Quantum Nonlinear Optics Research Articles

Quantum Nonlinear Optics with a Germanium-Vacancy Color Center in a Nanoscale Diamond Waveguide.

We demonstrate a quantum nanophotonics platform based on germanium-vacancy (GeV) color centers in fiber-coupled diamond nanophotonic waveguides. We show that GeV optical transitions have a high quantum efficiency and are nearly lifetime broadened in such nanophotonic structures. These properties yield an efficient interface between waveguide photons and a single GeV center without the use of a cavity or slow-light waveguide. As a result, a single GeV center reduces waveguide transmission by 18±1% on resonance in a single pass. We use a nanophotonic interferometer to perform homodyne detection of GeV resonance fluorescence. By probing the photon statistics of the output field, we demonstrate that the GeV-waveguide system is nonlinear at the single-photon level.

Self-Similar Nanocavity Design with Ultrasmall Mode Volume for Single-Photon Nonlinearities.

We propose a photonic crystal nanocavity design with self-similar electromagnetic boundary conditions, achieving ultrasmall mode volume (V_{eff}). The electric energy density of a cavity mode can be maximized in the air or dielectric region, depending on the choice of boundary conditions. We illustrate the design concept with a silicon-air one-dimensional photon crystal cavity that reaches an ultrasmall mode volume of V_{eff}∼7.01×10^{-5}λ^{3} at λ∼1550 nm. We show that the extreme light concentration in our design can enable ultrastrong Kerr nonlinearities, even at the single-photon level. These features open new directions in cavity quantum electrodynamics, spectroscopy, and quantum nonlinear optics.

Laser control of giant optical absorption and gain in quantum plasmonic particles

A quantum particle strongly interacting with a nearby metallic particle is a fundamental system in nanoplasmonics. The dielectric function of the quantum system can manifest rich quantum nonlinear optics phenomena when the spatial dependence of the vectorial nature of the probing laser field and the dipole moment are considered. We find that the quantum system can exhibit giant gain and giant absorption when the dipole moment orientation and the direction, polarization, and relative phase of the probe field components are properly tuned, especially in the near-field regime. This can be explained as due to the strong interactions between the quantum system and the metallic particle in the near-field regime at surface plasmon resonance. Interestingly, these giant features can be suppressed by a large probe Rabi frequency. The study enables remarkable coherent control of optical properties in quantum nanoplasmonics, useful for enhancing absorption in solar cells and light amplification for lasing and sensing.

Photon‐Pair Generation with a 100 nm Thick Carbon Nanotube Film

Nonlinear optics based on bulk materials is the current technique of choice for quantum-state generation and information processing. Scaling of nonlinear optical quantum devices is of significant interest to enable quantum devices with high performance. However, it is challenging to scale the nonlinear optical devices down to the nanoscale dimension due to relatively small nonlinear optical response of traditional bulk materials. Here, correlated photon pairs are generated in the nanometer scale using a nonlinear optical device for the first time. The approach uses spontaneous four-wave mixing in a carbon nanotube film with extremely large Kerr-nonlinearity (≈100 000 times larger than that of the widely used silica), which is achieved through careful control of the tube diameter during the carbon nanotube growth. Photon pairs with a coincidence to accidental ratio of 18 at the telecom wavelength of 1.5 µm are generated at room temperature in a ≈100 nm thick carbon nanotube film device, i.e., 1000 times thinner than the smallest existing devices. These results are promising for future integrated nonlinear quantum devices (e.g., quantum emission and processing devices).

Two-Photon Blockade in an Atom-Driven Cavity QED System.

Photon blockade is a dynamical quantum-nonlinear effect in driven systems with an anharmonic energy ladder. For a single atom strongly coupled to an optical cavity, we show that atom driving gives a decisively larger optical nonlinearity than cavity driving. This enhances single-photon blockade and allows for the implementation of two-photon blockade where the absorption of two photons suppresses the absorption of further photons. As a signature, we report on three-photon antibunching with simultaneous two-photon bunching observed in the light emitted from the cavity. Our experiment constitutes a significant step towards multiphoton quantum-nonlinear optics.

Fabrication of a centimeter-long cavity on a nanofiber for cavity quantum electrodynamics.

