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Molecular dynamics simulations were conducted using the generalized replica exchange method (gREM) on the 4-cyano-4′-n-alkyl biphenyl (nCB) system with n = 5, 6, 7, and 8, which exhibits a nematic–isotropic (NI) phase transition. Sampling near the phase transition temperature in systems undergoing first-order phase transitions, such as the NI phase transition, is demanding due to the substantial energy gap between the two phases. To address this, gREM, specifically designed for first-order phase transitions, was utilized to enhance sampling near the NI phase transition temperature. Free-energy calculations based on the energy representation (ER) theory were employed to characterize the NI phase transition. ER evaluates the insertion free energy of the nCB molecule for both nematic and isotropic phases, revealing a change in the temperature dependence across the NI phase transition. Further decomposition into energetic and entropic terms quantitatively shows the balance between these contributions at the NI phase transition temperature. [ABSTRACT FROM AUTHOR] more...

Much can be learned about molecular aggregates by modeling their fluorescence-type spectra. In this study, we systematically describe the accuracy of various methods for simulating fluorescence-type linear spectra in a dimer system with a complex system–environment interaction, which serves as a model for various molecular aggregates, including most photosynthetic light-harvesting complexes (LHCs). We consider the approximate full cumulant expansion (FCE), complex time-dependent Redfield (ctR), time-independent Redfield, and modified Redfield methods and calculate their accuracy as a function of the site energy gap and coupling, excitonic energy gap, and dipole factor (i.e., type of spectrum). We find that the FCE method is the most accurate method for couplings smaller than 300 cm−1 at 300 K, but this method fails for very strong couplings or low temperatures due to inaccurate modeling of the equilibrium initial state. The ctR method performs well for the calculation of fluorescence and linear anisotropy spectra but poorer for circularly polarized fluorescence spectra or for all spectra when the coupling is strong (∼ 100 c m − 1 ). The Redfield and modified Redfield methods generally perform much more poorly than the ctR and FCE methods—especially for small excitonic energy gaps and strong couplings. We show that accurate modeling of the Stokes shift is crucial and present a version of the ctR method that treats both the Stokes shift and initial state correctly for the parameter ranges in plant LHCs. Apart from the application to LHCs, our results will be useful for the spectral characterization and design of organic molecular aggregates. [ABSTRACT FROM AUTHOR] more...

Endohedral and exohedral fullerenes have both been employed as electron acceptors in polymer solar cells (PSCs). However, their differences in hot-electron relaxation dynamics remain unclear. Previous studies have shown that the location of a single atom, whether inside or outside the fullerene cage, results in significant differences in charge distribution. In this work, the hot-electron relaxations of endohedral B@C60+ and exohedral C60B+ are investigated using nonadiabatic molecular dynamics simulations. Our results reveal that the location of the boron atom—inside or outside the fullerene—significantly impacts the bonding interactions between boron and C60. Compared to C60B+, the weaker interactions in B@C60+ reduce the orbital overlap between LUMO+3 and LUMO+2 and increase the energy gap between them. This, in turn, slows hot-electron relaxation by weak nonadiabatic coupling, making B@C60+ more suitable for PSC applications. This study provides valuable insights into how atomic positioning affects the electronic properties in fullerene-based materials, contributing to the design of more efficient electron acceptors for photovoltaic devices. [ABSTRACT FROM AUTHOR] more...

Organic materials typically do not phosphoresce at room temperature because both intersystem crossing (ISC) and phosphorescence back to the electronic ground state are slow, compared to the nonradiative decay processes. A group of organic guest–host molecules breaks this rule. Their phosphorescence at room temperature can last seconds with a quantum efficiency of over 10%. This extraordinary phenomenon is investigated with comprehensive static and transient spectroscopic techniques. Time-resolved vibrational and fluorescence spectral results suggest that a singlet guest–host exciplex quickly forms after excitation. The formation of exciplex reduces the singlet–triplet energy gap and helps facilitate charge separation that can further diffuse into the host matrix. The heavy atoms (P or As) of the host molecule can also help enhance the spin orbital coupling of the guest molecule. Both boost the rate of ISC. After the singlet exciplex transforms into the triplet exciplex through the ISC process, UV–visible transient absorption spectroscopic measurements support that the triplet exciplex quickly transforms into the guest molecule triplet state that is at a lower energy level, thereby reducing the reverse ISC-induced triplet population loss. Finally, the long-lasting separated charges that diffused into the host matrix can diffuse back to the guest hole to form new triplets, and the dilution effect of the host molecules can effectively reduce the triplet quenching. All these factors contribute to the dramatic enhancement of phosphorescence at room temperature. [ABSTRACT FROM AUTHOR] more...

