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We present a flow-based system coupled with an optical interferometry setup for the extraction of single nanocrystal properties.
Abstract This article describes a calculation of the spontaneous emission limited linewidth of a semiconductor laser consisting of hybrid or heterogeneously integrated, silicon and III–V intracavity components. Central to the approach are a) description of the multi‐element laser cavity in terms of composite laser/free‐space eigenmodes, b) use of multimode laser theory to treat mode competition and multiwave mixing, and c) incorporation of quantum‐optical contributions to account for spontaneous emission effects. Application of the model is illustrated for the case of linewidth narrowing in an InAs quantum‐dot laser coupled to a high‐ SiN cavity.
We report a laser with a linear external cavity containing a near-IR injection semiconductor optical amplifier as a gain element and two acousto-optic tunable filters (AOTFs) with quasi-collinear interaction of acoustic and light waves. At identical frequencies of RF signals that control the filters and ensure compensation for the Doppler frequency shift of light passing through the AOTFs, the steady-state laser emission linewidth can be reduced to about 25 MHz, which is almost three orders of magnitude smaller than that in the case of one filter (20 GHz). The position of the emission line, which remains narrow, slowly fluctuates within a spectral range about 3 GHz wide, which seems to be due to the large length of the external cavity and insufficient thermal stabilization of its components. This does not prevent us from obtaining light with a large coherence length. In emission wavelength sweep mode, the instantaneous emission linewidth increases with tuning rate, reaching 0.022 nm (8.8 GHz) at the highest tuning rate: 10{sup 4} nm s{sup −1}. In the case of automatic control over the output optical power at a level of 3 mW, the tuning range is 815 – 875 nm. Such instruments are of practical interest for optical coherence tomography, spectroscopy, optical metrology, and other application areas. (lasers)
Diamond color centers have been widely studied in the field of quantum optics. The negatively charged silicon vacancy (SiV – ) center exhibits a narrow emission linewidth at the wavelength of 738 nm, a high Debye–Waller factor, and unique spin properties, making it a promising emitter for quantum information technologies, biological imaging, and sensing. In particular, nanodiamond (ND)-based SiV – centers can be heterogeneously integrated with plasmonic and photonic nanostructures and serve as in vivo biomarkers and intracellular thermometers. Out of all methods to produce NDs with SiV – centers, ion implantation offers the unique potential to create controllable numbers of color centers in preselected individual NDs. However, the formation of single color centers in NDs with this technique has not been realized. We report the creation of single SiV– centers featuring stable high-purity single-photon emission through Si implantation into NDs with an average size of ~20 nm. We observe room temperature emission, with zero-phonon line wavelengths in the range of 730–800 nm and linewidths below 10 nm. Our results offer new opportunities for the controlled production of group-IV diamond color centers with applications in quantum photonics, sensing, and biomedicine.
Colloidal Ag(In,Ga)S 2 nanocrystals (AIGS NCs) with the band gap tunability by their size and composition within visible range have garnered surging interest. High absorption cross-section and narrow emission linewidth of AIGS NCs make them ideally suited to address the challenges of Cd-free NCs in wide-ranging photonic applications. However, AIGS NCs have shown relatively underwhelming photoluminescence quantum yield (PL QY) to date, primarily because coherent heteroepitaxy has not been realized. Here, we report the heteroepitaxy for AIGS-AgGaS 2 (AIGS-AGS) core-shell NCs bearing near-unity PL QYs in almost full visible range (460 to 620 nm) and enhanced photochemical stability. Key to the successful growth of AIGS-AGS NCs is the use of the Ag-S-Ga(OA) 2 complex, which complements the reactivities among cations for both homogeneous AIGS cores in various compositions and uniform AGS shell growth. The heteroepitaxy between AIGS and AGS results in the Type I heterojunction that effectively confines charge carriers within the emissive core without optically active interfacial defects. AIGS-AGS NCs show higher extinction coefficient and narrower spectral linewidth compared to state-of-the-art heavy metal-free NCs, prompting their immediate use in practicable applications including displays and luminescent solar concentrators (LSCs).
