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Showing papers on "Optical microcavity published in 2019"


Journal ArticleDOI
TL;DR: In this paper, a ladder-type polymer in an optical microcavity was used to realize room-temperature operation of a polariton transistor through vibron-mediated stimulated polariton relaxation.
Abstract: Active optical elements with ever smaller footprint and lower energy consumption are central to modern photonics. The drive for miniaturization, speed and efficiency, with the concomitant volume reduction of the optically active area, has led to the development of devices that harness strong light–matter interactions. By managing the strength of light–matter coupling to exceed losses, quasiparticles, called exciton-polaritons, are formed that combine the properties of the optical fields with the electronic excitations of the active material. By making use of polaritons in inorganic semiconductor microcavities, all-optical transistor functionality was observed, albeit at cryogenic temperatures1. Here, we replace inorganic semiconductors with a ladder-type polymer in an optical microcavity and realize room-temperature operation of a polariton transistor through vibron-mediated stimulated polariton relaxation. We demonstrate net gain of ~10 dB μm−1, sub-picosecond switching time, cascaded amplification and all-optical logic operation at ambient conditions. Net gain of ~10 dB µm–1 and sub-picosecond switching time are shown at room temperature for optical transistors using polymers in a microcavity.

179 citations


Journal ArticleDOI
21 Oct 2019-Nature
TL;DR: A gated, ultralow-loss, frequency-tunable microcavity device that establishes a route to the development of semiconductor-based quantum photonics, such as single-photon sources and photon–photon gates.
Abstract: The strong-coupling regime of cavity quantum electrodynamics (QED) represents the light–matter interaction at the fully quantum level. Adding a single photon shifts the resonance frequencies—a profound nonlinearity. Cavity QED is a test bed for quantum optics1–3 and the basis of photon–photon and atom–atom entangling gates4,5. At microwave frequencies, cavity QED has had a transformative effect6, enabling qubit readout and qubit couplings in superconducting circuits. At optical frequencies, the gates are potentially much faster; the photons can propagate over long distances and can be easily detected. Following pioneering work on single atoms1–3,7, solid-state implementations using semiconductor quantum dots are emerging8–15. However, miniaturizing semiconductor cavities without introducing charge noise and scattering losses remains a challenge. Here we present a gated, ultralow-loss, frequency-tunable microcavity device. The gates allow both the quantum dot charge and its resonance frequency to be controlled electrically. Furthermore, cavity feeding10,11,13–17, the observation of the bare-cavity mode even at the quantum dot–cavity resonance, is eliminated. Even inside the microcavity, the quantum dot has a linewidth close to the radiative limit. In addition to a very pronounced avoided crossing in the spectral domain, we observe a clear coherent exchange of a single energy quantum between the ‘atom’ (the quantum dot) and the cavity in the time domain (vacuum Rabi oscillations), whereas decoherence arises mainly via the atom and photon loss channels. This coherence is exploited to probe the transitions between the singly and doubly excited photon–atom system using photon-statistics spectroscopy18. The work establishes a route to the development of semiconductor-based quantum photonics, such as single-photon sources and photon–photon gates. Strong coupling between a gated semiconductor quantum dot and an optical microcavity is observed in an ultralow-loss frequency-tunable microcavity device.

172 citations


Journal ArticleDOI
TL;DR: In this article, an organic molecule placed into an optical microcavity behaves as a coherent two-level quantum system, which allows the observation of 99% extinction of a laser beam by a single molecule, saturation with less than 0.5 photons and nonclassical generation of few-photons super-bunched light.
Abstract: The use of molecules in quantum optical applications has been hampered by incoherent internal vibrations and other phononic interactions with their environment. Here we show that an organic molecule placed into an optical microcavity behaves as a coherent two-level quantum system. This allows the observation of 99% extinction of a laser beam by a single molecule, saturation with less than 0.5 photons and non-classical generation of few-photons super-bunched light. Furthermore, we demonstrate efficient interaction of the molecule–microcavity system with single photons generated by a second molecule in a distant laboratory. Our achievements represent an important step towards linear and nonlinear quantum photonic circuits based on organic platforms. A molecule placed in an optical microcavity behaves as a model two-level quantum system, as demonstrated via laser extinction and interaction with single photons.

