Electron-phonon Coupling Strength Research Articles

Dual‐Doping Strategy of Metal Chlorides in Ambient Air with High Humidity for Achieving Highly Air‐Stable All‐Inorganic Perovskite Solar Cells

It is fundamentally challenging to achieve stable and efficient all‐inorganic perovskite solar cells (PSCs) in ambient air conditions for low‐cost commercial manufacturing, as the crystallinity, surface morphology, and optical activity of all‐inorganic perovskites exhibit high sensitivity to environmental factors such as moisture and illumination. Herein, a dual‐doping strategy is presented to prepare high‐quality dual‐doping CsPbI2Br films under ambient air with relative humidity of 70% (70% RH) by introducing CaCl2 and InCl3 additives into precursor solution. The results from the experiments and calculations reveal that the CaCl2 additive can isolate moisture by forming hydrates at the surface and grain boundary of perovskites. Meanwhile, the addition of InCl3 can significantly improve the optoelectronic properties via the heterovalent substitution of Pb2+ by a small amount of In3+. Moreover, the phase segregation can be significantly suppressed in the dual‐doping CsPbI2Br films owing to decreasing the electron–phonon coupling strength and increasing the activation energy of ion migration. The unencapsulated dual‐doping CsPbI2Br PSC with the power conversion efficiency (PCE) of 15.51% (70% RH) demonstrates high humidity storage and long‐term optical stability, remaining 90% of the original PCE after aging 2400 h under ambient air (50% RH) and 1500 h under continuous illumination, respectively.

Probing the origin of abnormally strong electron-phonon interaction in phonon transport of semiconductor C3B monolayer

Recently, the two-dimensional semiconductor C3B monolayer has attracted much attention owing to its excellent physical, optical, and electronic properties. In this work, the origin of electron-phonon interaction (EPI) on the thermal properties of C3B by n-type and p-type doping is systematically investigated via first-principles calculations to provide fundamental knowledge for the thermal management the C3B-based electronic devices. The carrier concentrations for the largest reduction of the lattice thermal conductivity (κ) appear at 4 × 1014 cm−2 for n-type and 9 × 1014 cm−2 for p-type, which is closely related to the electron density of states (DOS). The boron (B) atoms break the structural symmetry and induce mass disorder scattering, which renders C3B more prone to the influence of EPI. Moreover, the electronic band structure in the C3B monolayer exhibits multivalley characteristics, which leads to an intervalley scattering. It is worth noting that the anisotropy in the C3B monolayer can be significantly enhanced by EPI. Additionally, an abnormal phenomenon of strong electron-phonon scattering but low electron-phonon coupling strength is found in C3B monolayer, which indicates that large electron-phonon coupling strength is sufficient but not necessary for strong electron-phonon scattering.

Color Tunable Single-phase Cyclosilicate KBaScSi3O9: Eu2+/Tb3+/Sm3+ for n-UV pumped wLEDs

The exploration of stable/efficient phosphor for n-UV chip pumped white light-emitting diodes (wLEDs) remains an arduous task. Herein, a novel series of color tunable Eu2+/Tb3+/Sm3+ tridoped Sc-based cyclosilicate phosphors (KBaScSi3O9: Eu2+/Tb3+/Sm3+) have successfully designed and obtained via facile solid-state reaction based on comprehensive consideration of rigidly structural network of host, weak electron-phonon coupling strength and spectral adjustability of codopants via energy transfer (ET). The crystallographic occupancies of Eu, Tb and Sm primary in Ba/K, Ba and Ba sites in the monoclinic host, respectively were determined on the basis of the Rietveld refinements and crystal chemistry rules. The photoluminescence (PL) properties were systematically investigated in conjunction with structural analyses, implying that the ‘warm’ white light with excellent thermal stability is stemmed from combination of optimized blue (Eu2+), green (Tb3+) and red (Sm3+) emissions via Eu → Tb → Sm ET strategy. Interestingly, Tb ions play both roles of green light luminescent center and ET bridge to achieve cascade ET for connecting Eu/Sm ion pairs because of the adverse metal-metal charge transfer (MMCT) effect (Eu2+ + Sm3+ → Eu3+ + Sm2+). Furthermore, the phosphor-converted wLEDs (pc-wLEDs), by encapsulating the optimal KBS: 4%Eu/4%Tb/6%Sm with commercial n-UV LED chip, show high thermal stability with satisfactory electroluminescence (EL) performances. These results indicate the KBS: Eu/Tb/Sm phosphors are potential candidates for application in high power n-UV pumped pc-wLEDs.

