The methods producing cold molecules from cold atoms tend to leave molecular ensembles with substantial residual internal energy. For instance, Cs2 molecules initially formed via photoassociation of cold Cs atoms are in several vibrational levels, v, of the electronic ground state. Here we apply a broadband femtosecond laser that redistributes the vibrational population in the ground state via a few electronic excitation - spontaneous emission cycles. The laser pulses are shaped to remove the excitation frequency band of the v = 0 level, preventing re-excitation from that state. We observe a fast and efficient accumulation, about 70% of the initially detected molecules, in the lowest vibrational level, v = 0, of the singlet electronic state. The validity of this incoherent depopulation pumping method is very general and opens exciting prospects for laser cooling and manipulation of molecules.
Some of us have recently reported in Science 321 232 (2008) vibrational cooling of translationally cold Cs_2 molecules into the lowest vibrational level v=0 of the singlet X 1Sigma_g ground electronic state. Starting from a sample of cold molecules produced in a collection of vibrational levels of the ground state, our method was based on repeated optical pumping by laser light with a spectrum broad enough to excite all populated vibrational levels but frequency-limited in such a way to eliminate transitions from v=0 level, in which molecules accumulate. In this paper this method is generalize…
We have recently demonstrated that optical pumping methods combined with photoassociation of ultra-cold atoms can produce ultra-cold and dense samples of molecules in their absolute rovibronic ground state. More generally, both the external and internal degrees of freedom can be cooled by addressing selected rovibrational levels on demand. Here, we recall the basic concepts and main steps of our experiments, including the excitation schemes and detection techniques we use to achieve the rovibrational cooling of Cs2 molecules. In addition, we present the determination of formation pathways and …
The simple structure of the BH molecule makes it an excellent candidate for direct laser cooling. We measure the branching ratios for the decay of the ${\rm A}^{1}Π(v'=0)$ state to vibrational levels of the ground state, ${\rm X}^{1}Σ^{+}$, and find that they are exceedingly favourable for laser cooling. We verify that the branching ratio for the spin-forbidden transition to the intermediate ${\rm a}^{3}Π$ state is inconsequentially small. We measure the frequency of the lowest rotational transition of the X state, and the hyperfine structure in the relevant levels of both the X and A states, …
Molecular overtone transitions provide optical frequency transitions sensitive to variation in the proton-to-electron mass ratio ($μ\equiv m_p/m_e$). However, robust molecular state preparation presents a challenge critical for achieving high precision. Here, we characterize infrared and optical-frequency broadband laser cooling schemes for TeH$^+$, a species with multiple electronic transitions amenable to sustained laser control. Using rate equations to simulate laser cooling population dynamics, we estimate the fractional sensitivity to $μ$ attainable using TeH$^+$. We find that laser cooli…
We study laser cooling of $^{24}$Mg atoms in dipole optical trap with pumping field resonant to narrow $(3s3s)\,^1S_0 \rightarrow \, (3s3p)\,^{3}P_1$ ($λ= 457$ nm) optical transition. For description of laser cooling of atoms in the optical trap with taking into account quantum recoil effects we consider two quantum models. The first one is based on direct numerical solution of quantum kinetic equation for atom density matrix and the second one is simplified model based on decomposition of atom density matrix over vibration states in the dipole trap. We search pumping field intensity and detun…
Laser cycling of resonances can remove entropy from a system via spontaneously emitted photons, with electronic resonances providing the fastest cooling timescales because of their rapid relaxation rates. Although atoms are routinely laser cooled, even simple molecules pose two interrelated challenges for cooling: every populated rotational-vibrational state requires a different laser frequency, and electronic relaxation generally excites vibrations. Here, we cool trapped AlH+ molecules to their ground rotational-vibrational quantum state using an electronically-exciting broadband laser to sim…
