Tomographic imaging of molecular orbitals

J. Itatani, J. Lavesque, D. Zeidler, Hiromichi Niikura, H. Pépin, J. C. Kieffer, P. B. Corkum, D. M. Villeneuve

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Abstract

Single-electron wavefunctions, or orbitals, are the mathematical constructs used to describe the multi-electron wavefunction of molecules. Because the highest-lying orbitals are responsible for chemical properties, they are of particular interest To observe these orbitals change as bonds are formed and broken is to observe the essence of chemistry. Yet single orbitals are difficult to observe experimentally, and until now, this has been impossible on the timescale of chemical reactions. Here we demonstrate that the full three-dimensional structure of a single orbital can be imaged by a seemingly unlikely technique, using high harmonics generated from intense femtosecond laser pulses focused on aligned molecules. Applying this approach to a series of molecular alignments, we accomplish a tomographic reconstruction of the highest occupied molecular orbital of N2. The method also allows us to follow the attosecond dynamics of an electron wave packet.

Original languageEnglish
Pages (from-to)867-871
Number of pages5
JournalNature
Volume432
Issue number7019
DOIs
Publication statusPublished - 2004 Dec 16
Externally publishedYes

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Cite this

Itatani, J., Lavesque, J., Zeidler, D., Niikura, H., Pépin, H., Kieffer, J. C., Corkum, P. B., & Villeneuve, D. M. (2004). Tomographic imaging of molecular orbitals. Nature, 432(7019), 867-871. https://doi.org/10.1038/nature03183