Tunneling diodes under environmental effects

We examine the robustness of single-molecule tunneling diodes to thermal-environmental effects. The diode comprises three fragments: two different conjugated chemical groups at the boundaries, and a saturated moiety in between, breaking conjugation. In this setup, molecular electronic levels localized on the conjugated groups independently shift with applied bias. While in the forward polarity a resonance condition is met, enhancing conductance, in the reversed direction molecular electronic states shift away from each other, resulting in small tunneling currents. In the absence of interactions with a thermal environment (consisting e.g. internal vibrations, solvent), rectification ratios reach three orders of magnitude. We introduce decoherence and inelastic-dissipative effects phenomenologically, by using the "voltage probe" approach. We find that when $\gamma_d \lesssim v$, with $\gamma_d$ the interaction energy of electrons with the environment and $v$ the tunneling energy across the saturated link, the diode is still highly effective, though rectification ratios are cut down by a factor of 2-4 compared to the coherent limit. To further enhance rectification ratios in molecular diodes we suggest a refined design involving four orbitals, with a pair of closely spaced states at each conjugated moiety

Intermediate coherent-incoherent charge transport: DNA as a case study

We study an intermediate quantum coherent-incoherent charge transport mechanism in metal-molecule-metal junctions using B\"uttiker's probe technique. This tool allows us to include incoherent effects in a controlled manner, and thus to study situations in which partial decoherence affects charge transfer dynamics. Motivated by recent experiments on intermediate coherent-incoherent charge conduction in DNA molecules [L. Xiang {\it et al.}, Nature Chem. 7, 221-226 (2015)], we focus on two representative structures: alternating (GC)$_n$ and stacked G$_n$C$_n$ sequences; the latter structure is argued to support charge delocalization within G segments, and thus an intermediate coherent-incoherent conduction. We begin our analysis with a highly simplified 1-dimensional tight-binding model, while introducing environmental effects through B\"uttiker's probes. This minimal model allows us to gain fundamental understanding of transport mechanisms and derive analytic results for molecular resistance in different limits. We then use a more detailed ladder-model Hamiltonian to represent double-stranded DNA structures---with environmental effects captured by B\"uttiker's probes. We find that hopping conduction dominates in alternating sequences, while in stacked sequences charge delocalization (visualized directly through the electronic density matrix) supports significant resonant-ballistic charge dynamics reflected by an even-odd effect and a weak distance dependence for resistance. Our analysis illustrates that lessons learned from minimal models are helpful for interpreting charge dynamics in DNA.Comment: 16 pages, 14 figure

Forming Stable Coalitions: The Process Matters

Players are assumed to rank each other as coalition partners. Two processes of coalition formation are defined and illustrated: i) Fallback (FB): Players seek coalition partners by descending lower and lower in their preference rankings until some majority coalition, all of whose members consider each other mutually acceptable, forms. ii) Build-up (BU):Same descent as FB, except only majorities whose members rank each other highest form coalitions. BU coalitions are stable in the sense that no member would prefer to be in another coalition, whereas FB coalitions, whose members need not rank each other highest, may not be stable. BU coalitions are bimodally distributed in a random society, with peaks around simple majority and unanimity the distributions of majorities in the US Supreme Count and in the US House of Representatives follow this pattern. The dynamics of real-life coalition-formation processes are illustrated by two Supreme Court cases.Coalition dynamics, Fallback bargaining, Manipulability, Legislatures, US Supreme Court

Forming Stable Coalitions: The Process Matters

Players are assumed to rank each other as coalition partners. Two processes of coalition formation are defined and illustrated: i) Fallback (FB): Players seek coalition partners by descending lower and lower in their preference rankings until some majority coalition, all of whose members consider each other mutually acceptable, forms. ii) Build-up (BU):Same descent as FB, except only majorities whose members rank each other highest form coalitions. BU coalitions are stable in the sense that no member would prefer to be in another coalition, whereas FB coalitions, whose members need not rank each other highest, may not be stable. BU coalitions are bimodally distributed in a random society, with peaks around simple majority and unanimity the distributions of majorities in the US Supreme Count and in the US House of Representatives follow this pattern. The dynamics of real-life coalition-formation processes are illustrated by two Supreme Court cases

Single-peakedness and disconnected coalitions

Ordinally single-peaked preferences are distinguished from cardinally single-peaked preferences, in which all players have a similar perception of distances in some one-dimensional ordering. While ordinal single-peakedness can lead to disconnected coalitions that have a "hole" in the ordering, cardinal single-peakedness precludes this possibility, based on two models of coalition formation:• Fallback (FB): Players seek coalition partners by descending lower and lower in their preference rankings until a majority coalition forms.• Build-Up (BU): Similar to FB, except that when nonmajority subcoalitions form, they fuse into composite players, whose positions are defined cardinally and who are treated as single players in the convergence process.FB better reflects the unconstrained, or nonmyopic, possibilities of coalition formation, whereas BU—because all subcoalition members must be included in any majority coalition that forms—restricts combinatorial possibilities and tends to produce less compact majority coalitions. Applications of the models to legislatures, parliamentary coalitions, and military alliances are discussed

Geometric Deep Learning for Molecular Crystal Structure Prediction

We develop and test new machine learning strategies for accelerating molecular crystal structure ranking and crystal property prediction using tools from geometric deep learning on molecular graphs. Leveraging developments in graph-based learning and the availability of large molecular crystal data sets, we train models for density prediction and stability ranking which are accurate, fast to evaluate, and applicable to molecules of widely varying size and composition. Our density prediction model, MolXtalNet-D, achieves state-of-the-art performance, with lower than 2% mean absolute error on a large and diverse test data set. Our crystal ranking tool, MolXtalNet-S, correctly discriminates experimental samples from synthetically generated fakes and is further validated through analysis of the submissions to the Cambridge Structural Database Blind Tests 5 and 6. Our new tools are computationally cheap and flexible enough to be deployed within an existing crystal structure prediction pipeline both to reduce the search space and score/filter crystal structure candidates