This paper reports results of a study aimed at producing a Raman fibre laser based on a multicore fibre with high-reflectivity fibre Bragg gratings inscribed in its peripheral cores using femtosecond laser pulses. We present spectral and power characteristics of a Raman laser whose output power at a wavelength of 1090 nm is 2.5 W. The laser emission linewidth has been shown to decrease as a result of the reduction in nonlinear effects owing to the larger effective mode area in the multicore fibre in comparison with a standard single-mode fibre Raman laser. (paper)
The remarkable defect tolerant nature of inorganic cesium halide perovskites leading to near unity photoluminescence (PL) quantum yield (QY) and narrow emission linewidth across the entire visible spectrum, have provided a tantalizing platform for a development of a plethora of light-emitting applications. Recently, lower dimensional (2D, 1D, and 0D) perovskites have attracted further attention due to the enhanced thermal, photo and chemical stability as compared to their three-dimensional (3D) analogues. Combination of the external size quantization and internal octahedral organization provides a unique opportunity to study and harness “multidimensional” electronic properties engineered both on atomic scale and the nanoscale. However, crucial research to understand the elementary charge carrier dynamics in lower dimensional perovskites lags far behind the enormous effort to incorporate them into optoelectronic devices. In this Perspective, we provide a review of recent developments that focus on studies of the dynamics of excitonic complexes in Cs-based perovskite nanocrystals using single-particle time-resolved PL spectroscopy and photon correlation measurements. Single photon statistical studies not only offer the unprecedented level of detail to directly assess various recombination pathways but also provide insights into specifics of carrier’s localization. Further, we discuss the underlying physicochemical processes that govern PL emission and draw attention to a number of attributes within this class of the materials, especially lower-dimensional perovskites that may indicate the common origin of the PL emission, as well as provide a route map for the vast unexplored territories where single particle spectroscopy can be a powerful tool to unravel crucial information.
Abstract Metallic nanocavity lasers provide important technological advancement toward even smaller integrable light sources. They give access to widely unexplored lasing physics in which the distinction between different operational regimes, like those of thermal or coherent light emission, becomes increasingly challenging upon approaching a device with a near‐perfect spontaneous‐emission coupling factor . In fact, quantum‐optical studies have to be employed to reveal a transition to coherent emission in the intensity fluctuation behavior of nanolasers when the input–output characteristic appears thresholdless for nanolasers. Here, a new indicator for lasing operation in high‐ lasers is identified by showing that stimulated emission can give rise to a lineshape anomaly manifested as a transition from a Lorentzian to a Gaussian component in the emission linewidth that dominates the spectrum above the lasing threshold.
The collective modes of two-dimensional ordered atomic arrays can modify the radiative environment of embedded atomic impurities. We analyze the role of the lattice geometry on the impurity's emission linewidth by comparing the effective impurity decay rate obtained for all noncentered Bravais lattices and an additional honeycomb lattice. We demonstrate that the lattice geometry plays a crucial role in determining the effective decay rate for the impurity. In particular, we find that the minimal effective decay rate appears in lattices where the number of the impurity's nearest neighbors is maximal and the number of distinct distances among nearest neighbors is minimal. Here we further show that, in the choice between interstitial and substitutional placement of the impurity, the former always wins by exhibiting a lower decay rate and longer photon storage. For interstitial placements, we determine the optimal impurity position in the lattice plane, which is not necessarily found in the center of the lattice plaquette.
We investigate the potential for two-dimensional atom arrays to modify the radiation and interaction of individual quantum emitters. Specifically, we demonstrate that control over the emission linewidths, resonant frequency shifts, and local driving field enhancement in impurity atoms is possible due to strong dipole-dipole interactions within ordered, subwavelength atom array configurations. We demonstrate that these effects can be used to dramatically enhance coherent dipole-dipole interactions between distant impurity atoms within an atom array. Possible experimental realizations and potential applications are discussed.
III-nitride light-emitting diodes (LEDs) exhibit an injection-dependent emission blueshift and linewidth broadening that is severely detrimental to their color purity. By using first-principles multi-scale modeling that accurately captures the competition between polarization-charge screening, phase-space filling, and many-body plasma renormalization, we explain the current-dependent spectral characteristics of polar III-nitride LEDs fabricated with state-of-the-art quantum wells. Our analysis uncovers a fundamental connection between carrier dynamics and the injection-dependent spectral characteristics of light-emitting materials. For example, polar III-nitride LEDs offer poor control over their injection-dependent color purity due to their poor hole transport and slow carrier-recombination dynamics, which forces them to operate at or near degenerate carrier densities. Designs that accelerate carrier recombination and transport and reduce the carrier density required to operate LEDs at a given current density lessen their injection-dependent wavelength shift and linewidth broadening.
