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Band gap maps beyond the delocalization limit: correlation between optical band gaps and plasmon energies at the nanoscale.

ABSTRACT: Recent progresses in nanoscale semiconductor technology have heightened the need for measurements of band gaps with high spatial resolution. Band gap mapping can be performed through a combination of probe-corrected scanning transmission electron microscopy (STEM) and monochromated electron energy-loss spectroscopy (EELS), but are rare owing to the complexity of the experiments and the data analysis. Furthermore, although this method is far superior in terms of spatial resolution to any other techniques, it is still fundamentally resolution-limited due to inelastic delocalization of the EELS signal. In this work we have established a quantitative correlation between optical band gaps and plasmon energies using the Zn1-xCd x O/ZnO system as an example, thereby side-stepping the fundamental resolution limits of band gap measurements, and providing a simple and convenient approach to achieve band gap maps with unprecedented spatial resolution.

SUBMITTER: Zhan W

PROVIDER: S-EPMC5770386 | biostudies-other | 2018 Jan

REPOSITORIES: biostudies-other

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Band gap maps beyond the delocalization limit: correlation between optical band gaps and plasmon energies at the nanoscale.

Zhan Wei W Venkatachalapathy Vishnukanthan V Aarholt Thomas T Kuznetsov Andrej Yu AY Prytz Øystein Ø

Scientific reports 20180116 1

Recent progresses in nanoscale semiconductor technology have heightened the need for measurements of band gaps with high spatial resolution. Band gap mapping can be performed through a combination of probe-corrected scanning transmission electron microscopy (STEM) and monochromated electron energy-loss spectroscopy (EELS), but are rare owing to the complexity of the experiments and the data analysis. Furthermore, although this method is far superior in terms of spatial resolution to any other te ...[more]

PMID: 29339788

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Project description:We describe the electronic structure and the origin of ferromagnetic exchange coupling in two new metal complexes, NN-SQ-Co(III)(py)(2)Cat-NN (1) and NN-Ph-SQ-Co(III)(py)(2)Cat-Ph-NN (2) (NN = nitronylnitroxide radical, Ph = 1,4-phenylene, SQ = S = (1)/(2) semiquinone radical, Cat = S = 0 catecholate, and py = pyridine). Near-IR electronic absorption spectroscopy for 1 and 2 reveals a low-energy optical band that has been assigned as a Psi(u) --> Psi(g) transition involving bonding and antibonding linear combinations of delocalized dioxolene (SQ/Cat) valence frontier molecular orbitals. The ferromagnetic exchange interaction in 1 is so strong that only the high-spin quartet state (S(T) = (3)/(2)) is thermally populated at temperatures up to 300 K. The temperature-dependent magnetic susceptibility data for 2 reveals that an excited state spin doublet (S(T) = (1)/(2)) is populated at higher temperatures, indicating that the phenylene spacer modulates the magnitude of the magnetic exchange. The valence delocalization within the dioxolene dyad of 2 results in ferromagnetic alignment of two localized NN radicals separated by over 22 A. The ferromagnetic exchange in 1 and 2 results from a spin-dependent delocalization (double exchange type) process and the origin of this strong electron correlation has been understood in terms of a valence bond configuration interaction (VBCI) model. We show that ferromagnetic coupling promoted by organic mixed-valency provides keen insight into the ability of single molecules to communicate spin information over nanoscale distances. Furthermore, the strong interaction between the itinerant dioxolene electron and localized NN electron spins impacts our ability to understand the exchange interaction between delocalized electrons and pinned magnetic impurities in technologically important dilute magnetic semiconductor materials. The long correlation length (22 A) of the itinerant electron that mediates this coupling indicates that high-spin pi-delocalized organic molecules could find applications as nanoscale spin-polarized electron injectors and molecular wires.

Dataset Information

Band gap maps beyond the delocalization limit: correlation between optical band gaps and plasmon energies at the nanoscale.

Publications

Band gap maps beyond the delocalization limit: correlation between optical band gaps and plasmon energies at the nanoscale.

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