Colloidally stable suspensions of lead halide perovskite nanocrystals are prepared from high-quality lead halide nanocrystal seeds. Perovskite nanocrystals with different layered crystal structures are reported. These systems are well suited for investigations of the intrinsic photophysics and spectroscopy of organic-inorganic metal halide perovskites.

The conversion of photoexcitations into charge carriers in organic solar cells is facilitated by the dissociation of excitons at the donor/acceptor interface. The ultrafast timescale of charge separation demands sophisticated theoretical models and raises questions about the role of coherence in the charge-transfer mechanism. Here, we apply two-dimensional electronic spectroscopy to study the electron transfer process in poly(3-hexylthiophene)/PCBM (P3HT/PCBM) blends. We report dynamics maps showing the pathways of charge transfer that clearly expose the significance of hot electron transfer. During this ultrafast electron transfer, vibrational coherence is directly transferred from the P3HT exciton to the P3HT hole polaron in the crystalline domain. This result reveals that the exciton converts to a hole with a similar spatial extent on a timescale far exceeding other photophysical dynamics including vibrational relaxation.

Hierarchical, three-fold symmetrical, single-crystalline gold dendrites were synthesized by the reaction between a zinc plate and a solution of HAuCl 4 in the ionic liquid [BMIM][PF 6 ]. The unique dendritic gold nanostructures show a three-order hierarchy (i.e., a three-fold symmetrical <111>-oriented trunk, three groups of trident-like <111>-oriented branches grown on the trunk, and many <111>-oriented nanorod leaves grown on the branches symmetrically), indicating an interesting fractal growth. According to the investigation on the growth process of the gold dendrites, it was proposed that gold nuclei nanocrystals first formed on the zinc substrate through a direct surface reaction and that the subsequent crystal growth preferentially took place on the preformed gold crystals through a primary cell reaction, leading to the formation of the final hyperbranched dendrites under nonequilibrium conditions. In contrast, AuZn alloy dendrites consisting of aggregated primary nanoparticles were produced when the ionic liquid solution was replaced by an aqueous solution. It was proposed that the significantly lowered ion diffusivity and reaction rate in the ionic liquid medium could largely contribute to the formation of the pure singlecrystalline gold dendrites. Moreover, electrocatalytic measurements performed in alkaline solution suggested that the obtained dendritic gold nanostructures exhibited good electrocatalytic activity toward the oxidation of methanol, which might be related to the special three-order hierarchical architectures.

The origin and yield of charges in neat conjugated polymers has long been controversial. In this paper, we review the body of literature that has been created over the past three decades of research in this field and provide insight from our own recent work highlighting the importance of polymer microstructure in understanding the photophysics of these materials. We focus primarily on polythiophene, poly(p-phenylene vinylene), and ladder-type poly(p-phenylene) derivatives, as these three prototypical polymer backbone structures have undergone the most complete study. We find compelling evidence that the primary photoexcitations in conjugated polymers include both intrachain excitons and excimers, that charges are produced in a secondary process, primarily from breakup of intrachain excitons, and that the locus of long-lived charge generation is at the interface between amorphous and crystalline domains of the polymer. Interestingly, the existence of interchromophore complexes that we refer to as excimers has largely been ignored in the development of organic photovoltaics based on conjugated polymers. We suggest that the prevalence of this species may help explain certain mysterious features in that body of work, in particular the excess energy offset required for efficient charge separation in donor/acceptor blends and the requirement for intimately mixed phases of the two materials for maximally efficient photocurrent generation.

White organic light‐emitting diodes (WOLEDs) are currently under intensive research and development worldwide as a new generation light source to replace problematic incandescent bulbs and fluorescent tubes. One of the major challenges facing WOLEDs has been to achieve high energy efficiency and high color rendering index simultaneously to make the technology competitive against other alternative technologies such as inorganic LEDs. Here, an all‐phosphor, four‐color WOLEDs is presented, employing a novel device design principle utilizing molecular energy transfer or, specifically, triplet exciton conversion within common organic layers in a cascaded emissive zone configuration to achieve exceptional performance: an 24.5% external quantum efficiency (EQE) at 1000 cd/m2 with a color rendering index (CRI) of 81, and an EQE at 5000 cd/m2 of 20.4% with a CRI of 85, using standard phosphors. The EQEs achieved are the highest reported to date among WOLEDs of single or multiple emitters possessing such high CRI, which represents a significant step towards the realization of WOLEDs in solid‐state lighting.

Concurrence of the vibrational coherence and ultrafast electron transfer has been observed in polymer/fullerene blends. However, it is difficult to experimentally investigate the role that the excited-state vibrational coherence plays during the electron transfer process since vibrational coherence from the ground- and excited-electronic states is usually temporally and spectrally overlapped. Here, we performed 2-dimensional electronic spectroscopy (2D ES) measurements on poly(3-hexylthiophene) (P3HT) films. By Fourier transforming the whole 2D ES datasets (S(λ1,T̃2,λ3)) along the population time (T̃2) axis, we develop and propose a protocol capable of separating vibrational coherence from the ground- and excited-electronic states in 3D rephasing and nonrephasing beating maps (S(λ1,ν̃2,λ3)). We found that the vibrational coherence from pure excited electronic states appears at positive frequency (+ν̃2) in the rephasing beating map and at negative frequency (-ν̃2) in the nonrephasing beating map. Furthermore, we also found that vibrational coherence from excited electronic state had a long dephasing time of 244 fs. The long-lived excited-state vibrational coherence indicates that coherence may be involved in the electron transfer process. Our findings not only shed light on the mechanism of ultrafast electron transfer in organic photovoltaics but also are beneficial for the study of the coherence effect on photoexcited dynamics in other systems.

Using polarized 2D spectroscopy and state-of-the-art TDDFT calculations to uncover the vibronic structure of primary photosynthetic pigments and its effect on ultrafast photoexcited dynamics.

Broadband pump-probe spectroscopy is used to examine the ultrafast photophysics of the π-conjugated polymers poly(3-hexylselenophene) (P3HS) and poly(3-hexyltellurophene) (P3HTe) in solution. An excited-state absorption feature that we attribute to a transition in the triplet manifold appears on the picosecond time scale. Density functional theory (DFT) and time-dependent density functional theory (TD-DFT) calculations support this assignment. The formation of triplets is consistent with significant fluorescence quenching observed in solutions of the neat polymers. Triplet formation occurs in ~26 and ~1.8 ps (upper limit) for P3HS and P3HTe, respectively. The successive decrease in fluorescence quantum efficiency and triplet formation time are consistent with intersystem crossing facilitated by the heavier selenium and tellurium atoms. These results strongly suggest that primary photoexcitations are rapidly converted into triplet states in P3HS and P3HTe.