A stable light source obtained using sum-frequency generation (SFG) is developed for high-resolution spectroscopy at 578 nm. Hyperfine transitions of molecular iodine are observed by using the SFG light source with saturation spectroscopy. The light source is frequency stabilized to the observed hyperfine transition and achieves a stability of 2*10-12 for a 1-s averaging time. The absolute frequency of the light source stabilized on the a1 component of the R(37)16-1 transition is determined as 518304551833 (2) kHz. This transition serves as a frequency reference for the 1S0 - 3P0 optical clock transition in neutral ytterbium (Yb).
This article reports on laser absorption spectroscopy of iodine gas between 915 nm and 985 nm. This wavelength range is scanned utilizing a narrow linewidth and mode-hop-free tunable diode-laser whose frequency is actively controlled using a calibrated wavelength meter. This allows us to provide an iodine atlas that contains almost 10,000 experimentally observed reference lines with an uncertainty of 50 MHz. For common lines, good agreement is found with a publication by Gerstenkorn et al. [S. Gerstenkorn, P. Luc, Atlas du spectre d'absorption de la molecule d'iode 14800-20000 cm$^{-1}$, Paris…
In a frequency-modulation spectroscopy experiment, using the radiation from a single frequency diode laser, the spectra of molecular iodine hyperfine structure near 640 nm were recorded on the transition $B^3Π_{0_u^{+}}-X^1Σ^+_{g}$. The frequency reference given by the value of the modulation frequency (12.5 MHz in given experiment) allows determination of the frequency differences between hyperfine components with accuracy better than 0.1 MHz using the fitting procedure in experiment with only one laser.
We demonstrate a compact iodine-stabilized laser operating at 531 nm using a coin-sized light source consisting of a 1062-nm distributed-feedback diode laser and a frequency-doubling element. A hyperfine transition of molecular iodine is observed using the light source with saturated absorption spectroscopy. The light source is frequency stabilized to the observed iodine transition and achieves frequency stability at the 10$^{-12}$ level. The absolute frequency of the compact laser stabilized to the $a_{1}$ hyperfine component of the $R(36)32-0$ transition is determined as $564\,074\,632\,419(…
Absolute frequency measurement of molecular iodine hyperfine transitions at 554 nm and its application to stabilize a 369 nm laser for Yb+ ions cooling
We report absolute frequency measurements of the molecular iodine P(46) 5-4 $a_{1}$, $a_{10}$, and $a_{15}$ hyperfine transitions at 647 nm with a fiber-based frequency comb. The light source is based on a Littrow-type external-cavity diode laser. A frequency stability of 5 $\times$ 10$^{-12}$ at a 200 s integration time is achieved when the light source is stabilized to the P(46) 5-4 $a_{15}$ line. The pressure shift is determined to be -8.3(7) kHz/Pa. Our determination of the line centers reached a precision of 21 kHz. The light source can serve as a reference laser for lithium atom spectros…
We present the design of a compact absolute optical frequency reference for space applications based on hyperfine transitions in molecular iodine with a targeted fractional frequency instability of better than $3\cdot 10^{-14}$. It is based on a micro-integrated extended cavity diode laser with integrated optical amplifier, fiber pigtailed second harmonic generation wave-guide modules, and a quasi-monolithic spectroscopy setup with operating electronics. The instrument described here is scheduled for launch end of 2017 aboard the TEXUS 54 sounding rocket as an important qualification step towa…
We demonstrate two techniques for studying the features of three-level systems driven by two lasers (called control and probe), when the transitions are Doppler broadened as in room-temperature vapor. For $Λ$-type systems, the probe laser is split to produce a counter-propagating pump beam that saturates the transition for the zero-velocity atoms. Probe transmission then shows Doppler-free peaks, which can even have sub-natural linewidth. For V-type systems, the transmission of the control beam is detected as the probe laser is scanned. The signal shows Doppler-free peaks when the probe laser …
The feasibility of sub-Doppler broadband multi-heterodyne spectroscopy with two laser frequency combs is demonstrated with two-photon excitation spectra of the 5S-5D transitions of rubidium vapor.
