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David J. Norris

Publications and source records attributed to David J. Norris.

31 records · Page 2Linked to original sources

Optical Fourier surfaces

Gratings and holograms are patterned surfaces that tailor optical signals by diffraction. Despite their long history, variants with remarkable functionalities continue to be discovered. Further advances could exploit Fourier optics, which specifies the surface pattern that generates a desired diffracted output through its Fourier transform. To shape the optical wavefront, the ideal surface profile should contain a precise sum of sinusoidal waves, each with a well-defined amplitude, spatial frequency, and phase. However, because fabrication techniques typically yield profiles with at most a few depth levels, complex 'wavy' surfaces cannot be obtained, limiting the straightforward mathematical design and implementation of sophisticated diffractive optics. Here we present a simple yet powerful approach to eliminate this design-fabrication mismatch by demonstrating optical surfaces that contain an arbitrary number of specified sinusoids. We combine thermal scanning-probe lithography and templating to create periodic and aperiodic surface patterns with continuous depth control and sub-wavelength spatial resolution. Multicomponent linear gratings allow precise manipulation of electromagnetic signals through Fourier-spectrum engineering. Consequently, we immediately resolve an important problem in photonics by creating a single-layer grating that simultaneously couples red, green, and blue light at the same angle of incidence. More broadly, we analytically design and accurately replicate intricate two-dimensional moiré patterns, quasicrystals, and holograms, demonstrating a variety of previously impossible diffractive surfaces. Therefore, this approach provides instant benefit for optical devices (biosensors, lasers, metasurfaces, and modulators) and emerging topics in photonics (topological structures, transformation optics, and valleytronics).

physics.optics↗

Three-dimensional enantiomeric recognition of optically trapped single chiral nanoparticles

We optically trap freestanding single metallic chiral nanoparticles using a standing-wave optical tweezer. We also incorporate within the trap a polarimetric setup that allows to perform in situ chiral recognition of single enantiomers. This is done by measuring the S_3 component of the Stokes vector of a light beam scattered off the trapped nanoparticle in the forward direction. This unique combination of optical trapping and chiral recognition, all implemented within a single setup, opens new perspectives towards the control, recognition, and manipulation of chiral objects at nanometer scales.

physics.optics↗

Bright triplet excitons in lead halide perovskites

Nanostructured semiconductors emit light from electronic states known as excitons[1]. According to Hund's rules[2], the lowest energy exciton in organic materials should be a poorly emitting triplet state. Analogously, the lowest exciton level in all known inorganic semiconductors is believed to be optically inactive. These 'dark' excitons (into which the system can relax) hinder light-emitting devices based on semiconductor nanostructures. While strategies to diminish their influence have been developed[3-5], no materials have been identified in which the lowest exciton is bright. Here we show that the lowest exciton in quasi-cubic lead halide perovskites is optically active. We first use the effective-mass model and group theory to explore this possibility, which can occur when the strong spin-orbit coupling in the perovskite conduction band is combined with the Rashba effect [6-10]. We then apply our model to CsPbX3 (X=Cl,Br,I) nanocrystals[11], for which we measure size- and composition-dependent fluorescence at the single-nanocrystal level. The bright character of the lowest exciton immediately explains the anomalous photon-emission rates of these materials, which emit 20 and 1,000 times faster[12] than any other semiconductor nanocrystal at room[13-16] and cryogenic[17] temperatures, respectively. The bright exciton is further confirmed by detailed analysis of the fine structure in low-temperature fluorescence spectra. For semiconductor nanocrystals[18], which are already used in lighting[19,20], lasers[21,22], and displays[23], these optically active excitons can lead to materials with brighter emission and enhanced absorption. More generally, our results provide criteria for identifying other semiconductors exhibiting bright excitons with potentially broad implications for optoelectronic devices.

