We will report here on our progress to manipulate the internal degree of freedom of the cold molecules, formed via photoassociation, by using a femtosecond laser. The idea is to use the broadband character of the laser to excite the formed molecules and to modify by optical pumping the vibrational distribution of the molecules. The control of this distribution could then be obtained by shaping the laser. The first experimental attempts have revealed a reduction of the number of detected cold molecules. Simple rate-equation models of the dynamics have shown that optical pumping can be the predominant process: a sequence of femtoconde pulses modifying the distribution of the vibration levels. Using a REMPI molecular detection scheme we experimentally investigate the dynamics of the molecules after absorption of one femtoseconde laser photon: photoionization, (pre-)dissociation, or optical pumping with transfer of the molecules towards non detected molecules ? The next step would be to find and to optimize an interaction scheme in order to create molecules with a lower vibrational excitation, and ultimately with no vibration.
[1] "Bulk Bogoliubov excitations in a Bose-Einstein condensate", R. Ozeri, N. Katz, J. Steinhauer, and N. Davidson, Rev. of Mod. Phys. 77, 187 (2005).
Firstly, we will perform ionization studies of the fundamental three-electron system lithium by various projectiles ranging from intense laser pulses, synchrotron and free-electron-laser radiation to electrons and ions. Here results will be presented for ionization of lithium in intense laser pulses of 8 fs and 30 fs duration for the Li(2s) ground state and a mixture of Li(2s) and Li(2p) states. Pump-probe experiments with two 10 fs-laser pulses show momentum spectra which periodically change with the delay time between the pulses. This behaviour can be traced back to a coherent superposition of different states excited in the first laser pulse. In future we plan to do photo-association studies producing lithium dimers using pump-dump schemes with short laser pulses. Furthermore, a cold atomic ensemble produced in a MOT is the first step on the way to the production of a ultra-cold quantum gas. Implementation of a dipole trap would allow to reach temperatures typical for a BECs or a cold Fermi gases.
*work done in collaboration with M.J. Wright, J.A. Pechkis, J.L. Carini, C.E. Rogers III, S. Kallush, and R. Kosloff, and supported by DOE.
The main goal of this talk will be to outline the prospect for cold controlled chemistry. I will present our work on quantum dynamics of molecules at cold and ultracold temperatures in the presence of static and laser electromagnetic fields. The kinetic energy of molecules at subKelvin temperatures is smaller than perturbations due to interactions with external electric or magnetic fields available in the laboratory. External fields may therefore be used to induce dissociation of weakly bound molecules [2], stimulate forbidden electronic transitions and control dynamics of cold atoms and molecules in a variety of ways [3]. I will present our recent work on mechanisms of manipulating and controlling dynamics of cold molecules with external fields. In particular, I will discuss the possibility of using electric fields to induce Feshbach resonances [4, 5] in ultracold gases, to manipulate electron spin degrees of freedom of cold molecules [6] and to modify chemical reactions. I will describe interactions of molecules in a microwave laser cavity and show that microwave fields may alter the dynamics of molecular collisions at low temperatures. Finally, I will demonstrate that confining the motion of ultracold molecules to two dimensions, as can now routinely be done with ultracold atoms, may suppress inelastic collisions and chemical reactions at ultracold temperatures [7].
References:
[1] R. V. Krems, "Set for collision course", Nature Physics 3, 77 (2007).
[2] R. V. Krems, "Breaking van der Waals molecules with magnetic fields", Phys. Rev. Lett. 93, 013201 (2004).
[3] R. V. Krems, "Molecules near absolute zero and external field control of atomic and molecular dynamics", Int. Rev. Phys. Chem. 24, 99 (2005).
[4]. R. V. Krems, "Controlling collisions of ultracold atoms with dc electric fields", Phys. Rev. Lett. 96, 123202 (2006).
[5] Z. Li and R. V. Krems, Phys. Rev. A 75, 032709 (2007).
[6] T. V. Tscherbul and R. V. Krems, "Controlling electronic spin-relaxation of cold molecules with electric fields", Phys. Rev. Lett. 97, 083201 (2006).
[7] Z. Li, S. V. Alyabishev, R. V. Krems, "Ultracold Inelastic Collisions in Two Dimensions", to be published.
Closed loop optimizations on alkali dimers in a supersonic beam are first demonstrated for maximization of the ionization yield. Next, isotopomer selective optimizations are presented to examine the efficiency of the optimization procedure for the weak differences between the isotopic species. Surprisingly large enrichment factors are found and information about the dynamics on the involved vibrational states is extracted from the optimal pulse shapes, which provides a new spectroscopical approach of yielding distinct frequency pattern on fs-time scales. The experiments are compared with optimal control calculations in order to decipher the underlying processes in detail.
A main aspect of this contribution is the development of novel pulse shaping and optimal control methods. A major goal of this approach is to extract the most relevant information from the optimized laser field and hence to aid the interpretation. Moreover, novel pulse shaper schemes for combined phase, amplitude, and polarization pulse control were designed and applied on alkali dimers, even in a parametric encoding. The results demonstrate the perspectives of adding a new dimension by including also the polarization and hence all properties of the light field in the pulse modulation.
Currently, coherent control was applied to ultracold trapped ensembles motivated by the perspective to perform photoassociation and photostabilization of alkali systems. First results are received regarding optimized multi-photonic excitation to molecular ions and pump-probe experiments exposing signal oscillations. They provide indications for photoassociation and open the perspective for transitions to lower vibrational levels in the electronic ground state, which would be a first step to an internally cold molecular Bose Einstein condensate.
