Energy and spectral enhancement of femtosecond supercontinuum in a noble gas using a weak seed

We experimentally demonstrate that the use of a weak seed pulse of energy less than 0.4% of the pump results in a spectral energy enhancement that spans over 2 octaves and a total energy enhancement of more than 3 times for supercontinua generated by millijoule level femtosecond pulses in Krypton gas. Strong four-wave mixing of the pump-seed pulse interacting in the gas is observed. The spectral irradiance generated from the seeding process is sufficiently high to use white-light continuum as an alternative to conventional tunable sources of radiation for applications such as nonlinear optical spectroscopy

Design and implementation of a device based on an off-axis parabolic mirror to perform luminescence experiments in a scanning tunneling microscope

We present the design, implementation, and illustrative results of a light collection/injection strategy based on an off-axis parabolic mirror collector for a low-temperature Scanning Tunneling Microscope (STM). This device allows us to perform STM induced Light Emission (STM-LE) and Cathodoluminescence (STM-CL) experiments and in situ Photoluminescence (PL) and Raman spectroscopy as complementary techniques. Considering the \'Etendue conservation and using an off-axis parabolic mirror, it is possible to design a light collection and injection system that displays 72% of collection efficiency (considering the hemisphere above the sample surface) while maintaining high spectral resolution and minimizing signal loss. The performance of the STM is tested by atomically resolved images and scanning tunneling spectroscopy results on standard sample surfaces. The capabilities of our system are demonstrated by performing STM-LE on metallic surfaces and two-dimensional semiconducting samples, observing both plasmonic and excitonic emissions. In addition, we carried out in situ PL measurements on semiconducting monolayers and quantum dots and in situ Raman on graphite and hexagonal boron nitride (h-BN) samples. Additionally, STM-CL and PL were obtained on monolayer h-BN gathering luminescence spectra that are typically associated with intragap states related to carbon defects. The results show that the flexible and efficient light injection and collection device based on an off-axis parabolic mirror is a powerful tool to study several types of nanostructures with multiple spectroscopic techniques in correlation with their morphology at the atomic scale and electronic structure.Comment: 19 pages, 14 Figure

Size dependence of carrier dynamics and carrier multiplication in PbS quantum dots

The time dynamics of the photoexcited carriers and carrier-multiplication efficiencies in PbS quantum dots (QDs) are investigated. In particular, we report on the carrier dynamics, including carrier multiplication, as a function of QD size and compare them to the bulk value. We show that the intraband 1P - \u3e 1S decay becomes faster for smaller QDs, in agreement with the absence of a phonon bottleneck. Furthermore, as the size of the QDs decreases, the energy threshold for carrier multiplication shifts from the bulk value to higher energies. However, the energy threshold shift is smaller than the band-gap shift and, therefore, for the smallest QDs, the threshold approaches 2.35 E(g), which is close to the theoretical energy conservation limit of twice the band gap. We also show that the carrier-multiplication energy efficiency increases with decreasing QD size. By comparing to theoretical models, our results suggest that impact ionization is sufficient to explain carrier multiplication in QDs

Three-Photon Absorption Spectra and Bandgap Scaling In Direct-Gap Semiconductors

This paper presents three-photon absorption (3PA) measurement results for nine direct-gap semiconductors, including full 3PA spectra for ZnSe, ZnS, and GaAs. These results, along with our theory of 3PA using an eight-band Kane model (four bands with double spin degeneracy), help to explain the significant disagreements between experiments and theory in the literature to date. 3PA in the eight-band model exhibits quantum interference between the various possible pathways that is not observed in previous two-band theories. We present measurements of degenerate 3PA coefficients in InSb, GaAs, CdTe, CdSe, ZnTe, CdS, ZnSe, ZnO, and ZnS. We examine bandgap, Eg, scaling using -band tunneling and perturbation theories that show agreement with the predicted Eg−7 dependence; however, for those semiconductors for which we measured full 3PA spectra, we observe significant discrepancies with both two-band theories. On the other hand, our eight-band model shows excellent agreement with the spectral data. We then use our eight-band theory to predict the 3PA spectra for 15 different semiconductors in their zinc-blende form. These results allow prediction and interpretation of the 3PA coefficients for various narrow to wide bandgap semiconductors

Engineered nonlinear materials using gold nanoantenna array

Gold dipole nanoantennas embedded in an organic molecular film provide strong local electromagnetic fields to enhance both the nonlinear refractive index (n(2)) and two-photon absorption (2PA) of the molecules. An enhancement of 53x for 2PA and 140x for nonlinear refraction is observed for BDPAS (4,4'-bis(diphenylamino) stilbene) at 600 nm with only 3.7% of gold volume fraction. The complex value of the third-order susceptibility enhancement results in a sign change of n(2) for the effective composite material relative to the pure BDPAS film. This complex nature of the enhancement and the tunability of the nanoantenna resonance allow for engineering the effective nonlinear response of the composite film8119Agências de fomento estrangeiras apoiaram essa pesquisa, mais informações acesse artig

Spectral and temperature dependence of two-photon and free-carrier absorption in InSb

The nonlinear absorption spectrum of InSb was measured using a combination of tunable similar to 160 fs, similar to 10 ps, and similar to 150 ns IR sources along with a cryostat for controlling the sample temperature to vary the band gap energy from 0.17 to 0.23 eV. The measured nonlinear optical properties in InSb are consistent with those predicted by the models which include two-and three-photon absorption (2PA and 3PA), multiphoton generated free-carrier absorption (FCA) and various recombination mechanisms. Temperature-dependent Z-scan and nonlinear transmission measurements yield information on the temperature and spectral dependence of 2PA, FCA, and carrier recombination processes of Shockley-Read-Hall, and Auger mechanisms. We find good agreement between the measured and the modeled nonlinear properties is possible only when the recently predicted temperature dependence of the FCA is considered. The wavelength-and temperature-dependent 2PA and 3PA coefficients in InSb were experimentally obtained. The inferred values of the 2PA and 3PA are consistent with the scaling rules of a simple two-parabolic band model. We further determine recombination rates from nonlinear transmittance of nanosecond pulses of CO2 laser