Detailed analysis of spectral line broadening and variations in relative intensities of hyperfine spectral components due to optical pumping is presented. Hyperfine levels of sodium $3p_{1/2}$ and $3p_{3/2}$ levels are selectively excited in a supersonic beam at various laser intensities under the conditions when optical pumping time is shorter than transit time of atoms through the laser beam. The excitation spectra exhibit significant line broadening at laser intensities well below the saturation intensity, and redistribution of intensities of hyperfine spectral components is observed, which in some cases is contradicting with intuitive expectations. Theoretical analysis of the dynamics of optical pumping shows that spectral line broadening depends sensitively on branching coefficient of the laser-driven transition. Analytical expressions for branching ratio dependent critical Rabi frequency and critical laser intensity are derived, which give the threshold for onset of noticeable line broadening by optical pumping. Transitions with larger and smaller branching coefficients are relatively less affected. The theoretical excitation spectra were calculated numerically by solving density matrix equations of motion using the split propagation technique, and they well reproduce the observed effects of line broadening and peak intensity variations. The calculations also show that presence of dark (i.e., not laser- coupled) Zeeeman sublevels in the lower state results in effective branching coefficients which vary with laser intensity and differ from those implied by the sum rules, and this can lead to peculiar changes in peak ratios of hyperfine components of the spectra.
We observe a density-dependent collective suppression of optical pumping between the hyperfine ground states in an array of submicrometer-sized clouds of cold rubidium atoms. The suppressed Raman transition rate can be explained by strong resonant dipole-dipole interactions that are enhanced by increasing atom density. The observations are consistent with stochastic electrodynamics simulations that incorporate the effects of the nonlinear population transfer via internal atomic levels embedded in a coupled-dipole model.
We describe an atom trapping mechanism based upon differential optical pumping between metastable hyperfine states by partially-displaced laser beams in the absence of a magnetic field. With realistic laser powers, trap spring constants should match or exceed those typical of magneto-optical traps, and highly flexible tailored trap shapes should be achievable. In a proof-of-principle experiment, we have combined a 1D implementation with magneto-optical trapping in the orthogonal directions, capturing ~10000 85Rb atoms. This is an author-created, un-copyedited version of an article published in…
We present measurements of the hyperfine splitting in the Yb-173 $6s6p~^1P_1^{\rm o} (F^{\prime}=3/2,7/2)$ states that disagree significantly with those measured previously by Das and Natarajan [Phys. Rev. A 76, 062505 (2007)]. We point out inconsistencies in their measurements and suggest that their error is due to optical pumping and improper determination of the atomic line center. Our measurements are made using an optical frequency comb. We use an optical pumping scheme to improve the signal-to-background ratio for the $F^{\prime}=3/2$ component.
Efficient optical pumping is an important tool for state initialization in quantum technologies, such as optical quantum memories. In crystals doped with Kramers rare-earth ions, such as erbium and neodymium, efficient optical pumping is challenging due to the relatively short population lifetimes of the electronic Zeeman levels, of the order of 100 ms at around 4 K. In this article we show that optical pumping of the hyperfine levels in isotopically enriched $^{145}$Nd$^{3+}$:Y$_2$SiO$_5$ crystals is more efficient, owing to the longer population relaxation times of hyperfine levels. By optic…
Hyperfine and Zeeman Optical Pumping and Transverse Laser Cooling of a Thermal Atomic Beam of Dysprosium Using a Single 421 nm Laser
Johannes Gutenberg-Universität Mainz（约翰内斯·古腾堡美因茨大学）；Helmholtz-Institut Mainz, GSI Helmholtzzentrum für Schwerionenforschung（亥姆霍兹美因茨研究所，GSI重离子研究中心）；Department of Physics, Indian Institute of Technology Tirupati（蒂鲁帕蒂印度理工学院物理系）；Korea National University of Education（韩国国立教育大学）；Department of Physics, University of California, Berkeley（加州大学伯克利分校物理系）
