In this paper, we introduce the Floquet mean-field dynamics and Floquet surface hopping approaches to study the nonadiabatic dynamics in periodically driven solid systems. We demonstrate that these two approaches can be formulated in both real and reciprocal spaces. Using the two approaches, we are able to simulate the interaction between electronic carriers and phonons under periodic drivings, such as strong light-matter interactions. Employing the Holstein and Peierls models, we show that strong light-matter interactions can effectively modulate the dynamics of electronic population and mobility. Notably, our study demonstrates the feasibility and effectiveness of modeling low-momentum carriers' interactions with phonons using a truncated reciprocal space basis, an approach impractical in real space frameworks. Moreover, we reveal that even with a significant truncation, carrier populations derived from surface hopping maintain greater accuracy compared to those obtained via mean-field dynamics. These results underscore the potential of our proposed methods in advancing the understanding of carrier-phonon interactions in various periodically driven materials.
Music is omnipresent among human cultures and moves us both physically and emotionally. The perception of emotions in music is influenced by both psychophysical and cultural factors. Chinese traditional instrumental music differs significantly from Western music in cultural origin and music elements. However, previous studies on music emotion perception are based almost exclusively on Western music. Therefore, the construction of a dataset of Chinese traditional instrumental music is important for exploring the perception of music emotions in the context of Chinese culture. The present dataset included 273 10-second naturalistic music excerpts. We provided rating data for each excerpt on ten variables: familiarity, dimensional emotions (valence and arousal), and discrete emotions (anger, gentleness, happiness, peacefulness, sadness, solemnness, and transcendence). The excerpts were rated by a total of 168 participants on a seven-point Likert scale for the ten variables. Three labels for the excerpts were obtained: familiarity, discrete emotion, and cluster. Our dataset demonstrates good reliability, and we believe it could contribute to cross-cultural studies on emotional responses to music.
Emotions , Music , Humans , Music/psychology , Emotions/physiology , Female , Male , Adult , China , Young Adult , Auditory Perception/physiology , Reproducibility of Results , Recognition, Psychology/physiology , Arousal/physiology , East Asian People
Lithium-oxygen (Li-O2) batteries, renowned for their exceptionally high theoretical energy density, have garnered significant interest as a prime candidate for future electric device development. However, practical testing often yields unsatisfactory capacity due to the tendency of their solid-phase discharge products to cover active sites on the electrode surface. Optimizing the growth mechanism of these solid-phase products and addressing the storage issue to narrow the gap between actual and theoretical capacities stands as the core challenge in Li-O2 battery development. Here, a fluorine-doped bimetallic cobalt-nickel oxide (CoNiO2-xFx/CC) with an interlaced catalytic surface (ICS) and an open, corncob-like structure is proposed as an oxygen electrode. Unlike conventional oxide electrodes with a "single adsorption catalytic mechanism", the ICS of the CoNiO2-xFx/CC electrode offers a compelling "competitive adsorption catalytic mechanism". This is attributed to the diverse selective sites within the ICS, where oxygen sites preferentially facilitate oxygen conversion due to their higher affinity for oxygen, while fluorine sites preferentially contribute to the growth of Li2O2 owing to their stronger affinity for LiO2. This transformation in the formation mechanism of Li2O2 and its morphology from film along the electrode surface to toroidal particles effectively mitigates the issue of buried active sites. Additionally, the unique structure of the CoNiO2-xFx/CC electrode aids in the storage and decomposition of Li2O2 products. Its corncob-like open architecture not only promotes the capture and release of oxygen but also facilitates the formation of well-contacted Li2O2/electrode interfaces, akin to a "corn on the cob" design. Consequently, the Li-O2 battery employing the CoNiO2-xFx/CC cathode demonstrates a high specific capacity of up to 30923 mAh g-1 and a lifespan exceeding 580 cycles, surpassing most reported metal oxide-based cathodes. This work offers a promising solution to the issues of buried active sites and storage of insoluble products in metal-air batteries. This article is protected by copyright. All rights reserved.
Electron transfer (ET) at molecule-metal or molecule-semiconductor interfaces is a fundamental reaction that underlies all electrochemical processes and substrate-mediated surface photochemistry. In this study, we show that ET rates near a metal surface can be significantly manipulated by periodic driving (e.g., Floquet engineering). We employ the Floquet surface hopping and Floquet electronic friction algorithms developed previously to calculate the ET rates near the metal surface as a function of driving amplitudes and driving frequencies. We find that ET rates have a turnover effect when the driving frequencies increase. A Floquet Marcus theory is further formulated to analyze such a turnover effect. We then benchmark the Floquet Marcus theory against Floquet surface hopping and Floquet electronic friction methods, indicating that the Floquet Marcus theory works in the strong nonadiabatic regimes but fails in the weak nonadiabatic regimes. We hope these theoretical tools will be useful to study ET rates in the plasmonic cavity and plasmon-assisted photocatalysis.
