A detailed understanding of strong matter-photon interactions requires first-principle methods that can solve the fundamental Pauli-Fierz Hamiltonian of non-relativistic quantum electrodynamics efficiently. A possible way to extend well-established electronic-structure methods to this situation is to embed the Pauli-Fierz Hamiltonian in a higher-dimensional light-matter hybrid auxiliary configuration space. In this work we show the importance of the resulting hybrid Fermi-Bose statistics of the polaritons, which are the new fundamental particles of the ``photon-dressed'' Pauli-Fierz Hamiltonian for systems in cavities. We show that violations of these statistics can lead to unphysical results. We present an efficient way to ensure the proper symmetry of the underlying wave functions by enforcing representability conditions on the dressed one-body reduced density matrix. We further present a general prescription how to extend a given first-principles approach to polaritons and as an example introduce polaritonic Hartree-Fock theory. While being a single-reference method in polariton space, polaritonic Hartree-Fock is a multi-reference method in the electronic space, i.e. it describes electronic correlations. We also discuss possible applications to polaritonic QEDFT. We apply this theory to a lattice model and find that the more delocalized the bound-state wave function of the particles is, the stronger it reacts to photons. The main reason is that within a small energy range many states with different electronic configurations are available as opposed to a strongly bound (and hence energetically separated) ground-state wave function. This indicates that under certain conditions coupling to the quantum vacuum of a cavity can indeed modify ground state properties.
The elementary optical excitations of a two-dimensional electron system strongly coupled to a microcavity are trion-polaritons. Using a variational approach, we demonstrate that the competition between Coulomb interaction and light-matter coupling plays a crucial role in determining the lowest-energy orbital and spin properties of trion-polaritons. When the light-matter interaction exceeds the bare trion binding, singlet and triplet trion states are mixed due to a cavity-mediated spin-orbit effect, which in turn results in a strong increase of the outer electron Bohr radius. In this strong cav…
We report the experimental investigation and theoretical modeling of a rotating polariton superfluid relying on an innovative method for the injection of angular momentum. This novel, multi-pump injection method uses four coherent lasers arranged in a square, resonantly creating four polariton populations propagating inwards. The control available over the direction of propagation of the superflows allows injecting a controllable non-quantized amount of optical angular momentum. When the density at the center is low enough to neglect polariton-polariton interactions, optical singularities, ass…
Using a high-quality GaAs planar microcavity, we optically generate polariton pairs, and verify their correlations by means of time-resolved single-photon detection. We find that correlations between the different modes are consistently lower than identical mode correlations, which is attributed to the presence of uncorrelated background. We discuss a model to quantify the effects of such a background on the observed correlations. Using spectral and temporal filtering, the background can be suppressed and a change in photon statistics towards non-classical correlations is observed. These resul…
The use of a Kerr nonlinearity to generate squeezed light is a well-known way to surpass the quantum noise limit along a given field quadrature. Nevertheless, in the most common regime of weak nonlinearity, a single Kerr resonator is unable to provide the proper interrelation between the field amplitude and squeezing required to induce a sizable deviation from Poissonian statistics. We demonstrate experimentally that weakly coupled bosonic modes allow exploration of the interplay between squeezing and displacement, which can give rise to strong deviations from the Poissonian statistics. In par…
We study a hybrid semiconductor-optomechanical system, which consists of a cavity with an oscillating mirror made by semiconducting materials or with a semiconducting membrane inside. The cavity photons and the excitons in the oscillating mirror or semiconducting membrane form into polaritons. And correspondingly, the optomechanical interaction between the cavity photons and the mirror or membrane is changed into the polariton-mechanical interaction. We theoretically study the eigenenergies and eigenfunctions of this tripartite hybrid system with the generalized rotating-wave approximation. We…
Controlling the quantum field statistics of confined light is a long-standing goal in integrated photonics. We show that by coupling molecular vibrations with a confined mid-infrared cavity vacuum, the photocount and quadrature field statistics of the cavity field can be reversibly manipulated over sub-picosecond timescales. The mechanism involves changing the cavity resonance frequency through a modulation of the dielectric response of the cavity materials using femtosecond UV pulses. For a single anharmonic molecular vibration in an infrared cavity under ultrastrong coupling conditions, the …
We study a 2D system of trion-polaritons at the quantum level and demonstrate that for monolayer semiconductors they can exhibit a strongly nonlinear optical response. The effect is due to the composite nature of trion-based excitations resulting in their nontrivial quantum statistical properties, and enhanced phase space filling effects. We present the full quantum theory to describe the statistics of trion-polaritons, and demonstrate that the associated nonlinearity persists at the level of few quanta, where two qualitatively different regimes of photon antibunching are present for weak and …
Recently, the creation of photonic Landau levels in a twisted cavity has been demonstrated in Nature \textbf{534}, 671 (2016). Here we propose a scheme to adiabatically transfer flux quanta in multiples of $3\hbar$ simultaneously to all cavity photons by coupling the photons through flux-threaded cones present in such cavity setup. The flux transfer is achieved using external light fields with orbital angular momentum and a near-resonant dense atomic medium as mediator. Furthermore, coupling the cavity fields to a Rydberg state in a configuration supporting electromagnetically induced transpar…
A full quantum theory beyond the mean-field regime is developed for an exciton polariton condensate, to gain a complete understanding of quantum fluctuations. We find analytical solution for the polariton density matrix, showing the polariton nonlinearity causing fast relaxation correlated with the pump so as to yield the condensation at threshold. Increasing the pump intensity, a nonequilibrium phase transition towards the condensation of lower polaritons emerges, with a statistics transiting from a thermal, through a super-Poissonian and to a nonclassical distribution beyond the understandin…
Modeling the Quantum Photon Statistics in Hybrid Light-Matter Integrated Circuits
Hewlett Packard Labs（惠普实验室）；Institute of Nanotechnology, National Research Council（国家研究委员会纳米技术研究所）；Institute of Semiconductor and Solid State Physics, Johannes Kepler University（约翰内斯开普勒大学半导体与固态物理研究所）
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 …
We present a new method to study the semiclassical dynamics of the Jaynes-Cummings dimer model, describing two coupled cavities each containing a two-level system (qubit). We develop a Fock space WKB approach in the polariton basis where each site is treated exactly while the intersite polariton hopping is treated semiclassically. We show that the self-trapped states can be viewed as Fock space localized states. We find that this picture yields the correct critical value of interaction strength at which the delocalization-localization transition occurs. Moreover, the validity of our WKB approa…
Light propagating in a nondispersive medium is accompanied by a mass density wave (MDW) of atoms set in motion by the optical force of the field itself [Phys. Rev. A 95, 063850 (2017)]. This recent result is in strong contrast with the approximation of fixed atoms, which assumes that atoms are fixed to their equilibrium positions when light propagates in a medium and which is deeply rooted in the conventional electrodynamics of continuous media. In many photonic materials, the atoms carry the majority of the total momentum of light and their motion also gives rise to net transfer of medium mas…
The first exact quantum simulation of a real molecular system (HD$^+$) under strong ro-vibrational coupling to a quantized optical cavity mode in thermal equilibrium is presented. Theoretical challenges in describing strongly coupled systems of mixed quantum statistics (Bosons and Fermions) are discussed and circumvented by the specific choice of our molecular system. Our exact simulations reveal the absence of a zero temperature for the strongly coupled matter and light subsystems, due to cavity induced non-equilibrium conditions. Furthermore, we explore the temperature dependency of light-ma…
Motivated by the experiment [St-Jean {\it et al}., Nature Photon. {\bf 11}, 651 (2017)] on topological phases with collective photon modes in a zigzag chain of polariton micropillars, we study spinless $p$-orbital fermions with local interorbital hoppings and repulsive interactions between $p_x$ and $p_y$ bands in zigzag optical lattices. We show that spinless $p$-band fermions in zigzag optical lattices can mimic the interacting Su-Schrieffer-Heeger model and the effective transverse field Ising model in the presence of local hoppings. We analytically and numerically discuss the ground-state …
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…
Recent experimental progress in the field of cavity quantum electrodynamics allows to study the regime of strong interaction between quantized light and complex matter systems. Due to the coherent coupling between photons and matter-degrees of freedom, polaritons -- hybrid light-matter quasiparticles -- emerge, which can significantly influence matter properties and complex processes such as chemical reactions (strong coupling). In this thesis we propose a way to overcome these problems by reformulating the coupled electron-photon problem in an exact way in a different, purpose-build Hilbert s…
We study the photon statistics of weak coherent pulses propagating through a cold Rydberg atomic ensemble in the regime of Rydberg electromagnetically induced transparency. We show experimentally that the value of the second-order autocorrelation function of the transmitted light strongly depends on the position within the pulse and heavily varies during the transients of the pulse. In particular, we show that the falling edge of the transmitted pulse displays much lower values than the rest of the pulse. We derive a theoretical model that quantitatively predicts our results and explains the p…
On-chip photon sources carrying orbital angular momentum (OAM) are in demand for high-capacity optical information processing in both classical and quantum regimes. However, currently-exploited integrated OAM sources have been primarily limited to the classical regime. Herein, we demonstrate a room-temperature on-chip integrated OAM source that emits well-collimated single photons, with a single-photon purity of g(2)(0) = 0.22, carrying entangled spin and orbital angular momentum states and forming two spatially separated entangled radiation channels with different polarization properties. The…
