Ultrafast optical control of polariton energy in an organic semiconductor microcavity
Kirsty E. McGhee, Michele Guizzardi, Rahul Jayaprakash, Kyriacos Georgiou, Till Jessewitsch, Ullrich Scherf, Giulio Cerullo, Anton Zasedatelev, Tersilla Virgili… 展开作者
Kirsty E. McGhee, Michele Guizzardi, Rahul Jayaprakash, Kyriacos Georgiou, Till Jessewitsch, Ullrich Scherf, Giulio Cerullo, Anton Zasedatelev, Tersilla Virgili, Pavlos G. Lagoudakis, David G. Lidzey
The manipulation of exciton-polaritons and their condensates is of great interest due to their applications in polariton simulators and high-speed, all-optical logic devices. Until now, methods of trapping and manipulating such condensates are not dynamically reconfigurable or result in an undesirable reduction in the exciton-photon coupling strength. Here, we present a new strategy for the ultrafast control of polariton resonances via transient modification of an optical cavity mode. We have constructed multilayer organic semiconductor microcavities that contain two absorbers: one strongly- and one weakly-coupled to the cavity photon mode. By selectively exciting the weakly-coupled absorber with ultrashort laser pulses, we modulate the cavity refractive index and generate fully-reversible blueshifts of the lower polariton branch by up to 8 meV in sub-ps timescales with no corresponding reduction in the exciton-photon coupling strength. Our work demonstrates the ability to manipulate polariton energy landscapes over ultrafast timescales with important applications in emerging computing technologies.
We resonantly inject polaritons into a microcavity and track them in time and space as they feel a force due to the cavity gradient. This is an example of "slow reflection," as the polaritons, which can be viewed as renormalized photons, slow down to zero velocity and then move back in the opposite direction. These measurements accurately measure the lifetime of the polaritons in our samples, which is 180 $\pm$ 10 ps, corresponding to a cavity leakage time of 135 ps and a cavity $Q$ of 320,000. Such long-lived polaritons propagate millimeters in these wedge-shaped microcavities. Additionally, …
We present a microcavity structure with a shifted photonic stop-band to enable efficient non-resonant injection of a polariton condensate with spectrally broad femtosecond pulses. The concept is demonstrated theoretically and confirmed experimentally for a planar GaAs/AlGaAs multilayer heterostructure pumped with ultrashort near-infrared pulses while photoluminescence is collected to monitor the optically injected polariton density. As the excitation wavelength is scanned, a regime of polariton condensation can be reached in our structure at a consistently lower fluence threshold than in a sta…
Atomically thin transition metal dichalcogenides possess valley dependent functionalities that are usually available only at crogenic temperatures, constrained by various valley depolarization scatterings. The formation of exciton polaritons by coherently superimposing excitons and microcavity photons potentially harnesses the valley polarized polariton polariton interactions for novel valleytronics devices. Robust EPs have been demonstrated at room temperature in TMDs microcavity, however, the coherent polariton lasing and condensation remain elusive. Herein, we demonstrate for the first time…
A ring dark soliton is a dark soltion occurring in higher dimensions. It is still unknown in microcavity-polariton condensates due to its instability. We find that a stable RDS cannot exist in a MPC without a defect. We then propose a way to create a stable RDS in a MPC by adding a defect with a ring structure to the system. A RDS pinned by the defect potential becomes stable. For various pump powers, we also investigate the stable regime of the RDS by tuning the strength and width of the defect potential. We conclude that the stable RDSs can be obtained.
We report an experimental observation of polaritonic optical bistability of the laser emission in a planar semiconductor microcavity with a $100Å$ GaAs single quantum well in the strong-coupling regime. The bistability curves show crossings that indicate a competition between a Kerr-like effect induced by the polariton population and thermal effects. Associated with the bistability, laser-like emission occurs at the bare cavity mode.