The non-equilibrium Green's function (NEGF) and quantum master equation (QME) are two main classes of approaches for electronic transport. We discuss various Floquet variances of these formalisms for transport properties of a quantum dot driven via interaction with an external periodic field. We first derived two versions of the Floquet NEGF. We also explore an ansatz of the Floquet NEGF formalism for the interacting systems. In addition, we derived two versions of Floquet QME in the weak interaction regime. With each method, we elaborate on the evaluation of the expectation values of the number and current operators. We examined these methods for transport through a two-level system that is subject to periodic driving. The numerical results of all four methods show good agreement for non-interacting systems in the weak regime. Furthermore, we have observed that circular light can introduce spin current. We expect these Floquet quantum transport methods to be useful in studying molecular junctions exposed to light.
The molecular dynamics with electronic friction (MDEF) approach can accurately describe nonadiabatic effects at metal surfaces in the weakly nonadiabatic limit. That being said, the MDEF approach treats nuclear motion classically such that the nuclear quantum effects are completely missing in the approach. To address this limitation, we combine Electronic Friction with Ring Polymer Molecular Dynamics (EF-RPMD). In particular, we apply the averaged electronic friction from the metal surface to the centroid mode of the ring polymer. We benchmark our approach against quantum dynamics to show that EF-RPMD can accurately capture zero-point energy as well as transition dynamics. In addition, we show that EF-RPMD can correctly predict the electronic transfer rate near metal surfaces in the tunneling limit as well as the barrier crossing limit. We expect that our approach will be very useful to study nonadiabatic dynamics near metal surfaces when nuclear quantum effects become essential.
With light-matter interaction extending into the strong regime, as well as rapid development of laser technology, systems subjecting to a time-periodic perturbation have attracted broad attention. Floquet theorem and Floquet time-independent Hamiltonian are powerful theoretical frameworks to investigate the systems subjected to time-periodic drivings. In this study, we extend the previous generalized surface hopping (SH) algorithm near a metal surface (J. Chem. Theory Comput. 2017, 13, 6, 2430-2439) to the Floquet space, and hence, we develop a generalized Floquet representation-based SH (FR-SH) algorithm. Here, we consider an open quantum system with fast drivings. We expect that the present algorithm will be useful for understanding the chemical processes of molecules under time-periodic driving near the metal surface.
Rechargeable lithium batteries using 5 V positive electrode materials can deliver considerably higher energy density as compared to state-of-the-art lithium-ion batteries. However, their development remains plagued by the lack of electrolytes with concurrent anodic stability and Li metal compatibility. Here we report a new electrolyte based on dimethyl 2,5-dioxahexanedioate solvent for 5 V-class batteries. Benefiting from the particular chemical structure, weak interaction with lithium cation and resultant peculiar solvation structure, the resulting electrolyte not only enables stable, dendrite-free lithium plating-stripping, but also displays anodic stability up to 5.2 V (vs. Li/Li+), in additive or co-solvent-free formulation, and at low salt concentration of 1 M. Consequently, the Li | |LiNi0.5Mn1.5O4 cells using the 1 M LiPF6 in 2,5-dioxahexanedioate based electrolyte retain >97% of the initial capacity after 250 cycles, outperforming the conventional carbonate-based electrolyte formulations, making this, and potentially other dicarbonate solvents promising for future Lithium-based battery practical explorations.
OBJECTIVE: Alterations of empathy have been observed in patients with various mental disorders. The Perth Empathy Scale (PES) was recently developed to measure a multidimensional construct of empathy across positive and negative emotions. However, its psychometric properties and clinical applications have not been examined in the Chinese context. METHODS: The Chinese version of the PES was developed and administered to a large Chinese sample (n = 1090). Factor structure, internal consistency, test-retest reliability, and convergent, discriminant, as well as concurrent validity were examined. Moreover, 50 patients with major depressive disorder (MDD) and 50 healthy controls were recruited to explore the clinical utility of the PES. RESULTS: Confirmatory factor analyses supported a theoretically congruent three-factor structure of empathy, namely Cognitive Empathy, Negative Affective Empathy and Positive Affective Empathy. The PES showed good to excellent internal consistency reliability, good convergent and discriminant validity, acceptable concurrent validity, and moderate to high test-retest reliability. Patients with MDD had significantly lower PES scores compared to healthy controls. Linear discriminant function comprised of the three factors correctly differentiated 71% of participants, which further verified the clinical utility of the PES. CONCLUSIONS: Our findings indicated that the Chinese version of the PES is a reliable and valid instrument to measure cognitive and affective empathy across negative and positive emotions, and could therefore be used in both research and clinical practice.
