique capabilities:
\begin{denumerate}
\item resolving congested states \cite{ZhaoWei1999b, DonaldsonPaulMurray2008a}
\item extracting spectra that would otherwise be selection-rule disallowed
\cite{BoyleErinSelene2013b, BoyleErinSelene2014b},
\item resolving fully coherent dyanmics \cite{PakoulevAndreiV2009a},
\item measuring coupling \cite{WrightJohnCurtis2011a}, and
\item resolving ultrafast dynamics. % TODO: cite
\end{denumerate}
CMDS can be collected in the frequency or the time domain, and each approach has advantages and
disadvantages. \cite{ParkKisam1998a} %
Frequency domain ``Multi-resonant'' CMDS (MR-CMDS) requires pulsed ultrafast light sources with
tunable output frequencies. %
These pulses are directed into a material under investigation. %
The pulses interact with the material, and due to the specific interference between the multiple
fields the material is driven to emit a new pulse: the MR-CMDS signal. %
This signal may be different in frequency from the input pulses, and it may travel in a new
direction depending on the exact experiment being performed. %
The MR-CMDS experiment involves tracking the intensity of this output signal as a function of
different properties of the excitation pulses. %
These properties include
1. frequency
2. relative arrival time and separation (delay)
3. fluence \cite{OmariAbdoulghafar2012a, SheikBahaeMansoor1990a}, and
4. polarization \cite{FournierFrederic2009a}, among others. %
Thus MR-CMDS can be thought of as a multidimensional experimental space, where experiments
typically involve explorations in one to four of the properties above. %
Because MR-CMDS is a family of related-but-separate experiments, each of them a multidimensional
space, there are special challenges that must be addressed when designing a general-purpose MR-CMDS
instrument. %
These issues require development of software, hardware, and theory. %
Five different improvements to MR-CMDS are presented in this dissertation: 1. processing software
(\autoref{cha:pro}), 2. acquisition software (\autoref{cha:acq}) 3, active artifact correction
(\autoref{cha:act}), 4. automated OPA calibration (\autoref{cha:opa}), and 5. finite pulse
accountancy (\autoref{cha:mix}). %
\hyperref[prt:background]{Part I: Background} introduces relevant literature which informs on this
development work. %
Finally, \hyperref[prt:applications]{Part III: Applications} presents three examples where these
instruments, with these improvements, have been used to address chemical questions in
semiconductor systems. %
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