Photoassociation of two ultracold rubidium atoms and the subsequent formation of stable molecules in the singlet ground and lowest triplet states is investigated theoretically. The method employs laser pulses inducing transitions via excited states correlated to the $5S+5P_{1/2}$ asymptote. Weakly bound molecules in the singlet ground or lowest triplet state can be created by a single pulse while the formation of more deeply bound molecules requires a two-color pump-dump scenario. More deeply bound molecules in the singlet ground or lowest triplet state can be produced only if efficient mechanisms for both pump and dump steps exist. While long-range $1/R^3$-potentials allow for efficient photoassociation, stabilization is facilitated by the resonant spin-orbit coupling of the $0_u^+$ states. Molecules in the singlet ground state bound by a few wavenumbers can thus be formed. This provides a promising first step toward ground state molecules which are ultracold in both translational and vibrational degrees of freedom.
Photoassociation of ultracold rubidium atoms with femtosecond laser pulses is studied theoretically. The spectrum of the pulses is cut off in order to suppress pulse amplitude at and close to the atomic resonance frequency. This leads to long tails of the laser pulse as a function of time giving rise to coherent transients in the photoassociation dynamics. They are studied as a function of cutoff position and chirp of the pulse. Molecule formation in the electronically excited state is attributed to off-resonant excitation in the strong-field regime.
We experimentally investigate various processes present in the photoassociative interaction of an ultracold atomic sample with shaped femtosecond laser pulses. We demonstrate the photoassociation of pairs of rubidium atoms into electronically excited, bound molecular states using spectrally cut femtosecond laser pulses tuned below the rubidium D1 or D2 asymptote. Time-resolved pump-probe spectra reveal coherent oscillations of the molecular formation rate, which are due to coherent transient dynamics in the electronic excitation. The oscillation frequency corresponds to the detun-ing of the sp…
An experimental pump-probe study of the photoassociative creation of translationally ultracold rubidium molecules is presented together with numerical simulations of the process. The formation of loosely bound excited-state dimers is observed as a first step towards a fully coherent pump-dump approach to the stabilization of Rb$_2$ into its lowest ground vibrational states. The population that contributes to the pump-probe process is characterized and found to be distinct from a background population of pre-associated molecules.
Two atoms in an ultracold gas are correlated at short inter-atomic distances due to threshold effects where the potential energy of their interaction dominates the kinetic energy. The correlations manifest themselves in a distinct nodal structure of the density matrix at short inter-atomic distances. Pump-probe spectroscopy has recently been suggested [Phys. Rev. Lett. 103, 260401 (2009)] to probe these pair correlations: A suitably chosen, short photoassociation laser pulse depletes the ground state pair density within the photoassociation window, creating a non-stationary wave packet in the …
This theoretical paper investigates the formation of ground state molecules from ultracold cesium atoms in a two-color scheme. Following previous work on photoassociation with chirped picosecond pulses [Luc-Koenig et al., Phys. Rev. A {\bf 70}, 033414 (2004)], we investigate stabilization by a second (dump) pulse. By appropriately choosing the dump pulse parameters and time delay with respect to the photoassociation pulse, we show that a large number of deeply bound molecules are created in the ground triplet state. We discuss (i) broad-bandwidth dump pulses which maximize the probability to f…
Photoassociation of ultracold atoms induced by chirped picosecond pulses is analyzed in a non-perturbative treatment by following the wavepackets dynamics on the ground and excited surfaces. The initial state is described by a Boltzmann distribution of continuum scattering states. The chosen example is photoassociation of cesium atoms at temperature T=54 $μK$ from the $a^3 Σ_u^+(6s,6s)$ continuum to bound levels in the external well of the $0_g^-(6s+6p_{3/2})$ potential. We study how the modification of the pulse characteristics (carrier frequency, duration, linear chirp rate and intensity) ca…
This theoretical paper presents numerical calculations for photoassociation of ultracold cesium atoms with a chirped laser pulse and detailed analysis of the results. In contrast with earlier work, the initial state is represented by a stationary continuum wavefunction. In the chosen example, it is shown that an important population transfer is achieved to $\approx 15$ vibrational levels in the vicinity of the v=98 bound level in the external well of the $0_g^-(6s+6p_{3/2})$ potential. Such levels lie in the energy range swept by the instantaneous frequency of the pulse, thus defining a ``phot…
We analyze the formation of Rb_2 molecules with short photoassociation pulses applied to a cold Rb-85 sample. A pump laser pulse couples a continuum level of the ground electronic state X ^1Σ_{g}^+ with bound levels in the 0_{u}^+ (5S+5P_{1/2}) and 0_{u}^+ (5S+5P_{3/2}) vibrational series. The nonadiabatic coupling between the two excited channels induces time-dependent beatings in the populations. We propose to take advantage of these oscillations to design further laser pulses that probe the photoassociation process via photoionization or that optimize the stabilization in deep levels of the…
