Room Temperature Single Photon Emitters Research Articles

Hexagonal Boron Nitride Based Photonic Quantum Technologies.

Hexagonal boron nitride is rapidly gaining interest as a platform for photonic quantum technologies, due to its two-dimensional nature and its ability to host defects deep within its large band gap that may act as room-temperature single-photon emitters. In this review paper we provide an overview of (1) the structure, properties, growth and transfer of hexagonal boron nitride; (2) the creationof colour centres in hexagonal boron nitride and assignment of defects by comparison with ab initio calculations for applications in photonic quantum technologies; and (3) heterostructure devices for the electrical tuning and charge control of colour centres that form the basis for photonic quantum technology devices. The aim of this review is to provide readers a summary of progress in both defect engineering and device fabrication in hexagonal boron nitride based photonic quantum technologies.

Transfer of hexagonal boron nitride quantum emitters onto arbitrary substrates with zero thermal budget

The van der Waals material hexagonal boron nitride (hBN) has emerged as a promising candidate for hosting room temperature single-photon emitters (SPEs) for next-generation quantum technologies. However, the requirement of a high temperature anneal (850 °C or higher) to activate the SPEs in hBN makes it difficult to integrate into hybrid structures that cannot tolerate such temperatures, including all silicon-based circuits. In this work, we present a method to deterministically activate quantum emitters in multilayered hBN on a process substrate, followed by a zero thermal budget transfer to a target substrate. This technique does not lead to any degradation or loss of photon purity in the hBN emitters and provides a procedure for combining high-purity emitters with other exciting photonic, magnetic, or electrical properties to explore new physical phenomena. The ability to transfer hBN emitters onto arbitrary substrates creates new technological possibilities to incorporate these quantum photonic properties into photonic integrated circuits and plasmonic devices.

Recent advances in room temperature single-photon emitters

Recent advances in room temperature single-photon emitters

Organic Molecules as Origin of Visible-Range Single Photon Emission from Hexagonal Boron Nitride and Mica.

The discovery of room-temperature single-photon emitters (SPEs) hosted by two-dimensional hexagonal boron nitride (2D hBN) has sparked intense research interest. Although emitters in the vicinity of 2 eV have been studied extensively, their microscopic identity has remained elusive. The discussion of this class of SPEs has centered on point defects in the hBN crystal lattice, but none of the candidate defect structures have been able to capture the great heterogeneity in emitter properties that is observed experimentally. Employing a widely used sample preparation protocol but disentangling several confounding factors, we demonstrate conclusively that heterogeneous single-photon emission at ∼2 eV associated with hBN originates from organic molecules, presumably aromatic fluorophores. The appearance of those SPEs depends critically on the presence of organic processing residues during sample preparation, and emitters formed during heat treatment are not located within the hBN crystal as previously thought, but at the hBN/substrate interface. We further demonstrate that the same class of SPEs can be observed in a different 2D insulator, fluorophlogopite mica.

First-Principle Prediction of Stress-Tunable Single-Photon Emitters at Telecommunication Band from Point Defects in GaN

Point defect-based single-photon emitters (SPEs) in GaN have aroused a great deal of interest due to their room-temperature operation, narrow line width and high emission rate. The room-temperature SPEs at the telecommunication bands have also been realized recently by localized defects in GaN in experiments, which are highly desired for the practical applications of SPEs in quantum communication with fiber compatibility. However, the origin and underlying mechanism of the SPEs remain unclear to date. Herein, our first-principle calculations predict and identify an intrinsic point defect NGa in GaN that owns a zero-phonon line (ZPL) at telecommunication windows. By tuning the triaxial compressive strain of the crystal structure, the ZPL of NGa can be modulated from 0.849 eV to 0.984 eV, covering the fiber telecommunication windows from the O band to the E band. Besides the ZPL, the formation energy, band structure, transition process and lifetime of the SPEs under different strains are investigated systematically. Our work gives insight into the emission mechanism of the defect SPEs in GaN and also provides effective guidance for achieving wavelength-tunable SPEs working in fiber telecommunication windows.

