Cryogenic Silicon Optical Reference Cavities

Thermodynamical fluctuations in temperature and position exist in every physical system, and show up as a fundamental noise limit whenever we choose to measure some quantity in a laboratory environment. Thermodynamical fluctuations in the position of the atoms in the dielectric coatings on the mirrors for optical cavities at the forefront of precision metrology (e.g., LIGO, the cavities which probe atomic transitions to define the second) are a current limiting noise source for these experiments, and anything which involves locking a laser to an optical cavity. These thermodynamic noise sources scale physical geometry of experiment, material properties (such as mechanical loss in our dielectric coatings), and temperature. The temperature scaling provides a natural motivation to move to lower temperatures, with a potential huge benefit for redesigning a room temperature experiment which is limited by thermal noise for cryogenic operation.

We design, build, and characterize a pair of linear Fabry-Perot cavities to explore limitations to ultra low noise laser stabilization experiments at cryogenic temperatures. We use silicon as the primary material for the cavity and mirrors, due to a zero crossing in its linear coefficient of thermal expansion (CTE) at 123 K, and other desirable material properties. We use silica tantala coatings, which are currently the best for making high finesse low noise cavities at room temperature. The material properties of these coating materials (which set the thermal noise levels) are relatively unknown at cryogenic temperatures, which motivates us to study them at these temperatures. We were not able to measure any thermal noise source with our experiment due to excess noise. In this work we analyze the design and performance of the cavities, and recommend a design shift from mid length cavities to short cavities in order to facilitate a direct measurement of cryogenic coating noise.

In addition, we measure the cavities (frequency dependent) photo-thermal response. This can help characterize thermooptic noise in the coatings, which is poorly understood at cryogenic temperatures. We also explore the feasibility of using the cavity to do macroscopic quantum optomechanics such as ground state cooling.

Quantum Electromechanics with Two Tone Drive

In the field of mechanics, it is a long standing goal to measure quantum behavior in ever larger and more massive objects. It may now seem like an obvious conclusion, but until recently it was not clear whether a macroscopic mechanical resonator -- built up from nearly 10¹³ atoms -- could be fully described as an ideal quantum harmonic oscillator. With recent advances in the fields of opto- and electro-mechanics, such systems offer a unique advantage in probing the quantum noise properties of macroscopic electrical and mechanical devices, properties that ultimately stem from Heisenberg's uncertainty relations. Given the rapid progress in device capabilities, landmark results of quantum optics are now being extended into the regime of macroscopic mechanics.

The purpose of this dissertation is to describe three experiments -- motional sideband asymmetry, back-action evasion (BAE) detection, and mechanical squeezing -- that are directly related to the topic of measuring quantum noise with mechanical detection. These measurements all share three pertinent features: they explore quantum noise properties in a macroscopic electromechanical device driven by a minimum of two microwave drive tones, hence the title of this work: "Quantum electromechanics with two tone drive".

In the following, we will first introduce a quantum input-output framework that we use to model the electromechanical interaction and capture subtleties related to interpreting different microwave noise detection techniques. Next, we will discuss the fabrication and measurement details that we use to cool and probe these devices with coherent and incoherent microwave drive signals. Having developed our tools for signal modeling and detection, we explore the three-wave mixing interaction between the microwave and mechanical modes, whereby mechanical motion generates motional sidebands corresponding to up-down frequency conversions of microwave photons. Because of quantum vacuum noise, the rates of these processes are expected to be unequal. We will discuss the measurement and interpretation of this asymmetric motional noise in a electromechanical device cooled near the ground state of motion.

Next, we consider an overlapped two tone pump configuration that produces a time-modulated electromechanical interaction. By careful control of this drive field, we report a quantum non-demolition (QND) measurement of a single motional quadrature. Incorporating a second pair of drive tones, we directly measure the measurement back-action associated with both classical and quantum noise of the microwave cavity. Lastly, we slightly modify our drive scheme to generate quantum squeezing in a macroscopic mechanical resonator. Here, we will focus on data analysis techniques that we use to estimate the quadrature occupations. We incorporate Bayesian spectrum fitting and parameter estimation that serve as powerful tools for incorporating many known sources of measurement and fit error that are unavoidable in such work.

