Conformational heterogeneity of molecules physisorbed on a gold surface at room temperature
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- Conformational heterogeneity of molecules physisorbed on a gold surface at room temperature
- Kang, Mingu; Kim, Hyun Woo; Oleiki, Elham; Koo, Yeonjeong; Lee, Hyeongwoo; Joo, Huitae; Choi, Jinseong; Eom, Taeyong; Lee, Geunsik; Suh, Yung Doug; Park, Kyoung-Duck
- Issue Date
- NATURE PORTFOLIO
- NATURE COMMUNICATIONS, v.13, no.1, pp.4133
- 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 Al2O3 capping layer, which suppresses spectral diffusions and inhibits chemical reactions and contamination 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. Tip-enhanced vibrational spectroscopy at room temperature is complicated by molecular conformational dynamics, photobleaching, contaminations, and chemical reactions in air. This study demonstrates that a sub-nm protective layer of Al2O3 provides robust conditions for probing single-molecule conformations.
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