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Displaying Results 151 - 175 of 13365 on page 7 of 535
Marked
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Using Perceptual Feedback To Determine Time-Space Threshold Values For Dead Reckoning
(2006)
Kenny, Alan; McLoone, Seamus; Ward, Tomas E.; Delaney, Declan
Using Perceptual Feedback To Determine Time-Space Threshold Values For Dead Reckoning
(2006)
Kenny, Alan; McLoone, Seamus; Ward, Tomas E.; Delaney, Declan
Abstract:
Entity state prediction mechanisms are used in order to reduce the number of packets required to maintain a consistent state in a Distributed Interactive Application (DIA). Typically in the case where the entity is representing a participant in a networked game this is achieved by continually comparing the output of a prediction algorithm against a player’s actual state. The state usually comprises position and orientation information in such cases. If the error exceeds a pre-defined threshold value, then an update packet is transmitted, which contains the player’s latest trajectory information. However, obtaining a suitable threshold value remains one of the key challenges that face such entity state prediction techniques. Furthermore, these methods can employ two different threshold metrics. These are spatial, which exploits distance measures, and time space, which uses both time and distance measures. While a spatial threshold value can be arguably determined based on a prior kno...
http://mural.maynoothuniversity.ie/1282/
Marked
Mark
Recent Advances in Real-Time Musical Effects, Synthesis, and Virtual Analog Models
(2011)
Pakarinen, Jyri; Valimaki, Vesa; Fontana, Federico; Lazzarini, Victor; Abel, Jonathan
Recent Advances in Real-Time Musical Effects, Synthesis, and Virtual Analog Models
(2011)
Pakarinen, Jyri; Valimaki, Vesa; Fontana, Federico; Lazzarini, Victor; Abel, Jonathan
Abstract:
Real.-time musical effects processing and synthesis play a part in nearly all musical sounds encountered in the contemporary enviroflDlent. Virtually all recorded or electrically amplified music in the last few decades uses effects processing, such as artificial reverberation or dynamic compression, and synthetic instrument sounds play an increasingly larger part in the total musical spectrum. Furthermore, the vast majority of these effects are presently implemented using digital signal processing (DSP), mainly due to the flexibility and low cost of modern digital devices. For live music, realtime operation of these effec.:ts and synthesis algorithms is obviously of paramount importance. However, also recorded music typically requires real-time operation of these devices and algorithms, because performers usually wish to hear the final, processed sound of their instrument while playing. The purpose of this article is to provide the reader with an overview of some of the recent advan...
http://mural.maynoothuniversity.ie/4696/
Marked
Mark
Sinusoids, noise and transients: spectral analysis, feature detection and real-time transformations of audio signals for musical applications
(2012)
Glover, John C.
Sinusoids, noise and transients: spectral analysis, feature detection and real-time transformations of audio signals for musical applications
(2012)
Glover, John C.
Abstract:
This thesis examines the possibilities for real-time transformations of musical audio signals using sinusoidal models. Four open-source software libraries were developed with the goal of providing real-time spectral synthesis by analysis tools for composers, musicians, researchers and audio signal processing developers. The first of these, called Simpl, provides a consistent API for interacting with established sinusoidal modelling systems from the literature, and integrates seamlessly with a powerful suite of libraries for scientific computing. Sinusoidal models have been used to transform slowly-varying quasi-harmonic signals with much success, but they have well-documented weaknesses in dealing with transient signal regions. This problem is significant, as in monophonic musical sounds, transient locations often correspond with the attack section of notes and this region plays a large part in our perception of timbre. However in order to improve the synthesis of note attack transi...
