Temperature dependence of photoluminescence lifetime of atomically-thin WSe2 layer.

At cryogenic temperatures, the photoluminescence (PL) spectrum of monolayer WSe2 features a number of lines related to the recombination of so-called localized excitons (LEs). The intensity of these lines strongly decreases with increasing temperature. In order to understand the mechanism behind this phenomenon we carried out a time-resolved experiment, which revealed a similar trend in the PL decay time. Our results identify the opening of additional non-radiative relaxation channels as a primary cause of the observed temperature quenching of the LEs' PL.

Energy Spectrum of Two-Dimensional Excitons in a Nonuniform Dielectric Medium.

We demonstrate that, in monolayers (MLs) of semiconducting transition metal dichalcogenides, the s-type Rydberg series of excitonic states follows a simple energy ladder: ε_{n}=-Ry^{*}/(n+δ)^{2}, n=1,2,…, in which Ry^{*} is very close to the Rydberg energy scaled by the dielectric constant of the medium surrounding the ML and by the reduced effective electron-hole mass, whereas the ML polarizability is accounted for only by δ. This is justified by the analysis of experimental data on excitonic resonances, as extracted from magneto-optical measurements of a high-quality WSe_{2} ML encapsulated in hexagonal boron nitride (hBN), and well reproduced with an analytically solvable Schrödinger equation when approximating the electron-hole potential in the form of a modified Kratzer potential. Applying our convention to other MoSe_{2}, WS_{2}, MoS_{2} MLs encapsulated in hBN, we estimate an apparent magnitude of δ for each of the studied structures. Intriguingly, δ is found to be close to zero for WSe_{2} as well as for MoS_{2} monolayers, what implies that the energy ladder of excitonic states in these two-dimensional structures resembles that of Rydberg states of a three-dimensional hydrogen atom.

Probing and Manipulating Valley Coherence of Dark Excitons in Monolayer WSe_{2}.

Monolayers of semiconducting transition metal dichalcogenides are two-dimensional direct-gap systems which host tightly bound excitons with an internal degree of freedom corresponding to the valley of the constituting carriers. Strong spin-orbit interaction and the resulting ordering of the spin-split subbands in the valence and conduction bands makes the lowest-lying excitons in WX_{2} (X being S or Se) spin forbidden and optically dark. With polarization-resolved photoluminescence experiments performed on a WSe_{2} monolayer encapsulated in a hexagonal boron nitride, we show how the intrinsic exchange interaction in combination with the applied in-plane and/or out-of-plane magnetic fields enables one to probe and manipulate the valley degree of freedom of the dark excitons.

Cloning of Dirac fermions in graphene superlattices.

Superlattices have attracted great interest because their use may make it possible to modify the spectra of two-dimensional electron systems and, ultimately, create materials with tailored electronic properties. In previous studies (see, for example, refs 1-8), it proved difficult to realize superlattices with short periodicities and weak disorder, and most of their observed features could be explained in terms of cyclotron orbits commensurate with the superlattice. Evidence for the formation of superlattice minibands (forming a fractal spectrum known as Hofstadter's butterfly) has been limited to the observation of new low-field oscillations and an internal structure within Landau levels. Here we report transport properties of graphene placed on a boron nitride substrate and accurately aligned along its crystallographic directions. The substrate's moiré potential acts as a superlattice and leads to profound changes in the graphene's electronic spectrum. Second-generation Dirac points appear as pronounced peaks in resistivity, accompanied by reversal of the Hall effect. The latter indicates that the effective sign of the charge carriers changes within graphene's conduction and valence bands. Strong magnetic fields lead to Zak-type cloning of the third generation of Dirac points, which are observed as numerous neutrality points in fields where a unit fraction of the flux quantum pierces the superlattice unit cell. Graphene superlattices such as this one provide a way of studying the rich physics expected in incommensurable quantum systems and illustrate the possibility of controllably modifying the electronic spectra of two-dimensional atomic crystals by varying their crystallographic alignment within van der Waals heterostuctures.

Singlet and triplet trions in WS2 monolayer encapsulated in hexagonal boron nitride.

Embedding a WS2 monolayer in flakes of hexagonal boron nitride allowed us to resolve and study the photoluminescence response due to both singlet and triplet states of negatively charged excitons (trions) in this atomically thin semiconductor. The energy separation between the singlet and triplet states has been found to be relatively small reflecting rather weak effects of the electron-electron exchange interaction for the trion triplet in a WS2 monolayer, which involves two electrons with the same spin but from different valleys. Polarization-resolved experiments demonstrate that the helicity of the excitation light is better preserved in the emission spectrum of the triplet trion than in that of the singlet trion. Finally, the singlet (intravalley) trions are found to be observable even at ambient conditions whereas the emission due to the triplet (intervalley) trions is only efficient at low temperatures.

Magneto-Optical Signature of Massless Kane Electrons in Cd_{3}As_{2}.