Two-dimensional electron gas (2DEG) confined at the interface of SrTiO3-based heterostructure exhibits intriguing electronic and optoelectronic properties. In this work, we study the ultrafast dynamics of 2DEG at the Al2O3/SrTiO3 interface using surface-specific terahertz difference-frequency spectroscopy. Through proper polarization selection, we have resolved simultaneously the evolution of 2DEG confined in the quantum well and the surface potential after optical pump with different photon energies. The hot electrons excited from 2DEG with pump photon energy below the band gap relax to the ground state through two processes, a fast interfacial process associated with electron–electron and electron–phonon scattering on the order of tens of picoseconds and a slow surface-to-bulk transport on the order of hundreds of picoseconds. When the pump photon energy exceeds the bandgap, electrons are directly injected from the valence band to 2DEG at the interface and relax via electron–hole recombination in 3 ps. The recorded dynamic change of interfacial potential provides the key information to identify the drift and diffusion of photocarriers at the interface. Our results broaden the horizon of investigation on the comprehension of complex oxide interfaces and their photonics capabilities. [ABSTRACT FROM AUTHOR] more...

The CO reduction reaction (CORR) for the production of high-value-added multi-carbon (C2+) products is currently being actively investigated, where searching for high-efficiency catalysts with moderate CO intermediate binding strength and low kinetic barrier for C–C coupling poses a significant challenge. In this study, we employed density functional theory computations to design four synergistic coupling dual sites catalysts for CORR to C2 products, namely, TM-P@melon, by co-doping transition metals (TM = Mn, Fe, Co, and Ni) and phosphorus (P) into the polymeric carbon nitride (i.e., melon-CN). Mn–P@melon and Ni–P@melon exhibit higher selectivity toward C2H5OH and C2H6, respectively, with limiting potentials (C–C coupling kinetic energy barriers) of −0.43 V (0.52 eV) and −0.17 V (0.26 eV), respectively. The introduction of TM and P atoms not only narrows the band gap of melon-CN but also favors the coupling of CO and *CHO, providing an active site for C–C coupling, thus facilitating the catalytic reaction. Our work provides rational insights for the design of stable, low-cost, and efficient CORR dual sites catalysts that facilitate the sustainable production of high-value C2 chemicals and fuels. [ABSTRACT FROM AUTHOR] more...

The technologically important Cu-chalcogenides, such as Cu2Se and CuInSe2, usually have relatively small band gaps. Achieving a reliable yet efficient description of the electronic properties has proven to be quite challenging for the popular exchange-correlation functionals of density functional theory, primarily due to the involvement of full-yet-shallow Cu-3d orbitals. In this study, we evaluate the applicability of several meta-generalized gradient approximation (GGA) functionals that have been recently developed. We find that the r2SCAN (regularized-restored strongly constrained and appropriately normed) functional significantly improves upon conventional local density approximation and GGA in terms of geometry and electronic band structure; however, there is still a notable discrepancy with experimental results due to the remaining delocalization error. This error is mitigated by combining r2SCAN with a Hubbard-like U correction applied to the Cu-3d orbitals. For predicting band gaps, both the TASK functional and the mBJ potential, when combined with the U correction, demonstrate similar accuracies with a mean absolute error of 0.17–0.19 eV. This accuracy is lower than that achieved with the many-body Hedin's GW approximation method but more accurate than that of hybrid functionals. Moreover, the r2SCAN+U approach well reproduces the phonon dispersion in CuInSe2, revealing a neglected computational problem in previous reports. We conclude that the meta-GGA+U approach represents a significant advancement by striking a balance between reliability and computational effort, and further efforts are still required to describe the Cu-3d orbitals more accurately. [ABSTRACT FROM AUTHOR] more...

