Phase-space analysis of bosonic spontaneous emission

We present phase-space techniques for the modelling of spontaneous emission in two-level bosonic atoms. The positive-P representation is shown to give a full and complete description within the limits of our model. The Wigner representation, even when truncated at second order, is shown to need a doubling of the phase-space to allow for a positive-definite diffusion matrix in the appropriate Fokker-Planck equation and still fails to agree with the full quantum results of the positive-P representation. We show that quantum statistics and correlations between the ground and excited states affect the dynamics of the emission process, so that it is in general non-exponential. (c) 2005 Elsevier B.V. All rights reserved.

Asymptotically exact probability distribution for the Sinai model with finite drift

We obtain the exact asymptotic result for the disorder-averaged probability distribution function for a random walk in a biased Sinai model and show that it is characterized by a creeping behavior of the displacement moments with time, similar to v(mu n), where mu <1 is dimensionless mean drift. We employ a method originated in quantum diffusion which is based on the exact mapping of the problem to an imaginary-time Schrodinger equation. For nonzero drift such an equation has an isolated lowest eigenvalue separated by a gap from quasicontinuous excited states, and the eigenstate corresponding to the former governs the long-time asymptotic behavior.

Investigation of EDFA power transients in circuit-switched and packet-switched optical networks

Erbium-doped fibre amplifiers (EDFA’s) are a key technology for the design of all optical communication systems and networks. The superiority of EDFAs lies in their negligible intermodulation distortion across high speed multichannel signals, low intrinsic losses, slow gain dynamics, and gain in a wide range of optical wavelengths. Due to long lifetime in excited states, EDFAs do not oppose the effect of cross-gain saturation. The time characteristics of the gain saturation and recovery effects are between a few hundred microseconds and 10 milliseconds. However, in wavelength division multiplexed (WDM) optical networks with EDFAs, the number of channels traversing an EDFA can change due to the faulty link of the network or the system reconfiguration. It has been found that, due to the variation in channel number in the EDFAs chain, the output system powers of surviving channels can change in a very short time. Thus, the power transient is one of the problems deteriorating system performance. In this thesis, the transient phenomenon in wavelength routed WDM optical networks with EDFA chains was investigated. The task was performed using different input signal powers for circuit switched networks. A simulator for the EDFA gain dynamicmodel was developed to compute the magnitude and speed of the power transients in the non-self-saturated EDFA both single and chained. The dynamic model of the self-saturated EDFAs chain and its simulator were also developed to compute the magnitude and speed of the power transients and the Optical signal-to-noise ratio (OSNR). We found that the OSNR transient magnitude and speed are a function of both the output power transient and the number of EDFAs in the chain. The OSNR value predicts the level of the quality of service in the related network. It was found that the power transients for both self-saturated and non-self-saturated EDFAs are close in magnitude in the case of gain saturated EDFAs networks. Moreover, the cross-gain saturation also degrades the performance of the packet switching networks due to varying traffic characteristics. The magnitude and the speed of output power transients increase along the EDFAs chain. An investigation was done on the asynchronous transfer mode (ATM) or the WDM Internet protocol (WDM-IP) traffic networks using different traffic patterns based on the Pareto and Poisson distribution. The simulator is used to examine the amount and speed of the power transients in Pareto and Poisson distributed traffic at different bit rates, with specific focus on 2.5 Gb/s. It was found from numerical and statistical analysis that the power swing increases if the time interval of theburst-ON/burst-OFF is long in the packet bursts. This is because the gain dynamics is fast during strong signal pulse or with long duration pulses, which is due to the stimulatedemission avalanche depletion of the excited ions. Thus, an increase in output power levelcould lead to error burst which affects the system performance.

Multimodal spectral control of a quantum-dot diode laser for THz difference frequency generation

Generation of stable dual and/or multiple longitudinal modes emitted from a single quantum dot (QD) laser diode (LD) over a broad wavelength range by using volume Bragg gratings (VBG's) in an external cavity setup is reported. The LD operates in both the ground and excited states and the gratings give a dual-mode separation around each emission peak of 5 nm, which is suitable as a continuous wave (CW) optical pump signal for a terahertz (THz) photomixer device. The setup also generates dual modes around both 1180m and 1260 nm simultaneously, giving four simultaneous narrow linewidth modes comprising two simultaneous difference frequency pump signals. (C) 2011 American Institute of Physics.

