scispace - formally typeset
Search or ask a question

Showing papers on "Spontaneous emission published in 2018"


Journal ArticleDOI
TL;DR: It is shown that a PLQY up to 79% and linewidth of 20 nm can be reached by controlling crystal rigidity and electron–phonon interactions, and that molecular motion is slowest, and rigidity greatest, in the brightest emitter.
Abstract: Low-dimensional perovskites have—in view of their high radiative recombination rates—shown great promise in achieving high luminescence brightness and colour saturation. Here we investigate the effect of electron–phonon interactions on the luminescence of single crystals of two-dimensional perovskites, showing that reducing these interactions can lead to bright blue emission in two-dimensional perovskites. Resonance Raman spectra and deformation potential analysis show that strong electron–phonon interactions result in fast non-radiative decay, and that this lowers the photoluminescence quantum yield (PLQY). Neutron scattering, solid-state NMR measurements of spin–lattice relaxation, density functional theory simulations and experimental atomic displacement measurements reveal that molecular motion is slowest, and rigidity greatest, in the brightest emitter. By varying the molecular configuration of the ligands, we show that a PLQY up to 79% and linewidth of 20 nm can be reached by controlling crystal rigidity and electron–phonon interactions. Designing crystal structures with electron–phonon interactions in mind offers a previously underexplored avenue to improve optoelectronic materials' performance. Films of exfoliated crystals of two-dimensional hybrid metal halide perovskites with phenyl groups as organic cations show increased molecular rigidity, reduced electron–phonon interactions and blue emission with photoluminescence quantum yield approaching 80%.

396 citations


Journal ArticleDOI
TL;DR: The fully inorganic, perovskite‐derived zero‐dimensional SnII material Cs4SnBr6 is presented that exhibits room‐temperature broad‐band photoluminescence centered at 540 nm with a quantum yield (QY) of 15±5 %.
Abstract: The spatial localization of charge carriers to promote the formation of bound excitons and concomitantly enhance radiative recombination has long been a goal for luminescent semiconductors. Zero-dimensional materials structurally impose carrier localization and result in the formation of localized Frenkel excitons. Now the fully inorganic, perovskite-derived zero-dimensional SnII material Cs4 SnBr6 is presented that exhibits room-temperature broad-band photoluminescence centered at 540 nm with a quantum yield (QY) of 15±5 %. A series of analogous compositions following the general formula Cs4-x Ax Sn(Br1-y Iy )6 (A=Rb, K; x≤1, y≤1) can be prepared. The emission of these materials ranges from 500 nm to 620 nm with the possibility to compositionally tune the Stokes shift and the self-trapped exciton emission bands.

206 citations


Journal ArticleDOI
TL;DR: In high-efficiency PeLEDs based on colloidal perovskite nanocrystals synthesized at room temperature possessing dominant first-order excitonic radiation, it is found that the Auger nonradiative recombination is effectively suppressed in low driving current density range.
Abstract: Lead-halide perovskites have been attracting attention for potential use in solid-state lighting Following the footsteps of solar cells, the field of perovskite light-emitting diodes (PeLEDs) has been growing rapidly Their application prospects in lighting, however, remain still uncertain due to a variety of shortcomings in device performance including their limited levels of luminous efficiency achievable thus far Here we show high-efficiency PeLEDs based on colloidal perovskite nanocrystals (PeNCs) synthesized at room temperature possessing dominant first-order excitonic radiation (enabling a photoluminescence quantum yield of 71% in solid film), unlike in the case of bulk perovskites with slow electron–hole bimolecular radiative recombination (a second-order process) In these PeLEDs, by reaching charge balance in the recombination zone, we find that the Auger nonradiative recombination, with its significant role in emission quenching, is effectively suppressed in low driving current density range

189 citations


Journal ArticleDOI
TL;DR: Proposed molecular quantum gate takes advantage of internal coherence and resonant electric dipolar interaction with high fidelity and optical scalability to solve the problem of quantum entanglement in liquid chromatography.
Abstract: We propose a two-qubit gate based on dipolar exchange interactions between individually addressable ultracold polar molecules in an array of optical dipole traps. Our proposal treats the full Hamiltonian of the 1Σ+ molecule NaCs, utilizing a pair of nuclear spin states as storage qubits. A third rotationally excited state with rotation-hyperfine coupling enables switchable electric dipolar exchange interactions between two molecules to generate an iSWAP gate. All three states are insensitive to external magnetic and electric fields. Impacts on gate fidelity due to coupling to other molecular states, imperfect ground-state cooling, blackbody radiation and vacuum spontaneous emission are small, leading to potential fidelity above 99.99% in a coherent quantum system that can be scaled by purely optical means.