The dynamics of molecular excitonic systems are complicated by a competition between electronic coupling (which drives delocalization) and vibrational-electronic (vibronic) interactions (which tend to encourage electronic localization). A particular challenge of molecular systems is that they typically possess a large number of independent vibrations, with frequencies often spanning the entire spectrum of relevant electronic energy gaps. Recent spectroscopic observations and numerical simulations on a water-soluble chlorophyll-binding protein (WSCP) reveal a transition between two regimes of vibronic behavior, a Redfield-like regime in which low-frequency vibrations respond to a delocalized excitonic state, and a Förster-like regime where high-frequency vibrations act as incoherent excitations on individual pigments. Although numerical simulations can reproduce these effects, there is a need for a simple, systematic theory that accurately describes the smooth transition between these two regimes in experimental spectra. Here we address this challenge by generalizing the variational polaron transform approach of [Bloemsma et al., Chem. Phys. 481, 250 (2016)] to include arbitrary bath densities for systems with or without symmetry. We benchmark this theory against both numerical matrix-diagonalization methods and experimental 77 K fluorescence spectra for two WSCP variants, obtaining quite satisfactory agreement in both cases. We apply this theory to offer an explanation for the large loss in apparent electronic coupling in the WSCP Q57K mutant and to examine the likely impact of the interplay between excitonic delocalization and vibrational localization on vibrational sideband shapes and apparent coupling strengths in high-resolution optical spectra for chlorophyll-protein complexes such as WSCP. [ABSTRACT FROM AUTHOR] more...

Experimental rate coefficients for the quenching of vibrational levels 0 and 1 of the N 2 + A 2 Π u state by N2 are presented. The experiments were performed using near-infrared observations of the N 2 + Meinel bands excited by electron impact at several pressures of the N2 target/quenching gas. The total removal rate coefficients were derived from a Stern–Volmer analysis of the Meinel band intensities as a function of N2 density and yielded rate coefficients of (2.5 ± 0.5 × 10−10) and (5.6 ± 0.6 × 10−10) cm3⋅molecule−1⋅s−1 for vibrational levels 0 and 1, respectively. It is shown that rate coefficients increase with increasing vibrational level and decreasing energy gap. Our results impact modeling studies of the disturbed atmosphere and ionosphere as the reduced quenching rate coefficients for the preferentially excited A-state vibrational levels <2 lower the quenching altitude in the atmosphere by one scale height, or about 6 km. [ABSTRACT FROM AUTHOR] more...

I applied photovoltaic cells equipped with singlet fission (SF) of molecular systems to dual-wavelength laser power converters (DW-LPCs) that efficiently convert two laser lights of different wavelengths to electricity. When the SF-DW-LPC is illuminated by eye-safe laser light of 1470 nm wavelength emitted from a laser diode, a single photon is converted to a single carrier. On the other hand, a single high-energy photon emitted from a high-power and low-cost laser diode of 808 nm is converted to two carriers by SF owing to its endothermic feature, even though the photon energy is slightly lower than twice the fundamental energy gap. Furthermore, the SF-DW-LPC operates as a highly efficient solar cell. These functions are required for optical wireless power transmission to moving objects including electric vehicles and flying drones. I modeled the photovoltaic process with SF and evaluated the limiting conversion efficiencies by detailed-balance calculations. Conversion efficiencies of the SF-DW-LPC for these two laser lights are competitive with those of the conventional single-junction LPCs dedicated to these wavelengths, respectively. The efficiency under solar light is close to that of the optimally designed SF solar cell. Furthermore, the SF-DW-LPC outperforms other types of DW-LPCs designed on the basis of intermediate band, triplet–triplet annihilation, and multiple exciton generation solar cells. Endothermic SF and carrier/energy extraction into the neighboring acceptors have already been demonstrated. However, molecular systems that apply to 1470 nm have not yet been realized, which is the top-priority issue to be solved to realize highly efficient SF-DW-LPCs. [ABSTRACT FROM AUTHOR] more...

Cobalt oxides are known for their excellent heat transfer properties. The main component of cobalt oxides is the CoO2 monolayer, which exhibits high-temperature superconductivity caused by strong electron–phonon coupling (EPC). We here systematically investigate the structural stability, electronic structure, and magnetism of the CoO2 monolayer using first-principles and Monte Carlo simulations. On this basis, we further study the changes in the spin energy gap, magnetic axis direction, and other properties of the CoO2 monolayer with the changes in carrier concentration. By appropriately doping the CoO2 monolayer with holes, the magnetic axis direction of the CoO2 monolayer can be reversed, thereby enhancing its potential application in the field of spin electronic devices. Monte Carlo simulation is used to study the regulation of different factors on the magnetothermal properties of the CoO2 monolayer. Through the analysis of physical parameters such as Curie temperature (TC) and bandgap, we find that the appropriate carrier concentration and magnetic field can not only regulate the magnetothermal properties of materials but also further improve the efficiency of materials in low-temperature environments. [ABSTRACT FROM AUTHOR] more...