Measurement of single spin asymmetry and fifth structure function for the p( e&ar; ,e'K +)Λ reaction with CEBAF Large Acceptance Spectrometer (CLAS)

The single spin asymmetry, ALT ′, and the polarized structure function, σ LT′, for the p( e&ar; , e′K +)Λ reaction in the resonance region have been measured and extracted using the CEBAF Large Acceptance Spectrometer (CLAS) at Jefferson Lab. Data were taken at an electron beam energy of 2.567 GeV. The large acceptance of CLAS allows for full azimuthal angle coverage over a large range of center-of-mass scattering angles. Results were obtained that span a range in Q 2 from 0.5 to 1.3 GeV2 and W from threshold up to 2.1 GeV and were compared to existing theoretical calculations. The polarized structure function is sensitive to the interferences between various resonant amplitudes, as well as to resonant and non-resonant amplitudes. This measurement is essential for understanding the structure of nucleons and searching for previously undetected nucleon excited states (resonances) predicted by quark models. The W dependence of the σ LT′ in the kinematic regions dominated by s and u channel exchange (cos qcmk = −0.50, −0.167, 0.167) indicated possible resonance structures not predicted by theoretical calculations. The σLT ′ behavior around W = 1.875 GeV could be the signature of a resonance predicted by the quark models and possibly seen in photoproduction. In the very forward angles where the reaction is dominated by the t-channel, the average σLT ′ was zero. There was no indication of the interference between resonances or resonant and non-resonant amplitudes. This might be indicating the dominance of a single t-channel exchange. Study of the sensitivity of the fifth structure function data to the resonance around 1900 MeV showed that these data were highly sensitive to the various assumptions of the models for the quantum number of this resonance. This project was part of a larger CLAS program to measure cross sections and polarization observables for kaon electroproduction in the nucleon resonance region. ^

Spectroscopy of Electroproduced Light to Medium Mass Lambda Hypernuclei

The E01-011 experiment at Jefferson Laboratory (JLab) studied light-to-medium mass Λ hypernuclei via the AZ + e → [special characters omitted] + e' + K+ electroproduction reaction. Precise measurement of hypernuclear ground state masses and excitation energies provides information about the nature of hyperon-nucleon interactions. Until recently, hypernuclei were studied at accelerator facilities with intense π+ and K- meson beams. The poor quality of these beams limited the resolution of the hypernuclear excitation energy spectra to about 1.5 MeV (FWHM). This resolution is not sufficient for resolving the rich structure observed in the excitation spectra. By using a high quality electron beam and employing a new high resolution spectrometer system, this study aims to improve the resolution to a few hundred keV with an absolute precision of about 100 keV for excitation energies. In this work the high-resolution excitation spectra of [special characters omitted], and [special characters omitted] hypernuclei are presented. In an attempt to emphasize the presence of the core-excited states we introduced a novel likelihood approach to particle identification (PID) to serve as an alternative to the commonly used standard hard-cut PID. The new method resulted in almost identical missing mass spectra as obtained by the standard approach. An energy resolution of approximately 400–500 keV (FWHM) has been achieved, an unprecedented value in hypernuclear reaction spectroscopy. For [special characters omitted] the core-excited configuration has been clearly observed with significant statistics. The embedded Λ hyperon increases the excitation energies of the 11B nuclear core by 0.5–1 MeV. The [special characters omitted] spectrum has been observed with significant statistics for the first time. The ground state is bound deeper by roughly 400 keV than currently predicted by theory. Indication for the core-excited doublet, which is unbound in the core itself, is observed. The measurement of [special characters omitted] provides the first study of a d-shell hypernucleus with sub-MeV resolution. Discrepancies of up to 2 MeV between measured and theoretically predicted binding energies are found. Similar disagreement exists when comparing to the [special characters omitted] mirror hypernucleus. Also the core-excited structure observed between the major s-, p- and d-shell Λ orbits is not consistent with the available theoretical calculations. In conclusion, the discrepancies found in this study will provide valuable input for the further development of theoretical models.

Quiralidade, superfície de energia potencial e dinâmica de complexos envolvendo H2O2 + gases nobres

Tese (doutorado)—Universidade de Brasília, Instituto de Física, 2015.

Analysis and control of transient spectra using time-dependent density functional theory.

215 p.

