Structurally Flexible 2D Spacer for Suppressing the Electron-Phonon Coupling Induced Non-Radiative Decay in Perovskite Solar Cells

This study presents experimental evidence of the dependence of non-radiative recombination processes on the electron-phonon coupling of perovskite in perovskite solar cells(PSCs).Via A-site cation engineering,a weaker electron-phonon coupling in perovskite has been achieved by introducing the structurally soft cyclohexane methylamine(CMA^(+))cation,which could serve as a damper to alleviate the mechanical stress caused by lattice oscillations,compared to the rigid phenethyl methylamine(PEA^(+))analog.It demonstrates a significantly lower non-radiative recombination rate,even though the two types of bulky cations have similar chemical passivation effects on perovskite,which might be explained by the suppressed carrier capture process and improved lattice geometry relaxation.The resulting PSCs achieve an exceptional power conversion efficiency(PCE)of 25.5%with a record-high opencircuit voltage(V_(OC))of 1.20 V for narrow bandgap perovskite(FAPbI_(3)).The established correlations between electron-phonon coupling and non-radiative decay provide design and screening criteria for more effective passivators for highly efficient PSCs approaching the Shockley-Queisser limit.

Polaronic Electron-Phonon Interactions on the Third-Harmonic Generation in a Square Quantum Well

The influence of electron-phonon interactions on third-harmonic generation in a square quantum well is investigated. The first- and third-harmonic generation coefficient is obtained by using compact-density-matrix approach and iterative method, and the numerical results are presented for a GaAs square quantum well. The results show that the third-harmonic generation coefficient is obviously enhanced after considering the influence of electron-phonon interactions.

Measurements of electron-phonon coupling factor and interfacial thermal resistance of metallic nano-films using a transient thermoreflectance technique

Using a transient thermoreflectance （TTR） technique, several Au films with different thicknesses on glass and SiC substrates are measured for thermal characterization of metMlic nano-films, including the electron phonon coupling factor G, interfazial thermal resistance R, and thermal conductivity Ks of the substrate. The rear heating-front detecting （RF） method is used to ensure the femtosecond temporal resolution. An intense laser beam is focused on the rear surface to heat the film, and another weak laser beam is focused on the very spot of the front surface to detect the change in the electron temperature. By varying the optical path delay between the two beams, a complete electron temperature profile can be scanned. Different from the normally used single-layer model, the double-layer model involving interfaciM thermal resistance is studied here. The electron temperature cooling profile can be affected by the electron energy transfer into the substrate or the electron-phonon interactions in the metallic films. For multiple-target optimization, the genetic algorithm （GA） is used to obtain both G and R. The experimental result gives a deep understanding of the mechanism of ultra-fast heat transfer in metals.

Improved Ligand-Field Theory with Effect of Electron-Phonon Interaction

Traditional ligand-field theory has to be improved by taking into account both 'pure electronic' contribution and electron-phonon interaction one (including lattice-vibrational relaxation energy). By means of improved ligand-field theory, R1, R2, R'3, R'2, and R'1 lines, U band, ground-state zero-field-splitting (GSZFS), and ground-state g factors of ruby and/or GSGG: Cr3+ as well as thermal shifts of GSZFS, R1 line and R2 line of ruby have been calculated.The results are in very good agreement with the experimental data. Moreover, it is found that the value of cubic-field parameter given by traditional ligand-field theory is inappropriately large. For thermal shifts of GSZFS, R1 line and R2 line of ruby, several conclusions have also been obtained.

Photo-Induced Ultrafast Electron Dynamics in Anatase and Rutile TiO_(2):Effects of Electron-Phonon Interaction

The photo-induced ultrafast electron dynamics in both anatase and rutile TiO_(2) are investigated by using the Boltzmann transport equation with the explicit incorporation of electron-phonon scattering rates.All structural parameters required for dynamic simulations are obtained from ab initio calculations.The results show that although the longitudinal optical modes significantly affect the electron energy relaxation dynamics in both phases due to strong Fr?hlich-type couplings,the detailed relaxation mechanisms have obvious differences.In the case of a single band,the energy relaxation time in anatase is 24.0 fs,twice longer than 11.8 fs in rutile.This discrepancy is explained by the different diffusion distributions over the electronic Bloch states and different scattering contributions from acoustic modes in the two phases.As for the multiple-band situation involving the lowest six conduction bands,the predicted overall relaxation times are about 47 fs and 57 fs in anatase and rutile,respectively,very different from the case of the single band.The slower relaxation in rutile is attributed to the existence of multiple rate-controlled steps during the dynamic process.The present findings may be helpful to control the electron dynamics for designing efficient TiO_(2)-based devices.

