Carrier Multiplication (CM) is a Coulomb-driven non-radiative recombination mechanism which leads to the generation of multiple electron-hole pairs after absorption of a single high-energy photon. Recently a new CM process, termed space separated quantum cutting, was introduced to explain a set of new experiments conducted in dense arrays of silicon nanocrystals. The occurrence of this effect was hypothesized to generate the formation of Auger unaffected multiexciton configurations constituted by single electron-hole pairs distributed on different interacting naocrystals. In this work we discuss ab-initio results obtained by our group in the study of CM effects in systems of strongly interacting silicon nanocrystals. By solving a set of rate equations, we simulate the time evolution of the number of electron-hole pairs generated in dense arrays of silicon nanocrystals after absorption of high energy photons, by describing the circumstances under which CM dynamics can lead to the generation of Auger unaffected multiexciton configurations.
Carrier multiplication is a non-radiative recombination mechanism that leads to the generation of two or more electron-hole pairs after absorption of a single photon. By reducing the occurrence of dissipative effects, this process can be exploited to increase solar cell performance. In this work we introduce two different theoretical fully ab-initio tools that can be adopted to study carrier multiplication in nanocrystals. The tools are described in detail and compared. Subsequently we calculate carrier multiplication lifetimes in H- and OH- terminated silicon nanocrystals, pointed out the rol…
Being a source of clean and renewable energy, the possibility to convert solar radiation in electric current with high efficiency is one of the most important topics of modern scientific research. Currently the exploitation of interaction between nanocrystals seems to be a promising route to foster the establishment of third generation photovoltaics. Here we adopt a fully ab-initio scheme to estimate the role of nanoparticle interplay on the carrier multiplication dynamics of interacting silicon nanocrystals. Energy and charge transfer-based carrier multiplication events are studied as a funct…
The distribution of rates of carrier multiplication (CM) following photon absorption is calculated for semiconductor nanocrystals (NCs). The NC electronic structure is described using a screened pseudopotential method known to give reliable description of NC excitons. The rates of biexciton generation are calculated using the Fermi golden rule with all relevant Coulomb matrix elements, taking into account proper selection rules. In CdSe and InAs NCs we find a broad distribution biexciton generation rates depending strongly on the exciton energy and size of the NC. The process becomes inefficie…
For Si and Ge nanocrystals (NCs) embedded in wide band-gap matrices, Auger recombination (AR) and carrier multiplication (CM) lifetimes are computed exactly in a three-dimensional real space grid using empirical pseudopotential wave functions. Our results in support of recent experimental data offer new predictions. We extract simple Auger constants valid for NCs. We show that both Si and Ge NCs can benefit from photovoltaic efficiency improvement via CM due to the fact that under an optical excitation exceeding twice the band gap energy, the electrons gain lion's share from the total excess e…
We report here an assessment of carrier multiplication (CM) yields in PbSe and PbS nanocrystals (NCs) by a quantitative analysis of biexciton and exciton dynamics in transient photoluminescence decays. Interest in CM, the generation of more than one electron and hole in a semiconductor after absorption of one photon, has renewed in recent years because of reports suggesting greatly increased efficiencies in nanocrystalline materials compared to the bulk form, in which CM was otherwise too weak to be of consequence in photovoltaic energy conversion devices. In our PbSe and PbS NC samples, howev…
Nanocrystals based on metal-halide perovskites offer a promising material platform for highly efficient lighting. Using transient optical spectroscopy, we study excitation recombination dynamics in manganese-doped CsPb(Cl,Br)3 perovskite nanocrystals. We find an increase in the intrinsic excitonic radiative recombination rate upon doping, which is typically a challenging material property to tailor. Supported by ab initio calculations, we can attribute the enhanced emission rates to increased exciton localization through lattice periodicity breaking from Mn dopants, which increases exciton eff…
We propose a novel mechanism for photogeneration of multiexcitons by single photons (carrier multiplication) in semiconductor nanocrystals. In this mechanism, the Coulomb interaction between two valence-band electrons involving their transfer to the conduction band creates a virtual biexciton from vacuum that is then converted into a real biexciton by photon absorption on an intraband optical transition. This mechanism is inactive in bulk semiconductors as momentum conservation suppresses intraband absorption. However, it becomes highly efficient in zero-dimensional nanocrystals and can provid…
Engineering semiconductors to enhance carrier multiplication (CM) could lead to increased photovoltaic cell performance and a significant widening of the materials range suitable for future solar technologies. Semiconductor nanocrystals (NCs) have been proposed as a favourable structure for CM enhancement, and recent measurements by transient absorption have shown evidence for highly efficient CM in lead chalcogenide and CdSe NCs. We report here an assessment of CM yields in CdSe and CdTe NCs by a quantitative analysis of biexciton and exciton signatures in transient photoluminescence decays. …
We demonstrate for the first time that impact ionization (II) [the inverse of Auger recombination (AR)] occurs with very high efficiency in semiconductor nanocrystals (NCs). Interband optical excitation of PbSe NCs at low pump intensities, for which less than one exciton is initially generated per NC on average, results in the formation of two or more excitons (carrier multiplication) when pump photon energies are more than three times the NC band gap energy. Generation of multiexcitons from a single photon absorption event is observed to take place on an ultrafast (picosecond) timescale and o…
Dynamics of hot carriers confined in Si nanocrystals is studied theoretically using atomistic tight binding approach. Radiative, Auger-like and phonon-assisted processes are considered. The Auger-like energy exchange between electrons and holes is found to be the fastest process in the system. However the energy relaxation of hot electron-hole pair is governed by the single optical phonon emission. For a considerable number of states in small nanocrystals single-phonon processes are ruled out by energy conservation law.
