scholarly journals Giant isotope effect on phonon dispersion and thermal conductivity in methylammonium lead iodide

2020 ◽  
Vol 6 (31) ◽  
pp. eaaz1842
Author(s):  
M. E. Manley ◽  
K. Hong ◽  
P. Yin ◽  
S. Chi ◽  
Y. Cai ◽  
...  
Keyword(s):  
Thermal Conductivity ◽  
High Performance ◽  
Phonon Scattering ◽  
Light Emission ◽  
Phonon Dispersion ◽  
Acoustic Phonons ◽  
Lead Iodide ◽  
Phonon Bottleneck ◽  
Optic Phonon ◽  
Methylammonium Lead Iodide

Lead halide perovskites are strong candidates for high-performance low-cost photovoltaics, light emission, and detection applications. A hot-phonon bottleneck effect significantly extends the cooling time of hot charge carriers, which thermalize through carrier–optic phonon scattering, followed by optic phonon decay to acoustic phonons and finally thermal conduction. To understand these processes, we adjust the lattice dynamics independently of electronics by changing isotopes. We show that doubling the mass of hydrogen in methylammonium lead iodide by replacing protons with deuterons causes a large 20 to 50% softening of the longitudinal acoustic phonons near zone boundaries, reduces thermal conductivity by ~50%, and slows carrier relaxation kinetics. Phonon softening is attributed to anticrossing with the slowed libration modes of the deuterated molecules and the reduced thermal conductivity to lowered phonon velocities. Our results reveal how tuning the organic molecule dynamics enables control of phonons important to thermal conductivity and the hot-phonon bottleneck.

Enhanced Grain Size and Crystallinity in CH3NH3PbI3 Perovskite Films by Metal Additives to the Single-Step Solution Fabrication Process

MRS Advances ◽  
2018 ◽  
Vol 3 (55) ◽  
pp. 3237-3242 ◽  
Author(s):  
Zahrah S. Almutawah ◽  
Suneth C. Watthage ◽  
Zhaoning Song ◽  
Ramez H. Ahangharnejhad ◽  
Kamala K. Subedi ◽  
...  
Keyword(s):  
Grain Size ◽  
Solar Cells ◽  
High Performance ◽  
High Efficiency ◽  
Perovskite Solar Cells ◽  
Precursor Solution ◽  
Single Step ◽  
Fabrication Process ◽  
Lead Iodide ◽  
Methylammonium Lead Iodide

ABSTRACTMethods of obtaining large grain size and high crystallinity in absorber materials play an important role in fabrication of high-performance methylammonium lead iodide (MAPbI3) perovskite solar cells. Here we study the effect of adding small concentrations of Cd2+, Zn2+, and Fe2+salts to the perovskite precursor solution used in the single-step solution fabrication process. Enhanced grain size and crystallinity in MAPbI3 films were obtained by using 0.1% of Cd2+ or Zn2+in the precursor solution. Consequently, solar cells constructed with Cd- and Zn-doped perovskite films show a significant improvement in device performance. These results suggest that the process may be an effective and facile method to fabricate high-efficiency perovskite photovoltaic devices.

Phonon Scattering in Bi2Te3/Sb2Te3 Superlattice

2011 ◽  
Author(s):  
Yaguo Wang ◽  
Xianfan Xu ◽  
Rama Venkatasubramanian
Keyword(s):  
Thermal Conductivity ◽  
Thermoelectric Materials ◽  
Phonon Scattering ◽  
Quantum Confinement Effect ◽  
Theoretical Models ◽  
Heat Transfer Process ◽  
Acoustic Phonons ◽  
Time Resolved ◽  
Hetero Structure ◽  
Phonon Velocity

Thermoelectric materials are characterized with the figure of merit, ZT = S2σT/κ, where T is the temperature, S the Seebeck coefficient, σ the electrical conductivity and κ the thermal conductivity. Many researches have been focused on reducing lattice thermal conductivity through increasing phonon scattering at interfaces. Thin-film superlattices are one of the promising candidates for high ZT thermoelectric materials. Several theoretical models have been used to explain the large ZT in superlattice. One comes from the extra scattering channels at interfaces introduced by the hetero-structure. Another is a result of quantum confinement effect which reduces the phonon group velocity propagating perpendicularly through the superlattice layers through flattening the dispersion curve of acoustic phonons. In this work, ultrafast time-resolved measurements were conducted on Bi2Te3, Sb2Te3 and Bi2Te3/Sb2Te3 superlattice (SL) films to detect coherent acoustic phonons in these materials. Scattering of these phonons is revealed in the Bi2Te3/Sb2Te3 SLs, which comes from the interfaces of the hetero-structure in SL. Also, a decrease of acoustic phonon velocity resulted from folding and flattening of phonons branches is observed. Results show that both interface scattering and the reduced phonon velocity contribute to suppressing the heat transfer process.

