Experimental and ab initio ultrafast carrier dynamics in plasmonic nanoparticles
arXiv:1608.03309 · doi:10.1103/PhysRevLett.118.087401
Abstract
Ultrafast pump-probe measurements of plasmonic nanostructures probe the non-equilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions which allow us to avoid effective electron temperature approximations. Using this calculation method, we obtain excellent quantitative agreement with spectral and temporal features in transient-absorption measurements. In both our experiments and calculations, we identify the two major contributions of the initial response with distinct signatures: short-lived highly non-thermal excited carriers and longer-lived thermalizing carriers.
arXiv commentSupplementary information available as SI.pdf in source
References in corpus (4)
Cited by in corpus (32)
- JDFTx: software for joint density-functional theory
- Challenges in Plasmonic Catalysis
- Ultrafast Studies of Hot-Hole Dynamics in Au/p-GaN Heterostructures
- Hot Carrier Dynamics in Photoexcited Gold Nanostructures: Role of Interband Excitations and Evidence for Ballistic Transport
- Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure
- Hot carrier dynamics in plasmonic transition metal nitrides
- Transient optical symmetry breaking for ultrafast broadband dichroism in plasmonic metasurfaces
- Advances in ultrafast plasmonics
- Spin-phonon relaxation from a universal \emph{ab initio} density-matrix approach
- Microscopic Origins of Hydrodynamic Transport in Type-II Weyl Semimetal WP
- Transport of hot carriers in plasmonic nanostructures
- Effective electron temperature measurement using time-resolved anti-Stokes photoluminescence
- Parametric dependence of hot electron relaxation timescales on electron-electron and electron-phonon interaction strengths
- Tailoring hot-carrier distributions of plasmonic nanostructures through surface alloying
- Pump-probe Spectroscopy Study of Ultrafast Temperature Dynamics in Nanoporous Gold
- Ab initio Ultrafast Spin Dynamics in Solids
- Thermometric Calibration of the Ultrafast Relaxation Dynamics in Plasmonic Au Nanoparticles
- Plasmonics in Argentene
- Non-Equilibrium Phonon Transport Across Nanoscale Interfaces
- Non-Hermitian Hamiltonians for Linear and Nonlinear Optical Response: a Model for Plexcitons
- Quantum-mechanical effects in photoluminescence from thin crystalline gold films
- Time-resolved single-particle x-ray scattering reveals electron-density as coherent plasmonic-nanoparticle-oscillation source
- Electric fields and substrates dramatically accelerate spin relaxation in graphene
- Theory of Non-equilibrium "Hot" Carriers in Direct Band-gap Semiconductors Under Continuous Illumination
- Unified description of thermal and nonthermal hot carriers in plasmonic photocatalysis
- Machine Learning Models Capture Plasmon Dynamics in Ag Nanoparticles
- Excitation and Relaxation of Nonthermal Electron Energy Distributions in Metals with Application to Gold
- Ultrafast transport and relaxation of hot plasmonic electrons in metal-dielectric heterostructures
- Fermi surface anisotropy in plasmonic metals increases the potential for efficient hot carrier extraction
- Hot carrier dynamics in a dispersionless plasmonic system
- Quantum plasmons with optical-range frequencies in doped few-layer graphene
- Differentiating Contributions of Electrons and Phonons to the Thermoreflectance Spectra of Gold