Charge transport properties of thin films of sol--gel processed undoped and Al-doped zinc oxide nanoparticles with variable doping level between 0.8 at% and 10 at% were investigated. The X-ray diffraction studies revealed a decrease of the average crystallite sizes in highly doped samples. We provide estimates of the conductivity and the resulting charge carrier densities with respect to the doping level. The increase of charge carrier density due to extrinsic doping were compared to the accumulation of charge carriers in field effect transistor structures. This allowed to assess the scatterin…
In this paper we report the first measurements of carrier mobilities in an inorganic nanocrystal: conducting polymer composite. The composite material in question (lead sulphide nanocrystals in the conducting polymer MEH-PPV was made using a new single-pot, surfactant-free synthesis. Mobilties were measured using time of flight (ToF) and steady-state techniques. We have found that the inclusion of PbS nanocrystals in MEH-PPV both balances and markedly increases the hole and electron mobilities - the hole mobility is increased by a factor of ~105 and the electron mobility increased by ~107 unde…
We study the role of the effective mass, band mixing and phonon emission on multiexciton generation in IV-VI nanocrystals. A 4-band k dot p effective mass model, which allows for an independent variation of these parameters, is adopted to describe the electronic structure of the nanocrystals. Multiexciton generation efficiencies are calculated using a Green's function formalism, providing results that are numerically similar to impact excitation. We find that multiexciton generation efficiencies are maximized when the effective mass of the electron and hole are small and similar. Contact with …
While being extensively studied as an important physical process to alter exciton population in nanostructures at fs time scale, carrier multiplication has not been considered seriously as a major mechanism for phase transition. Real-time time-dependent density functional theory study of Ge2Sb2Te5 reveals that carrier multiplication can induce ultrafast phase transition in solid state despite that the lattice remains cold. The results also unify the experimental findings in other semiconductors for which the explanation remains to be the 30-year old phenomenological plasma annealing model.
The microscopic origin of slow carrier cooling in lead-halide perovskites remains debated, and has direct implications for applications. Slow carrier cooling has been attributed to either polaron formation or a hot-phonon bottleneck effect at high excited carrier densities (> 10$^{18}$ cm$^{-3}$). These effects cannot be unambiguously disentangled from optical experiments alone. However, they can be distinguished by direct observations of ultrafast lattice dynamics, as these effects are expected to create qualitatively distinct fingerprints. To this end, we employ femtosecond electron diffract…
The decay of the optical phonon into the two phonons of smaller energy is calculated for Si nanocrystals. The rate of the process is in the range of 1 to 10 ps. Such anharmonic phonon decay may control the energy relaxation rate of excited carriers in Si/SiO$_2$ nanocrystals. Relevance of the phonon decay to the experimentally observed hot carrier photoluminescence is discussed.