Effects of Electron-Phonon Interaction on Linear and Nonlinear Optical Absorption in Cylindrical Quantum Wires

The electron-phonon interaction influences on lineax and nonfineax optical absorption in cylindrical quantum wires （CQW） with an infinite confining potential axe investigated. The optical absorption coefficients are obtained by using the compact-density-matrix approach and iterative method, and the numerical results are presented for GaAs CQW. The results show that the electron-phonon interaction makes a distinct influence on optical absorption in CQW. The electron-phonon interaction on the wave functions of electron dominates the values of absorption coefficients and the correction of the electron-phonon effect on the energies of the electron makes the absorption peaks blue shift and become wider. Moreover, the electron-phonon interaction influence on optical absorption with an infinite confining potential is different from that with a finite confining potential.

PERSISTENT CURRENT IN A ONE-DIMENSIONAL MESOSCOPIC RING WITH ELECTRON-PHONON INTERACTION IN THE LATTICE MODEL

A new non-perturbative method is used to discuss the persistent current in a one-dimensional mesoscopic ring threaded by a flux φ with electron-phonon interaction in the lattice model. The current is periodic in φ with a flux quantum φ 0 and the electron-phonon interaction suppresses the persistent current. By considering the contributions of many-phonon correlations, we could obtain more accurate results.

Electron-Phonon Interaction in an Annular Quantum Dot

The confined longitudinal-optical （LO） phonon and surface-optical （SO） phonon modes of a free-standing annular cylindrical quantum dot are derived within the framework of dielectric continuum approximation. It is found that there exist two types of SO phonon modes： top SO （TSO） mode and side SO（SSO） mode in a cylindrical quantum annulus. Numerical calculation on CdS annulus system has been performed. Results reveal that the two different solutions of SSO mode distribute mainly at the inner or outer surfaces of the annulus. The dispersion relations and the coupling intensions of phonons in a quantum annulus are compared with those in a cylindrical quantum dot. It is found that the dispersion relations of the two different structures are similar, but the coupling intension of the phonon-electron interaction in quantum annulus is larger than that in quantum dot. The Hamiltonians describing the free phonon modes and their interactions with electrons in the system are also derived.

Electron-phonon coupling in cuprate and iron-based superconductors revealed by Raman scattering

Electron-phonon coupling （EPC） in cuprate and iron-based superconducting systems, as revealed by Raman scat- tering, is briefly reviewed. We introduce how to extract the coupling information through phonon lineshape. Then we discuss the strength of EPC in different high-temperature superconductor （HTSC） systems and possible factors affecting the strength. A comparative study between Raman phonon theories and experiments allows us to gain insight into some crucial electronic properties, especially superconductivity. Finally, we summarize and compare EPC in the two existing HTSC systems, and discuss what role it may play in the HTSC.

Propagating Optical Phonon Modes and Their Electron-Phonon Interaction Hamiltonians in Asymmetric Wurtzite Nitride Semiconductor Quantum Wells

Within the framework of the dielectric continuum model and Loudon ＇s uniaxial crystal model, the properties of frequency dispersion of the propagating （PR） optical phonon modes and the coupling functions of electron-PR phonons interaction in an asymmetrical wurtzite quantum well （QW） are deduced and analyzed via the method of electrostatic potential expanding. Numerical calculation on an asymmetrical Alo.25Gao.75N/GaN/Alo.15Gao.ssN wurtzite QW were performed. The results reveal that there are infinite branches of PR phonon modes in the systems. The behaviors of frequency forbidden of PR modes in the asymmetric QWs have been clearly observed. The mathematical and physical origins for these features have been analyzed in depth. The PR optical phonon branches have been distinguished and labelled reasonably in terms of the oscillating properties of the PR modes in the well-layer material. Moreover, the amplitudes and frequency properties of the electron-PR modes coupling functions in the barrier and well materials have also been analyzed from both of the mathematical and physical viewpoints.

A novel electron-phonon coupling thermoelasticity with Burgers electronic heat transfer

The electron-phonon interaction can reveal the microscopic mechanism of heat transfer in metals.The two-step heat conduction considering electron-phonon interaction has become an effective theoretical model for extreme environments,such as micro-scale and ultrafast processes.In this work,the two-step heat transfer model is further extended by considering the Burgers heat conduction model with the secondorder heat flux rate for electrons.Then,a novel generalized electron-phonon coupling thermoelasticity is proposed with the Burgers electronic heat transfer.Then,the problem of one-dimensional semi-infinite copper strip subject to a thermal shock at one side is studied by the Burgers two-step(BTS)model.The thermoelastic analytical solutions are systematically derived in the Laplace domain,and the numerical Laplace inversion method is adopted to obtain the transient responses.The new model is compared with the parabolic two-step(PTS)model and the hyperbolic two-step(HTS)model.The results show that in ultrafast heating,the BTS model has the same wave front jump as the HTS model.The present model has the faster wave speed,and predicts the bigger disturbed regions than the HTS model.More deeply,all two-step models also have the faster wave speeds than one-step models.This work may benefit the theoretical modeling of ultrafast heating of metals.

