The Photon wave function Formalism provides an alternative description of some quantum optical phenomena in a more intuitive way. We use this formalism to describe the process of correlated Stokes--anti-Stokes Raman scattering. In this process, two photons from a laser beam are inelastically scattered by a phonon created by the first photon (Stokes processes) and annihilated by the second photon (anti-Stokes process), producing a Stokes--anti-Sokes (SaS) photon pair. We arrive at an expression for the two-photon wave function of the scattered SaS photon pair, which is in agreement with a number of experimental results.
We investigate the arrival statistics of Stokes (S) and anti-Stokes (aS) Raman photons generated in diamond membranes. Strong quantum correlations between the S and aS signals are observed, which implies that the two processes share the same phonon, that is, the phonon excited by the S process is consumed in the aS process. We show that the intensity cross-correlation $g_{\rm S,aS}^{(2)}(0)$, which describes the simultaneous detection of Stokes and anti-Stokes photons, decreases steadily with laser power as $1/{\rm P_L}$. Contrary to many other material systems, diamond exhibits a maximum $g_{…
Addressing the correlation of Stokes-shifted photons emitted from two quantum emitters
Centro de Física de Materiales (CMF-MPC), CSIC-UPV/EHU（材料物理中心）；University of the Basque Country (UPV/EHU)（巴斯克大学）；Université de Bordeaux, LP2N（波尔多大学）；Institut d’Optique & CNRS, LP2N（光学研究所与法国国家科学研究中心）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；Université de Bordeaux, CNRS, LOMA, UMR 5798（波尔多大学）；Université de Strasbourg, CNRS, Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504（斯特拉斯堡大学）；Ikerbasque, Basque Foundation for Science（伊克拉巴斯科，巴斯克科学基金会）
The production of correlated Stokes (S) and anti-Stokes (aS) photons (SaS process) mediated by real or virtual phonon exchange has been reported in many transparent materials. In this work, we investigate the polarization and time correlations of SaS photon pairs produced in a diamond sample. We demonstrate that both S and aS photons have mainly the same polarization of the excitation laser. We also perform a pump-and-probe experiment to measure the decay rate of the SaS pair production, evidencing the fundamental diference between the real and virtual (phonon exchange) processes. In real proc…
We study Stokes and anti-Stokes processes in cavity optomechanics in the regime of strong coupling. The Stokes and anti-Stokes signals exhibit prominently the normal-mode splitting. We report gain for the Stokes signal. We also report lifetime splitting when the pump power is less than the critical power for normal-mode splitting. The nonlinear Stokes processes provide a useful method for studying strong coupling regime of cavity optomechanics. We also investigate the correlations between the Stokes and anti-Stokes photons produced spontaneously by the optomechanical system. At zero temperatur…
Photons interact with each other in condensed matter through the same mechanism that forms Cooper pairs in superconductors -- the exchange of virtual phonons [PRL 119, 193603 (2017)]. It is however unclear which consequences of this interaction will be observable and potentially lead to further analogy with superconductivity. We investigate the energy, momentum and production rate of correlate Stokes-anti-Stokes (SaS) photons in diamond and other transparent media, experiencing properties akin to those of electronic Cooper pairs. The rate of correlated SaS production depends on the energy shif…
A quantum model of the Raman process with the independent Stokes and anti-Stokes nonlinear interactions is developed to study nonclassical correlations between the photons in the Stokes and anti-Stokes fields. The role of the laser pump amplitude, the ratio of the Stokes and anti-Stokes coupling constants and the population and losses of the vibrational mode in forming the correlations is elucidated. The $ g^{(2)} $ intensity cross-correlation function, noise-reduction-factor, two-mode principal squeezing variance, logarithmic negativity, non-classicality depth, steering parameter and the Bell…
We propose a new technique for comparing two Raman active samples. The method employs optical interference of the signals generated via coherent anti-Stokes Raman scattering (CARS) of broadband laser pulses with noisy spectra. It does not require spectrally resolved detection, and no prior knowledge about either the Raman spectrum of the samples, or the spectrum of the incident light is needed. We study the proposed method theoretically, and demonstrate it in a proof-of-principle experiment on Toluene and ortho-Xylene samples.
