[en] Laser-driven dynamics in polyatomic molecules poses a complex many-body problem. Understanding intense light-matter interaction is crucial for steering intramolecular quantum dynamical processes. Here, we record time-resolved x-ray diffraction images of [Formula: see text] molecules during and after their interaction with intense near-infrared fields, giving direct access to structural changes of the molecules and their fragmentation in real time. Tuning the intensity of the excitation pulses, we uncover a transition from a weak-field regime of excited but stable molecules to a high-field regime dominated by Coulomb explosion. In the transition region, the molecules expand by up to 50% of their initial size within just 140 fs, with major fragmentation only setting in afterward. This work demonstrates that x-ray diffractive imaging is capable of retrieving time-resolved structural information of large molecules reshaped by intense laser fields. Laser-driven fragmentation is a first step toward observing molecular processes modified by laser fields of increasing intensity.
Disciplines :
Physics
Author, co-author :
Schnorr, Kirsten ; Paul Scherrer Institut, 5232 Villigen, Switzerland ; Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany
Augustin, Sven ; Paul Scherrer Institut, 5232 Villigen, Switzerland ; Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany ; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
Schmid, Georg; Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany
Rouzée, Arnaud; Max Born Institut, 12489 Berlin, Germany
Obaid, Razib ; University of Connecticut, Storrs, CT 06269, USA
AlHaddad, Andre; Paul Scherrer Institut, 5232 Villigen, Switzerland ; Argonne National Laboratory, Argonne, IL 60439, USA
Berrah, Nora ; University of Connecticut, Storrs, CT 06269, USA
Blaga, Cosmin I; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA ; The Ohio State University, Columbus, OH 43210, USA
Bostedt, Christoph ; Paul Scherrer Institut, 5232 Villigen, Switzerland ; Argonne National Laboratory, Argonne, IL 60439, USA ; École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland
Cardosa-Gutierrez, Manuel Alejandro ; Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de chimie physique théorique
Carini, Gabriella; SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA ; Brookhaven National Laboratory, Upton, NY 11973, USA
Coffee, Ryan ; SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA
DiMauro, Louis F ; The Ohio State University, Columbus, OH 43210, USA
Hart, Philip ; SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA
Ito, Yuta; IMRAM, Tohoku University, 980-8577 Sendai, Japan
Kubicek, Katharina ; SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA ; Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany ; Centre for Ultrafast Imaging, Universität Hamburg, 22761 Hamburg, Germany ; Max-Planck-Institut für biophysikalische Chemie, 37077 Göttingen, Germany
Kumagai, Yoshiaki ; IMRAM, Tohoku University, 980-8577 Sendai, Japan
Küpper, Jochen ; Centre for Ultrafast Imaging, Universität Hamburg, 22761 Hamburg, Germany ; Department of Physics, Universität Hamburg, 22761 Hamburg, Germany ; Center for Free-Electron Laser Science, Deutsches Elektronen-Synchrotron, 22607 Hamburg, Germany
Lai, Yu Hang; The Ohio State University, Columbus, OH 43210, USA
Lindenblatt, Hannes ; Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany
Livingstone, Ruth A; Centre for Ultrafast Imaging, Universität Hamburg, 22761 Hamburg, Germany ; Center for Free-Electron Laser Science, Deutsches Elektronen-Synchrotron, 22607 Hamburg, Germany
Meister, Severin ; Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany
Moshammer, Robert ; Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany
Motomura, Koji; IMRAM, Tohoku University, 980-8577 Sendai, Japan
Möller, Thomas ; Technische Universität Berlin, 10623 Berlin, Germany
Nakahara, Kaz; SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA
Osipov, Timur; SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA
Pandey, Gaurav ; Université de Liège - ULiège > Molecular Systems (MolSys)
Ray, Dipanwita; SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA
Remacle, Françoise ; Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de chimie physique théorique
Rolles, Daniel ; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
Rost, Jan Michael; Max-Planck-Institut für Physik komplexer Systeme, 01187 Dresden, Germany
