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

Mingu Kang, Hyunwoo Kim, Elham Oleiki, Yeonjeong Koo, Hyeongwoo Lee, Huitae Joo, Jinseong Choi, Taeyong Eom, Geunsik Lee, Yung Doug Suh () and Kyoung-Duck Park ()
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Mingu Kang: Pohang University of Science and Technology (POSTECH)
Hyunwoo Kim: Korea Research Institute of Chemical Technology (KRICT)
Elham Oleiki: Ulsan National Institute of Science and Technology (UNIST)
Yeonjeong Koo: Pohang University of Science and Technology (POSTECH)
Hyeongwoo Lee: Pohang University of Science and Technology (POSTECH)
Huitae Joo: Ulsan National Institute of Science and Technology (UNIST)
Jinseong Choi: Ulsan National Institute of Science and Technology (UNIST)
Taeyong Eom: Korea Research Institute of Chemical Technology (KRICT)
Geunsik Lee: Ulsan National Institute of Science and Technology (UNIST)
Yung Doug Suh: Korea Research Institute of Chemical Technology (KRICT)
Kyoung-Duck Park: Pohang University of Science and Technology (POSTECH)

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract 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.

Date: 2022
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DOI: 10.1038/s41467-022-31576-x

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