Defect induced crystal lattice disorder and its effect on the electron-phonon coupling in Fe doped ZnO thin films

We established a strong correlation between the crystal lattice disorder in Fe doped ZnO (FexZn1-xO) thin films and its effect on the electron phonon (e-p) coupling strength (I2LO/I1LO) which decreased with Fe doping concentration, improved with annealing temperature and showed a mixed increasing/decreasing trend by the variation of the argon (Ar) to oxygen (O2) gas ratio (Ar + O2, Ar) in the deposition chamber. Fe doping raised the number of phonon modes, intensity and full width at half maximum (FWHM) of the 1LO phonon modes suggesting the confinement of phonons due to the increased crystal lattice disorder in the FexZn1-xO films. High temperature annealing enhanced the e-p coupling strength reaching a maximum at 500 °C indicating better crystal quality at high temperature. Furthermore, the e-p coupling strength dropped with the doping concentration for the films prepared in Ar + O2 atmosphere and that showed a mixed increasing/decreasing trend for films prepared in Ar atmosphere. This unique physical phenomena confirmed that the coupling strength not only depend on the dopant concentration but also the dopant induced micro/nano defects that modulate the crystal lattice disorder and the coupling strength in doped ZnO. The as prepared FexZn1-xO thin films were highly oriented along the c-axis displaying columnar nanorod (film) like morphology at low (high) Fe doping concentration with the co-existence of both Fe2+ and Fe3+ ions. Fe doping increased the band gap from 3.28 eV for un-doped ZnO to 3.35 eV (1.40 at.% of Fe) and 3.42 eV (3.5 at.% of Fe). Nearly forty (40) thin films were used for a detailed investigation.

Electron-phonon coupling dictates electron mean free paths and negative thermal diffusion in metals

The spatiotemporal dynamics of the fundamental energy carriers in metals underpin the efficiency of a wide array of technologies. Although much progress in our understanding of the temporal response of electronic relaxation processes following an external field perturbation has been achieved, the spatial relaxation dynamics of electrons after excitation remains unclear. Here, we employ a scanning ultrafast microscopy with high spatial resolution to directly measure the mean free paths of electrons in different metals. We show that the strength of electron-phonon coupling not only dictates the mean free paths, but also controls a peculiar spatial shrinking of the electronic temperature profile immediately after the electrons have thermalized with the ‘colder’ lattice. More specifically, from our experimental tracking of the spatial relaxation profiles, a clear observation of an effective negative thermal diffusion is apparent for metals with weaker electron-phonon coupling, while for metals with stronger electron-phonon coupling, the negative thermal diffusion effect is not observable. Our spatiotemporal modeling based on the two-temperature approach provides evidence that although negative diffusion occurs universally for materials with two different species that have varying diffusivities and are thermodynamically coupled, effective negative diffusion is masked for cases with stronger coupling between the species.

Van Hove singularity driven enhancement of superconductivity in two-dimensional tungsten monofluoride (WF)

Superconductivity in two-dimensional materials has gained significant attention in the last few years. In this work, we report phonon-mediated superconductivity investigations in monolayer Tungsten monofluoride (WF) by solving anisotropic Migdal Eliashberg equations as implemented in EPW. By employing first-principles calculations, our examination of phonon dispersion spectra suggests that WF is dynamically stable. Our results show that WF has weak electron–phonon coupling (EPC) strength (λ) of 0.49 with superconducting transition temperature (T c ) of 2.6 K. A saddle point is observed at 0.11 eV below the Fermi level (E F ) of WF, which corresponds to the Van Hove singularity (VHS). On shifting the Fermi level to the VHS by hole doping (3.7 × 1014 cm−2), the EPC strength increases to 0.93, which leads to an increase in the T c to 11 K. However, the superconducting transition temperature of both pristine and doped WF increases to approximately 7.2 K and 17.2 K, respectively, by applying the Full Bandwidth (FBW) anisotropic Migdal–Eliashberg equations. Our results provide a platform for the experimental realization of superconductivity in WF and enhancement of the superconducting transition temperature by adjusting the position of E F to the VHS.