Schlichting, Ilme ; Max-Planck-Institut für Medizinische Forschung, 69120 Heidelberg, Germany
Schmidt, Rüdiger; Technische Universität Dresden, 01062 Dresden, Germany
K.S. acknowledges support through Starting Grant TMSGI2_211288 from the Swiss National Science Foundation. K.S. and K.K. thank the Volkswagen Foundation for awarding them a Peter Paul Ewald fellowship. S.A. acknowledges the European Union\u2019s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement no. 701647 for awarding a fellowship. S.A. and D.Ro. thank the US Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division under contract no. DEFG02-86ER13491 for support. R.O. and N.B. acknowledge support from the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy, grant no DE-SC0012376. C.I.B. thanks the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-FG02-04ER15614 for support. J.K. and K.K. acknowledge support from the Cluster of Excellence \u201CAdvanced Imaging of Matter\u201D of the Deutsche Forschungsgemeinschaft (DFG), EXC 2056, project ID 390715994. J.K. and R.A.L. thank the Cluster of Excellence \u201CCenter for Ultrafast Imaging\u201D (CUI, EXC 1074, ID 194651731) of the Deutsche Forschungsgemeinschaft for support. J.K. and K.K. acknowledge support from Deutsches Elektronen-Synchrotron DESY, a member of the Helmholtz Association (HGF). L.F.D. thanks the US National Science Foundation under contract no. 1605042 for support. T.P. acknowledges support by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany\u2019s Excellence Strategy EXC2181/1-390900948 (the Heidelberg STRUCTURES Excellence Cluster). All authors acknowledge support of the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515.Acknowledgments: We thank the lclS staff for optimal beamtime conditions and B. Mignolet for discussions. Funding: K.S. acknowledges support through Starting Grant tMSGi2_211288 from the Swiss National Science Foundation. K.S. and K.K. thank the volkswagen Foundation for awarding them a Peter Paul ewald fellowship. S.A. acknowledges the european Union\u2019s horizon 2020 research and innovation program under the Marie Sklodowska-curie grant agreement no. 701647 for awarding a fellowship. S.A. and d.Ro. thank the US department of energy, Office of Science, Basic energy Sciences, chemical Sciences, Geosciences, and Biosciences division under contract no. deFG02-86eR13491 for support. R.O. and N.B. acknowledge support from the chemical Sciences, Geosciences and Biosciences division, Office of Basic energy Sciences, Office of Science, US department of energy, grant no de-Sc0012376. c.i.B. thanks the US department of energy, Office of Science, Office of Basic energy Sciences under contract no. de-FG02-04eR15614 for support. J.K. and K.K. acknowledge support from the cluster of excellence \u201CAdvanced imaging of Matter\u201Dof the deutsche Forschungsgemeinschaft (dFG), eXc 2056, project id 390715994. J.K. and R.A.l. thank the cluster of excellence \u201Ccenter for Ultrafast imaging\u201D(cUi, eXc 1074, id 194651731) of the deutsche Forschungsgemeinschaft for support. J.K. and K.K. acknowledge support from deutsches elektronen-Synchrotron deSY, a member of the helmholtz Association (hGF). l.F.d. thanks the US National Science Foundation under contract no. 1605042 for support. t.P. acknowledges support by the deutsche Forschungsgemeinschaft (dFG, German Research Foundation) under Germany\u2019s excellence Strategy eXc2181/1-390900948 (the heidelberg StRUctUReS excellence cluster). All authors acknowledge support of the US department of energy, Office of Science, Office of Basic energy Sciences under contract no. de-Ac02-76SF00515. Author contributions: the experiment was carried out by K.S., S.A., G.S., A.R., R.O., A.A., N.B., c.B., G.c., R.c., P.h., Y.i., K.K., Y.K., J.K., Y.h.l., h.l., R.A.l., S.M., K.M., K.N., t.O., d.Ra., d.Ro., S.t., F.t., K.U., J.U., J.Z., c.P.S., and t.P. theory work was performed by U.S., J.M.R., R.S., M.c.-G., G.P., and F.R. the original draft was prepared by K.S., S.A., U.S., F.R., c.P.S., and t.P. the manuscript was reviewed and edited by all authors. Competing interests: the authors declare that they have no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials.
1. A. D. Bandrauk, Molecules in Laser Fields (Springer Netherlands, Dordrecht, 1995), pp. 131–150.
2. B. J. Sussman, D. Townsend, M. Y. Ivanov, A. Stolow, Dynamic stark control of photochemical processes. Science 314, 278 (2006).
