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- Title
- Theoretical Study of Negative Molecular Ions Relevant to the Interstellar and Laboratory Plasma.
- Creator
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Khamesian, Marjan, Kokoouline, Viatcheslav, Argenti, Luca, Saha, Haripada, Masunov, Artem, University of Central Florida
- Abstract / Description
-
Recently, several negative molecular ions, CnN? (n = 1, 3, 5) and CnH? (n = 4, 6, 8), were observed in the interstellar medium (ISM). It was suggested that the anions are formed in the ISM by the process of radiative electron attachment (REA). A simple statistical model was developed in 1980's to estimate rate coefficients of the REA reactions. Some of the rate coefficients obtained in the model are consistent with the observations, the others are not. More importantly, some of the...
Show moreRecently, several negative molecular ions, CnN? (n = 1, 3, 5) and CnH? (n = 4, 6, 8), were observed in the interstellar medium (ISM). It was suggested that the anions are formed in the ISM by the process of radiative electron attachment (REA). A simple statistical model was developed in 1980's to estimate rate coefficients of the REA reactions. Some of the rate coefficients obtained in the model are consistent with the observations, the others are not. More importantly, some of the approximations employed in the model are not physically justified.The aim of this thesis is a development of a quantum-mechanical approach to study the process of radiative electron attachment to linear molecules of astrophysical interest. The approach is based on accurate ab initio calculations of electronic bound and continuum states of the negative ion. Cross sections and rate coefficients for formation of the following molecular negative ions by REA were determined: CN?, C2H?, C3N?, C4H?, C5N?, C6H?, and C8H?. All the calculations presented in the thesis were carried out using the MOLPRO and UK R-matrix (Quantemol)suites of programs. Uncertainty quantification of the results, obtained for each studied system, was performed. A second process, closely related to the radiative electron attachment, photodetachment (PD), was also studied in the thesis. Photodetachment cross sections for the CnN? (n = 1, 3, 5), CnH? (n = 4, 6, 8) and C2? molecules were determined using an approach similar to the one employed for REA from the same transition dipole moment matrix elements. The obtained REA cross sections and rate coefficients were validated by comparing the present theoretical results with the experimental data from recent photodetachment experiments.The present results suggest that the observed abundance of these ions in the ISM can hardly be explained by the REA process. In other words, these anions are formed in the interstellar medium by a process different than radiative electron attachment.Dissociative electron attachment (DEA) is another process of anion formation, which could possibly explain formation of certain molecular anions in the ISM. The ClF attachment was studied using a first principle approach.A good agreement with experimental data was demonstrated.A theoretical approach to evaluate cross sections for rotational excitation of linear neutral molecules by an electron impact was developed and applied to acetylene, HCCH. The differential cross sections for e-HCCH scattering were calculated between energies 0.1 eV and 10 eV. The momentum transfer cross section and eigenphases for e-HCCH scattering were also calculated.
Show less - Date Issued
- 2017
- Identifier
- CFE0006612, ucf:51295
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0006612
- Title
- Prediction of Optical Properties of Pi-Conjugated Organic Materials for Technological Innovations.
- Creator
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Nayyar, Iffat, Masunov, Artem, Saha, Haripada, Stolbov, Sergey, Gesquiere, Andre, University of Central Florida
- Abstract / Description
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Organic ?-conjugated solids are promising candidates for new optoelectronic materials. The large body of evidence points at their advantageous properties such as high charge-carrier mobility, large nonlinear polarizability, mechanical flexibility, simple and low cost fabrication and superior luminescence. They can be used as nonlinear optical (NLO) materials with large two-photon absorption (2PA) and as electronic components capable of generating nonlinear neutral (excitonic) and charged ...
