A unique feature of the 5d-iridates is that the spin-orbit interaction (SOI) and Coulomb interactions U are of comparable strength and therefore compete vigorously. The relative strength of these interactions stabilizes new exotic ground states that provide a fertile ground for studying new physics. SOI is proportional to Z^4 (Z is the atomic number), and it is now recognized that strong SOI can drive novel narrow-gap insulating states in heavy transition metal oxides such as iridates. Indeed, strong SOI necessarily introduces strong lattice degrees of freedom that become critical to new physics in the iridates. This dissertation thoroughly examines a wide array of newly observed novel phenomena induced by adjusting the relative strengths of U and SOI interactions via slight chemical doping and application of hydrostatic pressure in the layered iridates, particularly, BaIrO3 and Sr2IrO4.

We investigate two medium-facilitated interactions between properties of light upon propagation through optical fiber. The first is interaction between the spin and intrinsic orbital angular momentum in a linear optical medium. This interaction gives rise to fine structure in the longitudinal momenta of fiber modes and manifests in rotational beating effects. We probe those beating effects experimentally in cutback experiments, where small segments are cut from the output of a fiber to probe the evolution of both output polarization and spatial orientation, and find agreement between theoretical predictions and measured behavior. The second is nonlinear optical interaction due to cross- and self-phase modulation between the complex-valued temporal amplitude profile of pump pulses and the amplitude profiles of generated signal and idler pulses in optical fiber photon-pair sources utilizing the four-wave mixing process named modulation instability. We develop a model including the effects of these nonlinear phase modulations (NPM) describing the time-domain wave function of the output biphoton in the low-gain regime. Assuming Gaussian temporal amplitude profiles for the pump pulse, we numerically simulate the structure of the biphoton wave function, in symmetric and asymmetric group velocity matching configurations. Comparing the overlap of the joint temporal amplitudes with and without NPM indicates how good of an approximation neglecting NPM is, and we investigate the effects of NPM on the Schmidt modes. We find that effects of NPM are small on temporally separable sources utilizing symmetric group velocity matching, but appreciably change the state of temporally entangled sources with the same group velocity matching scheme. For sources designed to produce entangled biphotons, our simulations suggest that NPM increases the Schmidt number, which may increase entanglement resource availability with utilization of a phase-sensitive detection scheme. We find that NPM effects on temporally separable sources designed with asymmetric group velocity matching produce non-negligible changes in the state structure. The purity is unaffected at perfect asymmetric group velocity matching, but if the pump is detuned from the correct wavelength, the purity degrades. The largest changes to the state due to NPM occur in long fibers with long pulse durations and low repetition rates.

A partir da teoria de resposta linear (formalismo de Kubo) calculamos a condutividade de spin $\\sigma_^$ para um gás bidimensional de elétrons formado num poço quântico com duas subbandas devido a atuação de um novo tipo de interação spin-órbita [Bernardes et al. \\textit{Phys. Rev. Lett.} \\textbf, 076603 (2007) \\& Calsaverini \\textit{et al}. \\textit{Phys. Rev. B} \\textbf, 155313 (2008)]. Este novo termo é não-nulo mesmo em estruturas simétricas e surge devido ao acoplamento entre os estados confinados no poço de paridades diferentes. Encontramos um valor para $\\sigma_^$ não-nulo e não-universal (dependente da intensidade do acoplamento $\\eta$) quando somente uma das subbandas está ocupada, ao contrário de Rashba. Para encontrarmos valores realistas para $\\sigma_^$, determinamos $\\eta$ via cálculo autoconsistente. Esse cálculo é executado para diferentes valores de densidade eletrônica em poços simples e duplos. Obtivemos que $\\sigma_^$ possui um comportamento não-monótono e sofre inversão de sinal como função da energia de Fermi (densidade de elétrons) conforme ela varia entre as duas subbandas. Contudo nossos resultados indicam que a condutividade Hall de spin é muito pequena $\\left(``\\ll \\frac{8\\pi}\"ight)$ nesses sistemas (poços simples e duplos) e possivelmente não mensurável. / Using the Kubo linear response theory, we investigate spin Hall conductivity $\\sigma_^$ in a two-dimensional electron gas in quantum wells with two subbands, when intersubband-induced spin-orbit coupling is operative [Bernardes et al. \\textit{Phys. Rev. Lett.} \\textbf, 076603 (2007) \\& Calsaverini \\textit{et al}. \\textit{Phys. Rev. B} \\textbf, 155313 (2008)]. This new spin-orbit term is non-zero even in symmetric structures and it arises from the distinct parity of the confined states. We find non-zero and non-universal $\\sigma_^$ (dependent on spin-orbit coupling strength $\\eta$) when only one of the subbands is occupied. This is in contrast to the Rashba spin-orbit interaction for which $\\sigma_^$ is identically zero. To obtain realistic values for $\\sigma_^$, we develop a self-consistent scheme to calculate $\\eta$. We performed this calcultion for different values of the eletronic density in single and double wells. We find that $\\sigma_^$ shows a non-monotonic behavior and a sign change as the Fermi energy (carrier density) varies between the two subband edges. However, our results indicate that $\\sigma_^$ is extremely small $\\left(``\\ll \\frac{8\\pi}\"ight)$ and possibly not measurable.