Two-color photoassociation of ground state $^6$Li$^{87}$Rb molecules via the $\mathrm{B}^1Π$ electronic state using short pulses near a magnetic Feshbach resonance is studied theoretically. A near-resonant magnetic field is applied to mix the hyperfine singlet and triplet components of the initial wave function and enhance the photoassociation rate, before the population is transferred to the ground state by a second pulse. We show that an increase of up to three orders of magnitude in the absolute number of molecules produced is attainable for deeply bound vibrational levels. This technique c…
Utilizing single-photon photoassociation, we have achieved ultracold rubidium molecules with a high number density that provides a new efficient approach toward molecular quantum degeneracy. A new detection mechanism for ultracold molecule utilizing the inelastic atom-molecule collision is demonstrated. The resonant coupling effect on the formation of the ${\rm X^1Σ^+_g}$ ground state ${\rm ^{85}Rb_2}$ allows for a sufficient number of more deeply bound ultracold molecules, which induced an additional trap loss and heating of the co-existing atoms owing to the inelastic atom-molecule collision…
We model the formation of stable heteronuclear molecules via pulsed Raman photoassociation of a two-component Bose-Einstein condensate near a strong Feshbach resonance, for both counterintuitive and intuitive pulse sequencing. Compared to lasers alone, weak Raman photoassociation is enhanced by as much as a factor of ten (five) for a counterintuitive (intuitive) pulse sequence, whereas strong Raman photoassociation is barely enhanced at all--regardless of pulse sequence. Stronger intra-atom, molecule, or atom-molecule collisions lead to an expected decrease in conversion efficiency, but strong…
The paper investigates cold molecules formation in the photoassociation of two cold atoms by a strong laser pulse applied at short interatomic distances, which lead to a molecular dynamics taking place in the light-induced (adiabatic) potentials. A two electronic states model in the cesium dimer is used to analyse the effects of this strong coupling regime and to show specific results: i) acceleration of the ground state population to the inner zone due to a non-impulsive regime of coupling at short and intermediate interatomic distances; ii) formation of cold molecules in strongly bound level…
We develop the theory for the Adiabatic Raman Photoassociation (ARPA) of ultracold atoms to form ultracold molecules in the presence of scattering resonances. Based on a computational method in which we replace the continuum with a discrete set of "effective modes", we show that the existence of resonances greatly aids in the formation of deeply bound molecular states. We illustrate our general theory by computationally studying the formation of $^{85}$Rb$_2$ molecules from pairs of colliding ultracold $^{85}$Rb atoms. The single-event transfer yield is shown to have a near-unity value for wid…
Two-photon photoassociation of hot magnesium atoms by femtosecond laser pulses, creating electronically excited magnesium dimer molecules, is studied from first principles, combining \textit{ab initio} quantum chemistry and molecular quantum dynamics. This theoretical framework allows for rationalizing the generation of molecular rovibrational coherence from thermally hot atoms [L. Rybak \textit{et al.}, Phys. Rev. Lett. {\bf 107}, 273001 (2011)]. Random phase thermal wave functions are employed to model the thermal ensemble of hot colliding atoms. Comparing two different choices of basis func…
Employing recent developed magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) combining cold atom, strong laser pulse, and ultrafast technologies, we study momentum distributions of the multiply ionized cold rubidium (Rb) induced by the elliptically polarized laser pulses (35 fs, $1.3 \times 10^{15}$ W/cm$^2$). The complete vector momenta of Rbn+ ions up to charge state n = 4 are recorded with extremely high resolution (0.12 a.u. for Rb$^+$). Variations of characteristic multi-bands displayed in momentum distributions, as the ellipticity varies from the linear to circular polariza…
We present a new mechanism contributing to the detection of photoassociated long-range Rydberg molecules via pulsed-field ionization: ionic products, created by the decay of a long-range Rydberg molecule, modify the excitation spectrum of surrounding ground-state atoms and facilitate the excitation of further atoms into Rydberg states by the photoassociation light. Such an ion-mediated excitation mechanism has been previously called "Coulomb anti-blockade". Pulsed-field ionisation typically doesn't discriminate between the ionization of a long-range Rydberg molecule and an isolated Rydberg ato…
We have measured the radiative lifetimes of ns, np and nd Rydberg states of rubidium in the range 28 < n < 45. To enable long-lived states to be measured, our experiment uses slow-moving Rb atoms in a magneto-optical trap (MOT). Two experimental techniques have been adopted to reduce random and systematic errors. First, a narrow-bandwidth pulsed laser is used to excite the target Rydberg state, resulting in minimal shot-to-shot variation in the initial state population. Second, we monitor the target state population as a function of time delay from the laser pulse using a short-duration, milli…
Revivals of optical coherence of molecular photoassociation driven by two ultrashort laser pulses are addressed in the Condon approach. Based on textbook examples and numerical simulation of KrF excimer molecules, a prediction is made about an existence of photon echo on free-bound transitions. Delayed rise and fall of nonlinear polarization in the half-collisions are to be resulted from the resonant quantum states interference whether it be in gas, liquid or solid phases.