We consider the use of pulse-shaped broadband femtosecond lasers to optically cool rotational and vibrational degrees of freedom of molecules. Since this approach relies on cooling rotational and vibrational quanta by exciting an electronic transition, it is most easily applicable to molecules with similar ground and excited potential energy surfaces, such that the vibrational state is usually unchanged during electronic relaxation. Compared with schemes that cool rotations by exciting vibrations, this approach achieves internal cooling on the orders-of- magnitude faster electronic decay times…
We demonstrate the conversion of cold Cs_{2} molecules initially distributed over several vibrational levels of the lowest triplet state a^{3}Σ_{u}^{+} into the singlet ground state X^{1}Σ_{g}^{+}. This conversion is realized by a broadband laser exciting the molecules to a well-chosen state from which they may decay to the singlet state throug\textcolor{black}{h two sequential single-photon emission steps: Th}e first photon populates levels with mixed triplet-singlet character, making possible a second spontaneous emission down to several vibrational levels of the X^{1}Σ_{g}^{+} states. By ad…
We demonstrate rotational and vibrational cooling of cesium dimers by optical pumping techniques. We use two laser sources exciting all the populated rovibrational states, except a target state that thus behaves like a dark state where molecules pile up thanks to absorption-spontaneous emission cycles. We are able to accumulate photoassociated cold Cs2 molecules in their absolute ground state (v = 0, J = 0) with up to 40% efficiency. Given its simplicity, the method could be extended to other molecules and molecular beams. It also opens up general perspectives in laser cooling the external deg…
Fast and efficient state preparation of molecules can be accomplished by optical pumping. Molecular structure that most obviously facilitates cycling involves a strong electronic transition, with favorable vibrational branching (diagonal Franck-Condon factors, aka FCFs) and without any intervening electronic states. Here, we propose important adjustments to those criteria, based on our experience optically pumping SiO$^+$. Specifically, the preference for no intervening electronic states should be revised, and over-reliance on FCFs can miss important features. The intervening electronic state …
We utilize the dark state in a Λ-type three-level system to cool an ensemble of 85Rb atoms in an optical lattice [Morigi et al., Phys. Rev. Lett. 85, 4458 (2000)]. The common suppression of the carrier transition of atoms with different vibrational frequencies allows them to reach a subrecoil temperature of 100 nK after being released from the optical lattice. A nearly zero vibrational quantum number is determined from the time-of-flight measurements and adiabatic expansion process. The features of sideband cooling are examined in various parameter spaces. Our results show that dark-state side…
In order to use a collection of trapped ions for experiments where a well defined preparation of vibrational states is necessary, all vibrational modes have to be cooled to ensure precise and repeatable manipulation of the ions' quantum states. A method for simultaneous sideband cooling of all axial vibrational modes is proposed. By application of a magnetic field gradient the absorption spectrum of each ion is modified such that sideband resonances of different vibrational modes coincide. The ion string is then irradiated with monochromatic electromagnetic radiation, in the optical or microwa…
Alkaline earth monoalkoxide free radicals (MORs) have molecular properties conducive to direct laser cooling to sub-millikelvin temperatures. Using dispersed laser induced fluorescence (DLIF) measurements from a pulsed supersonic molecular beam source we determine vibrational branching ratios and Franck-Condon factors for the MORs CaOH and CaOCH$_{3}$. With narrow linewidth continuous-wave dye laser excitation, we precisely measure fluorescence branching for both $\tilde{X}-\tilde{A}$ and $\tilde{X}-\tilde{B}$ electronic systems in each molecule. Weak symmetry-forbidden decays to excited bendi…
We excite YbF molecules to low-lying vibrational levels of the $A^2Π_{1/2}$ state, and of the nearby perturber state sometimes called [18.6]0.5. By dispersing the fluorescence, we measure branching ratios for the radiative decay to vibrational levels of the $X^2Σ^+$ state. These ratios help to determine the optimum laser cooling scheme for the molecule. Our results establish the practicality of a scheme that was previously suggested [Tarbutt et al., New J. Phys. 15 (2013) 053034] and show how the scheme can be modified to provide a stronger radiative cooling force.