The 5d transition metal oxides have drawn substantial interest for predictions of being suitable candidates for hosting exotic electronic and magnetic states, including unconventional superconductors, magnetic skyrmions, topological insulators, and Weyl semimetals. In addition to the electron-electron correlation notable in high-temperature 3d transition metal superconductors, the 5d oxides contain a large spin-orbit interaction term in their ground state, which is largely responsible for the intricate phase diagram of these materials. Iridates, or compounds containing 5d iridium bonded with oxygen, are of particular interest for their spin-orbit split Jeff = 1/2 state, which is partially filled without the presence of any additional electron correlation. However, the comparable energetics between a small, finite electron correlation energy and the spin-orbit interaction make the band structure of iridates amenable to small perturbations of the crystalline lattice and ideal for exploring the interplay between these two interactions. While altering the spin-orbit interaction strength of iridium is tenably not feasible, the electron correlation energy can be tuned using a variety of experimental techniques. In this dissertation, the electronic and magnetic properties of iridates at various electron correlation energies are studied by altering the epitaxial lattice strain, dimensionality, and the radius size of the A-site cation. These parameters tune the effective electronic bandwidth of the system, which is inversely proportional to the effective electron correlation energy. The lattice strain and the cationic radius size achieve this by altering the Ir-O-Ir bond angle between nearest neighbor Ir ions. In the case of dimensionality tuning, the effective bandwidth is controlled via the coordination number of each Ir ion. In the first study, a metal-to-insulator transition is observed in thin films of the semi-metallic SrIrO3 as in-plane compressive lattice strain is increased. This observation is consistent with the expectation of compressive lattice strain increasing the effective correlation energy; however, optical spectroscopy spectra reveal the increase is not sufficient for opening an insulating Mott gap. In the second part, the effective correlation energy is adjusted using a dimensional confinement of the layered iridate Sr2IrO4. Here, the coordination number of each Ir ion is reduced using an a-axis oriented superlattice of one-dimensional IrO2 quantum stripes, where several emergent features are revealed in its insulating Jeff = 1/2 state. In the final study, the effective correlation is tuned in a series of mixed-phase pyrochlore iridate thin films, where the Ir atoms take a corner-shared tetrahedral configuration. Here, a transition between conducting to insulating magnetic domain walls is revealed as the correlation energy is increased via A-site chemical doping. Each of these studies sheds light on the pronounced role the effective correlation energy plays in determining the local subset of phases predicted for iridates and related systems featuring strong spin-orbit interactions.

