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 spectroscopy-determined temperatures has been investigated, including the "hidden" weak lines overlapped with the selected transition for DBT measurements. The reproducibility has also been examined to be better than 10 ppm, and it indicates that the instrument is feasible for DBT measurement toward a precision at the ppm level.
We report on observations of thermal motion of a single, Doppler-cooled ion along the axis of a linear radio-frequency quadrupole trap. We show that for a harmonic potential the thermal occupation of energy levels leads to Gaussian distribution of the ion's axial position. The dependence of the spatial thermal spread on the trap potential is used for precise calibration of our imaging system's point spread function and sub-milliKelvin thermometry. We employ this technique to investigate the laser detuning dependence of the Doppler temperature.
We study the time-dependent fluorescence of an initially hot, multi-level, single atomic ion trapped in a radio-frequency Paul trap during Doppler cooling. We have developed an analytical model that describes the fluorescence dynamics during Doppler cooling which is used to extract the initial energy of the ion. While previous models of Doppler cooling thermometry were limited to atoms with a two-level energy structure and neglected the effect of the trap oscillating electric fields, our model applies to atoms with multi-level energy structure and takes into account the influence of micromotio…
Spatially Resolved Temperature Measurement Using Rydberg Doppler Broadening Thermometry
Università di Pisa（比萨大学）；CNR-INO（意大利国家研究委员会光学研究所）；University of Florence（佛罗伦萨大学）；ETH Zürich（苏黎世联邦理工学院）；Universität Innsbruck（因斯布鲁克大学）；Institut für Quantenoptik und Quanteninformation, Österreichische Akademie der Wissenschaften（奥地利科学院量子光学与量子信息研究所）；Observatoire de Paris, Université PSL, CNRS, Sorbonne Université（巴黎天文台，巴黎文理研究大学，法国国家科学研究中心，索邦大学）
Efficient self-interference of single-photons emitted by a sideband-cooled Barium ion is demonstrated. First, the technical tools for performing efficient coupling to the quadrupolar transition of a single $^{138}$Ba$^{+}$ ion are presented. We show efficient Rabi oscillations of the internal state of the ion using a highly stabilized 1.76 $μm$ fiber laser resonant with the S$_{1/2}$-D$_{5/2}$ transition. We then show sideband cooling of the ion's motional modes and use it as a means to enhance the interference contrast of the ion with its mirror-image to up to 90%. Last, we measure the depend…
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…
Doppler broadening in thermal ensembles degrades the absorption cross-section and the coherence time of collective excitations. In two photon transitions, it is common to assume that this problem becomes worse with larger wavelength mismatch. Here we identify an opposite mechanism, where such wavelength mismatch leads to cancellation of Doppler broadening via the counteracting effects of velocity-dependent light-shifts and Doppler shifts. We show that this effect is general, common to both absorption and transparency resonances, and favorably scales with wavelength mismatch. We experimentally …
We report on our on-going effort to measure the Boltzmann constant, kB, using the Doppler Broadening Technique. The main systematic effects affecting the measurement are discussed. A revised error budget is presented in which the global uncertainty on systematic effects is reduced to 2.3 ppm. This corresponds to a reduction of more than one order of magnitude compared to our previous Boltzmann constant measurement. Means to reach a determination of kB at the part per million accuracy level are outlined.
The spin noise of cesium atoms vapor with admixture of buffer gas is experimentally investigated by measuring the spin induced Faraday rotation fluctuations in the vicinity of D 2 line. The line, under these conditions, is known to be strongly inhomogeneously broadened due to the Doppler effect. Despite that, optical spectrum of the spin noise power, as we have found, has the characteristic shape of the homogeneously broadened line with the dip at the line center. This fact is in stark contrast with the results of previous studies of inhomogeneous quantum dot ensembles. In addition, the two-co…
The relation between the jump length probability distribution function and the spectral line profile in resonance atomic radiation trapping is considered for Partial Frequency Redistribution (PFR) between absorbed and reemitted radiation. The single line Opacity Distribution Function [M.N. Berberan-Santos et.al. J.Chem.Phys. 125, 174308 (2006)] is generalized for PFR and used to discuss several possible redistribution mechanisms (pure Doppler broadening, combined natural and Doppler broadening and combined Doppler, natural and collisional broadening). It is shown that there are two coexisting …
We propose a general theoretical scheme to investigate the crossover from electromagnetically induced transparency (EIT) to Autler-Townes splitting (ATS) in open ladder-type atomic and molecular systems with Doppler broadening. We show that when the wavenumber ratio $k_c/k_p\approx -1$, EIT, ATS, and EIT-ATS crossover exist for both ladder-I and ladder-II systems, where $k_c$ ($k_p$) is the wavenumber of control (probe) field. Furthermore, when $k_c/k_p$ is far from $-1$ EIT can occur but ATS is destroyed if the upper state of the ladder-I system is a Rydberg state. In addition, ATS exists but…
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…
New feasibity of coherent quantum control of four-wave mixing processes in a resonant Doppler-broadened medium are studied. We propose a technique which enables one to enhance the quantum efficiency of nonlinear optical conversion. At the same time, it allows one to decrease the required intensities of the fundamental beams compared to those necessary in the approach based on coherent population trapping. The major outcomes of the analysis are illustrated with numerical simulation addressed within a practical medium.
