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Tomasz Jakubczyk

Publications and source records attributed to Tomasz Jakubczyk.

At least 19 recordsLinked to original sources

Efficient Quasi-Resonant, Polarization-Selective Excitation of GaN Quantum Emitters

Defect centers in GaN emerge as bright sources of single-photons which recently have been demonstrated to optically interface a localized spin. However, the structure and composition of these defects as well as their efficient excitation techniques were not a subject of thorough studies. This work presents evidence that by tuning the excitation laser energy to specific resonance values the excitation efficiency can be enhanced, resulting in relative increase of photoluminescence intensity by up to an order of magnitude. The resonances can be selectively addressed with linearly polarized light, while the emission dipole remains unchanged, enabling polarization-controlled enhancement. These results establish an efficient way of excitation for GaN-based emitters, thereby increasing the generation rate of photons. The data is consistent with excitation via localized vibrational modes associated with point-defect complexes, establishing a practical quasi-resonant route to brighter, polarization-addressable operation of GaN defect emitters and clarifying their energy-level structure.

cond-mat.mtrl-sci

Off-resonant photoluminescence spectroscopy of high-optical quality single photon emitters in GaN

In this work, we analyze the relevance of excitation parameters on the emission from single-photon emitting defect centers in GaN. We investigate the absorption spectrum of different emitters by photoluminescence excitation technique at 10\,K. We report large spectral jumps (shifts up to 22\,meV) in the emitters' zero-phonon line (ZPL). The likelihood of such jumps is increased by the change in excitation energy. The shifts indicate a large built-in dipole moment of the defects and suggest a possibility to electrically tune their ZPL in a wide range. From the photoluminescence excitation studies, we observe that for majority of the emitters the absorption peaks exist between 2 and 2.55\,eV. The absorption peaks vary from emitter to emitter, and no universal absorption pattern is apparent. Finally, for selected emitters we observe significantly reduced spectral diffusion and instrument-limited linewidth of $138\,μeV$ (0.04\,nm).These findings show a new perspective for atomic defect GaN emitters as sources of coherent photons, shine new light on their energy level structure and show the possibility of tuning the ZPL, paving the way to fully harness their potential for applications in quantum technologies.

cond-mat.mtrl-sci

A numerical toy model of Langevin dynamics provides real-time visualization of colloidal microdroplet evaporation

We have developed and tested a simplified but versatile numerical model of nanoparticles' aggregation using Langevin dynamics. The model is particularly capable of simulating aggregation in an evaporating (or condensing) microdroplet. It runs on a graphics processing unit (GPU), which makes it sufficiently fast for real-time conceptualization tasks. We have verified the results of modeling against the findings from two types of experiments we conducted in electrodynamic traps. Firstly, our model helped us to elucidate the phenomenon of scattering `revival', often observed during the evaporation of composite microdroplets. Further on, we were able to mimic our experiments, in which the microdroplets were dried up to form nanoparticle (NP) aggregates, and then soft-landed. Thus we could compare model predictions with SEM imaging. The model was tested for up to $2.5\times 10^5$ nanoparticles of several coexisting types. Several types of interactions can be accounted for: inter-particle: Lennard-Jones and Coulomb; external: dispersion medium viscosity, centrifugal force, gravity, surface tension, and interface movement. Brownian motion of nanoparticles can be freely controlled. The core program is accompanied by scripts extracting statistical NP aggregates properties in post-processing -- fractal dimension and radial distribution functions. The codes are made available in public repositories. Several diverse evolution scenarios are presented.

cond-mat.soft

Luminescent nanoparticles in a shrinking spherical cavity -- probing the evaporating microdroplets of colloidal suspension -- optical lattices and structural transitions