http://mural.maynoothuniversity.ie/4523/
Marked
Mark
A Simple and Effective Real-Time Controller for Wave Energy Converters
(2013)
Fusco, Francesco; Ringwood, John
A Simple and Effective Real-Time Controller for Wave Energy Converters
(2013)
Fusco, Francesco; Ringwood, John
Abstract:
A novel strategy for the real-time control of oscillating wave energy converters (WECs) is proposed. The controller tunes the oscillation of the system such that it is always in phase with the wave excitation force and the amplitude of the oscillation is within given constraints. Based on a nonstationary, harmonic approximation of the wave excitation force, the controller is easily tuned in real-time for performance and constraints handling, through one single parameter of direct physical meaning. The effectiveness of the proposed solution is assessed for a heaving system in one degree of freedom, in a variety of irregular (simulated and real) wave conditions. A performance close to reactive control and to model predictive control is achieved. Additional benefits in terms of simplicity and robustness are obtained.
http://mural.maynoothuniversity.ie/4411/
Marked
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Time-stretching using the instantaneous frequency distribution and partial tracking
(2005)
Lazzarini, Victor; Timoney, Joseph; Lysaght, Thomas
Time-stretching using the instantaneous frequency distribution and partial tracking
(2005)
Lazzarini, Victor; Timoney, Joseph; Lysaght, Thomas
Abstract:
This article presents a method of signal timescale modification using spectral analysis-resynthesis. It discusses an alternative technique for instantaneous frequency estimation, the Instantaneous Frequency Distribution (IFD). The partial tracking analysis employed in this process is explained in some detail, followed by a look into the resynthesis method. The article discusses this technique of time-stretching in comparison to the standard phase vocoder process. Performance details and specific aspects of this implementation are examined, including the C++ code for a time-stretching application.
http://mural.maynoothuniversity.ie/4178/
Marked
Mark
Metamorph: Real-Time High-Level Sound Transformations Based On A Sinusoids Plus Noise Plus Transients Model
(2012)
Glover, John C.; Lazzarini, Victor; Timoney, Joseph
Metamorph: Real-Time High-Level Sound Transformations Based On A Sinusoids Plus Noise Plus Transients Model
(2012)
Glover, John C.; Lazzarini, Victor; Timoney, Joseph
Abstract:
Spectral models provide ways to manipulate musical audio signals that can be both powerful and intuitive, but high-level control is often required in order to provide flexible real-time control over the potentially large parameter set. This paper introduces Metamorph, a new open source library for high-level sound transformation. We describe the real-time sinusoids plus noise plus transients model that is used by Metamorph and explain the opportunities that it provides for sound manipulation.
http://mural.maynoothuniversity.ie/4122/
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Time-lapse resistivity analysis of Quaternary sediments in the Midlands of Ireland
(2012)
Pellicer, Xavier M.; Zarroca, Mario; Gibson, Paul
Time-lapse resistivity analysis of Quaternary sediments in the Midlands of Ireland
(2012)
Pellicer, Xavier M.; Zarroca, Mario; Gibson, Paul
Abstract:
Electrical Resistivity Tomography (ERT) data are influenced by a number of factors associated with the subsurface such as porosity, moisture content and lithology; as well as external factors such as rainfall and temperature. Two time-lapse ERT profiles with 5 m and two with 2 m electrode spacings were acquired over a range of Quaternary sediment types encompassing till, esker gravel, glaciofluvial sand and silt and glaciolacustrine silt/clay. Data were collected on a monthly basis during 2006 at a site located in the Midlands of Ireland in order to evaluate the influence of such conditioning factors on the resistivity of the subsurface. Effective recharge, the depth of investigation, the texture and the internal architecture of the different sediment types and temperature variation are the main factors influencing the resistivity seasonal variation. The shallow subsurface (b3 m depth) showed a direct relationship between resistivity variation and effective recharge, whereas, an inc...
http://mural.maynoothuniversity.ie/4063/
Marked
Mark
Time-Dependent Density Functional Theory as a Foundation for a Firmer Understanding of Sum-Over-States Density Functional Perturbation Theory: “Loc.3” Approximation
(2003)
Fadda, Elisa; Casida, Mark E.; Salahub, Dennis R.
