Dynamics of a multilevel molecular absorber interacting with a train of optical pulses

M. J. Potasek; M. F. Arend; Y. Gao

doi:10.1364/JOSAB.24.000839

Journal of the Optical Society of America B
Vol. 24,
Issue 4,
pp. 839-848
(2007)
•https://doi.org/10.1364/JOSAB.24.000839

Dynamics of a multilevel molecular absorber interacting with a train of optical pulses

M. J. Potasek, M. F. Arend, and Y. Gao

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M. J. Potasek, M. F. Arend, and Y. Gao, "Dynamics of a multilevel molecular absorber interacting with a train of optical pulses," J. Opt. Soc. Am. B 24, 839-848 (2007)

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Abstract

The spatial and temporal dynamics of multilevel systems are studied by combining a multilevel rate equation model with a finite difference propagation code. Special attention is given to multiple pulse laser sequences. By studying the complex material response, the nonlinear absorption characteristics are explored for both picosecond and nanosecond pulse trains. The complex interrelationship between the multilevel decay rate parameters and the time scales describing the multipulse excitation sequence reverses the reverse saturation effect. By tracking of the dynamics of the level populations, we optimize the time scales of the photophysical parameters to produce a particular transmission response.

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Parameters	Description	Symbol
Material parameters	Concentration of the chromophore	$N_{T}$
	Absorption coefficient from state 0 to state 1	$σ_{01}$
	Absorption coefficient from state 1 to state 2	$σ_{12}$
	Absorption coefficient from state 3 to state 4	$σ_{34}$
	Decay rate from state 1 to state 0	$k_{10}$
	Decay rate from state 1 to state 3	$k_{13}$
	Decay rate from state 2 to state 1	$k_{21}$
	Decay rate from state 3 to state 0	$k_{30}$
	Decay rate from state 4 to state 3	$k_{43}$
	Material thickness	L
Optical parameters	Temporal $1 ∕ e$ pulse half-width	$t_{0}$
	Temporal interval between pulses	$t_{r}$
	Temporal length of pulse train	$t_{T}$
	Number of pulses in the pulse train	N
	Radial $1 ∕ e$ pulse width	$r_{0}$
	Input energy of the $n th$ pulse	$E_{n}$
	Input intensity of the $n th$ pulse	$I_{n}$
	Wavelength of the laser beam	λ

Parameters	Material
Parameters	SiPc	$C_{60}$
$N_{T}$ $(10^{18} {cm}^{- 3})$	4.8	1.5^b
$σ_{01}$ $(10^{- 18} {cm}^{2})$	2.4^a	3.1^b
$σ_{12}$ $(10^{- 18} {cm}^{2})$	30.0^a	16.0^b
$σ_{34}$ $(10^{- 18} {cm}^{2})$	48.0^a	14.0^b
$k_{10}$ $({ns}^{- 1})$	0.144^a	0.03^b
$k_{13}$ $(μ s^{- 1})$	77.8^a	740.0^b
$k_{21}$ $({ps}^{- 1})$	1.0^a	1.0^{b, c, d}
$k_{30}$ $({ms}^{- 1})$	50.0^a	25.0^b
$k_{43}$ $({ps}^{- 1})$	1.0^a	1.0^{b, c, d}
L (mm)	0.6	1.0^b
$t_{0}$ (ns)	20.0
$t_{0}$ (ns)	1.0
$t_{0}$ (ps)	40.0
$t_{FWHM}$ (ps)		8^b
$t_{FWHM}$ (ps)		30^b
$r_{0}$ $(μ m)$	40	33.4^b
λ (nm)	532	532^b

Parameters	Description	Symbol
Material parameters	Concentration of the chromophore	$N_{T}$
	Absorption coefficient from state 0 to state 1	$σ_{01}$
	Absorption coefficient from state 1 to state 2	$σ_{12}$
	Absorption coefficient from state 3 to state 4	$σ_{34}$
	Decay rate from state 1 to state 0	$k_{10}$
	Decay rate from state 1 to state 3	$k_{13}$
	Decay rate from state 2 to state 1	$k_{21}$
	Decay rate from state 3 to state 0	$k_{30}$
	Decay rate from state 4 to state 3	$k_{43}$
	Material thickness	L
Optical parameters	Temporal $1 ∕ e$ pulse half-width	$t_{0}$
	Temporal interval between pulses	$t_{r}$
	Temporal length of pulse train	$t_{T}$
	Number of pulses in the pulse train	N
	Radial $1 ∕ e$ pulse width	$r_{0}$
	Input energy of the $n th$ pulse	$E_{n}$
	Input intensity of the $n th$ pulse	$I_{n}$
	Wavelength of the laser beam	λ

Parameters	Material
Parameters	SiPc	$C_{60}$
$N_{T}$ $(10^{18} {cm}^{- 3})$	4.8	1.5^b
$σ_{01}$ $(10^{- 18} {cm}^{2})$	2.4^a	3.1^b
$σ_{12}$ $(10^{- 18} {cm}^{2})$	30.0^a	16.0^b
$σ_{34}$ $(10^{- 18} {cm}^{2})$	48.0^a	14.0^b
$k_{10}$ $({ns}^{- 1})$	0.144^a	0.03^b
$k_{13}$ $(μ s^{- 1})$	77.8^a	740.0^b
$k_{21}$ $({ps}^{- 1})$	1.0^a	1.0^{b, c, d}
$k_{30}$ $({ms}^{- 1})$	50.0^a	25.0^b
$k_{43}$ $({ps}^{- 1})$	1.0^a	1.0^{b, c, d}
L (mm)	0.6	1.0^b
$t_{0}$ (ns)	20.0
$t_{0}$ (ns)	1.0
$t_{0}$ (ps)	40.0
$t_{FWHM}$ (ps)		8^b
$t_{FWHM}$ (ps)		30^b
$r_{0}$ $(μ m)$	40	33.4^b
λ (nm)	532	532^b

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Journal of the Optical Society of America B