Early theoretical works on coherent anti-Stokes Raman scattering in optically active medium consider only heterodyne signal and subsequently, fourth- and fifth-rank tensor averages have been used. In this work, we presented a full signal expression of coherent anti-Stokes Raman scattering in optically active medium with the help of eighth- and ninth-rank tensor averaging for simplest experimental configuration namely, measurements of post-selected circularly polarized components of scattered anti-Stokes field in the presence of three incident laser beams all linearly polarized along the same a…
A general fundamental relation connecting the correlation of Stokes and anti-Stokes modes to the quantum statistical behavior of vibration and pump modes in Raman-active materials is derived. We show that under certain conditions this relation can be used to determine the equilibrium number variance of phonons.Time and temperature ranges for which such conditions can be satisfied are studied and found to be available in todays' experimental standards. Furthermore, we examine the results in the presence of multi-mode pump as well as for the coupling of pump to the many vibration modes and discu…
A formalism for two-photon Stokes parameters is introduced to describe the polarization entanglement of photon pairs. This leads to the definition of a degree of two-photon polarization, which describes the extent to which the two photons act as a pair and not as two independent photons. This pair-wise polarization is complementary to the degree of polarization of the individual photons. The approach provided here has a number of advantages over the density matrix formalism: it allows the one- and two-photon features of the state to be separated and offers a visualization of the mixedness of t…
Light with high mutual correlations at different frequencies can be used to create heralded single-photon sources, which may serve as the basic elements of existing quantum cryptography and quantum teleportation schemes. One of the important examples in natural systems of light with high mutual correlations is the light produced by spontaneous Raman scattering on an ensemble of molecules. In this paper, we investigate the possibility of using Raman light to create a heralded single-photon source. We show that when using Stokes scattered light for postselection of an anti-Stokes scattered light…
A new interferometric technique is demonstrated for measuring Coherent Anti-Stokes Raman Scattering (CARS) signals. Two forward-directed CARS signals are generated, one in each arm of an interferometer. The deterministic nature of the CARS process allows for these two signals, when spatially and temporally overlapped, to interfere with one another. Heterodyne detection can therefore be employed to increase the sensitivity in CARS signal detection. In addition, nonlinear CARS interferometry will facilitate the use of this spectroscopic technique for molecular contrast in Optical Coherence Tomog…
We experimentally demonstrate efficient Raman conversion to respective Stokes and anti-Stokes fields in both pulsed and continuous modes with a Rb-87 atomic vapor cell. The conversion efficiency is about 40-50% for the Stokes field and 20-30% for the anti-Stokes field, respectively. This conversion process is realized with feedback of both the Raman pump and the frequency-converted fields (Stokes or anti-Stokes). The experimental setup is very simple and can be applied easily to produce the light source with larger frequency difference using other Raman media. They may have wide applications i…
We propose and demonstrate a versatile technique to measure the lifetime of the one-phonon Fock state using two-color pump-probe Raman scattering and spectrally-resolved, time-correlated photon counting. Following pulsed laser excitation, the $n=1$ phonon Fock state is probabilistically prepared by projective measurement of a single Stokes photon. The detection of an anti-Stokes photon generated by a second, time-delayed laser pulse probes the phonon population with sub-picosecond time resolution. We observe strongly non-classical Stokes--anti-Stokes correlations, whose decay maps the single p…