In the ultracold regime, the initial state has to be a s-wave stationary scattering wavefunction describing a pair of colliding atoms. Two methods for performing the Boltzmann average have been implemented [4]. Recently, we have investigated [5] how the pulse is carving out a dynamical hole in the pair probability density. Considering photoassociation into loosely bound levels of Cs2 0g-(6P3/2), we analyze the depletion of the ground triplet state wavepacket and its evolution after the pulse. We show that, due to a "momentum kick", a significant flux of population is moving to short distances, at the timescale of the vibrational motion in the excited state. This compression effect markedly increases the pair density probability at short distances, so that photoassociation with a conveniently delayed red-detuned second pulse will populate deeply bound levels of Cs2 0g-(6P3/2). Another signature of the hole is the formation of correlated pairs of hot atoms.
In collaboration with Jordi Mur-Petit and Pascal Naidon [6], we study how short pulse photoassociation can probe the pair correlation function in an atomic condensate. Calculations are performed for a metastable helium condensate, where the correlated pairs of hot atoms are detected in the experiment of the Westbrook's group [7].
References:
[1] E. Luc-Koenig, R. Kosloff, F. Masnou-Seeuws and M. Vatasescu, Phys. Rev. A 70, 034414 (2004),
E. Luc-Koenig, M. Vatasescu and F. Masnou-Seeuws, Eur. Phys. J. D 31, 239-262 (2004).
[2] C. P. Koch, E. Luc-Koenig and F. Masnou-Seeuws, Phys. Rev. A 73, 033408 (2006).
[3] C. P. Koch, F. Masnou-Seeuws and R. Kosloff, Phys. Rev. A 73, 043409 (2006),
J. Mur-Petit, E. Luc-Koenig and F. Masnou-Seeuws, Phys. Rev. A 75, 061404(R) (2007).
[4] C. P. Koch, R. Kosloff, E. Luc-Koenig, F. Masnou-Seeuws and A. Crubellier, J. Phys. B 39, S1017 (2006).
[5] E. Luc-Koenig, F. Masnou-Seeuws and R. Kosloff, Phys. Rev. A 75, 054711 (2007).
[6] P. Naidon and F. Masnou-Seeuws, Phys. Rev. A73, 043611 (2006).
[7] M. Schellekens, R. Hoppeler, A. Perrin, J. Viana Gomes, D. Boiron, A. Aspect, C. Westbrook, Science 310, 648 (2005),
J. Jeltes et al., Nature 445, 402 (2007).
In a recent experiment, we have exploited this atom-photon entanglement in order to couple two single 171Yb atomic ions separated by one meter. The ions are simultaneously excited with an ultrafast pulse and the resulting two scattered photons are detected in an antisymmetric Bell state [5,6]. This projects the quantum state of the two ions in a likewise antisymmetric superposition state. We demonstrate entanglement using a photonic frequency qubit [3] as well as a polarization qubit [4] and fully characterize the produced entangled state using quantum state tomography. Even though this entanglement scheme is probabilistic, it allows for high fidelity entanglement that can be used as a resource for entangling larger numbers of qubits or for the propagation of quantum information over very large distances. .
[1] J.J. Garcia-Ripoll, P. Zoller, and J. I. Cirac, Phys. Rev. Lett.
91, 157901 (2003)
[2] L.-M. Duan, Phys. Rev. Lett. 93, 100502 (2004).
[3] M. J. Madsen, et. al., Phys. Rev. Lett. 97, 040505 (2006).
[4] B. B. Blinov, et. al., Nature 428, 153 (2004).
[5] C. Simon and W.T.M. Irvine, Phys. Rev. Lett. 91, 110405 (2003)
[6] D.L. Moehring et al., Nature 449, 68 (2007)
In the talk, I will show that there are three regimes of photoassociation in a Bose-Einstein condensate, and that they all can be understood on the basis of time-dependent two-body theory. In particular, the rogue dissociation is not a many-body effect, but results from a "universal" transient response of individual atom pairs. Finally, I will illustrate how the three regimes could be observed by photoassociating condensates of alkaline-earth atoms.
As a starting point for the creation of ultracold polar molecules, we report on the creation of heteronuclear Feshbach molecules from an ultracold gas mixture of 40K-87Rb in an optical dipole trap. We create more than 30,000 molecules at about 200 nK. We have studied the inelastic loss of the molecules as a function of the heteronuclear scattering length and find that the quantum statistics of the particles involved in the collision has a dramatic effect on the loss rate of the Feshbach molecules in the optical dipole trap. In particular, we demonstrate that these weakly bound Feshbach molecules can be long-lived. The ensemble is therefore an excellent starting point for the application of transfer schemes into more deeply bound vibrational levels.
Towards this end, we report on one-photon spectroscopy to probe excited electronic states and and two-photon Raman spectroscopy to probe more deeply bound ground state vibration levels. We discuss prospects of reaching the ground state of the molecular system using coherent optical schemes.
References
[1] E.A. Shapiro, V. Milner, C. Menzel-Jones, and M. Shapiro,
Phys. Rev. Lett. 99: 033002 (2007)
[2] S. Zhdanovich, E.A. Shapiro, M. Shapiro, J.W. Hepburn, V. Milner,
arXiv:0710.3145v1 [physics.atom-ph].
[3] E.A. Shapiro, A. Pe'er, J. Ye, M. Shapiro,
arXiv:0710.5502v1 [quant-ph].
We investigated the behavior of Rb85 atoms trapped in a magneto optical trap (MOT) in the field of a sequence of counter-propagating frequency chirped short (in the range of ns) laser pulses for coherent manipulation in the adiabatic passage regime. Measurements at various chirp rates were carried out to find the region of the chirp and the intensity of the frequency modulated light pulses, where the adiabatic excitation and de-excitation gives the maximal force for the acceleration of the atoms without temperature increase.
