From 90f80c97c9ea72083a317f3ae6f81424cfb51e9e Mon Sep 17 00:00:00 2001 From: linjiez Date: Thu, 26 Sep 2019 19:57:18 +0200 Subject: [PATCH] rough_manuscript1 --- biblio.bib | 92 ++++++++++++++++++ figure/12ax.png | Bin 0 -> 197425 bytes figure/3ato5d.png | Bin 0 -> 72907 bytes figure/6ato7b.png | Bin 0 -> 110538 bytes figure/crosssection.png | Bin 0 -> 5405 bytes figure/figure1.png | Bin 0 -> 112822 bytes figure/neutralUloss.png | Bin 0 -> 5387 bytes figure/proporMainFrag.png | Bin 0 -> 5186 bytes figure/sphere.png | Bin 0 -> 409926 bytes paper_UAR.tex | 196 +++++++++++++++++++++++++++++++++++--- 10 files changed, 273 insertions(+), 15 deletions(-) create mode 100644 biblio.bib create mode 100644 figure/12ax.png create mode 100644 figure/3ato5d.png create mode 100644 figure/6ato7b.png create mode 100644 figure/crosssection.png create mode 100644 figure/figure1.png create mode 100644 figure/neutralUloss.png create mode 100644 figure/proporMainFrag.png create mode 100644 figure/sphere.png diff --git a/biblio.bib b/biblio.bib new file mode 100644 index 0000000..67dde3e --- /dev/null +++ b/biblio.bib @@ -0,0 +1,92 @@ +%This is an auxiliary file used by the `achemso' bundle. +%This file may safely be deleted. It will be recreated as required. + +% @Control{achemso-control, +% ctrl-article-title = "yes", +% ctrl-chapter-title = "no", +% ctrl-etal-number = "10", +% ctrl-etal-firstonly = "no", +% } + +@article{Rasmussen2010, + title={Hydration of the Lowest Triplet States of the DNA/RNA Pyrimidines}, + author={Rasmussen, Andrew M and Lind, Maria C and Kim, Sunghwan and Schaefer III, Henry F}, + journal={Journal of chemical theory and computation}, + volume={6}, + number={3}, + pages={930--939}, + year={2010}, + publisher={ACS Publications} +} + +@article{Coates2018, + title={Binding energies of hydrated cobalt (II) by collision-induced dissociation and theoretical studies: evidence for a new critical size}, + author={Coates, Rebecca A and Armentrout, PB}, + journal={Physical Chemistry Chemical Physics}, + volume={20}, + number={2}, + pages={802--818}, + year={2018}, + publisher={Royal Society of Chemistry} +} + +@article{Imhoff2007, + title={Ionizing fragmentation of uracil and 5-bromouracil by electron impact in gas phase and hyperthermal Ar+ ion irradiation in condensed phase}, + author={Imhoff, Marjorie and Deng, Zongwu and Huels, Michael A}, + journal={International Journal of Mass Spectrometry}, + volume={262}, + number={1-2}, + pages={154--160}, + year={2007}, + publisher={Elsevier} +} + +@article{Abdoul2000, + title={Dissociative electron attachment to gas-phase 5-bromouracil}, + author={Abdoul-Carime, H and Huels, MA and Br{\"u}ning, F and Illenberger, E and Sanche, L}, + journal={The journal of chemical physics}, + volume={113}, + number={7}, + pages={2517--2521}, + year={2000}, + publisher={AIP} +} + +@article{Champeaux2010, + title={Dehalogenation of 5-halo-uracil molecules induced by 100 keV proton collisions}, + author={Champeaux, Jean-Philippe and {\c{C}}ar{\c{c}}abal, Pierre and Rabier, Julien and Cafarelli, Pierre and Sence, Martine and Moretto-Capelle, Patrick}, + journal={Physical Chemistry Chemical Physics}, + volume={12}, + number={20}, + pages={5454--5461}, + year={2010}, + publisher={Royal Society of Chemistry} +} + + +@article{Delaunay2014, + title={Prompt and delayed fragmentation of bromouracil cations ionized by multiply charged ions}, + author={Delaunay, Rudy and Champeaux, Jean-Philippe and Maclot, Sylvain and Capron, Michael and Domaracka, Alicja and M{\'e}ry, Alain and Manil, Bruno and Adoui, Lamri and Rousseau, Patrick and Moretto-Capelle, Patrick and others}, + journal={The European Physical Journal D}, + volume={68}, + number={6}, + pages={162}, + year={2014}, + publisher={Springer} +} + + + + + +@article{Tomsic2013, +author = {Tomsic,Anna and Andersson,Patrik U. and Marković,Nikola and Pettersson,Jan