Floquet engineering is a promising tool to manipulate quantum systems coherently. A well-known example is the optical Stark effect, which has been used for optical trapping of atoms and breaking time-reversal symmetry in solids. However, as a coherent nonlinear optical effect, Floquet engineering typically requires high field intensities obtained in ultrafast pulses, severely limiting its use.
View Article and Find Full Text PDFPhosphorescent organic light-emitting diodes (PHOLEDs) feature high efficiency, brightness and colour tunability suitable for both display and lighting applications. However, overcoming the short operational lifetime of blue PHOLEDs remains one of the most challenging high-value problems in the field of organic electronics. Their short lifetimes originate from the annihilation of high-energy, long-lived blue triplets that leads to molecular dissociation.
View Article and Find Full Text PDFA series of bimetallic carbene-metal-amide (cMa) complexes have been prepared with bridging biscarbene ligands to serve as a model for the design of luminescent materials with large oscillator strengths and small energy differences between the singlet and triplet states (Δ). The complexes have a general structure (RN)Au(:carbene─carbene:)Au(NR). The bimetallic complexes show solvation-dependent absorption and emission that is analyzed in detail.
View Article and Find Full Text PDFAtomically thin transition metal dichalcogenides (TMDs), a subclass of two-dimensional (2D) layered materials, have numerous fascinating properties that make them a promising platform for photonic and optoelectronic devices. In particular, excited state transport by TMDs is important in energy harvesting and photonic switching; however, long-range transport in TMDs is challenging due to the lack of availability of large area films. Whereas most previous studies have focused on small, exfoliated monolayer flakes, in this work we demonstrate metal-organic chemical vapor deposition grown centimeter-scale monolayers of WS that support polariton propagation lengths of up to 60 μm.
View Article and Find Full Text PDFWe derive the thermodynamic limit for organic light-emitting diodes (OLEDs), and show that strong exciton binding in these devices requires a higher voltage to achieve the same luminance as a comparable inorganic LED. The OLED overpotential, which does not reduce the power conversion efficiency, is minimized by having a small exciton binding energy, a long exciton lifetime, and a large Langevin coefficient for electron-hole recombination. Based on these results, it seems likely that the best phosphorescent and thermally activated delayed fluorescence OLEDs reported to date approach their thermodynamic limit.
View Article and Find Full Text PDFFor organic photovoltaic (OPV) devices to achieve consistent performance and long operational lifetimes, organic semiconductors must be processed with precise control over their purity, composition, and structure. This is particularly important for high volume solar cell manufacturing where control of materials quality has a direct impact on yield and cost. Ternary-blend OPVs containing two acceptor-donor-acceptor (A-D-A)-type nonfullerene acceptors (NFAs) and a donor have proven to be an effective strategy to improve solar spectral coverage and reduce energy losses beyond that of binary-blend OPVs.
View Article and Find Full Text PDFTension control is critical for maintaining good product quality in most roll-to-roll (R2R) production systems. Previous work has primarily focused on improving the disturbance rejection performance of tension controllers. Here, a robust linear parameter-varying model predictive control (LPV-MPC) scheme is designed to enhance the tension tracking performance of a pilot R2R system for deposition of materials used in flexible thin film applications.
View Article and Find Full Text PDFRecent advances in thermophotovoltaic (TPV) power generation have produced notable gains in efficiency, particularly at very high emitter temperatures. However, there remains substantial room for improving TPV conversion of waste, solar, and nuclear heat streams at temperatures below 1,100°C. Here, we demonstrate the concept of transmissive spectral control that enables efficient recuperation of below-bandgap photons by allowing them to transmit through the cell to be absorbed by a secondary emitter.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2022
The thermal stability of inverted, halogen-rich non-fullerene acceptor (NFA)-based organic photovoltaics with MoO as the hole transporting layer is studied at temperatures up to 80 °C. Over time, the power conversion efficiency shows a "check-mark" shaped thermal aging pattern, featuring an early decrease, followed by a long-term recovery. A high Cl concentration at the bulk heterojunction (BHJ)/MoO interface in the thermally aged device is found using energy dispersive X-ray spectroscopy.
View Article and Find Full Text PDFOrganic photovoltaic cells (OPVs) have the potential of becoming a productive renewable energy technology if the requirements of low cost, high efficiency and prolonged lifetime are simultaneously fulfilled. So far, the remaining unfulfilled promise of this technology is its inadequate operational lifetime. Here, we demonstrate that the instability of NFA solar cells arises primarily from chemical changes at organic/inorganic interfaces bounding the bulk heterojunction active region.
View Article and Find Full Text PDFWe report a method to neutralize the mid-gap defect states in MoS monolayers using laser soaking of an organic/transition metal oxide (TMO) blend thin film. The treated MoS monolayer shows negligible emission from defect states as compared to the as-exfoliated MoS, accompanied by a photoluminescence quantum yield improvement from 0.018 to 4.
View Article and Find Full Text PDFThe orientation of facial (fac) tris-cyclometalated iridium complexes in doped films prepared by vacuum deposition is investigated by altering the physical shape and electronic asymmetry in the molecular structure. Angle-dependent photoluminescence spectroscopy and Fourier-plane imaging microscopy show that the orientation of roughly spherical fac-tris(2-phenylpyridyl)iridium (Ir(ppy) ) is isotropic, whereas complexes that are oblate spheroids, fac-tris(mesityl-2-phenyl-1H-imidazole)iridium (Ir(mi) ) and fac-tris((3,5-dimethyl-[1,1'-biphenyl]-4-yl)-2-phenyl-1H-imidazole)iridium (Ir(mip) ), have a net horizontal alignment of their transition dipole moments. Optical anisotropy factors of 0.
