Gallium-doped Zinc Oxide: Nonlinear Reflection and Transmission Measurements and Modeling in the ENZ Region

Strong nonlinear materials have been sought after for decades for applications in telecommunications, sensing, and quantum optics. Gallium-doped zinc oxide is a II-VI transparent conducting oxide that shows promising nonlinearities similar to indium tin oxide and aluminum-doped zinc oxide for the telecommunications band. Here we explore its nonlinearities in the epsilon near zero (ENZ) region and show n2,eff values on the order of 4.5x10-3 cm2GW-1 for IR pumping on 200-300 nm thin films. Measuring nonlinear changes in transmission and reflection with a white light source probe in the near-IR while exciting in the near-IR provides data in both time and wavelength. Three films varying in thickness, optical loss, and ENZ crossover wavelength are numerically modeled and compared to experimental data showing agreement for both dispersion and temporal relaxation. In addition, we discuss optimal excitation and probing wavelengths occur around ENZ for thick films but are red-shifted for thin films where our model provides an additional degree of freedom to explore. Obtaining accurate nonlinear measurements is a difficult and time-consuming task where our method in this paper provides experimental and modeled data to the community for an ENZ material of interest.Comment: 18 pages, 10 figure

Double-crowned 2D semiconductor nanoplatelets with bicolor power-tunable emission

Nanocrystals (NCs) are now established building blocks for optoelectronics and their use as down converters for large gamut displays has been their first mass market. NC integration relies on a combination of green and red NCs into a blend, which rises post-growth formulation issues. A careful engineering of the NCs may enable dual emissions from a single NC population which violates Kasha’s rule, which stipulates that emission should occur at the band edge. Thus, in addition to an attentive control of band alignment to obtain green and red signals, non-radiative decay paths also have to be carefully slowed down to enable emission away from the ground state. Here, we demonstrate that core/crown/crown 2D nanoplatelets (NPLs), made of CdSe/CdTe/CdSe, can combine a large volume and a type-II band alignment enabling simultaneously red and narrow green emissions. Moreover, we demonstrate that the ratio of the two emissions can be tuned by the incident power, which results in a saturation of the red emission due to non-radiative Auger recombination that affects this emission much stronger than the green one. Finally, we also show that dual-color, power tunable, emission can be obtained through an electrical excitation

High-Temperature Photoluminescence of CdSe/CdS Core/Shell Nanoheterostructures

The steady-state and time-resolved photoluminescence properties of CdSe/CdS heterostructures are studied as a function of temperature from 300 to 600 K. The emission properties of samples are found to behave similarly to bulk CdSe, with the samples maintaining high color purity and a slightly contracting band gap at elevated temperature. Photoluminescence from CdSe/CdS samples is maintained with high stability over prolonged illumination and multiple heating and cooling cycles. Structures synthesized with variation in the core and the shell dimensions show that the preservation of emission intensity at high temperature depends strongly on the microscopic structure of the samples. For samples synthesized by seeded growth, the size of the CdSe core is highly correlated with the fraction of preserved sample photoluminescence intensity at high temperature. Temperature-dependent lifetime data suggest that the core structure predicts the stability of photoluminescence at elevated temperatures by controlling the radiative rate. The rate of electron capture, for which the volume fraction of the core is a structural proxy, underpins the ability for radiative processes to compete with thermally induced nonradiative decay pathways. Heterostructures synthesized below 200 °C using highly reactive organometallic precursors show markedly lower thermal stability than samples prepared by seeded growth at 360 °C, suggesting that the temperature of nanocrystal synthesis has direct consequences for the thermal stability of photoluminescence

Optical anisotropy of CsPbBr3 perovskite nanoplatelets

Abstract The two-dimensional CsPbBr3 nanoplatelets have a quantum well electronic structure with a band gap tunable with sample thicknesses in discreet steps based upon the number of monolayers. The polarized optical properties of CsPbBr3 nanoplatelets are studied using fluorescence anisotropy and polarized transient absorption spectroscopies. Polarized spectroscopy shows that they have absorption and emission transitions which are strongly plane-polarized. In particular, photoluminescence excitation and transient absorption measurements reveal a band-edge polarization approaching 0.1, the limit of isotropic two-dimensional ensembles. The degree of anisotropy is found to depend on the thickness of the nanoplatelets: multiple measurements show a progressive decrease in optical anisotropy from 2 to 5 monolayer thick nanoplatelets. In turn, larger cuboidal CsPbBr3 nanocrystals, are found to have consistently positive anisotropy which may be attributed to symmetry breaking from ideal perovskite cubes. Optical measurements of anisotropy are described with respect to the theoretical framework developed to describe exciton fine structure in these materials. The observed planar absorption and emission are close to predicted values at thinner nanoplatelet sizes and follow the predicted trend in anisotropy with thickness, but with larger anisotropy than theoretical predictions. Dominant planar emission, albeit confined to the thinnest nanoplatelets, is a valuable attribute for enhanced efficiency of light-emitting devices