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Making Optical Waves, Tracing Electrons in Real-Time: the Onset of the Attosecond Realm (Invited Review)

By Eleftherios Goulielmakis and Ferenc Krausz
Progress In Electromagnetics Research, Vol. 147, 127-140, 2014


Tracing the dynamics of electrons inside atoms molecules or solids as they occur in real time resides at the forefront of modern science and technology. Advances in attosecond physics over the last decade and beyond are now enabling this essential experimental capability. Here we discuss some of the key developments in light sciences that made possible attosecond metrology and control of electronic processes inside matter on native time scales. These developments hold the promise for new, fundamental insights into the innerworkings of the microcosm as well as the identification of innovative routes for light-based electronic and photonic devices operating at PHz rates.


Eleftherios Goulielmakis and Ferenc Krausz, "Making Optical Waves, Tracing Electrons in Real-Time: the Onset of the Attosecond Realm (Invited Review)," Progress In Electromagnetics Research, Vol. 147, 127-140, 2014.


    1. Maiman, T. H., "Stimulated optical radiation in ruby," Nature, Vol. 187, No. 4736, 493-494, 1960.

    2. Hansch, T. W., "Passion for precision," Chem. Phys. Chem., Vol. 7, No. 6, 1170-1187, 2006.

    3. Koningsberger, D. C. and R. Prins, "X-ray absorption: Principles, applications, techniques of EXAFS, SEXAFS, and XANES," Chemical Analysis, Wiley, New York, 1988.

    4. Hassan, M. T., A. Wirth, I. Grguras, A. Moulet, T. T. Luu, J. Gagnon, V. Pervak, and E. Goulielmakis, "Attosecond photonics: Synthesis and control of light transients," Review of Scienti¯c Instruments, Vol. 83, No. 11, 111301, 2012.

    5. Zewail, A. H., "Femtochemistry: Atomic-scale dynamics of the chemical bond using ultrafast lasers (nobel lecture) copyright((c)) the nobel foundation 2000. We thank the Nobel Foundation, Stockholm, for permission to print this lecture," Angew. Chem. Int. Ed. Engl., Vol. 39, No. 15, 2586-2631, 2000.

    6. Weiner, A. M., "Femtosecond pulse shaping using spatial light modulators," Review of Scientific Instruments, Vol. 71, No. 5, 1929-1960, 2000.

    7. Assion, A., T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, "Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses," Science, Vol. 282, No. 5390, 919, 1998.

    8. Remacle, F., M. Nest, and R. D. Levine, "Laser steered ultrafast quantum dynamics of electrons in LiH," Physical Review Letters, Vol. 99, 183902, 2007.

    9. Muskatel, B. H., F. Remacle, and R. D. Levine, "Ultrafast predissociation mechanism of the (1)pi(u) states of n-14(2) and its isotopomers upon attosecond excitation from the ground state," Journal of Physical Chemistry A, Vol. 116, No. 46, 11311-11318, 2012.

    10. Remacle, F. and R. D. Levine, "An electronic time scale in chemistry," Proceedings of the National Academy of Sciences of the United States of America, Vol. 103, No. 18, 6793-6798, 2006.

    11. Mignolet, B., A. Gijsbertsen, M. J. J. Vrakking, R. D. Levine, and F. Remacle, "Stereocontrol of attosecond time-scale electron dynamics in ABCU using ultrafast laser pulses: A computational study," Physical Chemistry Chemical Physics, Vol. 13, No. 18, 8331-8344, 2011.

    12. Mignolet, B., R. D. Levine, and F. Remacle, "Electronic dynamics by ultrafast pump photoelectron detachment probed by ionization: A dynamical simulation of negative-neutral-positive in LiH-," J. Phys. Chem. A, Vol. 118, No. 33, 6721-6729, 2014.

    13. Corkum, P. B. and F. Krausz, "Attosecond science," Nature Physics, Vol. 3, No. 6, 381, 2007.

    14. Udem, T., R. Holzwarth, and T. W. Hansch, "Optical frequency metrology," Nature, Vol. 416, No. 6877, 233-237, 2002.

    15. Keldysh, L. V., "Ionization in ¯eld of a strong electromagnetic wave," Soviet Physics JETP-USSR, Vol. 20, No. 5, 1307, 1965.

    16. Macklin, J. J., J. D. Kmetec, and C. L. Gordon, "High-order harmonic-generation using intense femtosecond pulses," Physical Review Letters, Vol. 70, No. 6, 766-769, 1993.

