Footprints of atomic-scale features in plasmonic nanoparticles as revealed by electron energy loss spectroscopy.

We present a first-principles theoretical study of the atomistic footprints in the valence electron energy loss spectroscopy (EELS) of nanometer-size metallic particles. Charge density maps of excited plasmons and EEL spectra for specific electron paths through a nanoparticle (Na380 atom cluster) are modeled using ab initio calculations within time-dependent density functional theory. Our findings unveil the atomic-scale sensitivity of EELS within this low-energy spectral range. Whereas localized surface plasmons (LSPs) are particularly sensitive to the atomistic structure of the surface probed by the electron beam, confined bulk plasmons (CBPs) reveal quantum size effects within the nanoparticle's volume. Moreover, we prove that classical local dielectric theories mimicking the atomistic structure of the nanoparticles reproduce the LSP trends observed in quantum calculations, but fall short in describing the CBP behavior observed under different electron trajectories.

SEMA3: A free smartphone platform for daily life surveys.

Traditionally, behavioral, social, and health science researchers have relied on global/retrospective survey methods administered cross-sectionally (i.e., on a single occasion) or longitudinally (i.e., on several occasions separated by weeks, months, or years). More recently, social and health scientists have added daily life survey methods (also known as intensive longitudinal methods or ambulatory assessment) to their toolkit. These methods (e.g., daily diaries, experience sampling, ecological momentary assessment) involve dense repeated assessments in everyday settings. To facilitate research using daily life survey methods, we present SEMA3 ( http://www.SEMA3.com ), a platform for designing and administering intensive longitudinal daily life surveys via Android and iOS smartphones. SEMA3 fills an important gap by providing researchers with a free, intuitive, and flexible platform with basic and advanced functionality. In this article, we describe SEMA3's development history and system architecture, provide an overview of how to design a study using SEMA3 and outline its key features, and discuss the platform's limitations and propose directions for future development of SEMA3.

Neuroticism may not reflect emotional variability.

Neuroticism is one of the major traits describing human personality, and a predictor of mental and physical disorders with profound public health significance. Individual differences in emotional variability are thought to reflect the core of neuroticism. However, the empirical relation between emotional variability and neuroticism may be partially the result of a measurement artifact reflecting neuroticism's relation with higher mean levels-rather than greater variability-of negative emotion. When emotional intensity is measured using bounded scales, there is a dependency between variability and mean levels: at low (or high) intensity, it is impossible to demonstrate high variability. As neuroticism is positively associated with mean levels of negative emotion, this may account for the relation between neuroticism and emotional variability. In a metaanalysis of 11 studies (N = 1,205 participants; 83,411 observations), we tested whether the association between neuroticism and negative emotional variability was clouded by a dependency between variability and the mean. We found a medium-sized positive association between neuroticism and negative emotional variability, but, when using a relative variability index to correct for mean negative emotion, this association disappeared. This indicated that neuroticism was associated with experiencing more intense, but not more variable, negative emotions. Our findings call into question theory, measurement scales, and data suggesting that emotional variability is central to neuroticism. In doing so, they provide a revisionary perspective for understanding how this individual difference may predispose to mental and physical disorders.

Re-appraising stressors from a distance: effects of linguistic distancing on cognitive appraisals and emotional responses to interpersonal conflict.

Reflecting on stressors from a detached perspective - a strategy known as distancing - can facilitate emotional recovery. Researchers have theorised that distancing works by enabling reappraisals of negative events, yet few studies have investigated specifically how distancing impacts stressor appraisals. In this experiment, we investigated how participants' (N = 355) emotional experience and appraisals of an interpersonal conflict differed depending on whether they wrote event-reflections from a linguistically immersed (first-person) or distanced (second/third-person) perspective. Partly replicating previous findings, distanced reflection predicted increases in positive affect, but not reductions in negative affect, relative to immersed reflection. Linguistic distancing also predicted increases in motivational congruence appraisals (i.e. perceived advantageousness of the event), but did not influence other appraisal dimensions. We discuss how linguistic distancing may facilitate emotional recovery by illuminating the benefits of stressful experiences, enabling people to "see the good in the bad".