Effect of phonon anharmonicity on thermal conductivity of ZnTe Thin films

The ZnTe thin film is a potential material for optoelectronic devices in extreme temperature and radiation environments. In this report, the thermal conductivity of ZnTe films is measured non-invasively using the micro-Raman method and correlated with the phonon anharmonic effect. The evolution of crystalline ZnTe thin films from Te/ZnO bilayer by thermal annealing at 450 ∘C has been observed above the melting point of Te, which is confirmed from x-ray diffraction and high-resolution transmission electron microscopy. The ZnTe thin films illustrate three longitudinal phonon modes with higher harmonics of nLO (n = 3) at room temperature. Temperature-dependent Raman spectra in the range of 93–303 K are used to analyze the phonon anharmonicity from Raman shift, FWHM, and Phonon lifetime of the thin films. The Balkanski model is used to fit the anharmonicity-induced phonon frequency shift of nLO modes as a function of temperature, taking into account three- and four-phonon interactions. The intensity ratio of the I 2LO /I 1LO and I 3LO /I 2LO provide information about the electron-phonon coupling strength, which is influenced by the anharmonic effect. The laser power-dependent Raman spectra are used to determine the thermal conductivity of the ZnTe films, which is found to be approximately 9.68 Wm−1K−1, remains relatively constant for all nLO modes, indicating that multi-phonon scattering process. The correlation between thermal conductivity and phonon anharmonicity can pave the way for understanding the phonon scattering process in ZnTe thin films for high-performance optoelectronic device applications in harsh conditions.

Exploring the lead-free halide Cs2MGaBr6 (M = Li, Na) double perovskites for sustainable energy applications

In recent years, there has been a growing emphasis on the exploration of sustainable and eco-friendly materials well-suited for advanced applications in the realms of thermoelectrics and optoelectronics. Lead-free halide double perovskites have emerged as a compelling class of materials in this context. Nevertheless, despite their potential utility, thorough investigations into their thermal transport characteristics remain limited. In this systematic investigation, we employ density functional theory (DFT) and post-DFT techniques to elucidate the essential stability parameters, transport properties, and carrier-lattice interactions of the metal halide-based Cs2MGaBr6 (X = Li, Ga) double perovskites. Our assessment of structural stability involves a meticulous description of stability index parameters and the optimization of pristine structures using the GGA-PBE potential. Additionally, we calibrate the electronic structure while taking spin–orbit coupling (SOC) effects into consideration by using a combination of GGA and GGA + mBJ potentials. Our findings reveal that the TB-mBJ derived band gaps of 1.82 eV and 1.78 eV for Cs2LiGaBr6 and Cs2NaGaBr6 reside within the visible spectrum, prompting further investigation into their thermal transport characteristics. Moreover, we analyze the phonon characteristics and vibrational modes, extending our investigation to examine the electron–phonon coupling strength. The scrutiny of the Fröhlich coupling constant and the Feynman polaron radius unveils a stronger electron–phonon coupling strength. In the domain of thermoelectrics, the significant figure of merit (zT) values of 1.08 and 1.04 for Cs2LiGaBr6 and Cs2NaGaBr6, respectively, emphasize the considerable potential of these materials for deployment in renewable energy applications. Furthermore, our computational investigation into optical properties, including the dielectric constant, optical absorption, and refractive index, demonstrates optimal performance within the visible spectrum. Specifically, elevated absorption coefficient values of 30×10\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$30\ imes 10$$\\end{document}4cm-1\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${{\ ext{cm}}}^{-1}$$\\end{document} for Cs2LiGaBr6 and 40×10\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$40\ imes 10$$\\end{document}4cm-1\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${{\ ext{cm}}}^{-1}$$\\end{document} for Cs2NaGaBr6 are noted across visible and infrared spectra, highlighting their promising potential in optoelectronic and solar cell technologies.

Influence of spin–orbit interaction on the effective mass of bound polaron in a parabolic quantum well

Using Tokuda's linear combination operator method and variational technique, we derive the effective mass of strongly coupled bound polaron in a parabolic quantum well. Due to the spin–orbit interaction, the effective mass of bound polaron splits into two branches. In the present calculation, we discuss dependence of effective mass on vibration frequency, electron–phonon coupling strength, Coulomb-bound potential strength, spin–orbit and velocity. The theoretical results show that effective mass of polaron is an increasing function of vibration frequency, Coulomb-bound potential strength and electron–phonon coupling strength. The absolute value of the total spin-splitting effective mass increases with the increase of spin–orbit, but decreases with the increase of velocity. It is found that, due to the heavy hole characteristic of spin–orbit interaction, the total spin-splitting effective mass is negative.

