arXiv subjects

Liang Z. Tan

Publications and source records attributed to Liang Z. Tan.

49 records · Page 3Linked to original sources

arXiv2018

How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites

Here we develop a microscopic approach aimed at the description of a suite of physical effects related to carrier transport in, and the optical properties of, halide perovskites. Our theory is based on the description of the nuclear dynamics to all orders and goes beyond the common assumption of linear electron-phonon coupling in describing the carrier dynamics and band gap characteristics. When combined with first-principles calculations and applied to the prototypical MAPbI$_{3}$ system, our theory explains seemingly disparate experimental findings associated with both the charge-carrier mobility and optical absorption properties, including their temperature dependencies. Our findings demonstrate that orbital overlap fluctuations in the lead-halide structure plays a significant role in determining the optoelectronic features of halide perovskites.

cond-mat.mtrl-sci↗

arXiv2017

Anion Exchange in II-VI Semiconducting Nanostructures via Atomic Templating

Controlled chemical transformation of nanostructures is a promising technique to obtain precisely designed novel materials which are difficult to synthesize otherwise. We report high-temperature vapor phase anion exchange reactions to chemically transform II-VI semiconductor nanostructures (100-300 nm length scale) while retaining the single crystallinity, crystal structure, morphology and even defect distribution of the parent material via atomic templating. The concept of atomic templating is employed to obtain kinetically controlled, thermodynamically metastable structural phases such as zincblende CdSe and CdS from zincblende CdTe upon complete chemical replacement of Te with Se or S. The underlying transformation mechanisms are explained through first-principles density functional theory calculations. Atomic templating is a unique path to independently tune materials phase and composition at the nanoscale allowing synthesis of novel materials.

cond-mat.mtrl-sci↗

arXiv2017

Spin-orbit enhanced carrier lifetimes in noncentrosymmetric semiconductors

We show that the carrier recombination rate of noncentrosymmetric materials can be strongly modified by spin-orbit coupling. Our proposed mechanism involves the separation of conduction and valence bands into their respective spin components, which changes the transition dipole moments between them. The change in the carrier recombination can be either positive or negative in sign, or vary depending on the location of carriers in the Brillouin zone. We have performed a large scale DFT screening study to identify candidate materials that display this effect. We have selected three materials, Pb$_4$SeBr$_6$, ReTe$_3$Br$_5$, and CsCu(BiS$_2$)$_2$, which span the range of behaviors, and discuss their electronic band structure in greater detail. We find transition dipole moment enhancement factors of up to three orders of magnitude, reflecting the physical impact of spin-orbit coupling on the carrier lifetime. Therefore, further explorations of the spin-orbit coupling and lattice symmetry could prove to be useful for manipulating the photophysics of materials.

cond-mat.mtrl-sci↗

arXiv2017

Upper limit on nonlinear optical processes: shift current and second harmonic generation in extended systems

The response functions of a material characterize its behavior under external stimuli, such as electromagnetic radiation. Such responses may grow linearly with the amplitude of the incident radiation, as is the case of absorption, or may be nonlinear. The latter category includes a diverse set of phenomena such as second harmonic generation (SHG), shift current, sum frequency generation, and excited state absorption, among others. Despite decades of research into nonlinear response theory, and the occasional discovery of materials with large nonlinear responses, there has been no systematic investigation into the maximum amount of nonlinear optical response attainable in solid-state materials. In this work, we present an upper bound on the second-order response functions of materials, which controls the SHG and shift current responses. We show that this bound depends on the band gap, band width, and geometrical properties of the material in question. We find that Kuzyk's bound for the maximum SHG of isolated molecules can be exceeded by conjugation or condensation of molecules to form molecular solids, and that strongly coupled systems generally have larger responses than weakly coupled or isolated ones. As a proof of principle, we perform first-principles calculations of the response tensors of a wide variety of materials, finding that the materials in our database do not yet saturate the upper bound. This suggests that new large SHG and shift current materials will likely be discovered by future materials research guided by the factors mentioned in this work.

