Optical magnetometry plays a critical role in low-energy precision measurements and numerous other applications. In particular, permanent electric dipole moment (EDM) searches impose strict requirements on magnetic field sensitivity of the underlying atomic or molecular species. Other magnetometer properties -- such as chemical reactivity, dielectric strength, and interaction cross-sections with other species -- also impose limitations on experimental conditions. Here, we explore a novel approach to optical magnetometry, using multiphoton transitions of diamagnetic atoms to detect Larmor precession of polarized nuclei. Resonant probes are possible at moderate ultraviolet wavelengths, and hyperfine structure couples spin precession to fluorescence transitions with negligible backgrounds; paramagnetic rotation due to intensity-dependent dispersion may also be detectable. Nuclear spins and nonlinear optical excitation introduce new degrees of freedom, and evade limitations arising from rapid electronic decoherence. This dissertation reports progress towards two-photon optical magnetometry using ytterbium, rubidium, and xenon. We characterize the influence of probe polarization and magnetic fields on fluorescence spectra, for one- and two-photon continuous-wave (cw) excitation of ytterbium. Resolved hyperfine and isotope structure allow us to use spin-zero isotopes for diagnostics and normalization, and we develop analysis for overlapping two-photon resonances. We also report measurements of two-photon excitation in ytterbium and rubidium using picosecond laser pulses, and in xenon using a cw laser. Although hyperfine structure is unresolved, the rubidium measurements are sensitive to probe field polarization. Fluorescence spectra from two-photon excitation of ytterbium with femtosecond pulses show modulation when the repetition rate changes. Although techniques for polarizing noble gas nuclei are mature, existing cell designs are incompatible with two-photon magnetometry. We describe development of silicate-assisted hydroxide-catalysis bonding for both aluminosilicate EDM cells with silicon electrodes, and sapphire-windowed cells that transmit ultraviolet excitation light. Progress in measuring the 129Xe nuclear EDM is discussed. Absolute referencing of the picosecond laser to potassium transitions is proposed for two-photon spectroscopy of ytterbium and xenon, and a compatible frequency-tripling method is outlined to produce excitation light for xenon. Novel possibilities including spatial resolution and multiphoton optical pumping of nuclear spins are considered.
Optical magnetometry plays a critical role in low-energy precision measurements and numerous other applications. In particular, permanent electric dipole moment (EDM) searches impose strict requirements on magnetic field sensitivity of the underlying atomic or molecular species. Other magnetometer properties -- such as chemical reactivity, dielectric strength, and interaction cross-sections with other species -- also impose limitations on experimental conditions. Here, we explore a novel approach to optical magnetometry, using multiphoton transitions of diamagnetic atoms to detect Larmor precession of polarized nuclei. Resonant probes are possible at moderate ultraviolet wavelengths, and hyperfine structure couples spin precession to fluorescence transitions with negligible backgrounds; paramagnetic rotation due to intensity-dependent dispersion may also be detectable. Nuclear spins and nonlinear optical excitation introduce new degrees of freedom, and evade limitations arising from rapid electronic decoherence. This dissertation reports progress towards two-photon optical magnetometry using ytterbium, rubidium, and xenon. We characterize the influence of probe polarization and magnetic fields on fluorescence spectra, for one- and two-photon continuous-wave (cw) excitation of ytterbium. Resolved hyperfine and isotope structure allow us to use spin-zero isotopes for diagnostics and normalization, and we develop analysis for overlapping two-photon resonances. We also report measurements of two-photon excitation in ytterbium and rubidium using picosecond laser pulses, and in xenon using a cw laser. Although hyperfine structure is unresolved, the rubidium measurements are sensitive to probe field polarization. Fluorescence spectra from two-photon excitation of ytterbium with femtosecond pulses show modulation when the repetition rate changes. Although techniques for polarizing noble gas nuclei are mature, existing cell designs are incompatible with two-photon magnetometry. We describe development of silicate-assisted hydroxide-catalysis bonding for both aluminosilicate EDM cells with silicon electrodes, and sapphire-windowed cells that transmit ultraviolet excitation light. Progress in measuring the 129Xe nuclear EDM is discussed. Absolute referencing of the picosecond laser to potassium transitions is proposed for two-photon spectroscopy of ytterbium and xenon, and a compatible frequency-tripling method is outlined to produce excitation light for xenon. Novel possibilities including spatial resolution and multiphoton optical pumping of nuclear spins are considered.