    17. Lhuillier, A. and P. Balcou, "High-order garmonic-generation in rare-gases with a 1-ps 1053-nm laser," Physical Review Letters, Vol. 70, No. 6, 774-777, 1993.

    18. Petite, G., P. Agostini, and H. G. Muller, "Intensity dependence of non-perturbative above-threshold ionization spectra --- Experimental-study," Journal of Physics B --- Atomic Molecular and Optical Physics, Vol. 21, No. 24, 4097-4105, 1988.

    19. Fabre, F., G. Petite, P. Agostini, and M. Clement, "Multiphoton above-threshold ionization of Xenon at 0.53 and 1.06 μm," Journal of Physics B --- Atomic Molecular and Optical Physics, Vol. 15, No. 9, 1353-1369, 1982.

    20. Baltuska, A., T. Udem, M. Uiberacker, M. Hentschel, E. Goulielmakis, C. Gohle, R. Holzwarth, V. S. Yakovlev, A. Scrinzi, T. W. Hansch, and F. Krausz, "Attosecond control of electronic processes by intense light fields," Nature, Vol. 421, No. 6928, 611-615, 2003.

    21. Paul, P. M., E. S. Toma, P. Breger, G. Mullot, F. Auge, P. Balcou, H. G. Muller, and P. Agostini, "Observation of a train of attosecond pulses from high harmonic generation," Science, Vol. 292, No. 5522, 1689-1692, 2001.

    22. Mairesse, Y., A. de Bohan, L. J. Frasinski, H. Merdji, L. C. Dinu, P. Monchicourt, P. Breger, M. Kovacev, R. Taieb, B. Carre, H. G. Muller, P. Agostini, and P. Salieres, "Attosecond synchronization of high-harmonic soft X-rays," Science, Vol. 302, No. 5650, 1540-1543, 2003.

    23. Drescher, M., M. Hentschel, R. Kienberger, G. Tempea, C. Spielmann, G. A. Reider, P. B. Corkum, and F. Krausz, "X-ray pulses approaching the attosecond frontier," Science, Vol. 291, No. 5510, 1923-1927, 2001.

    24. Hentschel, M., R. Kienberger, C. Spielmann, G. A. Reider, N. Milosevic, T. Brabec, P. Corkum, U. Heinzmann, M. Drescher, and F. Krausz, "Attosecond metrology," Nature, Vol. 414, No. 6863, 509-513, 2001.

    25. Gaarde, M. B., M. Murakami, and R. Kienberge, "Spatial separation of large dynamical blueshift and harmonic generation," Physical Review A, Vol. 74, 053401, 2006.

    26. Drescher, M., M. Hentschel, R. Kienberger, M. Uiberacker, V. Yakovlev, A. Scrinzi, T. Westerwalbesloh, U. Kleineberg, U. Heinzmann, and F. Krausz, "Time-resolved atomic inner-shell spectroscopy," Nature, Vol. 419, No. 6909, 803-807, 2002, 607BD Times Cited: 768 Cited References Count: 23.

    27. Brabec, T. and F. Krausz, "Intense few-cycle laser fields: Frontiers of nonlinear optics," Reviews of Modern Physics, Vol. 72, No. 2, 545-591, 2000.

    28. Corkum, P. B., "Plasma perspective on strong-field multiphoton ionization," Physical Review Letters, Vol. 71, No. 13, 1994-1997, 1993.

    29. Paulus, G. G., F. Lindner, H. Walther, A. Baltuska, E. Goulielmakis, M. Lezius, and F. Krausz, "Measurement of the phase of few-cycle laser pulses," Physical Review Letters, Vol. 91, 253004, 2003.

    30. Lindner, F., M. G. Schatzel, H. Walther, A. Baltuska, E. Goulielmakis, F. Krausz, D. B. Milosevic, D. Bauer, W. Becker, G. G. Paulus, and H. Walther, "Attosecond double-slit experiment," Physical Review Letters, Vol. 95, 040401, 2005.

    31. Liu, X., H. Rottke, E. Eremina, W. Sandner, E. Goulielmakis, K. O. Keee, M. Lezius, F. Krausz, F. Lindner, M. G. Schatzel, G. G. Paulus, and H. Walther, "Nonsequential double ionization at the single-optical-cycle limit," Physical Review Letters, Vol. 93, 263001, Dec. 2004.

    32. Kling, M. F., C. Siedschlag, A. J. Verhoef, J. I. Khan, M. Schultze, T. Uphues, Y. Ni, M. Uiberacker, M. Drescher, F. Krausz, and M. J. J. Vrakking, "Control of electron localization in molecular dissociation," Science, Vol. 312, No. 5771, 246-248, 2006.

