From 96c0fcb08e1a4fa3ee29c71c8f612bcefd57f42a Mon Sep 17 00:00:00 2001 From: linjiez Date: Fri, 27 Sep 2019 18:55:30 +0200 Subject: [PATCH] manu_with_reference --- biblio.bib | 388 +++++++++++++++++++++++++++++++++++++++- figure/12ad.png | Bin 0 -> 195551 bytes figure/12ax.png | Bin 197425 -> 0 bytes figure/6ato7b.png | Bin 110538 -> 110383 bytes figure/crosssection.png | Bin 5405 -> 5418 bytes figure/neutralUloss.png | Bin 5387 -> 4285 bytes paper_UAR.tex | 41 ++--- 7 files changed, 408 insertions(+), 21 deletions(-) create mode 100644 figure/12ad.png delete mode 100644 figure/12ax.png diff --git a/biblio.bib b/biblio.bib index 67dde3e..dbe9853 100644 --- a/biblio.bib +++ b/biblio.bib @@ -63,6 +63,18 @@ publisher={Royal Society of Chemistry} } +@article{Korchagina2017, + title={Molecular dynamics study of the collision-induced reaction of h with co on small water clusters}, + author={Korchagina, Kseniia A and Spiegelman, Fernand and Cuny, Jerome}, + journal={The Journal of Physical Chemistry A}, + volume={121}, + number={49}, + pages={9485--9494}, + year={2017}, + publisher={ACS Publications} +} + + @article{Delaunay2014, title={Prompt and delayed fragmentation of bromouracil cations ionized by multiply charged ions}, @@ -75,12 +87,187 @@ publisher={Springer} } +@article{Bacchus2009, + title={Ab initio molecular treatment of charge-transfer processes induced by collision of carbon ions with 5-halouracil molecules}, + author={Bacchus-Montabonel, MC and Tergiman, YS and Talbi, Dahbia}, + journal={Physical Review A}, + volume={79}, + number={1}, + pages={012710}, + year={2009}, + publisher={APS} +} + +@article{Kossoski2015, + title={Negative ion states of 5-bromouracil and 5-iodouracil}, + author={Kossoski, Fabris and Varella, MT do N}, + journal={Physical Chemistry Chemical Physics}, + volume={17}, + number={26}, + pages={17271--17278}, + year={2015}, + publisher={Royal Society of Chemistry} +} + +@article{Maclot2011, + title={Ion-Induced Fragmentation of Amino Acids: Effect of the Environment}, + author={Maclot, Sylvain and Capron, Michael and Maisonny, R{\'e}mi and {\L}awicki, Arkadiusz and M{\'e}ry, Alain and Rangama, Jimmy and Chesnel, Jean-Yves and Bari, Sadia and Hoekstra, Ronnie and Schlath{\"o}lter, Thomas and others}, + journal={ChemPhysChem}, + volume={12}, + number={5}, + pages={930--936}, + year={2011}, + publisher={Wiley Online Library} +} + +@inproceedings{Domaracka2012, + title={Ion interaction with biomolecular systems and the effect of the environment}, + author={Domaracka, Alicja and Capron, Michael and Maclot, Sylvain and Chesnel, Jean-Yves and M{\'e}ry, Alain and Poully, Jean-Christophe and Rangama, Jimmy and Adoui, Lamri and Rousseau, Patrick and Huber, Bernd A}, + booktitle={Journal of Physics: Conference Series}, + volume={373}, + number={1}, + pages={012005}, + year={2012}, + organization={IOP Publishing} +} + +@article{Markush2016, + title={The role of the environment in the ion induced fragmentation of uracil}, + author={Markush, Pal and Bolognesi, Paola and Cartoni, Antonella and Rousseau, Patrick and Maclot, Sylvain and Delaunay, Rudy and Domaracka, Alicja and Kocisek, Jaroslav and Castrovilli, Mattea C and Huber, Bernd A and others}, + journal={Physical Chemistry Chemical Physics}, + volume={18}, + number={25}, + pages={16721--16729}, + year={2016}, + publisher={Royal Society of Chemistry} +} + +@article{Castrovilli2017, + title={Fragmentation of pure and hydrated clusters of 5Br-uracil by low energy carbon ions: observation of hydrated fragments}, + author={Castrovilli, MC and Markush, P and Bolognesi, P and Rousseau, P and Maclot, S and Cartoni, A and Delaunay, R and Domaracka, A and Ko{\v{c}}i{\v{s}}ek, J