The light pulses were generated by transmitting the frequency modulated light of a cw diode laser with sinusoidally modulated pump current through a Fabry-Perot (F-P) interferometer tuned to the resonance with the working transition. The central frequency of the diode laser was regulated around the resonance frequency of the spectral line by a dc bias current, resulting in variation of the rate of the frequency chirp of the light pulse transmitted by the F-P interferometer. The spatial displacement of the atomic cloud, which depends on the mechanical momentum transferred to the atoms as a result of interaction with a sequence of the frequency chirped laser pulses, was detected by the fluorescence of the Rb atoms. The displacement of the atoms in case of counter-propagating beams is measured to be larger than in case of a single beam only in a restricted interval of the chirp rate. Otherwise the ratio of the two beam/one beam displacement is fluctuating around 1 or is smaller than one. This result is in qualitative agreement with results of numerical simulations of the temporal behavior of populations of the hyperfine levels manifold of the D2 line of the Rb85 atom using a computer code based on solution of Bloch equations for density matrix elements taking into account spontaneous decay of the excited states.
Monte Carlo simulations for a two-level atom have shown that the momentum transferred to the atoms by a single counter-propagating partially overlapping pulse pair can be several times the value of non-overlapping chirped pulses. In certain parameter regions, the momentum transfer is accompanied by negligible heating of the atoms and they are returned to the ground state at the end of the interaction, avoiding the de-coherency effects initiated by the spontaneous decay of the excited state.
We investigated experimentally the mechanical effect of partially overlapping chirped pulse pairs for trapped Rb85 atoms. The experimentally observed displacement of the atomic packet agreed well with the theoretical prediction. For further investigations of such kind with a wider range of experimental parameters we are preparing chirped laser pulses in the ns range by using electro-optical modulators.
Unlike isotropic solitons predicted for the moments aligned with the confinement axis, no sign reversal of the dipole-dipole interaction is necessary to support the solitons. Direct 3D numerical simulations confirm the stability of the 2D solitons and suggest interesting dynamical effects in their rotation and collisions.
The preparation of ultracold ground state molecules is still challenging. One class of preparation strategies are optical methods, which have been enormously successful for atoms. Adapted versions of laser cooling, which try to optimize optical pumping into the molecular ground state, have been proposed [1], but their efficiency is limited by the absence of closed transitions in molecules. We present a theoretical approach [2,3] for the simulation of the cooling of internal and external molecular degrees of freedom in a cavity. The idea is to sequentially depopulate excited rovibrational levels by vacuum-stimulated Raman scattering into the mode of a high-finesse cavity. As model systems we choose the OH and the NO radicals. By using a combination of ab initio quantum chemical and experimental data we are able to determine the molecular properties needed for our cooling scheme. We discuss the details of the cooling process and predict the time scales needed to prepare a molecule in its ground state.
Molecules in their rotational and vibrational groundstate are suitable candidates for quantum computing [4]. Non-resonant stimulated Raman processes in the femtosecond regime are applied to implement quantum gates for vibrational qubits. One of the advantages of this idea, compared to our first approach in the IR regime [4], is the high flexibility in the choice of laser wavelengths in combination with well established shaping techniques in the visible frequency domain. The quantum gates can be optimized by a modified Krotov-OCT-scheme including restrictions on the laser fields in the frequency domain to assure simple pulse spectra. Stimulated Raman quantum gates are presented for a 2D-qubit system. Combination of both ideas might open a way to realize molecular quantum computing in the gas phase.
References
1. J.T. Bahns, W.C. Stwalley, and P.L. Gould, J. Chem. Phys. 104, 9689 (1996).
2. G. Morigi, P. W. H. Pinkse, M. Kowalewski and R. de Vivie-Riedle, Phys. Rev. Lett. 99, 073001 (2007).
3. M. Kowalewski, G. Morigi, P. W. H. Pinkse and R. de Vivie-Riedle, Appl. Phys. B, accepted.
4 C. Tesch, R. de Vivie-Riedle, Phys. Rev. Lett. 343, 633 (2002).
[1] W. Salzmann et al., submitted.
[2] W. Salzmann et al., Phys. Rev. A 73, (2006) 023414
[3] B. L. Brown et al., Phys. Rev. Lett. 96, (2006) 173002
[4] M. J. Wright et al., Phys. Rev. A, 75 (2007) 051401
[1] R. V. Krems, Int. Rev. Phys. Chem. 24, 99 (2005); P. F. Weck and N. Balakrishnan, Int. Rev. Phys. Chem. 25, 283 (2006)
[2] P. Staanum, S. D. Kraft, J. Lange, R. Wester, M. Weidemüller, Phys. Rev. Lett. 96, 023201 (2006); N. Zahzam, T. Vogt, M. Mudrich, D. Comparat, P. Pillet, Phys. Rev. Lett. 96, 023202 (2006)
[3] S. D. Kraft, P. Staanum, J. Lange, L. Vogel, R. Wester, M. Weidemüller, J. Phys. B 39, S993 (2006)
We investigate the effects of a strong static electric field on the rovibrational spectra of diatomic heteronuclear molecules in their electronic ground state. A full rovibrational approach was developed including the coupling of the vibrational and rotational motions and taking into account the dependence of the electric dipole moment on the internuclear distance. For several alkali dimers, LiCs, KRb and RbCs [1-3], a detailed analysis of the impact of the electric field is performed: the hybridized and oriented rotational motion, the mixing of angular momenta and the squeezing of the vibrational motion. In addition, we will discuss the formation of ultracold molecules via stimulated emission followed by a radiative deexcitation cascade in the presence of a static electric field [4,5]. Taking as an example the LiCs, the dependence of the corresponding cross section on the final rovibrational bound state, on the energy of the continuum, and also on the static electric field strength are analyzed in detail. We consider the cold and ultracold regime where transitions from s-wave are the dominant, which means that in absence of the static electric field only bound states with angular momentum equal to one are populated. We will show that in the presence of the static electric field transitions to bound states evolving from field-free levels with zero angular momentums become possible. Hence, we demonstrate the possibility to populate the lowest rotational excitations via photoassociation. The modification of the radiative cascade due to the electric field leads to narrow rotational state distributions in the vibrational ground state. External fields might therefore represent an additional valuable tool towards the ultimate goal of quantum state preparation of molecules.
