Highlights (EN)

Ultra-long-working-distance spectroscopy of single nanostructures with aspherical solid immersion microlenses

In light science and applications, equally important roles are played by efficient light emitters/detectors and by the optical elements responsible for light extraction and delivery. The latter should be simple, cost effective, broadband, versatile and compatible with other components of widely desired micro-optical systems. Ideally, they should also operate without high-numerical-aperture optics. Here, we demonstrate that all these requirements can be met with elliptical microlenses 3D printed on top of light emitters. Importantly, the microlenses we propose readily form the collected light into an ultra-low divergence beam (half-angle divergence below 1°) perfectly suited for ultra-long-working-distance optical measurements (600 mm with a 1-inch collection lens), which are not accessible to date with other spectroscopic techniques. Our microlenses can be fabricated on a wide variety of samples, including semiconductor quantum dots and fragile van der Waals heterostructures made of novel two-dimensional materials, such as monolayer and few-layer transition metal dichalcogenides.


Narrow Excitonic Lines and Large-Scale Homogeneity of Transition-Metal Dichalcogenide Monolayers Grown by Molecular Beam Epitaxy on Hexagonal Boron Nitride

Monolayer transition-metal dichalcogenides (TMDs) manifest exceptional optical properties related to narrow excitonic resonances. However, these properties have been so far explored only for structures produced by techniques inducing considerable large-scale inhomogeneity. In contrast, techniques which are essentially free from this disadvantage, such as molecular beam epitaxy (MBE), have to date yielded only structures characterized by considerable spectral broadening, which hinders most of the interesting optical effects. Here, we report for the first time on the MBE-grown TMD exhibiting narrow and resolved spectral lines of neutral and charged exciton. Moreover, our material exhibits unprecedented high homogeneity of optical properties, with variation of the exciton energy as small as ±0.16 meV over a distance of tens of micrometers. Our recipe for MBE growth is presented for MoSe2 and includes the use of atomically flat hexagonal boron nitride substrate. This recipe opens a possibility of producing TMD heterostructures with optical quality, dimensions, and homogeneity required for optoelectronic applications.


Direct measurement of hyperfine shifts and radiofrequency manipulation of the nuclear spins in individual CdTe/ZnTe quantum dots

We achieve direct detection of electron hyperfine shifts in individual CdTe/ZnTe quantum dots. For the previously inaccessible regime of strong magnetic fields Bz>0.1T, we demonstrate robust polarization of a few-hundred-particle nuclear spin bath, with an optical initialization time of 1ms and polarization lifetime exceeding 1s. Nuclear magnetic resonance spectroscopy of individual dots reveals strong electron-nuclear interactions characterized by Knight fields |Be|>50mT, an order of magnitude stronger than in III–V semiconductor quantum dots. Our studies confirm II–VI semiconductor quantum dots as a promising platform for hybrid electron-nuclear spin qubit registers, combining the excellent optical properties comparable to III–V dots and the dilute nuclear spin environment similar to group-IV semiconductors.


Triple threshold lasing from a photonic trap in a Te/Se-based optical microcavity

Lasing relies on light amplification in the active medium of an optical resonator. There are three lasing regimes in the emission from a quantum well coupled to a semiconductor microcavity. Polariton lasing in the strong light–matter coupling regime arises from the stimulated scattering of exciton-polaritons. Photon lasing in the weak coupling regime relies on either of two mechanisms: the stimulated recombination of excitons, or of an electron–hole plasma. So far, only one or two out of these three regimes have been reported for a given structure, independently of the material system studied. Here, we report on all three lasing regimes and provide evidence for a three-threshold behavior in the emission from a photonic trap in a Se/Te-based planar microcavity comprising a single CdSe/(Cd,Mg)Se quantum well. Our work establishes the so far unsettled relation between lasing regimes that differ by their light-matter coupling strength and degree of electron–hole Coulomb correlation.


Optical fiber micro-connector with nanometer positioning precision for rapid prototyping of photonic devices

Prototyping of fiber-coupled integrated photonic devices requires robust and reliable way of docking optical fibers to other structures, often with sub-micron accuracy. We have developed an optical fiber micro-connector 3D-printed with Direct Laser Writing on a planar substrate. The connector provides fiber core precision positioning better than 120 nm and sustains cryogenic cycling without any signs of degradation. It can be fabricated and used on glass and non-transparent substrates, including photonic integrated circuits, semiconductor samples, and microfluidic systems.


