Monolayers of semiconducting transition metal dichalcogenides (TMDs) have long attracted interest for their intriguing optical and electronic properties. Recently TMDs in their quasi-bulk form have started to show considerable promise for nanophotonics thanks to their high refractive indices, large optical anisotropy, wide transparency windows reaching to the visible, and robust room temperature excitons promising for nonlinear optics. Adherence of TMD layers to any substrate via van der Waals forces is a further key enabler for nanofabrication of sophisticated photonic structures requiring heterointegration. Here, we capitalize on these attractive properties and realize topological spin-Hall photonic lattices made of arrays of triangular nanoholes in 50 to 100 nm thick WS$_2$ flakes exfoliated on SiO$_2$/Si substrates. High quality structures are achieved taking advantage of anisotropic dry etching dictated by the crystal axes of WS$_2$. Reflectance measurements at room temperature show a photonic gap opening in the near-infrared in trivial and topological phases. Unidirectional propagation along the domain interface is demonstrated in real space via circularly polarized laser excitation in samples with both zigzag and armchair domain boundaries. Finite-difference time-domain simulations are used to interpret optical spectroscopy results. Our work opens the way for future sophisticated nanophotonic devices based on the layered (van der Waals) materials platform.
Integration of 2D semiconductors with photonic crystal slabs provides an attractive approach to achieve strong light--matter coupling and exciton-polariton formation in a planar chip-compatible geometry. However, for the development of practical devices, it is crucial that the polariton excitations in the structure are easily tunable and exhibit strong nonlinear response. Here we study neutral and charged exciton-polaritons in an electrostatically gated planar photonic crystal slab with an embedded monolayer semiconductor MoSe$_2$ and experimentally demonstrate strong polariton nonlinearity, which can be tuned via gate voltage. We find that modulation of dielectric environment within the photonic crystal results in the formation of two distinct resonances with significantly different nonlinear response, which enables optical switching with ultrashort laser pulses. Our results open new avenues towards development of active polaritonic devices in a compact chip-compatible implementation.
Maxim Makhonin, Anthonin Delphan, Kok Wee Song, Paul Walker, Tommi Isoniemi, Peter Claronino, Konstantinos Orfanakis, Sai Kiran Rajendran, Hamid Ohadi, Julian Heckötter, Marc Aßmann, Manfred Bayer, Alexander Tartakovskii, Maurice Skolnick, Oleksandr Kyriienko, Dmitry Krizhanovskii Rydberg excitons (analogues of Rydberg atoms in condensed matter systems) are highly excited bound electron-hole states with large Bohr radii. The interaction between them as well as exciton coupling to light may lead to strong optical nonlinearity, with applications in sensing and quantum information processing. Here, we achieve strong effective photon-photon interactions (Kerr-like optical nonlinearity) via the Rydberg blockade phenomenon and the hybridisation of excitons and photons forming polaritons in a Cu$_2$O-filled microresonators. Under pulsed resonant excitation polariton resonance frequencies are renormalised due to the reduction of the photon-exciton coupling with increasing exciton density. Theoretical analysis shows that the Rydberg blockade plays a major role in the experimentally observed scaling of the polariton nonlinearity coefficient as $\propto n^{4.4 \pm 1.8}$ for principal quantum numbers up to n = 7. Such high principal quantum numbers studied in a polariton system for the first time are essential for realisation of high Rydberg optical nonlinearities, which paves the way towards quantum optical applications and fundamental studies of strongly-correlated photonic (polaritonic) states in a solid state system.
C. E. Whittaker, T. Isoniemi, S. Lovett, P. M. Walker, S. Kolodny, V. Kozin, I. V. Iorsh, I. Farrer, D. A. Ritchie, M. S. Skolnick, D. N. Krizhanovskii We report the observation of band gaps for low loss exciton-polaritons propagating outside the light cone in GaAs-based planar waveguides patterned into two-dimensional photonic crystals. By etching square lattice arrays of shallow holes into the uppermost layer of our structure, we open gaps on the order of 10 meV in the photonic mode dispersion, whose size and light-matter composition can be tuned by proximity to the strongly coupled exciton resonance. We demonstrate gaps ranging from almost fully photonic to highly excitonic. Opening a gap in the exciton-dominated part of the polariton spectrum is a promising first step towards the realization of quantum-Hall-like states arising from topologically nontrivial hybridization of excitons and photons.
We present and experimentally study the effects of the photonic spin-orbit coupling on real space propagetion of polariton wavepackets in planar semiconductor microcavities and polaritonic analogs of graphene. In particular, we demonstrate the appearance of an analog Zitterbewegung effect, a term which translates as 'trembling motion' in english, which was originally proposed for relativistic Dirac electrons and consists of the oscillations of the center of mass of a wavepacket in the direction perpendicular to its propagation. For a planar microcavity we observe regular Zitterbewegung oscillations whose amplitude and period depend on the wavevector of the polaritons. We then extend these results to a honeycomb lattice of coupled microcavity resonators. Compared to the planar cavity such lattices are inherently more tuneable and versatile, allowing simulation of the Hamilitonians of a wide range of important physical systems. We observe an oscillation pattern related to the presence of the spin-split Dirac cones in the dispersion. In both cases the experimentally observed oscillations are in good agreement with theoretical modelling and independently measured bandstructure parameters, providing strong evidence for the observation of Zitterbewegung.
Microcavity polaritons are strongly interacting hybrid light-matter quasiparticles, which are promising for the development of novel light sources and active photonic devices. Here, we report polariton lasing in the UV spectral range in microring resonators based on GaN/AlGaN slab waveguides, with experiments carried out from 4 K up to room temperature. Stimulated polariton relaxation into multiple ring resonator modes is observed, which exhibit threshold-like dependence of the emission intensity with pulse energy. The strong exciton-photon coupling regime is confirmed by the significant reduction of the free spectral range with energy and the blueshift of the exciton-like modes with increasing pulse energy. Importantly, the exciton emission shows no broadening with power, further confirming that lasing is observed at electron-hole densities well below the Mott transition. Overall, our work paves the way towards development of novel UV devices based on the high-speed slab waveguide polariton geometry operating up to room temperature with potential to be integrated into complex photonic circuits.
Quantum states of light and matter can be manipulated on the nanoscale to provide a technological resource for aiding the implementation of scalable photonic quantum technologies [1-3]. Experimental progress relies on the quality and efficiency of the coupling between photons and internal states of quantum emitters [4-6]. Here we demonstrate a nanophotonic waveguide platform with embedded quantum dots (QDs) that enables both Purcell-enhanced emission and strong chiral coupling. The design uses slow-light effects in a glide-plane photonic crystal waveguide with QD tuning to match the emission frequency to the slow-light region. Simulations were used to map the chirality and Purcell enhancement depending on the position of a dipole emitter relative to the air holes. The highest Purcell factors and chirality occur in separate regions, but there is still a significant area where high values of both can be obtained. Based on this, we first demonstrate a record large radiative decay rate of 17 ns^-1 (60 ps lifetime) corresponding to a 20 fold Purcell enhancement. This was achieved by electric-field tuning of the QD to the slow-light region and quasi-resonant phonon-sideband excitation. We then demonstrate a 5 fold Purcell enhancement for a dot with high degree of chiral coupling to waveguide modes, substantially surpassing all previous measurements. Together these demonstrate the excellent prospects for using QDs in scalable implementations of on-chip spin-photonics relying on chiral quantum optics.
