Ultrafast-nonlinear ultraviolet pulse modulation in an AlInGaN polariton waveguide operating up to room temperature.

Ultrafast nonlinear photonics enables a host of applications in advanced on-chip spectroscopy and information processing. These rely on a strong intensity dependent (nonlinear) refractive index capable of modulating optical pulses on sub-picosecond timescales and on length scales suitable for integrated photonics. Currently there is no platform that can provide this for the UV spectral range where broadband spectra generated by nonlinear modulation can pave the way to new on-chip ultrafast (bio-) chemical spectroscopy devices. We demonstrate the giant nonlinearity of UV hybrid light-matter states (exciton-polaritons) up to room temperature in an AlInGaN waveguide. We experimentally measure ultrafast nonlinear spectral broadening of UV pulses in a compact 100 µm long device and deduce a nonlinearity 1000 times that in common UV nonlinear materials and comparable to non-UV polariton devices. Our demonstration promises to underpin a new generation of integrated UV nonlinear light sources for advanced spectroscopy and measurement.

Highly nonlinear trion-polaritons in a monolayer semiconductor.

Highly nonlinear optical materials with strong effective photon-photon interactions are required for ultrafast and quantum optical signal processing circuitry. Here we report strong Kerr-like nonlinearities by employing efficient optical transitions of charged excitons (trions) observed in semiconducting transition metal dichalcogenides (TMDCs). By hybridising trions in monolayer MoSe2 at low electron densities with a microcavity mode, we realise trion-polaritons exhibiting significant energy shifts at small photon fluxes due to phase space filling. We find the ratio of trion- to neutral exciton-polariton interaction strength is in the range from 10 to 100 in TMDC materials and that trion-polariton nonlinearity is comparable to that in other polariton systems. The results are in good agreement with a theory accounting for the composite nature of excitons and trions and deviation of their statistics from that of ideal bosons and fermions. Our findings open a way to scalable quantum optics applications with TMDCs.

Pulse control protocols for preserving coherence in dipolar-coupled nuclear spin baths.

Coherence of solid state spin qubits is limited by decoherence and random fluctuations in the spin bath environment. Here we develop spin bath control sequences which simultaneously suppress the fluctuations arising from intrabath interactions and inhomogeneity. Experiments on neutral self-assembled quantum dots yield up to a five-fold increase in coherence of a bare nuclear spin bath. Numerical simulations agree with experiments and reveal emergent thermodynamic behaviour where fluctuations are ultimately caused by irreversible conversion of coherence into many-body quantum entanglement. Simulations show that for homogeneous spin baths our sequences are efficient with non-ideal control pulses, while inhomogeneous bath coherence is inherently limited even under ideal-pulse control, especially for strongly correlated spin-9/2 baths. These results highlight the limitations of self-assembled quantum dots and advantages of strain-free dots, where our sequences can be used to control the fluctuations of a homogeneous nuclear spin bath and potentially improve electron spin qubit coherence.

Tunable Photon Statistics Exploiting the Fano Effect in a Waveguide.

A strong optical nonlinearity arises when coherent light is scattered by a semiconductor quantum dot coupled to a nanophotonic waveguide. We exploit the Fano effect in such a waveguide to control the phase of the quantum interference underpinning the nonlinearity, experimentally demonstrating a tunable quantum optical filter which converts a coherent input state into either a bunched or an antibunched nonclassical output state. We show theoretically that the generation of nonclassical light is predicated on the formation of a two-photon bound state due to the interaction of the input coherent state with the quantum dot. Our model demonstrates that the tunable photon statistics arise from the dependence of the sign of two-photon interference (either constructive or destructive) on the detuning of the input relative to the Fano resonance.

Direct Measurement of Hyperfine Shifts and Radio Frequency Manipulation of Nuclear Spins in Individual CdTe/ZnTe Quantum Dots.

