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.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.

Jan 1, 20120 citations

Ultracold photoassociation spectroscopy: Long-range molecules and atomic scattering

K. M. Jones, Eite Tiesinga, Paul D. Lett +1 more

Photoassociation is the process in which two colliding atoms absorb a photon to form an excited molecule. The development of laser-cooling techniques for producing gases at ultracold $(<1\phantom{\rule{0.3em}{0ex}}\mathrm{mK})$ temperatures allows photoassociation spectroscopy to be performed with very high spectral resolution. Of particular interest is the investigation of molecular states whose properties can be related, with high precision, to the properties of their constituent atoms with the ``complications'' of chemical binding accounted for by a few parameters. These include bound long-range or purely long-range vibrational states in which two atoms spend most or all of their time at large internuclear separations. Low-energy atomic scattering states also share this characteristic. Photoassociation techniques have made important contributions to the study of all of these. This review describes what is special about photoassociation spectroscopy at ultracold temperatures, how it is performed, and a sampling of results including the determination of scattering lengths, their control via optical Feshbach resonances, precision determinations of atomic lifetimes from molecular spectra, limits on photoassociation rates in a Bose-Einstein condensate, and briefly, production of cold molecules. Discussions are illustrated with examples on alkali-metal atoms as well as other species. Progress in the field is already past the point where this review can be exhaustive, but an introduction is provided on the capabilities of photoassociation spectroscopy and the techniques presently in use.Photoassociation is the process in which two colliding atoms absorb a photon to form an excited molecule. The development of laser-cooling techniques for producing gases at ultracold $(<1\phantom{\rule{0.3em}{0ex}}\mathrm{mK})$ temperatures allows photoassociation spectroscopy to be performed with very high spectral resolution. Of particular interest is the investigation of molecular states whose properties can be related, with high precision, to the properties of their constituent atoms with the ``complications'' of chemical binding accounted for by a few parameters. These include bound long-range or purely long-range vibrational states in which two atoms spend most or all of their time at large internuclear separations. Low-energy atomic scattering states also share this characteristic. Photoassociation techniques have made important contributions to the study of all of these. This review describes what is special about photoassociation spectroscopy at ultracold temperatures, how it is performed, and a sampling of results including the determination of scattering lengths, their control via optical Feshbach resonances, precision determinations of atomic lifetimes from molecular spectra, limits on photoassociation rates in a Bose-Einstein condensate, and briefly, production of cold molecules. Discussions are illustrated with examples on alkali-metal atoms as well as other species. Progress in the field is already past the point where this review can be exhaustive, but an introduction is provided on the capabilities of photoassociation spectroscopy and the techniques presently in use.

Reviews of Modern PhysicsMay 22, 2006873 citations

Photoassociation of Ultracold Atoms: A New Spectroscopic Technique

William C. Stwalley, He Wang

Journal of Molecular SpectroscopyJun 1, 1999259 citations

Optical tuning of the scattering length of cold alkaline earth atoms

Eite Tiesinga, R. Ciuryło, Paul S. Julienne

Bulletin of the American Physical SocietyMar 23, 20053 citations

Intensity effects in ultracold photoassociation line shapes

Andrea Simoni, Paul S. Julienne, Eite Tiesinga +1 more

We derive ultracold atom-atom photoassociation line shapes valid for intense light fields and investigate laser power effects in sodium and rubidium photoassociation to the purely long-range ${0}_{g}^{\ensuremath{-}}$ symmetry state. We consider intensities up to a few hundreds ${\mathrm{W}/\mathrm{c}\mathrm{m}}^{2},$ a strongly saturating intensity for typical transitions of experimental interest. For these intensities the ${0}_{g}^{\ensuremath{-}}$ rotational spectrum is still well resolved; however, it is essential to couple the photoassociation resonance to both s- and d-wave ground-state channels. A low-energy d-wave shape resonance can have a profound effect on the line shape. Understanding the line shape is essential for precision spectroscopic analysis and could improve the extraction of ground-state scattering properties such as scattering lengths.We derive ultracold atom-atom photoassociation line shapes valid for intense light fields and investigate laser power effects in sodium and rubidium photoassociation to the purely long-range ${0}_{g}^{\ensuremath{-}}$ symmetry state. We consider intensities up to a few hundreds ${\mathrm{W}/\mathrm{c}\mathrm{m}}^{2},$ a strongly saturating intensity for typical transitions of experimental interest. For these intensities the ${0}_{g}^{\ensuremath{-}}$ rotational spectrum is still well resolved; however, it is essential to couple the photoassociation resonance to both s- and d-wave ground-state channels. A low-energy d-wave shape resonance can have a profound effect on the line shape. Understanding the line shape is essential for precision spectroscopic analysis and could improve the extraction of ground-state scattering properties such as scattering lengths.

Physical Review ADec 13, 200240 citations

Photoassociation is the process in which two colliding atoms absorb a photon to form an excited molecule. The development of laser-cooling techniques for producing gases at ultracold

(<1\phantom{\rule{0.3em}{0ex}}\mathrm{mK})

temperatures allows photoassociation spectroscopy to be performed with very high spectral resolution. Of particular interest is the investigation of molecular states whose properties can be related, with high precision, to the properties of their constituent atoms with the ``complications'' of chemical binding accounted for by a few parameters. These include bound long-range or purely long-range vibrational states in which two atoms spend most or all of their time at large internuclear separations. Low-energy atomic scattering states also share this characteristic. Photoassociation techniques have made important contributions to the study of all of these. This review describes what is special about photoassociation spectroscopy at ultracold temperatures, how it is performed, and a sampling of results including the determination of scattering lengths, their control via optical Feshbach resonances, precision determinations of atomic lifetimes from molecular spectra, limits on photoassociation rates in a Bose-Einstein condensate, and briefly, production of cold molecules. Discussions are illustrated with examples on alkali-metal atoms as well as other species. Progress in the field is already past the point where this review can be exhaustive, but an introduction is provided on the capabilities of photoassociation spectroscopy and the techniques presently in use.

{\mathrm{W}/\mathrm{c}\mathrm{m}}^{2},

a strongly saturating intensity for typical transitions of experimental interest. For these intensities the ${0}_{g}^{\ensuremath{-}}$ rotational spectrum is still well resolved; however, it is essential to couple the photoassociation resonance to both s- and d-wave ground-state channels. A low-energy d-wave shape resonance can have a profound effect on the line shape. Understanding the line shape is essential for precision spectroscopic analysis and could improve the extraction of ground-state scattering properties such as scattering lengths.