Show moreOrganic ?-conjugated solids are promising candidates for new optoelectronic materials. The large body of evidence points at their advantageous properties such as high charge-carrier mobility, large nonlinear polarizability, mechanical flexibility, simple and low cost fabrication and superior luminescence. They can be used as nonlinear optical (NLO) materials with large two-photon absorption (2PA) and as electronic components capable of generating nonlinear neutral (excitonic) and charged (polaronic) excitations. In this work, we investigate the appropriate theoretical methods used for the (a) prediction of 2PA properties for rational design of organic materials with improved NLO properties, and (b) understanding of the essential electronic excitations controlling the energy-transfer and charge-transport properties in organic optoelectronics. Accurate prediction of these electro-optical properties is helpful for structure-activity relationships useful for technological innovations.In Chapter 1 we emphasize on the potential use of the organic materials for these two applications. The 2PA process is advantageous over one-photon absorption for deep-tissue fluorescence microscopy, photodynamic therapy, microfabrication and optical data storage owing to the three-dimensional spatial selectivity and improved penetration depth in the absorbing or scattering media. The design of the NLO materials with large 2PA cross-sections may reduce the optical damage due to the use of the high intensity laser beams for excitation. The organic molecules also possess self-localized excited states which can decay radiatively or nonradiatively to form excitonic states. This suggests the use of these materials in the electroluminescent devices such as light-emitting diodes and photovoltaic cells through the processes of exciton formation or dissociation, respectively. It is therefore necessary to understand ultrafast relaxation processes required in understanding the interplay between the efficient radiative transfer between the excited states and exciton dissociation into polarons for improving the efficiency of these devices. In Chapter 2, we provide the detailed description of the various theoretical methods applied for the prediction as well as the interpretation of the optical properties of a special class of substituted PPV [poly (p-phenylene vinylene)] oligomers. In Chapter 3, we report the accuracy of different second and third order time dependent density functional theory (TD-DFT) formalisms in prediction of the 2PA spectra compared to the experimental measurements for donor-acceptor PPV derivatives. We recommend a posteriori Tamm-Dancoff approximation method for both qualitative and quantitative analysis of 2PA properties. Whereas, Agren's quadratic response methods lack the double excitations and are not suitable for the qualitative analysis of the state-specific contributions distorting the overall quality of the 2PA predictions. We trace the reasons to the artifactual excited states above the ionization threshold. We also study the effect of the basis set, geometrical constraints and the orbital exchange fraction on the 2PA excitation energies and cross-sections. Higher exchange (BMK and M05-2X) and range-separated (CAM-B3LYP) hybrid functionals are found to yield inaccurate predictions both quantitatively and qualitatively. The failure of the exchange-correlation (XC) functionals with correct asymptotic is traced to the inaccurate transition dipoles between the valence states, where functionals with low HF exchange succeed. In Chapter 4, we test the performance of different semiempirical wavefunction theory methods for the prediction of 2PA properties compared to the DFT results for the same set of molecules. The spectroscopic parameterized (ZINDO/S) method is relatively better than the general purpose parameterized (PM6) method but the accuracy is trailing behind the DFT methods. The poor performances of PM6 and ZINDO/S methods are attributed to the incorrect description of excited-to-excited state transition and 2PA energies, respectively. The different semiempirical parameterizations can at best be used for quantitative analysis of the 2PA properties. The ZINDO/S method combined with different orders of multi-reference configuration interactions provide an improved description of 2PA properties. However, the results are observed to be highly dependent on the specific choice for the active space, order of excitation and reference configurations.In Chapter 5, we present a linear response TD-DFT study to benchmark the ability of existing functional models to describe the extent of self-trapped neutral and charged excitations in PPV and its derivative MEH-PPV considered in their trans-isomeric forms. The electronic excitations in question include the lowest singlet (S1) and triplet (T1†) excitons, positive (P+) and negative (P-) polarons and the lowest triplet (T1) states. Use of the long-range-corrected DFT functional, such as LC-wPBE, is found to be crucial in order to predict the physically correct spatial localization of all the electronic excitations in agreement with experiment. The inclusion of polarizable dielectric environment play an important role for the charged states. The particle-hole symmetry is preserved for both the polymers in trans geometries. These studies indicate two distinct origins leading to self-localization of electronic excitations. Firstly, distortion of molecular geometry may create a spatially localized potential energy well where the state wavefunction self-traps. Secondly, even in the absence of geometric and vibrational dynamics, the excitation may become spatially confined due to energy stabilization caused by polarization effects from surrounding dielectric medium.In Chapter 6, we aim to separate these two fundamental sources of spatial localization. We observe the electronic localization of P+ and P- is determined by the polarization effects of the surrounding media and the character of the DFT functional. In contrast, the self-trapping of the electronic wavefunctions of S1 and T1(T1†) mostly follows their lattice distortions. Geometry relaxation plays an important role in the localization of the S1 and T1† excitons owing to the non-variational construction of the excited state wavefunction. While, mean-field calculated P+, P- and T1 states are always spatially localized even in ground state S0 geometry. Polaron P+ and P- formation is signified by the presence of the localized states for the hole or the electron deep inside the HOMO-LUMO gap of the oligomer as a result of the orbital stabilization at the LC-wPBE level. The broadening of the HOMO-LUMO band gap for the T1 exciton compared to the charged states is associated with the inverted bond length alternation observed at this level. The molecular orbital energetics are investigated to identify the relationships between state localization and the corresponding orbital structure.In Chapter 7, we investigate the effect of various conformational defects of trans and cis nature on the energetics and localization of the charged P+ and P- excitations in PPV and MEH-PPV. We observe that the extent of self-trapping for P+ and P- polarons is highly sensitive on molecular and structural conformations, and distribution of atomic charges within the polymers. The particle-hole symmetry is broken with the introduction of trans defects and inclusion of the polarizable environment in consistent with experiment. The differences in the behavior of PPV and MEH-PPV is rationalized based on their orbital energetics and atomic charge distributions. We show these isomeric defects influence the behavior and drift mobilities of the charge carriers in substituted PPVs.
