Abstract
Controlling attosecond electron wave packets and soft X-ray pulses represents a formidable challenge of general implication to many areas of science1,2,3,4. A strong laser field interacting with atoms or molecules drives ultrafast intra-atomic/molecular electron wave packets on a subfemtosecond timescale, resulting in the emission of attosecond bursts of extreme-ultraviolet light5,6. Controlling the intra-atomic/molecular electron dynamics enables steering of the attosecond emission7,8. Here, we carry out a coherent control in linear molecules, where the interaction of the laser-driven electron wave packet with the core leads to quantum interferences9,10,11,12. We demonstrate that these interferences can be finely controlled by turning the molecular axis relative to the laser polarization, that is, changing the electron recollision angle. The wave-packet coulombic distortion modifies the spectral phase jump measured in the extreme-ultraviolet emission. Our attosecond control of the interference results in attosecond pulse shaping, useful for future applications in ultrafast coherent control of atomic and molecular processes.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 12 print issues and online access
$259.00 per year
only $21.58 per issue
Buy this article
- Purchase on SpringerLink
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Drescher, M. et al. Time-resolved atomic inner-shell spectroscopy. Nature 419, 803–807 (2002).
Remetter, T. et al. Attosecond electron wave packet interferometry. Nature Phys. 2, 323–326 (2006).
Baker, S. et al. Probing proton dynamics in molecules on an attosecond time scale. Science 312, 424–427 (2006).
Cavallieri, A. et al. Attosecond spectroscopy in condensed matter. Nature 449, 1029–1032 (2007).
Paul, P. M. et al. Observation of a train of attosecond pulses from high harmonic generation. Science 292, 1689–1692 (2001).
Hentschel, M. et al. Attosecond metrology. Nature 414, 509–513 (2001).
Sola, I. et al. Controlling attosecond electron dynamics by phase-stabilized polarization gating. Nature Phys. 2, 319–322 (2006).
Pfeifer, T. et al. Single attosecond pulse generation in the multicycle-driver regime by adding a weak second-harmonic field. Opt. Lett. 31, 975–977 (2005).
Lein, M., Velotta, R., Marangos, J. P. & Knight, P. L. Role of the intramolecular phase in high-harmonic generation. Phys. Rev. Lett. 88, 183903 (2002).
Lagmago Kamta, G. & Bandrauk, A. D. Three-dimensional time-profile analysis of high-order harmonic generation in molecules: Nuclear interferences in H2+. Phys. Rev. A 71, 053407 (2005).
Kanai, T., Minemoto, S. & Sakai, H. Quantum interference during high-order harmonic generation from aligned molecules. Nature 435, 470–474 (2005).
Vozzi, C. et al. Controlling two-center interference in molecular high harmonic generation. Phys. Rev. Lett. 95, 153902 (2005).
McPherson, A. et al. Studies of multiphoton production of vacuum-ultraviolet radiation in the rare gases. J. Opt. Soc. Am. B 4, 595–601 (1987).
Ferray, M. et al. Multiple-harmonic conversion of 1064 nm radiation in rare gases. J. Phys. B 21, L31–L35 (1988).
Corkum, P. B. Plasma perspective on strong field multiphoton ionization. Phys. Rev. Lett. 71, 1994–1997 (1993).
Schafer, K. J., Yang, B., DiMauro, L. F. & Kulander, K. C. Above threshold ionization beyond the high harmonic cutoff. Phys. Rev. Lett. 70, 1599–1602 (1993).
Mairesse, Y. et al. Attosecond synchronization of high-harmonic soft X-rays. Science 302, 1540–1543 (2003).
Lein, M., Hay, N., Velotta, R., Marangos, J. P. & Knight, P. L. Interference effects in high-order harmonic generation with molecules. Phys. Rev. A 66, 023805 (2002).
Ciappina, M. F., Chirila, C. C. & Lein, M. Influence of Coulomb continuum wave functions in the description of high-order harmonic generation with H2+. Phys. Rev. A 75, 043405 (2007).
Le, A.-T., Tong, X.-M. & Lin, C. D. Evidence of two-center interference in high-order harmonic generation from CO2 . Phys. Rev. A 73, 041402 (2006).
Itatani, J. et al. Tomographic imaging of molecular orbitals. Nature 432, 867–871 (2004).
Rosca-Pruna, F. & Vrakking, M. Experimental observation of revival structures in picosecond laser-induced alignment of I2 . Phys. Rev. Lett. 87, 153902 (2001).
Wabnitz, H. et al. Generation of attosecond pulses in molecular nitrogen. Eur. Phys. J. D 40, 305–311 (2006).
Levesque, J., Zeidler, D., Marangos, J. P., Corkum, P. B. & Villeneuve, D. M. High harmonic generation and the role of atomic orbital wave functions. Phys. Rev. Lett. 98, 183903 (2007).
Dudovich, N., Oron, D. & Silberberg, Y. Coherent transient enhancement of optically induced resonant transitions. Phys. Rev. Lett. 88, 123004 (2002).
Smirnova, O., Mouritzen, A. S., Patchkovskii, S. & Ivanov, M. Yu. Coulomb–laser coupling in laser-assisted photoionization and molecular tomography. J. Phys. B 40, F197–F206 (2007).
Xie, X. et al. Subcycle dynamics in the laser ionization of molecules. Phys. Rev. A 76, 023426 (2007).
Patchkovskii, S., Zhao, Z., Brabec, T. & Villeneuve, D. M. High harmonic generation and molecular orbital tomography in multielectron systems: Beyond the single active electron approximation. Phys. Rev. Lett. 97, 123003 (2006).
Zhao, Z., Yuan, J. & Brabec, T. Multielectron signatures in the polarization of high-order harmonic radiation. Phys. Rev. A 76, 031404 (2007).
Acknowledgements
We acknowledge financial support from the EU-FP6 XTRA (MRTN-CT-2003-505138) and LASERLAB (RII3-CT-2003-506350) programmes, the ANR Attoscience and the Engineering and Physical Sciences Research Council (UK) (GR/S22424/01).
Author information
Authors and Affiliations
Contributions
P.S. with B.C., H.M. and P.M. planned the project. W.B., H.M., P.B., P.M., B.C. and P.S. designed and installed the experiment. W.B. and S.H., with assistance from H.M., P.B., G.W., M.S., L.J.F., P.M. and P.S. carried out the measurements. W.B., S.H., H.M. and P.S. analysed the data. R.T., J.C. and A.M. carried out the dipole simulations. All authors discussed the results and contributed to the final manuscript. W.B. and S.H. contributed equally to this work.
Corresponding author
Rights and permissions
About this article
Cite this article
Boutu, W., Haessler, S., Merdji, H. et al. Coherent control of attosecond emission from aligned molecules. Nature Phys 4, 545–549 (2008). https://doi.org/10.1038/nphys964
Received:
Accepted:
Published:
Issue date:
DOI: https://doi.org/10.1038/nphys964
This article is cited by
-
Coulomb and Quantum Interference Effects in the Spectra of High-Order Harmonics Generated by Aligned Molecules
Radiophysics and Quantum Electronics (2023)
-
Vectorized optoelectronic control and metrology in a semiconductor
Nature Photonics (2020)
-
Spatial molecular interferometry via multidimensional high-harmonic spectroscopy
Nature Photonics (2020)
-
Attosecond imaging of molecules using high harmonic spectroscopy
Nature Reviews Physics (2019)
-
Laser-induced blurring of molecular structure information in high harmonic spectroscopy
Scientific Reports (2017)