The main theme covered in this thesis is experimentalstudies of quantum dynamics and coherent control in homonuclearalkali diatomic molecules by ultrafast laser spectroscopy iththe implementation of pump-probe techniques. A series of experiments have been performed on the Rb2molecules in a molecular beam as well as in a thermal oven. Thereal-time molecular quantum dynamics of the predissociatingelectronically excited D(3)1Πu state of Rb2, which couples to/intersects several otherneighbouring states, is investigated using wavepackets. Thepredissociation of the D state, explored by this wavepacketmethod, arises from two independent states, the (4)3Σu+and (1)3∆u, for which the second corresponds to a much fasterdecay channel above a sharp energy threshold around 430 nm. Thelifetime of the D state above the energy threshold is obtained,τ ≈ 5 ps, by measuring the decay time of thewavepacket in a thermal oven. Further experimentalinvestigation performed in a molecular beam together withquantum calculations of wavepacket dynamics on the D state haveexplored new probe channels of wavepacket evolution: theD′(3)1Σu+ channel, which exhibits vibrational motionin a shelf state and the (4)3Σu+ channel, where direct build-up of thewavefunction is observed due to its spin-orbit oupling to the Dstate. The real-time quantum dynamics of wavepackets confined totwo bound states, A1Σu+(0u+) and b3Πu(0u+), have been studied by experiment andcalculations. It is shown that these two states are fullycoupled by spin-orbit interaction, characterised by itsintermediate strength. The intermediate character of thedynamics is established by complicated wavepacket oscillationatterns and a value of 75 cm-1is estimated for the coupling strength at thestate crossing. The experiments on the Li2molecule are performed by coherent control ofrovibrational molecular wavepackets. First, the Deutsch-Jozsaalgorithm is experimentally demonstrated for three-qubitfunctions using a pure coherent superposition of Li2rovibrational eigenstates. The function’scharacter, either constant or balanced, is evaluated by firstimprinting the function, using a phase-tailored femtosecond(fs) pulse, on a coherent superposition of the molecularstates, and then projecting the superposition onto an ionicfinal state using a second fs pulse at a specific delay time.Furthermore, an amplitude-tailored fs pulse is used to exciteselected rovibrational eigenstates and collision induceddephasing of the wavepacket signal, due to Li2-Ar collisions, is studied experimentally. Theintensities of quantum beats decaying with the delay time aremeasured under various pressures and the collisional crosssections are calculated for each well-defined rovibrationalquantum beat, which set the upper limitsfor ure dephasingcross sections. <b>Keywords:</b>Ultrafast laser spectroscopy, pump-probetechnique, predissociation, wavepacket, pin-orbit interaction,coherent control, (pure) dephasing

<p>The main theme covered in this thesis is experimentalstudies of quantum dynamics and coherent control in homonuclearalkali diatomic molecules by ultrafast laser spectroscopy iththe implementation of pump-probe techniques.</p><p>A series of experiments have been performed on the Rb2molecules in a molecular beam as well as in a thermal oven. Thereal-time molecular quantum dynamics of the predissociatingelectronically excited D(3)¹Πu state of Rb₂, which couples to/intersects several otherneighbouring states, is investigated using wavepackets. Thepredissociation of the D state, explored by this wavepacketmethod, arises from two independent states, the (4)³Σ_u⁺and (1)³∆_u, for which the second corresponds to a much fasterdecay channel above a sharp energy threshold around 430 nm. Thelifetime of the D state above the energy threshold is obtained,τ ≈ 5 ps, by measuring the decay time of thewavepacket in a thermal oven. Further experimentalinvestigation performed in a molecular beam together withquantum calculations of wavepacket dynamics on the D state haveexplored new probe channels of wavepacket evolution: theD′(3)1Σu+ channel, which exhibits vibrational motionin a shelf state and the (4)³Σu+ channel, where direct build-up of thewavefunction is observed due to its spin-orbit oupling to the Dstate.