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000459129 1001_ $$00000-0001-6286-4064$$aBoll, Rebecca$$b0$$eCorresponding author
000459129 245__ $$aX-ray multiphoton-induced Coulomb explosion images complex single molecules
000459129 260__ $$aBasingstoke$$bNature Publishing Group$$c2022
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000459129 520__ $$aFollowing structural dynamics in real time is a fundamental goal towards a better understanding of chemical reactions. Recording snapshots of individual molecules with ultrashort exposure times is a key ingredient towards this goal, as atoms move on femtosecond (10$< {−15}$ s) timescales. For condensed-phase samples, ultrafast, atomically resolved structure determination has been demonstrated using X-ray and electron diffraction. Pioneering experiments have also started addressing gaseous samples. However, they face the problem of low target densities, low scattering cross sections and random spatial orientation of the molecules. Therefore, obtaining images of entire, isolated molecules capturing all constituents, including hydrogen atoms, remains challenging. Here we demonstrate that intense femtosecond pulses from an X-ray free-electron laser trigger rapid and complete Coulomb explosions of 2-iodopyridine and 2-iodopyrazine molecules. We obtain intriguingly clear momentum images depicting ten or eleven atoms, including all the hydrogens, and thus overcome a so-far impregnable barrier for complete Coulomb explosion imaging—its limitation on molecules consisting of three to five atoms. In combination with state-of-the-art multi-coincidence techniques and elaborate theoretical modelling, this allows tracing ultrafast hydrogen emission and obtaining information on the result of intramolecular electron rearrangement. Our work represents an important step towards imaging femtosecond chemistry via Coulomb explosion.
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000459129 7001_ $$0P:(DE-H253)PIP1032687$$aSchäfer, Julia M.$$b1$$udesy
000459129 7001_ $$0P:(DE-H253)PIP1091506$$aRichard, Benoit$$b2
000459129 7001_ $$0P:(DE-H253)PIP1087378$$aFehre, Kilian$$b3
000459129 7001_ $$0P:(DE-H253)PIP1014655$$aKastirke, Gregor$$b4
000459129 7001_ $$0P:(DE-H253)PIP1013492$$aJurek, Zoltan$$b5$$udesy
000459129 7001_ $$aSchöffler, Markus S.$$b6
000459129 7001_ $$aAbdullah, Malik M.$$b7
000459129 7001_ $$aAnders, Nils$$b8
000459129 7001_ $$aBaumann, Thomas M.$$b9
000459129 7001_ $$aEckart, Sebastian$$b10
000459129 7001_ $$0P:(DE-H253)PIP1011809$$aErk, Benjamin$$b11
000459129 7001_ $$aDe Fanis, Alberto$$b12
000459129 7001_ $$aDörner, Reinhard$$b13
000459129 7001_ $$aGrundmann, Sven$$b14
000459129 7001_ $$aGrychtol, Patrik$$b15
000459129 7001_ $$aHartung, Alexander$$b16
000459129 7001_ $$aHofmann, Max$$b17
000459129 7001_ $$aIlchen, Markus$$b18
000459129 7001_ $$0P:(DE-H253)PIP1023594$$aInhester, Ludger$$b19
000459129 7001_ $$aJanke, Christian$$b20
000459129 7001_ $$0P:(DE-H253)PIP1086222$$aJin, Rui$$b21$$udesy
000459129 7001_ $$aKircher, Max$$b22
000459129 7001_ $$aKubicek, Katharina$$b23
000459129 7001_ $$00000-0001-6543-8722$$aKunitski, Maksim$$b24
000459129 7001_ $$aLi, Xiang$$b25
000459129 7001_ $$aMazza, Tommaso$$b26
000459129 7001_ $$aMeister, Severin$$b27
000459129 7001_ $$aMelzer, Niklas$$b28
000459129 7001_ $$aMontano, Jacobo$$b29
000459129 7001_ $$aMusic, Valerija$$b30
000459129 7001_ $$aNalin, Giammarco$$b31
000459129 7001_ $$aOvcharenko, Yevheniy$$b32
000459129 7001_ $$aPassow, Christopher$$b33
000459129 7001_ $$aPier, Andreas$$b34
000459129 7001_ $$aRennhack, Nils$$b35
000459129 7001_ $$aRist, Jonas$$b36
000459129 7001_ $$aRivas, Daniel E.$$b37
000459129 7001_ $$0P:(DE-H253)PIP1007320$$aRolles, Daniel$$b38
000459129 7001_ $$aSchlichting, Ilme$$b39
000459129 7001_ $$aSchmidt, Lothar Ph. H.$$b40
000459129 7001_ $$aSchmidt, Philipp$$b41
000459129 7001_ $$aSiebert, Juliane$$b42
000459129 7001_ $$aStrenger, Nico$$b43
000459129 7001_ $$aTrabert, Daniel$$b44
000459129 7001_ $$aTrinter, Florian$$b45
000459129 7001_ $$aVela-Perez, Isabel$$b46
000459129 7001_ $$aWagner, Rene$$b47
000459129 7001_ $$aWalter, Peter$$b48
000459129 7001_ $$aWeller, Miriam$$b49
000459129 7001_ $$aZiolkowski, Pawel$$b50
000459129 7001_ $$0P:(DE-H253)PIP1012452$$aSon, Sang-Kil$$b51
000459129 7001_ $$aRudenko, Artem$$b52
000459129 7001_ $$aMeyer, Michael$$b53
000459129 7001_ $$0P:(DE-H253)PIP1012203$$aSantra, Robin$$b54$$eCorresponding author
000459129 7001_ $$0P:(DE-H253)PIP1084564$$aJahnke, Till$$b55$$eCorresponding author$$udesy
000459129 773__ $$0PERI:(DE-600)2206346-8$$a10.1038/s41567-022-01507-0$$gVol. 18, no. 4, p. 423 - 428$$n4$$p423 - 428$$tNature physics$$v18$$x1745-2473$$y2022
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