Wavelength-dependent polarization state of light carries crucial information about light-matter interactions. However, its measurement is limited to bulky, energy-consuming devices, which prohibits many modern, portable applications. Here, we propose and demonstrate a chip-scale spectropolarimeter implemented using a CMOS-compatible silicon photonics technology. Four compact Vernier microresonator spectrometers are monolithically integrated with a broadband polarimeter consisting of a 2D nanophotonic antenna and a polarimetric circuit to achieve full-Stokes spectropolarimetric analysis. The pr…
Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light emitting diodes and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite Anti-Stokes process, where excitation is performed with lower energy photons. We report that the process is sufficiently efficient to excite even a single quantum system, namely…
We consider the Minkowskian norm of the n-photon Stokes tensor, a scalar invariant under the group realized by the transformations of stochastic local quantum operations and classical communications (SLOCC). This invariant is offered as a candidate entanglement measure for n-qubit states and discussed in relation to measures of quantum state entanglement for certain important classes of two-qubit and three-qubit systems. This invariant can be directly estimated via a quantum network, obviating the need to perform laborious quantum state tomography. We also show that this invariant directly cap…
A chirped-pulse quantum control scheme applicable to Coherent Anti-Stokes Raman Scattering spectroscopy, named as C-CARS, is presented aimed at maximizing the vibrational coherence in molecules. It implies chirping of three incoming pulses in the four-wave mixing process of CARS, the pump, the Stokes and the probe, to fulfil the conditions of adiabatic passage. The scheme is derived in the framework of rotating wave approximation and adiabatic elimination of excited state manifold simplifying the four-level model system into a ``super-effective'' two level system. The robustness, spectral sele…
We show that far field diffraction image of spontaneously scattered Stokes photons can be used for detection of spin entanglement and for metrology of fields gradients in cold atomic ensembles. For many-body states with small or maximum uncertainty in spin-excitation number, entanglement is simply witnessed by the presence of a sharp diffraction peak or dip. Gradient vector of external fields is measured by the displacement of a diffraction peak due to inhomogeneous spin precessions, which suggests a new possibility for precision measurement beyond the standard quantum limit without entangleme…
We demonstrate theoretically the bundle emission of $n$ strongly correlated phonons in an acoustic cavity QED system. The mechanism relies on anti-Stokes resonances that generate super-Rabi oscillations between states with a large difference in their number of excitations, which, combined with dissipation, transfer coherently pure $n$-phonon states outside of the cavity. This process works with close to perfect purity over a wide range of parameters and is tunable optically with well-resolved operation conditions. This broadens the realm of quantum phononics, with potential applications for on…
We introduce a simplified form of Stokes operators for quantum optical fields that involve the known concept of binning. Behind polarization analyzer photon numbers (more generally intensities) are measured. If the value obtained in one of the outputs, say H, is greater the than in the other one, V, then the value of the simplified Stokes operator is, say, 1, otherwise it is -1. For equal photon numbers we put 0. Such observables do not have all properties of the Stokes operators, but surprisingly can be employed in Bell type measurements, involving polarization analyzers. They are especially …
Quantum protocols will be more efficient with high-dimensional entangled states. Photons carrying orbital angular momenta can be used to create a high-dimensional entangled state. In this paper we experimentally demonstrate the entanglement of the orbital angular momentum between the Stokes and anti-Stokes photons generated in a hot atomic ensemble using spontaneous four-wave-mixing. This experiment also suggests the existence of the entanglement concerned with spatial degrees of freedom between the hot atomic ensemble and the Stokes photon.
We use the Stokes photon of a biphoton pair to set the time origin for electro-optic modulation of the wave function of the anti-Stokes photon thereby allowing arbitrary phase and amplitude modulation. We demonstrate conditional single-photon wave functions composed of several pulses, or instead, having gaussian or exponential shapes.
