Nanofabrication for On-Chip Optical Levitation, Atom-Trapping, and Superconducting Quantum Circuits

Researchers have spent decades refining and improving their methods for fabricating smaller, finer-tuned, higher-quality nanoscale optical elements with the goal of making more sensitive and accurate measurements of the world around them using optics. Quantum optics has been a well-established tool of choice in making these increasingly sensitive measurements which have repeatedly pushed the limits on the accuracy of measurement set forth by quantum mechanics. A recent development in quantum optics has been a creative integration of robust, high-quality, and well-established macroscopic experimental systems with highly-engineerable on-chip nanoscale oscillators fabricated in cleanrooms. However, merging large systems with nanoscale oscillators often require them to have extremely high aspect-ratios, which make them extremely delicate and difficult to fabricate with an "experimentally reasonable" repeatability, yield and high quality. In this work we give an overview of our research, which focused on microscopic oscillators which are coupled with macroscopic optical cavities towards the goal of cooling them to their motional ground state in room temperature environments. The quality factor of a mechanical resonator is an important figure of merit for various sensing applications and observing quantum behavior. We demonstrated a technique for pushing the quality factor of a micromechanical resonator beyond conventional material and fabrication limits by using an optical field to stiffen and trap a particular motional mode of a nanoscale oscillator. Optical forces increase the oscillation frequency by storing most of the mechanical energy in a nearly loss-less optical potential, thereby strongly diluting the effects of material dissipation. By placing a 130 nm thick SiO₂ pendulum in an optical standing wave, we achieve an increase in the pendulum center-of-mass frequency from 6.2 to 145 kHz. The corresponding quality factor increases 50-fold from its intrinsic value to a final value of Q_m = 5.8(1.1) x 10⁵, representing more than an order of magnitude improvement over the conventional limits of SiO₂ for a pendulum geometry. Our technique may enable new opportunities for mechanical sensing and facilitate observations of quantum behavior in this class of mechanical systems. We then give a detailed overview of the techniques used to produce high-aspect-ratio nanostructures with applications in a wide range of quantum optics experiments. The ability to fabricate such nanodevices with high precision opens the door to a vast array of experiments which integrate macroscopic optical setups with lithographically engineered nanodevices. Coupled with atom-trapping experiments in the Kimble Lab, we use these techniques to realize a new waveguide chip designed to address ultra-cold atoms along lithographically patterned nanobeams which have large atom-photon coupling and near 4π Steradian optical access for cooling and trapping atoms. We describe a fully integrated and scalable design where cold atoms are spatially overlapped with the nanostring cavities in order to observe a resonant optical depth of d₀ ≈ 0.15. The nanodevice illuminates new possibilities for integrating atoms into photonic circuits and engineering quantum states of atoms and light on a microscopic scale. We then describe our work with superconducting microwave resonators coupled to a phononic cavity towards the goal of building an integrated device for quantum-limited microwave-to-optical wavelength conversion. We give an overview of our characterizations of several types of substrates for fabricating a low-loss high-frequency electromechanical system. We describe our electromechanical system fabricated on a Si₃N₄ membrane which consists of a 12 GHz superconducting LC resonator coupled capacitively to the high frequency localized modes of a phononic nanobeam. Using our suspended membrane geometry we isolate our system from substrates with significant loss tangents, drastically reducing the parasitic capacitance of our superconducting circuit to ≈ 2.5$ fF. This opens up a number of possibilities in making a new class of low-loss high-frequency electromechanics with relatively large electromechanical coupling. We present our substrate studies, fabrication methods, and device characterization.

