Nitrides of late transition metals possess interesting properties leading to different technological applications, yet, due to many factors, synthesis and reliable characterization of the physical properties of these materials constitute a big challenge. In this work, we present a detailed firstprinciples investigation of the structural, the electronic and the optical properties of the bulk crystalline MNx (where M = Pd, Pt, Cu, Ag or Au; and x = 1/3, 1 or 2) and ZnN. The studied structural properties include energy-volume equation of state (EOS), equilibrium lattice structural parameters, cohesive and formation energies, relative phase stabilities, bulk modulus and its pressure derivative. By means of the enthalpy-pressure EOS, some possiblepressure-induced structural phase transitions are carefully examined. Electronic properties of the energetically most stable phases are investigated via the analysis of their band structure and their total and partial densities of states (DOSs). The frequency-dependent optical constants (absorption coefficient, reflectivity, refractive index, and energy-loss spectrum) of some phases are derived from the calculated frequency-dependent microscopic dielectric tensor. Our calculations of the structural and the electronic properties are based on density functional theory (DFT) within the projector-augmented wave (PAW) formulation and the generalised-gradient approximation (GGA) to the exchange-correlation functional. In order to improve the calculated electronic structure, and to investigate the optical spectra, we carry out expensive GW0 calculations within the the random-phase approximation (RPA) to the dielectric tensor. Obtained results are discussed within the employed theoretical methods of calculations. Whenever possible, our obtained results are compared with experiment and with previous theoretical studies. We report the discovery of some possible low-energy competitive phases which are more stable at zero pressure than the synthesized and other hypothetical structural phases. To the best of our knowledge, our calculated optical spectra may be considered as the first, and thus, the most accurate, calculations within the many-body perturbation GWA calculations, so far.

Adolescents with Autism and their families experience a significant increase in the number and nature of challenges faced when leaving the structure of the formal education system. Increased support and planning is required in order to prepare for and better manage this period, as a successful transition is associated with family well-being. An ecosystemic approach was used in order to better understand the experiences of the individual, the family, the school and the community during this period. The purpose of this study was to gain an understanding of parent and professional perspectives on various elements of the transition process, including planning and support, predicted outcomes and the feelings experienced, in order to develop awareness, improved planning and consequently; outcomes. A sample of 14 participants (7 parents and 7 professionals) was engaged in semi-structured interviews. The results indicate that both parents and professionals feel an overwhelming sense of fear and uncertainty with regards to the future of the adolescent with Autism; however a sense of optimism and hope also exists, as participants reported effective interventions were beginning to occur. The knowledge and understanding of the needs of these individuals is continuously growing within the parents and professionals who are directly involved in the lives of adolescents with Autism; however increased awareness is required within the community and government sectors in order to gain increased access to resources and services. With the appropriate support, individuals with Autism can experience increased quality of life within residential, employment, social and community settings. The results of the current study are discussed with reference to previous research studies, and recommendations for further research are provided.

Historically, school counselors have been the primary facilitators in supporting the career and college transition process for students, but many school counselors do not have the knowledge, resources, or materials to support students in this transition (Belasco, 2013). One way to help support career and college readiness is to develop comprehensive career and college readiness plans that involve more stakeholders than just the counselor and engage the community in supporting students to define and prepare for their paths for after high school (Alleman & Holly, 2013). This convergent parallel mixed methods study investigated what educators,students, and community partners in rural Oregon think is important to include in a career and college readiness plan that supports all students. I used Bronfenbrenner’s (1994) Ecological Model of Human Development to inform my data collection activities, casting a wide net to identify the stakeholder groups that have a potential impact on supporting students in their pursuit of a career or college education beyond high school. The qualitative data came from interviews with five Douglas County high school career and college readiness teams (n=8 participants), three student focus groups (n=24), and two partner meetings (n=15). The quantitative data was gathered through a career and college readiness survey administered to the staff and faculty at 14 Douglas County high schools (n=74 respondents). I used Farrell & Coburn’s (2016) Absorptive Capacity Theory as the lens through which to analyze the data, coding for the theory’s constructs around how prior knowledge, communication pathways, strategic knowledge leadership, and resources for partnering can be shared and leveraged between high schools and external partners. Findings from this study provide lessons learned about what should be included in a rural high schools’ career and college readiness plan that will help rural communities better support students in their transitions beyond high school.