    33. Alnaser, A. S., M. Kubel, R. Siemering, B. Bergues, N. G. Kling, K. J. Betsch, Y. Deng, J. Schmidt, Z. A. Alahmed, A. M. Azzeer, J. Ullrich, I. Ben-Itzhak, R. Moshammer, U. Kleineberg, F. Krausz, R. de Vivie-Riedle, and M. F. Kling, "Subfemtosecond steering of hydrocarbon deprotonation through superposition of vibrational modes," Nat. Commun., Vol. 5, 2014.

    34. Znakovskaya, I., P. von den Ho, G. Marcus, S. Zherebtsov, B. Bergues, X. Gu, Y. Deng, M. J. J. Vrakking, R. Kienberger, F. Krausz, R. de Vivie-Riedle, and M. F. Kling, "Subcycle controlled charge-directed reactivity with few-cycle midinfrared pulses," Physical Review Letters, Vol. 108, 063002, 2012.

    35. Borot, A., A. Malvache, X. W. Chen, A. Jullien, J. P. Geindre, P. Audebert, G. Mourou, F. Quere, and R. Lopez-Martens, "Attosecond control of collective electron motion in plasmas," Nature Physics, Vol. 8, No. 5, 416-421, 2012.

    36. Kruger, M., M. Schenk, and P. Hommelho, "Attosecond control of electrons emitted from a nanoscale metal tip," Nature, Vol. 475, 78-81, Jul. 2011.

    37. Sekikawa, T., A. Kosuge, T. Kanai, and S.Watanabe, "Nonlinear optics in the extreme ultraviolet," Nature, Vol. 432, No. 7017, 605-608, 2004.

    38. Tzallas, P., D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, "Direct observation of attosecond light bunching," Nature, Vol. 426, No. 6964, 267-271, 2003.

    39. Goulielmakis, E., M. Uiberacker, R. Kienberger, A. Baltuska, V. Yakovlev, A. Scrinzi, T. Westerwalbesloh, U. Kleineberg, U. Heinzmann, M. Drescher, and F. Krausz, "Direct measurement of light waves," Science, Vol. 305, No. 5688, 1267, 2004.

    40. Kienberger, R., E. Goulielmakis, M. Uiberacker, A. Baltuska, V. Yakovlev, F. Bammer, A. Scrinzi, T. Westerwalbesloh, U. Kleineberg, U. Heinzmann, M. Drescher, and F. Krausz, "Atomic transient recorder," Nature, Vol. 427, No. 6977, 817-821, 2004.

    41. Sansone, G., E. Benedetti, F. Calegari, C. Vozzi, L. Avaldi, R. Flammini, L. Poletto, P. Villoresi, C. Altucci, R. Velotta, S. Stagira, S. De Silvestri, and M. Nisoli, "Isolated single-cycle attosecond pulses," Science, Vol. 314, No. 5798, 443-446, 2006.

    42. Goulielmakis, E., M. Schultze, M. Hofstetter, V. S. Yakovlev, J. Gagnon, M. Uiberacker, A. L. Aquila, E. M. Gullikson, D. T. Attwood, R. Kienberger, F. Krausz, and U. Kleineberg, "Single-cycle nonlinear optics," Science, Vol. 320, No. 5883, 1614-1617, 2008.

    43. Yakovlev, V. S., J. Gagnon, N. Karpowicz, and F. Krausz, "Attosecond streaking enables the measurement of quantum phase," Physical Review Letters, Vol. 105, 073001, 2010.

    44. Itatani, J., F. Quere, G. L. Yudin, M. Y. Ivanov, F. Krausz, and P. B. Corkum, "Attosecond streak camera," Physical Review Letters, Vol. 88, 173903, 2002.

    45. Schultze, M., M. Fie¼, N. Karpowicz, J. Gagnon, M. Korbman, M. Hofstetter, S. Neppl, A. L. Cavalieri, Y. Komninos, T. Mercouris, C. A. Nicolaides, R. Pazourek, S. Nagele, J. Feist, J. Burgdorfer, A. M. Azzeer, R. Ernstorfer, R. Kienberger, U. Kleineberg, E. Goulielmakis, F. Krausz, and V. S. Yakovlev, "Delay in photoemission," Science, Vol. 328, No. 5986, 1658-1662, 2010.