Scalable Methods for Deterministic Integration of Quantum Emitters in Photonic Crystal Cavities

We investigated four unique methods for achieving scalable, deterministic integration of quantum emitters into ultra-high Q{V photonic crystal cavities, including selective area heteroepitaxy, engineered photoemission from silicon nanostructures, wafer bonding and dimensional reduction of III-V quantum wells, and cavity-enhanced optical trapping. In these areas, we were able to demonstrate site-selective heteroepitaxy, size-tunable photoluminescence from silicon nanostructures, Purcell modification of QW emission spectra, and limits of cavity-enhanced optical trapping designs which exceed any reports in the literature and suggest the feasibility of capturing- and detecting nanostructures with dimensions below 10 nm. In addition to process scalability and the requirement for achieving accurate spectral- and spatial overlap between the emitter and cavity, these techniques paid specific attention to the ability to separate the cavity and emitter material systems in order to allow optimal selection of these independently, and eventually enable monolithic integration with other photonic and electronic circuitry.

We also developed an analytic photonic crystal design process yielding optimized cavity tapers with minimal computational effort, and reported on a general cavity modification which exhibits improved fabrication tolerance by relying exclusively on positional- rather than dimensional tapering. We compared several experimental coupling techniques for device characterization. Significant efforts were devoted to optimizing cavity fabrication, including the use of atomic layer deposition to improve surface quality, exploration into factors affecting the design fracturing, and automated analysis of SEM images. Using optimized fabrication procedures, we experimentally demonstrated 1D photonic crystal nanobeam cavities exhibiting the highest Q/V reported on substrate. Finally, we analyzed the bistable behavior of the devices to quantify the nonlinear optical response of our cavities.

Classical and Quantum Effects in Plasmonic Metals

The field of plasmonics exploits the unique optical properties of metallic nanostructures to concentrate and manipulate light at subwavelength length scales. Metallic nanostructures get their unique properties from their ability to support surface plasmons– coherent wave-like oscillations of the free electrons at the interface between a conductive and dielectric medium. Recent advancements in the ability to fabricate metallic nanostructures with subwavelength length scales have created new possibilities in technology and research in a broad range of applications.

In the first part of this thesis, we present two investigations of the relationship between the charge state and optical state of plasmonic metal nanoparticles. Using experimental bias-dependent extinction measurements, we derive a potential- dependent dielectric function for Au nanoparticles that accounts for changes in the physical properties due to an applied bias that contribute to the optical extinction. We also present theory and experiment for the reverse effect– the manipulation of the carrier density of Au nanoparticles via controlled optical excitation. This plasmoelectric effect takes advantage of the strong resonant properties of plasmonic materials and the relationship between charge state and optical properties to eluci- date a new avenue for conversion of optical power to electrical potential.

The second topic of this thesis is the non-radiative decay of plasmons to a hot-carrier distribution, and the distribution’s subsequent relaxation. We present first-principles calculations that capture all of the significant microscopic mechanisms underlying surface plasmon decay and predict the initial excited carrier distributions so generated. We also preform ab initio calculations of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We extend these first-principle methods to calculate the electron-temperature dependent dielectric response of hot electrons in plasmonic metals, including direct interband and phonon-assisted intraband transitions. Finally, we combine these first-principles calculations of carrier dynamics and optical response to produce a complete theoretical description of ultrafast pump-probe measurements, free of any fitting parameters that are typical in previous analyses.

Solution combustion synthesis, structure and luminescence of Y3Al5O12 : Tb3+ phosphors

The synthesis and optical properties of Y3Al5O12:Tb3+ phosphors are reported in this paper. Y3Al5O12:Tb3+ phosphors were synthesized by a facile solution combustion method. Citric acid traps the constituent cations and also acts as a fuel. Y3Al5O12 (YAG) phase can crystallize through sintering at 900 degrees C for 2 h, and there were no intermediate phases such as YAlO3 (YAP) and Y4Al2O9 (YAM) in the sintering process. The excitation spectra of crystalline Y3Al5O12:Tb3+ are different from that of amorphous one due to the crystal field effect. The emission spectra mainly show D-5(4) -> F-7(6) transition under UV excitation. The higher concentration quenching in Y3Al5O12:Tb3+ nanophosphors may be due to the confinement effect on resonant energy transfer of nanocrystalline. It is also indicated that the solution combustion synthesis method provides a good distribution of Tb3+ activators in Y3Al5O12 host. (c) 2005 Published by Elsevier B.V.