156 citations


Journal ArticleDOI
TL;DR: An acoustical analog of a circuit quantum electrodynamics system that leverages acoustic properties to enable strong multimode coupling in the dispersive regime while suppressing spontaneous emission to unconfined modes is demonstrated.
Abstract: We demonstrate an acoustical analog of a circuit quantum electrodynamics system that leverages acoustic properties to enable strong multimode coupling in the dispersive regime while suppressing spontaneous emission to unconfined modes. Specifically, we fabricate and characterize a device that comprises a flux tunable transmon coupled to a $300\text{ }\text{ }\ensuremath{\mu}\mathrm{m}$ long surface acoustic wave resonator. For some modes, the qubit-cavity coupling reaches 6.5 MHz, exceeding the cavity loss rate (200 kHz), qubit linewidth (1.1 MHz), and the cavity free spectral range (4.8 MHz), placing the device in both the strong coupling and strong multimode regimes. With the qubit detuned from the confined modes of the cavity, we observe that the qubit linewidth strongly depends on its frequency, as expected for spontaneous emission of phonons, and we identify operating frequencies where this emission rate is suppressed.

146 citations


Journal ArticleDOI
TL;DR: The different modulating effects of photonic crystal dimensions, light-emitter positions, Photonic crystal structure type, and the refractive index of photonics crystal building blocks are highlighted with the aim of evaluating the fundamental principles that determine light propagation.
Abstract: The modulation of luminescence is essential because unwanted spontaneous-emission modes have a negative effect on the performance of luminescence-based photonic devices. Photonic crystals are promising materials for the control of light emission because of the variation in the local density of optical modes within them. They have been widely investigated for the manipulation of the emission intensity and lifetime of light emitters. Several groups have achieved greatly enhanced emission by depositing emitters on the surface of photonic crystals. Herein, the different modulating effects of photonic crystal dimensions, light-emitter positions, photonic crystal structure type, and the refractive index of photonic crystal building blocks are highlighted, with the aim of evaluating the fundamental principles that determine light propagation. The applications of using photonic crystals to manipulate spontaneous emission in light-emitting diodes and sensors are also reviewed. In addition, potential future challenges and improvements in this field are presented.

134 citations


Journal ArticleDOI
TL;DR: Strong enhancement of spontaneous emission rate of a single silicon-vacancy center in diamond embedded within a monolithic optical cavity is demonstrated, reaching a regime in which the excited-state lifetime is dominated by spontaneous emission into the cavity mode.
Abstract: Quantum emitters are an integral component for a broad range of quantum technologies, including quantum communication, quantum repeaters, and linear optical quantum computation. Solid-state color centers are promising candidates for scalable quantum optics due to their long coherence time and small inhomogeneous broadening. However, once excited, color centers often decay through phonon-assisted processes, limiting the efficiency of single-photon generation and photon-mediated entanglement generation. Herein, we demonstrate strong enhancement of spontaneous emission rate of a single silicon-vacancy center in diamond embedded within a monolithic optical cavity, reaching a regime in which the excited-state lifetime is dominated by spontaneous emission into the cavity mode. We observe 10-fold lifetime reduction and 42-fold enhancement in emission intensity when the cavity is tuned into resonance with the optical transition of a single silicon-vacancy center, corresponding to 90% of the excited-state energy decay occurring through spontaneous emission into the cavity mode. We also demonstrate the largest coupling strength (g/2π = 4.9 ± 0.3 GHz) and cooperativity (C = 1.4) to date for color-center-based cavity quantum electrodynamics systems, bringing the system closer to the strong coupling regime.

129 citations


Journal ArticleDOI
04 Jan 2018-ACS Nano
TL;DR: It is demonstrated, experimentally and theoretically, that the photon emission from gold nanorods can be viewed as a Purcell effect enhanced radiative recombination of hot carriers and the main photoluminescence peak coinciding with the longitudinal surface plasmon resonance.
Abstract: We demonstrate, experimentally and theoretically, that the photon emission from gold nanorods can be viewed as a Purcell effect enhanced radiative recombination of hot carriers. By correlating the single-particle photoluminescence spectra and quantum yields of gold nanorods measured for five different excitation wavelengths and varied excitation powers, we illustrate the effects of hot carrier distributions evolving through interband and intraband transitions and the photonic density of states on the nanorod photoluminescence. Our model, using only one fixed input parameter, describes quantitatively both emission from interband recombination and the main photoluminescence peak coinciding with the longitudinal surface plasmon resonance.

