Quantum coherent control of ultrafast bond making and the subsequent molecular dynamics is crucial for the realization of a new photochemistry, where a shaped laser field is actively driving the chemical system in a coherent way from the thermal initial state of the reactants to the final state of the desired products. We demonstrate here coherent control over the relative yields of Mg2 molecules that are generated via photoassociation and subsequently photodriven into different groups of final states. The strong-field process involves non-resonant multiphoton femtosecond photoassociation of a pair of thermally hot magnesium atoms into a bound Mg2 molecule and subsequent molecular dynamics on electronically excited states. The branching-ratio control is achieved with linearly chirped laser pulses, utilizing the different chirp dependence that various groups of final molecular states display for their post-pulse population. Our joint experimental and theoretical study establishes the feasibility of high degree coherent control over quantum molecular dynamics that is initiated by femtosecond photoassociation of thermal atoms.Quantum coherent control of ultrafast bond making and the subsequent molecular dynamics is crucial for the realization of a new photochemistry, where a shaped laser field is actively driving the chemical system in a coherent way from the thermal initial state of the reactants to the final state of the desired products. We demonstrate here coherent control over the relative yields of Mg2 molecules that are generated via photoassociation and subsequently photodriven into different groups of final states. The strong-field process involves non-resonant multiphoton femtosecond photoassociation of a pair of thermally hot magnesium atoms into a bound Mg2 molecule and subsequent molecular dynamics on electronically excited states. The branching-ratio control is achieved with linearly chirped laser pulses, utilizing the different chirp dependence that various groups of final molecular states display for their post-pulse population. Our joint experimental and theoretical study establishes the feasibility of high degree coherent control over quantum molecular dynamics that is initiated by femtosecond photoassociation of thermal atoms.

Jan 1, 20226 citations

Coherently Driven Molecular Vibrations and Light Modulation

E. Garmire, F. Pandarese, Charles Hard Townes

Physical Review LettersAug 15, 1963220 citations

Coherent control of ultrafast bond making and subsequent molecular dynamics: demonstration of final-state branching ratio control

Liat Levin, Daniel M. Reich, Moran Geva +3 more

Abstract Quantum coherent control of ultrafast bond making and the subsequent molecular dynamics is crucial for the realization of a new photochemistry, where a shaped laser field is actively driving the chemical system in a coherent way from the thermal initial state of the reactants to the final state of the desired products. We demonstrate here coherent control over the relative yields of Mg 2 molecules that are generated via photoassociation and subsequently photodriven into different groups of final states. The strong-field process involves non-resonant multiphoton femtosecond photoassociation of a pair of thermally hot magnesium atoms into a bound Mg 2 molecule and subsequent molecular dynamics on electronically excited states. The branching-ratio control is achieved with linearly chirped laser pulses, utilizing the different chirp dependence that various groups of final molecular states display for their post-pulse population. Our joint experimental and theoretical study establishes the feasibility of high degree coherent control over quantum molecular dynamics that is initiated by femtosecond photoassociation of thermal atoms.Abstract Quantum coherent control of ultrafast bond making and the subsequent molecular dynamics is crucial for the realization of a new photochemistry, where a shaped laser field is actively driving the chemical system in a coherent way from the thermal initial state of the reactants to the final state of the desired products. We demonstrate here coherent control over the relative yields of Mg 2 molecules that are generated via photoassociation and subsequently photodriven into different groups of final states. The strong-field process involves non-resonant multiphoton femtosecond photoassociation of a pair of thermally hot magnesium atoms into a bound Mg 2 molecule and subsequent molecular dynamics on electronically excited states. The branching-ratio control is achieved with linearly chirped laser pulses, utilizing the different chirp dependence that various groups of final molecular states display for their post-pulse population. Our joint experimental and theoretical study establishes the feasibility of high degree coherent control over quantum molecular dynamics that is initiated by femtosecond photoassociation of thermal atoms.

arXiv:2104.11786Journal of Physics B Atomic Molecular and Optical PhysicsJul 9, 20210 citations

Broadband Modulation of Light by Coherent Molecular Oscillations

Andrea Burzo, Alexei V. Sokolov

Elsevier eBooksJan 1, 20091 citation

All-optical control of pendular qubit states with nonresonant two-color laser pulses

Je Hoi Mun, Shinichirou Minemoto, Dong Eon Kim +1 more

Abstract Practical methodologies for quantum qubit controls are established by two prerequisites, i.e., preparation of a well-defined initial quantum state and coherent control of that quantum state. Here we propose a new type of quantum control method, realized by irradiating nonresonant nanosecond two-color ( $\omega$ and 2 $\omega$ ) laser pulses to molecules in the pendular (field-dressed) ground state. The two-color field nonadiabatically splits the initial pendular ground state $\vert\tilde{0},\tilde{0}\rangle$ to a superposition state of $\vert\tilde{0},\tilde{0}\rangle$ and $\vert\tilde{1},\tilde{0}\rangle$ , whose relative probability amplitudes can be controlled by the peak intensity of one wavelength component ( $\omega$ ) while the peak intensity of the other component (2 $\omega$ ) is fixed. The splitting of the quantum paths is evidenced by observing degrees of orientation of ground-state-selected OCS molecules by the velocity map imaging technique. This quantum control method is highly advantageous in that any type of polar molecules can be controlled regardless of the molecular parameters, such as rotational energy, permanent dipole moment, polarizability, hyperpolarizability, and hyperfine energy structures.Abstract Practical methodologies for quantum qubit controls are established by two prerequisites, i.e., preparation of a well-defined initial quantum state and coherent control of that quantum state. Here we propose a new type of quantum control method, realized by irradiating nonresonant nanosecond two-color ($\omega$ and 2$\omega$) laser pulses to molecules in the pendular (field-dressed) ground state. The two-color field nonadiabatically splits the initial pendular ground state $\vert\tilde{0},\tilde{0}\rangle$ to a superposition state of $\vert\tilde{0},\tilde{0}\rangle$ and $\vert\tilde{1},\tilde{0}\rangle$, whose relative probability amplitudes can be controlled by the peak intensity of one wavelength component ($\omega$) while the peak intensity of the other component (2$\omega$) is fixed. The splitting of the quantum paths is evidenced by observing degrees of orientation of ground-state-selected OCS molecules by the velocity map imaging technique. This quantum control method is highly advantageous in that any type of polar molecules can be controlled regardless of the molecular parameters, such as rotational energy, permanent dipole moment, polarizability, hyperpolarizability, and hyperfine energy structures.

Communications PhysicsSep 14, 20224 citations

STRONG FIELD COHERENT CONTROL IN MOLECULES

Brett J. Pearson, D. S. MORRIS, P. H. Bucksbaum +1 more

May 1, 20021 citation

\omega

and 2

\omega

) laser pulses to molecules in the pendular (field-dressed) ground state. The two-color field nonadiabatically splits the initial pendular ground state

\vert\tilde{0},\tilde{0}\rangle

to a superposition state of

\vert\tilde{0},\tilde{0}\rangle

and

\vert\tilde{1},\tilde{0}\rangle

, whose relative probability amplitudes can be controlled by the peak intensity of one wavelength component (

\omega

) while the peak intensity of the other component (2

\omega

) is fixed. The splitting of the quantum paths is evidenced by observing degrees of orientation of ground-state-selected OCS molecules by the velocity map imaging technique. This quantum control method is highly advantageous in that any type of polar molecules can be controlled regardless of the molecular parameters, such as rotational energy, permanent dipole moment, polarizability, hyperpolarizability, and hyperfine energy structures.