Prolonged photostability in hexagonal boron nitride quantum emitters

Single-photon emitters are crucial building blocks for optical quantum technologies. Hexagonal boron nitride (hBN) is a promising two-dimensional material that hosts bright, room-temperature single-photon emitters. However, photo instability is a persistent challenge preventing practical applications of these properties. Here, we reveal the ubiquitous photobleaching of hBN vacancy emitters. Independent of the source or the number of hBN layers, we find that the photobleaching of a common emission at 1.98 ± 0.05 eV can be described by two consistent time constants, namely a first bleaching lifetime of 5 to 10 s, and a second bleaching lifetime in the range of 150 to 220 s. Only the former is environmentally sensitive and can be significantly mitigated by shielding O2, whereas the latter could be the result of carbon-assisted defect migration. Annular dark-field scanning transmission electron microscopy of photobleached hBN allows for visualizing vacancy defects and carbon substitution at single atom resolution, supporting the migration mechanism along with X-ray photoelectron spectroscopy. Thermal annealing at 850 °C of liquid exfoliated hBN eliminates both bleaching processes, leading to persistent photostability. These results represent a significant advance to potentially engineer hBN vacancy emitters with the photostability requisite for quantum applications.

Uncovering the morphological effects of high-energy Ga+ focused ion beam milling on hBN single-photon emitter fabrication.

Many techniques to fabricate complex nanostructures and quantum emitting defects in low dimensional materials for quantum information technologies rely on the patterning capabilities of focused ion beam (FIB) systems. In particular, the ability to pattern arrays of bright and stable room temperature single-photon emitters (SPEs) in 2D wide-bandgap insulator hexagonal boron nitride (hBN) via high-energy heavy-ion FIB allows for direct placement of SPEs without structured substrates or polymer-reliant lithography steps. However, the process parameters needed to create hBN SPEs with this technique are dependent on the growth method of the material chosen. Moreover, morphological damage induced by high-energy heavy-ion exposure may further influence the successful creation of SPEs. In this work, we perform atomic force microscopy to characterize the surface morphology of hBN regions patterned by Ga+ FIB to create SPEs at a range of ion doses and find that material swelling, and not milling as expected, is most strongly and positively correlated with the onset of non-zero SPE yields. Furthermore, we simulate vacancy concentration profiles at each of the tested doses and propose a qualitative model to elucidate how Ga+ FIB patterning creates isolated SPEs that is consistent with observed optical and morphological characteristics and is dependent on the consideration of void nucleation and growth from vacancy clusters. Our results provide novel insight into the formation of hBN SPEs created by high-energy heavy-ion milling that can be leveraged for monolithic hBN photonic devices and could be applied to a wide range of low-dimensional solid-state SPE hosts.

Photon‐Correlation Studies on Multichromophore Macrocycles of Perylene Dyes

AbstractOrganic dyes offer unique properties for their application as room temperature single photon emitters. By means of photon‐correlation, the emission characteristics of macrocyclic para‐xylylene linked perylene bisimide (PBI) trimers and tetramers dispersed in polymethyl methacrylate matrices are analyzed. The optical data indicate that, despite of the strong emission enhancement of PBI trimers and tetramers according to their larger number of chromophores, the photon‐correlation statistics still obeys that of single photon emitters. Moreover, driving PBI trimers and tetramers at higher excitation powers, saturated emission behavior for monomers is found while macrocycle emission is still far‐off saturation but shows enhanced fluctuations. This observation is attributed to fast singlet–singlet annihilation, i.e., faster than the radiative lifetime of the excited S1 state, and the enlarged number of conformational arrangements of multichromophores in the polymeric host. Finally, embedding trimeric PBI macrocycles in active organic light‐emitting diode matrices, electrically driven bright fluorescence together with an indication for antibunching at room temperature can be detected. This, so far, has only been observed for phosphorescent emitters that feature much longer lifetimes of the excited states and, thus, smaller radiative recombination rates. The results are discussed in the context of possible effects on the g(2) behavior of molecular emitters.

