ABSTRACT
Determining the correlation between the size of a single quantum dot (QD) and its photoluminescence (PL) properties is a challenging task. In the study, we determine the size of each QD by measuring its absorption cross section, which allows for accurate investigation of size-dependent PL blinking mechanisms and volume scaling of the biexciton Auger recombination at the single-particle level. A significant correlation between the blinking mechanism and QD size is observed under low excitation conditions. When the QD size is smaller than their Bohr diameter, single CsPbI3 perovskite QDs tend to exhibit BC-blinking, whereas they tend to exhibit Auger-blinking when the QD size exceeds their Bohr diameter. In addition, by extracting bright-state photons from the PL intensity trajectories, the effects of QD charging and surface defects on the biexcitons are effectively reduced. This allows for a more accurate measurement of the volume scaling of biexciton Auger recombination in weakly confined CsPbI3 perovskite QDs at the single-dot level, revealing a superlinear volume scaling (τXX,Auger â σ1.96).
ABSTRACT
Twisted stacking of two-dimensional materials with broken inversion symmetry, such as spiral MoTe2 nanopyramids and supertwisted spiral WS2, emerge extremely strong second- and third-harmonic generation. Unlike well-studied nonlinear optical effects in these newly synthesized layered materials, photoluminescence (PL) spectra and exciton information involving their optoelectronic applications remain unknown. Here, we report layer- and power-dependent PL spectra of the supertwisted spiral WS2. The anomalous layer-dependent PL evolutions that PL intensity almost linearly increases with the rise of layer thickness have been determined. Furthermore, from the power-dependent spectra, we find the power exponents of the supertwisted spiral WS2 are smaller than 1, while those of the conventional multilayer WS2 are bigger than 1. These two abnormal phenomena indicate the enlarged interlayer spacing and the decoupling interlayer interaction in the supertwisted spiral WS2. These observations provide insight into PL features in the supertwisted spiral materials and may pave the way for further optoelectronic devices based on the twisted stacking materials.
ABSTRACT
The tunable optical display is vital for many application fields in telecommunications, sensors, and military devices. However, most optical materials have a strong wavelength dependence, which limits their spectral operation range. In this work, we develop an electrically reconfigurable optical medium based on graphene, demonstrating a cycle-controlled display covering the electromagnetic spectrum from the visible to the infrared wavelength. Through an electro-intercalation method, the graphene-based surface enables rich colors from gray to dark blue to dark red to yellow, and the response time is about 1 min from the start gray color to the final yellow color. Simultaneously, it exhibits a remarkable change in infrared emissivity (from 0.63 to 0.80 reduction to 0.20) with a response time of 1 s. This modification of optical properties of lithiated multilayer graphene (MLG) is the increase of Fermi energy (Ef) due to the charge transfer from lithium (Li) to graphene layers, which causes changes in interband and intraband electronic transitions. Our findings imply potential value in fabricating multispectral optical materials with high tunability.
ABSTRACT
The fabrication of conformal nanostructures on microarchitectures is of great significance for diverse applications. Here a facile and universal method was developed for conformal self-assembly of nanospheres on various substrates including convex bumps and concave holes. Hydrophobic microarchitectures could be transferred into superhydrophilic ones using plasma treatment due to the formation of numerous hydroxyl groups. Because of superhydrophilicity, the nanosphere suspension spread on the microarchitectures quickly and conformal self-assembly of nanospheres can be realized. Besides, the feature size of the conformal nanospheres on the substrates could be further regulated by plasma treatment. After transferring two-dimensional tungsten disulfide sheets onto the conformal nanospheres, the periodic nanosphere array was demonstrated to be able to enhance the light harvesting of WS2. Based on this, a light-enhanced room-temperature gas sensor with a fast recovery speed (<35 s) and low detecting limit (500 ppb) was achieved. Moreover, the WS2-covered nanospheres on the microarchitectures were very sensitive to the changes in air pressure due to the formation of suspended sheets on the convex bumps and concave holes. A sensitive photoelectronic pressure sensor that was capable of detecting the airtightness of vacuum devices was developed using the WS2-decorated hierarchical architectures. This work provides a simple method for the fabrication of conformal nanospheres on arbitrary substrates, which is promising for three-dimensional microfabrication of multifunctional hierarchical microarchitectures for diverse applications, such as biomimetic compound eyes, smart wetting surfaces and photonic crystals.
ABSTRACT
Intercalation is a unique degree of freedom for tuning the physical and chemical properties of two-dimensional (2D) materials, providing an ideal system to study various electronic states (such as superconductivity, ferromagnetism, and charge density waves). Here, we demonstrate the inversion symmetry breaking in lithium (Li)-intercalated ultrathin graphite (about 20-100 graphene layers) by optical second-harmonic generation (SHG). This inversion symmetry breaking is attributed to nanoscale inhomogeneities (i.e., lattice distortion and dislocations) in lithiated graphite. In addition, the efficiency of the SHG signal in an ultrathin graphite flake is widely tunable by the electrochemical lithiation process, and the efficiency of fully lithiated graphite (LiC6) is comparable to that of other noncentrosymmetric 2D crystals. Our results reveal a novel intercalation-induced inversion symmetry breaking effect and open up possibilities for building 2D intercalated-compounds-based nonlinear optical devices.
