Understanding Charge Transfer in Donor-Acceptor/Metal Systems: A Combined Theoretical and Experimental Study

We develop an effective potential approach for assessing the flow of charge within a two-dimensional donor-acceptor/metal network based on core-level shifts. To do so, we perform both density functional theory (DFT) calculations and x-ray photoemission spectroscopy (XPS) measurements of the core-level shifts for three different monolayers adsorbed on a Ag substrate. Specifically, we consider perfluorinated pentacene (PFP), copper phthalocyanine (CuPc) and their 1:1 mixture (PFP+CuPc) adsorbed on Ag(111).Comment: 12 pages, 10 figure

Inversed linear dichroism in F <em>K</em>-edge NEXAFS spectra of fluorinated planar aromatic molecules

et al.The symmetry and energy distribution of unoccupied molecular orbitals is addressed in this work by means of NEXAFS and density functional theory calculations for planar, fluorinated organic semiconductors (perfluorinated copper phthalocyanines and perfluoropentacene). We demonstrate how molecular orbitals with significant density of states on the fluorine atoms show different symmetry from those mainly located on C and N atoms. As a result, the angle-dependent linear dichroism in NEXAFS F K-edge spectra is inversed with respect to that in the C and N K-edges. In addition, the significant overlap in energy of π * and σ * orbitals throughout the F K-edge spectrum hampers its use for analysis of molecular orientations from angle-dependent NEXAFS measurements. © 2012 American Physical Society.J.E.O. and A.R. acknowledge funding from the Spanish MEC through Grants No. FIS2011-65702-C02-01, No. MAT2010-21156-C03-01, and No. PIB2010US-00652, and from the Basque Government through Grants No. IT-257-07 and No. IT-319-07. A.R. additionally acknowledges that financial support was provided by ACI-Promociona Grant No. ACI2009-1036 and the European Research Council Advanced Grant DYNamo (ERC-2010-AdG, Proposal No. 267374). A.S. acknowledges the support of the Research Funds of the University of Helsinki and the Academy of Finland through Contract No. 1127462, Centers of Excellence Program, and the National Graduate School in Materials Physics. J.M.G.L. acknowledges support from The Lundbeck Foundation’s Center for Atomic-Scale Materials Design and the Danish Center for Scientific Computing.Peer Reviewe

Providing Green SLAs in High Performance Computing Clouds

Abstract—Demand for clean products and services is increasing as society is becoming increasingly aware of climate change. In response, many enterprises are setting explicit sustainability goals and implementing initiatives to reduce carbon emissions. Quantification and disclosure of such goals and initiatives have become important marketing tools. As enterprises and individuals shift their workloads to the cloud, this drive toward quantification and disclosure will lead to demand for quantifiable green cloud services. Thus, we argue that cloud providers should offer a new class of green services, in addition to existing (energy-sourceoblivious) services. This new class would provide clients with explicit service-level agreements (which we call Green SLAs) for the percentage of renewable energy used to run their workloads. In this paper, we first propose an approach for High Performance Computing cloud providers to offer such a Green SLA service. Specifically, each client job specifies a Green SLA, which is the minimum percentage of green energy that must be used to run the job. The provider earns a premium for meeting the Green SLA, but is penalized if it accepts the job but violates the Green SLA. We then propose (1) a power distribution and control infrastructure that uses a small amount of hardware to support Green SLAs, (2) an optimization-based framework for scheduling jobs and power sources that maximizes provider profits while respecting Green SLAs, and (3) two scheduling policies based on the framework. We evaluate our framework and policies extensively through simulations. Our main results show the tradeoffs between our policies, and their advantages over simpler greedy heuristics. We conclude that a Green SLA service that uses our policies would enable the provider to attract environmentally conscious clients, especially those who require strict guarantees on their use of green energy. I

Effect of surface reconstruction on the photoemission cross-section of the Au(111) surface state