[1] R. Gonzalez-Ferez, M. Mayle, and P. Schmelcher, Chemical Physics 329
(2006) 203-215.
[2] M. Mayle, R. Gonzalez-Ferez, and P. Schmelcher, Physical Review A 75
(2007) 013421.
[3] P. Sanchez-Moreno, M. Mayle, R. Gonzalez-Ferez, and P. Schmelcher, in
preparation (2007).
[4] R. Gonzalez-Ferez, M. Mayle, and P. Schmelcher, Europhys. Lett. 78,
53001 (2007).
[5] R. Gonzalez-Ferez, M. Weidemueller, and P. Schmelcher, Physical Review
A
76, 023402 (2007).
Details of the apparatus housing the Rb and Cs magneto optical trap will be given, along with the femtosecond and detection laser systems. A compact time of flight mass spectrometer has been designed to offer both high resolution and excellent optical access to the MOT in the entire horizontal and one vertical plane. This design uses six independent rod electrodes, in a Wiley-McLaren configuration, and allows both the time focusing of the ions and the deflection of the unwanted atomic ions out of the ion detector.
The long term goal of our work is to produce efficiently molecules in their lowest electronic, vibrational and rotational states that can subsequently be held in optical or magnetic traps for long periods without collisional dissociation.
1. V. A. Yurovsky, M. Olshanii, and D. S. Weiss, Adv. At. Mol. Opt. Phys., 55, 61, (2007).
2. T. Kinoshita, T. R. Wenger, and D. S. Weiss, Nature, 440, 900, (2006).
3. V. A. Yurovsky, A. Ben-Reuven, and M. Olshanii, Phys. Rev. Lett, 96, 163201, (2006).
4. V. A. Yurovsky, physics/0703168; Phys. Rev. A (in press).
We report on producing nanosecond pulses of laser light whose frequency is arbitrarily chirped and whose amplitude is arbitrarily controlled. The chirp is achieved by sending the output from a 780 nm diode laser through a fiber-based electro-optical phase modulator within a fiber delay loop. Upon exiting the fiber, the light has accumulated the desired time-dependent phase. It then re-injection locks the diode laser, thus maintaining the high optical power. Larger phase modulations can be accumulated by using multiple passes through this loop, re-injection locking after each pass. We are able to produce arbitrary chirps by driving the phase modulator with an arbitrary waveform generator. Currently, we have been able to achieve chirp rates up to approximately 100 GHz/μs. To produce an arbitrary pulse amplitude, the light is sent through a fiber-based electro-optical amplitude modulator, driven with an arbitrary waveform generator. Using this technique, we have been able to achieve pulses as short as 4 ns FWHM. Such pulses will be useful in controlling collisions between ultracold Rb atoms.
[1] L.Chuntonov, L.Rybak, A.Gandman, and Z.Amitay,
arXiv:0709.0615
Population transfer to a target state or creation of a given coherent superposition of metastable states in multilevel quantum systems have numerous applications in the control of chemical reactions, improving efficiency of nonlinear processes in resonant media, quantum computing and processing of quantum and classical information, electromagnetically induced transparency, etc.
In this communication, we analyze possibilities of using ultrashort laser pulses with frequency chirp for effective and robust transfer of populations between the quantum states of multilevel systems (atoms or molecules) or creation of coherent superposition of these states.
The result of interaction of a short frequency chirped laser pulse with a two-level atom in the adiabatically following regime is well known: such pulse provides complete inversion of the atom at the end of the interaction. In more complex multilevel quantum systems, such pulses interact superposition of the working states and transfer the corresponding population to the target states leaving intact superposition of the states.
At the end of the interaction, one has population transferred to a target state along with a coherent superposition corresponding to superposition state left without change. An important peculiarity of such control of the states is that it depends on the relative phase of the interacting frequency-chirped laser pulses that provides a tool for governing the population transfer and induced coherence by varying the relative phase of the laser pulses.
Different schemes of the coherent control are considered including different structures of the working levels of the quantum systems: , V- and ladder- structured atoms and molecules. Among the considered schemes those ones are singled out that allow performing population transfer between metastable states or creation of coherent superposition of these states without appreciable excitation of the quantum system providing immunity of such schemes to decoherence due to the decay of the excited states. Such schemes are discussed in details in this communication.
The considered schemes are not sensitive to small-to-medium variations of the pulse area, speed of the frequency chirp or other parameters of the laser pulses and the quantum system. Because of no strict resonance conditions for the frequency chirped pulses, the proposed schemes are effective in media with homogeneously as well as inhomogeneously broadened transition lines.
[1] C. P. Koch, R. Kosloff and F. Masnou-Seeuws, Phys. Rev. A 73, 043409 (2006)
Based on our ab initio data we derived a system Hamiltonian which is suitable to describe the multidimensional dissociation process in a reduced reactive coordinate space [3]. Quantum dynamical calculations suggest that dissociation induced by a Fourier limited femtosecond laser pulse provides the ion pair as the main product in gas phase despite its higher potential energy. Selective addressability of the reaction channels by laser control will be discussed.
