Abstract
Manipulation and control of molecular electron dynamics is currently in the spotlight for numerous multidisciplinary applications in physics, chemistry and biology. During the last decade, free electron lasers and sources based on high-order harmonic generation have been successfully developed to enable the generation of femtosecond and attosecond intense radiation pulses in the ultraviolet and soft X-ray regions. These tools have lead to an outbreak of pump-probe experiments suited to explore structural dynamics in atoms and molecules with spatial and temporal resolutions on the atomic length and intrinsic electronic time scales, respectively. Such experiments, using hydrogen molecules (H2, D2) as prototypical examples, have been performed to study molecular dissociative single and multi-photon ionization, photon-induced symmetry breaking in molecular dissociation, and time-resolved imaging of coherent nuclear wave-packets. The counterpart state-of-the-art time-dependent theoretical methods, able to provide a solid groundwork for describing and interpreting the underlying ultrafast physical molecular dynamics in such experiments, are still scarce. The difficulty is to achieve an accurate description accounting for the full dimensionality of the problem. A proper treatment of nuclear degrees of freedom is already indispensable to study multiphoton single ionization of diatomic molecules. This is discussed in the present manuscript in different applications. We first examine the role of the coupled electronic and nuclear motions in problems that probe coherent nuclear wave-packets using intense UV pulses and in resonance-enhanced multiphoton single ionization (REMPI) processes, whose rates are underestimated when using approaches within the fixed nuclei approximation. Later, we show that for highly intense fields the presence of vibrational structure leads to step-ladder Rabi oscillations that are probed in the REMPI probabilities. Finally, we demonstrate the suitability of these time-dependent full-dimensional treatments to provide time-resolved images of autoionization of H2, following the time evolution of both electron and proton distributions after the interaction with ultrashort pulses.
Access this chapter
Tax calculation will be finalised at checkout
Purchases are for personal use only
References
J. Seres, E. Seres, A.J. Verhoef, G. Tempea, C. Streli, P. Wobrauschek, V. Yakovlev, A. Scrinzi, C. Spielmann, F. Krausz, Nature 433, 596 (2005)
A.H. Zewail, Annu. Rev. Phys. Chem. 57(1), 65–103 (2006)
S. Lunnemann, A.I. Kuleff, L.S. Cederbaum, J. Chem. Phys. 129(10), 104305 (2008)
A.H. Zewail, J. Phys. Chem. A 104(24), 5660–5694 (2000)
