Abstract
High-order harmonic generation (HHG) from atoms and molecules offers potential application as a coherent ultrashort radiation source in the extreme ultraviolet and soft X-ray regions1,2,3. In the three-step model4,5,6 of HHG, an electron tunnels out from the atom and may recombine with the parent ion (emitting a high-energy photon) after undergoing laser-driven motion in the continuum. Aligned molecules7,8,9,10,11 can be used to study quantum phenomena in HHG associated with molecular symmetries; in particular, simultaneous observations of both ion yields and harmonic signals under the same conditions serve to disentangle the contributions from the ionization and recombination processes. Here we report evidence for quantum interference of electron de Broglie waves12,13,14 in the recombination process of HHG from aligned CO2 molecules. The interference takes place within a single molecule and within one optical cycle. Characteristic modulation patterns of the harmonic signals measured as a function of the pump–probe delay are explained with simple formulae determined by the valence orbital of the molecules. We propose that simultaneous observations of both ion yields and harmonic signals can serve as a new route to probe the instantaneous structure of molecular systems.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 51 print issues and online access
$199.00 per year
only $3.90 per issue
Buy this article
- Purchase on Springer Link
- 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
Hentschel, M. et al. Attosecond metrology. Nature 414, 509–513 (2001)
Drescher, M. et al. Time-resolved atomic inner-shell spectroscopy. Nature 419, 803–807 (2002)
Chang, Z., Rundquist, A., Wang, H., Murnane, M. M. & Kapteyn, H. C. Generation of coherent soft X rays at 2.7 nm using high harmonics. Phys. Rev. Lett. 79, 2967–2970 (1997)
Corkum, P. B. Plasma perspective on strong field multiphoton ionization. Phys. Rev. Lett. 71, 1994–1997 (1993)
Krause, J. L., Schafer, K. J. & Kulander, K. C. High-order harmonic generation from atoms and ions in the high intensity regime. Phys. Rev. Lett. 68, 3535–3538 (1992)
Lewenstein, M. et al. Theory of high-harmonic generation by low-frequency laser fields. Phys. Rev. A 49, 2117–2132 (1994)
Rosca-Pruna, F. & Vrakking, M. J. J. Experimental observation of revival structures in picosecond laser-induced alignment of I2 . Phys. Rev. Lett. 87, 153902 (2001)
Litvinyuk, I. V. et al. Alignment-dependent strong field ionization of molecules. Phys. Rev. Lett. 90, 233003 (2003)
Sakai, H. et al. Controlling the alignment of neutral molecules by a strong laser field. J. Chem. Phys. 110, 10235–10238 (1999)
Velotta, R., Hay, H., Mason, M. B., Castillejo, M. & Marangos, J. P. High-order harmonic generation in aligned molecules. Phys. Rev. Lett. 87, 183901 (2001)
Sakai, H., Minemoto, S., Nanjo, H., Tanji, H. & Suzuki, T. Controlling the orientation of polar molecules with combined electrostatic and pulsed, nonresonant laser fields. Phys. Rev. Lett. 90, 083001 (2003)
Lein, M., Hay, N., Velotta, R., Marangos, J. P. & Knight, P. L. Role of the intramolecular phase in high-harmonic generation. Phys. Rev. Lett. 88, 183903 (2002)
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)
Lein, M., Corso, P. P., Marangos, J. P. & Knight, P. L. Orientation dependence of high-order harmonic generation in molecules. Phys. Rev. A 67, 023819 (2003)
Sakai, H. et al. Nonsequential double ionization of D2 molecules with intense 20-fs pulses. Phys. Rev. A 67, 063404 (2003)
Lein, M., Marangos, J. P. & Knight, P. L. Electron diffraction in above-threshold ionization of molecules. Phys. Rev. A 66, 051404(R) (2002)
Sakai, H. & Miyazaki, K. High-order harmonic-generation in nitrogen molecules with subpicosecond visible dye-laser pulses. Appl. Phys. B 61, 493–498 (1995)
Liang, Y., Augst, S., Chin, S. L., Beaudoin, Y. & Chaker, M. High harmonic generation in atomic and diatomic molecular gases using intense picosecond laser pulses—a comparison. J. Phys. B 27, 5119–5130 (1994)
Lyngå, C., L'Huillier, A. & Wahlström, C.-G. High-order harmonic generation in molecular gases. J. Phys. B 29, 3293–3302 (1996)
Muth-Böhm, J., Becker, A. & Faisal, F. H. M. Suppressed molecular ionization for a class of diatomics in intense femtosecond laser fields. Phys. Rev. Lett. 85, 2280–2283 (2000)
Tong, X. M., Zhao, Z. X. & Lin, C. D. Theory of molecular tunneling ionization. Phys. Rev. A 66, 033402 (2002)
Itatani, J. et al. Tomographic imaging of molecular orbitals. Nature 432, 867–871 (2004)
Kaku, M., Masuda, K. & Miyazaki, K. Observation of revival structure in femtosecond-laser-induced alignment of N2 with high-order harmonic generation. Jpn. J. Appl. Phys. 43, L591–L593 (2004)
Dooley, P. W. et al. Direct imaging of rotational wave-packet dynamics of diatomic molecules. Phys. Rev. A 68, 023406 (2003)
de Nalda, R. et al. Role of orbital symmetry in high-order harmonic generation from aligned molecules. Phys. Rev. A 69, 031804(R) (2004)
Young, T. Experiments and calculations relative to physical optics. Phil. Trans. R. Soc. Lond. 94, 1–16 (1804)
Shan, B., Ghimire, S. & Chang, Z. Effect of orbital symmetry on high-order harmonic generation from molecules. Phys. Rev. A 69, 021404(R) (2004)
Sakai, H. & Miyazaki, K. Effect of multiphoton ionization on high-order harmonic generation and propagation in rare gases with subpicosecond laser pulses. Phys. Rev. A 50, 4204–4211 (1994)
Acknowledgements
This work was supported by Grants-in-Aid from the Japan Society for the Promotion of Science and from the Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Competing interests
Reprints and permissions information is available at npg.nature.com/reprintsandpermissions. The authors declare no competing financial interests.
Rights and permissions
About this article
Cite this article
Kanai, T., Minemoto, S. & Sakai, H. Quantum interference during high-order harmonic generation from aligned molecules. Nature 435, 470–474 (2005). https://doi.org/10.1038/nature03577
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1038/nature03577
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)
-
High-order harmonic generation from aligned HCN molecules under orthogonally and linearly polarized two-color laser fields
Journal of Molecular Modeling (2023)
-
All-optical control of pendular qubit states with nonresonant two-color laser pulses
Communications Physics (2022)
-
Field-free molecular orientation by delay- and polarization-optimized two fs pulses
Scientific Reports (2020)
-
The quantum-optical nature of high harmonic generation
Nature Communications (2020)
Comments
By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.