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Register a new userQuantifying the interplay between fine structure and geometry of an individual molecule on a surface
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Added by
Alexander Khajetoorians
Publication date
2020
fields
Physics
and research's language is
English
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The pathway toward the tailored synthesis of materials starts with precise characterization of the conformational properties and dynamics of individual molecules. Electron spin resonance based scanning tunneling microscopy can potentially address molecular structure with unprecedented resolution. Here, we determine the fine structure and geometry of an individual TiH molecule, utilizing a combination of a newly developed mK ESR-STM in a vector magnetic field and ab initio approaches. We demonstrate a strikingly large anisotropy of the g-tensor unusual for a spin doublet ground state, resulting from a non-trivial orbital angular momentum stemming from the molecular ground state. We quantify the relationship between the resultant fine structure, hindered rotational modes, and orbital excitations. Our model system provides new avenues to determine the structure and dynamics of individual molecules.
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We demonstrate that nanocavity plasmons generated a few nanometers away from a molecule can induce molecular motion. For this, we study the well-known rapid shuttling motion of zinc phthalocyanine molecules adsorbed on ultrathin NaCl films by combining scanning tunneling microscopy (STM) and spectroscopy (STS) with STM-induced light emission. Comparing spatially resolved single-molecule luminescence spectra from molecules anchored to a step edge with isolated molecules adsorbed on the free surface, we found that the azimuthal modulation of the Lamb shift is diminished in case of the latter. This is evidence that the rapid shuttling motion is remotely induced by plasmon-exciton coupling. Plasmon-induced molecular motion may open an interesting playground to bridge the nanoscopic and mesoscopic worlds by combining molecular machines with nanoplasmonics to control directed motion of single molecules without the need for local probes.
We study the interplay between the effects of surface anisotropy and dipolar interactions in monodisperse assemblies of nanomagnets with oriented anisotropy. We derive asymptotic formulas for the assembly magnetization taking account of temperature, applied field, core and surface anisotropy, and dipolar inter-particle interactions. We find that the interplay between surface anisotropy and dipolar interactions is well described by the analytical expression of the assembly magnetization derived here: the overall sign of the product of the two parameters governing the surface and the dipolar contributions determines whether intrinsic and collective terms compete or have synergistic effects on the magnetization. This is illustrated by the magnetization curves of $gamma-Fe_{2}O_{3}$ nanoparticles assemblies in the low concentration limit.
Transistors, regardless of their size, rely on electrical gates to control the conductance between source and drain contacts. In atomic-scale transistors, this conductance is exquisitely sensitive to single electrons hopping via individual orbitals. Single-electron transport in molecular transistors has been previously studied using top-down approaches to gating, such as lithography and break junctions. But atomically precise control of the gate - which is crucial to transistor action at the smallest size scales - is not possible with these approaches. Here, we used individual charged atoms, manipulated by a scanning tunnelling microscope, to create the electrical gates for a single-molecule transistor. This degree of control allowed us to tune the molecule into the regime of sequential single-electron tunnelling, albeit with a conductance gap more than one order of magnitude larger than observed previously. This unexpected behaviour arises from the existence of two different orientational conformations of the molecule, depending on its charge state. Our results show that strong coupling between these charge and conformational degrees of freedom leads to new behaviour beyond the established picture of single-electron transport in atomic-scale transistors.
A molecular wire containing an emitting molecular center is controllably suspended between the plasmonic electrodes of a cryogenic scanning tunneling microscope. Passing current through this circuit generates an ultra narrow-line emission at an energy of ? 1.5 eV which is assigned to the fluorescence of the molecular center. Control over the linewidth is obtained by progressively detaching the emitting unit from the surface. The recorded spectra also reveal several vibronic peaks of low intensities that can be viewed as a fingerprint of the emitter. Surface-plasmon localized at the tip-sample interface are shown to play a major role on both excitation and emission of the molecular excitons.
Peoples interests and peoples social relationships are intuitively connected, but understanding their interplay and whether they can help predict each other has remained an open question. We examine the interface of two decisive structures forming the backbone of online social media: the graph structure of social networks - who connects with whom - and the set structure of topical affiliations - who is interested in what. In studying this interface, we identify key relationships whereby each of these structures can be understood in terms of the other. The context for our analysis is Twitter, a complex social network of both follower relationships and communication relationships. On Twitter, hashtags are used to label conversation topics, and we examine hashtag usage alongside these social structures. We find that the hashtags that users adopt can predict their social relationships, and also that the social relationships between the initial adopters of a hashtag can predict the future popularity of that hashtag. By studying weighted social relationships, we observe that while strong reciprocated ties are the easiest to predict from hashtag structure, they are also much less useful than weak directed ties for predicting hashtag popularity. Importantly, we show that computationally simple structural determinants can provide remarkable performance in both tasks. While our analyses focus on Twitter, we view our findings as broadly applicable to topical affiliations and social relationships in a host of diverse contexts, including the movies people watch, the brands people like, or the locations people frequent.
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