Raman-scattering noise in silica has been the key obstacle toward the realisation of high quality fiber-based photon-pair sources. Here, we experimentally demonstrate how to get past this limitation by dispersion tailoring a xenon-filled hollow-core photonic crystal fiber. The source operates at room temperature, and is designed to generate Raman-free photon-pairs at useful wavelength ranges, with idler at the telecom, and signal at a visible range. We achieve a coincidence-to-accidentals ratio (2) as high as 2740 combined with an ultra low heralded g H (0) = 0.002, indicating a very high signal to noise ratio and a negligible multi-photon emission probability. Moreover, by gas-pressure tuning, we demonstrate the control of photon frequencies over a range as large as 13 THz, covering S-C and L telecom band for the idler photon. This work demonstrates that hollow-core photonic crystal fiber is an excellent platform to design high quality photon-pair sources, and could play a driving role in the emerging quantum technology.
We report on the experimental characterization of a novel nonlinear liquid-filled hollow-core photonic-crystal fiber for the generation of photon pairs at telecommunication wavelength through spontaneous four-wave-mixing. We show that the optimization procedure in view of this application links the choice of the nonlinear liquid to the design parameters of the fiber, and we give an example of such an optimization at telecom wavelengths. Combining the modeling of the fiber and classical characterization techniques at these wavelengths, we identify, for the chosen fiber and liquid combination, s…
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.
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…
We propose a dual-pump third-order nonlinear scheme for producing pairs of correlated photons that is less susceptible to Raman noise than typical spontaneous four wave mixing methods (SFWM). Beginning with the full multimode Hamiltonian we derive a general expression for the joint spectral amplitude, from which the probability of producing a pair of photons can be calculated. As an example, we demonstrate that a probability of 0.028 pairs per pulse can be achieved in an appropriately designed fused silica microfiber. As compared with single pump SFWM in standard fiber, we calculate that our p…
We report a novel source of twin beams based on modulational instability in high-pressure argon-filled hollow-core kagomé-style photonic-crystal fibre. The source is Raman-free and manifests strong photon-number correlations for femtosecond pulses of squeezed vacuum with a record brightness of ~2500 photons per mode. The ultra-broadband (~50 THz) twin beams are frequency tunable and contain one spatial and less than 5 frequency modes.
A scheme of generating controllable (2+1) photons in a double-$% Λ$ atomic system based on active-Raman-gain is presented in this paper. Such (2+1) photons can be a potential candidate to generate a correlated photon pair as the photon `1' acts as a trigger. Compared to other schemes of generating correlated photon pairs, our scheme exhibits a number of advantages due to the exploit of the stimulated Raman process.
We study the scattering problem of photon and polariton in a one-dimensional coupled-cavity system. Analytical approximate analysis and numerical simulation show that a photon can stimulate the photon emission from a polariton through polariton-photon collisions. This observation opens the possibility of photon-stimulated transition from insulating to radiative phase in a coupled-cavity QED system. Inversely, we also find that a polariton can be generated by a two-photon Raman scattering process. This paves the way towards single photon storage by the aid of atom-cavity interaction.
In this work, we investigate three different compact fibered systems generating vacuum squeezing that involve optical cavities limited by the end surface of a fiber and by a curved mirror and containing a thin parametric crystal. These systems have the advantage to couple squeezed states directly to a fiber, allowing the user to benefit from the flexibility of fibers in the use of squeezing. Three types of fibers are investigated: standard single-mode fibers, photonic-crystal large mode area single-mode fibers and short multi-mode fiber taped to a single-mode fiber. The observed squeezing is m…
We propose a novel femtosecond stimulated Raman spectroscopy (FSRS) technique that combines entangled photons with interference detection to select matter pathways and enhance the resolution. Following photo excitation by an actinic pump, the measurement uses a pair of broadband entangled photons, one (signal) interacts with the molecule together with a third narrowband pulse induces the Raman process. The other (idler) photon provides a reference for the coincidence measurement. This interferometric photon-coincidence counting detection allows to separately measure Raman gain and loss signals…
Spontaneous Raman processes in cold atoms have been widely used in the past decade for generating single photons. Here, we present a method to optimize their efficiencies for given atomic coherences and optical depths. We give a simple and complete recipe that can be used in present-day experiments, attaining near-optimal single photon emission while preserving the photon purity.