Measurement of picosecond lifetimes in neutron-rich Xe isotopes

Background: Lifetimes of nuclear excited states in fission fragments have been studied in the past following isotope separation, thus giving access mainly to the fragments' daughters and only to long-lived isomeric states in the primary fragments. For the first time now, short-lived excited states in the primary fragments, produced in neutron-induced prompt fission of U-235 and Pu-241, were studied within the EXILL&FATIMA campaign at the intense neutron-beam facility of the Institute Laue-Langevin in Grenoble. Purpose: We aim to investigate the quadrupole collective properties of neutron-rich even-even Xe-138,Xe-140,Xe-142 isotopes lying between the double shell closure N = 82 and Z = 50 and a deformed region with octupole collectivity. Method: The gamma rays emitted from the excited fragments were detected with a mixed array consisting of 8 HPGe EXOGAM Clover detectors (EXILL) and 16 LaBr3(Ce) fast scintillators (FATIMA). The detector system has the unique ability to select the interesting fragment making use of the high resolution of the HPGe detectors and determine subnanosecond lifetimes using the fast scintillators. For the analysis the generalized centroid difference method was used. Results: We show that quadrupole collectivity increases smoothly with increasing neutron number above the closed N = 82 neutron shell. Our measurements are complemented by state-of-the-art theory calculations based on shell-model descriptions. Conclusions: The observed smooth increase in quadrupole collectivity is similar to the evolution seen in the measured masses of the xenon isotopic chain and is well reproduced by theory. This behavior is in contrast to higher Z even-even nuclei where abrupt change in deformation occurs around N = 90.

Direct experimental evidence for a multiparticle-hole ground state configuration of deformed Mg-33

The first direct experimental evidence of a multiparticle-hole ground state configuration of the neutron-rich Mg-33 isotope has been obtained via intermediate energy (400 A MeV) Coulomb dissociation measurement. The major part similar to(70 +/- 13)% of the cross section is observed to populate the excited states of Mg-32 after the Coulomb breakup of Mg-33. The shapes of the differential Coulomb dissociation cross sections in coincidence with different core excited states favor that the valence neutron occupies both the s(1/2) and p(3/2) orbitals. These experimental findings suggest a significant reduction and merging of sd-pf shell gaps at N similar to 20 and 28. The ground state configuration of Mg-33 is predominantly a combination of Mg-32(3.0,3.5MeV; 2(-), 1(-)) circle times nu(s1/2), Mg-32(2.5MeV; 2(+)) circle times nu(p3/2), and Mg-32(0; 0(+)) circle times nu(p3/2). The experimentally obtained quantitative spectroscopic information for the valence neutron occupation of the s and p orbitals, coupled with different core states, is in agreement with Monte Carlo shell model (MCSM) calculation using 3 MeV as the shell gap at N = 20.

Theoretical Rationalization of the Singlet–Triplet Gap in OLEDs Materials: Impact of Charge-Transfer Character

New materials for OLED applications with low singlet–triplet energy splitting have been recently synthesized in order to allow for the conversion of triplet into singlet excitons (emitting light) via a Thermally Activated Delayed Fluorescence (TADF) process, which involves excited-states with a non-negligible amount of Charge-Transfer (CT). The accurate modeling of these states with Time-Dependent Density Functional Theory (TD-DFT), the most used method so far because of the favorable trade-off between accuracy and computational cost, is however particularly challenging. We carefully address this issue here by considering materials with small (high) singlet–triplet gap acting as emitter (host) in OLEDs and by comparing the accuracy of TD-DFT and the corresponding Tamm-Dancoff Approximation (TDA), which is found to greatly reduce error bars with respect to experiments thanks to better estimates for the lowest singlet–triplet transition. Finally, we quantitatively correlate the singlet–triplet splitting values with the extent of CT, using for it a simple metric extracted from calculations with double-hybrid functionals, that might be applied in further molecular engineering studies.

Photophysics and photochemistry of azole fungicides: triadimefon and triadimenol

Photophysics and photochemistry of pesticides triadimefon {1-(4-chlorophenoxy)-3,3-dimethyl-1-(1H-1,2,4-triazol-1-yl) butanone} and triadimenol {1-(4-chlorophenoxy)-3,3-dimethyl-1-(1H-1,2,4-triazol-1-yl) butan-2-ol} were studied in the solution. The excited singlet states were identified by comparison with the absorption spectra of adequate model compounds, in several solvents. The first excited singlet state of triadimefon is an n, pi* state localized on the carbonyl group, while higher excited states are localized on the chlorophenoxy group and have a pi, pi* character. The lowest singlet state of triadimenol is pi, pi* state, since a methoxyl group replaces the carbonyl group of triadimefon. Triadimefon shows a weak fluorescence from the n, pi* state, upon excitation at both 310 and 250 nm. This suggests a fast intramolecular energy transfer process from the localized pi, pi* state of the chlorophenoxy group to the n, pi* state of the carbonyl group. The photodegradation quantum yield of triadimefon in cyclohexane at 313 run is 0.022. Triadimenol is photostable, under the same conditions. Two major photodegradation products of triadimefon and triadimenol were identified: 4-chlorophenol and 1,2,4-triazole. 4-Chlorophenoxyl radicals were detected by flash photolysis, suggesting a homolytic cleavage of the C-O bond of the asymmetric carbon. (C) 2001 Elsevier Science B.V. All rights reserved.