We report the fabrication of a 1.2 cm long cavity directly on a nanofiber using femtosecond laser ablation. The cavity modes with finesse values in the range of 200-400 can enable the "strong-coupling" regime of cavity QED, with high cooperativity of 10-20, for a single atom trapped 200 nm away from the fiber surface [Phys. Rev. A80, 053826 (2009)PLRAAN1050-294710.1103/PhysRevA.80.053826]. Such cavity modes can still maintain the transmission between 40%-60%, suggesting a one-pass intracavity transmission of 99.53%. Other cavity modes, which can enable cooperativity in the range of 3-10, show transmission over 60%-85% and are suitable for fiber-based single-photon sources and quantum nonlinear optics in the "Purcell" regime.

Large optical Stark shifts in single quantum dots coupled to core-shell GaAs/AlGaAs nanowires.

Nanowire quantum dots (NW-QDs) can be used for future compact and efficient optoelectronic devices. Many efforts have been made to control the QD states by inserting the QDs in doped structures and applying an electric field in a nanowire system. In this paper, we use down-conversion and up-conversion photoluminescence excitations to explore the optical and electronic properties of single quantum dots in GaAs/AlGaAs core-shell nanowires. We investigate a large optical Stark shift in this system as a new method to tune the QD states. When the tunable laser lies within the spectral bandwidth of ZB/WZ GaAs (780 nm-860 nm), we observe an extremely large optical Stark shift of 1.3 nm (0.5 nm) with increasing excitation power at a resonant wavelength of 800 nm (840 nm) in GaAs states. The ability to in situ control the energy states of self-catalyzed NW-QDs should open a new way for quantum light sources and nonlinear optics in a nanowire system.

Ultra-broadband dispersion engineering of nanophotonic waveguides.

We propose double-cladded and multi-cladded waveguide structures that enable flexible engineering of group-velocity dispersion over multi-octave spanning spectral range, allowing to produce intriguing dispersion characteristics that oscillate between normal and anomalous dispersion in a sinusoidal-like fashion with controllable magnitude, which will be very useful for nonlinear photonic applications. The proposed waveguides are easy to fabricate in practice, which we expect to have great potential for broad applications in nonlinear photonics, quantum optics, and optical communication.

A high repetition rate experimental setup for quantum non-linear optics with cold Rydberg atoms

Using electromagnetically induced transparency and photon storage, the strong dipolar interactions between Rydberg atoms and the resulting dipole blockade can be mapped onto light fields to realise optical non-linearities and interactions at the single photon level. We report on the realisation of an experimental apparatus designed to study interactions between single photons stored as Rydberg excitations in optically trapped microscopic ensembles of ultracold 87Rb atoms. A pair of in-vacuum high numerical aperture lenses focus excitation and trapping beams down to 1 μm, well below the Rydberg blockade. Thanks to efficient magneto-optical trap (MOT) loading from an atomic beam generated by a 2D MOT and the ability to recycle the microscopic ensembles more than 20000 times without significant atom loss, we achieve effective repetition rates exceeding 110 kHz to obtain good photon counting statistics on reasonable time scales. To demonstrate the functionality of the setup, we present evidence of strong photon interactions including saturation of photon storage and the retrieval of non-classical light. Using in-vacuum antennae operating at up to 40 GHz, we perform microwave spectroscopy on photons stored as Rydberg excitations and observe an interaction induced change in lineshape depending on the number of stored photons.

Cascade correlation-enhanced Raman scattering in atomic vapors**Project supported by the National Natural Science Foundation of China (Grant Nos. 11474095, 11274118, and 91536114).

A new Raman process can be used to realize efficient Raman frequency conversion by coherent feedback at low light intensity [Chen B, Zhang K, Bian C L, Qiu C, Yuan C H, Chen L Q, Ou Z Y, and Zhang W P 2013 Opt. Express 21, 10490]. We present a theoretical model to describe this enhanced Raman process, termed as cascade correlation-enhanced Raman scattering, which is a Raman process injected by a seeded light field. It is correlated with the initially prepared atomic spin excitation and driven by the quasi-standing-wave pump fields, and the processes are repeated until the Stokes intensities are saturated. Such an enhanced Raman scattering may find applications in quantum information, nonlinear optics, and optical metrology due to its simplicity.

