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Femtosecond coherence and quantum control of single molecules at room temperature

Nature Physics volume 7, pages 172–177 (2011)Cite this article

Abstract

Quantum-mechanical phenomena, such as electronic coherence and entanglement, play a key role in several remarkably efficient natural processes including ultrafast electronic energy transfer and charge separation in photosynthetic light-harvesting. To gain insight into such dynamic processes of biomolecules it is vital to reveal relations between structural and quantum-mechanical properties. However, ensemble experiments targeting ultrafast coherences are hampered by the large intrinsic heterogeneity in these systems at physiological conditions, and single-molecule techniques have not been available until now. Here we show, by employing femtosecond pulse-shaping techniques, that quantum coherences in single organic molecules can be created, probed and manipulated at ambient conditions even in highly disordered solid environments. We find broadly distributed coherence decay times for different individual molecules giving direct insight into the structural heterogeneity of the local surroundings. Most importantly, we induce Rabi oscillations and control the coherent superposition state in a single molecule, thus carrying out a basic femtosecond single-qubit operation at room temperature.

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Figure 1: Concept of the experiment.
Figure 2: Quantum coherence in single molecules: Coherence decay and Rabi oscillations.
Figure 3: Controlling the coherent superposition state of a single molecule.

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Acknowledgements

We thank T. H. Taminiau, F. D. Stefani and F. Kulzer for discussions and assistance with the experimental set-up, and K. Müllen for providing the molecules. Financial support by the Körber Foundation (Hamburg), the Spanish Ministry of Science and Innovation (CSD2007-046-NanoLight.es and MAT2006-08184) and the European Union (FP6, Bio-Light-Touch) is gratefully acknowledged.

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Authors and Affiliations

  1. ICFO—Institut de Ciencies Fotoniques, Mediterranean Technology Park, 08860 Castelldefels (Barcelona), Spain

    Richard Hildner, Daan Brinks & Niek F. van Hulst

  2. ICREA—Institucio Catalana de Recerca i Estudis Avancats, 08015 Barcelona, Spain

    Niek F. van Hulst

Authors
  1. Richard Hildner
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  2. Daan Brinks
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  3. Niek F. van Hulst
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Contributions

R.H. carried out the measurements, analysed the data and conducted the simulations. D.B. and R.H. constructed the experimental set-up and carried out control experiments. R.H., D.B. and N.F.v.H. conceived and designed the experiment, and discussed the data. R.H. wrote the paper. N.F.v.H. supervised the project.

Corresponding author

Correspondence to Niek F. van Hulst.

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The authors declare no competing financial interests.

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Hildner, R., Brinks, D. & van Hulst, N. Femtosecond coherence and quantum control of single molecules at room temperature. Nature Phys 7, 172–177 (2011). https://doi.org/10.1038/nphys1858

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