Neural patterns during anticipation predict emotion regulation success for reappraisal.

The ability to exert control over emotions, termed emotion regulation (ER), is vital for everyday functioning. ER success may be influenced by processes relating to the anticipation (prior to active regulation) and implementation (during active regulation) of ER strategy use. We investigated whether brain activity patterns recorded using electroencephalography (EEG) during the first second of anticipation and implementation of two ER strategies-distraction and reappraisal-were related to regulation success. Participants viewed negative images that evoked disgust and sadness. Before each image was presented, participants were cued to either passively view the image or decrease their emotional responses. ER success scores were calculated from subsequent self-reported disgust and sadness ratings. Using multivariate support vector regression, ER success scores were predicted from spatiotemporal patterns of event-related potentials during the first second of anticipation and implementation phases of each ER strategy. For both sadness and disgust, reappraisal success could be predicted during anticipation, while distraction success could be predicted during implementation. These findings suggest that early anticipatory cognitive processes are a key determinant of reappraisal success, but may not be similarly important for distraction. This may be because reappraisal is more cognitively demanding than distraction, requiring enhanced preparation of mental resources.

Siesta: Recent developments and applications.

A review of the present status, recent enhancements, and applicability of the Siesta program is presented. Since its debut in the mid-1990s, Siesta's flexibility, efficiency, and free distribution have given advanced materials simulation capabilities to many groups worldwide. The core methodological scheme of Siesta combines finite-support pseudo-atomic orbitals as basis sets, norm-conserving pseudopotentials, and a real-space grid for the representation of charge density and potentials and the computation of their associated matrix elements. Here, we describe the more recent implementations on top of that core scheme, which include full spin-orbit interaction, non-repeated and multiple-contact ballistic electron transport, density functional theory (DFT)+U and hybrid functionals, time-dependent DFT, novel reduced-scaling solvers, density-functional perturbation theory, efficient van der Waals non-local density functionals, and enhanced molecular-dynamics options. In addition, a substantial effort has been made in enhancing interoperability and interfacing with other codes and utilities, such as wannier90 and the second-principles modeling it can be used for, an AiiDA plugin for workflow automatization, interface to Lua for steering Siesta runs, and various post-processing utilities. Siesta has also been engaged in the Electronic Structure Library effort from its inception, which has allowed the sharing of various low-level libraries, as well as data standards and support for them, particularly the PSeudopotential Markup Language definition and library for transferable pseudopotentials, and the interface to the ELectronic Structure Infrastructure library of solvers. Code sharing is made easier by the new open-source licensing model of the program. This review also presents examples of application of the capabilities of the code, as well as a view of on-going and future developments.

Recent developments in the PySCF program package.

PySCF is a Python-based general-purpose electronic structure platform that supports first-principles simulations of molecules and solids as well as accelerates the development of new methodology and complex computational workflows. This paper explains the design and philosophy behind PySCF that enables it to meet these twin objectives. With several case studies, we show how users can easily implement their own methods using PySCF as a development environment. We then summarize the capabilities of PySCF for molecular and solid-state simulations. Finally, we describe the growing ecosystem of projects that use PySCF across the domains of quantum chemistry, materials science, machine learning, and quantum information science.

Emotion regulation and mood brightening in daily life vary with depressive symptom levels.

Naturalistic studies of emotional reactivity in depression have repeatedly found larger decreases in negative affect (NA) among depressed individuals in response to daily positive events. This so-called mood-brightening (MB) effect represents a theoretical and empirical oddity. The current study is a secondary analysis investigating whether the MB effect is moderated by spontaneous use of emotion regulation strategies, which have been implicated in the maintenance and modulation of NA in prior work. Participants (N = 95) representing a large spectrum of depressive symptom severity reported their experiences of NA and the occurrence of positive events in daily life over the course of seven days using the experience sampling method. Our findings replicate and build upon those of prior studies relating to the MB effect in the following ways: (1) we observed the MB effect for specific negative emotions of sadness, anger, anxiety; and (2) we found evidence that the MB effect is moderated by spontaneous use of rumination, distraction, and expressive suppression, which have been shown to enhance or dampen NA. The role of emotion regulation strategies in daily emotional reactivity to pleasant events is discussed.