Show less - Date Issued
- 2013
- Identifier
- CFE0005110, ucf:50722
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005110
- Title
- Towards High-Flux Isolated Attosecond Pulses with a 200 TW CPA.
- Creator
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Cunningham, Eric, Chang, Zenghu, Saleh, Bahaa, Soileau, MJ, Saha, Haripada, University of Central Florida
- Abstract / Description
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Attosecond pulses have been developed as a means for investigating phenomena that proceed on the order of the atomic unit of time (24 as). Unfortunately, these extreme ultraviolet (XUV) pulses by themselves contain too few photons to initiate nonlinear dynamics or dress states in an attosecond pump--attosecond probe scheme. As a result, most attosecond experiments thus far have featured complementary near infrared (NIR) femtosecond lasers for instigating electron dynamics. In order to access...
Show moreAttosecond pulses have been developed as a means for investigating phenomena that proceed on the order of the atomic unit of time (24 as). Unfortunately, these extreme ultraviolet (XUV) pulses by themselves contain too few photons to initiate nonlinear dynamics or dress states in an attosecond pump--attosecond probe scheme. As a result, most attosecond experiments thus far have featured complementary near infrared (NIR) femtosecond lasers for instigating electron dynamics. In order to access the benefits of all-attosecond measurements and open attosecond physics to new fields of exploration, the photon flux of these pulses must be increased.One way to boost the attosecond pulse energy is to scale up the energy of the NIR pulse responsible for driving high-harmonic generation (HHG). With generalized double optical gating (GDOG), isolated attosecond pulses can be generated with multi-cycle laser systems, wherein the pulse energy can be boosted more easily than in the few-cycle laser systems required by other gating methods. At the Institute for the Frontier of Attosecond Science and Technology (IFAST), this scalability was demonstrated using a 350 mJ, 15 fs (10 TW) Ti:sapphire laser, which was used to generate a 100 nJ XUV continuum. This represented an order-of-magnitude improvement over typical attosecond pulse energies achievable by millijoule-level few-cycle lasers.To obtain the microjoule-level attosecond pulse energy required for performing all-attosecond experiments, the attosecond flux generated by the IFAST 10 TW system was still deficient by an order of magnitude. To this end, the laser system was upgraded to provide joule-level output energies while maintaining pulse compression to 15 fs, with a targeted peak power of 200 TW. This was accomplished by adding an additional Ti:sapphire amplifier to the existing 10 TW system and implementing a new pulse compression system to accommodate the higher pulse energy.Because this system operated at a 10 Hz repetition rate, stabilization of the carrier-envelope phase (CEP) -- important for controlling attosecond pulse production -- could not be achieved using traditional methods. Therefore, a new scheme was developed, demonstrating the first-ever control of CEP in a chirped-pulse amplifier (CPA) at low repetition rates.Finally, a new variation of optical gating was proposed as a way to improve the efficiency of the attosecond pulse generation process. This method was also predicted to allow for the generation of isolated attosecond pulses with longer driving laser pulses, as well as the extension of the high-energy photon cut-off of the XUV continuum.
Show less - Date Issued
- 2015
- Identifier
- CFE0005938, ucf:50804
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005938
- Title
- Generation of high-flux attosecond pulses and towards attosecond-attosecond pump-probe experiments.