The Zeeman hyperfine state dependent force in a Stern-Gerlach (SG) experiment has been exploited to separate and detect atoms having different Zeeman hyperfine states in a cold atom cloud. Utilizing this SG technique, we have made the quantitative estimate of atoms in different Zeeman hyperfine states in an atom cloud, which has been helpful in optimizing the optical pumping of atoms for efficient preparation of atomic state. Employing an optimized optical pumping, nearly $92 \% $ of cold $^{87}Rb$ atoms from a grey magneto-optical trap (G-MOT) on atom-chip have been optically pumped to the tr…
We consider the degree of conservation of nuclear spin polarization in the process of optical pumping under typical spin-exchange optical pumping conditions. Previous analyses have assumed that negligible nuclear spin precession occurs in the brief periods of time the alkali-metal atoms are in the excited state after absorbing photons and before undergoing quenching collisions with nitrogen molecules. We include excited-state hyperfine interactions, electronic spin relaxation in collisions with He and N_2, spontaneous emission, quenching collisions, and a simplified treatment of radiation trap…
We consider the coherent population trapping phenomenon in a thermal sodium atomic beam. We compare the different coherent population trapping schemes that can be established on the D1 line using the Zeeman sublevels of a given ground hyperfine state. The coherent population trapping preparation is examined by means of a Hanle effect configuration. The efficiency of the coherent population trapping phenomenon has been examined in presence of optical pumping into hyperfine levels external to those of the excited transition. We show that both the contrast and the width of the coherent population…
We apply optical pumping to prepare the lithium beam of our atom interferometer in a single hyperfine-Zeeman sublevel: we use two components of the D1-line for pumping the 7Li atoms in a dark state F,mF=+2 (or -2) sublevel. The optical pumping efficiency has been characterized by two techniques: state-selective laser atom deflection or magnetic dephasing of the atom interferometer signals. The first technique has not achieved a high sensitivity, because of a limited signal to noise ratio, but magnetic dephasing signals have shown that about 95% of the population has been transferred in the aim…
The creation and detection of atomic polarization is examined theoretically, through the study of basic optical-pumping mechanisms and absorption and fluorescence measurements, and the dependence of these processes on the size of ground- and excited-state hyperfine splittings is determined. The consequences of this dependence are studied in more detail for the case of nonlinear magneto-optical rotation in the Faraday geometry (an effect requiring the creation and detection of rank-two polarization in the ground state) with alkali atoms. Analytic formulas for the optical rotation signal under v…
We propose an optical pumping scheme to prepare trapped $\mathrm{AlH}^+$ molecules in a pure state, the stretched hyperfine state $\lvert F=\frac{7}{2},\, m_F=\frac{7}{2}\rangle$ of the rovibronic ground manifold $\lvert \mathrm{X}^2Σ^+,\, v=0,\, N=0\rangle$. Our scheme utilizes linearly-polarized and circularly-polarized fields of a broadband pulsed laser to cool the rotational degree of freedom and drive the population to the hyperfine state, respectively. We simulate the population dynamics by solving a representative system of rate equations that accounts for the laser fields, blackbody ra…
We experimentally demonstrate hyperfine optical pumping of rubidium atoms probed by an evanescent electromagnetic field at a dielectric-vapor interface. This light-atom interaction at the nanoscale is investigated using a right angle prism integrated with a vapor cell and excited by evanescent wave under total internal reflection. An efficient hyperfine optical pumping, leading to a complete suppression of absorption on the probed evanescent signal, is observed when a pump laser beam is sent at normal incidence to the interface. In contrast, when the pump and probe beams are co-propagating in …
We present measurements of the hyperfine coefficients and isotope shifts of the Dy I $683.731 $nm transition, using saturated absorption spectroscopy on an atomic beam. A King Plot is drawn resulting in an updated value for the specific mass shift $δν_\mathrm{684,sms}^\mathrm{164-162}=-534 \pm 17 MHz$. Using fluorescence spectroscopy we measure the excited state lifetime $τ_{684}=1.68(5) μ$s, yielding a linewidth of $γ_\mathrm{684} = 95 \pm 3 kHz$. We give an upper limit to the branching ratio between the two decay channels from the excited state showing that this transition is useable for opt…