Optical Feshbach resonances [Phys. Rev. Lett. 94, 193001 (2005)] and pump-dump photoassociation with short laser pulses [Phys. Rev. A 73, 033408 (2006)] have been proposed as means to coherently form stable ultracold alkali dimer molecules. In an optical Feshbach resonance, the intensity and possibly frequency of a cw laser are ramped up linearly followed by a sudden switch-off of the laser. This is applicable to tightly trapped atom pairs. In short-pulse photoassociation, the pump pulse forms a wave-packet in an electronically excited state. The ensuing dynamics carry the wave-packet to short…
State-of-the-art {\em ab initio} techniques have been applied to compute the potential energy curves for the SrYb molecule in the Born-Oppenheimer approximation for the ground state and first fifteen excited singlet and triplet states within the coupled-cluster framework. The leading long-range coefficients describing the dispersion interactions at large interatomic distances are also reported. The electric transition dipole moments have been obtained as the first residue of the polarization propagator computed with the linear response coupled-cluster method restricted to single and double exc…
We use frequency-chirped light on the nanosecond time scale to produce ultracold $^{87}$Rb$_{2}$ molecules in the lowest triplet state via the process of photoassociation. Comparing to quantum simulations of the molecular formation, we conclude that coherent stimulated emission plays an important role and is primarily responsible for the significant difference observed between positive and negative chirps.
The photoionisation of rubidium in strong infra-red laser fields based on ab initio calculations was investigated. The bound and the continuum states are described with Slater orbitals and Coulomb wave packets, respectively. The bound state spectra were calculated with the variational method and we found it reproduced the experimental data within a few percent accuracy. Using the similar approach, ionisation of Rb was also successfully investigated. The effects of the shape and the parameters of the pulse to the photoionisation probabilities and the energy spectrum of the ionised electron are …
We present an experimental investigation of ultrafast-laser driven Rabi oscillations of atomic rubidium. Since the broadband spectrum of an ultrafast laser pulse simultaneously couples all the electronic hyperfine transitions between the excited and ground states, the complex excitation linkages involved with the D1 or D2 transition are energy degenerate. Here, by applying the Morris-Shore transformation, it is shown that this multi-state system is reduced to a set of independent two-state systems and dark states. In experiments performed by ultrafast laser interactions of atomic rubidium in t…
Nowadays the development of novel particle accelerators is a hot topic for both experimental and theoretical sciences. In the CERN-AWAKE experiment electrons are accelerated in a cold rubidium plasma, generated by a short, intense laser pulse. We describe the corresponding photoionisation process with ab initio quantum mechanical calculations. In this paper we primarily investigate how the frequency chirping of the applied laser pulse influences the photoionisation. Secondarily we also study how the results of the numerical simulations depend on the shape of the envelope of the laser pulse. Ba…
We describe experiments and associated quantum simulations involving the production of ultracold $^{87}$Rb$_{2}$ molecules with nanosecond pulses of frequency-chirped light. With appropriate chirp parameters, the formation is dominated by coherent processes. For a positive chirp, excited molecules are produced by photoassociation early in the chirp, then transferred into high vibrational levels of the lowest triplet state by stimulated emission later in the chirp. Generally good agreement is seen between the data and the simulations. Shaping of the chirp can lead to a significant enhancement o…
