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Physical Review A

Heterodyne measurement of vibrational wave packets of diatomic molecules

A. Zucchetti, W. Vogel, D.‐G. Welsch, Ian A. Walmsley

Published Oct 1, 1999• 14 citations
Publisher

Abstract

A method is presented for reconstructing the quantum state of vibrational wave packets in diatomic molecules by a heterodyne experiment. After the preparation of a wave packet, a femtosecond laser pulse interferes with the induced polarization and the resulting signal is frequency filtered and measured by a photodetector. The conditions are analyzed under which the resulting time- and frequency-resolved photocurrent contains the information needed to recover the quantum state of the prepared wave packet. It is shown that the vibrational wave function in the excited electronic state can be measured directly without the need of involved numerical reconstruction. Simulations of the proposed experiment are performed for sodium dimers.

DOI
10.1103/physreva.60.2716

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A method is presented for reconstructing the quantum state of vibrational wave packets in diatomic molecules by a heterodyne experiment. After the preparation of a wave packet, a femtosecond laser pulse interferes with the induced polarization and the resulting signal is frequency filtered and measured by a photodetector. The conditions are analyzed under which the resulting time- and frequency-resolved photocurrent contains the information needed to recover the quantum state of the prepared wave packet. It is shown that the vibrational wave function in the excited electronic state can be measured directly without the need of involved numerical reconstruction. Simulations of the proposed experiment are performed for sodium dimers.
We analyze and further develop our method of quantum-state holography for reconstructing quantum superposition states in molecules or atoms [Phys. Rev. Lett. 80, 1418 (1998)]. The technique is based on mixing the unknown object state with a known reference state generated in the same system by two delayed laser pulses, and detecting the total time- and frequency-integrated fluorescence as a function of the delay. The feasibility of the method is demonstrated by reconstructing various vibrational wave packets in sodium dimers. Both the cases of completely controlled and noisy relative phase between the laser pulses are considered. In the latter case, we use the technique of coherence observation by interference noise to recover the interference component of the fluorescence signal. Our results clearly demonstrate the robustness of quantum-state holography and the high quality of reconstruction even in the presence of the external noise.
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We demonstrate an experimental approach to read and write populations and relative phases of vibrational eigenstates within a wave packet created in the BBB state of the iodine molecule by using a pair of phase-locked femtosecond laser pulses. Our highly stabilized optical interferometer provides attosecond stability and resolution in the interpulse delay. The stability and resolution have realized an exquisite tuning of the interference of two vibrational wave packets to manipulate the relative populations and the relative quantum phases among the vibrational eigenstates within the wave packets. These populations and phases have been retrieved by measuring fluorescence from the upper EEE state induced by another nanosecond (ns) or femtosecond (fs) probe laser pulse. The bandwidth of the ns probe pulse is narrow enough to select only a small portion of the rotational progression of a particular vibrational band of the $E\ensuremath{-}B$ transition. By scanning the probe wavelength, we measure the population distribution of the vibrational eigenstates within the wave packet. The fs probe pulse is used to measure quantum beats arising from the temporal evolution of the wave packet. Combining these two complementary measurements, we can read both population and phase information written and stored in the wave packet.