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diff --git a/PbSe_global_analysis/SI.tex b/PbSe_global_analysis/SI.tex deleted file mode 100644 index d3cb783..0000000 --- a/PbSe_global_analysis/SI.tex +++ /dev/null @@ -1,279 +0,0 @@ -% document -\documentclass[11pt, full]{article} -\usepackage[letterpaper, portrait, margin=0.75in]{geometry} -\usepackage{setspace} -\usepackage{color} - -% text -\usepackage[utf8]{inputenc} -\setlength\parindent{0pt} -\setlength{\parskip}{1em} -\usepackage{enumitem} -\renewcommand{\familydefault}{\sfdefault} -\newcommand{\RomanNumeral}[1]{\textrm{\uppercase\expandafter{\romannumeral #1\relax}}} - -% math -\usepackage{amssymb} -\usepackage{amsmath} -\usepackage[cm]{sfmath} -\usepackage{commath} -\usepackage{multirow} -\DeclareMathAlphabet{\mathpzc}{OT1}{pzc}{m}{it} - -% graphics -\usepackage{graphics} -\usepackage{graphicx} -\usepackage{epsfig} -\usepackage{epstopdf} -\usepackage{xpatch} -\graphicspath{{./figures/}} - -% "S" prefix -\renewcommand{\theequation}{S\arabic{equation}} -\renewcommand{\thefigure}{S\arabic{figure}} -\renewcommand{\thetable}{S\arabic{table}} - -% bibliography -\usepackage[backend=biber, natbib=true, url=false, sorting=none, maxbibnames=99]{biblatex} -\bibliography{mybib} - -% hyperref -\usepackage[colorlinks=true, linkcolor=black, urlcolor=blue, citecolor=black, anchorcolor=black]{hyperref} -\usepackage[all]{hypcap} % helps hyperref work properly - -\begin{document} -\pagenumbering{gobble} - -\begin{center} - \LARGE - - Supplementary Information - - Global Analysis of Transient Grating and Transient Absorption \\ of PbSe Quantum Dots - - \normalsize - - \textit{Daniel D. Kohler, Blaise J. Thompson, John C. Wright*} - - Department of Chemistry, University of Wisconsin--Madison\\ - 1101 University Ave., Madison, Wisconsin 53706 -\end{center} - -\vspace{\fill} - -*Corresponding Author \\ -\hspace*{2ex} email: wright@chem.wisc.edu \\ -\hspace*{2ex} phone: (608) 262-0351 \\ -\hspace*{2ex} fax: (608) 262-0381 - -\pagebreak -\renewcommand{\baselinestretch}{0.75}\normalsize -\tableofcontents -\renewcommand{\baselinestretch}{1.0}\normalsize - -\pagebreak -\setcounter{page}{1} -\pagenumbering{arabic} - -\section{Absorbance} % --------------------------------------------------------------------------- - -\autoref{figure:absorbance} displays the absorbance spectra of the two batches considered in this -work. -The lower spectra are plotted relative to each batches 1S peak center, -emphasizing the peak-shape differences around the 1S. - -\begin{figure}[!htb] - \centering - \includegraphics[scale=0.5]{absorbance} - \label{figure:absorbance} - \caption{Normalized absorbance spectra of the two baches considered in this - work. In the upper plot, the spectra are plotted directly against energy. In - the lower plot the spectra are plotted relative to the 1S peak center.} -\end{figure} - -To extract peak parameters from the rising continuum absorption, the data was fitted on the second -derivative level, as described in the supplementary information of \textcite{Czech2015}. -The script used to accomplish this fit, full parameter output, and additional figures showing the -separate excitonic features and fit remainder are contained in the supplementary repository, as -described in \autoref{section:repository}. - -Note that the aliquots used for each of the two Batch A experiments were at -slightly different concentrations, a crucial detail for m-factor corrections -(see \autoref{section:m-factors}). The two Batch B experiments were done using -the same aliquot. The absorbance spectrum of each sample is kept in an -associated ``cal'' directory in the supplementary repository (see \autoref{section:repository}). - - -\pagebreak -\section{Artifact correction} % ------------------------------------------------------------------ - -\subsection{Spectral delay correction} - -\begin{figure}[!htb] - \centering - \includegraphics[scale=0.5]{spectral_delay_correction} - \label{figure:spectral_delay_correction} - \caption{Frequency dependent delay calibration using CCl$_4$. (a) Measurement - of the pulse overlap position in $\tau_{21}$ space with respect to - $\omega_1$ ($\omega_2$ = 7500 cm$^{-1}$). The thick black line shows the - center of the temporal profile, as determined by Gaussian fits. (b) Same as - (a), but now $\omega_1$ is kept static while $\omega_2$ is scanned. (c) Same - as (a), but now active spectral delay corrections have been applied. (d) - Two-dimensional frequency-frequecy scan of CCl$_4$ with spectral delay - correction applied.