Optical spectroscopy in high magnetic fields B ≤ 65 T is used to reveal the very different nature of carriers in monolayer and bulk transition metal dichalcogenides. In monolayer WSe2, the exciton ...emission shifts linearly with the magnetic field and exhibits a splitting that originates from the magnetic field induced valley splitting. The monolayer data can be described using a single particle picture with a Dirac-like Hamiltonian for massive Dirac Fermions, with an additional term to phenomenologically include the valley splitting. In contrast, in bulk WSe2 where the inversion symmetry is restored, transmission measurements show a distinctly excitonic behavior with absorption to the 1s and 2s states. Magnetic field induces a spin splitting together with a small diamagnetic shift and cyclotron like behavior at high fields, which is best described within the hydrogen model.
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.
Raman scattering and photoluminescence (PL) emission are used to investigate a single layer of tungsten disulfide (WS sub(2)) obtained by exfoliating n-type bulk crystals. Direct gap emission with ...both neutral and charged exciton recombination is observed in the low temperature PL spectra. The ratio between the trion and exciton emission can be tuned simply by varying the excitation power. Moreover, the intensity of the trion emission can be independently tuned using additional subband gap laser excitation.
Perovskite solar cells with record power conversion efficiency are fabricated by alloying both hybrid and fully inorganic compounds. While the basic electronic properties of the hybrid perovskites ...are now well understood, key electronic parameters for solar cell performance, such as the exciton binding energy of fully inorganic perovskites, are still unknown. By performing magneto-transmission measurements, we determine with high accuracy the exciton binding energy and reduced mass of fully inorganic CsPbX3 perovskites (X = I, Br, and an alloy of these). The well-behaved (continuous) evolution of the band gap with temperature in the range of 4–270 K suggests that fully inorganic perovskites do not undergo structural phase transitions like their hybrid counterparts. The experimentally determined dielectric constants indicate that at low temperature, when the motion of the organic cation is frozen, the dielectric screening mechanism is essentially the same for both hybrid and inorganic perovskites and is dominated by the relative motion of atoms within the lead halide cage.
Multilayer epitaxial graphene is investigated using far infrared transmission experiments in the different limits of low magnetic fields and high temperatures. The cyclotron-resonance-like absorption ...is observed at low temperature in magnetic fields below 50 mT, probing the nearest vicinity of the Dirac point. The carrier mobility is found to exceed 250,000 cm2/(V x s). In the limit of high temperatures, the well-defined Landau level quantization is observed up to room temperature at magnetic fields below 1 T, a phenomenon unusual in solid state systems. A negligible increase in the width of the cyclotron resonance lines with increasing temperature indicates that no important scattering mechanism is thermally activated.
Stacking atomic monolayers of semiconducting transition metal dichalcogenides (TMDs) has emerged as an effective way to engineer their properties. In principle, the staggered band alignment of TMD ...heterostructures should result in the formation of interlayer excitons with long lifetimes and robust valley polarization. However, these features have been observed simultaneously only in MoSe2/WSe2 heterostructures. Here we report on the observation of long-lived interlayer exciton emission in a MoS2/MoSe2/MoS2 trilayer van der Waals heterostructure. The interlayer nature of the observed transition is confirmed by photoluminescence spectroscopy, as well as by analyzing the temporal, excitation power, and temperature dependence of the interlayer emission peak. The observed complex photoluminescence dynamics suggests the presence of quasi-degenerate momentum-direct and momentum-indirect bandgaps. We show that circularly polarized optical pumping results in long-lived valley polarization of interlayer exciton. Intriguingly, the interlayer exciton photoluminescence has helicity opposite to the excitation. Our results show that through a careful choice of the TMDs forming the van der Waals heterostructure it is possible to control the circular polarization of the interlayer exciton emission.
From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed ...with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet (S = 0) and dark triplet quintet (S = 1, 2) configurations: This induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3–5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site selectivity can be achieved for organic spin pairs in a broad range of systems.
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