The Relation Between Valence and Arousal in Subjective Experience Varies With Personality and Culture.

OBJECTIVE: While in general arousal increases with positive or negative valence (a so-called V-shaped relation), there are large differences among individuals in how these two fundamental dimensions of affect are related in people's experience. In two studies, we examined two possible sources of this variation: personality and culture. METHOD: In Study 1, participants (Belgian university students) recalled a recent event that was characterized by high or low valence or arousal and reported on their feelings and their personality in terms of the Five-Factor Model. In Study 2, participants from Canada, China/Hong Kong, Japan, Korea, and Spain reported on their feelings in a thin slice of time and on their personality. RESULTS: In Study 1, we replicated the V-shape as characterizing the relation between valence and arousal, and identified personality correlates of experiencing particular valence-arousal combinations. In Study 2, we documented how the V-shaped relation varied as a function of Western versus Eastern cultural background and personality. CONCLUSIONS: The results showed that the steepness of the V-shaped relation between valence and arousal increases with Extraversion within cultures, and with a West-East distinction between cultures. Implications for the personality-emotion link and research on cultural differences in affect are discussed.

The Wisdom to Know the Difference.

The ability to regulate emotions is central to well-being, but healthy emotion regulation may not merely be about using the "right" strategies. According to the strategy-situation-fit hypothesis, emotion-regulation strategies are conducive to well-being only when used in appropriate contexts. This study is the first to test the strategy-situation-fit hypothesis using ecological momentary assessment of cognitive reappraisal-a putatively adaptive strategy. We expected people who used reappraisal more in uncontrollable situations and less in controllable situations to have greater well-being than people with the opposite pattern of reappraisal use. Healthy participants ( n = 74) completed measures of well-being in the lab and used a smartphone app to report their use of reappraisal and perceived controllability of their environment 10 times a day for 1 week. Results supported the strategy-situation-fit hypothesis. Participants with relatively high well-being used reappraisal more in situations they perceived as lower in controllability and less in situations they perceived as higher in controllability. In contrast, we found little evidence for an association between greater well-being and greater mean use of reappraisal across situations.

Emotional inertia contributes to depressive symptoms beyond perseverative thinking.

The autocorrelation or inertia of negative affect reflects how much negative emotions carry over from moment to moment and has been associated with increased depressive symptoms. In this study, we posed three challenges to this association by examining: (1) whether emotional inertia is relevant for depressive symptoms when assessed on a longer timescale than usual; (2) whether inertia is uniquely related to depressive symptoms after controlling for perseverative thoughts; and (3) whether inertia is related to depressive symptoms over and above the within-person association between affect and perseverative thoughts. Participants (N = 101) provided ratings of affect and perseverative thoughts for 100 days; depressive symptoms were reported before and after the study, and again after 2.5 years. Day-to-day emotional inertia was related to depressive symptoms over and above trait and state perseverative thoughts. Moreover, inertia predicted depressive symptoms when adjusting for its association with perseverative thoughts. These findings establish the relevance of emotional inertia in depressive symptoms independent of perseverative thoughts.

Emotion regulation and the temporal dynamics of emotions: Effects of cognitive reappraisal and expressive suppression on emotional inertia.

The tendency for emotions to be predictable over time, labelled emotional inertia, has been linked to low well-being and is thought to reflect impaired emotion regulation. However, almost no studies have examined how emotion regulation relates to emotional inertia. We examined the effects of cognitive reappraisal and expressive suppression on the inertia of behavioural, subjective and physiological measures of emotion. In Study 1 (N = 111), trait suppression was associated with higher inertia of negative behaviours. We replicated this finding experimentally in Study 2 (N = 186). Furthermore, in Study 2, instructed suppressors and reappraisers both showed higher inertia of positive behaviours, and reappraisers displayed higher inertia of heart rate. Neither suppression nor reappraisal were associated with the inertia of subjective feelings in either study. Thus, the effects of suppression and reappraisal on the temporal dynamics of emotions depend on the valence and emotional response component in question.

