Colloidal quantum dots (QDs) are promising materials for use in solar cells, light-emitting diodes, lasers, and photodetectors, but the mechanism and length of exciton transport in QD materials is not well understood. We use time-resolved optical microscopy to spatially visualize exciton transport in CdSe/ZnCdS core/shell QD assemblies. We find that the exciton diffusion length, which exceeds 30 nm in some cases, can be tuned by adjusting the inorganic shell thickness and organic ligand length, offering a powerful strategy for controlling exciton movement. Moreover, we show experimentally and through kinetic Monte Carlo simulations that exciton diffusion in QD solids does not occur by a random-walk process; instead, energetic disorder within the inhomogeneously broadened ensemble causes the exciton diffusivity to decrease over time. These findings reveal new insights into exciton dynamics in disordered systems and demonstrate the flexibility of QD materials for photonic and optoelectronic applications.

To optimize the interaction between chiral matter and highly twisted light, quantities that can help characterize chiral electromagnetic fields near nanostructures are needed. Here, by analogy with Poynting's theorem, we formulate the time-averaged conservation law of optical chirality in lossy dispersive media and identify the optical chirality flux as an ideal far-field observable for characterizing chiral optical near fields. Bounded by the conservation law, we show that it provides precise information, unavailable from circular dichroism spectroscopy, on the magnitude and handedness of highly twisted fields near nanostructures.

Long linear carbon chains (LLCCs) encapsulated inside double-walled carbon nanotubes (DWCNTs) are regarded as a promising realization of carbyne, the truly one-dimensional allotrope of carbon. While the electronic and vibronic properties of the encapsulated LLCC are expected to be influenced by its nanotube host, this dependence has not been investigated experimentally so far. Here we bridge this gap by studying individual LLCCs encapsulated in DWCNTs with tip-enhanced Raman scattering (TERS). We reveal that the nanotube host, characterized by its chirality, determines the vibronic and electronic properties of the encapsulated LLCC. By choice of chirality, the fundamental Raman mode (C-mode) of the chain is tunable by ∼95 cm and its band gap by ∼0.6 eV, suggesting this one-dimensional hybrid system to be a promising building block for nanoscale optoelectronics. No length dependence of the chain's C-mode frequency is evident, making LLCCs a close to perfect representation of carbyne.

Conspectus Chirality in Nature can be found across all length scales, from the subatomic to the galactic. At the molecular scale, the spatial dissymmetry in the atomic arrangements of pairs of mirror-image molecules, known as enantiomers, gives rise to fascinating and often critical differences in chemical and physical properties. With increasing hierarchical complexity, protein function, cell communication, and organism health rely on enantioselective interactions between molecules with selective handedness. For example, neurodegenerative and neuropsychiatric disorders including Alzheimer’s and Parkinson’s diseases have been linked to distortion of chiral-molecular structure. Moreover, d-amino acids have become increasingly recognized as potential biomarkers, necessitating comprehensive analytical methods for diagnosis that are capable of distinguishing l- from d-forms and quantifying trace concentrations of d-amino acids. Correspondingly, many pharmaceuticals and agrochemicals consist of chiral molecules that target particular enantioselective pathways. Yet, despite the importance of molecular chirality, it remains challenging to sense and to separate chiral compounds. Chiral-optical spectroscopies are designed to analyze the purity of chiral samples, but they are often insensitive to the trace enantiomeric excess that might be present in a patient sample, such as blood, urine, or sputum, or pharmaceutical product. Similarly, existing separation schemes to enable enantiopure solutions of chiral products are inefficient or costly. Consequently, most pharmaceuticals or agrochemicals are sold as racemic mixtures, with reduced efficacy and potential deleterious impacts. Recent advances in nanophotonics lay the foundation toward highly sensitive and efficient chiral detection and separation methods. In this Account, we highlight our group’s effort to leverage nanoscale chiral light–matter interactions to detect, characterize, and separate enantiomers, potentially down to the single molecule level. Notably, certain resonant nanostructures can significantly enhance circular dichroism for improved chiral sensing and spectroscopy as well as high-yield enantioselective photochemistry. We first describe how achiral metallic and dielectric nanostructures can be utilized to increase the local optical chirality density by engineering the coupling between electric and magnetic optical resonances. While plasmonic nanoparticles locally enhance the optical chirality density, high-index dielectric nanoparticles can enable large-volume and uniform-sign enhancements in the optical chirality density. By overlapping these electric and magnetic resonances, local chiral fields can be enhanced by several orders of magnitude. We show how these design rules can enable high-yield enantioselective photochemistry and project a 2000-fold improvement in the yield of a photoionization reaction. Next, we discuss how optical forces can enable selective manipulation and separation of enantiomers. We describe the design of low-power enantioselectiv...

Chiral metallic nanostructures can generate evanescent fields which are more highly twisted than circularly polarized light. However, it remains unclear how best to exploit this phenomenon, hindering the optimal utilization of chiral electromagnetic fields. Here, inspired by optical antenna theory, we address this challenge by introducing chiral antenna parameters: the chirality flux efficiency and the chiral antenna aperture. These quantities, which are based on chirality conservation, quantify the generation and dissipation of chiral light. We then present a label-free experimental technique, chirality flux spectroscopy, which measures the chirality flux efficiency, providing valuable information on chiral near fields in the far field. This principle is verified theoretically and experimentally with two-dimensionally chiral coupled nanorod antennas, for which we show that chiral near and far fields are linearly dependent on the magnetoelectric polarizability. This elementary system confirms our concept to quantify chiral electromagnetic fields and paves the way toward broadly tunable chiral optical applications including ultrasensitive detection of molecular chirality or optical information storage and transfer.