Identifying the origin of delayed electroluminescence in a polariton organic light-emitting diode.

Modifying the energy landscape of existing molecular emitters is an attractive challenge with favourable outcomes in chemistry and organic optoelectronic research. It has recently been explored through strong light-matter coupling studies where the organic emitters were placed in an optical cavity. Nonetheless, a debate revolves around whether the observed change in the material properties represents novel coupled system dynamics or the unmasking of pre-existing material properties induced by light-matter interactions. Here, for the first time, we examined the effect of strong coupling in polariton organic light-emitting diodes via time-resolved electroluminescence studies. We accompanied our experimental analysis with theoretical fits using a model of coupled rate equations accounting for all major mechanisms that can result in delayed electroluminescence in organic emitters. We found that in our devices the delayed electroluminescence was dominated by emission from trapped charges and this mechanism remained unmodified in the presence of strong coupling.

Developing Solution-Processed Distributed Bragg Reflectors for Microcavity Polariton Applications.

Improving the performance of organic optoelectronics has been under vigorous research for decades. Recently, polaritonics has been introduced as a technology that has the potential to improve the optical, electrical, and chemical properties of materials and devices. However, polaritons have been mainly studied in optical microcavities that are made by vacuum deposition processes, which are costly, unavailable to many, and incompatible with printed optoelectronics methods. Efforts toward the fabrication of polariton microcavities with solution-processed techniques have been utterly absent. Herein, we demonstrate for the first time strong light-matter coupling and polariton photoluminescence in an organic microcavity consisting of an aluminum mirror and a distributed Bragg reflector (DBR) made by sequential dip coating of titanium hydroxide/poly(vinyl alcohol) (TiOH/PVA) and Nafion films. To fabricate and develop the solution-processed DBRs and microcavities, we automatized a dip-coating device that allowed us to produce sub-100 nm films consistently over many dip-coating cycles. Owning to the solution-based nature of our DBRs, our results pave the way to the realization of polariton optoelectronic devices beyond physical deposition methods.

Stereoselective Construction of Fluorinated Quaternary Stereogenic Centers via an Organocatalytic Asymmetric exo-Selective Diels-Alder Reaction in the Presence of Water.

A catalytic, asymmetric Diels-Alder reaction of α-fluoro α,ß-unsaturated aldehydes and cyclopentadiene was developed using diarylprolinol silyl ether as an organocatalyst. The reaction proceeds in toluene with trifluoroacetic acid as an additive (condition A). Perchloric acid salt of diarylprolinol silyl ether also promotes the reaction using water as a reaction medium (condition B). In both cases, excellent exo-selectivity and enantioselectivity were obtained with generation of a fluorinated quaternary chiral center.

Spatial and Temporal Coherence in Strongly Coupled Plasmonic Bose-Einstein Condensates.

We report first-order spatial and temporal correlations in strongly coupled plasmonic Bose-Einstein condensates. The condensate is large, more than 20 times the spatial coherence length of the polaritons in the uncondensed system and 100 times the healing length, making plasmonic lattices an attractive platform for studying long-range spatial correlations in two dimensions. We find that both spatial and temporal coherence display nonexponential decay; the results suggest power-law or stretched exponential behavior with different exponents for spatial and temporal correlation decays.

Sub-picosecond thermalization dynamics in condensation of strongly coupled lattice plasmons.

Bosonic condensates offer exciting prospects for studies of non-equilibrium quantum dynamics. Understanding the dynamics is particularly challenging in the sub-picosecond timescales typical for room temperature luminous driven-dissipative condensates. Here we combine a lattice of plasmonic nanoparticles with dye molecule solution at the strong coupling regime, and pump the molecules optically. The emitted light reveals three distinct regimes: one-dimensional lasing, incomplete stimulated thermalization, and two-dimensional multimode condensation. The condensate is achieved by matching the thermalization rate with the lattice size and occurs only for pump pulse durations below a critical value. Our results give access to control and monitoring of thermalization processes and condensate formation at sub-picosecond timescale.

Converting an Organic Light-Emitting Diode from Blue to White with Bragg Modes.

Organic light-emitting diodes (OLEDs) have been established as versatile light sources that allow for easy integration in large-area surfaces and flexible substrates. In addition, the low fabrication cost of OLEDs renders them particularly attractive as general lighting sources. Current methods for the fabrication of white-light OLEDs rely on the combination of multiple organic emitters and/or the incorporation of multiple cavity modes in a thick active medium. These architectures introduce formidable challenges in both device design and performance improvements, namely, the decrease of efficiency with increasing brightness (efficiency roll-off) and short operational lifetime. Here we demonstrate, for the first time, white-light generation in an OLED consisting of a sub-100 nm thick blue single-emissive layer coupled to the photonic Bragg modes of a dielectric distributed Bragg reflector (DBR). We show that the Bragg modes, although primarily located inside the DBR stack, can significantly overlap with the emissive layer, thus efficiently enhancing emission and outcoupling of photons at selected wavelengths across the entire visible light spectrum. Moreover, we show that color temperature can be tuned by the DBR parameters, offering great versatility in the optimization of white-light emission spectra.

Singlet-Oxygen-Mediated Synthesis of Pandanusine A and Pandalizine C and Structural Revision of Pandanusine B.

The first synthesis of racemic pandanusines A and B and pandalizine C, isolated from Pandanus amaryllifolius, is reported. The key synthetic step is an efficient tandem reaction sequence initiated by the photooxidation of an easily prepared furylalkylamine precursor. In this reaction sequence, methylene blue plays a dual catalytic role of photosensitizer and redox catalyst, first in generating singlet oxygen and second in facilitating a triplet oxygen reaction. Through the synthesis of pandanusine B, the proposed structure has been revised.

Ultrafast Pulse Generation in an Organic Nanoparticle-Array Laser.

Nanoscale coherent light sources offer potentially ultrafast modulation speeds, which could be utilized for novel sensors and optical switches. Plasmonic periodic structures combined with organic gain materials have emerged as promising candidates for such nanolasers. Their plasmonic component provides high intensity and ultrafast nanoscale-confined electric fields, while organic gain materials offer fabrication flexibility and a low acquisition cost. Despite reports on lasing in plasmonic arrays, lasing dynamics in these structures have not been experimentally studied yet. Here we demonstrate, for the first time, an organic dye nanoparticle-array laser with more than a 100 GHz modulation bandwidth. We show that the lasing modulation speed can be tuned by the array parameters. Accelerated dynamics is observed for plasmonic lasing modes at the blue side of the dye emission.

Asymmetric and Site-Selective [3 + 2]-Annulations for the Synthesis of High-Value Bicyclic Lactams.

Asymmetric and site-selective formal [3 + 2]-annulations of γ-alkyl-ß,γ-unsaturated γ-lactams with α,ß-unsaturated aldehydes have been developed. These organocatalysed transformations yield high value enantioenriched bicyclic γ-lactams with up to four new stereocenters (sometimes including a quarternary carbon). The overall transformation starts from simple and readily accessible furans and oversees a rapid, controlled, and dramatic enhancement in 3D complexity.