arXiv subjects

Sunghyun Kim

Publications and source records attributed to Sunghyun Kim.

35 records · Page 2Linked to original sources

arXiv2020

Upper limit to the photovoltaic efficiency of imperfect crystals

The Shockley-Queisser (SQ) limit provides a convenient metric for predicting light-to-electricity conversion efficiency of a solar cell based on the band gap of the light-absorbing layer. In reality, few materials approach this radiative limit. We develop a formalism and a computational method to predict the maximum photovoltaic efficiency of imperfect crystals from first principles. Our scheme includes equilibrium populations of native defects, their carrier-capture coefficients, and the associated recombination rates. When applied to kesterite solar cells, we reveal an intrinsic limit of 20% for $\mathrm{Cu_2ZnSnSe_4}$, which falls far below the SQ limit of 32%. The effects of atomic substitution and extrinsic doping are studied, leading to pathways for enhanced efficiency of 31%. This approach can be applied to support targeted-materials selection for future solar-energy technologies.

physics.comp-ph↗

arXiv2019

Anharmonic Lattice Relaxation during Non-radiative Carrier Capture

Lattice vibrations of point defects are essential for understanding non-radiative electron and hole capture in semiconductors as they govern properties including persistent photoconductivity and Shockley-Read-Hall recombination rate. Although the harmonic approximation is sufficient to describe a defect with small lattice relaxation, for cases of large lattice relaxation it is likely to break down. We describe a first-principles procedure to account for anharmonic carrier capture and apply it to the important case of the \textit{DX} center in GaAs. This is a system where the harmonic approximation grossly fails. Our treatment of the anharmonic Morse-like potentials accurately describes the observed electron capture barrier, predicting the absence of quantum tunnelling at low temperature, and a high hole capture rate that is independent of temperature. The model also explains the origin of the composition-invariant electron emission barrier. These results highlight an important shortcoming of the standard approach for describing point defect ionization that is accompanied by large lattice relaxation, where charge transfer occurs far from the equilibrium configuration.

cond-mat.mtrl-sci↗

arXiv2019

A Metal-Insulator Transition via Wigner Crystallization in Boron Triangular Kagome Lattice

The flat band has attracted a lot of attention because it gives rise to many exotic phases, as recently demonstrated in magic angle twisted bilayer graphene. Here, based on first-principles calculations, we identify a metal-insulator transition in boron triangular Kagome lattice with a spin-polarized flat band at 2/3-filling. This phase transition is accompanied by the formation of a Wigner crystal, which is driven by Fermi surface nesting effect and thereby strong electron-phonon interactions, keeping ferromagnetism. Our calculation results suggest that boron triangular Kagome lattices with partially filled flat bands may open a new playground for many exotic quantum phases in two-dimensional systems, such as Winger crystallization and fractional quantum Hall states.

cond-mat.mtrl-sci↗

arXiv2018

Open-Circuit Voltage Deficit in Cu2ZnSnS4 Solar Cells by Interface Band Gap Narrowing

There is evidence that interface recombination in Cu2ZnSnS4 solar cells contributes to the open-circuit voltage deficit. Our hybrid density functional theory calculations suggest that electron-hole recombination at the Cu2ZnSnS4/CdS interface is caused by a deeper conduction band that slows electron extraction. In contrast, the bandgap is not narrowed for the Cu2ZnSnSe4/CdS interface, consistent with a lower open-circuit voltage deficit.

cond-mat.mtrl-sci↗

arXiv2018

Lone-pair effect on carrier capture in Cu$_2$ZnSnS$_4$ solar cells

The performance of kesterite thin-film solar cells is limited by a low open-circuit voltage due to defect-mediated electron-hole recombination. We calculate the non-radiative carrier-capture cross sections and Shockley-Read-Hall recombination coefficients of deep-level point defects in Cu$_2$ZnSnS$_4$ (CZTS) from first-principles. While the oxidation state of Sn is +4 in stoichiometric CZTS, inert lone pair (5$s^2$) formation lowers the oxidation state to +2. The stability of the lone pair suppresses the ionization of certain point defects, inducing charge transition levels deep in the band gap. We find large lattice distortions associated with the lone-pair defect centers due to the difference in ionic radii between Sn(II) and Sn(IV). The combination of a deep trap level and large lattice distortion facilitates efficient non-radiative carrier capture, with capture cross-sections exceeding $10^{-12}$ cm$^2$. The results highlight a connection between redox active cations and `killer' defect centres that form giant carrier traps. This lone pair effect will be relevant to other emerging photovoltaic materials containing n$s^2$ cations.