The spin of a charged semiconductor quantum dot (QD) coupled to an optical cavity is a promising candidate for high fidelity spin-photon interfaces; the cavity selectively modifies the decay rates of optical transitions such that spin initialisation, manipulation, and readout are all possible in a single magnetic field geometry. By performing cavity QED calculations, we show that a cavity with a single, linearly-polarised mode can simultaneously support both high-fidelity optical spin initialisation and readout in a single, in-plane (Voigt geometry) magnetic field. Furthermore, we demonstrate that single mode cavities always outperform bi-modal cavities in experimentally favourable driving regimes. Our analysis, when combined with established methods of control in a Voigt geometry field, provides optimal parameter regimes for high-fidelity initialisation and readout, and coherent control in both cavity configurations, providing insights for the design and development of QD spin-photon interfaces as the basis of quantum network nodes and for the generation of photonic graph states.
Recently reported large values of exciton-polariton nonlinearity of transition metal dichalcogenide (TMD) monolayers coupled to optically resonant structures approach the values characteristic for GaAs-based systems in the regime of strong light-matter coupling. Contrary to the latter, TMD-based polaritonic devices remain operational at ambient conditions and therefore have greater potential for practical nanophotonic applications. Here we present the study of the nonlinear properties of Ta$_2$O$_5$ slab waveguide coupled to a WSe$_2$ monolayer. We first confirm that the hybridization between waveguide photon mode and a 2D semiconductor exciton resonance gives rise to the formation of exciton-polaritons with Rabi splitting of 36 meV. By measuring transmission of ultrashort optical pulses through this TMD-based polaritonic waveguide, we demonstrate for the first time the strong nonlinear dependence of the output spectrum on the input pulse energy. Our theoretical model provides semi-quantitative agreement with experiment and gives insights into the dominating microscopic processes which determine the nonlinear pulse self-action: Coulomb inter-particle interaction and scattering to incoherent excitonic reservoir. We also confirm that at intermediate pump energies the system supports quasi-stationary solitonic regime of pulse propagation. Our results are essential for the development of nonlinear on-chip polaritonic devices based of 2D semiconductors.
The capacity to devise order metrics for microstructures of multiphase heterogeneous media is a highly challenging task, given the richness of the possible geometries and topologies of the phases that can arise. This investigation initiates a program to formulate order metrics to characterize the degree of order/disorder of the microstructures of two-phase media in $d$-dimensional Euclidean space $\mathbb{R}^d$ across length scales. In particular, we propose the use of the local volume-fraction variance $\sigma^2_{_V}(R)$ associated with a spherical window of radius $R$ as an order metric. We determine $\sigma^2_{_V}(R)$ as a function of $R$ for 22 different models across the first three space dimensions, including both hyperuniform and nonhyperuniform systems with varying degrees of short- and long-range order. We find that the local volume-fraction variance as well as asymptotic coefficients and integral measures derived from it provide reasonably robust and sensitive order metrics to categorize disordered and ordered two-phase media across all length scales.
It is well-known that the degeneracy of two-phase microstructures with the same volume fraction and two-point correlation function $S_2(\mathbf{r})$ is generally infinite. To elucidate the degeneracy problem explicitly, we examine Debye random media, which are entirely defined by a purely exponentially decaying two-point correlation function $S_2(r)$. In this work, we consider three different classes of Debye random media. First, we generate the "most probable" class using the Yeong-Torquato construction algorithm [Yeong and Torquato, Phys. Rev. E, 57, 495 (1998)]. A second class of Debye random media is obtained by demonstrating that the corresponding two-point correlation functions are effectively realized in the first three space dimensions by certain models of overlapping, polydisperse spheres. A third class is obtained by using the Yeong-Torquato algorithm to construct Debye random media that are constrained to have an unusual prescribed pore-size probability density function. We structurally discriminate these three classes of Debye random media from one another by ascertaining their other statistical descriptors, including the pore-size, surface correlation, chord-length probability density, and lineal-path functions. We also compare and contrast the percolation thresholds as well as the diffusion and fluid transport properties of these degenerate Debye random media. We find that these three classes of Debye random media are generally distinguished by the aforementioned descriptors and their microstructures are also visually distinct from one another. Our work further confirms the well-known fact that scattering information is insufficient to determine the effective physical properties of two-phase media. Additionally, our findings demonstrate the importance of the other two-point descriptors considered here in the design of materials with a spectrum of physical properties.
Tintu Kuriakose, Paul M. Walker, Toby Dowling, Oleksandr Kyriienko, Ivan A. Shelykh, Phillipe St-Jean, Nicola Carlon Zambon, Aristide Lemaître, Isabelle Sagnes, Luc Legratiet, Abdelmounaim Harouri, Sylvain Ravets, Maurice S. Skolnick, Alberto Amo, Jacqueline Bloch, Dmitry N. Krizhanovskii Photonic platforms are an excellent setting for quantum technologies because weak photon-environment coupling ensures long coherence times. The second key ingredient for quantum photonics is interactions between photons, which can be provided by optical nonlinearities in the form of cross-phase-modulation (XPM). This approach underpins many proposed applications in quantum optics and information processing, but achieving its potential requires strong single-photon-level nonlinear phase shifts and also scalable nonlinear elements. In this work we show that the required nonlinearity can be provided by exciton-polaritons in micropillars with embedded quantum wells. These combine the strong interactions of excitons with the scalability of micrometer-sized emitters. We observe XPM up to $3 \pm 1$ mrad per particle using laser beams attenuated to below single photon average intensity. With our work serving as a first stepping stone, we lay down a route for quantum information processing in polaritonic lattices.
The concept of gauge fields plays a significant role in many areas of physics from particle physics and cosmology to condensed matter systems, where gauge potentials are a natural consequence of electromagnetic fields acting on charged particles and are of central importance in topological states of matter. Here, we report on the experimental realization of a synthetic non-Abelian gauge field for photons in a honeycomb microcavity lattice. We show that the effective magnetic field associated with TE-TM splitting has the symmetry of Dresselhaus spin-orbit interaction around Dirac points in the dispersion, and can be regarded as an SU(2) gauge field. The symmetry of the field is revealed in the optical spin Hall effect (OSHE), where under resonant excitation of the Dirac points precession of the photon pseudospin around the field direction leads to the formation of two spin domains. Furthermore, we observe that the Dresselhaus field changes its sign in the same Dirac valley on switching from s to p bands in good agreement with the tight binding modelling. Our work demonstrating a non-Abelian gauge field for light on the microscale paves the way towards manipulation of photons via spin on a chip.
Mengyao Li, Ivan Sinev, Fedor Benimetskiy, Tatyana Ivanova, Ekaterina Khestanova, Svetlana Kiriushechkina, Anton Vakulenko, Sriram Guddala, Maurice Skolnick, Vinod Menon, Dmitry Krizhanovskii, Andrea Alù, Anton Samusev, Alexander B. Khanikaev The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. One promising platform to reach such strong light-matter interacting regimes is offered by polaritonic metasurfaces, which represent ultrathin artificial media structured on nano-scale and designed to support polaritons - half-light half-matter quasiparticles. Topological polaritons, or 'topolaritons', offer an ideal platform in this context, with unique properties stemming from topological phases of light strongly coupled with matter. Here we explore polaritonic metasurfaces based on 2D transition metal dichalcogenides (TMDs) supporting in-plane polarized exciton resonances as a promising platform for topological polaritonics. We enable a spin-Hall topolaritonic phase by strongly coupling valley polarized in-plane excitons in a TMD monolayer with a suitably engineered all-dielectric topological photonic metasurface. We first show that the strong coupling between topological photonic bands supported by the metasurface and excitonic bands in MoSe2 yields an effective phase winding and transition to a topolaritonic spin-Hall state. We then experimentally realize this phenomenon and confirm the presence of one-way spin-polarized edge topolaritons. Combined with the valley polarization in a MoSe2 monolayer, the proposed system enables a new approach to engage the photonic angular momentum and valley degree of freedom in TMDs, offering a promising platform for photonic/solid-state interfaces for valleytronics and spintronics.
