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Átomos alcalinos são boas sondas para compreender as propriedades do He líquido. Considerável atenção experimental tem sido empregada para analisar as mudanças da posição e da largura da linha do espectro de absorção de átomos alcalinos imersos em um ambiente de He líquido. No lado teórico, vários estudos têm usado modelos simplificados como o modelo de bolhas e o modelo de agregado. Considerações de modelos mais realista agora são oportunas e relevantes. Neste trabalho, nós usamos a combinação da simulação de Monte Carlo (MC) e cálculos ab-initio de mecânica quântica (MQ). As configurações do líquido foram geradas para cálculos posteriores de MQ.Umimportante aspecto é a complexa interação interatômica do par He-He. Usando potenciais parametrizados, as simulações clássicas de MC foram efetuadas para sistemas alcalinos (Na, Rb, Cs e Na2) em He líquido e as condições foram T = 3 K e p = 1 atm. Estruturas estatisticamente descorrelacionadas formadas por um elemento alcalino central, envolvido pela primeira camada de solvatação completa, são amostradas e submetidas em um cálculo do espectro com DFT dependente do tempo usando diferentes funcionais híbridos e conjuntos de bases. Usando os funcionais PBE1PBE e O3LYP com conjuntos de bases extensos obtemos o deslocamento espectral em excelente concordância com os resultados experimentais para os sistemas de um único átomo alcalino. Para comparação, também usamos um modelo de agregado com 14 átomos de He em volta do átomo alcalino obtendo excelentes resultados também. O raio do modelo de agregado convergiu para perto do máximo da primeira camada de solvatação da função de distribuição radial. Um ponto adicional a ser considerado é o cálculo da largura da linha obtido com a simulação em He líquido que é discutida neste trabalho. Para o átomo de Rb, a energia de excitação em He líquido é em torno de -18,9 nm. Com a simulação em ambiente de He líquido obtivemos os melhores resultados entre -16,3 nm e -23,3 nm. O valor do deslocamento espectral usando o modelo de agregado ficou entre os -17,3 nm e - 22,3 nm. Os dois modelos apresentam o mesmo raio da bolha, por volta de 6-7Å. Para outros sistemas, como Na e Cs, encontramos a mesma convergência entre o modelo de agregado, a simulação do He líquido e os resultados experimentais. Para o sistema contendo Na2, os valores obtidos ficaram em boa concordância com os valores experimentais. / Alkali atoms are good probes for the understanding of liquid He properties. As such considerable experimental attention has been devoted to the analysis of the changes of line position and widths of the absorption spectra of alkali atoms in liquid He environment. On the theoretical side, several studies have used simplified models such as bubble and cluster models. Considerations of more realistic models are now timely and relevant. In this work, we use a combination of Monte Carlo (MC) simulation and ab initio quantum mechanical (QM) calculations. Liquid configurations are generated for subsequent QM calculations. One important aspect is the consideration of the complex interatomic interaction of the He-He pair. Using parametrized potentials, classical MC simulations are made for the alkali systems (Na, Rb, Cs and Na2) in liquid He. The conditions were T=3K and p=1 atm. Statistically uncorrelated configurations composed of a central alkaline element, surrounded by the full first solvation shell, are sampled and submitted to time-dependent DFT calculations of the spectrum using dierent hybrids functionals and dierents basis sets. Using the PBE1PBE and O3LYP functionals with large basis sets we obtained a spectral shift in excellent agreement with experiment for the systems of single alkaline atom. For comparison, we also used a cluster model and obtained 14 He atoms around the alkali atom with excellent results too. The radius of the cluster model converged to a value close to the maximum of the first solvation shell in radial distribution function. An additional point considered is the calculation of the spectral line width using the liquid simulation also discussed in this work. For Rb atom, the excitation energy in liquid He is about -18.9 nm. With the liquid He environment simulation we obtained the best results between -16.3 nm and -23.3 nm. The values of the spectral shift using the cluster model were between -17.3 nm and 22.3 nm. The two models show the same bubble radius, about 6-7Å. For the others system, like Na and Cs, we found the same convergence between the cluster model, the simulation of the He liquid and the experimental results. For Na2, the values obtained were in good agreement to the experimental values.