- Creator
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Wang, Yang, Chang, Zenghu, Hagan, David, Wu, Shintson, Saha, Haripada, University of Central Florida
- Abstract / Description
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At present, the energy of a single isolated attosecond pulse is limited to nanojoule levels. As a result, an intense femtosecond pulse has always been used in combination with a weak attosecond pulse in time-resolved experiments. To reach the goal of conducting true attosecond pump-attosecond probe experiments, a high flux laser source has been developed that can potentially deliver microjoule level isolated attosecond pulses in the 50 eV range, and a unique experimental end station has been...
Show moreAt present, the energy of a single isolated attosecond pulse is limited to nanojoule levels. As a result, an intense femtosecond pulse has always been used in combination with a weak attosecond pulse in time-resolved experiments. To reach the goal of conducting true attosecond pump-attosecond probe experiments, a high flux laser source has been developed that can potentially deliver microjoule level isolated attosecond pulses in the 50 eV range, and a unique experimental end station has been fabricated and implemented that can provide precision control of the attosecond-attosecond pump-probe pulses. In order to scale up the attosecond flux, a unique Ti:-Sapphire laser system with a three-stage amplifier that delivers pulses with a 2 J energy at a 10 Hz repetition rate was designed and built. The broadband pulse spectrum covering from 700 nm to 900 nm was generated, supporting a pulse duration of 12 fs. The high flux high-order harmonics were generated in a gas tube filled with argon by a loosely focused geometry under a phase-matching condition. The wavefront distortions for the driving laser were corrected by a deformable mirror with a Shack-Hartmann sensor to significantly improve the extreme ultraviolet radiation conversion efficiency due to the excellent beam profile at focus. A high-damage-threshold beam splitter is demonstrated to eliminate energetic driving laser pulses from high-order harmonics. The extreme ultraviolet pulse energy is measured to be 0.3 microjoule at the exit of the argon gas target. The experimental facilities developed will lead to the generation of microjoule level isolated attosecond pulses and the demonstration of true atto pump-atto probe experiments in near future. Finally, in experiment, we show the first demonstration of carrier-envelope phase controlled filamentation in air using millijoule-level few-cycle mid-infrared laser pulses.
Show less - Date Issued
- 2017
- Identifier
- CFE0006926, ucf:51688
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0006926
- Title
- Attosecond Transient Absorption Spectroscopy of Atoms and Molecules.
- Creator
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Cheng, Yan, Chang, Zenghu, Saha, Haripada, Chow, Lee, Vanstryland, Eric, University of Central Florida
- Abstract / Description
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One of the most fundamental goals of attosecond science is to observe and to control the dynamic evolutions of electrons in matter. The attosecond transient absorption spectroscopy is a powerful tool to utilize attosecond pulse to measure electron dynamics in quantum systems directly. In this work, isolated single attosecond pulses are used to probe electron dynamics in atoms and to study dynamics in hydrogen molecules using the attosecond transient absorption spectroscopy technique. The...
Show moreOne of the most fundamental goals of attosecond science is to observe and to control the dynamic evolutions of electrons in matter. The attosecond transient absorption spectroscopy is a powerful tool to utilize attosecond pulse to measure electron dynamics in quantum systems directly. In this work, isolated single attosecond pulses are used to probe electron dynamics in atoms and to study dynamics in hydrogen molecules using the attosecond transient absorption spectroscopy technique. The target atom/molecule is first pumped to excited states and then probed by a subsequent attosecond extreme ultraviolet (XUV) pulse or by a near infrared (NIR) laser pulse. By measuring the absorbed attosecond XUV pulse spectrum, the ultrafast electron correlation dynamics can be studied in real time. The quantum processes that can be studied using the attosecond transient absorption spectroscopy include the AC stark shift, multi-photon absorption, intermediate states of atoms, autoionizing states, and transitions of vibrational states in molecules. In all experiments, the absorption changes as a function of the time delay between the attosecond XUV probe pulse and the dressing NIR laser pulse, on a time scale of sub-cycle laser period, which reveals attosecond electron dynamics. These experiments demonstrate that the attosecond transient absorption spectroscopy can be performed to study and control electronic and nuclear dynamics in quantum systems with high temporal and spectral resolution, and it opens door for the study of electron dynamics in large molecules and other more complex systems.
Show less - Date Issued
- 2015
- Identifier
- CFE0006284, ucf:51595
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0006284
- Title
- Characterization and Application of Isolated Attosecond Pulses.