We determine the frequency of the ultranarrow $^{87}\text{Sr}$ ${^{1}\text{S}_{0}} - {^{3}\text{P}_{2}}$ transition by spectroscopy of an ultracold gas. This transition is referenced to four molecular iodine lines that are observed by Doppler-free saturation spectroscopy of hot iodine vapor. The frequency differences between the Sr and the I$_2$ transitions are measured with an uncertainty of 250 kHz. The absolute frequency of the $^{87}\text{Sr}$ ${^{1}\text{S}_{0}} - {^{3}\text{P}_{2}}$ ($\text{F}'=7/2$) transition is 446648775(30) MHz and limited in accuracy by the iodine reference. This wo…
We have carried out theoretical research on ultra-high resolution spectroscopy of atoms (or molecules) in the suggested cell with a series of plane-parallel thin gas layers between spatially separated gas regions of this cell for optical pumping and probing. It is shown the effective velocity selection of optically pumped atoms because of their specific transit time and collisional relaxation in such a cell, which lead to narrow sub-Doppler resonances in absorption of the probe monochromatic light beam. Resolution of this spectroscopic method is analyzed in cases of stationary and definite non…
We describe Doppler spectroscopy of Bose-Einstein condensates of ytterbium atoms using a narrow optical transition. We address the optical clock transition around 578 nm between the ${^1}S_0$ and ${^3}P_0$ states with a laser system locked on a high-finesse cavity. We show how the absolute frequency of the cavity modes can be determined within a few tens of kHz using high-resolution spectroscopy on molecular iodine. We show that optical spectra reflect the velocity distribution of expanding condensates in free fall or after releasing them inside an optical waveguide. We demonstrate sub-kHz spe…
The method of Doppler - free comb - spectroscopy for dipole transitions was proposed. The calculations for susceptibility spectrum for moving two-level atoms driving by strong counter propagating combs have been done. The used theoretical method based on the Fourier expansion of the components of density matrix on two rows on kv (v-velocity of group of atoms, k-projection of wave vector) and Ω (frequency between comb components). For testing of validity of this method the direct numerical integration was done. The narrow peaks with homogeneous width arise on the background of Doppler counter. …
Compactness, robustness and autonomy of optical frequency references are prerequisites for reliable operation in mobile systems, on ground as well as in space. We present a standalone plug and play optical frequency reference device based on frequency modulation spectroscopy of the D2-transition in rubidium at 780 nm. After a single button press the hand-sized laser module, based on the micro-integrated laser-optical bench described in [J. Opt. Soc. Am. B 38, 1885-1891 (2021)], works fully autonomous and generates 6 mW of frequency stabilized light with a relative frequency instability of 1.4e…
An optical frequency comb generated with an electro-optic phase modulator and a chirped radiofrequency waveform is used to perform saturation and pump-probe spectroscopy on the $D_1$ and $D_2$ transitions of atomic potassium. With a comb tooth spacing of 200 kHz and an optical bandwidth of 2 GHz the hyperfine transitions can be simultaneously observed. Interferograms are recorded in as little as 5 $μ$s (a timescale corresponding to the inverse of the comb tooth spacing). Importantly, the sub-Doppler features can be measured as long as the laser carrier frequency lies within the Doppler profile…
Pressure broadening and pressure shift coefficients for 127I2 (diatomic iodine) in the presence of various buffer gases were determined respectively from the line-widths and line-center shifts observed in Doppler-limited, steady-state, linear absorption spectra near 675 nm as a function of buffer gas pressure through a nonlinear regression analysis of observed line shapes against a Gaussian-Lorentzian convolution line shape model. A line shape model, obtained from a first-order perturbation solution of the time-dependent Schrodinger equation for randomly occurring interactions between a two-le…
Doppler-free spectroscopy using two counter-propagating dual-frequency laser beams in alkali vapor cells has been demonstrated recently, providing the detection of high-contrast sign-reversed natural-linewidth sub-Doppler resonances. However, to date, only a qualitative theory based on a simplified $Λ$-scheme model has been reported to explain underlying physics of this phenomenon. In this work, we develop a general and extended theoretical model of dual-frequency sub-Doppler spectroscopy (DF SDS) for Cs D1 line. The latter considers the real atomic energy structure, main relaxation processes …