117 citations


Journal ArticleDOI
TL;DR: The emission properties and luminescence mechanism of all-inorganic perovskite CsPbBr3 nanosheets (NSs) were investigated using steady-state and time-resolved photoluminescence (PL) spectroscopic techniques and shed some light on the complicated luminescent mechanism.
Abstract: Very recently, all-inorganic perovskite CsPbX3 (X = Cl, Br, I) nanostructures such as nanoparticles, nanoplates, and nanorods have been extensively explored. These CsPbX3 nanostructures exhibit excellent optical properties; however, the photophysics involved is not yet clear. Herein, the emission properties and luminescence mechanism of CsPbBr3 nanosheets (NSs) were investigated using steady-state and time-resolved photoluminescence (PL) spectroscopic techniques. Moreover, two kinds of excitonic emissions (Peak 1 and Peak 2) are observed at low temperatures (<80 K) under the conditions of low excitation level. They are revealed to stem from the radiative recombination of trapped and free excitons by examining their spectral features and emission intensity dependences on excitation power. Thermally induced exchange between the two kinds of excitons is found and modeled quantitatively; this has led to the determination of an activation energy of 13 meV. Thermal redistribution of trapped excitons and thermal expansion-induced blueshift of the bandgap are jointly responsible for the abnormal temperature dependence of the position of Peak 1, whereas the latter is predominant for the monotonic blueshift of the position of Peak 2 with an increase in temperature. These results and findings shed some light on the complicated luminescence mechanism of CsPbBr3 NSs.

112 citations


Journal ArticleDOI
TL;DR: In this article, the authors proposed a new paradigm for quantum simulation of spin-1/2 arrays providing unprecedented flexibility and allowing one to explore domains beyond the reach of other platforms by transcribing the system of interest into another with the same dynamics but with interaction parameters under control and with experimental access to all relevant observables.
Abstract: The main objective of quantum simulation is an in-depth understanding of many-body physics. It is important for fundamental issues (quantum phase transitions, transport, . . . ) and for the development of innovative materials. Analytic approaches to many-body systems are limited and the huge size of their Hilbert space makes numerical simulations on classical computers intractable. A quantum simulator avoids these limitations by transcribing the system of interest into another, with the same dynamics but with interaction parameters under control and with experimental access to all relevant observables. Quantum simulation of spin systems is being explored with trapped ions, neutral atoms and superconducting devices. We propose here a new paradigm for quantum simulation of spin-1/2 arrays providing unprecedented flexibility and allowing one to explore domains beyond the reach of other platforms. It is based on laser-trapped circular Rydberg atoms. Their long intrinsic lifetimes combined with the inhibition of their microwave spontaneous emission and their low sensitivity to collisions and photoionization make trapping lifetimes in the minute range realistic with state-of-the-art techniques. Ultra-cold defect-free circular atom chains can be prepared by a variant of the evaporative cooling method. This method also leads to the individual detection of arbitrary spin observables. The proposed simulator realizes an XXZ spin-1/2 Hamiltonian with nearest-neighbor couplings ranging from a few to tens of kHz. All the model parameters can be tuned at will, making a large range of simulations accessible. The system evolution can be followed over times in the range of seconds, long enough to be relevant for ground-state adiabatic preparation and for the study of thermalization, disorder or Floquet time crystals. This platform presents unrivaled features for quantum simulation.

111 citations


Journal ArticleDOI
TL;DR: In this paper, a transmon qubit is coupled to a superconducting metamaterial with a deep sub-wavelength lattice constant (λ/60), which is formed by periodically loading a transmission line with compact, low-loss, low disorder lumped-element microwave resonators.
Abstract: Embedding tunable quantum emitters in a photonic bandgap structure enables control of dissipative and dispersive interactions between emitters and their photonic bath. Operation in the transmission band, outside the gap, allows for studying waveguide quantum electrodynamics in the slow-light regime. Alternatively, tuning the emitter into the bandgap results in finite-range emitter–emitter interactions via bound photonic states. Here, we couple a transmon qubit to a superconducting metamaterial with a deep sub-wavelength lattice constant (λ/60). The metamaterial is formed by periodically loading a transmission line with compact, low-loss, low-disorder lumped-element microwave resonators. Tuning the qubit frequency in the vicinity of a band-edge with a group index of ng = 450, we observe an anomalous Lamb shift of −28 MHz accompanied by a 24-fold enhancement in the qubit lifetime. In addition, we demonstrate selective enhancement and inhibition of spontaneous emission of different transmon transitions, which provide simultaneous access to short-lived radiatively damped and long-lived metastable qubit states.

