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Bulletin of the American Physical Society

Quantum control of spin-orbit mixed quantum states in a four-level molecule system coupled by three lasers

Jianbing Qi

Published May 31, 2018• 0 citations
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Sequences for controlling laser excitation with femtosecond three-pulse four-wave mixing

Igor Pastirk, Emily J. Brown, Bruna Irene Grimberg +2 more

Three-pulse four-wave mixing (FWM) is used here to study and control laser excitation processes. For general laser excitation processes, after a molecule interacts resonantly with a laser pulse, the molecule has a probability of being in the ground or in the excited state. Control over this process depends on the phase and amplitude of the electric fields that interact with the molecular system. Here we show how three-pulse FWM can be used to control the excitation of iodine molecules. Depending on the time delay between the first two pulses, the observed signal reflects the dynamics of the ground or excited state. A theoretical formalism based on the density matrix formulation is presented and solved for a four-level system. Experiments are found to be in excellent agreement with the theory. The influence of linear chirp on three-pulse FWM experiments is explored. Spectrally dispersed three-pulse FWM is found to be extremely useful for studying the effect of chirp on laser excitation of molecular systems. Experimental demonstrations of these effects are included.

Faraday Discussions•Jan 1, 1999•22 citations

Laser cooling of CaBr molecules and production of ultracold Br atoms: A theoretical study including spin–orbit coupling

Mingkai Fu, Haitao Ma, Jianwei Cao +1 more

Owing to the exciting potential applications of ultracold atoms and molecules in many fields, developing new cooling schemes has attracted great interests in recent years. Here, we investigate laser cooling of CaBr molecules and design a photonic scheme for the production of ultracold Br atoms using the highly accurate ab initio and dynamical methods. We find that the AΠ1/22(ν′=0)→X2Σ1/2+(ν=0) transition for CaBr features a large vibrational branching ratio, a significant photon-scattering rate, and no intermediate electronic-state interference, indicating that the ultracold CaBr could be produced through a three-laser cooling scheme. Moreover, an efficient four-pulse excitation scheme from the ground rovibrational level of the cooled CaBr molecules is proposed to yield ultracold Br atoms, in which a few spin–orbit excited states are utilized as the intermediate states. The importance of the spin–orbit coupling is underscored in this work.

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Vibrational stabilization of ultracold KRb molecules: A comparative study

Mamadou Ndong, Christiane P. Koch

The transfer of weakly bound KRb molecules from levels just below the dissociation threshold into the vibrational ground state with shaped laser pulses is studied. Optimal control theory is employed to calculate the pulses. The complexity of modeling the molecular structure is successively increased in order to study the effects of the long-range behavior of the excited-state potential, resonant spin-orbit coupling, and singlet-triplet mixing.

arXiv:1007.1898•Physical Review A•Oct 29, 2010•28 citations
Three-pulse four-wave mixing (FWM) is used here to study and control laser excitation processes. For general laser excitation processes, after a molecule interacts resonantly with a laser pulse, the molecule has a probability of being in the ground or in the excited state. Control over this process depends on the phase and amplitude of the electric fields that interact with the molecular system. Here we show how three-pulse FWM can be used to control the excitation of iodine molecules. Depending on the time delay between the first two pulses, the observed signal reflects the dynamics of the ground or excited state. A theoretical formalism based on the density matrix formulation is presented and solved for a four-level system. Experiments are found to be in excellent agreement with the theory. The influence of linear chirp on three-pulse FWM experiments is explored. Spectrally dispersed three-pulse FWM is found to be extremely useful for studying the effect of chirp on laser excitation of molecular systems. Experimental demonstrations of these effects are included.
Owing to the exciting potential applications of ultracold atoms and molecules in many fields, developing new cooling schemes has attracted great interests in recent years. Here, we investigate laser cooling of CaBr molecules and design a photonic scheme for the production of ultracold Br atoms using the highly accurate ab initio and dynamical methods. We find that the AΠ1/22(ν′=0)→X2Σ1/2+(ν=0) transition for CaBr features a large vibrational branching ratio, a significant photon-scattering rate, and no intermediate electronic-state interference, indicating that the ultracold CaBr could be produced through a three-laser cooling scheme. Moreover, an efficient four-pulse excitation scheme from the ground rovibrational level of the cooled CaBr molecules is proposed to yield ultracold Br atoms, in which a few spin–orbit excited states are utilized as the intermediate states. The importance of the spin–orbit coupling is underscored in this work.