B. C. }, +title = {Collision dynamics of large water clusters on graphite}, +journal = {The Journal of Chemical Physics}, +volume = {119}, +number = {9}, +pages = {4916-4922}, +year = {2003}, +doi = {10.1063/1.1594717}, +URL = {https://doi.org/10.1063/1.1594717} +} diff --git a/figure/12ax.png b/figure/12ax.png new file mode 100644 index 0000000000000000000000000000000000000000..645d06a00a5c75ce5dbb5e4fc4e8fb0c57e7cedd GIT binary patch literal 197425 zcmYg%by$>N)UBdO3eq5>-UVH7(k4iGnF<)Xndi3bI><3AeM~|KiKYH}|4*ePM8>ghr zVBiOa{Rd6xqeu7~51+>d&kVaCJwaKMm6Z78mbRacn)Yeqs@Hc6zQD2|hxvht$z{<> zU#L86>QHIFtTlbA#lnE3qiiVT^S4BARFT)Mbz zRu;%+2+Lsz8~yTu)-hi5MrdT}-!E)1AUW*fU_vSIH(uEScW2o%sfXv}wBMmt0gped zIQ(8xBB`aNmBaoXcqj_fTRWgSm ziZB&!B^*xRH36(9`rp<5YQ^d+Cj;!g{Rzw!r$a)W8;*T0se?f`H(n9sd`gR_YHDh9 z{tdqOcXca4=}fbyt6Q^Pz`HkiJ?hxp3w7b);Zl;S+z?Y! z*#g@JcUAtegw)d-!VM`rtZDwMVFyk;ow)*rO z*ra)wd1BeBVA4ENVZrINV2^Jti`799s|Iid5~AV%oT6VHONv8^GmtB(>fLE`HSIiA 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zOs*IHtsYs&sB_eoHBc89yeZquE;yZ2v+EBZR3beLyUhbJ5yrxcoOH@x$HOJ?-ltUbXFk-+aLy;hS`-r6Nwrg zyNH6#*-&!3t9F@Whm)^$5hnFF;k7S#k%j-1-ShB^;J3tNZN9UU_9TbrPNuK|BLakZ z{CfSj=SmG5!LLXP&jgkKHU&bi|JPmjf4u|{`t<){6aPo proportion (W-H-U form) > proportion (U-H form). In other words, it is obvious that the neutral uracil loss proportions of clusters (H$_2$O)$_{n=3-7, 12}$UH$^+$ are significantly affected by the initial configuration of the clusters. However, for cluster (H$_2$O)$_{12}$UH$^+$, even the excess proton is the W-H form, it didn’t have a too high proportion owing to the structural rearrangements that the excess proton goes back to uracil after collision of cluster (H$_2$O)$_{12}$UH$^+$ and Ar. It’s worth noticing that why cluster (H$_2$O)$_{12}$UH$^+$ has structural rearrangements prior to dissociation. We propose for cluster (H$_2$O)$_{12}$UH$^+$, there are more hydrogen bonds than the small clusters, which needs more energy to lose water molecules, so the proton has time to go back to uracil before dissociation. + +\textbf{Total Fragmentation Cross Section} Formula of calculating the cross section: + +In the light of the results of 600(2R + 3) dynamics collision simulations for each lowest-energy (H$_2$O)$_{n=3-7}$UH$^+$ cluster, the total fragmentation cross sections of the (H$_2$O)$_{n=3-7}$UH$^+$ clusters were determined and compared with those in experiment. As shown in Table \ref{tab:table1}, for different isomers of lowest-energy (H$_2$O)$_{n=3-7, 12}$UH$^+$ clusters, the total fragmentation cross sections are very close. So in this part, we only discuss the total fragmentation cross section of the lowest-energy (H$_2$O)$_{n=3-7}$UH$^+$ cluster who has the closest neutral uracil loss proportion compared with the one in experiment. + +The total fragmentation cross sections of mixed (H$_2$O)$_{n=3-7}$UH$^+$ clusters from our simulation results of collision with Ar and Zamith’s experiment results of collision with Ne are plotted in Figure \ref{fig:crosssection} as a function of the number of water molecules n at 7.2 eV center of mass collision energy. (In Zamith’s experiment, collisions of cluster (H$_2$O)$_{n=1-15}$UH$^+$ with M (H$_2$O, D$_2$O, Ne, and Ar) were performed. They found no matter which M was used, the results were the same. They only showed the results with Ne.) As displayed in Figure \ref{fig:crosssection}, the curves in theory and in experiment have the same overall trend that the total fragmentation cross sections of mixed (H$_2$O)$_{n=3-7}$UH$^+$ clusters increase according to the number of water molecules. This indicates when the size of the clusters increase, the Ar and the cluster has a higher opportunity to collide. For (H$_2$O)$_7$UH$^+$ cluster, the value in theory is slightly lower than the one of (H2O)6UH+ cluster but the difference is only 1.3 Å$^2$, which is within the limit of error. Additionally, the absolute value of total