We investigated the possibility of using charged luminescent nanoparticles as nanoprobes for studying the evolution scenarios of surface and internal structure of slowly evaporating free (light-absorbing) microdroplets of suspension. Three concentrations (1, 10 and 50 mg/ml) of luminescent nanoparticles were used. Single microdroplets were kept in a linear electrodynamic quadrupole trap and the luminescence was excited with a CW IR laser with an irradiance of ~50 W/mm2. Since the microdroplet acted as an optical spherical resonance cavity, the interaction of nanoparticles with light both reflected and modified the internal light field mode structure. Depending on the nanoparticle concentration used, it led, among others, to a very significant increase in modulation depth and narrowing of spherical cavity resonance maxima (morphology dependent resonances - MDRs) observed both in luminescence and scattering, the abrupt changes in the ratio between the luminescence and the scattering and the bi-stability in luminescence signal. The observed phenomena could be attributed to the interaction of optical MDRs with nanoparticle lattice shells forming and changing their structure at the microdroplet surface. In this way, the formation and collapse of such lattices could be detected.

physics.optics

Coherent dynamics of a single Mn-doped quantum dot revealed by four-wave mixing spectroscopy

For future quantum technologies the combination of a long quantum state lifetime and an efficient interface with external optical excitation are required. In solids, the former is for example achieved by individual spins, while the latter is found in semiconducting artificial atoms combined with modern photonic structures. One possible combination of the two aspects is reached by doping a single quantum dot, providing a strong excitonic dipole, with a magnetic ion, that incorporates a characteristic spin texture. Here, we perform four-wave mixing spectroscopy to study the system's quantum coherence properties. We characterize the optical properties of the undoped CdTe quantum dot and find a strong photon echo formation which demonstrates a significant inhomogeneous spectral broadening. Incorporating the Mn$^{2+}$ ion introduces its spin-5/2 texture to the optical spectra via the exchange interaction, manifesting as six individual spectral lines in the coherent response. The random flips of the Mn-spin result in a special type of spectral wandering between the six transition energies, which is fundamentally different from the quasi-continuous spectral wandering that results in the Gaussian inhomogeneous broadening. Here, the discrete spin-ensemble manifests in additional dephasing and oscillation dynamics.

cond-mat.mes-hall

A chiral one-dimensional atom using a quantum dot in an open microcavity

In nanostructures, the light-matter interaction can be engineered to be chiral. In the fully quantum regime, a chiral one-dimensional atom, a photon propagating in one direction interacts with the atom; a photon propagating in the other direction does not. Chiral quantum optics has applications in creating nanoscopic single-photon routers, circulators, phase-shifters and two-photon gates. Furthermore, the directional photon-exchange between many emitters in a chiral system may enable the creation of highly exotic quantum states. Here, we present a new way of implementing chiral quantum optics $-$ we use a low-noise quantum dot in an open microcavity. Specifically, we demonstrate the non-reciprocal absorption of single photons, a single-photon diode. The non-reciprocity, the ratio of the transmission in the forward-direction to the transmission in the reverse direction, is as high as 10.7 dB, and is optimised $\textit{in situ}$ by tuning the photon-emitter coupling to the optimal operating condition ($β= 0.5$). Proof that the non-reciprocity arises from a single quantum emitter lies in the nonlinearity with increasing input laser power, and in the photon statistics $-$ ultralow-power laser light propagating in the diode's reverse direction results in a highly bunched output ($g^{(2)}(0) = 101$), showing that the single-photon component is largely removed. The results pave the way to a single-photon phase shifter, and, by exploiting a quantum dot spin, to two-photon gates and quantum non-demolition single-photon detectors.

quant-ph

Low charge-noise nitrogen-vacancy centers in diamond created using laser writing with a solid-immersion lens