Metal-bonded perovskite lead hydride with phonon-mediated superconductivity exceeding 46 K under ambient pressure

In the search for high-temperature superconductivity in hydrides, a plethora of multi-hydrogen superconductors have been theoretically predicted, and some have been synthesized experimentally under ultrahigh pressures of several hundred GPa. However, the impracticality of these high-pressure methods has been a persistent issue. In response, we propose a new approach to achieve high-temperature superconductivity under ambient pressure by implanting hydrogen into lead to create a stable few-hydrogen binary perovskite, Pb4H. This approach diverges from the popular design methodology of multi-hydrogen covalent high critical temperature (Tc ) superconductors under ultrahigh pressure. By solving the anisotropic Migdal–Eliashberg equations, we demonstrate that perovskite Pb4H presents a phonon-mediated superconductivity exceeding 46 K with inclusion of spin–orbit coupling, which is six times higher than that of bulk Pb (7.22 K) and comparable to that of MgB2, the highest Tc achieved experimentally at ambient pressure under the Bardeen, Cooper, and Schrieffer framework. The high Tc can be attributed to the strong electron–phonon coupling strength of 2.45, which arises from hydrogen implantation in lead that induces several high-frequency optical phonon modes with a relatively large phonon linewidth resulting from H atom vibration. The metallic-bonding in perovskite Pb4H not only improves the structural stability but also guarantees better ductility than the widely investigated multi-hydrogen, iron-based and cuprate superconductors. These results suggest that there is potential for the exploration of new high-temperature superconductors under ambient pressure and may reignite interest in their experimental synthesis in the near future.

Enhanced thermoelectric performance of graphene at room temperature by cut-off phonon frequency

Based on the full electron-phonon interactions and temperature-induced phonon renormalization, both electrical transport and thermal transport of graphene are systematically studied under different cut-off phonon frequencies. When the electron concentration is less than 1013 cm−2, the electrical transport properties increase with the cut-off phonon frequency. Otherwise, the electrical transport properties are nearly the same between 1013 cm−2 and 1015 cm−2, indicating that the contribution of cut-off phonon frequency decreases with the electron concentration. Considering the three-phonon, four-phonon, and phonon-electron scattering processes, the lattice thermal conductivity is studied, showing a value of 1357 W/mK at room temperature. At Van Hove singularity (5 × 1014 cm−2), the lattice thermal conductivity changes from 1357 W/mK to 557 W/mK. The effect of cut-off phonon frequency on thermal transport is nearly negligible. The electrical/phonon transport property accumulation concerning the mean free path shows the quantitative relationship between the mean free path and transport property, indicating a key mean free path of 186 nm. With a grain boundary of 186 nm, the ZT changes from 0.22 to 0.56 under a cut-off phonon frequency of 0 cm−1, while increasing from 0.64 to 1.23 under a cut-off phonon frequency of 30 cm−1. This work provides a strategy to enhance the thermoelectric property by regulating the electron-phonon coupling strength through cut-off phonon frequency.

Prediction of superconductivity in a series of tetragonal transition metal dichalcogenides.

Transition metal dichalcogenides (TMDCs) represent a well-known material family with diverse structural phases and rich electronic properties; they are thus an ideal platform for studying the emergence and exotic phenomenon of superconductivity (SC). Herein, we propose the existence of tetragonal TMDCs with a distorted Lieb (dLieb) lattice structure and the stabilized transition metal disulfides (MS2), including dLieb-ZrS2, dLieb-NbS2, dLieb-MnS2, dLieb-FeS2, dLieb-ReS2, and dLieb-OsS2. Except for semiconducting dLieb-ZrS2 and magnetic dLieb-MnS2, the rest of metallic dLieb-MS2 was found to exhibit intrinsic SC with the transition temperature (TC) ranging from ∼5.4 to ∼13.0 K. The TC of dLieb-ReS2 and dLieb-OsS2 exceeded 10 K and was higher than that of the intrinsic SC in the known metallic TMDCs, which is attributed to the significant phonon-softening enhanced electron-phonon coupling strength. Different from the Ising spin-orbit coupling (SOC) effect in existing non-centrosymmetric TMDCs, the non-magnetic dLieb-MS2 monolayers exhibit the Dresselhaus SOC effect, which is featured by in-plane spin orientations and will give rise to the topological SC under proper conditions. In addition to enriching the structural phases of TMDCs, our work predicts a series of SC candidates with high intrinsic TC and topological non-triviality used for fault-tolerant quantum computation.