Transferable room-temperature single-photon emitters in hexagonal boron nitride grown by molecular beam epitaxy

The solid-state single-photon source is the core of applications such as quantum cryptography, quantum sensing, and quantum computing. Recently, the point defects in two-dimensional (2D) hexagonal boron nitride (h-BN) have become excellent candidates for next-generation single-photon sources due to their chemical and physical stability and ultra-high brightness at room temperature. The 2D layered structure of h-BN allows the single-photon emitters (SPEs) in it to have high photon extraction efficiency and be integrated into photonic circuits easily. However, most of the SPEs found in h-BN flakes are present at the edges or wrinkles. Here, we report on the room-temperature SPEs in h-BN film grown by molecular beam epitaxy followed by a high-temperature post-annealing process and their deterministic transfer. Using the all-dry viscoelastic stamping method, the h-BN film grown on the Al2O3 substrate can be transferred to other substrates. The transferred SPEs are discretely distributed among the continuous h-BN flakes, and the SPE density is as high as ∼0.17 μm−2. After identification, the determined SPE can be deterministically transferred to other structures by the all-dry transfer method. The deterministic transfer of SPEs distributed on the h-BN flakes promises the potential to integrate SPEs into many quantum technology applications.

Creating Quantum Emitters in Hexagonal Boron Nitride Deterministically on Chip-Compatible Substrates

Two-dimensional hexagonal boron nitride (hBN) that hosts room-temperature single-photon emitters (SPEs) is promising for quantum information applications. An important step toward the practical application of hBN is the on-demand, position-controlled generation of SPEs. Strategies reported for deterministic creation of hBN SPEs either rely on substrate nanopatterning that is not compatible with integrated photonics or utilize radiation sources that might introduce unpredictable damage or contamination to hBN. Here, we report a radiation- and lithography-free route to deterministically activate hBN SPEs by nanoindentation with atomic force microscopy (AFM). The method applies to hBN flakes on flat silicon dioxide-silicon substrates that can be readily integrated into on-chip photonic devices. The achieved SPE yields are above 30% for multiple indent sizes, and a maximum yield of 36% is demonstrated for indents around 400 nm. Our results mark an important step toward the deterministic creation and integration of hBN SPEs with photonic and plasmonic devices.

Band gap measurements of monolayer h-BN and insights into carbon-related point defects

Being a flexible wide band gap semiconductor, hexagonal boron nitride (h-BN) has great potential for technological applications like efficient deep ultraviolet light sources, building block for two-dimensional heterostructures and room temperature single photon emitters in the ultraviolet and visible spectral range. To enable such applications, it is mandatory to reach a better understanding of the electronic and optical properties of h-BN and the impact of various structural defects. Despite the large efforts in the last years, aspects such as the electronic band gap value, the exciton binding energy and the effect of point defects remained elusive, particularly when considering a single monolayer. Here, we directly measured the density of states of a single monolayer of h-BN epitaxially grown on highly oriented pyrolytic graphite, by performing low temperature scanning tunneling microscopy (STM) and spectroscopy (STS). The observed h-BN electronic band gap on defect-free regions is (6.8 ± 0.2) eV. Using optical spectroscopy to obtain the h-BN optical band gap, the exciton binding energy is determined as being of (0.7 ± 0.2) eV. In addition, the locally excited cathodoluminescence and photoluminescence show complex spectra that are typically associated to intragap states related to carbon defects. Moreover, in some regions of the monolayer h-BN we identify, using STM, point defects which have intragap electronic levels around 2.0 eV below the Fermi level.

Single-photon emission from two-dimensional hexagonal boron nitride annealed in a carbon-rich environment

For quantum photonic applications, such as quantum communication, optical quantum information processing, and metrology, solid-state sources of single-photon emitters are highly needed. Recently, single-photon emitters in two-dimensional (2D) van der Waals materials have attracted tremendous attention because of their atomic thickness, allowing for high photon extraction efficiency and easy integration into photonic circuits. In particular, a defect hosted by 2D hexagonal boron nitride (hBN) is expected to be a promising candidate for next-generation single-photon sources due to its chemical and thermal stability and high brightness at room temperature. Here, we report an effective method for generating single-photon emission in mechanically exfoliated hBN flakes by annealing in a carbon-rich environment. The one-step annealing in a mixed atmosphere (Ar:CH4:H2 = 15:5:1) greatly increases the single-photon emitter density in hBN. The resulting single-photon emission shows high stability and brightness. Our results provide an effective method for generating room-temperature single-photon emitters in 2D hBN.

