arXiv subjects

Nien-En Lee

Publications and source records attributed to Nien-En Lee.

6 recordsLinked to original sources

arXiv2022

Intermediate Polaronic Charge Transport in Organic Crystals from a Many-Body First-Principles Approach

Predicting the electrical properties of organic molecular crystals (OMCs) is challenging due to their complex crystal structures and electron-phonon (e-ph) interactions. Charge transport in OMCs is conventionally categorized into two limiting regimes $-$ band transport, characterized by weak e-ph interactions, and charge hopping due to localized polarons formed by strong e-ph interactions. However, between these two limiting cases there is a less well understood intermediate regime where polarons are present but transport does not occur via hopping. Here we show a many-body first-principles approach that can accurately predict the carrier mobility in OMCs in the intermediate regime and shed light on its microscopic origin. Our approach combines a finite-temperature cumulant method to describe strong e-ph interactions with Green-Kubo transport calculations. We apply this parameter-free framework to naphthalene crystal, demonstrating electron mobility predictions within a factor of 1.5$-$2 of experiment between 100$-$300 K. Our analysis reveals that electrons couple strongly with both inter- and intramolecular phonons in the intermediate regime, as evidenced by the formation of a broad polaron satellite peak in the electron spectral function and the failure of the Boltzmann equation. Our study advances quantitative modeling of charge transport in complex organic crystals.

cond-mat.mtrl-sci↗

arXiv2020

Facile ab initio approach for self-localized polarons from canonical transformations

Electronic states in a crystal can localize due to strong electron-phonon (e-ph) interactions, forming so-called small polarons. Methods to predict the formation and energetics of small polarons are either computationally costly or not geared toward quantitative predictions. Here we show a formalism based on canonical transformations to compute the polaron formation energy and wavefunction using ab initio e-ph interactions. Comparison of the calculated polaron and band edge energies allows us to determine whether charge carriers in a material favor a localized small polaron over a delocalized Bloch state. Due to its low computational cost, our approach enables efficient studies of the formation and energetics of small polarons, as we demonstrate by investigating electron and hole polaron formation in alkali halides and metal oxides and peroxides. We outline refinements of our scheme and extensions to compute transport in the polaron hopping regime.

cond-mat.mtrl-sci↗

arXiv2019

Next-to-Leading Order Ab Initio Electron-Phonon Scattering

Electron-phonon (e-ph) interactions are usually treated in the lowest order of perturbation theory. Here we derive next-to-leading order e-ph interactions, and compute from first principles the associated two-phonon e-ph scattering rates. The derivation involves Matsubara sums of the relevant two-loop Feynman diagrams, and the numerical calculations are challenging since they involve Brillouin zone integrals over two crystal momenta and depend critically on the intermediate state lifetimes. Using random grids and Monte Carlo integration, together with a self-consistent update of the intermediate state lifetimes, we compute and converge the two-phonon scattering rates, using GaAs as a case study. For the longitudinal optical phonon in GaAs, we find that the two-phonon scattering rates are as large as nearly half the value of the leading-order rates. The energy and temperature dependence of the two-phonon processes are analyzed. We show that including the two-phonon processes is important to accurately predicting the electron mobility in GaAs.

cond-mat.mes-hall↗

arXiv2018

Charge Transport in Organic Molecular Semiconductors from First Principles: The Band-Like Hole Mobility in Naphthalene Crystal

Predicting charge transport in organic molecular crystals is notoriously challenging. Carrier mobility calculations in organic semiconductors are dominated by quantum chemistry methods based on charge hopping, which are laborious and only moderately accurate. We compute from first principles the electron-phonon scattering and the phonon-limited hole mobility of naphthalene crystal in the framework of ab initio band theory. Our calculations combine GW electronic bandstructures, ab initio electron-phonon scattering, and the Boltzmann transport equation. The calculated hole mobility is in very good agreement with experiment between 100$-$300 K, and we can predict its temperature dependence with high accuracy. We show that scattering between inter-molecular phonons and holes regulates the mobility, though intra-molecular phonons possess the strongest coupling with holes. We revisit the common belief that only rigid molecular motions affect carrier dynamics in organic molecular crystals. Our work provides a quantitative and rigorous framework to compute charge transport in organic crystals, and is a first step toward reconciling band theory and carrier hopping computational methods.

cond-mat.mtrl-sci↗

arXiv2014

Novel Parity Violating Transport Coefficients in 2+1 Dimensions from Holography

We construct a 3+1 dimensional holographic model dual to a parity violating hydrodynamic system in 2+1 dimensions. Our model contains gravitational and electrodynamic Chern-Simons terms coupled to a neutral pseudo scalar $θ$, and a potential composed of quadratic and quartic terms in $θ$. The background is a charged black brane. We study the hydrodynamics to first order in spacetime derivatives near the probe limit of the pseudo scalar, by extracting the transport coefficients from the scalar, vector, and tensor modes of bulk perturbations. We study two mechanisms for breaking the parity of the boundary fluid: the parity is either spontaneously broken by the nonzero vev of the dual pseudo scalar operator, or by the pseudo scalar source on the boundary. The resulting transport coefficients have unusual behaviors compared to those in ordinary materials.

hep-th↗

arXiv2012

A Holographic Model For Hall Viscosity

We have modified the holographic model of Saremi and Son by using a charged black brane, instead of a neutral one, such that when the bulk pseudo scalar potential is made of quadratic and quartic terms, parity can still be broken spontaneously in the boundary theory. In our model, the 3+1 dimensional bulk has a pseudo scalar coupled to the gravitational Chern-Simons term in the anti de Sitter charged black brane back ground. Parity could be broken spontaneously in the bulk by the pseudo scalar hairy solution and give rise to non-zero Hall viscosity at the boundary theory.

hep-th↗