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arXiv:1307.8129 · Frontiers in Physics

Manipulating scattering of ultracold atoms with light-induced dissipation

Mikhail Lemeshko

Published Jan 1, 2013• 2 citations
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Abstract

Recently it has been shown that pairs of atoms can form metastable bonds due to non-conservative forces induced by dissipation [Lemeshko\&Weimer, Nature Comm. \textbf{4}, 2230 (2013)]. Here we study the dynamics of interaction-induced coherent population trapping -- the process responsible for the formation of dissipatively bound molecules. We derive the effective dissipative potentials induced between ultracold atoms by laser light, and study the time evolution of the scattering states. We demonstrate that binding occurs on short timescales of $\sim10~\mu$s, even if the initial kinetic energy of the atoms significantly exceeds the depth of the dissipative potential. Dissipatively-bound molecules with preordained bond lengths and vibrational wavefunctions can be created and detected in current experiments with ultracold atoms.

DOI
10.3389/fphy.2013.00017

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Recently it has been shown that pairs of atoms can form metastable bonds due to non-conservative forces induced by dissipation [Lemeshko&Weimer, Nature Comm. \textbf{4}, 2230 (2013)]. Here we study the dynamics of interaction-induced coherent population trapping -- the process responsible for the formation of dissipatively bound molecules. We derive the effective dissipative potentials induced between ultracold atoms by laser light, and study the time evolution of the scattering states. We demonstrate that binding occurs on short timescales of ∼10 μ\sim10~\mu∼10 μs, even if the initial kinetic energy of the atoms significantly exceeds the depth of the dissipative potential. Dissipatively-bound molecules with preordained bond lengths and vibrational wavefunctions can be created and detected in current experiments with ultracold atoms.
The establishment of robust laser-cooling techniques for the formation of ultracold atoms has provided a test-bed for low-temperature science, with scattering events changing character from incoherent thermal interactions to coherent quantum mechanical events. A natural extension is the pursuit of ultracold molecules in prescribed low-energy internal states. Atomic cooling techniques, however, do not generalize to the molecular regime due to the complex energy-level structure afforded by its extra degrees of motion. An indirect approach to ultracold molecule formation - photoassociation using ultrafast laser pulses - is the focus of this thesis. A broadband field associates atom pairs into a localized molecular wavepacket that evolves within the attractive excited-state potential. A suitably timed dump pulse may thus be applied to stabilize population into deeply bound ground vibrational states. This strategy may be generalized to any species whose spectroscopy matches the pulse spectrum, and offers a coherent population transfer scheme that does not require precise knowledge of the system. This thesis presents experiments using high-energy photoassociation pulses applied to ultracold rubidium atoms. The pulses quench the background ground-state molecular population but form bound dimers within the excited state. A pump-probe experiment was designed to chart the excited-state dynamics; however, the oscillations predicted by theoretical calculations were not evident in the molecular signal. The nature of the dynamics is expected to be strongly dependent on the initial state of the atom pairs addressed by the ultrafast pulse: a bound molecular population provides an additional candidate to free atoms. A spectroscopic measurement characterizes these bound molecules and identifies their formation mechanism. A subsequent experiment provides evidence that the predominant contributor to the pump-probe signal is the unbound initial population. The consequences with regard to both the observation of excited-state dynamics and the subsequent application of a dump pulse are discussed.
In this work, the coherence properties of the matter is studied in the frame of photoassociation of ultracold alkali atoms by using short and ultrashort laser pulses. Ultracold can be described with temperatures below 100 microK. When energy approaches the ultracold regime, quantum properties of matter becomes visible. In this regime matter such as atoms and molecules show wave properties. Coherent control employs the wave properties of matter to steer a physical process toward a desired target. It can be implemented with coherent radiation such as laser light. In particular, femtosecond laser pulses can be shaped. They thus have become a standard tool for coherent control. Since matter shows its wave properties most clearly at ultralow temperatures, ultracold matter represents the perfect object for coherent control. In the other hand using incoherent fields on ultracold matter does not give us good opportunities to drive quantum properties of it. In this work, it is aimed to bring together ultracold and ultrafast regimes in the frame of photoassociation. Photoassociation, excitation of two colliding atoms by laser light creates very weakly bound molecules. In the first part of this study, femtosecond photoassociation experiments are simulated. In these experiments and simulations, the broad spectrum of the femtosecond pulses addressing both atomic and molecular transitions is manipulated in a way to