Coupling Perovskite Quantum Dot Pairs in Solution using a Nanoplasmonic Assembly.

Perovskite quantum dots (PQDs) provide a robust solution-based approach to efficient solar cells, bright light emitting devices, and quantum sources of light. Quantifying heterogeneity and understanding coupling between dots is critical for these applications. We use double-nanohole optical trapping to size individual dots and correlate to emission energy shifts from quantum confinement. We were able to assemble a second dot in the trap, which allows us to observe the coupling between dots. We observe a systematic red-shift of 1.1 ± 0.6 meV in the emission wavelength. Theoretical analysis shows that the observed shift is consistent with resonant energy transfer and is unusually large due to moderate-to-large quantum confinement in PQDs. This demonstrates the promise of PQDs for entanglement in quantum information applications. This work enables future in situ control of PQD growth as well as studies of the coupling between small PQD assemblies with quantum information applications in mind.

Practical implementation of high-resolution electron ptychography and comparison with off-axis electron holography.

Ptychography is a coherent diffractive imaging technique that can determine how an electron wave is transmitted through an object by probing it in many small overlapping regions and processing the diffraction data obtained at each point. The resulting electron transmission model describes both phase and amplitude changes to the electron wave. Ptychography has been adopted in transmission electron microscopy in recent years following advances in high-speed direct electron detectors and computer algorithms which now make the technique suitable for practical applications. Its ability to retrieve quantitative phase information at high spatial resolution makes it a plausible alternative or complement to electron holography. Furthermore, unlike off-axis electron holography, it can provide phase information without an electron bi-prism assembly or the requirement of a minimally structured region adjacent to the region of interest in the object. However, it does require a well-calibrated scanning transmission electron microscope and a well-managed workflow to manage the calibration, data acquisition and reconstruction process to yield a practical technique. Here we detail this workflow and highlight how this is greatly assisted by acquisition management software. Through experimental data and modelling we also explore the similarities and differences between high-resolution ptychography and electron holography. Both techniques show a dependence of the recovered phase on the crystalline orientation of the material which is attributable to dynamical scattering. However, the exact nature of the variation differs reflecting fundamental expectations, but nonetheless equally useful information is obtained from electron holography and the ptychographically determined object transmission function.

Direct imaging and electronic structure modulation of moiré superlattices at the 2D/3D interface.

The atomic structure at the interface between two-dimensional (2D) and three-dimensional (3D) materials influences properties such as contact resistance, photo-response, and high-frequency electrical performance. Moiré engineering is yet to be utilized for tailoring this 2D/3D interface, despite its success in enabling correlated physics at 2D/2D interfaces. Using epitaxially aligned MoS2/Au{111} as a model system, we demonstrate the use of advanced scanning transmission electron microscopy (STEM) combined with a geometric convolution technique in imaging the crystallographic 32 Å moiré pattern at the 2D/3D interface. This moiré period is often hidden in conventional electron microscopy, where the Au structure is seen in projection. We show, via ab initio electronic structure calculations, that charge density is modulated according to the moiré period, illustrating the potential for (opto-)electronic moiré engineering at the 2D/3D interface. Our work presents a general pathway to directly image periodic modulation at interfaces using this combination of emerging microscopy techniques.

Nanoparticle size and 3D shape measurement by electron tomography: An Inter-Laboratory Comparison.

Electron tomography (ET) has been used for quantitative measurement of shape and size of objects in three dimensions (3D) for many years. However, systematic investigation of repeatability and reproducibility of ET has not been evaluated in detail. To assess the reproducibility and repeatability of a protocol for measuring size and three-dimensional (3D) shape parameters for nanoparticles (NPs) by ET, an inter-laboratory comparison (ILC) has been performed. The ILC included six laboratories and six instruments models from three instrument manufacturers following a standard measurement protocol. A technical specification describing the normative steps of the protocol is published by the International Standards Organization (ISO). Gold NPs with 30 nm nominal diameter contained within a rod-shaped carbon support were measured. The use of a rod-shaped sample support eliminated the missing wedge effect in the experimental tilt series of projected images for improved quantification. A total of 443 NPs were initially measured by NRC-NANO and then 115 out of the 443 NPs were measured by five other labs to compare measurands such as the Volume (V), maximum Feret diameter (Fmax), minimum Feret diameter (Fmin), volume-equivalent diameter (Deq) and aspect ratio (Frat) of the NPs. The results of the five labs were compared with the results obtained at NRC-NANO. The maximum disagreement in measurements of Fmin and Fmax obtained by the participating labs did not exceed 7 %. The measured Deq was between 27.5 nm and 30.3 nm in agreement with the NP manufacturer's specification (28 nm-32 nm). In addition to the above, the influence of the missing wedge effect and beam-induced NP movement was quantified based on the differences of the results between labs.

Particle diameter, signal-to-noise ratio and beam requirements for extended Rayleigh resolution measurements in the scanning electron microscope.

The extended Rayleigh resolution measure was introduced to give a generalized resolution measure that can be readily applied to imaging and resolving particles that have finite size. Here, we make a detailed analysis of the influence of the particle size on this resolution measure. We apply this to scanning electron microscopy, under simple assumption of a Gaussian electron beam intensity distribution and a directly proportional emitted signal yield without detailed consideration of scattering internal to the sample, other than being proportional to the sample thickness. From this, we produce beam-width normalized characteristics relating the particle diameter and resolution measure, while also taking consideration of the reduced signal yield that occurs from smaller particles. From our analysis of these characteristics, which we fit to experimental image data, we see that particle diameters <0.7 times the beam 1/e full width, d, give agreement better than 10% with the true extended Rayleigh resolution. Furthermore, we consider the signal current that must be collected to reliably distinguish between the mid-gap and peak intensity regions in the particle images. This leads to a practical guide that the signal-to-noise ratio (SNR) occurring between large area, continuous regions made of the same materials as the particle and background should typically be 10-30 times greater than the SNR that is desired to be achieved between the peak and mid-gap regions of just resolved adjacent identical particles having diameters in the size range 0.4-0.7d.

Parameters affecting the accuracy of nanoparticle shape and size measurement in 3D.

While electron tomography can be used to visualize objects at nanoscale, it is difficult to perform reproducible quantitative measurements. Here we measure the shape and size of nanoparticles (NPs) in three dimensions (3D) using electron tomography. We evaluated the accuracy of maximum Feret diameter (Feretmax), minimum Feret diameter (Feretmini) and volume of NPs measurements from reconstructed 3D images which were obtained from data acquired with varied electron dose. We perform both simulations and experiment to clarify what factors effect on the accuracy of the NP shape measurement. Based on the results, suitable reconstruction methods and threshold for binarization were evaluated. We also report comparison results obtained on exactly the same samples in two different laboratories.

Catalytic chemical vapor deposition of single-wall carbon nanotubes at low temperatures.

We report surface-bound growth of single-wall carbon nanotubes (SWNTs) at temperatures as low as 350 degrees C by catalytic chemical vapor deposition from undiluted C2H2. NH3 or H2 exposure critically facilitates the nanostructuring and activation of sub-nanometer Fe and Al/Fe/Al multilayer catalyst films prior to growth, enabling the SWNT nucleation at lower temperatures. We suggest that carbon nanotube growth is governed by the catalyst surface without the necessity of catalyst liquefaction.