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Register a new userSingle-Photon Molecular Cooling
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Added by
Edvardas Narevicius
Publication date
2009
fields
Physics
and research's language is
English
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We propose a general method to cool the translational motion of molecules. Our method is an extension of single photon atomic cooling which was successfully implemented in our laboratory. Requiring a single event of absorption followed by a spontaneous emission, this method circumvents the need for a cycling transition and can be applied to any paramagnetic or polar molecule. In our approach, trapped molecules would be captured near their classical turning points in an optical dipole or RF-trap following an irreversible transition process.
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We report the cooling of an atomic ensemble with light, where each atom scatters only a single photon on average. This is a general method that does not require a cycling transition and can be applied to atoms or molecules which are magnetically trapped. We discuss the application of this new approach to the cooling of hydrogenic atoms for the purpose of precision spectroscopy and fundamental tests.
Ultracold molecular gases are promising as an avenue to rich many-body physics, quantum chemistry, quantum information, and precision measurements. This richness, which flows from the complex internal structure of molecules, makes the creation of ultracold molecular gases using traditional methods (laser plus evaporative cooling) a challenge, in particular due to the spontaneous decay of molecules into dark states. We propose a way to circumvent this key bottleneck using an all-optical method for decelerating molecules using stimulated absorption and emission with a single ultrafast laser. We further describe single-photon cooling of the decelerating molecules that exploits their high dark state pumping rates, turning the principal obstacle to molecular laser cooling into an advantage. Cooling and deceleration may be applied simultaneously and continuously to load molecules into a trap. We discuss implementation details including multi-level numerical simulations of strontium monohydride (SrH). These techniques are applicable to a large number of molecular species and atoms with the only requirement being an electric dipole transition that can be accessed with an ultrafast laser.
We provide a unified theoretical approach to the quantum dynamics of absorption of single photons and subsequent excitonic energy transfer in photosynthetic light-harvesting complexes. Our analysis combines a continuous mode <n>-photon quantum optical master equation for the chromophoric system with the hierarchy of equations of motion describing excitonic dynamics in presence of non-Markovian coupling to vibrations of the chromophores and surrounding protein. We apply the approach to simulation of absorption of single-photon coherent states by pigment-protein complexes containing between one and seven chromophores, and compare with results obtained by excitation using a thermal radiation field. We show that the values of excitation probability obtained under single-photon absorption conditions can be consistently related to bulk absorption cross-sections. Analysis of the timescale and efficiency of single-photon absorption by light-harvesting systems within this full quantum description of pigment-protein dynamics coupled to a quantum radiation field reveals a non-trivial dependence of the excitation probability and the excited state dynamics induced by exciton-phonon coupling during and subsequent to the pulse, on the bandwidth of the incident photon pulse. For bandwidths equal to the spectral bandwidth of Chlorophyll a, our results yield an estimation of an average time of ~0.09 s for a single chlorophyll chromophore to absorb the energy equivalent of one (single-polarization) photon under irradiation by single-photon states at the intensity of sunlight.
For the description of an H2 molecule an effective one-electron model potential is proposed which is fully determined by the exact ionization potential of the H2 molecule. In order to test the model potential and examine its properties it is employed to determine excitation energies, transition moments, and oscillator strengths in a range of the internuclear distances, 0.8 < R < 2.5 a.u. In addition, it is used as a description of an H2 target in calculations of the cross sections for photoionization and for partial excitation in collisions with singly-charged ions. The comparison of the results obtained with the model potential with literature data for H2 molecules yields a good agreement and encourages therefore an extended usage of the potential in various other applications or in order to consider the importance of two-electron and anisotropy effects.
Single-Photon Cooling (SPC), noted for its potential as a versatile method for cooling a variety of atomic species, has recently been demonstrated experimentally. In this paper, we study possible ways to improve the performance of SPC by applying it to atoms trapped inside a wedge billiard. The main feature of wedge billiard for atoms, also experimentally realized recently, is that the nature of atomic trajectories within it changes from stable periodic orbit to random chaotic motion with the change in wedge angle. We find that a high cooling efficiency is possible in this system with a relatively weak dependence on the wedge angle, and that chaotic dynamics, rather than regular orbit, is more desirable for enhancing the performance of SPC.
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