The photoemission cross-section of the Shockley surface state of Au(111) is studied over a wide range of photon energies both experimentally and theoretically. The measurements are fully understood based on the theoretical analysis within a one-step abinitio theory of photoemission. The constant initial state spectrum is shown to be very sensitive to the structure of the topmost atomic layer. A maximum in the constant initial spectrum at 60eV is identified as a fingerprint of the Au(111) surface reconstruction. © 2012 IOP Publishing Ltd.This work was supported by the Spanish Ministerio de Ciencia e Innovación (Grants No. FIS2009-08355, FIS2010-19609-C02-02, MAT2010-21156-C03-01 and through the Research Program Ramón y Cajal) and the Basque Government (IT-257-07). The SRC is funded by the National Science Foundation (Award No. DMR-0084402).Peer Reviewe

Molecular-Level Realignment in Donor-Acceptor Bilayer Blends on Metals

Molecular bilayers made up of a donor-acceptor blend in contact with the metal and capped with a single-component layer show a tunable energy level alignment at both metal-organic and organic-organic interfaces. To ensure sharp heteromolecular interfaces, a contact layer is formed by a stable blend of pentacene (PEN) and perfluorinated copper phthalocyanine (F16CuPc) on Au(111) and Ag(111) and of perfluoropentacene (PFP) and copper phthalocyanine (CuPc) on Ag(111). Core-level and valence band photoemission reveal that, upon capping with pure F16CuPc, CuPc, and PEN, the electronic states of both contact and capping layers "realign" with respect to the monolayer and the multilayer references. The sign of the shift depends clearly on whether the capping layer is donor-like (PEN, CuPc) or acceptor-like (F16CuPc). As revealed by NEXAFS, the shift in electronic levels of the contact layer upon capping leads to a spectral density variation across the Fermi edge (EF); i.e., it induces molecule/metal charge transfer

A reliable power management scheme for consistent hashing based distributed key value storage systems

Distributed key value storage systems are among the most important types of distributed storage systems currently deployed in data centers. Nowadays, enterprise data centers are facing growing pressure in reducing their power consumption. In this paper, we propose GreenCHT, a reliable power management scheme for consistent hashing based distributed key value storage systems. It consists of a multi-tier replication scheme, a reliable distributed log store, and a predictive power mode scheduler (PMS). Instead of randomly placing replicas of each object on a number of nodes in the consistent hash ring, we arrange the replicas of objects on nonoverlapping tiers of nodes in the ring. This allows the system to fall in various power modes by powering down subsets of servers while not violating data availability. The predictive PMS predicts workloads and adapts to load fluctuation. It cooperates with the multi-tier replication strategy to provide power proportionality for the system. To ensure that the reliability of the system is maintained when replicas are powered down, we distribute the writes to standby replicas to active servers, which ensures failure tolerance of the system. GreenCHT is implemented based on Sheepdog, a distributed key value storage system that uses consistent hashing as an underlying distributed hash table. By replaying 12 typical real workload traces collected from Microsoft, the evaluation results show that GreenCHT can provide significant power savings while maintaining a desired performance. We observe that GreenCHT can reduce power consumption by up to 35%–61%

Asymmetric Response toward Molecular Fluorination in Binary Copper–Phthalocyanine/Pentacene Assemblies

We report a didactic and simple example of the subtleness in the balance of intermolecular and molecule-substrate interactions and its effect on molecular self-assembly. The study is performed on two closely related molecular blends of copper phthalocyanines and pentacene, in each of which one of the two molecules is fluorinated. Reversing the fluorination brings about changes in the intermolecular hydrogen bonds, as well as in the interactions with the substrate. As a result, on Au(100) substrates one blend assembles into a crystalline structure, whereas the other, displaying weaker intermolecular interactions and a larger corrugation in the molecule-substrate interaction potential, results in a disordered layer. However, the difference between the two blend's structures vanishes when substrates with less corrugated interaction potentials are used. © 2014 American Chemical Society.This work was supported by the Spanish Grant Nos. MAT2010-21156-C03- and PIB2010US-00652 and the Basque Government Grant No. IT-621-13. J.M.G.-L. acknowledges support from the Spanish Ministry of Economy and Competitiveness under projects FIS2012-30996 and FIS2010-21282-C02-01 and from the ReLiable project funded by the Danish Council for Strategic Research-Programme Commission on Sustainable Energy and Environment (project no. 11-116792).Peer Reviewe