Abstract
Manipulation of the molecular-axis distribution is an important ingredient in experiments aimed at understanding and controlling molecular processes1,2,3,4,5,6. Samples of aligned or oriented molecules can be obtained following the interaction with an intense laser field7,8,9, enabling experiments in the molecular rather than the laboratory frame10,11,12. However, the degree of impulsive molecular orientation and alignment that can be achieved using a single laser field is limited13 and crucially depends on the initial states, which are thermally populated. Here we report the successful demonstration of a new technique for laser-field-free orientation and alignment of molecules that combines an electrostatic field, non-resonant femtosecond laser excitation14 and the preparation of state-selected molecules using a hexapole2. As a unique quantum-mechanical wavepacket is formed, a large degree of orientation and alignment is observed both during and after the femtosecond laser pulse, which is even further increased (to 〈cosθ〉=−0.74 and 〈cos2θ〉=0.82, respectively) by tailoring the shape of the femtosecond laser pulse. This work should enable new applications such as the study of reaction dynamics or collision experiments in the molecular frame, and orbital tomography11 of heteronuclear molecules.
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Change history
25 March 2009
NOTE: In the version of this Letter originally published online, the author list of ref. 29 was incorrect. It has now been corrected in all versions of this Letter.
References
Kuipers, E. W., Tenner, M. G., Kleyn, A. W. & Stolte, S. Observation of steric effects in gas–surface scattering. Nature 334, 420–422 (1988).
Parker, D. H. & Bernstein, R. B. Oriented molecule beams via the electrostatic hexapole: Preparation, characterization, and reactive scattering. Ann. Rev. Phys. Chem. 40, 561–595 (1989).
Rischel, C. et al. Femtosecond time-resolved X-ray diffraction from laser-heated organic films. Nature 390, 490–492 (1997).
Rakitzis, T. P., Van den Brom, A. J. & Janssen, M. H. M. Directional dynamics in the photodissociation of oriented molecules. Science 303, 1852–1854 (2004).
Brooks, P. R. Reactions of oriented molecules. Science 193, 11–16 (1976).
Loesch, H. J. & Remscheid, A. Brute force in molecular reaction dynamics: A novel technique for measuring steric effects. J. Chem. Phys. 93, 4779–4790 (1990).
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).
Stapelfeldt, H. & Seideman, T. Colloquium: Aligning molecules with strong laser pulses. Rev. Mod. Phys. 75, 543–557 (2003).
Goban, A., Minemoto, S. & Sakai, H. Laser field-free molecular orientation. Phys. Rev. Lett. 101, 013001 (2008).
Litvinyuk, I. V. et al. Alignment-dependent strong field ionization of molecules. Phys. Rev. Lett. 90, 233003 (2003).
Itatani, J. et al. Tomographic imaging of molecular orbitals. Nature 432, 867–871 (2004).
Kanai, T., Minemoto, S. & Sakai, H. Quantum interference during high-order harmonic generation from aligned molecules. Nature 435, 470–474 (2005).
Leibscher, M., Averbukh, I. Sh. & Rabitz, H. Molecular alignment by trains of short laser pulses. Phys. Rev. Lett. 90, 213001 (2003).
Cai, L., Marango, J. & Friedrich, B. Time-dependent alignment and orientation of molecules in combined electrostatic and pulsed nonresonant laser fields. Phys. Rev. Lett. 86, 775–778 (2001).
Zare, R. N. Laser control of chemical reactions. Science 279, 1875–1879 (1998).
Judson, R. S. & Rabitz, H. Teaching lasers to control molecules. Phys. Rev. Lett. 68, 1500–1503 (1992).
Assion, et al. Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses. Science 282, 919–922 (1998).
Sakai, H. et al. Controlling the alignment of neutral molecules by a strong laser field. J. Chem. Phys. 110, 10235–10238 (1999).
Bisgaard, C. Z., Poulsen, M. D., Peronne, E., Viftrup, S. S. & Stapelfeldt, H. Observation of enhanced field-free molecular alignment by two laser pulses. Phys. Rev. Lett. 92, 173004 (2004).
Rouzée, A., Hertz, E., Lavorel, B. & Faucher, O. Towards the adaptive optimization of field-free molecular alignment. J. Phys. B 41, 074002 (2008).
Suzuki, T., Sugawara, Y., Minemoto, S. & Sakai, H. Optimal control of nonadiabatic alignment of rotationally cold N2 molecules with the feedback of degree of alignment. Phys. Rev. Lett. 100, 033603 (2008).
Neutze, R., Wouts, R., Van der Spoel, D., Weckert, E. & Hajdu, J. Potential for biomolecular imaging with femtosecond X-ray pulses. Nature 406, 752–757 (2000).
Chapman, H. N. et al. Femtosecond diffractive imaging with a soft-X-ray free-electron laser. Nature Phys. 2, 839–843 (2006).
Vrakking, M. J. J. & Stolte, S. Coherent control of molecular orientation. Chem. Phys. Lett. 271, 209–215 (1997).
Machholm, M. & Henriksen, N. E. Field-free orientation of molecules. Phys. Rev. Lett. 87, 193001 (2001).
Friedrich, B. & Herschbach, D. Enhanced orientation of polar molecules by combined electrostatic and nonresonant induced dipole forces. J. Chem. Phys. 111, 6157–6160 (1999).
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).
Baumfalk, R., Nahler, N. H. & Buck, U. Photodissociation of oriented HXeI molecules in the gas phase. J. Chem. Phys. 114, 4755–4758 (2001).
Holmegaard, L. et al. Laser-induced alignment and orientation of quantum-state-selected large molecules. Phys. Rev. Lett. 102, 023001 (2009).
Gijsbertsen, et al. Direct determination of the sign of the NO dipole moment. Phys. Rev. Lett. 99, 213003 (2007).
Meijer, A. S. et al. Controlling rotational state distributions using two-pulse stimulated Raman excitation. Phys. Rev. A 76, 023411 (2007).
Acknowledgements
We acknowledge P. Johnsson for discussions and technical assistance provided during this project. This work is part of the research program of the ‘Stichting voor Fundamenteel Onderzoek der Materie (FOM)’, which is financially supported by the ‘Nederlandse organisatie voor Wetenschappelijk Onderzoek (NWO)’. Financial support by the Marie Curie Research Training Networks ‘XTRA’ is gratefully acknowledged.
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Ghafur, O., Rouzée, A., Gijsbertsen, A. et al. Impulsive orientation and alignment of quantum-state-selected NO molecules. Nature Phys 5, 289–293 (2009). https://doi.org/10.1038/nphys1225
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DOI: https://doi.org/10.1038/nphys1225
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