We present a self-consistent quantum optics approach to calculating the surface enhanced Raman spectrum of molecules coupled to arbitrarily shaped plasmonic systems. Our treatment is intuitive to use and provides fresh analytical insight into the physics of the Raman scattering near metallic surfaces and can be applied to a wide range of geometries including resonators, waveguides, as well as hybrid photonic-plasmonic systems. Our general theory demonstrates that the detected Raman spectrum originates from an interplay between nonlinear light generation and propagation. Counter intuitively, at…
We study polarization squeezing of a pure photon number state which is obviously polarized but the mere change in the basis of polarization leads to simultaneous polarization squeezing in all the components of Stokes operator vector except those falling along or perpendicular to the direction of polarization state, is observed. We use the most general definition of polarization squeezing and discuss the experimental feasibility of the result. We also observe that a squeezing operation like non-degenerate parametric amplification of the state does not reveal simultaneous squeezing in all Stokes…
Optical spectroscopy with broadband femtosecond laser pulses often involves simultaneous excitation of multiple molecular species with close resonance frequencies. Interpreting the collective optical response from molecular mixtures typically requires Fourier analysis of the detected time-resolved signal. We propose an alternative method of separating coherent optical responses from two molecular species with neighboring excitation resonances (here, vibrational modes of oxygen and carbon dioxide). We utilize ro-vibrational coupling as a mechanism of suppressing the strong vibrational response …
Quantum Zeno and anti-Zeno effects are studied in an asymmetric nonlinear optical coupler composed of a probe waveguide and a system waveguide. The system is a nonlinear waveguide operating under non-degenerate hyper-Raman process, while both the pump modes in the system are constantly interacting with the probe waveguide. The effect of the presence of probe on the temporal evolution of the system in terms of the number of photons in Stokes and anti-Stokes modes as well as phonon number is quantified as Zeno parameter. The negative (positive) values of the Zeno parameter in the specific mode a…
We use a Langevin approach to analyze the quantum noise in Coherent Anti-Stokes Raman Spectroscopy (CARS) in several experimental scenarios: with continuous wave input fields acting simultaneously and with fast sequential pulsed lasers where one field scatters off the coherence generated by other fields; and for interactions within a cavity and in free space. In all the cases, the signal as well as the quantum noise due to spontaneous decay and decoherence in the medium are shown to be described by the same general expression. Our theory in particular shows that for short interaction times, th…
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 me…
We report that the true intrinsic degree of freedom of the photon is neither the polarization nor the spin. It describes a local property in momentum space and is represented in the local representation by the Pauli matrices. This result is achieved by treating the transversality condition on the vector wavefunction as a nonholonomic quantum constraint. We find that the quantum constraint makes it possible to generalize the Stokes parameters to characterize the polarization of a general state. Unexpectedly, the generalized Stokes parameters are specified in a momentum-space local reference sys…
The temperature dependence of the asymmetry between Stokes and anti-Stokes Raman scattering can be exploited for self-calibrating, optically-based thermometry. In the context of cavity optomechanics, we observe the cavity-enhanced scattering of light interacting with the standing-wave drumhead modes of a silicon nitride membrane mechanical resonator. The ratio of the amplitude of Stokes to anti-Stokes scattered light is used to measure temperatures of optically-cooled mechanical modes down to the level of a few vibrational quanta. We demonstrate that the Raman-ratio technique is able to measur…
We propose a temporally multiplexed version of the Duan-Lukin-Cirac-Zoller (DLCZ) quantum repeater protocol using controlled inhomogeneous spin broadening in atomic gases. A first analysis suggests that the advantage of multiplexing is negated by noise due to spin wave excitations corresponding to unobserved directions of Stokes photon emission. However, this problem can be overcome with the help of a moderate-finesse cavity which is in resonance with Stokes photons, but invisible to the anti-Stokes photons. Our proposal promises greatly enhanced quantum repeater performance with atomic gases.
In the quantum process of stimulated Raman scattering (SRS), a laser photon propagating in a resonance medium undergoes multifold conversions into a Stokes photon and back. The nontrivial ``cooperative'' behavior of the Stokes component of light transmitted through the medium is proven to be completely determined by the interference of scattering amplitudes in different sub-channels of the Stokes channel, which obviously combines all the sub-channels with an odd number of photon conversions. The theory of superfluorescence is then derived as the limiting case of the SRS theory.
We present a fully quantum mechanical treatment of recent experiments on creation of collective quantum memory and generation of non-classically correlated photon pairs from an atomic ensemble via the protocol of Duan et al. [Nature {\bf 414,} 413(2001)]. The temporal evolution of photon numbers, photon statistics and cross-correlation between the Stokes and anti-Stokes fields is found by solving the equation of motion for atomic spin-wave excitations. We consider a low-finesse cavity model with collectively enhanced signal-to-noise ratio, which remains still considerably large in the free-spa…
We propose a scheme of generating and verifying mesoscopic-level entanglement between two atomic ensembles using non-resonant stimulated Raman scattering. Entanglement can be generated by direct detection or balanced homodyne detection of the Stokes fields from the two cells, after they interfere on a beam splitter. The entanglement of the collective atomic fields can be transferred to the anti-Stokes fields in a readout process. By measuring the operator moments of the anti-Stokes fields, we can verify the presence of entanglement. We model the effects of practical factors such as Stokes fiel…
Time-resolved correlation engineering in DLCZ Raman photon sources
National Cheng Kung University（国立成功大学）；National Tsing Hua University（国立清华大学）；Center for Quantum Science and Technology, National Tsing Hua University（国立清华大学量子科学与技术中心）；National Center for Excellence in Quantum Information Science and Engineering, National Tsing Hua University（国立清华大学国家量子信息与工程卓越中心）
We considered the two-photon adiabatic rapid passage excitation of a single atom from the ground to a Rydberg state. Three schemes were analyzed: both pump and Stokes fields chirped and pulsed, only the pump field is chirped, and only the pump field is pulsed and chirped while the Stokes field is continuous wave (CW). In all three cases high transfer efficiencies $>99\%$ were achieved for the experimentally realizable Rabi frequencies and the pulse durations of the fields.