} -\end{figure} - -\pagebreak -\subsection{Power factors} - -\begin{figure}[!htb] - \centering - \includegraphics[scale=0.5]{power_factors} - \label{figure:power_factors} - \caption{TODO} -\end{figure} - -\pagebreak -\subsection{m factors} \label{section:m-factors} - -\begin{figure}[!htb] - \centering - \includegraphics[scale=0.5]{m_factors} - \label{figure:power_factors} - \caption{TODO} -\end{figure} - -\pagebreak -\subsection{Processing} - -\begin{figure}[!htb] - \centering - \includegraphics[scale=0.5]{TG_artifacts} - \label{figure:power_factors} - \caption{TODO} -\end{figure} - -\begin{figure}[!htb] - \centering - \includegraphics[scale=0.5]{TA_artifacts} - \label{figure:power_factors} - \caption{TODO} -\end{figure} - - -\pagebreak -\section{Auger recombination dynamics} % --------------------------------------------------------- - -%\begin{figure}[!htb] -% \centering -% \includegraphics[scale=0.5]{"fsb19-3"} -% \label{fig:matrix_flow_diagram} -% \caption{$S_{\mathsf{TG}}$ measured before and after multiexciton relaxation dynamics.} -%\end{figure} - -Using a Poisson distribution to model the effects here: keep in mind that -Poisson is only valid when excitation probability is "low". m -Scholes thinks an equations of motion approach might be more fitting. -Others have approached this by truncating the Poisson model so that dots are effectively "off" at -high fluence (this is when pumping the continuum, so no SE contributions from the pump). - -According to the Poisson distribution, initial population created by pump is given by - -\begin{equation} -P(k;\lambda) = \frac{\lambda^k e^{-\lambda}}{k!}. -\end{equation} - -Assumes all absorption events have equal probability. -The absorption of the pumped sample will be proportional to - -\begin{eqnarray} -a_{\mathsf{NL}} &=& a_0 \left(1-e^{-\lambda}\sum_{k=1}\frac{\lambda^k}{k!}\right) -+ e^{-\lambda}\sum_{k=1}a_k\frac{\lambda^k}{k!} \\ -&=& a_0 - e^{-\lambda}\sum_{k=1} (a_0 - a_k)\frac{\lambda^k}{k!}. -\end{eqnarray} - -So the difference in the absorption is - -\begin{equation} -S(T=0) = a_{\mathsf{NL}} - a_0 = -e^{-\lambda}\sum_{k=1}(a_0-a_k)\frac{\lambda^k}{k!}. -\end{equation} - -We will assume that absorption is proportional to the number of ground state excitons: $a_k = ck$ -for all $k$. -Then - -\begin{eqnarray} -S(T=0) &=& ce^{-\lambda}\sum_{k=1}k\frac{\lambda^k}{k!} \\ -&=& c\lambda e^{-\lambda}\sum_{k=0}\frac{\lambda^k}{k!} \\ -&=& c \lambda, -\end{eqnarray} - -and the mean value corresponds to the response (as we expect when the relationship between -occupation and signal is linear i.e. $<ck> = c\lambda$). - -After Auger recombination, the excited state distribution has homogenized to $k=1$. -Signal is thus given by - -\begin{eqnarray} -S &=& ce^{-\lambda}(a_0-a_1)\sum_{k=1}\frac{\lambda^k}{k!} \\ -&=& ce^{-\lambda}(e^\lambda-1) \\ -&=& c(1-e^{-\lambda}). -\end{eqnarray} - -Previous work has analyzed this. - -Comparing the distribution theory with our results. - -The mean number of excitations should be proportional to our fluence: $\lambda = mI$. -This predicts the linear scaling of intensity close to zero delay, and it also predicts the -exponential saturation observed at longer delays. -Both observations qualitatively agree with our results. -Quantitatively, however, our two delays suggest different scaling constants with respect to pump -fluence: the long-time $m$-value is roughly 40\% larger than the short time scaling. -This means that our initial scaling underestimates how quickly the band saturates. - -Philosophically, there are two problems with this distribution: (1) I should use the equations of -motion for degenerate pumping, and (2) the pump is filtered by $k$-vector conservation (two pumps). -My strategy: come up with an expression for the distribution using coupled equations of motion. -Assume the driven limit, so that a steady state is reached. -We can account for these issues by utilizing the more general Conway-Maxwell-Poisson distribution. - -Estimate spot size as 300 um: 1 um ~ 1 mJ per cm squared. - -I think I should revisit the scaling of my exciton signal---I do not expect it to be the same as a -Poisson distribution because of the stimulated emission channels. - -\begin{eqnarray} -\frac{d \rho_{00}}{dt} &=& \frac{i}{\hbar} E \rho_{01} + \Gamma\rho_{11} \\ -\frac{d \rho_{00}}{dt} &=& \frac{i}{\hbar} E \rho_{01} + \Gamma\rho_{11} \\ -\frac{d \rho_{00}}{dt} &=& \cdots -\end{eqnarray} - -\pagebreak -\section{Supplementary repository} \label{section:repository} % ---------------------------------- - -All scripts and raw data used in this work have been uploaded to the Open Science Framework (OSF), -a project of the Center for Open Science. -These can be found at DOI: \href{http://dx.doi.org/10.17605/OSF.IO/N9CDP}{10.17605/OSF.IO/N9CDP}. - -To download the contents of this repository from your command line... % TODO - -To completely reproduce this work, simply execute \texttt{./run.sh all} from your terminal. -You will require the following: - -\begin{enumerate} - \item python 3.6 - \item WrightTools VERSION TODO (and dependencies) - \item latex -\end{enumerate} - -You can replace \texttt{all} with one of \texttt{data}, \texttt{simulations}, \texttt{figures}, -or \texttt{documents}. - -Otherwise, the OSF repository attempts to be generally self-explanatory. -README files and comments are used to explain what was done. - -\pagebreak -\printbibliography - -\end{document} |