The Voigt profile - a convolution of a Gaussian and a Lorentzian - accurately describes the absorption lines of atomic and molecular gases at low probe powers. Fitting such to experimental spectra yields both the Lorentzian natural linewidth and the Gaussian Doppler broadening. However, as the probe power increases saturation effects introduce spurious power dependence into the fitted Doppler width. Using a simple atomic model, we calculate power-dependent corrections to the Voigt profile, which are parametrized by the Gaussian Doppler width, the Lorentzian natural linewidth, and the optical d…
We report the first use of an extremely thin vapor cell (thickness ~ 400 nm) to study the magnetic-field dependence of laser-induced-fluorescence excitation spectra of alkali atoms. This thin cell allows for sub-Doppler resolution without the complexity of atomic beam or laser cooling techniques. This technique is used to study the laser-induced-fluorescence excitation spectra of Rb in a 50 G magnetic field. At this field strength the electronic angular momentum J and nuclear angular momentum I are only partially decoupled. As a result of the mixing of wavefunctions of different hyperfine stat…
We report on Doppler-free continuous-wave optical UV-spectroscopy resolving the hyperfine structure of the $\mathrm{A}\,^2Σ^+ \leftarrow \mathrm{X}\,^2Π_{3/2}$ transition in nitric oxide for total angular momenta $J_X=1.5-19.5$ on the $\mathrm{oP_{12ee}}$ branch. The resulting line splittings are compared to calculated splittings and fitted determining new values for the molecular constants $b, c, eQq_0$ and $b_F$ for the $\mathrm{A}\,^2Σ^+$ state. The constants are in good agreement with values previously determined by quantum beat spectroscopy.
The $3p^{4}$ $^{3}$P$_{J}$ - $3p^{3}4p$ $^{3}$P$_{J}$ transition in the sulphur atom is investigated in a precision two-photon excitation scheme under Doppler-free and collision-free circumstances yielding an absolute accuracy of 0.0009 cm$^{-1}$, using a narrowband pulsed laser. This verifies and improves the level separations between amply studied odd parity levels with even parity levels in S I. An improved value for the $^{3}$P$_{2}$ - $^{3}$P$_{1}$ ground state fine structure splitting is determined at $396.0564$ (7) cm$^{-1}$. A $^{34}$S - $^{32}$S atomic isotope shift was measured from …
Quantitative spectroscopy has been used to measure accurately the Doppler-broadening of atomic transitions in $^{85}$Rb vapor. By using a conventional platinum resistance thermometer and the Doppler thermometry technique, we were able to determine $k_B$ with a relative uncertainty of $4.1\times 10^{-4}$, and with a deviation of $2.7\times 10^{-4}$ from the expected value. Our experiment, using an effusive vapour, departs significantly from other Doppler-broadened thermometry (DBT) techniques, which rely on weakly absorbing molecules in a diffusive regime. In these circumstances, very different…
We report on Doppler-free laser spectroscopy in a Cs vapor cell using a dual-frequency laser system tuned on the Cs D$_1$ line. Using counter-propagating beams with crossed linear polarizations, an original sign-reversal of the usual saturated absorption dip and large increase in Doppler-free atomic absorption is observed. This phenomenon is explained by coherent population trapping (CPT) effects. The impact of laser intensity and light polarization on absorption profiles is reported in both single-frequency and dual-frequency regimes. In the latter, frequency stabilization of two diode lasers…
We demonstrate Doppler-free saturated absorption spectroscopy of cold molecular radicals formed by laser ablation inside a cryogenic buffer gas cell. By lowering the temperature, congested regions of the spectrum can be simplified, and by using different temperatures for different regions of the spectrum a wide range of rotational states can be studied optimally. We use the technique to study the optical spectrum of YbF radicals with a resolution of 30 MHz, measuring the magnetic hyperfine parameters of the electronic ground state. The method is suitable for high resolution spectroscopy of a g…
Interpretation of Doppler-Shift spectroscopy measurement of neutral beams species content requires an assumption about distribution of populations of thin structure of excited state (hydrogen n=3). In the paper several effects caused mixing of sublevel population are discussed and correction factors for different models of thin structure population are calculated. Such mixing can lead to tens percent uncertainty of results of measurements of beam species content. A possible way for experimental verification of sublevel population mixing is proposed.
