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arXiv · 2506.15095

Nano-resolved sensing of 3D electromagnetic fields via single emitters' extreme variation of enhanced spontaneous emission

R. Margoth Córdova-Castro·Dirk Jonker·Clément Cabriel·Mario Zapata-Herrera·Bart van Dam·Yannick De Wilde·Robert W. Boyd·Arturo Susarrey-Arce·Ignacio Izeddin·Valentina Krachmalnicoff
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Abstract

Controlling quantum light-matter interactions at scales smaller than the diffraction limit at the single quantum emitter level is a critical challenge to the goal of advancing quantum technologies. We introduce a novel material platform that enables precise engineering of spontaneous emission changes in molecular single emitters through 3D nanofields. This platform is based on a 3D hollow plasmonic nanomaterial arranged in a square lattice, uniformly scalable to the centimeter scale while maintaining unit cell geometry. This coupled system leads to billions of Purcell-enhanced single emitters integrated into a nanodevice. Using far-field single-molecule super-resolution microscopy, we investigate emission modifications at the single-emitter level, enabling molecular position sensing with resolution surpassing the diffraction limit. By combining the nanolocalization with time correlation single photon counting, we probe molecule per molecule enhanced quantum light-matter interactions. This 3D plasmonic geometry significantly enhances light-matter interactions, revealing a broad range of lifetimes -- from nanoseconds to picoseconds -- significantly increasing the local density of states in a manner that depends on both molecular position and dipole orientation, offering extreme position sensitivity within the 3D electromagnetic landscape. By leveraging these plasmonic nanostructures and our method for measuring single-molecule Purcell-enhanced nano-resolved maps, we enable fine-tuned control of light-matter interactions. This approach enables the on-demand control of fast single-photon sources at room temperature, providing a powerful tool for molecular sensing and quantum applications at the single-emitter level.

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R. Margoth Córdova-Castro, Dirk Jonker, Clément Cabriel, Mario Zapata-Herrera, Bart van Dam, Yannick De Wilde, Robert W. Boyd, Arturo Susarrey-Arce, Ignacio Izeddin, Valentina Krachmalnicoff. 2025-06-18. Nano-resolved sensing of 3D electromagnetic fields via single emitters' extreme variation of enhanced spontaneous emission. https://arxiv.org/abs/2506.15095

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