Time-Dependent Density Functional Theory as a Foundation for a Firmer Understanding of Sum-Over-States Density Functional Perturbation Theory: “Loc.3” Approximation
(2003)
Fadda, Elisa; Casida, Mark E.; Salahub, Dennis R.
Abstract:
Sum-over-states density functional perturbation theory (SOS-DFPT) (Malkin, V. G.; Malkina, O. L.; Casida, M. E.; Salahub, D. R. J Am Chem Soc 1994, 116, 5898) has been successful as a method for calculating nuclear magnetic resonance (NMR) chemical shifts. The key to this success is the introduction of an ad hoc correction to the excitation energies represented by simple orbital energy differences in uncoupled density functional theory. It has been suggested (Jamorski, C.; Casida, M. E.; Salahub, D. R. J Chem Phys 1996, 104, 5134) that the good performance of this methodology could be partly explained by the resemblance of the corrected excitation energy to the orbital energy difference given by time-dependent density functional theory (TDDFT). In fact, according to exact (wave function) time-dependent perturbation theory, both magnetic and electric perturbations may be described using essentially the same simple SOS expression. However in adiabatic TDDFT, with no explicit relativis...
http://mural.maynoothuniversity.ie/7831/
Marked
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It's a Man's World: A Qualitative Study of the (Non) Mediation of Women and Politics on Prime Time During the 2011 General Election
(2014)
O'Brien, Anne
It's a Man's World: A Qualitative Study of the (Non) Mediation of Women and Politics on Prime Time During the 2011 General Election
(2014)
O'Brien, Anne
Abstract:
The manner in which women appear, or disappear, within the Irish politics–media intersection is a question central to understanding the nature of contemporary politics for Irish women. This article explores the manner in which the 2011 General Election coverage broadcast on RTE´ ’s flagship current affairs series Prime Time was gendered. The representation of Irish women’s engagement in politics was constituted through four dominant frames. Firstly, women are marginalised by being ‘framed out’ of the political picture, secondly, they are framed through a visual gendering of politicians which presents women in a limited manner, thirdly, the source-frame is not applied equally to men and women on Prime Time and finally, women are framed as participants only in a limited set of topics for discussion.
http://mural.maynoothuniversity.ie/11851/
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Have the England and Wales Guidelines affected sentencing severity? An Empirical analysis using a scale of severity and time-series analyses.
(2019)
Pina-Sánchez, Jose; Gosling, John Paul; Chung, Hye-In; Bourgeois, Elizabeth; Geneletti,...
Have the England and Wales Guidelines affected sentencing severity? An Empirical analysis using a scale of severity and time-series analyses.
(2019)
Pina-Sánchez, Jose; Gosling, John Paul; Chung, Hye-In; Bourgeois, Elizabeth; Geneletti, Sara; Marder, Ian D.
Abstract:
Sentence severity has increased in England and Wales in recent years. The causes of the increase remain unclear. One possible explanation relates to the introduction of sentencing guidelines, which seem to coincide in time with the increase in sentence severity. To date, investigations of this hypothesis have been limited to simple exploratory analyses or to specific offences. We use a new scale of sentence severity—developed using Thurstone scaling and the participation of 21 magistrates— and time-series modelling to explore whether a causal effect can be attributed to seven different guidelines. We corroborate the existence of an increase in sentence severity; however, we do not find conclusive evidence pointing at the guidelines having caused it.
http://mural.maynoothuniversity.ie/11732/
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Data imputation in a short-run space-time series: A Bayesian approach
(2017)
Pforte, Lars; Brunsdon, Chris; Cahalane, Conor; Charlton, Martin
Data imputation in a short-run space-time series: A Bayesian approach
(2017)
Pforte, Lars; Brunsdon, Chris; Cahalane, Conor; Charlton, Martin
Abstract:
This paper discusses a project on the completion of a database of socio-economic indicators across the European Union for the years from 1990 onward at various spatial scales. Thus the database consists of various time series with a spatial component. As a substantial amount of the data was missing a method of imputation was required to complete the database. A Markov Chain Monte Carlo approach was opted for. We describe the Markov Chain Monte Carlo method in detail. Furthermore, we explain how we achieved spatial coherence between different time series and their observed and estimated data points.