En raison du changement climatique, le monde doit de plus en plus faire face aux urgences environnementales. Plusieurs questions écologiques, notamment énergétiques, surgissent globalement d’une manière préoccupante et impose dans les esprits la nécessité d’une « transition énergétique » comme solution. Cette transition implique des changements économiques, politiques et sociétaux n’engagent plus la seule responsabilité gouvernementale. Et c’est au nom de ce principe que les autorités ont appelé tout à chacun à se prononcer sur ces questions lors du Débat National sur la Transition Énergétique (DNTE) en France en 2013. L’objectif principal de cette thèse est d’exposer les spécificités discursives et textuelles de ce débat national, depuis son origine jusqu’à son aboutissement présenté sous forme de synthèse. En situant dans le cadre théorique de l’analyse du discours, ce travail recourt à diverses approches : historique, communicationnelle, socio-politique et linguistique. Il entend en particulier décrire la fabrication des synthèses de ce débat et leur dimension textuelle pour à la fois rendre compte des caractéristiques propres du DNTE et son issue, laquelle devant permettre en principe au gouvernement de délibérer et décider sur des politiques à adopter. / Due to climate change, the world is experiencing numerous environmental problems, which are in urgent need of solutions. Among the major ecological concerns being discussed globally are energy-related problems. The "energy transition" is known as an effective solution to such a situation. This implies the economic, political and societal changes that the government is no longer solely responsible for this global issue. In France, everyone is called upon to take a stand as evidenced by the National Debate on Energy Transition (DNTE) in 2013. The main objective of this thesis is to demonstrate the discursive and textual specificities of this national debate, from its origin to its completion presented in the form of synthesis. Within the theoretical framework of the French discourse analysis, this thesis combines historical, communicational, socio-political and linguistic approaches to analyze the debate. It focuses particularly on describing the production of the synthesis of this debate and their textual dimension in order to show the specific characteristics of the DNTE as well as its result which allows the government to deliberate and decide on the policies to adopt.

Bakgrund: Hjärtinfarkt är en av de vanligaste sjukdomarna och innebär livsomvälvande förändringar. Tiden efter hjärtinfarkten präglas av sårbarhet och att anpassa sig till den nya livssituationen. Återhämtningsperioden efter hjärtinfarkten är en transition i livet, som innebär att gå från ett tillstånd till ett annat, och påverkas av inre och yttre faktorer i personens liv. För att kunna ge ett bra stöd och främja en hälsosam transition är det viktigt att sjuksköterskan har en god förståelse för vad som påverkar återhämtningsperioden i en positiv eller negativ riktning. Syfte: Syftet var att beskriva personers upplevelser av återhämtningsperioden efter en hjärtinfarkt för att uppmärksamma vad som främjar och hämmar en hälsosam transition. Metod: För att svara på syftet gjordes en systematisk litteraturöversikt med inspiration från Roséns (2017) beskrivning. Nio kvalitativa artiklar inkluderades i analysen som genomfördes enligt Elo och Kyngäs (2008) beskrivning av deduktiv innehållsanalys. Resultat: Resultatet visade att det som främjar en hälsosam transition handlar om positiv livshantering, välgörande livsstil och stödjande socialt nätverk. Vidare visade resultatet att det som hämmar en hälsosam transition handlar om negativa känslor, begränsad fysisk kapacitet och problematik i socialt nätverk. Slutsats: För att kunna se personens unika förutsättningar för att uppnå en hälsosam transition, är det viktigt att sjuksköterskan ökar sin kunskap om den transition som personen genomgår och har en god och öppen relation med personen.

Thesis advisor: Irwin Blumer / This study examines the perceived impact of a parental empowerment project on parents of students of color transitioning into high school. The overarching problem addressed is the achievement gap. The study is an investigation of a means to increase the involvement of parents of color at an important transition. This is a gap closing measure because research dictates that this type of intervention can lead to higher academic achievement for minority students. To this end, seven participants constitute the sample group. Each sample member is treated as an individual case in keeping with the study's design as a qualitative case study. This study seeks to determine how these seven parents had their attitudes and behaviors shifted as a result of their participation in the aforementioned project, and which factors supported and inhibited their involvement as their children transitioned into high school. The researcher finds that all of the sample members perceived some benefit from their participation. These benefits for the parents include fostering a greater role understanding, increased ability to hold their children accountable, and an increased understanding of the high school curriculum. The monthly parent meetings, one of the three elements comprising the empowerment program, were most helpful for parents. Whereas, the scheduling of meetings made it difficult for members of the sample to be as involved as they wanted to be. Ultimately, the study concludes that a program which involves parents during their children's high school transition can help them increase their own sense of efficacy. It suggests opportunities for further research to be done on the impact of such a program on the actual academic performance of students. / Thesis (EdD) — Boston College, 2009. / Submitted to: Boston College. Lynch School of Education. / Discipline: Educational Administration.

Presented herein is the development, optimization and mechanistic investigation of an Cu catalytic system for the oxidation of sp 3 C-H bond of simple arenes to form C-N bond in a direct manner. Due to the prevalence of nitrogen containing molecules among biologically active synthetic and natural compounds, synthetic chemists have always been motivated to develop new efficient ways to directly transform ubiquitous carbonhydrogen (C-H) bonds into carbon- nitrogen (C-N) bonds. Recent advances in transition metal catalyzed C-H amination has demonstrated that it is not only possible but also practical to functionalize C-H bonds that are often considered inert in one step, circumventing more classical, sequential functional group interconversion approaches. Existing catalytic systems that promote the transition metal-catalyzed, amination of sp 3 C-H bonds displayed certain limitations, especially the lack of built-in versatility and stability in their amination reagents. To overcome these drawbacks of these existing catalytic system, our group developed a new Cu amination protocol that deployed versatile hydroxylamine-based with general structure RSO 2 NH-OAc as amination reagents. Although the reactivity of the catalytic system ranges from moderate to good, the catalytic system provided promising results using simple arene substrates. Further detailed mechanistic studies revealed that the reaction undergoes an unprecedented two subsequent cycles divided by a major intermediate PhCH 2 (NTsOAc). The proposed mechanism is consistent with radical clock experiments, observed reaction profiles, the need for excess of substrate, and the documented role of the ligand in the catalytic system. The exciting proposed mechanism led to a new type of copper catalyzed amination reaction using N- fluorobenzenesulfonimide (NFSI) as oxidant, which overcomes the need to use an excess of substrate. A wide range of unactivated amines HNR 1 R 2 , including sulfonamide and benzamide, can be used as amine sources, which enables the installation of different nitrogen groups on benzylic sp 3 C-H bond of a variety of substrates in moderate to excellent yield. Moreover, mechanistic experiments and critical analysis of related reactivity in the literature provide insight into the catalytic cycle, resulting in a proposal that details the role of both oxidant and amine source in the new system.

