We demonstrate that judicious shaping of a nanosecond-time-scale frequency chirp can dramatically enhance the formation rate of ultracold $^{87}$Rb$_{2}$ molecules. Starting with ultracold $^{87}$Rb atoms, we apply pulses of frequency-chirped light to first photoassociate the atoms into excited molecules and then, later in the chirp, de-excite these molecules into a high vibrational level of the lowest triplet state, $a \, ^{3}Σ_{u}^{+}$. The enhancing chirp shape passes through the absorption and stimulated emission transitions relatively slowly, thus increasing their adiabaticity, but jumps quickly between them to minimize the effects of spontaneous emission. Comparisons with quantum simulations for various chirp shapes support this enhancement mechanism.
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.
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…
We demonstrate the ability to coherently control ultracold atomic Rb collisions using frequency-chirped light on the nanosecond time scale. For certain center frequencies of the chirp, the rate of inelastic trap-loss collisions induced by negatively chirped light is dramatically suppressed compared to the case of a positive chirp. We attribute this to a fundamental asymmetry in the system: an excited wavepacket always moves inward on the attractive molecular potential. For a positive chirp, the resonance condition moves outward in time, while for a negative chirp, it moves inward, in the same …
We implement a 4-level semiclassical model of a single pulse interacting with the hyperfine structure in ultracold rubidium aimed at control of population dynamics and quantum state preparation. We discuss a method based on pulse chirping to achieve population inversion between hyperfine states of the 5S shell. The results may prove useful for quantum operations with ultracold atoms.
A semiclassical, four-level model of a nanosecond, chirped pulse interacting with all optically accessible hyperfine states in the ultracold Rb atom is analyzed aiming at population inversion within $5S_{1/2}$ electronic state. The nature of two-photon adiabatic passage performed by such a single pulse having a bandwidth smaller than the hyperfine splitting of $5S_{1/2}$ state is investigated in the framework of the dressed state picture. It is shown that two dressed states are involved in the adiabatic dynamics of population inversion. The excited state manifold appeared to play an important …
We present results on coherent control of ultracold trap-loss collisions using 40 ns pulses of nonlinearly frequency-chirped light. The chirps, either positive or negative, sweep ~1 GHz in 100 ns and are centered at various detunings below the D2 line of 85Rb. At each center detuning, we compare the collisional rate constant beta for chirps that are linear in time, concave-down and concave-up. For positive chirps, we find that beta generally depends very little on the shape of the chirp. For negative chirps, however, we find that beta can be enhanced by up to 50(20)% for the case of the concav…
We report on the dynamics of ultracold collisions induced by near-resonant frequency-chirped light. A series of identical chirped pulses, separated by a variable delay, is applied to an ultracold sample of 85Rb, and the rate of inelastic trap-loss collisions is measured. For small detunings of the chirped light below the atomic resonance, we observe that the rate of collisions induced by a given pulse can be increased by the presence of an earlier pulse. We attribute this to the enhancement of short-range collisional flux by the long-range excitation of atom pairs to an attractive molecular po…
We have studied the effects of chirped femtosecond laser pulses on the formation of ultracold molecules in a Rb magneto-optical trap. We have found that application of chirped femtosecond pulses suppressed the formation of 85Rb-2 and 87Rb-2 lowest triplet state molecules in contrast to comparable non-chirped pulses, cw illumination, and background formation rates. Variation of the amount of chirp indicated that this suppression is coherent in nature, suggesting that coherent control is likely to be useful for manipulating the dynamics of ultracold quantum molecular gases.
When a gas of ultracold atoms is suddenly illuminated by light that is nearly resonant with an atomic transition, the atoms cannot respond instantaneously. This non-instantaneous response means the gas is initially more transparent to the applied light than in steady-state. The timescale associated with the development of light absorption is set by the atomic excited state lifetime. Similarly, the index of refraction in the gas also requires time to reach a steady-state value, but the development of the associated phase response is expected to be slower than absorption effects. Faraday rotatio…
We describe a system for generating frequency-chirped and amplitude-shaped pulses on time scales from sub-nanosecond to ten nanoseconds. The system starts with cw diode-laser light at 780 nm and utilizes fiber-based electro-optical phase and intensity modulators, driven by an arbitrary waveform generator, to generate the shaped pulses. These pulses are subsequently amplified to several hundred mW with a tapered amplifier in a delayed double-pass configuration. Frequency chirps up to 5 GHz in 2 ns and pulse widths as short as 0.15 ns have been realized.
