Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

A molecular conveyor belt by controlled delivery of single molecules into ultrashort laser pulses

Abstract

Trapping and laser cooling in atomic physics enables control of single particles and their dynamics at the quantum level in a background-free environment. Ultrashort intense laser pulses reveal the ultimate control of electromagnetic fields, enabling the imaging of matter, in principle down to a single molecule or virus resolved on atomic scales. However, current methods fall short in overlapping each target with a pulse of comparable size. We combine the two fields by demonstrating a deterministic molecular conveyor, formed of electric trapping potentials. We deliver individual diatomic ions at millikelvin temperatures and with submicrometre positioning into few-femtosecond ultraviolet laser pulses. We initiate and probe the molecule’s femtosecond dynamics and detect it and its response with 100% efficiency. This experiment might become key for investigations of individual molecules, such as structural determinations using few-femtosecond X-ray lasers. Our scheme may overlap each single molecule with a pulse, focused to (sub)micrometre size, providing the required number of photons at the repetition rate of the laser.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Schematic of the set-up combining the fields of single-particle preparation on the quantum level and single, ultrashort laser pulses.
Figure 2: Preparation of a single molecular ion as a cold, micropositioned target.
Figure 3: Schematic representation of our experiment on a deterministically positioned single molecule, based on the ab initio potential-energy curves of the electronic states involved.
Figure 4: Vibrational motion of molecules derived from the dissociation of single molecules as a function of pump–probe delay for 4 fs laser pulses.

Similar content being viewed by others

References

  1. Webster, G. & Hilgenfeld, R. Perspectives on single molecule diffraction using the X-ray free electron laser. Single Mol. 3, 63–68 (2002).

    Article  ADS  Google Scholar 

  2. Henderson, R. The potential and limitations of neutrons, electrons and X-rays for atomic resolution microscopy of unstained biological molecules. Q. Rev. Biophys. 28, 171–193 (1995).

    Article  Google Scholar 

  3. 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).

    Article  ADS  Google Scholar 

  4. Chapman, H. N. et al. Femtosecond time-delay X-ray holography. Nature 448, 676–679 (2007).

    Article  ADS  Google Scholar 

  5. Young, L. et al. Femtosecond electronic response of atoms to ultra-intense X-rays. Nature 466, 56–61 (2010).

    Article  ADS  Google Scholar 

  6. Seibert, M. M. et al. Single mimivirus particles intercepted and imaged with an X-ray laser. Nature 470, 78–81 (2011).

    Article  ADS  Google Scholar 

  7. Chapman, H. N. et al. Femtosecond X-ray protein nanocrystallography. Nature 470, 73–77 (2011).

    Article  ADS  Google Scholar 

  8. Yamashita, M. & Fenn, J. B. Negative ion production with the electrospray ion source. J. Phys. Chem. 88, 4671–4675 (1984).

    Article  Google Scholar 

  9. Marklund, E. G., Larsson, D. S. D., Spoel, D. v. d., Patriksson, A. & Caleman, C. Structural stability of electrosprayed proteins: temperature and hydration effects. Phys. Chem. Chem. Phys. 11, 8069–8078 (2009).

    Article  Google Scholar 

  10. Chou, C. W., Hume, D. B., Rosenband, T. & Wineland, D. J. Optical clocks and relativity. Science 329, 1630–1633 (2010).

    Article  ADS  Google Scholar 

  11. Home, J. P. et al. Complete methods set for scalable ion trap quantum information processing. Science 325, 1227–1230 (2009).

    Article  ADS  MathSciNet  Google Scholar 

  12. Barrett, M. D. et al. Deterministic quantum teleportation of atomic qubits. Nature 429, 737–739 (2004).

    Article  ADS  Google Scholar 

  13. Molhave, K. & Drewsen, M. Formation of translationally cold MgH+ and MgD+ molecules in an ion trap. Phys. Rev. A 62, 011401 (2000).

    Article  ADS  Google Scholar 

  14. Offenberg, D., Zhang, C. B., Wellers, C., Roth, B. & Schiller, S. Translational cooling and storage of protonated proteins in an ion trap at subkelvin temperatures. Phys. Rev. A 78, 061401 (2008).

    Article  ADS  Google Scholar 

  15. Birkl, G., Kassner, S. & Walther, H. Multiple-shell structures of laser-cooled Mg ions in a quadrupole storage ring. Nature 357, 310–313 (1992).

    Article  ADS  Google Scholar 

  16. Friedenauer, A. et al. High power all solid state laser system near 280 nm. Appl. Phys. B 84, 371–373 (2006).

    Article  ADS  Google Scholar 

  17. Schiller, S. & Lämmerzahl, C. Molecular dynamics simulation of sympathetic crystallization of molecular ions. Phys. Rev. A 68, 053406 (2003).

