Doctor of Philosophy / Department of Physics / Brian R. Washburn / Optical frequency combs produced by mode-locked fiber lasers are useful tools for high precision frequency metrology and molecular spectroscopy in a robust and portable format. We have specifically investigated erbium doped fiber mode-locked lasers that use single-walled carbon nanotubes as a saturable absorber. We have, for the first time, developed and phase- stabilized a carbon nanotube fiber laser (CNFL) frequency comb. The carbon nanotube saturable absorber, which was fabricated using an optically driven deposition method, permits a high repetition frequency (>150 MHz) since an optical nonlinearity of fibers is not used for mode-locking. The CNFL comb combined with a parabolic pulse erbium doped fiber amplifier (EDFA) has shown a compact, robust, and cost-effective supercontinuum source. The amplified pulse from the parabolic pulse EDFA was compressed with a hollow-core photonic bandgap fiber, which produced a wave-breaking-free pulse with an all-fiber set-up. The stabilized comb has demonstrated a fractional instability of 1.2 ×10[superscript]-11 at 1 sec averaging time, the reference-limited instability. We have performed optical frequency metrology with the CNFL comb and have measured an optical frequency, P(13) which is a molecular overtone transition of C2H2. The measured frequency has shown a good agreement with the known value within an uncertainty of 10 kHz. In order to extend the application of the CNFL comb such as multi-heterodyne dual comb spectroscopy, we have investigated the noise of the CNFL comb and particularly, the broad carrier envelope offset frequency (f[subscript]0) linewidth of the CNFL comb. The primary noise source is shown to be white amplitude noise on the oscillator pump laser combined with the sensitivity of the mode-locked laser to pump power fluctuations. The control bandwidth of f[subscipt]0 was limited by the response dynamics of the CNFL comb. The significant reduction of comb noise has been observed by implementing a phase-lead compensation to extend control bandwidth of the comb and by reducing the pump relative intensity noise simultaneously. Therefore the f[subscipt]0 linewidth has been narrower from 850 kHz to 220 kHz. The integrated phase noise for the f[subscipt]0 lock is 1.6 radians from 100 Hz to 102 kHz.

Les horloges à réseau optique montrent des performances impressionnantes et sont en train de soulever la question de la redéfinition de la seconde. Dans ces systèmes, un laser ultra-stable est utilisé en tant qu’oscillateur local pour sonder des transitions optiques très étroites d’atomes neutres piégés dans un réseau optique. La stabilité ultime de ces dispositifs, déterminée par le nombre d’atomes interrogés à chaque cycle et évaluée à quelques 10−17/sqrt(tau) (où tau est le temps d’intégration), n’est actuellement pas atteinte et est limitée à quelques 10−16/sqrt(tau) par les fluctuations de phase du laser sonde. Si l’amélioration des cavités ultra-stables sur lesquels sont stabilisés les lasers sonde est largement étudiée, le LNE-SYRTE a opté pour une approche plus récente, dans laquelle la référence de fréquence utilisée est un trou brûlé spectral creusé dans un cristal dopé terres rares refroidi à température cryogénique (environ 4 K). Une stabilité court terme de quelques 10−18 pourrait alors être atteinte. Cette thèse décrit la construction de l’expérience et montre ensuite les résultats d’une étude spectroscopique à haute résolution sur des trous brûlés spectraux étroits (FWHM = 3.3 kHz) creusés dans le cristal Eu3+ : Y2SiO5. L’influence du cryostat à cycle fermé sur la stabilité des trous brûlés spectraux est notamment mise en évidence et diminuée. Enfin, une méthode d’asservissement originale basée sur une détection hétérodyne d’un trou brûlé spectral et un asservissement numérique via un FPGA qui permet de verrouiller le laser sur le sommet du trou brûlé spectral étroit est décrit et montre une stabilité court terme de quelques 10−14, ce qui est un premier résultat encourageant pour la suite du projet. / Optical lattice clocks show impressive performances and are begining to raise the question of the redefinition of the SI second. In these systems, an ultra-stable laser is used as local oscillator to probe very narrow optical transitions of neutral atoms trapped in an optical lattice. The ultime stability of these systems, determined by the number of atoms interrogated at each clock cycle, evaluated at a few 10−17/sqrt(tau) (where tau is the integration time), is currently not reached and is limited to a few 10−16/sqrt(tau) by the phase fluctuations of the probe laser. If the enhancement of the ultra-stable cavities, on which are currently stabilized the probe lasers, is widely studied, LNE-SYRTE has adopted a more recent approach where the frequency reference is a spectral hole burned in rare earth doped crystal cooled down at cryogenic temperature (around 4 K). A short term stability of a few 10−18 could be achieved. This thesis describes the construction of the experiment and present the results of a high resolution spectroscopy of narrow spectral holes (FWHM = 3.3 kHz) burned in the crystal Eu3+ : Y2SiO5. The influence of the closed cycle cryostat on the behaviour of the spectral holes is hightlighted and reduced. Finally, an original locking scheme based on a heterodyne detection of a spectral hole and a numerical lock program using FPGA in order to stabilize the laser frequency on the top of the narrow spectral hole is described and shows a short term stability of a few 10−14, which is a first promising result for the future of the project.

