Assessing Effects of Near-Field Synergistic Light Absorption on Ordered Inorganic Phototropic Growth

Assessing Effects of Near-Field Synergistic Light Absorption on Ordered Inorganic Phototropic Growth
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评估近场协同光吸收对有序无机向光性生长的影响

DOI:
10.1021/jacs.0c13085
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发表时间:
2021
影响因子:
15
通讯作者:
Lewis, Nathan S.
Lewis, Nathan S.
中科院分区:
化学1区
文献类型:
--
作者:
Carim, Azhar I.;Meier, Madeline C.;Kennedy, Kathleen M.;Richter, Matthias H.;Hamann, Kathryn R.;Lewis, Nathan S.

文献摘要

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我们在此报告,光学近场中的协同光吸收能够在无机向光性生长过程中实现纳米级自组织。 Se-Te 在几何受限的波长尺度区域中,在不相干、非结构光源的照射下以电化学方式生长。尽管尺寸有限,在单个亚微米尺寸中产生的离散特征少至两个,但沉积物形态表现出明确的有序性和各向异性。对模拟结构中光吸收的计算机建模分析揭示了一种协同作用,其中纳米级特征中的光捕获通过附加相邻特征的存在而得到增强,并且协同效应主要源自最近邻贡献。此外,建模表明,协同吸收是通过单个纳米级特征对入射照明的散射产生的,导致近场强度的局部增加,从而增加邻近特征的吸收。这些光学过程之间的相互作用为通过无机向光性生长自发有序产生奠定了基础。
We report herein that synergistic light absorption in the optical near-field enables nanoscale self-organization during inorganic phototropic growth. Se–Te was grown electrochemically under illumination from an incoherent, unstructured light source in geometrically constrained, wavelength scale areas. Despite the limited dimensions, with as few as two discrete features produced in a single sub-micron dimension, the deposit morphology exhibited defined order and anisotropy. Computer modeling analysis of light absorption in simulated structures revealed a synergy wherein light capture in a nanoscale feature was enhanced by the presence of additional adjacent features, with the synergistic effect originating predominantly from nearest neighbor contributions. Modeling moreover indicated that synergistic absorption is produced by scattering of the incident illumination by individual nanoscale features, leading to a local increase in the near-field intensity and consequently increasing the absorption in neighboring features. The interplay between these optical processes establishes the basis for spontaneous order generation via inorganic phototropic growth.