We bring fresh insight into the ensemble properties of PbS colloidal quantum dots with a critical review of the literature on semiconductors followed by systematic comparisons between steady-state photocurrent and photoluminescence measurements. Our experiments, performed with sufficiently low powers to neglect nonlinear effects, indicate that the photoluminescence spectra have no other noticeable contribution beside the radiative recombination of thermalized photocarriers (i.e. photocarriers in thermodynamic quasi-equilibrium). A phenomenological model based on the local Kirchhoff law is prop…
Degenerately doped semiconductor nanocrystals (NCs) are of recent interest to the NC community due to their tunable localized surface plasmon resonances (LSPRs) in the near infrared (NIR). The high level of doping in such materials with carrier densities in the range of 1021 cm^-3 leads to degeneracy of the doping levels and intense plasmonic absorption in the NIR. The lower carrier density in degenerately doped semiconductor NCs compared to noble metals enables LSPR tuning over a wide spectral range, since even a minor change of the carrier density strongly affects the spectral position of th…
Networks of ligand-free semiconductor nanocrystals (NCs) offer a valuable combination of high carrier mobility and optoelectronic properties tunable via quantum confinement. In principle, maximizing carrier mobility entails crossing the insulator-metal transition (IMT), where carriers become delocalized. A recent theoretical study predicted that this transition occurs at nρ^3 ~ 0.3, where n is the carrier density and ρis the interparticle contact radius. In this work, we satisfy this criterion in networks of plasma-synthesized ZnO NCs by using intense pulsed light (IPL) annealing to tune n and…
We use first-principles models to demonstrate how an organic oxidizing agent, F4 -TCNQ (7,7,8,8- tetracyano-2,3,5,6-tetrafluoroquinodimethane), modifies the electronic structure of silicon nanocrys- tals, suggesting it may enhance p-type carrier density and mobility. The proximity of the lowest unoccupied level of F4 -TCNQ to the highest occupied level of the Si-nanocrystals promotes the formation of an empty hybrid state overlapping both nanocrystal and molecule, reducing the exci- tation energy to about 0.8-1 eV in vacuum. Hence, it is suggested that F4 -TCNQ can serve both as a surface oxid…
Methods of exceeding the detailed balance limit for a single junction solar cell have included down-converting high energy photons to produce two photons; and carrier multiplication, whereby high energy photons produce more than one electron-hole pair. Both of the methods obey the conservation of energy in similar ways, and effectively produce a higher current in the solar cell. Due to this similarity, it has been assumed that there is no thermodynamic difference between the two methods. Here, we compare the two methods using a generalized approach based on Kirchhoff's law of radiation and dev…
Two-dimensional halide perovskite nanoplatelets (NPLs) have exceptional light-emitting properties, including wide spectral tunability, ultrafast radiative decays, high quantum yields (QY), and oriented emission. To realize efficient devices, it is imperative to understand how exciton transport progresses in NPL thin films. Due to the high binding energies of electron-hole pairs, excitons are generally considered the dominant species responsible for carrier transfer. We employ spatially and temporally resolved optical microscopy to map exciton diffusion in perovskite nanocrystal (NC) thin films…
It was shown in the recent experiments that the hybrid organic/inorganic resonant structures can provide a flexible materials platform aimed at the design of novel light emitting devices. The applications of hybrid structures for photovoltaic solar cell can also be useful. We pay attention in this note that the resonant energy transfer in hybrid structure from the organic thin layer to the semiconductor nanostructures can drastically increase the intensity of the free carrier generation. To demonstrate this idea we use the results of recently published paper by Zhang et al., Nature Nanotechnol…
We report an optically gated transistor composed of CdSe nanocrystals (NCs), sensitized with the dye Zinc beta-tetraaminophthalocyanine for operation in the first telecom window. This device shows a high ON/OFF ratio of six orders of magnitude in the red spectral region and an unprecedented 4.5 orders of magnitude at 847 nm. By transient absorption spectroscopy, we reveal that this unexpected infrared sensitivity is due to electron transfer from the dye to the CdSe NCs within 5 ps. We show by time-resolved photocurrent measurements that this enables fast rise times during near-infrared optical…