The light induced dissociation of the related diphenylmethane provides two different competing reaction channels, one of triplett formation and one of laser induced tunneling. Selective enhancement of the tunneling process offers the possibility to control the dissociation.
References
1. J. Bartl, S. Steenken, H. Mayr, and R.A. McClelland, J. Am. Chem. Soc. 112, 6918 (1990).
[1] D. Meshulach and Y. Silberberg, Nature (London) 396, 239 (1998); Phys. Rev. A 60, 1287 (1999).
Note: Implemented code uses REALISTIC potentials.
It is straitforward to study with implemented approach such
processes like phohoassociation
[for example we are authors of PRA76,022704].
We study the effect of decoherence on inter-particle entanglement and dynamical quantum depletion in the two-site Bose-Hubbard model of a Bose-Einstein condensate (BEC). Starting with the odd parity excited coherent state, the initial collisional loss of single particle coherence varies from small bound oscillations in the weak coupling regime, through hyperbolic depletion in the strong interaction regime, to a Gaussian decay under the pure collisional Hamiltonian.
The inclusion of pure phase noise, as in the continuous measurement of the relative number difference between the modes, is shown to enhance this quantum depletion. In comparison, the measurement of relative number between even and odd superpositions of the modes, slows down the loss of single-particle coherence. Decoherence can thus either restore or suppress quantum-field behavior, depending on the details of system-bath coupling and the overlap of decoherence pointer states with collisional-entanglement pointer states. The slowing down of collisional dephasing due to the coupling with the environment may be viewed as a many-body quantum-Zeno suppression of dynamical quantum depletion through continuous relative-number measurements. The extended effective decay times in the presence of projective measurement, are further enhanced with increasing number of particles N, by a bosonic factor of N/log(N).
*in collaboration with
with Toru Morishita, Anh-Thu Le, X. X. Zhou and Zhangjin Chen
[1] Toru Morishita, Anh-Thu Le, Zhangjin Chen and C. D.Lin,
Phys. Rev.Lett. (in press). Eprint:
arXiv:0707.3157
In order to describe interacting many-particle systems different
approaches have been developed over the years. A promising method is
the multi-configuration time-dependent Hartree-Fock (MCTDHF) method
which allows to systematically improve the accuracy of the
wavefunction from the Hartree-Fock level to the fully correlated
result. On this poster we discuss the combination of MCTDHF and
optimal control theory. Since the MCTDHF equations are nonlinear
equations, common optimal control algorithms for the Schroedinger
equation cannot be applied and nonlinear optimal control theory has to
be used.
Molecules formation at μK temperature range offer new opportunities and phenomena in chemistry, metrology, and even quantum physics. We will present an experimental progress of using an ultrafast laser system in conjunction with magneto optical trap recoil ion momentum spectroscopy (MOTRIMS) to investigate the products formed in the interaction of ultrafast laser pulses with cold trapped Rubidium atoms. We aim to produce cold molecular sample using femtosecond laser pulses for further investigations. The diagnostic system and the specific photo-association process will be described in detail. These investigations of molecular photo-association by femtosecond laser pulses contribute to the theoretical and experimental development which has impacts on new physics, chemistry and quantum computations.
References
[1] Y. Ohtsuki, G. Turinici and H. Rabitz, J. Chem Phys. 120, 5509 (2004).
Strings of laser cooled ions in a Paul trap provide a yet unmatched degree of quantum control[1].
The drawback of this concept lies in the limited scalability, which can be overcome by operating a microstructured array of Paul traps and shuttling the ions between different trap sites. The shuttling operations are carried out by dynamically changing the confining voltages at the trap segments.
They have to be fast, robust and should not contribute excess energy to the ion qubit as this would spoil subsequent quantum logic operations. This setting suggests the application of optimal control (OCT) techniques. We present numerical results showing that OCT should indeed make such shuttling operations possible[2].
Furthermore, quantum logic logic gates can benefit from OCT as well since achieving high fidelities is crucial for attaining the quantum error correction threshold. We demonstrate numerically that shaped pulse sequences obtained by OCT allow for the implicit compensation of parameter offsets. Analogously to NMR experiments, the logic operations can therefore be robustified[3,4].
[1] H.Häffner et al., Nature 438, 643 (2005)
[1] L.Rybak, L. Chuntonov, A. Gandman, N. Shakour, and Z. Amitay, http://arxiv.org/abs/arXiv:0710.1226
We investigate the rotational dynamics of heteronuclear diatomic molecules
possessing a $^1\Sigma^+$ electronic ground state exposed to a strong
external time-dependent homogeneous electric field. The switching on and
off of the electric field is performed by exponential functions. Due to
the large absolute value of its permanent electric dipole moment as well
as the availability of the corresponding potential energy curve [1] and
electric dipole moment function [2], as well as its current interest we
focus on the LiCs molecule. We analyze the orientation and hybridization
of the angular motion, together with the population of pendular and
rotational states in the constant field and field-free regimes, as the
switching times are modified. We concentrate on the rovibrational ground
state as initial wave packet and on the regime of maximal field strengths
F=51.4-514 kV/cm. The switching times are taken in the interval from 800
fs to 800 ps, which covers the time regime between short laser pulse
duration and switching dc-fields. The exact results are compared with
those of an N-mode approach to the rotational dynamics derived within the
effective rotor approximation [3]. We demonstrate that it is possible to
predict in a robust way the amount of pendular states or partial waves
needed to properly describe the rotational dynamics in the constant field
and final field-free regimes, respectively. However, we show that once the
field is off the specific contribution of a certain rotational level is
rather sensible to the characteristic of the process, especially to the
switching on and off times. The final wave packet shows a wide variety of
localization and orientation phenomena arranged in characteristic
patterns, which alternate between two angular hemispheres and are periodic
in time.
