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Chinese Physics B

Suppressing the weakly bound states in the photoassociation dynamics by using a frequency cut-off laser pulse

Feng Lin, Wei Zhang, Zeyu Zhao, Shu‐Lin Cong

Published Jul 1, 2012• 6 citations
Publisher

Abstract

The photoassociation dynamics of ultracold lithium atoms controlled by a cut-off pulse has been investigated theoretically by solving numerically the time-dependent Schrodinger equation using the mapped Fourier grid method. The frequency components of the laser pulse close to the atomic resonance are partly cut off. Compared with the typical Gauss-type pulses, the cut-off pulse is helpful to suppress efficiently the weakly bound states and prepare the associated molecules in the lower vibrational states. Especially, the dependence of photoassociation probability on the cut-off position of the laser pulse is explored.

DOI
10.1088/1674-1056/21/7/073203

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Suppressing the weakly bound states in the photoassociation dynamics by using a frequency cut-off laser pulse

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The photoassociation dynamics of ultracold lithium atoms controlled by a cut-off pulse has been investigated theoretically by solving numerically the time-dependent Schrodinger equation using the mapped Fourier grid method. The frequency components of the laser pulse close to the atomic resonance are partly cut off. Compared with the typical Gauss-type pulses, the cut-off pulse is helpful to suppress efficiently the weakly bound states and prepare the associated molecules in the lower vibrational states. Especially, the dependence of photoassociation probability on the cut-off position of the laser pulse is explored.
The photoassociation dynamics of ultracold lithium atoms controlled by a cut-off pulse has been investigated theoretically by solving numerically the time-dependent Schro¨dinger equation using the mapped Fourier grid method. The frequency components of the laser pulse close to the atomic resonance are partly cut off. Compared with the typical Gauss-type pulses, the cut-off pulse is helpful to suppress efficiently the weakly bound states and prepare the associated molecules in the lower vibrational states. Especially, the dependence of photoassociation probability on the cut-off position of the laser pulse is explored.
The formation of ultracold Cs 2 molecules via photoassociation (PA) with a spectral π-jump laser pulse is theoretically investigated by solving the time-dependent Schrödinger equation using the mapped Fourier grid method. Numerical calculations show that the population distributions of associated molecules mainly result from the off-resonant excitation of the π-jump laser pulse. Compared with the transform-limited pulse, an efficient population accumulation in the PA process is achieved with the π-jump pulse. An oscillation pattern appears in the population on the vibrational levels of the state owing to the action of the post-half-pulse in the π-jump pulse. The PA efficiency is related to the Rabi angle of the laser pulse. A π-jump pulse can be used to enhance more effectively the PA efficiency than a transform-limited pulse with the same Rabi angle.
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 cut-off position and chirp of the pulse. Molecule formation in the electronically excited state is attributed to off-resonant excitation in the strong-field regime.
The photoassociation (PA) dynamics of ultracold cesium atoms steered by the picosecond laser pulse with cubic-phase modulation has been investigated theoretically by solving numerically the time-dependent Schr\"odinger equation using the mapped Fourier grid method. The temporal duration of the pulse is prolonged, and the pulse area is enlarged by modulating the cubic phase. The PA efficiency is related to the pulse area. When the pulse area is larger than a certain value, the cubic-phase pulses noticeably enhance the PA efficiency, although they have lower energies.
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.
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 spectral cut position to the asymptotic transition frequency of the rubidium D1 or D2 lines, respectively. Measurements of the molecular photoassociation signal as a function of the pulse energy reveal a non-linear dependence and indicate a non-perturbative excitation process. Chirping the association laser pulse allowed us to change the phase of the coherent transients. Furthermore, a signature for molecules in the electronic ground state is found, which is attributed to molecule formation by femtosecond photoassociation followed by spontaneous decay. In a subsequent article [A. Merli et al., submitted] quantum mechanical calculations are presented, which compare well with the experimental data and reveal further details about the observed coherent transient dynamics.