and Huber, BA and others}, + journal={Physical Chemistry Chemical Physics}, + volume={19}, + number={30}, + pages={19807--19814}, + year={2017}, + publisher={Royal Society of Chemistry} +} + +@incollection{Hayes1990, + title={[10] Collision-induced dissociation}, + author={Hayes, Roger N and Gross, Michael L}, + booktitle={Methods in enzymology}, + volume={193}, + pages={237--263}, + year={1990}, + publisher={Elsevier} +} + +@article{Coates2017, + title={Thermochemical Investigations of Hydrated Nickel Dication Complexes by Threshold Collision-Induced Dissociation and Theory}, + author={Coates, Rebecca A and Armentrout, PB}, + journal={The Journal of Physical Chemistry A}, + volume={121}, + number={19}, + pages={3629--3646}, + year={2017}, + publisher={ACS Publications} +} + +@article{Neustetter2017, + title={Study of Electron Ionization and Fragmentation of Non-hydrated and Hydrated Tetrahydrofuran Clusters}, + author={Neustetter, Michael and Mahmoodi-Darian, Masoomeh and Denifl, Stephan}, + journal={Journal of The American Society for Mass Spectrometry}, + volume={28}, + number={5}, + pages={866--872}, + year={2017}, + publisher={Springer} +} + +@article{Nelson1994, + title={Collision-induced dissociation of uracil and its derivatives}, + author={Nelson, Chad C and McCloskey, James A}, + journal={Journal of the American Society for Mass Spectrometry}, + volume={5}, + number={5}, + pages={339--349}, + year={1994}, + publisher={Springer} +} + +@article{Molina2015, + title={Elucidating collision induced dissociation products and reaction mechanisms of protonated uracil by coupling chemical dynamics simulations with tandem mass spectrometry experiments}, + author={Molina, Estefan{\'\i}a Rossich and Ortiz, Daniel and Salpin, Jean-Yves and Spezia, Riccardo}, + journal={Journal of mass spectrometry}, + volume={50}, + number={12}, + pages={1340--1351}, + year={2015}, + publisher={Wiley Online Library} +} + +@article{Molina2016, + title={On the gas phase fragmentation of protonated uracil: a statistical perspective}, + author={Molina, Estefan{\'\i}a Rossich and Salpin, Jean-Yves and Spezia, Riccardo and Martinez-Nunez, Emilio}, + journal={Physical Chemistry Chemical Physics}, + volume={18}, + number={22}, + pages={14980--14990}, + year={2016}, + publisher={Royal Society of Chemistry} +} + +@article{Sadr2014, + title={Theoretical and experimental study of the fragmentation of protonated uracil}, + author={Sadr-Arani, Leila and Mignon, Pierre and Chermette, Henry and Douki, Thierry}, + journal={Chemical Physics Letters}, + volume={605}, + pages={108--114}, + year={2014}, + publisher={Elsevier} +} + +@article{Bakker2008, + title={Tautomerism of uracil probed via infrared spectroscopy of singly hydrated protonated uracil}, + author={Bakker, Joost M and Sinha, Rajeev K and Besson, Thierry and Brugnara, Maurizio and Tosi, Paolo and Salpin, Jean-Yves and Ma{\^\i}tre, Philippe}, + journal={The Journal of Physical Chemistry A}, + volume={112}, + number={48}, + pages={12393--12400}, + year={2008}, + publisher={ACS Publications} +} + +@article{Simon2017, + title={Dissociation of polycyclic aromatic hydrocarbons: molecular dynamics studies}, + author={Simon, Aude and Rapacioli, Mathias and Rouaut, Guillaume and Trinquier, Georges and Gad{\'e}a, FX}, + journal={Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences}, + volume={375}, + number={2092}, + pages={20160195}, + year={2017}, + publisher={The Royal Society Publishing} +} +@article{Rapacioli2018, +Author = {Rapacioli, Mathias and Cazaux, Stephanie and Foley, Nolan and Simon, + Aude and Hoekstra, Ronnie and Schlatholter, Thomas}, +Title = {{Atomic hydrogen interactions with gas-phase coronene cations: + hydrogenation versus fragmentation}}, +Journal = {{PHYSICAL CHEMISTRY CHEMICAL PHYSICS}}, +Year = {{2018}}, +Volume = {{20}}, +Number = {{35}}, +Pages = {{22427-22438}}, +Month = {{SEP 21}}, +DOI = {{10.1039/c8cp03024c} +} @article{Tomsic2013, -author = {Tomsic,Anna and Andersson,Patrik U. and Marković,Nikola and Pettersson,Jan B. C. }, +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}, @@ -90,3 +277,202 @@ year = {2003}, doi = {10.1063/1.1594717}, URL = {https://doi.org/10.1063/1.1594717} } + + +@article{Elstner2014, + title={Density functional tight binding}, + author={Elstner, Marcus and Seifert, Gotthard}, + journal={Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences}, + volume={372}, + number={2011}, + pages={20120483}, + year={2014}, + publisher={The Royal Society Publishing} +} + +@article{Kruger2005, + title={Validation of the density-functional based tight-binding approximation method for the calculation of reaction energies and other data}, + author={Kr{\"u}ger, Thomas and Elstner, Marcus and Schiffels, Peter and Frauenheim, Thomas}, + journal={The Journal of chemical physics}, + volume={122}, + number={11}, + pages={114110}, + year={2005}, + publisher={AIP} +} + +@article{Elstner1998, + title={Self-consistent-charge density-functional tight-binding method for simulations of complex materials properties}, + author={Elstner, Marcus and Porezag, Dirk and Jungnickel, G and Elsner, J and Haugk, M and Frauenheim, Th and Suhai, Sandor and Seifert, Gotthard}, + journal={Physical Review B}, + volume={58}, + number={11}, + pages={7260--7268}, + year={1998}, + publisher={APS} +} + +@article{Rapacioli2009, + title={Correction for dispersion and Coulombic interactions in molecular clusters with density functional derived methods: Application to polycyclic aromatic hydrocarbon clusters}, + author={Rapacioli, Mathias and Spiegelman, Fernand and Talbi, Dahbia and Mineva, Tzonka and Goursot, Annick and Heine, Thomas and Seifert, Gotthard}, + journal={The Journal of chemical physics}, + volume={130}, + number={24}, + pages={244304}, + year={2009}, + publisher={AIP} +} + +@article{Simon2012, + title={Vibrational spectroscopy and molecular dynamics of water monomers and dimers adsorbed on polycyclic aromatic hydrocarbons}, + author={Simon, Aude and Rapacioli, Mathias and Mascetti, Jo{\"e}lle and Spiegelman, Fernand}, + journal={Physical Chemistry Chemical Physics}, + volume={14}, + number={19}, + pages={6771--6786}, + year={2012}, + publisher={Royal Society of Chemistry} +} + +@article{Simon2013, + title={Conformational dynamics and finite-temperature infrared spectra of the water octamer adsorbed on coronene}, + author={Simon, Aude and Spiegelman, Fernand}, + journal={Computational and Theoretical Chemistry}, + volume={1021}, + pages={54--61}, + year={2013}, + publisher={Elsevier} +} + +@article{demonnanoCode, + author={Heine, T.; Rapacioli, M.; Patchkovskii, S.; Frenzel, J.; Koster, A.; +Calaminici, P.; Duarte, H.; Escalante, S.; Flores-Moreno, R.; Goursot, +A.; et al.}, + publisher={deMonNano. http://demon-nano.ups-tlse.fr/ (accessed 24 October 2016).} + } + +@article{Braud2019, + title={Size-dependent proton localization in hydrated uracil clusters: A joint experimental and theoretical study}, + author={Braud, Isabelle and Zamith, S{\'e}bastien and Cuny, J{\'e}r{\^o}me and Zheng, Linjie and L’Hermite, Jean-Marc}, + journal={The Journal of chemical physics}, + volume={150}, + number={1}, + pages={014303}, + year={2019}, + publisher={AIP Publishing} +} + +@article{Sugita1999, + title={Replica-exchange molecular dynamics method for protein folding}, + author={Sugita, Yuji and Okamoto, Yuko}, + journal={Chemical physics