M. Koperski

Single photon emitters in exfoliated WSe2 structures.

Crystal structure imperfections in solids often act as efficient carrier trapping centres, which, when suitably isolated, act as sources of single photon emission. The best known examples of such attractive imperfections are well-width or composition fluctuations in semiconductor heterostructures (resulting in the formation of quantum dots) and coloured centres in wide-bandgap materials such as diamond. In the recently investigated thin films of layered compounds, the crystal imperfections may logically be expected to appear at the edges of commonly investigated few-layer flakes of these materials exfoliated on alien substrates. Here, we report comprehensive optical micro-spectroscopy studies of thin layers of tungsten diselenide (WSe2), a representative semiconducting dichalcogenide with a bandgap in the visible spectral range. At the edges of WSe2 flakes (transferred onto Si/SiO2 substrates) we discover centres that, at low temperatures, give rise to sharp emission lines (100 μeV linewidth). These narrow emission lines reveal the effect of photon antibunching, the unambiguous attribute of single photon emitters. The optical response of these emitters is inherently linked to the two-dimensional properties of the WSe2 monolayer, as they both give rise to luminescence in the same energy range, have nearly identical excitation spectra and have very similar, characteristically large Zeeman effects. With advances in the structural control of edge imperfections, thin films of WSe2 may provide added functionalities that are relevant for the domain of quantum optoelectronics.

Designing quantum dots for solotronics

Solotronics, optoelectronics based on solitary dopants, is an emerging field of research and technology reaching the ultimate limit of miniaturization. It aims at exploiting quantum properties of individual ions or defects embedded in a semiconductor matrix. It has already been shown that optical control of a magnetic ion spin is feasible using the carriers confined in a quantum dot. However, a serious obstacle was the quenching of the exciton luminescence by magnetic impurities. Here we show, by photoluminescence studies on thus-far-unexplored individual CdTe dots with a single cobalt ion and CdSe dots with a single manganese ion, that even if energetically allowed, nonradiative exciton recombination through single-magnetic-ion intra-ionic transitions is negligible in such zero-dimensional structures. This opens solotronics for a wide range of as yet unconsidered systems. On the basis of results of our single-spin relaxation experiments and on the material trends, we identify optimal magnetic-ion quantum dot systems for implementation of a single-ion-based spin memory.

Exciton band structure in layered MoSe2: from a monolayer to the bulk limit

We present the micro-photoluminescence (μPL) and micro-reflectance contrast (μRC) spectroscopy studies on thin films of MoSe(2) with layer thicknesses ranging from a monolayer (1L) up to 5L. The thickness dependent evolution of the ground and excited state excitonic transitions taking place at various points of the Brillouin zone is determined. Temperature activated energy shifts and linewidth broadenings of the excitonic resonances in 1L, 2L and 3L flakes are accounted for by using standard formalisms previously developed for semiconductors. A peculiar shape of the optical response of the ground state (A) exciton in monolayer MoSe(2) is tentatively attributed to the appearance of a Fano-type resonance. Rather trivial and clearly decaying PL spectra of monolayer MoSe(2) with temperature confirm that the ground state exciton in this material is optically bright in contrast to a dark exciton ground state in monolayer WSe(2).

Picosecond charge variation of quantum dots under pulsed excitation

We present a spectroscopic study of excitation dynamics in self-assembled CdTe/ZnTe quantum dots. Insight into details of kinetics is obtained from the time-resolved microphotoluminescence, single photon correlation, and subpicosecond excitation correlation measurements done on single quantum dots. It is shown that the pulsed excitation at an energy above the energy gap of the barrier material results in separate capture of electrons and holes. We found that the capture of electrons by the quantum dot is delayed with respect to the capture of holes: the electron capture takes place in 20\char21{}40 ps after the excitation pulse, while the capture of holes is much faster.

Radiatively Limited Dephasing and Exciton Dynamics in MoSe2 Monolayers Revealed with Four-Wave Mixing Microscopy

By implementing four-wave mixing (FWM) microspectroscopy, we measure coherence and population dynamics of the exciton transitions in monolayers of MoSe2. We reveal their dephasing times T2 and radiative lifetime T1 in a subpicosecond (ps) range, approaching T2 = 2T1 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 the nanosecond range, we observe the residual FWM produced by the incoherent excitons, which initially disperse toward the dark states but then relax back to the optically active states within the light cone. By introducing polarization-resolved excitation, we infer intervalley exciton dynamics, revealing an initial polarization degree of around 30%, constant during the initial subpicosecond decay, followed by the depolarization on a picosecond time scale. The FWM hyperspectral imaging reveals the doped and undoped areas of the sample, allowing us to investigate the neutral exciton, the charged one, or both transitions at the same time. In the latter, we observe the exciton–trion beating in the coherence evolution indicating their coherent coupling.