136 citations


Journal ArticleDOI
TL;DR: In this article, the authors integrated a single-photon source hosted by hexagonal boron nitride (hBN) into a tunable optical microcavity.
Abstract: Sources of pure and indistinguishable single-photons are critical for near-future optical quantum technologies. Recently, color centers hosted by two-dimensional hexagonal boron nitride (hBN) have emerged as a promising platform for high luminosity room temperature single-photon sources. Despite the brightness of the emitters, the spectrum is rather broad and the single-photon purity is not sufficient for practical quantum information processing. Here, we report integration of such a quantum emitter hosted by hBN into a tunable optical microcavity. A small mode volume of the order of $\lambda^3$ allows us to Purcell enhance the fluorescence, with the observed excited state lifetime shortening. The cavity significantly narrows the spectrum and improves the single-photon purity by suppression of off-resonant noise. We explore practical applications by evaluating the performance of our single-photon source for quantum key distribution and quantum computing. The complete device is compact and implemented on a picoclass satellite platform, enabling future low-cost satellite-based long-distance quantum networks.

78 citations


Journal ArticleDOI
09 May 2019-Chem
TL;DR: In this paper, a polaritonic (hybrid photonic-molecular) device was proposed to support ultrafast tuning of reaction yields even when the catalyst and reactant are spatially separated across several optical wavelengths.

70 citations


Journal ArticleDOI
TL;DR: It is shown that the photon energy loss from optical gap to open-circuit voltage can be reduced to unprecedented values by embedding organic solar cells in optical microcavities, simply by manipulating the device architecture.
Abstract: Strong light-matter coupling can re-arrange the exciton energies in organic semiconductors. Here, we exploit strong coupling by embedding a fullerene-free organic solar cell (OSC) photo-active layer into an optical microcavity, leading to the formation of polariton peaks and a red-shift of the optical gap. At the same time, the open-circuit voltage of the device remains unaffected. This leads to reduced photon energy losses for the low-energy polaritons and a steepening of the absorption edge. While strong coupling reduces the optical gap, the energy of the charge-transfer state is not affected for large driving force donor-acceptor systems. Interestingly, this implies that strong coupling can be exploited in OSCs to reduce the driving force for electron transfer, without chemical or microstructural modifications of the photo-active layer. Our work demonstrates that the processes determining voltage losses in OSCs can now be tuned, and reduced to unprecedented values, simply by manipulating the device architecture.

63 citations


Journal ArticleDOI
TL;DR: The latest progress in exciton-polaritons and polariton lasers of perovskites are reviewed and Polaritons in planar and nanowires Fabry-Pérot microcavities are discussed with particular reference to material and photophysics.
Abstract: The semiconductor exciton-polariton, arising from the strong coupling between excitons and confined cavity photon modes, is not only of fundamental importance in macroscopic quantum effects but also has wide application prospects in ultralow-threshold polariton lasers, slowing-light devices, and quantum light sources. Very recently, metallic halide perovskites have been considered as a great candidate for exciton-polariton devices owing to their low-cost fabrication, large exciton oscillator strength, and binding energy. Herein, the latest progress in exciton-polaritons and polariton lasers of perovskites are reviewed. Polaritons in planar and nanowires Fabry-Perot microcavities are discussed with particular reference to material and photophysics. Finally, a perspective on the remaining challenges in perovskite polaritons research is given.

50 citations


Journal ArticleDOI
TL;DR: In this paper, a time-local master equation was developed for the population dynamics of chemically relevant species in different regimes of emitter coupling to the condensed phase vibrational bath and to the microcavity photonic mode.
Abstract: We explore the electroluminescence efficiency for a quantum mechanical model of a large number of molecular emitters embedded in an optical microcavity. We characterize the circumstances under which a microcavity enhances harvesting of triplet excitons via reverse intersystem-crossing (R-ISC) into singlet populations that can emit light. For that end, we develop a time-local master equation in a variationally optimized frame, which allows for the exploration of the population dynamics of chemically relevant species in different regimes of emitter coupling to the condensed phase vibrational bath and to the microcavity photonic mode. For a vibrational bath that equilibrates faster than R-ISC (in emitters with weak singlet-triplet mixing), our results reveal that significant improvements in efficiencies with respect to the cavity-free counterpart can be obtained for strong coupling of the singlet exciton to a photonic mode, as long as the singlet to triplet exciton transition is within the inverted Marcus regime; under these circumstances, the activation energy barrier from the triplet to the lower polariton can be greatly reduced with respect to that from the triplet to the singlet exciton, thus overcoming the detrimental delocalization of the polariton states across a macroscopic number of molecules. On the other hand, for a vibrational bath that equilibrates slower than R-ISC (i.e., emitters with strong singlet-triplet mixing), we find that while enhancements in photoluminescence can be obtained via vibrational relaxation into polaritons, this only occurs for a small number of emitters coupled to the photon mode, with delocalization of the polaritons across many emitters eventually being detrimental to electroluminescence efficiency. These findings provide insight into the tunability of optoelectronic processes in molecular materials due to weak and strong light-matter coupling.

