Tip-Enhanced Sum Frequency Generation for Molecular Vibrational Nanospectroscopy

Fuente: arXiv
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Autori principali: Sakurai, Atsunori, Takahashi, Shota, Mochizuki, Tatsuto, Sugimoto, Toshiki
Natura: Preprint
Pubblicazione: 2024
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author Sakurai, Atsunori
Takahashi, Shota
Mochizuki, Tatsuto
Sugimoto, Toshiki
author_facet Sakurai, Atsunori
Takahashi, Shota
Mochizuki, Tatsuto
Sugimoto, Toshiki
contents Vibrational sum frequency generation (SFG) is a nonlinear spectroscopic technique widely used to study the molecular structure and dynamics of surface systems. However, the spatial resolution achieved by far-field observations is constrained by the diffraction limit, obscuring molecular details in inhomogeneous structures smaller than the wavelength of light. To overcome this limitation, we developed a system for tip-enhanced SFG (TE-SFG) spectroscopy based on a scanning tunneling microscope. We successfully detected vibrational TE-SFG signals from adsorbed molecules on a gold substrate under ambient conditions. The phase analysis of interferometric SFG spectra provided information on molecular orientation. Furthermore, the observed TE-SFG signal was confirmed to originate from a highly localized region within a gap between the tip apex and the sample substrate. This method offers a novel platform for nonlinear optical nanospectroscopy, paving the way for the investigation of surface molecular systems beyond the diffraction limit.
format Preprint
id arxiv_https___arxiv_org_abs_2411_18909
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Tip-Enhanced Sum Frequency Generation for Molecular Vibrational Nanospectroscopy
Sakurai, Atsunori
Takahashi, Shota
Mochizuki, Tatsuto
Sugimoto, Toshiki
Optics
Mesoscale and Nanoscale Physics
Chemical Physics
Vibrational sum frequency generation (SFG) is a nonlinear spectroscopic technique widely used to study the molecular structure and dynamics of surface systems. However, the spatial resolution achieved by far-field observations is constrained by the diffraction limit, obscuring molecular details in inhomogeneous structures smaller than the wavelength of light. To overcome this limitation, we developed a system for tip-enhanced SFG (TE-SFG) spectroscopy based on a scanning tunneling microscope. We successfully detected vibrational TE-SFG signals from adsorbed molecules on a gold substrate under ambient conditions. The phase analysis of interferometric SFG spectra provided information on molecular orientation. Furthermore, the observed TE-SFG signal was confirmed to originate from a highly localized region within a gap between the tip apex and the sample substrate. This method offers a novel platform for nonlinear optical nanospectroscopy, paving the way for the investigation of surface molecular systems beyond the diffraction limit.
title Tip-Enhanced Sum Frequency Generation for Molecular Vibrational Nanospectroscopy
topic Optics
Mesoscale and Nanoscale Physics
Chemical Physics
url https://arxiv.org/abs/2411.18909