arXiv subjects

Carlo Bradac

Publications and source records attributed to Carlo Bradac.

31 records · Page 2Linked to original sources

arXiv2019

Room Temperature Initialisation and Readout of Intrinsic Spin Defects in a Van der Waals Crystal

Optically addressable spins in widebandgap semiconductors have become one of the most prominent platforms for exploring fundamental quantum phenomena. While several candidates in 3D crystals including diamond and silicon carbide have been extensively studied, the identification of spindependent processes in atomically thin 2D materials has remained elusive. Although optically accessible spin states in hBN are theoretically predicted, they have not yet been observed experimentally. Here, employing rigorous electron paramagnetic resonance techniques and photoluminescence spectroscopy, we identify fluorescence lines in hexagonal boron nitride associated with a particular defect, the negatively charged boron vacancy and determine the parameters of its spin Hamiltonian. We show that the defect has a triplet ground state with a zero field splitting of 3.5 GHz and establish that the centre exhibits optically detected magnetic resonance at room temperature. We also demonstrate the spin polarization of this centre under optical pumping, which leads to optically induced population inversion of the spin ground state a prerequisite for coherent spin manipulation schemes. Our results constitute a leap forward in establishing two dimensional hBN as a prime platform for scalable quantum technologies, with extended potential for spin based quantum information and sensing applications, as our ODMR studies on hBN NV diamonds hybrid structures show.

physics.optics↗

arXiv2019

Suppression of Spectral Diffusion by Anti-Stokes Excitation of Quantum Emitters in Hexagonal Boron Nitride

Solid-state quantum emitters are garnering a lot of attention due to their role in scalable quantum photonics. A notable majority of these emitters, however, exhibit spectral diffusion due to local, fluctuating electromagnetic fields. In this work, we demonstrate efficient Anti-Stokes (AS) excitation of quantum emitters in hexagonal boron nitride (hBN), and show that the process results in the suppression of a specific mechanism responsible for spectral diffusion of the emitters. We also demonstrate an all-optical gating scheme that exploits Stokes and Anti-Stokes excitation to manipulate spectral diffusion so as to switch and lock the emission energy of the photon source. In this scheme, reversible spectral jumps are deliberately enabled by pumping the emitter with high energy (Stokes) excitation; AS excitation is then used to lock the system into a fixed state characterized by a fixed emission energy. Our results provide important insights into the photophysical properties of quantum emitters in hBN, and introduce a new strategy for controlling the emission wavelength of quantum emitters.

physics.optics↗

arXiv2018

Effects of microstructure and growth conditions on quantum emitters in Gallium Nitride

Single-photon emitters in gallium nitride (GaN) are gaining interest as attractive quantum systems due to the well-established techniques for growth and nanofabrication of the host material, as well as its remarkable chemical stability and optoelectronic properties. We investigate the nature of such single-photon emitters in GaN with a systematic analysis of various samples produced under different growth conditions. We explore the effect that intrinsic structural defects (dislocations and stacking faults), doping and crystal orientation in GaN have on the formation of quantum emitters. We investigate the relationship between the position of the emitters (determined via spectroscopy and photoluminescence measurements) and the location of threading dislocations (characterised both via atomic force microscopy and cathodoluminescence). We find that quantum emitters do not correlate with stacking faults or dislocations; instead, they are more likely to originate from point defects or impurities whose density is modulated by the local extended defect density.

physics.app-ph↗

arXiv2018

Anti-Stokes excitation of solid-state quantum emitters for nanoscale thermometry

Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light emitting diodes and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite Anti-Stokes process, where excitation is performed with lower energy photons. We report that the process is sufficiently efficient to excite even a single quantum system, namely the germanium-vacancy center in diamond. Consequently, we leverage the temperature-dependent, phonon-assisted mechanism to realize an all-optical nanoscale thermometry scheme that outperforms any homologous optical method employed to date. Our results frame a promising approach for exploring fundamental light-matter interactions in isolated quantum systems, and harness it towards the realization of practical nanoscale thermometry and sensing.

