Optimal control of mode-selective femtochemistry in multidimensional systems

Journal Article · Sat Sep 15 00:00:00 EDT 2007 · Physical Review. A

DOI:https://doi.org/10.1103/PHYSREVA.76.031405· OSTI ID:21015905

Mitric, Roland; Bonacic-Koutecky, Vlasta ^[1]

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1. Department of Chemistry, Humboldt-University Berlin, Brook-Taylor-Strasse 2, 12489 Berlin (Germany)

We present a strategy for optimal control of the ground-state dynamics in multidimensional systems based on a combination of the semiclassical Wigner distribution approach with direct quantum chemical molecular dynamics (MD) 'on the fly'. This allows one to treat all degrees of freedom without the need for precalculation of global potential energy surfaces. We demonstrate the scope of our theoretical procedure on two prototype systems representing rigid symmetrical molecules (Na{sub 3}F) and flexible biomolecules with low-frequency modes (glycine). We show that the ground-state isomerization process can be selectively driven by ultrashort laser pulses with different shapes which are characteristic of the prototype systems. Thus, our method opens perspectives for control of the functionality of biomolecules. Moreover, assignment of the underlying processes to pulse shapes based on MD allows one to use optimal control as a tool for analysis.

• OSTI ID: 21015905
• Journal Information: Physical Review. A, Vol. 76, Issue 3; Other Information: DOI: 10.1103/PhysRevA.76.031405; (c) 2007 The American Physical Society; Country of input: International Atomic Energy Agency (IAEA); ISSN 1050-2947
• Country of Publication: United States
• Language: English

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
DEGREES OF FREEDOM
GROUND STATES
ISOMERIZATION
MOLECULAR DYNAMICS METHOD
MOLECULAR STRUCTURE
MOLECULES
OPTIMAL CONTROL
PHOTOCHEMISTRY
PHOTON-MOLECULE COLLISIONS
POTENTIAL ENERGY
PULSE SHAPERS
PULSES
SEMICLASSICAL APPROXIMATION
SODIUM FLUORIDES
SURFACES
WIGNER DISTRIBUTION