Precise measurements of both absolute frequencies and small frequency differences of atomic energy levels have played an important role in the development of physics. For example, high precision measurements of absolute frequencies of the 2S½ → 2P ½ transition (D1 line) of alkali atoms form an important link in the measurement of the fine structure constant, α. Similarly, precise interferometric measurements of the local gravitational acceleration (g) rely on the knowledge of the absolute frequencies of the 2S½ → 2P 3/2 transition (D2line) in alkali atoms. Difference frequency measurements of hyperfine structure and isotope shifts of atomic energy levels provide valuable information about the structure of the nucleus, which in turn helps in fine tuning the atomic wave functions used in theoretical calculations. The work reported in this thesis starts with the development and refinement of high precision measurement of absolute frequencies using a ring-cavity resonator. The measurement technique is relatively simple and cost-effective, but the accuracy is comparable to that achieved with the frequency comb technique (10¯11) when the accuracy is limited by the natural linewidth of the transition being measured. The technique combines the advantages of using tunable diode lasers to access atomic transitions with the fact that the absolute frequency of the D2 line in87Rb is known with an accuracy of 6 kHz. A frequency-stabilized diode laser locked to this line is used as a frequency reference, along with a ring-cavity resonator whose length is locked to the reference laser. For a given cavity length, an unknown laser locked to an atomic transition has a small frequency offset from the nearest cavity resonance. We use an acousto-optic modulator (AOM) to compensate for this frequency offset. The measured offset is combined with the cavity mode number to obtain a precise value for the frequency of The unknown laser. We have used this technique for absolute frequency measurements Of the D lines in133Cs and 6,7Li, and the 398.8nm line in Yb. We have also developed a technique to measure the ‘difference frequency’ of atomic energy levels using a single diode laser and an AOM. In this technique, the laser is first locked to a given hyperfine transition. The laser frequency is then shifted using the AOM to another hyperfine transition and the AOM frequency is locked to this difference. Thus the AOM frequency directly gives a measurement of the hyperfine interval. Applying this AOM technique we have measured the hyperfine interval of the D1 lines of all alkali atoms with high precision. We have further developed a technique of coheren-tcontrol spectroscopy (CCS) using co-propagating control and probe beam that is useful for highresolution spectroscopy. In this technique, the probe beam is locked to a transition and its absorption signal is monitored while the control beam is scanned through neighbouring transition. As the control comes into resonance with another transition, the probe absorption is reduced and the signal shows a Doppler free dip. This technique allows us to resolve transitions that are otherwise swamped by crossover resonances in conventional saturated absorption spectroscopy (SAS). We have applied this technique to measure hyperfine intervals in the D2 line of several alkali atoms. Thus, we were able to do high-precision measurements of both absolute and difference frequency of atomic transitions. The precision of the absolute frequency measurement is finally limited by the accuracy of 6 kHz with which the reference frequency is known. The nearby two photon transition in Rb, i.e. the 5S1/2→5D3/2 transition at 778 nm, is known with an accuracy of 1 kHz. In future, we hope to improve the accuracy of our technique using this transition as the reference. This thesis is organized as follows: In Chapter1,we give a brief introduction to our work.. We review the importance of frequency measurements and precision spectroscopy, followed by a comparison of the frequency comb and our ring cavity technique. In Chapter2, we describe measurements of the absolute frequency of the D lines of 133Cs using the ring cavity. We give a detailed discussion of the technique, the Possible sources of errors, and ways to check for the errors. The measurement of the absolute frequency of the D lines of Cs allows a direct comparison to frequency comb measurements, and thus acts as a good check on our technique. In Chapter 3, we describe the absolute frequency and isotope shift measurements in the 398.8 nm line in Yb. We probed this line by frequency doubling the output of a tunable Ti:Sapphire laser. We obtained< 60 kHz precision in our measurements and were able to resolve several discrepancies in previous measurements on this line. In Chapter 4, we describe the measurement of hyperfine structure in the D1 lines of alkali atoms. We used conventional saturated-absorption spectroscopy in a vapor cell to probe different hyperfine transitions and then used our AOM technique to measure the hyperfine interval with high precision. In Chapter 5 we discuss our measurements of hyperfine structure in the D2 lines of several alkali atoms. In the case of 23Na and 39K, the closely-spaced hyperfine transitions are not completely resolved in conventional saturatedabsorption spectroscopy due to the presence of cross over resonances. We have used coherent control spectroscopy to obtain crossover-free spectra and then measured the hyperfine intervals using an AOM. This technique was also used for high resolution spectroscopy in the D2 line of 133Cs. Finally, we describe our measurements of hyperfine structure in the D2 line of Rb using normal saturated absorption spectroscopy. Chapter 6, describes the relative and absolute frequency measurements in the D lines of6,7 Li at 670nm. High-precision measurements in lithium are of special interest because theoretical calculations of atomic properties in this simple three electron system are fairly advanced. Lithium spectroscopy poses an experimental challenge and we describe our efforts in doing highresolution spectroscopy on this system. Chapter 7 describes the hyperfine spectroscopy on the1P 1 state of 173Yb. Measurement of hyperfine structure in 173Yb has a problem because two of the hyperfine transitions overlap with the transition in 172Yb. In our earlier work (described in chapter 4), we had solved this problem by using multipeak fitting to the partially resolved spectrum. Here, we directly resolve the hyperfine transitions by using transverse laser cooling to selectively deflect the 173Yb isotope. In Chapter 8 , we give a broad conclusion to the work reported in this thesis and suggest future avenues of research to continue the work commenced here.