cond-mat.mtrl-sci↗

arXiv2018

Stability and electronic properties of planar defects in quaternary I2-II-IV-VI4 semiconductors

Extended defects such as stacking faults and anti-site domain boundaries can perturb the band edges in Cu$_2$ZnSnS$_4$ and Cu$_2$ZnSnSe$_4$, acting as a weak electron barrier or a source for electron capture, respectively. In order to find ways to prohibit the formation of planar defects, we investigated the effect of chemical substitution on the stability of the intrinsic stacking fault and metastable polytypes and analyze their electrical properties. Substitution of Ag for Cu makes stacking faults less stable, whereas the other substitutions (Cd and Ge) promote their formation. Ge substitution has no effect on the electron barrier of the intrinsic stacking fault, but Cd substitution reduces the barrier energy and Ag substitution makes the stacking fault electron capture. While Cd substitution stabilizes the stannite structure, chemical substitutions make the primitive-mixed CuAu (PMCA) structure less stable with respect to the ground-state kesterite structure.

cond-mat.mtrl-sci↗

arXiv2018

Role of electron-phonon coupling and thermal expansion on band gaps, carrier mobility, and interfacial offsets in kesterite thin-film solar cells

The efficiencies of solar cells based on kesterite Cu$_2$ZnSnS$_4$ (CZTS) and Cu$_2$ZnSnSe$_4$ (CZTSe) are limited by a low open-circuit voltage due to high rates of non-radiative electron-hole recombination. To probe the origin of this bottleneck, we calculate the band offset of CZTS(Se) with CdS, confirming a weak spike of 0.1 eV for CZTS/wurtzite-CdS and a strong spike of 0.4 eV for CZTSe/wurtzite-CdS. We also consider the effects of temperature on the band alignment, finding that increasing temperature significantly enhances the spike-type offset. We further resolve an outstanding discrepancy between measured and calculated phonon frequencies for the kesterites, and use these to estimate the upper limit of electron and hole mobilities based on optic phonon Fröhlich scattering, which uncovers an intrinsic asymmetry with faster (minority carrier) electron mobility.

cond-mat.mtrl-sci↗

arXiv2018

Opposing effects of stacking faults and antisite domain boundaries on the conduction band edge in kesterite quaternary semiconductors

We investigated stability and the electronic structure of extended defects including anti-site domain boundaries and stacking faults in the kesterite-structured semiconductors, Cu$_2$ZnSnS$_4$ (CZTS) and Cu$_2$ZnSnSe$_4$ (CZTSe). Our hybrid density functional theory calculations show that stacking faults in CZTS and CZTSe induce a higher conduction band edge than the bulk counterparts, and thus the stacking faults act as electron barriers. Antisite domain boundaries, however, accumulate electrons as the conduction band edge is reduced in energy, having an opposite role. An Ising model was constructed to account for the stability of stacking faults, which shows the nearest neighbour interaction is stronger in the case of the selenide.

cond-mat.mtrl-sci↗

arXiv2017

A New Phosphorus Allotrope with Direct Band Gap and High Mobility

Based on ab initio evolutionary crystal structure search computation, we report a new phase of phosphorus called green phosphorus (λ-P), which exhibits the direct band gaps ranging from 0.7 to 2.4 eV and the strong anisotropy in optical and transport properties. Free energy calculations show that a single-layer form, termed green phosphorene, is energetically more stable than blue phosphorene and a phase transition from black to green phosphorene can occur at temperatures above 87 K. Due to its buckled structure, green phosphorene can be synthesized on corrugated metal surfaces rather than clean surfaces.

