Understanding Capacitance Variation in Sub-nanometer Pores by in Situ Tuning of Interlayer Constrictions.

The contribution of subnanometer pores in carbon electrodes to the charge-storage mechanism in supercapacitors has been the subject of intense debate for over a decade. Here, we provide a model system based on graphene oxide, which employs interlayer constrictions as a model for pore sizes that can be both controllably tuned and studied in situ during supercapacitor device use. Correlating electrochemical performance and in situ tuning of interlayer constrictions, we observe a peak in specific capacitance when interlayer constriction size reaches the diameters of unsolvated ions, supporting the hypothesized link between loss of ion solvation shell and anomalous capacitance increase for subnanometer pores.DTLG acknowledges technical support by J. N. R. Grundy (University of Cambridge) and financial support from Newnham College, Cambridge and the Cambridge Commonwealth Trust. GAJA acknowledges partial support for this work from Dyson Ltd. BCB acknowledges a College Research Fellowship at Hughes Hall, Cambridge. DTLG and GAJA thank Ananda Hettiarachchy and K. M. N. de Silva for discussions on activated carbon.This is the author accepted manuscript. The final version is available from the American Chemical Society via http://dx.doi.org/10.1021/acsnano.5b0581

Study and mitigation of spurious electron emission from cathodic wires in noble liquid time projection chambers

Noble liquid radiation detectors have long been afflicted by spurious electron emission from their cathodic electrodes. This phenomenon must be understood and mitigated in the next generation of liquid xenon (LXe) experiments searching for WIMP dark matter or neutrinoless double beta decay, and in the large liquid argon (LAr) detectors for the long-baseline neutrino programmes. We present a systematic study of this spurious emission involving a series of slow voltage-ramping tests on fine metal wires immersed in a two-phase xenon time projection chamber with single electron sensitivity. Emission currents as low as 10−18A can thus be detected by electron counting, a vast improvement over previous dedicated measurements. Emission episodes were recorded at surface fields as low as ∼ 10 kV/cm in some wires and observed to have complex emission patterns, with average rates of 10–200 counts per second (c/s) and outbreaks as high as ∼ 106c/s. A fainter, less variable type of emission was also present in all untreated samples. There is evidence of a partial conditioning effect, with subsequent tests yielding on average fewer emitters occurring at different fields for the same wire. We find no evidence for an intrinsic threshold particular to the metal-LXe interface which might have limited previous experiments up to fields of at least 160 kV/cm. The general phenomenology is not consistent with enhanced field emission from microscopic filaments, but it appears instead to be related to the quality of the wire surface in terms of corrosion and the nature of its oxide layer. This study concludes that some surface treatments, in particular nitric acid cleaning applied to stainless steel wires, can bring about at least order-of-magnitude improvements in overall electron emission rates, and this should help the next generation of detectors achieve the required electrostatic performance

Nucleation control for large, single crystalline domains of monolayer hexagonal boron nitride via Si-doped Fe catalysts.

The scalable chemical vapor deposition of monolayer hexagonal boron nitride (h-BN) single crystals, with lateral dimensions of ∼0.3 mm, and of continuous h-BN monolayer films with large domain sizes (>25 μm) is demonstrated via an admixture of Si to Fe catalyst films. A simple thin-film Fe/SiO2/Si catalyst system is used to show that controlled Si diffusion into the Fe catalyst allows exclusive nucleation of monolayer h-BN with very low nucleation densities upon exposure to undiluted borazine. Our systematic in situ and ex situ characterization of this catalyst system establishes a basis for further rational catalyst design for compound 2D materials.S.C. acknowledges funding from EPSRC (Doctoral training award). R.S.W. acknowledges a Research Fellowship from St. John ’ s College. B.C.B acknowledges a Research Fellowship at Hughes Hall. A.C.-V. acknowledges the Conacyt Cambridge Scholarship and Roberto Rocca Fellowship. S.H. acknowledges funding from ERC grant InsituNANO (No. 279342). B.B., S.J.S., K.M., and A.J.P. would like to acknowledge the National Measurement O ffi ce (NMO) for funding through the Innovation, Research and Development (IRD) programme (Project No. 115948). We acknowledge the European Synchrotron Radiation Fac ility (ESRF) for provision of synchrotron radiation, and we thank the sta ff for assistance in using beamline BM20/ROBL. We would also like to acknowl- edge Prof. Bonnie J. Tyler for discussions related to the manuscript.This is the final published article. It first appeared at http://pubs.acs.org/doi/abs/10.1021/nl5046632

Electric-field-induced coherent coupling of the exciton states in a single quantum dot

The signature of coherent coupling between two quantum states is an anticrossing in their energies as one is swept through the other. In single semiconductor quantum dots containing an electron-hole pair the eigenstates form a two-level system that can be used to demonstrate quantum effects in the solid state, but in all previous work these states were independent. Here we describe a technique to control the energetic splitting of these states using a vertical electric field, facilitating the observation of coherent coupling between them. Near the minimum splitting the eigenstates rotate in the plane of the sample, being orientated at 45{\deg} when the splitting is smallest. Using this system we show direct control over the exciton states in one quantum dot, leading to the generation of entangled photon pairs