fragmentation cross sections of (H$_2$O)$_{n=3-7}$UH$^+$ clusters in theory and experiment are close to each other. The biggest and smallest differences of the total fragmentation cross section for (H$_2$O)$_{n=3-7}$UH$^+$ clusters are 7.0 and 1.5 Å$^2$, separately between our calculation results and those in the experiment. Those results imply our simulations results are good enough. + +If it needs to make a further detailed description of the total fragmentation cross sections? + + \begin{figure} + \includegraphics[width=0.5\linewidth]{/home/linjie/Documents/uracil/collision/Paper_U/figure/crosssection} + \centering + \caption{Total fragmentation cross section in both theory (pink line) and experiment (green line) of clusters (H$_2$O)$_{n=3-7}$UH$^+$ who the closest neutral uracil loss proportion compared with those in experiment.} + \label{fig:crosssection} + \end{figure} + +\textbf{Mass Spectrum of Fragments with Excess Proton} +Formula of calculating the fragment ratio: + +To explore the collision products, the branching ratios of different fragments with the excess proton were extracted from the dynamics collision simulations and compared with the mass spectrum obtained by colliding cluster (H$_2$O)$_7$UH$^+$ with Ne at 7.2 eV center of mass collision energy in experiment.[doi: 10.1063/1.5044481] Table \ref{tab:massspectrum} displays the specific fragment ratio in the total fragments from the collision of the second lowest-energy cluster (H$_2$O)$_7$UH$^+$ with Ar. Fragments (H$_2$O)$_{3-5}$H$^+$ were not found in our calculation, which agrees with the very low intensity of fragments (H$_2$O)$_{3-5}$H$^+$ in experiment. This implies when (H$_2$O)$_{3-5}$ leave, they don’t have enough proton affinity to take away the excess proton. The intensity of fragments (H$_2$O)$_{6-7}$H$^+$ are higher than fragments (H$_2$O)$_{3-5}$H$^+$ in experiment results and we also determined the fragments (H$_2$O)$_{6-7}$H$^+$ in our calculation, which indicate the proton affinity of (H$_2$O)$_{6-7}$ is higher than (H$_2$O)$_{3-5}$ that in line with the previous study. [Title: The first twenty-eight gas-phase proton hydration energies] + +As shown in Table \ref{tab:massspectrum}, we didn’t get UH$^+$ but it was detected in experiment with time of flight 60 $\mu$s. For each dynamics collision simulation of cluster (H$_2$O)$_7$H$^+$ was performed with simulation time 15 ps, we cannot assert that the UH$^+$ will not appear in longer simulation. Modeling the complete duration of the experiment (up to $\mu$s) is out of reach with MD/SCC-DFTB simulations. Additionally, we calculated the energy of (H$_2$O)$_6$H$^+$, which is from (H$_2$O)$_7$H$^+$ cluster with the dissociation of one water after collision with Ar at SCC-DFTB level (see Table \ref{tab:fragenergy}). We also calculated the lowest energies of (H$_2$O)$_5$H$^+$ and water (see Table \ref{tab:fragenergy}). From the data in Table \ref{tab:fragenergy}, the relative energies between energy of (H$_2$O)$_6$H$^+$ and lowest energy of (H$_2$O)$_5$H$^+$ plus H$_2$O can reach 1.007 eV, so it is possible for the fragment (H$_2$O)$_6$H$^+$ to lose more water molecules. From this, we suggest if the dynamics collision simulation is long enough, finally UH$^+$ can be obtained. + +As displayed in Table \ref{tab:fragenergy}, ratios of fragments (H$_2$O)$_{n=1-4}$UH$^+$ increase with the number of n which is in line with the results in experiment. It indicates the second lowest-energy cluster (H$_2$O)$_7$UH$^+$ has more chances to lose three water molecules than to lose six water molecules. Ratio of fragment (H$_2$O)$_5$UH$^+$ is close to it of fragment (H$_2$O)$_4$UH$^+$ in theory which agree with the one in experiment. The ratio of fragment (H$_2$O)$_6$UH$^+$ increases a lot in the calculated results but it is not so high in experiment, which indicates in our simulations, the dissociation of the second lowest-energy cluster (H$_2$O)$_7$UH$^+$ losing one water molecule is dominant. The parent cluster (H$_2$O)$_7$UH$^+$ has the highest ratio among all fragments, which is fully consistent with it in experiment. From the analyses of the mass spectrum in theory and experiment, it implies our simulations can quantitatively describe the fragment ratios. + + +\begin{table} + \begin{center} + \caption{Fragment ratios in the total fragments from the dissociation of the second lowest-energy cluster (H$_2$O)$_7$UH$^+$ with simulation time 15 ps.