The surface quality of lead halide perovskite crystals can extremely influence their optoelectronic properties and device performance. Here, we report a surface engineering crystallization technique in which we in situ grow a polycrystalline methylammonium lead tribromide (MAPbBr3) film on top of bulk mm-sized single crystals. Such MAPbBr3 crystals with a MAPbBr3 passivating film display intense green emission under UV light. X-ray photoelectron spectroscopy demonstrates that these crystals with emissive surfaces are compositionally different from typical MAPbBr3 crystals that show no emission under UV light. Time-resolved photoluminescence and electrical measurements indicate that the MAPbBr3 film/MAPbBr3 crystals possess less surface defects compared to the bare MAPbBr3 crystals. Therefore, X-ray detectors fabricated using the surface-engineered MAPbBr3 crystals provide an almost 5 times improved sensitivity to X-rays and a more stable baseline drift with respect to the typical MAPbBr3 crystals.
The high built-in polarization field is a fingerprint of III-nitride heterostructures. Alloy composition and doping profile significantly affect the magnitude of the electric field present in subsequent layers, but the sign of the electric field is usually defined by substrate polarity and external bias. Here, we propose to utilize acceptor and donor doping concentrations exceeding 1020 cm−3 to obtain a high junction field that can solely abolish built-in polarization for a polar (0001) InGaN/GaN quantum well (QW). We have used photoluminescence (PL), time-resolved PL (TRPL), and contactless electroreflectance in order to gain insight into the strength of the electric field present in the grown heterostructures. Good match between expected and measured electric field values was obtained. A dramatic decrease in the luminescence lifetime for a flat QW was confirmed using TRPL. The presented results open a way to realize devices that profit from the low built-in field, like photodetectors, using abundant polar substrates.
We present experimental studies on low-temperature ([Formula: see text]) carrier dynamics in (Ga,In)(Sb,Bi)/GaSb quantum wells (QWs) with the nominal In content of 3.7% and the Bi ranging from 6 to 8%. The photoreflectance experiment revealed the QW bandgap evolution with [Formula: see text] % Bi, which resulted in the bandgap tunability roughly between 629 and [Formula: see text], setting up the photon emission wavelength between 1.97 and [Formula: see text]. The photoluminescence experiment showed a relatively small 3-10[Formula: see text] Stokes shift regarding the fundamental QW absorption edge, indicating the exciton localisation beneath the QW mobility edge. The localised state's distribution, being the origin of the PL, determined carrier dynamics in the QWs probed directly by the time-resolved photoluminescence and transient reflectivity. The intraband carrier relaxation time to the QW ground state, following the non-resonant excitation, occurred within 3-25[Formula: see text] and was nearly independent of the Bi content. However, the interband relaxation showed a strong time dispersion across the PL emission band and ranging nearly between 150 and [Formula: see text], indicating the carrier transfer among the localised state's distribution. Furthermore, the estimated linear dispersion variation parameter significantly decreased from [Formula: see text] to [Formula: see text] with increasing the Bi content, manifested the increasing role of the non-radiative recombination processes with Bi in the QWs.
Dielectric engineering of heterostructures made from two-dimensional van der Waals semiconductors is a unique and powerful tool to tailor the electric and optical band gaps solely via the dielectric environment and the crystal thickness modulation. Here, we utilize high quality MoTe2 monolayer and bilayer crystals as a candidate for near-infrared photonic applications. The crystals are exfoliated on various technologically relevant carrier substrates: silicon/silicon dioxide, poly(methyl methacrylate), hexagonal boron nitride, silicon carbide, and silicon nitride. These substrates provide a large range of high frequency dielectric constants from 2.1 to 7.0 for MoTe2-containing heterostructures. We assess the relationship between the environmental dielectric function and Coulomb screening by combining detailed spectroscopic measurements, utilizing low-temperature and high-spatially resolved photoluminescence and contrast reflectivity, with microscopic many-body modeling, to explore the potential of this less-recognized material platform for applications in optoelectronics at photon wavelengths above 1 μm. We observe a redshift of the optical gap emission energy from the monolayer to bilayer regime on the order of 30 meV. Furthermore, the thickness controlled shift is slightly larger than the one induced by the local dielectric environment, which ranges on the order of 20 meV for the MoTe2 monolayers and on the order of 8 meV for the MoTe2 bilayers. We also show that the local dielectric screening barely affects the trion binding energy, which is captured by our microscopic model, accounting for the screened Coulomb potential for the heterostructures.