Davide Maria Di Paola, Paul M. Walker, Ruggero P. A. Emmanuele, Alexey V. Yulin, Joachim Ciers, Zaffar Zaidi, Jean-François Carlin, Nicolas Grandjean, Ivan Shelykh, Maurice S. Skolnick, R. Butté, Dmitry N. Krizhanovskii 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 $\mu$m 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.
V. Kravtsov, A. D. Liubomirov, R. V. Cherbunin, A. Catanzaro, A. Genco, D. Gillard, E. M. Alexeev, T. Ivanova, E. Khestanova, I. A. Shelykh, I. V. Iorsh, A. I. Tartakovskii, M. S. Skolnick, D. N. Krizhanovskii Van der Waals heterobilayers based on 2D transition metal dichalcogenides have been recently shown to support robust and long-lived valley polarization for potential valleytronic applications. However, the role of the band structure and alignment of the constituent layers in the underlying dynamics remains largely unexplored. Here we study spin--valley relaxation dynamics in heterobilayers with different band structures engineered via the use of alloyed monolayer semiconductors. Through a combination of time-resolved Kerr rotation spectroscopic measurements and theoretical modelling for Mo$_{1-x}$W$_{x}$Se$_2$/WSe$_2$ samples with different chemical compositions and stacking angles, we uncover the roles of interlayer exciton recombination and charge carrier spin depolarization in the overall valley dynamics. Our results provide insights into the microscopic spin--valley polarization mechanisms in van der Waals heterostructures for the development of future 2D valleytronic devices.
Spectral filtering of resonance fluorescence is widely employed to improve single photon purity and indistinguishability by removing unwanted backgrounds. For filter bandwidths approaching the emitter linewidth, complex behaviour is predicted due to preferential transmission of components with differing photon statistics. We probe this regime using a Purcell-enhanced quantum dot in both weak and strong excitation limits, finding excellent agreement with an extended sensor theory model. By changing only the filter width, the photon statistics can be transformed between antibunched, bunched, or Poissonian. Our results verify that strong antibunching and a sub-natural linewidth cannot simultaneously be observed, providing new insight into the nature of coherent scattering.
R. P. A. Emmanuele, M. Sich, O. Kyriienko, V. Shahnazaryan, F. Withers, A. Catanzaro, P. M. Walker, F. A. Benimetskiy, M. S. Skolnick, A. I. Tartakovskii, I. A. Shelykh, D. N. Krizhanovskii Highly nonlinear optical materials with strong effective photon-photon interactions (Kerr-like nonlinearity) are required in the development of novel quantum sources of light as well as for ultrafast and quantum optical signal processing circuitry. Here we report very large Kerr-like nonlinearities by employing strong optical transitions of charged excitons (trions) observed in semiconducting transition metal dichalcogenides (TMDCs). By hybridising trions in monolayer MoSe$_2$ at low electron densities with a microcavity mode, we realise trion-polaritons exhibiting significant energy shifts at very small photon fluxes due to phase space filling. Most notably, the strong trion-polariton nonlinearity is found to be 10 to 1000 larger than in other polariton systems, including neutral exciton-polaritons in TMDCs. Furthermore it exceeds by factors of $\sim 10^3-10^5$ the magnitude of Kerr nonlinearity in bare TMDCs, graphene and other widely used optical materials (e.g. Si, AlGaAs etc) in weak light-matter coupling regimes. The results are in good agreement with a theory which accounts for the composite nature of excitons and trions and deviation of their statistics from that of ideal bosons and fermions. This work opens a new highly nonlinear system for quantum optics applications enabling in principle scalability and control through nano-engineering of van der Waals heterostructures.
F. Benimetskiy, V. Sharov, P.A. Alekseev, V. Kravtsov, K. Agapev, I. Sinev, I. Mukhin, A. Catanzaro, R. Polozkov, A. Tartakovskii, A. Samusev, M. S. Skolnick, D. N. Krizhanovskii, I. A. Shelykh, I. Iorsh Strain engineering is a powerful tool for tuning physical properties of 2D materials, including monolayer transition metal dichalcogenides (TMD) -- direct bandgap semiconductors with strong excitonic response. Here, we demonstrate an approach for local characterization of strain-induced modification of excitonic photoluminescence in TMD-based materials. We reversibly stress a monolayer of MoSe$_2$ with an AFM tip and perform spatio-spectral mapping of the excitonic photoluminescence in the vicinity of the indentation point. To fully reproduce the experimental data, we introduce the linear dependence of the exciton energy and corresponding photoluminescence intensity on the induced strain. Careful account for the optical resolution allows extracting these quantities with good agreement with the previous measurements, which involved macroscopic sample deformation. Our approach is a powerful tool for the study of local optomechanical properties of 2D direct bandgap semiconductors with strong excitonic response.
V. Kravtsov, E. Khestanova, F. A. Benimetskiy, T. Ivanova, A. K. Samusev, I. S. Sinev, D. Pidgayko, A. M. Mozharov, I. S. Mukhin, M. S. Lozhkin, Y. V. Kapitonov, A. S. Brichkin, V. D. Kulakovskii, I. A. Shelykh, A. I. Tartakovskii, P. M. Walker, M. S. Skolnick, D. N. Krizhanovskii, I. V. Iorsh Optical bound states in the continuum (BICs) provide a way to engineer very narrow resonances in photonic crystals. The extended interaction time in such systems is particularly promising for enhancement of nonlinear optical processes and development of the next generation of active optical devices. However, the achievable interaction strength is limited by the purely photonic character of optical BICs. Here, we mix optical BIC in a photonic crystal slab with excitons in atomically thin semiconductor MoSe$_2$ to form nonlinear exciton-polaritons with a Rabi splitting of 27~meV, exhibiting large interaction-induced spectral blueshifts. The asymptotic BIC-like suppression of polariton radiation into far-field towards the BIC wavevector, in combination with effective reduction of excitonic disorder through motional narrowing, results in small polariton linewidths below 3~meV. Together with strongly wavevector-dependent Q-factor, this provides for enhancement and control of polariton--polariton interactions and resulting nonlinear optical effects, paving the way towards tunable BIC-based polaritonic devices for sensing, lasing, and nonlinear optics.
Alistair J. Brash, Jake Iles-Smith, Catherine L. Phillips, Dara P. S. McCutcheon, John O'Hara, Edmund Clarke, Benjamin Royall, Jesper Mørk, Maurice S. Skolnick, A. Mark Fox, Ahsan Nazir Coherent scattering of light by a single quantum emitter is a fundamental process at the heart of many proposed quantum technologies. Unlike atomic systems, solid-state emitters couple to their host lattice by phonons. Using a quantum dot in an optical nanocavity, we resolve these interactions in both time and frequency domains, going beyond the atomic picture to develop a comprehensive model of light scattering from solid-state emitters. We find that even in the presence of a cavity, phonon coupling leads to a sideband that is completely insensitive to excitation conditions, and to a non-monotonic relationship between laser detuning and coherent fraction, both major deviations from atom-like behaviour.
We study the effect of photonic spin-orbit coupling (SOC) in micropillar lattices on the topological edge states of a one-dimensional chain with a zigzag geometry, corresponding to the Su-Schrieffer-Heeger model equipped with an additional internal degree of freedom. The system combines the strong hopping anisotropy of the $p$-type pillar modes with the large TE-TM splitting in Bragg microcavities. By resolving the photoluminescence emission in energy and polarization we probe the effects of the resulting SOC on the spatial and spectral properties of the edge modes. We find that the edge modes feature a fine structure of states that penetrate by different amounts into the bulk of the chain, depending on the strength of the SOC terms present, thereby opening a route to manipulation of the topological states in the system.
