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Optimal control in a dissipative system: Vibrational excitation of by IR pulses
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10.1063/1.2206593
/content/aip/journal/jcp/124/23/10.1063/1.2206593
http://aip.metastore.ingenta.com/content/aip/journal/jcp/124/23/10.1063/1.2206593

Figures

Image of FIG. 1.
FIG. 1.

Decay of the ∣1, 3, 0⟩ state at . Upper panel: system energy; lower panel: populations of individual states.

Image of FIG. 2.
FIG. 2.

Two- (a) and three-state (b) models for excitation of the CO stretch mode, one-mode model, . (a) Population of target state ∣1⟩, obtained with pulses Eq. (20), for , , and . Solid lines: no dissipation; dashed: energy (and nonpure phase) relaxation only, and dotted: full relaxation. (b) Population of target state ∣2⟩, obtained with pulses: pulses Eq. (20) (no symbols, solid: energy relaxation only; dashed: full relaxation); OCT pulses (with symbols; dashed, bullets: energy relaxation only; solid, squares: full relaxation). The inset in (b) shows the ratio for the case of an OCT pulse (solid, with symbols) and pulses (solid, without symbols), in both cases with full dissipation included.

Image of FIG. 3.
FIG. 3.

Electric field and Husimi plot for OCT control pulses and (a) and (b) for excitation of the CO stretch mode, to its overtone ∣2⟩. The maxima of the Husimi distributions have been normalized to one. The three-level model at has been considered, with full dissipation included.

Image of FIG. 4.
FIG. 4.

Electric field (a) and target state population (b) for OCT control pulses and excitation of the CO stretch mode. The solid lines refer to a three-mode (17-level) model and the dashed lines to a one-mode (two-level) model. The bath temperature was , and pure dephasing was neglected.

Image of FIG. 5.
FIG. 5.

Electric field (a) and state populations (b) for a OCT control pulse and excitation of the CO stretch mode. Some of the states are labeled. The bath temperature was , and pure dephasing was neglected.

Image of FIG. 6.
FIG. 6.

IR excitation of the state ∣0,1,0⟩ within the three-mode model, at . (a) ; (b) . From top to bottom: optimal control field , populations of selected vibrational states, and Husimi distribution (with the maximum normalized to 1, same color coding as in Fig. 3).

Image of FIG. 7.
FIG. 7.

IR excitation of the state ∣0, 0, 2⟩ (a) and the combination mode ∣0, 1, 2⟩ (b) within the three-mode model, at , with pulses. From top to bottom: optimal control field , populations of selected vibrational states, and Husimi distribution (with the maximum normalized to 1, same color coding as in Fig. 3).

Tables

Generic image for table
Table I.

Eigenenergies relative to the ground state and quantum numbers for the 16 lowest states plus the state . For the calculation, the sinc-function DVR method has been used with a grid consisting of 18 points in the interval , 33 points along in the interval , and 55 points along in the interval . Selected values of Ref. 24, obtained with the same potential but from a 6D model, are in parentheses.

Generic image for table
Table II.

Selected dipole matrix elements (in units of ) in the upper right half of the table and transition energies in in the lower left half.

Generic image for table
Table III.

Downward and upward (reciprocal) rates for the three vibrational modes considered in this work, for temperature of 0, 10, and . Adapted form Ref. 18.

Generic image for table
Table IV.

Parameters used in the three-state model for excitation of the CO stretch mode .

Generic image for table
Table V.

Populations of states ∣1⟩ and ∣2⟩, and their ratio, immediately after application of pulses with varying pulse length but constant fluence . The three-state model at with full dissipation has been used.

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/content/aip/journal/jcp/124/23/10.1063/1.2206593
2006-06-16
2014-04-25
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Optimal control in a dissipative system: Vibrational excitation of CO∕Cu(100) by IR pulses
http://aip.metastore.ingenta.com/content/aip/journal/jcp/124/23/10.1063/1.2206593
10.1063/1.2206593
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