J. Ullrich, R. Moshammer, A. Dorn, R. Dörner, L.P.H. Schmidt, H. Schmidt-Böcking, Rep. Prog. Phys. 66(9), 1463–1545 (2003)
C. Bostedt, H.N. Chapman, J.T. Costello, J.R. Crespo López-Urrutia, S. Düsterer, S.W. Epp, J. Feldhaus, A. Föhlisch, M. Meyer, T. Möller, Nucl. Instrum. Methods Phys. Res., Sect. A, Accel. Spectrom. Detect. Assoc. Equip. 601(1–2), 108–122 (2009)
A. Barty, J. Phys. B, At. Mol. Opt. Phys. 43(19), 194014 (2010)
J.U.H. Chapman, J.M. Rost, J. Phys. B, At. Mol. Opt. Phys. 43(19), 190201 (2010)
M. Drescher, M. Hentschel, R. Kienberger, G. Tempea, C. Spielmann, G.A. Reider, P.B. Corkum, F. Krausz, Science 291(5510), 1923–1927 (2001)
M. Hentschel, R. Kienberger, C. Spielmann, G.A. Reider, N. Milosevic, T. Brabec, P. Corkum, U. Heinzmann, M. Drescher, F. Krausz, Nature 414, 509–513 (2001)
P. Salières, M. Lewenstein, Meas. Sci. Technol. 12, 1818 (2001)
G. Sansone, E. Benedetti, F. Calegari, C. Vozzi, L. Avaldi, R. Flammini, L. Poletto, P. Villoresi, C. Altucci, R. Velotta, S. Stagira, S. De Silvestri, M. Nisoli, Science 314(5798), 443–446 (2006)
A. Scrinzi, M.Y. Ivanov, R. Kienberger, D.M. Villeneuve, J. Phys. B, At. Mol. Opt. Phys. 39(1), 1 (2006)
E. Goulielmakis, V.S. Yakovlev, A.L. Cavalieri, M. Uiberacker, V. Pervak, A. Apolonski, R. Kienberger, U. Kleineberg, F. Krausz, Science 317(5839), 769–775 (2007)
M.F. Kling, M.J.J. Vrakking, Annu. Rev. Phys. Chem. 59(1), 463–492 (2008)
F. Krausz, M. Ivanov, Rev. Mod. Phys. 81, 163–234 (2009)
B. Sheehy, B. Walker, L.F. DiMauro, Phys. Rev. Lett. 74(24), 4799–4802 (1995)
J.H. Posthumus, Rep. Prog. Phys. 67(5), 623 (2004)
C.R. Calvert, W.A. Bryan, W.R. Newell, I.D. Williams, Phys. Rep. 491(1), 1–28 (2010)
A. Lafosse, M. Lebech, J.C. Brenot, P.M. Guyon, L. Spielberger, O. Jagutzki, J.C. Houver, D. Dowek, J. Phys. B, At. Mol. Opt. Phys. 36(23), 4683 (2003)
F. Martín, J. Fernández, T. Havermeier, L. Foucar, T. Weber, K. Kreidi, M. Schöffler, L. Schmidt, T. Jahnke, O. Jagutzki, A. Czasch, E.P. Benis, T. Osipov, A.L. Landers, A. Belkacem, M.H. Prior, H. Schmidt-Böcking, C.L. Cocke, R. Dörner, Science 315(5812), 629–633 (2007)
D. Dowek, J.F. Pérez-Torres, Y.J. Picard, P. Billaud, C. Elkharrat, J.C. Houver, J.L. Sanz-Vicario, F. Martín, Phys. Rev. Lett. 104(23), 2–5 (2010)
T. Reddish, A. Padmanabhan, M. MacDonald, L. Zuin, J. Fernández, A. Palacios, F. Martín, Phys. Rev. Lett. 108(2), 1–5 (2012)
M. Glass-Maujean, J. Chem. Phys. 85, 4830–4834 (1986)
M. Glass-Maujean, J. Chem. Phys. 89, 2839 (1988)
M. Glass-Maujean, H. Schmoranzer, J. Phys. B, At. Mol. Opt. Phys. 38(8), 1093–1105 (2005)
E.M. García, J.A. Ruiz, S. Menmuir, E. Rachlew, P. Erman, A. Kivimäki, M. Glass-Maujean, R. Richter, M. Coreno, J. Phys. B, At. Mol. Opt. Phys. 39(2), 205 (2006)