- Creator
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Chini, Michael, Chang, Zenghu, Saha, Haripada, Chow, Lee, Schulzgen, Axel, University of Central Florida
- Abstract / Description
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Tracking and controlling the dynamic evolution of matter under the influence of external fields is among the most fundamental goals of physics. In the microcosm, the motion of electrons follows the laws of quantum mechanics and evolves on the timescale set by the atomic unit of time, 24 attoseconds. While only a few time-dependent quantum mechanical systems can be solved theoretically, recent advances in the generation, characterization, and application of isolated attosecond pulses and few...
Show moreTracking and controlling the dynamic evolution of matter under the influence of external fields is among the most fundamental goals of physics. In the microcosm, the motion of electrons follows the laws of quantum mechanics and evolves on the timescale set by the atomic unit of time, 24 attoseconds. While only a few time-dependent quantum mechanical systems can be solved theoretically, recent advances in the generation, characterization, and application of isolated attosecond pulses and few-cycle femtosecond lasers have given experimentalists the necessary tools for dynamic measurements on these systems. However, pioneering studies in attosecond science have so far been limited to the measurement of free electron dynamics, which can in most cases be described approximately using classical mechanics. Novel tools and techniques for studying bound states of matter are therefore desired to test the available theoretical models and to enrich our understanding of the quantum world on as-yet unprecedented timescales.In this work, attosecond transient absorption spectroscopy with ultrabroadband attosecond pulses is presented as a technique for direct measurement of electron dynamics in quantum systems, demonstrating for the first time that the attosecond transient absorption technique allows for state-resolved and simultaneous measurement of bound and continuum state dynamics. The helium atom is the primary target of the presented studies, owing to its accessibility to theoretical modeling with both ab initio simulations and to model systems with reduced dimensionality. In these studies, ultrafast dynamics (-) on timescales shorter than the laser cycle (-) are observed in prototypical quantum mechanical processes such as the AC Stark and ponderomotive energy level shifts, Rabi oscillations and electromagnetically-induced absorption and transparency, and two-color multi-photon absorption to (")dark(") states of the atom. These features are observed in both bound states and quasi-bound autoionizing states of the atom. Furthermore, dynamic interference oscillations, corresponding to quantum path interferences involving bound and free electronic states of the atom, are observed for the first time in an optical measurement. These first experiments demonstrate the applicability of attosecond transient absorption spectroscopy with ultrabroadband attosecond pulses to the study and control of electron dynamics in quantum mechanical systems with high fidelity and state selectivity. The technique is therefore ideally suited for the study of charge transfer and collective electron motion in more complex systems.The transient absorption studies on atomic bound states require ultrabroadband attosecond pulses ? attosecond pulses with large spectral bandwidth compared to their central frequency. This is due to the fact that the bound states in which we are interested lie only 15-25 eV above the ground state, so the central frequency of the pulse should lie in this range. On the other hand, the bandwidth needed to generate an isolated 100 as pulse exceeds 18 eV (-) comparable to or even larger than the central frequency. However, current methods for characterizing attosecond pulses require that the attosecond pulse spectrum bandwidth is small compared to its central frequency, known as the central momentum approximation. We therefore explore the limits of attosecond pulse characterization using the current technology and propose a novel method for characterizing ultrabroadband attosecond pules, which we term PROOF (phase retrieval by omega oscillation filtering). We demonstrate the PROOF technique with both simulated and experimental data, culminating in the characterization of a world-record-breaking 67 as pulse.
Show less - Date Issued
- 2012
- Identifier
- CFE0004781, ucf:49802
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0004781
- Title
- The effect of electron-hole pairs in semiconductor and topological insulator nanostructures on plasmon resonances and photon polarizations.
- Creator
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Paudel, Hari, Leuenberger, Michael, Rahman, Talat, Saha, Haripada, Gesquiere, Andre, University of Central Florida
- Abstract / Description
-
The generation of electron-hole pairs in materials has great importance. In directbandgap semiconductor materials, the mechanism of radiative recombination of electron-holepairs leads to the emission of photons, which is the basis of Light Emitting Diodes(LEDs). The excitation of electron-hole pairs by absorption of photons is the active processin photodiodes, solar cells, and other semiconductor photodetector devices. In optoelectronicdevices such as optical switches which are based on...