We study modulation spectroscopy of the potassium D2 transitions at 766.7 nm. The vapour pressure, controlled by heating a commercial reference cell, is optimized using conventional saturated absorption spectroscopy. Subsequent heterodyne detection yields sub-Doppler frequency discriminants suitable for stabilizing lasers in experiments with cold atoms. Comparisons are made between spectra obtained by direct modulation of the probe beam, and those using modulation transfer from the pump via nonlinear mixing. Finally, suggestions are made for further optimization of the signals.
We have demonstrated Doppler-free intermodulated fluorescence spectroscopy of helium $2^3P-3^{1,3}D$ transitions in an rf discharged sealed-off cell using a compact laser system at 588 nm. An external cavity diode laser at 1176 nm was constructed to seed a Raman fiber amplifier. Laser power of more than one watt at 588 nm was produced by frequency doubling of the fiber amplifier output using a MgO:PPLN crystal. A doubling efficiency of 23 % was achieved. The power-dependent spectra of the $2^3P-3^3D$ transitions were investigated. Furthermore, the Doppler-free spectrum of the spin-forbidden $2…
We report on the demonstration of Doppler-free spectroscopy of metastable Sr atoms using a hollow cathode lamp (HCL). We employed a custom Sr HCL which is filled with a mixture of 0.5-Torr Ne and 0.5-Torr Xe as a buffer gas to suppress velocity changing collisions and increase the populations in all the $(5s5p){}^3P_J(J=0,\ 1,\ 2)$ metastable states. We performed frequency-modulation spectroscopy for the $(5s5p){}^3P_0-(5s6s){}^3S_1$, $(5s5p){}^3P_1-(5s6s){}^3S_1$, $(5s5p){}^3P_2-(5s5d){}^3D_2$, and $(5s5p){}^3P_2-(5s5d){}^3D_3$ transitions with sufficient signal to noise ratios for laser freq…
A Doppler broadening thermometry (DBT) instrument is built based on cavity ring-down spectroscopy (CRDS) for precise determination of the Boltzmann constant. Compared with conventional direct absorption methods, the high-sensitivity of CRDS allows to reach a satisfied precision at lower sample pressures, which also reduces the influence due to collisions. By recording the spectrum of C$_2$H$_2$ at 787 nm, we demonstrate a statistical uncertainty of 6 ppm (part per million) in the determined linewidth values by several hours' measurement at a sample pressure of 1.5 Pa. The influence on the spec…
We report the construction of a simple, light weight and compact atomic beam spectroscopy cell for Strontium atoms. The cell is built using glass blowing technique and includes a simple Titanium Sublimation Pump for active pumping of the residual and background gases to maintain ultra-high vacuum. Commercially available and electrically heated dispenser source is used to generate the beam of Sr atoms. We perform spectroscopy on the $5s^2\ ^1S_0\longrightarrow 5s\ 5p\ ^1P_1$ transition to obtain a well resolved Doppler free spectroscopic signal for frequency stabilization of the laser source. T…
We show that a thermal vapor confined in a nanostructure is of spectroscopic interest. We perform reflection spectroscopy on a Cs vapour cell whose window is covered with a thin opal film (typically, 10 or 20 layers of ~ 1μm diameter spheres). Sub-Doppler structures appear in the optical spectrum in a purely linear regime of optical excitation and the signal is shown to originate from the interstitial regions of the opal. These narrow spectral structures, observable for a large range of oblique incidence angles (~ 30-50°), are an original feature associated to the 3-D vapor confinement. It …
We propose and demonstrate pump-probe spectroscopy of rubidium absorption which reveals the sub-Doppler hyperfine structure of the $^{5}$S$_{1/2} \leftrightarrow$ $^{5}$P$_{3/2}$ (D2) transitions. The counter propagating pump and probe lasers are independently tunable in frequency, with the probe operating at the single-photon-level. The two-dimensional spectrum measured as the laser frequencies are scanned shows fluorescence, Doppler-broadened absorption dips and sub-Doppler features. The detuning between the pump and probe lasers allows compensation of the Doppler shift for all atomic veloci…