M. Sich, L. E. Tapia-Rodriguez, H. Sigurdsson, P. M. Walker, E. Clarke, I. A. Shelykh, B. Royall, E. S. Sedov, A. V. Kavokin, D. V. Skryabin, M. S. Skolnick, D. N. Krizhanovskii We report stable orthogonally polarised domains in high-density polariton solitons propagating in a semiconductor microcavity wire. This effect arises from spin dependent polariton-polariton interactions and pump-induced imbalance of polariton spin populations. The interactions result in an effective magnetic field acting on polariton spin across the soliton profile, leading to the formation of polarisation domains. Our experimental findings are in excellent agreement with theoretical modelling taking into account these effects.
We achieve direct detection of electron hyperfine shifts in individual CdTe/ZnTe quantum dots. For the previously inaccessible regime of strong magnetic fields $B_z\gtrsim0.1$ T, we demonstrate robust polarization of a few-hundred-particle nuclear spin bath, with optical initialization time of $\sim$ 1 ms and polarization lifetime exceeding $\sim$ 1 s. Nuclear magnetic resonance spectroscopy of individual dots reveals strong electron-nuclear interactions characterized by the Knight fields $|B_e|\gtrsim50$ 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 quantum registers, combining the excellent optical properties comparable to III-V dots, and the dilute nuclear spin environment similar to group-IV semiconductors.
S. Dufferwiel, T. P. Lyons, D. D. Solnyshkov, A. A. P. Trichet, F. Withers, G. Malpuech, J. M. Smith, K. S. Novoselov, M. S. Skolnick, D. N. Krizhanovskii, A. I. Tartakovskii Two-dimensional transition metal dichalcogenide (TMD) semiconductors provide a unique possibility to access the electronic valley degree of freedom using polarized light, opening the way to valley information transfer between distant systems. Excitons with a well-defined valley index (or valley pseudospin) as well as superpositions of the exciton valley states can be created with light having circular and linear polarization, respectively. However, the generated excitons have short lifetimes (ps) and are also subject to the electron-hole exchange interaction leading to fast relaxation of the valley pseudospin and coherence. Here we show that control of these processes can be gained by embedding a monolayer of WSe$_2$ in an optical microcavity, where part-light-part-matter exciton-polaritons are formed in the strong light-matter coupling regime. We demonstrate the optical initialization of the valley coherent polariton populations, exhibiting luminescence with a linear polarization degree up to 3 times higher than that of the excitons. We further control the evolution of the polariton valley coherence using a Faraday magnetic field to rotate the valley pseudospin by an angle defined by the exciton-cavity-mode detuning, which exceeds the rotation angle in the bare exciton. 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.
Lattice matched GaAs/AlGaAs epitaxial structures with quantum dots are studied under static uniaxial stress applied either along the $[001]$ or $[110]$ crystal directions. We conduct simultaneous measurements of the spectral shifts in the photoluminescence of the bulk GaAs substrate, which relate to strain via deformation potentials $a$ and $b$, and the quadrupolar shifts in the optically detected nuclear magnetic resonance spectra of the quantum dots, which relate to the same strain via the gradient-elastic tensor $S_{ijkl}$. Measurements in two uniaxial stress configurations are used to derive the ratio $b/a=0.241\pm0.008$ in good agreement with previous studies on GaAs. Based on the previously estimated value of $a\approx-8.8$ eV we derive the product of the nuclear quadrupolar moment $Q$ and the $S$-tensor diagonal component in GaAs to be $QS_{11}\approx+0.76\times10^{-6}$ V for $^{75}$As and $QS_{11}\approx-0.37\times10^{-6}$ V for $^{69}$Ga nuclei. In our experiments the signs of $S_{11}$ are directly measurable, which was not possible in the earlier nuclear acoustic resonance studies. Our $QS_{11}$ values are a factor of $\sim$1.4 smaller than those derived from the nuclear acoustic resonance experiments [Phys. Rev. B 10, 4244 (1974)]. The gradient-elastic tensor values measured in this work can be applied in structural analysis of strained III-V semiconductor nanostructures via accurate modelling of their magnetic resonance spectra.
We report strongly non-reciprocal behaviour for quantum dot exciton spins coupled to nano-photonic 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.
M. Sich, J. K. Chana, O. A. Egorov, H. Sigurdsson, I. A. Shelykh, D. V. Skryabin, P. M. Walker, E. Clarke, B. Royall, M. S. Skolnick, D. N. Krizhanovskii We explore nonlinear transitions of polariton wavepackets, first, to a soliton and then to a standing wave polariton condensate in a multi-mode microwire system. At low polariton density we observe ballistic propagation of the multi-mode polariton wavepackets arising from the interference between different transverse modes. With increasing polariton density, the wavepackets transform into single mode bright solitons due to effects of both inter-modal and intra-modal polariton-polariton scattering. Further increase of the excitation density increases thermalisation speed leading to relaxation of the polariton density distribution in momentum space with the resultant formation of a non-equilibrium condensate manifested by a standing wave pattern across the whole sample.
Electron spin qubit coherence in quantum dots is ultimately limited by random nuclear spin bath fluctuations. Here we aim to eliminate this randomness by making spin bath evolution deterministic. We introduce spin bath control sequences, which systematically combine Hahn and solid echoes to suppress inhomogeneous broadening and nuclear-nuclear interactions. Experiments on self-assembled quantum dots show a five-fold increase in nuclear spin coherence. Numerical simulations show that these sequences can be used to suppress decoherence via qubit-qubit interaction in point defect and dopant spin systems.
Local control of the generation and interaction of indistinguishable single photons is a key requirement for photonic quantum networks. Waveguide-based architectures, in which embedded quantum emitters act as both highly coherent single photon sources and as nonlinear elements to mediate photon-photon interactions, offer a scalable route to such networks. However, local electrical control of a quantum optical nonlinearity has yet to be demonstrated in a waveguide geometry. Here, we demonstrate local electrical tuning and switching of single photon generation and nonlinear interaction by embedding a quantum dot in a nano-photonic waveguide with enhanced light-matter interaction. A power-dependent transmission extinction as large as 40$\pm$2% and clear, voltage-controlled bunching in the photon statistics of the transmitted light demonstrate the single photon character of the nonlinearity. The deterministic nature of the nonlinearity is particularly attractive for the future realization of photonic gates for scalable nano-photonic waveguide-based quantum information processing.
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 electro-mechanical 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.
C. E. Whittaker, E. Cancellieri, P. M. Walker, D. R. Gulevich, H. Schomerus, D. Vaitiekus, B. Royall, D. M. Whittaker, E. Clarke, I. V. Iorsh, I. A. Shelykh, M. S. Skolnick, D. N. Krizhanovskii 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 work shows the potential of polariton lattices for emulating flat band Hamiltonians with spin-orbit coupling, orbital degrees of freedom and interactions.
We report on growth and characterization of individual InAsP/GaInP quantum dots with variable nominal As molar fraction. Magneto-photoluminescence experiments reveal QD emission in a wide range from 1.3 to 1.8 eV confirming incorporation of As into quantum dots. Transmission electron microscopy reveals a core-cap structure of InAsP quantum dots with an InAs-rich core capped by an InP-rich layer. Inside the core, an As molar fraction up to x=0.12 is observed. The heavy hole g-factor is found to be strongly dependent on As molar fraction, while the electron g-factor is close to the InP values. This suggests type-II carrier confinement in the studied InAsP dots with holes (electrons) localized in the core (cap) region. Finally, dynamic nuclear polarization is observed which allows for further insight into structural properties using nuclear magnetic resonance.