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.
Cooling the rotation and the vibration of molecules by broadband light sources was possible for trapped molecular ions or ultracold molecules. Because of a low power spectral density, the cooling timescale has never fell below than a few milliseconds. Here we report on rotational and vibrational cooling of a supersonic beam of barium monofluoride molecules in less than 440 $μ$s. Vibrational cooling was optimized by enhancing the spectral power density of a semiconductor light source at the underlying molecular transitions allowing us to transfer all the populations of $v''=1-3$ into the vibrat…
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）
We report on the implementation of degenerate Raman sideband cooling of $^{40}$K atoms. The scheme incorporates a 3D optical lattice, which confines the atoms and drives the Raman transitions. The optical cooling cycle is closed by two optical pumping beams. The wavelength of the laser beams forming the lattice is close to the D$_2$ atomic transition, while the optical pumping is operated near the D$_1$ transition. With this cooling method, we achieve temperature of $\sim$$1μ$K of a cloud with $\sim$$10^7$ atoms. This corresponds to a phase space density of $\ge$$10^{-3}$. Moreover, the fermio…
Laser cooling of molecules employing broadband optical pumping involves a timescale separation between laser excitation and spontaneous emission. Here, we optimize the optical pumping step using shaped laser pulses. We derive two optimization functionals to drive population into those excited state levels that have the largest spontaneous emission rates to the target state. We show that, when using optimal control, laser cooling of molecules works even if the Franck-Condon map governing the transitions is preferential to heating rather than cooling. Our optimization functional is also applicab…
We demonstrate the laser cooling of 85Rb atoms in a two-dimensional optical lattice. We follow the two-step degenerate Raman sideband cooling scheme [Kerman et al., Phys. Rev. Lett. 84, 439 (2000)], where a fast cooling of atoms to an auxiliary state is followed by a slow cooling to a dark state. This method has the advantage of independent control of the heating rate and cooling rate from the optical pumping beam. We operate the lattice at a Lamb-Dicke parameter eta=0.45 and show the cooling of spin-polarized 85Rb atoms to the recoil temperature in both dimension within 2.4 ms with the aid of…
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…
We report on the production of cold, state-selected H$_2^+$ molecular ions in a linear RF trap. The ions are produced by (3+1) resonance-enhanced multi-photon ionisation (REMPI) of H$_2$, and sympathetically cooled by laser-cooled Be$^+$ ions. After demonstrating and characterizing the REMPI process, we use photodissociation by a deep UV laser at 213~nm to verify the high vibrational purity of the produced H$_2^+$ ion samples. Moreover, the large difference between the photodissociation efficiencies of ions created in the $v=0$ and $v=1$ levels provides a way to detect a $v=0 \to 1$ transition…
We propose an alternative method to laser cooling. Our approach utilizes the extreme brightness of a supersonic atomic beam, and the adiabatic atomic coilgun to slow atoms in the beam or to bring them to rest. We show how internal-state optical pumping and stimulated optical transitions, combined with magnetic forces can be used to cool the translational motion of atoms. This approach does not rely on momentum transfer from photons to atoms, as in laser cooling. We predict that our method can surpass laser cooling in terms of flux of ultra-cold atoms and phase-space density, with lower require…
We derive an exact and analytical form for the cold-atom momentum distribution after a large number of one-dimensional (1D) Raman cooling cycles has been applied. Our result shows that one can select pulse profiles and lengths rather freely in order to obtain efficient cooling. Our approach takes into account optical pumping (resonant excitation followed by spontaneous emission) as an intergral part of the process, and it is noted that it does not affect the final momentum distribution. Thus subrecoil cooling is possible in general, and not just for carefully selected combinations of pulse for…
Through a combination of spin-exchange collisions in a magnetic field and optical pumping, it is possible to cool a gas of atoms without requiring the loss of atoms from the gas. We investigated this technique, Collision Assisted Zeeman Cooling, using 85Rb and 87Rb. We experimentally confirmed that our measured two isotope CAZ cooling rate agreed with a cooling rate predicted though a simple analytic model. As part of the measured cooling rate, we quantitatively characterized the heating rates associated with our actual implementation of this cooling technique and found hyperfine-changing coll…
