Liuyang Sun

Direct measurement of exciton valley coherence in monolayer WSe2

Coherent valley exciton dynamics are directly probed in a monolayer transition metal dichalcogenide, providing access to the valley coherence time and decoherence mechanisms — crucial for developing methods for manipulating the valley pseudospin.

Chirality detection of enantiomers using twisted optical metamaterials

Many naturally occurring biomolecules, such as amino acids, sugars and nucleotides, are inherently chiral. Enantiomers, a pair of chiral isomers with opposite handedness, often exhibit similar physical and chemical properties due to their identical functional groups and composition, yet show different toxicity to cells. Detecting enantiomers in small quantities has an essential role in drug development to eliminate their unwanted side effects. Here we exploit strong chiral interactions with plasmonic metamaterials with specifically designed optical response to sense chiral molecules down to zeptomole levels, several orders of magnitude smaller than what is typically detectable with conventional circular dichroism spectroscopy. In particular, the measured spectra reveal opposite signs in the spectral regime directly associated with different chiral responses, providing a way to univocally assess molecular chirality. Our work introduces an ultrathin, planarized nanophotonic interface to sense chiral molecules with inherently weak circular dichroism at visible and near-infrared frequencies.

Impact of grain boundaries on efficiency and stability of organic-inorganic trihalide perovskites

Organic–inorganic perovskite solar cells have attracted tremendous attention because of their remarkably high power conversion efficiencies. To further improve device performance, it is imperative to obtain fundamental understandings on the photo-response and long-term stability down to the microscopic level. Here, we report the quantitative nanoscale photoconductivity imaging on two methylammonium lead triiodide thin films with different efficiencies by light-stimulated microwave impedance microscopy. The microwave signals are largely uniform across grains and grain boundaries, suggesting that microstructures do not lead to strong spatial variations of the intrinsic photo-response. In contrast, the measured photoconductivity and lifetime are strongly affected by bulk properties such as the sample crystallinity. As visualized by the spatial evolution of local photoconductivity, the degradation process begins with the disintegration of grains rather than nucleation and propagation from visible boundaries between grains. Our findings provide insights to improve the electro-optical properties of perovskite thin films towards large-scale commercialization.Probing the nanoscale photoconductivity of methylammonium lead triiodide is important for understanding the microstructures of the solar cell devices, but scanning probe methods suffer from sample degradation. Here Chu et al. solve the problem with noncontact microwave impedance microscopy.

Self-Assembled Epitaxial Au–Oxide Vertically Aligned Nanocomposites for Nanoscale Metamaterials

Metamaterials made of nanoscale inclusions or artificial unit cells exhibit exotic optical properties that do not exist in natural materials. Promising applications, such as super-resolution imaging, cloaking, hyperbolic propagation, and ultrafast phase velocities have been demonstrated based on mostly micrometer-scale metamaterials and few nanoscale metamaterials. To date, most metamaterials are created using costly and tedious fabrication techniques with limited paths toward reliable large-scale fabrication. In this work, we demonstrate the one-step direct growth of self-assembled epitaxial metal-oxide nanocomposites as a drastically different approach to fabricating large-area nanostructured metamaterials. Using pulsed laser deposition, we fabricated nanocomposite films with vertically aligned gold (Au) nanopillars (∼20 nm in diameter) embedded in various oxide matrices with high epitaxial quality. Strong, broad absorption features in the measured absorbance spectrum are clear signatures of plasmon resonances of Au nanopillars. By tuning their densities on selected substrates, anisotropic optical properties are demonstrated via angular dependent and polarization resolved reflectivity measurements and reproduced by full-wave simulations and effective medium theory. Our model predicts exotic properties, such as zero permittivity responses and topological transitions. Our studies suggest that these self-assembled metal-oxide nanostructures provide an exciting new material platform to control and enhance optical response at nanometer scales.

