Origin of Plasmon Lineshape and Enhanced Hot Electron Generation in Metal Nanoparticles

You, Xinyuan; Ramakrishna, S.; Seideman, Tamar

doi:10.1021/acs.jpclett.7b03126

Cited by 15 publications

(16 citation statements)

References 43 publications

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“…For example, in Ag 55 cluster individual electronhole transitions couple strongly to plasmon, 38 which is often referred to as plasmon fragmentation. 43,44 Corre-spondingly, the time-domain response can exhibits occasional energy transfer back from the resonant transitions to the plasmon 32,45 (Supplementary Fig. 4) due to the incomplete Landau damping enabling the re-emergence of coherence between plasmonic transitions.…”

Section: Resultsmentioning

confidence: 99%

Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure

2020

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Metal nanoparticles are attractive for plasmon-enhanced generation of hot carriers, which may be harnessed in photochemical reactions. In this work, we analyze the coherent femtosecond dynamics of photon absorption, plasmon formation, and subsequent hot-carrier generation through plasmon dephasing using first-principles simulations. We predict the energetic and spatial hot-carrier distributions in small metal nanoparticles and show that the distribution of hot electrons is very sensitive to the local structure. Our results show that surface sites exhibit enhanced hot-electron generation in comparison to the bulk of the nanoparticle. Although the details of the distribution depend on particle size and shape, as a general trend, lower-coordinated surface sites such as corners, edges, and {100} facets exhibit a higher proportion of hot electrons than higher-coordinated surface sites such as {111} facets or the core sites. The present results thereby demonstrate how hot carriers could be tailored by careful design of atomic-scale structures in nanoscale systems.

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Section: Resultsmentioning

confidence: 99%

Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure

2020

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“…( 47)-( 51), the presence of numerous electrons, even in submicro-scale metallic structures, would make a feasibility of numerical calculations difficult. The approach based on the first-principles calculation 27,28 has more limited applications than the analytical approach based on our formulation. Note also that we can overcome this difficulty for several nanostructures, e.g., a 2D sheet (including graphene) and rectangular rod.…”

Section: Discussionmentioning

confidence: 99%

“…For the offresonant condition, a coherent Rabi oscillation between the plasmon and SPE was found. You et al also elucidated the bidirectional energy transfer between the plasmon and SPE based on a model Hamiltonian with the Coulomb interaction 28 , considering excited, injected, and extracted electrons.…”

Section: Introductionmentioning

confidence: 99%

“…In the present work, we focus on the fact that the coupling between plasmons and SPEs via the T field, as well as the treatment of the microscopic nonlocal response involving the T field, has been missed in the previous frameworks, which is particularly related with the latter case in the above discussion. Recent ab initio calculations successfully implemented coherent coupling or hybridization between plasmon-like and single-particle-like excitations [26][27][28][29][30][31][32] . In those studies, the Coulomb interaction corresponding to part of the induced L field was considered.…”

Section: Introductionmentioning

confidence: 99%

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Comprehensive Microscopic Theory for Coupling of Longitudinal--Transverse Fields and Individual--Collective Excitations

Yokoyama,

Iio,

Kinoshita

et al. 2021

Preprint

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A plasmon is a collective excitation of electrons due to the Coulomb interaction. Both plasmons and single-particle excitations (SPEs) are eigenstates of bulk metallic systems and they are orthogonal to each other. However, in non-translationally symmetric systems such as nanostructures, plasmons and SPEs coherently interact. It has been well discussed that the plasmons and SPEs, respectively, can couple with transverse (T) electric field in such systems, and also that they are coupled with each other via longitudinal (L) field. However, there has been a missing link in the previous studies: the coherent coupling between the plasmons and SPEs mediated by the T field. Herein, we develop a theoretical framework to describe the self-consistent relationship between plasmons and SPEs through both the L and T fields. The excitations are described in terms of the charge and current densities in a constitutive equation with a nonlocal susceptibility, where the densities include the L and T components. The electromagnetic fields originating from the densities are described in terms of the Green's function in the Maxwell equations. The T field is generated from both densities, whereas the L component is attributed to the charge density only. We introduce a four-vector representation incorporating the vector and scalar potentials in the Coulomb gauge, in which the T and L fields are separated explicitly. The eigenvalues of the matrix for the self-consistent equations appear as the poles of the system excitations. The developed formulation enables to approach unknown mechanisms for enhancement of the coherent coupling between plasmons and the hot carriers generated by radiative fields.

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“…There are four potential pathways by which excitation of LSPRs in a PMN enhances the catalytic performance of the surrounding catalytic component ( Figure ). [ 2–20,22–27,117–140 ] These pathways are 1) LSPR‐mediated indirect hot‐carrier transfer (HCT), 2) chemical interface damping (CID), 3) LSPR‐mediated energy‐transfer, and 4) heating of the medium surrounding the nanoparticle by thermal dissipation of excited charge carriers through electron‐phonon and phonon‐phonon scattering. The LSPR‐mediated energy‐transfer pathways include non‐radiative processes such as plasmon‐induced resonant energy transfer (PIRET) and radiative processes where scattered photons are reabsorbed by the surrounding medium (labeled as 3.2 in Figure 7).…”

Section: Lspr‐mediated Pathways Responsible For Photocatalytic Enhancement On Hpnsmentioning

confidence: 99%

Photoinduced Electron and Energy Transfer Pathways and Photocatalytic Mechanisms in Hybrid Plasmonic Photocatalysis

Ramakrishnan

Mohammadparast

Dadgar

et al. 2021

Advanced Optical Materials

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Hybrid plasmonic nanostructures are built on plasmonic metalnanostructures surrounded by catalytic metals or metal oxides. Recent studies have shown that hybrid plasmonic nanocatalysts can concurrently utilize thermal energy and photon stimuli and exhibit high catalytic activity, selectivity, and stability that are not attainable in conventional purely thermally activated catalytic processes. The hybrid plasmonic photocatalytic approach has recently emerged as an attractive concept for the conversion of solar energy into chemical energy, the distributed synthesis of valuable chemicals such as ammonia with little to no requirement of external heating, and the development of coke‐resistant and selective catalytic processes. The field of hybrid plasmonic photocatalysis has grown tremendously in the last decade. In this review article, the advantages of visible‐light‐augmented hybrid plasmonic photocatalysis over conventional pure thermally activated heterogeneous catalysis are discussed. Fundamental insights are provided into photocatalytic mechanisms by which the photoexcited charge carriers (electrons and holes) are formed and transferred to adsorbates triggering chemical transformations on the surface of hybrid plasmonic nanocatalysts. Computational modeling used for predicting and understanding the photocatalytic activity and selectivity on hybrid plasmonic nanostructures is also reviewed. The review closes with a discussion of the current challenges, new opportunities, and future outlook for hybrid plasmonic photocatalysis.

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Origin of Plasmon Lineshape and Enhanced Hot Electron Generation in Metal Nanoparticles

Cited by 15 publications

References 43 publications

Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure

Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure

Comprehensive Microscopic Theory for Coupling of Longitudinal--Transverse Fields and Individual--Collective Excitations

Photoinduced Electron and Energy Transfer Pathways and Photocatalytic Mechanisms in Hybrid Plasmonic Photocatalysis

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