Intermediate State Research Articles

Unraveling the interplay between the leucine zipper and forkhead domains of FOXP2: Implications for DNA binding, stability and dynamics.

FOXP2 is a transcription factor associated with speech and language. Like other FOX transcription factors, it has a DNA binding region called the forkhead domain (FHD). This domain can exist as a monomer or a domain swapped dimer. In addition to the FHD, the leucine zipper region (LZ) of FOXP2 is also believed to be associated with both DNA binding and oligomerization. To better understand the relationship between DNA binding and oligomerization of FOXP2, we investigated its structure, stability and dynamics, focusing specifically on the FHD and the LZ. We did this by using two constructs: one containing the isolated FHD and one containing both the LZ and the FHD (LZ-END). We demonstrate in this work, that while the FHD maintains a monomeric form that is capable of binding DNA, the LZ-END undergoes a dynamic transition between oligomeric states in the presence of DNA. Our findings suggest that FOXP2's LZ domain influences DNA binding affinity through a change in oligomeric state. We show through hydrogen exchange mass spectroscopy that certain parts of the FHD and interlinking region become less dynamic when in the presence of DNA, confirming DNA binding and oligomerization in these regions. Moreover, the detection of a stable equilibrium intermediate state during LZ-END unfolding supports the idea of cooperation between these two domains. Overall, our study sheds light on the interplay between two FOXP2 domains, providing insight into the protein's ability to respond dynamically to DNA, and enriching our understanding of FOXP2's role in gene regulation.

Electromagnetically-induced transparency assists the Raman gradient echo memory at moderate detuning, dependent on gradient order

Abstract Optical quantum memories are essential for quantum communications and photonic quantum technologies. Ensemble optical memories based on 3-level interactions are a popular basis for implementing these memories. All such memories, however, suffer from loss due to scattering. In off-resonant 3-level interactions, such as the Raman gradient echo memory (GEM), scattering loss can be reduced by a large detuning from the intermediate state. In this work, we show how electromagnetically induced transparency adjacent to the Raman absorption line plays a crucial role in reducing scattering loss, so that maximum efficiency is in fact achieved at a moderate detuning. Furthermore, the effectiveness of the transparency, and therefore the efficiency of GEM, depends on the order in which gradients are applied to store and recall the light. We provide a theoretical analysis and show experimentally how the efficiency depends on gradient order and detuning.

Unveiling the Multielectron Acceptor Properties of π-Expanded Pyracylene: Reversible Boat to Chair Conversion.

In this work, the chemical reduction of a hybrid pyracylene-hexa-peri-hexabenzocoronene (HPH) nanographene was investigated with different alkali metals (Na, K, Rb) to reveal its remarkable multielectron acceptor abilities. The UV-vis and 1H NMR spectroscopy monitoring of the stepwise reduction reactions supports the existence of all intermediate reduction states up to the hexaanion for HPH. Tuning the experimental conditions enabled the synthesis of the HPH anions with gradually increasing reduction states (up to -5) isolated with different alkali metal ions as crystalline materials. The single-crystal X-ray diffraction structure analysis demonstrates that the highly negatively charged HPH anions (-4 and -5) exhibit a drastic geometry change from boat-shaped (observed in the neutral parent, mono- and dianions) to a chair conformation, which was proved to be fully reversible by NMR spectroscopy. DFT calculations show that this geometry change is induced by an enhanced interaction between the coordinated metal ions and negatively charged HPH core in the chair conformation.

Analysis of early intermediate states of the nitrogenase reaction by regularization of EPR spectra

Due to the complexity of the catalytic FeMo cofactor site in nitrogenases that mediates the reduction of molecular nitrogen to ammonium, mechanistic details of this reaction remain under debate. In this study, selenium- and sulfur-incorporated FeMo cofactors of the catalytic MoFe protein component from Azotobacter vinelandii are prepared under turnover conditions and investigated by using different EPR methods. Complex signal patterns are observed in the continuous wave EPR spectra of selenium-incorporated samples, which are analyzed by Tikhonov regularization, a method that has not yet been applied to high spin systems of transition metal cofactors, and by an already established grid-of-error approach. Both methods yield similar probability distributions that reveal the presence of at least four other species with different electronic structures in addition to the ground state E0. Two of these species were preliminary assigned to hydrogenated E2 states. In addition, advanced pulsed-EPR experiments are utilized to verify the incorporation of sulfur and selenium into the FeMo cofactor, and to assign hyperfine couplings of 33S and 77Se that directly couple to the FeMo cluster. With this analysis, we report selenium incorporation under turnover conditions as a straightforward approach to stabilize and analyze early intermediate states of the FeMo cofactor.