cond-mat.mes-hall↗

Colloidal-quantum-dot spasers and plasmonic amplifiers

Colloidal quantum dots are robust, efficient, and tunable emitters now used in lighting, displays, and lasers. Consequently, when the spaser, a laser-like source of surface plasmons, was first proposed, quantum dots were specified as the ideal plasmonic gain medium. Subsequent spaser designs, however, have required a single material to simultaneously provide gain and define the plasmonic cavity, an approach ill-suited to quantum dots and other colloidal nanomaterials. Here we develop a more open architecture that decouples the gain medium from the cavity, leading to a versatile class of quantum-dot-based spasers that allow controlled generation, extraction, and manipulation of plasmons. We first create high-quality-factor, aberration-corrected, Ag plasmonic cavities. We then incorporate quantum dots via electrohydrodynamic printing18,19 or drop-casting. Photoexcitation under ambient conditions generates monochromatic plasmons above threshold. This signal is extracted, directed through an integrated amplifier, and focused at a nearby nanoscale tip, generating intense electromagnetic fields. This spaser platform, deployable at different wavelengths, size scales, and geometries, can enable more complex on-chip plasmonic devices.

physics.optics↗

Direct Patterning of Colloidal Quantum-Dot Thin Films for Enhanced and Spectrally Selective Out-Coupling of Emission

We report on a template-stripping method for the direct surface patterning of colloidal quantum-dot thin films to produce highly luminescent structures with feature sizes less than 100 nm. Through the careful design of high quality bulls-eye gratings we can produce strong directional beaming (10° divergence) with up to six-fold out-coupling enhancement of spontaneous emission in the surface-normal direction. A transition to narrow single-mode lasing is observed in these same structures at thresholds as low as 120 μJ/cm2. Furthermore, making use of the size-tunable character of colloidal quantum dots, we demonstrate spectrally selective out-coupling of light from mixed quantum-dot films. Our results provide a straightforward route towards significantly improved optical properties of colloidal quantum-dot assemblies.

cond-mat.mes-hall↗

Full-Spectrum Flexible Color Printing at the Diffraction Limit

Color printing at the diffraction limit has been recently explored by fabricating nanoscale plasmonic structures with electron beam lithography. However, only a limited color range and constant intensity throughout the structure have been demonstrated. Here we show an alternative, facile approach relying on the direct, open-atmosphere electrohydrodynamic rapid nanodrip printing of controlled amounts of red, green and blue (RGB) quantum dots at a resolution of 250 nm. The narrow emission spectrum of the dots allows the coverage of a very broad color space, exceeding standard RGB (sRGB) of modern display devices. We print color gradients of variable intensity, which to date could not be achieved with diffraction-limited resolution. Showcasing the capabilities of the technology, we present a photo-realistic printed image of a colorful parrot with a pixel size of 250 nm.

physics.optics↗

Charge Effects and Nanoparticle Pattern Formation in Electrohydrodynamic NanoDrip Printing of Colloids

Advancing open atmosphere printing technologies to produce features in the nanoscale range has important and broad applications ranging from electronics, to photonics, plasmonics and biology. Recently an electrohydrodynamic printing regime has been demonstrated in a rapid dripping mode (termed NanoDrip), where the ejected colloidal droplets from nozzles of diameters of O(1 μm) can controllably reach sizes an order of magnitude smaller than the nozzle and can generate planar and out-of-plane structures of similar sizes. Despite demonstrated capabilities, our fundamental understanding of important aspects of the physics of NanoDrip printing needs further improvement. Here we address the topics of charge content and transport in NanoDrip printing. We employ quantum dot and gold nanoparticle dispersions in combination with a specially designed, auxiliary, asymmetric electric field, targeting the understanding of charge locality (particles vs. solvent) and particle distribution in the deposits as indicated by the dried nanoparticle patterns (footprints) on the substrate. We show that droplets of alternating charge can be spatially separated when applying an ac field to the nozzle. The nanoparticles within a droplet are distributed asymmetrically under the influence of the auxiliary lateral electric field, indicating that they are the main carriers. We also show that the ligand length of the nanoparticles in the colloid affects their mobility after deposition (in the sessile droplet state).

cond-mat.soft↗

Printable Nanoscopic Metamaterial Absorbers and Images with Diffraction-Limited Resolution