We have experimentally observed switching between photon-photon correlations (bunching) and anti-correlations (anti-bunching) between two orthogonally polarized laser beams in an EIT configuration in Rb vapor. The bunching and anti-bunching sswitching occurs at a specific magnetic field strength.
New time-dependent integrals of motion are found for stimulated Raman scattering. Explicit formula for the photon-number probability distribution as a function of the laser-field intensity and the medium parameters is obtained in terms of Hermite polynomials of two variables.
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…
Semiconductor quantum dots embedded in optical cavities are promising on-demand sources of single photons. Here, we theoretically study single photon emission from an optically driven two-photon Raman transition between the biexciton and the ground state of a quantum dot. The advantage of this process is that it allows all-optical control of the properties of the emitted single photon with a laser pulse. However, with the presence of other decay channels and excitation-induced quantum interference, on-demand emission of the single Raman photon is generally difficult to achieve. Here we show th…
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 …
Entangled multi-qubit states are an essential resource for quantum information and computation. Solid-state emitters can mediate interactions between subsequently emitted photons via their spin, thus offering a route towards generating entangled multi-photon states. However, existing schemes typically rely on the incoherent emission of single photons and suffer from severe practical limitations, for self-assembled quantum dots most notably the limited spin coherence time due to Overhauser magnetic field fluctuations. We here propose an alternative approach of employing spin-flip Raman scatteri…
We develop an ultrafast frequency-resolved Raman spectroscopy with entangled photons for polyatomic molecules in condensed phases, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions that are not accessible by either classical pulses or the fields without entanglement. We develop a microscopic theory for this Raman spectroscopy, revealing the electronic coherence dynamics which often shows a rapid decay within $\sim$50fs. The heterodyne-detected Raman signal is further devel…
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）
Photonics is a promising platform for quantum technologies. However, photon sources and two-photon gates currently only operate probabilistically. Large-scale photonic processing will therefore be impossible without a multiplexing strategy to actively select successful events. High time-bandwidth-product quantum memories - devices that store and retrieve single photons on-demand - provide an efficient remedy via active synchronisation. Here we interface a GHz-bandwidth heralded single-photon source and a room-temperature Raman memory with a time-bandwidth product exceeding 1000. We store heral…
We propose an approach to simultaneously excite two atoms by using cavity-assisted Raman process in combination with cavity photon-mediated interaction. The system consists of a two-level atom and a $Λ$-type or V-type three-level atom, which are coupled together with a cavity mode. Having derived the effective Hamiltonian, we find that under certain circumstances a single photon can simultaneously excite two atoms. In addition, multiple photons and even a classical field can also simultaneously excite two atoms. As an example, we show a scheme to realize our proposal in a circuit QED setup, wh…
We provide a theoretical framework to study the effect of dephasing on the quantum indistinguishability of single photons emitted from a coherently driven cavity QED $Λ$-system. We show that with a large excited-state detuning, the photon indistinguishability can be drastically improved provided that the fluctuation rate of the noise source affecting the excited state is fast compared with the photon emission rate. In some cases a spectral filter is required to realize this improvement, but the cost in efficiency can be made small.