Optomechanical Inertial Sensors and Feedback Cooling

The optomechanical interaction is an extremely powerful tool with which to measure mechanical motion. The displacement resolution of chip-scale optomechanical systems has been measured on the order of 1⁄10th of a proton radius. So strong is this optomechanical interaction that it has recently been used to remove almost all thermal noise from a mechanical resonator and observe its quantum ground-state of motion starting from cryogenic temperatures.

In this work, chapter 1 describes the basic physics of the canonical optomechanical system, optical measurement techniques, and how the optomechanical interaction affects the coupled mechanical resonator. In chapter 2, we describe our techniques for realizing this canonical optomechanical system in a chip-scale form factor.

In chapter 3, we describe an experiment where we used radiation pressure feedback to cool a mesoscopic mechanical resonator near its quantum ground-state from room-temperature. We cooled the resonator from a room temperature phonon occupation of <n> = 6.5 million to an occupation of <n> = 66, which means the resonator is in its ground state approximately 2% of the time, while being coupled to a room-temperature thermal environment. At the time of this work, this is the closest a mesoscopic mechanical resonator has been to its ground-state of motion at room temperature, and this work begins to open the door to room-temperature quantum control of mechanical objects.

Chapter 4 begins with the realization that the displacement resolutions achieved by optomechanical systems can surpass those of conventional MEMS sensors by an order of magnitude or more. This provides the motivation to develop and calibrate an optomechanical accelerometer with a resolution of approximately 10 micro-g/rt-Hz over a bandwidth of approximately 30 kHz. In chapter 5, we improve upon the performance and practicality of this sensor by greatly increasing the test mass size, investigating and reducing low-frequency noise, and incorporating more robust optical coupling techniques and capacitive wavelength tuning. Finally, in chapter 6 we present our progress towards developing another optomechanical inertial sensor - a gyroscope.

Dynamics of non-Abelian Aharonov-Bohm systems

This thesis examines several examples of systems in which non-Abelian magnetic flux and non-Abelian forms of the Aharonov-Bohm effect play a role. We consider the dynamical consequences in these systems of some of the exotic phenomena associated with non-Abelian flux, such as Cheshire charge holonomy interactions and non-Abelian braid statistics. First, we use a mean-field approximation to study a model of U(2) non-Abelian anyons near its free-fermion limit. Some self-consistent states are constructed which show a small SU(2)-breaking charge density that vanishes in the fermionic limit. This is contrasted with the bosonic limit where the SU(2) asymmetry of the ground state can be maximal. Second, a global analogue of Chesire charge is described, raising the possibility of observing Cheshire charge in condensedmatter systems. A potential realization in superfluid He-3 is discussed. Finally, we describe in some detail a method for numerically simulating the evolution of a network of non-Abelian (S₃) cosmic strings, keeping careful track of all magnetic fluxes and taking full account of their non-commutative nature. I present some preliminary results from this simulation, which is still in progress. The early results are suggestive of a qualitatively new, non-scaling behavior.

I. Phosphorescence and the true lifetime of triplet states in fluid solutions. II. Why is condensed oxygen blue?

I. PHOSPHORESCENCE AND THE TRUE LIFETIME OF TRIPLET STATES IN FLUID SOLUTIONS

Phosphorescence has been observed in a highly purified fluid solution of naphthalene in 3-methylpentane (3-MP). The phosphorescence lifetime of C₁₀H₈ in 3-MP at -45 °C was found to be 0.49 ± 0.07 sec, while that of C₁₀D₈ under identical conditions is 0.64 ± 0.07 sec. At this temperature 3-MP has the same viscosity (0.65 centipoise) as that of benzene at room temperature. It is believed that even these long lifetimes are dominated by impurity quenching mechanisms. Therefore it seems that the radiationless decay times of the lowest triplet states of simple aromatic hydrocarbons in liquid solutions are sensibly the same as those in the solid phase. A slight dependence of the phosphorescence lifetime on solvent viscosity was observed in the temperature region, -60° to -18°C. This has been attributed to the diffusion-controlled quenching of the triplet state by residual impurity, perhaps oxygen. Bimolecular depopulation of the triplet state was found to be of major importance over a large part of the triplet decay.