Strong coupling between molecular vibrations and microcavity modes has been demonstrated to modify physical and chemical properties of the molecular material. Here, we study the much less explored coupling between lattice vibrations (phonons) and microcavity modes. Embedding thin layers of hexagonal boron nitride (hBN) into classical microcavities, we demonstrate the evolution from weak to ultrastrong phonon-photon coupling when the hBN thickness is increased from a few nanometers to a fully filled cavity. Remarkably, strong coupling is achieved for hBN layers as thin as 10 nm. Further, the ul…
Microcavity polaritons are light-matter quasiparticles that arise from the strong coupling between excitons and photons confined in a semiconductor microcavity. They typically operate at visible or near visible wavelengths. They combine the properties of confined electromagnetic fields, including a sizeable spin-orbit coupling, and the sensitivity to external magnetic fields and particle interactions inherited from their partly matter nature. These features make polaritons an excellent platform to study topological phases in photonics in one and two dimensional lattices, which band properties …
Interactions of few-cycle terahertz pulses with the induced optical polarization in a quantum-well microcavity reveal that the lower and higher exciton-polariton modes together with the optically forbidden 2p-exciton state form a unique Λ-type three-level system. Pronounced nonlinearities are observed via time-resolved strong-terahertz and weak-optical excitation spectroscopy and explained with a fully microscopic theory. The results show that the terahertz pulses strongly couple the exciton-polariton states to the 2p-exciton state while no resonant transition between the two polariton levels …
Polariton lattice condensates provide a platform for on chip quantum emulations. Interactions in extended polariton lattices are currently limited by the intrinsic photonic disorder of microcavities. Here, we fabricate a strain compensated planar GaAs/AlAs microcavity with embedded InGaAs quantum wells and report on polariton condensation under non-resonant optical excitation. Evidence of polariton condensation is supported spectroscopically both in reflection and transmission geometry, whilst the observation of a second threshold to photon lasing allows us to conclusively distinguish between …
The ultrafast scattering dynamics of intersubband polaritons in dispersive cavities embedding GaAs/AlGaAs quantum wells are studied directly within their band structure using a non-collinear pump-probe geometry with phase-stable mid-infrared pulses. Selective excitation of the lower polariton at a frequency of ~25 THz and at a finite in-plane momentum, $k_{||}$, leads to the emergence of a narrowband maximum in the probe reflectivity at $k_{||}=0$. A quantum mechanical model identifies the underlying microscopic process as stimulated coherent polariton-polariton scattering. These results mark …
Exciton-polaritons have become an emerging platform for implementing non-Hermitian physics. The implementation commonly requires control of both the real and imaginary parts of the eigenmodes of the system. We present an experimental method to achieve this purpose using microcavities with sub-wavelength gratings as reflectors. The reflectivity and reflection phase of the grating can be changed by its geometric parameters and they determine the energy and linewidth of the polariton modes. We demonstrate that this method allows a wide range of possible polariton energy and linewidth, suitable fo…
We study theoretically optomechanical interactions in a semiconductor microcavity with embedded quantum well under the optical pumping by a Bessel beam, carrying a non-zero orbital momentum. Due to the transfer of orbital momentum from light to phonons, the microcavity can act as an acoustic circulator: it rotates the propagation direction of the incident phonon by a certain angle clockwise or anticlockwise. Due to the optomechanical heating and cooling effects, the circulator can also function as an acoustic laser emitting sound with nonzero angular momentum. Our calculations demonstrate the …
Topological photonics provides an important platform for the development of photonic devices with robust disorder-immune light transport and controllable helicity. Mixing photons with excitons (or polaritons) gives rise to nontrivial polaritonic bands with chiral modes, allowing the manipulation of helical lasers in strongly coupled light-matter systems. In this work, we demonstrate helical polariton lasing from topological valleys of an organic anisotropic microcrystalline cavity based on tailored local nontrivial band geometry. This polariton laser emits light of different helicity along dif…
We have measured time-resolved the photon storage time and the quality factor of an ultrafast photonic cavity using an autocorrelator. The cavity consists of a $λ$-thick GaAs layer sandwiched between GaAs/AlAs distributed Bragg reflectors and resonates at 985 nm wavelength. The inverse relative linewidth measured with white light reflectivity is 830, while the quality factor obtained from the time resolved measurements is 1500. The photon storage time in the cavity is 0.78 ps. We show that the difference between the quality factor and the inverse relative linewidth results from inhomogeneous b…
We propose all-optical neural networks characterized by very high energy efficiency and performance density of inference. We argue that the use of microcavity exciton-polaritons allows to take advantage of the properties of both photons and electrons in a seamless manner. This results in strong optical nonlinearity without the use of optoelectronic conversion. We propose a design of a realistic neural network and estimate energy cost to be at the level of attojoules per bit, also when including the optoelectronic conversion at the input and output of the network, several orders of magnitude be…