Quantum optical sensing is a maturing field that offers the capability to achieve extraor- dinary sensitivity. Atomic magnetometers, for example, now have the capability to detect brain signals and to precisely measure Earth’s gravity field. In optical atomic magnetome- ters, the electronic spins of the atoms in vapor form are aligned in the same direction by “pumping” the ensemble using laser light at a select frequency. Any magnetic field alters the spin states, which changes the optical properties of the vapor, such as the transmission of the laser light, providing a way to measure magnetic fields. After reviewing the theory of atomic structure and atom-light interactions relevant to the research presented here, I describe in the first part of this thesis a vector magnetometry method using microwave-assisted optical pumping, in which a microwave field resonant to the ground state hyperfine splitting of 87Rb pumps an ensemble of warm rubidium vapor, in addition to a strong optical pump beam, and a weaker optical probe beam. I present theoretical details as well as preliminary data demonstrating magnetic field measurements of a DC magnetic field. The measurements were taken when the DC field was aligned at various angles relative to the microwave magnetic field alignment. I compare theoretical and experimental differences in the measurements. With new methods for quantum devices comes the need for portability. In the second part of this thesis, we demonstrate the fabrication of millimeter-sized rubidium vapor cells using silicon micro-machining techniques. This method is relatively inexpensive compared to glass-blowing methods and allows rapid, large-scale production. I describe our process flow and demonstrate the presence of rubidium atoms inside our vapor cells. To conclude, suggestions for improvement are discussed.
The development of an experimental apparatus to produce Bose-Einstein condensates (BECs) of ⁸⁷Rb atoms and their application to magnetometry are discussed. Optical detection of atomic Larmor precession is a widely explored method for high-sensitivity measurements of magnetic fields. In this context, short laser/atom interaction time, atomic thermal diffusion and decoherence effects are among the main limitations. In this thesis, we overcome such problems by using spin-polarised ⁸⁷Rb ultra-cold atoms as the sensing element. After the atoms are polarised, a resonant pulse of radio-frequency excites Larmor precession, which is sensitive to external magnetic fields. By measuring the perturbations of the radio-frequency induced spin precession, information on the magnetic fields of interest. This is achieved by monitoring the polarisation plane’s rotation of a linearly polarised resonant laser probe. In the first part of this thesis, the building and optimisation of a laser-cooling set up to obtain a BEC in a hybrid trap is reported. In order to achieve the Phase Space Density (PSD) required for BEC, several different stages of trapping and cooling are necessary. Each phase has been implemented and optimised. The first step consists in the magneto-optical trap (MOT). Here a velocity dependent damping force and a spatially dependent confining force give the largest changes in PSD. Then atoms are loaded into a hybrid trap obtained by overlapping a quadrupole magnetic potential and a far detuned optical crossed dipole trap. The final stage for the condensation consists of forced evaporative cooling, both via magnetic and optical evaporation. In the second part of the thesis, a general overview of the principles of optical atomic magnetometry is provided and the advantages of using ultra-cold atoms with respect to conventional thermal vapours are discussed. The implementation, operation and a preliminary characterisation of the ultra-cold atom magnetometer are described along with the preliminary results collected. Finally, a plan for future improvements of its sensitivity is presented.
Introduction Shortly after the inception of atomic magnetometry, alkali-vapor magnetometers were being used to measure the Earth's magnetic field to unprecedented precision. During the same era, Bell and Bloom first demonstrated all-optical atomic magnetometry through synchronous optical pumping [1] (see Chapters 1 and 6). In this approach, optical-pumping light is frequency- or amplitude-modulated at harmonics of the Larmor frequency ω L to generate a precessing spin polarization within an alkali vapor at finite magnetic field [2, 3]. Although this technique received considerable attention from the atomic physics community for its applicability to optical pumping experiments, Earth's-field alkali-vapor atomic magnetometers continued to rely on radiofrequency (RF) field excitation for several decades (see Chapter 4). Upon the advent of diode lasers addressing alkali and metastable helium transitions, synchronously pumped magnetometers experienced a revival beginning in the late 1980s. In recent years, such magnetometers have found applications in nuclear magnetic resonance detection [4] (see also Chapter 14), quantum control experiments [5], and chip-scale devices intended for spacecraft use [6] (see also Chapters 7 and 15). All-optical magnetometers possess several advantages over devices that employ RF coils. RF-driven magnetometers can suffer from cross-talk if two sensors are placed in close proximity, since the AC magnetic field driving resonance in one vapor cell can adversely affect the other. All-optical magnetometers are free from such interference. When operated in self-oscillating mode [7], RF-driven magnetometers require an added ±90° electronic phase shift in the feedback loop to counter the intrinsic phase shift between the RF field and the probe-beam modulation.
