The DOI matches its Crossref record; 26 of the 26 references it cites were found in a registry or an index.
Controlled dissociation of I2 via optical transitions between the X and B electronic states
Open accessAbstract
Recent progress in both theoretical and experimental methods has led to the widespread belief that control of chemical reactions with ultrashort laser pulses is in principle achievable. In this article, the I2 molecule, which has been the subject of a great deal of femtosecond work, is studied theoretically as a prospect for experimental control. An unconstrained optimization of the electric field is performed, with the objective of dissociation on the B state. Krotov's optimization theory is used for this unconstrained optimization, which reduces the CPU time usage by a factor of four. The field which results from the optimization yields a probability of 99% for B state dissociation. The Husimi transform of the optimal field indicates a simple underlying structure, in contrast with many previous fields obtained by optimal control theory: the optimal field closely resembles a sequence of three Gaussian pulses with the same central frequency. Analysis of the optimal field indicates it operates by a quasi-cw excitation directly into the B continuum. A constrained optimization was then performed: the electric field was restricted onto the frequency interval from 0 to 19752 cm−1 to avoid the quasi-continuous-wave excitation mechanism. The optimal solution of this problem uses a three-photon pump—dump—pump (PDP) mechanism. The optimal field was approximated by sequences of three and four Gaussian-shaped laser pulses; the optimal and the two approximating fields gave 34%, 6% and 11% for the dissociation probability, respectively. The fields from the constrained optimization have fwhm on the order of 30–50 fs and intensities in the range of 1010 W/cm2 and should be experimentally producible with available technology.
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“The bound on the minimum transfer time is then given by T QSL / ( N -1) ≥ max { π 2∆ E 1 ; π 2∆ E 2 } , which needs to be satisfied by any H ( t ) that brings | ψ (0) 〉 to the target state | ψ G 〉 in a time T .”
From Optimal Control at the Quantum Speed Limit (2009) · cites this paper as [7]
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Metadata
- Authors
- Somlói, J., Kazakov, V. A., & Tannor, D. J.
- Affiliations
- University of Notre Dame (US)
- ORCID
- Tannor, David J.
- Venue
- Chemical Physics
- Publisher
- Elsevier BV
- Published
- 1993-05
- Volume
- 172
- Issue
- 1
- Pages
- 85-98
- ISSN
- 0301-0104 (ISSN-L)
- OpenAlex
- W1971368733
- Cited by
- 188
- References
- 26
- Citations by year
- 2026: 6 · 2025: 8 · 2024: 3 · 2023: 5 · 2022: 4 · 2021: 7 · 2020: 8 · 2019: 8 · 2018: 10 · 2017: 4 · 2016: 9 · 2015: 7 · 2014: 11 · 2013: 5 · 2012: 5
- FWCI
- 2.70
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Licence
- Locations
- Chemical Physics (publishedVersion, cc-by-nc-nd)
- Funders
- University of Illinois at Urbana-Champaign
- National Supercomputing Center, Korea Institute of Science and Technology Information
- Office of Naval Research
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
- Keywords
- molecular iodine, laser-induced dissociation, femtosecond pulses
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