Ultrafast energy redistribution in C60 fullerenes: A real time study by two-color femtosecond spectroscopy

Journal of Chemical Physics

Volumn 129, Issue 20, 2008, Pages

  Shchatsinin, Ihar ^a   Laarmann, Tim ^a,b   Zhavoronkov, Nick ^a   Schulz, Claus Peter ^a   Hertel, Ingolf V ^a,c  

^a MAX BORN INSTITUT   (Germany)

^b DESY   (Germany)

^c FREIE UNIVERSITÄT BERLIN   (Germany)

Author keywords

[No Author keywords available]

Indexed keywords

DYNAMICS; FULLERENES; HIGH PERFORMANCE LIQUID CHROMATOGRAPHY; MASS SPECTROMETRY; MOLECULAR MODELING; MOLECULAR ORBITALS; PUMPING (LASER); PUMPS; RELAXATION PROCESSES;

C60 FULLERENES; CHARACTERISTIC RELAXATION TIMES; CHARGE STATES; COLLECTIVE EFFECTS; DEGREES OF FREEDOMS; ELECTRONIC SYSTEMS; ENERGY DEPOSITIONS; ENERGY REDISTRIBUTIONS; ENERGY SHARING; EXCITATION PROCESSES; EXCITED ELECTRONS; FEMTOSECOND PUMPS; FEMTOSECOND SPECTROSCOPIES; FIELD EXCITATIONS; FORMATION DYNAMICS; FRAGMENT IONS; FS PULSES; HIGHEST OCCUPIED MOLECULAR ORBITALS; LASER PULSE INTENSITIES; LOWEST UNOCCUPIED MOLECULAR ORBITALS; MICROCANONICAL ENSEMBLES; MULTIPLE IONIZATIONS; MULTIPLY CHARGED; NEUTRAL SPECIES; NONEQUILIBRIUM DISTRIBUTIONS; REAL TIMES; SET-UPS; TIME-RESOLVED; TOTAL ENERGIES; ULTRA FASTS; VIBRATIONAL MODES;

PULSED LASER APPLICATIONS;

EID: 57149144729     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.3026734     Document Type: Article

References (39)