prevent the atomic transitions and to promote the molecular transitions. Then the effect of chirp and the effect of additional phase to the pulse are examined. Excited and ground state population are monitored by carrying out quantum dynamical simulations. The driving ultrafast dipole dynamics are presented. The photoassociation rate is limited by the low initial atomic pair density at inter-nuclear separations where photoassociation is feasible. In the second part of this study, a new scheme is proposed in order to manage this low pair density by manipulating the shape resonances of the initial atom pair. A shape resonance which is a metastable state occurs when some part of the wavefunction of partial waves with J > 0 trapped by a rotational barrier shows a bound structure in the closer internuclear distances where the rest of it shows a scattering wavefunction behavior. Most of the shape resonances in alkaline and alkaline earth metals occur typically at temperatures of a few milli-Kelvin. Therefore, the thermal weight of a shape resonance at photoassociation temperatures is quite small. By applying a non-resonant laser to the system the energy of the resonant state is brought close to the energies those corresponding to the photoassociation temperatures. Thus, the thermal weight of a shape resonance is amplified and initial pair density is enhanced. This effect is studied in both adiabatic and non-adiabatic time scales with respect to the rotational period of the system, intensity effects on the resonance energy and lifetime are presented.
The light scattered by cold atoms induces mutual optical forces between them, which can lead to bound states. In addition to the trapping potential, this light-induced interaction generates a velocity-dependent force which damps or amplifies the stretching vibrational mode of the two-atom ``molecule.'' This velocity-dependent force acts on time scales much longer than the mode period or the dipole dynamics, determining the true stability of the bound state. We show that, for two atoms, the stochastic heating due to spontaneous emission always exceeds the bounding effect, so pairs of cold atoms cannot be truly stable without an extra cooling mechanism.
Coherent femtosecond optical pulses provide a unique means to manipulate the collision process between a pair of ultracold atoms. The capability to arbitrarily shape strong electric fields gives the possibility of dynamically sculpting the system Hamiltonian on the collisional timescale. In this paper we explore theoretically physically intuitive excitation schemes by which a control field can manipulate the vibronic state populations in an ultracold molecular system, with the goal of bringing atom pairs to short ( R < 10 Å) separations where they may form a tightly bound molecule. The microscopic dynamics of individual pairs of colliding atoms under the influence of an external optical field are explored through explicitly time-dependent numerical simulations. The results provide physical justification for the employment of optimal control techniques for the achievement of state-selective formation of ultracold molecules.
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 levels of the ground state, where the population at the end of the pulse is much bigger than the population photoassociated in bound levels of the excited state; iii) the final momentum distribution of the ground state wavepacket keeping the signatures of the maxima in the initial wavefunction continuum. It is shown that the topology of the light-induced potentials plays an important role in dynamics.
In the ultracold regime, where the interactions between atoms become quantum mechanical in nature, we can investigate the fundamental properties of matter. A natural progression from the catalogue of pioneering experiments using ultracold atoms is to extend the size of our quantum system by producing ultracold molecules in prescribed low-energy internal states. Techniques for cold molecule production are split into two methods: direct and indirect cooling. While direct cooling methods have yet to realize ultracold temperatures, collisional relaxation in the molecules leads to low internal energy states. By contrast, indirect cooling — the association of molecules from pre-cooled atoms—has produced a range of molecules at ultracold temperatures; the challenge with this technique is to control the internal state.This thesis concentrates on a technique that is complementary to those already in existence: ultrafast photoassociation. Key to this technique is the formation of time non-stationary wavepackets in the excited-state in order to improve FranckCondon overlap of the excited state with deeply bound ground-state vibrational levels. A pump-probe experiment was designed and built to demonstrate the formation of bound excited-state dimers. In this work we show that the initial state from which the wavepacket originates is of critical importance to the evolution of excited-state population. We find that the internuclear separation of the wavepacket produced in a rubidium magneto-optical trap is too large to observe coherent oscillations in the excited state. The implications of this are discussed along with recommendations for future ultrafast photoassociation experiments. Consequently, a new ultracold atom apparatus was built utilizing magnetic and dipole-force trapping to increase the density of the atomic sample; this apparatus will enable future experiments combining the exciting fields of ultracold matter and ultrafast light.