[1] P. Staanum, A. Pashov, H. Knöckel, and E. Tiemann, Phys. Rev. A 75,
042513 (2007).
We have realized a universal deterministic single ion
source on the basis of an ion trap applicable to a wide range of
elements and molecules[1]. Initially, ultra cold Ca
ion crystals are trapped within a segmented linear trap. Those
ions are then deterministically extracted and shot into a detector
at a distance of 25 cm from the trap. With single ions, more than
90% of these extractions were successful. The kinetic energy
distribution of the ions amounts to less than 0.1%. We have also
demonstrated the extraction of mixed crystals containing other
dopant ions. For the implantation with nm precision, we plan to
utilize an electrostatic Einzel-lens to further improve the
spatial resolution of the extracted ions. These can then be used
to generate color centers in diamond for optical detection or to
implant P into Si. Both systems provide the foundation for the
realization of a solid state quantum computer [2,3]. In addition,
the electrical properties of semiconductor devices can be greatly
enhanced by the deterministic implantation of single ions [4].
[1] J. Meijer et. al., Appl. Phys. A 83, 321 (2006).
We study the effect of tight confinement on the collective, stimulated dissociation of molecular Bose-Einstein condensates (BECs) into boson constituents. In contrast to thermal reactions where outcomes are set solely by local variables, the long coherence length in this stimulated process implies that global length-scales can become crucially important. When the characteristic trap size is small with respect to the resonance healing length, confinement leads to the elimination of unstable dissociation modes and thereby to the stabilization of the condensate. This effect is analogous to the stabilization of attractively-interacting BECs against collapse due to the trap potential. The shape of the condensate affects the critical Feshbach coupling frequency. Both single-channel [1] and two-channel [2] dissociation processes were considered, suggesting the possibility to control coherent dissociation by manipulation of the size and shape of the trapping potentials.
References
[1]I. Tikhonenkov and A. Vardi, Phys. Rev. Lett. 98, 080403 (2007).
We present experiments on ultracold rubidium in a magneto-optical trap:
In a closed loop experiment, the multi-photon ionization of Rb_2 is optimized using a parametric evolutionary algorithm. The result is approved by a systematic investigation of the relevant frequency components and allows to assign the transitions to certain electronic states [3].
In a pump probe scheme, the photoassociation process is investigated. Molecules are produced in their first electronically excited state by a pump, ionized by a probe pulse and mass selectively detected. The pump pulse is shaped with a frequency filter to avoid trap loss due to atomic resonances.
The ion signal shows oscillatory dynamics, caused by coherent interactions of molecular electronic dipole with the electric field. The observed characteristic structure is simulated by quantum dynamical calculations, which provide detailed insight in the underlying processes [4].
References
[1] C. P. Koch, R. Kosloff, and F Masnou-Seeuws, Phys. Rev. A 73, 043409 (2006)
[2] L.Chuntonov, L.Rybak, A.Gandman, and Z.Amitay,
arXiv:0709.0486
Gagik Djotyan, J.S. Bakos, G. Demeter,
Zs. Sörlei, J. Szigeti, D. Dzsotjan, KFKI Budapest, Hungary
Robust coherent control of quantum states
by frequency-chirped ultrashort laser pulses
Frauke Eimer, Andrea Merli, Fabian Weise, Sascha Birkner, Franziska Sauer, Stefan M. Weber, Ludger Wöste, Albrecht Lindinger, Wenzel Salzmann*, Terry Mullins*, Simone Götz, Judith Eng*, Magnus Albert*, Roland Wester* and Matthias Weidemüller*,
Freie Universität Berlin & *Universität Freiburg, Germany
Photoassociation of ultracold rubidium atoms by femtosecond-laserpulses
One promising mechanism for creating ultracold molecules is based on the photoassociation of ultracold atoms by ultrashort laser-pulses [1]. We investigate the photoassociation process with femtosecond-pulses in a magneto-optical 85Rb trap. For this purpose a two-colour pump-probe setup is used in which the amplitude of the pump-pulse spectrum is modulated. The observed molecular ion rate shows an oscillatory structure which is qualitatively reproduced by quantum-mechanical simulations. This oscillatory dynamic can be explained by coherent interactions of molecular electronic dipole with the spectrally modulated electric field. By varying the atomic density we were able to demonstrate, that photoassociation by femtosecond-laserpulses occurs. Also, the relevant frequency components could be determined by different modulations of the pump-pulse spectrum.
Benjamin Fingerhut, Dorothee Geppert and Regina de Vivie-Riedle,
Ludwig Maximilian University Munich, Germany
Ultrafast Dissociation Pathways of Diphenylmethanes:
Challenges of a Reactive Multi-Level System
The primary processes in the formation of electrophilic precursor ions, key intermediates in organic synthesis, are studied on a microscopic scale by quantum chemical and quantum dynamical methods. We investigate ultrafast dissociation processes of diphenylmethanes in gas phase. For the competing reaction channels of the photochemically induced heterolysis and homolysis of diphenylmethyl chloride the interaction of different electronic states leads to the initial charge transfer from the phenyl π-system to the σ-bond of the leaving group. The formation of ionic and radicalic products is observed in polar solvents [1] and is attributed to the existence of conical intersections [2]. We were able to localize and characterize three conical intersections for the first time, which constitute the minima in the intersection space.
