Stokes Photons Research Articles

Heralded Entanglement Distribution Between Two Spin‐Wave Memories Using Temporally Multiplexed Scheme

AbstractThe elementary link, which is formed by entanglement between two remote atomic ensembles, is a fundamental component of Duan–Lukin–Cirac–Zoller (DLCZ) quantum repeater. For practical realization of quantum repeaters, it is required that entanglement between two atomic‐ensemble‐based memories can be generated with high rates and retrieved with high efficiencies. However, so far, such quantum‐repeater links remain challenge in experiments. Here, heralded entanglement distribution between atomic‐ensemble‐based memories is demonstrated via temporally multiplexed scheme. A train of 12 write pulses in time is applied to a cloud of cold atoms along different directions, which generates temporally multiplexed pairs of Stokes photons and spin waves via DLCZ processes. The Stokes fields propagating in the two spatial modes, which are paired with two spin waves are combined to perform a single‐photon Bell‐state measurement. A successful detection projects the two spin waves into a single‐excitation entanglement, which represents entanglement distribution in an elementary link. Compared with single‐mode storage scheme, the temporally multiplexed scheme gives rise to a 11.8‐fold increase in entanglement generation rate. By using cavity‐enhanced scheme, spin waves stored in the atoms are retrieved on demand and the retrieval efficiencies are up to 70%, which is beneficial for the subsequent entanglement swapping between adjacent links.

Fundamental detectability of Raman scattering: A unified diagrammatic approach.

Both spontaneous Raman scattering and stimulated Raman scattering (SRS) are cornerstones of modern photonics, spectroscopy, and imaging. However, a unified understanding of the ultimate detectability of Raman scattering is lacking, due to both historical and technical reasons. Starting from quantum electrodynamics, we formulate the fundamental detectability for both spontaneous Raman scattering and SRS. The key concept is recognizing spontaneous Raman scattering as stimulated Raman process driven by vacuum field fluctuation. A simple and unified expression, Eq. (17), is derived, which can be depicted on a two-dimensional phase-diagram-like graph with inherent symmetry. It turns out that the particle nature of light dictates the ultimate detectability of spontaneous Raman scattering, which can be represented by a line on this detectability diagram. Importantly, if provided with a reasonably strong Stokes photon flux, SRS can breach this fundamental limit and open uncharted territory of drastically accelerated measurement speed and much lower detection concentration relevant to biological imaging. Such new territory in the detectability diagram is otherwise forbidden by the spontaneous counterpart. Diagrammatical analysis explains the empirical observations, provides quantitative insights, and makes new predictions. Notably, recent experimental applications of SRS microscopy can almost entirely be captured by this diagram, further supporting the explanatory power of the theory. Thus, this unified diagrammatic approach outlines a framework to understand all Raman-based measurement and provides a theoretical explanation for the remarkable utility of the emerging SRS microscopy.

Coherent Electron-Vibron Interactions in Surface-Enhanced Raman Scattering (SERS).

In this Letter we identify coherent electron-vibron interactions between near-resonant and nonresonant electronic levels that contribute beyond standard optomechanical models for off-resonant or resonance surface-enhanced Raman scattering (SERS). By developing an open-system quantum model using first molecular interaction principles, we show how the Raman interference of both resonant and nonresonant contributions can provide several orders of magnitude modifications of the SERS peaks with respect to former optomechanical models and over the fluorescence backgrounds. This cooperative optomechanical mechanism allows for generating an enhancement of nonclassical photon pair correlations between Stokes and anti-Stokes photons, which can be detected by photon-counting measurements. Our results demonstrate Raman enhancements and suppressions of coherent nature that significantly impact the standard estimations of the optomechanical contribution from SERS spectra and their quantum mechanical observable effects.

Biphoton generation enhanced by nonlocal nonlinearity via Rydberg interactions.

Strongly correlated Stokes and anti-Stokes photon pairs (biphotons) exhibiting very large generation rates and spectral brightnesses could be attained at extremely low pump powers and optical depths. This is realized via spontaneous four-wave mixing in cold atoms with enhanced nonlocal (Rydberg) optical nonlinearities and prepared into a dark state with a large population imbalance. The scheme works with all light fields on resonance yet with negligible linear absorption and Raman gain.

Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid

Spontaneous vibrational Raman scattering is a ubiquitous form of light–matter interaction whose description necessitates quantization of the electromagnetic field. It is usually considered as an incoherent process because the scattered field lacks any predictable phase relationship with the incoming field. When probing an ensemble of molecules, the question therefore arises: What quantum state should be used to describe the molecular ensemble following spontaneous Stokes scattering? We experimentally address this question by measuring time-resolved Stokes–anti-Stokes two-photon coincidences on a molecular liquid consisting of several sub-ensembles with slightly different vibrational frequencies. When spontaneously scattered Stokes photons and subsequent anti-Stokes photons are detected into a single spatiotemporal mode, the observed dynamics is inconsistent with a statistical mixture of individually excited molecules. Instead, we show that the data are reproduced if Stokes–anti-Stokes correlations are mediated by a collective vibrational quantum, i.e. a coherent superposition of all molecules interacting with light. Our results demonstrate that the degree of coherence in the vibrational state of the liquid is not an intrinsic property of the material system, but rather depends on the optical excitation and detection geometry.

Cavity-enhanced and temporally multiplexed atom-photon entanglement interface.

Practical realization of quantum repeaters requires quantum memories with high retrieval efficiency, multi-mode storage capacities, and long lifetimes. Here, we report a high-retrieval-efficiency and temporally multiplexed atom-photon entanglement source. A train of 12 write pulses in time is applied to a cold atomic ensemble along different directions, which generates temporally multiplexed pairs of Stokes photons and spin waves via Duan-Lukin-Cirac-Zoller processes. The two arms of a polarization interferometer are used to encode photonic qubits of 12 Stokes temporal modes. The multiplexed spin-wave qubits, each of which is entangled with one Stokes qubit, are stored in a "clock" coherence. A ring cavity that resonates simultaneously with the two arms of the interferometer is used to enhance retrieval from the spin-wave qubits, with the intrinsic retrieval efficiency reaching 70.4%. The multiplexed source gives rise to a ∼12.1-fold increase in atom-photon entanglement-generation probability compared to the single-mode source. The measured Bell parameter for the multiplexed atom-photon entanglement is 2.21(2), along with a memory lifetime of up to ∼125 µs.

Optical Supercontinuum Generation via Rotational and Vibrational Molecular Cavity Optomechanics

AbstractThe solid high quality (Q) factor whispering gallery mode microcavities are demonstrated as an excellent experimental platform for enhanced light–matter interactions, and are applied in the studies of nonlinear optics, quantum optics, and sensing. However, the interaction between the microcavity and liquid anisotropic molecule, which is unique for abundant vibrational and rotational degrees of freedom, is rarely studied. Here, the gap is bridged by filling an optofluidic microbubble resonator with carbon disulfide, and the related anisotropic molecular cavity optomechanics effects are investigated. Due to the enhanced coupling between the optical mode and the rotation/vibration of molecules, stimulated Rayleigh–Kerr/Raman–Kerr scattering effects are observed. Molecular cavity optomechanics provides a broadband gain for generating Stokes photons in high‐Q optical modes, and eventually allows quasi‐supercontinuum generation with a bandwidth of 436 nm under a low continuous laser pump power of about 10 mW. This work opens a new avenue for strong light–matter interactions by exploring rotational and vibrational molecular cavity optomechanics, which provides a promising platform for nonlinear optics, cavity‐enhanced molecular reorientation dynamics, and novel optical sources.

Stimulated Raman generation of aqueous singlet oxygen without photosensitizers.

Singlet oxygen is traditionally produced via photosensitizer molecules such as methylene blue, which function as catalysts. Here we investigate stimulated Raman generation of singlet oxygen from dissolved oxygen in both water (H2O) and heavy water (D2O) using nanosecond-pulsed visible blue laser light in the 400-440nm spectral region without singlet oxygen photosensitizers. We report an oxygen-dependent Stokes peak in the red spectrum (600-670nm) that is identical when produced in H2O and D2O. These red Stokes photons are not detected when an oxygen quencher is present. Temporal photodepletion of the uric acid absorbance peak at 294nm is consistent with singlet oxygen generation. We postulate that a two-photon stimulated Raman process produces singlet oxygen from O2 dissolved within the solvents. We note that the energy difference between input and output photons of 0.97eV is precisely the energy needed to excite O2 to its singlet state.