Copper binary compounds are often intrinsic p-type semiconductors due to the presence of Cu(I) vacancies, with corresponding hole carriers in the valence band. If the free carrier concentration is high enough, localized plasmon resonances can be sustained in nanocrystals, with frequencies in the infra-red (<1 eV), with respect to the typical resonances seen in the visible range in the case of metals (Ag, Au, ...). The localization of the resonances can be demonstrated with scanning transmission electron energy loss spectroscopy (STEM-EELS) by combining high spatial and high energy resolutions.…
Using Localized Surface Plasmon Resonance (LSPR) as an optical probe we demonstrate the presence of free carriers in phosphorus doped silicon nanocrystals (SiNCs) embedded in a silica matrix. In small SiNCs, with radius ranging from 2.6 to 5.5 nm, the infrared spectroscopy study coupled to numerical simulations allows us to determine the number of electrically active phosphorus atoms with a precision of a few atoms. We demonstrate that LSP resonances can be supported with only about 10 free electrons per nanocrystal, confirming theoretical predictions and probing the limit of the collective na…
Carrier multiplication is a many-particle process giving rise to the generation of multiple electron-hole pairs. This process holds the potential to increase the power conversion efficiency of photovoltaic devices. In graphene, carrier multiplication has been theoretically predicted and recently experimentally observed. However, due to the absence of a bandgap and competing phonon-induced electron-hole recombination, the extraction of charge carriers remains a substantial challenge. Here we present a new strategy to benefit from the gained charge carriers by introducing a Landau quantization t…
Magnetic doping of semiconductor nanostructures is actively pursued for applications in magnetic memory and spin-based electronics. Central to these efforts is a drive to control the interaction strength between carriers (electrons and holes) and the embedded magnetic atoms. In this respect, colloidal nanocrystal heterostructures provide great flexibility via growth-controlled `engineering' of electron and hole wavefunctions within individual nanocrystals. Here we demonstrate a widely tunable magnetic sp-d exchange interaction between electron-hole excitations (excitons) and paramagnetic manga…
Si nanocrystals have been extensively studied because of their novel properties and their potential applications in electronic, optoelectronic, photovoltaic, thermoelectric and biological devices. These new properties are achieved through the combination of the quantum confinement of carriers and the strong influence of surface chemistry. As in the case of bulk Si the tuning of the electronic, optical and transport properties is related to the possibility of doping, in a controlled way, the nanocrystals. This is a big challenge since several studies have revealed that doping in Si nanocrystals…
We study theoretically the role of carrier multiplication due to impact ionization after an ultrafast optical excitation in a model system of a quasi-two dimensional material with a small band gap. As a mechanism for the photo-induced band gap narrowing we use coherent phonons, which mimics the quenching of an insulator phase. We discuss the importance of impact ionization in the ultrafast response, and investigate the interplay between carrier and band dynamics. Our model allows us to compare with recent experiments and identify signatures of carrier multiplication in typical electronic distr…
Complex electron-microscopic, energy-dispersed and wide-temperature optical absorption and photoluminescence (PL) investigations are carried out into Bridgeman-grown layered In2Se3 crystals. It is shown that In2Se3 crystals as a whole have a homogeneous concentration of In and Se atoms, corresponding with In2Se3 stoichiometry. Nevertheless, In2Se3 crystals contain a significant amount of dislocations, on which nano-sized interspersions of crystal phases of pure InSe, In6Se7 and monoclinic red Se settle down. Optical wide-temperature investigations of In2Se3 allow us to do the following: establ…
Outstanding optoelectronic properties and a facile synthesis render halide perovskite nanocrystals (NCs) a promising material for nanostructure-based devices. However, the commercialization is hindered mainly by the lack of NC stability under ambient conditions and inefficient charge carrier injection. Here, we investigate solutions to both problems, employing methylammonium lead bromide (MAPbBr_3) NCs encapsulated in diblock copolymer core-shell micelles of tunable size. We confirm that the shell does not prohibit energy transfer, as FRET efficiencies between these NCs and 2D CsPbBr_3 nanopla…
Time- and angle-resolved photoemission measurements on two doped graphene samples displaying different doping levels reveal remarkable differences in the ultrafast dynamics of the hot carriers in the Dirac cone. In the more strongly ($n$-)doped graphene, we observe larger carrier multiplication factors ($>$ 3) and a significantly faster phonon-mediated cooling of the carriers back to equilibrium compared to in the less ($p$-)doped graphene. These results suggest that a careful tuning of the doping level allows for an effective manipulation of graphene's dynamical response to a photoexcitation.
