TY - JOUR
T1 - Theory of “Hot” Photoluminescence from Drude Metals
AU - Sivan, Yonatan
AU - Dubi, Yonatan
N1 - Funding Information:
Y.S. was supported by Israel Science Foundation (ISF) grant (340/20) and MWK Niedersachsen funded project no. 76251-99-7/20 (ZN 3637). The authors would like to acknowledge many useful conversations with I.W. Un, M. Caldarola, and M. Orrit.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/4/27
Y1 - 2021/4/27
N2 - We provide a complete quantitative theory for light emission from Drude metals under continuous wave illumination, based on our recently derived steady-state nonequilibrium electron distribution. We show that the electronic contribution to the emission exhibits a dependence on the emission frequency which is very similar to the energy dependence of the nonequilibrium distribution, and characterize different scenarios determining the measurable emission line shape. This enables the identification of experimentally relevant situations, where the emission lineshapes deviate significantly from predictions based on the standard theory (namely, on the photonic density of states), and enables the differentiation between cases where the emission scales with the metal object surface or with its volume. We also provide an analytic description (which is absent from the literature) of the (polynomial) dependence of the metal emission on the electric field, its dependence on the pump laser frequency, and its nontrivial exponential dependence on the electron temperature, both for the Stokes and anti-Stokes regimes. Our results imply that the emission does not originate from either Fermion statistics (due to e-e interactions), and even though one could have expected the emission to follow boson statistics due to involvement of photons (as in Planck's Black Body emission), it turns out that it deviates from that form as well. Finally, we resolve the arguments associated with the effects of electron and lattice temperatures on the emission, and which of them can be extracted from the anti-Stokes emission.
AB - We provide a complete quantitative theory for light emission from Drude metals under continuous wave illumination, based on our recently derived steady-state nonequilibrium electron distribution. We show that the electronic contribution to the emission exhibits a dependence on the emission frequency which is very similar to the energy dependence of the nonequilibrium distribution, and characterize different scenarios determining the measurable emission line shape. This enables the identification of experimentally relevant situations, where the emission lineshapes deviate significantly from predictions based on the standard theory (namely, on the photonic density of states), and enables the differentiation between cases where the emission scales with the metal object surface or with its volume. We also provide an analytic description (which is absent from the literature) of the (polynomial) dependence of the metal emission on the electric field, its dependence on the pump laser frequency, and its nontrivial exponential dependence on the electron temperature, both for the Stokes and anti-Stokes regimes. Our results imply that the emission does not originate from either Fermion statistics (due to e-e interactions), and even though one could have expected the emission to follow boson statistics due to involvement of photons (as in Planck's Black Body emission), it turns out that it deviates from that form as well. Finally, we resolve the arguments associated with the effects of electron and lattice temperatures on the emission, and which of them can be extracted from the anti-Stokes emission.
KW - "Hot" photoluminescence
KW - non-thermal electrons
KW - plasmonics
UR - http://www.scopus.com/inward/record.url?scp=85106513068&partnerID=8YFLogxK
U2 - 10.1021/acsnano.1c00835
DO - 10.1021/acsnano.1c00835
M3 - Article
C2 - 33904296
SN - 1936-0851
VL - 15
SP - 8724
EP - 8732
JO - ACS Nano
JF - ACS Nano
IS - 5
ER -