S. Arai, T. Kamosaki, M. Ukai, K. Shinsaka, Y. Hatano, Y. Ito, H. Koizumi, A. Yagishita, K. Ito, K. Tanaka, J. Chem. Phys. 88, 3016 (1988)
T. Odagiri, M. Murata, M. Kato, N. Kouchi, J. Phys. B, At. Mol. Opt. Phys. 37(19), 3909 (2004)
J.D. Bozek, J.E. Furst, T.J. Gay, H. Gould, A.L.D. Kilcoyne, J.R. Machacek, F. Martín, K.W. McLaughlin, J.L. Sanz-Vicario, J. Phys. B, At. Mol. Opt. Phys. 39(23), 4871 (2006)
J.R. Machacek, V.M. Andrianarijaona, J.E. Furst, A.L.D. Kilcoyne, A.L. Landers, E.T. Litaker, K.W. McLaughlin, T.J. Gay, J. Phys. B, At. Mol. Opt. Phys. 44(4), 045201 (2011)
K. Hoshina, A. Hishikawa, K. Kato, T. Sako, K. Yamanouchi, E.J. Takahashi, Y. Nabekawa, K. Midorikawa, J. Phys. B, At. Mol. Opt. Phys. 39(4), 813–829 (2006)
Y.H. Jiang, A. Rudenko, J.F. Pérez-Torres, O. Herrwerth, L. Foucar, M. Kurka, K.U. Kühnel, M. Toppin, E. Plésiat, F. Morales, F. Martín, M. Lezius, M.F. Kling, T. Jahnke, R. Dörner, J.L. Sanz-Vicario, J. van Tilborg, A. Belkacem, M. Schulz, K. Ueda, T.J.M. Zouros, S. Düsterer, R. Treusch, C.D. Schröter, R. Moshammer, J. Ullrich, Phys. Rev. A 81(5), 1–4 (2010)
Y.H. Jiang, A. Rudenko, E. Plésiat, L. Foucar, M. Kurka, K.U. Kühnel, T. Ergler, J.F. Pérez-Torres, F. Martín, O. Herrwerth, M. Lezius, M.F. Kling, J. Titze, T. Jahnke, R. Dörner, J.L. Sanz-Vicario, M. Schöffler, J. van Tilborg, A. Belkacem, K. Ueda, T.J.M. Zouros, S. Düsterer, R. Treusch, C.D. Schröter, R. Moshammer, J. Ullrich, Phys. Rev. A 81(2), 1–4 (2010)
P.M. Paul, E.S. Toma, P. Breger, G. Mullot, F. Augé, P. Balcou, H.G. Muller, P. Agostini, Science 292(5522), 1689–1692 (2001)
K.P. Singh, F. He, P. Ranitovic, W. Cao, S. De, D. Ray, S. Chen, U. Thumm, A. Becker, M.M. Murnane, H.C. Kapteyn, I.V. Litvinyuk, C.L. Cocke, Phys. Rev. Lett. 104(2), 1–4 (2010)
G. Sansone, F. Kelkensberg, J.F. Pérez-Torres, F. Morales, M.F. Kling, W. Siu, O. Ghafur, P. Johnsson, M. Swoboda, E. Benedetti, F. Ferrari, F. Lépine, J.L. Sanz-Vicario, S. Zherebtsov, I. Znakovskaya, A. L’Huillier, M.Y. Ivanov, M. Nisoli, F. Martín, M.J.J. Vrakking, Nature 465(7299), 763–766 (2010)
F. Kelkensberg, W. Siu, J.F. Pérez-Torres, F. Morales, G. Gademann, A. Rouzée, P. Johnsson, M. Lucchini, F. Calegari, J.L. Sanz-Vicario, F. Martín, M.J.J. Vrakking, Phys. Rev. Lett. 107, 043002 (2011)
C.H. Greene, B. Yoo, J. Phys. Chem. 99(6), 1711–1718 (1995)
J. Colgan, D. Glass, K. Higgins, P. Burke, J. Phys. B, At. Mol. Opt. Phys. 34, 2089 (2001)
A. Apalategui, A. Saenz, J. Phys. B, At. Mol. Opt. Phys. 35, 1909 (2002)
A. Awasthi, Y.V. Vanne, A. Saenz, J. Phys. B, At. Mol. Opt. Phys. 38, 3973 (2005)
C. Meier, V. Engel, Phys. Rev. Lett. 73, 3207–3210 (1994)
Z. Sun, N. Lou, Phys. Rev. Lett. 91, 023002 (2003)
I. Sánchez, F. Martín, J. Chem. Phys. 106(18), 7720 (1997)
I. Sánchez, F. Martín, Phys. Rev. Lett. 79, 1654–1657 (1997)