42 citations


Journal ArticleDOI
TL;DR: The fabrication and characterization of a dielectric, anisotropic optical microcavity based on nonpolar ZnO that implements a non-Hermitian system and mimics the behavior of Voigt points in natural crystals, paving the way for exploiting exceptional points in widespread optoelectronic devices such as vertical cavity surface emitting lasers and resonant cavity light emitting diodes.
Abstract: Voigt points represent propagation directions in anisotropic crystals along which optical modes degenerate, leading to a single circularly polarized eigenmode. They are a particular class of exceptional points. Here, we report the fabrication and characterization of a dielectric, anisotropic optical microcavity based on nonpolar ZnO that implements a non-Hermitian system and mimics the behavior of Voigt points in natural crystals. We prove the exceptional-point nature by monitoring the complex-square-root topology of the mode eigenenergies (real and imaginary parts) around the Voigt points. Polarization state analysis shows that these artificially engineered Voigt points behave as vortex cores for the linear polarization and sustain chiral modes. Our findings apply to any planar microcavity with broken cylindrical symmetry and, thus, pave the way for exploiting exceptional points in widespread optoelectronic devices such as vertical cavity surface emitting lasers and resonant cavity light emitting diodes.

37 citations


Journal ArticleDOI
TL;DR: In this article, a large Rabi splitting was achieved at ambient conditions in the strong coupling regime by embedding Ag-WS2 heterostructure in an optical microcavity, where the generated quasiparticle with part-plasmon, part-exciton and part-light was analyzed with Hopfield coefficients that were calculated by using three-coupled oscillator model.
Abstract: Manipulation of light-matter interaction is critical in modern physics, especially in the strong coupling regime, where the generated half-light, half-matter bosonic quasiparticles as polaritons are important for fundamental quantum science and applications of optoelectronics and nonlinear optics. Two-dimensional transition metal dichalcogenides (TMDs) are ideal platforms to investigate the strong coupling because of their huge exciton binding energy and large absorption coefficients. Further studies on strong exciton-plasmon coupling by combining TMDs with metallic nanostructures have generated broad interests in recent years. However, because of the huge plasmon radiative damping, the observation of strong coupling is significantly limited at room temperature. Here, we demonstrate that a large Rabi splitting (~300 meV) can be achieved at ambient conditions in the strong coupling regime by embedding Ag-WS2 heterostructure in an optical microcavity. The generated quasiparticle with part-plasmon, part-exciton and part-light is analyzed with Hopfield coefficients that are calculated by using three-coupled oscillator model. The resulted plasmon-exciton polaritonic hybrid states can efficiently enlarge the obtained Rabi splitting, which paves the way for the practical applications of polaritonic devices based on ultrathin materials.

37 citations


Journal ArticleDOI
TL;DR: Time-resolved spectroscopy revealed that energy transfer from the inorganic to the organic microcavity creates sufficient polaritons densities for a visible-light LED, thanks to a delocalized quantum state that forms over both chambers.
Abstract: Polaritons are quasi-particles composed of a superposition of excitons and photons that can be created within a strongly coupled optical microcavity. Here, we describe a structure in which a strongly coupled microcavity containing an organic semiconductor is coupled to a second microcavity containing a series of weakly coupled inorganic quantum wells. We show that optical hybridisation occurs between the optical modes of the two cavities, creating a delocalised polaritonic state. By electrically injecting electron–hole pairs into the inorganic quantum-well system, we are able to transfer energy between the cavities and populate organic-exciton polaritons. Our approach represents a new strategy to create highly efficient devices for emerging ‘polaritonic’ technologies. Researchers have optically connected organic semiconductors and inorganic thin films to produce a light-emitting diode powered by quasi-particles that are part light and part matter. Polaritons, which form when electron–hole pairs in a semiconductor interact with photons, can be energy efficient sources of coherent light. Rahul Jayaprakash from the University of Sheffield in the United Kingdom and co-workers have now developed a device that generates electron-hole pairs inside a reflective microcavity filled with gallium–indium–phosphorus thin films. Then, they coupled the chamber’s optical resonance to a second microcavity containing light-absorbing phthalocyanine dye molecules. Time-resolved spectroscopy revealed that energy transfer from the inorganic to the organic microcavity creates sufficient polaritons densities for a visible-light LED, thanks to a delocalized quantum state that forms over both chambers.