We report on pulsed-laser induced generation of nitrogen-vacancy (NV) centers in diamond facilitated by a solid-immersion lens (SIL). The SIL enables laser writing at energies as low as 5.8 nJ per pulse and allows vacancies to be formed close to a diamond surface without inducing surface graphitization. We operate in the previously unexplored regime where lattice vacancies are created following tunneling breakdown rather than multiphoton ionization. We present three samples in which NV-center arrays were laser-written at distances between ~1 $μ$m and 40 $μ$m from a diamond surface, all presenting narrow distributions of optical linewidths with means between 62.1 MHz and 74.5 MHz. The linewidths include the effect of long-term spectral diffusion induced by a 532 nm repump laser for charge-state stabilization, thereby emphasizing the particularly low charge-noise environment of the created color centers. Such high-quality NV centers are excellent candidates for practical applications employing two-photon quantum interference with separate NV centers. Finally, we propose a model for disentangling power broadening from inhomogeneous broadening in the NV center optical linewidth.

physics.optics

High quality-factor diamond-confined open microcavity

With a highly coherent, optically addressable electron spin, the nitrogen vacancy (NV) centre in diamond is a promising candidate for a node in a quantum network. However, the NV centre is a poor source of coherent single photons owing to a long radiative lifetime, a small branching ratio into the zero-phonon line (ZPL) and a poor extraction efficiency out of the high-index host material. In principle, these three shortcomings can be addressed by resonant coupling to a single mode of an optical cavity. Utilising the weak-coupling regime of cavity electrodynamics, resonant coupling between the ZPL and a single cavity-mode enhances the transition rate and branching ratio into the ZPL. Furthermore, the cavity channels the light into a well-defined mode thereby facilitating detection with external optics. Here, we present an open Fabry-Perot microcavity geometry containing a single-crystal diamond membrane, which operates in a regime where the vacuum electric field is strongly confined to the diamond membrane. There is a field anti-node at the diamond-air interface. Despite the presence of surface losses, quality factors exceeding $120\,000$ and a finesse $\mathcal{F}=11\,500$ were observed. We investigate the interplay between different loss mechanisms, and the impact these loss channels have on the performance of the cavity. This analysis suggests that the "waviness" (roughness with a spatial frequency comparable to that of the microcavity mode) is the mechanism preventing the quality factors from reaching even higher values. Finally, we apply the extracted cavity parameters to the NV centre and calculate a predicted Purcell factor exceeding 150.

quant-ph

Assessing the properties of a colloidal suspension with the aid of deep learning

Convolution neural networks were applied to classify speckle images generated from nano-particle suspensions and thus to recognise suspensions. The speckle images in the form of movies were obtained from suspensions placed in a thin cuvette. The classifier was trained, validated and tested on both single component monodispersive suspensions, as well as on two-component suspensions. It was able to properly recognise all the 73 classes - different suspensions from the training set, which is far beyond the capabilities of the human experimenter, and shows the capability of learning many more. The classes comprised different nanoparticle material and size, as well as different concentrations of the suspended phase. We also examined the capability of the system to generalise, by testing a system trained on single-component suspensions with two-component suspensions. The capability to generalise was found promising but significantly limited. A classification system using neural network was also compared with the one using support vector machine (SVM). SVM was found much more resource-consuming and thus could not be tested on full-size speckle images. Using image fragments very significantly deteriorates results for both SVM and neural networks. We showed that nanoparticle (colloidal) suspensions comprising even a large multi-parameter set of classes can be quickly identified using speckle images classified with convolution neural network.

physics.app-ph

Statistically Modeling Optical Linewidths of Nitrogen Vacancy Centers in Post-Implanted Nanostructures

We investigate the effects of a novel approach to diamond nanofabrication and nitrogen vacancy (NV) center formation on the optical linewidth of the NV zero-phonon line (ZPL). In this post-implantation method, nitrogen is implanted after all fabrication processes have been completed. We examine three post-implanted samples, one implanted with $^{14}$N and two with $^{15}$N isotopes. We perform photoluminescence excitation (PLE) spectroscopy to assess optical linewidths and optically detected magnetic resonance (ODMR) measurements to isotopically classify the NV centers. From this, we find that NV centers formed from nitrogen naturally occuring in the diamond lattice are characterized by a linewidth distribution peaked at an optical linewidth nearly two orders of magnitude smaller than the distribution characterizing most of the NV centers formed from implanted nitrogen. Surprisingly, we also observe a number of $^{15}$NV centers with narrow ($<500\,\mathrm{MHz}$) linewidths, implying that implanted nitrogen can yield NV centers with narrow optical linewidths. We further use a Bayesian approach to statistically model the linewidth distributions, to accurately quantify the uncertainty of fit parameters in our model, and to predict future linewidths within a particular sample. Our model is designed to aid comparisons between samples and research groups, in order to determine the best methods of achieving narrow NV linewidths in structured samples.

