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Minimizing broadband excitation under dissipative conditions
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10.1063/1.2136155
/content/aip/journal/jcp/123/23/10.1063/1.2136155
http://aip.metastore.ingenta.com/content/aip/journal/jcp/123/23/10.1063/1.2136155
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

The pulse intensity spectrum along with absorption (solid line) and fluorescence (dashed line) spectra of LDS750 molecule in acetonitrile. Adapted from Ref. 2.

Image of FIG. 2.
FIG. 2.

Excited-state population as a function of the linear chirp for the isolated system . The population is shown at the end of the pulse for the high (solid line) and the low (dashed line) fluences. The duration of the corresponding transform-limited pulse is . Note the different scale for the excited population for two energy regimes.

Image of FIG. 3.
FIG. 3.

(Top panel) Time evolution of the excited-state population of the isolated system for the high-energy excitation. The population is calculated for a negatively [, solid line] and a positively [, dashed line] chirped pulses. (Bottom panel) The imaginary part of the transition dipole moment multiplied by the field amplitude.

Image of FIG. 4.
FIG. 4.

(Color online) (Top panel) Trajectories of the transition dipole moment renormalized by its maximal amplitude for excitation by the linear negatively chirped pulse . (Bottom panel) Excited-state population at the end of the pulse as a function of the linear chirp parameter . The calculations are performed for the system without dissipation (solid line) and for the system with vibrational relaxation with weak (, dashed line), medium (, dashed-dotted line), and strong (, dotted line) system-bath couplings.

Image of FIG. 5.
FIG. 5.

(Color online) (Top panel) Trajectories of the transition dipole moment renormalized by its maximal amplitude for excitation by the linear negatively chirped pulse . (Bottom panel) Excited-state population at the end of the pulse as a function of the linear chirp parameter . The calculations are performed for the isolated system (solid line) and for the system with pure electronic dephasing: weak (, dashed line), medium (, dashed-dotted line) and strong (, dotted line) couplings.

Image of FIG. 6.
FIG. 6.

Time evolution of the excited-state population of the isolated system for the high-energy excitation. The population is calculated for a linear negatively chirped pulse (solid line) and for the optimal pulse (dashed line) obtained by using a genetic algorithm with the random phases, generated at discrete points of the frequency spectrum. The inset figure shows the temporal profile of the optimized pulse.

Image of FIG. 7.
FIG. 7.

(Color) Calculations for nondissipative system. Time-frequency Wigner distribution corresponding to the optimized linear (top panel) and nonlinear (bottom panel) chirped pulses. The right sides show the frequency spectra of the pulses, while their temporal profiles are shown in the upper panels. The phase is expanded in the Taylor series up to the second order (linear chirp) and in the basis of periodic functions (nonlinear chirp).

Image of FIG. 8.
FIG. 8.

(Top panel) Evolution of the excited-state population of the isolated system for the high-energy excitation. The population is calculated for a linear negatively chirped pulse (solid line) and for the optimal pulse (dashed line) obtained by using a genetic algorithm with the phase expanded in the basis of periodic functions. (Bottom panel) Trajectories of the transition dipole moment renormalized by its maximal amplitude. Solid and dashed lines refer to the linear chirped pulse and its nonlinear analog, respectively.

Image of FIG. 9.
FIG. 9.

(Top panel) Time evolution of the excited-state population of the dissipative system for the high-energy excitation. The population is calculated for a linear negatively chirped pulse (solid line) and for the optimal pulse obtained by using a genetic algorithm (dashed line). (Bottom panel) Trajectories of the transition dipole moment renormalized by its maximal amplitude. Calculations were performed for the system with weak vibrational relaxation and medium pure electronic dephasing .

Image of FIG. 10.
FIG. 10.

(Color) Calculations for the dissipative system. Time-frequency Wigner distribution corresponding to the optimal linear (top panel) and nonlinear (bottom panel) chirped pulses. Calculations were performed for the system with medium vibrational relaxation and electronic dephasing .

Image of FIG. 11.
FIG. 11.

(Color) (Top panel) Time evolution of the excited-state population of the dissipative system for the high-energy excitation. The population is calculated for a linear negatively chirped pulse (solid line) and for the optimal pulse obtained by using a genetic algorithm (dashed line). (Bottom panel) Time-frequency Wigner distribution corresponding to the optimized nonlinear chirped pulse. The calculations were performed for the primary system with the following parameters: the ground-state and the excited-state frequencies and the dimensionless displacement of . The right sides show the frequency spectra of the pulses, while their temporal profiles are shown in the upper panels. The phase is expanded in the basis of periodic functions.

Image of FIG. 12.
FIG. 12.

Effect of the intensity for linearly chirped pulses. The value of the linear chirp is plotted as a function of the pulse fluence (the amplitude of the corresponding transform-limited pulse). Calculations were performed for the isolated system (squares) and as well as for a dissipative system (triangles) with f medium vibrational relaxation and medium pure electronic dephasing .

Image of FIG. 13.
FIG. 13.

The excited-state population at the end of the pulse as function of the pulse fluence (the amplitude of the corresponding transform-limited pulse). Calculations were performed (top panel) for the system without dissipation and (bottom panel) for the system with medium vibrational relaxation ) and medium pure electronic dephasing . The arrow points to the maximal fluence used in the experiment by Nahmias et al. (Ref. 2)

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/content/aip/journal/jcp/123/23/10.1063/1.2136155
2005-12-19
2014-04-25
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Minimizing broadband excitation under dissipative conditions
http://aip.metastore.ingenta.com/content/aip/journal/jcp/123/23/10.1063/1.2136155
10.1063/1.2136155
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