Átomos alcalinos são boas sondas para compreender as propriedades do He líquido. Considerável atenção experimental tem sido empregada para analisar as mudanças da posição e da largura da linha do espectro de absorção de átomos alcalinos imersos em um ambiente de He líquido. No lado teórico, vários estudos têm usado modelos simplificados como o modelo de bolhas e o modelo de agregado. Considerações de modelos mais realista agora são oportunas e relevantes. Neste trabalho, nós usamos a combinação da simulação de Monte Carlo (MC) e cálculos ab-initio de mecânica quântica (MQ). As configurações do líquido foram geradas para cálculos posteriores de MQ.Umimportante aspecto é a complexa interação interatômica do par He-He. Usando potenciais parametrizados, as simulações clássicas de MC foram efetuadas para sistemas alcalinos (Na, Rb, Cs e Na2) em He líquido e as condições foram T = 3 K e p = 1 atm. Estruturas estatisticamente descorrelacionadas formadas por um elemento alcalino central, envolvido pela primeira camada de solvatação completa, são amostradas e submetidas em um cálculo do espectro com DFT dependente do tempo usando diferentes funcionais híbridos e conjuntos de bases. Usando os funcionais PBE1PBE e O3LYP com conjuntos de bases extensos obtemos o deslocamento espectral em excelente concordância com os resultados experimentais para os sistemas de um único átomo alcalino. Para comparação, também usamos um modelo de agregado com 14 átomos de He em volta do átomo alcalino obtendo excelentes resultados também. O raio do modelo de agregado convergiu para perto do máximo da primeira camada de solvatação da função de distribuição radial. Um ponto adicional a ser considerado é o cálculo da largura da linha obtido com a simulação em He líquido que é discutida neste trabalho. Para o átomo de Rb, a energia de excitação em He líquido é em torno de -18,9 nm. Com a simulação em ambiente de He líquido obtivemos os melhores resultados entre -16,3 nm e -23,3 nm. O valor do deslocamento espectral usando o modelo de agregado ficou entre os -17,3 nm e - 22,3 nm. Os dois modelos apresentam o mesmo raio da bolha, por volta de 6-7Å. Para outros sistemas, como Na e Cs, encontramos a mesma convergência entre o modelo de agregado, a simulação do He líquido e os resultados experimentais. Para o sistema contendo Na2, os valores obtidos ficaram em boa concordância com os valores experimentais. / Alkali atoms are good probes for the understanding of liquid He properties. As such considerable experimental attention has been devoted to the analysis of the changes of line position and widths of the absorption spectra of alkali atoms in liquid He environment. On the theoretical side, several studies have used simplified models such as bubble and cluster models. Considerations of more realistic models are now timely and relevant. In this work, we use a combination of Monte Carlo (MC) simulation and ab initio quantum mechanical (QM) calculations. Liquid configurations are generated for subsequent QM calculations. One important aspect is the consideration of the complex interatomic interaction of the He-He pair. Using parametrized potentials, classical MC simulations are made for the alkali systems (Na, Rb, Cs and Na2) in liquid He. The conditions were T=3K and p=1 atm. Statistically uncorrelated configurations composed of a central alkaline element, surrounded by the full first solvation shell, are sampled and submitted to time-dependent DFT calculations of the spectrum using dierent hybrids functionals and dierents basis sets. Using the PBE1PBE and O3LYP functionals with large basis sets we obtained a spectral shift in excellent agreement with experiment for the systems of single alkaline atom. For comparison, we also used a cluster model and obtained 14 He atoms around the alkali atom with excellent results too. The radius of the cluster model converged to a value close to the maximum of the first solvation shell in radial distribution function. An additional point considered is the calculation of the spectral line width using the liquid simulation also discussed in this work. For Rb atom, the excitation energy in liquid He is about -18.9 nm. With the liquid He environment simulation we obtained the best results between -16.3 nm and -23.3 nm. The values of the spectral shift using the cluster model were between -17.3 nm and 22.3 nm. The two models show the same bubble radius, about 6-7Å. For the others system, like Na and Cs, we found the same convergence between the cluster model, the simulation of the He liquid and the experimental results. For Na2, the values obtained were in good agreement to the experimental values.

