Huitae Joo | Searcharxiv

arXiv2025

Tip-enhanced quantum-sensing spectroscopy for bright and reconfigurable solid-state single-photon emitters

Atom-like defects in hexagonal boron nitride (hBN) provide room-temperature single-photon emission and coherent spin states, making them attractive for quantum-computing and -sensing applications. However, their random spatial and spectral characteristics hamper deterministic coupling with nano-optical cavities, limiting their use as bright single-photon sources and sensitive quantum sensors. Here, we present tip-enhanced quantum-sensing spectroscopy of single-photon emitters in hBN. Through precise spatial positioning of individual emitters within tip-cavities with different plasmon resonances, we adaptively control the enhancement rates of both excitation and emission, as well as the single-photon purity. In this way, optimal selection of their relative contributions can effectively reconfigure solid-state single-photon sources, with simultaneous nano-spectroscopic space- and time-resolved analyses. Furthermore, we demonstrate tip-enhanced quantum-sensing with single spin defects through optically detected magnetic resonance (ODMR) experiments in tip-coupled hBN nanoflakes. Our approach provides a unique pathway toward highly-sensitive and deterministic quantum-sensing with room-temperature single-photon emitters.

quant-ph↗

arXiv2022

Conformational heterogeneity of molecules physisorbed on a gold surface at room temperature

A quantitative single-molecule tip-enhanced Raman spectroscopy (TERS) study at room temperature remained a challenge due to the rapid structural dynamics of molecules exposed to air. Here, we demonstrate the hyperspectral TERS imaging of single or a few brilliant cresyl blue (BCB) molecules at room temperature, along with quantitative spectral analyses. Robust chemical imaging is enabled by the freeze-frame approach using a thin Al$_{2}$O$_{3}$ capping layer, which suppresses spectral diffusions and inhibits chemical reactions and contaminations in air. For the molecules resolved spatially in the TERS image, a clear Raman peak variation up to 7.5 cm$^{-1}$ is observed, which cannot be found in molecular ensembles. From density functional theory-based quantitative analyses of the varied TERS peaks, we reveal the conformational heterogeneity at the single-molecule level. This work provides a facile way to investigate the single-molecule properties in interacting media, expanding the scope of single-molecule vibrational spectroscopy studies.

physics.optics↗