We achieve direct detection of electron hyperfine shifts in individual CdTe/ZnTe quantum dots. For the previously inaccessible regime of strong magnetic fields B_{z}≳0.1 T, we demonstrate robust polarization of a few-hundred-particle nuclear spin bath, with an optical initialization time of ∼1 ms and polarization lifetime exceeding ∼1 s. Nuclear magnetic resonance spectroscopy of individual dots reveals strong electron-nuclear interactions characterized by Knight fields |B_{e}|≳50 mT, an order of magnitude stronger than in III-V semiconductor quantum dots. Our studies confirm II-VI semiconductor quantum dots as a promising platform for hybrid electron-nuclear spin qubit registers, combining the excellent optical properties comparable to III-V dots and the dilute nuclear spin environment similar to group-IV semiconductors.

Valley coherent exciton-polaritons in a monolayer semiconductor.

Two-dimensional transition metal dichalcogenides (TMDs) provide a unique possibility to generate and read-out excitonic valley coherence using linearly polarized light, opening the way to valley information transfer between distant systems. However, these excitons have short lifetimes (ps) and efficiently lose their valley coherence via the electron-hole exchange interaction. Here, we show that control of these processes can be gained by embedding a monolayer of WSe2 in an optical microcavity, forming part-light-part-matter exciton-polaritons. We demonstrate optical initialization of valley coherent polariton populations, exhibiting luminescence with a linear polarization degree up to 3 times higher than displayed by bare excitons. We utilize an external magnetic field alongside selective exciton-cavity-mode detuning to control the polariton valley pseudospin vector rotation, which reaches 45° at B = 8 T. This work provides unique insight into the decoherence mechanisms in TMDs and demonstrates the potential for engineering the valley pseudospin dynamics in monolayer semiconductors embedded in photonic structures.

Nonreciprocal Transmission and Reflection of a Chirally Coupled Quantum Dot.

We report strongly nonreciprocal behavior for quantum dot exciton spins coupled to nanophotonic waveguides under resonant laser excitation. A clear dependence of the transmission spectrum on the propagation direction is found for a chirally coupled quantum dot, with spin up and spin down exciton spins coupling to the left and right propagation directions, respectively. The reflection signal shows an opposite trend to the transmission, which a numerical model indicates is due to direction-selective saturation of the quantum dot. The chiral spin-photon interface we demonstrate breaks reciprocity of the system and opens the way to spin-based quantum optical components such as optical diodes and circulators in a chip-based solid-state environment.

Transition from Propagating Polariton Solitons to a Standing Wave Condensate Induced by Interactions.

We explore phase transitions of polariton wave packets, first, to a soliton and then to a standing wave polariton condensate in a multimode microwire system, mediated by nonlinear polariton interactions. At low excitation density, we observe ballistic propagation of the multimode polariton wave packets arising from the interference between different transverse modes. With increasing excitation density, the wave packets transform into single-mode bright solitons due to effects of both intermodal and intramodal polariton-polariton scattering. Further increase of the excitation density increases thermalization speed, leading to relaxation of the polariton density from a solitonic spectrum distribution in momentum space down to low momenta, with the resultant formation of a nonequilibrium condensate manifested by a standing wave pattern across the whole sample.

Electro-mechanical control of an on-chip optical beam splitter containing an embedded quantum emitter.

We demonstrate electro-mechanical control of an on-chip GaAs optical beam splitter containing a quantum dot single-photon source. The beam splitter consists of two nanobeam waveguides, which form a directional coupler (DC). The splitting ratio of the DC is controlled by varying the out-of-plane separation of the two waveguides using electromechanical actuation. We reversibly tune the beam splitter between an initial state, with emission into both output arms, and a final state with photons emitted into a single output arm. The device represents a compact and scalable tuning approach for use in III-V semiconductor integrated quantum optical circuits.

Exciton Polaritons in a Two-Dimensional Lieb Lattice with Spin-Orbit Coupling.

