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arXiv:1005.4837

Observation of single- and two-photon beating between independent Raman scattering

L. Q. Chen, Cheng-ling Bian, Guo-Wan Zhang, Z. Y. Ou, Weiping Zhang

Published May 26, 2010• 0 citations
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Abstract

By using spontaneous Raman processes in the high gain regime, we produce two independent Raman Stokes fields from an atomic ensemble. Temporal beating is observed between the two directly generated Stokes fields in a single realization. The beat frequency is found to be a result of an AC Stark frequency shift effect. However, due to the spontaneous nature of the process, the phases of the two Stokes fields change from one realization to another so that the beat signal disappears after average over many realizations. On the other hand, the beat signal is recovered in a two-photon correlation measurement, showing a two-photon interference effect. The two-photon beat signal enables us to obtain dephasing information in the Raman process. The dephasing effect is found to depend on the temperature of the atomic medium.

DOI
10.48550/arxiv.1005.4837

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By using spontaneous Raman processes in the high gain regime, we produce two independent Raman Stokes fields from an atomic ensemble. Temporal beating is observed between the two directly generated Stokes fields in a single realization. The beat frequency is found to be a result of an AC Stark frequency shift effect. However, due to the spontaneous nature of the process, the phases of the two Stokes fields change from one realization to another so that the beat signal disappears after average over many realizations. On the other hand, the beat signal is recovered in a two-photon correlation measurement, showing a two-photon interference effect. The two-photon beat signal enables us to obtain dephasing information in the Raman process. The dephasing effect is found to depend on the temperature of the atomic medium.
By using spontaneous Raman processes in the high-gain regime, we produce two independent Raman Stokes fields from an atomic ensemble. Temporal beating is observed between the two directly generated Stokes fields in a single realization. The beat frequency is found to be a result of an ac Stark frequency shift effect. However, due to the spontaneous nature of the process, the phases of the two Stokes fields change from one realization to another so that the beat signal disappears after averaging over many realizations. On the other hand, the beat signal is recovered in an intensity correlation measurement, showing a two-photon interference effect. The beat signal in intensity correlation enables us to obtain dephasing information in the Raman process. The dephasing effect is found to depend on the temperature of the atomic medium.
By using spontaneous Raman processes in the high-gain regime, we create instantaneous coherence between two independent atomic ensembles. The coherence is confirmed by the observation of temporal beating between the two subsequent readout fields converted from the atomic excitations through another enhanced Raman process. The beat frequency is found to be a result of an AC Stark frequency shift effect. We find that, due to the spontaneous nature of the process, the phases of the two ensembles change from one realization to another even though there is good coherence for a single realization.
In spontaneous Raman process in atomic cell at high gain, both the Stokes field and the accompanying collective atomic excitation (atomic spin wave) are coherent. We find that, due to the spontaneous nature of the process, the phases of the Stokes field and the atomic spin wave change randomly from one realization to another but are anti-correlated. The phases of the atomic ensembles are read out via another Raman process at a later time, thus realizing phase memory in atoms. The observation of phase correlation between the Stokes field and the collective atomic excitations is an important step towards macroscopic EPR-type entanglement of continuous variables between light and atoms.
The phenomenon of coherent Raman beats observed recently by Shoemaker and Brewer is analyzed through solutions of the coupled Maxwell-Schr\"odinger equations. The effect arises in coherently prepared molecular samples where the level degeneracy is suddenly removed by Stark-pulse switching. The problem divides into two parts: (a) a steady-state preparative regime whereby the initially degenerate quantum levels are placed in superposition by a resonant laser field, and (b) a transient regime in which coherent forward Raman scattering decays in the presence of the same laser field during a nonresonant condition. The laser and Raman light thus propagate together and produce at a detector a coherent beat with a frequency that corresponds to the level splitting between initial and final states. The beat signal possesses the remarkable property of being entirely independent of longitudinal molecular velocity in the case of a plane-wave laser beam and of being almost so for milliradian divergence. It follows that relaxation involving velocity-changing collisions and that Doppler dephasing effects are absent in coherent Raman beats, in agreement with experimental measurements of the decay rate. The effect of off-resonance excitation on the dephasing time and on the period of the beat signal is also discussed, and the possibility of a small rotation of the plane of polarization of the scattered light is included. The subject presents a new aspect of Raman scattering which can now yield precise radio-frequency splittings directly and offers a selective way of examining relaxation phenomena.
With the development of quantum optics, photon correlations acquired a prominent role as a tool to test our understanding of physics, and played a key role in verifying the validity of quantum mechanics. The spatial and temporal correlations in a light field also reveal information about its origin, and allow us to probe the nature of the physical systems interacting with it. Additionally, with the advent of quantum technologies, they have acquired technological relevance, as they are expected to play an important role in quantum communication and quantum information processing. This thesis develops techniques that combine spontaneous Raman scattering with Time Correlated Single Photon Counting, and uses them to study the quantum mechanical nature of high frequency vibrations in crystals and molecules. We demonstrate photon bunching in the Stokes and anti-Stokes fields scattered from two ultrafast laser pulses, and use their cross-correlation to measure the 3.9 ps decay time of the optical phonon in diamond. We then employ this method to measure molecular vibrations in CS2, where we are able to excite the respective vibrational modes of the two isotopic species present in the sample in a coherent superposition, and observe quantum beating between the two signals. Stokes scattering, when combined with a projective measurement, leads to a well defined quantum state. We demonstrate this by measuring the second order correlation function of the anti-Stokes field conditional on detecting one or more photons in the Stokes field, which allows us to observe a phonon modeâ s transition form a thermal state into the first excited Fock state, and measure its decay over the characteristic phonon lifetime. Finally, we use this technique to prepare a highly entangled photon-phonon state, which violates a Bell-type inequality. We measure S = 2.360 ± 0.025, violating the CHSH inequality, compatible with the non-locality of the state. The techniques we developed open the door to the study of a broad range of physical systems, where spectroscopic information is obtained with the preparation of specific quantum states. They also hold potential for future technological use, and promote vibrational Raman scattering to a resource in nonlinear quantum optics -- where it used to be considered as a source of noise instead.
In spontaneous Raman scattering in an atomic ensemble, a collective atomic spin wave is created in correlation with the Stokes field. When the Stokes photons from two or more such atomic ensembles are made indistinguishable, a 'which-way' collective atomic spin excitation is generated among the independent atomic ensembles. We demonstrate this phenomenon experimentally by reading out the atomic spin excitations and observing interference between the read-out beams. When a single-photon projective measurement is made on the indistinguishable Stokes photons, this simple scheme can be used to entangle independent atomic ensembles. Compared to other currently used methods, this scheme can be easily scaled up and has greater efficiency.