Pressure-Induced Shift of R-Line of MgO：Cr^3＋ with Electron-Phonon Interaction Effect

By means of improved ligand-field theory, the ＂pure electronic＂ pressure-induced shift （PS） and the PS due to electron-phonon interaction （EPI） of R-line of MgO：Cr^3＋ have been calculated, respectively. The calculated results are in very good agreement with the experimental data. The behaviors of the pure electronic PS of R-line of MgO：Cr^3＋ and the PS of its R-line due to EPI are different. It is the combined effect of them that gives rise to the total PS of R-line, which has satisfactorily explained the experimental results. The comparison between the feature of R-line PS of MgO：Cr^3＋ and that of R1-line PS of ruby has been made.

Dynamic Deformation Electron-Phonon Interaction in Disordered Bulk Semiconductor

We present our theoretical investigations on the effects of disorder on the electron-phonon interaction in semiconducting GaAs system. Both the temperature (T) and disorder (electron mean free path l) dependences of the electron-phonon scattering rate have been determined. On consideration of the dynamic screening, we find a significant change in the temperature exponent as well as the pre factor from the earlier reported temperature power law dependence result ?T6 obtained under static screening. Also the dynamic screening makes a noticeable change in the character of the dependence of scattering rate on the mean free path from the static screening result.

Purity-dependent Lorenz number,electron hydrodynamics and electron-phonon coupling in WTe_(2)

We present a study of electrical and thermal transport in Weyl semimetal WTe_(2)down to 0.3 K.The Wiedemann-Franz law holds below 2 K and a downward deviation starts above.The deviation is more pronounced in cleaner samples,as expected in the hydrodynamic picture of electronic transport,where a fraction of electron-electron collisions conserve momentum.Phonons are the dominant heat carriers and their mean-free-path does not display a Knudsen minimum.This is presumably a consequence of weak anharmonicity,as indicated by the temperature dependence of the specific heat.Frequent momentum exchange between phonons and electrons leads to quantum oscillations of the phononic thermal conductivity.Bloch-Grüneisen picture of electron-phonon scattering breaks down at low temperature when Umklapp ph-ph collisions cease to be a sink for electronic flow of momentum.Comparison with semi-metallic Sb shows that normal ph-ph collisions are amplified by anharmonicity.In both semimetals,at cryogenic temperature,e-ph collisions degrade the phononic flow of energy but not the electronic flow of momentum.

金属卤素钙钛矿CsPbBr3的电声耦合输运特性研究

金属卤素钙钛矿CsPbBr_(3)在发光方面(Light emitter)的优良表现吸引了许多人把它作为下一代发光、显示与量子信息的可选材料,但其关键的漂移迁移率会受到声子限制.本文将以第一性原理计算得到CsPbBr_(3)的包括极性光学声子(Polar optical phonon)在内的电声耦合特性,然后使用线性玻尔兹曼方程给出在电场下的解,从而得出漂移迁移率.在论文详述中会给出CsPbBr_(3)的各向异性载流子输运特性的研究,为金属卤素钙钛矿的应用提供一些必要信息.

Correlation-enhanced electron-phonon coupling for accurate evaluation of the superconducting transition temperature in bulk FeSe

It has been widely recognized that,based on standard density functional theory calculations of the electron-phonon coupling,the superconducting transition temperature(T_(c))in bulk FeSe is exceptionally low(almost 0 K)within the Bardeen-Cooper-Schrieffer formalism.Yet the experimentally observed T_(c)is much higher(∼10 K),and the underlying physical origin remains to be fully explored,especially at the quantitative level.Here we present the first accurate determination of T_(c)in FeSe where the correlation-enhanced electron-phonon coupling is treated within first-principles dynamical mean-field theory.Our studies treat both the multiple electronic bands across the Fermi level and phononic bands,and reveal that all the optical phonon modes are effectively coupled with the conduction electrons,including the important contributions of a single breathing mode as established by previ-ous experiments.Accordingly,each of those phonon modes contributes pronouncedly to the electron pairing,and the resultant T_(c)is drastically enhanced to the experimentally observed range.The approach developed here should be broadly applicable to other superconducting systems where correlation-enhanced electron-phonon coupling plays an important role.