We study exciton polaritons in a two-dimensional Lieb lattice of micropillars. The energy spectrum of the system features two flat bands formed from S and P_{x,y} photonic orbitals, into which we trigger bosonic condensation under high power excitation. The symmetry of the orbital wave functions combined with photonic spin-orbit coupling gives rise to emission patterns with pseudospin texture in the flat band condensates. Our Letter shows the potential of polariton lattices for emulating flat band Hamiltonians with spin-orbit coupling, orbital degrees of freedom, and interactions.

Backward Cherenkov radiation emitted by polariton solitons in a microcavity wire.

Exciton-polaritons in semiconductor microcavities form a highly nonlinear platform to study a variety of effects interfacing optical, condensed matter, quantum and statistical physics. We show that the complex polariton patterns generated by picosecond pulses in microcavity wire waveguides can be understood as the Cherenkov radiation emitted by bright polariton solitons, which is enabled by the unique microcavity polariton dispersion, which has momentum intervals with positive and negative group velocities. Unlike in optical fibres and semiconductor waveguides, we observe that the microcavity wire Cherenkov radiation is predominantly emitted with negative group velocity and therefore propagates backwards relative to the propagation direction of the emitting soliton. We have developed a theory of the microcavity wire polariton solitons and of their Cherenkov radiation and conducted a series of experiments, where we have measured polariton-soliton pulse compression, pulse breaking and emission of the backward Cherenkov radiation.

Dark Solitons in High Velocity Waveguide Polariton Fluids.

We study exciton-polariton nonlinear optical fluids in the high momentum waveguide regime for the first time. We demonstrate the formation of dark solitons with the expected dependence of width on fluid density for both main classes of soliton-forming fluid defects. The results are well described by numerical modeling of the fluid propagation. We deduce a continuous wave nonlinearity more than ten times that on picosecond time scales, arising due to interaction with the exciton reservoir.

Measurement of the spin temperature of optically cooled nuclei and GaAs hyperfine constants in GaAs/AlGaAs quantum dots.

Deep cooling of electron and nuclear spins is equivalent to achieving polarization degrees close to 100% and is a key requirement in solid-state quantum information technologies. While polarization of individual nuclear spins in diamond and SiC (ref. ) reaches 99% and beyond, it has been limited to 50-65% for the nuclei in quantum dots. Theoretical models have attributed this limit to formation of coherent 'dark' nuclear spin states but experimental verification is lacking, especially due to the poor accuracy of polarization degree measurements. Here we measure the nuclear polarization in GaAs/AlGaAs quantum dots with high accuracy using a new approach enabled by manipulation of the nuclear spin states with radiofrequency pulses. Polarizations up to 80% are observed-the highest reported so far for optical cooling in quantum dots. This value is still not limited by nuclear coherence effects. Instead we find that optically cooled nuclei are well described within a classical spin temperature framework. Our findings unlock a route for further progress towards quantum dot electron spin qubits where deep cooling of the mesoscopic nuclear spin ensemble is used to achieve long qubit coherence. Moreover, GaAs hyperfine material constants are measured here experimentally for the first time.

Publisher's Note: Spin Textures of Exciton-Polaritons in a Tunable Microcavity with Large TE-TM Splitting [Phys. Rev. Lett. 115, 246401 (2015)].

This corrects the article DOI: 10.1103/PhysRevLett.115.246401.

Tuning Nonlinear Mechanical Mode Coupling in GaAs Nanowires Using Cross-Section Morphology Control.

We investigate the nonlinear mechanical properties of GaAs nanowires with anisotropic cross-section. Fundamental and second order flexural modes are studied using laser interferometry with good agreement found between experiment and theory describing the nonlinear response under mechanical excitation. In particular, we demonstrate that the sign of the nonlinear coupling between orthogonal modes is dependent on the cross-section aspect ratio. The findings are of interest for applications such as amplitude to frequency conversion and vectorial force sensing.

Chirality of nanophotonic waveguide with embedded quantum emitter for unidirectional spin transfer.

