Nonmelting Disordering Facilitated by Electron Delocalization

IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY ACS Nano Pub Date : 2025-02-26 DOI:10.1021/acsnano.5c00755
Dasol Kim, Sungwon Kim, Jisu Jung, Jaeseung Kim, Sungwook Choi, Carl-Friedrich Schön, Changwoo Lee, Hyeonwook Lim, Jaehun Jeong, Sanghyuck Yu, Yeonsu Jeong, Hanjoo Lee, Sangsoo Kim, Daewoong Nam, Intae Eom, Dogeun Jang, Kyung Sook Kim, Seongil Im, Seungwu Han, Hyunjung Kim, Mann-Ho Cho
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Abstract

Disordering atomic structures offers a functionality hardly expected in ordered states, including phase-change memory and photonic computing, offering the potential to renovate von Neumann architecture for neuromorphic engineering with low latency. However, significant energy consumption during the disordering compromises the data reliability and integration efficiency, which is traditionally regarded to take place after melting. Here, we investigate time for disordering in isochronal and isochoric manners, challenging the conventional melt-quenching theory. The disordering times of pure Sb, Ag–In–Sb–Te, and In surpass that of InSb by over 50 times, despite a higher melting point and a lower laser absorption rate of Sb compared to InSb. This nontrivial contrast is elucidated by theoretical calculation that delocalized electrons enable flexible modification of bond lengths even below the melting points where undermined bond directionality provides room for atoms to depart from their original positions. Facilitated by delocalized electrons, specifically through metavalent and metallic bonding rather than covalent bonding, atoms can be disordered without undergoing melting, which aligns with the rapid disordering of Sb compared to that of InSb. The results bridge the unaddressed gap between chemical interaction and kinetic behaviors during the disordering and suggest design rules highlighting electron-delocalization rather than solely relying on melting points to improve energy efficiency.

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电子离域促进的非熔化无序
无序原子结构提供了在有序状态下难以预料的功能,包括相变记忆和光子计算,为低延迟的神经形态工程提供了革新冯·诺伊曼结构的潜力。然而,在无序过程中,大量的能量消耗会影响数据的可靠性和集成效率,传统上认为这是在熔化之后发生的。在这里,我们以等时和等时的方式研究无序的时间,挑战传统的熔体淬火理论。纯Sb、Ag-In-Sb-Te和In的无序次数超过InSb的50倍以上,尽管Sb的熔点比InSb高,激光吸收率比InSb低。理论计算表明,离域电子甚至可以在熔点以下灵活地修改键长,在熔点以下,键的方向性被破坏,为原子离开其原始位置提供了空间。在离域电子的促进下,特别是通过元价键和金属键而不是共价键,原子可以在不熔化的情况下无序化,这与Sb相比InSb的快速无序化是一致的。研究结果弥合了无序过程中化学相互作用和动力学行为之间未解决的差距,并建议设计规则强调电子离域,而不是仅仅依靠熔点来提高能源效率。
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来源期刊
ACS Nano
ACS Nano 工程技术-材料科学:综合
CiteScore
26.00
自引率
4.10%
发文量
1627
审稿时长
1.7 months
期刊介绍: ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.
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