Directional Quantum-Controlled Chemistry: Generating Aligned Ultracold Molecules via Photoassociation

Abstract

Photoassociation of ultracold atoms is shown to lead to alignment of the product molecules along the excitation laser polarization axis. We theoretically investigate pulsed photoassociation of ${}^{87}Rb$ atoms into a specific weakly-bound level of the a ${}^3{\Sigma }_u^{+}$ metastable electronic state and find both stationary and time-dependent field-free alignment. Although a transform-limited pulse yields significant alignment, a frequency-chirped pulse dramatically enhances the molecular formation rate at the cost of a slight decrease in the alignment. Employing multiple pulses synchronized with the vibrational and rotational periods leads to coherent enhancement of both population and alignment of the target state.

References in corpus (11)

• Manipulation of Molecules with Electromagnetic Fields
• Field-free orientation of CO molecules by femtosecond two-color laser fields
• Coherent Control of Bond Making
• Femtosecond two-photon photoassociation of hot magnesium atoms: A quantum dynamical study using thermal random phase wavefunctions
• Enhancement of Ultracold Molecule Formation Using Shaped Nanosecond Frequency Chirps
• Generation of Arbitrary Frequency Chirps with a Fiber-Based Phase Modulator and Self-Injection-Locked Diode Laser
• Nanosecond Pulse Shaping with Fiber-Based Electro-Optical Modulators and a Double-Pass Tapered Amplifier
• Orientational decomposition of molecular high harmonic emission in three dimensions
• Probing the axis alignment of an ultracold spin-polarized ${\text{Rb}}_2$ molecule
• Production of Ultracold Molecules with Chirped Nanosecond Pulses: Evidence for Coherent Effects
• Efficient Formation of Ultracold Molecules with Chirped Nanosecond Pulses

Cited by in corpus (3)

• Observation of Quantum Interference and Coherent Control in a Photochemical Reaction
• An approximation scheme and non-Hermitian re-normalization for description of atom-field system evolution
• Coherent Control of Ultrafast Bond Making and Subsequent Molecular Dynamics: Demonstration of Final-State Branching Ratio Control