2. K. S. Peters, Chem. Rev. 107, 859 (2007).
3. B. Fingerhut, D. Geppert, and R. de Vivie-Riedle, Chem. Phys. in press (2007).
Andrei Gandman, Lev Chuntonov, Leonid Rybak, Zohar Amitay,
Technion Haifa, Israel
Multi-Channel Selective Femtosecond Coherent Control
Based on Symmetry Properties
The present experimental work implements a new scheme for extended multi-channel selective femtosecond coherent control based on symmetry properties of the excitation channels. Here, an atomic non-resonant two-photon absorption channel [1] is coherently incorporated in a resonance-mediated (2+1) three-photon absorption channel [2]. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, the three-photon absorption is tuned independently over order-of-magnitude yield range for any possible two-photon absorption yield. Noticeable is a family of shaped pulses that are all dark with respect to the two-photon absorption (i.e., inducing zero two-photon absorption), while inducing widely tunable range of three-photon absorption. The work is conducted in the weak-field regime for which the two- and three-photon absorption are described, respectively, by second- and third-order perturbation theory. The model system is the Na atom. Figure 1 shows the two-channel excitation scheme of Na together with the phase patterns used for implementing the selective femtosecond coherent control. Each phase pattern results from the addition of two patterns: (i) a simple phase step that sets the two-photon absorption level, and (ii) a pattern that is anti-symmetric around one-half of the two photon transition frequency that tunes the three-photon absorption without affecting the two photon absorption.
[2] A. Gandman, L. Chuntonov, L. Rybak, and Z. Amitay, Phys. Rev. A 75, 031401 (R) (2007); Phys. Rev. A 76, 053419 (2007).
Sergej Grishkevich, Humboldt-Universität Berlin, Germany
Exact theoretical description of two ultracold atoms in a
single site of the 3D optical lattice using realistic potentials
A theoretical approach was developed that allows
for a full numerical description of a pair of ultracold atoms
trapped in a three-dimensional optical lattice. This approach
includes the possible coupling between center-of-mass and
relative motion coordinates in a configuration-interaction
type of calculations. The atoms are allowed to interact by
their full interaction potential that is, presently, only
limited to be central. With the aid of the newly developed
method deviations from the harmonic approximation are
discussed for the heteronuclear pairs. The developed method
is used to model experimental data.
Michael Khasin, Hebrew University Jerusalem, Israel
Yuri Khodorkovsky, Amichay Vardi & Gershon Kurizki,
Ben-Gurion University, Beer-Sheva & Weizmann Institute, Rehovot, Israel
Decoherence and entanglement in an open two-mode BEC: Bose enhancement of the quantum Zeno effect
Chii-Dong Lin, Kansas State University, Manhattan, KS, USA
Accurate retrieval of time-resolved atomic and molecular structure from laser induced photoelectron and high-harmonic spectra by few-cycle laser pulses
*
When atoms or molecules are placed in a short laser pulse, the electrons which are released by the laser' electric field earlier may return to recollide with the target ions. By analyzing accurate theoretical results from the solution of the time-dependent Schrödinger equation for rare gas atoms in few-cycle laser pulses, we established the general conclusion that the high-energy photoelectron momentum spectra and the high-order harmonics spectra can be used to extract differential elastic scattering and photo-recombination cross sections of the target ions by free electrons, respectively. [1] For high-harmonic generation, we have also shown that the phase of the electric dipole moment can be extracted from the phase of the high harmonics. [2] Using negative ions as targets, it is also possible to extract electron-atom scattering cross sections.[3] Since both electron scattering and photoionization (the reverse of photo-recombination) cross sections are the conventional means for determining the structure of atoms and molecules, these results imply that existing few-cycle infrared laser pulses can be implemented for ultrafast imaging of transient molecules with temporal resolution from a few down to sub-femtoseconds. [4] Recent experimental results for extracting structural information from laser-induced electron spectra will also be presented. [5]
[2] A. T. Le et al, submitted. Eprint:
arXiv:0712.3577
[3] X. X. Zhou et al, submitted. Eprint:
arXiv:0712.0334
[4] Toru Morishita et al., New J.Phys. (in press). Eprint:
arXiv:0709.2391
[5] C. L. Cocke and K. Ueda, Private communications.
Michael Mundt, Weizmann Institute, Israel
Optimal control theory for interacting particles: a
multi-configuration time-dependent Hartree-Fock approach
Applying optimal control theory to interacting many-particle
systems
is a great challenge due to the immense efforts required to solve the
time-dependent Schroedinger equation for such systems. This is
especially true in situations in which perturbation theory breaks down
and solving the exact time-dependent Schroedinger equation is
especially true in situations in which perturbation theory breaks down
and solving the exact time-dependent Schroedinger equation is
required as, e.g., in strong-field physics.
Hai Nguyen, University of Wisconsin Stevens Point, USA
Coherent Laser Matter Interactions: An experimental progress
José Palao, Christiane P. Koch, Ronnie Kosloff,
Universidad de La Laguna, Spain &
Freie Universität Berlin, Germany & Hebrew University Jerusalem,
Israel
Constrained Optimal Control Theory:
Avoiding population leakage to undesired states
A quantum system can be steered from an initial to a desired final state, or more generally, a given unitary transformation can be implemented by utilizing quantum interferences. Optimal control theory (OCT) is employed to design such laser pulses. The optimal pulses often imply high intensities and might thus drive unwanted multi-photon transitions, e.g. ionization, leading to loss of population. If population of the intermediate states in the multi-photon excitation pathways can be avoided at any time, the transition to the lossy channels is blocked. This can be formulated as an additional constraint in the formulation of OCT. The Krotov method is used to derive the algorithm for both optimization of a state-to-state transition and of a unitary transformation. The resulting algorithm turns out to be similar to formulating the control problem for a time-dependent target in previous work based on the variational approach to OCT [1-3]. The Krotov method offers the advantage that the conditions for monotonic convergence can be analyzed. The algorithm is illustrated with a simple molecular model containing three electronic states. Population transfer between levels in the electronic ground state is achieved by optical transitions through the first excited state, but avoiding population leakage to the second excited state.