An ongoing spectroscopic investigation of atomic rubidium utilizes a two-photon, single-laser excitation process. Transitions accessible with our tunable laser include 5P1/2 (F ′ ) ← 5S1/2 (F) and 5P3/2 (F ′ ) ← 5S1/2 (F). The laser is split into a pump and probe beam to allow for Doppler-free measurements of transitions between hyperfine levels. The pump and probe beams are overlapped in a counter-propagating geometry and the laser frequency scans over a transition. Absorption, fluorescence and polarization spectroscopy techniques are applied to this basic experimental setup. The temperature of the vapor cell and the power of the pump and probe beams have been varied to explore line broadening effects and signal-to-noise of each technique. This humble setup will hopefully grow into a more robust experimental arrangement in which double resonance, two-laser excitations are used to explore hyperfine state changing collisions between rubidium atoms and noble gas atoms. Rb-noble gas collisions can transfer population between hyperfine levels, such as 5P3/2 (F ′ = 3) Collision ←− 5P3/2 (F ′ = 2), and the probe beam couples 7S1/2 (F ′′ = 2) ← 5P3/2 (F ′ = 3). Polarization spectroscopy signal depends on the rate of population transfer due to the collision as well as maintaining the orientation created by the pump laser. Fluorescence spectroscopy relies only on transfer of population due to the collision. Comparison of these techniques yields information regarding the change of the magnetic sublevels, mF , during hyperfine state changing collisions.
Introduction Soon after the development of optical magnetometers based on the radio-optical double resonance method (see Chapter 4), it was realized by Bell and Bloom [1] that an alternative method for optical magnetometry was to modulate the light used for optical pumping at a frequency resonant with the Larmor precession of atomic spins. In a Bell-Bloom optical magnetometer, circularly polarized light resonant with an atomic transition propagates through an atomic vapor along a direction transverse to a magnetic field B . Atomic spins immersed in B precess at the Larmor frequency Ω L , and when the light intensity is modulated at Ω m = Ω L , a resonance in the transmitted light intensity is observed. The essential ideas of the Bell–Bloom optical magnetometer are reviewed in Chapter 1 (Section 1.2), and can be summarized in terms of what Bell and Bloom termed optically driven spin precession: in analogy with a driven harmonic oscillator, in a magnetic field B atomic spins precess at a natural frequency equal to Ω L and the light acts as a driving force oscillating at the modulation frequency Ω m . From another point of view, the Bell-Bloom optical magnetometer can be described in terms of synchronous optical pumping: when Ω m = Ω L , there is a “stroboscopic” resonance in which atoms are optically pumped into a spin state stationary in the frame rotating with Ω L . Depending on the details of the atomic structure, the spin state stationary in the rotating frame can be either a dark state that does not interact with the modulated light or a bright state for which the strength of the light–atom interaction is increased.
We have developed a technique for precise measurement of small magnetic fields using nonlinear magneto-optic rotation (NMOR). The technique relies on the resonant laser beam being chopped. During the on time, the atoms are optically pumped into an aligned ground state (Delta m=2 coherence). During the off time, they freely precess around the magnetic field at the Larmor frequency. If the on-off modulation frequency matches (twice) the Larmor precession frequency, the rotation is resonantly enhanced in every cycle, thereby making the process like a repeated Ramsey measurement of the Larmor frequency. We study chopped-NMOR in a paraffin-coated Cs vapor cell. The out-of-phase demodulated rotation shows a Lorentzian peak of linewidth 85 mu G, corresponding to a sensitivity of 0.15nG/root Hz. We discuss the potential of this technique for the measurement of an atomic electric-dipole moment. Copyright (C) EPLA, 2011