Photoassociation with short laser pulses has been proposed as a technique to create ultracold ground state molecules. A broad-band excitation seems the natural choice to drive the series of excitation and deexcitation steps required to form a molecule in its vibronic ground state from two scattering atoms. First attempts at femtosecond photoassociation were, however, hampered by the requirement to eliminate the atomic excitation leading to trap depletion. On the other hand, molecular levels very close to the atomic transition are to be excited. The broad bandwidth of a femtosecond laser then a…
We investigate pump-dump photoassociation of ultracold molecules with amplitude- and phase-modulated femtosecond laser pulses. For this purpose a perturbative model for the light-matter interaction is developed and combined with a genetic algorithm for adaptive feedback control of the laser pulse shapes. The model is applied to the formation of 85Rb2 molecules in a magneto-optical trap. We find for optimized pulse shapes an improvement for the formation of ground state molecules by more than a factor of 10 compared to unshaped pulses at the same pump-dump delay time, and by 40% compared to uns…
We demonstrate that a near-dissociation photoassociation resonance can be used to create a deeply bound molecular sample of ultracold NaCs. To probe the resulting vibrational distribution of the sample, we use a new technique that can be applied to any ultracold molecular system. We utilize a tunable pulsed dye laser to produce efficient spectroscopic scans ($\sim700$ cm$^{-1}$ at a time) in which we observe the $1^{1} Σ^{+}\rightarrow 2^{1}Σ^{+}-2^{3}Π$ vibrational progression, as well as the dissociation limit to the Cs 6$^{2}$P$_{3/2}$ asymptote. We assign $1^{1} Σ^{+}$$(\emph{v}$ = 4, 5, 6…
We discuss the production of ultracold molecules in their electronic ground state by photoassociation employing electronically excited states with ion-pair character and strong spin-orbit interaction. A short photoassociation laser pulse drives a non-resonant three-photon transition for alkali atoms colliding in their lowest triplet state. The excited state wave packet is transferred to the ground electronic state by a second laser pulse, driving a resonant two-photon transition. After analyzing the transition matrix elements governing the stabilization step, we discuss the efficiency of popul…
An experimental realization of high-precision direct frequency comb spectroscopy using counter-propagating femtosecond pulses on two-photon atomic transitions is presented. Doppler broadened background signal, hampering precision spectroscopy with ultrashort pulses, is effectively eliminated with a simple pulse shaping method. As a result, all four 5S-7S two-photon transitions in a rubidium vapor are determined with both statistical and systematic uncertainties below 10$^{-11}$, which is an order of magnitude better than previous experiments on these transitions.
We consider the leakage suppression problem of a three-level system in which the first two levels are the qubit system and the third, weakly-coupled to the second, is the leakage state. We show that phase- and amplitude-controlled two (three) pulses are sufficient for arbitrary qubit controls from the ground (an arbitrary) initial state, with leakage suppressed up to the first order of perturbation without additional pulse-area cost. A proof-of-principle experiment was performed with shaped femtosecond optical pulses and atomic rubidium showing a good agreement with the theory.
