2018-04-13 18:16

3 files changed, 68 insertions, 32 deletions

diff --git a/abstract.tex b/abstract.tex
index fdaf7b9..8dd75a3 100644
--- a/abstract.tex
+++ b/abstract.tex
@@ -45,6 +45,6 @@ development work.  %
 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}).  %
-Finally, \hyperref[prt:applications]{Part III: Applications} presents three examples where these
+Finally, \hyperref[prt:applications]{Part III: Applications} presents four examples where these
 instruments, with these improvements, have been used to address chemical questions in semiconductor
 systems.  %
\ No newline at end of file
diff --git a/dissertation.cls b/dissertation.cls
index d7fc4b2..e540902 100644
--- a/dissertation.cls
+++ b/dissertation.cls
@@ -190,6 +190,8 @@
 anchorcolor=black]{hyperref}
 \RequirePackage[all]{hypcap}  % helps hyperref work properly
 
+\renewcommand{\chapterautorefname}{Chapter}
+
 % --- bibliography --------------------------------------------------------------------------------
 
 \RequirePackage[backend=biber, natbib=true, sorting=none, maxbibnames=99, isbn=false]{biblatex}
diff --git a/introduction/chapter.tex b/introduction/chapter.tex
index 18ffd06..fe43cb4 100644
--- a/introduction/chapter.tex
+++ b/introduction/chapter.tex
@@ -25,9 +25,9 @@ dimensionality and selection rules.  %
 With the advent of ultrafast lasers, CMDS can resolve dynamics in excited states and the coupling

 between them. \cite{RentzepisPM1970a}  %

 

-CMDS is most often performed in the time domain, where multiple broadband pulses are scanned to

-collect a multidimensional interferogram. \cite{MukamelShaul2009a, GallagherSarahM1998a}  %

-% BJT: scanned in WHAT? delay? time?

+CMDS is most often performed in the time domain, where multiple broadband pulses are scanned in

+time (phase) to collect a multidimensional interferogram. \cite{MukamelShaul2009a,

+  GallagherSarahM1998a}  %

 This technique is fast and robust---it has even been performed on a single shot.

 \cite{HarelElad2010a}  %

 However time-domain CMDS has some fundamental limitations:

@@ -132,7 +132,6 @@ decreased acquisition times by up to two orders of magnitude.  %
 Like any analytical technique, MR-CMDS is subject to artifacts: features of the data that are

 caused by instrumental imperfections or limitations, and do not reflect the intrinsic material

 response that is of interest.  %

-% JCW: HOW THE EXPERIMENT WAS DONE, NOT WHAT IT IS HOPING TO MEASURE

 For example, consider well-known artifacts such as absorptive effects \cite{CarlsonRogerJohn1989a},

 pulse effects \cite{SpencerAustinP2015a}, and window contributions \cite{MurdochKiethM2000a}.  %

 Since MR-CMDS is a very active experiment, with many moving motors, an active approach to artifact

@@ -154,13 +153,13 @@ Resonant responses are impulsive, like a hammer hitting a bell.  %
 The impulsive limit is particularly well suited for describing time domain experiments.  %

 In the driven limit, pulses are narrow in frequency and long in time compared to material

 response.  %

-Resonant responses are driven, like a jiggling jello dessert sitting on a washing machine.  %

+Resonant responses are driven, like jiggling jello dessert sitting on a washing machine.  %

 The expected spectrum in both of these limits can be computed analytically.  %

 Things get more complicated in the mixed domain, where pulses have similar bandwidth as the

 material response. %

 Experiments in this domain are a practical necessity as CMDS addresses systems with very fast

-dephasing times. \cite{SmallwoodChristopherL2016a, PerlikVaclav2017a}  % BJT: connect bw and

-                                % dephasing

+dephasing times. \cite{SmallwoodChristopherL2016a, PerlikVaclav2017a}

+% BJT: connect bw and dephasing

 At the same time, the marginal resolution in frequency \emph{and} time that the mixed domain

 possess promises huge potential in pathway resolution and decongestion.

 \cite{PakoulevAndreiV2009a}  %

@@ -170,34 +169,69 @@ An intuitive description of mixed-domain experiments is given.  %
 False signatures of material correlation are discussed, and strategies for resolving true material

 correlation are defined.  %

 

-In \hyperref[prt:applications]{Part III: Applications}, three projects in which MR-CMDS was used to

+In \hyperref[prt:applications]{Part III: Applications}, four projects in which MR-CMDS was used to

 answer chemical questions in materials systems are described.  %

 These chapters do not directly address improvements to the MR-CMDS methodology, but instead serve

 as case studies in the potential of MR-CMDS and the utility of the improvements described in

 \autoref{prt:development}.  %

 

-[PARAGRAPH ABOUT PbSe QUANTUM DOTS]

-

-%Chapter \ref{cha:pbx} describes a series of experiments performed on PbSe quantum dots.  %

-%Quantum dots are an excellent [STARTING SAMPLE... BEGINNING]

-%PbSe quantum dots are useful because [...]  %

-%We learned [...]  %

-

-[PARAGRAPH ABOUT MOS2]

-

-%Chapter [...] describes an experiment performed on MoS2.