In this paper, we describe an experiment performed at the Laboratoire de Physique des Lasers and dedicated to an optical measurement of the Boltzmann constant. With the proposed innovative technique, determining comes down to an ordinary frequency measurement. The method consists in measuring as accurately as possible the Doppler absorption profile of a rovibrational line of ammonia in thermal equilibrium. This profile is related to the Maxwell-Boltzmann molecular velocity distribution along the laser beam. A fit of the absorption line shape leads to a determination of the Doppler width propor…
Negatively-charged nitrogen-vacancy (NV$^-$) centers in diamond have generated much recent interest for their use in sensing. The sensitivity improves when the NV ground-state microwave transitions are narrow, but these transitions suffer from inhomogeneous broadening, especially in high-density NV ensembles. To better understand and remove the sources of broadening, we demonstrate room-temperature spectral "hole burning" of the NV ground-state transitions. We find that hole burning removes the broadening caused by magnetic fields from $^{13}$C nuclei and demonstrate that it can be used for ma…
We propose the new method of essential decrease of transit-time broadening of Doppler-free absorption resonances on transitions between long-lived quantum levels of atoms (or molecules) of a rarefied gas medium. This method is based on preliminary optical pumping of the ground term of atoms (molecules) by additional radiation which is spatially separated from the recording light beam. The proposed method may be applied in atomic (molecular) spectroscopy of ultra high resolution and also in frequency and time standards.
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. …
A prerequisite for laser cooling a molecular anion, which has not been achieved so far, is the precise knowledge of the relevant transition frequencies in the cooling scheme. To determine these frequencies we present a versatile method that uses one pump and one photodetachment light beam. We apply this approach to C$_{2}^{-}$ and study the laser cooling transitions between the electronic ground state and the second electronic excited state in their respective vibrational ground levels, $B ^{2} Σ_{u} ^{+}(v=0) \leftarrow X ^{2} Σ_{g} ^{+}(v=0) $. Measurements of the R(0), R(2), and P(2) transi…
We present a quantum-mechanical calculation of Stark line widths from electron-ion collisions for the $2s_{1/2}-2p_{1/2,3/2}$, lambda = 2066 and 2067 A, resonance transitions in B III. The results confirm the previous quantum-mechanical R-matrix calculations but contradict recent measurements and semi-classical and some semi-empirical calculations. The differences between the calculations can be attributed to the dominance of small L partial waves in the electron-atom scattering, while the large Stark widths inferred from the measurements would be substantially reduced if allowance is made for…
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 principle of coherent Dicke narrowing in a thin vapour cell, in which sub-Doppler spectral lineshapes are observed under a normal irradiation for a l/2 thickness, is generalized to two-photon spectroscopy. Only the sum of the two wave vectors must be normal to the cell, making the two-photon scheme highly versatile. A comparison is provided between the Dicke narrowing with copropagating fields, and the residual Doppler-broadening occurring with counterpropagating geometries. The experimental feasibility is discussed on the basis of a first observation of a two-photon resonance in a 300 nm-…
In this paper, we investigate mechanical motion of ultra-slow single atoms considering each atom is coherently coupled to a traveling-wave light. The main noise in this system is originated from Doppler broadening due to the continuous momentum distribution in atom wave packet. Here, it is proved that the Doppler broadening could be effectively suppressed in strong coupling regime. Under the coherent coupling, individual neutral atoms periodically walk in a definite direction. Direction of the motion depends on occupation of the atom in its two internal states related to the optical transition…
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 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 …
In this paper, we present significant progress performed on an experiment dedicated to the determination of the Boltzmann constant, k, by accurately measuring the Doppler absorption profile of a line in a gas of ammonia at thermal equilibrium. This optical method based on the first principles of statistical mechanics is an alternative to the acoustical method which has led to the unique determination of k published by the CODATA with a relative accuracy of 1.7 ppm. We report on the first measurement of the Boltzmann constant by laser spectroscopy with a statistical uncertainty below 10 ppm, mo…