Hong–Ou–Mandel interference linking independent room-temperature quantum memories

To realize a large-scale quantum network, both quantum memory and the interference of retrieved indistinguishable photons are essentially required to perform multi-photon synchronization and quantum-interference-mediated entanglement swapping. Significant progress has been achieved in low-temperature and well-isolated systems. However, linking independent quantum memories at room temperature remain challenging. Here, we present an experimental demonstration of Hong–Ou–Mandel interference between single photons from two independent room-temperature quantum memories. We manage to simultaneously operate two such quantum memories and individually obtain a memory-built-in quantum correlation of Stokes and anti-Stokes photons by a far-off-resonance Duan–Lukin–Cirac–Zoller protocol. We also successfully enhance the Hong–Ou–Mandel interference rate up to about 15 times by increasing each photon rate, which is achieved by coordinating two quantum memories with a repeat-until-success fashion. We observe the visibility of quantum interference up to 75.0% without reduction of any background noise, well exceeding the classical limit of 50%. Our results, together with its straightforward, broadband, and room-temperature features, open up a promising way towards realizing large-scale quantum networks at ambient conditions.

Heralded single-photon source based on an ensemble of Raman-active molecules

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 anti-Stokes scattered light, the latter may possess single-photon properties. We analyze the influence of various negative factors on the characteristics of such a heralded single-photon source, which include a time delay between Stokes and anti-Stokes photons, the finiteness of the correlation radius of an external source, and background radiation. We show that the low value of the second-order autocorrelation function of the single-photon source is preserved even when the flow of uncorrelated photons exceeds the flow of correlated photons in scattered Raman light by an order of magnitude.

Solid-Phase Reference Baths for Fiber-Optic Distributed Sensing.

Observations from Raman backscatter-based Fiber-Optic Distributed Sensing (FODS) require reference sections of the fiber-optic cable sensor of known temperature to translate the primary measured intensities of Stokes and anti-Stokes photons to the secondary desired temperature signal, which also commonly forms the basis for other derived quantities. Here, we present the design and the results from laboratory and field evaluations of a novel Solid-Phase Bath (SoPhaB) using ultrafine copper instead of the traditional mechanically stirred liquid-phase water bath. This novel type is suitable for all FODS applications in geosciences and industry when high accuracy and precision are needed. The SoPhaB fully encloses the fiber-optic cable which is coiled around the inner core and surrounded by tightly interlocking parts with a total weight of 22 kg. The SoPhaB is thermoelectrically heated and/or cooled using Peltier elements to control the copper body temperature within ±0.04 K using commercially available electronic components. It features two built-in reference platinum wire thermometers which can be connected to the distributed temperature sensing instrument and/or external measurement and logging devices. The SoPhaB is enclosed in an insulated carrying case, which limits the heat loss to or gains from the outside environment and allows for mobile applications. For thermally stationary outside conditions the measured spatial temperature differences across SoPhaB parts touching the fiber-optic cable are <0.05 K even for stark contrasting temperatures of 40 K between the SoPhaB’s setpoint and outside conditions. The uniform, stationary known temperature of the SoPhaB allows for substantially shorter sections of the fiber-optic cable sensors of less than <5 bins at spatial measurement resolution to achieve an even much reduced calibration bias and spatiotemporal uncertainty compared to traditional water baths. Field evaluations include deployments in contrasting environments including the Arctic polar night as well as peak summertime conditions to showcase the wide range of the SoPhaB’s applicability.

Measuring High-Order Phonon Correlations in an Optomechanical Resonator.

We use single photon detectors to probe the motional state of a superfluid ^{4}He resonator of mass ∼1 ng. The arrival times of Stokes and anti-Stokes photons (scattered by the resonator's acoustic mode) are used to measure the resonator's phonon coherences up to the fourth order. By postselecting on photon detection events, we also measure coherences in the resonator when ≤3 phonons have been added or subtracted. These measurements are found to be consistent with predictions that assume the acoustic mode to be in thermal equilibrium with a bath through a Markovian coupling.