Atomic precision measurements provide a strong testing ground for new theoretical ideas and fundamental laws of physics. Measurement of the Lamb shift in the hydrogen atom is one of the best examples towards this -it resulted in the birth of QED in 1949 by Dyson, Feynman, Schwinger and Tomonaga. The precision measurements of the hyperfine structure in hydrogen and deuterium by Nafe, Nelson and Rabi indicated that the g-factor for the electron was not exactly 2 as predicted by Dirac, but slightly greater, due to QED effects. Thus the precision measurements are indispensable not only for developing new theory but also for the verification and fine-tuning of theoretical parameters. Precision measurement of hyperfine structure provide valuable information about the nucleus structure, which is helpful in fine tuning of atomic wave-functions used in theoretical calculations. The aim of the work reported in this thesis is the measurement of hyperfine frequency and the observation of hyperfine structure constant in alkali atoms and in Yb atom. This thesis is organized as follows. In Chapter 1, an introduction to the importance of Alkali atoms and Yb atom in the field of precision measurement will be discussed. The scope of this thesis is also discussed in this chapter. In Chapter 2, an introduction to hyperfine structure starting from the beginning of the atomic physics will be discussed. We have discussed about the LS-coupling, jj-coupling, and the influence of the atomic nucleus on atomic spectra. We have also discussed the Zeeman effect and Doppler broadening. In chapter 3, the detail of experimental technique used in this thesis as copropagating satabs, hyperfine frequency measurement using AOM scan, AOM lock and ring cavity has been discussed. Experimental technique to observe the EIT signal in two electron Yb system has been discussed, which can be improved the precision in frequency measurement because of the narrow line-width. In chapter 4, we describe the co-propagating saturated-absorption spectroscopy and its application in frequency measurement. Saturated-absorption spectroscopy (satabs) in a vapor cell is a standard technique used to stabilise the laser frequency. In normal satabs we are getting some extra peaks known as a crossover peaks because laser interact with different velocity group in a vapor cell. In satabs the crossover peaks are stronger and often swamp the true peaks. So we have developed a technique of co-propagating satabs to remove the spurious peak, which has several advantages over conventional satabs. The co-propagating satabs signal appears on a flat background (Doppler-free) with good signal-to-noise ratio and does not have the problem of crossover resonances in between hyperfine transitions. We have adapted this technique to make measurements of hyperfine intervals by using one laser along with an acousto-optic modulator (to produce the scanning pump beam). In chapter 5, we describe the measurement of the hyperfine interval in the 2P1/2 state of 7Li using the SAS technique in hot Li vapor. This technique produces spurious ground crossover resonances that are more prominent that the real peaks. So we have used this ground crossover to measure the hyperfine interval using AOM locking technique. We have developed a technique to measure the absolute frequencies of optical transitions by using an evacuated Rb-stabilized ring-cavity resonator as a transfer cavity. In chapter 6, we study the wavelength-dependent errors due to dispersion at the cavity mirrors by measuring the frequency of the same transition in the Cs D 2 line (at 852 nm) at three cavity lengths. The spread in the values shows that dispersion errors are below 30 kHz, corresponding to a relative precision of 10−10 . We give an explanation for reduced dispersion errors in the ring-cavity geometry by calculating errors due to the lateral shift and the phase shift at the mirrors, and show that they are roughly equal but occur with opposite signs. In chapter 7, we describe precision measurement of hyperfine structure in the 3P2 state of 171,173Yb, and see an unambiguous signature of the magnetic octupole coefficient C in 173Yb. The frequencies