Show moreThe generation of electron-hole pairs in materials has great importance. In directbandgap semiconductor materials, the mechanism of radiative recombination of electron-holepairs leads to the emission of photons, which is the basis of Light Emitting Diodes(LEDs). The excitation of electron-hole pairs by absorption of photons is the active processin photodiodes, solar cells, and other semiconductor photodetector devices. In optoelectronicdevices such as optical switches which are based on transmission and reflection of the photons,electron-hole pairs excitation is a key for the device performance. Diodes and transistorsare also great discoveries in electronics which rely on the generation and recombination ofelectron-hole pairs at p-n junctions. In three-dimensional topological insulators (3D TIs)materials nanostructures excitation of electron-hole pairs can be utilized for the quantummemory, quantum information and quantum teleportation. In two-dimensional (2D) layeredmaterials like graphene, MoS_2, MoSe_2, WS_2 and WSe_2 generation and recombination ofelectron hole pairs is main process at p-n junctions, infrared detectors and sensors.This PhD thesis is concerned with the physics of different types of electron-hole pairsin various materials, such as wide-bandgap semiconductors, 3D topological insulators, andplasmonic excitations in metallic nanostructures. The materials of interest are wide bandgap semiconductors such as TiO_2 , 3D TIs such as Pb_1?xSn_xTe and the 2D layered materials such as MoS_2 and MoO_3. We study the electronic and optical properties in bulk and nanostructures and find applications in the area of semiclassical and quantum information processing. One of the interesting applications we focus in this thesis is shift in surface plasmon resonance due to reduction in index of refraction of surrounding dielectric environment which inturns shifts the wavelength of surface plasmon resonance up to 125 nm for carrier density of10^22/cm^3. Employing this effect, we present a model of a light controlled plasmon switching using a hybrid metal-dielectric heterostructures.In 3D TIs nanostructures, the time reversible spin partners in the valence and conductionband can be coupled by a left and a right handed circular polarization of the light.Such coupling of light with electron-hole pair polarization provides an unique opportunityto utilize 3D TIs in quantum information processing and spintronics devices. We present a model of a 3D TI quantum dot made of spherical core-bulk heterostructure. When a 3D TI QD is embedded inside a cavity, the single-photon Faraday rotation provides the possibility to implement optically mediated quantum teleportation and quantum information processing with 3D TI QDs, where the qubit is defined by either an electron-hole pair, a single electron spin, or a single hole spin in a 3D TI QD.Due to excellent transport properties in single and multiple layers of 2D layeredmaterials, several efforts have demonstrated the possibility to engineer electronic and optoelectronic devices based on MoS_2. In this thesis, we focus on theoretical and experimental study of electrical property and photoluminescence tuning, both in a single-layer of MoS_2.We present theoretical analysis of experimental results from the point of view of stability of MoO_3 defects in MoS_2 single layer and bandstructures calculation. In experiment, the electrical property of a single layer of MoS_2 can be tuned from semiconducting to insulating regime via controlled exposure to oxygen plasma. The quenching of photoluminescence of asingle sheet of MoS_2 has also been observed upon exposure to oxygen plasmas. We calculatethe direct to indirect band gap transitions by going from MoS_2 single sheet to MoO_3 singlesheet during the plasma exposure, which is due to the formation of MoO_3 rich defect domainsinside a MoS_2 sheet.
Show less - Date Issued
- 2014
- Identifier
- CFE0005397, ucf:50454
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005397
- Title
- Generation and characterization of sub-70 isolated attosecond pulses.
- Creator
-
Zhang, Qi, Chang, Zenghu, Delfyett, Peter, Gaume, Romain, Saha, Haripada, University of Central Florida
- Abstract / Description
-
Dynamics occurring on microscopic scales, such as electronic motion inside atoms and molecules, are governed by quantum mechanics. However, the Schr(&)#246;dinger equation is usually too complicated to solve analytically for systems other than the hydrogen atom. Even for some simple atoms such as helium, it still takes months to do a full numerical analysis. Therefore, practical problems are often solved only after simplification. The results are then compared with the experimental outcome in...