    46. Cavalieri, A. L., N. Muller, T. Uphues, V. S. Yakovlev, A. Baltuska, B. Horvath, B. Schmidt, L. Blumel, R. Holzwarth, S. Hendel, M. Drescher, U. Kleineberg, P. M. Echenique, R. Kienberger, F. Krausz, and U. Heinzmann, "Attosecond spectroscopy in condensed matter," Nature, Vol. 449, No. 7165, 1029-1032, 2007.

    47. Goulielmakis, E., V. S. Yakovlev, A. L. Cavalieri, M. Uiberacker, V. Pervak, A. Apolonski, R. Kienberger, U. Kleineberg, and F. Krausz, "Attosecond control and measurement: Lightwave electronics," Science, Vol. 317, No. 5839, 769-775, 2007.

    48. Chan, H.-S., Z.-M. Hsieh, W.-H. Liang, A. H. Kung, C.-K. Lee, C.-J. Lai, R.-P. Pan, and L.-H. Peng, "Synthesis and measurement of ultrafast waveforms from ¯ve discrete optical harmonics," Science, Vol. 331, No. 6021, 1165-1168, 2011.

    49. Sokolov, A. V., D. D. Yavuz, and S. E. Harris, "Subfemtosecond pulse generation by rotational molecular modulation," Optics Letters, Vol. 24, No. 8, 557-559, 1999.

    50. Nisoli, M., S. DeSilvestri, and O. Svelto, "Generation of high energy 10 fs pulses by a new pulse compression technique," Applied Physics Letters, Vol. 68, No. 20, 2793-2795, 1996.

    51. Nisoli, M., S. Stagira, S. De Silvestri, O. Svelto, S. Sartania, Z. Cheng, M. Lenzner, C. Spielmann, and F. Krausz, "A novel-high energy pulse compression system: Generation of multigigawatt sub-5-fs pulses," Applied Physics B, Vol. 65, No. 2, 189-196, 1997.

    52. Nisoli, M., S. DeSilvestri, O. Svelto, R. Szipocs, K. Ferencz, C. Spielmann, S. Sartania, and F. Krausz, "Compression of high-energy laser pulses below 5 fs," Optics Letters, Vol. 22, No. 8, 522-524, 1997.

    53. Reiter, F., U. Graf, E. E. Serebryannikov, W. Schweinberger, M. Fiess, M. Schultze, A. M. Azzeer, R. Kienberger, F. Krausz, A. M. Zheltikov, and E. Goulielmakis, "Route to attosecond nonlinear spectroscopy," Physical Review Letters, Vol. 105, 243902, 2010.

    54. Wirth, A., M. T. Hassan, I. Grgura·s, J. Gagnon, A. Moulet, T. T. Luu, S. Pabst, R. Santra, Z. A. Alahmed, A. M. Azzeer, V. S. Yakovlev, V. Pervak, F. Krausz, and E. Goulielmakis, "Synthesized light transients," Science, Vol. 334, No. 6053, 195, 2011.

    55. Szipocs, R., C. Spielmann, F. Krausz, and K. Ferencz, "Chirped multilayer coatings for broadband dispersion control in femtosecond lasers," Optics Letters, Vol. 19, No. 3, 201-203, Feb. 1994.

    56. Pervak, V., A. V. Tikhonravov, M. K. Trubetskov, S. Naumov, F. Krausz, and A. Apolonski, "1.5-octave chirped mirror for pulse compression down to sub-3 fs," Applied Physics B --- Lasers and Optics, Vol. 87, No. 1, 5-12, 2007.

    57. Iaconis, C. and I. A. Walmsley, "Spectral phase interferometry for direct electric-field reconstruction of ultrashort optical pulses," Optics Letters, Vol. 23, No. 10, 792-794, 1998.

    58. Trebino, R., Frequency-resolved Optical Gating: The Measurement of Ultrashort Laser Pulses, Springer, 2002.

    59. Goulielmakis, E., Z. H. Loh, A. Wirth, R. Santra, N. Rohringer, V. S. Yakovlev, S. Zherebtsov, T. Pfeifer, A. M. Azzeer, M. F. Kling, S. R. Leone, and F. Krausz, "Real-time observation of valence electron motion," Nature, Vol. 466, No. 7307, 739-743, 2010.

    60. Wirth, A., R. Santra, and E. Goulielmakis, "Real time tracing of valence-shell electronic coherences with attosecond transient absorption spectroscopy," Chemical Physics, Vol. 414, 149-159, 2013.

    61. Barnes, W. L., A. Dereux, and T. W. Ebbesen, "Surface plasmon subwavelength optics," Nature, Vol. 424, No. 6950, 824-830, 2003.