Dynamic Sculpting of Photon Statistics in a Raman-Coupled Cavity QED System
Center for Quantum-Enabled Computing, Center for Theoretical Physics, Polish Academy of Sciences（波兰科学院理论与量子计算中心）；Department of Physics, Sahand University of Technology（萨汗理工大学物理系）；Department of Physics, Payame Noor University（帕亚梅诺尔大学物理系）
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_{…
The long-standing goal of deterministically controlling a single photon using another was recently realized in various experimental settings. Among these, a particularly attractive demonstration relied on single-photon Raman interaction (SPRINT) in a three-level Lambda-system coupled to a single-mode waveguide. Beyond the ability to control the direction of propagation of one photon by the direction of another photon, this scheme has the potential to perform as a passive quantum memory and a universal quantum gate. Relying on interference, this all-optical, coherent scheme requires no addition…
We examine the dynamics associated with the creation of a vortex in a Bose-Einstein condensate (BEC), from another nonrotating BEC using two-photon Raman transition with Gaussian (G) and Laguerre-Gaussian (LG) laser pulses. In particular, we consider BEC of Rb atoms at their hyperfine ground states confined in a quasi two dimensional harmonic trap. Optical dipole potentials created by G and LG laser pulses modify the harmonic trap in such a way that density profiles of the condensates during the Raman transition process depend on the sign of the generated vortex. We investigate the role played…
A perturbative analytic operator solution of a completely quantum mechanical Hamiltonian of multi-photon pump non-degenerate hyper-Raman process is obtained. It is shown that the obtained solution is general in nature as the solutions of non-degenerate hyper-Raman and stimulated Raman processes can be obtained as special cases of the present solution. The analytic solutions obtained here are used to investigate the nonclassical properties of the different modes in the stimulated, spontaneous and partially spontaneous multi-photon pump non-degenerate hyper-Raman processes. The nonclassical natu…
We show that spontaneous Raman scattering of incident radiation can be observed in cavity-QED systems without external enhancement or coupling to any vibrational degree of freedom. Raman scattering processes can be evidenced as resonances in the emission spectrum, which become clearly visible as the cavity-QED system approaches the ultrastrong coupling regime. We provide a quantum mechanical description of the effect, and show that ultrastrong light-matter coupling is a necessary condition for the observation of Raman scattering. This effect, and its strong sensitivity to the system parameters…
We investigate the prospects of using two-mode intensity squeezed twin-beams, generated in Rb vapor, to improve the sensitivity of spectroscopic measurements by engaging two-photon Raman transitions. As a proof of principle demonstration, we demonstrated the quantum-enhanced measurements of the Rb $5D_{3/2}$ hyperfine structure with reduced requirements for the Raman pump laser power and Rb vapor number density.
Quantum emitters with a $Λ$-type level structure enable numerous protocols and applications in quantum science and technology. Understanding and controlling their dynamics is, therefore, one of the central research topics in quantum optics. Here, we drive two-photon Rabi oscillations between the two ground states of cesium atoms and observe the associated oscillatory Raman gain and absorption that stems from the atom-mediated coherent photon exchange between the two drive fields. The atoms are efficiently and homogeneously coupled with the probe field by means of a nanofiber-based optical inte…
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 show that an absolute coherent phase of a laser can be used to manipulate the entanglement of photon pairs of two-photon laser. Our focus is on the generation of a continuous source of entangled photon pairs in the double $Λ$ (or Raman) scheme. We study the dependence of steady state entanglement on the phase and laser parameters. We obtain a relationship between entanglement and two-photon correlation. We derive conditions that give steady state entanglement for the Raman-EIT scheme and use it to identify region of steady state macroscopic entanglement. No entanglement is found for the dou…
Solid state quantum emitters have shown strong potential for applications in quantum information, but spectral inhomogeneity of these emitters poses a significant challenge. We address this issue in a cavity-quantum dot system by demonstrating cavity-stimulated Raman spin flip emission. This process avoids populating the excited state of the emitter and generates a photon that is Raman shifted from the laser and enhanced by the cavity. The emission is spectrally narrow and tunable over a range of at least 125 GHz, which is two orders of magnitude greater than the natural linewidth. We obtain t…
