Revealing Grain Boundaries and Defect Formation in Nanocrystal Superlattices by Nanodiffraction
Nastasia Mukharamova, Dmitry Lapkin, Ivan A. Zaluzhnyy, Alexander André, Sergey Lazarev, Young Y. Kim, Michael Sprung, Ruslan P. Kurta, Frank Schreiber, Ivan A.… 展开作者
Nastasia Mukharamova, Dmitry Lapkin, Ivan A. Zaluzhnyy, Alexander André, Sergey Lazarev, Young Y. Kim, Michael Sprung, Ruslan P. Kurta, Frank Schreiber, Ivan A. Vartanyants, Marcus Scheele
X-ray nanodiffraction is applied to study the formation and correlation of domain boundaries in mesocrystalline superlattices of PbS nanocrystals with face-centered cubic structure. Each domain of the superlattice can be described with one of two mesocrystalline polymorphs with different orientational order. Close to a grain boundary, the lattice constant decreases and the superlattice undergoes an out-of-plane rotation, while the orientation of the nanocrystals with respect to the superlattice remains unchanged. These findings are explained with the release of stress on the expense of specific nanocrystal-substrate interactions. The fact that correlations between adjacent nanocrystals are found to survive the structural changes at most grain boundaries implies that the key to nanocrystal superlattices with macroscopic domain sizes are strengthened interactions with the substrate.
Rock-salt lead selenide nanocrystals can be used as building blocks for large scale square superlattices via two-dimensional assembly of nanocrystals at a liquid-air interface followed by oriented attachment. Here we report measurements of the local density of states of an atomically coherent superlattice with square geometry made from PbSe nanocrystals. Controlled annealing of the sample permits the imaging of a clean structure and to reproducibly probe the band gap and the valence hole and conduction electron states. The measured band gap and peak positions are compared to the results of opt…
We correlate spatially resolved fluorescence (-lifetime) measurements with X-ray nanodiffraction to reveal surface defects in supercrystals of self-assembled caesium lead halide perovskite nanocrystals and study their effect on the fluorescence properties. Upon comparison with density functional modelling, we show that a loss in structural coherence, an increasing atomic misalignment between adjacent nanocrystals, and growing compressive strain near the surface of the supercrystal are responsible for the observed fluorescence blueshift and decreased fluorescence lifetimes. Such surface defect-…
The annealing-induced formation of (Mn,Ga)As nanocrystals in (Ga,Mn)As/GaAs superlattices was studied by X-ray diffraction, transmission electron microscopy and magnetometry. The superlattice structures with 50 A thick (Ga,Mn)As layers separated by 25, 50 and 100 A thick GaAs spacers were grown by molecular beam epitaxy at low temperature (250 C), and then annealed at high temperatures of: 400, 560 and 630 C. The high temperature annealing causes decomposition to GaMnAs ternary alloy and formation of (Mn,Ga)As nanocrystals inside the GaAs matrix. The nanocrystals are confined in the planes tha…
Diffraction from a lattice of periodically spaced crystals is a topic of current interest because of the great development of self-organised superlattices (SL) of nanocrystals (NC). The self-organisation of NC into SL has theoretical interest, but especially a rich application prospect, as the coherent organisation has large effects on a wide range of material properties. Diffraction is a key method to understand the type and quality of SL ordering. Hereby the characteristic diffraction signature of a SL of NC - together with the characteristic types of disorder - are theoretically explored.
Semiconductive nanocrystals (NCs) can be self-assembled into ordered superlattices (SLs) to create artificial solids with emerging collective properties. Computational studies have predicted that properties such as electronic coupling or charge transport are determined not only by the individual NCs but also by the degree of their organization and structure. However, experimental proof for a correlation between structure and charge transport in NC SLs is still pending. Here, we perform X-ray nano-diffraction and apply Angular X-ray Cross-Correlation Analysis (AXCCA) to characterize the structu…
Probing Plasmonic Oscillations in 2D Moiré Nanocrystal Superlattices by Low-Loss EELS
University of Pennsylvania（宾夕法尼亚大学）；University of Washington（华盛顿大学）；SuperSTEM, SciTech Daresbury Science and Innovation Campus（超级扫描透射电子显微镜，科学技术达尔斯伯里科学与创新园区）；University of Leeds（利兹大学）
Sinusoidal Displacement Describes Disorder in CsPbBr3 Nanocrystal Superlattices
Istituto Italiano di Tecnologia（意大利理工大学）；Università Cattolica del Sacro Cuore（天主教大学）；Lund University（隆德大学）；Massachusetts Institute of Technology（麻省理工学院）；Istituto di Cristallografia (CNR-IC)（晶体学研究所（国家研究委员会））；MAX IV Laboratory（MAX IV 实验室）
We show that the combination of X-ray scattering with a nanofocused beam and X-ray cross correlation analysis is an efficient means for the full structural characterization of mesocrystalline nanoparticle assemblies with a single experiment. We analyze several hundred diffraction patterns of individual sample locations, i.e. individual grains, to obtain a meaningful statistical distribution of the superlattice and atomic lattice ordering. Simultaneous small- and wide-angle X-ray scattering of the same sample location allows us to determine the structure and orientation of the superlattice as w…
The nucleation and growth kinetics of highly ordered nanocrystal superlattices during the evaporation of nanocrystal colloidal droplets was elucidated by in situ time resolved small-angle x-ray scattering. We demonstrated for the first time that evaporation kinetics can affect the dimensionality of the superlattices. The formation of two-dimensional nanocrystal superlattices at the liquid-air interface of the droplet has an exponential growth kinetics that originates from interface "crushing".
Semiconducting, core-shell nanocrystals (NCs) are promising building blocks for the construction of higher dimensional artificial nanostructures using oriented attachment. However, the assembly and epitaxial attachment steps critical to this construction introduce disorder and defects which inhibit the observation of desirable emergent electronic phenomena. Consequently, understanding defect formation and remediation in these systems as a function of dimensionality is a crucial step to perfecting their synthesis. In this work, we use in situ high resolution transmission electron microscopy to …