Spin–orbit coupling induces a current density in the ground state, which consequently requires a generalization for meta-generalized gradient approximations. That is, the exchange–correlation energy has to be constructed as an explicit functional of the current density, and a generalized kinetic energy density has to be formed to satisfy theoretical constraints. Herein, we generalize our previously presented formalism of spin–orbit current density functional theory [Holzer et al., J. Chem. Phys. 157, 204102 (2022)] to non-magnetic and magnetic periodic systems of arbitrary dimension. In addition to the ground-state exchange–correlation potential, analytical derivatives such as geometry gradients and stress tensors are implemented. The importance of the current density is assessed for band gaps, lattice constants, magnetic transitions, and Rashba splittings. In the latter, the impact of the current density may be larger than the deviation between different density functional approximations. [ABSTRACT FROM AUTHOR] more...

Environmental effects in excitation energy transfer have mostly been modeled by baths of harmonic oscillators, but to what extent such modeling provides a reliable description of actual interactions between molecular systems and environments remains an open issue. We address this issue by investigating fluctuations in the excitation energies of the light harvesting 2 complex using a realistic all-atomistic simulation of the potential energy surface. Our analyses reveal that molecular motions exhibit significant anharmonic features, even for underdamped intramolecular vibrations. In particular, we find that the anharmonicity contributes to the broadening of spectral densities and substantial overlaps between neighboring peaks, which complicates the meaning of mode frequencies constituting a bath model. Thus, we develop a strategy to construct a minimally underdamped harmonic bath that has a clear connection to all-atomistic dynamics by utilizing actual normal modes of molecules but optimizing their frequencies such that the resulting bath model can best reproduce the all-atomistic simulation results. By subtracting the underdamped contribution from the entire fluctuations, we also show that identifying a residual spectral density representing all other contributions with overdamped behavior is possible. We find that this can be fitted well with a well-established analytic form of a spectral density function or, alternatively, modeled as explicit time dependent fluctuations with muti-exponential or power law type correlation functions. We provide an assessment and the implications of these possibilities. The approach presented here can also serve as a general strategy to construct a simplified bath model that can effectively represent the underlying all-atomistic bath dynamics. [ABSTRACT FROM AUTHOR] more...

Optical eigenstates with a high quality (Q) factor provide substantial advantages for a broad spectrum of optical devices, particularly those demanding strong light–matter interactions. Recently, it has been demonstrated that ultrahigh- Q resonances can be realized in planar photonic structures by merging multiple bound states in the continuum (BICs) in the momentum space. Photonic lattices with thin-film geometry are known to support abundant TE-polarized and TM-polarized BICs. While prior research has explored the merging of TE-polarized BICs, this paper presents analytical and numerical results concerning the merging of TM-polarized BICs in laterally periodic one-dimensional photonic lattices. As the thickness of photonic lattices increases, TM-polarized accidental BICs descend along the dispersion curves and eventually merge at the upper edge of the second stop band. Employing coupled-mode analysis, we calculate the analytical merging thickness at which multiple TM-polarized BICs come together at the second-order Γ point. We confirm the merging of TM-polarized BICs through finite-element method simulations. Our results can be beneficial for achieving ultrahigh- Q resonances through the merging of BICs. [ABSTRACT FROM AUTHOR] more...

Continuum- or discrete-polarizable models for the study of optoelectronic processes in embedded subsystems rely mostly on the restriction of the surrounding electronic dielectric response to its low frequency limit. Such a description hinges on the assumption that the electrons in the surrounding medium react instantaneously to any excitation in the central subsystem, thus treating the environment in the adiabatic limit. Exploiting a recently developed embedded GW formalism with an environment described at the fully ab initio level, we assess the merits of the adiabatic limit with respect to an environment where the full dynamics of the dielectric response are considered. Furthermore, we show how to properly take the static limit of the environment's susceptibility by introducing the so-called Coulomb-hole and screened-exchange contributions to the reaction field. As a first application, we consider a C60 molecule at the surface of a C60 crystal, namely, a case where the dynamics of the embedded and embedding subsystems are similar. The common adiabatic assumption, when properly treated, generates errors below 10% on the polarization energy associated with frontier energy levels and associated energy gaps. Finally, we consider a water molecule inside a metallic nanotube, the worst case for the environment's adiabatic limit. The error on the gap polarization energy remains below 10%, even though the error on the frontier orbital polarization energies can reach a few tenths of an electronvolt. [ABSTRACT FROM AUTHOR] more...

