We use plasmon rulers to follow the conformational dynamics of a single protein for up to 24 h at a video rate. The plasmon ruler consists of two gold nanospheres connected by a single protein linker. In our experiment, we follow the dynamics of the molecular chaperone heat shock protein 90 (Hsp90), which is known to show “open” and “closed” conformations. Our measurements confirm the previously known conformational dynamics with transition times in the second to minute time scale and reveals new dynamics on the time scale of minutes to hours. Plasmon rulers thus extend the observation bandwidth 3–4 orders of magnitude with respect to single-molecule fluorescence resonance energy transfer and enable the study of molecular dynamics with unprecedented precision.
Incorporating metal nanocrystals with semiconductor photoanodes significantly enhances the efficiency of the energy conversion in the visible range during water splitting due to the excitation of hot electrons. While extensively studied on ensemble samples, hot electron response of metal nanocrystals in a photoelectrochemical cell remains unexploited at the single-particle level. Herein, we systematically investigate hot electron response of individual single-crystalline gold nanocrystals (AuNCs) on a TiO2 photoanode during water splitting. We directly correlate the morphology of the AuNC and its plasmonic property to the efficiencies involving hot electrons with the help of single-particle dark-field microscopy and photocurrent mapping. Our results show that the efficiencies of individual AuNCs are dependent on a variety of factors including interface condition, applied bias, excitation power, incident angle, and AuNC size. Our research may shed light on optimizing the light-harvesting capability of metal/semiconductor photoanodes by providing insights into the photocatalytic processes.
Plasmon sensors respond to local changes of their surrounding environment with a shift in their resonance wavelength. This response is usually detected by measuring light scattering spectra to determine the resonance wavelength. However, single wavelength detection has become increasingly important because it simplifies the setup, increases speed, and improves statistics. Therefore, we investigated theoretically how the sensitivity toward such single wavelength scattering intensity changes depend on the material and shape of the plasmonic sensor. Surprisingly, simple equations describe this intensity sensitivity very accurately and allow us to distinguish the various contributions: Rayleigh scattering, dielectric contrast, plasmon shift, and frequency-dependent plasmon bulk damping. We find very good agreement of theoretical predictions and experimental data obtained by single particle spectroscopy.
We present a study that allows us to explain the chemical changes behind the often observed but so far ununderstood drift of the plasmon resonance of chemically prepared gold nanorods in microfluidic devices. We systematically monitored the evolution of the plasmon scattering signal from thousands of single nanoparticles in parallel, from different gold nanorod batches, prepared by both, silver-assisted and silver-free seeded growth. By varying the experimental conditions, we confirmed the presence of a silver surface layer for nanorods prepared by the silver-assisted method. Although the silver layer is initially protected by the surfactant CTAB, it gets oxidized as soon as CTAB desorbs because of a reduced concentration in the flowing solution. We propose that these findings should be taken into account at the time of devising technological applications of gold nanorods, including the design of new nanorod synthetic routes, but in particular for applications that depend on the precise plasmon resonance position, for the plasmon sensing capabilities and to consider the nanoparticle surface reactivity.
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