    Article  ADS  Google Scholar 

  18. Gerlich, D. & Borodi, G. Buffer gas cooling of polyatomic ions in RF multi-electrode traps. Faraday Discuss. 142, 57–72 (2009).

    Article  ADS  Google Scholar 

  19. Smith, I. W. M. Low Temperatures And Cold Molecules (Imperial College Press, 2008).

    Book  Google Scholar 

  20. Paul, W. Electromagnetic traps for charged and neutral particles. Rev. Mod. Phys. 62, 531–540 (1990).

    Article  ADS  Google Scholar 

  21. Kjægaard, N., Hornekær, L., Thommesen, A., Videsen, Z. & Drewsen, M. Isotope selective loading of an ion trap using resonance-enhanced two-photon ionization. Appl. Phys. B 71, 207–210 (2000).

    Article  ADS  Google Scholar 

  22. Graf, U. et al. Intense few-cycle light pulses in the deep ultraviolet. Opt. Express 16, 18956–18963 (2008).

    Article  ADS  Google Scholar 

  23. Jørgensen, S., Drewsen, M. & Kosloff, R. Intensity and wavelength control of a single molecule reaction: Simulation of photodissociation of cold-trapped MgH+. J. Chem. Phys. 123, 094302 (2005).

    Article  ADS  Google Scholar 

  24. Brinks, D. e. a. Visualizing and controlling vibrational wave packets of single molecules. Nature 465, 905–908 (2010).

    Article  ADS  Google Scholar 

  25. Hamm, P. et al. Femtosecond spectroscopy of the photoisomerisation of the protonated Schiff base of all-trans retinal. ChemPhysChem 263, 613–621 (1996).

    ADS  Google Scholar 

  26. Kuehner, D. E. et al. Lysozyme net charge and ion binding in concentrated aqueous electrolyte solutions. J. Phys. Chem. B 103, 1368–1374 (1999).

    Article  Google Scholar 

  27. http://www.xfel.eu/sites/site_xfel-gmbh/content/e63594/e63599/e%81234/e65128/e76474/sqs-wg-ii-report_eng.pdf.

  28. Schätz, T., Schramm, U. & Habs, D. Crystalline ion beams. Nature 412, 717–720 (2001).

    Article  ADS  Google Scholar 

  29. Schramm, U., Schatz, T. & Habs, D. Three-dimensional crystalline ion beams. Phys. Rev. E 66, 036501 (2002).

    Article  ADS  Google Scholar 

  30. Boutet, S. & Williams, G. J. The Coherent X-ray Imaging (CXI) instrument at the Linac Coherent Light Source (LCLS). New J. Phys. 12, 035024 (2010).

    Article  ADS  Google Scholar 

  31. Leschhorn, G., Hasegawa, T. & Schaetz, T. Efficient photoionization for barium ion trapping using a dipole-allowed resonant two-photon transition. Preprint at http://arxiv.org/abs/1110.4040 (2011).

  32. Schaetz, T. et al. Towards (scalable) quantum simulations in ion traps. J. Mod. Opt. 54, 2317–2325 (2007).

    Article  ADS  Google Scholar 

  33. Barrett, M. D. et al. Sympathetic cooling of 9Be+ and 24Mg+ for quantum logic. Phys. Rev. A 68, 042302 (2003).

    Article  ADS  Google Scholar 

  34. Lee, K. F., Villeneuve, D. M., Corkum, P. B., Stolow, A. & Underwood, J. G. Field-free three-dimensional alignment of polyatomic molecules. Phys. Rev. Lett. 97, 173001 (2006).

    Article  ADS  Google Scholar 

Download references

Acknowledgements

Financial support is gratefully acknowledged by the Deutsche Forschungsgemeinschaft (DFG), the DFG Cluster of Excellence: Munich Centre for Advanced Photonics, the International Max Planck Research School on Advanced Photon Science and the EU research project PICC: the Physics of Ion Coulomb Crystals, funded under the European Communities Seventh Framework Programme. The authors would like to thank J. Britton, W. Schmid, C. Hackenberger, J. Bayerl, M. Schulze, T. Dou and C. Kerzl for their contributions and H. J. Neusser for support of a continuous-wave cooling laser. We also thank D. Habs for the triggering discussion and G. Rempe for his intellectual and financial support.

Author information

Authors and Affiliations

Authors

Contributions

S.K. and G.L. contributed equally to this work. M.K., W.F. and R.d.V-R. developed the theory. A.S., E.B., R.E., F.K., R.K. and T.S. contributed to the experimental work.

Corresponding author

Correspondence to Tobias Schaetz.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

Supplementary Information (PDF 244 kb)

Rights and permissions

Reprints and permissions

About this article

Cite this article

Kahra, S., Leschhorn, G., Kowalewski, M. et al. A molecular conveyor belt by controlled delivery of single molecules into ultrashort laser pulses. Nature Phys 8, 238–242 (2012). https://doi.org/10.1038/nphys2214

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nphys2214

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing