Phonon damping is the main source of pure dephasing in the solid state, limiting many fundamental quantum effects to low temperature observations. Here we show how excitons in semiconductors can be totally decoupled from the phonon bath, even at room temperature, thanks to their strong interaction with photons. To do so, we investigated ZnO microwires, a new semiconductor nanostructure made of large band-gap material where the light can be trapped and guided into whispering gallery modes. In this system, the very large coupling regime between exciton and photon results in unusual exciton-polariton of one-dimensional character and Rabi splitting as large as 300meV. We find that polariton modes of excitonic fraction up to 75% exhibit no thermal broadening up to room temperature. We show that this remarkable behavior is due to the very large Rabi splitting as compared to the LO phonon energy.
We demonstrate edge-emitting exciton-polariton (polariton) lasing from 5 to 300 K and amplification of non-radiative guided polariton modes within ZnO waveguides. The mode dispersion below and above the lasing threshold is directly measured using gratings present on top of the sample, fully demonstrating the polaritonic nature of the lasing modes. The threshold is found to be similar to that of radiative polarions in planar ZnO microcavities. These results open broad perspectives for guided polaritonics by allowing an easier and more straightforward implementation of polariton integrated circu…
A cavity-polariton, formed due to the strong coupling between exciton and cavity mode, is one of the most promising composite bosons for realizing macroscopic spontaneous coherence at high temperature. Up to date, most of polariton quantum degeneracy experiments were conducted in the complicated two-dimensional (2D) planar microcavities. The role of dimensionality in coherent quantum degeneracy of a composite bosonic system of exciton polaritons remains mysterious. Here we report the first experimental observation of a one-dimensional (1D) polariton condensate in a ZnO microwire at room temper…
We propose a scheme of an optical amplifier based on GaN and ZnO waveguides operating in the regime of strong coupling between photonic modes and excitonic resonances. Amplification of the guided exciton-polaritons is obtained by stimulated scattering from the excitonic reservoir, which is found to be fast enough compared with the large velocity of the guided polariton modes. We analyze the device parameters at different temperatures. We find that an 80 $μ$m-long amplifier can provide a gain of 10dB at room temperature, being supplied by 5 mA current in the $cw$ regime.
We report direct observation of the strong exciton-photon coupling in ZnO tapered whispering gallery (WG) microcavity at room temperature. By scanning excitations along the tapered arm of ZnO tetrapod using micro-photoluminescence spectrometer with different polarizations, we observed a transition from the pure WG optical modes in the weak interaction regime to the excitonic polariton in the strong coupling regime. The experimental observations are well described by using the plane wave model including excitonic polariton dispersion relation. This provides a direct mapping of the polariton dis…
A new platform for fabricating polariton lasers operating at room temperature is introduced: nitride-based distributed Bragg reflectors epitaxially grown on patterned silicon substrates. The patterning allows for an enhanced strain relaxation thereby enabling to stack a large number of crack-free AlN/AlGaN pairs and achieve cavity quality factors of several thousands with a large spatial homogeneity. GaN and ZnO active regions are epitaxially grown thereon and the cavities are completed with top dielectric Bragg reflectors. The two structures display strong-coupling and polariton lasing at roo…
The formation and propagation of a polariton condensate under tightly focused excitation is investigated in a ZnO microcavity both experimentally and theoretically. 2D near-field and far-field images of the condensate are measured under quasi-continuous non-resonant excitation. The corresponding spatial profiles are compared to a model based on the Gross-Pitaevskii equation under cylindrical geometry. This work allows to connect the experiments performed with a small excitation laser spot and the previous kinetic models of condensation in a 2D infinite microcavity, and to determine the relevan…
A laser threshold is determined by the gain condition, which has been progressively reduced by the use of heterostructures and of quantum confinement. The polariton laser is the ultimate step of this evolution: coherent emission is obtained from the spontaneous decay of an exciton-polariton condensate, without the achievement of any gain condition. ZnO, with its unique excitonic properties, is the best choice for a blue/UV-emitting polariton laser device. We report on the fabrication of a new family of fully hybrid microcavities that combine the best-quality ZnO material available (bulk substr…
We implement externally excited ZnO Mie resonators in a framework of a generalized Hubbard Hamiltonian to investigate the lifetimes of excitons and exciton-polaritons out of thermodynamical equilibrium. Our results are derived by a Floquet-Keldysh-Green's formalism with Dynamical Mean Field Theory (DMFT) and a second order iterative perturbation theory solver (IPT). We find that the Fano resonance which originates from coupling of the continuum of electronic density of states to the semiconductor Mie resonator yields polaritons with lifetimes between 0.6 ps and 1.45 ps. These results are compa…
We present a high quality two-dimensional cavity structure based on ZnO nanowires coated with concentrical Bragg reflectors. The spatial mode distribution leads to the simultaneous appearance of the weak and strong coupling regime even at room temperature. Photoluminescence measurements agree with FDTD simulations. Furthermore the ZnO core nanowires allow for the observation of middle polariton branches between the A- and B-exciton ground state resonances. Further, lasing emission up to room temperature is detected in excitation dependent photoluminescence measurements.
We theoretically study the transport of exciton polaritons under different applied photon potentials. The relation between the photon potentials and the thickness of the cavity layer is calculated by the finite element simulation. The theoretical analysis and numerical calculation indicate that the cavity photon potential is proportional to the thickness of the cavity layer with the coefficient being about $1.8$ meV/nm. Further, the periodic and linear photon potentials are considered to control the transport of the exciton polaritons in weak- and strong-field pump situations. In both situatio…
We present indications, that the wave function-stiffness condition during energy-relaxation as observed in single-phase state quantum systems manifests also in a single particle ensemble. This is demonstrated for exciton-polaritons in the strong coupling regime in a ZnO-based microcavity at T = 10 K for non-resonant excitation. It is well known that the pump-induced spatially inhomogeneous background potential leads to nearly equally spaced energy levels in the k-space distribution for propagating polariton Bose-Einstein condensates. Surprisingly this particular pattern is also observable for …
Based on the semiclassical model Hamiltonian of the surface plasmon polariton and the nonequilibrium Green-function approach, we present a microscopic kinetic theory to study the influence of the electron scattering on the dynamics of the surface plasmon polariton in semiconductor nanowires. The damping of the surface plasmon polariton originates from the resonant absorption by the electrons (Landau damping), and the corresponding damping exhibits size-dependent oscillations and distinct temperature dependence without any scattering. The scattering influences the damping by introducing a broad…
Using femtosecond pump-probe spectroscopy, we identify excitation induced dephasing as a major mechanism responsible for the breaking of the strong-coupling between excitons and photons in a semiconductor microcavity. The effects of dephasing are observed on the transmitted probe pulse spectrum as a density dependent broadening of the exciton-polariton resonances and the emergence of a third resonance at high excitation density. A striking asymmetry in the energy shift between the upper and the lower polaritons is also evidenced. Using the excitonic Bloch equations, we quantify the respective …
Electronic resonances can significantly enhance the photon-phonon coupling in cavity optomechanics, but are normally avoided due to absorption losses and dephasing by inhomogeneous broadening. We experimentally demonstrate that exciton-polaritons in semiconductor microcavities enable GHz optomechanics with single-particle resonant couplings reaching record values in the 10s of MHz range. Moreover, this resonant enhancement is protected from inhomogeneous broadening by the Rabi gap. Single-polariton non-linearities and the optomechanical strong-coupling regime become accessible in this platform…
Adjusting the free-electron concentration, the surface plasmon frequency of the semiconductor ZnOGa is tuned into resonance with the molecular vibrations of the n-alkane tetracontane. Closed molecular films deposited on the semiconductor's surface in the monolayer regime generate distinct signatures in total-attenuated-reflection spectra at the frequencies of the symmetric and asymmetric stretching vibrations of the CH2 group. Their line shape undergoes profound changes from absorptive to dispersive and even anti-resonance behavior when moving along the surface- plasmon dispersion by the angel…
We present Floquet-Keldysh non-equilibrium dynamical mean field calculations (DMFT) with an iterative perturbative solver (IPT) for high pump-power induced Stark states yielding a closing gap within semiconductor bulk and nano-cavities. Our model predicts unusual broadening of bands in systems like ZnO random lasers. This can be explained as an exciton-polariton coupling within the single crystalline pillar meeting the Mie resonance condition. Extraordinary enhancement of the lifetime of electronic states within the gap can lead to stable lasing modes and gain narrowing.