Optical resonator-based frequency stabilization plays a critical role in ultra-low linewidth laser emission and precision sensing, atom clocks, and quantum applications. However, there has been limited success in translating traditional bench-top stabilization cavities to compact on-chip integrated waveguide structures that are compatible with photonic integration. The challenge lies in realizing waveguides that not only deliver low optical loss but also exhibit a low thermo-optic coefficient and frequency noise stability. Given the problematic sources of frequency noise within dielectrics, such as thermorefractive noise, resonators with small thermo-optic response are desirable for on-chip reference cavities. We report the first demonstration of a Ta 2 O 5 (tantala) waveguide core fabricated on a crystal quartz substrate lower cladding with TEOS-PECVD SiO 2 upper cladding. This waveguide offers significant advantages over other waveguides in terms of its low thermo-optic coefficient and reduced thermorefractive-related frequency noise. We describe the waveguide structure and key design parameters as well as fabrication considerations for processing tantala on quartz waveguides. We report a waveguide thermo-optic coefficient of -1.14 × 10 -6 RIU/K, a value that is over 6 times smaller in magnitude than that of SiO 2 -substrate tantala waveguides, with a propagation loss of 1.19 dB/cm at 1550 nm and <1.33 dB/cm across the 1525 nm–1610 nm wavelength range. Within a 1.6 mm radius ring resonator, we demonstrate a 2.54 × 10 5 intrinsic Q factor. With the potential for very low loss and the ability to control the thermal response, this waveguide platform takes a key step toward creating thermally stable integrated resonators for on-chip laser frequency stabilization and other applications.
InP-based quantum dots (QDs) have Stokes shifts and photoluminescence (PL) line widths that are larger than in II–VI semiconductor QDs with comparable exciton energies. The mechanisms responsible for these spectral characteristics are investigated in this paper. Upon comparing different semiconductors, we find the Stokes shift decreases in the following order: InP > CdTe > CdSe. We also find that the Stokes shift decreases with core size and decreases upon deposition of a ZnSe shell. We suggest that the Stokes shift is largely due to different absorption and luminescent states in the angular momentum fine structure. The energy difference between the fine structure levels, and hence the Stokes shifts, are controlled by the electron–hole exchange interaction. Luminescence polarization results are reported and are consistent with this assignment. Spectral widths are controlled by the extent of homogeneous and inhomogeneous broadening. Here, we report PL and PL excitation (PLE) spectra that facilitate assessing the roles of homogeneous and different inhomogeneous broadening mechanisms in the spectra of zinc-treated InP and InP/ZnSe/ZnS particles. There are two distinct types of inhomogeneous broadening: size inhomogeneity and core–shell interface inhomogeneity. The latter results in a distribution of core–shell band offsets and is caused by interfacial dipoles associated with In–Se or P–Zn bonding. Quantitative modeling of the spectra shows that the offset inhomogeneity is comparable to but somewhat smaller than the size inhomogeneity. The combination of these two types of inhomogeneity also explains several aspects of reversible hole trapping dynamics involving localized In 3+ /V Zn 2– impurity states in the ZnSe shells.
Rare-earth containing wide band gap oxides, which provide spin-photon interface and narrow linewidth optical emission, are getting significant attention as the most promising candidate materials in advancing quantum transduction and memories. Here, in this work, from ab initio calculations, we identify antiferromagnetic ground states in structurally preferred monoclinic CePO 4 and tetragonal CeVO 4 exhibiting localized occupied and unoccupied Ce 4𝑓 states with 4𝑓−4𝑓 transition characteristics. Interestingly, in CePO 4 , O 2𝑝 and P 3𝑝 states hybridize negligibly with Ce 4𝑓 states, while in CeVO 4 , V 3𝑑 and O 2𝑝 states hybridize and appear as extended states in between the occupied and unoccupied Ce 4𝑓 states. Here, phonon calculations and analysis identify and differentiate Raman active phonon modes along with the spin phonon coupling of Ce in both CePO 4 and CeVO 4 that ultimately lead to different 4𝑓 ground-state crystal-field multiplets, which are critical to accurately describe electronic transitions for foundational quantum transduction and memories. Further, the identified 𝐶 1 site symmetry of Ce, lacking inversion symmetry in CePO 4 , is relevant for quantum memories and 𝐷 2𝑑 site symmetry of Ce exhibiting inversion symmetry in CeVO 4 is relevant for quantum transduction.