We study exciton-polariton nonlinear optical fluids in a high momentum regime for the first time. Defects in the fluid develop into dark solitons whose healing length decreases with increasing density. We deduce interaction constants for continuous wave polaritons an order of magnitude larger than with picosecond pulses. Time dependent measurements show a 100ps time for the buildup of the interaction strength suggesting a self-generated excitonic reservoir as the source of the extra nonlinearity. The experimental results agree well with a model of coupled photons, excitons and the reservoir.
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 reaches 99% and beyond, it has been limited to 60-65% 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.
S. Dufferwiel, T. P. Lyons, D. D. Solnyshkov, A. A. P. Trichet, F. Withers, S. Schwarz, G. Malpuech, J. M. Smith, K. S. Novoselov, M. S. Skolnick, D. N. Krizhanovskii, A. I. Tartakovskii While conventional semiconductor technology relies on the manipulation of electrical charge for the implementation of computational logic, additional degrees of freedom such as spin and valley offer alternative avenues for the encoding of information. In transition metal dichalcogenide (TMD) monolayers, where spin-valley locking is present, strong retention of valley chirality has been reported for MoS$_2$, WSe$_2$ and WS$_2$ while MoSe$_2$ shows anomalously low valley polarisation retention. In this work, chiral selectivity of MoSe$_2$ cavity polaritons under helical excitation is reported with a polarisation degree that can be controlled by the exciton-cavity detuning. In contrast to the very low circular polarisation degrees seen in MoSe$_2$ exciton and trion resonances, we observe a significant enhancement of up to 7 times when in the polaritonic regime. Here, polaritons introduce a fast decay mechanism which inhibits full valley pseudospin relaxation and thus allows for increased retention of injected polarisation in the emitted light. A dynamical model applicable to cavity-polaritons in any TMD semiconductor, reproduces the detuning dependence through the incorporation of the cavity-modified exciton relaxation, allowing an estimate of the spin relaxation time in MoSe$_2$ which is an order of magnitude faster than those reported in other TMDs. The valley addressable exciton-polaritons reported here offer robust valley polarised states demonstrating the prospect of valleytronic devices based upon TMDs embedded in photonic structures, with significant potential for valley-dependent nonlinear polariton-polariton interactions.
C. E. Whittaker, B. Dzurnak, O. A. Egorov, G. Buonaiuto, P. M. Walker, E. Cancellieri, D. M. Whittaker, E. Clarke, S. S. Gavrilov, M. S. Skolnick, D. N. Krizhanovskii We report on the formation of a diverse family of transverse spatial polygon patterns in a microcavity polariton fluid under coherent driving by a blue-detuned pump. Patterns emerge spontaneously as a result of energy-degenerate polariton-polariton scattering from the pump state to interfering high order vortex and antivortex modes, breaking azimuthal symmetry. The interplay between a multimode parametric instability and intrinsic optical bistability leads to a sharp spike in the value of second order coherence $g^{(2)}(0)$ of the emitted light, which we attribute to the strongly superlinear kinetics of the underlying scattering processes driving the formation of patterns. We show numerically by means of a linear stability analysis how the growth of parametric instabilities in our system can lead to spontaneous symmetry breaking, predicting the formation and competition of different pattern states in good agreement with experimental observations.
We demonstrate a scheme for in-plane initialization and readout of a single exciton spin in an InGaAs quantum dot (QD) coupled to a GaAs nanobeam waveguide. The chiral coupling of the QD and the optical mode of the nanobeam enables spin initialization and readout fidelity approaching unity in magnetic field $B=1$ T and $\sim$0.9 without the field. We further show that this in-plane excitation scheme is independent of the incident excitation laser polarization and depends solely on the excitation direction. This scheme provides a robust in-plane spin excitation basis for a photon-mediated spin network for quantum information applications.
The orbital angular momentum and the polarisation of light are physical quantities widely investigated for classical and quantum information processing. In this work we propose to take advantage of strong light-matter coupling, circular-symmetric confinement, and transverse-electric transverse-magnetic splitting to exploit states where these two degrees of freedom are combined. To this end we develop a model based on a spin-orbit Poincaré hypersphere. Then we consider the example of semiconductor polariton systems and demonstrate full ultrafast Stark control of spin-orbit states. Moreover, by controlling states on three different spin-orbit spheres and switching from one sphere to another we demonstrate the control of different logic bits within one single physical system.
The electron-phonon coupling in self-assembled InGaAs quantum dots is relatively weak at low light intensities, which means that the zero-phonon line in emission is strong compared to the phonon sideband. However, the coupling to acoustic phonons can be dynamically enhanced in the presence of an intense optical pulse tuned within the phonon sideband. Recent experiments have shown that this dynamic vibronic coupling can enable population inversion to be achieved when pumping with a blue-shifted laser and for rapid de-excitation of an inverted state with red detuning. In this paper we con?rm the incoherent nature of the phonon-assisted pumping process and explore the temperature dependence of the mechanism. We also show that a combination of blue- and red-shifted pulses can create and destroy an exciton within a timescale ~20 ps determined by the pulse duration and ultimately limited by the phonon thermalisation time.
In this work, we demonstrate the on-chip two-photon interference between single photons emitted by a single self-assembled InGaAs quantum dot and an external laser. The quantum dot is embedded within one arm of an air-clad directional coupler which acts as a beam-splitter for incoming light. Photons originating from an attenuated external laser are coupled to the second arm of the beam-splitter and then combined with the quantum dot photons, giving rise to two-photon quantum interference between dissimilar sources. We verify the occurrence of on-chip Hong-Ou-Mandel interference by cross-correlating the optical signal from the separate output ports of the directional coupler. This experimental approach allows us to use classical light source (laser) to assess in a single step the overall device performance in the quantum regime and probe quantum dot photon indistinguishability on application realistic time scales.
We demonstrate ultrafast incoherent depopulation of a quantum dot from above to below the transparency point using LA-phonon-assisted emission stimulated by a redshifted laser pulse. The QD is turned from a weakly vibronic system into a strongly vibronic one by laser driving which enables the phonon-assisted relaxation between the excitonic components of two dressed states. The depopulation is achieved within a laser pulse-width-limited time of 20 ps and exhibits a broad tuning range of a few meV. Our experimental results are well reproduced by path-integral calculations.
Optical solitons are an ideal platform for the implementation of communication lines, since they can be packed extremely close one to another without risking partial loss of the encoded information due to their interaction. On the other hand, soliton-soliton interactions are needed to implement computations and achieve all-optical information processing. Here we study how bright dissipative polariton solitons interact and exploit their interaction to implement AND and OR gates with state of the art technology. Moreover, we show that soliton-soliton interaction can be used to determine the sign of \alpha2, the parameter describing the interaction between polaritons with opposite spin.
GaAs/AlGaAs quantum dots grown by in-situ droplet etching and nanohole infilling offer a combination of strong charge confinement, optical efficiency, and spatial symmetry required for polarization entanglement and spin-photon interface. Here we study spin properties of such dots. We find nearly vanishing electron $g$-factor ($g_e<0.05$), providing a route for electrically driven spin control schemes. Optical manipulation of the nuclear spin environment is demonstrated with nuclear spin polarization up to $60\%$ achieved. NMR spectroscopy reveals the structure of two types of quantum dots and yields the small magnitude of residual strain $\epsilon_b<0.02\%$ which nevertheless leads to long nuclear spin lifetimes exceeding 1000 s. The stability of the nuclear spin environment is advantageous for applications in quantum information processing.