We use two-laser optical pumping on a continuous atomic fountain in order to prepare cold cesium atoms in the same quantum ground state. A first laser excites the F=4 ground state to pump the atoms toward F=3 while a second pi-polarized laser excites the F=3 -> F'=3 transition of the D2 line to produce Zeeman pumping toward m=0. To avoid trap states, we implement the first laser in a 2D optical lattice geometry, thereby creating polarization gradients. This configuration has the advantage of simultaneously producing Sisyphus cooling when the optical lattice laser is tuned between the F=4 -> F'…
With a specific choice of laser parameters resulting into a so-called exceptional point in the wavelength-intensity plane, it is possible to produce the coalescence of two Floquet resonances describing the photodissociation of the molecule Na$_2$, which is one of the candidates for molecular cooling. Appropriately tuning laser parameters, following a contour around the exceptional point, the resonances exchange their labels. This represents a laser control of the vibrational transfer from one field-free state to another, through an adiabatic transport involving these resonances. The proportion…
A method of sideband Raman cooling to the vibrational ground state of the $m=0$ Zeeman sublevel in a far-detuned two-dimensional optical lattice is proposed. In our scheme, the Raman coupling between vibrational manifolds of the adjacent Zeeman sublevels is shifted to the red sideband due to the ac Stark effect induced by a weak pump field. Thus, cooling and optical pumping to $m=0$ is achieved by purely optical means with coplanar cw laser beams. The optical lattice and cooling parameters are estimated in the framework of simple theoretical models. An application of the transverse sideband co…
We present a method for producing three-dimensional Bose-Einstein condensates using only laser cooling. The phase transition to condensation is crossed with $2.5 {\times} 10^{4}$ $^{87}\mathrm{Rb}$ atoms at a temperature of $T_{\mathrm{c}} = 0.6\ μ\mathrm{K}$ after 1.4 s of cooling. Atoms are trapped in a crossed optical dipole trap and cooled using Raman cooling with far-off-resonant optical pumping light to reduce atom loss and heating. The achieved temperatures are well below the effective recoil temperature. We find that during the final cooling stage at atomic densities above $10^{14}\ \m…
Recently, laser cooling methods have been extended from atoms to molecules. The complex rotational and vibrational energy level structure of molecules makes laser cooling difficult, but these difficulties have been overcome and molecules have now been cooled to a few microkelvin and trapped for several seconds. This opens many possibilities for applications in quantum science and technology, controlled chemistry, and tests of fundamental physics. This article explains how molecules can be decelerated, cooled and trapped using laser light, reviews the progress made in recent years, and outlines…
Using a laser polarization gradient, we realize 3D Sisyphus cooling of $^{171}$Yb$^+$ ions confined in and near the Lamb-Dicke regime in a linear Paul trap. The cooling rate and final mean motional energy of a single ion are characterized as a function of laser intensity and compared to semiclassical and quantum simulations. Sisyphus cooling is also applied to a linear string of four ions to obtain a mean energy of 1-3 quanta for all vibrational modes, an approximately order-of-magnitude reduction below Doppler cooled energies. This is used to enable subsequent, efficient sideband laser coolin…
The dispersed fluorescence following pulsed dye laser excitation of the $\textrm{B}_2 Σ^+ - \textrm{X}^2 Σ^+(0,0)$ band of a cold sample of SiO$^+$ has been recorded and analyzed. The branching ratios for $\textrm{B}_2 Σ^+ (v=0) \rightarrow \textrm{X}^2 Σ^+(v)$ and $\textrm{B}_2 Σ^+ (v=0) \rightarrow \textrm{A}^2 Π_i(v)$ emission were determined and compared with values predicted based upon existing experimental and theoretical data. The experimentally determined branching ratios show that the $\textrm{B}_2 Σ^+ (v=0) \rightarrow \textrm{X}^2 Σ^+(v)$ transitions are somewhat less diagonal than …
We demonstrate the possibility of energy-selective removal of cold atoms from a tight optical trap by means of parametric excitation of the trap vibrational modes. Taking advantage of the anharmonicity of the trap potential, we selectively remove the most energetic trapped atoms or excite those at the bottom of the trap by tuning the parametric modulation frequency. This process, which had been previously identified as a possible source of heating, also appears to be a robust way for forcing evaporative cooling in anharmonic traps.