Understanding the Impact of Chain Mobility on Conformational Evolution and Kinetics of Mesophase Formation in Poly(ʟ-lactide) under Low-Pressure CO2

Although the mesomorphic phase as an intermediate state has been introduced to understand polymer crystallization, the understanding of the mesomorphic phase is far from complete. Here, the effect of chain mobility on the mesophase structuring in melt-quenched poly(ʟ-lactide) (PLLA) treated in low-pressure CO2 at 1.6–2.0 MPa and 0 °C was investigated using infrared (IR) spectroscopy, differential scanning calorimetry (DSC), and atomic force microscopy (AFM). The IR and AFM results demonstrated that the final degree of order and the kinetics of structural evolution during the CO2-induced mesophase formation were critically dependent on the CO2 pressure. This was attributed to the distinct dynamics of conformational evolution (gg to gt conformer transition) due to the different CO2 pressures. The thermal behavior from the DSC results showed that CO2 pressure dominated both the scale and dynamics of the chain motion of PLLA. At a lower CO2 pressure of 1.6 MPa, smaller-scale segmental motion was not replaced by the larger-scale cooperative motion that occurred at a relatively higher CO2 pressure of 2 MPa, which was favorable for faster mesophase formation. Consequently, by inhibiting direct crystallization under limited mobility conditions, it was demonstrated that varying the chain mobility controlled by CO2 pressure and thus CO2 solubility impacted the dynamics of the mesophase formation of PLLA. The present results have implications for understanding the role of chain mobility in determining the intermediate structural phases in semicrystalline polymers.

Long‐time high‐pressure processing of a patatin‐rich potato proteins isolate: impact on aggregation and surface properties

SummaryIn this study, a 4% (w/w) dispersion of a commercial patatin‐rich potato protein isolate (Po‐PI) was pressurised at 400 MPa up to 48 h at 20 °C. Protein aggregation induced by high‐pressure processing (HHP) was followed by dynamic light scattering, intrinsic fluorescence (in‐situ or ex‐situ) or SAXS analysis. Surface properties (surface hydrophobicity and interfacial properties) of the HHP‐induced aggregates were also investigated. A gradual dimer dissociation/protein unfolding was observed under pressure. Po‐PI exhibited a slow relaxation time under pressure. Long‐time HHP (>4 h) induced significant modification of the Po‐PI protein structure with partial non‐reversible unfolding. After 48 h of pressurisation at 400 MPa, large aggregates (160 nm) were obtained and a monomodal distribution in intensity and in number frequency was observed indicating a controlled aggregation. Up to 24 h of pressurisation at 400 MPa, intermediate states were obtained after high‐pressure release. SDS‐PAGE profiles showed that HHP‐induced aggregation of Po‐PI was driven by non‐covalent interactions. All high‐pressure processed dispersions displayed a higher surface hydrophobicity as compared to non‐treated Po‐PI. Po‐PI dispersion treated for 8 h at 400 MPa presented the lowest adsorption rate, the highest final surface tension and formed the most rigid interfacial film. Po‐PI showed resistance to moderate pressure levels (400 MPa) and long pressure application times were required to induce significant protein denaturation/aggregation (≥24 h) and to optimally modify its interfacial properties (8 h).

Integration of Co Single Atoms and Ni Clusters on Defect-Rich ZrO2 for Strong Photothermal Coupling Boosts Photocatalytic CO2 Reduction.

We report a solvothermal method for the synthesis of an oxygen vacancy-enriched ZrO2 photocatalyst with Co single atoms and Ni clusters immobilized on the surface. This catalyst presents superior performance for the reduction of CO2 in H2O vapor, with a CO yield reaching 663.84 μmol g-1 h-1 and a selectivity of 99.52%. The total solar-to-chemical energy conversion efficiency is up to 0.372‰, which is among the highest reported values. The success, on one hand, depends on the Co single atoms and Ni clusters for both extended spectrum absorption and serving as dual-active centers for CO2 reduction and H2O dissociation, respectively; on the other hand, this is attributed to the enhanced photoelectric and thermal effect induced by concentrated solar irradiation. We demonstrate that an intermediate impurity state is formed by the hybridization of the d-orbital of single-atom Co with the molecular orbital of H2O, enabling visible-light-driven excitation over the catalyst. In addition, Ni clusters play a crucial role in altering the adsorption configuration of CO2, with the localized surface plasmon resonance effect enhancing the activation and dissociation of CO2 induced by visible-near-infrared light. This study provides valuable insights into the synergistic effect of the dual cocatalyst toward both efficient photothermal coupling and surface redox reactions for solar CO2 reduction.