Journal ArticleDOI
TL;DR: In this paper, the spectral selectivity of solar absorbers under certain optical concentration could boom the photothermal conversion efficiency by improving the solar absorptance in quasi-optical microcavity-based absorbers.

Journal ArticleDOI
20 Dec 2019-Science
TL;DR: An on-chip optical microcavity allows laser initiation of clusters of quasi–two-dimensional vortices and nondestructive observation of their decay in a single shot, and establishes an on- chip platform with which to study emergent phenomena in strongly interacting superfluids and to develop quantum technologies such as precision inertial sensors.
Abstract: Quantized vortices are fundamental to the two-dimensional dynamics of superfluids, from quantum turbulence to phase transitions. However, surface effects have prevented direct observations of coherent two-dimensional vortex dynamics in strongly interacting systems. Here, we overcome this challenge by confining a thin film of superfluid helium at microscale on the atomically smooth surface of a silicon chip. An on-chip optical microcavity allows laser initiation of clusters of quasi-two-dimensional vortices and nondestructive observation of their decay in a single shot. Coherent dynamics dominate, with thermal vortex diffusion suppressed by five orders of magnitude. This establishes an on-chip platform with which to study emergent phenomena in strongly interacting superfluids and to develop quantum technologies such as precision inertial sensors.

Journal ArticleDOI
TL;DR: In this article, strong coupling of vibrational modes was explored using a planar optical microcavity and a surface plasmon mode associated with a single metal surface, where the surface plasmons on planar metal films have momenta that cannot be accessed easily by incident light.
Abstract: DOI: 10.1002/adom.201900403 to hybridize excitonic resonances associated with two different species.[17,18,15] Hybridization of different vibrational overtones of an excitonic resonance of a single molecular species has also been achieved.[19,20] Meanwhile, in the infrared regime, hybridization of vibrational resonances associated with two distinct molecular species has also been reported recently.[21,22] While hybridization of two different vibrational resonances of a single molecular species to a cavity mode were reported by George et al.[23] Here we present results of experiments that show hybridization of three vibrational resonances of a single mode species to first a cavity mode and second a surface plasmon mode, thereby adding a potentially important component in the strong coupling toolbox, one that may further the degree of control possible over molecular vibrational states in any future polaritonic chemistry. Strong coupling of vibrational modes was first explored using a planar cavity filled with the polymer polymethyl-methacrylate (PMMA) where the cavity mode was strongly coupled to the CO vibrational resonance in the polymeric material.[24,25] Several further investigations have since been reported,[26–33] involving vibrational resonances in liquids,[34] transition metal complexes,[33] and liquid crystals.[35] Strong coupling of vibrational resonances has also been reported to help catalyze and inhibit chemical reactions[36] and to control the nonlinear optical response in the infrared.[37] 2D spectroscopy of molecular vibrations in an optical microcavity has also been explored.[38,39] In the present work, we make use of two different types of confined light field. First we use the well-established planar optical microcavity, second we make use of the surface plasmon mode associated with a single metal surface. Surface plasmons on planar metal films have momenta that cannot be accessed easily by incident light; therefore, we employ grating coupling to overcome this problem, an approach previously explored for strong coupling of excitonic resonances.[40,41] In what follows, we briefly describe the sample structure and material properties. The main probe we use to explore the coupling between vibrational resonances and the optical modes of our confined light fields is to determine the dispersion of the polaritons involved. We describe how these data are acquired and present results from both types of cavity. We then discuss the modeling we have undertaken, both numerical and analytical, before summarizing our findings.