Scalable quantum technologies may be achieved by faithful conversion between matter qubits and photonic qubits in integrated circuit geometries. Within this context, quantum dots possess well-defined spin states (matter qubits), which couple efficiently to photons. By embedding them in nanophotonic waveguides, they provide a promising platform for quantum technology implementations. In this paper, we demonstrate that the naturally occurring electromagnetic field chirality that arises in nanobeam waveguides leads to unidirectional photon emission from quantum dot spin states, with resultant in-plane transfer of matter-qubit information. The chiral behaviour occurs despite the non-chiral geometry and material of the waveguides. Using dot registration techniques, we achieve a quantum emitter deterministically positioned at a chiral point and realize spin-path conversion by design. We further show that the chiral phenomena are much more tolerant to dot position than in standard photonic crystal waveguides, exhibit spin-path readout up to 95±5% and have potential to serve as the basis of spin-logic and network implementations.

Spin Textures of Exciton-Polaritons in a Tunable Microcavity with Large TE-TM Splitting.

We report an extended family of spin textures of zero-dimensional exciton-polaritons spatially confined in tunable open microcavity structures. The transverse-electric-transverse-magnetic (TE-TM) splitting, which is enhanced in the open cavity structures, leads to polariton eigenstates carrying quantized spin vortices. Depending on the strength and anisotropy of the cavity confining potential and of the TE-TM induced splitting, which can be tuned via the excitonic or photonic fractions, the exciton-polariton emissions exhibit either spin-vortex-like patterns or linear polarization, in good agreement with theoretical modeling.

Exciton-polaritons in van der Waals heterostructures embedded in tunable microcavities.

Layered materials can be assembled vertically to fabricate a new class of van der Waals heterostructures a few atomic layers thick, compatible with a wide range of substrates and optoelectronic device geometries, enabling new strategies for control of light-matter coupling. Here, we incorporate molybdenum diselenide/hexagonal boron nitride (MoSe2/hBN) quantum wells in a tunable optical microcavity. Part-light-part-matter polariton eigenstates are observed as a result of the strong coupling between MoSe2 excitons and cavity photons, evidenced from a clear anticrossing between the neutral exciton and the cavity modes with a splitting of 20 meV for a single MoSe2 monolayer, enhanced to 29 meV in MoSe2/hBN/MoSe2 double-quantum wells. The splitting at resonance provides an estimate of the exciton radiative lifetime of 0.4 ps. Our results pave the way for room-temperature polaritonic devices based on multiple-quantum-well van der Waals heterostructures, where polariton condensation and electrical polariton injection through the incorporation of graphene contacts may be realized.

Ultra-low-power hybrid light-matter solitons.

New functionalities in nonlinear optics will require systems with giant optical nonlinearity as well as compatibility with photonic circuit fabrication techniques. Here we introduce a platform based on strong light-matter coupling between waveguide photons and quantum-well excitons. On a sub-millimetre length scale we generate picosecond bright temporal solitons at a pulse energy of only 0.5 pJ. From this we deduce a nonlinear refractive index three orders of magnitude larger than in any other ultrafast system. We study both temporal and spatio-temporal nonlinear effects and observe dark-bright spatio-temporal polariton solitons. Theoretical modelling of soliton formation in the strongly coupled system confirms the experimental observations. These results show the promise of our system as a high speed, low power, integrated platform for physics and devices based on strong interactions between photons.

Phonon-assisted population inversion of a single InGaAs/GaAs quantum dot by pulsed laser excitation.

We demonstrate a new method to realize the population inversion of a single InGaAs/GaAs quantum dot excited by a laser pulse tuned within the neutral exciton phonon sideband. In contrast to the conventional method of inverting a two-level system by performing coherent Rabi oscillation, the inversion is achieved by rapid thermalization of the optically dressed states via incoherent phonon-assisted relaxation. A maximum exciton population of 0.67±0.06 is measured for a laser tuned 0.83 meV to higher energy. Furthermore, the phonon sideband is mapped using a two-color pump-probe technique, with its spectral form and magnitude in very good agreement with the result of path-integral calculations.