Journal ArticleDOI
TL;DR: The dynamic tuning of spontaneous emission from a Mie-resonant dielectric metasurface that is situated on a fluorescent substrate and embedded into a liquid crystal cell is experimentally demonstrated and is demonstrated to be a viable strategy to realize flat tunable light sources based on dielectrics meetasurfaces.
Abstract: Mie-resonant dielectric metasurfaces offer comprehensive opportunities for the manipulation of light fields with high efficiency. Additionally, various strategies for the dynamic tuning of the optical response of such metasurfaces were demonstrated, making them important candidates for reconfigurable optical devices. However, dynamic control of the light-emission properties of active Mie-resonant dielectric metasurfaces by an external control parameter has not been demonstrated so far. Here, we experimentally demonstrate the dynamic tuning of spontaneous emission from a Mie-resonant dielectric metasurface that is situated on a fluorescent substrate and embedded into a liquid crystal cell. By switching the liquid crystal from the nematic state to the isotropic state via control of the cell temperature, we induce a shift of the spectral position of the metasurface resonances. This results in a change of the local photonic density of states, which, in turn, governs the enhancement of spontaneous emission fro...

Journal ArticleDOI
01 Jul 2018-Nature
TL;DR: In this article, the decay of an excited atom undergoing spontaneous photon emission into the fluctuating quantum-electrodynamic vacuum is an emblematic example of the dynamics of an open quantum system.
Abstract: The decay of an excited atom undergoing spontaneous photon emission into the fluctuating quantum-electrodynamic vacuum is an emblematic example of the dynamics of an open quantum system. Recent experiments have demonstrated that the gapped photon dispersion in periodic structures, which prevents photons in certain frequency ranges from propagating, can give rise to unusual spontaneous-decay behaviour, including the formation of dissipative bound states1–3. So far, these effects have been restricted to the optical domain. Here we demonstrate similar behaviour in a system of artificial emitters, realized using ultracold atoms in an optical lattice, which decay by emitting matter-wave, rather than optical, radiation into free space. By controlling vacuum coupling and the excitation energy, we directly observe exponential and partly reversible non-Markovian dynamics and detect a tunable bound state that contains evanescent matter waves. Our system provides a flexible platform for simulating open-system quantum electrodynamics and for studying dissipative many-body physics with ultracold atoms4–6. An open quantum system containing ultracold rubidium atoms trapped in an optical lattice undergoes spontaneous emission of matter waves into free space.

Journal ArticleDOI
TL;DR: The Mie resonances in silicon nanoparticles are utilized to demonstrate visible white-light emission, both from free-standing spheres and particles etched on a silicon-on-insulator substrate.
Abstract: As one of the most important semiconductors, silicon has been used to fabricate electronic devices, waveguides, detectors, solar cells, etc However, the indirect bandgap and low quantum efficiency (10−7) hinder the use of silicon for making good emitters For integrated photonic circuits, silicon-based emitters with sizes in the range of 100−300 nm are highly desirable Here, we show the use of the electric and magnetic resonances in silicon nanoparticles to enhance the quantum efficiency and demonstrate the white-light emission from silicon nanoparticles with feature sizes of ~200 nm The magnetic and electric dipole resonances are employed to dramatically increase the relaxation time of hot carriers, while the magnetic and electric quadrupole resonances are utilized to reduce the radiative recombination lifetime of hot carriers This strategy leads to an enhancement in the quantum efficiency of silicon nanoparticles by nearly five orders of magnitude as compared with bulk silicon, taking the three-photon-induced absorption into account As an indirect semiconductor, silicon shows notoriously inefficient luminescence Here, the authors utilize the Mie resonances in silicon nanoparticles to demonstrate visible white-light emission, both from free-standing spheres and particles etched on a silicon-on-insulator substrate

Journal ArticleDOI
TL;DR: In this article, quasi-2D CsPbBr3 quantum wells homogeneously surrounded by inorganic crystalline Cs4pbBr6 of large bandgap are grown.
Abstract: Metal halide perovskites are rising as a competitive material for next-generation light-emitting diodes (LEDs). However, the development of perovskite LEDs is impeded by their fast carriers diffusion and poor stability in bias condition. Herein, quasi-2D CsPbBr3 quantum wells homogeneously surrounded by inorganic crystalline Cs4PbBr6 of large bandgap are grown. The centralization of carriers in nanoregion facilitates radiative recombination and brings much enhanced luminescence quantum yield. The external quantum efficiency and luminescence intensity of the LEDs based on this nanocomposite are one order of magnitude higher than the conventional low-dimensional perovskite. Meanwhile, the use of inorganic nanocomposite materials brings much improved device operation lifetime under constant electrical field.