Journal ArticleDOI
19 Mar 2019
TL;DR: In this article, an alternative scheme based on a semiconductor quantum dot (QD) embedded in an optical microcavity in a magnetic field was proposed, where a single charge carrier trapped in the dot has an associated spin that can be controlled by ultrashort optical pulses.
Abstract: Aquantum computer has the potential to revolutionize multiple industries by enabling a drastic speed-up relative to classical computers for certain quantum algorithms and simulations. Linear optical quantum computing is an approach that uses photons as qubits, which are known for suffering little from decoherence. A source of multiple entangled and indistinguishable photons would be a significant step in the development of an optical quantum computer. Consequently, multiple proposals for the generation of such a stream of photons have recently been put forward. Here we introduce an alternative scheme based on a semiconductor quantum dot (QD) embedded in an optical microcavity in a magnetic field.A single charge carrier trapped in the dot has an associated spin that can be controlled by ultrashort optical pulses. Photons are sequentially generated by resonant scattering from the QD, while the charge spin is used to determine the encoding of the photons into time-bins. In this way a multi-photon entangled state can be gradually built up. With a simple optical pulse sequence we demonstrate a proof of principle experiment of our proposal by showing that the time-bin of a single photon is dependent on the measured state of the trapped charge spin.

Journal ArticleDOI
TL;DR: In this paper, a time-local master equation was developed for the population dynamics of chemically relevant species in different regimes of emitter coupling to the condensed phase vibrational bath and to the microcavity photonic mode.
Abstract: We explore the electroluminescence efficiency for a quantum mechanical model of a large number of molecular emitters embedded in an optical microcavity. We characterize the circumstances under which a microcavity enhances harvesting of triplet excitons via reverse intersystem-crossing (R-ISC) into singlet populations that can emit light. For that end, we develop a time-local master equation in a variationally optimized frame which allows for the exploration of the population dynamics of chemically relevant species in different regimes of emitter coupling to the condensed phase vibrational bath and to the microcavity photonic mode. For a vibrational bath that equilibrates faster than R-ISC (in emitters with weak singlet-triplet mixing), our results reveal that significant improvements in efficiencies with respect to the cavity-free counterpart can be obtained for strong coupling of the singlet exciton to a photonic mode, as long as the singlet to triplet exciton transition is within the inverted Marcus regime; under these circumstances, we show the possibility to overcome the detrimental delocalization of the polariton states across a macroscopic number of molecules. On the other hand, for a vibrational bath that equilibrates slower than R-ISC (i.e., emitters with strong singlet-triplet mixing), we find that while enhancemnents in photoluminiscence can be obtained via vibrational relaxation into polaritons, this only occurs for small number of emitters coupled to the photon mode, with delocalization of the polaritons across many emitters eventually being detrimental to electroluminescence efficiency. These findings provide insight on the tunability of optoelectronic processes in molecular materials due to weak and strong light-matter coupling.

Journal ArticleDOI
TL;DR: In this article, self-assembled organic microspheres of (E)-3-(4-(dip-tolylamino)phenyl)-1-(4-fluoro-2-hydroxyphenyl)prop-2en-1-one (DTPHP) are fabricated, which serve as active WGM resonators, and a dispersion relationship between the group refractive index (ng) and wavelength (λ) is revealed.
Abstract: The self-assembled organic microspheres of (E)-3-(4-(dip-tolylamino)phenyl)-1-(4-fluoro-2-hydroxyphenyl)prop-2-en-1-one (DTPHP) are fabricated, which serve as active WGM resonators. In addition, a dispersion relationship between the group refractive index (ng) and wavelength (λ) is revealed to demonstrate the strong light–matter interaction inside the WGM microcavity with a maximum ng to be 7.7.

Journal ArticleDOI
TL;DR: An intuitive coupled mode model reveals that a distinct optical pathway highlighting the cavity-mediated activation of nanoantennas is key for absorption enhancement, and shows that the linewidth of the enhancement can be widely tunable, and that the maximum power transferred to the antennas is attained under critical coupling.
Abstract: Nanoantenna–microcavity hybrid systems offer unique platforms for the study and manipulation of light at the nanoscale, since their constituents have either low mode volume or long photon storage time. A nearby dielectric optical cavity can modify the photonic environment surrounding a plasmonic nanoantenna, presenting opportunities to sculpt its spectral response. However, matching the polar opposites for enhanced light–matter interactions remains challenging, as the antenna can be rendered transparent by the cavity through destructive Fano interferences. In this work, we tackle this issue by offering a new plasmonic–photonic interaction framework. By coupling to a photonic crystal guided resonance, a gold nanostar delivers 1 order of magnitude amplified absorption, and the ultrasharp Lorentzian-line-shaped hybrid resonance is continuously tunable over a broad spectral range by scanning of the incidence angle. Our intuitive coupled mode model reveals that a distinct optical pathway highlighting the cavit...

