Real-time monitoring of fast gas dynamics with a single-molecule resolution by frequency-comb-referenced plasmonic phase spectroscopy

1.
Department of Mechanical Engineering, Korea Advanced Institute of Science and Technology (KAIST), Science Town, Daejeon, 34141, South Korea
2.
Department of Mechatronic Engineering, Faculty of Mechanical Engineering, Ho Chi Minh City University of Technology (HCMUT), Vietnam National University, Ho Chi Minh City, Vietnam
3.
Department of Cogno-Mechatronics Engineering, College of Nanoscience and Nanotechnology, Pusan National University, Busan, 46241, South Korea
4.
Department of Optics and Mechatronics Engineering, College of Nanoscience and Nanotechnology, Pusan National University, Busan, 46241, South Korea
5.
School of Mechanical and Aerospace Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore, 639798, Singapore
6.
, 156, Gajeongbuk-Ro, Yuseong-Gu, Daejeon, 34103, South Korea

Funds: This work was supported by the National Research Foundation of the Republic of Korea (NRF-2019K1A3A1A20092429, NRF-2020R1A2C2102338, NRF-2022M1A3C2069728 and RS-2024-00401786), and the Basic Research Program (NK236C) funded by the Korea Institute of Machinery and Materials (KIMM). This work was also supported by the KAIST UP Program and the Commercializations Promotion Agency for R&D Outcomes (COMPA) under grant RS-2023-00260002 and the Ministry of Small and Medium-sized Enterprises (SMEs) and Startups under grant RCMS-S3207602. We acknowledge the support of time and facilities from Ho Chi Minh City University of Technology (HCMUT), Viet Nam National University Ho Chi Minh City (VNU-HCM)

摘要

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Abstract: Surface plasmon resonance (SPR) sensors are based on photon-excited surface charge density oscillations confined at metal-dielectric interfaces, which makes them highly sensitive to biological or chemical molecular bindings to functional metallic surfaces. Metal nanostructures further concentrate surface plasmons into a smaller area than the diffraction limit, thus strengthening photon-sample interactions. However, plasmonic sensors based on intensity detection provide limited resolution with long acquisition time owing to their high vulnerability to environmental and instrumental noises. Here, we demonstrate fast and precise detection of noble gas dynamics at single molecular resolution via frequency-comb-referenced plasmonic phase spectroscopy. The photon-sample interaction was enhanced by a factor of 3,852 than the physical sample thickness owing to plasmon resonance and thermophoresis-assisted optical confinement effects. By utilizing a sharp plasmonic phase slope and a high heterodyne information carrier, a small atomic-density modulation was clearly resolved at 5 Hz with a resolution of 0.06 Ar atoms per nano-hole (in 10^–11 RIU) in Allan deviation at 0.2 s; a faster motion up to 200 Hz was clearly resolved. This fast and precise sensing technique can enable the in-depth analysis of fast fluid dynamics with the utmost resolution for a better understanding of biomedical, chemical, and physical events and interactions.

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