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Register a new userScale-up of room-temperature constructive quantum interference from single molecules to self-assembled molecular-electronic films
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The realization of self-assembled molecular-electronic films, whose room-temperature transport properties are controlled by quantum interference (QI), is an essential step in the scale-up QI effects from single molecules to parallel arrays of molecules. Recently, the effect of destructive QI (DQI) on the electrical conductance of self-assembled monolayers (SAMs) has been investigated. Here, through a combined experimental and theoretical investigation, we demonstrate chemical control of different forms of constructive QI (CQI) in cross-plane transport through SAMs and assess its influence on cross-plane thermoelectricity in SAMs. It is known that the electrical conductance of single molecules can be controlled in a deterministic manner, by chemically varying their connectivity to external electrodes. Here, by employing synthetic methodologies to vary the connectivity of terminal anchor groups around aromatic anthracene cores, and by forming SAMs of the resulting molecules, we clearly demonstrate that this signature of CQI can be translated into SAM-on-gold molecular films. We show that the conductance of vertical molecular junctions formed from anthracene-based molecules with two different connectivities differ by a factor of approximately 16, in agreement with theoretical predictions for their conductance ratio based on constructive QI effects within the core. We also demonstrate that for molecules with thiol anchor groups, the Seebeck coefficient of such films is connectivity dependent and with an appropriate choice of connectivity can be boosted by ~50%. This demonstration of QI and its influence on thermoelectricity in SAMs represents a critical step towards functional ultra-thin-film devices for future thermoelectric and molecular-scale electronics applications.
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We studied the magnetic properties of self-assembled aggregates of BiFeO3 nanoparticles (~ 20-40 nm). The aggregates formed two different structures - one with limited and another with massive cross-linking - via `drying-mediated self-assembly process following dispersion of the nanoparticles within different organic solvents. They exhibit large coercivity H_C (>1000 Oe) and exchange bias field H_E (~ 350-900 Oe) in comparison to what is observed in isolated nanoparticles (H_C ~ 250 Oe; H_E ~ 0). The H_E turns out to be switching from negative to positive depending on the structure of the aggregates with |H_E| being larger. The magnetic force microscopy reveals the magnetic domains (extending across 7-10 nanoparticles) as well as the domain switching characteristics and corroborate the results of magnetic measurements. Numerical simulation of the `drying-mediated-self-assembly process shows that the nanoparticle-solvent interaction plays an important role in forming the `nanoparticle aggregate structures observed experimentally. Numerical simulation of the magnetic hysteresis loops, on the other hand, points out the importance of spin pinning at the surface of nanoparticles as a result of surface functionalization of the particles in different suspension media. Depending on the concentration of pinned spins at the surface pointing preferably along the easy-axis direction - from greater than 50% to less than 50% - H_E switches from negative to positive. Quite aside from bulk sample and isolated nanoparticle, nanoparticle aggregates - resulting from surface functionalization - therefore, offer remarkable tunability of properties depending on structures.
In the field of condensed matter, graphene plays a central role as an emerging material for nanoelectronics. Nevertheless, graphene is a semimetal, which constitutes a severe limitation for some future applications. Therefore, a lot of efforts are being made to develop semiconductor materials whose structure is compatible with the graphene lattice. In this perspective, little pieces of graphene represent a promising alternative. In particular, their electronic, optical and spin properties can be in principle controlled by designing their size, shape and edges. As an example, graphene nanoribbons with zigzag edges have localized spin polarized states. Likewise, singlet-triplet energy splitting can be chosen by designing the structure of graphene quantum dots. Moreover, bottom-up molecular synthesis put these potentialities at our fingertips. Here, we report on a single emitter study that directly addresses the intrinsic properties of a single graphene quantum dot. In particular, we show that graphene quantum dots emit single photons at room temperature with a high purity, a high brightness and a good photostability. These results pave the way to the development of new quantum systems based on these nanoscale pieces of graphene.
Multiferroic materials have driven significant research interest due to their promising technological potential. Developing new room-temperature multiferroics and understanding their fundamental properties are important to reveal unanticipated physical phenomena and potential applications. Here, a new room temperature multiferroic nanocomposite comprised of an ordered ferrimagnetic spinel LiFe5O8 (LFO) and a ferroelectric perovskite BiFeO3 (BFO) is presented. We observed that lithium (Li)-doping in BFO favors the formation of LFO spinel as a secondary phase during the synthesis of LixBi1-xFeO3 nanoceramics. Multimodal functional and chemical imaging methods are used to map the relationship between doping-induced phase separation and local ferroic properties in both the BFO-LFO composite ceramics and self-assembled nanocomposite thin films. The energetics of phase separation in Li doped BFO and the formation of BFO-LFO composites is supported by first principles calculations. These findings shed light on Li-ion role in the formation of a functionally important room temperature multiferroic and open a new approach in the synthesis of light element doped nanocomposites.
Self-assembled semiconductor quantum dot is a new type of artificially designed and grown function material which exhibits quantum size effect, quantum interference effect, surface effect, quantum tunneling-Coulumb-blockade effect and nonlinear optical effect. Due to advantages like less crystal defects and relatively simpler fabrication technology, that material may be of important value in future nanoelectronic device researches. In the order of vertical transport, lateral transport and charge storage, this paper gives a brief introduction of recent advances in the electronic properties of that material and an analysis of problems and perspectives.
We present a general analytical formula and an ab initio study of quantum interference in multi-branch molecules. Ab initio calculations are used to investigate quantum interference in a benzene-1,2-dithiolate (BDT) molecule sandwiched between gold electrodes and through oligoynes of various lengths. We show that when a point charge is located in the plane of a BDT molecule and its position varied, the electrical conductance exhibits a clear interference effect, whereas when the charge approaches a BDT molecule along a line normal to the plane of the molecule and passing through the centre of the phenyl ring, interference effects are negligible. In the case of olygoynes, quantum interference leads to the appearance of a critical energy $E_c$, at which the electron transmission coefficient $T(E)$ of chains with even or odd numbers of atoms is independent of length. To illustrate the underlying physics, we derive a general analytical formula for electron transport through multi-branch structures and demonstrate the versatility of the formula by comparing it with the above ab-initio simulations. We also employ the analytical formula to investigate the current inside the molecule and demonstrate that large counter currents can occur within a ring-like molecule such as BDT, when the point charge is located in the plane of the molecule. The formula can be used to describe quantum interference and Fano resonances in structures with branches containing arbitrary elastic scattering regions connected to nodal sites.
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