</p><p>The real-time quantum dynamics of wavepackets confined totwo bound states, A¹Σ_u⁺(0_u⁺) and b³Π_u(0_u⁺), have been studied by experiment andcalculations. It is shown that these two states are fullycoupled by spin-orbit interaction, characterised by itsintermediate strength. The intermediate character of thedynamics is established by complicated wavepacket oscillationatterns and a value of 75 cm^-1is estimated for the coupling strength at thestate crossing.</p><p>The experiments on the Li₂molecule are performed by coherent control ofrovibrational molecular wavepackets. First, the Deutsch-Jozsaalgorithm is experimentally demonstrated for three-qubitfunctions using a pure coherent superposition of Li₂rovibrational eigenstates. The function’scharacter, either constant or balanced, is evaluated by firstimprinting the function, using a phase-tailored femtosecond(fs) pulse, on a coherent superposition of the molecularstates, and then projecting the superposition onto an ionicfinal state using a second fs pulse at a specific delay time.Furthermore, an amplitude-tailored fs pulse is used to exciteselected rovibrational eigenstates and collision induceddephasing of the wavepacket signal, due to Li₂-Ar collisions, is studied experimentally. Theintensities of quantum beats decaying with the delay time aremeasured under various pressures and the collisional crosssections are calculated for each well-defined rovibrationalquantum beat, which set the upper limitsfor ure dephasingcross sections.</p><p><b>Keywords:</b>Ultrafast laser spectroscopy, pump-probetechnique, predissociation, wavepacket, pin-orbit interaction,coherent control, (pure) dephasing</p>

A partir da teoria de resposta linear (formalismo de Kubo) calculamos a condutividade de spin $\\sigma_^$ para um gás bidimensional de elétrons formado num poço quântico com duas subbandas devido a atuação de um novo tipo de interação spin-órbita [Bernardes et al. \\textit{Phys. Rev. Lett.} \\textbf, 076603 (2007) \\& Calsaverini \\textit{et al}. \\textit{Phys. Rev. B} \\textbf, 155313 (2008)]. Este novo termo é não-nulo mesmo em estruturas simétricas e surge devido ao acoplamento entre os estados confinados no poço de paridades diferentes. Encontramos um valor para $\\sigma_^$ não-nulo e não-universal (dependente da intensidade do acoplamento $\\eta$) quando somente uma das subbandas está ocupada, ao contrário de Rashba. Para encontrarmos valores realistas para $\\sigma_^$, determinamos $\\eta$ via cálculo autoconsistente. Esse cálculo é executado para diferentes valores de densidade eletrônica em poços simples e duplos. Obtivemos que $\\sigma_^$ possui um comportamento não-monótono e sofre inversão de sinal como função da energia de Fermi (densidade de elétrons) conforme ela varia entre as duas subbandas. Contudo nossos resultados indicam que a condutividade Hall de spin é muito pequena $\\left(``\\ll \\frac{8\\pi}\"ight)$ nesses sistemas (poços simples e duplos) e possivelmente não mensurável. / Using the Kubo linear response theory, we investigate spin Hall conductivity $\\sigma_^$ in a two-dimensional electron gas in quantum wells with two subbands, when intersubband-induced spin-orbit coupling is operative [Bernardes et al. \\textit{Phys. Rev. Lett.} \\textbf, 076603 (2007) \\& Calsaverini \\textit{et al}. \\textit{Phys. Rev. B} \\textbf, 155313 (2008)]. This new spin-orbit term is non-zero even in symmetric structures and it arises from the distinct parity of the confined states. We find non-zero and non-universal $\\sigma_^$ (dependent on spin-orbit coupling strength $\\eta$) when only one of the subbands is occupied. This is in contrast to the Rashba spin-orbit interaction for which $\\sigma_^$ is identically zero. To obtain realistic values for $\\sigma_^$, we develop a self-consistent scheme to calculate $\\eta$. We performed this calcultion for different values of the eletronic density in single and double wells. We find that $\\sigma_^$ shows a non-monotonic behavior and a sign change as the Fermi energy (carrier density) varies between the two subband edges. However, our results indicate that $\\sigma_^$ is extremely small $\\left(``\\ll \\frac{8\\pi}\"ight)$ and possibly not measurable.

