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 discuss their validity in these cases.
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 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…
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…
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…
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 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_{…
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 present the possibility of steering the direction of correlations between the off-resonant Raman scattered photons from the angularly multimode atomic memory based on warm rubidium vapors. Using acousto-optic deflectors (AOD) driven by different modulation frequencies we experimentally change the angle of incidence of the laser beams on the atomic ensemble. Performing correlations measurements for various deflection angles we verify that we can choose the anti-Stokes light propagation direction independently of the correlated Stokes scattered light in the continuous way. As a result we can …
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…
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…
In this article, non-classical properties of Raman modes are investigated. The original goal, actually, is to identify how and by which method we can induce non-classicality in Raman modes. We introduce a plasmonic system in which Raman dye molecules are buried between two shells of the plasmonic materials similar to onion-like core/shell nanoparticle. This system is excited by the entangled photons, followed by analyzing its dynamics of motion using the Heisenberg-Langevin equations by which the time evolution of the signal-idler mode and Raman modes are derived. Interestingly, the entangled …
We demonstrate the generation of coherent Stokes pulses with randomized linear-polarization in diamond, when the pump wave-vector and linear polarization were oriented along the $[110]$ and $[1\bar{1}0]$ axes respectively. In this configuration the excitation of multiple Raman modes produces isotropic gain, preventing the Stokes pulse from acquiring a deterministic orientation and is instead randomized by the zero-point motion of the crystal. Experimental polarization measurements were consistent with an independent, identical distribution with an estimated entropy rate of 6.67 bits per pulse.
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…
Entanglement and Optical Nonreciprocity in spontaneous Raman Scattering
Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质结构与动力学研究所）；University of Hamburg（汉堡大学）；The Hamburg Centre for Ultrafast Imaging（汉堡超快成像中心）
The manipulation of massive ro-vibronic superpositions using time-frequency-resolved coherent anti-Stokes Raman scattering (TFRCARS): from quantum control to quantum computing
We analyze the properties of a Raman quantum light-atom interface in long atomic ensemble and its applications as a quantum memory or two-mode squeezed state generator. We consider the weak-coupling regime and include both Stokes and anti-Stokes scattering and the effects of Doppler broadening in buffer gas assuming frequent velocity-averaging collisions. We find the Green functions describing multimode transformation from input to output fields of photons and atomic excitations. Proper mode basis is found via singular value decomposition for short interaction times. It reveals that triples of…
Thanks to their highly coherent emission and compact form factor, single axial mode diamond Raman lasers have been identified as a valuable asset for applications including integrated quantum technology, high resolution spectroscopy or coherent optical communications. While the fundamental emission linewidth of these lasers can be Fourier limited, their thermo-optic characteristics lead to drifts in their carrier frequency, posing important challenges for applications requiring ultra-stable emission. We propose here a method for measuring accurately the temperature-dependent index of refractio…
We consider a method of sub-wavelength superlocalization and patterning of atomic matter waves via a two dimensional stimulated Raman adiabatic passage (2D STIRAP) process. An atom initially prepared in its ground level interacts with a doughnut-shaped optical vortex pump beam and a traveling wave Stokes laser beam with a constant (top-hat) intensity profile in space. The beams are sent in a counter-intuitive temporal sequence, in which the Stokes pulse precedes the pump pulse. The atoms interacting with both the traveling wave and the vortex beam are transferred to a final state through the 2…
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 develop a Hamiltonian formalism to study energy and position/momentum correlations between a single Stokes photon and a single material excitation that are created as a pair in the spontaneous Raman scattering process. Our approach allows for intuitive separation of the effects of spectral linewidth, chromatic dispersion, and collection angle on these correlations, and we compare the predictions of the model to experiment. These results have important implications for the use of Raman scattering in quantum protocols that rely on spectrally unentangled photons and collective excitations.
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…
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 numbe…