cond-mat.mes-hall↗

arXiv2017

Hybrid functional pseudopotentials

The consistency between the exchange-correlation functional used in pseudopotential construction and in the actual density functional theory calculation is essential for the accurate prediction of fundamental properties of materials. However, routine hybrid density functional calculations at present still rely on GGA pseudopotentials due to the lack of hybrid functional pseudopotentials. Here, we present a scheme for generating hybrid functional pseudopotentials, and we analyze the importance of pseudopotential density functional consistency for hybrid functionals. We benchmark our PBE0 pseudopotentials for structural parameters and fundamental electronic gaps of the G2 molecular dataset and some simple solids. Our results show that using our new PBE0 pseudopotentials in PBE0 calculations improves agreement with respect to all-electron calculations.

physics.chem-ph↗

arXiv2017

Local polar fluctuations in lead halide perovskite crystals

Hybrid lead-halide perovskites have emerged as an excellent class of photovoltaic materials. Recent reports suggest that the organic molecular cation is responsible for local polar fluctuations that inhibit carrier recombination. We combine low frequency Raman scattering with first-principles molecular dynamics (MD) to study the fundamental nature of these local polar fluctuations. Our observations of a strong central peak in both hybrid (CH$_3$NH$_3$PbBr$_3$) and all-inorganic (CsPbBr$_3$) lead-halide perovskites show that anharmonic, local polar fluctuations are intrinsic to the general lead-halide perovskite structure, and not unique to the dipolar organic cation. MD simulations show that head-to-head Cs motion coupled to Br face expansion, on a few hundred femtosecond time scale, drives the local polar fluctuations in CsPbBr$_3$.

cond-mat.mtrl-sci↗

arXiv2016

Enhancement of bulk photovoltaic effect in topological insulators

We investigate the shift current bulk photovoltaic response of materials close to a band inversion topological phase transition. We find that the bulk photocurrent reverses direction across the band inversion transition, and that its magnitude is enhanced in the vicinity of the phase transition. These results are demonstrated with first principles DFT calculations of BiTeI and CsPbI$_3$ under hydrostatic pressure, and explained with an analytical model, suggesting that this phenomenon remains robust across disparate material systems.

cond-mat.mes-hall↗

arXiv2015

Strain Induced Ferroelectric Topological Insulator

The simultaneous presence of seemingly incompatible properties of solids often provides a unique opportunity to address questions of fundamental and practical importance. The coexistence of ferroelectric and topological orders is one such example. Ferroelectrics, which have a spontaneous macroscopic polarization switchable by an applied electric field, usually are semiconductors with a well-developed wide band gap with a few exceptions. On the other hand, time-reversal symmetric $Z_2$ topological insulators (TI), characterized by robust metallic surface states protected by the topology of the bulk, usually are narrow-gap semiconductors ($< 0.7$ eV) which allow band inversion induced by the spin-orbit interaction. To date, a ferroelectric topological insulator (FETI) has remained elusive, owing to the seemingly contradictory characters of the ferroelectric and topological orders. Here, we report that the FETI can be realized in halide perovskite CsPbI$_3$ under strain. Our first-principles study reveals that a non-centrosymmetric ferroelectric structure of CsPbI$_3$ is energetically favored under a wide range of pressures, while maintaining its topological order. The proposed FETI is characterized by switchable polar surfaces with spin-momentum locked Dirac cones, which allows for electric-field control of topological surface states (TSSs) and the surface spin current. Our demonstration of a FETI in a feasible material opens doors for future studies combining ferroelectric and topological orders, and offers a new paradigm for diverse applications in electronics, spintronics, and quantum information.

cond-mat.mtrl-sci↗

arXiv2015

SU(4) symmetry breaking revealed by magneto-optical spectroscopy in epitaxial graphene

Refined infrared magnetotransmission experiments have been performed in magnetic fields B up to 35 T on a series of multilayer epitaxial graphene samples. Following the main optical transition involving the n=0 Landau level (LL), we observe a new absorption transition increasing in intensity with magnetic fields B>26 T. Our analysis shows that this is a signature of the breaking of the SU(4) symmetry of the n=0 LL. Using a quantitative model, we show that the only symmetry-breaking scheme consistent with our experiments is a charge density wave (CDW).