View Article and Find Full Text PDFThermophotovoltaic approaches that take advantage of near-field evanescent modes are being actively explored due to their potential for high-power density and high-efficiency energy conversion. However, progress towards functional near-field thermophotovoltaic devices has been limited by challenges in creating thermally robust planar emitters and photovoltaic cells designed for near-field thermal radiation. Here, we demonstrate record power densities of ~5 kW/m at an efficiency of 6.
View Article and Find Full Text PDFOrganic photovoltaics (OPVs) based on nonfullerene acceptors are now approaching commercially viable efficiencies. One key to their success is efficient charge separation with low potential loss at the donor-acceptor heterojunction. Due to the lack of spectroscopic probes, open questions remain about the mechanisms of charge separation.
View Article and Find Full Text PDFControlling matter-light interactions with cavities is of fundamental importance in modern science and technology. This is exemplified in the strong-coupling regime, where matter-light hybrid modes form, with properties that are controllable by optical-wavelength photons. By contrast, matter excitations on the nanometre scale are harder to access.
View Article and Find Full Text PDFOver the past 3 decades, there has been a vast expansion of research in both tissue engineering and organic electronics. Although the two fields have interacted little, the materials and fabrication technologies which have accompanied the rise of organic electronics offer the potential for innovation and translation if appropriately adapted to pattern biological materials for tissue engineering. In this work, we use two organic electronic materials as adhesion points on a biocompatible poly(-xylylene) surface.
View Article and Find Full Text PDFMoiré lattices formed in twisted van der Waals bilayers provide a unique, tunable platform to realize coupled electron or exciton lattices unavailable before. While twist angle between the bilayer has been shown to be a critical parameter in engineering the moiré potential and enabling novel phenomena in electronic moiré systems, a systematic experimental study as a function of twist angle is still missing. Here we show that not only are moiré excitons robust in bilayers of even large twist angles, but also properties of the moiré excitons are dependant on, and controllable by, the moiré reciprocal lattice period via twist-angle tuning.
View Article and Find Full Text PDFWe determine precise nanoscale information about the morphologies of several organic thin film structures using Fourier plane imaging microscopy (FIM). We used FIM microscopy to detect the orientation of molecular transition dipole moments from an extremely low density of luminescent dye molecules, which we call "morphology sensors". The orientation of the sensor molecules is driven by the local film structure and thus can be used to determine details of the host morphology without influencing it.
View Article and Find Full Text PDFFast deposition of thin films is essential for achieving low-cost, high-throughput phosphorescent organic light-emitting diode (PHOLED) production. In this work, we demonstrate rapid and uniform growth of semiconductor thin films by organic vapor phase deposition (OVPD). A green PHOLED comprising an emission layer (EML) grown at 50 Å/s with bis[2-(2-pyridinyl-)phenyl-](acetylacetonato)iridium(III) (Ir(ppy)(acac)) doped into 4,4'-bis(-carbazolyl)-1,1'-biphenyl (CBP) exhibits a maximum external quantum efficiency of 20 ± 1%.
View Article and Find Full Text PDFThermophotovoltaic cells are similar to solar cells, but instead of converting solar radiation to electricity, they are designed to utilize locally radiated heat. Development of high-efficiency thermophotovoltaic cells has the potential to enable widespread applications in grid-scale thermal energy storage, direct solar energy conversion, distributed co-generation and waste heat scavenging. To reach high efficiencies, thermophotovoltaic cells must utilize the broad spectrum of a radiative thermal source.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
September 2020
Semitransparent organic photovoltaic cells (ST-OPVs) are emerging as a solution for solar energy harvesting on building facades, rooftops, and windows. However, the trade-off between power-conversion efficiency (PCE) and the average photopic transmission (APT) in color-neutral devices limits their utility as attractive, power-generating windows. A color-neutral ST-OPV is demonstrated by using a transparent indium tin oxide (ITO) anode along with a narrow energy gap nonfullerene acceptor near-infrared (NIR) absorbing cell and outcoupling (OC) coatings on the exit surface.
View Article and Find Full Text PDFFour new donor-acceptor-acceptor' (D-A-A')-configured donors, CPNT, DCPNT, CPNBT, and DCPNBT equipped with naphtho[1,2-c:5,6-c']bis([1,2,5]-thiadiazole) (NT) or naphtho[2,3-c][1,2,5]thiadiazole (NBT) as the central acceptor (A) unit bridging triarylamine donor (D) and cyano or dicyanovinylene acceptor (A'), were synthesized and characterized. All molecules exhibit bathochromic absorption shifts as compared to those of the benzothiadiazole (BT)-based analogues owing to improved electron-withdrawing and quinoidal character of NT and NBT cores that lead to stronger intramolecular charge transfer. Favorable energy level alignments with C , together with the good thermal stability and the antiparallel dimeric packing render CPNT and DCPNT suitable donors for vacuum-processed organic photovoltaics (OPV)s.
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