LED pumped Raman laser: Towards the design of an on-chip all-silicon laser

Design of an on-chip silicon Raman laser is proposed based on a slotted photonic crystal nanocavity. The slot has been considered to be filled with the silicon nanocrystal material having ultra-high Raman gain coefficient, which has further been fortified by the tight spatio-temporal optical confinement inside the nanocavity. Consequently, the threshold power as required for the lasing is miniaturized substantially, and a light emitting diode (LED) suffices for optical pumping. The LED is amenable for integration on the same platform as of the silicon nanocrystal embedded slotted photonic crystal nanocavity exploiting the efficient electroluminescence of the silicon nanocrystal material. The coupled mode equations for stimulated Raman scattering interactions, which govern the evolution of the pump and the Stokes photons, have been solved using a novel self-consistent algorithm to analyze the characteristics of the proposed laser. A lasing threshold-power, as small as, 5 μW has been achieved. Moreover, small-signal frequency response of the proposed LED pumped laser has also been evaluated in steady-state condition, and a modulation bandwidth as high as ∼1.6 GHz has been demonstrated which is almost two orders of magnitude higher than that of the conventional Raman lasers.

A polarizability driven ab initio molecular dynamics approach to stimulating Raman activity: Application to C20

We describe a novel variant of the driven molecular dynamics (DMD) method derived for probing Raman active vibrations. The method is an extension of the conventional μ-DMD formulation for simulating IR activity by means of coupling an oscillating electric field to the molecule’s dipole moment, μ, and inducing absorption of energy via tuning the field to a resonant frequency. Presently, we modify the above prescription to invoke Raman activity by coupling two electric fields, i.e. a ‘Pump’ photon of frequency ωP and a Stokes photon of frequency ωS to the molecule’s polarizability tensor, α, with the difference in the frequencies ω = ωP – ωS corresponding to the Stokes Raman shift. If ω is close to a Raman active vibrational frequency, energy absorption ensues. Varying ω allows identifying and assigning all Raman active vibrational modes, including anharmonic corrections, by means of trajectory analysis. We show that only one element of the full polarizability tensor, and its nuclear derivative, is needed for an α-DMD trajectory, making this method well suited for ab initio dynamics implementation. Numerical results using first-principles calculations are presented and discussed for the vibrational fundamentals, combination bands, overtones of H2O, CH4, and the C20 fullerene.

Ideal pairing of the Stokes and anti-Stokes photons in the Raman process

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 parameter are analyzed side-by-side to shed light to the correlations between the Stokes and anti-Stokes fields. Conditions for having the Stokes and anti-Stokes fields composed of only photon pairs, similarly as it occurs in twin beams in parametric down-conversion, are revealed. They allow for nonzero mean thermal phonon numbers.

High efficiency Brillouin random fiber laser with replica symmetry breaking enabled by random fiber grating.

We report a high efficiency Brillouin random fiber laser (BRFL) enabled by a random fiber grating (RFG) with demonstration of replica symmetry breaking (RSB). The RFG was characterized by optical coherence tomography (OCT) method, which measured the spatially resolved reflectivity of RFG by a tunable delay line. Multiple narrow linewidth peaks appeared in reflection spectrum of RFG, created by frozen scattering centers acting as narrow linewidth filters to select random modes in random fiber lasers based on Brillouin gain. With the scattering from RFG as disordered feedback, a BRFL with slope efficiency of 29.3% and lasing threshold of 10.2 mW was demonstrated with 1 kHz linewidth. Intensity dynamics show that RFG can reduce the noise of BRFL with a symmetric phase portrait, indicating the increased mean path length and coherence time of the Stokes photons. The probability distribution of the Parisi overlap parameter of intensity fluctuation spectra from trace to trace reveal a photonic spin-glass phase with RSB in the RFG enabled BRFL, providing a photonic platform to study the photon glassy behavior of random fiber lasers.