Introduction of element Bi in the P-block promotes N2 activation for efficient electrocatalytic nitrogen reduction to produce ammonia

The synthesis of ammonia through electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is a presumable strategy. However, it still faces the problems of poor activity and low Faradic efficiency, so the development of efficient, stable and highly selective catalysts is of the importance. Molybdenum disulfide (MoS2) materials are widely used in NRR reactions owing to good electrical conductivity and abundant active sites, but the edge active site is the dual active site of NRR and competitive hydrogen evolution reaction (HER). Encouragingly, the strong interaction between elements in the P-block and N 2p orbitals results in excellent performance in adsorbing and activating nitrogen. Meanwhile, the partial occupation of p-orbitals by elements in the P-block also leads to poor HER activity. Herein, we introduced the P-block element Bi into 1 T-MoS2 and prepared Bi2S3/MoS2 composite. Taking advantage of the high conductivity of 1 T-MoS2 and the N2 adsorption and activation advantages of Bi element, an ammonia yield rate of 54.64 µg h−1 mg−1cat. and a high Faradic efficiency of 58.56 % were obtained. In addition, the active site and the evolution pathway of N2 reduction were investigated by in-situ infrared spectroscopy measurements and density functional theory (DFT). The in-situ infrared spectroscopy measurement results manifested the presence of the main intermediate transition state during the reduction of N2 to NH3. The calculation results indicated that N2 had the best adsorption on the introduced P-block element Bi, and the entire NRR reaction process followed an alternating pathway. This study reveals the synergistic effect of P-block elements and transition metal-based electrocatalytic materials on nitrogen reduction to ammonia synthesis.

Testing the hypothesis that solvent exchange limits the rates of calcite growth and dissolution.

It is established that the rates of solvent exchange at interfaces correlate with the rates of a number of mineral reactions, including growth, dissolution and ion sorption. To test if solvent exchange is limiting these rates, quasi-elastic neutron scattering (QENS) is used here to benchmark classical molecular dynamics (CMD) simulations of water bound to nanoparticulate calcite. Four distributions of solvent exchanges are found with residence times of 8.9 ps for water bound to calcium sites, 14 ps for that bound to carbonate sites and 16.7 and 85.1 ps for two bound waters in a shared calcium-carbonate conformation. By comparing rates and activation energies, it is found that solvent exchange limits reaction rates neither for growth nor dissolution, likely due to the necessity to form intermediate states during ion sorption. However, solvent exchange forms the ceiling for reaction rates and yields insight into more complex reaction pathways.

Structural and Computational Insights into Dynamics and Intermediate States of Orexin 2 Receptor Signaling.

Orexin 2 receptor (OX2R) is a G protein-coupled receptor (GPCR) whose activation is crucial to regulation of the sleep-wake cycle. Recently, inactive and active state structures were determined from X-ray crystallography and cryo-electron microscopy single particle analysis, and the activation mechanisms have been discussed based on these static data. GPCRs have multiscale intermediate states during activation, and insights into these dynamics and intermediate states may aid the precise control of intracellular signaling by ligands in drug discovery. Molecular dynamics (MD) simulations are used to investigate dynamics induced in response to thermal perturbations, such as structural fluctuations of main and side chains. In this study, we proposed collective motions of the TM domain during activation by performing 30 independent microsecond-scale MD simulations for various OX2R systems and applying relaxation mode analysis. The analysis results suggested that TM3 had a vertical structural movement relative to the membrane surface during activation. In addition, we extracted three characteristic amino acid residues on TM3, i.e., Q1343.32, V1423.40, and R1523.50, which exhibited large conformational fluctuations. We quantitatively evaluated the changes in their equilibrium during activation in relation to the movement of TM3. We also discuss the regulation of ligand binding recognition and intracellular signal selectivity by changes in the equilibrium of Q1343.32 and R1523.50, respectively, according to MD simulations and GPCR database. Additionally, the OX2R-Gi signaling complex is stabilized in the conformation resembling a non-canonical (NC) state, which was previously proposed as an intermediate state during activation of neurotensin 1 receptor. Insights into the dynamics and intermediate states during activation gained from this study may be useful for developing biased agonists for OX2R.

