1. National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada
2. University of Ottawa, 150 Louis Pasteur, Ottawa, Ontario K1N 6N5, Canada
3. INRS- Energie et Materiaux, 1650 boulevard Lionel-Boulet, CP 1020, Varennes, Québec J3X 1S2, Canada
4. PRESTO, Japan Science and Technology Agency, 4-1-8 Honcho Kawaguchi Saitama, 332-0012, Japan

Correspondence to: D. M. Villeneuve¹ Email: david.villeneuve@nrc.ca

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.

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