Imaging material functionality through three-dimensional nanoscale tracking of energy flow

Imaging material functionality through three-dimensional nanoscale tracking of energy flow
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DOI:
10.1038/s41563-019-0498-x
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发表时间:
2020-01-01
期刊:
影响因子:
41.2
通讯作者:
Ginsberg, Naomi S.
Ginsberg, Naomi S.
中科院分区:
材料科学1区
文献类型:
--
作者:
Delor, Milan;Weaver, Hannah L.;Ginsberg, Naomi S.

文献摘要

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能量载体在原子和分子之间移动的能力是生化和材料功能的基础。然而,理解和控制能量流需要在超小和超快的时空尺度上进行观察,其中能量和结构障碍决定了能量载体的命运。在这里,我们开发了一种非侵入式光学方案,利用非共振干涉散射来跟踪能量载体产生的材料极化率的微小变化。因此,我们以几纳米的横向精度绘制了时空四个维度中不断变化的能量载体分布,并将它们与材料形态直接相关联。我们可视化多并苯、硅和钙钛矿半导体中的激子、电荷和热传输,并阐明无序如何影响三维能量流。例如,我们表明多晶金属卤化物钙钛矿的形态边界具有横向和深度依赖的电阻率,阻碍表面而不是体载流子的横向传输。我们还揭示了解释无序环境中能量传输的策略,这将指导未来半导体行业容错材料的设计。
The ability of energy carriers to move between atoms and molecules underlies biochemical and material function. Understanding and controlling energy flow, however, requires observing it on ultrasmall and ultrafast spatio-temporal scales, where energetic and structural roadblocks dictate the fate of energy carriers. Here, we developed a non-invasive optical scheme that leverages non-resonant interferometric scattering to track tiny changes in material polarizability created by energy carriers. We thus map evolving energy carrier distributions in four dimensions of spacetime with few-nanometre lateral precision and directly correlate them with material morphology. We visualize exciton, charge and heat transport in polyacene, silicon and perovskite semiconductors and elucidate how disorder affects energy flow in three dimensions. For example, we show that morphological boundaries in polycrystalline metal halide perovskites possess lateral- and depth-dependent resistivities, blocking lateral transport for surface but not bulk carriers. We also reveal strategies for interpreting energy transport in disordered environments that will direct the design of defect-tolerant materials for the semiconductor industry of tomorrow.