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Institute of Physics eBooks

Interaction of light pulses with ensembles of chromophores: wavepackets

Joel Y. Yuen-Zhou, Jacob J. Krich, Ivan Kassal, Allan S. Johnson, Alán Aspuru‐Guzik

Published Sep 1, 2014• 0 citations
Publisher
DOI
10.1088/978-0-750-31062-8ch4

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Ultrafast Dynamics and Nonlinear Interactions in Alkali Atoms and Diatomics

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Ultrafast laser pump-probe techniques have been used to study the rovibrational dynamics of the B, C, and D states of the Cesium dimer and to study atomic wavepackets and nonlinear effects in Rubidium and Potassium. Two color, pump-probe techniques have been used to probe the time evolution of wavepackets in the B, C, and D rovibrational levels of Cs$\sb2$. The temporal history of the wavepacket is inferred from the time and energy-integrated photoelectron signal produced when the excited state is photoionized by a time-delayed probe pulse. Oscillatory motion is observed in the photoionization signals, corresponding to the vibrational energy differences of the state begin studied. The period of oscillation ranges between 2.2 and 1.1 ps depending on the state. Quantum mechanical simulations of the wavepacket motion show excellent agreement with the experimental data. Experiments have been carried out in which atomic wavepackets interact with a four-wave mixing process in Rb and K to produce spatially and temporally coherent pulses of UV radiation. Wave packets are produced by coherently exciting an ensemble of states using the broad bandwidth of a femtosecond pulse. Oscillations corresponding to the energy differences between the levels in the wavepacket are superimposed on the UV signal when two identical pump and delayed probe pulses are introduced into the alkali vapor. Analyses of the UV emission line profiles show excellent agreement with the four-wave mixing process.

•Dec 1, 1997•0 citations
The study of dephasing time in a material by using time-resolved two-photon near-field scanning optical microscope (NSOM) with classical light has been of great interest due to its many applications. If a material shows longer coherence time between molecules and excitation pulse,it can contain information about the material for a longer time. On the contrary, the use of quantum light for studying the molecular structure has also been of great interest in many applications. In this study, a correlation between quantum coherence of the material and the probability of absorbing classical and quantum light has been shown. The dephasing time in rhodamine-B (Rh-B) chromophores doped in polystyrene nanospheres (PS-Rh) and bare Rh-B chromophores has been observed using time-resolved two-photon NSOM at room temperature. It has been observed that the quantum coherence on a single PS bead doped with Rh-B chromophores has a longer lifetime compared to the bare Rh-B chromophores. A possible reason for longer coherence time in PS-Rh nanospheres could be the isolation of Rh-B chromophores inside the PS nanospheres, which removes the heterogeneity and local environment effects and increases the interference between the laser pulse and superposition state. The interaction of these PS-Rh nanospheres and Rh-B chromophores with classical and entangled light has also been investigated using classical and entangled two-photon absorption spectroscopies, and the cross-sections have been calculated. It was observed that doped PS-Rh nanospheres show higher nonlinear optical properties than the Rh-B chromophores. In this study, it has been shown that, in addition to the transition dipole moment and detuning energy, classical and entangled two-photon cross-sections are also being affected by the quantum coherence.
Experiments have been carried out in which atomic wavepackets produced on the /spl sim/100 fs time scale interact with a 4-wave mixing process in Rb or K vapor to produce spatially and temporally coherent pulses of UV radiation. Wavepackets are produced by coherently exciting the 9 d, 10 d, 11 s, and 12 s states ensemble of Rb with red (/spl sim/625 nm) pulses from an amplified CPM system. Two pulses of approximately equal energy (/spl sim/75 /spl mu/J) are produced in a beamsplitter and one delayed in time with respect to the other by a delay stage in one leg of a Michelson interferometer.
Ultrafast laser pump-probe techniques have been used to study the rovibrational dynamics of the B, C, and D states of the Cesium dimer and to study atomic wavepackets and nonlinear effects in Rubidium and Potassium. Two color, pump-probe techniques have been used to probe the time evolution of wavepackets in the B, C, and D rovibrational levels of Cs$\sb2$. The temporal history of the wavepacket is inferred from the time and energy-integrated photoelectron signal produced when the excited state is photoionized by a time-delayed probe pulse. Oscillatory motion is observed in the photoionization signals, corresponding to the vibrational energy differences of the state begin studied. The period of oscillation ranges between 2.2 and 1.1 ps depending on the state. Quantum mechanical simulations of the wavepacket motion show excellent agreement with the experimental data. Experiments have been carried out in which atomic wavepackets interact with a four-wave mixing process in Rb and K to produce spatially and temporally coherent pulses of UV radiation. Wave packets are produced by coherently exciting an ensemble of states using the broad bandwidth of a femtosecond pulse. Oscillations corresponding to the energy differences between the levels in the wavepacket are superimposed on the UV signal when two identical pump and delayed probe pulses are introduced into the alkali vapor. Analyses of the UV emission line profiles show excellent agreement with the four-wave mixing process.