Due to the low sensitivity of the thulium optical clock to black-body radiation and good accuracy and stability estimations, it appears to be one of the most promising transportable optical clocks. One of the leading systematic effects for Tm clock transition, namely the second-order Zeeman effect, can be canceled by probing two clock transitions between different hyperfine levels of ground and metastable states during the clock operation. We prepare the atoms in $m_F=0$ state of both ground hyperfine levels simultaneously and excite alternately two clock transitions. Here we demonstrate effic…
Nonlinear magneto-optical Faraday rotation (NMOR) on the potassium D1 and D2 lines was used to study Zeeman relaxation rates in an antirelaxation paraffin-coated 3-cm diameter potassium vapor cell. Intrinsic Zeeman relaxation rates of $γ^{NMOR}/2π=2.0(6) {\rm Hz}$ were observed. The relatively small hyperfine intervals in potassium lead to significant differences in NMOR in potassium compared to rubidium and cesium. Using laser optical pumping, widths and frequency shifts were also determined for transitions between ground-state hyperfine sublevels of $^{39}$K atoms contained in the same paraf…
We provide a universal discussion of the interplay between Rydberg-state electromagnetically induced transparency (EIT) and optical pumping (OP) in a thermal Rb87 medium. By pumping the population to one single Hyperfine/Zeeman state, we can enhance the interaction strength and, in principle, amplify the EIT peak. According to our measurements, the EIT peak height can be improved by a factor of two or reduced by one order of magnitude, and linewidth was slightly narrowed by the pumping effect. Similar behavior is also seen by increasing the optical density (OD) of the medium. The EIT feature i…
We establish the existence of a fundamental limit to the efficiency of spin-exchange optical pumping of 3He nuclei by collisions with spin-polarized alkali-metal atoms. Using accurate ab initio calculations of molecular interactions and scattering properties, we show that the maximum 3He spin polarization that can be achieved in spin-exchange collisions with potassium (39K) and silver (107Ag) atoms is limited by the anisotropic hyperfine interaction. We find that spin exchange in Ag-He collisions occurs much faster than in K-He collisions, suggesting the possibility of using Ag in spin-exchang…
Molecular hydrogen ions in weakly bound states close to the first dissociation threshold are attractive quantum sensors for measuring the proton-to-electron mass ratio and hyperfine-induced ortho-para mixing. The experimental accuracy of previous spectroscopic studies relying on fast ion beams could be improved by using state-of-the-art ion trap setups. With the electric dipole moment vanishing in H$_2^+$ and preventing fast spontaneous emission, radiative lifetimes of the order of weeks are found. We include the effect of black-body radiation that can lead to photodissociation and rovibronic …
We perform Zeeman spectroscopy on a Rydberg electromagnetically induced transparency (EIT) system in a room-temperature Cs vapor cell, in magnetic fields up to 50~Gauss and for several polarization configurations. The magnetic interactions of the $\vert 6S_{1/2}, F_g=4 \rangle$ ground, $\vert 6P_{3/2}, F_e=5 \rangle$ intermediate, and $\vert 33S_{1/2} \rangle$ Rydberg states that form the ladder-type EIT system are in the linear Zeeman, quadratic Zeeman, and the deep hyperfine Paschen-Back regimes, respectively. Starting in magnetic fields of about 5~Gauss, the spectra develop an asymmetry tha…
The precise control and knowledge over the atomic dynamics is central to the advancement of quantum technology. The different experimental conditions namely, atoms in a vacuum, an anti-relaxation coated and a buffer gas filled atomic cell provides complementary platform for such investigations. The extent of changes in optical pumping, velocity changing collision and hyperfine changing collision rates associated with these conditions are discussed. There is a phenomenal change in the optical density by a factor of >25 times in presence of a control field in buffer gas environment. In contrary …
The $6S_{1/2}-5D_{5/2}$ electric quadrupole transition is investigated in Cesium vapor at room temperature via nonlinear Doppler-free 6P-6S-5D three-level spectroscopy. Frequency-resolved studies of individual E2 hyperfine lines allow one to analyze optical pumping dynamics, polarization selection rules and line intensities. It opens the way to studies of transfer of light orbital angular momentum to atoms, and the influence of metamaterials on E2 line spectra.