scholarly journals Thermal transport in nanocrystalline Si and SiGe by ab initio based Monte Carlo simulation

2017 ◽  
Vol 7 (1) ◽  
Author(s):  
Lina Yang ◽  
Austin J. Minnich
Keyword(s):  
Thermal Conductivity ◽  
Monte Carlo ◽  
Ab Initio ◽  
Grain Boundaries ◽  
Thermal Transport ◽  
Phonon Scattering ◽  
Phonon Dispersion ◽  
Computational Study ◽  
Phonon Transport ◽  
Nanocrystalline Si

Abstract Nanocrystalline thermoelectric materials based on Si have long been of interest because Si is earth-abundant, inexpensive, and non-toxic. However, a poor understanding of phonon grain boundary scattering and its effect on thermal conductivity has impeded efforts to improve the thermoelectric figure of merit. Here, we report an ab-initio based computational study of thermal transport in nanocrystalline Si-based materials using a variance-reduced Monte Carlo method with the full phonon dispersion and intrinsic lifetimes from first-principles as input. By fitting the transmission profile of grain boundaries, we obtain excellent agreement with experimental thermal conductivity of nanocrystalline Si [Wang et al. Nano Letters 11, 2206 (2011)]. Based on these calculations, we examine phonon transport in nanocrystalline SiGe alloys with ab-initio electron-phonon scattering rates. Our calculations show that low energy phonons still transport substantial amounts of heat in these materials, despite scattering by electron-phonon interactions, due to the high transmission of phonons at grain boundaries, and thus improvements in ZT are still possible by disrupting these modes. This work demonstrates the important insights into phonon transport that can be obtained using ab-initio based Monte Carlo simulations in complex nanostructured materials.

Spectral Detail of Phonon Conduction and Scattering in Graphene

2011 ◽  
Author(s):  
Dhruv Singh ◽  
Jayathi Y. Murthy ◽  
Timothy S. Fisher
Keyword(s):  
Thermal Conductivity ◽  
Phonon Scattering ◽  
Interatomic Potential ◽  
Phonon Dispersion ◽  
Transition Probabilities ◽  
Transition Probability ◽  
Phonon Transport ◽  
Temperature Perturbation ◽  
Boltzmann Transport ◽  
Wide Range

This paper examines the thermodynamic and thermal transport properties of the 2D graphene lattice. The interatomic interactions are modeled using the Tersoff interatomic potential and are used to evaluate phonon dispersion curves, density of states and thermodynamic properties of graphene as functions of temperature. Perturbation theory is applied to calculate the transition probabilities for three-phonon scattering. The matrix elements of the perturbing Hamiltonian are calculated using the anharmonic interatomic force constants obtained from the interatomic potential as well. An algorithm to accurately quantify the contours of energy balance for three-phonon scattering events is presented and applied to calculate the net transition probability from a given phonon mode. Under the linear approximation, the Boltzmann transport equation (BTE) is applied to compute the thermal conductivity of graphene, giving spectral and polarization-resolved information. Predictions of thermal conductivity for a wide range of parameters elucidate the behavior of diffusive phonon transport. The complete spectral detail of selection rules, important phonon scattering pathways, and phonon relaxation times in graphene are provided, contrasting graphene with other materials, along with implications for graphene electronics. We also highlight the specific scattering processes that are important in Raman spectroscopy based measurements of graphene thermal conductivity, and provide a plausible explanation for the observed dependence on laser spot size.

