Ramsey-type microwave spectroscopy on CO (a3Πa^3\Pi)

Using a Ramsey-type setup, the lambda-doublet transition in the $J=1,\, \Omega=1$ level of the $a^3\Pi$ state of CO was measured to be 394 064 870(10) Hz. In our molecular beam apparatus, a beam of metastable CO is prepared in a single quantum level by expanding CO into vacuum and exciting the molecules using a narrow-band UV laser system. After passing two microwave zones that are separated by 50 cm, the molecules are state-selectively deflected and detected 1 meter downstream on a position sensitive detector. In order to keep the molecules in a single $m_J^B$ level, a magnetic bias field is applied. We find the field-free transition frequency by taking the average of the $m_J^B = +1 \rightarrow m_J^B = +1$ and $m_J^B = -1 \rightarrow m_J^B = -1$ transitions, which have an almost equal but opposite Zeeman shift. The accuracy of this proof-of-principle experiment is a factor of 100 more accurate than the previous best value obtained for this transition

Non-destructive characterization of nitrogen-implanted silicon-on-insulator structures by spectroscopic ellipsometry

Silicon-on-insulator (SOI) structures implanted with 200 or 400 keV N+ ions at a dose of 7.5 × 1017cm−2 were studied by spectroscopic ellipsometry (SE). The SE measurements were carried out in the 300–700 nm wavelength (4.13-1.78 eV photon energy) range. The SE data were analysed by the conventional method of using appropriate optical models and linear regression analysis. We applied a seven-layer model (a surface oxide layer, a thick silicon layer, upper two interface layers, a thick nitride layer and lower two interface layers) with good results. The fitted parameters were the layer thickness and compositions. The results were compared with data obtained from Rutherford backscattering spectroscopy (RBS) and transmission electron microscopy. The sensitivity of our optical model and fitting technique was good enough to distinguish between the silicon-rich transition layers near the upper and lower interfaces of the nitride layer, which are unresolvable in RBS measurements

Vicinal Surfaces and the Calogero-Sutherland Model

A miscut (vicinal) crystal surface can be regarded as an array of meandering but non-crossing steps. Interactions between the steps are shown to induce a faceting transition of the surface between a homogeneous Luttinger liquid state and a low-temperature regime consisting of local step clusters in coexistence with ideal facets. This morphological transition is governed by a hitherto neglected critical line of the well-known Calogero-Sutherland model. Its exact solution yields expressions for measurable quantities that compare favorably with recent experiments on Si surfaces.Comment: 4 pages, revtex, 2 figures (.eps

Integration Results

The H2020 What to do With the Wi-Fi Wild West (Wi-5) project combines research and innovation to propose a Software Defined Networking (SDN) architecture based on an integrated and coordinated set of smart Wi-Fi networking solutions. In this document, we present the integration methodologies and provide the integration test results of the developed functionalities of Wi-5. The integration of the functionalities is being developed within Work Package 5. First, the smart and cooperative solutions provided by the SDN based Wi-5 architecture will be briefly described. Next, we will define and explain the modular approach to be applied in Wi-5 APs and the Wi-5 controller. According to this approach, we will describe the functionalities of both the Wi-5 APs that are modelled as a combination of the monitoring and network configuration modules, and the Wi-5 controller which is composed of the monitoring, decision, and network configuration modules. Following this, we will define and explain the Wi-5 integration strategy that was utilized to integrate the smart and cooperative functionalities in terms of assembly of the modules utilized to model the Wi-5 AP and the Wi-5 controller. The integration approach and steps of the proposed functionalities are then given and the limitations that have been faced during the integration progress of the functionalities are clearly explained in each subsection. Moreover, the design criteria and possible evaluation approaches of such nonintegrated functionalities are explicitly provided. During the integration process, coordinated work between WP3 and WP4 was carried out and, after the feedback was shared for WP5-WP3 and WP5WP4, some novel innovations and contributions are introduced. The online integration approach for the channel assignment algorithm of the radio resource management solution is proposed, and integrated as a product of this mutual feedback. Also, the proactive handover application for seamless handover functionality is another product of this collaboration. After the integration process, the test definitions and evaluation results of the integrated functionalities are presented. Also, the available test metrics and network deployments for each of the functionality tests are provided. The test results prove that the proposed functionalities perform well in meeting the design objectives. We observe that the Wi-5 solutions give the expected performance gains in most of the conducted test cases

Nanometer control in plasmonic systems through discrete layer-by-layer macrocycle-cation deposition.

In this work, we demonstrate that coordination interactions between Fe3+ and cucurbit[7]uril (CB[7]) can be utilised to build up defined nanoscale spacing layers in metallic nanosystems. We begin by characterising the layer-by-layer deposition of CB[7] and FeCl3·6H2O coordination layers through the use of a Quartz-Crystal Microbalance (QCM) and contact angle measurements. We then apply this layered structure to accurately control the spacing, and thus optical properties, of gold nanoparticles in a Nanoparticle-on-Mirror (NPoM) structure, which is demonstrated via normalising plasmon resonance spectroscopy.European Commission for a Marie Curie Fellowship (NANOSPHERE, 658360) ERC starting investigator grant (ASPiRe 240629) RC acknowledges support from the Dr. Manmohan Singh scholarship from St. John’s College BdN acknowledges support from the Leverhulme Trust and the Isaac Newton trust ECF

Pulsed Molecular Optomechanics in Plasmonic Nanocavities: From Nonlinear Vibrational Instabilities to Bond-Breaking

