Ryan Beams

Raman characterization of defects and dopants in graphene

In this article we review Raman studies of defects and dopants in graphene as well as the importance of both for device applications. First a brief overview of Raman spectroscopy of graphene is presented. In the following section we discuss the Raman characterization of three defect types: point defects, edges, and grain boundaries. The next section reviews the dependence of the Raman spectrum on dopants and highlights several common doping techniques. In the final section, several device applications are discussed which exploit doping and defects in graphene. Generally defects degrade the figures of merit for devices, such as carrier mobility and conductivity, whereas doping provides a means to tune the carrier concentration in graphene thereby enabling the engineering of novel material systems. Accurately measuring both the defect density and doping is critical and Raman spectroscopy provides a powerful tool to accomplish this task.

Voltage-controlled quantum light from an atomically thin semiconductor

Although semiconductor defects can often be detrimental to device performance, they are also responsible for the breadth of functionality exhibited by modern optoelectronic devices. Artificially engineered defects (so-called quantum dots) or naturally occurring defects in solids are currently being investigated for applications ranging from quantum information science and optoelectronics to high-resolution metrology. In parallel, the quantum confinement exhibited by atomically thin materials (semi-metals, semiconductors and insulators) has ushered in an era of flatland optoelectronics whose full potential is still being articulated. In this Letter we demonstrate the possibility of leveraging the atomically thin semiconductor tungsten diselenide (WSe2) as a host for quantum dot-like defects. We report that this previously unexplored solid-state quantum emitter in WSe2 generates single photons with emission properties that can be controlled via the application of external d.c. electric and magnetic fields. These new optically active quantum dots exhibit excited-state lifetimes on the order of 1 ns and remarkably large excitonic g-factors of 10. It is anticipated that WSe2 quantum dots will provide a novel platform for integrated solid-state quantum photonics and quantum information processing, as well as a rich condensed-matter physics playground with which to explore the coupling of quantum dots and atomically thin semiconductors.

Highly Reproducible Near-Field Optical Imaging with Sub-20-nm Resolution Based on Template-Stripped Gold Pyramids

With a template-stripping fabrication technique, we demonstrate the mass fabrication of high-quality, uniform, ultrasharp (10 nm) metallic probes suitable for single-molecule fluorescence imaging, tip-enhanced Raman spectroscopy (TERS), and other near-field imaging techniques. We achieve reproducible single-molecule imaging with sub-20-nm spatial resolution and an enhancement in the detected fluorescence signal of up to 200. Similar results are obtained for TERS imaging of carbon nanotubes. We show that the large apex angle (70.5°) of our pyramidal tip is well suited to scatter the near-field optical signal into the far-field, leading to larger emission enhancement and hence to a larger quantum yield. Each gold or silver pyramidal probe is used on-demand, one at a time, and the unused tips can be stored for extended times without degradation or contamination. The high yield (>95%), reproducibility, durability, and massively parallel fabrication (1.5 million identical probes over a wafer) of the probes hold promise for reliable optical sensing and detection and for cementing near-field optical imaging and spectroscopy as a routine characterization technique.

Graphene transfer with reduced residue

Abstract We present a new transfer procedure for graphene using acetic acid, which removes the residue that is common in standard acetone treatments. Post-transfer samples cleaned with acetic acid and acetone were characterized using Raman spectroscopy and atomic force microscopy for comparison. We further illustrate the quality of our transfer process by using fluorescence quenching to create an optical map of surface contaminants.

Integrated nanophotonics based on nanowire plasmons and atomically thin material

The continually increasing demands for higher-speed and lower-operating-power devices have resulted in the continued impetus to shrink photonic components. We demonstrate a primitive nanophotonic integrated circuit element composed of a single silver nanowire and single-layer molybdenum disulfide (MoS2) flake. Using scanning confocal fluorescence microscopy and spectroscopy, we find that nanowire plasmons can excite MoS2 photoluminescence and that MoS2 excitons can decay into nanowire plasmons. Finally, we show that the nanowire may serve the dual purpose of both exciting MoS2 photoluminescence via plasmons and recollecting the decaying exciton as nanowire plasmons. The potential for subwavelength light guiding and strong nanoscale light–matter interaction afforded by our device may facilitate compact and efficient on-chip optical processing.

Low Temperature Raman Study of the Electron Coherence Length near Graphene Edges

This paper reports the experimental determination of the phase-breaking length Lφ of conduction electrons in graphene using Raman spectroscopy. Based on the double-resonance model, we extract Lφ from the spatial dependence of the D band susceptibility χD near the graphene edge. By using prior knowledge of sample properties and the excitation point-spread function we are able to determine the spatial variation of the Raman susceptibilities with high accuracy, and the results reveal a phase-breaking length Lφ = 40nm near the graphene edge.We developed a novel optical defocusing method for studying spatial coherence of photoexcited electrons and holes near edges of graphene. Our method is applied to measure the localization l(D) of the disorder-induced Raman D band (∼1350 cm(-1)) with a resolution of a few nanometers. Raman scattering experiments performed in a helium bath cryostat reveal that as temperature is decreased from 300 to 1.55 K, the length l(D) increases. We found that the localization of the D band varies as 1/T(1/2), giving strong evidence that l(D) scales with the coherence length of photoexcited electrons near graphene edges.

Nanoscale Fluorescence Lifetime Imaging of an Optical Antenna with a Single Diamond NV Center

Solid-state quantum emitters, such as artificially engineered quantum dots or naturally occurring defects in solids, are being investigated for applications ranging from quantum information science and optoelectronics to biomedical imaging. Recently, these same systems have also been studied from the perspective of nanoscale metrology. In this letter, we study the near-field optical properties of a diamond nanocrystal hosting a single nitrogen vacancy center. We find that the nitrogen vacancy center is a sensitive probe of the surrounding electromagnetic mode structure. We exploit this sensitivity to demonstrate nanoscale fluorescence lifetime imaging microscopy (FLIM) with a single nitrogen vacancy center by imaging the local density of states of an optical antenna.

Nanoscale spectroscopy with optical antennas

Optical antennas made of gold nanoparticles are used to enhance the spectroscopic response of single molecules. With a scannable optical half-wave antenna in the form of a gold nanorod we achieve a spatial resolution of 20nm in fluorescence imaging. We explore simultaneous fluorescence and Raman enhancement of dye molecules in the junction of two gold nanoparticles and find similar enhancements as a function of interparticle distance for both fluorescence and Raman scattering. We compare our results with theoretical predictions and provide possible explanations.

Background Suppression in Near-Field Optical Imaging

In several recent studies, antenna-based optical microscopy has demonstrated its potential to resolve features as small as 10 nm. Most studies are concerned with well-separated features on flat surfaces, and there are only few studies that deal with samples of high feature density or even three-dimensional objects. The reason is that the external laser irradiation of the optical antenna (e.g., tip or particle) also directly irradiates the sample and therefore gives rise to a background. Here we introduce an efficient background suppression scheme that makes use of feedback modulation. The method is widely applicable and not restricted to cantilever-based scanning schemes. We apply this technique to both dense samples of dye molecules and ion channel proteins in plasma membranes and demonstrate effective background suppression and strongly improved sensitivity. The feedback modulation scheme is expected to find application for biological studies in liquid environments and for investigations of subsurface features in material science.

Controllable optical negative refraction and phase conjugation in graphite thin films

Metamaterials can negatively diffract optical-wavelength light; however, they suffer from high losses and only work over a narrow band of frequencies. Researchers now show how nonlinear optics in thin films of graphite can offer a solution. The negligible thickness of the layers reduces the losses, and the linear band structure of the material ensures broadband operation.