-%MoS2 is useful because [...]  %

-%We learned [...]  %

-

-[PARAGRAPH ABOUT PEDOT:PSS]

-

-%Chapter [...] describes an experiment performed on PEDOT:PSS.

-%useful because...

-%we learned...

-

-% BJT: consider getting rid of the following paragraph

-% if it remains, it needs to address a more 'broader impacts approach' rather than simply

-% re-summarizing

+In \autoref{cha:pss}, we employ transient grating MR-CMDS to interrogate the photophysics of

+lead selenide (PbSe) quantum dots (QDs).  %

+PbSe QDs are an interesting semiconductor system with many appealing properties for basic method

+development work.  %

+They are easy to synthesize, store and prepare in the solution phase, and they have bright and

+relatively narrow band-edge excitons which are easy to interrogate using MR-CMDS.  %

+In \autoref{cha:pss}, we describe a simple approach to extracting the quantitative third-order

+susceptibility of PbSe quantum dots using MR-CMDS.  %

+Using a simple approach of standard dilutions, we define this susceptibility in ratio to the known

+well-quantified susceptibility of our solvent and cuvette windows.  %

+A few-parameter model is employed to extract this ratio.  %

+We are optimistic that this approach will be generally applicable, making it simple to perform

+quantitative solution-phase MR-CMDS.  %

+

+In \autoref{cha:psg} we continue to investigate PbSe QDs.  %

+Here we combine transient grating and transient absorption MR-CMDS to learn more about the

+nonlinear spectrum near the band edge, around the 1S exciton.  %

+By combining both methods with the information from \autoref{cha:pss}, we are able to extract the

+complete amplitude and phase of the non-linear susceptibility.  %

+We develop a simulation that relates the microscopic physics of PbSe electronic states to transient

+grating and transient absorption spectra, and fit our model to both spectra simultaneously.  %

+Our model reveals the presence of continuum transitions, mostly invisible in typical transient

+absorption experiments.  %

+We show that our model is able to describe spectra from two different syntheses with two different

+sizes of quantum dot.  %

+

+In \autoref{cha:mx2} we report the first MR-CMDS study performed on a molybdenum disulfide thin

+film.  %

+MoS\textsubscript{2} is a member of a class of materials called transition metal dichacolgenides

+which have recently attracted a large amount of attention for their unique photophysical

+properties.  %

+These thin films have relatively low optical density and are highly scattering, making them

+particularly challenging for MR-CMDS experiments.  %

+We employed several strategies to overcome these challenges, and performed three dimensional

+frequency-frequency-delay transient grating spectroscopy to understand the basic coupling and

+dynamics of MoS\textsubscript{2}.  %

+We show that the band-edge excitons of MoS\textsubscript{2} are not easily resolved, and the

+dynamics of MoS\textsubscript{2} are fast.  %

+We develop a picture of MoS\textsubscript{2} electronic states that is consistent with our

+results.  %

+

+In \autoref{cha:pps} we use MR-CMDS to interrogate the dynamics of electronic states of

+(PEDOT:PSS).  %

+PEDOT:PSS is a transparent, electrically conductive polymer.  %

+The exact origin of the conductivity is not well understood, so it is unclear how to improve the

+conductivity or synthesize other conductive polymers.  %

+We performed photon echo experiments on PEDOT:PSS, directly interrogating the electronic states

+that are responsible for conductivity in the polymer.  %

+Using a sophisticated model extended from the work in \autoref{cha:mix}, we constrain the pure and

+ensemble dephasing lifetimes of PEDOT:PSS.  %

+These lifetimes can be directly related to the homogeneous and inhomogeneous broadening parameters

+in PEDOT:PSS.  %

+Amazingly, we find that PEDOT:PSS has very broad homogeneous \emph{and} inhomogeneous

+linewidths.  %

+We cannot constrain either quantity, but we can put lower limits on both.  %

+This basic information is complementary to other experiments in the ongoing effort to fully

+understand PEDOT:PSS.  %

 

 Despite challenges in software, hardware, and theory MR-CMDS is a crucial tool in the hands of

 scientists.  %

@@ -206,4 +240,4 @@ hardware development.  %
 PyCMDS has enabled new experiments, and has made data collection faster and more artifact-free.  %

 WrightTools has trivialized data processing, tightening the loop between idea and execution.  %

 Theory can be used to guide experimental insight in the promising, if challenging, mixed domain.  %

-Applications of these ideas in three materials are presented.  %

+Applications of these ideas in three material systems are presented.  %