http://mural.maynoothuniversity.ie/11351/
Marked
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An Investigation of Hypofrontality in an Animal Model of Schizophrenia Using Real-Time Microelectrochemical Sensors for Glucose, Oxygen, and Nitric Oxide
(2013)
Finnerty, Niall J.; Bolger, Fiachra B.; Pålsson, Erik; Lowry, John P.
An Investigation of Hypofrontality in an Animal Model of Schizophrenia Using Real-Time Microelectrochemical Sensors for Glucose, Oxygen, and Nitric Oxide
(2013)
Finnerty, Niall J.; Bolger, Fiachra B.; Pålsson, Erik; Lowry, John P.
Abstract:
Glucose, O2, and nitric oxide (NO) were monitored in real time in the prefrontal cortex of freely moving animals using microelectrochemical sensors following phencyclidine (PCP) administration. Injection of saline controls produced a decrease in glucose and increases in both O2 and NO. These changes were short-lived and typical of injection stress, lasting ca. 30 s for glucose and between 2 and 6 min for O2 and NO, respectively. Subchronic PCP (10 mg/kg) resulted in increased motor activity and increases in all three analytes lasting several hours: O2 and glucose were uncoupled with O2 increasing rapidly following injection reaching a maximum of 70% (ca. 62 μM) after ca. 15 min and then slowly returning to baseline over a period of ca. 3 h. The time course of changes in glucose and NO were similar; both signals increased gradually over the first hour post injection reaching maxima of 55% (ca. 982 μM) and 8% (ca. 31 nM), respectively, and remaining elevated to within 1 h of returning...
http://mural.maynoothuniversity.ie/7005/
Marked
Mark
The phenomenology of time: reflections from the Lebenswelt
(2013)
Costello, Gabriel J.; Donnellan, Brian
The phenomenology of time: reflections from the Lebenswelt
(2013)
Costello, Gabriel J.; Donnellan, Brian
Abstract:
The aim of this study is to reflect on how time was perceived by different actors during a longitudinal study of innovation in the lebenswelt –in this case a multi-national subsidiary (Costello, 2010). It aims to address the call by Markus (2000) that information systems (IS) research must incorporate the concepts of both history and time in their management and organization studies.
http://mural.maynoothuniversity.ie/10887/
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The Origin of Time
(2017)
Stifter, David
The Origin of Time
(2017)
Stifter, David
Abstract:
One of the words for ‘time’ in the Celtic languages is the etymon represented by OIr. aimser (ā, f), W amser (masc.), OCorn. anser (n for m probably a scribal error), OBret. amser, ModBret. amzer (fem.). In OW, amser occurs as a temporal and causal conjunction ‘when; because’ (Falileyev 2000: 6). In accordance with a cross-linguistic tendency, these words for ‘time’ can also refer to the ‘wea-ther’,2 thereby evidencing a remarkable semantic shift of reference from a primary abstract3 concept to a phenomenon of daily practical experience.
http://mural.maynoothuniversity.ie/10164/
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Absolute stability and Lyapunov–Krasovskii functionals for switched nonlinear systems with time-delay
(2014)
Aleksandrov, Alexander; Mason, Oliver
Absolute stability and Lyapunov–Krasovskii functionals for switched nonlinear systems with time-delay
(2014)
Aleksandrov, Alexander; Mason, Oliver
Abstract:
We derive conditions for the existence of Lyapunov–Krasovskii functionals for a number of classes of nonlinear switched systems with time-delay. In particular, we first give conditions for systems of retarded type that relax those recently described in Sun and Wang (2013) [18]. Using similar techniques, related results are then derived for coupled differential-difference systems and for systems of neutral type. Finally, we briefly note some corresponding results for discrete-time systems.
http://mural.maynoothuniversity.ie/10025/
Marked
Mark
The Persistence of Sperm and the Development of Time Since Intercourse (TSI) Guidelines in Sexual Assault Cases at Forensic Science Ireland, Dublin, Ireland
(2017)
Casey, David G.; Domijan, Katarina; MacNeill, Sarah; Rizet, Damien; O'Connell, Dec...
