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Second-harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS 2 , that shows strong optical oscillator strength for the intra- but also interlayer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations. Since interlayer exciton transitions are highly tunable also by choosing twist angle and material combination our results open up new approaches for designing the SHG response of layered materials. Efficient second-harmonic generation (SHG) occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here the authors show SHG tuning in bilayer MoS 2 - an inversion-symmetric crystal - mediated by interlayer excitons.

Transition metal dichalcogenides (TMDs) constitute a versatile platform for atomically thin optoelectronics devices and spin–valley memory applications. In monolayer TMDs the optical absorption is strong, but the transition energy cannot be tuned as the neutral exciton has essentially no out-of-plane static electric dipole1,2. In contrast, interlayer exciton transitions in heterobilayers are widely tunable in applied electric fields, but their coupling to light is substantially reduced. In this work, we show tuning over 120 meV of interlayer excitons with a high oscillator strength in bilayer MoS2 due to the quantum-confined Stark effect3. We optically probed the interaction between intra- and interlayer excitons as they were energetically tuned into resonance. Interlayer excitons interact strongly with intralayer B excitons, as demonstrated by a clear avoided crossing, whereas the interaction with intralayer A excitons is substantially weaker. Our observations are supported by density functional theory (DFT) calculations, which include excitonic effects. In MoS2 trilayers, our experiments uncovered two types of interlayer excitons with and without in-built electric dipoles. Highly tunable excitonic transitions with large in-built dipoles and oscillator strengths will result in strong exciton–exciton interactions and therefore hold great promise for non-linear optics with polaritons.Interlayer excitons in bilayer MoS2 exhibit both a high oscillator strength and highly tunable energies in an applied electric field.

The spin diffusion length is a key parameter to describe the transport properties of spin polarized electrons in solids. Electrical spin injection in semiconductor structures, a major issue in spintronics, critically depends on this spin diffusion length. Gate control of the spin diffusion length could be of great importance for the operation of devices based on the electric field manipulation and transport of electron spin. Here we demonstrate that the spin diffusion length in a GaAs quantum well can be electrically controlled. Through the measurement of the spin diffusion coefficient by spin grating spectroscopy and of the spin relaxation time by time-resolved optical orientation experiments, we show that the diffusion length can be increased by more than 200% with an applied gate voltage of 5 V. These experiments allow at the same time the direct simultaneous measurements of both the Rashba and Dresselhaus spin-orbit splittings. An important parameter in spintronics is the spin-diffusion length: the length over which the travelling electron spin keeps its orientation. Here, the authors show control over this length in quantum wells using a gate voltage, which also allows for an elegant measurement of the spin-orbit terms.

We study the electron spin relaxation in both symmetric and asymmetric GaAs AlGaAs quantum wells (QWs) grown on (110) substrates in an external magnetic field B applied along the QW normal. The spin polarization is induced by circularly polarized light and is detected using the time-resolved Kerr rotation technique. In the asymmetric structure, where a -doped layer on one side of the QW produces the Rashba contribution to the conduction-band spin-orbit splitting, the lifetime of electron spins aligned along the growth axis exhibits an anomalous dependence on B in the range 0 < B < 0.5 T; this results from the interplay between the Dresselhaus and Rashba effective fields which are perpendicular to each other. For larger magnetic fields, the spin lifetime increases, which is a consequence of the cyclotron motion of the electrons and is also observed in (001)-grown quantum wells. The experimental results are in agreement with the calculation of the spin lifetimes in (110)-grown asymmetric quantum wells described by the point group Cs, where the growth direction is not the principal axis of the spin-relaxation-rate tensor.

The impact of Ga 3+ centers in the spin-filtering effect observed in GaAsN samples is investigated through a model based on the master equation approach. Our results, compared with experimental data, show that, Ga 3+ are essential to understanding the behavior of the photoluminescence intensity and degree of circular polarization as functions of a Faraday configuration magnetic field. The model presented here takes into account the interplay of Ga 2+ and Ga 3+ centers, Zeeman and hyperfine interaction. The various processes that drive the spin-filtering effect, as the spin selective capture of conduction band electrons into Ga centers are also considered here.

Second-harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS , that shows strong optical oscillator strength for the intra- but also interlayer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations. Since interlayer exciton transitions are highly tunable also by choosing twist angle and material combination our results open up new approaches for designing the SHG response of layered materials.

. We propose an experimental procedure to track the evolution of electronic and nuclear spins in Ga 2+ centers in GaAsN dilute semiconductors. The method is based on a pump-probe scheme that enables to monitor the time evolution of the three components of the electronic and nuclear spin variables. In contrast to other characterization methods, as nuclear magnetic resonance, this one only needs moderate magnetic fields ( B ≈ 10 mT), and does not require microwave irradiation. Specifically, we carry out a series of tests for different experimental conditions in order to optimize the procedure for maximum sensitivity in the measurement of the circular degree of polarization. Based on previous experimental results and the theoretical calculations presented here, we estimate that the method could yield a time resolution of about 10ps.

(In,Ga)As/GaP(001) quantum dots (QDs) are grown by molecular beam epitaxy and studied both theoretically and experimentally. The electronic band structure is simulated using a combination of k·p and tight-binding models. These calculations predict an indirect to direct crossover with the In content and the size of the QDs. The optical properties are then studied in a low-In-content range through photoluminescence and time-resolved photoluminescence experiments. It suggests the proximity of two optical transitions of indirect and direct types.

We investigate the ultrafast dynamics of excitons in a 2.6 nm-thick \\(ZnO/Zn_0.84Mg_0.16O\\) quantum well grown on a c-axis sapphire substrate, using non-degenerate time-resolved pump-probe spectroscopy. A pump pulse at 266 nm generates photocarriers within the ZnMgO barriers, and their dynamics is monitored through time-resolved differential reflectance measurements using a supercontinuum probe spanning the 345-400 nm spectral range. Photocarriers generated in the barriers rapidly relax into the quantum well, where they form excitons within sub-picosecond timescales. These excitons quickly thermalize and become localized, likely due to interface disorder or well-width fluctuations, as supported by photoluminescence measurements showing a clear Stokes shift and the absence of free exciton emission. A phonon-assisted absorption process, leading to the effective thermalization of excitons, is observed and analyzed. We identify moreover a negative differential reflectance feature as a photoinduced absorption into a biexciton state, with a binding energy ranging from 18 to 22 meV depending on temperature.

Nanoscale quantum light sources are essential building blocks for integrated quantum photonic systems. Here, we report a wavelength-scale entangled-photon source based on van der Waals-engineered NbOBr\\(_2\\), and benchmark its performance for telecom-wavelength quantum light generation. By exploiting the material's second-order nonlinearity, we generate quantum-correlated photon pairs via spontaneous parametric down-conversion. We then use a 90\\(^\\) twisted stacking to induce quantum interference in photon-pair generation, yielding polarization-entangled photons. This approach enables tunability of the quantum optical state via control of the excitation laser polarization. We experimentally obtain entanglement fidelities exceeding 95% for Bell states, along with a high coincidence-to-accidental ratio of \\(\\)335, and a brightness approximately one order of magnitude higher than recently reported telecom sources based on transition metal dichalcogenide (TMD) 2D materials. These results establish twisted van der Waals engineering as a powerful platform for highly tunable, high-brightness quantum light sources at telecom wavelengths.