Dynamic upconversion multicolour editing enabled by molecule-assisted opto-electrochemical modulation

Yiming Wu,Xiaogang Liu,Xian Qin,Jiahui Xu,Jun Xu

doi:10.1038/s41467-021-22387-7

Abstract

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.

Highlights

Controlling nonlinear optical signals electrically offers many opportunities for technological developments
Temporal modulation of upconversion emission can be realised by varying excitation wavelengths or by adjusting excitation power densities[15,16,17,18,19]
Dynamic modulation of upconversion emission colour and intensity can be achieved with molecular-assisted surface electrochemical tuning (MASET) (Fig. 1a)

Summary

Introduction

Controlling nonlinear optical signals electrically offers many opportunities for technological developments. 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. Nonlinear photonic devices capable of detecting and modulating infrared signals as a communication medium are essential for technological developments in thermography, night vision, medical diagnosis, information encryption, and optical communication[1,2,3,4,5,6] Such optoelectronic applications can be accomplished by using nonlinear nanocrystals that enable frequency conversion of invisible infrared radiation to visible luminescence. A recovery of upconversion emission can be rapidly achieved through a reversible redox reaction under a reverse electric field (Fig. 1b)

Methods

Results

Conclusion