Journal ArticleDOI
TL;DR: In this article, the authors show that strong light-matter coupling can be used to overcome a long-standing problem that has prevented efficient optical emission from carbon nanotubes, which is due to the fast nonradiative scattering to the dark exciton state having a lower energy.
Abstract: We show that strong light–matter coupling can be used to overcome a long-standing problem that has prevented efficient optical emission from carbon nanotubes. The luminescence from the nominally bright exciton state of carbon nanotubes is quenched due to the fast nonradiative scattering to the dark exciton state having a lower energy. We present a theoretical analysis to show that by placing carbon nanotubes in an optical microcavity the bright excitonic state may be split into two hybrid exciton–polariton states, while the dark state remains unaltered. For sufficiently strong coupling between the bright exciton and the cavity, we show that the energy of the lower polariton may be pushed below that of the dark exciton. This overturning of the relative energies of the bright and dark excitons prevents the dark exciton from quenching the emission. Our results pave the way for a new approach to band-engineering the properties of nanoscale optoelectronic devices.

Journal ArticleDOI
TL;DR: In this article, a gold nanoparticles were coupled to WGM resonators to increase the magnitude of resonance shifts via plasmonic enhancement of the electric field, which results in increased scattering from the WGM which degrades its quality (Q) factor, making it less sensitive to extremely small frequency shifts caused by small molecules or protein conformational changes.
Abstract: Whispering gallery mode (WGM) microtoroid optical resonators have been effectively used to sense low concentrations of biomolecules down to the single molecule limit. Optical WGM biochemical sensors such as the microtoroid operate by tracking changes in resonant frequency as particles enter the evanescent near field of the resonator. Previously, gold nanoparticles have been coupled to WGM resonators to increase the magnitude of resonance shifts via plasmonic enhancement of the electric field. However, this approach results in increased scattering from the WGM, which degrades its quality (Q) factor, making it less sensitive to extremely small frequency shifts caused by small molecules or protein conformational changes. Here, we show using simulation that precisely positioned trimer gold nanostructures generate dark modes that suppress radiation loss and can achieve high (>106) Q with an electric-field intensity enhancement of 4300, which far exceeds that of a single rod (∼2500 times). Through an overall evaluation of a combined enhancement factor, which includes the Q factor of the system, the sensitivity of the trimer system was improved 105× versus 84× for a single rod. Further simulations demonstrate that unlike a single rod system, the trimer is robust to orientation changes and has increased capture area. We also conduct stability tests to show that small positioning errors do not greatly impact the result.

Journal ArticleDOI
24 Apr 2019-ACS Nano
TL;DR: An optical microcavity approach capable of efficient in-plane and out-of-plane confinement of light is presented, which results in a WS2 photoluminescence enhancement by a factor of 10 compared to that of the unstructured substrate at room temperature.
Abstract: Light-matter interactions with two-dimensional materials gained significant attention in recent years, leading to the reporting of weak and strong coupling regimes and effective nanolaser operation with various structures. Particularly, future applications involving monolayer materials in waveguide-coupled on-chip-integrated circuitry and valleytronic nanophotonics require controlling, directing, and optimizing photoluminescence. In this context, photoluminescence enhancement from monolayer transition-metal dichalcogenides on patterned semiconducting substrates becomes attractive. It is demonstrated in our work using focused-ion-beam-etched GaP and monolayer WS2 suspended on hexagonal boron nitride buffer sheets. We present an optical microcavity approach capable of efficient in-plane and out-of-plane confinement of light, which results in a WS2 photoluminescence enhancement by a factor of 10 compared to that of the unstructured substrate at room temperature. The key concept is the combination of interference effects in both the horizontal direction using a bull's-eye-shaped circular Bragg grating and in the vertical direction by means of a multiple-reflection model with optimized etch depth of circular air-GaP structures for maximum constructive interference effects of the applied pump and expected emission light.