physics.app-ph↗

arXiv2018

Enhanced Emission from WSe2 Monolayers Coupled to Circular Bragg Gratings

Two-dimensional transition-metal dichalcogenides (TMDC) are of great interest for on-chip nanophotonics due to their unique optoelectronic properties. Here, we propose and realize coupling of tungsten diselenide (WSe2) monolayers to circular Bragg grating structures to achieve enhanced emission. The interaction between WSe2 and the resonant mode of the structure results in Purcell-enhanced emission, while the symmetric geometrical structure improves the directionality of the out-coupling stream of emitted photons. Furthermore, this hybrid structure produces a record high contrast of the spin valley readout (> 40%) revealed by the polarization resolved photoluminescence (PL) measurements. Our results are promising for on-chip integration of TMDC monolayers with optical resonators for nanophotonic circuits.

physics.optics↗

arXiv2018

Bottom up engineering of near-identical quantum emitters in atomically thin materials

Quantum technologies require robust and photostable single photon emitters (SPEs) that can be reliably engineered. Hexagonal boron nitride (hBN) has recently emerged as a promising candidate host to bright and optically stable SPEs operating at room temperature. However, the emission wavelength of the fluorescent defects in hBN has, to date, been shown to be uncontrolled. The emitters usually display a large spread of zero phonon line (ZPL) energies spanning over a broad spectral range (hundreds of nanometers), which hinders the potential development of hBN-based devices and applications. We demonstrate bottom-up, chemical vapor deposition growth of large-area, few layer hBN that hosts large quantities of SPEs: 100 per 10x10 μm2. Remarkably, more than 85 percent of the emitters have a ZPL at (580{\pm}10)nm, a distribution which is over an order of magnitude narrower than previously reported. Exploiting the high density and uniformity of the emitters, we demonstrate electrical modulation and tuning of the ZPL emission wavelength by up to 15 nm. Our results constitute a definite advancement towards the practical deployment of hBN single photon emitters in scalable quantum photonic and hybrid optoelectronic devices based on 2D materials.

physics.app-ph↗

arXiv2017

Super-resolution imaging of quantum emitters in layered materials

Layered van der Waals materials are emerging as compelling two-dimensional (2D) platforms for studies of nanophotonics, polaritonics, valleytronics and spintronics, and have the potential to transform applications in sensing, imaging and quantum information processing. Amongst these, hexagonal boron nitride (hBN) is unique in that it hosts ultra-bright, room temperature single photon emitters (SPEs). However, an outstanding challenge is to locate SPEs in hBN with high precision, a task which requires breaking the optical diffraction limit. Here, we report the imaging of SPEs in layered hBN with a spatial resolution of 63 nm using ground state depletion (GSD) nanoscopy. Furthermore, we show that SPEs in hBN possess nonlinear photophysical properties which can be used to realize a new variant of GSD that employs a coincident pair of doughnut-shaped lasers to reduce the laser power that is needed to achieve a given resolution target. Our findings expand the current understanding of the photophysics of quantum emitters in layered hBN and demonstrate the potential for advanced nanophotonic and bio-imaging applications which require localization of individual emitters with super-resolution accuracy.

physics.optics↗

arXiv2017

Photophysics of GaN single photon sources in the visible spectral range

In this work, we present a detailed photophysical analysis of recently-discovered optically stable, single photon emitters (SPEs) in Gallium Nitride (GaN). Temperature-resolved photoluminescence measurements reveal that the emission lines at 4 K are three orders of magnitude broader than the transform-limited widths expected from excited state lifetime measurements. The broadening is ascribed to ultra-fast spectral diffusion. Continuing the photophysics study on several emitters at room temperature (RT), a maximum average brightness of ~427 kCounts/s is measured. Furthermore, by determining the decay rates of emitters undergoing three-level optical transitions, radiative and non-radiative lifetimes are calculated at RT. Finally, polarization measurements from 14 emitters are used to determine visibility as well as dipole orientation of defect systems within the GaN crystal. Our results underpin some of the fundamental properties of SPE in GaN both at cryogenic and RT, and define the benchmark for future work in GaN-based single-photon technologies.