The Phonon Thermal Conductivity of a Single-Layer Graphene From Complete Phonon Dispersion Relations

2010 ◽  
Author(s):  
Yunfeng Gu ◽  
Zhonghua Ni ◽  
Minhua Chen ◽  
Kedong Bi ◽  
Yunfei Chen
Keyword(s):  
Thermal Conductivity ◽  
Acoustic Phonon ◽  
Phonon Scattering ◽  
Phonon Dispersion ◽  
Single Layer ◽  
Single Layer Graphene ◽  
Optical Phonons ◽  
Relaxation Rates ◽  
Phonon Thermal Conductivity ◽  
Transverse Acoustic

In this paper, the phonon scattering mechanisms of a single layer graphene are investigated based on the complete phonon dispersion relations. According to the selection rules that a phonon scattering process should obey the energy and momentum conservation conditions, the relaxation rates of combing and splitting Umklapp processes can be calculated by integrating the intersection lines between different phonon mode surfaces in the phonon dispersion relation space. The dependence of the relaxation rates on the wave vector directions is presented with a three dimensional surfaces over the first Brillion zone. It is found that the reason for the optical phonons contributing a little to heat transfer is attributed to the strong Umklapp processes but not to their low group velocities. The combing Umklapp scattering processes involved by the optical phonons mainly decrease the acoustic phonon thermal conductivity, while the splitting Umklapp scattering processes of the optical phonons mainly restrict heat conduction by the optical phonons themselves. Neglecting the splitting processes, the optical phonons can contribute more energy than that carried by the acoustic phonons. Based on the calculated phonon relaxation time, the thermal conductivities contributed from different mode phonons can be evaluated. At low temperatures, both longitudinal and in-plane transverse acoustic phonon thermal conductivities have T2 temperature dependence, and the out-of-plane transverse acoustic phonon thermal conductivity is proportion to T3/2. At room temperature, the calculated thermal conductivity is on the order of a few thousands W/m.K depending on the sample size and the edge roughness, which is in agreement with the recently measured data.

A first principles study of the phonon anharmonicity, electronic structure and optical characteristics of LaAlO3

2018 ◽  
Vol 1 (1) ◽  
pp. 161-180 ◽  
Author(s):  
Bahaa Ilyas ◽  
Badal Elias
Keyword(s):  
Thermal Conductivity ◽  
Electronic Structure ◽  
Ab Initio ◽  
Conversion Efficiency ◽  
First Principles ◽  
Phonon Scattering ◽  
Phonon Dispersion ◽  
Optical Spectra ◽  
Hybrid Functional ◽  
The Way

The way elementary excitations work together with their couplings and interact as condensed matter systems is very important when designing optimum energy-conversion devices. We investigated the electronic structure of LaAlO3, and we show that the bandgap insulator of LaAlO3 obtained theoretically by the hybrid functional HSE06 is an indirect 5.649eV that show a very good agreement with experimental data. The lattice constant is obtained exactly as experiment. In thermos-electric materials, the concept of conversion-efficiency (heat to electricity) is improved instantly by suppressing the phonon quasi-particles propagations that are responsible for draft macroscopic thermal transport. The material presented here for thermo-electric conversion-efficiency of cubic perovskite LaAlO3, show that it has an ultralow thermal-conductivity, while the formalism to its strong phonon scattering interactions resides mostly unclear. From the bases of Ab-initio simulations, the 4-dimensional phonon-dispersion surfaces of the cubic perovskite LaAlO3, have been mapped and we found that the origins of the ionic potential an-harmonicity being responsible for the unique behaviour and properties of LaAlO3. It is investigated that these phonon scattering arise solely from the LaAlO3 unstable electronic-structure, with its orbital interactions resulting to lattice instability similar to the ferroelectric instabilities. Our results show a microscopic insight bonding electronic-structure and phonon an-harmonicity in LaAlO3, and provides some new picture the way interactions happen between phonon–electron and phonon–phonon this lead to understand the concept of ultralow thermal-conductivity. Ab-initio calculations was performed on cubic perovskite LaAlO3 to obtain the phonon density of states (DOS) from 50 K to 5000 K, we find that the anharmonic behaviour starts around temperature limits of 500 K. The computed optical spectra were obtained using both the Beth Slapter Equation BSE and compared with the perturbed method using HSE06, optical spectra show that the inter-band transition occur precisely from the O-valence bands to the La-conduction bands throughout the low energy area. The energy-loss spectrum, optical conductivity and reflectivity and the refractive index are computed from first principles by using HSE06 hybrid functional. The optical band gap of material shows about 6.21 eV, which agrees with some cited experimental measurements.