Nano-modification inside transparent materials by femtosecond laser single beam

Periodic nanostructures along the polarization direction of light are observed inside silica glasses and tellurium dioxide single crystal after irradiation by a focused single femtosecond laser beam. Backscattering electron images of the irradiated spot inside silica glass reveal a periodic structure of stripe-like regions of similar to 20 nm width with a low oxygen concentration. In the case of the tellurium dioxide single crystal, secondary electron images within the focal spot show the formation of a periodic structure of voids with 30 nm width. Oxygen defects in a silica glass and voids in a tellurium dioxide single crystal are aligned perpendicular to the laser polarization direction. These are the smallest nanostructures below the diffraction limit of light, which are formed inside transparent materials. The phenomenon is interpreted in terms of interference between the incident light field and the electric field of electron plasma wave generated in the bulk of material.

Three-dimensional micro- and nano-fabrication in transparent materials by femtosecond laser

Femtosecond pulsed lasers have been widely used for materials microprocessing. Due to their ultrashort pulse width and ultrahigh light intensity, the process is generally characterized by the nonthermal diffusion process. We observed various induced microstructures such as refractive-index-changed structures, color center defects, microvoids and microcracks in transparent materials (e.g., glasses after the femtosecond laser irradiation), and discussed the possible applications of the microstructures in the fabrication of various micro optical devices [e.g., optical waveguides, microgratings, microlenses, fiber attenuators, and three-dimensional (3D) optical memory]. In this paper, we review our recent research developments on single femtosecond-laser-induced nanostructures. We introduce the space-selective valence state manipulation of active ions, precipitation and control of metal nanoparticles and light polarization-dependent permanent nanostructures, and discuss the mechanisms and possible applications of the observed phenomena.

Eu:Y2O3 nano-phosphor prepared by novel energy-saving solution combustion method

A novel energy- and time-saving solution combustion method has been developed to prepare Eu:Y2O3 nano-crystal line phosphor. This novel method employs anhydrous ethanol as solvent and fuel. The prepared nano-crystals after heat-treatment own narrow size distribution, well dispersibility and sinterability, confirmed by XRD, TEM and FTIR. The emission spectra of nano-Eu:Y2O3 Samples show clear nano-size related phenomena. (c) 2007 Elsevier B.V. All rights reserved.

Spray combustion synthesis of nanocrystalline Y2O3 and its thermodynamical and morphological study

Nano Y2O3 particles with a spherical shape and narrow size distribution have been prepared by a novel spray combustion method. The experimental procedure is briefly described and the thermodynamical process of the post-heat treatment is investigated in this paper. The precursor fully crystallized when treated at as low as 400 degrees C. Prepared particles showed spherical shape and well dispersibility under different treating conditions. Narrow size distribution of particles was achieved even when the precursor was treated at 1373 K. (C) 2007 Elsevier B.V. All rights reserved.

Structure and magnetic properties of CoNiP nanowire arrays embedded in AAO template

Ternary CoNiP nanowire (NW) arrays have been synthesized by electrochemical deposition inside the nanochannels of anodic aluminum oxide (AAO) template. The CoNiP NWs deposited at room temperature present soft magnetic properties, with both parallel and perpendicular coercivities less than 500 Oe. In contrast, as the electrolyte temperature (T-elc) increases from 323 to 343 K, the NWs exhibit hard magnetic properties with coercivities in the range of 1000-2500 Oe. This dramatic increase in coercivities can be attributed to the domain wall pinning that is related to the formation of Ni and Co nanocrystallites and the increase of P content. The parallel coercivity (i.e. the applied field perpendicular to the membrane surface) maximum as high as 2500 Oe with squareness ratio up to 0.8 is achieved at the electrolyte temperature of 328 K. It has been demonstrated that the parallel coercivity of CoNiP NWs can be tuned in a wide range of 200-2500 Oe by controlling the electrolyte temperature, providing an easy way to control magnetic properties and thereby for their integration with magnetic-micro-electromechanical systems (MEMS). (C) 2008 Elsevier B.V. All rights reserved.