cond-mat.mes-hall

Dynamics of resonantly excited excitons in MoSe$_2$ and WS$_2$ single-layers monitored with four-wave mixing

We investigate dynamics of resonantly excited excitons in single-layers of MoSe$_2$ and WS$_2$ down to 4.5 K. To this end, we measure the delay dependence of the heterodyne four-wave mixing (FWM) amplitude induced by three, short laser pulses. This signal depends not only on the population of optically active excitons, which affects the absorption of the probe, but also on the population of optically inactive states, by interaction-induced energy shift, influencing the refractive index experienced by the probe. As such, it offers insight into density dynamics of excitons which do not directly couple to photons. Reproducing the coherent signal detected in amplitude and phase, the FWM delay dependence is modeled by a coherent superposition of several exponential decay components, with characteristic time constants from 0.1 picosecond up to 1 nanosecond. With increasing excitation intensity and/or temperature, we observe strong interference effects in the FWM field amplitude, resulting in progressively more complex and nonintuitive signal dynamics. We attribute this behaviour to increasingly populated exciton dark states, which change the FWM field phase by the relative effect on absorption and refractive index. We observe that exciton recombination occurs on a significantly longer timescale in WS$_2$ with respect to MoSe$_2$, which is attributed to the dark character of exciton ground state in the former and the bright in the latter.

cond-mat.mes-hall

Coherence and density dynamics of excitons in a single-layer MoS$_2$ reaching the homogeneous limit

We measure the coherent nonlinear response of excitons in a single-layer of molybdenum disulphide embedded in hexagonal boron nitride, forming a $h$-BN/MoS$_2$/$h$-BN heterostructure. Using four-wave mixing microscopy and imaging, we correlate the exciton homogeneous and inhomogeneous broadenings. We find that the exciton dynamics is governed by microscopic disorder on top of the ideal crystal properties. Analyzing the exciton ultra-fast density dynamics using amplitude and phase of the response, we investigate the relaxation pathways of the resonantly driven exciton population. The surface protection via encapsulation provides stable monolayer samples with low disorder, avoiding surface contaminations and the resulting exciton broadening and modifications of the dynamics. We identify areas localized to a few microns where the optical response is totally dominated by homogeneous broadening. Across the sample of tens of micrometers, weak inhomogeneous broadening and strain effects are observed, attributed to the remaining interaction with the $h$-BN and imperfections in the encapsulation process.

cond-mat.mes-hall

Exploring coherence of individual excitons in InAs quantum dots embedded in natural photonic defects: influence of the excitation intensity

The exact optical response of quantum few-level systems depends crucially on the exact choice of the incoming pulse areas. We use four-wave mixing (FWM) spectroscopy to infer the coherent response and dynamics of single InAs quantum dots (QDs) and study their pulse area dependence. By combining atomic force microscopy with FWM hyperspectral imaging, we show that the retrieved FWM signals originate from individual QDs enclosed in natural photonic defects. The optimized light-matter coupling in these defects allows us to perform our studies in a wide range of driving field amplitudes. When varying the pulse areas of the exciting laser pulses the so-called Rabi rotations can be resolved by the two-pulse FWM technique. We investigate these Rabi rotations within two- and three-level systems, both theoretically and experimentally, and explain their damping by the coupling to acoustic phonons. To highlight the importance of the pulse area influence, we show that the phonon-induced dephasing of QD excitons depends on the pulse intensity.

cond-mat.mes-hall

Coherent coupling of individual quantum dots measured with phase-referenced two-dimensional spectroscopy: photon echo versus double quantum coherence