3. P. H. Bucksbaum, A. Zavriyev, H. G. Muller, D. W. Schumacher, Softening of the H+ 2 molecular bond in intense laser fields. Phys. Rev. Lett. 64, 1883 (1990).
4. L. J. Frasinski, J. H. Posthumus, J. Plumridge, K. Codling, P. F. Taday, A. J. Langley, Manipulation of bond hardening in H+ 2 by chirping of intense femtosecond laser pulses. Phys. Rev. Lett. 83, 3625 (1999).
5. M. E. Corrales, J. González-Vázquez, G. Balerdi, I. R. Solá, R. de Nalda, L. Bañares, Control of ultrafast molecular photodissociation by laser-field-induced potentials. Nat. Chem. 6, 785 (2014).
6. J. Kim, H. Tao, J. L. White, V. S. Petrović, T. J. Martinez, P. H. Bucksbaum, Control of 1,3-cyclohexadiene photoisomerization using light-induced conical intersections. J. Phys. Chem. A 116, 2758–2763 (2012).
7. H. W. Kroto, J. R. Heath, S. C. O’Brien, R. F. Curl, R. E. Smalley, C60: Buckminsterfullerene. Nature 318, 162 EP (1985).
8. W. Krätschmer, L. D. Lamb, K. Fostiropoulos, D. R. Huffman, Solid C60: A new form of carbon. Nature 347, 354–358 (1990).
9. F. Lépine, Multiscale dynamics of C60 from attosecond to statistical physics. J. Phys. B At. Mol. Opt. Phys. 48, 122002 (2015).
10. E. E. B. Campbell, K. Hansen, K. Hoffmann, G. Korn, M. Tchaplyguine, M. Wittmann, I. V. Hertel, From above threshold ionization to statistical electron emission: The laser pulse-duration dependence of C60 photoelectron spectra. Phys. Rev. Lett. 84, 2128 (2000).
11. I. V. Hertel, T. Laarmann, C. P. Schulz, Ultrafast excitation, ionization, and fragmentation of C60. Adv. Atom. Mol. Optic. Phys. 50, 219–286 (2005).
12. N. Berrah, A. Sanchez-Gonzalez, Z. Jurek, R. Obaid, H. Xiong, R. J. Squibb, T. Osipov, A. Lutman, L. Fang, T. Barillot, J. D. Bozek, J. Cryan, T. J. A. Wolf, D. Rolles, R. Coffee, K. Schnorr, S. Augustin, H. Fukuzawa, K. Motomura, N. Niebuhr, L. J. Frasinski, R. Feifel, C. P. Schulz, K. Toyota, S. K. Son, K. Ueda, T. Pfeifer, J. P. Marangos, R. Santra, Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following x-ray multiphoton ionization. Nat. Phys. 15, 1279–1283 (2019).
13. G. P. Zhang, T. F. George, Controlling vibrational excitations in C60 by laser pulse durations. Phys. Rev. Lett. 93, 147401 (2004).
14. M. Fischer, J. Handt, G. Seifert, R. Schmidt, Orientation dependence of energy absorption and relaxation dynamics of C60 in fs-laser pulses. Phys. Rev. A 88, 061403 (2013).
15. V. R. Bhardwaj, P. B. Corkum, D. M. Rayner, Internal laser-induced dipole force at work in C60 molecule. Phys. Rev. Lett. 91, 203004 (2003).
16. M. Boyle, T. Laarmann, I. Shchatsinin, C. P. Schulz, I. V. Hertel, Fragmentation dynamics of fullerenes in intense femtosecond-laser fields: Loss of small neutral fragments on a picosecond time scale. J. Chem. Phys. 122, 181103 (2005).
17. T. Laarmann, I. Shchatsinin, A. Stalmashonak, M. Boyle, N. Zhavoronkov, J. Handt, R. Schmidt, C. P. Schulz, I. V. Hertel, Control of giant breathing motion in C60 with temporally shaped laser pulses. Phys. Rev. Lett. 98, 058302 (2007).
