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中国物理B：英文版

Polarization and phase control of two-photon absorption in an isotropic molecular system

卢晨晖, Hui Zhang, 张诗按, S Rộng

Published Jan 1, 2012• 0 citations
OpenAlex

Abstract

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.
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.
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.
Abstract We theoretically and experimentally demonstrate the control of the intermediate state absorption in an ( n + m ) resonance-mediated multi-photon absorption process by the polarization-modulated femtosecond laser pulse. An analytical solution of the intermediate state absorption in a resonance-mediated multi-photon absorption process is obtained based on the time-dependent perturbation theory. Our theoretical results show that the control efficiency of the intermediate state absorption by the polarization modulation is independent of the laser intensity when the transition from the intermediate state to the final state is coupled by the single-photon absorption, but will be affected by the laser intensity when this transition is coupled by the non-resonant multi-photon absorption. These theoretical results are experimentally confirmed via a two-photon fluorescence control in (2 + 1) resonance-mediated three-photon absorption of Coumarin 480 dye and a single-photon fluorescence control in (1 + 2) resonance-mediated three-photon absorption of IR 125 dye.
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 demonstrate the up-conversion fluorescence control via resonance-mediated two-photon absorption in rare-earth ions by varying both the laser polarization and phase. We show that both the laser polarization and phase can control the up-conversion fluorescence, and the up-conversion fluorescence intensity is decreased when the laser polarization changes from linear through elliptical to circular. We also show that the laser polarization will affect the control efficiency of the up-conversion fluorescence by varying the laser phase, and the circular polarization will reduce the control efficiency. Furthermore, we suggest that the control efficiency by varying the laser polarization and the effect of the laser polarization on the control efficiency by varying the laser phase can be artificially manipulated by controlling the laser spectral bandwidth. This optical control method opens a new opportunity to control the up-conversion fluorescence of rare-earth ions, which may have significant impact on the related applications of rare-earth ions.
A femtosecond laser pulse can be tailored to control the two-photon transitions using the ultra-fast pulse-shaping technique. This paper theoretically and experimentally demonstrates that two-photon transitions in molecular system with broad absorption line can be effectively controlled by square phase-modulation in frequency domain, and the influence of all parameters characterizing the square phase-modulation on two-photon transitions is systemically investigated and discussed. The obtained results have potential application in nonlinear spectroscopy and molecular physics.