Nanoscale Mapping of Bromide Segregation on the Cross Sections of 2 Complex Hybrid Perovskite Photovoltaic Films Using Secondary 3 Electron Hyperspectral Imaging in a Scanning Electron Microscope

Mixed halide (I/Br) complex organic/inorganic hybrid perovskite materials have attracted much attention recently because of their excellent photovoltaic properties. Although it has been proposed that their stability is linked to the chemical inhomogeneity of I/Br, no direct proof has been offered to date. Here, we report a new method, secondary electron hyperspectral imaging (SEHI), which allows direct imaging of the local variation in Br concentration in mixed halide (I/Br) organic/inorganic hybrid perovskites on a nanometric scale. We confirm the presence of a nonuniform Br distribution with variation in concentration within the grain interiors and boundaries and demonstrate how SEHI in conjunction with low-voltage scanning electron microscopy can enhance the understanding of the fundamental physics and materials science of organic/inorganic hybrid photovoltaics, illustrating its potential for research and development in “real-world” applications

Rapid scalable processing of tin oxide transport layers for perovskite solar cells

The development of scalable deposition methods for perovskite solar cell materials is critical to enable the commercialization of this nascent technology. Herein, we investigate the use and processing of nanoparticle SnO2 films as electron transport layers in perovskite solar cells and develop deposition methods for ultrasonic spray coating and slot-die coating, leading to photovoltaic device efficiencies over 19%. The effects of postprocessing treatments (thermal annealing, UV ozone, and O2 plasma) are then probed using structural and spectroscopic techniques to characterize the nature of the np-SnO2/perovskite interface. We show that a brief “hot air flow” method can be used to replace extended thermal annealing, confirming that this approach is compatible with high-throughput processing. Our results highlight the importance of interface management to minimize nonradiative losses and provide a deeper understanding of the processing requirements for large-area deposition of nanoparticle metal oxides

Ultrafast optical control of polariton energy in an organic semiconductor microcavity

The manipulation of exciton–polaritons and their condensates is of great interest due to their applications in polariton simulators and high-speed, all-optical logic devices. Until now, methods of trapping and manipulating such condensates are not dynamically reconfigurable or resulted in an undesirable reduction in the exciton–photon coupling strength. Here, a new strategy for the ultrafast control of polariton resonances via transient modification of an optical cavity mode is presented. Multilayer organic semiconductor microcavities that contain two absorbers are constructed: one strongly-coupled to the cavity photon mode and one that is out-of-resonance. By selectively exciting the out-of-resonance absorber using ultrashort laser pulses, the cavity refractive index is modulated, and fully-reversible blueshifts of the lower polariton branch by up to 8 meV in sub-ps timescales with no corresponding reduction in the exciton–photon coupling strength are generated. This work demonstrates the ability to manipulate polariton energy landscapes over ultrafast timescales with important applications in emerging computing technologies

Minority-carrier effects in poly-phenylenevinylene as studied by electrical characterization

Electrical measurements have been performed on poly[2-methoxy, 5 ethyl (2' hexyloxy) paraphenylenevinylene] in a pn junction with silicon. These included current-voltage measurements, capacitance-voltage measurements, capacitance-transient spectroscopy, and admittance spectroscopy. The measurements show evidence for large minority-carrier injection into the polymer possibly enabled by interface states for which evidence is also found. The shallow acceptor level depth (0.12 eV) and four deep trap level activation energies (0.30 and 1.0 eV majority-carrier type; 0.48 and 1.3 eV minority-carrier type) are found. Another trap that is visible at room temperature has point-defect nature. (C) 2001 American Institute of Physics

Direct evidence of Rabi oscillations and antiresonance in a strongly coupled organic microcavity

We report the direct observation of 30-fs period Rabi oscillations between excitons and cavity photons in a strongly coupled J-aggregate microcavity by means of time-resolved up-conversion and spectral interferometry measurements. The time structure of the transmitted electric field, measured by linear spectral interferometry, shows pronounced ultrafast beats. Its spectral phase reveals a distinct signature caused by destructive interference between the coherent drive and the field radiated by the exciton. This antiresonance selectively probes the uncoupled exciton excitation, and its observation uncovers the coherent and ultrafast exchange of energy between the optically excited cavity and the J-aggregate excitons, as confirmed by transfer matrix calculations.</p

The nanoscale structure and stability of organic photovoltaic blends processed with solvent additives

Controlling the nanomorphology in bulk heterojunction photoactive blends is crucial for optimizing the performance and stability of organic photovoltaic (OPV) technologies. A promising approach is to alter the drying dynamics and consequently, the nanostructure of the blend film using solvent additives such as 1,8-diiodooctane (DIO). Although this approach is demonstrated extensively for OPV systems incorporating fullerene-based acceptors, it is unclear how solvent additive processing influences the morphology and stability of nonfullerene acceptor (NFA) systems. Here, small angle neutron scattering (SANS) is used to probe the nanomorphology of two model OPV systems processed with DIO: a fullerene-based system (PBDB-T:PC71BM) and an NFA-based system (PBDB-T:ITIC). To overcome the low intrinsic neutron scattering length density contrast in polymer:NFA blend films, the synthesis of a deuterated NFA analog (ITIC-d52) is reported. Using SANS, new insights into the nanoscale evolution of fullerene and NFA-based systems are provided by characterizing films immediately after fabrication, after thermal annealing, and after aging for 1 year. It is found that DIO processing influences fullerene and NFA-based systems differently with NFA-based systems characterized by more phase-separated domains. After long-term aging, SANS reveals both systems demonstrate some level of thermodynamic induced domain coarsening

Interspecies exciton interactions lead to enhanced nonlinearity of dipolar excitons and polaritons in MoS2 homobilayers

This is the final version. Available from Nature Research via the DOI in this record. Data availability: The data that support the findings of this study are available in the MARVEL public repository (MARVEL Materials Cloud Archive: https:// archive.materialscloud.org) with the same title as this paper.Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS2 to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons (dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS2 monolayers, both hIX and dipolaritons exhibit ≈ 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This provides access to an unusual nonlinear regime which we describe theoretically as a mixed effect of Pauli exclusion and exciton-exciton interactions enabled through charge tunnelling. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations.Engineering and Physical Sciences Research Council (EPSRC)European Graphene Flagship ProjectEngineering and Physical Sciences Research Council (EPSRC)Engineering and Physical Sciences Research Council (EPSRC)Engineering and Physical Sciences Research Council (EPSRC)Engineering and Physical Sciences Research Council (EPSRC)European Union Marie Sklodowska-Curie ActionsEngineering and Physical Sciences Research Council (EPSRC)JSPS KAKENHIJSPS KAKENHIJSPS KAKENHIWorld Premier International Research Centre Initiative (WPI)Royal Society, ERC Consolidator grant QTWISTEngineering and Physical Sciences Research Council (EPSRC)Engineering and Physical Sciences Research CouncilEngineering and Physical Sciences Research CouncilEuropean Quantum Technology Flagship Project 2DSIPCNATO SPS projectEngineering and Physical Sciences Research Council (EPSRC)European Union’s Horizon 202