diff options
| -rw-r--r-- | bibliography.bib | 13 | ||||
| -rw-r--r-- | introduction/chapter.tex | 30 | ||||
| -rw-r--r-- | todo.org | 5 |
3 files changed, 36 insertions, 12 deletions
diff --git a/bibliography.bib b/bibliography.bib index 0eca1d0..4e1e234 100644 --- a/bibliography.bib +++ b/bibliography.bib @@ -1451,6 +1451,19 @@ publisher = {The Optical Society},
}
+@article{KeustersDorine1999a,
+ author = {Dorine Keusters and Howe-Siang Tan and Warren},
+ title = {Role of Pulse Phase and Direction in Two-Dimensional Optical Spectroscopy},
+ journal = {The Journal of Physical Chemistry A},
+ volume = 103,
+ number = 49,
+ pages = {10369--10380},
+ year = 1999,
+ doi = {10.1021/jp992325b},
+ month = {dec},
+ publisher = {American Chemical Society ({ACS})},
+}
+
@article{KeustersDorine2004a,
author = {Keusters, Dorine and Warren, Warren S.},
title = {{Propagation effects on the peak profile in two-dimensional optical photon echo
diff --git a/introduction/chapter.tex b/introduction/chapter.tex index f6adc46..b3d9df5 100644 --- a/introduction/chapter.tex +++ b/introduction/chapter.tex @@ -16,10 +16,10 @@ Coherent multidimensional spectroscopy (CMDS) is a family of experimental strategies capable of
providing unique insights into microscopic material physics. %
-It is similar to more familiar multidimensional NMR experiments \cite{ZhaoWei2000b,
- PakoulevAndreiV2006a}, although the implementation is different due to differences between the
-behavior of nuclear spin states (probed by NMR) and electronic and vibrational states (probed by
-CMDS). %
+It is similar to more familiar multidimensional NMR experiments \cite{KeustersDorine1999a,
+ ZhaoWei2000b, PakoulevAndreiV2006a}, although the implementation is different due to differences
+between the behavior of nuclear spin states (probed by NMR) and electronic and vibrational states
+(probed by CMDS). %
CMDS can resolve couplings between states, and can decongest spectra by taking advantage of
dimensionality and selection rules. %
With the advent of ultrafast lasers, CMDS can resolve dynamics in excited states and the coupling
@@ -146,6 +146,16 @@ complementary to chopping. % Automated poynting correction and power correction can account for non-idealities in OPA
performance. %
+MR-CMDS instruments rely on OPAs as tunable light sources. %
+OPAs are very sensitive to changes in upstream lasers and lab conditions, so OPA tuning is
+regularly required. %
+Manual OPA tuning can easily take a full day of human effort. %
+Furthermore, manual tuning typically results in inferior tuning curves, since it is difficult for
+humans to consider all available information simultaneously. %
+Automated OPA tuning makes OPA upkeep easier, faster and more reproducible, facilitating higher
+throughput, higher quality frequency domain experiments. %
+Chapter \ref{cha:opa} describes fully automated tuning algorithms which I have developed. %
+
The theory that is used to describe CMDS is typically derived in one of two limits. %
In the impulsive limit, pulses are broad in frequency and short in time compared to material
resonances. %
@@ -183,8 +193,8 @@ They are easy to synthesize, store and prepare in the solution phase, and they h 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. %
+Using 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. %
@@ -213,23 +223,23 @@ frequency-frequency-delay transient grating spectroscopy to understand the basic 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
+We describe 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. %
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. %
+that are speculated to participate in conductivity. %
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. %
+We cannot fully determine 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. %
@@ -1,4 +1,5 @@ -* TODO headers :int: +* CANCELED headers :int: + CLOSED: [2018-04-15 Sun 15:50] * TODO cite important CMDS discoveries, reviews :int: * TODO incorporate Nancy's comments :int: * TODO incorporate Claire's comments :int: @@ -56,7 +57,7 @@ * TODO generalizability :opa: * TODO future directions :opa: * TODO figure captions :opa: -* DONE insert content from main 0:00:00 :pss: +* DONE insert content from main :pss: CLOSED: [2018-04-12 Thu 21:04] * IDEA insert content from SI :pss: * DONE insert content from main :psg: |