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Abstract Above‐equilibrium “hot”‐carrier generation in metals is a promising route to convert photons into electrical charge for efficient near‐infrared optoelectronics. However, metals that offer both hot‐carrier generation in the near‐infrared and sufficient carrier lifetimes remain elusive. Alloys can offer emergent properties and new design strategies compared to pure metals. Here, it is shown that a noble‐transition alloy, AuxPd1−x, outperforms its constituent metals concerning generation and lifetime of hot carriers when excited in the near‐infrared. At optical fiber wavelengths (e.g., 1550 nm), Au50Pd50provides a 20‐fold increase in the number of ≈0.8 eV hot holes, compared to Au, and a threefold increase in the carrier lifetime, compared to Pd. The discovery that noble‐transition alloys can excel at hot‐carrier generation reveals a new material platform for near‐infrared optoelectronic devices.
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Emergent properties from CuPd alloy films under near-infrared excitation
Noble-transition metal alloys offer emergent optical and electronic properties for near-infrared (NIR) optoelectronic devices. We investigate the optical and electronic properties of CuxPd1−x alloy thin films and their ultrafast electron dynamics under NIR excitation. Ultraviolet photoelectron spectroscopy measurements supported by density functional theory calculations show strong d-band hybridization between the Cu 3d and Pd 4d bands. These hybridization effects result in emergent optical properties, most apparent in the dilute Pd case. Time-resolved terahertz spectroscopy with NIR (e.g., 1550 nm) excitation displays composition-tunable electron dynamics. We posit that the negative peak in the normalized increment of transmissivity (ΔT/T) below 2 ps from dilute Pd alloys is due to non-thermalized hot-carrier generation. On the other hand, Pd-rich alloys exhibit an increase in ΔT/T due to thermalization effects upon ultrafast NIR photoexcitation. CuxPd1−x alloys in the dilute Pd regime may be a promising material for future ultrafast NIR optoelectronic devices.
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- Award ID(s):
- 2114312
- PAR ID:
- 10440308
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 157
- Issue:
- 17
- ISSN:
- 0021-9606
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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