Femtosecond coherent control of thermal photoassociation of magnesium atoms

Rybak, Leonid; Amitay, Zohar; Amaran, Saieswari; Kosloff, Ronnie; Tomza, Michał; Moszyński, Robert; Koch, Christiane P.

doi:10.1039/c1fd00052g

Cited by 19 publications

(11 citation statements)

References 32 publications

(30 reference statements)

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“…The experimental signature is the periodic modulation of the pump probe signal. 30,31 The purity for an incoherent ensemble is inversely proportional to the number of occupied quantum states of a pair of atoms. This number is completely determined by the temperature T = 1000 K, and density, ρ = 4.8 · 10…”

Section: Interplay Of Coherence and Photoassociation Yieldmentioning

confidence: 99%

“…30,31 It is summarized in Figure 1. Magnesium in its electronic ground state is a closed shell atom.…”

mentioning

confidence: 99%

“…10 We have recently demonstrated generation of both rotational and vibrational coherences by two-photon femtosecond photoassociation of hot atoms. 30,31 This is a crucial step toward the coherent control of photoinduced binary reactions since the fate of bond making and breaking is determined by the vibrational motion.…”

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confidence: 99%

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Femtosecond two-photon photoassociation of hot magnesium atoms: A quantum dynamical study using thermal random phase wavefunctions

Amaran

Kosloff

Tomza

et al. 2013

The Journal of Chemical Physics

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Two-photon photoassociation of hot magnesium atoms by femtosecond laser pulses, creating electronically excited magnesium dimer molecules, is studied from first principles, combining ab initio quantum chemistry and molecular quantum dynamics. This theoretical framework allows for rationalizing the generation of molecular rovibrational coherence from thermally hot atoms [L. Rybak et al., Phys. Rev. Lett. 107, 273001 (2011)]. Random phase thermal wave functions are employed to model the thermal ensemble of hot colliding atoms. Comparing two different choices of basis functions, random phase wavefunctions built from eigenstates are found to have the fastest convergence for the photoassociation yield. The interaction of the colliding atoms with a femtosecond laser pulse is modeled non-perturbatively to account for strong-field effects.

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Section: Interplay Of Coherence and Photoassociation Yieldmentioning

confidence: 99%

“…30,31 It is summarized in Figure 1. Magnesium in its electronic ground state is a closed shell atom.…”

mentioning

confidence: 99%

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Femtosecond two-photon photoassociation of hot magnesium atoms: A quantum dynamical study using thermal random phase wavefunctions

Amaran

Kosloff

Tomza

et al. 2013

The Journal of Chemical Physics

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“…On the other hand, and in striking contrast, no experimental study has previously demonstrated coherent control of bond making. The photoinduced creation of a chemical bond between the colliding reactants, also termed photoassociation, using femtosecond laser pulses has proven to be much more challenging [12][13][14][15][16]. Particularly at high temperature, a typical situation for chemical reactions, the starting point for photoassociation is rather unfavorable to coherent control since many scattering states are incoherently populated.…”

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confidence: 99%

Coherent Control of Bond Making

et al. 2015

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We demonstrate coherent control of bond making, a milestone on the way to coherent control of photoinduced bimolecular chemical reactions. In strong-field multiphoton femtosecond photoassociation experiments, we find the yield of detected magnesium dimer molecules to be enhanced for positively chirped pulses and suppressed for negatively chirped pulses. Our ab initio model shows that control is achieved by purification combined with chirp-dependent Raman transitions. Experimental closed-loop phase optimization using a learning algorithm yields an improved pulse that utilizes vibrational coherent dynamics in addition to chirp-dependent Raman transitions. Our results show that coherent control of binary photoreactions is feasible even under thermal conditions.

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“…4,5 Investigating photoassociation in this regime is very important, since this is a situation more often encountered in the laboratory. In the present work, we investigate photoassociation in a thermal gas composed of two different atomic species.…”

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Effects of rotation in the laser-pulse photoassociation in a thermal gas of atoms

Lima

2013

SPIE Proceedings

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Photoassociation is a possible route for the formation of chemical bonds. In this process, the binding of colliding atoms can be induced by means of a laser field. Photoassociation has been studied in the ultracold regime and also with temperatures well above millikelvins in the thermal energy domain, which is a situation commonly encountered in the laboratory. A photoassociation mechanism can be envisioned based on the use of infrared pulses to drive a transition from free colliding atoms on the electronic ground state to form a molecule directly on that state. This work takes a step in this direction, investigating the laser-pulse-driven formation of heteronuclear diatomic molecules in a thermal gas of atoms including rotational effects. Based on the assumption of full system controllability, the maximum possible photoassociation yield is deduced. The photoassociation probability is calculated as a function of the laser parameters for different temperatures. Additionally, the photoassociation yield induced by subpicosecond pulses of a priori fixed shape is compared to the maximum possible yield.

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Femtosecond coherent control of thermal photoassociation of magnesium atoms

Cited by 19 publications

References 32 publications

Femtosecond two-photon photoassociation of hot magnesium atoms: A quantum dynamical study using thermal random phase wavefunctions

Femtosecond two-photon photoassociation of hot magnesium atoms: A quantum dynamical study using thermal random phase wavefunctions

Coherent Control of Bond Making

Effects of rotation in the laser-pulse photoassociation in a thermal gas of atoms

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