Integrated electro-optical switches are essential as one of the fundamental elements in the development of modern optoelectronics. As an architecture for photonic systems, exciton polaritons, that are hybrid bosonic quasiparticles that possess unique properties derived from both excitons and photons, have shown much promise. For this system, we demonstrate a significant improvement of emitted intensity and condensation threshold by applying an electric field to a microcavity filled with an organic microbelt. Our theoretical investigations indicate that the electric field makes the excitons dip…
Lead-halide perovskites are highly promising for various optoelectronic applications including laser devices. However, fundamental photophysics describing the lasing behaviour in this material family have not been investigated systematically, and thus the detailed lasing mechanism remains veiled. Here, we demonstrate that an all-inorganic perovskite shows a lasing emission based on a novel principle. A series of photoluminescence experiment results reveals that the excited state of CsPbBr3 single crystal exhibits free carrier nature. In a form of microcavity, on the other hand, the CsPbBr3 sin…
Gain and loss modulation are ubiquitous in nature. An exceptional point arises when both the eigenvectors and eigenvalues coalesce, which in a physical system can be achieved by engineering the gain and loss coefficients, leading to a wide variety of counter-intuitive phenomena. In this work we demonstrate the existence of an exceptional point in an exciton polariton condensate in a double-well potential. Remarkably, near the exceptional point, the polariton condensate localized in one potential well can be switched off by an additional optical excitation in the other well with very low (far b…
We present experimental observations of a non-resonant dynamic Stark shift in strongly coupled microcavity quantum well exciton-polaritons - a system which provides a rich variety of solid-state collective phenomena. The Stark effect is demonstrated in a GaAs/AlGaAs system at 10K by femtosecond pump-probe measurements, with the blue shift approaching the meV scale for a pump fluence of 2 mJcm^-2 and 50 meV red detuning, in good agreement with theory. The energy level structure of the strongly coupled polariton Rabi-doublet remains unaffected by the blue shift. The demonstrated effect should al…
Dibenzo[\emph{hi,st}]ovalene (DBOV) - a quasi-zero-dimensional `nanographene' - displays strong, narrow, and well-defined optical-absorption transitions at room temperature. On placing a DBOV-doped polymer film into an optical microcavity, we demonstrate strong coupling of the \textbf{0 $\rightarrow$ 0'} electronic and \textbf{0 $\rightarrow$ 1'} vibrational transitions to a confined cavity mode, with coupling energies of 104 meV and 40 meV, respectively. Photoluminescence measurements indicate that the polariton population is distributed between the lower and middle polariton branches at ener…
We study the time-resolved reflectivity spectrum of a switched planar GaAs-AlAs microcavity. Between 5 and 40 ps after the switching (pump) pulse we observe a strong excess probe reflectivity and a change of the frequency of light trapped in the cavity up to 5 linewidths away from the cavity resonance. This frequency change does not adiabatically follow the fast-changing cavity resonance. The frequency change is attributed to an accumulated phase change due to the time-dependent refractive index. An analytical model predicts dynamics in qualitative agreement with the experiments, and points to…
Solitons and vortices obtain widespread attention in different physical systems as they offer potential use in information storage, processing, and communication. In exciton-polariton condensates in semiconductor microcavities, solitons and vortices can be created optically. However, dark solitons are unstable and vortices cannot be spatially controlled. In the present work we demonstrate the existence of stable dark solitons and vortices under non-resonant incoherent excitation of a polariton condensate with a simple spatially periodic pump. In one dimension, we show that an additional cohere…
We present a microscopic theory for the description of the bias-controlled operation of an exciton-polariton-based heterostructure, in particular, the polariton laser. Combining together the Poisson equations for the scalar electric potential and Fermi quasi-energies of electrons and holes in a semiconductor heterostructure, the Boltzmann equation for the incoherent excitonic reservoir and the Gross-Pitaevskii equation for the exciton-polariton mean field, we simulate the dynamics of the system minimising the number of free parameters and for the first time build a theoretical threshold charac…
Exciton-polaritons in semiconductor microcavities generate fascinating effects such as long-range spatial coherence and Bose-Einstein Condensation (BEC), which are attractive for their potential use in low threshold lasers, vortices and slowing light, etc. However, currently most of exciton-polariton effects either occur at cryogenic temperature or rely on expensive cavity fabrication procedures. Further exploring new semiconductor microcavities with stronger exciton photon interaction strength is extensively needed. Herein, we demonstrate room temperature photon exciton strong coupling in hyb…
Electrically reconfigurable dipolar polaritons with highly tunable nonlinearity in a homobilayer microcavity
Tsinghua University（清华大学）；University of Washington（华盛顿大学）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）；National Institute for Materials Science（国立材料研究所）；Nanyang Technological University（南洋理工大学）；Frontier Science Center for Quantum Information（量子信息前沿科学中心）
Realizing nonlinear coupling across space can enable new scientific and technological advances, including ultrafast operation and propagation of information in IR photonic circuitry, remote triggering or catalyzing of chemical reactions, and new platforms for quantum simulations with increased complexities. In this report, we show that ultrafast nonlinear couplings are achieved between polaritons residing in different cavities, in the mid-infrared (IR) regime, e.g. by pumping polaritons in one cavity, the polaritons in the adjacent cavity can be affected. By hybridizing photon and molecular vi…
