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تسجيل مستخدم جديدManifestation of the Verwey Transition in the Tunneling Spectra of Magnetite Nanocrystals
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Tunneling transport measurements performed on single particles and on arrays of Fe3O4 (magnetite) nanocrystals provide strong evidence for the existence of the Verwey metal-insulator transition at the nanoscale. The resistance measurements on nanocrystal arrays show an abrupt increase of the resistance around 100 K, consistent with the Verwey transition, while the current-voltage characteristics exhibit a sharp transition from an insulator gap to a peak structure around zero bias voltage. The tunneling spectra obtained on isolated particles using a Scanning Tunneling Microscope reveal an insulator-like gap structure in the density of states below the transition temperature that gradually disappeared with increasing temperature, transforming to a small peak structure at the Fermi energy. These data provide insight into the roles played by long- and short-range charge ordering in the Verwey transition.
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By combining {it ab initio} results for the electronic structure and phonon spectrum with the group theory, we establish the origin of the Verwey transition in Fe$_3$O$_4$. Two primary order parameters with $X_3$ and $Delta_5$ symmetries are identifi
ed. They induce the phase transformation from the high-temperature cubic to the low-temperature monoclinic structure. The on-site Coulomb interaction $U$ between 3d electrons at Fe ions plays a crucial role in this transition -- it amplifies the coupling of phonons to conduction electrons and thus opens a gap at the Fermi energy. {it Published in Phys. Rev. Lett. {bf 97}, 156402 (2006).}
We present infrared and Raman measurements of magnetite (Fe_3O_4). This material is known to undergo a metal-insulator and a structural transition (Verwey transition) at T_V=120K. At temperatures below T_V, we observe a strong gap-like suppression of
the optical conductivity below 1000 cm^-1. The structural aspect of the Verwey transition demonstrates itself by the appearance of additional infrared- and Raman-active phonons. The frequencies of the infrared-active phonons show no significant singularities at the transition whereas their linewidths increase. The frequency and linewidth of the Raman-active phonon at 670 cm^-1 changes abruptly at the transition. For T<T_V, we observe fine structures in the infrared and Raman spectra which may indicate strong anharmonicity of the system below the transition. Our estimate of the effective mass of the carriers above the transition to be about 100 m, where m is the free electron mass. Our measurements favor a polaronic mechanism of conductivity and underline the importance of the electron-phonon interaction in the mechanism of the Verwey transition.
Effects of the Verwey transition on the (100) surface of magnetite were studied using scanning tunelling microscopy and spin polarized low-energy electron microsccopy. On cooling through the transition temperature Tv, the initially flat surface under
goes a roof-like distortion with a periodicity of ~0.5 um due to ferroelastic twinning within monoclinic domains of the low-temperature monoclinic structure. The monoclinic c axis orients in the surface plane, along the [001]c directions. At the atomic scale, the charge-ordered sqrt2xsqrt2R45 reconstruction of the (100) surface is unperturbed by the bulk transition, and is continuous over the twin boundaries. Time resolved low-energy electron microscopy movies reveal the structural transition to be first-order at the surface, indicating that the bulk transition is not an extension of the Verwey-like sqrt2xsqrt2R45 reconstruction. Although conceptually similar, the charge-ordered phases of the (100) surface and sub-Tv bulk of magnetite are unrelated phenomena.
We incorporate single crystal Fe$_3$O$_4$ thin films into a gated device structure and demonstrate the ability to control the Verwey transition with static electric fields. The Verwey transition temperature ($T_V$) increases for both polarities of th
e electric field, indicating the effect is not driven by changes in carrier concentration. Energetics of induced electric polarization and/or strain within the Fe$_3$O$_4$ film provide a possible explanation for this behavior. Electric field control of the Verwey transition leads directly to a large magnetoelectric effect with coefficient of 585 pT m/V.
We have studied the electronic structure of bulk single crystals and epitaxial films of magnetite Fe$_3$O$_4$. Fe $2p$ core-level spectra show clear differences between hard x-ray (HAX-) and soft x-ray (SX-) photoemission spectroscopy (PES), indicati
ve of surface effects. The bulk-sensitive spectra exhibit temperature ($T$)-dependent charge excitations across the Verwey transition at $T_V$=122 K, which is missing in the surface-sensitive spectra. An extended impurity Anderson model full-multiplet analysis reveals roles of the three distinct Fe-species (A-Fe$^{3+}$, B-Fe$^{2+}$, B-Fe$^{3+}$) below $T_V$ for the Fe $2p$ spectra, and its $T-$dependent evolution. The Fe $2p$ HAXPES spectra show a clear magnetic circular dichroism (MCD) in the metallic phase of magnetized 100-nm-thick films. The model calculations also reproduce the MCD and identify the magnetically distinct sites associated with the charge excitations. Valence band HAXPES shows finite density of states at $E_F$ for the polaronic metal with remnant order above $T_V$, and a clear gap formation below $T_V$. The results indicate that the Verwey transition is driven by changes in the strongly correlated and magnetically active B-Fe$^{2+}$ and B-Fe$^{3+}$ electronic states, consistent with resistivity and bulk-sensitive optical spectra.
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