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1.
Entropy (Basel) ; 26(6)2024 Jun 05.
Artículo en Inglés | MEDLINE | ID: mdl-38920501

RESUMEN

Recent theoretical investigations have revealed unconventional transport mechanisms within high Brillouin zones of two-dimensional superlattices. Electrons can navigate along channels we call superwires, gently guided without brute force confinement. Such dynamical confinement is caused by weak superlattice deflections, markedly different from the static or energetic confinement observed in traditional wave guides or one-dimensional electron wires. The quantum properties of superwires give rise to elastic dynamical tunneling, linking disjoint regions of the corresponding classical phase space, and enabling the emergence of several parallel channels. This paper provides the underlying theory and mechanisms that facilitate dynamical tunneling assisted by chaos in periodic lattices. Moreover, we show that the mechanism of dynamical tunneling can be effectively conceptualized through the lens of a paraxial approximation. Our results further reveal that superwires predominantly exist within flat bands, emerging from eigenstates that represent linear combinations of conventional degenerate Bloch states. Finally, we quantify tunneling rates across various lattice configurations and demonstrate that tunneling can be suppressed in a controlled fashion, illustrating potential implications in future nanodevices.

2.
Phys Rev Lett ; 132(18): 186303, 2024 May 03.
Artículo en Inglés | MEDLINE | ID: mdl-38759174

RESUMEN

Quantum acoustics-a recently developed framework parallel to quantum optics-establishes a nonperturbative and coherent treatment of the electron-phonon interaction in real space. The quantum-acoustical representation reveals a displaced Drude peak hiding in plain sight within the venerable Fröhlich model: the optical conductivity exhibits a finite frequency maximum in the far-infrared range and the dc conductivity is suppressed. Our results elucidate the origin of the high-temperature absorption peaks in strange or bad metals, revealing that dynamical lattice disorder steers the system towards a non-Drude behavior.

3.
Nature ; 623(7989): 949-955, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-38030777

RESUMEN

Pyridinium electrolytes are promising candidates for flow-battery-based energy storage1-4. However, the mechanisms underlying both their charge-discharge processes and overall cycling stability remain poorly understood. Here we probe the redox behaviour of pyridinium electrolytes under representative flow battery conditions, offering insights into air tolerance of batteries containing these electrolytes while providing a universal physico-chemical descriptor of their reversibility. Leveraging a synthetic library of extended bispyridinium compounds, we track their performance over a wide range of potentials and identify the singlet-triplet free energy gap as a descriptor that successfully predicts the onset of previously unidentified capacity fade mechanisms. Using coupled operando nuclear magnetic resonance and electron paramagnetic resonance spectroscopies5,6, we explain the redox behaviour of these electrolytes and determine the presence of two distinct regimes (narrow and wide energy gaps) of electrochemical performance. In both regimes, we tie capacity fade to the formation of free radical species, and further show that π-dimerization plays a decisive role in suppressing reactivity between these radicals and trace impurities such as dissolved oxygen. Our findings stand in direct contrast to prevailing views surrounding the role of π-dimers in redox flow batteries1,4,7-11 and enable us to efficiently mitigate capacity fade from oxygen even on prolonged (days) exposure to air. These insights pave the way to new electrolyte systems, in which reactivity of reduced species is controlled by their propensity for intra- and intermolecular pairing of free radicals, enabling operation in air.

4.
Proc Natl Acad Sci U S A ; 118(40)2021 10 05.
Artículo en Inglés | MEDLINE | ID: mdl-34580232

RESUMEN

We report unexpected classical and quantum dynamics of a wave propagating in a periodic potential in high Brillouin zones. Branched flow appears at wavelengths shorter than the typical length scale of the ordered periodic structure and for energies above the potential barrier. The strongest branches remain stable indefinitely and may create linear dynamical channels, wherein waves are not confined directly by potential walls as electrons in ordinary wires but rather, indirectly and more subtly by dynamical stability. We term these superwires since they are associated with a superlattice.

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