Band-Like Transport and Cation Off-Centring in Ag/Bi-Based Solar Absorbers
Inorganic Chemistry Laboratory, University of Oxford(牛津大学无机化学实验室);Graduate Institute of Photonics and Optoelectronics and Department of Electrical Engineering, National Taiwan University(台湾大学光电子学研究所及电气工程系);Department of Materials, University of Oxford(牛津大学材料系);Department of Chemistry, University of Manchester(曼彻斯特大学化学系);Centre for Nano Science and Engineering, Indian Institute of Science(印度科学学院纳米科学与工程中心);Department of Physics, University of Warwick(华威大学物理系);Warwick Centre for Ultrafast Spectroscopy, University of Warwick(华威大学超快光谱学中心);Catalonia Institute for Energy Research (IREC)(加泰罗尼亚能源研究所);Facultat de Fisica, Universitat de Barcelona(巴塞罗那大学物理学院);Cavendish Laboratory, University of Cambridge(剑桥大学卡文迪许实验室);ISIS Neutron and Muon Source, Science and Technology Facilities Council, Rutherford Appleton Laboratory(科学和技术设施委员会卢瑟福阿普尔顿实验室ISIS中子和缪子源);Institut Laue-Langevin(朗之万研究所);School of Chemistry, University of Birmingham(伯明翰大学化学学院);Departament d'Enginyeria Electrònica i Biomèdica, IN2UB, Universitat de Barcelona(巴塞罗那大学电子与生物医学工程系);Institute for Solar Fuels, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH(柏林亥姆霍兹材料与能源研究所太阳能燃料研究所);Yusuf Hamied Department of Chemistry, University of Cambridge(剑桥大学优素福·哈米德化学系)
The development of next generation perovskite-based optoelectronic devices relies critically on the understanding of the interaction between charge carriers and the polar lattice in out-of-equilibrium conditions. While it has become increasingly evident for CsPbBr3 perovskites that the Pb-Br framework flexibility plays a key role in their light-activated functionality, the corresponding local structural rearrangement has not yet been unambiguously identified. In this work, we demonstrate that the photoinduced lattice changes in the system are due to a specific polaronic distortion, associated …
We have prepared light emitting nanocrystalline porous silicon (PS) layers by electrochemical anodization of crystalline silicon (c-Si) wafer and characterized the c-Si/PS heterojunctions using temperature dependence of dark current-voltage (I-V) characteristics. The reverse bias I-V characteristics of c-Si/PS heterojunctions are found to behave like Schottky junctions where carrier transport is mainly governed by the carrier generation-recombination in the depletion region formed on the PS side. Fermi level of c-Si gets pinned to the defect levels at the interface resulting in ln(I) proportio…
Instead of normal non-Arrhenius relationship, the carrier mobility $ln(μ)$ v.s. $1/T^2$ showed abnormal dependence in an MEH-PPV / InP nanocrystal composite system that a critical temperature $(T_c)$ behavior is prominent in temperature range of 233 K to 333 K. Here, in the model of variable range hopping theory, an analytical model is developed within a Gaussian trap distribution, which is successfully implemented on that phenomenon. The results show that Tc becomes the transition temperature as long as trap-filling factor (FF) ~1, which means a transition point from Boltzmann to Fermi distri…
Excitons play major roles in optical processes in modern semiconductors, such as single-wall carbon nanotubes (SWCNTs), transition metal dichalcogenides, and 2D perovskite quantum wells. They possess extremely large binding energies (>100~meV), dominating absorption and emission spectra even at high temperatures. The large binding energies imply that they are stable, that is, hard to ionize, rendering them seemingly unsuited for optoelectronic devices that require mobile charge carriers, especially terahertz emitters and solar cells. Here, we have conducted terahertz emission and photocurrent …
A critical requirement for high gain and low noise avalanche photodiodes is the single-carrier avalanche multiplication. We propose that the single-carrier avalanche multiplication can be achieved in materials with a limited width of the conduction or valence band resulting in a restriction of kinetic energy for one of the charge carriers. This feature is not common to the majority of technologically relevant semiconductors, but it is observed in chalcogenides, such as Selenium and compound I2-II-IV-VI4 alloys.