letters}, + volume={314}, + number={1-2}, + pages={141--151}, + year={1999}, + publisher={Elsevier} +} + +@article{Earl2005, + title={Parallel tempering: Theory, applications, and new perspectives}, + author={Earl, David J and Deem, Michael W}, + journal={Physical Chemistry Chemical Physics}, + volume={7}, + number={23}, + pages={3910--3916}, + year={2005}, + publisher={Royal Society of Chemistry} +} + +@article{Nose1984, + title={A unified formulation of the constant temperature molecular dynamics methods}, + author={Nos{\'e}, Shuichi}, + journal={The Journal of chemical physics}, + volume={81}, + number={1}, + pages={511--519}, + year={1984}, + publisher={AIP} +} + +@article{Hoover1985, + title={Canonical dynamics: Equilibrium phase-space distributions}, + author={Hoover, William G}, + journal={Physical review A}, + volume={31}, + number={3}, + pages={1695--1697}, + year={1985}, + publisher={APS} +} + +@article{Pedersen2014, + title={Structures of protonated thymine and uracil and their monohydrated gas-phase ions from ultraviolet action spectroscopy and theory}, + author={Pedersen, Sara {\O}vad and Byskov, Camilla Skinnerup and Turecek, Frantisek and Nielsen, Steen Br{\o}ndsted}, + journal={The Journal of Physical Chemistry A}, + volume={118}, + number={24}, + pages={4256--4265}, + year={2014}, + publisher={ACS Publications} +} + +@article{Weigend2005, + title={Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: Design and assessment of accuracy}, + author={Weigend, Florian and Ahlrichs, Reinhart}, + journal={Physical Chemistry Chemical Physics}, + volume={7}, + number={18}, + pages={3297--3305}, + year={2005}, + publisher={The Royal Society of Chemistry} +} + +@article{Weigend2006, + title={Accurate Coulomb-fitting basis sets for H to Rn}, + author={Weigend, Florian}, + journal={Physical chemistry chemical physics}, + volume={8}, + number={9}, + pages={1057--1065}, + year={2006}, + publisher={Royal Society of Chemistry} +} + +@article{GaussianCode, + author={M. J. Frisch, G. W. Trucks, H. B. Schlegel, G. E. Scuseria, M. A. Robb, J. R. Cheeseman, G. Scalmani, V. Barone, B. Mennucci, G. A. Petersson et al.}, + publisher={G AUSSIAN 09, Revision D.01, Gaussian, Inc., Wallingford, CT, 2009.} +} + +@article{Warshel1976, + title={Theoretical studies of enzymic reactions: dielectric, electrostatic and steric stabilization of the carbonium ion in the reaction of lysozyme}, + author={Warshel, Arieh and Levitt, Michael}, + journal={Journal of molecular biology}, + volume={103}, + number={2}, + pages={227--249}, + year={1976}, + publisher={Elsevier} +} + +@article{Kukk2015, + title={Internal energy dependence in X-ray-induced molecular fragmentation: an experimental and theoretical study of thiophene}, + author={Kukk, Edwin and Ha, DT and Wang, Y and Piekarski, Dariusz Grzegorz and Diaz-Tendero, Sergio and Kooser, Kuno and It{\"a}l{\"a}, Eero and Levola, Helena and Alcam{\'\i}, Manuel and Rachlew, Elisabeth and others}, + journal={Physical Review A}, + volume={91}, + number={4}, + pages={043417}, + year={2015}, + publisher={APS} +} + +@article{Magnera1991, + title={The first twenty-eight gas-phase proton hydration energies}, + author={Magnera, Thomas F and David, Donald E and Michl, Josef}, + journal={Chemical physics letters}, + volume={182}, + number={3-4}, + pages={363--370}, + year={1991}, + publisher={Elsevier} +} \ No newline at end of file diff --git a/figure/12ad.png b/figure/12ad.png new file mode 100644 index 0000000000000000000000000000000000000000..39f4600ffc0718ba11f33016cf683e77eaf127f7 GIT binary patch literal 195551 zcmYg&Wl$Ym(`^Ko-~_~23gm{Ef?