Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2.

Atomically thin two-dimensional crystals have revolutionized materials science. In particular, monolayer transition metal dichalcogenides promise novel optoelectronic applications, owing to their direct energy gaps in the optical range. Their electronic and optical properties are dominated by Coulomb-bound electron-hole pairs called excitons, whose unusual internal structure, symmetry, many-body effects and dynamics have been vividly discussed. Here we report the first direct experimental access to all 1s A excitons, regardless of momentum--inside and outside the radiative cone--in single-layer WSe2. Phase-locked mid-infrared pulses reveal the internal orbital 1s-2p resonance, which is highly sensitive to the shape of the excitonic envelope functions and provides accurate transition energies, oscillator strengths, densities and linewidths. Remarkably, the observed decay dynamics indicates an ultrafast radiative annihilation of small-momentum excitons within 150 fs, whereas Auger recombination prevails for optically dark states. The results provide a comprehensive view of excitons and introduce a new degree of freedom for quantum control, optoelectronics and valleytronics of dichalcogenide monolayers.

Optimum photoluminescence excitation and recharging cycle of single nitrogen-vacancy centers in ultrapure diamond.

Important features in the spectral and temporal photoluminescence excitation of single nitrogen-vacancy (NV) centers in diamond are reported at conditions relevant for quantum applications. Bidirectional switching occurs between the neutral (NV(0)) and negatively charged (NV(-)) states. Luminescence of NV(-) is most efficiently triggered at a wavelength of 575 nm which ensures optimum excitation and recharging of NV(0). The dark state of NV(-) is identified as NV(0). A narrow resonance is observed in the excitation spectra at 521 nm, which mediates efficient conversion to NV(0).

The structure and optical properties of ZnO nanocrystals embedded in SiO2 fabricated by radio-frequency sputtering.

Zinc oxide (ZnO) nanocrystals (NCs) with high crystalline quality were prepared via radio-frequency magnetron sputtering as a SiO(2)/ZnO/SiO(2) trilayer on Si(100) and Al(2)O(3)(0001) substrates with an intermediate in situ annealing step. Transmission electron microscopy reveals a uniform dispersion of ZnO NCs in the amorphous SiO(2) matrix with typical sizes up to 16 nm with a larger fraction of smaller crystals. The size distribution analysis yields a mean grain size of 5 nm for small particles. Individual ZnO NCs show a well-defined hexagonal close packed wurtzite structure and lattice parameters close to those of bulk ZnO, confirming their high crystalline quality. Mapping of the Zn distribution by means of energy-filtered transmission electron microscopy reveals a strongly non-uniform distribution of Zn within the SiO(2) matrix, corroborating the chemical separation of ZnO NCs from surrounding SiO(2). Optical transmittance measurements confirm the findings of the electron microscopy analysis. The fabrication technique described opens up new possibilities in the preparation of ZnO NCs with high crystalline quality, including growth in monolithic optical cavities without intermediate ex situ fabrication steps.

Efficient nonlinear light emission of single gold optical antennas driven by few-cycle near-infrared pulses.

Individual nanometer-sized plasmonic antennas are excited resonantly with few-cycle laser pulses in the near infrared. Intense third-harmonic emission of visible light prevails for fundamental photon energies below 1.1 eV. Interband luminescence and second harmonic generation occur solely at higher driving frequencies. We attribute these findings to multiphoton resonances with the d-band transitions of gold. The strong third-order signal allows direct measurement of a subcycle plasmon dephasing time of 2 fs, highlighting the efficient radiation coupling and broadband response of the devices.

Few-cycle THz generation for imaging and tomography applications.

The methods for generating few-cycle THz radiation from semiconductors without external applied fields are reviewed. Their spectral characteristics, efficiency and prospects for imaging and tomography at terahertz frequencies are discussed.

Ultrafast coherent electron transport in semiconductor quantum cascade structures.

Coherent electron transport is studied in an electrically driven quantum cascade structure. Ultrafast quantum transport from the injector into the upper laser state is investigated by midinfrared pump-probe experiments directly monitoring the femtosecond saturation and subsequent recovery of electrically induced optical gain. We demonstrate for the first time pronounced gain oscillations giving evidence for a coherent electron motion. The coexistence of a long dephasing time of quantum coherence and high Coulomb scattering rates in the injector points to the occurrence of scattering-induced coherence in electron transport.

Monitoring the ultrafast electric field change at a mid-infrared plasma Bragg mirror.

The electric field change of a femtosecond mid-infrared (MIR) pulse reflected by a new type of Bragg mirror is directly measured by time-resolved cross-correlation spectroscopy. The refractive-index contrast of the plasma Bragg mirror is achieved by use of different doping levels of only one type of semiconductor material (n(+) -doped GaAs and undoped GaAs). The direct measurement of the time dependence of the electric field of a reflected MIR pulse permits the observation of a noninstantaneous response of a Bragg mirror compared with a metallic surface, which is due to the penetration of the pulse into the multilayer structure.

Sampling a terahertz dipole transition with subcycle time resolution.

We present a time-resolved technique to measure optical excitation processes with a time resolution shorter than the oscillation period of the exciting light. Our terahertz (THz) experiments fully resolve the polarization dynamics of electrons in semiconductor heterostructures when they are excited by a THz pulse. The time resolution of the polarization enables us to deduce the population dynamics of the excited state, which includes the dynamics of a virtual population in the case of off-resonant excitation.