The Persistence of Sperm and the Development of Time Since Intercourse (TSI) Guidelines in Sexual Assault Cases at Forensic Science Ireland, Dublin, Ireland
(2017)
Casey, David G.; Domijan, Katarina; MacNeill, Sarah; Rizet, Damien; O'Connell, Declan; Ryan, Jennifer M.
Abstract:
The persistence of sperm using confirmatory microscopic analysis, the persistence of sperm with tails, time since intercourse (TSI) analysis, and results from the acid phosphatase (AP) reaction from approximately 5581 swabs taken from circa 1450 sexual assault cases are presented. The observed proportions of sperm in the vagina and anus declines significantly after 48 h TSI, and sperm on oral swabs were observed up to 15 h TSI. The AP reaction as a predictor of sperm on intimate swabs is questioned. All AP reaction times gave a low true positive rate; 23% of sperm‐positive swabs gave a negative AP reaction time. We show the AP reaction is an unsafe and an unreliable predictor of sperm on intimate swabs. We propose that TSI not AP informs precase assessment and the evaluative approach for sexual assault cases. To help inform an evaluative approach, TSI guidelines are presented.
http://mural.maynoothuniversity.ie/10013/
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Model Parameter And Time Delay Estimation Using Gradient Methods
(1994)
O'Dwyer, Aidan; Ringwood, John
Model Parameter And Time Delay Estimation Using Gradient Methods
(1994)
O'Dwyer, Aidan; Ringwood, John
Abstract:
A number of approaches have been proposed for parameter and time delay estimation of process models in single input, single output (SISO) control systems using gradient descent algorithms; some of these approaches involve the selection of a rational polynomial that is used to approximate time delay variations. This paper takes a generalised approach to the investigation of the most appropriate choice of the rational polynomial, and the gradient descent algorithm, to be used.
http://mural.maynoothuniversity.ie/9537/
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Mark
Short-Term Wave Forecasting for Real-Time Control of Wave Energy Converters
(2010)
Fusco, Francesco; Ringwood, John
Short-Term Wave Forecasting for Real-Time Control of Wave Energy Converters
(2010)
Fusco, Francesco; Ringwood, John
Abstract:
Real-time control of wave energy converters requires knowledge of future incident wave elevation in order to approach optimal efficiency of wave energy extraction. We present an approach where the wave elevation is treated as a time series and it is predicted only from its past history. A comparison of a range of forecasting methodologies on real wave observations from two different locations shows how the relatively simple linear autoregressive model, which implicitly models the cyclical behavior of waves, can offer very accurate predictions of swell waves for up to two wave periods into the future.
http://mural.maynoothuniversity.ie/9486/
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Mark
A classification of techniques for the compensation of time delayed processes. Part 2. Structurally optimised controllers
(1999)
O'Dwyer, Aidan; Ringwood, John
A classification of techniques for the compensation of time delayed processes. Part 2. Structurally optimised controllers
(1999)
O'Dwyer, Aidan; Ringwood, John
Abstract:
Structurally optimised controllers are those in which the controller structure and parameters are adapted optimally to the structure and parameters of the process model [1, 2]. A classification of such controllers for time delay processes is provided.