We report an increase of up to 60% on the count rates of the rare $^{81}\mathrm{Kr}$ and $^{85}\mathrm{Kr}$ isotopes in the Atom Trap Trace Analysis method by enhancing the production of metastable atoms in the discharge source. Additional atoms in the metastable $ 1s_5 $ level (Paschen notation) are obtained via optically pumping the $1s_4-2p_6$ transition at 819 nm. By solving the master equation for the system, we identify this transition to be the most suitable one and can describe the measured increase in metastable population as a function of the 819-nm laser power. We calculate the prev…
We report our study of the optical pumping effect in absorption imaging of $^{23}$Na atoms in the $F=1$ hyperfine spin states. Solving a set of rate equations for the spin populations in the presence of a probe beam, we obtain an analytic expression for the optical signal of the $F=1$ absorption imaging. Furthermore, we verify the result by measuring the absorption spectra of $^{23}$Na Bose-Einstein condensates prepared in various spin states with different probe beam pulse durations. The analytic result can be used in the quantitative analysis of $F=1$ spinor condensate imaging and readily ap…
Electro-optic frequency combs with tooth spacings as low as 100 Hz were employed to probe electromagnetically induced transparency (EIT) and hyperfine pumping in rubidium and potassium vapor cells. From the potassium EIT transition we were able to determine the ground state hyperfine splitting with a fit uncertainty of 8 Hz. Importantly, because of the mutual coherence between the control and probe beams, which originate from a single laser, features with linewidths several orders-of-magnitude narrower than the laser linewidth could be observed in a multiplexed fashion. This approach removes t…
We demonstrate the first application of a liquid-metal ion source for collinear laser spectroscopy in proof-of-principle measurements on naturally abundant In$^+$. The superior beam quality, i.e., the actively stabilized current and energy of a beam with very low transverse emittance, allowed us to perform precision spectroscopy on the $5s^2\;^1\mathrm{S}_0 \rightarrow 5s5p\;^3\mathrm{P}_1$ intercombination transition in $^{115}$In$^+$, which is to our knowledge the slowest transition measured with collinear fluorescence laser spectroscopy so far. By applying collinear and anticollinear spectr…
Efficient Separation of the Isomeric State $^{26\text{m}}\text{Al}$ from the Intense Ground State Background via Sequential Optical Pumping in Collinear Laser Spectroscopy
We study the excitation redistribution from cesium $7\mathrm{P}_{1/2}$ or $7\mathrm{P}_{3/2}$ to neighboring energy levels by Black Body Radiation (BBR) and inter atomic collisions using pump-probe spectroscopy inside a vapor cell. At low vapor densities we measure redistribution of the initial, velocity-selected, atomic excitation by BBR. This preserves the selected atomic velocities allowing us to perform high resolution spectroscopy of the $\mathrm{6D\rightarrow 7F}$ transitions. This transfer mechanism could also be used to perform sub-Doppler spectroscopy of the cesium highly-excited $\ma…
The structure of the excited $2^{3}$S and $2^{3}$P triplet states of $^{3}$He and $^{4}$He in an applied magnetic field B is studied using different approximations of the atomic Hamiltonian. All optical transitions (line positions and intensities) of the 1083 nm $2^{3}$S-$2^{3}$P transition are computed as a function of B. The effect of metastability exchange collisions between atoms in the ground state and in the $2^{3}$S metastable state is studied, and rate equations are derived, for the populations these states in the general case of an isotopic mixture in an arbitrary field B. It is shown…
Hyperfine spectroscopy and laser cooling of the fermionic isotopes $^{47}$Ti and $^{49}$Ti
University of California, Berkeley（加州大学伯克利分校）；Challenge Institute for Quantum Computation（挑战量子计算研究所）；Joint Quantum Institute, National Institutes for Standards and Technology（国家标准与技术研究院联合量子研究所）；Department of Physics, University of Chicago（芝加哥大学物理系）；Department of Physics and Astronomy, University of Delaware（特拉华大学物理与天文学系）