Journal ArticleDOI
21 Mar 2018-ACS Nano
TL;DR: By effectively controlling the crystal growth, perovskite films composed of uniform nanosized single crystals produced by introducing bulky amine ligands and performing the growth at a lower temperature maximized the radiative bimolecular recombination yield by reducing the trap density and spatially confining the charges.
Abstract: Organic–inorganic hybrid perovskites are emerging as promising emitting materials due to their narrow full-width at half-maximum emissions, color tunability, and high photoluminescence quantum yields (PLQYs). However, the thermal generation of free charges at room temperature results in a low radiative recombination rate and an excitation-intensity-dependent PLQY, which is associated with the trap density. Here, we report perovskite films composed of uniform nanosized single crystals (average diameter = 31.7 nm) produced by introducing bulky amine ligands and performing the growth at a lower temperature. By effectively controlling the crystal growth, we maximized the radiative bimolecular recombination yield by reducing the trap density and spatially confining the charges. Finally, highly bright and efficient green emissive perovskite light-emitting diodes that do not suffer from electroluminescence blinking were achieved with a luminance of up to 55 400 cd m–2, current efficiency of 55.2 cd A–1, and exte...

Journal ArticleDOI
TL;DR: In this article, the sharp corner of a metal nanocube is used to deform a two-dimensional material for electric field enhancement and cavity-enhancement of a single-quantum emitter.
Abstract: Solid-state single-quantum emitters are a crucial resource for on-chip photonic quantum technologies and require efficient cavity-emitter coupling to realize quantum networks beyond the single-node level. Previous approaches to enhance light-matter interactions rely on forming nanocavities around randomly located quantum dots or color centers but lack spatial control of the quantum emitter itself that is required for scaling. Here we demonstrate a deterministic approach to achieve Purcell-enhancement at lithographically defined locations using the sharp corner of a metal nanocube for both electric field enhancement and to deform a two-dimensional material. For a 3 by 4 array of strain-induced exciton quantum emitters formed into monolayer WSe2 we show spontaneous emission rate enhancement with Purcell-factors (FP) up to FP=1050 (average FP=272), single-photon purification, and cavity-enhanced quantum yields increasing from initially 1 % to 15 %. The utility of our nanoplasmonic platform is applicable to other 2D material, including boron nitride, opening new inroads in quantum photonics.

Journal ArticleDOI
TL;DR: In this article, the authors studied light emission from square arrays of Mie-resonant silicon nano-antennas situated on a fluorescent glass substrate, showing that the spectral maximum of the emission coincides with the antenna resonance positions observed in linear-optical transmittance spectra, and observed that the nanoantenna array induces a reshaping of the resonantly enhanced emission in the air half-space into a narrow lobe directed out of the substrate plane.
Abstract: We study light emission from square arrays of Mie-resonant silicon nanoantennas situated on a fluorescent glass substrate When the spectral positions of the silicon nanoantennas’ resonances overlap with the intrinsic emission from the glass, the emission is selectively enhanced for certain spectral and spatial frequencies detemined by the design of the nanoantenna array We measure the emission spectra of the coupled system for a systematic variation of the nanoantenna geometry, showing that the spectral maximum of the emission coincides with the antenna resonance positions observed in linear-optical transmittance spectra Furthermore, we study the directionality of the emission by back focal plane imaging and numerical calculations based on the Fourier modal method and the reciprocity principle We observe that the nanoantenna array induces a reshaping of the resonantly enhanced emission in the air half-space into a narrow lobe directed out of the substrate plane This reshaping is explained by coherent

Journal ArticleDOI
TL;DR: In this paper, a strain induced single photon source using a WSe2 monolayer on a silver substrate, coated with a very thin dielectric layer, is described.
Abstract: Atomic monolayers of transition metal dichalcogenides represent an emerging material platform for the implementation of ultracompact quantum light emitters via strain engineering. In this framework, we discuss experimental results on creation of strain induced single photon sources using a WSe2 monolayer on a silver substrate, coated with a very thin dielectric layer. We identify quantum emitters that are formed at various locations in the sample. Their emission is highly linearly polarized, stable in linewidth, and decay times down to 100 ps are observed. We provide numerical calculations of our monolayer-metal device platform to assess the strength of the radiative decay rate enhancement by the presence of the plasmonic structure. We believe that our results represent a crucial step toward the ultracompact integration of high performance single photon sources in nanoplasmonic devices and circuits.

