Optical pulse-shaping for internal cooling of molecules

Abstract

We consider the use of pulse-shaped broadband femtosecond lasers to optically cool rotational and vibrational degrees of freedom of molecules. Since this approach relies on cooling rotational and vibrational quanta by exciting an electronic transition, it is most easily applicable to molecules with similar ground and excited potential energy surfaces, such that the vibrational state is usually unchanged during electronic relaxation. Compared with schemes that cool rotations by exciting vibrations, this approach achieves internal cooling on the orders-of- magnitude faster electronic decay timescale and is potentially applicable to apolar molecules. For AlH+, a candidate species, a rate-equation simulation indicates that rovibrational equilibrium should be achievable in 8 μs. In addition, we report laboratory demonstration of optical pulse shaping with sufficient resolution and power for rotational cooling of AlH+.

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Cited by in corpus (14)

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• Quantum logic for control and manipulation of molecular ions using a frequency comb
• Cooling of a Zero-Nuclear-Spin Molecular Ion to a Selected Rotational State
• Cooling molecular vibrations with shaped laser pulses: Optimal control theory exploiting the timescale separation between coherent excitation and spontaneous emission
• Rotational State Analysis of AlH+ by Two-Photon Dissociation
• Quantum-State-Specific Reaction Rate Measurements for the Photo-induced Reaction Ca${}^{+}$ + O${}_2$ $\to$ CaO${}^{+}$ + O
• Electronic spectroscopy of a cold SiO${}^{+}$ sample: Implications for optical pumping
• Optical Pumping of TeH+: Implications for the Search for Varying mp/me
• Resonant Few-Photon Excitation of a Single-Ion Oscillator
• IP determination and 1+1 REMPI spectrum of SiO at 210-220 nm with implications for SiO${}^{+}$ ion trap loading
• Radium-containing molecular cations amenable for laser cooling
• Protocol for Optically Pumping AlH${}^{+}$ to a Pure Quantum State