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The Journal of Chemical Physics

Wave packet interferometry and quantum state reconstruction by acousto-optic phase modulation

Patrick F. Tekavec, Thomas R. Dyke, Andrew H. Marcus

Published Nov 16, 2006• 106 citations
Publisher

Abstract

Studies of wave packet dynamics often involve phase-selective measurements of coherent optical signals generated from sequences of ultrashort laser pulses. In wave packet interferometry (WPI), the separation between the temporal envelopes of the pulses must be precisely monitored or maintained. Here we introduce a new (and easy to implement) experimental scheme for phase-selective measurements that combines acousto-optic phase modulation with ultrashort laser excitation to produce an intensity-modulated fluorescence signal. Synchronous detection, with respect to an appropriately constructed reference, allows the signal to be simultaneously measured at two phases differing by 90 degrees. Our method effectively decouples the relative temporal phase from the pulse envelopes of a collinear train of optical pulse pairs. We thus achieve a robust and high signal-to-noise scheme for WPI applications, such as quantum state reconstruction and electronic spectroscopy. The validity of the method is demonstrated, and state reconstruction is performed, on a model quantum system--atomic Rb vapor. Moreover, we show that our measurements recover the correct separation between the absorptive and dispersive contributions to the system susceptibility.

DOI
10.1063/1.2386159

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Studies of wave packet dynamics often involve phase-selective measurements of coherent optical signals generated from sequences of ultrashort laser pulses. In wave packet interferometry (WPI), the separation between the temporal envelopes of the pulses must be precisely monitored or maintained. Here we introduce a new (and easy to implement) experimental scheme for phase-selective measurements that combines acousto-optic phase modulation with ultrashort laser excitation to produce an intensity-modulated fluorescence signal. Synchronous detection, with respect to an appropriately constructed reference, allows the signal to be simultaneously measured at two phases differing by 90 degrees. Our method effectively decouples the relative temporal phase from the pulse envelopes of a collinear train of optical pulse pairs. We thus achieve a robust and high signal-to-noise scheme for WPI applications, such as quantum state reconstruction and electronic spectroscopy. The validity of the method is demonstrated, and state reconstruction is performed, on a model quantum system--atomic Rb vapor. Moreover, we show that our measurements recover the correct separation between the absorptive and dispersive contributions to the system susceptibility.
Two-dimensional electronic coherence spectroscopy (ECS) is an important method to study the coupling between distinct optical modes of a material system. Such studies often involve excitation using a sequence of phased ultrashort laser pulses. In conventional approaches, the delays between pulse temporal envelopes must be precisely monitored or maintained. Here, we introduce a new experimental scheme for phase-selective nonlinear ECS, which combines acousto-optic phase modulation with ultrashort laser excitation to produce intensity modulated nonlinear fluorescence signals. We isolate specific nonlinear signal contributions by synchronous detection, with respect to appropriately constructed references. Our method effectively decouples the relative temporal phases from the pulse envelopes of a collinear train of four sequential pulses. We thus achieve a robust and high signal-to-noise scheme for phase-selective ECS to investigate the resonant nonlinear optical response of photoluminescent systems. We demonstrate the validity of our method using a model quantum three-level system-atomic Rb vapor. Moreover, we show how our measurements determine the resonant complex-valued third-order susceptibility.
We study wave packet interferometry (WPI) considering the laser pulse fields both classical and quantum mechanically. WPI occurs in a molecule after subjecting it to the interaction with a sequence of phase-locked ultrashort laser pulses. Typically, the measured quantity is the fluorescence of the molecule from an excited electronic state. This signal has imprinted the interference of the vibrational wave packets prepared by the different laser pulses of the sequence. The consideration of the pulses as quantum entities in the analysis allows us to study the entanglement of the laser pulse states with the molecular states. With a simple model for the molecular system, plus several justified approximations, we solve for the fully quantum mechanical molecule-electromagnetic field state. We then study the reduced density matrices of the molecule and the laser pulses separately. We calculate measurable corrections to the case where the fields are treated classically.
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.
In this series of papers we report on the generation and application of multiple pulse phase coherent sequences in optical spectroscopy.In this paper the effects of intense pulse trains on systems with only two resonant energy levels are analyzed, with particular attention to the effects of extreme inhomogeneous broadening and population depletion to nonresonant levels.It is shown that these effects, which are present in virtually all optical systems, make the simple gyroscopic model of optical coherent transients invalid.Exact calculations show, e.g., that a two-pulse photon echo is not maximized by a 1:2 length ratio for the pulses; that the maximum excited state population is not created by a 180" pulse; and that three equal pulses are almost as effective as a 1:2:1 ratio for producing three pulse echoes.The role of pulse phase is extensively analyzed.Pulse sequences are proposed and experimentally demonstrated which permit optical phase sensitive detection and measurement of ground state relaxation parameters.The experimental results are based on an extension of the acousto-optic modulation and fluoresence detection techniques of Zewail and Orlowski [Zewail et al., Chem.Phys.Lett.48, 256 (1977); Orlowski et al., ibid.54, 197 (1978)).The relative merits offluorescence and transverse polarization detection are discussed, and fluorescence detection is shown to be more generally useful for these new sequences.Finally, composite pulse trains are shown to be capable of substantially increasing the signal available from highly inhomogenously broadened transitions.In paper II we extend the treatment to multilevel systems with some emphasis on solid state applications.
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.
High resolution quantum beat spectroscopy has been realized to study atomic wave packet dynamics. Wave packets comprising pairs of low quantum number (n = 5 - 8) electronic states were formed in Rb vapor with ultrafast laser pulses, and their dynamics was observed by an all-optical technique of parametric four wave mixing (PFWM). The experimental apparatus designed, constructed and automated for this work provided unprecedented signal intensity that enabled time-frequency-resolved analysis of wave packet dynamics with picosecond temporal resolution over the course of 1100 ps. Both time-resolved and non-time-resolved discrete Fourier methods were applied to measure the concurrent formation of multiple wave packets. Many novel effects and interactions have been measured either for the first time or with greatly improved signal-to-noise ratio. Among them were the formation of the 8S1/2 - 6D5/2 wave packet that was not directly excited by the ultrafast radiation, formation and relative dynamics of quantum beating harmonics up to 73 THz, and quantum beating revivals. The effects of vapor number density and temperature were analyzed experimentally. Interference between the 7S1/2 - 5D5/2 and 8S1/2 - 6D5/2 wave packets (frequencies of 18.225 THz and 10.73 THz, respectively) has been observed for the first time and will be described in detail.