The multiplication rates of hot carriers in CdSe quantum dots are quantified using an atomistic pseudopotential approach and first order perturbation theory. Both excited holes and electrons are considered, and electron-hole Coulomb interactions are accounted for. We find that holes have much higher multiplication rates than electrons with the same excess energy due to the larger density of final states (positive trions). When electron-hole pairs are generated by photon absorption, however, the net carrier multiplication rate is dominated by photogenerated electrons, because they have on avera…
Atomistically detailed computational studies of nanocrystals, such as those derived from the promising lead-halide perovskites, are challenging due to the large number of atoms and lack of symmetries to exploit. Here, focusing on methylammonium lead iodide nanocrystals, we combine a real-space tight binding model with the GW approximation to the self-energy and obtain exciton wavefunctions and absorption spectra via solutions of the associated Bethe-Salpeter equation. We find that the size dependence of carrier confinement, dielectric contrast, electron-hole exchange, and exciton binding energ…
In conventional solar cell semiconductor materials (predominantly Si) photons with energy higher than the band gap initially generate hot electrons and holes, which subsequently cool down to the band edge by phonon emission. Due to the latter process, the energy of the charge carriers in excess of the band gap is lost as heat and does not contribute to the conversion of solar to electrical power. If the excess energy is more than the band gap it can in principle be utilized through a process known as carrier multiplication (CM) in which a single absorbed photon generates two (or more) pairs of…
Graphene is an ideal material to study fundamental Coulomb- and phonon-induced carrier scattering processes. Its remarkable gapless and linear band structure opens up new carrier relaxation channels. In particular, Auger scattering bridging the valence and the conduction band changes the number of charge carriers and gives rise to a significant carrier multiplication - an ultrafast many-particle phenomenon that is promising for the design of highly efficient photodetectors. Furthermore, the vanishing density of states at the Dirac point combined with ultrafast phonon-induced intraband scatteri…
The description of carrier dynamics in spatially confined semiconductor nanocrystals (NCs), which have enhanced electron-hole and exciton-phonon interactions, is a great challenge for modern computational science. These NCs typically contain thousands of atoms and tens of thousands of valence electrons with a discrete spectrum at low excitation energies, similar to atoms and molecules, that converges to the continuum bulk limit at higher energies. Computational methods developed for molecules are limited to very small nanoclusters, and methods for bulk systems with periodic boundary conditions…
We report a study of the photoconductivity (PC) induced in different types of diamonds (type IIa single crystals and CVD) by femtosecond XUV pulses (high order harmonics - up to 19th - of a titanium doped laser). We also reprot UPS spectras obtained with harmonics 13 to 29. Depending on the harmonic's order, the PC signal first increases (orders 9 to 13) and then decreases. If the increase is easily interpreted as resulting from a carrier multiplication process, the further decrease has not yet received an explanation. The UPS measurements also suggest a strong effect of the plasmon relaxation…
Solar cells with a heterojunction between colloidal CuInS$_2$ and ZnO nanocrystals are an innovative concept in solution-processed photovoltaics, but the conversion efficiency cannot compete yet with devices employing lead chalcogenide quantum dots. Here, we present a detailed study on the charge collection in CuInS$_2$/ZnO solar cells. An inverted device architecture was utilized, in which the ZnO played an additional role as optical spacer layer. Variations of the ZnO thickness were exploited to create different charge generation profiles within the light-harvesting CuInS$_2$ layer, which st…
We present a theory of highly excited interacting carriers confined in a semiconductor nanostructure, incorporating Auger coupling between excited states with different number of excitations. The Coulomb matrix elements connecting exciton, bi-exciton and tri-exciton complexes are derived and an intuitive picture of breaking neutral multi-exction complexes into positively and negatively charged multi-exciton complexes is given. The general approach is illustrated by analyzing the coupling of biexciton and exciton in CdSe spherical nanocrystals. The electron and hole states are computed using at…
We propose a mechanism of energy relaxation for carriers confined in a non-polar quantum dot surrounded by an amorphous polar environment. The carrier transitions are due to their interaction with the oscillating electric field induced by the local vibrations in the surrounding amorphous medium. We demonstrate that this mechanism controls energy relaxation for electrons in Si nanocrystals embedded in a SiO$_2$ matrix, where conventional mechanisms of electron-phonon interaction are not efficient.
Ultrafast light-matter interaction is a powerful tool for the study of solids. Upon laser excitation, carrier multiplication and lattice acceleration beyond thermal velocity can occur, as a result of far-from-equilibrium carrier relaxation. The roles of electron-electron and electron-phonon scatterings are identified by first-principles dynamic simulations, from which a unified phase diagram emerges. It not only explains the experimentally-observed "inertial" melting but also predicts abnormal damping by Pauli Exclusion Principle with a new perspective on ultrahigh-intensity laser applications…
Band-like Carriers in a Soft, Anharmonic Lattice: Lead-Halide Perovskites
Pohang Accelerator Laboratory, POSTECH(浦项加速器实验室,浦项科技大学);YUHS-KRIBB Medical Convergence Research Institute, College of Medicine, Yonsei University(延世大学医学院佑山-韩国生命科学研究院医学融合研究所);Department of Physics, University of Seoul(首尔大学物理系);Global Institute of Future Technology, Shanghai Jiao Tong University(上海交通大学未来技术学院)