[2] A. Kaiser and V. May, J. Chem. Phys. 121, 2528 (2004).
[3] I. Serban, J. Werschnik, and E. K. U. Gross, Phys. A 71, 053810 (2005).
Ulrich Poschinger, Kilian Singer and Ferdinand Schmidt-Kaler,
Universität Ulm, Germany
Application of optimal control techniques in scalable ion trap quantum logic
[2] S. Schulz et al., Progress of Physics, Wiley 54, No. 8-10, 648 (2006)
[3] N. Khaneja et al., J. Magn. Reson. 172, 296-305 (2005)
[4] N. Timoney et al. quant-ph/0612106 (2006)
Yair Rezek, Hebrew University Jerusalem, Israel
Leonid Rybak, Lev Chuntonov, Andrey Gandman, Zohar Amitay,
Technion Haifa, Israel
NIR Femtosecond Control of Resonance-Mediated Generation of Coherent Broadband UV Emission
We use shaped near-infrared (NIR) excitation pulses to control the generation of coherent broadband ultraviolet (UV) radiation in an atomic resonance-mediated (2+1) three-photon excitation. The intensity and phase of each UV spectral component UV are determined by the interferences between all the multi-photon excitation pathways that lead to the final excitation energy corresponding to UV. There is a manifold of such pathways due to broad spectral bandwidth of the NIR femtosecond pulse. Thus, by shaping the driving NIR pulse, one can control the yield and shape of the emitted UV pulse. The resonance-mediated nature of the process allows for much higher degree of control over the UV emission, as compared to a non-resonant excitation. Experimental and theoretical results are presented for phase controlling the total yield of the UV emission in atomic sodium (Na) [1]. The corresponding excitation scheme is shown of Fig. 1. Based on our confirmed understanding, we also present a new simple scheme for producing shaped femtosecond pulses in the UV/VUV spectral range.
Pablo Sanchez Moreno, Rosario González-Férez, Peter Schmelcher,
Universidad Granada
Molecular Rotational Dynamics in Nonadiabatically Switching
Homogeneous Electric Fields
[2] M. Aymar and O. Dulieu, J. Chem. Phys. 122, 204302, (2005).
[3] R. Gonzalez Ferez and P. Schmelcher, Phys. Rev. A 69, 023402 (2004).
[4] P. Sanchez-Moreno, R. Gonzalez-Ferez, and P. Schmelcher, accepted PRA
(2007).
Kilian Singer, W. Schnitzler, N. M. Linke, J. Eble F. Schmidt-Kaler,
Universität Ulm, Germany
Experimental demonstration of a deterministic single ion source with an expected implantation resolution of a few nm
[2] F. Jelezko et. al., Phys. Rev. Lett. 93, 130501 (2004).
[3] B. E. Kane, Nature 393, 133 (1998).
[4] T. Shinada et. al., Nature 437, 1128 (2005)
Haim Suchowski, Thomas Polack, and David J. Tannor,
Weizmann Institute, Israel
Uncontrollable quantum systems: Connectivity, Irreducibility and Dynamical symmetries
It is well-known that a finite-dimensional quantum system is controllable if the Lie algebra of its generators has full rank. When the rank of the algebra is not full, there is a rich mathematical and physical structure that to date has been analyzed only in special cases.
We show that uncontrollable systems can be classified into reducible and irreducible ones. We argue that irreducibility is a more general criteria than connectivity, applying to degenerate as well as non-degenerate systems. We give an example from 3-level systems, and then extend this to general multi-level systems.
I.Tikhonenkov and A. Vardi,
Ben-Gurion University, Beer-Sheva, Israel
Confinement controlled dissociation of a molecular BEC
[2] I. Tikhonenkov and A. Vardi, J. Phys. B 40, S299 (2007).
Fabian Weise,
Andrea Merli, Frauke Eimer, Sascha Birkner, Franziska Sauer, Stefan M. Weber,
Ludger Wöste, Albrecht Lindinger, Wenzel Salzmann, Terry Mullins,
Simone Götz, Judith Eng, Magnus Albert, Roland Wester, Matthias
Weidemüller,
Freie Universität Berlin, & Universität Freiburg, Germany
Control of ultracold rubidium with shaped femtosecond laser pulses
By applying femtosecond laser pulse shaping techniques on ultracold gases, a next step in atomic and molecular physics is taken. So far, this emerging field is mainly treated in theory e.g. proposing photoassociation of ultracold atoms [1] or photostabilization [2] of ground state molecules.
[2] B. Schäfer-Bung, R. Mitric, and V. Bonacic-Koutecky, J. Phys. B: At. Mol. Opt. Phys. 39 S1043 (2006)
[3] F. Weise, S. Birkner, A. Merli, S. M. Weber, F. Sauer, L. Wöste, A. Lindinger, W. Salzmann, T. Mullins, J. Eng, M. Albert, R. Wester, and M. Weidemüller, Phys. Rev. A 76, 063404 (2007)
[4] W. Salzmann, T. Mullins, J. Eng, M. Albert, R. Wester, M. Weidemüller,
A. Merli, S. M. Weber, F. Sauer, M. Plewicki, F. Weise, L. Wöste, and A. Lindinger, Phys. Rev. Lett., submitted
Last updated: 12/02/2008
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or Christiane Koch.