Journal ArticleDOI
TL;DR: Efficient and stable green emissive perovskite light‐emitting diodes (PeLEDs) with an external quantum efficiency of 14.6% are demonstrated through compositional, dimensional, and interfacial modulations of MHPs for significantly improved device efficiency, photostability, and operational stability of PeLEDs.
Abstract: Metal halide perovskites (MHPs) have emerged as promising materials for light-emitting diodes owing to their narrow emission spectrum and wide range of color tunability. However, the low exciton binding energy in MHPs leads to a competition between the trap-mediated nonradiative recombination and the bimolecular radiative recombination. Here, efficient and stable green emissive perovskite light-emitting diodes (PeLEDs) with an external quantum efficiency of 14.6% are demonstrated through compositional, dimensional, and interfacial modulations of MHPs. The interfacial energetics and optoelectronic properties of the perovskite layer grown on a nickel oxide (NiO x ) and poly(3,4-ethylenedioxythiophene):polystyrene sulfonate hole injection interfaces are investigated. The better interface formed between the NiO x /perovskite layers in terms of lower density of traps/defects, as well as more balanced charge carriers in the perovskite layer leading to high recombination yield of carriers are the main reasons for significantly improved device efficiency, photostability of perovskite, and operational stability of PeLEDs.

Journal ArticleDOI
TL;DR: In this article, the role of the Purcell effect in the stimulated and spontaneous emission rates of semiconductor lasers is investigated, taking into account the carriers' spatial distribution in the volume of the active region over a wide range of cavity dimensions and emitter/cavity linewidths, enabling the detailed modeling of the static and dynamic characteristics of either micro- or nano-scale lasers using singlemode rate-equations analysis.
Abstract: Nanoscale semiconductor lasers have been developed recently using either metal, metallo-dielectric, or photonic crystal nanocavities. While the technology of nanolasers is steadily being deployed, their expected performance for on-chip optical interconnects is still largely unknown due to a limited understanding of some of their key features. Specifically, as the cavity size is reduced with respect to the emission wavelength, the stimulated and the spontaneous emission rates are modified, which is known as the Purcell effect in the context of cavity quantum electrodynamics. This effect is expected to have a major impact in the “threshold-less” behavior of nanolasers and in their modulation speed; but its role is poorly understood in practical laser structures, characterized by significant homogeneous and inhomogeneous broadening and by a complex spatial distribution of the active material and cavity field. In this paper, we investigate the role of the Purcell effect in the stimulated and spontaneous emission rates of semiconductor lasers taking into account the carriers’ spatial distribution in the volume of the active region over a wide range of cavity dimensions and emitter/cavity linewidths, enabling the detailed modeling of the static and dynamic characteristics of either micro- or nano-scale lasers using single-mode rate-equations analysis. The ultimate limits of scaling down these nanoscale light sources in terms of Purcell enhancement and modulation speed are also discussed showing that the ultrafast modulation properties predicted in nanolasers are a direct consequence of the enhancement of the stimulated emission rate via reduction of the mode volume.

Journal ArticleDOI
TL;DR: In this article, the authors demonstrate a swap operation between the states of a single photon and a single atom using a nanofibre-coupled microsphere resonator coupled to single Rb atoms.
Abstract: Deterministic quantum interactions between single photons and single quantum emitters are a vital building block towards the distribution of quantum information between remote systems1–4. Deterministic photon–atom state transfer has previously been demonstrated with protocols that include active feedback or synchronized control pulses5–10. Here we demonstrate a passive swap operation between the states of a single photon and a single atom. The underlying mechanism is single-photon Raman interaction11–15—an interference-based scheme that leads to deterministic interaction between two photonic modes and the two ground states of a Λ-system. Using a nanofibre-coupled microsphere resonator coupled to single Rb atoms, we swap a photonic qubit into the atom and back, demonstrating fidelities exceeding the classical threshold of 2/3 in both directions. In this simultaneous write and read process, the returning photon, which carries the readout of the atomic qubit, also heralds the successful arrival of the write photon. Requiring no control fields, this single-step gate takes place automatically at the timescale of the atom’s cavity-enhanced spontaneous emission. Applicable to any waveguide-coupled Λ-system, this mechanism, which can also be harnessed to construct universal gates16,17, provides a versatile building block for the modular scaling up of quantum information systems. Demonstration of a passive swap gate between the states of a fibre-guided photonic qubit and a single atom.