Whispering gallery modes in a microwire are characterized by a nearly equidistant energy spectrum. In the strong exciton-photon coupling regime, this system represents a bosonic cascade: a ladder of discrete energy levels that sustains stimulated transitions between neighboring steps. In this work, by using femtosecond angle-resolved spectroscopic imaging technique, the ultrafast dynamics of polaritons in a bosonic cascade based on a one-dimensional ZnO whispering gallery microcavity is explicitly visualized. Clear ladder-form build-up process from higher to lower energy branches of the polari…
Embedding a monolayer of a transition metal dichalcogenide in a high-Q optical cavity results in the formation of distinct exciton polariton modes. The polaritons are affected by the strong exciton-phonon interaction in the monolayer. We use a time convolutionless master equation to calculate the phonon influence on the spectra of the polaritons. We discuss the non-trivial dependence of the line shapes of both branches on temperature and detuning. The peculiar polariton dispersion relation results in a linewidth of the lower polariton being largely independent of the coupling to acoustic phono…
We predict the spontaneous modulated emission from a pair of exciton-polariton condensates due to coherent (Josephson) and dissipative coupling. We show that strong polariton-polariton inter- action generates complex dynamics in the weak-lasing domain way beyond Hopf bifurcations. As a result, the exciton-polariton condensates exhibit self-induced oscillations and emit an equidistant frequency comb light spectrum. A plethora of possible emission spectra with asymmetric peak dis- tributions appears due to spontaneously broken time-reversal symmetry. The lasing dynamics is affected by the shot n…
The coherent optical response from 140~nm and 65~nm thick ZnO epitaxial layers is studied using transient four-wave-mixing spectroscopy with picosecond temporal resolution. Resonant excitation of neutral donor-bound excitons results in two-pulse and three-pulse photon echoes. For the donor-bound A exciton (D$^0$X$_\text{A}$) at temperature of 1.8~K we evaluate optical coherence times $T_2=33-50$~ps corresponding to homogeneous linewidths of $13-19~μ$eV, about two orders of magnitude smaller as compared with the inhomogeneous broadening of the optical transitions. The coherent dynamics is deter…
Quantum correlations and dissipative blockade of polaritons in a tunable fiber cavity
Institut für Quantenelektronik, ETH Zürich（苏黎世联邦理工学院量子电子学研究所）；Physikalisches Institut, Universität Bonn（波恩大学物理研究所）；Department of Physics, Universität Basel（巴塞尔大学物理系）；Univerité Paris-Saclay, UVSQ, CNRS, GEMaC（巴黎萨克雷大学、凡尔赛大学、法国国家科学研究中心、GEMaC）；Laboratorium für Festkörperphysik, ETH Zürich（苏黎世联邦理工学院固体物理实验室）
We present a semi-analytic and asymptotically exact solution to the problem of phonon-induced decoherence in a quantum dot-microcavity system. Particular emphasis is placed on the linear polarization and optical absorption, but the approach presented herein may be straightforwardly adapted to address any elements of the exciton-cavity density matrix. At its core, the approach combines Trotter's decomposition theorem with the linked cluster expansion. The effects of the exciton-cavity and exciton-phonon couplings are taken into account on equal footing, thereby providing access to regimes of co…
Frenkel polaritons, hybrid light-matter quasiparticles, offer promises for the designing of new opto-electronic devices. However, their technological implementations are hindered by sensitivity to imperfections. Topology has raised as a way to circumvent defects and fabrication limitations. Here, we propose a lattice of cavities to realize the one-dimensional Su-Schrieffer-Heeger model (SSH) for topological Frenkel polaritons. By engineering the configuration of the cavities we demonstrate that the SSH topological and trivial phases can be accessed, which we unravel by complementary classical …
Monolayered MoSe2 is a promising new material to investigate advanced light-matter coupling as it hosts stable and robust excitons with comparably narrow optical resonances. In this work, we investigate the evolution of the lowest lying excitonic transition, the so-called A-valley exciton, with temperature. We find a strong, phonon-induced temperature broadening of the resonance, and more importantly, a reduction of the oscillator strength for increased temperatures. Based on these experimentally extracted, temperature dependent parameters, we apply a coupled oscillator model to elucidate the …
Robustness of quantized Hall resistivity under cavity coupling at zero temperature
Instituto de Nanociencia y Materiales de Aragón (INMA), CSIC-Universidad de Zaragoza（阿拉贡纳米科学与材料研究所）；Departamento de Física de la Materia Condensada, Universidad de Zaragoza（萨拉戈萨大学凝聚态物理系）；International Center for Quantum Materials, Peking University（北京大学量子材料中心）；Beijing Key Laboratory of Quantum Devices, Peking University（北京量子器件重点实验室）；Max Planck Institute for the Structure and Dynamics of Matter（马普物质结构与动力学研究所）；The Flatiron Institute（平顿研究所）；Villanova University（维拉诺瓦大学）
The dispersion properties of exciton polaritons in multiple-quantum-well based resonant photonic crystals are studied. In the case of structures with an elementary cell possessing a mirror symmetry with respect to its center, a powerful analytical method for deriving and analyzing dispersion laws of the respective normal modes is developed. The method is used to analyze band structure and dispersion properties of several types of resonant photonic crystals, which would not submit to analytical treatment by other approaches. These systems include multiple quantum well structures with an arbitra…