Pentacene is one of the most investigated organic semiconductors. It is well known that the motion of excitons in pentacene and other organic semiconductors is determined by inter-molecular exciton coupling based on charge-transfer processes. In the present study, we demonstrate the impact of the admixture of tetracene, which has a larger band gap and interrupts the pentacene–pentacene interaction, on the exciton behavior in pentacene. Using a combination of optical absorption and electron energy-loss spectroscopy, we show that both the Davydov splitting and the exciton band width in pentacene strongly decrease with increasing tetracene concentration, while the decrease of the exciton band width is substantially larger. [ABSTRACT FROM AUTHOR] more...

We present a systematic study of the electronic properties of dangling bonds (DBs) in a variety of semiconductors and examine the relationship between DBs and the charge neutrality level (CNL) in the context of band alignments of semiconductors. We use first-principles calculations based on density functional theory to assess the energetics of DBs in a set of diamond-structure group-IV and III–V or II–VI zinc-blende-structure semiconductors, considering both cation and anion-derived states. We examine the charge-state transition levels of DBs to assess whether they can serve as a CNL to align band structures, by comparing with offsets calculated from interface calculations. Our results show that this approach for evaluating the CNL yields quantitative results for band offsets and provides useful insights. We discuss the relation with alternative approaches for determination of CNLs based on branch-point energies or transition levels of interstitial hydrogen. [ABSTRACT FROM AUTHOR] more...

Two-dimensional (2D) piezoelectric nanomaterials have widely been studied recently due to their promise for various applications in technology. Investigation of vertical piezoelectricity will contribute to a deeper understanding of the intrinsic mechanism of piezoelectric effects in the 2D structures. In this paper, we report a first-principle study for the structural, electronic, piezoelectric, and transport properties of new-designed Janus WSi Z 3 H (Z = N, P, and As) monolayers. The structural stability of WSi Z 3 H is theoretically confirmed based on the energetic, phonon dispersion, and also elastic analyses. At the ground state, while WSiN 3 H is an indirect semiconductor, both WSiP 3 H and WSiAs 3 H are predicted to be direct semiconductors with smaller bandgaps. When the spin-orbit coupling effects are taken into account, a large valley spin splitting is observed at the K point of WSi Z 3 H materials. Interestingly, a giant Rashba spin splitting is found in WSiP 3 H and WSiAs 3 H with Rashba constant α R up to 770.91 meV Å. Additionally, our first-principles study indicates that Janus WSi Z 3 H monolayers are piezoelectric semiconductors with high out-of-plane piezoelectric coefficient | d 31 | , up to 0.15 pm/V, due to the broken mirror symmetry. Besides, with high electron mobilities and also possessing direct band gaps, WSiP 3 H and WSiAs 3 H monolayers are favorable for applications in optoelectronics. [ABSTRACT FROM AUTHOR] more...

The second order cumulant method offers a promising pathway to predicting optical properties in condensed phase systems. It allows for the computation of linear absorption spectra from excitation energy fluctuations sampled along molecular dynamics (MD) trajectories, fully accounting for vibronic effects, direct solute–solvent interactions, and environmental polarization effects. However, the second order cumulant approximation only guarantees accurate line shapes for energy gap fluctuations obeying Gaussian statistics. A third order correction has recently been derived but often yields unphysical spectra or divergent line shapes for moderately non-Gaussian fluctuations due to the neglect of higher order terms in the cumulant expansion. In this work, we develop a corrected cumulant approach, where the collective effect of neglected higher order contributions is approximately accounted for through a dampening factor applied to the third order cumulant term. We show that this dampening factor can be expressed as a function of the skewness and kurtosis of energy gap fluctuations and can be parameterized from a large set of randomly sampled model Hamiltonians for which exact spectral line shapes are known. This approach is shown to systematically remove unphysical contributions in the form of negative absorbances from cumulant spectra in both model Hamiltonians and condensed phase systems sampled from MD and dramatically improves over the second order cumulant method in describing systems exhibiting Duschinsky mode mixing effects. We successfully apply the approach to the coumarin-153 dye in toluene, obtaining excellent agreement with experiment. [ABSTRACT FROM AUTHOR] more...