We demonstrate slowing and longitudinal cooling of a supersonic beam of CaF molecules using counter-propagating laser light resonant with a closed rotational and almost closed vibrational transition. A group of molecules are decelerated by about 20 m/s by applying light of a fixed frequency for 1.8 ms. Their velocity spread is reduced, corresponding to a final temperature of about 300 mK. The velocity is further reduced by chirping the frequency of the light to keep it in resonance as the molecules slow down.
We measure the upper state lifetime and two ratios of vibrational branching fractions f_{v'v} on the B^{3}Π_{1}(v') - X^{1}Σ^{+}(v) transition of TlF. We find the B state lifetime to be 99(9) ns. We also determine that the off-diagonal vibrational decays are highly suppressed: f_{01}/f_{00} < 2x10^{-4} and f_{02}/f_{00} = 1.10(6)%, in excellent agreement with their predicted values of f_{01}/f_{00} < 8x10^{-4} and f_{02}/f_{00} = 1.0(2)% based on Franck-Condon factors calculated using Morse and RKR potentials. The implications of these results for the possible laser cooling of TlF and fundamen…
We investigate the temporal dynamics of Doppler cooling of an initially hot single trapped atom in the weak binding regime using a semiclassical approach. We develop an analytical model for the simplest case of a single vibrational mode for a harmonic trap, and show how this model allows us to estimate the initial energy of the trapped particle by observing the fluorescence rate during the cooling process. The experimental implementation of this temperature measurement provides a way to measure atom heating rates by observing the temperature rise in the absence of cooling. This method is techn…
We present a study of Sisyphus cooling of molecules: the scattering of a single-photon remove a substantial amount of the molecular kinetic energy and an optical pumping step allow to repeat the process. A review of the produced cold molecules so far indicates that the method can be implemented for most of them, making it a promising method able to produce a large sample of molecules at sub-mK temperature. Considerations of the required experimental parameters, for instance the laser power and linewidth or the trap anisotropy and dimensionality, are given. Rate equations, as well as scattering…
We demonstrate 3D microwave projection sideband cooling of trapped, neutral atoms. The technique employs state-dependent potentials that enable microwave photons to drive vibration-number reducing transitions. The particular cooling sequence we employ uses minimal spontaneous emission, and works even for relatively weakly bound atoms. We cool 76% of atoms to their 3D vibrational ground states in a site-resolvable 3D optical lattice.