Weak electron-phonon coupling contributing to enhanced thermoelectric performance in n-type TiCoSb half-Heusler alloys

n-type TiCoSb half-Heusler (HH) alloys show lower thermoelectric performance may be notably owing to the low valley degeneracy of the conduction band. Here, we show that this drawback can be counterbalanced by a decrease in the deformation potential coefficient and hence, weak electron-phonon coupling strength driven by the substitution of Nb for Ti in the n-type alloys Ti1-xNbxCoSb0.96Bi0.04. The combined substitutions of Nb and Bi yield a reduction of ∼86% in the deformation potential of the conduction band minimum, with the lowest value of ∼5 eV at 300 K achieved in Ti0.85Nb0.15CoSb0.96Bi0.04. This effect leads to enhanced power factor from ∼0.018 mW m−1 K−2 for x = 0 to ∼1.69 mW m−1 K−2 for x = 0.15 at RT due to the resulting strong increase in electron mobility by one order of magnitude. Both the isovalent Bi and aliovalent Nb substitutions further contribute to decrease the lattice thermal conductivity owing to enhanced mass and strain field fluctuations. The beneficial combined effects of weaker electron-phonon coupling and enhanced point-defect phonon scattering results in a higher dimensionless thermoelectric figure of merit ZT, with a peak value ∼ 0.37 at 870 K in Ti0.85Nb0.15CoSb0.96Bi0.04, representing a ∼ 375% improvement with respect to pristine TiCoSb.

Imaging Ultrafast Dynamics of Pressure-Driven Phase Transitions in Black Phosphorus and Anomalous Coherent Phonon Softening.

Applying high pressure to effectively modulate the electronic and lattice structures of materials could unravel various physical properties associated with phase transitions. In this work, high-pressure-compatible femtosecond pump-probe microscopy was constructed to study the pressure-dependent ultrafast dynamics in black phosphorus (BP) thin films. We observed pressure-driven evolution of the electronic topological transition and three structural phases as the pressure reached ∼22 GPa, which could be clearly differentiated in the transient absorption images containing spatially resolved ultrafast carrier and coherent phonon dynamics. Surprisingly, an anomalous coherent acoustic phonon mode with pressure softening behavior was observed within the range of ∼3-8 GPa, showing distinct laser power and time dependences. Density functional theory calculations show that this mode, identified as the shear mode along the armchair orientation, gains significant electron-phonon coupling strength from out-of-plane compression that leads to decreased phonon frequency. Our results provide insights into the structure evolution of BP with pressure and hold potential for applications in microelectromechanical devices.

Chemical composition effect on superconductivity in noncentrosymmetric [formula omitted]-Mn-type high-entropy alloys

We report the effect of chemical composition variation on the superconductivity in noncentrosymmetric β-Mn-type high-entropy alloys (HEAs) studied in two very similar Ta5+xMo35−xW5Re35Ru20C20 and Ta5+yW35−yMo5Re35Ru20C20 series. It is found that both HEAs consist of a single cubic β-Mn-type phase for 0 ≤x≤ 6 and 0 ≤y≤ 9. Bulk fully gapped superconductivity is observed for all these HEAs and their zero-temperature upper critical fields approach the Pauli paramagnetic limit. While our analysis suggests that Tc of these HEAs is mainly controlled by the electron–phonon coupling strength, Tc of the Ta5+xMo35−xW5Re35Ru20C20 series is always higher than that of the Ta5+yW35−yMo5Re35Ru20C20 one even for (nearly) the same valence electron concentration and unit-cell volume. This difference is attributed to the different contributions of Mo and W to the electronic structure, which is supported by the first-principles calculations. Our study suggests that the chemical composition effect should be considered to better understand the superconducting behavior in noncentrosymmetric HEAs.

A Strategy for Tuning Electron-Phonon Coupling and Carrier Cooling in Lead Halide Perovskite Nanocrystals.

Perovskites have been recognized as a class of promising materials for optoelectronic devices. We intentionally include excessive Cs+ cations in precursors in the synthesis of perovskite CsPbBr3 nanocrystals and investigate how the Cs+ cations influence the lattice strain in these perovskite nanocrystals. Upon light illumination, the lattice strain due to the addition of alkali metal Cs+ cations can be compensated by light-induced lattice expansion. When the Cs+ cation in precursors is about 10% excessive, the electron-phonon coupling strength can be reduced by about 70%, and the carrier cooling can be slowed down about 3.5 times in lead halide perovskite CsPbBr3 nanocrystals. This work reveals a new understanding of the role of Cs+ cations, which take the A-site in ABX3 perovskite and provide a new way to improve the performance of perovskites and their practical devices further.