Diffusion of electrons over distances on the order of 100 μm has been observed in crystals of a small tetraheme cytochrome (STC) from Shewanella oneidensis [J. Huang et al. J. Am. Chem. Soc. 142, 10459–10467 (2020)]. Electron transfer between hemes in adjacent subunits of the crystal is slower and more strongly dependent on temperature than had been expected based on semiclassical electron-transfer theory. We here explore explanations for these findings by molecular-dynamics simulations of crystalline and monomeric STC. New procedures are developed for including time-dependent quantum mechanical energy differences in the gap between the energies of the reactant and product states and for evaluating fluctuations of the electronic-interaction matrix element that couples the two hemes. Rate constants for electron transfer are calculated from the time- and temperature-dependent energy gaps, coupling factors, and Franck–Condon-weighted densities of states using an expression with no freely adjustable parameters. Back reactions are considered, as are the effects of various protonation states of the carboxyl groups on the heme side chains. Interactions with water are found to dominate the fluctuations of the energy gap between the reactant and product states. The calculated rate constant for electron transfer from heme IV to heme Ib in a neighboring subunit at 300 K agrees well with the measured value. However, the calculated activation energy of the reaction in the crystal is considerably smaller than observed. We suggest two possible explanations for this discrepancy. The calculated rate constant for transfer from heme I to II within the same subunit of the crystal is about one-third that for monomeric STC in solution. [ABSTRACT FROM AUTHOR] more...

Transient absorption (TA) spectroscopy of semiconductor nanocrystals (NCs) is often used for excited state population analysis, but recent results suggest that TA bleach signals associated with multiexcitons in NCs do not scale linearly with exciton multiplicity. In this manuscript, we probe the factors that determine the intensities and spectral positions of exciton and biexciton components in the TA spectra of CdSe quantum dots (QDs) of five diameters. We find that, in all cases, the peak intensity of the biexciton TA spectrum is less than 1.5 times that of the single exciton TA spectrum, in stark contrast to a commonly made assumption that this ratio is 2. The relative intensities of the biexciton and exciton TA signals at each wavelength are determined by at least two factors: the TA spectral intensity and the spectral offset between the two signals. We do not observe correlations between either of these factors and the particle diameter, but we find that both are strongly impacted by replacing the native organic surface-capping ligands with a hole-trapping ligand. These results suggest that surface trapping plays an important role in determining the absolute intensities of TA features for CdSe QDs and not just their decay kinetics. Our work highlights the role of spectral offsets and the importance of surface trapping in governing absolute TA intensities. It also conclusively demonstrates that the biexciton TA spectra of CdSe QDs at the band gap energy are less than twice as intense as those of the exciton. [ABSTRACT FROM AUTHOR] more...

Mn-doped phosphors exhibiting self-reduction behavior have garnered significant attention in the study of luminescent materials due to the defects generated during the self-reduction process and their unique luminescent behavior. In this paper, LiScGeO 4 red phosphors activated by the self-reduction of Mn4+ to Mn2+ were synthesized by high-temperature solid-state reaction in an air atmosphere. The defects generated during the self-reduction process were leveraged to attain exceptional anti-thermal quenching characteristics, with luminescent intensity at a high temperature of 430 K being 1.23 times compared to that at room temperature of 300 K. In addition, a peculiar phenomenon occurred where the emission peak initially blueshifts and subsequently redshifts with the increasing temperature. This study includes an analysis of the Rietveld-refined lattice parameters and surface micromorphology of the samples. The theoretical energy gap of the perfect LiScGeO 4 matrix was calculated using density functional theory. Furthermore, the unique emission peak shift characteristics of Mn2+ were elucidated through the interaction between Mn2+ ions and the strength of the crystal field. Utilizing a defect model, the self-reduction mechanism and the anti-thermal quenching behavior were clarified. These findings will enhance the understanding of the effects of crystal defects and ion pair interactions on luminescent materials, and encourage further explorations of self-reducing phosphors to develop new high thermal stability phosphors for practical applications. [ABSTRACT FROM AUTHOR] more...