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1.
Phys Rev Lett ; 132(13): 133602, 2024 Mar 29.
Article in English | MEDLINE | ID: mdl-38613288

ABSTRACT

A levitated nanomechanical oscillator under ultrahigh vacuum is highly isolated from its environment. It has been predicted that this isolation leads to very low mechanical dissipation rates. However, a gap persists between predictions and experimental data. Here, we levitate a silica nanoparticle in a linear Paul trap at room temperature, at pressures as low as 7×10^{-11} mbar. We measure a dissipation rate of 2π×69(22) nHz, corresponding to a quality factor exceeding 10^{10}, more than 2 orders of magnitude higher than previously shown. A study of the pressure dependence of the particle's damping and heating rates provides insight into the relevant dissipation mechanisms.

2.
Phys Rev Lett ; 130(10): 106204, 2023 Mar 10.
Article in English | MEDLINE | ID: mdl-36962055

ABSTRACT

Single-molecule electron sources of fullerenes driven via constant electric fields, approximately 1 nm in size, produce peculiar emission patterns, such as a cross or a two-leaf pattern. By illuminating the electron sources with femtosecond light pulses, we discovered that largely modulated emission patterns appeared from single molecules. Our simulations revealed that emission patterns, which have been an intractable question for over seven decades, represent single-molecule molecular orbitals. Furthermore, the observed modulations originated from variations of single-molecule molecular orbitals, practically achieving the subnanometric optical modulation of an electron source.

3.
Sci Rep ; 12(1): 2714, 2022 Feb 17.
Article in English | MEDLINE | ID: mdl-35177727

ABSTRACT

Applying strong direct current (DC) electric fields on the apex of a sharp metallic tip, electrons can be radially emitted from the apex to vacuum. Subsequently, they magnify the nanoscopic information on the apex, which serves as a field emission microscope (FEM). When depositing molecules on such a tip, peculiar electron emission patterns such as clover leaves appear. These phenomena were first observed seventy years ago. However, the source of these emission patterns has not yet been identified owing to the limited experimental information about molecular configurations on a tip. Here, we used fullerene molecules and characterized the molecule-covered tip by an FEM. In addition to the experiments, simulations were performed to obtain optimized molecular configurations on a tip. Both results indicate that the molecules, the source of the peculiar emission patterns, appear on a molecule layer formed on the tip under strong DC electric fields. Furthermore, the simulations revealed that these molecules are mostly isolated single molecules forming single-molecule-terminated protrusions. Upon the excellent agreements in both results, we concluded that each emission pattern originates from a single molecule. Our work should pave the way to revive old-fashioned electron microscopy as a powerful tool for investigating a single molecule.

4.
ACS Nano ; 15(2): 2458-2467, 2021 Feb 23.
Article in English | MEDLINE | ID: mdl-32941001

ABSTRACT

Several fields of applications require a reliable characterization of the photothermal response and heat dissipation of nanoscopic systems, which remains a challenging task for both modeling and experimental measurements. Here, we present an implementation of anti-Stokes thermometry that enables the in situ photothermal characterization of individual nanoparticles (NPs) from a single hyperspectral photoluminescence confocal image. The method is label-free, potentially applicable to any NP with detectable anti-Stokes emission, and does not require any prior information about the NP itself or the surrounding media. With it, we first studied the photothermal response of spherical gold NPs of different sizes on glass substrates, immersed in water, and found that heat dissipation is mainly dominated by the water for NPs larger than 50 nm. Then, the role of the substrate was studied by comparing the photothermal response of 80 nm gold NPs on glass with sapphire and graphene, two materials with high thermal conductivity. For a given irradiance level, the NPs reach temperatures 18% lower on sapphire and 24% higher on graphene than on bare glass. The fact that the presence of a highly conductive material such as graphene leads to a poorer thermal dissipation demonstrates that interfacial thermal resistances play a very significant role in nanoscopic systems and emphasize the need for in situ experimental thermometry techniques. The developed method will allow addressing several open questions about the role of temperature in plasmon-assisted applications, especially ones where NPs of arbitrary shapes are present in complex matrixes and environments.

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