cond-mat.mtrl-sci↗

arXiv2017

Boron Triangular Kagome Lattice with Half-Metallic Ferromagnetism

Based on the first-principles evolutionary materials design, we report a stable boron Kagome lattice composed of triangles in triangles on a two-dimensional sheet. The Kagome lattice can be synthesized on a silver substrate, with selecting Mg atoms as guest atoms. While the isolated Kagome lattice is slightly twisted without strain, it turns into an ideal triangular Kagome lattice under tensile strain. In the triangular Kagome lattice, we find the exotic electronic properties, such as topologically non-trivial flat band near the Fermi energy and half-metallic ferromagnetism, and predict the quantum anomalous Hall effect in the presence of spin-orbit coupling.

cond-mat.mtrl-sci↗

arXiv2016

Semimetallic carbon allotrope with topological nodal line in mixed $sp^2$-$sp^3$ bonding networks

Graphene is known as a two-dimensional Dirac semimetal, in which electron states are described by the Dirac equation of relativistic quantum mechanics. Three-dimensional analogues of graphene are characterized by Dirac points or lines in momentum space, which are protected by symmetry. Here, we report a novel 3D carbon allotrope belonging to a class of topological nodal line semimetals, discovered by using an evolutionary structure search method. The new carbon phase in monoclinic $C$2$/m$ space group, termed $m$-$C_8$, consists of five-membered rings with $sp^3$ bonding interconnected by $sp^2$-bonded carbon networks. Enthalpy calculations reveal that $m$-$C_8$ is more favorable over recently reported topological semimetallic carbon allotropes, and the dynamical stability of $m$-$C_8$ is verified by phonon spectra and molecular dynamics simulations. Simulated x-ray diffraction spectra propose that $m$-$C_8$ would be one of the unidentified carbon phases observed in detonation shoot. The analysis of electronic properties indicates that $m$-$C_8$ exhibits the nodal line protected by both inversion and time-reversal symmetries in the absence of spin-orbit coupling and the surface band connecting the projected nodal points. Our results may help design new carbon allotropes with exotic electronic properties.

cond-mat.mes-hall↗

arXiv2016

Role of a Relay in Bursty Multiple Access Channels

We investigate the role of a relay in multiple access channels (MACs) with bursty user traffic, where intermittent data traffic restricts the users to bursty transmissions. As our main result, we characterize the degrees of freedom (DoF) region of a $K$-user bursty multi-input multi-output (MIMO) Gaussian MAC with a relay, where Bernoulli random states are introduced to govern bursty user transmissions. To that end, we extend the noisy network coding scheme to achieve the cut-set bound. Our main contribution is in exploring the role of a relay from various perspectives. First, we show that a relay can provide a DoF gain in bursty channels, unlike in conventional non-bursty channels. Interestingly, we find that the relaying gain can scale with additional antennas at the relay to some extent. Moreover, observing that a relay can help achieve collision-free performances, we establish the necessary and sufficient condition for attaining collision-free DoF. Lastly, we consider scenarios in which some physical perturbation shared around the users may generate data traffic simultaneously, causing transmission patterns across them to be correlated. We demonstrate that for most cases in such scenarios, the relaying gain is greater when the users' transmission patterns are more correlated, hence when more severe collisions take place. Our results have practical implications in various scenarios of wireless networks such as device-to-device systems and random media access control protocols.

cs.IT↗

arXiv2016

Top-$K$ Ranking from Pairwise Comparisons: When Spectral Ranking is Optimal

We explore the top-$K$ rank aggregation problem. Suppose a collection of items is compared in pairs repeatedly, and we aim to recover a consistent ordering that focuses on the top-$K$ ranked items based on partially revealed preference information. We investigate the Bradley-Terry-Luce model in which one ranks items according to their perceived utilities modeled as noisy observations of their underlying true utilities. Our main contributions are two-fold. First, in a general comparison model where item pairs to compare are given a priori, we attain an upper and lower bound on the sample size for reliable recovery of the top-$K$ ranked items. Second, more importantly, extending the result to a random comparison model where item pairs to compare are chosen independently with some probability, we show that in slightly restricted regimes, the gap between the derived bounds reduces to a constant factor, hence reveals that a spectral method can achieve the minimax optimality on the (order-wise) sample size required for top-$K$ ranking. That is to say, we demonstrate a spectral method alone to be sufficient to achieve the optimality and advantageous in terms of computational complexity, as it does not require an additional stage of maximum likelihood estimation that a state-of-the-art scheme employs to achieve the optimality. We corroborate our main results by numerical experiments.

