The plasmon resonance of a structure is primarily dictated by its optical properties and geometry, which can be modified to enable hot-carrier photodetectors with superior performance. Recently, metal alloys have played a prominent role in tuning the resonance of plasmonic structures through chemical composition engineering. However, it has been unclear how alloying modifies the time dynamics of the generated hot-carriers. In this work, we elucidate the role of chemical composition on the relaxation time of hot-carriers for the archetypal AuxAg1−xthin film system. Through time-resolved optical spectroscopy measurements in the visible wavelength range, we measure composition-dependent relaxation times that vary up to 8× for constant pump fluency. Surprisingly, we find that the addition of 2% of Ag into Au films can increase the hot-carrier lifetime by approximately 35% under fixed fluence, as a result of a decrease in optical loss. Further, the relaxation time is found to be inversely proportional to the imaginary part of the permittivity. Our results indicate that alloying is a promising approach to effectively control hot-carrier relaxation time in metals.
Surface plasmon mediated hot-carrier generation is utilized widely for the manipulation of electron–photon interactions in many types of optoelectronic devices including solar cells, photodiodes, and optical modulators. A diversity of plasmonic systems such as nanoparticles, resonators, and waveguides has been introduced to enhance hot-carrier generation; however, the impact of propagating surface plasmons on hot-carrier lifetime has not been clearly demonstrated. Here, we systematically study the hot-carrier relaxation in thin film gold (Au) samples under surface plasmon coupling with the Kretschmann configuration. We observe that the locally confined electric field at the surface of the metal significantly affects the hot-carrier distribution and electron temperature, which results in a slowing of the hot electrons’ relaxation time, regardless of the average value of the absorbed power in the Au thin film. This result could be extended to other plasmonic nanostructures, enabling the control of hot-carrier lifetimes throughout the optical frequency range.
more » « less- NSF-PAR ID:
- 10156491
- Publisher / Repository:
- Optical Society of America
- Date Published:
- Journal Name:
- Optica
- Volume:
- 7
- Issue:
- 6
- ISSN:
- 2334-2536
- Page Range / eLocation ID:
- Article No. 608
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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