http://mural.maynoothuniversity.ie/9516/
Marked
Mark
A classification of techniques for the compensation of time delayed processes. Part 1. Parameter optimised controllers
(1999)
O'Dwyer, Aidan; Ringwood, John
A classification of techniques for the compensation of time delayed processes. Part 1. Parameter optimised controllers
(1999)
O'Dwyer, Aidan; Ringwood, John
Abstract:
Modern Applied Mathematical Techniques in Circuits, Systems An extensive literature exists on the compensation of time delayed processes. It is possible to identify themes that are common to many of the available techniques. The intention of the two parts of this paper is to provide a framework against which the literature may be viewed; Part 1 of the paper considers the use of parameter optimised controllers for the compensation problem, with Part 2 of the paper considering the use of structurally optimised compensators. Conclusions are drawn at the end of Part 2.
http://mural.maynoothuniversity.ie/9514/
Marked
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Examining the Effects of Time-Space Measures on the Hybrid Strategy Model in Networked Virtual Environments
(2006)
Marshall, Damien; McLoone, Seamus; Delaney, Declan; Ward, Tomas E.
Examining the Effects of Time-Space Measures on the Hybrid Strategy Model in Networked Virtual Environments
(2006)
Marshall, Damien; McLoone, Seamus; Delaney, Declan; Ward, Tomas E.
Abstract:
Scalability is an important issue in the design of networked virtual environments (NVEs). In order to achieve scalability, it is essential to minimise the network traffic required to maintain overall consistency in the NVE. A popular method of achieving this is via entity behaviour prediction mechanisms, such as dead reckoning and the hybrid strategy model (HSM). Typically, the performance of such mechanisms is rated by the number of network packets they generate. However, it is also important that their impact on overall consistency is investigated. Absolute consistency is the degree to which different views of a NVE on remote hosts correspond. In previous work, it was shown that the use of a spatial threshold with dead reckoning can result in unbounded local absolute consistency. A solution that employed a time-space error threshold measure was shown to remedy this issue. In this paper, the scope of the time-space measure is extended to include the HSM. It is shown how the HSM can...
http://mural.maynoothuniversity.ie/8772/
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Mark
Real-time large-scale dense RGB-D SLAM with volumetric fusion
(2015)
Whelan, Thomas; Kaess, Michael; Johannsson, Hordur; Fallon, Maurice; Leonard, John J.; ...
Real-time large-scale dense RGB-D SLAM with volumetric fusion
(2015)
Whelan, Thomas; Kaess, Michael; Johannsson, Hordur; Fallon, Maurice; Leonard, John J.; McDonald, John
Abstract:
We present a new simultaneous localization and mapping SLAM system capable of producing high-quality globally consistent surface reconstructions over hundreds of meters in real time with only a low-cost commodity RGB-D sensor. By using a fused volumetric surface reconstruction we achieve a much higher quality map over what would be achieved using raw RGB-D point clouds. In this paper we highlight three key techniques associated with applying a volumetric fusion-based mapping system to the SLAM problem in real time. First, the use of a GPU-based 3D cyclical buffer trick to efficiently extend dense every-frame volumetric fusion of depth maps to function over an unbounded spatial region. Second, overcoming camera pose estimation limitations in a wide variety of environments by combining both dense geometric and photometric camera pose constraints. Third, efficiently updating the dense map according to place recognition and subsequent loop closure constraints by the use of an 'as-r...
http://mural.maynoothuniversity.ie/8270/
Marked
Mark
Economical LBS for public transport: Real-time monitoring and dynamic scheduling service
(2008)
Zheng, Jianghua; Winstanley, Adam C.; Yan, Lei; Fotheringham, Stewart
Economical LBS for public transport: Real-time monitoring and dynamic scheduling service
(2008)
Zheng, Jianghua; Winstanley, Adam C.; Yan, Lei; Fotheringham, Stewart
Abstract:
Public transportation plays an increasingly important role in building sustainable cities. However, a major deterrent to using public transport is the uncertainty of the length of waiting times at stops. This research suggests a solution based on location tracking based on an example of the use of tram transportation in Blackpool, north-west England. It utilises two mobile services: one involving real-time monitoring; the other involving dynamic scheduling. The former is intended for use by public transport managers. The later is intended for use by the general public. Both provide information on the current location of the next tram and its estimated arrival time. The system, TramInfo, was built by PHP and AJAX and the embedded application software was developed by J2ME based on Symbian OS. Future work is also discussed.