Small numbers of surface-bound molecules are shown to behave as would be expected for opto-mechanical oscillators placed inside plasmonic nano-cavities that support extreme confinement of optical fields. Pulsed Raman scattering reveals superlinear Stokes emission above a threshold, arising from the stimulated vibrational pumping of molecular bonds under pulsed excitation shorter than the phonon decay time, and agreeing with pulsed optomechanical quantum theory. Reaching the parametric instability (equivalent to a phonon laser or ‘phaser’ regime) is however hindered by motion of gold atoms and molecular reconfiguration at phonon occupations approaching unity. We show how this irreversible bond breaking can ultimately limit the exploitation of molecules as quantum mechanical oscillators, but accesses optically-driven chemistry

Accelerated Molecular Vibrational Decay and Suppressed Electronic Nonlinearities in Plasmonic Cavities through Coherent Raman Scattering

Molecular vibrations and their dynamics are of outstanding importance for electronic and thermal transport in nanoscale devices as well as for molecular catalysis. The vibrational dynamics of <100 molecules are studied through three-colour time-resolved coherent anti-Stokes Raman spectroscopy (trCARS) using plasmonic nanoantennas. This isolates molecular signals from four-wave mixing (FWM), while using exceptionally low nanowatt powers to avoid molecular damage via single-photon lock-in detection. FWM is found to be strongly suppressed in nm-wide plasmonic gaps compared to plasmonic nanoparticles. The ultrafast vibrational decay rates of biphenyl-4-thiol molecules are accelerated ten-fold by a transient rise in local non-equilibrium temperature excited by enhanced, pulsed optical fields within these plasmonic nanocavities. Separating the contributions of vibrational population decay and dephasing carefully explores the vibrational decay channels of these tightly confined molecules. Such extreme plasmonic enhancement within nanogaps opens up prospects for measuring single-molecule vibrationally-coupled dynamics and diverse molecular optomechanics phenomena

Contact angle as a powerful tool in anisotropic colloid synthesis

Nucleation and growth is a technique widely used to prepare colloids, in which droplets are adsorbed onto substrate particles. Changing the contact angle of the substrates can greatly alter the morphology of the product particles. Here, we investigate the nucleation and growth of 3-methacryloxypropyltrimethoxysilane (MPTMS) both onto Stöber spheres and onto (cross-linked) MPTMS* spheres. The former results in ‘snowman’ particles with a cap-shaped MPTMS* compartment, and we show that their morphology is highly controllable via the MPTMS content in the reaction mixture. The contact angle of the MPTMS* compartment decreases with droplet diameter, suggesting that this wetting process is affected not only by surface tension but also by line tension. In contrast to Stöber spheres, MPTMS* substrate particles yield highly reproducible and tuneable ‘engulfed-sphere’ colloids with an internal reference axis (but a homogeneous mass distribution). These engulfed-sphere particles can be fully index-matched for confocal microscopy on account of their homogeneous refractive index. Suitable index-matching mixtures of polar and of low-polar media are presented, where cyclohexyl iodide (CHI) is introduced as a new medium for colloids of high refractive index. Finally, the index-matched engulfed-sphere colloids are self-assembled into (close-packed and long-range) plastic phases, and the particles’ rotational diffusion inside the crystal phases is tracked via confocal microscopy

Single-molecule strong coupling at room temperature in plasmonic nanocavities.

Photon emitters placed in an optical cavity experience an environment that changes how they are coupled to the surrounding light field. In the weak-coupling regime, the extraction of light from the emitter is enhanced. But more profound effects emerge when single-emitter strong coupling occurs: mixed states are produced that are part light, part matter1, 2, forming building blocks for quantum information systems and for ultralow-power switches and lasers. Such cavity quantum electrodynamics has until now been the preserve of low temperatures and complicated fabrication methods, compromising its use. Here, by scaling the cavity volume to less than 40 cubic nanometres and using host–guest chemistry to align one to ten protectively isolated methylene-blue molecules, we reach the strong-coupling regime at room temperature and in ambient conditions. Dispersion curves from more than 50 such plasmonic nanocavities display characteristic light–matter mixing, with Rabi frequencies of 300 millielectronvolts for ten methylene-blue molecules, decreasing to 90 millielectronvolts for single molecules—matching quantitative models. Statistical analysis of vibrational spectroscopy time series and dark-field scattering spectra provides evidence of single-molecule strong coupling. This dressing of molecules with light can modify photochemistry, opening up the exploration of complex natural processes such as photosynthesis and the possibility of manipulating chemical bonds.We acknowledge financial support from EPSRC grants EP/G060649/1 and EP/I012060/1, and ERC grant LINASS 320503. RC acknowledges support from the Dr. Manmohan Singh scholarship from St. John’s College. FB acknowledges support from the Winton Programme for the Physics of Sustainability. SJB acknowledges support from the European Commission for a Marie Curie Fellowship (NANOSPHERE, 658360).This is the author accepted manuscript. The final version is available from Nature Publishing Group via http://dx.doi.org/10.1038/nature17974

SERS Sensing of Dopamine with Fe(III)-Sensitized Nanogaps in Recleanable AuNP Monolayer Films

Sensing of neurotransmitters (NTs) down to nm concentrations is demonstrated by utilizing self-assembled monolayers of plasmonic 60 nm Au nanoparticles in close-packed arrays immobilized onto glass substrates. Multiplicative surface-enhanced Raman spectroscopy enhancements are achieved by integrating Fe(III) sensitizers into the precisely-defined <1 nm nanogaps, to target dopamine (DA) sensing. The transparent glass substrates allow for efficient access from both sides of the monolayer aggregate films by fluid and light, allowing repeated sensing in different analytes. Repeated reusability after analyte sensing is shown through oxygen plasma cleaning protocols, which restore pristine conditions for the nanogaps. Examining binding competition in multiplexed sensing of two catecholamine NTs, DA and epinephrine, reveals their bidentate binding and their interactions. These systems are promising for widespread microfluidic integration enabling a wide range of continuous biofluid monitoring for applications in precision health