A. M. Waeber, M. Hopkinson, I. Farrer, D. A. Ritchie, J. Nilsson, R. M. Stevenson, A. J. Bennett, A. J. Shields, G. Burkard, A. I. Tartakovskii, M. S. Skolnick, E. A. Chekhovich One of the key challenges in spectroscopy is inhomogeneous broadening that masks the homogeneous spectral lineshape and the underlying coherent dynamics. A variety of techniques including four-wave mixing and spectral hole-burning are used in optical spectroscopy while in nuclear magnetic resonance (NMR) spin-echo is the most common way to counteract inhomogeneity. However, the high-power pulses used in spin-echo and other sequences often create spurious dynamics obscuring the subtle spin correlations that play a crucial role in quantum information applications. Here we develop NMR techniques that allow the correlation times of the fluctuations in a nuclear spin bath of individual quantum dots to be probed. This is achieved with the use of frequency comb excitation which allows the homogeneous NMR lineshapes to be measured avoiding high-power pulses. We find nuclear spin correlation times exceeding 1 s in self-assembled InGaAs quantum dots - four orders of magnitude longer than in strain-free III-V semiconductors. The observed freezing of the nuclear spin fluctuations opens the way for the design of quantum dot spin qubits with a well-understood, highly stable nuclear spin bath.
Scalable quantum technologies require faithful conversion between matter qubits storing the quantum information and photonic qubits carrying the information in integrated circuits and waveguides. We demonstrate that the electromagnetic field chirality which arises in nanophotonic waveguides leads to unidirectional emission from an embedded quantum dot quantum emitter, with resultant in-plane transfer of matter-qubit (spin) information. The chiral behavior 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 measure and compare the phenomena in single mode nanobeam and photonic crystal waveguides. The former is much more tolerant to dot position, exhibits experimental spin-path readout as high as 95 +/- 5% and has potential to serve as the basis of future spin-logic and network implementations.
We demonstrate an on-demand hole spin qubit initialization scheme meeting four key requirements of quantum information processing: fast initialization (1/e ~ 100 ps), high fidelity (F > 99%), long qubit lifetime $(2T_{1}>T_{2}^{*}\simeq10\:\mathrm{ns})$, and compatibility with optical coherent control schemes. This is achieved by rapidly ionizing an exciton in an InGaAs quantum dot with very low fine-structure splitting at zero magnetic field. Furthermore, we show that the hole spin fidelity of an arbitrary quantum dot can be increased by optical Stark effect tuning of the fine-structure splitting close to zero.
S. Dufferwiel, S. Schwarz, F. Withers, A. A. P. Trichet, F. Li, M. Sich, O. Del Pozo-Zamudio, C. Clark, A. Nalitov, D. D. Solnyshkov, G. Malpuech, K. S. Novoselov, J. M. Smith, M. S. Skolnick, D. N. Krizhanovskii, A. I. Tartakovskii Layered materials can be assembled vertically to fabricate a new class of van der Waals (VDW) 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/boron nitride (MoSe$_2$/hBN) quantum wells (QWs) in a tunable optical microcavity. Part-light-part-matter polariton eigenstates are observed as a result of the strong coupling between MoSe$_2$ 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 MoSe$_2$ monolayer QW, enhanced to 29 meV in MoSe$_2$/hBN/MoSe$_2$ double-QWs. 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-QW VDW heterostructures, where polariton condensation and electrical polariton injection through the incorporation of graphene contacts may be realised.
S. Dufferwiel, F. Li, E. Cancellieri, L. Giriunas, A. A. P. Trichet, D. M. Whittaker, P. M. Walker, F. Fras, E. Clarke, J. M. Smith, M. S. Skolnick, D. N. Krizhanovskii We report an extended family of spin textures in coexisting modes of zero-dimensional polariton condensates spatially confined in tunable open microcavity structures. The coupling between photon spin and angular momentum, which is enhanced in the open cavity structures, leads to new eigenstates of the polariton condensates carrying quantised spin vortices. Depending on the strength and anisotropy of the cavity confinement potential and the strength of the spin-orbit coupling, which can be tuned via the excitonic/photonic fractions, the condensate emissions exhibit either spin-vortex-like patterns or linear polarization, in good agreement with theoretical modelling.
We demonstrate an approach to realize the population inversion of a single InGaAs/GaAs quantum dot, which is driven by a laser pulse tuned within the neutral exciton phonon sideband. The inversion is achieved by rapid thermalization of the optically dressed states via phonon-assisted relaxation. A maximum exciton population of 0.67 $\pm$ 0.06 is measured for a laser tuned 0.83 meV to higher energy and the phonon sideband is mapped using a two-color pump-probe technique. Our experiments reveal that, in accordance with theory, the phonon-bath provides additional functionality for an optically driven quantum dot qubit.
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 new platform based on strong light-matter coupling between waveguide photons and quantum-well excitons. On a sub-millimeter length scale we generate sub-picosecond bright temporal solitons at a pulse energy of only 0.5 pico-Joules. From this we deduce an unprecedented nonlinear refractive index 3 orders of magnitude larger than in any other ultrafast system. We study both temporal and spatio-temporal nonlinear effects and for the first time observe dark-bright spatio-temporal 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.
S. Schwarz, S. Dufferwiel, P. M. Walker, F. Withers, A. A. P. Trichet, M. Sich, F. Li, E. A. Chekhovich, D. N. Borisenko, N. N. Kolesnikov, K. S. Novoselov, M. S. Skolnick, J. M Smith, D. N. Krizhanovskii, A. I. Tartakovskii Quasi-two-dimensional (2D) films of layered metal-chalcogenides have attractive optoelectronic properties. However, photonic applications of thin films may be limited owing to weak light absorption and surface effects leading to reduced quantum yield. Integration of 2D films in optical microcavities will permit these limitations to be overcome owing to modified light coupling with the films. Here we present tunable microcavities with embedded monolayer MoS2 or few monolayer GaSe films. We observe significant modification of spectral and temporal properties of photoluminescence (PL): PL is emitted in spectrally narrow and wavelength-tunable cavity modes with quality factors up to 7400; PL life-time shortening by a factor of 10 is achieved, a consequence of Purcell enhancement of the spontaneous emission rate. This work has potential to pave the way to microcavity-enhanced light-emitting devices based on layered 2D materials and their heterostructures, and also opens possibilities for cavity QED in a new material system of van der Waals crystals.
J. K. Chana, M. Sich, F. Fras, A. V. Gorbach, D. V. Skryabin, E. Cancellieri, E. A. Cerda-Méndez, K. Biermann, R. Hey, P. V. Santos, M. S. Skolnick, D. N. Krizhanovskii Semiconductor microcavities operating in the polaritonic regime are highly non-linear, high speed systems due to the unique half-light, half-matter nature of polaritons. Here, we report for the first time the observation of propagating multi-soliton polariton patterns consisting of multi-peak structures either along (x) or perpendicular to (y) the direction of propagation. Soliton arrays of up to 5 solitons are observed, with the number of solitons controlled by the size or power of the triggering laser pulse. The break-up along the x direction occurs due to interplay of bistability, negative effective mass and polariton-polariton scattering, while in the y direction the break-up results from nonlinear phase-dependent interactions of propagating fronts. We show the experimental results are in good agreement with numerical modelling. Our observations are a step towards ultrafast all-optical signal processing using sequences of solitons as bits of information.