The lifetime of triplet C₁₀H₈ at room temperature was also measured in highly purified benzene by means of both phosphorescence and triplet-triplet absorption. The lifetime was estimated to be at least ten times shorter than that in 3-MP. This is believed to be due not only to residual impurities in the solvent but also to small amounts of impurities produced through unavoidable irradiation by the excitation source. In agreement with this idea, lifetime shortening caused by intense flashes of light is readily observed. This latter result suggests that experiments employing flash lamp techniques are not suitable for these kinds of studies.

The theory of radiationless transitions, based on Robinson's theory, is briefly outlined. A simple theoretical model which is derived from Fano's autoionization gives identical result.

Il. WHY IS CONDENSED OXYGEN BLUE?

The blue color of oxygen is mostly derived from double transitions. This paper presents a theoretical calculation of the intensity of the double transition (a ¹Δ_g) (a ¹Δ_g)←(X ³Σ_g^-) (X ³Σ_g^-), using a model based on a pair of oxygen molecules at a fixed separation of 3.81 Å. The intensity enhancement is assumed to be derived from the mixing (a ¹Δ_g) (a ¹Δ_g) _~~~ (X ³Σ_g^-) (X ³Σ_u^-) and (a ¹Δ_g) (¹Δ_u) _~~~ (X ³Σ_g^-) (X ³Σ_g^-). Matrix elements for these interactions are calculated using a π-electron approximation for the pair system. Good molecular wavefunctions are used for all but the perturbing (B ³Σ_u^-) state, which is approximated in terms of ground state orbitals. The largest contribution to the matrix elements arises from large intramolecular terms multiplied by intermolecular overlap integrals. The strength of interaction depends not only on the intermolecular separation of the two oxygen molecules, but also as expected on the relative orientation. Matrix elements are calculated for different orientations, and the angular dependence is fit to an analytical expression. The theory therefore not only predicts an intensity dependence on density but also one on phase at constant density. Agreement between theory and available experimental results is satisfactory considering the nature of the approximation, and indicates the essential validity of the overall approach to this interesting intensity enhancement problem.

Thermodynamic and kinetic behavior of an argon plasma jet. Decomposition of nitric oxide between 1300 - 1750 degrees K in an argon plasma

In the first part of the study, an RF coupled, atmospheric pressure, laminar plasma jet of argon was investigated for thermodynamic equilibrium and some rate processes.

Improved values of transition probabilities for 17 lines of argon I were developed from known values for 7 lines. The effect of inhomogeneity of the source was pointed out.

The temperatures, T, and the electron densities, n_e , were determined spectroscopically from the population densities of the higher excited states assuming the Saha-Boltzmann relationship to be valid for these states. The axial velocities, v_z, were measured by tracing the paths of particles of boron nitride using a three-dimentional mapping technique. The above quantities varied in the following ranges: 10¹² ˂ n_e ˂ 10¹⁵ particles/cm³, 3500 ˂ T ˂ 11000 °K, and 200 ˂ v_z ˂ 1200 cm/sec.

The absence of excitation equilibrium for the lower excitation population including the ground state under certain conditions of T and n_e was established and the departure from equilibrium was examined quantitatively. The ground state was shown to be highly underpopulated for the decaying plasma.

Rates of recombination between electrons and ions were obtained by solving the steady-state equation of continuity for electrons. The observed rates were consistent with a dissociative-molecular ion mechanism with a steady-state assumption for the molecular ions.

In the second part of the study, decomposition of NO was studied in the plasma at lower temperatures. The mole fractions of NO denoted by x_NO were determined gas-chromatographically and varied between 0.0012 ˂ x_NO ˂ 0.0055. The temperatures were measured pyrometrically and varied between 1300 ˂ T ˂ 1750°K. The observed rates of decomposition were orders of magnitude greater than those obtained by the previous workers under purely thermal reaction conditions. The overall activation energy was about 9 kcal/g mol which was considerably lower than the value under thermal conditions. The effect of excess nitrogen was to reduce the rate of decomposition of NO and to increase the order of the reaction with respect to NO from 1.33 to 1.85. The observed rates were consistent with a chain mechanism in which atomic nitrogen and oxygen act as chain carriers. The increased rates of decomposition and the reduced activation energy in the presence of the plasma could be explained on the basis of the observed large amount of atomic nitrogen which was probably formed as the result of reactions between excited atoms and ions of argon and the molecular nitrogen.