cond-mat.str-el↗

arXiv2015

Rashba Spin-Orbit Coupling Enhanced Carrier Lifetime in Organometal Halide Perovskites

Organometal halide perovskites are promising solar-cell materials for next-generation photovoltaic applications. The long carrier lifetime and diffusion length of these materials make them very attractive for use in light absorbers and carrier transporters. While these aspects of organometal halide perovskites have attracted the most attention, the consequences of the Rashba effect, driven by strong spin-orbit coupling, on the photovoltaic properties of these materials are largely unexplored. In this work, taking the electronic structure of methylammonium lead iodide as an example, we propose an intrinsic mechanism for enhanced carrier lifetime in 3D Rashba materials. Based on first-principles calculations and a Rashba spin-orbit model, we demonstrate that the recombination rate is reduced due to the spin-forbidden transition. These results are important for understanding the fundamental physics of organometal halide perovskites and for optimizing and designing the materials with better performance. The proposed mechanism including spin degrees of freedom offers a new paradigm of using 3D Rashba materials for photovoltaic applications.

cond-mat.mtrl-sci↗

arXiv2013

Theory of the Raman spectrum of rotated double-layer graphene

We study theoretically the Raman spectrum of the rotated double-layer graphene, consisting of two graphene layers rotated with respect to each other by an arbitrary angle θ. We find a relatively simple dependence of the Raman G peak intensity on the angle θ. On the other hand, the Raman 2D peak position, intensity, and width show a much more complicated dependence on the angle θ. We account for all of these effects, including dependence on the incoming photon energy, in good agreement with the experimental data. We find that it is sufficient to include the interaction between the graphene layers on the electronic degrees of freedom (resulting in the occurrence of van Hove singularities in the density of states). We assume that the phonon degrees of freedom are unaffected by the interaction between the layers. Furthermore, we decompose the Raman 2D peak into two components having very different linewidths; these widths are almost independent of the angle θ. The change in the intensity and the peak position of one of these two components gives insight into the dependence of the overall Raman 2D peak features as a function of the angle θ. Additionally, we show regions in the phonon spectrum giving rise to the Raman 2D peak signal. This work provides an insight into the interplay between the mechanical degree of freedom (angle θ) and the electronic degrees of freedom (singularities in the density of states) in rotated double-layer graphene. Additionally, this work provides a way to establish experimentally the value of the rotation angle θusing Raman spectroscopy measurement. This procedure becomes even more robust if one repeats the Raman spectroscopy measurement with a different incoming photon energy.

cond-mat.mes-hall↗

arXiv2012

Resonant Excitation of Graphene K-Phonon and Intra-Landau-Level Excitons in Magneto-Optical Spectroscopy

Precise infrared magnetotransmission experiments have been performed in magnetic fields up to 32 T on a series of multilayer epitaxial graphene samples. We observe changes in the spectral features and broadening of the main cyclotron transition when the incoming photon energy is in resonance with the lowest Landau level separation and the energy of a K point optical phonon. We have developed a theory that explains and quantitatively reproduces the frequency and magnetic field dependence of the phenomenon as the absorption of a photon together with the simultaneous creation of an intervalley, intra-Landau-level exciton, and a K phonon.

cond-mat.mes-hall↗

arXiv2012

Raman spectroscopy study of rotated double-layer graphene: Misorientation-angle dependence of electronic structure

We present a systematic Raman study of unconventionally-stacked double-layer graphene, and find that the spectrum strongly depends on the relative rotation angle between layers. Rotation-dependent trends in the position, width and intensity of graphene 2D and G peaks are experimentally established and accounted for theoretically. Our theoretical analysis reveals that changes in electronic band structure due to the interlayer interaction, such as rotational-angle dependent Van Hove singularities, are responsible for the observed spectra features. Our combined experimental and theoretical study provides a deeper understanding of the electronic band structure of rotated double-layer graphene, and leads to a practical way to identify and analyze rotation angles of misoriented double-layer graphene.

cond-mat.mes-hall↗