We report on optical reflectivity experiments performed on Cd_{3}As_{2} over a broad range of photon energies and magnetic fields. The observed response clearly indicates the presence of 3D massless charge carriers. The specific cyclotron resonance absorption in the quantum limit implies that we are probing massless Kane electrons rather than symmetry-protected 3D Dirac particles. The latter may appear at a smaller energy scale and are not directly observed in our infrared experiments.

Quality Heterostructures from Two-Dimensional Crystals Unstable in Air by Their Assembly in Inert Atmosphere.

Many layered materials can be cleaved down to individual atomic planes, similar to graphene, but only a small minority of them are stable under ambient conditions. The rest react and decompose in air, which has severely hindered their investigation and potential applications. Here we introduce a remedial approach based on cleavage, transfer, alignment, and encapsulation of air-sensitive crystals, all inside a controlled inert atmosphere. To illustrate the technology, we choose two archetypal two-dimensional crystals that are of intense scientific interest but are unstable in air: black phosphorus and niobium diselenide. Our field-effect devices made from their monolayers are conductive and fully stable under ambient conditions, which is in contrast to the counterparts processed in air. NbSe2 remains superconducting down to the monolayer thickness. Starting with a trilayer, phosphorene devices reach sufficiently high mobilities to exhibit Landau quantization. The approach offers a venue to significantly expand the range of experimentally accessible two-dimensional crystals and their heterostructures.

Landau level spectroscopy of electron-electron interactions in graphene.

We present magneto-Raman scattering studies of electronic inter-Landau level excitations in quasineutral graphene samples with different strengths of Coulomb interaction. The band velocity associated with these excitations is found to depend on the dielectric environment, on the index of Landau level involved, and to vary as a function of the magnetic field. This contradicts the single-particle picture of noninteracting massless Dirac electrons but is accounted for by theory when the effect of electron-electron interaction is taken into account. Raman active, zero-momentum inter-Landau level excitations in graphene are sensitive to electron-electron interactions due to the nonapplicability of the Kohn theorem in this system, with a clearly nonparabolic dispersion relation.

Magneto-optics of massive dirac fermions in bulk Bi2Se3.

We report on magneto-optical studies of Bi2Se3, a representative member of the 3D topological insulator family. Its electronic states in bulk are shown to be well described by a simple Dirac-type Hamiltonian for massive particles with only two parameters: the fundamental band gap and the band velocity. In a magnetic field, this model implies a unique property-spin splitting equal to twice the cyclotron energy: Es=2Ec. This explains the extensive magnetotransport studies concluding a fortuitous degeneracy of the spin and orbital split Landau levels in this material. The Es=2Ec match differentiates the massive Dirac electrons in bulk Bi2Se3 from those in quantum electrodynamics, for which Es=Ec always holds.

Intrinsic terahertz plasmons and magnetoplasmons in large scale monolayer graphene.

We show that in graphene epitaxially grown on SiC the Drude absorption is transformed into a strong terahertz plasmonic peak due to natural nanoscale inhomogeneities, such as substrate terraces and wrinkles. The excitation of the plasmon modifies dramatically the magneto-optical response and in particular the Faraday rotation. This makes graphene a unique playground for plasmon-controlled magneto-optical phenomena thanks to a cyclotron mass 2 orders of magnitude smaller than in conventional plasmonic materials such as noble metals.

Cyclotron motion in the vicinity of a Lifshitz transition in graphite.

Graphite, a model (semi)metal with trigonally warped bands, is investigated with a magnetoabsorption experiment and viewed as an electronic system in the vicinity of the Lifshitz transition. A characteristic pattern of up to 20 cyclotron resonance harmonics has been observed. This large number of resonances, their relative strengths and characteristic shapes trace the universal properties of the electronic states near a separatrix in momentum space. Quantum-mechanical perturbative methods with respect to the trigonal warping term hardly describe the data which are, on the other hand, fairly well reproduced within a quasiclassical approach and conventional band structure model. Trigonal symmetry is preserved in graphite in contrast to a similar system, bilayer graphene.

Resonant excitation of graphene k-phonon and intra-landau-level excitons in magneto-optical spectroscopy [corrected].

Precise infrared magnetotransmission experiments have been performed in magnetic fields up to 32 T on a series of multilayer epitaxial graphene samples. We observe changes in the spectral features and broadening of the main cyclotron transition when the incoming photon energy is in resonance with the lowest Landau level separation and the energy of a K point optical phonon. We have developed a theory that explains and quantitatively reproduces the frequency and magnetic field dependence of the phenomenon as the absorption of a photon together with the simultaneous creation of an intervalley, intra-Landau-level exciton, and a K phonon.

Magneto-Raman scattering of graphene on graphite: electronic and phonon excitations.