OBJECTIVE: The purpose was to look into the diagnostic value of serum CRP, PCT and IL-6 in children with nephrotic syndrome co-infection. METHODS: One hundred and forty-nine children with nephrotic syndrome who met the inclusion and exclusion criteria were included in this study. The children were divided into three groups: bacterial infection group, non-bacterial infection group, and non-infection group. The diagnostic value was analyzed and compared using the ROC curve. RESULTS: There was no statistically significant difference in the Leukocyte counts among three groups. The mean results of serum CRP, PCT and IL-6 were significantly higher in the bacterial infection group compared to those in the non-infection group (p < 0.05). AUC of CRP, PCT, IL-6 in bacterial infection were 0.791, 0.859, 0.783. The following combinations CRP + PCT + IL-6, IL-6 + PCT, CRP + PCT significantly increased the efficiency of bacterial infection diagnosis, the AUCs were 0.881, 0.884, and 0.884, respectively. AUC of PCT in non-bacterial infection was 0.663. The combinations of these three clinical indicators performed no better than PCT in ROC analysis. CONCLUSION: Normal CRP or IL-6 levels do not rule out the diagnosis of bacterial infection in children on long-term glucocorticoid therapy. The appropriate combination of two or three indicators can improve the diagnostic value. IMPACT: This study evaluated the diagnostic value of the serum concentrations of CRP, PCT and IL-6 and assessed whether the value of their combined application is better than when used alone for diagnosing primary nephrotic syndrome complicated by infection. The elevation in leukocyte count cannot be used to diagnose children with nephrotic syndromes on long-term glucocorticoid treatment who have bacterial infections. Normal CRP or IL-6 levels do not rule out the diagnosis of bacterial infection in children on long-term glucocorticoid therapy. The appropriate combination of two or three indicators can improve diagnostic value, sensitivity, and specificity.
Bacterial Infections , Nephrotic Syndrome , Child , Humans , Retrospective Studies , Interleukin-6 , Nephrotic Syndrome/complications , Nephrotic Syndrome/diagnosis , Calcitonin , C-Reactive Protein/analysis , Glucocorticoids/therapeutic use , Bacterial Infections/complications , Bacterial Infections/diagnosis , ROC Curve , Biomarkers
Phase regulation of noble metal-based nanomaterials provides a promising strategy for boosting the catalytic performance. However, realizing the continuous phase modulation in two-dimensional structures and unveiling the relevant structure-performance relationship remain significant challenges. In this work, we present the first example of continuous phase modulation in a library of Pd-Te hexagonal nanoplates (HNPs) from cubic-phase Pd4Te, rhombohedral-phase Pd20Te7, rhombohedral-phase Pd8Te3, and hexagonal-phase PdTe to hexagonal-phase PdTe2. Notably, the continuous phase regulation of the well-defined Pd-Te HNPs enables the successful modulation of the distance between adjacent Pd active sites, triggering an exciting way for tuning the relevant catalytic reactions intrinsically. The proof-of-concept oxygen reduction reaction (ORR) experiment shows a Pd-Pd distance-dependent ORR performance, where the hexagonal-phase PdTe HNPs present the best electrochemical performance in ORR (mass activity and specific activity of 1.02 A mg-1Pd and 1.83 mA cm-2Pd at 0.9 V vs RHE). Theoretical investigation reveals that the increased Pd-Pd distance relates to the weak *OH adsorption over Pd-Te HNPs, thus contributing to the remarkable ORR activity of PdTe HNPs. This work advances the phase-controlled synthesis of noble metal-based nanostructures, which gives huge impetus to the design of high-efficiency nanomaterials for diverse applications.