The reversal of carbonate wettability via alumina nanofluids: Implications for hydrogen geological storage

Underground hydrogen storage (UHS) has been recognized as a key enabler of the industrial-scale implementation of a hydrogen-based economy. However, the efficiency and storage capacity of hydrogen (H2) in carbonate aquifers can be influenced by the presence of organic acids. Nevertheless, the existing literature contains few investigations of H2/calcite/brine wettability and the influence of organic acids on H2 storability in carbonate reservoirs. Therefore, the present study examines the influence of stearic acid on the dynamic H2/brine wettability of calcite substrates (as a proxy of carbonate formation) under various geological conditions (0.1–20 MPa at 323 K), equilibrated in 10 wt% NaCl brine. In addition, the application of various alumina nanofluid concentrations (0.05, 0.1, 0.25, and 0.75 wt%) is evaluated under the same experimental conditions for enhancing the organic-aged calcite wettability. The results demonstrate a significant impact of stearic acid on the dynamic (advancing and receding) contact angles of the calcite substrates, thereby resulting in a shift from intermediate water-wet to H2-wet conditions, representing an unfavorable state for H2 geological storage. Conversely, the application of alumina nanofluid on the organic-aged calcite substrate enhances the H2/brine/calcite wettability towards an intermediate water-wet state, which is more favorable for H2 residual trapping in carbonate formations. The optimal concentration of alumina nanofluid for the wettability modification of the organically aged calcite samples is found to be 0.25 wt%. These findings highlight the influence of organic acid contamination and the potential of alumina nanofluid application in enhancing H2 geo-storage conditions in carbonate reservoirs.

Stereotactic body radiotherapy takes on Lung Oligometastases: Latest breakthroughs

AbstractLung oligometastases represent an intermediate state of cancer dissemination between localized and widespread metastases. Stereotactic body radiation therapy (SBRT) has emerged as an effective treatment option, with an efficacy comparable to that of surgical resection. This review aimed to provide a comprehensive summary of the latest advancements and controversial issues regarding SBRT for lung oligometastases. It focuses on four crucial perspectives: efficacy of SBRT, optimal patient selection criteria, technological innovations, and synergistic effects of SBRT combined with systemic therapy. Relevant clinical trials investigating SBRT for lung oligometastases have been conducted, with median 1‐ and 5‐year local control rates of 90% and 79%, respectively. The origin of the primary tumor, size and number of lesions, and biomarker profiles were highlighted as pivotal considerations in patient selection. The precise dose delivery was enhanced using robotic SBRT and optimized dose fractionation schemes. Evidence suggests that dose escalation above 100 Gy biologically effective dose may improve tumor control. Combined immunotherapy and SBRT have demonstrated synergistic effects in prolonging progression‐free survival and overall survival. This review provides valuable insights into the precise treatment of oligometastatic lung diseases using SBRT. Further multicenter randomized trials are warranted to develop definitive patient selection criteria and optimize the integration with systemic therapies.

In Vivo Mapping of Myocardial Injury Outside the Infarct Zone: Tissue at an Intermediate Pathological State.