Properties of nonadiabatic quantum fluctuations of the strongly coupled electron-phonon systems

A new variational-ansatz of states of electrons and phonons was proposed on the basis of the Holstein model in strongly coupled electron-phonon systems for studying the influence of nonadiabatic phonon fluctuation,arising from the motion and density fluctuation of electrons,on the properties of ground state,uncertainty relation,stability of polarons,charge density wave (CDW) and phonon staggered ordering. The new ansatz represents the correlation among the displacement and squeezing states of phonons and polaron’s state of electrons as well as the squeezing-antisqueezing effect. The correlation and squeezing-antisqueezing ef-fect result in the decrease of ground state energy,enhancement of stability of the systems,increase of binding energy of the polarons,weakening of the growing speed of polaron narrowing of the electron band,increase of the charge density wave order and suppression of the increased tendency of anomalous quantum fluctuation of the phonons in such a case,when compared with the uncorrelated case in the systems. The results obtained show that the ground state determined by the new state ansatz is most stable,thus the new ansatz describing the properties of the coupled electron phonon systems is very relevant and available,especially in strongly coupled and largely squeezed cases.

Calculating electron-phonon coupling matrix: Theory introduction,code development and preliminary application

Electron-phonon coupling(EPC) in bulk materials is an important effect in multifarious physical and chemical phenomena. It is the key to explaining the mechanisms for superconductivity, electronic transport, etc. The EPC matrix describes the coupling of the electronic eigenstates of the studied system under the perturbation of phonons. Although the EPC matrix is closely relevant to many fundamental physicochemical properties, it remains a challenge to calculate the EPC matrix precisely due to the high computational cost. In recent years, Giustino et al. developed the EPW method on open-source ab-initio software Quantum Espresso, which uses Wannier functions(WFs) to calculate EPC matrix. However, due to the limitation of their implementation,it is not possible yet to calculate the EPC matrix under some important computational conditions, e.g., for DFT+U and HSE calculation. Given the importance of these computational conditions(e.g., for transition metal oxides), we have developed our own implementation of EPC matrix calculation based on the domestic ab-initio software PWmat. Our code allows the DFT+U and HSE correction, so we can get a more accurate EPC matrix in the related problems. In this article, we will first review the formulae and elucidate how to calculate the EPC matrix by constructing WFs. Then we will introduce our code along with its workflow on PWmat and present our test results of two classical semiconductor systems Al As and Si, showing consistency with EPW. Next, the EPC matrix of Li Co O_(2), a classical cathode material for lithium-ion batteries, is calculated using different exchange correlation(XC) functionals including LDA, PBE, DFT+U and HSE. A comparison is provided for the related EPC matrix. It shows there could be a significant difference for the EPC matrix elements due to the use of different XC functionals.Our implementation thus opens the way for fast calculation of EPC for the important class of materials, like the transition metal oxides.

Versatile band structure and electron-phonon coupling in layered PtSe_(2) with strong interlayer interaction

The large tunability in the band structure is ubiquitous in two-dimensional(2D)materials,and PtSe_(2) is not an exception,which has attracted considerable attention in electronic and optoelectronic applications due to its high carrier mobility and long-term airstability.Such dimensional dependent properties are closely related to the evolution of electronic band structures.Critical points(CPs),the extrema or saddle points of electronic bands,are the cornerstone of condensed-matter physics and fundamentally determine the optical and transport phenomena of the layered PtSe_(2).Here,we have experimentally revealed the detailed electronic structures in layered PtSe_(2),including the CPs in the Brillouin zones(BZs),by means of reflection contrast spectroscopy and spectroscopic ellipsometry(SE).There are three critical points in the BZs attributed to the excitonic transition,quasi-particle band gap,and the band nesting effect related transition,respectively.Three CPs show red-shifting trends with increasing layer number under the mechanism of strong interlayer coupling.We have further revealed the electron–phonon(e–ph)interaction in such layered material,utilizing temperature-dependent absorbance spectroscopy.The strength of e–ph interaction and the average phonon energy also decline with the increasement of layer number.Our findings give a deep understanding to the physics of the layer-dependent evolution of the electronic structure of PtSe_(2),potentially leading to applications in optoelectronics and electronic devices.

Detection of electron-phonon coupling in two-dimensional materials by light scattering

Electron-phonon coupling affects the properties of two-dimensional(2D)materials significantly,leading to a series of novel phenomena.Inelastic light scattering provides a powerful experimental tool to explore electron-phonon interaction in 2D materials.This review gives an overview of the basic theory and experimental advances of electron-phonon coupling in 2D materials detected by Raman and Brillouin scattering,respectively.In the Raman scattering part,we review Raman spectroscopy studies of electron-phonon coupling in graphene,transition metal disulfide compounds,van der Waals heterostructures,strongly correlated systems,and 2D magnetic materials.In the Brillouin scattering part,we extensively introduce Brillouin spectroscopy in non-van der Waals 2D structures,including temperature sensors for phonons and magnons,interfacial Dzyaloshinsky-Moriya interaction and spin torque in multilayer magnetic structures,as well as exciton-polariton in semiconductor quantum well.