Magneto-Raman-scattering experiments from the surface of graphite reveal novel features associated to purely electronic excitations which are observed in addition to phonon-mediated resonances. Graphene-like and graphite domains are identified through experiments with ∼1 µm spatial resolution performed in magnetic fields up to 32 T. Polarization resolved measurements emphasize the characteristic selection rules for electronic transitions in graphene. Graphene on graphite displays the unexpected hybridization between optical phonon and symmetric across the Dirac point inter Landau level transitions. The results open new experimental possibilities--to use light scattering methods in studies of graphene under quantum Hall effect conditions.

Quantum interference in exciton-Mn spin interactions in a CdTe semiconductor quantum dot.

We show theoretically and experimentally the existence of a new quantum-interference effect between the electron-hole interactions and the scattering by a single Mn impurity. The theoretical model, including electron-valence-hole correlations, the short- and long-range exchange interaction of a Mn ion with the heavy hole and with electron and anisotropy of the quantum dot, is compared with photoluminescence spectroscopy of CdTe dots with single magnetic ions. We show how the design of the electronic levels of a quantum dot enables the design of an exciton, control of the quantum interference, and hence engineering of light-Mn interaction.

Carrier scattering from dynamical magnetoconductivity in quasineutral epitaxial graphene.

The energy dependence of the electronic scattering time is probed by Landau level spectroscopy in quasineutral multilayer epitaxial graphene. From the broadening of overlapping Landau levels we find that the scattering rate 1/τ increases linearly with energy ϵ. This implies a surprising property of the Landau level spectrum in graphene-the number of resolved Landau levels remains constant with the applied magnetic field. Insights are given about possible scattering mechanisms and carrier mobilities in the graphene system investigated.

Carrier relaxation in epitaxial graphene photoexcited near the Dirac point.

We study the carrier dynamics in epitaxially grown graphene in the range of photon energies from 10 to 250 meV. The experiments complemented by microscopic modeling reveal that the carrier relaxation is significantly slowed down as the photon energy is tuned to values below the optical-phonon frequency; however, owing to the presence of hot carriers, optical-phonon emission is still the predominant relaxation process. For photon energies about twice the value of the Fermi energy, a transition from pump-induced transmission to pump-induced absorption occurs due to the interplay of interband and intraband processes.

Valley pseudospin relaxation of charged excitons in monolayer MoTe2.

Zeeman effect induced by the magnetic field introduces a splitting between the two valleys at K + and K - points of the Brillouin zone in monolayer semiconducting transition metal dichalcogenides. In consequence, the photoluminescence signal exhibits a field dependent degree of circular polarization. We present a comprehensive study of this effect in the case of a trion in monolayer MoTe2, showing that although time integrated data allows us to deduce a g-factor of the trion state, such an analysis cannot be substantiated by the timescales revealed in the time-resolved experiments.

Spatially resolved optical spectroscopy in extreme environment of low temperature, high magnetic fields and high pressure.

We present an experimental setup developed to perform optical spectroscopy experiments (Raman scattering and photoluminescence measurements) with a micrometer spatial resolution in an extreme environment of low temperature, high magnetic field, and high pressure. This unique experimental setup, to the best of our knowledge, allows us to deeply explore the phase diagram of condensed matter systems by independently tuning these three thermodynamic parameters while monitoring the low-energy excitations (electronic, phononic, or magnetic excitations) to spatially map the Raman scattering response or to investigate objects with low dimensions. We apply this technique to bulk FePS3, a layered antiferromagnet with a Néel temperature of T ≈ 120 K.

The optical response of artificially twisted MoS[Formula: see text] bilayers.

Two-dimensional layered materials offer the possibility to create artificial vertically stacked structures possessing an additional degree of freedom-the interlayer twist. We present a comprehensive optical study of artificially stacked bilayers (BLs) MoS[Formula: see text] encapsulated in hexagonal BN with interlayer twist angle ranging from 0[Formula: see text] to 60[Formula: see text] using Raman scattering and photoluminescence spectroscopies. It is found that the strength of the interlayer coupling in the studied BLs can be estimated using the energy dependence of indirect emission versus the A[Formula: see text]-E[Formula: see text] energy separation. Due to the hybridization of electronic states in the valence band, the emission line related to the interlayer exciton is apparent in both the natural (2H) and artificial (62[Formula: see text]) MoS[Formula: see text] BLs, while it is absent in the structures with other twist angles. The interlayer coupling energy is estimated to be of about 50 meV. The effect of temperature on energies and intensities of the direct and indirect emission lines in MoS[Formula: see text] BLs is also quantified.

Towards practical applications of quantum emitters in boron nitride.

We demonstrate quantum emission capabilities from boron nitride structures which are relevant for practical applications and can be seamlessly integrated into a variety of heterostructures and devices. First, the optical properties of polycrystalline BN films grown by metalorganic vapour-phase epitaxy are inspected. We observe that these specimens display an antibunching in the second-order correlation functions, if the broadband background luminescence is properly controlled. Furthermore, the feasibility to use flexible and transparent substrates to support hBN crystals that host quantum emitters is explored. We characterise hBN powders deposited onto polydimethylsiloxane films, which display quantum emission characteristics in ambient environmental conditions.