cs.LG↗

arXiv2016

Direct band gap carbon superlattices with efficient optical transition

We report pure carbon-based superlattices that exhibit direct band gaps and excellent optical absorption and emission properties at the threshold energy. The structures are nearly identical to that of cubic diamond except that defective layers characterized by five- and seven-membered rings are intercalated in the diamond lattice. The direct band gaps lie in the range of 5.6~5.9 eV, corresponding to wavelengths of 210~221 nm. The dipole matrix elements of direct optical transition are comparable to that of GaN, suggesting that the superlattices are promising materials as an efficient deep ultraviolet light emitter. Molecular dynamics simulations show that the superlattices are thermally stable even at a high temperature of 2000 K. We provide a possible route to the synthesis of superlattices through wafer bonding of diamond (100) surfaces.

cond-mat.mtrl-sci↗

arXiv2015

A Relay Can Increase Degrees of Freedom in Bursty Interference Networks

We investigate the benefits of relays in multi-user wireless networks with bursty user traffic, where intermittent data traffic restricts the users to bursty transmissions. To this end, we study a two-user bursty MIMO Gaussian interference channel with a relay, where two Bernoulli random states govern the bursty user traffic. We show that an in-band relay can provide a degrees of freedom (DoF) gain in this bursty channel. This beneficial role of in-band relays in the bursty channel is in direct contrast to their role in the non-bursty channel which is not as significant to provide a DoF gain. More importantly, we demonstrate that for certain antenna configurations, an in-band relay can help achieve interference-free performances with increased DoF. We find the benefits particularly substantial with low data traffic, as the DoF gain can grow linearly with the number of antennas at the relay. In this work, we first derive an outer bound from which we obtain a necessary condition for interference-free DoF performances. Then, we develop a novel scheme that exploits information of the bursty traffic states to achieve them.

cs.IT↗

arXiv2015

Dipole-Allowed Direct Band Gap Silicon Superlattices

Silicon is the most popular material used in electronic devices. However, its poor optical properties owing to its indirect band gap nature limit its usage in optoelectronic devices. Here we present the discovery of super-stable pure-silicon superlattice structures that can serve as promising materials for solar cell applications and can lead to the realization of pure Si-based optoelectronic devices. The structures are almost identical to that of bulk Si except that defective layers are intercalated in the diamond lattice. The superlattices exhibit dipole-allowed direct band gaps as well as indirect band gaps, providing ideal conditions for the investigation of a direct-to-indirect band gap transition. The transition can be understood in terms of a novel conduction band originating from defective layers, an overlap between the valence- and conduction-band edge states at the interface layers, and zone folding with quantum confinement effects on the conduction band of non-defective bulk-like Si. The fact that almost all structural portions of the superlattices originate from bulk Si warrants their stability and good lattice matching with bulk Si. Through first-principles molecular dynamics simulations, we confirmed their thermal stability and propose a possible method to synthesize the defective layer through wafer bonding.

cond-mat.mtrl-sci↗

arXiv2014

A Finite-Size Supercell Correction Scheme for Charged Defects in One-Dimensional Systems

We propose a new finite-size correction scheme for the formation energy of charged defects and impurities in one-dimensional systems within density functional theory. The energy correction in a supercell geometry is obtained by solving the Poisson equation in a continuum model which is described by an anistrotropic permittivity tensor, with the defect charge distribution derived from first-principles calculations. We implement our scheme to study impurities and dangling bonds in silicon nanowires and demonstrate that the formation energy of charged defects rapidly converges with the supercell size.

cond-mat.mtrl-sci↗