The three Mn I lines at 17325, 17339 and 17349 Å~are among the 25 strongest lines ($\log(gf)>0.5$) in the H-band. They are all heavily broadened due to hyperfine structure and the profiles of these lines have so far not been understood. Earlier studies of these lines even suggested that they were blended. In this work, the profiles of these three infra-red (IR) lines have been studied theoretically and compared to experimental spectra to assist in the complete understanding of the solar spectrum in the IR. It is shown that the structure of these lines can not be described in the conventional w…
We present our work on High Energy Material detection based on thin film of Lithium using the phenomenon of Optical Pumping. The Li atoms present in the thin film are optically pumped to one of the ground hyperfine energy levels so that they can no more absorb light from the resonant light source. Now in presence of a RF signal, which quantifies the ambient magnetic field, this polarized atomic system is again randomized thus making it reabsorb the resonant light. This gives a quantified measurement of the magnetic field surrounding the thin film detector. This is then mapped to the presence o…
Using laser optical pumping, widths and frequency shifts are determined for microwave transitions between ground-state hyperfine components of $^{85}$Rb and $^{87}$Rb atoms contained in vapor cells with alkane anti-relaxation coatings. The results are compared with data on Zeeman relaxation obtained in nonlinear magneto-optical rotation (NMOR) experiments, a comparison important for quantitative understanding of spin-relaxation mechanisms in coated cells. By comparing cells manufactured over a forty-year period we demonstrate the long-term stability of coated cells, an important property for a…
We study the Doppler-broadened absorption of a weak monochromatic probe beam in a thermal rubidium vapour cell on the D lines. A detailed model of the susceptibility is developed which takes into account the absolute linestrengths of the allowed electric dipole transitions and the motion of the atoms parallel to the probe beam. All transitions from both hyperfine levels of the ground term of both isotopes are incorporated. The absorption and refractive index as a function of frequency are expressed in terms of the complementary error function. The absolute absorption profiles are compared with…
Doppler broadening plays an important role in laser rovibrational spectroscopy of trapped deuterated molecular hydrogen ions (HD$^+$), even at the millikelvin temperatures achieved through sympathetic cooling by laser-cooled beryllium ions. Recently, Biesheuvel \textit{et al.} \cite{Biesheuvel2016} presented a theoretical lineshape model for such transitions which not only considers linestrengths and Doppler broadening, but also the finite sample size and population redistribution by blackbody radiation, which are important in view of the long storage and probe times achievable in ion traps. H…
A new nano-cell with smoothly varying longitudinal thickness of the atomic vapour layer L in the range of 350 - 5100 nm allowing to study the resonant absorption of D1 and D2 lines of Cs atoms for thicknesses changing from L = Lambda/2 to L = 6 Lambda with the step of Lambda/2 (Lambda = 852 nm or 894 nm are the resonant laser wavelengths) and for different intensities is developed. It is revealed that for low laser intensities there is narrowing of the resonant absorption spectrum for the thicknesses L = (2n + 1)Lambda/2 (where n is an integer) up to L = 7Lambda /2 and broadening of the spectr…
State-Dependent Diffusion and Spectra of Strongly Driven Thermal Atoms
School of Electronics, Peking University（北京大学电子学院）；National Key Laboratory of Advanced Micro and Nano Manufacture Technology, School of Integrated Circuits, Peking University（北京大学集成电路学院先进微纳制造技术国家重点实验室）；Beijing Advanced Innovation Center for Integrated Circuits（北京集成电路创新中心）；Hefei National Laboratory（合肥国家实验室）
Analytical model for polarization transfer during gas-phase collision events in spin-exchange optical pumping: Spin-$\frac{1}{2}$ $^{129}$Xe versus spin-$\frac{3}{2}$ $^{131}$Xe
We report on a two-channel magnetometer based on nonlinear magneto-optical rotation in a Cs glass cell with buffer gas. The Cs atoms are optically pumped and probed by free running diode lasers tuned to the D$_2$ line. A wide frequency modulation of the pump laser is used to produce both synchronous Zeeman optical pumping and hyperfine repumping. The magnetometer works in an unshielded environment and spurious signal from distant magnetic sources is rejected by means of differential measurement. In this regime the magnetometer simultaneously gives the magnetic field modulus and the field diffe…
