skip to main content


Title: Widely Varying Kondo and Magnetic Interactions in Molecule Gold Nanostructured Materials by Changing the Gold Nanoarchitecture
Delocalized−localized electron interactions are central to strongly correlated electron phenomena. Here, we study the Kondo effect, a prototypical strongly correlated phenomena, in a tunable fashion using gold nanostructures (nanoparticle, NP, and nanoshell, NS) + molecule cross-linkers (butanedithiol, BDT). NP films exhibit hallmark signatures of the Kondo effect, including (1) a log temperature resistance upturn as temperature decreases in a metallic regime, and (2) zero-bias conductance peaks (ZBCPs) that are well fit by a Frota function near a percolation insulator transition, previously used to model Kondo peaks observed using tunnel junctions. Remarkably, NP + NS films exhibit ZBCPs that persist to >220 K, i.e., >10-fold higher than that in NP films. Magnetic measurements reveal that moments in NP powders align, and in NS powders, they antialign at low temperatures. Based on these observations, we propose a mechanism in which varying such material nanobuilding blocks can modify electron−electron interactions to such a large degree.  more » « less
Award ID(s):
1719875
NSF-PAR ID:
10411992
Author(s) / Creator(s):
; ; ; ;
Date Published:
Journal Name:
Nano Letters
ISSN:
1530-6984
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. null (Ed.)
    Topology and strong electron correlations are crucial ingredients in emerging quantum materials, yet their intersection in experimental systems has been relatively limited to date. Strongly correlated Weyl semimetals, particularly when magnetism is incorporated, offer a unique and fertile platform to explore emergent phenomena in novel topological matter and topological spintronics. The antiferromagnetic Weyl semimetal Mn 3 Sn exhibits many exotic physical properties such as a large spontaneous Hall effect and has recently attracted intense interest. In this work, we report synthesis of epitaxial Mn 3+ x Sn 1− x films with greatly extended compositional range in comparison with that of bulk samples. As Sn atoms are replaced by magnetic Mn atoms, the Kondo effect, which is a celebrated example of strong correlations, emerges, develops coherence, and induces a hybridization energy gap. The magnetic doping and gap opening lead to rich extraordinary properties, as exemplified by the prominent DC Hall effects and resonance-enhanced terahertz Faraday rotation. 
    more » « less
  2. Abstract

    Strongly correlated electronic systems exhibit a wealth of unconventional behavior stemming from strong electron-electron interactions. The LaAlO3/SrTiO3(LAO/STO) heterostructure supports rich and varied low-temperature transport characteristics including low-density superconductivity, and electron pairing without superconductivity for which the microscopic origins is still not understood. LAO/STO also exhibits inexplicable signatures of electronic nematicity via nonlinear and anomalous Hall effects. Nanoscale control over the conductivity of the LAO/STO interface enables mesoscopic experiments that can probe these effects and address their microscopic origins. Here we report a direct correlation between electron pairing without superconductivity, anomalous Hall effect and electronic nematicity in quasi-1D ballistic nanoscale LAO/STO Hall crosses. The characteristic magnetic field at which the Hall coefficient changes directly coincides with the depairing of non-superconducting pairs showing a strong correlation between the two distinct phenomena. Angle-dependent Hall measurements further reveal an onset of electronic nematicity that again coincides with the electron pairing transition, unveiling a rotational symmetry breaking due to the transition from paired to unpaired phases at the interface. The results presented here highlights the influence of preformed electron pairs on the transport properties of LAO/STO and provide evidence of the elusive pairing “glue” that gives rise to electron pairing in SrTiO3-based systems.

     
    more » « less
  3. Abstract

    2D materials exhibit strong excitonic effects due to low dimensionality and enhanced Coulomb interactions, resulting in fascinating many‐particle phenomena like excitons. Though perovskite is a classical type of material hosting abundant correlated electronic phases, freestanding 2D perovskite oxides are not easy to fabricate and yet to be extensively studied. Here the realization of large size (1 × 1 cm2) freestanding perovskite SrTiO3films, which show unexpected excitonic photoluminescence (PL) spectra and carrier dynamics, is reported. Two pronounced broad PL peaks emerge in 2D freestanding SrTiO3films at 2.34–2.4 and 1.8–1.9 eV, of which the 2.34–2.4 eV emission originates from self‐trapped excitons localized within TiO6octahedra, and the 1.8–1.9 eV peak from Ti vacancies. The time‐resolved PL shows a remarkable enhancement of nonradiative Auger recombination through three‐particle process, in which electron–hole excitons transfer their kinetic energy to other free electrons or holes. The results demonstrate unique excitonic properties in 2D perovskite SrTiO3films and unravel their potential for high‐performance optoelectronic devices.

     
    more » « less
  4. The observation of quantum criticality in diverse classes of strongly correlated electron systems has been instrumental in establishing ordering principles, discovering new phases, and identifying the relevant degrees of freedom and interactions. At focus so far have been insulators and metals. Semimetals, which are of great current interest as candidate phases with nontrivial topology, are much less explored in experiments. Here, we study the Kondo semimetal CeRu 4 Sn 6 by magnetic susceptibility, specific heat, and inelastic neutron scattering experiments. The power-law divergence of the magnetic Grünesien ratio reveals that, unexpectedly, this compound is quantum critical without tuning. The dynamical energy over temperature scaling in the neutron response throughout the Brillouin zone and the temperature dependence of the static uniform susceptibility, indicate that temperature is the only energy scale in the criticality. Such behavior, which has been associated with Kondo destruction quantum criticality in metallic systems, could be generic in the semimetal setting. 
    more » « less
  5. Abstract Magnetic transition metal chalcogenides form an emerging platform for exploring spin-orbit driven Berry phase phenomena owing to the nontrivial interplay between topology and magnetism. Here we show that the anomalous Hall effect in pristine Cr 2 Te 3 thin films manifests a unique temperature-dependent sign reversal at nonzero magnetization, resulting from the momentum-space Berry curvature as established by first-principles simulations. The sign change is strain tunable, enabled by the sharp and well-defined substrate/film interface in the quasi-two-dimensional Cr 2 Te 3 epitaxial films, revealed by scanning transmission electron microscopy and depth-sensitive polarized neutron reflectometry. This Berry phase effect further introduces hump-shaped Hall peaks in pristine Cr 2 Te 3 near the coercive field during the magnetization switching process, owing to the presence of strain-modulated magnetic layers/domains. The versatile interface tunability of Berry curvature in Cr 2 Te 3 thin films offers new opportunities for topological electronics. 
    more » « less