Distinguishing between level and impact of rumination as predictors of depressive symptoms: an experience sampling study.

Rumination--repetitively thinking about one's emotional state, its causes and consequences--exacerbates negative mood and plays an important role in the aetiology and maintenance of depression. Yet, it is unclear whether increased vulnerability to depression is associated with simply how much a person ruminates, or the short-term impact rumination has on a person's negative mood. In the current study, we distinguish between the level versus the impact of rumination, and we examine how each uniquely predicts changes in depressive symptoms over time in an undergraduate sample. Using experience sampling, we assessed students' (N = 101) subjective experiences of positive and negative affect and their use of rumination and distraction in daily life for seven days. Participants also reported their depressive symptoms before and after the experience sampling. Increases in depressive symptoms over the week were predicted by how much people ruminated, but not by its impact on negative mood.

Negative emotion differentiation: its personality and well-being correlates and a comparison of different assessment methods.

Previous research has shown that individual differences in negative emotion differentiation may play a prominent role in well-being. Yet, many basic questions about negative emotion differentiation remain unanswered, including how it relates and overlaps with related and known dimensions of individual differences and what its possible underlying processes are. To answer these questions, in the current article we present three correlational studies that chart the nomological network of individual differences in negative emotion differentiation in terms of personality, difficulties in identifying and describing feelings, and several indicators of well-being, propose a novel paradigm to assess it in the lab, and explore relationships with a possible underlying mechanism in terms of the motivation to approach or avoid emotions. The results affirm consistent relations between negative emotion differentiation and indicators of adjustment like negative affect, self-esteem, neuroticism, depression and meta-knowledge about one's emotions, and show how it is related to the motivation to experience affective states.

Location-scale modeling as an integrative approach to symptom dynamics during psychotherapy: An illustration with depressive symptoms.

OBJECTIVE: Depressive symptom dynamics, including change trajectories and symptom variability, have been related to therapy outcomes. However, such dynamics have often been examined separately and related to outcomes of interest using two-step analyses, which are characterized by several limitations. Here, we show how to overcome these limitations using location-scale models in a dynamic structural equation modeling framework. METHOD: We introduce location-scale modeling in an accessible manner to pave the way for its use in research integrating within-person dynamics and intervention-related change in psychopathology, and we illustrate this modeling approach in a large-scale internet-based intervention for depression (N = 1,656). Using eight data points sampled across about 8 weeks, we predicted improvement across the intervention (50% symptom reduction) as a function of early change and symptom variability. RESULTS: Early symptom change was associated with a more likely improvement across therapy. Variability of symptoms beyond change trajectories during the intervention was associated with less likely improvement. CONCLUSIONS: Location-scale models, and dynamic structural equation modeling more generally, are well suited to modeling how patterns of symptom change during psychotherapy are related to important (e.g., therapy) outcomes. Our illustrative application of location-scale modeling showed that symptom variability was associated with less overall improvement in depressive symptoms. However, this finding requires replication with more intensive sampling of symptoms before final conclusions can be drawn on when and how to distinguish maladaptive from adaptive variability during psychotherapy. (PsycInfo Database Record (c) 2024 APA, all rights reserved).

The Cost-Effectiveness of a Novel Online Social Therapy to Maintain Treatment Effects From First-Episode Psychosis Services: Results From the Horyzons Randomized Controlled Trial.