Emergence of Phonon‐Mediated Superconductivity in Electron‐Doped Monolayer WS2: First‐Principles Study

Herein, the electronic properties for undoped and carrier‐doped tungsten disulfide (WS2) monolayer are systematically examined by using ab initio calculations. The results show that the pristine single‐layer WS2 is a semiconductor with a direct bandgap nature and the electronic properties of WS2 are similar to 2H‐MoS2 monolayer, which are consistent with previous reports. Besides, considerable changes are observed in the electron‐doped WS2 monolayer when compared to the hole‐doped. The dynamical stability of pristine and carrier‐doped WS2 monolayer is also investigated by performing the phonon dispersion calculations. Further, the possibility of superconducting nature in carrier‐doped single‐layer WS2 is also studied by using the isotropic Migdal–Eliashberg theory with the combination of Wannier–Fourier interpolation. From the computed Eliashberg function, it has been concluded that electron doping to WS2 monolayer promises electron–phonon coupling strength and maximum critical temperature of around 17 K with doping concentration ranging from 0.4 to 0.16 electrons cell−1.

Enhanced carrier transport in CsxSnBry perovskite by reducing electron-phonon coupling under compressive strain

Low-toxicity and environmentally friendly tin-based perovskite materials are attractive substitutes for lead halide perovskites in photovoltaic and optoelectronic devices. However, the polar perovskite lattice coupled with charge carrier, and strong polar optical phonon scattering severely affect the carrier transport. Here, we perform the first-principles calculation, and demonstrate that the carrier mobility can be significantly enhanced by applying compressive strain to the lattice, which can be attributed to the reduction of the electron-phonon coupling. Pressure-induced electron-phonon coupling strength evolutions correlate well with the polar optical phonon scattering changes. The maximum carrier mobility is 11 cm2 V−1s−1 and 143 cm2 V−1s−1 of Cs2SnBr6 with the unstrained and strained structure (13 % compression). The carrier mobility of CsSnBr3 with 1 % compression is improved due to a significant dielectric response induced by the dynamic lone pair activity of CsSnBr3. These studies indicate that compressive strain can significantly alter the structure and carrier transport characteristics of tin-based perovskite materials, which are important for photovoltaics and optoelectronics.

Phonon-assisted upconversion photoluminescence in Mn-doped two-dimensional hybrid metal halides

Phonon-assisted upconversion process is one of the important means to generate upconversion photoluminescence (UCPL), and has important applications in laser refrigeration and other fields. However, until now, the studies on UCPL behavior are still insufficient. Herein, this work synthesizes a series of Mn-doped two-dimensional hybrid metal halide (2D HMH) thin films and investigates their optical properties using various spectral techniques. Raman spectroscopic measurement confirms that Mn-doping is achieved via interstitial doping rather than Pb-substitution. By the measurement of the temperature-dependent PL spectrum, it is found that Mn-doping will weaken the thermal expansion effect of 2D HMHs, but will enhance the electron–phonon coupling strength. More importantly, both two-photon-excited and phonon-assisted UCPL are observed in Mn-doped 2D HMHs, with an extremely large phonon-assisted energy gain (approximately 500[Formula: see text]meV). Our experimental results are of significance for designing phonon-assisted UCPL materials and expanding their applications.

Separated Electron-Phonon and Phonon-Phonon Scatterings Across Interface in Thin Film LaCoO3 /SrTiO3.

Electron-phonon coupling (EPC) and phonon-phonon scattering (PPS) are at the core of the microscopic physics mechanisms of vast quantum materials. However, to date, there are rarely reports that these two processes can be spatially separated, although they are usually temporally detached with different characteristic lifetimes. Here, by employing ultrafast spectroscopy to investigate the photo-carrier ultrafast dynamics in a LaCoO3 thin film on a (100) SrTiO3 substrate, intriguing evidence is found that the two interactions are indeed spatially separated. The EPC mainly occurs in the thin film, whereas PPS is largely in the substrate, especially at the several atomic layers near the interface. Across-interface penetration and decay of optical phonons into acoustic phonons thus naturally occur. An EPC strength λEg =0.30 is also obtained and an acoustic phonon mode at 45.3GHz is observed. The finding lays out a cornerstone for future quantum nano device designs.