No description available.

Despite the breadth of research on the educational transition of young children, there has been little evidence, in Scotland, of this knowledge impacting on every day practice. The overall contention that emerges from the literature is that some children positively embrace the experience, while others face challenges and risk failure and regression. There is a need for research into the transition from the early years setting to school, which holds promise that the findings will be disseminated to stakeholders locally, nationally and internationally with the aim that the perspectives of young children are heard. This ethnographic study is an examination of the perspectives of 16 young children as they transition from an early years centre, Lilybank, to four primary schools, Northfield, Southfield, Eastfield and Westfield, in a Scottish city. Seven key qualitative questions were asked which explored how children, parents and professionals experienced this educational transition. Data was gathered from empirical methods such as participant observations, mind–mapping sessions, interviews and documentation – e.g., council procedures and school handbooks. Participant observations took place in the early years setting and the participating schools. Most of the interviews took place in the children’s homes, or in a convenient environment for the family, such as a local cafeteria. An analysis of the data shows that power is a central concept in understanding transitions. The voices of children, and their families, are often silenced by policy-makers, bureaucrats and professionals during the process, or overshadowed and undermined by mainstream procedures. Children are expected to become acquiescent, adjusting to coercive practices used in the school institution. However, the findings also show that some children find ways to creatively resist organisation. Unique life journeys involve differences and from their individual experiences, children construct elaborate knowledge. The views of children can (and do) add nuance to our understanding of how power impacts on their transition experience. Children’s accounts of discipline strategies used by the schools were insightful. The concept of power is under-theorised and under-explored in transitions. This study, therefore, adds to the growing body of transition research. Further, the findings of this study stress the need for policy makers and institutions to reflect on and question the complex role of power in young children’s transitions.

As an additional study, effect of tyrosine nitration on the BCD of protonated and metalated peptides was investigated. Some fragment ions that were inhibited in the ECD of protonated peptides were liberated in the ECD of metalated peptides. By theoretical calculation of the cation-pi and cation-nitro group coordination using the metal ions nitrated phenol complex as a model, it is found that the metal ions might favor coordinating with the nitro group of the nitrated tyrosine residue in the peptides. / In order to improve the performance of the electron capture dissociation (BCD) mass spectrometry for structural analysis of peptides/proteins, BCD of peptides cationized with various transition metal ions was investigated. It was found that peptides adducted with different divalent transition metal ions generated different BCD tandem mass spectra. For Mn2+and Zn2+, the incoming low-energy electron would not favor being trapped by the metal ions and instead trigger the usual BCD dissociation channel(s) via "hot-hydrogen" or "superbase" intermediates to form a series of c-/z·- fragments. For other first row transition metal ions, including Fe2+, Co2+, Ni 2+and Cu2+, reduction of the metal ions occurs preferentially during the electron capture event and lead to the formation of usual "slow-heating" type of fragment ions, i.e. metalated a-/y-fragments & metalated b-/y- fragments. / To further compare the behavior of metal ions with the same electronic configuration, BCD of Group IIB metal ions adducted peptides were investigated. In contrast to the ECD behavior of Zn2+ adducted peptides, peptide radical cations (M+· ) and fragment ions corresponding to losses of neutral side chain from M+· were observed in the ECD spectra of Hg2+ and Cd2+ adducted peptides. The experimental observations appeared to depend on the balance of the ionization energy of peptide and the solvation modulated ionization energies of the metal atom. The reduction of divalent metal ions by the electron capture event could induce spontaneous electron transfer from the peptide moiety to the monovalent metal centre and generate hydrogen-deficient M +· species. / Chen, Xiangfeng. / Adviser: T.-W. Dominic Chan. / Source: Dissertation Abstracts International, Volume: 73-06, Section: B, page: . / Thesis (Ph.D.)--Chinese University of Hong Kong, 2011. / Includes bibliographical references (leaves 131-139). / Electronic reproduction. Hong Kong : Chinese University of Hong Kong, [2012] System requirements: Adobe Acrobat Reader. Available via World Wide Web. / Electronic reproduction. [Ann Arbor, MI] : ProQuest Information and Learning, [201-] System requirements: Adobe Acrobat Reader. Available via World Wide Web. / Abstract also in Chinese.