Journal ArticleDOI
TL;DR: In this article, the authors demonstrate control over light-matter coupling at room temperature combining a field effect transistor (FET) with a tuneable optical microcavity, which enables strong Coulomb repulsion between free electrons.
Abstract: We demonstrate control over light-matter coupling at room temperature combining a field effect transistor (FET) with a tuneable optical microcavity. Our microcavity FET comprises a monolayer tungsten disulfide WS$_2$ semiconductor which was transferred onto a hexagonal boron nitride flake that acts as a dielectric spacer in the microcavity, and as an electric insulator in the FET. In our tuneable system, strong coupling between excitons in the monolayer WS$_2$ and cavity photons can be tuned by controlling the cavity length, which we achieved with excellent stability, allowing us to choose from the second to the fifth order of the cavity modes. Once we achieve the strong coupling regime, we then modify the oscillator strength of excitons in the semiconductor material by modifying the free electron carrier density in the conduction band of the WS$_2$. This enables strong Coulomb repulsion between free electrons, which reduces the oscillator strength of excitons until the Rabi splitting completely disappears. We controlled the charge carrier density from 0 up to 3.2 $\times$ 10$^{12}$ cm$^{-2}$, and over this range the Rabi splitting varies from a maximum value that depends on the cavity mode chosen, down to zero, so the system spans the strong to weak coupling regimes.

Journal ArticleDOI
TL;DR: The quasi-2D Ruddlesden-Popper perovskites possess a tailorable quantum well structure and outstanding optical properties as mentioned in this paper, which have evidently enhanced photoluminescence.
Abstract: Quasi-2D Ruddlesden-Popper perovskites possess a tailorable quantum well structure and outstanding optical properties. Herein, we study their diverse phase-separation phenomena and the resulting microcrystals (∼1 μm), which have evidently enhanced photoluminescence. Lasing based on these microcrystals in a vertical single-mode optical microcavity has also been achieved, featuring a low threshold of ∼500.0 μJ/cm2 pumped by a nanosecond pulsed laser (355 nm, pulse width 8 ns, 1 kHz). This work makes the quasi-2D perovskite microcrystals potential candidates to be gain materials for continuous wave lasing.

Posted Content
TL;DR: It is shown that, for single-molecule strong coupling with the photon mode, nonadiabatic molecular dynamics produces mixing of polariton manifolds with differing number of excitations, without the need of counterrotating light-matter coupling terms.
Abstract: Quantum dynamics of the photoisomerization of a single 3,3'-diethyl-2,2'-thiacynine iodide molecule embedded in an optical microcavity was theoretically studied. The molecule was coupled to a single cavity mode via the quantum Rabi Hamiltonian, and the corresponding time-dependent Schrodinger equation starting with a purely molecular excitation was solved using the Multiconfigurational Time-Dependent Hartree Method (MCTDH). We show that, for single-molecule strong coupling with the photon mode, nonadiabatic molecular dynamics produces mixing of polariton manifolds with differing number of excitations, without the need of counterrotating light-matter coupling terms. As a consequence, an electronic excitation of the molecule at {\it cis} configuration leads to the generation of photon pairs in the {\it trans} configuration upon isomerization. Conditions for this phenomenon to be operating in the collective strong light-matter coupling regime are discussed and found to be unfeasible for the present system, based on simulations of two molecules inside the microcavity. Yet, our finding suggests a new mechanism that, without ultrastrong coupling, achieves photon down-conversion by exploiting the emergent molecular dynamics arising in polaritonic architectures.

Journal ArticleDOI
TL;DR: This technique provides a new way to prepare semiconductor nanotubes for new photonic devices and photoelectric applications through a simple thermal evaporation co-deposition technique with Sn metal nanowire templating and ejection.
Abstract: Nanotubes are often formed by the folding of one-layer or multilayer compounds under microscopic catalytic growth conditions. Here, CdS nanotubes with tunable wall sizes and optical microcavities were prepared via a simple thermal evaporation co-deposition technique with Sn metal nanowire templating and ejection. Compared to core-shell Sn/CdS nanowires, which have poor microcavity quality, the hollow/CdS nanotubes have a higher quality factor (Q) that can reach approximately 400 in the spectral range of 550-800 nm when excited by a continuous-wave 405 nm laser. This high Q factor leads to low-threshold lasing and line-width narrowing due to the mode selection, which are important in many fields, including lasers, sensors, communications, and optical storage. A theoretical mode analysis of the hollow/CdS nanotubes with different thicknesses addressed their microcavity mode confinement and enhancements. This technique provides a new way to prepare semiconductor nanotubes for new photonic devices and photoelectric applications.


