Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 111, Issue 3, Pages 912-917Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1321999111
Keywords
chemical dynamics; electron dynamics; ultrafast
Categories
Funding
- Army Research Office
- National Science Foundation Physics Frontier Center
- European Research Council Advanced Grant [XCHEM 290853]
- European Marie Curie Reintegration Grant [ATTOTREND]
- European COST Actions [CM0702, CM1204]
- European Initial Training Network CORINF, Ministerio de Ciencia e Innovacion Project (Spain) [FIS2010-15127, CSD 2007-00010]
- ERA-Chemistry Project [PIM2010EEC-00751]
- Japan Society for the Promotion of Science [C24540421]
- HA-PACS (Highly Accelerated Parallel Advanced system for Computational Sciences)
- Grants-in-Aid for Scientific Research [24540421] Funding Source: KAKEN
- Direct For Mathematical & Physical Scien
- Division Of Physics [1125844] Funding Source: National Science Foundation
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High harmonic light sources make it possible to access attosecond timescales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics, the concept of attosecond chemistry has not yet been realized; this is because excitation and manipulation of molecular orbitals requires precisely controlled attosecond waveforms in the deep UV, which have not yet been synthesized. Here, we present a unique approach using attosecond vacuum UV pulse-trains to coherently excite and control the outcome of a simple chemical reaction in a deuterium molecule in a non-Born-Oppenheimer regime. By controlling the interfering pathways of electron wave packets in the excited neutral and singly ionized molecule, we unambiguously show that we can switch the excited electronic state on attosecond timescales, coherently guide the nuclear wave packets to dictate the way a neutral molecule vibrates, and steer and manipulate the ionization and dissociation channels. Furthermore, through advanced theory, we succeed in rigorously modeling multiscale electron and nuclear quantum control in a molecule. The observed richness and complexity of the dynamics, even in this very simplest of molecules, is both remarkable and daunting, and presents intriguing new possibilities for bridging the gap between attosecond physics and attochemistry.
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