Simulating dynamics of open quantum systems is sometimes a significant challenge, despite the availability of various exact or approximate methods. Particularly when dealing with complex systems, the huge computational cost will largely limit the applicability of these methods. In this work, we investigate the usage of dynamic mode decomposition (DMD) to evaluate the rate kernels in quantum rate processes. DMD is a data-driven model reduction technique that characterizes the rate kernels using snapshots collected from a small time window, allowing us to predict the long-term behaviors with only a limited number of samples. Our investigations show that whether the external field is involved or not, the DMD can give accurate prediction of the result compared with the traditional propagations, and simultaneously reduce the required computational cost.
Accumulating evidence indicates positive associations between physical activity (PA) and cognitive control. Proactive control, the ability to maintain goal-relevant information in preparation of upcoming task demands, is a critical component of cognitive control. However, little research has examined the association between PA and proactive control. To address this issue, a total of 132 university students were recruited and divided into two groups based on reported regular PA during past week. All participants completed two common cognitive control tasks: the AX Continuous Performance Task (AX-CPT) and the Cued Task-Switching Paradigm (CTS). In comparison with the low PA group, the high PA group showed greater proactive control efficiency on both tasks. Moreover, proactive control indices significantly correlated between the two tasks for the high but not for the low PA group. Further, working memory significantly modulated the association between PA and proactive control efficiency of CTS. Although the present cross-section design does not allow us to test the causal relationship between PA and proactive control, these findings may have important implications for developing effective intervention strategies which aim to promote proactive control through increasing PA or to promote PA through increasing proactive control. Moreover, individual differences in working memory are important to consider when we aim to design such interventions.
Cues , Memory, Short-Term , Humans , Exercise , Individuality , Psychomotor Agitation
In the previous study Wang and Dou [J. Chem. Phys. 158, 224109 (2023)], we have derived a Floquet classical master equation (FCME) to treat nonadiabatic dynamics near metal surfaces under Floquet engineering. We have also proposed a trajectory surface hopping algorithm to solve the FCME. In this study, we map the FCME into a Floquet Fokker-Planck equation in the limit of fast Floquet driving and fast electron motion as compared to nuclear motion. The Fokker-Planck equation is then being solved using Langevin dynamics with explicit friction and random force from the nonadiabatic effects of hybridized electrons and Floquet states. We benchmark the Floquet electronic friction dynamics against Floquet quantum master equation and Floquet surface hopping. We find that Floquet driving results in a violation of the second fluctuation-dissipation theorem, which further gives rise to heating effects.
Achieving self-consistent convergence with the conventional effective-mass approach at ultra-low temperatures (below 4.2 K) is a challenging task, which mostly lies in the discontinuities in material properties (e.g. effective-mass, electron affinity, dielectric constant). In this article, we develop a novel self-consistent approach based on cell-centered finite-volume discretization of the Sturm-Liouville form of the effective-mass Schrödinger equation and generalized Poisson's equation (FV-SP). We apply this approach to simulate the one-dimensional electron gas formed at the Si-SiO2interface via a top gate. We find excellent self-consistent convergence from high to extremely low (as low as 50 mK) temperatures. We further examine the solidity of FV-SP method by changing external variables such as the electrochemical potential and the accumulative top gate voltage. Our approach allows for counting electron-electron interactions. Our results demonstrate that FV-SP approach is a powerful tool to solve effective-mass Hamiltonians.
X-ray detectors have numerous applications in medical imaging, industrial inspection, and crystal structure analysis. Gallium oxide (Ga2O3) shows potential as a material for high-performance X-ray detectors due to its wide bandgap, relatively high mass attenuation coefficient, and resistance to radiation damage. In this study, we present Sn-doped Ga2O3 microwire detectors for solar-blind and X-ray detection. The developed detectors exhibit a switching ratio of 1.66 × 102 under X-ray irradiation and can operate stably from room temperature to 623 K, which is one of the highest reported operating temperatures for Ga2O3 X-ray detectors to date. These findings offer a promising new direction for the design of Ga2O3-based X-ray detectors.
We develop a Floquet surface hopping approach to deal with nonadiabatic dynamics of molecules near metal surfaces subjected to time-periodic drivings from strong light-matter interactions. The method is based on a Floquet classical master equation (FCME) derived from a Floquet quantum master equation (FQME), followed by a Wigner transformation to treat nuclear motion classically. We then propose different trajectory surface hopping algorithms to solve the FCME. We find that a Floquet averaged surface hopping with electron density (FaSH-density) algorithm works the best as benchmarked with the FQME, capturing both the fast oscillations due to the driving and the correct steady-state observables. This method will be very useful to study strong light-matter interactions with a manifold of electronic states.