} + \label{tab:massspectrum} + \begin{tabular}{c|c} + \textbf{Fragment} & \textbf{Ratio (\%)} \\ + \hline + (H$_2$O)$_3$H$^+$ & 0.00 \\ + (H$_2$O)$_4$H$^+$ & 0.00 \\ + (H$_2$O)$_5$H$^+$ & 0.00 \\ + (H$_2$O)$_6$H$^+$ & 2.62 \\ + (H$_2$O)$_7$H$^+$ & 2.14 \\ + UH$^+$ & 0.00 \\ + (H$_2$O)UH$^+$ & 0.07 \\ + (H$_2$O)$_2$UH$^+$ & 0.41 \\ + (H$_2$O)$_3$UH$^+$ & 1.60 \\ + (H$_2$O)$_4$UH$^+$ & 3.66 \\ + (H$_2$O)$_5$UH$^+$ & 7.56 \\ + (H$_2$O)$_6$UH$^+$ & 18.09 \\ + (H$_2$O)$_7$UH$^+$ & 63.83 \\ + \end{tabular} + \end{center} +\end{table} + +\begin{table} + \begin{center} + \caption{Energies of different (H$_2$O)$_6$UH$^+$ fragments selected from the dissociation of the second lowest-energy cluster (H$_2$O)$_7$UH$^+$ at SCC-DFTB level, and the lowest energies (H$_2$O)$_5$UH$^+$ and (H$_2$O) at SCC-DFTB level. And the relative energies E$_{rela}$ between energy of (H$_2$O)$_6$UH$^+$ and energy of (H$_2$O)$_5$UH$^+$ plus (H$_2$O). All energies here are given in eV.} + \label{tab:fragenergy} + \begin{tabular}{c|c|c|c} + \textbf{E((H$_2$O)$_6$UH$^+$)} & \textbf{E(H$_2$O)$_5$UH$^+$)} & \textbf{E(H$_2$O)} & \textbf{E$_{rela}$}\\ + \hline + -44.361 & -40.312 & -4.06 & 0.190 \\ + -44.331 & -40.312 & -4.06 & 1.007 \\ + -44.331 & -40.312 & -4.06 & 1.007 \\ + -44.334 & -40.312 & -4.06 & 0.925 \\ + \end{tabular} + \end{center} +\end{table} + + \begin{figure} + \includegraphics[width=0.8\linewidth]{/home/linjie/Documents/uracil/collision/Paper_U/figure/proporMainFrag} + \centering + \caption{The proportions of the main fragment from the second lowest-energy parent cluster (H$_2$O)$_7$UH$^+$ as a function of time (The values 200 and 1000 in horizontal axis correspond to 3 ps and 15 ps, respectively).} + \label{fig:proporEachFrag} + \end{figure} + +\textbf{Time-Dependent Proportion of Each Fragment} +In addition, we got the time-dependent proportion of each fragment which confirm that up to 7 water molecules a direct dissociation mechanism occurs. For (H$_2$O)$_{12}$UH$^+$, the cluster undergoes structural rearrangements prior to dissociation, which is proof of a statistical dissociation mechanism. + +In addition, the time-dependent proportion of each fragment was extracted from 600(2R + 3) dynamics collision simulations. Here we take the time-dependent proportion of each fragment from second lowest-energy parent cluster (H$_2$O)$_7$UH$^+$ as an example. For the sake of seeing clearly, only the main fragment proportions plotted as a function of simulation time are showed in Figure 7. The proportions of the main fragment of clusters (H$_2$O)$_{3-6, 12}$UH$^+$ are shown in SI Figure SX. From Figure \ref{fig:proporEachFrag}, it clear that the parent cluster (H$_2$O)$_7$UH$^+$ exists from the beginning and different fragments starts to appear after collision. It can be seen when the collision is finished, the fragment proportions almost doesn’t change any more. It is worth noticing the fragment (H$_2$O)$_6$UH$^+$ increase first and then it decreases, which indicates there are water molecules dissociated form it. + +From the time-dependent proportion of each fragment from clusters (H$_2$O)$_{3-6, 12}$UH$^+$, it confirms that up to 7 water molecules a direct dissociation mechanism occurs. For cluster (H$_2$O)$_{12}$UH$^+$, it undergoes structural rearrangements prior to dissociation, which is proof of a statistical dissociation mechanism.