Ran Li

This paper describes a nanofabrication procedure that can generate multiscale substrates with quasi-random microregions of nanoparticle arrays having different periodicities and metals. We combine cycles of large-area nanoparticle array fabrication with solvent-assisted wrinkle lithography to mask and etch quasi-random areas of prefabricated nanoparticles to control the fill factors of the arrays. The approach is highly flexible, and parameters, including nanoparticle size and material, array geometry, and fill factor, can be tailored independently. Multimetallic nanoparticle arrays can support surface lattice resonances at fill factors as low as 20% and can function as nanoscale cavities for lasing action with as few as 10% of the nanoparticles in an array. We demonstrated that multimetallic nanoparticle substrates that combine two or three arrays with different periodicities can exhibit lasing responses over visible and near-infrared wavelengths. Our work showcases the robust optical responses of multimetallic and periodic devices for broadband light manipulation.

Significance: Molecules interacting with metallic nanostructures can show tunable exciton-plasmon coupling, ranging from weak to strong. One factor that influences the interactions is the spatial organization of the molecules relative to the localized plasmon-enhanced electromagnetic fields. In this work, we show that the arrangement of aromatic dye molecules can be tuned within plasmonic hotspots by interfacial engineering of nanoparticle surfaces. By controlling the local chemical and physical interactions, we could modulate lasing thresholds. Surface-functionalized plasmonic metasurfaces open prospects for programmable light-matter interactions at the nanoscale.

A plasmonic nanolaser architecture that can produce white‐light emission is reported. A laser device is designed based on a mixed dye solution used as gain material sandwiched between two aluminum nanoparticle (NP) square lattices of different periodicities. The (±1, 0) and (±1, ±1) band‐edge surface lattice resonance (SLR) modes of one NP lattice and the (±1, 0) band‐edge mode of the other NP lattice function as nanocavity modes for red, blue, and green lasing respectively. From a single aluminum NP lattice, simultaneous red and blue lasing is realized from a binary dye solution, and the relative intensities of the two colors are controlled by the volume ratio of the dyes. Also, a laser device is constructed by sandwiching dye solutions between two Al NP lattices with different periodicities, which enables red–green and blue–green lasing. With a combination of three dyes as liquid gain, red, green, and blue lasing for a white‐light emission profile is realized.

Because of translational symmetry, electromagnetic fields confined within 2D periodic optical structures can be represented within the first Brillouin zone (BZ). In contrast, the wavevectors of scattered electromagnetic fields outside the lattice are constrained by the 3D light cone, the free-photon dispersion in the surrounding medium. Here, we report that light-cone surface lattice resonances (SLRs) from plasmonic nanoparticle lattices can be used to observe the radiated electromagnetic fields from extended BZ edges. Our coupled dipole radiation theory reveals how lattice geometry and induced surface plasmon dipole orientation affect angular distributions of the radiated fields. Using dye molecules as local dipole emitters to excite the light-cone SLR modes, we experimentally identified high-order BZ edges by directional, in-plane lasing emission. These results provide insight into nanolaser architectures that can emit at multiple wavelengths and in-plane directions simply by rotating the nanocavity lattice.

Significance: The ability to control light has driven advances from optical microscopy to fast communication. Metal nanoparticles can trap light at the nanoscale in the form of surface plasmons; these localized excitations are important in sensing and designing miniaturized photonic devices. Although very narrow plasmon linewidths are desirable, they tend to be broad because of limitations in fabrication methods. Here, we describe how to achieve ultranarrow plasmon resonances with linewidths that approach the calculated limit by thermally annealing 2D lattices of metal nanoparticles. Our results indicate that exquisite control over structural features of nanoparticles can dramatically improve their plasmonic response and open promising strategies for manipulating light–matter interactions at the nanoscale.

The tailored spatial polarization of coherent light beams is important for applications ranging from microscopy to biophysics to quantum optics. Miniaturized light sources are needed for integrated, on-chip photonic devices with desired vector beams; however, this issue is unresolved because most lasers rely on bulky optical elements to achieve such polarization control. Here, we report on quantum dot-plasmon lasers with engineered polarization patterns controllable by near-field coupling of colloidal quantum dots to metal nanoparticles. Conformal coating of CdSe–CdS core–shell quantum dot films on Ag nanoparticle lattices enables the formation of hybrid waveguide-surface lattice resonance (W-SLR) modes. The sidebands of these hybrid modes at nonzero wavevectors facilitate directional lasing emission with either radial or azimuthal polarization depending on the thickness of the quantum dot film.

We report how the direction of quantum dot (QD) lasing can be engineered by exploiting high-symmetry points in plasmonic nanoparticle (NP) lattices. The nanolaser architecture consists of CdSe–CdS core–shell QD layers conformally coated on two-dimensional square arrays of Ag NPs. Using waveguide-surface lattice resonances (W-SLRs) near the Δ point in the Brillouin zone as optical feedback, we achieved lasing from the gain in CdS shells at off-normal emission angles. Changing the periodicity of the plasmonic lattices enables other high-symmetry points (Γ or M) of the lattice to overlap with the QD shell emission, which facilitates tuning of the lasing direction. We also increased the thickness of the QD layer to introduce higher-order W-SLR modes with additional avoided crossings in the band structure, which expands the selection of cavity modes for any desired lasing emission angle.