of the 3P23S1 transition at 770 nm → are measured using a Rb-stabilized ring-cavity resonator with an accuracy of 200 kHz. In 173Yb we obtain the hyperfine coefficients as A = − 742.11(2) MHz and B = 1339.2(2) MHz, which represent a two orders-of-magnitude improvement in precision, and C = 0.54(2) MHz. Using atomic-structure calculations for two-electron atoms, we extract the nuclear moments quadrupole Q =2.46(12)b and octupole Ω = 34.4(21)b × µN . The observation of nuclear octupole moment in two-electron atoms, to the best of our knowledge, was never reported before. In 171Yb we obtain the hyperfine coefficient A = 2678.49(8) MHz. Using this measurement as well as the previous measurement of A coefficient from our lab, we have compared the hyperfine anomalies for 1P1, 3P1 and 3P2 states. In chapter 8, we describe the EIT in two electron system of 174Yb from 1S0(Fg = 0) 3P1(Fe = 1). We have observed the EIT in degenerate two level system and → after lifting the degeneracy by applying the magnetic field we are getting five peaks. We have also observed the EIT in 173Yb. In 173Yb there are three degenerate two level system Fg =5/2 Fe =3/2, Fg =5/2 Fe =5/2, Fg =5/2 Fe =7/2. →→→ We have observed the same type of EIT signal for all the three transitions Fg = FFe = F, ±F + 1. → In Chapter 9, we give a broad conclusion to the work reported in this thesis and suggest future avenues of research to continue the work started here.

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.

Quantum memories are key components in photonics-based quantum information processing networks. Their ability to store and retrieve information on demand makes repeat-until-success strategies scalable. Warm alkali-metal vapours are interesting candidates for the implementation of such memories, thanks to their very long storage times as well as their experimental simplicity and versatility. Operation with the Raman memory protocol enables high time-bandwidth products, which denote the number of possible storage trials within the memory lifetime. Since large time-bandwidth products enable multiple synchronisation trials of probabilistically operating quantum gates via memory-based temporal multiplexing, the Raman memory is a promising tool for such tasks. Particularly, the broad spectral bandwidth allows for direct and technologically simple interfacing with other photonic primitives, such as heralded single photon sources. Here, this kind of light-matter interface is implemented using a warm caesium vapour Raman memory. Firstly, we study the storage of polarisation-encoded quantum information, a common standard in quantum information processing. High quality polarisation preservation for bright coherent state input signals can be achieved, when operating the Raman memory in a dual-rail configuration inside a polarisation interferometer. Secondly, heralded single photons are stored in the memory. To this end, the memory is operated on-demand by feed-forward of source heralding events, which constitutes a key technological capability for applications in temporal multiplexing. Prior to storage, single photons are produced in a waveguide-based spontaneous parametric down conversion source, whose bespoke design spectrally tailors the heralded photons to the memory acceptance bandwidth. The faithful retrieval of stored single photons is found to be currently limited by noise in the memory, with a signal-to-noise ratio of approximately 0.3 in the memory output. Nevertheless, a clear influence of the quantum nature of an input photon is observed in the retrieved light by measuring the read-out signal's photon statistics via the g⁽²⁾-autocorrelation function. Here, we find a drop in g⁽²⁾ by more than three standard deviations, from g⁽²⁾ ~ 1.69 to g⁽²⁾ ~ 1.59 upon changing the input signal from coherent states to heralded single photons. Finally, the memory noise processes and their scalings with the experimental parameters are examined in detail. Four-wave-mixing noise is determined as the sole important noise source for the Raman memory. These experimental results and their theoretical description point towards practical solutions for noise-free operation.