18. H. O. Jeschke, M. E. Garcia, J. Alonso, Nonthermal fragmentation of C60. Chem. Phys. Lett. 352, 154–162 (2002).
19. S. L. Dexheimer, D. M. Mittleman, R.W. Schoenlein, W. Vareka, X.-D. Xiang, A. Zettl, C.V. Shank, “Ultrafast dynamics of solid C60,” in Eighth International Conference on Ultrafast Phenomena. Technical Digest Series (Optica Publishing Group, 1992).
20. K. Nakai, H. Kono, Y. Sato, N. Niitsu, R. Sahnoun, M. Tanaka, Y. Fujimura, Ab initio molecular dynamics and wavepacket dynamics of highly charged fullerene cations produced with intense near-infrared laser pulses. Chem. Phys. 338, 127–134 (2007).
21. H. Fuest, Y. H. Lai, C. I. Blaga, K. Suzuki, J. Xu, P. Rupp, H. Li, P. Wnuk, P. Agostini, K. Yamazaki, M. Kanno, H. Kono, M. F. Kling, L. F. DiMauro, Diffractive imaging of C60 structural deformations induced by intense femtosecond midinfrared laser fields. Phys. Rev. Lett. 122, 053002 (2019).
22. T. Gorkhover, S. Schorb, R. Coffee, M. Adolph, L. Foucar, D. Rupp, A. Aquila, J. D. Bozek, S. W. Epp, B. Erk, L. Gumprecht, L. Holmegaard, A. Hartmann, R. Hartmann, G. Hauser, P. Holl, A. Hömke, P. Johnsson, N. Kimmel, K.-U. Kühnel, M. Messerschmidt, C. Reich, A. Rouzée, B. Rudek, C. Schmidt, J. Schulz, H. Soltau, S. Stern, G. Weidenspointner, B. White, J. Küpper, L. Strüder, I. Schlichting, J. Ullrich, D. Rolles, A. Rudenko, T. Möller, C. Bostedt, Femtosecond and nanometre visualization of structural dynamics in superheated nanoparticles. Nat. Photon. 10, 93–97 (2016).
23. M. P. Minitti, J. M. Budarz, A. Kirrander, J. S. Robinson, D. Ratner, T. J. Lane, D. Zhu, J. M. Glownia, M. Kozina, H. T. Lemke, M. Sikorski, Y. Feng, S. Nelson, K. Saita, B. Stankus, T. Northey, J. B. Hastings, P. M. Weber, Imaging molecular motion: Femtosecond x-ray scattering of an electrocyclic chemical reaction. Phys. Rev. Lett. 114, 255501 (2015).
24. J. M. Glownia, A. Natan, J. P. Cryan, R. Hartsock, M. Kozina, M. P. Minitti, S. Nelson, J. Robinson, T. Sato, T. van Driel, G. Welch, C. Weninger, D. Zhu, P. H. Bucksbaum, Self-referenced coherent diffraction x-ray movie of ångstrom- and femtosecond-scale atomic motion. Phys. Rev. Lett. 117, 153003 (2016).
25. K. Haldrup, G. Levi, E. Biasin, P. Vester, M. G. Laursen, F. Beyer, K. S. Kjær, T. Brandt van Driel, T. Harlang, A. O. Dohn, R. J. Hartsock, S. Nelson, J. M. Glownia, H. T. Lemke, M. Christensen, K. J. Gaffney, N. E. Henriksen, K. B. Møller, M. M. Nielsen, Ultrafast x-ray scattering measurements of coherent structural dynamics on the ground-state potential energy surface of a diplatinum molecule. Phys. Rev. Lett. 122, 063001 (2019).
26. B. Stankus, H. Yong, N. Zotev, J. M. Ruddock, D. Bellshaw, T. J. Lane, M. Liang, S. Boutet, S. Carbajo, J. S. Robinson, W. du, N. Goff, Y. Chang, J. E. Koglin, M. P. Minitti, A. Kirrander, P. M. Weber, Ultrafast x-ray scattering reveals vibrational coherence following rydberg excitation. Nat. Chem. 11, 716–721 (2019).
27. A. Guinier, G. Fournet, Small-Angle Scattering of X-rays (John Wiley & Sons, Inc., New York, 1st ed., 1955).
28. R. Ehlich, M. Westerburg, E. E. B. Campbell, Fragmentation of fullerenes in collisions with atomic and molecular targets. J. Chem. Phys. 104, 1900–1911 (1996).