We report on coherent control of excitation processes of translationally ultracold rubidium dimers in a magneto-optical trap by using shaped femtosecond laser pulses. Evolution strategies are applied in a feedback loop in order to optimize the photoexcitation of the Rb2 molecules, which subsequently undergo ionization or fragmentation. A superior performance of the resulting pulses compared to unshaped pulses of the same pulse energy is obtained by distributing the energy among specific spectral components. The demonstration of coherent control to ultracold ensembles opens a path to actively i…
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…
Experiments on the spectroscopy of the Förster resonance Rb(37P)+Rb(37P) -> Rb(37S)+Rb(38S) and microwave transitions nP -> n'S, n'D between Rydberg states of cold Rb atoms in a magneto-optical trap have been performed. Under ordinary conditions, all spectra exhibited a 2-3 MHz line width independently of the interaction time of atoms with each other or with microwave radiation, although the ultimate resonance width should be defined by the inverse interaction time. Analysis of the experimental conditions has shown that the main source of the line broadening was the inhomogeneous electric fiel…
We propose and demonstrate the method of population transfer by piecewise adiabatic passage between two quantum states. Coherent excitation of a two-level system with a train of ultrashort laser pulses is shown to reproduce the effect of an adiabatic passage, conventionally achieved with a single frequency-chirped pulse. By properly adjusting the amplitudes and phases of the pulses in the excitation pulse train, we achieve complete and robust population transfer to the target state. The effect is demonstrated experimentally by observing piecewise excitation of Rubidium atoms from 5s_1/2 to 5p_…
We have performed high resolution photoassociation spectroscopy of rubidium ultra long-range Rydberg molecules in the vicinity of the 25$P$ state. Due to the hyperfine interaction in the ground state perturber atom, the emerging mixed singlet-triplet potentials contain contributions from both hyperfine states. We show that this can be used to induce remote spin-flips in the perturber atom upon excitation of a Rydberg molecule. When furthermore the spin-orbit splitting of the Rydberg state is comparable to the hyperfine splitting in the ground state, the orbital angular momentum of the Rydberg …
Collective resonance of interacting particles has important implications in many-body quantum systems and their applications. Strong interactions can lead to a blockade that prohibits the excitation of a collective resonance of two or more nearby atoms. However, a collective resonance can be excited with the presence of weak interaction and has been observed for atoms in the first excited state ($P$ states). Here, we report the observation of collective resonance of rubidium atoms in a higher excited state ($D$ states) in addition to the first excited state. The collective resonance is excited…
We demonstrate the storage of $5$ ns light pulses in a single rubidium atom coupled to a fiber-based optical resonator. Our storage protocol addresses a regime beyond the conventional adiabatic limit and approaches the theoretical bandwidth limit. We extract the optimal control laser pulse properties from a numerical simulation of our system and measure storage efficiencies of $(8.2\pm 0.6)~\%$, in close agreement with the maximum expected efficiency. Such well-controlled and high-bandwidth atom-photon interfaces are key components for future hybrid quantum networks.
Two-photon ionization of Rubidium atoms in a magneto-optical trap and a Bose-Einstein condensate (BEC) is experimentally investigated. Using 100 ns laser pulses, we detect single ions photoionized from the condenstate with a 35(10)% efficiency. The measurements are performed using a quartz cell with external electrodes, allowing large optical access for BECs and optical lattices.
We investigate the possibility of forming deeply bound ultracold RbCs molecules by a two-color photoassociation experiment. We compare the results with those for Rb_2 in order to understand the characteristic differences between heteronuclear and homonuclear molecules. The major differences arise from the different long-range potential for excited states. Ultracold 85Rb and 133Cs atoms colliding on the X^1Sigma+ potential curve are initially photoassociated to form excited RbCs molecules in the region below the Rb(5S) + Cs(6P_1/2) asymptote. We explore the nature of the Omega=0^+ levels in thi…
It is well known that area pulses make Rabi oscillation and chirped pulses in the adiabatic interaction regime induce complete population inversion of a two-state system. Here we show that chirped zero-area pulses could engineer an interplay between the adiabatic evolution and Rabi-like oscillations. In a proof-of-principle experiment utilizing spectral chirping of femtosecond laser pulses with a resonant spectral hole, we demonstrate that the chirped zero-area pulses could induce, for example, complete population inversion and return of the cold rubidium atom two-state system. Experimental re…
The effects of high pulse intensity and chirp on two-dimensional electronic spectroscopy signals are experimentally investigated in the highly non-perturbative regime using atomic rubidium vapor as clean model system. Data analysis is performed based on higher-order Feynman diagrams and non-perturbative numerical simulations of the system response. It is shown that higher-order contributions may lead to a fundamental change of the static appearance and beating-maps of the 2D spectra and that chirped pulses enhance or suppress distinct higher-order pathways. We further give an estimate of the t…