Nesta dissertação são estudados Condensados de Bose-Einstein de átomos com pseudo-spin 1/2 cuja dinâmica orbital está acoplada a estes dois níveis de energia internos. A geração de tal sistema é possível induzindo transições entre os subníveis m_f = -1 e m_f = 0 do estado hiperfino atômico f = 1 usando um arranjo de lasers, os quais também introduzem junto uma dependência espacial dada por suas fases, as quais estão relacionadas a posição do átomo no campo, levando assim à interação acoplando spin e órbita. É considerado então um sistema unidimensional efetivo na mesma direção do acoplamento dos lasers, onde são estudado diferentes observáveis do estado fundamental, para uma varredura dos parâmetros presentes na equação, dando origem a três fases diferenciadas pela distribuição do momento. Foram determinadas estas fases do estado fundamental para interação atrativa, sendo elas modulada(striped), onda plana e de momento nulo, mostrando a localização onde cada uma ocorre no domínio de parâmetros da equação, através de diagramas de fase. São também mostrados, separadamente, observáveis relevantes como momento e desbalanço entre os estados internos nestas transições, os quais apresentaram variações bruscas, ditando valores críticos nos parâmetros, onde ocorrem. Posteriormente é estudado a dinâmica através de soluções do tipo sóliton, as quais não se propagam linearmente e são ditadas por oscilações do centro de massa e das populações, explorando diferentes situações iniciais. / In the present dissertation it has been studied Bose-Einstein Condensation of atoms with 1/2 pseudo-spin whose the orbital dynamics is coupled to these two internal energy levels. The generation of such a system is done by inducing transitions between the sub-levels m_f = -1 and m_f = 0 from the hyperfine atomic state f = 1 using an arrangement of lasers, that also introduce a spacial dependence due to their phases, that changes accordingly the atom\'s position in the light field, conducting in this way to a interaction that couples orbital motion with spin. It is then considered an effective one dimensional system in the same direction of the laser coupling, where it has been studied different ground state observables, making a sweeping in the equation parameters, showing three typical phases based on momentum distribution. So far, it was determined these phases for attractive interactions, named striped, plane wave and zero momentum, determining as well the location where each one occurs in the equation\'s parameters through a phase diagram. It is also reported, separately, a few relevant observables as individual momentum of each population and the unbalance between the internal spin states, in the transition among these phases, whose the values present abrupt variations, dictating critical values for the parameters, where it occurs. Lately is presented a dynamical study with soliton like solutions, that do not linearly propagate and instead, shows a center of mass and unbalance oscillation, probing different initial conditions.

Nesta dissertação são estudados Condensados de Bose-Einstein de átomos com pseudo-spin 1/2 cuja dinâmica orbital está acoplada a estes dois níveis de energia internos. A geração de tal sistema é possível induzindo transições entre os subníveis m_f = -1 e m_f = 0 do estado hiperfino atômico f = 1 usando um arranjo de lasers, os quais também introduzem junto uma dependência espacial dada por suas fases, as quais estão relacionadas a posição do átomo no campo, levando assim à interação acoplando spin e órbita. É considerado então um sistema unidimensional efetivo na mesma direção do acoplamento dos lasers, onde são estudado diferentes observáveis do estado fundamental, para uma varredura dos parâmetros presentes na equação, dando origem a três fases diferenciadas pela distribuição do momento. Foram determinadas estas fases do estado fundamental para interação atrativa, sendo elas modulada(striped), onda plana e de momento nulo, mostrando a localização onde cada uma ocorre no domínio de parâmetros da equação, através de diagramas de fase. São também mostrados, separadamente, observáveis relevantes como momento e desbalanço entre os estados internos nestas transições, os quais apresentaram variações bruscas, ditando valores críticos nos parâmetros, onde ocorrem. Posteriormente é estudado a dinâmica através de soluções do tipo sóliton, as quais não se propagam linearmente e são ditadas por oscilações do centro de massa e das populações, explorando diferentes situações iniciais. / In the present dissertation it has been studied Bose-Einstein Condensation of atoms with 1/2 pseudo-spin whose the orbital dynamics is coupled to these two internal energy levels. The generation of such a system is done by inducing transitions between the sub-levels m_f = -1 and m_f = 0 from the hyperfine atomic state f = 1 using an arrangement of lasers, that also introduce a spacial dependence due to their phases, that changes accordingly the atom\'s position in the light field, conducting in this way to a interaction that couples orbital motion with spin. It is then considered an effective one dimensional system in the same direction of the laser coupling, where it has been studied different ground state observables, making a sweeping in the equation parameters, showing three typical phases based on momentum distribution. So far, it was determined these phases for attractive interactions, named striped, plane wave and zero momentum, determining as well the location where each one occurs in the equation\'s parameters through a phase diagram. It is also reported, separately, a few relevant observables as individual momentum of each population and the unbalance between the internal spin states, in the transition among these phases, whose the values present abrupt variations, dictating critical values for the parameters, where it occurs. Lately is presented a dynamical study with soliton like solutions, that do not linearly propagate and instead, shows a center of mass and unbalance oscillation, probing different initial conditions.