General solution to nonlinear optical quantum graphs using Dalgarno–Lewis summation techniques

We develop an algorithm to apply the Dalgarno-Lewis (DL) perturbation theory to quantum graphs with multiple, connected edges. We use it to calculate the nonlinear optical hyperpolarizability tensors for graphs and show that it replicates the sum over states computations, but executes ten to fifty times faster. DL requires only knowledge of the ground state of the graph, eliminating the requirement to determine all possible degeneracies of a complex network. The algorithm is general and may be applied to any quantum graph.

Two photons co- and counterpropagating throughNcross-Kerr sites

A cross-Kerr interaction produces a phase shift on two modes of light proportional to the number of photons in both modes, and is sometimes called cross-phase modulation. Cross-Kerr nonlinearities have many applications in classical and quantum nonlinear optics, including the possibility of a deterministic and all-optical controlled-phase gate. We calculate the one- and two-photon S-matrix for fields propagating in a medium where the cross-Kerr interaction is spatially distributed at discrete interaction sites comprised of atoms. For the interactions considered, we analyze the cases where the photons co-propagate and counter-propagate through the medium and give a physical interpretation to the differences between the two cases. Finally, we obtain the S-matrix in the limit of infinitely long chains, showing that it corresponds to a perfect controlled-phase operation.

Frequency comb transferred by surface plasmon resonance

Frequency combs, millions of narrow-linewidth optical modes referenced to an atomic clock, have shown remarkable potential in time/frequency metrology, atomic/molecular spectroscopy and precision LIDARs. Applications have extended to coherent nonlinear Raman spectroscopy of molecules and quantum metrology for entangled atomic qubits. Frequency combs will create novel possibilities in nano-photonics and plasmonics; however, its interrelation with surface plasmons is unexplored despite the important role that plasmonics plays in nonlinear spectroscopy and quantum optics through the manipulation of light on a subwavelength scale. Here, we demonstrate that a frequency comb can be transformed to a plasmonic comb in plasmonic nanostructures and reverted to the original frequency comb without noticeable degradation of <6.51 × 10−19 in absolute position, 2.92 × 10−19 in stability and 1 Hz in linewidth. The results indicate that the superior performance of a well-defined frequency comb can be applied to nanoplasmonic spectroscopy, quantum metrology and subwavelength photonic circuits.

A naturally grown three-dimensional nonlinear photonic crystal

Nonlinear frequency conversion via three-dimensional (3D) quasi-phase matching (QPM) process is experimentally realized based on a Ba0.77Ca0.23TiO3 (BCT) crystal. The ferroelectric domains in BCT crystal are observed, and the results reveal that the antiparallel domains distribute in three dimensions and can provide 3D reciprocal lattice vectors for QPM processes. Broadband petal-like second-harmonic patterns are achieved, which are well consistent with the theoretical quasi-cubic model of 3D nonlinear photonic crystals. Our work not only promotes the development of QPM technique but also builds a platform for 3D nonlinear optics and quantum optics.

Zeolite Y Films as Ideal Platform for Evaluation of Third-Order Nonlinear Optical Quantum Dots

Zeolites are ideal host material for generation and stabilization of regular ultrasmall quantum dots (QDs) array with the size below 1.5 nm. Quantum dots (QDs) with high density and extinction absorption coefficient have been expected to give high level of third-order nonlinear optical (3rd-NLO) and to have great potential applications in optoelectronics. In this paper, we carried out a systematic elucidation of the third-order nonlinear optical response of various types of QDs including PbSe, PbS, CdSe, CdS, ZnSe, ZnS, Ag2Se, and Ag2S by manipulation of QDs into zeolites Y pores. In this respect, we could demonstrate that the zeolite offers an ideal platform for capability comparison 3rd-NLO response of various types of QDs with high sensitivities.