The Phonon Thermal Conductivity of Single-Layer Graphene From Complete Phonon Dispersion Relations

2012 ◽  
Vol 134 (6) ◽  
Author(s):  
Yunfeng Gu ◽  
Zhonghua Ni ◽  
Minhua Chen ◽  
Kedong Bi ◽  
Yunfei Chen
Keyword(s):  
Thermal Conductivity ◽  
Acoustic Phonon ◽  
Phonon Scattering ◽  
Phonon Dispersion ◽  
Single Layer ◽  
Single Layer Graphene ◽  
Optical Phonons ◽  
Relaxation Rates ◽  
Phonon Thermal Conductivity ◽  
Transverse Acoustic

In this paper, the phonon scattering mechanisms of single-layer graphene are investigated based on the complete phonon dispersion relations. According to the selection rules that a phonon scattering process should obey the energy and momentum conservation conditions, the relaxation rates of combining and splitting umklapp processes can be calculated by integrating the intersection lines between different phonon mode surfaces in the phonon dispersion relation space. The dependence of the relaxation rates on the wave vector directions is presented with a three-dimensional surface over the first Brillouin zone. It is found that the reason for the optical phonons contributing little to heat transfer is attributed to the strong umklapp processes but not to their low phonon group velocities. The combining umklapp scattering processes involving the optical phonons mainly decrease the acoustic phonon thermal conductivity, while the splitting umklapp scattering processes of the optical phonons mainly restrict heat conduction by the optical phonons themselves. Neglecting the splitting processes, the optical phonons can contribute more energy than that carried by the acoustic phonons. Based on the calculated phonon relaxation time, the thermal conductivities contributed from different mode phonons can be evaluated. At low temperatures, both longitudinal and in-plane transverse acoustic phonon thermal conductivities have T2 temperature dependence, and the out-of-plane transverse acoustic phonon thermal conductivity is proportion to T3/2. The calculated thermal conductivity is on the order of a few thousands W/(m K) at room temperature, depending on the sample size and the edge roughness, and is in agreement well with the recently measured data in the temperature range from about 350 K to 500 K.

Frequency Resolved Phonon Transport in Si/Ge Nanocomposites

2011 ◽  
Author(s):  
Dhruv Singh ◽  
Jayathi Y. Murthy ◽  
Timothy S. Fisher
Keyword(s):  
Thermal Conductivity ◽  
Energy Exchange ◽  
Phonon Dispersion ◽  
Low Frequency ◽  
Phonon Transport ◽  
Ballistic Regime ◽  
Acoustic Phonons ◽  
Length Scales ◽  
Diffusive Regime ◽  
Heterogeneous Interfaces

In this paper, we analyze cross plane phonon transport and thermal conductivity in two-dimensional Si/Ge nanocomposites. A non-gray BTE model that includes full details of phonon dispersion, the spread in phonon mean free paths and the frequency dependent transmissivity is used to simulate thermal transport. The general conclusions inferred from gray BTE simulations that the thermal conductivity of the nanocomposite is much lower than its constituent materials and interfacial density as the parameter determining thermal conductivity remain the same. However, it is found that the gray BTE significantly overpredicts thermal conductivity in the length scales of interest and quantitatively reliable results are obtained only upon inclusion of the details of phonon dispersion. The transition of phonon transport from ballistic regime to near diffusive regime is observed by looking at a large range of length scales. Non-equilibrium energy exchange between optical and acoustic phonons and the granularity in phonon mean free paths are found to significantly affect thermal conductivity leading to departures from the frequently employed gray approximation. It is also found that the frequency content of thermal conductivity in the nanocomposite extends out to a much larger frequency range unlike bulk Si and Ge. Scattering against heterogeneous interfaces is very effective in suppressing thermal conductivity contribution from the low frequency acoustic phonons but less so for high frequency phonons, which have much smaller mean free paths.

Structure of Methylammonium Lead Iodide Within Mesoporous Titanium Dioxide: Active Material in High-Performance Perovskite Solar Cells

Nano Letters ◽  
2013 ◽  
Vol 14 (1) ◽  
pp. 127-133 ◽  
Author(s):  
Joshua J. Choi ◽  
Xiaohao Yang ◽  
Zachariah M. Norman ◽  
Simon J. L. Billinge ◽  
Jonathan S. Owen
Keyword(s):  
Titanium Dioxide ◽  
Solar Cells ◽  
High Performance ◽  
Active Material ◽  
Perovskite Solar Cells ◽  
Lead Iodide ◽  
Mesoporous Titanium Dioxide ◽  
Methylammonium Lead Iodide
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