JDFTx: Software for joint density-functional theory

Sundararaman, Ravishankar; Letchworth‐Weaver, Kendra; Schwarz, Kathleen; Gunceler, Deniz; Ozhabes, Yalcin; Arias, T. A.

doi:10.1016/j.softx.2017.10.006

Cited by 368 publications

(295 citation statements)

References 84 publications

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“…We calculate electronic states, phonons, optical and electron–phonon matrix elements, and transform them to a Wannier basis using the density functional theory software JDFTx57. We then calculate the carrier-energy-resolved imaginary dielectric function Imɛ( ω , E ) due to direct and phonon-assisted transitions and the energy-dependent carrier mean-free path λ ( E ) and the resulting scattered energy distribution P ( E | E ′) due to electron–electron and electron–phonon scattering, using Fermi's golden rule814.…”

Section: Methodsmentioning

confidence: 99%

Plasmonic hot electron transport drives nano-localized chemistry

et al. 2017

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Nanoscale localization of electromagnetic fields near metallic nanostructures underpins the fundamentals and applications of plasmonics. The unavoidable energy loss from plasmon decay, initially seen as a detriment, has now expanded the scope of plasmonic applications to exploit the generated hot carriers. However, quantitative understanding of the spatial localization of these hot carriers, akin to electromagnetic near-field maps, has been elusive. Here we spatially map hot-electron-driven reduction chemistry with 15 nm resolution as a function of time and electromagnetic field polarization for different plasmonic nanostructures. We combine experiments employing a six-electron photo-recycling process that modify the terminal group of a self-assembled monolayer on plasmonic silver nanoantennas, with theoretical predictions from first-principles calculations of non-equilibrium hot-carrier transport in these systems. The resulting localization of reactive regions, determined by hot-carrier transport from high-field regions, paves the way for improving efficiency in hot-carrier extraction science and nanoscale regio-selective surface chemistry.

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Section: Methodsmentioning

confidence: 99%

Plasmonic hot electron transport drives nano-localized chemistry

et al. 2017

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“…43 These calculations employ norm-conserving 6 pseudopotentials, a 30 Hartree kinetic energy cutoff on the plane-wave basis, and the PBEsol 44 generalized gradient approximation for the exchange-correlation functional, with a rotationally-invariant +U correction 45 for localized d electrons. All calculations are fully relativistic, accounting for spin-orbit effects self-consistently, which is essential for accurately reproducing the quasiparticle band structure in agreement with photoemission measurements.…”

Section: Methodsmentioning

confidence: 99%

Cubic Nonlinearity Driven Up-Conversion in High-Field Plasmonic Hot Carrier Systems

Narang¹,

Sundararaman²,

Jermyn

et al. 2016

J. Phys. Chem. C

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Surface plasmon resonances confine electromagnetic fields to the nanoscale, producing high field strengths suitable for exploiting nonlinear optical properties. We examine the prospect of detecting and utilizing one such property in plasmonic metals: the imaginary part of the cubic susceptibility, which corresponds to two plasmons decaying together to produce high energy carriers. Here we present ab initio predictions of the rates and carrier distributions generated by direct interband and phonon-assisted intraband transitions in one and two-plasmon decay. We propose detection of the higher energy carriers generated from two-plasmon decays that are inaccessible in one-plasmon decay as a viable signature of these processes in ultrafast experiments.

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“…Additionally, we use the plane-wave basis with a kinetic energy cutoff of 30 Hartrees, norm-conserving pseudopotentials, [36] and the 'PBE' generalized-gradient approximation to the exchange-correlation functional, [37] all as implemented in our open-source DFT software, JDFTx. [38] See ref. [25] for further computational and implementation details.…”

Section: Doi: 101002/adom201600914mentioning

confidence: 99%

Effects of Interlayer Coupling on Hot‐Carrier Dynamics in Graphene‐Derived van der Waals Heterostructures

Narang

Zhao

Claybrook

et al. 2017

Advanced Optical Materials

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CommuniCation(1 of 5) 1600914 2D materials exhibit a diverse array of optical and electronic properties, ranging from insulating hexagonal boron nitride and semiconducting transition metal dichalcogenides to semimetallic graphene. [1][2][3][4][5] Stacked 2D materials, or van der Waals (vdW) heterostructures, [6][7][8] have generated considerable recent interest as designer plasmonic, photonic, and optoelectronic materials. Combining 2D layers in different arrangements makes it possible to realize a variety of new optical phenomena and nanophotonic devices, covering spectral ranges from the microwave to the ultraviolet. [9][10][11] Simultaneously, the field of utilizing the energetic 'hot' carriers generated by surface plasmon decay for photodetection Graphene exhibits promise as a plasmonic material with high mode confinement that could enable efficient hot carrier extraction. The lifetimes and mean free paths of energetic carriers have been investigated in free-standing graphene, graphite, and a heterostructure consisting of alternating graphene and hexagonal boron nitride layers using ab initio calculations of electron-electron and electron-phonon scattering in these materials. It is found that the extremely high lifetimes (3 ps) of low-energy carriers near the Dirac point in graphene, which are a 100 times larger than that in noble metals, are reduced by an order of magnitude due to interlayer coupling in graphite, but enhanced in the heterostructure due to phonon mode clamping. However, these lifetimes drop precipitously with increasing carrier energy and are smaller than those in noble metals at energies exceeding 0.5 eV. By analyzing the contribution of different scattering mechanisms and interlayer interactions, desirable spacer layer characteristics-high dielectric constant and heavy atoms-that could pave the way for plasmonic heterostructures with improved hot carrier transport have been identified. and solar energy conversion has grown rapidly. [12][13][14] Hot carrier extraction has also been demonstrated in graphene, [15,16] with experimental techniques such as pump-probe spectroscopy [17] and 4D electron microscopy [18,19] used to explore the energy relaxation dynamics. [20,21] However, these techniques conventionally provide indirect signatures of the response of a large number of thermalizing carriers, [22] and extensive theoretical modeling is necessary to extract information about the sub-picosecond nonequilibrium carrier dynamics of interest. [23] With an ab initio framework for calculating optical response and electronphonon interactions, we previously evaluated mechanisms of hot carrier generation and relaxation in plasmonic metals, [24,25] and identified their signatures in ultrafast pump-probe measurements. [26,27] In particular, the small mean free paths of higher energy carriers helped elucidate the efficiency limits in plasmonic energy conversion devices and potential strategies to overcome them. [13] Here, we investigate the dynamics of hot carriers in graphene and in graphene-derived v...

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JDFTx: Software for joint density-functional theory

Cited by 368 publications

References 84 publications

Plasmonic hot electron transport drives nano-localized chemistry

Plasmonic hot electron transport drives nano-localized chemistry

Cubic Nonlinearity Driven Up-Conversion in High-Field Plasmonic Hot Carrier Systems

Effects of Interlayer Coupling on Hot‐Carrier Dynamics in Graphene‐Derived van der Waals Heterostructures

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