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Register a new userMesoscopic order and the dimentionality of long-range resonance energy transfer in supramolecular semiconductors
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We present time-resolved photoluminescence measurements on two series of oligo-p-phenylenevinylene materials that self-assemble into supramolecular nanostructures with thermotropic reversibility in dodecane. One set of derivatives form chiral, helical stacks while the second set form less organised, frustrated stacks. Here we study the effects of supramolecular organisation on the resonance energy transfer rates. We measure these rates in nanoassemblies formed with mixed blends of oligomers and compare them with the rates predicted by Foerster theory. Our results and analysis show that control of supramolecular order in the nanometre lengthscale has a dominant effect on the efficiency and dimentionality of resonance energy transfer.
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Electronic and optical properties of doped organic semiconductors are dominated by local interactions between donor and acceptor molecules. However, when such systems are in crystalline form, long-range order competes against short-range couplings. In a first-principles study on three experimentally resolved bulk structures of quaterthiophene doped by (fluorinated) tetracyanoquinodimethane, we demonstrate the crucial role of long-range interactions in donor/acceptor co-crystals. The band structures of the investigated materials exhibit direct band-gaps decreasing in size with increasing amount of F atoms in the acceptors. The valence-band maximum and conduction-band minimum are found at the Brillouin zone boundary and the corresponding wave-functions are segregated on donor and acceptor molecules, respectively. With the aid of a tight-binding model, we rationalize that the mechanisms responsible for these behaviors, which are ubiquitous in donor/acceptor co-crystals, are driven by long-range interactions. The optical response of the analyzed co-crystals is highly anisotropic. The absorption onset is dominated by an intense resonance corresponding to a charge-transfer excitation. Long-range interactions are again responsible for this behavior, which enhances the efficiency of the co-crystals for photo-induced charge separation and transport. In addition to this result, which has important implications in the rational design of organic materials for opto-electronics, our study clarifies that cluster models, accounting only for local interactions, cannot capture the relevant impact of long-range order in donor/acceptor co-crystals.
We propose a method for nano-scale characterization of long range magnetic order in diluted magnetic systems to clarify the origins of the room temperature ferromagnetism. The GaN:Mn thin films are grown by metal-organic chemical vapor deposition with the concentration of Ga-substitutional Mn up to 3.8%. Atomic force microscope (AFM) and magnetic force microscope (MFM) characterizations are performed on etched artificial microstructures and natural dislocation pits. Numerical simulations and theoretical analysis on the AFM and MFM data have confirmed the formation of long range magnetic order and ruled out the possibility that nano-clusters contributed to the ferromagnetism. We suggest that delocalized electrons might play a role in the establishment of this long range magnetic order.
The nature of the unconventional ordered phase occurring in CeRu2Al10 below T0 = 27 K was investigated by neutron scattering. Powder diffraction patterns show clear superstructure peaks corresponding to forbidden (h + k)-odd reflections of the Cmcm space group. Inelastic neutron scattering experiments further reveal a pronounced magnetic excitation developing in the ordered phase at an energy of 8 meV.
We present a comprehensive study on the magnetic structure, dynamics, and phase evolution in the single-phase double perovskite $La_2CoMnO_6$. The mixed valence state due to oxygen deficiency is verified by X-ray photoelectron spectroscopy, and confirms a double ferromagnetic transition observed in DC magnetization. Neutron diffraction reveals that the magnetic structure is dominated by long-range ferromagnetic ordering, which is further corroborated by a critical exponents analysis of the paramagnetic to ferromagnetic phase transition. An analysis of the magnetization dynamics by means of linear and nonlinear ac magnetic susceptibilities marks the presence of two distinct cluster glass-like states that emerge at low temperatures. The isothermal entropy change as a function of temperature and magnetic field (H) is exploited to investigate the mechanism of stabilization of the magnetic phases across the H-T phase diagram. In the regime of the phase diagram where thermal energy is sufficiently low, regions of competing interactions due to local disorder become stabilized and display glass-like dynamics. The freezing mechanism of clusters is illustrated using a unique probe of transverse susceptibility that isolates the effects of the local anisotropy of the spin clusters. The results are summarized in a new H-T phase diagram of $La_2CoMnO_6$ revealed for the first time from these data.
Ultracold atom magnetic field microscopy enables the probing of current flow patterns in planar structures with unprecedented sensitivity. In polycrystalline metal (gold) films we observe long-range correlations forming organized patterns oriented at +/- 45 deg relative to the mean current flow, even at room temperature and at length scales orders of magnitude larger than the diffusion length or the grain size. The preference to form patterns at these angles is a direct consequence of universal scattering properties at defects. The observed amplitude of the current direction fluctuations scales inversely to that expected from the relative thickness variations, the grain size and the defect concentration, all determined independently by standard methods. This indicates that ultracold atom magnetometry enables new insight into the interplay between disorder and transport.
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