Potential for exciton condensation in a highly conductive amorphous polymer

Potential for exciton condensation in a highly conductive amorphous polymer
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高导电性无定形聚合物中激子凝聚的潜力

DOI:
10.1103/physrevmaterials.7.045001
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发表时间:
2023
影响因子:
3.4
通讯作者:
Mazziotti, David A.
Mazziotti, David A.
中科院分区:
材料科学3区
文献类型:
--
作者:
Schouten, Anna O.;Klevens, Jordan E.;Sager-Smith, LeeAnn M.;Xie, Jiaze;Anderson, John S.;Mazziotti, David A.

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在合成和理论上的一个突出的挑战是开发在环境条件下表现出高效能量转移的分子材料。在这里,我们证明了最近合成的,高导电性的非晶材料-镍四硫富瓦烯-四硫醇(NiTTFtt)聚合物-成为激子凝聚物-玻色-爱因斯坦凝聚的粒子-空穴对,称为激子,支持无耗散流的激发能量的潜力。虽然激子凝聚体最近已经实现了有序的材料,我们表明,先进的电子结构计算,这种高度相关的现象可以实现在分子量身定制的,无定形材料。在相反的Bechgaard盐,支持超导性在压缩的几何形状,需要高压,我们表明,最近合成的,无定形NiTTFtt聚合物表现出激子凝聚在实验上可实现的几何形状,在环境压力下发生的计算签名。结果表明,在这个系统和相关系统的超流性,包括货车德瓦尔斯结构,分子金属与扩展TTF二硫代配体,和Bechgaard盐,可能会发生通过一个非传统的激子机制可调根据系统的组成,几何形状,尺寸和电荷。这项研究提示进一步的实验研究的合理设计的分子尺度激子凝聚体与潜在的应用,以有效的传输技术相关的材料。
An outstanding challenge in synthesis and theory is to develop molecular materials at ambient conditions that exhibit highly efficient energy transfer. Here we demonstrate the potential of a recently synthesized, highly conductive amorphous material—a nickel tetrathiafulvalene-tetrathiolate (NiTTFtt) polymer—to become an exciton condensate—a Bose-Einstein condensate of particle-hole pairs, known as excitons, that supports dissipationless flow of excitation energy. While exciton condensates have recently been realized in ordered materials, we show by advanced electronic structure calculations that this highly correlated phenomenon can potentially be realized in molecularly tailored, amorphous materials. In contrast to the Bechgaard salts that support superconductivity at compressed geometries requiring high pressures, we show that the recently synthesized, amorphous NiTTFtt polymer exhibits the computational signature of exciton condensation at experimentally realizable geometries, occurring at ambient pressures. Results suggest that superfluidity in this system and related systems—including van der Waals structures, molecular metals with extended-TTF dithiolate ligands, and Bechgaard salts—may occur via a nontraditional excitonic mechanism tuneable according to system composition, geometry, size, and charge. This study prompts further experimental investigation of the rational design of molecularly scaled exciton condensates with potential applications to efficient transport in technologically relevant materials.
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