Stark Tuning of Single-Photon Emitters in Hexagonal Boron Nitride.

Single-photon emitters play an essential role in quantum technologies, including quantum computing and quantum communications. Atomic defects in hexagonal boron nitride ( h-BN) have recently emerged as new room-temperature single-photon emitters in solid-state systems, but the development of scalable and tunable h-BN single-photon emitters requires external methods that can control the emission energy of individual defects. Here, by fabricating van der Waals heterostructures of h-BN and graphene, we demonstrate the electrical control of single-photon emission from atomic defects in h-BN via the Stark effect. By applying an out-of-plane electric field through graphene gates, we observed Stark shifts as large as 5.4 nm per GV/m. The Stark shift generated upon a vertical electric field suggests the existence of out-of-plane dipole moments associated with atomic defect emitters, which is supported by first-principles theoretical calculations. Furthermore, we found field-induced discrete modification and stabilization of emission intensity, which were reversibly controllable with an external electric field.

Effects of High-Energy Electron Irradiation on Quantum Emitters in Hexagonal Boron Nitride.

Hexagonal boron nitride (hBN) mono and multilayers are promising hosts for room-temperature single photon emitters (SPEs). In this work we explore high-energy (∼MeV) electron irradiation as a means to generate stable SPEs in hBN. We investigate four types of exfoliated hBN flakes-namely, high-purity multilayers, isotopically pure hBN, carbon-rich hBN multilayers and monolayered material-and find that electron irradiation increases emitter concentrations dramatically in all samples. Furthermore, the engineered emitters are located throughout hBN flakes (not only at flake edges or grain boundaries) and do not require activation by high-temperature annealing of the host material after electron exposure. Our results provide important insights into controlled formation of hBN SPEs and may aid in identification of their crystallographic origin.

Room-temperature single-photon emitters in titanium dioxide optical defects.

Fluorescence properties of crystallographic point defects within different morphologies of titanium dioxide were investigated. For the first time, room-temperature single-photon emission in titanium dioxide optical defects was discovered in thin films and commercial nanoparticles. Three-level defects were identified because the g(2) correlation data featured prominent shoulders around the antibunching dip. Stable and blinking photodynamics were observed for the single-photon emitters. These results reveal a new room-temperature single-photon source within a wide bandgap semiconductor.

Single photon emission from ZnO nanoparticles

Room temperature single photon emitters are very important resources for photonics and emerging quantum technologies. In this work, we study single photon emission from defect centers in 20 nm zinc oxide (ZnO) nanoparticles. The emitters exhibit bright broadband fluorescence in the red spectral range centered at 640 nm with polarized excitation and emission. The studied emitters showed continuous blinking; however, bleaching can be suppressed using a polymethyl methacrylate coating. Furthermore, hydrogen termination increased the density of single photon emitters. Our results will contribute to the identification of quantum systems in ZnO.

Three-dimensional quantum photonic elements based on single nitrogen vacancy-centres in laser-written microstructures

To fully integrate quantum optical technology, active quantum systems must be combined with resonant microstructures and optical interconnects harvesting and routing photons in three diemsnsions (3D) on one chip. We fabricate such combined structures for the first time by using two-photon laser lithography and a photoresist containing nanodiamonds including nitrogen vacancy-centers. As an example for possible functionality, single-photon generation, collection, and transport is successfully accomplished. The single photons are efficiently collected via resonators and routed in 3D through waveguides, all on one optical chip. Our one-step fabrication scheme is easy to implement, scalable and flexible. Thus, other complex assemblies of 3D quantum optical structures are feasible as well.