Journal ArticleDOI
TL;DR: This work conducted spectroscopic studies of the excitons and biexciton dynamics in single CsPbBr3 perovskite quantum dots and found that while the rates of radiative recombination remain essentially constant, the overall relaxation process is dominated by nonradiative recombinations of single exciton and bIExcitons.
Abstract: Colloidal lead halide perovskite quantum dots, due to their optical versatility and facile solution processability, have been recently recognized as components of various optoelectronic devices. Detailed understanding of their exciton recombination dynamics at the single-particle level is necessary for utilizing their full potential. We conducted spectroscopic studies of the excitons and biexciton dynamics in single CsPbBr3 perovskite quantum dots. It was found that while the rates of radiative recombination remain essentially constant, the overall relaxation process is dominated by nonradiative recombination of single excitons and biexcitons. The radiative lifetime scaling is determined to be ∼1.0 for single exciton and ∼4.4 for biexcitons. A linear dependence of fluorescence lifetime vs intensity distribution agrees well with the prediction of the model of multiple recombination centers. The blinking mechanism of CsPbBr3 quantum dots is addressed by considering the trion states under higher excitation p...

Journal ArticleDOI
TL;DR: In this paper, the authors introduce the fabrication of 2D photonic crystal slab nanocavities with high quality factors and cubic wavelength mode volumes directly in bulk diamond, which can increase spontaneous emission rates and photon extraction efficiencies.
Abstract: Color centers in diamond are promising spin qubits for quantum computing and quantum networking. In photon-mediated entanglement distribution schemes, the efficiency of the optical interface ultimately determines the scalability of such systems. Nano-scale optical cavities coupled to emitters constitute a robust spin-photon interface that can increase spontaneous emission rates and photon extraction efficiencies. In this work, we introduce the fabrication of 2D photonic crystal slab nanocavities with high quality factors and cubic wavelength mode volumes—directly in bulk diamond. This planar platform offers scalability and considerably expands the toolkit for classical and quantum nanophotonics in diamond.

Journal ArticleDOI
TL;DR: In this article, the carrier dynamics in G-centers in silicon have been investigated by using time-resolved photoluminescence spectroscopy, and the authors obtained an estimation of 1.6$\pm$0.1 $\angstrom$ for the spatial extension of the electronic wave function in the G-center.
Abstract: We addressed the carrier dynamics in so-called G-centers in silicon (consisting of substitutional-interstitial carbon pairs interacting with interstitial silicons) obtained via ion implantation into a silicon-on-insulator wafer. For this point defect in silicon emitting in the telecommunication wavelength range, we unravel the recombination dynamics by time-resolved photoluminescence spectroscopy. More specifically, we performed detailed photoluminescence experiments as a function of excitation energy, incident power, irradiation fluence and temperature in order to study the impact of radiative and non-radiative recombination channels on the spectrum, yield and lifetime of G-centers. The sharp line emitting at 969 meV ($\sim$1280 nm) and the broad asymmetric sideband developing at lower energy share the same recombination dynamics as shown by time-resolved experiments performed selectively on each spectral component. This feature accounts for the common origin of the two emission bands which are unambiguously attributed to the zero-phonon line and to the corresponding phonon sideband. In the framework of the Huang-Rhys theory with non-perturbative calculations, we reach an estimation of 1.6$\pm$0.1 $\angstrom$ for the spatial extension of the electronic wave function in the G-center. The radiative recombination time measured at low temperature lies in the 6 ns-range. The estimation of both radiative and non-radiative recombination rates as a function of temperature further demonstrate a constant radiative lifetime. Finally, although G-centers are shallow levels in silicon, we find a value of the Debye-Waller factor comparable to deep levels in wide-bandgap materials. Our results point out the potential of G-centers as a solid-state light source to be integrated into opto-electronic devices within a common silicon platform.

Journal ArticleDOI
TL;DR: In this paper, a high-speed nonpolar InGaN/GaN micro-scale light-emitting diode (LED) with a record electrical −3 dB modulation bandwidth of 1.5 GHz at a current density of 1 kA/cm2 was presented.
Abstract: We demonstrate a high-speed nonpolar ${m}$ -plane InGaN/GaN micro-scale light-emitting diode (LED) with a record electrical −3 dB modulation bandwidth of 1.5 GHz at a current density of 1 kA/cm2. A differential carrier lifetime (DLT) of 200 ps at 1 kA/cm2 was extracted using a rate-equation model. The short DLT is attributed to the high electron–hole wave function overlap in polarization-free nonpolar InGaN/GaN quantum wells, which leads to a higher spontaneous emission rate at low current densities compared to polar $c$ -plane quantum wells. LEDs with improved high-speed performance at low current densities will help to reduce power dissipation and increase efficiency in Gb/s visible-light communication systems.