The fabrication of functional metamaterials with extreme feature resolution finds a host of applications such as the broad area of surface/light interaction. Non-planar features of such structures can significantly enhance their performance and tunability, but their facile generation remains a challenge. Here, we show that carefully designed out-of-plane nanopillars made of metal-dielectric composites integrated in a metal-dielectric-nanocomposite configuration, can absorb broadband light very effectively. We further demonstrate that electrohydrodynamic printing in a rapid nanodripping mode, is able to generate precise out-of-plane forests of such composite nanopillars with deposition resolutions at the diffraction limit on flat and non-flat substrates. The nanocomposite nature of the printed material allows the fine-tuning of the overall visible light absorption from complete absorption to complete reflection by simply tuning the pillar height. Almost perfect absorption (~95%) over the entire visible spectrum is achieved by a nanopillar forest covering only 6% of the printed area. Adjusting the height of individual pillar groups by design, we demonstrate on-demand control of the gray scale of a micrograph with a spatial resolution of 400 nm. These results constitute a significant step forward in ultra-high resolution facile fabrication of out-of-plane nanostructures, important to a broad palette of light design applications. nanostructures, important to a broad palette of light design applications.

physics.optics↗

How semiconductor nanoplatelets form

Colloidal nanoplatelets - quasi-two-dimensional sheets of semiconductor exhibiting efficient, spectrally pure fluorescence - form when liquid-phase syntheses of spherical quantum dots are modified. Despite intense interest in their properties, the mechanism behind their anisotropic shape and precise atomic-scale thickness remains unclear, and even counterintuitive when their crystal structure is isotropic. One commonly accepted explanation is that nanoclusters nucleate within molecular templates and then fuse. Here, we test this mechanism for zincblende nanoplatelets and show that they form instead due to an intrinsic instability in growth kinetics. We synthesize CdSe and CdS1-xSex nanoplatelets in template- and solvent-free isotropic melts containing only cadmium carboxylate and chalcogen, a finding incompatible with previous explanations. Our model, based on theoretical results showing enhanced growth on narrow surface facets, rationalizes nanoplatelet formation and experimental dependencies on temperature, time, and carboxylate length. Such understanding should lead to improved syntheses, controlled growth on surfaces, and broader libraries of nanoplatelet materials.

cond-mat.mtrl-sci↗

Plasmonic Films Can Easily Be Better: Rules and Recipes

High-quality materials are critical for advances in plasmonics, especially as researchers now investigate quantum effects at the limit of single surface plasmons or exploit ultraviolet- or CMOS-compatible metals such as aluminum or copper. Unfortunately, due to inexperience with deposition methods, many plasmonics researchers deposit metals under the wrong conditions, severely limiting performance unnecessarily. This is then compounded as others follow their published procedures. In this perspective, we describe simple rules collected from the surface-science literature that allow high-quality plasmonic films of aluminum, copper, gold, and silver to be easily deposited with commonly available equipment (a thermal evaporator). Recipes are also provided so that films with optimal optical properties can be routinely obtained.

cond-mat.mtrl-sci↗

The Optical Chirality Flux as a Useful Far-Field Probe of Chiral Near Fields

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.

physics.optics↗

Microscopic Theory of Cation Exchange in CdSe Nanocrystals

Although poorly understood, cation-exchange reactions are increasingly used to dope or transform colloidal semiconductor nanocrystals (quantum dots). We used density-functional theory and kinetic Monte Carlo simulations to develop a microscopic theory that explains structural, optical, and electronic changes observed experimentally in Ag-cation-exchanged CdSe nanocrystals. We find that Coulomb interactions, both between ionized impurities and with the polarized nanocrystal surface, play a key role in cation exchange. Our theory also resolves several experimental puzzles related to photoluminescence and electrical behavior in CdSe nanocrystals doped with Ag.

cond-mat.mes-hall↗

Ultrafast optical switching of three-dimensional Si inverse opal photonic band gap crystals

We present ultrafast optical switching experiments on 3D photonic band gap crystals. Switching the Si inverse opal is achieved by optically exciting free carriers by a two-photon process. We probe reflectivity in the frequency range of second order Bragg diffraction where the photonic band gap is predicted. We find good experimental switching conditions for free-carrier plasma frequencies between 0.3 and 0.7 times the optical frequency: we thus observe a large frequency shift of up to D omega/omega= 1.5% of all spectral features including the peak that corresponds to the photonic band gap. We deduce a corresponding large refractive index change of Dn'_Si/n'_Si= 2.0% and an induced absorption length that is longer than the sample thickness. We observe a fast decay time of 21 ps, which implies that switching could potentially be repeated at GHz rates. Such a high switching rate is relevant to future switching and modulation applications.

physics.optics↗