Advances in nanotechnology provide techniques for the realisation of integrated quantum-optical circuits for on-chip quantum information processing(QIP). The indistinguishable single photons, required for such devices can be generated by parametric down-conversion, or from quantum emitters such as colour centres and quantum dots(QDs). Among these, semiconductor QDs offer distinctive capabilities including on-demand operation, coherent control, frequency tuning and compatibility with semiconductor nanotechnology. Moreover, the coherence of QD photons can be significantly enhanced in resonance fluorescence(RF) approaching at its best the coherence of the excitation laser. However, the implementation of QD RF in scalable on-chip geometries remains challenging due to the need to suppress stray laser photons. Here we report on-chip QD RF coupled into a single-mode waveguide with negligible resonant laser background and show that the coherence is enhanced compared to off-resonant excitation. The results pave the way to a novel class of integrated quantum-optical devices for on-chip QIP with embedded resonantly-driven quantum emitters.
S. Dufferwiel, F. Fras, A. Trichet, P. M. Walker, F. Li, L. Giriunas, M. N. Makhonin, L. R. Wilson, J. M. Smith, E. Clarke, M. S. Skolnick, D. N. Krizhanovskii We present a method to implement 3-dimensional polariton confinement with in-situ spectral tuning of the cavity mode. Our tunable microcavity is a hybrid system consisting of a bottom semiconductor distributed Bragg reflector (DBR) with a cavity containing quantum wells (QWs) grown on top and a dielectric concave DBR separated by a micrometer sized gap. Nanopositioners allow independent positioning of the two mirrors and the cavity mode energy can be tuned by controlling the distance between them. When close to resonance we observe a characteristic anticrossing between the cavity modes and the QW exciton demonstrating strong coupling. For the smallest radii of curvature concave mirrors of 5.6 $\mu$m and 7.5 $\mu$m real-space polariton imaging reveals submicron polariton confinement due to the hemispherical cavity geometry.
Decoherence in quantum logic gates (qubits) due to interaction with the surrounding environment is a major obstacle to the practical realization of quantum information technologies. For solid state electron-spin qubits the interaction with nuclear spins is the main problem. One particular, neradicable source of electron decoherence arises from decoherence of the nuclear spin bath, driven by nuclear-nuclear dipolar interactions. Due to its many-body nature nuclear decoherence is difficult to predict, especially for an important class of strained nanostructures where nuclear quadrupolar effects have a significant but largely unknown impact. Here we report direct measurement of nuclear spin bath coherence in individual strained InGaAs/GaAs quantum dots: nuclear spin-echo coherence times in the range T2~1.2 - 4.5 ms are found. Based on these T2 values we demonstrate that quadrupolar interactions make nuclear fluctuations in strained quantum dots much slower compared to lattice matched GaAs/AlGaAs structures. Such fluctuation suppression is particularly strong for arsenic nuclei due to the effect of atomic disorder of gallium and indium alloying. Our findings demonstrate that quadrupolar effects can help to solve the long-standing challenge of designing a scalable hardware for quantum computation: III-V semiconductor spin-qubits can be engineered to have a noise-free nuclear spin bath (previously achievable only in nuclear spin-0 semiconductors, where qubit network interconnection and scaling is challenging).
We report an ultrafast optical tuning of the reflectivity of AlGaAs/InAlGaAs multiple quantum well photonic crystal waveguides using a reflection geometry, pump-probe technique.
D. O. Kundys, P. Murzyn, J.P. R. Wells, A. I. Tartakovskii, M. S. Skolnick, Le Si Dang, E. V. Lutsenko, N. P. Tarasuk, O. G. Lyublinskaya, A. A. Toropov, S. V. Ivanov We have used the variable stripe technique and pump-probe spectroscopy to investigate both gain and the dynamics of amplified spontaneous emission from CdSe quantum dot structures. We have found modal gain coefficients of 75 and 32 1/cm for asymmetric and symmetric waveguide structures, respectively. Amplified spontaneous emission decay times of 150 and 300 ps and carrier capture times of 15 and 40 ps were measured for the structures with high and low material gains respectively. The difference in the capture times are related to the fact that for the symmetric waveguide, carriers diffuse into the active region from the uppermost ZnMgSSe cladding layer, yielding a longer rise time for the pump-probe signals for this sample.
We report on two pulse, degenerate four wave mixing (DFWM) measurements on shallow InGaN/GaN multi-quantum wells (MQWs) grown on sapphire substrates. These reveal pulse length limited signal decays. We have found a 10:1 resonant enhancement of the DFWM signal at the excitonic transition frequencies which thereby give a sharp discrimination of the discrete excitonic contributions within the featureless distribution seen in absorption spectra. The exciton resonances have peak positions, which yield good overall agreement with a full k.P model calculation for the quantum well energy levels and optical transition matrix elements. InGaN/GaN MQWs generally exhibit strongly inhomogeneously broadened excitation spectra due to indium fluctuation effects; this approach therefore affords a practical method to extract information on the excited excitonic states not available previously
We study experimentally the dependence of dynamic nuclear spin polarization on the power of non-resonant optical excitation in two types of individual neutral semiconductor quantum dots: InGaAs/GaAs and GaAs/AlGaAs. We show that the mechanism of nuclear spin pumping via second order recombination of optically forbidden (''dark'') exciton states recently reported in InP/GaInP quantum dots [Phys. Rev. B 83, 125318 (2011)] is relevant for material systems considered in this work. In the InGaAs/GaAs dots this nuclear spin polarization mechanism is particularly pronounced, resulting in Overhauser shifts up to ~80 micro-eV achieved at optical excitation power ~1000 times smaller than the power required to saturate ground state excitons. The Overhauser shifts observed at low-power optical pumping in the interface GaAs/AlGaAs dots are generally found to be smaller (up to ~40 micro-eV). Furthermore in GaAs/AlGaAs we observe dot-to-dot variation and even sign reversal of the Overhauser shift which is attributed to dark-bright exciton mixing originating from electron-hole exchange interaction in dots with reduced symmetry. Nuclear spin polarization degrees reported in this work under ultra-low power optical pumping are comparable to those achieved by techniques such as resonant optical pumping or above-gap pumping with high power circularly polarized light. Dynamic nuclear polarization via second-order recombination of ''dark'' excitons may become a useful tool in single quantum dot applications, where manipulation of the nuclear spin environment or electron spin is required.
We demonstrate coherent control of a quantum dot exciton using photocurrent detection with a sinusoidal reverse bias. Optical control is performed at low bias, where tunneling-limited coherence times are long. Following this step, the tunneling rates are increased to remove the long-lived hole, achieving a high photocurrent signal. For a detection efficiency of 68%, electron and hole tunneling times during optical control of 200 ps and 20 ns can be achieved, compared to 120 ps and 7 ns for the constant bias case, respectively.
D. N. Krizhanovskii, E. A. Cerda, S. S. Gavrilov, D. Sarkar, K. Guda, R. Bradley, P. V. Santos, R. Hey, K. Biermann, M. Sich, F. Fras, M. S. Skolnick Polariton condensates are investigated in periodical potentials created by surface acoustic waves using both resonant and non-resonant optical excitation. Under resonant pumping condensates are formed due to polariton parametric scattering from the pump. In this case the single particle dispersion in the presence of the condensate shows a strong reduction of the energy gap arising from the acoustic modulation, indicating efficient screening of the surface acoustic wave potential by spatial modulation of the polariton density. The observed results are in good agreement with a model based on generalised Gross-Pitaveskii equations with account taken of the spatial dependence of the exciton energy landscape. In the case of incoherent, non-resonant pumping coexisting non-equilibrium condensates with s- and p- type wavefunctions are observed, which have different energies, symmetry and spatial coherence. The energy splitting between these condensate states is also reduced with respect to the gap of the one particle spectrum below threshold, but the screening effect is less pronounced than in the case of resonantly pumped system due to weaker modulation of the pump state.