The interaction of hot atoms with laser fields experiences a Doppler shift which can severely affect the precise spatial measurement of an atom. We suggest an experimentally realizable scheme to address this issue in three-dimension position measurement of a single atom in vapors of rubidium atoms. Three-level lambda type atom-field configuration is considered where a moving atom interacts with three orthogonal standing-wave laser fields and spatial information of the atom in 3D space is obtained via upper-level population using a weak probe laser field. The atom moves with a velocity along th…
Quantum enhancement and Doppler suppression of Kasevich-Chu atom interferometer with motional squeezing states
Zhejiang University of Technology（浙江工业大学）；Zhejiang Provincial Key Laboratory and Collaborative Innovation Center for Quantum Precise Measurement, Zhejiang University of Technology（浙江工业大学量子精密测量浙江省重点实验室与协同创新中心）；State Key Laboratory of Ocean Sensing and Institute of Quantum Sensing, School of Physics, Zhejiang University（浙江大学物理学院海洋感知国家重点实验室与量子传感研究所）
Spectroscopy has played the key role in revealing, and thereby understanding, the structure of atoms and molecules. A central drive in this field is the pursuit of higher precision and accuracy so that ever more subtle effects might be discovered. Here, we report on laser absorption spectroscopy that operates at the conventional quantum limit imposed by photon shot-noise. Furthermore, we achieve this limit without compromising the accuracy of the measurement. We demonstrate these properties by recording an absorption profile of cesium vapor at the 2 parts-per-million level. The extremely high …
We present precision spectroscopy on electrically trapped formaldehyde (H$_2$CO), demonstrating key attributes which will enable molecular spectroscopy with unprecedented precision. Our method makes use of a microstructured electric trap with homogeneous fields in the trap center and rotational transitions with minimal Stark broadening at a 'magic' offset electric field. Using molecules cooled to the low millikelvin temperature regime via optoelectrical Sisyphus cooling, we reduce Stark broadening on the $J=5\leftarrow4$ ($K=3$) transition at 364 GHz to well below 1 kHz, observe Doppler-limite…
Optical spectroscopy in the gas phase is a key tool to elucidate the structure of atoms and molecules and of their interaction with external fields. The line resolution is usually limited by a combination of first-order Doppler broadening due to particle thermal motion and of a short transit time through the excitation beam. For trapped particles, suitable laser cooling techniques can lead to strong confinement (Lamb-Dicke regime, LDR) and thus to optical spectroscopy free of these effects. For non-laser coolable spectroscopy ions, this has so far only been achieved when trapping one or two at…
We report on the improved measurement of the hyperfine structure of $4f^{12}(^3 H_6)5d_{5/2}6s^2$ $(J=9/2)$ excited state in Tm-169 which is involved in the second-stage laser cooling of Tm. To measure the absolute value of the hyperfine splitting interval we used Doppler-free frequency modulation saturated absorption spectroscopy of Tm atoms in a vapor cell. The sign of the hyperfine constant was determined independently by spectroscopy of laser cooled Tm atoms. The hyperfine constant of the level equals $A_J=-422.112(32)$ MHz that corresponds to the energy difference between two hyperfine su…
We consider the phase stability of a local oscillator (or laser) locked to a cavity QED system comprised of atoms with an ultra-narrow optical transition. The atoms are cooled to millikelvin temperatures and then released into the optical cavity. Although the atomic motion introduces Doppler broadening, the standing wave nature of the cavity causes saturated absorption features to appear, which are much narrower than the Doppler width. These features can be used to achieve an extremely high degree of phase stabilization, competitive with the current state-of-the-art. Furthermore, the inhomogen…
Rapid progress in cooling and trapping of molecules has enabled first experiments on high resolution spectroscopy of trapped diatomic molecules, promising unprecedented precision. Extending this work to polyatomic molecules provides unique opportunities due to more complex geometries and additional internal degrees of freedom. Here, this is achieved by combining a homogeneous-field microstructured electric trap, rotational transitions with minimal Stark broadening at a 'magic' offset electric field, and optoelectrical Sisyphus cooling of molecules to the low millikelvin temperature regime. We …