We present an experimental demonstration of simultaneous above-threshold oscillations of the Stokes and anti-Stokes fields together with the single pumping beam with rubidium atoms inside an optical standing-wave cavity. The triple resonant conditions can be achieved easily by making use of the large dispersions due to two-photon transitions in the three-level atomic system. This work provides a way to achieve high efficient nonlinear frequency conversion and the generated bright Stokes and anti-Stokes cavity output beams are potential resource for applications in quantum information science.
Time-bin entangled single-photons are highly demanded for long distance quantum communication. We propose a heralded source of tunable narrowband single photons entangled in well-separated multiple temporal modes (time bins) with controllable amplitudes. The detection of a single Stokes photon generated in a cold atomic ensemble via Raman scattering of a weak write pulse heralds the preparation of one spin excitation stored within the atomic medium. A train of read laser pulses deterministically converts the atomic excitation into a single anti-Stokes photon delocalized in multi-time-bins. The…
We present an experimental demonstration of the Hamiltonian manipulation in light-atom interface in Raman-type warm rubidium-87 vapor atomic memory. By adjusting the detuning of the driving beam we varied the relative contributions of the Stokes and anti-Stokes scattering to the process of four-wave mixing which reads out a spatially multimode state of atomic memory. We measured the temporal evolution of the readout fields and the spatial intensity correlations between write-in and readout as a function of detuning with the use of an intensified camera. The correlation maps enabled us to resol…
We experimentally demonstrate an angularly-multiplexed holographic memory capable of intrinsic generation, storage and retrieval of multiple photons, based on off-resonant Raman interaction in warm rubidium-87 vapors. The memory capacity of up to 60 independent atomic spin-wave modes is evidenced by analyzing angular distributions of coincidences between Stokes and time-delayed anti-Stokes light, observed down to the level of single spin-wave excitation during several-$μ$s memory lifetime. We also propose how to practically enhance rates of single and multiple photons generation by combining o…
Demonstration of traveling-wave interactions between spontaneous photon emissions and atoms in a chiral F-P cavity
State Key Laboratory of Quantum Optics and Quantum Optics Devices, Institute of Opto-Electronics, Shanxi University（山西大学光电研究所量子光学与量子光学器件国家重点实验室）；Collaborative Innovation Center of Extreme Optics, Shanxi University（山西大学极端光学协同创新中心）
Molecular ro-vibronic coherences, joint energy-time distributions of quantum amplitudes, are selectively prepared, manipulated, and imaged in Time-Frequency-Resolved Coherent Anti-Stokes Raman Scattering (TFRCARS) measurements using femtosecond laser pulses. The studies are implemented in iodine vapor, with its thermally occupied statistical ro-vibrational density serving as initial state. The evolution of the massive ro-vibronic superpositions, consisting of 1000 eigenstates, is followed through two-dimensional images. The first- and second-order coherences are captured using time-integrated …
Nonclassicality is studied through a quasidistribution of phases for the Raman process under both weak and strong pump conditions. In the former case, the solution is applicable to both resonant and off-resonant Raman processes, while strong classical pump is assumed at resonance. Under weak pump conditions (i.e., in a complete quantum treatment), the phase difference of phases described by single nonclassical modes is required to be filtered to describe a regular distribution function, which is not the case with strong pump. Compound Stokes-phonon mode shows nonclassical features of phases in…