Reactive intercalation and oxidation at the buried graphene-germanium interface

We explore a number of different electrochemical, wet chemical, and gas phase approaches to study intercalation and oxidation at the buried graphene-Ge interface. While the previous literature focused on the passivation of the Ge surface by chemical vapor deposited graphene, we show that particularly via electrochemical intercalation in a 0.25 N solution of anhydrous sodium acetate in glacial acetic acid, this passivation can be overcome to grow GeO2 under graphene. Angle resolved photoemission spectroscopy, Raman spectroscopy, He ion microscopy, and time-of-flight secondary ion mass spectrometry show that the monolayer graphene remains undamaged and its intrinsic strain is released by the interface oxidation. Graphene acts as a protection layer for the as-grown Ge oxide, and we discuss how these insights can be utilized for new processing approaches.We acknowledge financial support from the EPSRC (EP/K016636/1, EP/P51021X/1) and the Future Photonics Hub - Innovation Partnership Fund (EPSRC EP/L00044X/1). P.B.W. acknowledges EPSRC Cambridge NanoDTC EP/G037221/1. R.S.W. acknowledges funding from the European Union’s Horizon 2020 research and innovation programme through a EU Marie Skłodowska-Curie Individual Fellowship (Global) under grant ARTIST (no. 656870). R.W. acknowledges EPSRC Doctoral Training Award (EP/M506485/1)

Non-resonant dot-cavity coupling and its applications in resonant quantum dot spectroscopy

We present experimental investigations on the non-resonant dot-cavity coupling of a single quantum dot inside a micro-pillar where the dot has been resonantly excited in the s-shell, thereby avoiding the generation of additional charges in the QD and its surrounding. As a direct proof of the pure single dot-cavity system, strong photon anti-bunching is consistently observed in the autocorrelation functions of the QD and the mode emission, as well as in the cross-correlation function between the dot and mode signals. Strong Stokes and anti-Stokes-like emission is observed for energetic QD-mode detunings of up to ~100 times the QD linewidth. Furthermore, we demonstrate that non-resonant dot-cavity coupling can be utilized to directly monitor and study relevant QD s-shell properties like fine-structure splittings, emission saturation and power broadening, as well as photon statistics with negligible background contributions. Our results open a new perspective on the understanding and implementation of dot-cavity systems for single-photon sources, single and multiple quantum dot lasers, semiconductor cavity quantum electrodynamics, and their implementation, e.g. in quantum information technology.Comment: 17 pages, 4 figure

A semiconductor source of triggered entangled photon pairs?

The realisation of a triggered entangled photon source will be of great importance in quantum information, including for quantum key distribution and quantum computation. We show here that: 1) the source reported in ``A semiconductor source of triggered entangled photon pairs''[1. Stevenson et al., Nature 439, 179 (2006)]} is not entangled; 2) the entanglement indicators used in Ref. 1 are inappropriate, relying on assumptions invalidated by their own data; and 3) even after simulating subtraction of the significant quantity of background noise, their source has insignificant entanglement.Comment: 5 pages in pre-print format, 1 tabl

Improving a Natural CaMKII Inhibitor by Random and Rational Design

CaM-KIIN has evolved to inhibit stimulated and autonomous activity of the Ca(2+)/calmodulin (CaM)-dependent protein kinase II (CaMKII) efficiently, selectively, and potently (IC50 ∼100 nM). The CN class of peptides, derived from the inhibitory region of CaM-KIIN, provides powerful new tools to study CaMKII functions. The goal of this study was to identify the residues required for CaMKII inhibition, and to assess if artificial mutations could further improve the potency achieved during evolution.First, the minimal region with full inhibitory potency was identified (CN19) by determining the effect of truncated peptides on CaMKII activity in biochemical assays. Then, individual residues of CN19 were mutated. Most individual Ala substitutions decreased potency of CaMKII inhibition, however, P3A, K13A, and R14A increased potency. Importantly, this initial Ala scan suggested a specific interaction of the region around R11 with the CaMKII substrate binding site, which was exploited for further rational mutagenesis to generate an optimized pseudo-substrate sequence. Indeed, the potency of the optimized peptide CN19o was >250fold improved (IC50 <0.4 nM), and CN19o has characteristics of a tight-binding inhibitor. The selectivity for CaMKII versus CaMKI was similarly improved (to almost 100,000fold for CN19o). A phospho-mimetic S12D mutation decreased potency, indicating potential for regulation by cellular signaling. Consistent with importance of this residue in inhibition, most other S12 mutations also significantly decreased potency, however, mutation to V or Q did not.These results provide improved research tools for studying CaMKII function, and indicate that evolution fine-tuned CaM-KIIN not for maximal potency of CaMKII inhibition, but for lower potency that may be optimal for dynamic regulation of signal transduction

Engineering of quantum dot photon sources via electro-elastic fields

The possibility to generate and manipulate non-classical light using the tools of mature semiconductor technology carries great promise for the implementation of quantum communication science. This is indeed one of the main driving forces behind ongoing research on the study of semiconductor quantum dots. Often referred to as artificial atoms, quantum dots can generate single and entangled photons on demand and, unlike their natural counterpart, can be easily integrated into well-established optoelectronic devices. However, the inherent random nature of the quantum dot growth processes results in a lack of control of their emission properties. This represents a major roadblock towards the exploitation of these quantum emitters in the foreseen applications. This chapter describes a novel class of quantum dot devices that uses the combined action of strain and electric fields to reshape the emission properties of single quantum dots. The resulting electro-elastic fields allow for control of emission and binding energies, charge states, and energy level splittings and are suitable to correct for the quantum dot structural asymmetries that usually prevent these semiconductor nanostructures from emitting polarization-entangled photons. Key experiments in this field are presented and future directions are discussed.Comment: to appear as a book chapter in a compilation "Engineering the Atom-Photon Interaction" published by Springer in 2015, edited by A. Predojevic and M. W. Mitchel