Phonon Dephasing Dynamics in MoS2

A variety of quantum degrees of freedom, e.g., spins, valleys, and localized emitters, in atomically thin van der Waals materials have been proposed for quantum information applications, and they inevitably couple to phonons. Here, we directly measure the intrinsic optical phonon decoherence in monolayer and bulk MoS2 by observing the temporal evolution of the spectral interference of Stokes photons generated by pairs of laser pulses. We find that a prominent optical phonon mode E2g exhibits a room-temperature dephasing time of ∼7 ps in both the monolayer and bulk. This dephasing time extends to ∼20 ps in the bulk crystal at ∼15 K, which is longer than previously thought possible. First-principles calculations suggest that optical phonons decay via two types of three-phonon processes, in which a pair of acoustic phonons with opposite momentum are generated.

Optical cavity enhancement experiment of Duan-Lukin-Cirac-Zoller writing excitation process in atomic ensemble

The Duan-Lukin-Cirac-Zoller (DLCZ) process in the atomic ensemble is an important means to generate quantum correlation and entanglement between photons and atoms (quantum interface). When a write pulse acts on atoms, the DLCZ quantum memory process will be generated, which has been extensively studied. In the process a spontaneous Raman scattering (SRS) of a Stokes photon is generated, and a spin-wave excitation stored in the atomic ensemble is created at the same time. The higher probability of the generation of Stokes photons will cause more noise and reduce entanglement. On the contrary, the low generation probability of Stokes photons affects the success probability of entanglement distribution on a quantum repeater. How to increase generation probability of Stokes photons without causing more noise is an urgent problem to be resolved. In this work, a &lt;sup&gt;87&lt;/sup&gt;&lt;i&gt;Rb&lt;/i&gt; atomic ensemble is placed in a standing wave cavity which resonates with the Stokes photon. This cavity has a trip length of 0.6 m and a free spectral range (FSR) of 256 MHz. The optical loss of all the optical elements in this cavity is 9%, of which 4% loss originates from the other optical elements and 5% loss from the vacuum chamber of the magneto-optical trap (MOT). The fineness of the cavity with the cold atoms is measured to be ~19.1. By calculating the total probability of Stokes photon emission out of the cavity, we derive the enhancement factor of this standing wave cavity when the cavity loss is &lt;i&gt;l&lt;/i&gt;. When this cavity is locked with PDH frequency locking technique, we observe that the production probability of the Stokes photons is 8.7 times higher than that without cavity due to the optical cavity enhancement effect. Under this condition, the relationship between the generation probability of Stokes photons and the power of write beam is studied. The write excitation probability changes linearly with the power of write beam. This work provides an experimental solution to reducing the noise caused by time multimode operation in DLCZ scheme.

Effective Hamiltonian for Stokes–anti-Stokes pair generation with pump and probe polarized modes

In the correlated Stokes--anti-Stokes scattering (SAS) an incident photon interacts with a Raman-active material, creating a Stokes photon and exciting a quantum vibrational mode in the medium, which is posteriorly annihilated on contact with a second incident photon, producing in turn an anti-Stokes photon. This can be accomplished by real and virtual processes. In real process the quantum mode shared between the Stokes and anti-Stokes events is a real particle, whereas in virtual processes the pair formation is mediated by the exchange of virtual particles. Here, we introduce a Hamiltonian to describe the pair production in SAS scattering, for both types of process, when stimulated by two orthogonally polarized laser pulses in a pump-and-probe configuration. We also model the effect of the natural decay of the vibration created in the Stokes event and compute the probability of producing SAS pairs. Additionally, we follow the dynamics of the vibration by considering the Stokes and anti-Stokes fields as external reservoirs, obtaining thus a master equation for the reduced density matrix for the vibrational population. Finally, we compare our theoretical results with recently published experimental data.

Efficient generation of heralded narrowband color-entangled states.

We show that narrowband two-color entangled single Stokes photons can be generated in a ultra-cold atoms sample via selective excitation of two spontaneous four-wave mixing (SFWM) processes. Under certain circumstances, the generation, heralded by the respective common anti-Stokes photon, is robust against losses and phase-mismatching and is remarkably efficient owing to balanced resonant enhancement of the two four-wave mixing processes in a regime of combined induced transparency. Maximally color-entangled states can be easily attained by adjusting the detunings of the external couplings and driving fields, even when these are quite weak.