Demagnetization cooling relies on spin-orbit coupling that brings motional and spin degrees of freedom into thermal equilibrium. In the case of a gas, one has the advantage that the spin degree of freedom can be cooled very efficiently using optical pumping. We investigate demagnetization cooling of a chromium gas in a deep optical dipole trap over a large temperature range and reach high densities up to $5\times 10^{19} m^{-3}$. We study the loss mechanism under such extreme conditions and identify excited-state collisions as the main limiting process. We discuss that in some systems demagnet…
We propose a process to convert ultracold metastable Cs$_2$ molecules in their lowest triplet state into (singlet) ground state molecules in their lowest vibrational levels. Molecules are first pumped into an excited triplet state, and the triplet-singlet conversion is facilitated by a two-step spontaneous decay through the coupled $A^{1}Σ_{u}^{+} \sim b ^{3}Π_{u}$ states. Using spectroscopic data and accurate quantum chemistry calculations for Cs$_2$ potential curves and transition dipole moments, we show that this process has a high rate and competes favorably with the single-photon decay ba…
We report on vibrational ground-state cooling of a single neutral atom coupled to a high-bandwidth Fabry-Pérot cavity. The cooling process relies on degenerate Raman sideband transitions driven by dipole trap beams, which confine the atoms in three dimensions. We infer a one-dimensional motional ground state population close to $90~\%$ by means of Raman spectroscopy. Moreover, lifetime measurements of a cavity-coupled atom exceeding 40 s imply three-dimensional cooling of the atomic motion, which makes this resource-efficient technique particularly interesting for cavity experiments with limit…
We demonstrate optical cycling and sub-Doppler laser cooling of a cryogenic buffer-gas beam of calcium monohydride (CaH) molecules. We measure vibrational branching ratios for laser cooling transitions for both excited electronic states A and B. We measure further that repeated photon scattering via the $A\leftarrow X$ transition is achievable at a rate of $\sim$ $1.6\times10^6$ photons/s and demonstrate the interaction-time limited scattering of $\sim$ $200$ photons by repumping the largest vibrational decay channel. We also demonstrate the ability to sub-Doppler cool a molecular beam of CaH …
The dicarbon molecular anion is currently of interest as a candidate for laser cooling due to its electronic structure and favorable branching ratios to the ground electronic and vibrational states. Helium has been proposed as a buffer gas to cool the molecule's internal motion. We calculate the cross sections and corresponding rates for rovibrational inelastic collisions of the dicarbon anion with He, and also with Ne and Ar, on three-dimensional ab initio potential energy surfaces using quantum scattering theory. The rates for vibrational quenching with He and Ne are very small and are simil…
We predict that it is possible to cool rotational, vibrational and translational degrees of freedom of molecules by coupling a molecular dipole transition to an optical cavity. The dynamics is numerically simulated for a realistic set of experimental parameters using OH molecules. The results show that the translational motion is cooled to few $μ$K and the internal state is prepared in one of the two ground states of the two decoupled rotational ladders in few seconds. Shorter cooling times are expected for molecules with larger polarizability.
The translational motion of molecular ions can be effectively cooled sympathetically to temperatures below 100 mK in ion traps through Coulomb interactions with laser-cooled atomic ions. The distribution of internal rovibrational states, however, gets in thermal equilibrium with the typically much higher temperature of the environment within tens of seconds. We consider a concept for rotational cooling of such internally hot, but translationally cold heteronuclear diatomic molecular ions. The scheme relies on a combination of optical pumping from a few specific rotational levels into a ``dark …
Controlling the internal degrees of freedom is a key challenge for applications of cold and ultracold molecules. Here, we demonstrate rotational-state cooling of trapped methyl fluoride molecules (CH3F) by optically pumping the population of 16 M-sublevels in the rotational states J=3,4,5, and 6 into a single level. By combining rotational-state cooling with motional cooling, we increase the relative number of molecules in the state J=4, K=3, M=4 from a few percent to over 70%, thereby generating a translationally cold (~30mK) and nearly pure state ensemble of about 10^6 molecules. Our scheme …
Rapid and repeated photon cycling has enabled precision metrology and the development of quantum information systems using a variety of atoms and simple molecules. Extending optical cycling to structurally complex molecules would provide new capabilities in these areas, as well as in ultracold chemistry. Increased molecular complexity, however, makes realizing closed optical transitions more difficult. Building on the already established strong optical cycling of diatomic, linear triatomic, and symmetric top molecules, recent theoretical and experimental work has indicated that cycling will be…