Here, we present a first-principles study of the defect formation and electronic structure of erbium (Er)–doped yttria (Y 2 O 3 ). This is an emerging material for spin-photon interfaces in quantum information science due to the narrow-linewidth optical emission from Er dopants at standard telecommunication wavelengths and their potential for quantum memories and transducers. We calculate formation energies of neutral and negatively and positively charged Er dopants and find the charge-neutral configuration to be the most stable, consistent with experiment. Of the two substitutional sites of Er for Y, the C 2 (more relevant for quantum memories) and C 3i (more relevant for quantum transduction), we identify the former as possessing the lowest formation energy. The electronic properties are calculated using the Perdew-Burke-Ernzerhof functional along with the Hubbard U parameter and spin-orbit coupling, which yields a ~ 6 μ B orbital and a ~ 3 μ B spin magnetic moment, and 11 electrons in the Er 4 f shell, confirming the formation of charge-neutral Er 3+ . This standard density functional theory approach underestimates the band gap of the host and lacks a first-principles justification for U . To overcome these issues we performed screened hybrid functional calculations, including a negative U for the 4 f orbitals, with mixing (α) and screening (w) parameters. These produced robust electronic features with slight modifications in the band gap and the 4 f splittings depending on the choice of tuning parameters. We also computed the many-particle electronic excitation energies and compared them with experimental values from photoluminescence.
Abstract Stable laser emission with narrow linewidth is of critical importance in many applications, including coherent communications, LIDAR, and remote sensing. In this work, the physics underlying spectral narrowing of self-injection-locked on-chip lasers to Hz-level lasing linewidth is investigated using a composite-cavity structure. Heterogeneously integrated III–V/SiN lasers operating with quantum-dot and quantum-well active regions are analyzed with a focus on the effects of carrier quantum confinement. The intrinsic differences are associated with gain saturation and carrier-induced refractive index, which are directly connected with 0- and 2-dimensional carrier densities of states. Results from parametric studies are presented for tradeoffs involved with tailoring the linewidth, output power, and injection current for different device configurations. Though both quantum-well and quantum-dot devices show similar linewidth-narrowing capabilities, the former emits at a higher optical power in the self-injection-locked state, while the latter is more energy-efficient. Lastly, a multi-objective optimization analysis is provided to optimize the operation and design parameters. For the quantum-well laser, minimizing the number of quantum-well layers is found to decrease the threshold current without significantly reducing the output power. For the quantum-dot laser, increasing the quantum-dot layers or density in each layer increases the output power without significantly increasing the threshold current. These findings serve to guide more detailed parametric studies to produce timely results for engineering design.
Transition metal (i.e., Mn, Fe, Cr) and chalcogen (Se) substituents are introduced into single-crystalline NiPS 3 , and the evolution of the two emergent quasi-particle excitations characteristic to the XXZ correlated antiferromagnetism of NiPS 3 (i.e., spin orbit entangled exciton (SOX) and two-magnon scattering (2M )) are investigated as functions of substituent concentration through comprehensive room- and low-temperature photoluminescence (PL) and Raman spectroscopy studies. These findings are further correlated with the magnetic properties of the same set of compounds reported in prior studies. The work revealed that the SOX emission intensities and linewidths are mainly controlled by the magnetic anisotropy and spin orientations, and are strongly suppressed by the introduction of substituents. The suppression depends on the type of substituent, with Fe affecting the SOX emission more than Mn and Cr. The 2 M scattering is linked to short-range correlations and exhibits greater resiliency against metal atom substitution. While the 2M peak at low temperature gets suppressed and red-shifted in frequency with increasing concentrations of all the substituents, Fe induces the weakest suppression compared to all other substituents. Altogether, these findings revealed the introduction of substituents as a powerful route to control the emergent collective excitations in NiPS 3 and mixed-MPX 3 materials.
We report a reduction in the linewidth and suppression of spectral diffusion of quantum emitters in hexagonal boron nitride supported on a conductive substrate. In this work, we observe a temperature-dependent reduction in the spectral emission linewidth for CVD-grown and exfoliated crystals on conductive ITO relative to those seen on silicon dioxide (SiO 2 ) substrates. We show that the inhomogeneous linewidth can be suppressed by 45% as a result of using a conductive substrate. We investigate the zero-phonon line profile at temperatures ranging from 4 to 300 K and decompose the effects of thermal broadening and spectral diffusion at each temperature by Voigt fitting. The temperature dependence of homogeneous and inhomogeneous components of the broadening is discussed.