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…
The influence has been studied of the ionization laser polarization on the effective temperature of an ultracold electron source, which is based on near-threshold photoionization. This source is capable of producing both high-intensity and high-coherence electron pulses, with applications in for example electron diffraction experiments. For both nanosecond and femtosecond photoionization, a sinusoidal dependence of the temperature on polarization angle has been found. For most experimental conditions, the temperature is minimal when the polarization coincides with the direction of acceleration…
We describe a method for controlling many-body states in extended ensembles of Rydberg atoms, forming crystalline structures during laser excitation of a frozen atomic gas. Specifically, we predict the existence of an excitation number staircase in laser excitation of atomic ensembles into Rydberg states. Each step corresponds to a crystalline state with a well-defined of regularly spaced Rydberg atoms. We show that such states can be selectively excited by chirped laser pulses. Finally, we demonstarte that, sing quantum state transfer from atoms to light, such crystals can be used to create c…
An ultracold wave packet of bosonic atoms loaded into a travelling laser wave may form a many-atom soliton.This is disturbed by a homogeneous force field, for example by the inevitable gravitation. The wave packet is accelerated and therefore the laser frequency appears to be chirped in the rest frame of the atoms. We derive the effective nonlinear Schrödinger equation. It shows a time dependent nonlinearity coefficient which amounts to a damping or antidamping, respectively. The accelerated packet solution remains a soliton which changes its shape adiabatically. Similarly, an active shaping c…
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…
A method for creation of ultracold molecules by stepwise adiabatic passage from the Feshbach state to the fundamentally ground state using an optical frequency comb is presented within a semiclassical multilevel model. The sinusoidal modulation of the spectral phase of the comb is implemented that leads to a creation of a quasi-dark dressed state having an insignificant population of the excited state manifold and, thus, efficiently mitigating decoherence in the system. In contrast, the cosine modulation does not lead to the quasi-dark state formation. The results demonstrate the importance of…
We have studied the formation of ultracold RbSr molecules with laser pulses. After discussing the advantages of the Mott insulator phase for the control with pulses, we present two classes of strategies. The first class involves two electronic states. Two extensions of stimulated Raman adiabatic passage (STIRAP) for multi-level transitions are used : alternating STIRAP (A-STIRAP) and straddle STIRAP (S-STIRAP). Both transfer dynamics are modeled and compared. The second class of strategies involves only the electronic ground state and uses infrared (IR)/TeraHertz (THz) pulses. The chemical bon…
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…
Measurements of the electron's electric dipole moment (eEDM) are demanding tests of physics beyond the Standard Model. We describe how ultracold YbF molecules could be used to improve the precision of eEDM measurements by two to three orders of magnitude. Using numerical simulations, we show how the combination of magnetic focussing, two-dimensional transverse laser cooling, and frequency-chirped laser slowing, can produce an intense, slow, highly-collimated molecular beam. We show how to make a magneto-optical trap of YbF molecules and how the molecules could be loaded into an optical lattice…
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.
An accurate measurement of the bunching of photons in the fluorescent emission from an ultracold ensemble of thermal 87Rb atoms in a steady-state magneto-optical trap is presented. Time-delayed-intensity-interferometry (TDII) performed with a 5-nanosecond time resolution yielded a second-order intensity correlation function that has the ideal value of 2 at zero delay, and that shows coherent Rabi oscillations of upto 5 full periods - much longer than the spontaneous emission lifetime of the excited state of Rb. The oscillations are damped out by ~150ns, and thereafter, as expected from a therm…
We discuss femtosecond Raman type techniques to control molecular vibrations, which can be implemented for internal state cooling from Feshbach states with the use of optical frequency combs with and without modulation. The technique makes use of multiple two-photon resonances induced by optical frequencies present in the comb. It provides us with a useful tool to study the details of molecular dynamics at ultracold temperatures. In our theoretical model we take into account decoherence in the form of spontaneous emission and collisional dephasing in order to ascertain an accurate model of the…
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…