Vacuum-stimulated Raman scattering in strongly coupled atom-cavity systems allows one to generate free-running single photon pulses on demand. Most properties of the emitted photons are well defined, provided spontaneous emission processes do not contribute. Therefore, electronic excitation of the atom must not occur, which is assured for a system adiabatically following a dark state during the photon-generation process. We experimentally investigate the conditions that must be met for adiabatic following in a time-of-flight driven system, with atoms passing through a cavity and a pump beam or…
We demonstrate the storage and retrieval of an on-demand single photon generated by a collective Rydberg excitation in an ultra-low noise Raman quantum memory located in a different cold atomic ensemble. We generate single photons on demand by exciting a cold cloud of Rubidium atoms off resonantly to a Rydberg state, with a generation probability up to 15 $\%$ per trial. We then show that the single photons can be stored and retrieved with an efficiency of 21 $\%$ and a noise floor of $p_n= 2.3(3) \times 10^{-4}$ per trial in the Raman quantum memory. This leads to a signal-to-noise ratio rang…
The probability of emission of a single photon via Raman scattering of laser pulse on the three-level $Λ$ - type atom in microcavity is studied. The duration of the pulse is considered to be short enough, so that the hyperfine structure of the upper level remains totally unresolved, while that of the lower level is totally resolved. The coherent laser pulse is assumed to be in resonance with the transition between one hyperfine structure component of the lower atomic level and all hyperfine structure components of the upper level, while the quantized cavity field is assumed to be in resonance …
We introduce a scheme for creating continuous variable entanglement between an atomic beam and an optical field, by using squeezed light to outcouple atoms from a BEC via a Raman transition. We model the full multimode dynamics of the atom laser beam and the squeezed optical field, and show that with appropriate two-photon detuning and two-photon Rabi frequency, the transmitted light is entangled in amplitude and phase with the outcoupled atom laser beam. The degree of entanglement is controllable via changes in the two-photon Rabi frequency of the outcoupling process.
In the context of the quantum-mechanical description of single-molecule surface-enhanced Raman scattering, intensity-field correlation measurements of photons emitted from a plasmonic cavity are explored, theoretically, using the technique of conditional homodyne detection. The inelastic interplay between plasmons and vibrations of a diatomic molecule placed inside the cavity can be manifested in phase-dependent third-order fluctuations of the light recorded by the aforesaid technique, allowing us to reveal signatures of non-classicality (indicatives of squeezing) of the outgoing Raman photons…
We propose and experimentally demonstrate a scheme to generate optically-controlled delays based on off-resonant Raman absorption. Dispersion in a transparency window between two neighboring, optically-activated Raman absorption lines is used to reduce the group velocity of broadband 765 nm pulses. We implement this approach in a potassium titanyl phosphate (KTP) waveguide at room temperature, and demonstrate Raman-induced delays of up to 140 fs for a 650-fs duration, 1.8-THz bandwidth, signal pulse; the available delay-bandwidth product is $\approx1$. Our approach is applicable to single phot…
We report the observation of a novel nonlinear effect in the hard x-ray range. Upon illuminating Fe and Cu metal foils with intense x-ray pulses tuned near their respective K edges, photons at nearly twice the incoming photon energy are emitted. The signal rises quadratically with the incoming intensity, consistent with two-photon excitation. The spectrum of emitted high-energy photons comprises multiple Raman lines that disperse with the incident photon energy. Upon reaching the double K-shell ionization threshold, the signal strength undergoes a marked rise. Above this threshold, the lines c…
We investigate the efficiency of atom-cavity based photon-generation schemes to deliver single photons of arbitrary temporal shape. Our model applies to Raman transitions in three-level atoms with one branch of the transition driven by a laser pulse, and the other coupled to a cavity mode. For any possible shape of the single-photon wavepacket, we derive an unambiguous analytic expression for the shape of the required driving laser pulse. We furthermore discuss the constraints limiting the maximum probability for emitting any desired photon, and use these to estimate upper bounds for the effic…
We present recent results on the coherent control of an optical transition in a single rubidium atom, trapped in an optical tweezer. We excite the atom using resonant light pulses that are short (4 ns) compared with the lifetime of the excited state (26 ns). By varying the intensity of the laser pulses, we can observe an adjustable number of Rabi oscillations, followed by free decay once the light is switched off. To generate the pulses we have developed a novel laser system based on frequency doubling a telecoms laser diode at 1560 nm. By setting the laser intensity to make a pi-pulse, we use…