Journal ArticleDOI
TL;DR: This work designs metal/dielectric nanocavities to be resonant with the absorption and emission bands of the employed fluorophores, and discusses the possibility of tailoring the two ENZ wavelengths within the visible spectrum simply by finely designing the thickness of the two dielectric layers, which enables resonance matching with a broad variety of dyes.
Abstract: The enhancement of the photophysical response of fluorophores is a crucial factor for photonic and optoelectronic technologies that involve fluorophores as gain media. Recent advances in the development of an extreme light propagation regime, called epsilon-near-zero (ENZ), provide a promising approach in this respect. In this work, we design metal/dielectric nanocavities to be resonant with the absorption and emission bands of the employed fluorophores. Using CsPbBr3 perovskite nanocrystal films as light emitters, we study the spontaneous emission and decay rate enhancement induced by a specifically tailored double-epsilon-near-zero (double ENZ) structure. We experimentally demonstrate the existence of two ENZ wavelengths, by directly measuring their dielectric permittivity via ellipsometric analysis. The double ENZ nature of this plasmonic nanocavity has been exploited to achieve both surface plasmon enhanced absorption (SPEA) and surface plasmon coupled emission (SPCE), inducing a significant enhanceme...

Journal ArticleDOI
TL;DR: The hyperbolic metacavity laser shows a clear clamping of spontaneous emission above the threshold, which demonstrates a near complete radiation coupling of the MQW with the metac Cavity, which can greatly simplify the requirements of plasmonic nanolaser with a long plAsmonic structure.
Abstract: Given the high demand for miniaturized optoelectronic circuits, plasmonic devices with the capability of generating coherent radiation at deep subwavelength scales have attracted great interest for diverse applications such as nanoantennas, single photon sources, and nanosensors. However, the design of such lasing devices remains a challenging issue because of the long structure requirements for producing strong radiation feedback. Here, a plasmonic laser made by using a nanoscale hyperbolic metamaterial cube, called hyperbolic metacavity, on a multiple quantum-well (MQW), deep-ultraviolet emitter is presented. The specifically designed metacavity merges plasmon resonant modes within the cube and provides a unique resonant radiation feedback to the MQW. This unique plasmon field allows the dipoles of the MQW with various orientations into radiative emission, achieving enhancement of spontaneous emission rate by a factor of 33 and of quantum efficiency by a factor of 2.5, which is beneficial for coherent laser action. The hyperbolic metacavity laser shows a clear clamping of spontaneous emission above the threshold, which demonstrates a near complete radiation coupling of the MQW with the metacavity. This approach shown here can greatly simplify the requirements of plasmonic nanolaser with a long plasmonic structure, and the metacavity effect can be extended to many other material systems.

Journal ArticleDOI
TL;DR: In this article, the authors present near-lifetime-limited linewidths for quantum dots embedded in nanophotonic waveguides through a resonant transmission experiment.
Abstract: Establishing a highly efficient photon-emitter interface where the intrinsic linewidth broadening is limited solely by spontaneous emission is a key step in quantum optics. It opens a pathway to coherent light–matter interaction for, e.g., the generation of highly indistinguishable photons, few-photon optical nonlinearities, and photon-emitter quantum gates. However, residual broadening mechanisms are ubiquitous and need to be combated. For solid-state emitters charge and nuclear spin noise are of importance, and the influence of photonic nanostructures on the broadening has not been clarified. We present near-lifetime-limited linewidths for quantum dots embedded in nanophotonic waveguides through a resonant transmission experiment. It is found that the scattering of single photons from the quantum dot can be obtained with an extinction of 66 ± 4%, which is limited by the coupling of the quantum dot to the nanostructure rather than the linewidth broadening. This is obtained by embedding the quantum dot in...

Journal ArticleDOI
TL;DR: The cavity enables an unprecedented frequency tuning range of the Raman emission that significantly exceeds the spectral inhomogeneity of silicon-vacancy centers in diamond nanostructures and selectively suppresses the phonon-induced spontaneous emission that degrades the efficiency of Raman photon generation.
Abstract: We demonstrate cavity-enhanced Raman emission from a single atomic defect in a solid. Our platform is a single silicon-vacancy center in diamond coupled with a monolithic diamond photonic crystal cavity. The cavity enables an unprecedented frequency tuning range of the Raman emission (100 GHz) that significantly exceeds the spectral inhomogeneity of silicon-vacancy centers in diamond nanostructures. We also show that the cavity selectively suppresses the phonon-induced spontaneous emission that degrades the efficiency of Raman photon generation. Our results pave the way towards photon-mediated many-body interactions between solid-state quantum emitters in a nanophotonic platform.