The Si-based mid-infrared photonics is an emerging technology in which group-IV germanium-tin (Ge1-xSnx) binary alloys can play a fundamental role in the development of a Si-compatible photonic components including monolithically integrated coherent light sources and detectors, on the same Si or SOI substrate. Although the Ge(1-x)Sn(x-)on-Si lasers, at low temperatures, have already been demonstrated, the knowledge of the material properties necessary for such device optimization and real-life usage is very limited. In particular, carrier relaxation kinetics, relaxation pathways, and accompanied physical mechanisms, important for the laser's dynamics, have not been subjected to in-depth research and understanding. In this work, we present detailed spectroscopic studies on photoinjected carrier dynamics in Ge1-xSnx epilayers, as a function of Sn content (6-12%) and temperature (20-300 K), by utilizing time-resolved differential reflectivity and photo-luminescence. The latter technique allowed us to track separated electron and hole dynamics with a femtosecond time resolution, while the former experiment exploited a joined electron-hole recombination. This experimental approach allowed us to identify (i) two initial electron relaxation processes after photoexcitation; (ii) radiative electron-hole recombination on below-band gap states; (iii) nonradiative carrier recombination involving the Shockley-Read-Hall mechanism; and (iv) nonradiative recombination through the surface states. The research results significantly expand the knowledge on the initial carrier relaxation dynamics in the Ge1-xSnx epitaxial material. It provides unknown up-to-date kinetic parameters of the initial stage of electron relaxation and further carrier recombination dynamics, unveils the critical role of band gap inhomogeneity for the relaxation dynamics, and highlights the role of below-band gap states that can participate in the light generation process in Ge1-xSnx epilayers.
Optical properties and carrier dynamics in 6.6, 10.4, and 14.4 nm wide Ga(Sb, Bi)/GaSb quantum wells (QWs) with similar to 10%-11% of Bi were studied by photoluminescence (PL), time-resolved PL, and transient reflectivity. Experiments revealed that low temperature emission is strongly governed by the decay of excitonic population that undergoes weak localization on the QW potential fluctuations rather than the strong defect-like localization typically found for highly mismatched alloys. This statement is supported first by the nearly linear increase of the PL intensity with the excitation power, second, by the lack of the S-shape signature in the temperature-dependent PL studies, and third, the absence of a strong lifetime dispersion for excitons. The low-temperature intraband carrier relaxation time is established in the range of 14-19 ps, nearly independent on the well width, while the exciton lifetime exhibits a well width dependence, i.e. this time decreases from similar to 265 ps, through similar to 206 ps, to similar to 147 ps with the increase of the QW width from 6.6 to 14.4 nm. Our results demonstrate that in contrast to other dilute bismide alloys, GaSbBi behaves as a regular alloy rather than as a highly-mismatched material.
Carrier relaxation in self-assembled InAs/In0.53Ga0.23Al0.24As/InP(001) quantum dots emitting at 1.55 μm and quantum dots coupled to the In0.64Ga0.36As/In0.53Ga0.23Al0.24As quantum well through a thin In0.53Ga0.23Al0.24As barrier is investigated employing high-temporal-resolution (< 0.3 ps), time-resolved spectroscopic techniques at cryogenic temperatures, supported additionally with photoluminescence, photoluminescence excitation, and theoretical modelling. We focused on intra-band carrier relaxation pathways that solely determine the observed non-equilibrium carrier population kinetics. We ascertained relatively fast carrier capture and intra-band relaxation process in a reference structure with quantum dots only (∼8 ps time constant) and even faster initial relaxation in the coupled system (∼4 ps). An evident bottleneck effect is observed for the final relaxation stage in the coupled quantum dots-quantum well system slowing down the overall relaxation process by a factor of 5. The effect is attributed to a peculiar picture of the confined conduction band states in the coupled system exhibiting significant changes in the spatial distribution between the relevant lowest-lying electronic states.
We investigate a hybrid system containing an In0.53Ga0.47As quantum well (QW), separated by a thin 2 nm In0.53Ga0.23Al0.24As barrier from 1.55 µm emitting InAs quantum dots (QDs), grown by molecular beam epitaxy on an InP substrate. Photoreflectance and photoluminescence (PL) spectroscopies are used to identify optical transitions in the system, with support of 8-band kp modelling. The main part of the work constitute the measurements and analysis of thermal quenching of PL for a set of samples with different QW widths (3–6 nm). Basing on Arrhenius plots, carrier escape channels from the dots are identified, pointing at the importance of carrier escape into the QW. A simple two level rate equations model is proposed and solved, exhibiting qualitative agreement with experimental observations. We show that for a narrow QW the escape process is less efficient than carrier supply via the QW due to the narrow barrier, resulting in improved emission intensity at room temperature. It proves that with carefully designed energy level structure, a hybrid QW/QD system can be used as an active region in telecom lasers with improved efficiencies.