29. C. Rose-Petruck, K. J. Schafer, K. R. Wilson, C. P. J. Barty, Ultrafast electron dynamics and inner-shell ionization in laser driven clusters. Phys. Rev. A 55, 1182–1190 (1997).
30. P. B. Corkum, Plasma perspective on strong field multiphoton ionization. Phys. Rev. Lett. 71, 1994–1997 (1993).
31. J. Kou, V. Zhakhovskii, S. Sakabe, K. Nishihara, S. Shimizu, S. Kawato, M. Hashida, K. Shimizu, S. Bulanov, Y. Izawa, Y. Kato, N. Nakashima, Anisotropic coulomb explosion of C60 irradiated with a high-intensity femtosecond laser pulse. J. Chem. Phys. 112, 5012–5020 (2000).
32. E. E. B. Campbell, R. D. Levine, Delayed ionization and fragmentation en route to thermionic emission: Statistics and dynamics. Annu. Rev. Phys. Chem. 51, 65–98 (2000).
33. R. Boll, J. M. Schäfer, B. Richard, K. Fehre, G. Kastirke, Z. Jurek, M. S. Schöffler, M. M. Abdullah, N. Anders, T. M. Baumann, S. Eckart, B. Erk, A. de Fanis, R. Dörner, S. Grundmann, P. Grychtol, A. Hartung, M. Hofmann, M. Ilchen, L. Inhester, C. Janke, R. Jin, M. Kircher, K. Kubicek, M. Kunitski, X. Li, T. Mazza, S. Meister, N. Melzer, J. Montano, V. Music, G. Nalin, Y. Ovcharenko, C. Passow, A. Pier, N. Rennhack, J. Rist, D. E. Rivas, D. Rolles, I. Schlichting, L. P. H. Schmidt, P. Schmidt, J. Siebert, N. Strenger, D. Trabert, F. Trinter, I. Vela-Perez, R. Wagner, P. Walter, M. Weller, P. Ziolkowski, S. K. Son, A. Rudenko, M. Meyer, R. Santra, T. Jahnke, X-ray multiphoton-induced Coulomb explosion images complex single molecules. Nat. Phys. 18, 423–428 (2022).
34. X. Li, R. Boll, P. Vindel-Zandbergen, J. González-Vázquez, D. E. Rivas, S. Bhattacharyya, K. Borne, K. Chen, A. de Fanis, B. Erk, R. Forbes, A. E. Green, M. Ilchen, B. Kaderiya, E. Kukk, H. V. S. Lam, T. Mazza, T. Mullins, B. Senfftleben, F. Trinter, S. Usenko, A. S. Venkatachalam, E. Wang, J. P. Cryan, M. Meyer, T. Jahnke, P. J. Ho, D. Rolles, A. Rudenko, Imaging a light-induced molecular elimination reaction with an X-ray free-electron laser. Nat. Commun. 16, 7006 (2025).
35. B. Richard, R. Boll, S. Banerjee, J. M. Schäfer, Z. Jurek, G. Kastirke, K. Fehre, M. S. Schöffler, N. Anders, T. M. Baumann, S. Eckart, B. Erk, A. de Fanis, R. Dörner, S. Grundmann, P. Grychtol, M. Hofmann, M. Ilchen, M. Kircher, K. Kubicek, M. Kunitski, X. Li, T. Mazza, S. Meister, N. Melzer, J. Montano, V. Music, Y. Ovcharenko, C. Passow, A. Pier, N. Rennhack, J. Rist, D. E. Rivas, D. Rolles, I. Schlichting, L. P. H. Schmidt, P. Schmidt, D. Trabert, F. Trinter, R. Wagner, P. Walter, P. Ziolkowski, A. Rudenko, M. Meyer, R. Santra, L. Inhester, T. Jahnke, Imaging collective quantum fluctuations of the structure of a complex molecule. Science 389, 650–654 (2025).
36. Y. Inubushi, G. Yamaguchi, J. Yamada, Y. Kubota, I. Inoue, T. Osaka, T. Yabuuchi, K. Tono, M. Yabashi, Development of portable nanofocusing optics for X-ray free-electron laser pulses. J. Synchrotron Rad. 32, 534–538 (2025).