Optical properties of atomically thin transition metal dichalcogenides: observations and puzzles

Abstract Recent results on the optical properties of monolayer and few layers of semiconducting transition metal dichalcogenides are reviewed. Experimental observations are presented and discussed in the frame of existing models, highlighting the limits of our understanding in this emerging field of research. We first introduce the representative band structure of these systems and their interband optical transitions. The effect of an external magnetic field is then considered to discuss Zeeman spectroscopy and optical pumping experiments, both revealing phenomena related to the valley degree of freedom. Finally, we discuss the observation of single photon emitters in different types of layered materials, including wide band gap hexagonal boron nitride. While going through these topics, we try to focus on open questions and on experimental observations, which do not yet have a clear explanation.

Coherent Precession of an Individual 5/2 Spin.

We present direct observation of a coherent spin precession of an individual Mn^{2+} ion, having both electronic and nuclear spins equal to 5/2, embedded in a CdTe quantum dot and placed in a magnetic field. The spin state evolution is probed in a time-resolved pump-probe measurement of absorption of the single dot. The experiment reveals subtle details of the large-spin coherent dynamics, such as nonsinusoidal evolution of states occupation, and beatings caused by the strain-induced differences in energy levels separation. Sensitivity of the large-spin impurity on the crystal strain opens the possibility of using it as a local strain probe.

Single photon emitters in boron nitride: More than a supplementary material

Abstract We present comprehensive optical studies of recently discovered single photon sources in boron nitride, which appear in form of narrow lines emitting centres. Here, we aim to compactly characterise their basic optical properties, including the demonstration of several novel findings, in order to inspire discussion about their origin and utility. Initial inspection reveals the presence of narrow emission lines in boron nitride powder and exfoliated flakes of hexagonal boron nitride deposited on Si/SiO2 substrates. Generally rather stable, the boron nitride emitters constitute a good quality visible light source. However, as briefly discussed, certain specimens reveal a peculiar type of blinking effects, which are likely related to existence of meta-stable electronic states. More advanced characterisation of representative stable emitting centres uncovers a strong dependence of the emission intensity on the energy and polarisation of excitation. On this basis, we speculate that rather strict excitation selectivity is an important factor determining the character of the emission spectra, which allows the observation of single and well-isolated emitters. Finally, we investigate the properties of the emitting centres in varying external conditions. Quite surprisingly, it is found that the application of a magnetic field introduces no change in the emission spectra of boron nitride emitters. Further analysis of the impact of temperature on the emission spectra and the features seen in second-order correlation functions is used to provide an assessment of the potential functionality of boron nitride emitters as single photon sources capable of room temperature operation.

Magnetic-field-induced abrupt spin-state transition in a quantum dot containing magnetic ions

We present the results of a comprehensive magneto-optical characterization of single CdTe quantum dots containing a few Mn2+ ions. We find that some quantum dots exhibit an unexpected evolution of excitonic photoluminescence spectrum with the magnetic field. At a certain value of the magnetic field, specific for every quantum dot, each of the broad spectral lines related to the recombination of various excitonic complexes confined inside the dot transforms into a pair of narrow lines split by several meV. We interpret this abrupt change in the character of excitonic emission spectrum as a consequence of a transition from a non-polarized state of the Mn2+ spins in a low field regime to a highly (almost fully) polarized state above the critical magnetic field. Various optical experiments, including polarization-resolved studies, investigation of different excitation regimes and time-resolved measurements corroborate this scenario. However, these measurements indicate also that the observed effect is not related or influenced by the photo-created charge carriers, but it is rather originating from unusual spin configuration in the cluster of Mn2+ ions.

Compensation of the exciton-ion exchange interaction in a quantum dot by application of a magnetic field

The exchange interaction between band carriers and electrons from the d-shell of a single magnetic ion embedded in a semiconductor quantum dot leads to the splitting of exciton-ion states which allows to optically read the ion spin state. The influence of this interaction on ion states can be described in terms of an effective magnetic field induced by the exciton. It means that the exchange interaction can be partially compensated by the application of a magnetic field along the growth axis. We study this effect for CdTe/ZnTe quantum dots with a single Mn2+ ion. The in-plane component added to the perpendicular magnetic field induces mixing of different ion spin states, resulting in multiple anticrossings of the excitonic photoluminescence lines of the dot. This enables detailed investigation of the compensation.