Calculations relating to two experiments that demonstrate coherent control of preformed rubidium-85 molecules in a magneto-optical trap using ultrafast laser pulses are presented. In the first experiment, it is shown that pre-associated molecules in an incoherent mixture of states can be made to oscillate coherently using a single ultrafast pulse. A mechanism that can transfer molecular population to more deeply bound vibrational levels is used in the second. Optimal parameters of the control pulse are presented for the application of the mechanism to molecules in a magneto-optical trap. The c…
We report on the combined action of a cw diode laser and a train of ultrashort pulses when each of them drives one step of the 5S-5P-5D two-photon transition in rubidium vapor. The fluorescence from the 6P_{3/2} state is detected for a fixed repetition rate of the femtosecond laser while the cw-laser frequency is scanned over the rubidium D_{2} lines. This scheme allows for a velocity selective spectroscopy in a large spectral range including the 5D_{3/2} and 5D_{5/2} states. The results are well described in a simplified frequency domain picture, considering the interaction of each velocity g…
We have developed two configurations of an echo interferometer that rely on standing wave excitation of a laser-cooled sample of rubidium atoms that measures acceleration. For a two-pulse configuration, the interferometer signal is modulated at the recoil frequency and exhibits a sinusoidal frequency chirp as a function of pulse spacing. For a three-pulse stimulated echo configuration, the signal is observed without recoil modulation and exhibits a modulation at a single frequency. The three-pulse configuration is less sensitive to effects of vibrations and magnetic field curvature leading to …
We investigate the dynamics of molecular photoexcitation by unchirped femtosecond laser pulses using RbCs as a model system. This study is motivated by a goal of optimizing a two-color scheme of transferring vibrationally-excited ultracold molecules to their absolute ground state. In this scheme the molecules are initially produced by photoassociation or magnetoassociation in bound vibrational levels close to the first dissociation threshold. We analyze here the first step of the two-color path as a function of pulse intensity from the low-field to the high-field regime. We use two different a…
We experimentally demonstrate two-photon absorption (TPA) with broadband down-converted light (squeezed vacuum). Although incoherent and exhibiting the statistics of a thermal noise, broadband down-converted light can induce TPA with the same sharp temporal behavior as femtosecond pulses, while exhibiting the high spectral resolution of the narrowband pump laser. Using pulse-shaping methods, we coherently control TPA in Rubidium, demonstrating spectral and temporal resolutions that are 3-5 orders of magnitude below the actual bandwidth and temporal duration of the light itself. Such properties…
We propose an improved photoassociation scheme to produce ultracold molecules in their vibronic ground state for the generic case where non-adiabatic effects facilitating transfer to deeply bound levels are absent. Formation of molecules is achieved by short laser pulses in a Raman-like pump-dump process where an additional near-infrared laser field couples the excited state to an auxiliary state. The coupling due to the additional field effectively changes the shape of the excited state potential and allows for efficient population transfer to low-lying vibrational levels of the electronic gr…
The two-photon transition $5S-5P-5D$ in rubidium vapor is investigated by detecting the fluorescence from the $6P_{3/2}$ state when the atomic system is excited by the combined action of a cw diode laser and a train of ultrashort pulses. The cw-laser plays a role as a velocity-selective filter and allows for a spectroscopy over a large spectral range including the $5D_{3/2}$ and $5D_{5/2}$ states. For a counterpropagating beam configuration, the response of each atomic velocity group is well characterized within the Doppler profile, and the excited hyperfine levels are clearly resolved. The co…
The complexity of ultrafast molecular photoionization presents an obstacle to the modelling of pump-probe experiments. Here, a simple optimized model of atomic rubidium is combined with a molecular dynamics model to predict quantitatively the results of a pump-probe experiment in which long range rubidium dimers are first excited, then ionized after a variable delay. The method is illustrated by the outline of two proposed feasible experiments and the calculation of their outcomes. Both of these proposals use Feshbach 87Rb2 molecules. We show that long-range molecular pump-probe experiments sh…
The chirped-pulse interaction in the adiabatic coupling regime induces cyclic permutations of the energy states of a three-level system in the $V$-type configuration, which process is known as the three-level chirped rapid adiabatic passage. Here we show that a spectral hole in a chirped pulse can turn on and off one of the two adiabatic crossing points of this process, reducing the system to an effective two-level system. The given hybrid adiabatic-nonadiabatic transition results in selective excitation of the three-level system, controlled by the laser intensity and spectral position of the …
We report an experimental demonstration of optical 2DCS in cold atoms. The experiment integrates a collinear 2DCS setup with a magneto-optical trap (MOT), in which cold rubidium (Rb) atoms are prepared at a temperature of about 200 $μ$K and a number density of $10^{10}$ cm$^{-3}$. With a sequence of femtosecond laser pulses, we first obtained one-dimensional second- and fourth-order nonlinear signals and then acquired both one-quantum and zero-quantum 2D spectra of cold Rb atoms. The capability of performing optical 2DCS in cold atoms is an important step toward optical 2DCS study of many-body…