We show that, by monitoring the free carrier reservoir in a GaAs-based quantum well microcavity under nonresonant pulsed optical pumping, lasing supported by a fermionic reservoir (photon lasing) can be distinguished from lasing supported by a reservoir of bosons (polariton lasing). Carrier densities are probed by measuring the photocurrent between lateral contacts deposited directly on the quantum wells of a microcavity that are partially exposed by wet chemical etching. We identify two clear thresholds in the input-output characteristic of the photoluminescence signal which can be attributed…
The coherence of polaritons plays a fundamental role in numerous recent experimental observations, from strong coupling to Bose-Einstein condensation, but accessing the coherence of polaritons is a difficult task due to the high energy of plasmons and excitons. However, surface phonon polaritons offer similar promises at much lower energy. Here, we demonstrate the possibility to use visible ultrafast lasers to generate and time resolve coherent surface phonon polaritons in nanowires. We show that these modes are generated through the ultrafast screening of the surface depletion field. By compa…
Semiconductor microcavities can exhibit various macroscopic quantum phenomena, including Bose-Einstein condensation of polaritons, Bardeen-Cooper-Schrieffer (BCS) states of polaritons, and photon lasing (lasing with negligible Coulombic exciton effects). An important aspect of possible experimental identification of these states is a gap in the excitation spectrum (the BCS gap in the case of a polaritonic BCS state). Similar to the polaritonic BCS gap, a light-induced gap can exist in photon lasers. Although polaritonic BCS states have been observed on the basis of spectroscopy in the vicinity…
The artificial gauge field for electrically neutral exciton polaritons devoid from the polarization degree of freedom can be synthesized by means of applying crossed electric and magnetic fields. The appearance of the gauge potential can be ascribed to the motional (magneto-electric) Stark effect which is responsible for the presence of a linear-in-momentum contribution to the exciton kinetic energy. We study the interplay of this phenomenon with the competing effect which arises from the Rabi-splitting renormalization due the reduction of the electron-hole overlap for a moving exciton. Accoun…
The strong coupling of an IR-active molecular transition with an optical mode of the cavity results in vibrational polaritons, which opens a new way to control chemical reactivity via confined electromagnetic fields of the cavity. In this study, we design a voltage-tunable open microcavity and we show the formation of multiple vibrational polaritons in methyl salicylate. A Rabi splitting and polariton anticrossing behaviour is observed when the cavity mode hybridizes with the C=O stretching vibration of methyl salicylate. As this vibration contributes to the reaction coordinate of the photoind…
Two-dimensional (2D) semiconducting microcavity, where exciton-polaritons can be formed, constitues a promising setup for exploring and manipulating various regimes of light-matter interaction. Here, the coupling between 2D excitons and metallic cavity photons is studied by using first-principles propagator technique. The strength of exciton-photon coupling is characterised by its Rabi splitting to two exciton-polaritons, which can be tuned by cavity thickness. Maximum splitting of 128 meV is achieved in phosporene cavity, while remarkable value of about 440 meV is predicted in monolayer hBN d…
Resonant interaction between excitonic transitions of molecules and localized electromagnetic field allows the formation of hybrid light-matter polaritonic states. This hybridization of the light and the matter states has been shown to be able to significantly alter the intrinsic properties of molecular ensembles placed inside the optical cavity. Here, we have achieved strong coupling between the excitonic transition in typical oligonucleotide-based molecular beacons labelled with a pair of organic dye molecules, demonstrating an efficient donor to acceptor resonance energy transfer, and the t…
Ultrafast Nano-Imaging and Optical Control of Hyperbolic Phonon Polaritons at hBN/WS$_2$ Heterojunctions
Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学研究所分子科学研究所）；Department of Physics and Electronics, Graduate School of Engineering, Osaka Metropolitan University（大阪公立大学工学研究科物理电子学专业）；The Graduate University for Advanced Studies, SOKENDAI（日本高级研究院）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国立材料研究所物质结构纳米构造研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国立材料研究所电子光学材料研究中心）；Fritz-Haber-Institut der Max-Planck-Gesellschaft（马克斯·普朗克学会弗里茨·哈伯研究所）
Functionality of many nonlinear and quantum optical devices relies on the effect of optical bistability. Using the microcavity exciton-polaritons in a honeycomb arrangement of microcavity pillars, we report the resonance response and bistability of the topological edge states. A balance between the pump, loss and nonlinearity ensures a broad range of dynamical stability and controls the distribution of power between counter-propagating states on the opposite edges of the honeycomb lattice stripe. Tuning energy and polarization of the pump photons, while keeping their momentum constant, we demo…
While optical technology provides the best solution for the transmission of information, optical logics still calls for qualitative new concepts to be explored. Exciton-polaritons are composite particles, resulting from the strong coupling between excitons and photons, which have recently demonstrated exceptional properties like huge non-linearities, long range coherence and suppression of scattering. Here we demonstrate a switching scheme for polaritons moving in the plane of a microcavity which satisfy all the requirements for an all-optical transistor. Under resonant excitation, the power t…