Single quantum dot controls a plasmonic cavity’s scattering and anisotropy

Significance We experimentally demonstrate that a single semiconductor quantum dot placed in close proximity to a plasmonic cavity (i.e., a spherical metallic nanoparticle) can be used to control the scattering spectrum and anisotropy of the latter. The scattering spectrum of the hybrid structure features a Fano resonance mediated by single photon absorption/scattering. This result is highly counterintuitive because the scattering cross sections of these two nanoparticles differ by four orders of magnitude. Our work represents a critical step toward realizing quantum plasmonic nanostructures that are capable of producing scattered light, which, depending on its polarization state, obeys either quantum or classical statistics. Furthermore, our work enables a hybrid orientation sensor unaffected by photobleaching of quantum dots. Plasmonic cavities represent a promising platform for controlling light–matter interaction due to their exceptionally small mode volume and high density of photonic states. Using plasmonic cavities for enhancing light’s coupling to individual two-level systems, such as single semiconductor quantum dots (QD), is particularly desirable for exploring cavity quantum electrodynamic (QED) effects and using them in quantum information applications. The lack of experimental progress in this area is in part due to the difficulty of precisely placing a QD within nanometers of the plasmonic cavity. Here, we study the simplest plasmonic cavity in the form of a spherical metallic nanoparticle (MNP). By controllably positioning a semiconductor QD in the close proximity of the MNP cavity via atomic force microscope (AFM) manipulation, the scattering spectrum of the MNP is dramatically modified due to Fano interference between the classical plasmonic resonance of the MNP and the quantized exciton resonance in the QD. Moreover, our experiment demonstrates that a single two-level system can render a spherical MNP strongly anisotropic. These findings represent an important step toward realizing quantum plasmonic devices.

Interplay Between Optical Bianisotropy and Magnetism in Plasmonic Metamolecules

The smallness of natural molecules and atoms with respect to the wavelength of light imposes severe limits on the nature of their optical response. For example, the well-known argument of Landau and Lifshitz and its recent extensions that include chiral molecules show that the electric dipole response dominates over the magneto-electric (bianisotropic) and an even smaller magnetic dipole optical response for all natural materials. Here, we experimentally demonstrate that both these responses can be greatly enhanced in plasmonic nanoclusters. Using atomic force microscopy nanomanipulation technique, we assemble a plasmonic metamolecule that is designed for strong and simultaneous optical magnetic and magneto-electric excitation. Angle-dependent scattering spectroscopy is used to disentangle the two responses and to demonstrate that their constructive/destructive interplay causes strong directional scattering asymmetry. This asymmetry is used to extract both magneto-electric and magnetic dipole responses and to demonstrate their enhancement in comparison to ordinary atomistic materials.

Alignment-free three-dimensional optical metamaterials

Three-dimensional optical metamaterials based on multilayers typically rely on critical vertical alignment to achieve the desired functionality. Here the conditions under which three-dimensional metamaterials with different functionalities may be realized without constraints on alignment are analyzed and demonstrated experimentally. This study demonstrates that the release of alignment constraints for multilayered metamaterials is allowed, while their anomalous interaction with light is preserved.

Enhancement of Plasmonic Performance in Epitaxial Silver at Low Temperature

We report longer surface plasmon polariton propagation distance based on crystalline crystal silver at low temperature. Although enhanced plasmonic performance at low temperature has been predicted for a long time, it has not been directly observed on polycrystalline silver films which suffer from significant plasmonic losses due to grain boundaries and rough silver surface. Here we show that longer propagation distance can be achieved with epitaxial silver at low temperature. Importantly, the enhancement at low temperature are consistent across silver films grown with different methods.

High-sensitivity chiral molecular sensing with optical metasurfaces

Determination of the absolute handedness of single enantiomer at small quantities is essential in chiral drug developments. Here we provide theoretical insights, numerical analysis and experimental demonstrations of high sensitivity to zepto moles of chiral molecules using optical metasurfaces. We introduce a figure of merit (FoM) for metasurfaces that can be extracted from simple far-field scattering measurements at visible to near-infrared frequencies, establishing the optimal performance to detect molecular handedness. Our results experimentally show opposite signs of FoM for different molecular chirality. The properly designed metamaterial serves as an ultra-sensitive probe to enhance circular dichroism measurements at frequencies for which these signals would be otherwise undetectable.