The goal was to determine the feasibility of mapping the injured-but-not-infarcted myocardium using 99mTc-duramycin in the postischemic heart, with spatial information for its characterization as a pathophysiologically intermediate tissue, which is neither normal nor infarcted. Coronary occlusion was conducted in Sprague Dawley rats with preconditioning and 30-minute ligation. Invivo single-photon emission computed tomography was acquired after 3 hours (n=6) using 99mTc-duramycin, a phosphatidylethanolamine-specific radiopharmaceutical. The 99mTc-duramycin+ areas were compared with infarct and area-at-risk (n=8). Cardiomyocytes and endothelial cells were isolated for gene expression profiling. Cardiac function was measured with echocardiography (n=6) at 4 weeks. Invivo imaging with 99mTc-duramycin identified the infarct (3.9±2.4% of the left ventricle and an extensive area 23.7±2.2% of the left ventricle) with diffuse signal outside the infarct, which is pathologically between normal and infarcted (apoptosis 1.8±1.6, 8.9±4.2, 13.6±3.8%; VCAM-1 [vascular cell adhesion molecule 1] 3.2±0.8, 9.8±4.1, 15.9±4.2/mm2; tyrosine hydroxylase 14.9±2.8, 8.6±4.4, 5.6±2.2/mm2), with heterogeneous changes including scattered micronecrosis, wavy myofibrils, hydropic change, and glycogen accumulation. The 99mTc-duramycin+ tissue is quantitatively smaller than the area-at-risk (26.7% versus 34.4% of the left ventricle, P=0.008). Compared with infarct, gene expression in the 99mTc-duramycin+-noninfarct tissue indicated a greater prosurvival ratio (BCL2/BAX [B-cell lymphoma 2/BCL2-associated X] 7.8 versus 5.7 [cardiomyocytes], 3.7 versus 3.2 [endothelial]), and an upregulation of ion channels in electrophysiology. There was decreased contractility at 4 weeks (regional fractional shortening -8.6%, P<0.05; circumferential strain -52.9%, P<0.05). The injured-but-not-infarcted tissue, being an intermediate zone between normal and infarct, is mapped invivo using phosphatidylethanolamine-based imaging. The intermediate zone contributes significantly to cardiac dysfunction.

A cost-effective and high efficient Janus membrane for the treatment of oily brine using membrane distillation

Membrane distillation technology could utilize low-grade heat to desalinate brine, but the membrane material often suffers from disadvantages of low permeation flux and weak robustness to contaminants. To address these issues, the commercial polytetrafluoroethylene (PTFE) membrane was modified by cost-effective chemicals of tannic acid and (3-Aminopropyl)-triethoxysilane (APTES) to construct hydrophilic/underwater superoleophobic nano-rough structures on the surface to enhance its flux and oil-fouling resistance in direct contact membrane distillation. The results show that a high underwater oil contact angle of 180° is observed to the membrane surface due to the rough nanostructures functionalized by abundant hydroxyl groups. Despite the additional mass transfer resistance provided by the rough nanostructures, the flux was increased noticeably. This is mainly attributed to the strong interactions between the abundant hydroxyl groups of hydrophilic layer surface and water molecules, leading to a part of free water staying at intermediate transition state (IW). The mass transfer resistance of the hydrophilic layer itself is reduced as a consequence of decreased evaporation enthalpy of water, thereby increasing the flux. Moreover, while the flux of the pristine membrane is reduced by 84.18%, the flux of Janus membrane remains the same when treating mineral oil brine emulsions with oil concentration up to 1500 ppm in comparison with the result for 35 g l−1 brine solution, indicating that the Janus membrane is safe from the oil contamination. Our work provides a fine guidance for membrane distillation to treat high oily brine.

Midkine promotes renal fibrosis by stabilizing C/EBPβ to facilitate endothelial-mesenchymal transition

Numerous myofibroblasts are arisen from endothelial cells (ECs) through endothelial to mesenchymal transition (EndMT) triggered by TGF-β. However, the mechanism of ECs transforms to a different subtype, or whether there exists an intermediate state of ECs remains unclear. In present study, we demonstrate Midkine (MDK) mainly expressed by CD31 + ACTA2+ECs going through partial EndMT contribute greatly to myofibroblasts by spatial and single-cell transcriptomics. MDK is induced in TGF-β treated ECs, which upregulates C/EBPβ and increases EndMT genes, and these effects could be reversed by siMDK. Mechanistically, MDK promotes the binding ability of C/EBPβ with ACTA2 promoter by stabilizing the C/EBPβ protein. In vivo, knockout of Mdk or conditional knockout of Mdk in ECs reduces EndMT markers and significantly reverses fibrogenesis. In conclusion, our study provides a mechanistic link between the induction of EndMT by TGF-β and MDK, which suggests that blocking MDK provides potential therapeutic strategies for renal fibrosis.

Large-Area Near-Infrared Emission Enhancement on Single Upconversion Nanoparticles by Metal Nanohole Array.