Journal ArticleDOI
TL;DR: In this paper, an oscillatory behavior of the second-order photon number correlation function is observed in two-dimensional photon gases in a dye-filled optical microcavity and explained by a theoretical model derived from nonlinear rate equations.
Abstract: The dynamics of a Bose-Einstein condensate of photons is investigated experimentally and theoretically. An oscillatory behavior of the second-order photon number correlation function is observed in two-dimensional photon gases in a dye-filled optical microcavity and explained by a theoretical model derived from nonlinear rate equations. This behavior is traced back to the weakly driven-dissipative nature of the system, leading to a breaking of time-reversal symmetry.

Journal ArticleDOI
TL;DR: The experimental results demonstrate that WGM lasing has unique advantages in the real-time monitoring of enzymatic reactions compared, for instance, with observation of the optical appearance under a polarized optical microscope.
Abstract: A new strategy is reported here to monitor the enzymatic reactions in real time by using whispering gallery mode (WGM) lasing. The optical microcavity is formed via the self-assembly of an ultraviolet (UV)-treated nematic liquid crystal (LC) 4-cyano-4’-pentylbiphenyl (5CB). The single UV-treated 5CB microdroplet serves as both optical resonator and sensing reactor. The microdroplet configuration transitions induced wavelength shift in the WGM lasing spectra can be used as an indicator for the enzymatic reaction. The proposed sensor has a sub-microgram detection limit of urease (∼0.5 µg/ml), which is lower than the detection limit of currently available urease sensor based on LC materials. Our experimental results demonstrate that WGM lasing has unique advantages in the real-time monitoring of enzymatic reactions compared, for instance, with observation of the optical appearance under a polarized optical microscope.

Journal ArticleDOI
TL;DR: This study encapsulated organic molecules with relatively low unoriented dipole moments in the polymer matrix, placed them in tunable optical microcavity and realized controllable modification of the broad photoluminescence (PL) emission of these molecules in strong coupling regime at room temperature.
Abstract: Resonance interaction between a localized electromagnetic field and excited states in molecules paves the way to control fundamental properties of a matter. In this study, we encapsulated organic molecules with relatively low unoriented dipole moments in the polymer matrix, placed them in tunable optical microcavity and realized, for the first time, controllable modification of the broad photoluminescence (PL) emission of these molecules in strong coupling regime at room temperature. Notably, while in most previous studies it was reported that the single mode dominates in the PL signal (radiation of the so-called branch of the lower polariton), here we report on the observation of two distinct PL peaks, evolution of which has been followed as the microcavity mode is detuned from the excitonic resonance. A significant Rabi splitting estimated from the modified PL spectra was as large as 225 meV. The developed approach can be used both in fundamental research of resonant light-mater coupling and its practical applications in sensing and development of coherent spontaneous emission sources using a combination of carefully designed microcavity with a wide variety of organic molecules.

Journal ArticleDOI
TL;DR: In this article, a Se/Te-based planar microcavity comprising a single CdSe/(Cd,Mg)Se quantum well was designed to achieve coherent light generation.
Abstract: Lasing relies on light amplification in the active medium of an optical resonator. There are three lasing regimes in the emission from a quantum well coupled to a semiconductor microcavity. Polariton lasing in the strong light–matter coupling regime arises from the stimulated scattering of exciton-polaritons. Photon lasing in the weak coupling regime relies on either of two mechanisms: the stimulated recombination of excitons, or of an electron–hole plasma. So far, only one or two out of these three regimes have been reported for a given structure, independently of the material system studied. Here, we report on all three lasing regimes and provide evidence for a three-threshold behavior in the emission from a photonic trap in a Se/Te-based planar microcavity comprising a single CdSe/(Cd,Mg)Se quantum well. Our work establishes the so far unsettled relation between lasing regimes that differ by their light-matter coupling strength and degree of electron–hole Coulomb correlation. Semiconductor microcavities coupled to a quantum well can produce three regimes of coherent light generation depending on the nature of the light–matter and electron–hole interactions. The authors design a Se/Te based microcavity containing a single quantum well which enables them to achieve all three lasing regimes in the one device.