We employ two-dimensional (2D) coherent, nonlinear spectroscopy to investigate couplings within individual InAs quantum dots (QD) and QD molecules. Swapping pulse ordering in a two-beam sequence permits to distinguish between rephasing and non-rephasing four-wave mixing (FWM) configurations. We emphasize the non-rephasing case, allowing to monitor two-photon coherence dynamics. Respective Fourier transform yields a double quantum 2D FWM map, which is corroborated with its single quantum counterpart, originating from the rephasing sequence. We introduce referencing of the FWM phase with the one carried by the driving pulses, overcoming the necessity of its active-stabilization, as required in 2D spectroscopy. Combining single and double quantum 2D FWM, provides a pertinent tool in detecting and ascertaining coherent coupling mechanisms between individual quantum systems, as exemplified experimentally.

cond-mat.mes-hall

Radiatively limited dephasing and exciton dynamics in MoSe$_2$ monolayers

By implementing four-wave mixing (FWM) micro-spectroscopy we measure coherence and population dynamics of the exciton transitions in monolayers of MoSe$_2$. We reveal their dephasing times T$_2$ and radiative lifetime T$_1$ in a sub-picosecond (ps) range, approaching T$_2$=2T$_1$, and thus indicating radiatively limited dephasing at a temperature of 6$\,$K. We elucidate the dephasing mechanisms by varying the temperature and by probing various locations on the flake exhibiting a different local disorder. At a nanosecond range, we observe the residual FWM produced by the incoherent excitons, which initially disperse towards the dark states, but then relax back to the optically active states within the light cone. By introducing polarization-resolved excitation, we infer inter-valley exciton dynamics, showing an initial polarization degree of around 30$\,\%$, constant during the initial sub-picosecond decay, followed by the depolarization on a picosecond timescale. The FWM hyperspectral imaging reveals the doped and undoped areas of the sample, allowing to investigate the neutral exciton, the charged one or both transitions at the same time. In the latter case, we observe the exciton-trion beating in the coherence evolution indicating their coherent coupling.

cond-mat.mes-hall

Single-color, in situ photolithography marking of individual CdTe/ZnTe Quantum Dots containing a single Mn2+ ion

A simple, single-color method for permanent marking of the position of individual self-assembled semiconductor Quantum Dots (QDs) at cryogenic temperatures is reported. The method combines in situ photolithography with standard micro-photoluminescence spectroscopy. Its utility is proven by a systematic magnetooptical study of a single CdTe/ZnTe QD containing a Mn2+ ion, where a magnetic field of up to 10 T in two orthogonal, Faraday and Voigt, configurations is applied to the same QD. The presented approach can be applied to a wide range of solid state nanoemitters.

cond-mat.mes-hall

Frequency cavity pulling induced by a single semiconductor quantum dot

We investigate the emission properties of a single semiconductor quantum dot deterministically coupled to a confined optical mode in the weak coupling regime. A strong pulling, broadening and narrowing of the cavity mode emission is evidenced when changing the spectral detuning between the emitter and the cavity. These features are theoretically accounted for by considering the phonon assisted emission of the quantum dot transition. These observations highlight a new situation for cavity quantum electrodynamics involving spectrally broad emitters.

quant-ph

In-plane radiative recombination channel of a dark exciton in self-assembled quantum dots

We demonstrate evidence for a radiative recombination channel of dark excitons in self-assembled quantum dots. This channel is due to a light hole admixture in the excitonic ground state. Its presence was experimentally confirmed by a direct observation of the dark exciton photoluminescence from a cleaved edge of the sample. The polarization resolved measurements revealed that a photon created from the dark exciton recombination is emitted only in the direction perpendicular to the growth axis. Strong correlation between the dark exciton lifetime and the in-plane hole g-factor enabled us to show that the radiative recombination is a dominant decay channel of the dark excitons in CdTe/ZnTe quantum dots.

cond-mat.mes-hall