Strongly driven nonlinear quantum optics in microring resonators

We present a detailed analysis of strongly driven spontaneous four-wave mixing in a lossy integrated microring resonator side-coupled to a channel waveguide. A nonperturbative, analytic solution within the undepleted pump approximation is developed for a cw pump input of arbitrary intensity. In the strongly driven regime self- and cross-phase modulation, as well as multi-pair generation, lead to a rich variety of power-dependent effects; the results are markedly different than in the low power limit. The photon pair generation rate, single photon spectrum, and joint spectral intensity (JSI) distribution are calculated. Splitting of the generated single photon spectrum into a doublet structure associated with both pump detuning and cross-phase modulation is predicted, as well as substantial narrowing of the generated signal and idler bandwidths associated with the onset of optical parametric oscillation at intermediate powers. Both the correlated and uncorrelated contributions to the JSI are calculated, and for sufficient powers the uncorrelated part of the JSI is found to form a quadruplet structure. The pump detuning is found to play a crucial role in all of these phenomena, and a critical detuning is identified which divides the system behaviour into distinct regimes, as well as an optimal detuning strategy which preserves many of the low-power characteristics of the generated photons for arbitrary input power.

Determination of the atomic density of rubidium-87**Project supported by the Natural Science Foundation of China (Grant Nos. 11274118 and 11474095), the Innovation Program of Shanghai Municipal Education Commission of China (Grant No. 13ZZ036), and the Fundamental Research Funds for the Central Universities of China.

Atomic density is a basic and important parameter in quantum optics, nonlinear optics, and precision measurement. In the past few decades, several methods have been used to measure atomic density, such as thermionic effect, optical absorption, and resonance fluorescence. The main error of these experiments stemmed from depopulation of the energy level, self-absorption, and the broad bandwidth of the laser. Here we demonstrate the atomic density of 87Rb vapor in paraffin coated cell between 297 K and 334 K mainly using fluorescence measurement. Optical pumping, anti-relaxation coating, and absorption compensation approaches are used to decrease measurement error. These measurement methods are suitable for vapor temperature at dozens of degrees. The fitting function for the experimental data of 87Rb atomic density is given.

High-Q/V Monolithic Diamond Microdisks Fabricated with Quasi-isotropic Etching.

Optical microcavities enhance light-matter interactions and are essential for many experiments in solid state quantum optics, optomechanics, and nonlinear optics. Single crystal diamond microcavities are particularly sought after for applications involving diamond quantum emitters, such as nitrogen vacancy centers, and for experiments that benefit from diamond's excellent optical and mechanical properties. Light-matter coupling rates in experiments involving microcavities typically scale with Q/V, where Q and V are the microcavity quality-factor and mode-volume, respectively. Here we demonstrate that microdisk whispering gallery mode cavities with high Q/V can be fabricated directly from bulk single crystal diamond. By using a quasi-isotropic oxygen plasma to etch along diamond crystal planes and undercut passivated diamond structures, we create monolithic diamond microdisks. Fiber taper based measurements show that these devices support TE- and TM-like optical modes with Q > 1.1 × 10(5) and V < 11(λ/n) (3) at a wavelength of 1.5 μm.

Multiplasmon Absorption in Graphene.

We show that graphene possesses a strong nonlinear optical response in the form of multiplasmon absorption, with exciting implications in classical and quantum nonlinear optics. Specifically, we predict that graphene nanoribbons can be used as saturable absorbers with low saturation intensity in the far-infrared and terahertz spectrum. Moreover, we predict that two-plasmon absorption and extreme localization of plasmon fields in graphene nanodisks can lead to a plasmon blockade effect, in which a single quantized plasmon strongly suppresses the possibility of exciting a second plasmon.

Quantum engineering. Confining the state of light to a quantum manifold by engineered two-photon loss.

Physical systems usually exhibit quantum behavior, such as superpositions and entanglement, only when they are sufficiently decoupled from a lossy environment. Paradoxically, a specially engineered interaction with the environment can become a resource for the generation and protection of quantum states. This notion can be generalized to the confinement of a system into a manifold of quantum states, consisting of all coherent superpositions of multiple stable steady states. We have confined the state of a superconducting resonator to the quantum manifold spanned by two coherent states of opposite phases and have observed a Schrödinger cat state spontaneously squeeze out of vacuum before decaying into a classical mixture. This experiment points toward robustly encoding quantum information in multidimensional steady-state manifolds.