I. Sánchez, F. Martín, Phys. Rev. A 57(2), 1006–1017 (1998)
I. Sánchez, F. Martín, J. Chem. Phys. 110, 6702–6713 (1999)
H. Feshbach, Ann. Phys. 19, 287–313 (1962)
T. Brabec, F. Krausz, Rev. Mod. Phys. 72, 545–591 (2000)
A. Palacios, H. Bachau, F. Martín, Phys. Rev. Lett. 96(14), 143001 (2006)
A. Palacios, H. Bachau, F. Martin, Phys. Rev. A 74(3), 1–4 (2006)
J. Sanz-Vicario, H. Bachau, F. Martín, Phys. Rev. A 73(3), 1–12 (2006)
J. Sanzvicario, A. Palacios, J. Cardona, H. Bachau, F. Martín, J. Electron Spectrosc. Relat. Phenom. 161(1–3), 182–187 (2007)
A.S. Kheifets, Phys. Rev. A 71, 022704 (2005)
A.S. Kheifets, I. Bray, Phys. Rev. A 72, 022703 (2005)
J. Colgan, M.S. Pindzola, F. Robicheaux, Phys. Rev. Lett. 98, 153001 (2007)
T.-G. Lee, M.S. Pindzola, F. Robicheaux, J. Phys. B, At. Mol. Opt. Phys. 43(16), 165601 (2010)
W. Vanroose, F. Martín, T.N. Rescigno, C.W. McCurdy, Science 310(5755), 1787–1789 (2005)
L. Tao, C.W. McCurdy, T.N. Rescigno, Phys. Rev. A 82, 023423 (2010)
X. Guan, K. Bartschat, B.I. Schneider, Phys. Rev. A 83, 043403 (2011)
W. Vanroose, D. Horner, F. Martín, T. Rescigno, C. McCurdy, Phys. Rev. A 74(5), 1–19 (2006)
J. Colgan, M.S. Pindzola, F. Robicheaux, J. Phys. B, At. Mol. Opt. Phys. 41(12), 121002 (2008)
F. Morales, F. Martín, D.A. Horner, T.N. Rescigno, C.W. McCurdy, J. Phys. B, At. Mol. Opt. Phys. 42(13), 134013 (2009)
X. Guan, K. Bartschat, B.I. Schneider, Phys. Rev. A 82, 041404 (2010)
F. Martín, J. Phys. B, At. Mol. Opt. Phys. 32(16), 197 (1999)
M. Cortés, F. Martín, J. Phys. B, At. Mol. Opt. Phys. 27(23), 5741 (1994)
H. Bachau, E. Cormier, P. Decleva, J.E. Hansen, F. Martín, Rep. Prog. Phys. 64(12), 1815 (2001)
A. Palacios, H. Bachau, F. Martín, J. Phys. B, At. Mol. Opt. Phys. 38(6), 99 (2005)
S. Balay, J. Brown, K. Buschelman, W.D. Gropp, D. Kaushik, M.G. Knepley, L.C. McInnes, B.F. Smith, H. Zhang, PETSc web page (2011). http://www.mcs.anl.gov/petsc
M. Leventhal, R. Robiscoe, K. Lea, Phys. Rev. 158(1), 49–56 (1967)
S.L. Guberman, J. Chem. Phys. 78, 1404–1413 (1983)
L. Siebbeles, C.L. Sech, J. Phys. B, At. Mol. Opt. Phys. 27(19), 4443 (1994)
I. Borges Jr, C.E. Bielschowsky, J. Phys. B, At. Mol. Opt. Phys. 33(9), 1713 (2000)
I. Borges Jr., C.E. Bielschowsky, Chem. Phys. Lett. 342, 411–416 (2001)
A. González-Castrillo, J.F. Pérez-Torres, A. Palacios, F. Martín, Theor. Chem. Acc. 128(4–6), 735–742 (2010)
G. Sansone, F. Kelkensberg, F. Morales, J.F. Pérez-Torres, F. Martín, M.J.J. Vrakking, IEEE J. Sel. Top. Quantum Electron. 18, 520 (2012)
L.A.A. Nikolopoulos, P. Lambropoulos, J. Phys. B 39, 883–893 (2006)
Y. Furukawa, Y. Nabekawa, T. Okino, S. Saugout, K. Yamanouchi, K. Midorikawa, Phys. Rev. A 82(1), 1–5 (2010)
A. Palacios, H. Bachau, F. Martín, Phys. Rev. A 75(1) (2007)