Show moreDynamics occurring on microscopic scales, such as electronic motion inside atoms and molecules, are governed by quantum mechanics. However, the Schr(&)#246;dinger equation is usually too complicated to solve analytically for systems other than the hydrogen atom. Even for some simple atoms such as helium, it still takes months to do a full numerical analysis. Therefore, practical problems are often solved only after simplification. The results are then compared with the experimental outcome in both the spectral and temporal domain. For accurate experimental comparison, temporal resolution on the attosecond scale is required. This had not been achieved until the first demonstration of the single attosecond pulse in 2001. After this breakthrough, (")attophysics(") immediately became a hot field in the physics and optics community. While the attosecond pulse has served as an irreplaceable tool in many fundamental research studies of ultrafast dynamics, the pulse generation process itself is an interesting topic in the ultrafast field. When an intense femtosecond laser is tightly focused on a gaseous target, electrons inside the neutral atoms are ripped away through tunneling ionization. Under certain circumstances, the electrons are able to reunite with the parent ions and release photon bursts lasting only tens to hundreds of attoseconds. This process repeats itself every half cycle of the driving pulse, generating a train of single attosecond pulses which lasts longer than one femtosecond. To achieve true temporal resolution on the attosecond time scale, single isolated attosecond pulses are required, meaning only one attosecond pulse can be produced per driving pulse.Up to now, there are only a few methods which have been demonstrated experimentally to generate isolated attosecond pulses. Pioneering work generated single attosecond pulse using a carrier-envelope phase-stabilized 3.3 fs laser pulse, which is out of reach for most research groups. An alternative method termed as polarization gating generated single attosecond pulses with 5 fs driving pulses, which is still difficult to achieve experimentally. Most recently, a new technique termed as Double Optical Gating (DOG) was developed in our group to allow the generation of single attosecond pulse with longer driving pulse durations. For example, isolated 150 as pulses were demonstrated with a 25 fs driving laser directly from a commercially-available Ti:Sapphire amplifier. Isolated attosecond pulses as short as 107 as have been demonstrated with the DOG scheme before this work. Here, we employ this method to shorten the pulse duration even further, demonstrating world-record isolated 67 as pulses. Optical pulses with attosecond duration are the shortest controllable process up to now and are much faster than the electron response times in any electronic devices. In consequence, it is also a challenge to characterize attosecond pulses experimentally, especially when they feature a broadband spectrum. Similar challenges have previously been met in characterizing femtosecond laser pulses, with many schemes already proposed and well-demonstrated experimentally. Similar schemes can be applied in characterizing attosecond pulses with narrow bandwidth. The limitation of these techniques is presented here, and a method recently developed to overcome those limitations is discussed. At last, several experimental advances toward the characterization of the isolated 25 as pulses, which is one atomic unit time, are discussed briefly.
Show less - Date Issued
- 2014
- Identifier
- CFE0005450, ucf:50375
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0005450
- Title
- Electronic, Optical, and Magnetic Properties of Graphene and Single-Layer Transition Metal Dichalcogenides in the Presence of Defects.
- Creator
-
Khan, Mahtab, Leuenberger, Michael, Mucciolo, Eduardo, Saha, Haripada, Tetard, Laurene, Schoenfeld, Winston, University of Central Florida
- Abstract / Description
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Two-dimensional (2D) materials, such as graphene and single-layer (SL) transition metal dichalcogenides (TMDCs), have attracted a lot of attention due to their fascinating electronic and optical properties. Graphene was the first 2D material that has successfully been exfoliated from bulk graphite in 2004. In graphene, charge carriers interacting with the honeycomb lattice of carbonatoms of graphene to appear as massless Dirac fermions. Massless quasiparticles with linear dispersion are also...
Show moreTwo-dimensional (2D) materials, such as graphene and single-layer (SL) transition metal dichalcogenides (TMDCs), have attracted a lot of attention due to their fascinating electronic and optical properties. Graphene was the first 2D material that has successfully been exfoliated from bulk graphite in 2004. In graphene, charge carriers interacting with the honeycomb lattice of carbonatoms of graphene to appear as massless Dirac fermions. Massless quasiparticles with linear dispersion are also observed in surface states of 3D topological insulators and quantum Hall edgestates. My first project deals with the two-dimensional Hong-Ou-Mandel (HOM) type interferenceexperiment for massless Dirac fermions in graphene and 3D topological insulators. Since masslessDirac fermions exhibit linear dispersion, similar to photons in vacuum, they can be used to observethe HOM interference intensity pattern as a function of the delay time between two massless Dirac fermions. My further projects and the major part of this dissertation deal with single-layer (SL) transition metal dichalcogenides (TMDCs), such as MoS$_2$, WS$_2$, MoSe$_2$ and WSe$_2$, which have recently emerged as a new family of two-dimensional (2D) materials with great interest, not only from the fundamental point of view, but also because of their potential application to ultrathin electronic and optoelectronic devices. In contrast to graphene, SL TMDCs are direct band semiconductors and exhibit large intrinsic spin-orbit coupling (SOC), originating from the d orbitals of transition metal atoms. Wafer-scale production of SL TMDCs is required for industrial applications. It has been shown that artificially grown samples of SL TMDCs through various experimental techniques, such as physical vapor deposition (PVD), chemical vapor deposition (CVD), and molecular beam epitaxy (MBE), are not perfect, instead certain type of imperfections such as point defects are always found to be present in the grown samples. Defects compromise the crystallinity of the sample, which results in reduced carrier mobility and deteriorated optical efficiency. However, defects are not always unwanted; in fact, defects can play an important role in tailoring electronic, optical, and magnetic properties of materials. Using Density functional theory we investigate the impact of point defects on the electronic, optical, and magnetic properties of SL TMDCs. First, we show that certain vacancy defects lead to localized defect states, which in turn give rise to sharp transitions in in-plane and out-of-plane optical susceptibilities of SL TMDCs. Secondly, we show that a naturally occurring antisite defect Mo$_S$ in PVD grown MoS$_2$ is magnetic in nature with a magneticmoment of 2$\mu_B$, and remarkably exhibit an exceptionally large atomic scale magnetic anisotropy energy (MAE) of ~ 500 eV. Both magnetic moment and MAE can be tuned by shifting the position of the Fermi level which can be achieved either by gate voltage or by chemical doping. Thirdly, we argue that the antisite defect Se$_W$ in WSe$_2$ leads to long lived localized excited states, which can explain the observed single quantum emitters in CVD grown WSe$_2$ samples, with potential application to quantum cryptography.
Show less - Date Issued
- 2018
- Identifier
- CFE0007030, ucf:52047
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0007030
- Title
- Passive, Wireless SAW OFC Strain Sensor and Software Defined Radio Interrogator.
- Creator
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Humphries, James, Malocha, Donald, Richie, Samuel, Weeks, Arthur, Sundaram, Kalpathy, Saha, Haripada, University of Central Florida
- Abstract / Description
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Surface acoustic wave (SAW) devices have exhibited unique capabilities to meet the demands for many applications due to the inherent properties of SAW devices and piezoelectric materials. In particular, SAW devices have been adapted as sensors that can be configured to operate both passively and wirelessly. SAW sensors can be operated in harsh environmental extremes where typical sensor technologies are not able to operate. Because the sensors are passive, a radio transceiver is required to...
Show moreSurface acoustic wave (SAW) devices have exhibited unique capabilities to meet the demands for many applications due to the inherent properties of SAW devices and piezoelectric materials. In particular, SAW devices have been adapted as sensors that can be configured to operate both passively and wirelessly. SAW sensors can be operated in harsh environmental extremes where typical sensor technologies are not able to operate. Because the sensors are passive, a radio transceiver is required to interrogate the sensor and receive the reflected response that has been modulated by the SAW device. This dissertation presents the design of a passive, wireless SAW OFC strain sensor and software defined radio (SDR) interrogator.A SAW strain sensor has been designed and tested using orthogonal frequency coding (OFC) on YZ-LiNbO3. OFC for SAW devices has been previously developed at UCF and provides both frequency and time diversity in the RFID code as well as providing processing gain to improve the sensor SNR. Strain effects in SAW devices are discussed and two sensor embodiments are developed. The first embodiment is a cantilever structure and provides insight on how strain effects the SAW device. The second embodiment bonds the SAW die directly to a test structure to measure the strain on the structure. A commercial wired foil strain gage provides a performance comparison and shows that the wireless SAW sensor performs comparably. A commercial-off-the-shelf SDR platform has been employed as the SAW sensor interrogator. The Universal Software Radio Peripheral (USRP) is available in many embodiments and is capable of operation of to 6GHz and up to 160MHz of bandwidth. In particular, the USRP B200 is utilized as the RF transceiver platform. Custom FPGA modifications are discussed to fully utilize the USRP B200 bandwidth (56MHz) and synchronize the transmit and receive chains. External hardware has also been introduced to the B200 to improve RF performance, all of which are incorporated into a custom enclosure. Post-processing of the SAW sensor response is accomplished in Python using a matched filter correlator routine to extract sensor information. The system is demonstrated by interrogating wireless OFC SAW temperature and strain sensors at 915MHz.
Show less - Date Issued
- 2016
- Identifier
- CFE0006329, ucf:51560
- Format
- Document (PDF)
- PURL
- http://purl.flvc.org/ucf/fd/CFE0006329