In this paper, the noise performances of 1.5 um correlated photon pair generations based on spontaneous four wave-mixing in three types of fibers, i.e., dispersion shifted fiber, highly nonlinear fiber, and highly nonlinear microstructure fiber are investigated experimentally. Result of the comparison shows that highly nonlinear microstructure fiber has the lowest Raman noise photon generation rate among the three types of fibers while correlated photon pair generation rate is the same. Theoretical analysis shows that the noise performance is determined by the nonlinear index and Raman respons…
We report on the first observation of stimulated Raman scattering from a Lambda-type three-level atom, where the stimulation is realized by the vacuum field of a high-finesse optical cavity. The scheme produces one intracavity photon by means of an adiabatic passage technique based on a counter-intuitive interaction sequence between pump laser and cavity field. This photon leaves the cavity through the less-reflecting mirror. The emission rate shows a characteristic dependence on the cavity and pump detuning, and the observed spectra have a sub-natural linewidth. The results are in excellent a…
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 …
Using double optical Raman rephasing, an inversion-free resonant Raman echo is studied in an inhomogeneously broadened spin ensemble of a solid medium, where the Raman optical field-excited spin coherence has a frozen propagation vector. Unlike photon echoes whose quantum memory application is strictly limited due to πrephasing pulse-induced population inversion causing quantum noises, the optical Raman field-excited spin echo is inherently silent owing to the frozen propagation vector. Thus, the doubly rephased Raman echo can be directly applied for quantum interface in a population inversion…
We propose a scheme to realize a highly efficient solid state source of photon pairs using cavity-assisted stimulated Raman adiabatic passage (STIRAP) in a single quantum dot, where a single photon from pump pulse and two stokes photons from cavity mode drives the Raman transition. The Autler-Townes doublet, generated by using a resonant continuous wave laser between biexciton and exciton states, and two-photon-resonant transition through strongly coupled cavity mode are utilized to facilitate (1+2)type Raman transition in the quantum dot. We show in the case of weak pump although the probabil…
Single-photons of well-defined polarisation that are deterministically generated in a single spatio-temporal field mode are the key to the creation of multi-partite entangled states in photonic networks. Here, we present a novel scheme to produce such photons from a single atom in an optical cavity, by means of vacuum-stimulated Raman transitions between the Zeeman substates of a single hyperfine state. Upon each transition, a photon is emitted into the cavity, with a polarisation that depends on the direction of the Raman process.
The microscopic theory of superconductivity raised the disruptive idea that electrons couple through the elusive exchange of virtual phonons, overcoming the strong Coulomb repulsion to form Cooper pairs. Light is also known to interact with atomic vibrations, as for example in the Raman effect. We show that photon pairs exchange virtual vibrations in transparent media, leading to an effective photon-photon interaction identical to that for electrons in BCS theory of supercondutivity, in spite of the fact that photons are bosons. In this scenario, photons may exchange energy without matching a …
Broadband quantum memories hold great promise as multiplexing elements in future photonic quantum information protocols. Alkali vapour Raman memories combine high-bandwidth storage, on-demand read-out, and operation at room temperature without collisional fluorescence noise. However, previous implementations have required large control pulse energies and suffered from four-wave mixing noise. Here we present a Raman memory where the storage interaction is enhanced by a low-finesse birefringent cavity tuned into simultaneous resonance with the signal and control fields, dramatically reducing the…
The Stimulated Raman Adiabatic Passage (STIRAP) procedure is a robust and complete population transfer method which have various application in chemistry and atomic physics. Here, we study the effects of one-photon detuning, transition time, pulse width, and pulse delay parameters on the population transfer via STIRAP and b-STIRAP techniques. Moreover, the impact of the field amplitude which decreases the population transfer has been analyzed and it is shown that in b-STIRAP, the robustness of the complete transition can be improved by decreasing the field amplitude in the single-photon resona…
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…
Stimulated Raman scattering of atoms with $Λ$-configuration of levels is a promising tool for transducing microwave photons to optical photons. We consider an atomic Bose-Einstein condensate whose large phase-space density highly amplifies the coupling to the microwave field. Due momentum transfer to the condensate, stimulated photon scattering can occur outside of the phase-matched direction, which can be used to separate the converted photons from the strong Raman readout pulse. Conversely, in the phase-matched direction, superradiant scattering due to bosonic enhancement leads to increased …