`~lJO?0JuUWP!zWEW>lmf!D6craKgAvrnEVQ);fjVc^WR($>)Q&bW7 zOmL@2l`)vi6?NSVqg;1x5p@mj(XX{xYkxRHq;Gte$>sF(P*x>DOfabEzng~VPLuwU zfO1)J`dlcV9UU2ogqG@g>)w{a=|JJ%_0^yXXN>!d=jw0gASa(iKO^yDm$@AVm^>#1YXVVXsu=9Q| zn;}U-)V%EfdtKjLNHq6pXCyAmM2)FDTFS{{oiNF-So7pz@=b7+HJD)T>~`z%tV3K< z6283okh;#3x(wSUPObI7*O&E=;8he=)P#=Q%V0G}he5_8o0SchLy!%Zju{|jSiQV( z#cyhA0@2eaxz$E`KVQ!o5Ew5P<<^Q#Z~pnu-npPJ|4KD#7~L+7B(b;Exd@IZFc2p3 zq^hf{dz&ReTm%m{ClO&7lm<7)3;QcAF3QLL|Nr`pKkCa+Lhr;93&+OClg>(q%gQPH 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zIULzAh7~f~wCS`TTn>kix%`YZwP^PklzP3!2`_;2wDQ=)Seag9U&&jn`iMa-8T*6& zBH^wDp@-Lxb<1#`wkgx2t6WyKXQ9Y65;8>LIUrOTHb2Xb@avL?U{h*fQG8gPbDhV3 zT9N1_J8>{-mc4Uvb$w=RUgX{BXk>^o2cRan46S(5MvJj#(Z7P#m_SmamT>lQgg(WW zyxz`U`6k10HdCY16wg)mZulkx>batfun((U@vo87i{@LPl&|YXdeK&dE23893R%%7 zG|IkTKOz_b)rz>06>IDiWP_gQN=0+kn#35LyM_Yv5+xIj$&?(FwGYL7s0(1O&@1DMqpR$rqS_`HH)A8}$(MY7ZoC2-b7|3g1AMIjK7FJv^{a0m*gmMDGCR`jImo{-!7^CE z9zXa`JHm{Nnw&C2{o5(wUaJ%92LBxLh?%BeCmk+*hP= z?NfC(D0rqvJMb7+Dq462BDZ_o=MM;H#V%{E9S{&d#Z?tmrkkX40*f9C*EO*^u8k(} zoLBp=wSt&=V=Xn0wQChF%`3-8ve=g@5}3s%&Dy8OUAvkzjSPw~68P%XtxFPcd^K)< zkDXNAwS5(P^4&TfJE^+|lk#h9>zTzdzReEm?yPv7LJw#UZ%A=M$Kv|1W5d|KYu&u( z+^;3F8#Ki$*?kh(oZ@Ex-)0tz-oHl%ahn`{hvv!U>r1wWxxC%ox4+x4JyiTFH-ko^ z_SWz@+S}(Z`inEd(x%=0R{0;FOG+Fr);U!O?{v`MQ#T!+qU{YR%q*w1_y6`SzaAKt zjvM6XLTXwg6_yrIiKA_~U{@Ht$Mx;~qvx(`i*++IXdVmttvDUpBFC3`+EhEN@p^iv z<_zVzq;Ka6O*DG~w$D+$IzFN^8T*9$`0Zg|FJa>PuBGNq@qa7-|4>F?pvOjl>x$U9 z|9 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. +From Table \ref{tab:table1}, we can see for clusters (H$_2$O)$_{n=3-4}$UH$^+$ with U-H form, the proportions of neutral uracil loss are about 0.0\%. For different isomers of clusters (H$_2$O)$_{n=5-7}$UH$^+$ with the W-H form, they have a relative high proportion. For clusters (H$_2$O)$_{n=4-7}$UH$^+$ with W-H-U form, they have a relative low proportion and the proportion decreases with distance between the excess proton and the adjacent oxygen atom of uracil. For cluster (H$_2$O)$_{12}$UH$^+$, when the excess proton has the W-H form localization, it also has a higher proportion of neutral uracil loss than the one when the excess proton is the W-H-U form. In general, for any cluster of (H$_2$O)$_{n=3-7, 12}$UH$^+$, the neutral uracil loss proportion has a direct relationship with the localization form of the excess proton: proportion (W-H form) $>$ 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. +The total fragmentation cross sections of mixed (H$_2$O)$_{n=3-7}$UH$^+$ clusters from our simulation results of collision with Ar and the corresponding experiment results 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. 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 (H$_2$O)$_6$UH$^+$ 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? @@ -265,9 +266,9 @@ If it needs to make a further detailed description of the total fragmentation cr \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] +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.\cite{Braud2019} 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. \cite{Magnera1991} -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 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 energy $\Delta$E 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. @@ -298,10 +299,10 @@ As displayed in Table \ref{tab:fragenergy}, ratios of fragments (H$_2$O)$_{n=1-4 \begin{table} \begin{center} - \caption{Energies of different (H$_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.} + \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 $\Delta$E 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$_{rela}$}\\ + \textbf{E((H$_2$O)$_6$UH$^+$)} & \textbf{E(H$_2$O)$_5$UH$^+$)} & \textbf{E(H$_2$O)} & \textbf{$\Delta$E}\\ \hline -44.361 & -40.312 & -4.06 & 0.190 \\ -44.331 & -40.312 & -4.06 & 1.007 \\