研究目的
Investigating the formation and stabilization of picocavities at room temperature to observe and control chemical reactions at the single-molecule level.
研究成果
The research demonstrates the accessibility of single-molecule chemistry under ambient conditions through the observation and characterization of single gold adatom movement using robust nano-assembled constructs. The study opens up new avenues for exploring the chemistry of metal?atom?molecular binding, which underpins catalysis and electrochemistry.
研究不足
The study notes that picocavities are less stable at room temperature compared to cryogenic temperatures, making them harder to exploit for demanding light?matter applications. The underlying mechanism for the improved stability of picocavities with NC-BPT is yet unclear.
1：Experimental Design and Method Selection:
The study utilizes nanoparticle-on-mirror (NPoM) constructs to create reliable nanocavities for light confinement. High-speed surface-enhanced Raman spectroscopy (SERS) is employed to observe picocavity formation and decay at room temperature.
2：Sample Selection and Data Sources:
Self-assembled monolayers (SAMs) of biphenyl-4-thiol (BPT) and 4′-cyanobiphenyl-4-thiol (NC-BPT) are used as spacer layers in NPoM constructs. Over 2 million SERS spectra are collected from these constructs.
3：List of Experimental Equipment and Materials:
Equipment includes a 633 nm HeNe laser, Olympus LMPlanPLN 100× NA0.8 objective lens, Andor Newton EMCCD, Andor Shamrock 303i-B spectrometer, and Thorlabs NF-633-25 notch filters.
4：8 objective lens, Andor Newton EMCCD, Andor Shamrock 303i-B spectrometer, and Thorlabs NF-633-25 notch filters.
Experimental Procedures and Operational Workflow:
4. Experimental Procedures and Operational Workflow: NPoM constructs are irradiated with laser light while continuously collecting Raman scattered light with reduced integration times to observe fast picocavity dynamics.
5：Data Analysis Methods:
The anti-Stokes to Stokes (AS/S) intensity ratio is used to calculate effective temperatures for optomechanically pumped vibrational modes, characterizing the excited-state population.
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