Isaac J. Luxmoore, Romain Toro, Osvaldo Del Pozo-Zamudio, Nicholas A. Wasley, Evgeny A. Chekhovich, Ana M. Sanchez, Richard Beanland, A. Mark Fox, Maurice S. Skolnick, Huiyun Y. Liu, Alexander I. Tartakovskii Non-classical light sources offer a myriad of possibilities in fundamental science and applications including quantum cryptography and quantum lithography. Single photons can encode quantum information and multi-qubit gates in silica waveguide circuits have been used to demonstrate linear optical quantum computing. Scale-up requires miniaturisation of the waveguide circuit and multiple photon sources. Silicon photonics, driven by the incentive of optical interconnects, is a highly promising platform for the passive components, but integrated light sources are limited by silicon's indirect band-gap. III-V semiconductor quantum-dots, on the other hand, are proven quantum emitters. Here we demonstrate single-photon emission from quantum-dots coupled to photonic crystal nanocavities fabricated from III-V material grown directly on silicon substrates. The high quality of the III-V material and photonic structures is emphasized by observation of the strong-coupling regime. This work opens-up the advantages of silicon photonics to the integration and scale-up of solid-state quantum optical systems.
O. D. D. Couto Jr, D. Sercombe, J. Puebla, L. Otubo, I. J. Luxmoore, M. Sich, T. J. Elliott, E. A. Chekhovich, L. R. Wilson, M. S. Skolnick, H. Y. Liu, A. I. Tartakovskii We realize growth of self-catalyzed core-shell GaAs/GaAsP nanowires (NWs) on Si substrates using molecular-beam epitaxy. Transmission electron microscopy (TEM) of single GaAs/GaAsP NWs confirms their high crystal quality and shows domination of the zinc-blende phase. This is further confirmed in optics of single NWs, studied using cw and time-resolved photoluminescence (PL). A detailed comparison with uncapped GaAs NWs emphasizes the effect of the GaAsP capping in suppressing the non-radiative surface states: significant PL enhancement in the core-shell structures exceeding 2000 times at 10K is observed; in uncapped NWs PL is quenched at 60K whereas single core-shell GaAs/GaAsP NWs exhibit bright emission even at room temperature. From analysis of the PL temperature dependence in both types of NW we are able to determine the main carrier escape mechanisms leading to the PL quench.
A scalable optical quantum information processor is likely to be a waveguide circuit with integrated sources, detectors, and either deterministic quantum-logic or quantum memory elements. With microsecond coherence times, ultrafast coherent control, and lifetime-limited transitions, semiconductor quantum-dot spins are a natural choice for the static qubits. However their integration with flying photonic qubits requires an on-chip spin-photon interface, which presents a fundamental problem: the spin-state is measured and controlled via circularly-polarised photons, but waveguides support only linear polarisation. We demonstrate here a solution based on two orthogonal photonic nanowires, in which the spin-state is mapped to a path-encoded photon, thus providing a blue-print for a scalable spin-photon network. Furthermore, for some devices we observe that the circular polarisation state is directly mapped to orthogonal nanowires. This result, which is physically surprising for a non-chiral structure, is shown to be related to the nano-positioning of the quantum-dot with respect to the photonic circuit.
The preparation of a coherent heavy-hole spin via ionization of a spin-polarized electron-hole pair in an InAs/GaAs quantum dot in a Voigt geometry magnetic field is investigated. For a dot with a 17 ueV bright-exciton fine-structure splitting, the fidelity of the spin preparation is limited to 0.75, with optimum preparation occurring when the effective fine-structure of the bright-exciton matches the in-plane hole Zeeman energy. In principle, higher fidelities can be achieved by minimizing the bright-exciton fine-structure splitting.
Much new solid state technology for single-photon sources, detectors, photovoltaics and quantum computation relies on the fabrication of strained semiconductor nanostructures. Successful development of these devices depends strongly on techniques allowing structural analysis on the nanometer scale. However, commonly used microscopy methods are destructive, leading to the loss of the important link between the obtained structural information and the electronic and optical properties of the device. Alternative non-invasive techniques such as optically detected nuclear magnetic resonance (ODNMR) so far proved difficult in semiconductor nano-structures due to significant strain-induced quadrupole broadening of the NMR spectra. Here, we develop new high sensitivity techniques that move ODNMR to a new regime, allowing high resolution spectroscopy of as few as 100000 quadrupole nuclear spins. By applying these techniques to individual strained self-assembled quantum dots, we measure strain distribution and chemical composition in the volume occupied by the confined electron. Furthermore, strain-induced spectral broadening is found to lead to suppression of nuclear spin magnetization fluctuations thus extending spin coherence times. The new ODNMR methods have potential to be applied for non-invasive investigations of a wide range of materials beyond single nano-structures, as well as address the task of understanding and control of nuclear spins on the nanoscale, one of the central problems in quantum information processing.
Microcavity polaritons are composite half-light half-matter quasi-particles, which have recently been demonstrated to exhibit rich physical properties, such as non-equilibrium Bose-Einstein condensation, parametric scattering and superfluidity. At the same time, polaritons have some important advantages over photons for information processing applications, since their excitonic component leads to weaker diffraction and stronger inter-particle interactions, implying, respectively, tighter localization and lower powers for nonlinear functionality. Here we present the first experimental observations of bright polariton solitons in a strongly coupled semiconductor microcavity. The polariton solitons are shown to be non-diffracting high density wavepackets, that are strongly localised in real space with a corresponding broad spectrum in momentum space. Unlike solitons known in other matter-wave systems such as Bose condensed ultracold atomic gases, they are non-equilibrium and rely on a balance between losses and external pumping. Microcavity polariton solitons are excited on picosecond timescales, and thus have significant benefits for ultrafast switching and transfer of information over their light only counterparts, semiconductor cavity lasers (VCSELs), which have only nanosecond response time.
Decoherence caused by nuclear field fluctuations is a fundamental obstacle to the realization of quantum information processing using single electron spins. Alternative proposals have been made to use spin qubits based on valence band holes having weaker hyperfine coupling. However, it was demonstrated recently both theoretically and experimentally that the hole hyperfine interaction is not negligible, although a consistent picture of the mechanism controlling the magnitude of the hole-nuclear coupling is still lacking. Here we address this problem by performing isotope selective measurement of the valence band hyperfine coupling in InGaAs/GaAs, InP/GaInP and GaAs/AlGaAs quantum dots. Contrary to existing models we find that the hole hyperfine constant along the growth direction of the structure (normalized by the electron hyperfine constant) has opposite signs for different isotopes and ranges from -15% to +15%. We attribute such changes in hole hyperfine constants to the competing positive contributions of p-symmetry atomic orbitals and the negative contributions of d-orbitals. Furthermore, we find that the d-symmetry contribution leads to a new mechanism for hole-nuclear spin flips which may play an important role in hole spin decoherence. In addition the measured hyperfine constants enable a fundamentally new approach for verification of the computed Bloch wavefunctions in the vicinity of nuclei in semiconductor nanostructures.
We demonstrate control by applied electric fi?eld of the charge states in single self-assembled InP quantum dots placed in GaInP Schottky structures grown by metalorganic vapor phase epitaxy. This has been enabled by growth optimization leading to suppression of formation of large dots uncontrollably accumulating charge. Using bias- and polarization-dependent micro-photoluminescence, we identify the exciton multi-particle states and carry out a systematic study of the neutral exciton state dipole moment and polarizability. This analysis allows for the characterization of the exciton wavefunction properties at the single dot level for this type of quantum dots. Photocurrent measurements allow further characterization of exciton properties by electrical means, opening new possibilities for resonant excitation studies for such system.