http://mural.maynoothuniversity.ie/8097/
Marked
Mark
In vivo characterisation of a Nafion®-modified Pt electrode for real-time nitric oxide monitoring in brain extracellular fluid
(2011)
Finnerty, Niall J.; O'Riordan, Saidhbhe; Brown, Finbar O.; Serra, Pier A.; O'...
In vivo characterisation of a Nafion®-modified Pt electrode for real-time nitric oxide monitoring in brain extracellular fluid
(2011)
Finnerty, Niall J.; O'Riordan, Saidhbhe; Brown, Finbar O.; Serra, Pier A.; O'Neill, Robert D.; Lowry, John P.
Abstract:
A Nafion®-modified Pt sensor developed for real-time neurochemical monitoring in freely-moving animals has now been characterised in vivo for the detection of nitric oxide (NO). Experiments were undertaken to test sensitivity, selectivity and stability. In control experiments, local administration of aCSF resulted in a decrease in signal (42 ± 12 pA, n = 9), while systemic administration of saline caused a transient increase in signal (22 ± 3 pA, n = 9) from baseline levels. Local MD perfusions of known concentrations of NO (1 mM) and L-arginine (720 μM) caused significant increases in current (4 ± 1 nA (n = 7) and 271 ± 37 pA (n = 5) respectively) while systemic administration of the non-selective NOS inhibitor L-NAME produced a significant decrease in current (91 ± 19 pA, n = 4) compared to baseline levels. Confirmation that the sensor remained selective was achieved by injection of ascorbic acid (2 g kg−1, i.p). The oxidation current showed no variation over the selected time int...
http://mural.maynoothuniversity.ie/8024/
Marked
Mark
An investigation into the photochemistry of, and the electrochemically induced CO-loss from, [(CO)5MC(OMe)Me](M = Cr or W) using low-temperature matrix isolation, picosecond infrared spectroscopy, cyclic voltammetry, and time-dependent density functional theory
(2015)
McMahon, Suzanne; Amirjalayer, Saeed; Buma, Wybren J.; Halpin, Yvonne; Long, Conor; Roo...
An investigation into the photochemistry of, and the electrochemically induced CO-loss from, [(CO)5MC(OMe)Me](M = Cr or W) using low-temperature matrix isolation, picosecond infrared spectroscopy, cyclic voltammetry, and time-dependent density functional theory
(2015)
McMahon, Suzanne; Amirjalayer, Saeed; Buma, Wybren J.; Halpin, Yvonne; Long, Conor; Rooney, A. Denise; Woutersenc, Sander; Pryce, Mary T.
Abstract:
The photophysics and photochemistry of [(CO)5MC(OMe)Me] (M = Cr or W) were investigated using picosecond time-resolved infrared spectroscopy (M = Cr or W), low-temperature matrix isolation techniques (M = Cr), and time-dependent density functional calculations (M = Cr or W). These studies provide unambiguous evidence for the photochemical formation of a long-lived, 18-electron metallaketene species capable of acting as a synthetically useful intermediate. For the Cr complex, an intermediate metallacyclopropanone singlet excited state was detected on the reaction path to the metallaketene species. This metallacyclopropanone excited state species has a lifetime of less than 100 ps and a characteristic bridging carbonyl band at 1770 cm−1. The tungsten ketene species was also detected but in contrast to the chromium system, this forms directly from a low-lying triplet excited state. The electrochemical release of CO showed a greater efficiency for the chromium complex when compared to t...
http://mural.maynoothuniversity.ie/7810/
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