Beta and gamma vibrational bands in deformed nuclei

Energies and relative intensities of gamma transitions in ¹⁵²Sm, ¹⁵²Gd, ¹⁵⁴Gd, ¹⁶⁶Er, and ²³²U following radioactive decay have been measured with a Ge(Li) spectrometer. A peak fitting program has been developed to determine gamma ray energies and relative intensities with precision sufficient to give a meaningful test of nuclear models. Several previously unobserved gamma rays were placed in the nuclear level schemes. Particular attention has been paid to transitions from the beta and gamma vibrational bands, since the gamma ray branching ratios are sensitive tests of configuration mixing in the nuclear levels. As the reduced branching ratios depend on the multipolarity of the gamma transitions, experiments were performed to measure multipole mixing ratios for transitions from the gamma vibrational band. In ¹⁵⁴Gd, angular correlation experiments showed that transitions from the gamma band to the ground state band were predominantly electric quadrupole, in agreement with the rotational model. In ²³²U, the internal conversion spectrum has been studied with a Si(Li) spectrometer constructed for electron spectroscopy. The strength of electric monopole transitions and the multipolarity of some gamma transitions have been determined from the measured relative electron intensities.

The results of the experiments have been compared with the rotational model and several microscopic models. Relative B(E2) strengths for transitions from the gamma band in ²³²U and ¹⁶⁶Er are in good agreement with a single parameter band mixing model, with values of z₂= 0.025(10) and 0.046(2), respectively. Neither the beta nor the gamma band transition strengths in ¹⁵²Sm and ¹⁵⁴Gd can be accounted for by a single parameter theory, nor can agreement be found by considering the large mixing found between the beta and gamma bands. The relative B(E2) strength for transitions from the gamma band to the beta band in ²³²U is found to be five times greater than the strength to the ground state band, indicating collective transitions with strength approximately 15 single particle units.

I. Site effects and exciton structure in molecular crystals - Benzene. II. The first and second triplet states of solid benzene

The effect of intermolecular coupling in molecular energy levels (electronic and vibrational) has been investigated in neat and isotopic mixed crystals of benzene. In the isotopic mixed crystals of C₆H₆, C₆H₅D, m-C₆H₄D₂, p-C₆H₄D₂, sym-C₆H₃D₃, C₆D₅H, and C₆D₆ in either a C₆H₆ or C₆D₆ host, the following phenomena have been observed and interpreted in terms of a refined Frenkel exciton theory: a) Site shifts; b) site group splittings of the degenerate ground state vibrations of C₆H₆, C₆D₆, and sym-C₆H₃D₃; c) the orientational effect for the isotopes without a trigonal axis in both the ¹B_2u electronic state and the ground state vibrations; d) intrasite Fermi resonance between molecular fundamentals due to the reduced symmetry of the crystal site; and e) intermolecular or intersite Fermi resonance between nearly degenerate states of the host and guest molecules. In the neat crystal experiments on the ground state vibrations it was possible to observe many of these phenomena in conjunction with and in addition to the exciton structure.

To theoretically interpret these diverse experimental data, the concepts of interchange symmetry, the ideal mixed crystal, and site wave functions have been developed and are presented in detail. In the interpretation of the exciton data the relative signs of the intermolecular coupling constants have been emphasized, and in the limit of the ideal mixed crystal a technique is discussed for locating the exciton band center or unobserved exciton components. A differentiation between static and dynamic interactions is made in the Frenkel limit which enables the concepts of site effects and exciton coupling to be sharpened. It is thus possible to treat the crystal induced effects in such a fashion as to make their similarities and differences quite apparent.

A calculation of the ground state vibrational phenomena (site shifts and splittings, orientational effects, and exciton structure) and of the crystal lattice modes has been carried out for these systems. This calculation serves as a test of the approximations of first order Frenkel theory and the atom-atom, pair wise interaction model for the intermolecular potentials. The general form of the potential employed was V(r) = Be^-Cr - A/r⁶ ; the force constants were obtained from the potential by assuming the atoms were undergoing simple harmonic motion.

In part II the location and identification of the benzene first and second triplet states (³B_1u and ³E_1u) is given.