The layered iridates such as Sr2IrO4 and Sr3Ir2O7, have attracted substantial attention due to their novel electronic states originating from strong spin-orbit coupling and electron-correlation. Recent studies have revealed the possibilities of novel phases such as topological insulators, Weyl semimetals, and even a potential high-Tc superconducting state with a d-wave gap. However, there are still controversial issues regarding the fundamental electronic structure of these systems: the origin of the insulating gap is disputed as arising either from an antiferromagnetic ordering, i.e. Slater scheme or electron-correlation, i.e. Mott scheme. Moreover, it is a formidable task to unveil the physics of layered iridates due to the limited number of available materials for experimental characterizations. One way to overcome this limit and extend our investigation of the layered iridates is using metastable materials. These materials which are far from their equilibrium state, often have mechanical, electronic, and magnetic properties that different from their thermodynamically stable phases. However, these materials cannot be synthesized using thermodynamic equilibrium processes. One way to synthesize these materials is by using pulsed laser deposition (PLD). PLD is able to generate nonequilibrium material phases through the use of substrate strain and deposition conditions. Using this method, we have synthesized several thermodynamically metastable iridate thin-films and have investigated their electronic and optical properties. Synthesizing and investigating metastable iridates opens a path to expand the tunability further than the ability of the bulk methods. This thesis consists of four studies on metastable layered iridate thin film systems. In the first study, three-dimensional Mott variable-range hopping transport with decreased characteristic temperatures under lattice strain or isovalent doping has been observed in Sr2IrO4 thin films. Application of lattice strain or isovalent doping exerts metastable chemical pressure in the compounds, which changes both the bandwidth and electronic hopping. The variation of the characteristic temperature under lattice strain or isovalent doping implies that the density of states near the Fermi energy is reconstructed. The increased density of states in the Sr2IrO4 thin films with strain and isovalent doping could facilitate a condition to induce unprecedented electronic properties, opening a way for electronic device applications. In the second study, the effects of tuning the bandwidth via chemical pressure (i.e., Ca and Ba doping) on the optical properties of Sr2IrO4 epitaxial thin films has been investigated. Substitution of Sr by Ca and Ba ions exerts metastable chemical pressure in the system, which changes both the bandwidth and electronic hopping. The optical conductivity results of these thin films suggest that the two-peak-like optical conductivity spectra of the layered iridates originates from the overlap between the optically-forbidden spin-orbit exciton and the inter-site optical transitions within the Jeff = ½ band, which is consistent with the results obtained from a multi-orbital Hubbard model calculation. In the third study, thermodynamically metastable Ca2IrO4 thin- films have been synthesized. Since the perovskite structure of Ca2IrO4 is not thermodynamically stable, its bulk crystals do not exist in nature. We have synthesized the layered perovskite phase Ca2IrO4 thin- films from a polycrystalline hexagonal bulk crystal using an epitaxial stabilization technique. The smaller A-site in this compound compared to Sr2IrO4 and Ba2IrO4, increases the octahedral rotation and tilting, which enhance electron-correlation. The enhanced electron-correlation is consistent with the observation of increased gap energy in this compound. This study suggest that the epitaxial stabilization of metastable-phase thin-films can be used effectively for investigating complex-oxide systems. Finally, structural, transport, and optical properties of tensile strained (Sr1-xLax)3Ir2O7 (x = 0, 0.025, 0.05) thin-films have been investigated. While high-Tc superconductivity is predicted in the system, all of the samples are insulating. The insulating behavior of the La-doped Sr3Ir2O7 thin-films is presumably due to disorder-induced localization and ineffective electron-doping of La, which brings to light the intriguing difference between epitaxial thin films and bulk single crystals of the iridates. These studies thoroughly investigate a wide array of novel electronic and optical phenomena via tuning the relative strengths of electron correlation, electronic bandwidth, and spin-orbit coupling using perturbations such as chemical doping, and the stabilization of metastable phases in the layered iridates.