Two-photon absorption in atomic or molecular systems

A. Quattropani, B. Girlanda

Krishna Rai Dastidar

We have studied the fidelity of spatial entanglement between dissociated atom and ion from two photon dissociation of hydrogen molecular ion H 2 + . Two processes for two photon dissociation of molecular ion have been considered (i) sequential two photon (STP) absorption and (ii) correlated two photon (CTP) absorption by the molecular ion. We compared the results for fidelity of spatial entanglement (FSE) between dissociated atom and ion for these two types of dissociation. In a previous study in our group [1] we have shown that when an atom interact with nonlocal mode of electromagnetic field (which has been derived field theoretically), simultaneous phase-correlated two pho1 ton absorption by the atom occurs within a very short time δt << ω , where ω is the laser frequency, and the rate of this correlated two photon absorption is linear in intensity. This will happen when the photon flux in the interaction region is high i.e. laser intensity is higher than 10 10 W/cm 2 . In this work we have extended this formalism to study the correlated two photon dissociation of molecular ion and to explore the effect of correlation between two simultaneous photo-absorption processes on the fidelity for spatial entanglement of dissociated atom and ion. Dependence of fidelity for spatial entanglement on the photon frequency has been studied for both the STP and CTP dissociation, to show that photon frequency can be used as control parameter to achieve maximum fidelity. Saturation of fidelity with the increase in time at which fidelity was calculated shows the robustness of the processes considered here. A scheme for detection of spatial entanglement between ion and atom has been suggested.

Rafael Negreiros de Paiva

In the atomic, molecular, optical physics field, processes involving two photons are very well understood and used in applications ranging from spectroscopy to laser cooling technics. In this thesis is presented the study and experimental realization of two two-photon processes. Using sodium atoms trapped in a magnetic optical trap we could demonstrate two-photon cooperative absorption, and that the creation of a molecular bound state using only light fields, or photonic bound state, is possible. Two-photon cooperative absorption, very common in solid-state physics, is a process where a pair of atoms initially in the ground state is excited to the double excited state, via absorption of two photons with frequecy that is not ressonant with any excited state. Its experimental realization with cold atoms may open new and exciting possibilities to better understand nonlinear effects, and it is a new way to create correlated atoms and photons in cold atomic physics. This absorption was observed by ionization of the pair after the excitation. A simple model that considers only dipole-dipole interactions between the atoms allows us to understand the basic features observed in the experimental data. A photonic bound state uses two photons to create the two basic features of a molecular bound state: a repulsive part and an attractive part. A blue photon, blue detuned from the atomic transition, connects the ground state of the pair to the repulsive part of the first excited molecular state 1, and a red photon, red detuned from the atomic transition, connects the connects the ground state of the pair to the attractive part of the first excited molecular state. In the dressed state picture, when the light fields are strong, this three-states-two-photon system creates adiabatic bound potentials that are strongly dependent of the photon properties. Using a theoretical model we could study how this bound energies changes when we change the photon properties, and the experimental data shows that this photos are indeed dressing the potentials with a efficiency that would enable the creation of photonic molecules.

M. S. Pindzola

Y. B. Band, Paul S. Julienne

We propose a method for copiously producing ultracold ground electronic-state molecules by two-photon absorption to a Rydberg molecular level (that spontaneously radiates to the ground molecular state) during collisions of ultracold atoms in a laser trap. Using the ${\mathrm{Na}}_{2}$ molecule as an example, the sequential two-photon absorption is via an intermediate high-lying vibrational level of the excited ${1}_{\mathit{g}}$ state and results in the formation of a given vibrational level of a $^{1}\mathrm{\ensuremath{\Pi}}_{\mathit{u}}$ Rydberg molecular state. Realistic calculations demonstrating the validity of the method are presented.

Zhenlin Wu, Tim Duka, Mariano Isaza-Monsalve +8 more

Absorption spectroscopy is a fundamental tool for probing molecular structure. However, performing absorption spectroscopy on individual molecules is challenging due to the low signal-to-noise ratio. Here, we report on a nondestructive absorption spectroscopy on a mid-infrared vibrational transition in a single molecular ion that is co-trapped with an atomic ion. The absorption of a single photon is detected via the momentum transfer from the absorbed photon onto the molecule. This recoil signal is amplified using a non-classical state of motion of the two-ion crystal and subsequently read out via the atomic ion. We characterize the recoil detection method and use it to investigate the interaction between femtosecond laser pulses and the O-H stretching vibration in individual CaOH+ molecular ions. Furthermore, we present the single-photon absorption spectrum obtained for the vibrational transition. This method represents a milestone towards quantum non-demolition measurements of complex polyatomic molecules, providing high-fidelity methods for preparation and measurement of the quantum state of a wide range of molecular species.