Disorder driven transitions in non-equilibrium quantum systems

This thesis presents studies of the role of disorder in non-equilibrium quantum systems. The quantum states relevant to dynamics in these systems are very different from the ground state of the Hamiltonian. Two distinct systems are studied, (i) periodically driven Hamiltonians in two dimensions, and (ii) electrons in a one-dimensional lattice with power-law decaying hopping amplitudes. In the first system, the novel phases that are induced from the interplay of periodic driving, topology and disorder are studied. In the second system, the Anderson transition in all the eigenstates of the Hamiltonian are studied, as a function of the power-law exponent of the hopping amplitude.

In periodically driven systems the study focuses on the effect of disorder in the nature of the topology of the steady states. First, we investigate the robustness to disorder of Floquet topological insulators (FTIs) occurring in semiconductor quantum wells. Such FTIs are generated by resonantly driving a transition between the valence and conduction band. We show that when disorder is added, the topological nature of such FTIs persists as long as there is a gap at the resonant quasienergy. For strong enough disorder, this gap closes and all the states become localized as the system undergoes a transition to a trivial insulator.

Interestingly, the effects of disorder are not necessarily adverse, disorder can also induce a transition from a trivial to a topological system, thereby establishing a Floquet Topological Anderson Insulator (FTAI). Such a state would be a dynamical realization of the topological Anderson insulator. We identify the conditions on the driving field necessary for observing such a transition. We realize such a disorder induced topological Floquet spectrum in the driven honeycomb lattice and quantum well models.

Finally, we show that two-dimensional periodically driven quantum systems with spatial disorder admit a unique topological phase, which we call the anomalous Floquet-Anderson insulator (AFAI). The AFAI is characterized by a quasienergy spectrum featuring chiral edge modes coexisting with a fully localized bulk. Such a spectrum is impossible for a time-independent, local Hamiltonian. These unique characteristics of the AFAI give rise to a new topologically protected nonequilibrium transport phenomenon: quantized, yet nonadiabatic, charge pumping. We identify the topological invariants that distinguish the AFAI from a trivial, fully localized phase, and show that the two phases are separated by a phase transition.

The thesis also present the study of disordered systems using Wegner's Flow equations. The Flow Equation Method was proposed as a technique for studying excited states in an interacting system in one dimension. We apply this method to a one-dimensional tight binding problem with power-law decaying hoppings. This model presents a transition as a function of the exponent of the decay. It is shown that the the entire phase diagram, i.e. the delocalized, critical and localized phases in these systems can be studied using this technique. Based on this technique, we develop a strong-bond renormalization group that procedure where we solve the Flow Equations iteratively. This renormalization group approach provides a new framework to study the transition in this system.

Computational characterization of carbazole-benzonitrile derivatives for applications in Organic Light Emitting Diodes

The technology of Organic Light-Emitting Diodes has reached such a high level of reliability that it can be used in various applications. The required light emission efficiency can be achieved by transforming the triplet excitons into singlet states through Reverse InterSystem Crossing (RISC), which is the main process of a general mechanism called thermally activated delayed fluorescence (TADF). In this thesis, we theoretically analyzed two carbazole-benzonitrile (donor-acceptor) derivatives, 2,5-di(9H-carbazol-9-yl)benzonitrile (p-2CzBN) and 2,3,4,5,6-penta(9H-carbazol-9-yl)benzonitrile (5CzBN), and addressed the problem of how donor-acceptor (D-A) or donor-acceptor-donor (D-A-D) flexible molecular architectures influence the nature of the excited states and the emission intensity. Furthermore, we analyzed the RISC rates as a function of the conformation of the carbazole lateral groups, considering the first electronic states, S0, S1, T1 and T2, involved in TADF process. The two prototype molecules, p-2CzBN and 5CzBN, have a similar energy gap between the first singlet and triplet states (∆EST, a key parameter in the RISC rate), but different TADF performances. Therefore, other parameters must be considered to explain their different behavior. The oscillator strength of p-2CzBN, never tested as emitter in OLEDs, is similar to that of 5CzBN, which is an active TADF molecule. We also note that the presence of a second T2 triplet state, lower in energy than S1 only in 5CzBN, and the reorganization energies, associated with RISC processes involving T1 and T2, are important factors in differentiating the rates in p-2CzBN and 5CzBN. For p-2CzBN, the RISC rate from T2 to S1 is surprisingly higher than that from T1 to S1, in disagreement with El-Sayed rules, due to a large reorganization energy associated to the T1 to S1, process; while the contrary occurs for 5CzBN. These insights are important for designing new TADF emitters based on the benzo-carbazole architecture.