J.F. Pérez-Torres, J.L. Sanz-Vicario, H. Bachau, F. Martín, J. Phys. B, At. Mol. Opt. Phys. 43(1), 015204 (2010)
I.I. Rabi, Phys. Rev. 51, 652 (1937)
L. Allen, J.H. Eberly, Optical Resonances and Two-Level Atoms (Wiley, New York, 1975)
M.A. Quesada, A.M.F. Lau, D.H. Parker, D.W. Chandler, Phys. Rev. A 36, 4107–4110 (1987)
B. Girard, G.O. Sitz, R.N. Zare, N. Billy, J. Vigué, J. Chem. Phys. 97, 26 (1992)
S. Xu, G. Sha, B. Jiang, W. Sun, X. Chen, C. Zhang, Chem. Phys. 100, 6122 (1994)
J. Qi, G. Lazarov, X. Wang, L. Li, L.M. Narducci, A.M. Lyyra, F.C. Spano, Phys. Rev. Lett. 83, 288–291 (1999)
J. Qi, F.C. Spano, T. Kirova, A. Lazoudis, J. Magnes, L. Li, L.M. Narducci, R.W. Field, A.M. Lyyra, Phys. Rev. Lett. 88, 173003 (2002)
S. Ghosh, J.E. Sharping, D.G. Ouzounov, A.L. Gaeta, Phys. Rev. Lett. 94, 093902 (2005)
E. Ahmed, A. Hansson, P. Qi, T. Kirova, A. Lazoudis, S. Kotochigova, A.M. Lyyra, L. Li, J. Qi, S. Magnier, J. Chem. Phys. 124, 084308 (2006)
M. Kremer, B. Fischer, B. Feuerstein, V.L.B. de Jesus, V. Sharma, C. Hofrichter, A. Rudenko, U. Thumm, C.D. Schröter, R. Moshammer, J. Ullrich, Phys. Rev. Lett. 103(21), 213003 (2009)
B. Fischer, M. Kremer, T. Pfeifer, B. Feuerstein, V. Sharma, U. Thumm, C. Schröter, R. Moshammer, J. Ullrich, Phys. Rev. Lett. 105(22), 1–4 (2010)
E. Charron, A. Giusti-Suzor, F.H. Mies, Phys. Rev. Lett. 75(15), 2815–2818 (1995)
A. González-Castrillo, A. Palacios, F. Catoire, H. Bachau, F. Martín, J. Phys. Chem. A (2012)
Acknowledgements
This work was accomplished with an allocation of computer time from Mare Nostrum BSC and CCC-UAM, and was partially supported by the MICINN projects FIS2010-15127, ACI2008-0777 and CSD 2007-00010, the ERA-Chemistry project PIM2010EEC-00751, the European grants MC-ITN CORINF and MC-RG ATTOTREND, the European COST Action CM0702, and the XCHEM Advanced Grant 290853 of the European Research Council. AP and PR acknowledge a Juan de la Cierva post-doctoral Contract from MICINN.
Author information
Authors and Affiliations
Corresponding author
Editor information
Editors and Affiliations
Rights and permissions
Copyright information
© 2014 Springer International Publishing Switzerland
About this chapter
Cite this chapter
Palacios, A., Rivière, P., González-Castrillo, A., Martín, F. (2014). XUV Lasers for Ultrafast Electronic Control in H2 . In: de Nalda, R., Bañares, L. (eds) Ultrafast Phenomena in Molecular Sciences. Springer Series in Chemical Physics, vol 107. Springer, Cham. https://doi.org/10.1007/978-3-319-02051-8_2
Download citation
DOI: https://doi.org/10.1007/978-3-319-02051-8_2
Publisher Name: Springer, Cham
Print ISBN: 978-3-319-02050-1
Online ISBN: 978-3-319-02051-8
eBook Packages: Physics and AstronomyPhysics and Astronomy (R0)