1. A. N. Markevitch, D. A. Romanov, S. M. Smith, and R. J. Levis, Phys. Rev. A 1050-2947 10.1103/PhysRevA.75.053402 75, 053402 (2007).
2. I. V. Hertel, T. Laarmann, and C. P. Schulz, in Advances in Atomic, Molecular, and Optical Physics, edited by, B. Bederson, and, H. Walter, (Elsevier, Amsterdam, 2005), Vol. 50, pp. 219-286.
3. A. Jaroń-Becker, A. Becker, and F. H. M. Faisal, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.96.143006 96, 143006 (2006).
4. A. Jaroń-Becker, A. Becker, and F. H. M. Faisal, J. Chem. Phys. 0021-9606 10.1063/1.2712844 126, 124310 (2007).
5. B. Torralva, T. A. Niehaus, M. Elstner, S. Suhai, T. Frauenheim, and R. E. Allen, Phys. Rev. B 0163-1829 10.1103/PhysRevB.64.153105 64, 153105 (2001).
6. D. Bauer, F. Ceccherini, A. Macchi, and F. Cornolti, Phys. Rev. A 1050-2947 10.1103/PhysRevA.64.063203 64, 063203 (2001).
7. G. P. Zhang, X. Sun, and T. F. George, Phys. Rev. B 0163-1829 10.1103/PhysRevB.68.165410 68, 165410 (2003).
8. T. Brabec, M. Côt́, P. Boulanger, and L. Ramunno, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.95.073001 95, 073001 (2005).
9. I. Shchatsinin, T. Laarmann, G. Stibenz, G. Steinmeyer, A. Stalmashonak, N. Zhavoronkov, C. P. Schulz, and I. V. Hertel, J. Phys. Chem. 125, 194320 (2006). 0022-3654
10. M. Ruggenthaler, S. Popruzhenko, and D. Bauer, Phys. Rev. A 1050-2947 10.1103/PhysRevA.78.033413 78, 033413 (2008).
11. G. P. Zhang, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.95.047401 95, 047401 (2005).
12. M. Boyle, T. Laarmann, K. Hoffmann, M. Hed́n, E. E. B. Campbell, C. P. Schulz, and I. V. Hertel, Eur. Phys. J. D 1434-6060 10.1140/epjd/e2005- 00281-7 36, 339 (2005).
13. G. P. Zhang and T. F. George, Phys. Rev. B 0163-1829 10.1103/PhysRevB.76. 085410 76, 085410 (2007).
14. M. Boyle, T. Laarmann, I. Shchatsinin, C. P. Schulz, and I. V. Hertel, J. Chem. Phys. 0021-9606 10.1063/1.1903949 122, 181103 (2005).
15. G. P. Zhang and T. F. George, Phys. Rev. B 0163-1829 10.1103/PhysRevB.73. 035422 73, 035422 (2006).
16. R. Sahnoun, K. Nakai, Y. Sato, H. Kono, Y. Fujimura, and M. Tanaka, Chem. Phys. Lett. 0009-2614 10.1016/j.cplett.2006.08.108 430, 167 (2006).
17. R. Sahnoun, K. Nakai, Y. Sato, H. Kono, Y. Fujimura, and M. Tanaka, J. Chem. Phys. 0021-9606 10.1063/1.2371109 125, 184306 (2006).
18. T. Laarmann, I. Shchatsinin, A. Stalmashonak, M. Boyle, N. Zhavoronkov, J. Handt, R. Schmidt, C. P. Schulz, and I. Hertel, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.98.058302 98, 058302 (2007).
19. K. Nakai, H. Kono, Y. Sato, N. Niitsu, R. Sahnoun, M. Tanaka, and Y. Fujimura, Chem. Phys. 0301-0104 10.1016/j.chemphys.2007.04.011 338, 127 (2007).
20. T. Hertel and G. Moos, Chem. Phys. Lett. 0009-2614 10.1016/S0009-2614(00) 00256-6 320, 359 (2000).
21. E. E. B. Campbell, K. Hansen, K. Hoffmann, G. Korn, M. Tchaplyguine, M. Wittmann, and I. V. Hertel, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.84. 2128 84, 2128 (2000).
22. I. V. Hertel, H. Steger, J. DeVries, B. Weisser, C. Menzel, B. Kamke, and W. Kamke, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.68.784 68, 784 (1992).
23. E. E. B. Campbell, G. Ulmer, and I. V. Hertel, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.67.1986 67, 1986 (1991).
24. K. Hansen, K. Hoffmann, and E. E. B. Campbell, J. Chem. Phys. 0021-9606 10.1063/1.1584671 119, 2513 (2003).
25. R. Bauernschmitt, R. Ahlrichs, F. H. Hennrich, and M. M. Kappes, J. Am. Chem. Soc. 0002-7863 10.1021/ja9730167 120, 5052 (1998).
26. M. Boyle, M. Hed́n, C. P. Schulz, E. E. B. Campbell, and I. V. Hertel, Phys. Rev. A 1050-2947 10.1103/PhysRevA.70.051201 70, 051201 (2004).
27. T. Kunert and R. Schmidt, Eur. Phys. J. D 1434-6060 10.1140/epjd/e2003- 00086-8 25, 15 (2003).
28. A. N. Markevitch, D. A. Romanov, S. M. Smith, H. B. Schlegel, M. Y. Ivanov, and R. J. Levis, Phys. Rev. A 1050-2947 10.1103/PhysRevA.69.013401 69, 013401 (2004).
29. R. Trebino, K. W. DeLong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krumbügel, B. A. Richman, and D. J. Kane, Rev. Sci. Instrum. 0034-6748 10.1063/1.1148286 68, 3277 (1997).
30. M. Chergui, Low Temp. Phys. 26, 632 (2000).
31. G. P. Zhang and T. F. George, Phys. Rev. Lett. 0031-9007 10.1103/PhysRevLett.93.147401 93, 147401 (2004).
32. A. Reinköster, S. Korica, G. Prümper, J. Viefhaus, K. Godehusen, O. Schwarzkopf, M. Mast, and U. Becker, J. Phys. B 0953-4075 10.1088/0953-4075/37/10/010 37, 2135 (2004).
33. P. N. Juranic, D. Lukic, K. Barger, and R. Wehlitz, Phys. Rev. A 73, 042701 (2006).
34. S. Matt, D. Muigg, A. Ding, C. Lifshitz, P. Scheier, and T. D. Märk, J. Phys. Chem. 0022-3654 10.1021/jp960025d 100, 8692 (1996).
35. C. Lifshitz, Int. J. Mass Spectrom. 198, 1 (2000). 1387-3806
36. I. V. Hertel and C. P. Schulz, Atome, Moleküle und Optische Physik (Springer, Berlin, Heidelberg, 2008), Vol. 1.
37. We estimate the resonant dynamic Stark effect, equivalent to the Autler-Townes or Rabi splitting (see, e.g., Ref.) as e0 rab E0 with the transition dipole moment e0 rab from the measured oscillator strength f=0.015 for "feature a" of Ref. at 3.05 eV and the electric field strength E0 / (V/m) =2745 I0 / (W/ cm2) at our present intensities I0 =3.4× 1013 W/ cm2 to be ≃100 meV -which is larger than most of the vibrational level splittings in C60.
38. Assuming that the total energy of the system is-after a few picoseconds-statistically distributed over the vibrational degrees of freedom, the kinetic shift energy is required to allow for channeling the necessary dissociation energy with sufficient probability into the coordinates involved in the bond breaking.
39. Note that for higher charge states an even faster relaxation would be expected. These ions, however, cannot be detected here due to the relatively weak probe pulse.