37. P. Emma, R. Akre, J. Arthur, R. Bionta, C. Bostedt, J. Bozek, A. Brachmann, P. Bucksbaum, R. Coffee, F. J. Decker, Y. Ding, D. Dowell, S. Edstrom, A. Fisher, J. Frisch, S. Gilevich, J. Hastings, G. Hays, P. Hering, Z. Huang, R. Iverson, H. Loos, M. Messerschmidt, A. Miahnahri, S. Moeller, H. D. Nuhn, G. Pile, D. Ratner, J. Rzepiela, D. Schultz, T. Smith, P. Stefan, H. Tompkins, J. Turner, J. Welch, W. White, J. Wu, G. Yocky, J. Galayda, First lasing and operation of an ångstrom-wavelength free-electron laser. Nat. Photon. 4, 641–647 (2010).
38. T. Osipov, C. Bostedt, J. C. Castagna, K. R. Ferguson, M. Bucher, S. C. Montero, M. L. Swiggers, R. Obaid, D. Rolles, A. Rudenko, J. D. Bozek, N. Berrah, The lamp instrument at the linac coherent light source free-electron laser. Rev. Sci. Instrum. 89, 035112 (2018).
39. J. Tersoff, Modeling solid-state chemistry: Interatomic potentials for multicomponent systems. Phys. Rev. B 39, 5566–5568 (1989).
40. K. R. Ferguson, M. Bucher, J. D. Bozek, S. Carron, J. C. Castagna, R. Coffee, G. I. Curiel, M. Holmes, J. Krzywinski, M. Messerschmidt, M. Minitti, A. Mitra, S. Moeller, P. Noonan, T. Osipov, S. Schorb, M. Swiggers, A. Wallace, J. Yin, C. Bostedt, The atomic, molecular and optical science instrument at the linac coherent light source. J. Synchrotron Radiat. 22, 492–497 (2015).
41. L. Strüder, S. Epp, D. Rolles, R. Hartmann, P. Holl, G. Lutz, H. Soltau, R. Eckart, C. Reich, K. Heinzinger, C. Thamm, A. Rudenko, F. Krasniqi, K. U. Kühnel, C. Bauer, C. D. Schröter, R. Moshammer, S. Techert, D. Miessner, M. Porro, O. Hälker, N. Meidinger, N. Kimmel, R. Andritschke, F. Schopper, G. Weidenspointner, A. Ziegler, D. Pietschner, S. Herrmann, U. Pietsch, A. Walenta, W. Leitenberger, C. Bostedt, T. Möller, D. Rupp, M. Adolph, H. Graafsma, H. Hirsemann, K. Gärtner, R. Richter, L. Foucar, R. L. Shoeman, I. Schlichting, J. Ullrich, Large-format, high-speed, x-ray pnCCDs combined with electron and ion imaging spectrometers in a multipurpose chamber for experiments at 4th generation light sources. Nucl. Instrum. Methods Phys. Res. A 614, 483–496 (2010).
42. M. P. Minitti, J. S. Robinson, R. N. Coffee, S. Edstrom, S. Gilevich, J. M. Glownia, E. Granados, P. Hering, M. C. Hoffmann, A. Miahnahri, D. Milathianaki, W. Polzin, D. Ratner, F. Tavella, S. Vetter, M. Welch, W. E. White, A. R. Fry, Optical laser systems at the Linac Coherent Light Source. J. Synchrotron Radiat. 22, 526–531 (2015).
43. X. Lu, L. Feng, T. Akasaka, S. Nagase, Current status and future developments of endohedral metallofullerenes. Chem. Soc. Rev. 41, 7723–7760 (2012).
44. K. R. Ferguson, M. Bucher, T. Gorkhover, S. Boutet, H. Fukuzawa, J. E. Koglin, Y. Kumagai, A. Lutman, A. Marinelli, M. Messerschmidt, K. Nagaya, J. Turner, K. Ueda, G. J. Williams, P. H. Bucksbaum, C. Bostedt, Transient lattice contraction in the solid-to-plasma transition. Sci. Adv. 2, e1500837 (2016).
45. K. R. Ferguson, Crystal structure determination of xenon nanoparticles and x-ray induced transient lattice contraction in the solid-to-plasma transition, Ph.D. thesis, Stanford University (2016). https://stacks.stanford.edu/file/druid:qk328xg1417/SubmittedDissertation-augmented.pdf.