BACKGROUND: Digital interventions have potential applications in promoting long-term recovery and improving outcomes in first-episode psychosis (FEP). This study aimed to evaluate the cost-effectiveness of Horyzons, a novel online social therapy to support young people aged 16-27 years following discharge from FEP services, compared with treatment as usual (TAU) from a healthcare sector and a societal perspective. STUDY DESIGN: A cost-effectiveness analysis (CEA), based on the change in social functioning, and a cost-utility analysis (CUA) using quality-adjusted life years were undertaken alongside a randomized controlled trial. Intervention costs were determined from study records; resources used by patients were collected from a resource-use questionnaire and administrative data. Mean costs and outcomes were compared at 18 months and incremental cost-effectiveness ratios were calculated. Uncertainty analysis using bootstrapping and sensitivity analyses was conducted. STUDY RESULTS: The sample included 170 participants: Horyzons intervention group (n = 86) and TAU (n = 84). Total costs were significantly lower in the Horyzons group compared with TAU from both the healthcare sector (-AU$4789.59; P < .001) and the societal perspective (-AU$5131.14; P < .001). In the CEA, Horyzons was dominant, meaning it was less costly and resulted in better social functioning. In the CUA, the Horyzons intervention resulted in fewer costs but also yielded fewer QALYs. However, group differences in outcomes were not statistically significant. When young people engaged more with the platform, costs were shown to decrease and outcomes improved. CONCLUSIONS: The Horyzons intervention offers a cost-effective approach for improving social functioning in young people with FEP after discharge from early intervention services.

Interference resolution moderates the impact of rumination and reappraisal on affective experiences in daily life.

Research has shown that cognitive control processes play a central role in emotion regulation. While most research has examined whether individual differences in such processes are related to the use of these strategies, a crucial next step involves examining whether such differences influence their impact on people's feelings, especially in normal daily life. The present study examined whether impairments in cognitive control (measured using an affective interference resolution task) moderate the impact of using rumination and reappraisal on affective experiences in everyday life (assessed using experience sampling methods). Multilevel analyses revealed that difficulties removing previously relevant negative information from working memory were associated with a larger increase in negative affect following rumination, and smaller increase and decrease in positive and negative affect, respectively, following reappraisal. These findings show that impaired interference resolution for negative information aggravates the deleterious effects of rumination and curbs the benefits of reappraisal in daily life.

Molecular Doping in the Organic Semiconductor Diindenoperylene: Insights from Many-Body Perturbation Theory.

Molecular doping provides a route toward designing new organic compounds with improved performance for optoelectronics. Here, we investigate the p-type doping of crystalline diindenoperylene (DIP) with two recently proposed electron-accepting molecular dopants using many-body perturbation theory. For the pristine DIP crystal, the quasiparticle band structure and the optical absorption spectra are found in agreement with the experimental data. Using the same methodology, we then characterize the optical and electronic properties of the two doped DIP crystals. The bandgap of both doped crystals is narrowed considerably due to the formation of hybridized states at the valence band edge. Moreover, a hybrid unoccupied mid-gap band is created with a host-dopant charge-transfer characteristic, giving rise to broader absorption spectra and a much lower absorption onset as compared to pristine DIP. Our results highlight that the interaction and hybridization with the host environment, including many-body effects, must be carefully considered in order to identify appropriate molecular dopants for a given organic crystal.

Emotion regulation in everyday life: Mapping global self-reports to daily processes.

Recent theory conceptualizes emotion regulation as occurring across three stages: (a) identifying the need to regulate, (b) selecting a strategy, and (c) implementing that strategy to modify emotions. Yet, measurement of emotion regulation has not kept pace with these theoretical advances. In particular, widely used global self-report questionnaires are often assumed to index people's typical strategy selection tendencies. However, it is unclear how well global self-reports capture individual differences in strategy selection and/or whether they may also index other emotion regulation stages. To address this issue, we examined how global self-report measures correspond with the three stages of emotion regulation as modeled using daily life data. We analyzed data from nine daily diary and experience sampling studies (total N = 1,097), in which participants provided daily and global self-reports of cognitive reappraisal, expressive suppression, and rumination. We found only weak-to-moderate correlations between global self-reports and average daily self-reports of each regulation strategy (indexing strategy selection). Global self-reports also correlated with individual differences in the degree to which (a) preceding affect experience predicted regulation strategies (representing the identification stage), and (b) regulation strategies predicted subsequent changes in affective experience (representing the implementation stage). Our findings suggest that global self-report measures of reappraisal, suppression, and rumination may not strongly and uniquely correlate with individual differences in daily selection of these strategies. Moreover, global self-report measures may also index individual differences in the perceived need to regulate, and the affective consequences of regulation in daily life. (PsycInfo Database Record (c) 2023 APA, all rights reserved).