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Chinese Physics B

Coherent control of non-resonant two-photon transition in molecular system

Hui Zhang, Shian Zhang, Zugeng Wang, Zhenrong Sun

Published Nov 1, 2010• 4 citations
Publisher

Abstract

In this paper, we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system (Perylene dissolved in chloroform solution) by shaping the femtosecond pulses with simple phase patterns (cosinusoidal and π phase step-function shape). The control efficiency of the two-photon transition probability is correlated with both the laser field and the molecular absorption bandwidth. Our results demonstrate that, the two-photon transition probability in a molecular system can be reduced but not completely eliminated by manipulating the laser field, and the control efficiency is minimal when the molecular absorption bandwidth is larger than twice the laser spectral bandwidth.

DOI
10.1088/1674-1056/19/11/113208

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In this paper, we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system (Perylene dissolved in chloroform solution) by shaping the femtosecond pulses with simple phase patterns (cosinusoidal and π phase step-function shape). The control efficiency of the two-photon transition probability is correlated with both the laser field and the molecular absorption bandwidth. Our results demonstrate that, the two-photon transition probability in a molecular system can be reduced but not completely eliminated by manipulating the laser field, and the control efficiency is minimal when the molecular absorption bandwidth is larger than twice the laser spectral bandwidth.
Multiphoton transition probability can be manipulated by tailoring the ultrashort laser pulses. In this paper, we theoretically and experimentally investigate the influence of the absorption bandwidth and line shape on the coherent control of two-photon transitions in two-level system by manipulating the femtosecond laser pulse with the $\ensuremath{\pi}$ spectral phase step. A coherent feature with a coherent peak and two coherent dips can be achieved if the absorption bandwidth is less than twice of the laser spectral bandwidth. The absorption bandwidth decides the coherent peak or dip intensity, and the absorption line shape affects the symmetry of the two coherent dips.
In this paper, we theoretically investigate the control of the non-resonant two-photon absorption induced by two time-delayed laser pulses, and an analytical solution for the dependence of the two-photon transition probability on the time delay and relative carrier-envelope phase of the two laser pulses is achieved. We show that the two-photon absorption can be significantly enhanced or completely suppressed by varying the time delay between the two laser pulses or their relative carrier-envelope phase. We also show that the two-photon absorption can be selectively excited when two excited states are simultaneously excited. Furthermore, we discuss the two-photon absorption control in the molecular system and analyze the effect of the absorption bandwidth on the control efficiency of the two-photon absorption.
With femtosecond laser spectral phase shaping technique and polarization modulation technique,the coherent control of two-photon fluorescence(TPF)in Rhodamine B solution is studied.By shaping the femtosecond pulse with simple phase patterns(cosinusoidal andπphase step-function shape),two-photon fluorescence intensity of Rhodamine B can be controlled effectively.Theoretical simulation and calculation show that the variation of twophoton fluorescence intensity for Rhodamine B solution is ascribed to the constructive and destructive interference of various quantum paths in two-photon transitions.TPF of Rhodamine B solution displays periodical change by polarization modulation.TPF decreases when the laser polarization changes from linear through elliptical to circular.These experimental results are theoretically confirmed to be caused by the variation of laser polarization.
We theoretically and experimentally study the polarization and phase control of two-photon absorption in an isotropic molecular system.We theoretically show that the two-photon transition probability decreases when the laser polarization changes from linear through elliptical to circular,and the laser polarization does not affect the control efficiency of two-photon transition probability by shaping the spectral phase.These theoretical results are experimentally confirmed in coumarin 480.Furthermore,we propose that the combination of the laser polarization with the spectral phase modulation can further increase the control efficiency of the two-photon absorption.
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We theoretically and experimentally study the polarization and phase control of two-photon absorption in an isotropic molecular system. We theoretically show that the two-photon transition probability decreases when the laser polarization changes from linear through elliptical to circular, and the laser polarization does not affect the control efficiency of two-photon transition probability by shaping the spectral phase. These theoretical results are experimentally confirmed in coumarin 480. Furthermore, we propose that the combination of the laser polarization with the spectral phase modulation can further increase the control efficiency of the two-photon absorption.