The erbium atomic system is a promising candidate for an atomic Bose-Einstein condensate of atoms with a non-vanishing orbital angular momentum ($L \neq 0$) of the electronic ground state. In this paper we report on the frequency stabilization of a blue external cavity diode laser system on the 400.91 $nm$ laser cooling transition of atomic erbium. Doppler-free saturation spectroscopy is applied within a hollow cathode discharge tube to the corresponding electronic transition of several of the erbium isotopes. Using the technique of frequency modulation spectroscopy, a zero-crossing error sign…
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 demonstrate a simple technique to measure the resonant frequency of the 398.9 nm 1S0 - 1P1 transition for the different Yb isotopes. The technique, that works by observing and aligning fluorescence spots, has enabled us to measure transition frequencies and isotope shifts with an accuracy of 60 MHz. We provide wavelength measurements for the transition that differ from previously published work. Our technique also allows for the determination of Doppler shifted transition frequencies for photoionisation experiments when the atomic beam and laser beam are not perpendicular and furthermore al…
We demonstrate the use of the ultrafast spatial coherent-control method to resolve the fine-structure two-photon transitions of atomic rubidium. Counter-propagating ultrafast optical pulses with spectral phase and amplitude programmed with our optimized solutions successfully induced the two-photon transitions through $5S_{1/2}$-$5P_{1/2}$-$5D$ and $5S_{1/2}$-$5P_{3/2}$-$5D$ pathways, both simultaneously and at distinct spatial locations. Three different pulse-shaping solutions are introduced that combine amplitude shaping, which avoids direct intermediate resonances, and phase programming, wh…
We have performed for the first time direct laser spectroscopy of the 1S0-3P0 optical clock transition at 265.6 nm in fermionic isotopes of neutral mercury laser-cooled in a magneto-optical trap. Spectroscopy is performed by measuring the depletion of the magneto-optical trap induced by the excitation of the long-lived 3P0 state by a probe at 265.6 nm. Measurements resolve the Doppler-free recoil doublet allowing for a determination of the transition frequency to an uncer- tainty well below the Doppler-broadened linewidth. We have performed absolute measurement of the frequency with respect to…
We present the uncertainty discussion of a recent experiment performed at the GSI storage ring ESR for the accurate energy measurement of the He-like uranium 1s2p3P2- 1s2s3S1 intra-shell transition. For this propose we used a Johann-type Bragg spectrometer that enables to obtain a relative energy measurement between the He-like uranium transition, about 4.51 keV, and a calibration x-ray source. As reference, we used the Ka fluorescence lines of zinc and the Li-like uranium 1s22p2P3/2 - 1 s22s 2S1/2 intra-shell transition from fast ions stored in the ESR. A comparison of the two different refer…
Accurate molecular spectroscopy in the mid-infrared region allows precision measurements of fundamental constants. For instance, measuring the linewidth of an isolated Doppler-broadened absorption line of ammonia around 10 $μ$m enables a determination of the Boltzmann constant k B. We report on our latest measurements. By fitting this lineshape to several models which include Dicke narrowing or speed-dependent collisional effects, we find that a determination of k B with an uncertainty of a few ppm is reachable. This is comparable to the best current uncertainty obtained using acoustic methods…