Algorithms , Metals , Motion
Purpose: Onychopapilloma is a rare benign nail tumor affecting the distal matrix and the nail bed. Currently, the only available treatment is surgical resection, which has a recurrence rate of 20% and may lead to various complications. Here we report a new method to treat onychopapilloma with pulsed dye laser (PDL).Materials and methods: We retrospectively analyzed 13 cases and evaluated disease classification, dermoscopic examination, laser treatment parameters, photographs before and after treatment, and treatment outcome.Results: The site distribution of onychopapilloma was consistent with previous reports. PDL treatment was performed with 595 nm laser, with 1.5 ms pulse duration, spot diameter 3-5 mm, and 11.5-13.5 J/cm2 fluence. Irradiation covered the telangiectatic area up to the edge of the nail folds, with the terminal response of purpura occurrence. The overall effective rate was 77%; the effective rates for erythronychia, leukonychia, and melanonychia were 88%, 67%, and 50%, respectively.Conclusions: PDL treatment for onychopapilloma provides an alternative to traditional surgery with comparable effectiveness but much less risk for complications.
Lasers, Dye , Low-Level Light Therapy , Nail Diseases , Purpura , Humans , Lasers, Dye/therapeutic use , Retrospective Studies , Treatment Outcome , Low-Level Light Therapy/adverse effects , Nail Diseases/radiotherapy , Nail Diseases/surgery
BACKGROUND: IgA nephropathy (IgAN) is a common primary renal disease in childhood. METHODS: Twenty blood samples and renal tissue from patients with IgAN, 20 blood samples from healthy children and 10 normal renal tissue were collected. Serum Gd-IgA1 and renal Gd-IgA1, CD31, α-SMA and vimentin were measured. RESULTS: The serum Gd-IgA1 concentration in the IgAN group was significantly higher. Gd-IgA1 was not expressed in normal kidneys, which was positive in the IgAN group. Gd-IgA1 levels in serum and renal tissue were not related. The expression of CD31 decreased significantly in IgAN group, while the expression of α-SMA and vimentin increased significantly. There was no significant correlation between the renal concentration of Gd-IgA1 and CD31, α-SMA and vimentin. CONCLUSION: The increased Gd-IgA1 in the serum and kidney may promote the pathogenesis of IgAN. The serum Gd-IgA1 cannot predict the extent of its deposition in the kidney. Endothelial mesenchymal transition (EndMT) may be involved in the pathogenesis of renal fibrosis in IgAN.
Glomerulonephritis, IGA , Child , Humans , Glomerulonephritis, IGA/pathology , Vimentin , Endothelial Cells/metabolism , Endothelial Cells/pathology , Immunoglobulin A/metabolism , Kidney/pathology
Purpose: This systematic review aimed to analyze the characteristics of different diagnostic techniques for micrognathia, summarize the consistent diagnostic criteria of each technique, and provide a simple and convenient prenatal diagnosis strategy for micrognathia. Methods: In accordance with the Preferred Reporting Items for Systematic Reviews and Meta-Analyses (PRISMA) guidelines, the search was undertaken in three international databases (PubMed, Scopus, and Web of Science). The three reviewers assessed all papers and extracted the following variables: author's name and year of publication, country, study design, number of participants, gestational age, equipment for prenatal examination, biometric parameters related to micrognathia, main results. Results: A total of 25 articles included in the analysis. Nineteen articles described cross-sectional studies (76 percent), 4 (16 percent) were case-control studies, and 2 (8 percent) were cohort studies. Fifteen studies (60 percent) had a prospective design, 9 (36 percent) had a retrospective design, and one (4 percent) had both prospective and retrospective design. Thirty-two percent of the studies (n = 8) were performed in USA, and the remaining studies were performed in China (n = 4), Israel (n = 3), Netherlands (n = 3), UK (n = 1), France (n = 1), Italy (n = 1), Belgium(n = 1), Germany (n = 1), Spain (n = 1), and Austria (n = 1). The prenatal diagnosis of micrognathia can be performed as early as possible in the first trimester, while the second and third trimester of pregnancy were the main prenatal diagnosis period. The articles that were included in the qualitative synthesis describe 30 biometric parameters related to the mandible. Conclusion: Of the 30 biometric parameters related to the mandible, 15 can obtain the simple and convenient diagnostic criteria or warning value for micrognathia. Based on these diagnostic criteria or warning value, clinicians can quickly make a preliminary judgment on facial deformities, to carry out cytologic examination to further clarify the diagnosis of micrognathia.
