Curvature and self-assembly of semi-conducting nanoplatelets

Semi-conducting nanoplatelets are two-dimensional nanoparticles whose thickness is in the nanometer range and controlled at the atomic level. They have come up as a new category of nanomaterial with promising optical properties due to the efficient confinement of the exciton in the thickness direction. In this perspective, we first describe the various conformations of these 2D nanoparticles which display a variety of bent and curved geometries and present experimental evidences linking their curvature to the ligand-induced surface stress. We then focus on the assembly of nanoplatelets into superlattices to harness the particularly efficient energy transfer between them, and discuss different approaches that allow for directional control and positioning in large scale assemblies. We emphasize on the fundamental aspects of the assembly at the colloidal scale in which ligand-induced forces and kinetic effects play a dominant role. Finally, we highlight the collective properties that can be studied when a fine control over the assembly of nanoplatelets is achieved.

A Design Methodology for EV-WPT Systems to Resonate at Arbitrary Given Bands

Due to the effects of splitting frequency and cross coupling, the resonant frequency of the WPT system usually deviates from the given frequency band, and the system operating at the given frequency band suffers a very low output power. Ensuring that electric vehicle wireless power transfer (EV-WPT) systems operate at a resonant state is the prerequisite for efficient energy transfer. For this purpose, a novel design method by manipulating the eigenstate parameters is proposed in this paper. The proposed system can make a EV-WPT system with arbitrary coil successfully to resonate at any given bands, not just a single band. Therefore, the method designed in this article cannot only eliminate the problem of low power caused by frequency deviation, but also realize the application requirements of multiple frequency bands. Firstly, this article establishes an accurate state space model of an n-coil fully coupled EV-WPT system, and after that, the analytical current response on each circuit is derived. Based on that, a detailed frequency spectrum analysis is presented, along with several essential spectrum parameters’ derivations, including center frequencies and bandwidths. Then, with the center frequency and bandwidth as the design indexes, a novel methodology of designing to make EV-WPT systems achieve resonant-state at arbitrary given bands is derived. Finally, simulation and experimental verification are carried out. Simulation and experimental results show that whether it is a single-band or multi-band system, the accuracy of the value under designed resonant frequency is less than 0.01, which can effectively eliminate the frequency deviation phenomenon and obtain the maximum power output at the given frequency band.

Computational Discovery of TTF Molecules with Deep Generative Models

We present a computational workflow based on quantum chemical calculations and generative models based on deep neural networks for the discovery of novel materials. We apply the developed workflow to search for molecules suitable for the fusion of triplet-triplet excitations (triplet-triplet fusion, TTF) in blue OLED devices. By applying generative machine learning models, we have been able to pinpoint the most promising regions of the chemical space for further exploration. Another neural network based on graph convolutions was trained to predict excitation energies; with this network, we estimate the alignment of energy levels and filter molecules before running time-consuming quantum chemical calculations. We present a comprehensive computational evaluation of several generative models, choosing a modification of the Junction Tree VAE (JT-VAE) as the best one in this application. The proposed approach can be useful for computer-aided design of materials with energy level alignment favorable for efficient energy transfer, triplet harvesting, and exciton fusion processes, which are crucial for the development of the next generation OLED materials.

A Porphyrin Pentamer as a Bright Emitter for NIR OLEDs

The luminescence and electroluminescence of an ethyne-linked zinc(II) porphyrin pentamer have been investigated, by testing blends in two different conjugated polymer matrices, at a range of concentrations. The best results were obtained for blends with the conjugated polymer PIDT-2TPD, at a porphyrin loading of 1 wt%. This host matrix was selected because the excellent overlap between its emission spectrum and the absorption spectrum of the porphyrin oligomer leads to efficient energy transfer. Thin films of this blend exhibit intense fluorescence in the near-infrared (NIR), with a peak emission wavelength of 886 nm and a photoluminescent quantum yield (PLQY) of 27% in the solid state. Light-emitting diodes (LEDs) fabricated with this blend as the emissive layer achieve average external quantum efficiencies (EQE) of 2.0% with peak emission at 830 nm and a turn-on voltage of 1.6 V. This performance is remarkable for a singlet NIR-emitter; 93% of the photons are emitted in the NIR (λ > 700 nm), indicating that conjugated porphyrin oligomers are promising emitters for non-toxic NIR OLEDs.

Redox conditions correlated with vibronic coupling modulate quantum beats in photosynthetic pigment–protein complexes

Quantum coherences, observed as time-dependent beats in ultrafast spectroscopic experiments, arise when light–matter interactions prepare systems in superpositions of states with differing energy and fixed phase across the ensemble. Such coherences have been observed in photosynthetic systems following ultrafast laser excitation, but what these coherences imply about the underlying energy transfer dynamics remains subject to debate. Recent work showed that redox conditions tune vibronic coupling in the Fenna–Matthews–Olson (FMO) pigment–protein complex in green sulfur bacteria, raising the question of whether redox conditions may also affect the long-lived (>100 fs) quantum coherences observed in this complex. In this work, we perform ultrafast two-dimensional electronic spectroscopy measurements on the FMO complex under both oxidizing and reducing conditions. We observe that many excited-state coherences are exclusively present in reducing conditions and are absent or attenuated in oxidizing conditions. Reducing conditions mimic the natural conditions of the complex more closely. Further, the presence of these coherences correlates with the vibronic coupling that produces faster, more efficient energy transfer through the complex under reducing conditions. The growth of coherences across the waiting time and the number of beating frequencies across hundreds of wavenumbers in the power spectra suggest that the beats are excited-state coherences with a mostly vibrational character whose phase relationship is maintained through the energy transfer process. Our results suggest that excitonic energy transfer proceeds through a coherent mechanism in this complex and that the coherences may provide a tool to disentangle coherent relaxation from energy transfer driven by stochastic environmental fluctuations.