Department of Chemistry, National University of Singapore, Singapore, Singapore.
Center for Functional Materials, National University of Singapore Suzhou Research Institute, Suzhou, China.
Nat Commun. 2021 Apr 1;12(1):2022. doi: 10.1038/s41467-021-22387-7.
Controlling nonlinear optical signals electrically offers many opportunities for technological developments. Lanthanide-activated nanoparticles have recently emerged as leading platforms for nonlinear upconversion of infra-red excitation within nanometric volumes. However, manipulation of upconversion emission is restricted to varying percentages of component materials, nanocrystal structure, and optical pumping conditions. Here, we report temporal modulation of anti-Stokes luminescence by coupling upconversion nanoparticles with an electrochemically responsive molecule. By electrically tailoring orbital energy levels of the molecules anchored on nanoparticle surfaces, we demonstrate reversible control of molecular absorption, resulting in dynamic colour editing of anti-Stokes luminescence at single-particle resolution. Moreover, we show that a programmable logic gate array based on opto-electrochemical modulation can be constructed to convert information-encrypted electrical signals into visible patterns with millisecond photonic readout. These findings offer insights into precise control of anti-Stokes luminescence, while enabling a host of applications from low-threshold infrared logic switches to multichannel, high-fidelity photonic circuits.
电控制非线性光学信号为技术发展提供了许多机会。镧系激活纳米粒子最近成为在纳米体积内红外激发的非线性上转换的主要平台。然而，上转换发射的操纵仅限于改变组分材料、纳米晶体结构和光学泵浦条件的百分比。在这里，我们报告了通过将上转换纳米粒子与电响应分子耦合来对反斯托克斯发光进行时间调制。通过电修饰锚定在纳米粒子表面的分子的轨道能级，我们证明了分子吸收的可逆控制，从而以单粒子分辨率动态编辑反斯托克斯发光的颜色。此外，我们表明，可以构建基于光电化学调制的可编程逻辑门阵列，将信息加密的电信号转换为具有毫秒级光子读出的可见图案。这些发现为精确控制反斯托克斯发光提供了思路，同时为从低阈值红外逻辑开关到多通道、高保真光子电路的各种应用铺平了道路。