Single lanthanide (Ln) ion doped upconversion nanoparticles (UCNPs) exhibit great potential for biomolecule sensing and counting. Plasmonic structures can improve the emission efficiency of single UCNPs by modulating the energy transferring process. Yet, achieving robust and large-area single UCNP emission modulation remains a challenge, which obstructs investigation and application of single UCNPs. Here, we present a strategy using metal nanohole arrays (NHAs) to achieve energy-transfer modulation on single UCNPs simultaneously within large-area plasmonic structures. By coupling surface plasmon polaritons (SPPs) with higher-intermediate state (1D2 → 3F3, 1D2 → 3H4) transitions, we achieved a remarkable up to 10-fold enhancement in 800 nm emission, surpassing the conventional approach of coupling SPPs with an intermediate ground state (3H4 → 3H6). We numerically simulate the electrical field distribution and reveal that luminescent enhancement is robust and insensitive to the exact location of particles. It is anticipated that the strategy provides a platform for widely exploring applications in single-particle quantitative biosensing.

Contact-angle hysteresis on rough surfaces: mechanical energy balance framework

Using as a starting point conservation of momentum, a multiphase mechanical energy balance equation is derived that accounts for multiple material phases and interfaces present within a moving control volume. This balance is applied to a control volume that is anchored to a three-phase contact line as it advances continuously over the surface of a rough and chemically homogeneous and inert solid. Using semi-quantitative models for the material behaviour occurring within the control volume, an order of magnitude analysis is performed to neglect insignificant terms, producing an equation for predicting contact-angle hysteresis from a knowledge of the interface dynamics occurring around the three-phase contact line. It is shown that the viscous energy dissipation that occurs during the ‘stick–slip’ motion of the three-phase contact line, being the cause of contact-angle hysteresis on rough surfaces, can be calculated from changes in intermediate equilibrium interface states. The balance is applied to the Wenzel, Cassie–Baxter and Fakir (super-hydrophobic) wetting states, showing for the Fakir case that significant dissipation occurs during both interface advance and recede, and relating these dissipations to interfacial area changes that occur around the ‘stick–slip’ events.

Ion Dynamics at the Intermediate Charging State of the Sodium Vanadium Fluorophosphate Cathode.

Na super ionic conductor (NASICON)-type polyanionic vanadium fluorophosphate Na3V2O2(PO4)2F (NVOPF) is a promising cathode material for high-energy sodium-ion batteries. The dynamic diffusion and exchange of sodium ions in the lattice of NVOPF are crucial for its electrochemical performance. However, standard characterizations are mostly focused on the as-synthesized material without cycling, which is different from the actual battery operation conditions. In this work, we investigated the hopping processes of sodium in NVOPF at the intermediate charging state with 23Na solid-state nuclear magnetic resonance (ssNMR) and density functional theory (DFT) calculations. Our experimental characterizations revealed six distinct sodium coordination sites in the intermediate structure and determined the exchange rates among these sites at variable temperatures. The theoretical calculations showed that these dynamic processes correspond to different ion transport pathways in the crystalline lattice. Our combined experimental and theoretical study uncovered the underlying mechanisms of the ion transport in cycled NVOPF and these understandings may help the optimization of cathode materials for sodium-ion batteries.

Delayed room temperature phosphorescence enabled by phosphines

Organic ultralong room-temperature phosphorescence (RTP) usually emerges instantly and immediately decays after excitation removal. Here we report a new delayed RTP that is postponed by dozens of milliseconds after excitation removal and decays in two steps including an initial increase in intensity followed by subsequent decrease in intensity. The delayed RTP is achieved through introduction of phosphines into carbazole emitters. In contrast to the rapid energy transfer from single-molecular triplet states (T1) to stabilized triplet states (Tn*) of instant RTP systems, phosphine groups insert their intermediate states (TM) between carbazole-originated T1 and Tn* of carbazole-phosphine hybrids. In addition to markedly increasing emission lifetimes by ten folds, since TM → Tn* transition require >30 milliseconds, RTP is thereby postponed by dozens of milliseconds. The emission character of carbazole-phosphine hybrids can be used to reveal information through combining instant and delayed RTP, realizing multi-level time resolution for advanced information, biological and optoelectronic applications.

Energy decomposition analysis method using density matrix formulation.

In this work, an energy decomposition analysis (EDA) method with the strategy of density matrix, called DM-EDA, is proposed on the basis of single reference electronic structure calculations. Different from traditional EDA methods, instead of an intermediate state wave function, the EDA terms in DM-EDA are expressed in the forms of the density matrix. This method can be carried out with various kinds of density matrices. With the efficient implementation, DM-EDA not only greatly improves the computational efficiency but also provides quantitative knowledge of intermolecular interactions with a large number of monomers.