(Cd,Zn,Mg)Te-based microcavity on MgTe sacrificial buffer: Growth, lift-off, and transmission studies of polaritons

Opaque substrates precluded, so far, transmission studies of II-VI semiconductor microcavities. This work presents the design and molecular beam epitaxy growth of semimagnetic (Cd,Zn,Mn)Te quantum wells embedded into a (Cd,Zn,Mg)Te-based microcavity, which can be easily separated from the GaAs substrate. Our lift-off process relies on the use of a MgTe sacrificial layer which stratifies in contact with water. This allowed us to achieve a II-VI microcavity prepared for transmission measurements. We evidence the strong light-matter coupling regime using photoluminescence, reflectivity, and transmission measurements at the same spot on the sample. By comparing a series of reflectance spectra before and after lift-off, we prove that the microcavity quality remains high. Thanks to Mn content in quantum wells we show the giant Zeeman splitting of semimagnetic exciton-polaritons in our transmitting structure.


Tuning Valley Polarization in a WSe2 Monolayer with a Tiny Magnetic Field

In monolayers of semiconducting transition metal dichalcogenides, the light helicity (σ+ or σ−) is locked to the valley degree of freedom, leading to the possibility of optical initialization of distinct valley populations. However, an extremely rapid valley pseudospin relaxation (at the time scale of picoseconds) occurring for optically bright (electric-dipole active) excitons imposes some limitations on the development of opto-valleytronics. Here, we show that valley pseudospin relaxation of excitons can be significantly suppressed in a WSe2 monolayer, a direct-gap two-dimensional semiconductor with the exciton ground state being optically dark. We demonstrate that the already inefficient relaxation of the exciton pseudospin in such a system can be suppressed even further by the application of a tiny magnetic field of about 100 mT. Time-resolved spectroscopy reveals the pseudospin dynamics to be a two-step relaxation process. An initial decay of the pseudospin occurs at the level of dark excitons on a time scale of 100 ps, which is tunable with a magnetic field. This decay is followed by even longer decay (>1  ns), once the dark excitons form more complex pseudo-particles allowing for their radiative recombination. Our findings of slow valley pseudospin relaxation easily manipulated by the magnetic field open new prospects for engineering the dynamics of the valley pseudospin in transition metal dichalcogenides.


Magnetic ground state of an individual Fe2+ ion in strained semiconductor nanostructure

Single impurities with nonzero spin and multiple ground states offer a degree of freedom that can be utilized to store the quantum information. However, Fe2+ dopant is known for having a single nondegenerate ground state in the bulk host semiconductors and thus is of little use for spintronic applications. Here we show that the well-established picture of Fe2+ spin configuration can be modified by subjecting the Fe2+ ion to high strain, for example, produced by lattice mismatched epitaxial nanostructures. Our analysis reveals that high strain induces qualitative change in the ion energy spectrum and results in nearly doubly degenerate ground state with spin projection Sz=±2. We provide an experimental proof of this concept using a new system: a strained epitaxial quantum dot containing individual Fe2+ ion. Magnetic character of the Fe2+ ground state in a CdSe/ZnSe dot is revealed in photoluminescence experiments by exploiting a coupling between a confined exciton and the single-iron impurity. We also demonstrate that the Fe2+ spin can be oriented by spin-polarized excitons, which opens a possibility of using it as an optically controllable two-level system free of nuclear spin fluctuations.


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 heterostructures1, 2 (resulting in the formation of quantum dots) and coloured centres in wide-bandgap materials such as diamond3, 4, 5. 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 onfined 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.


Coherent Precession of an Individual 5/2 Spin

We present direct observation of a coherent spin precession of an individual Mn2+ 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.


Inhibition and Enhancement of the Spontaneous Emission of Quantum Dots in Micropillar Cavities with Radial-Distributed Bragg Reflectors

We present a micropillar cavity where nondesired radial emission is inhibited. The photonic confinement in such a structure is improved by implementation of an additional concentric radial-distributed Bragg reflector. Such a reflector increases the reflectivity in all directions perpendicular to the micropillar axis from a typical value of 15–31% to above 98%. An inhibition of the spontaneous emission of off-resonant excitonic states of quantum dots embedded in the microcavity is revealed by time-resolved experiments. It proves a decreased density of photonic states related to unwanted radial leakage of photons out of the micropillar. For on-resonance conditions, we find that the dot emission rate is increased, evidencing the Purcell enhancement of spontaneous emission. The proposed design can increase the efficiency of single-photon sources and bring to micropillar cavities the functionalities based on lengthened decay times.

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