quant-ph↗

arXiv2017

Photo-induced blinking in a solid state quantum system

Solid state single photon emitters (SPEs) are one of the prime components of many quantum nanophotonics devices. In this work, we report on an unusual, photo-induced blinking phenomenon of SPEs in gallium nitride (GaN). This is shown to be due to the modification in the transition kinetics of the emitter, via the introduction of additional laser-activated states. We investigate and characterize the blinking effect on the brightness of the source and the statistics of the emitted photons. Combining second-order correlation and fluorescence trajectory measurements, we determine the photo-dynamics of the trap states and characterize power dependent decay rates and characteristic off-time blinking. Our work sheds new light into understanding solid-state quantum system dynamics and, specifically, power-induced blinking phenomena in SPEs.

physics.optics↗

arXiv2017

Nanodiamonds with photostable, sub-gigahertz linewidths quantum emitters

Single photon emitters with narrow linewidths are highly sought after for applications in quantum information processing and quantum communications. In this letter, we report on a bright, highly polarized near infrared single photon emitter embedded in diamond nanocrystals with a narrow, sub GHz optical linewidths at 10K. The observed zero phonon line at ~ 780 nm is optically stable under low power resonant excitation and blue shifts as the excitation power increases. Our results highlight the prospect for using new near infrared color centers in nanodiamonds for quantum applications.

cond-mat.mes-hall↗

arXiv2016

Observation of room-temperature spontaneous superradiance from single diamond nanocrystals

We report the observation of room-temperature superradiance from single, highly luminescent diamond nanocrystals with spatial dimensions much smaller than the wavelength of light, and each containing a large number (~10^3) of embedded nitrogen-vacancy (NV) centres. After excitation of the nanodiamonds with an off-resonant, green laser pulse, we observe i) ultrafast radiative lifetimes down to ~ 1 ns, and ii) super-Poissonian photon bunching in the autocorrelation function of the light emitted from the fastest nanodiamonds. We explain our findings with a detailed theoretical model based on collective Dicke states and well-known properties of NV centres. Using a minimal set of fit parameters, the model captures both the wide range of different lifetimes and the nontrivial photon correlations found in the experiments. The results pave the way towards a systematic study of superradiance in a well controlled, solid-state quantum system at room temperature. Ultimately, quantum engineering of superradiance in diamond has the potential for advancing applications in quantum sensing, energy harvesting, and efficient photon detection.

quant-ph↗

arXiv2011

Enhanced spontaneous emission from nanodiamond colour centres on opal photonic crystal

Colour centres in diamond are promising candidates as a platform for quantum technologies and biomedical imaging based on spins and/or photons. Controlling the emission properties of colour centres in diamond is a key requirement for developing efficient single photon sources with high collection efficiency. A number of groups have produced enhancement in the emission rate over narrow wavelength ranges by coupling single emitters in nanodiamond crystals to resonant electromagnetic structures. Here we characterise in detail the spontaneous emission rates of nitrogen-vacancy centres positioned in various locations on a structured substrate. We show an average factor of 1.5 enhancement of the total emission rate when nanodiamonds are on an opal photonic crystal surface, and observe changes in the lifetime distribution. We present a model to explain these observations and associate the lifetime properties with dipole orientation and polarization effects.

quant-ph↗

arXiv2009

Prediction and measurement of the size-dependent stability of fluorescence in diamond over the entire nanoscale

Fluorescent defects in non-cytotoxic diamond nanoparticles are candidates for qubits in quantum computing, optical labels in biomedical imaging and sensors in magnetometry. For each application these defects need to be optically and thermodynamically stable, and included in individual particles at suitable concentrations (singly or in large numbers). In this letter, we combine simulations, theory and experiment to provide the first comprehensive and generic prediction of the size, temperature and nitrogen-concentration dependent stability of optically active NV defects in nanodiamonds.

cond-mat.mtrl-sci↗