46. M. Harmand, R. Coffee, M. R. Bionta, M. Chollet, D. French, D. Zhu, D. M. Fritz, H. T. Lemke, N. Medvedev, B. Ziaja, S. Toleikis, M. Cammarata, Achieving few-femtosecond time-sorting at hard x-ray free-electron lasers. Nat. Photon. 7, 215–218 (2013).
47. S. Schorb, T. Gorkhover, J. P. Cryan, J. M. Glownia, M. R. Bionta, R. N. Coffee, B. Erk, R. Boll, C. Schmidt, D. Rolles, A. Rudenko, A. Rouzee, M. Swiggers, S. Carron, J. C. Castagna, J. D. Bozek, M. Messerschmidt, W. F. Schlotter, C. Bostedt, X-ray–optical cross-correlator for gas-phase experiments at the Linac Coherent Light Source free-electron laser. Appl. Phys. Lett. 100, 121107 (2012).
48. B. F. Murphy, T. Osipov, Z. Jurek, L. Fang, S. K. Son, M. Mucke, J. H. D. Eland, V. Zhaunerchyk, R. Feifel, L. Avaldi, P. Bolognesi, C. Bostedt, J. D. Bozek, J. Grilj, M. Guehr, L. J. Frasinski, J. Glownia, D. T. Ha, K. Hoffmann, E. Kukk, B. K. McFarland, C. Miron, E. Sistrunk, R. J. Squibb, K. Ueda, R. Santra, N. Berrah, Femtosecond x-ray-induced explosion of C60 at extreme intensity. Nat. Comm. 5, 4281 (2014).
49. U. Saalmann, C. Siedschlag, J. M. Rost, Topical review: Mechanisms of cluster ionization in strong laser pulses. J. Phys. B At. Mol. Opt. Phys. 39, R39 (2006).
50. S. G. Kim, D. Tománek, Melting the fullerenes: A molecular dynamics study. Phys. Rev. Lett. 72, 2418–2421 (1994).
51. A. D. Bandrauk, S. Chelkowski, N. H. Shon, Measuring the electric field of few-cycle laser pulses by attosecond cross correlation. Phys. Rev. Lett. 89, 283903 (2002).
52. H. Li, B. Mignolet, G. Wachter, S. Skruszewicz, S. Zherebtsov, F. Süßmann, A. Kessel, S. A. Trushin, N. G. Kling, M. Kübel, B. Ahn, D. Kim, I. Ben-Itzhak, C. L. Cocke, T. Fennel, J. Tiggesbäumker, K. H. Meiwes-Broer, C. Lemell, J. Burgdörfer, R. D. Levine, F. Remacle, M. F. Kling, Coherent electronic wave packet motion in C60 controlled by the waveform and polarization of few-cycle laser fields. Phys. Rev. Lett. 114, 123004 (2015).
53. B. Mignolet, R. D. Levine, F. Remacle, Control of electronic dynamics visualized by angularly resolved photoelectron spectra: A dynamical simulation with an IR pump and xuv attosecond-pulse-train probe. Phys. Rev. A 89, 021403 (2014).
54. T. Yanai, Y. Kurashige, D. Ghosh, G. K.-L. Chan, Accelerating convergence in iterative solution for large-scale complete active space self-consistent-field calculations. Int. J. Quantum Chem. 109, 2178–2190 (2009).
55. B. Mignolet, J. O. Johansson, E. E. B. Campbell, F. Remacle, Probing rapidly-ionizing super-atom molecular orbitals in C60: A computational and femtosecond photoelectron spectroscopy study. ChemPhysChem 14, 3332–3340 (2013).
56. B. Mignolet, R. D. Levine, F. Remacle, Localized electron dynamics in attosecond-pulse-excited molecular systems: Probing the time-dependent electron density by sudden photoionization. Phys. Rev. A 86, 053429 (2012).
57. G. M. Seabra, I. G. Kaplan, V. G. Zakrzewski, J. V. Ortiz, Electron propagator theory calculations of molecular photoionization cross sections: The first-row hydrides. J. Chem. Phys. 121, 4143–4155 (2004).
