The theory for coherent Raman scattering (CRS) with broadband incoherent light is presented for a multiply resonant, multicomponent mixture of molecules that exhibits simultaneous multiple resonances with the frequencies of the driving fields. All possible pairwise hyperpolarizability contributions to the signal intensity are included in the theoretical treatment---(resonant-resonant, resonant-nonresonant, and nonresonant-nonresonant correlations between chromophores) and it is shown how the different types of correlations manifest themselves as differently behaved components of the signal intensity. The Raman resonances are modeled as Lorentzians in the frequency domain, as is the spectral density of the incoherent light. The analytic results for this multiply resonant mixture are presented and applied to a specific binary mixture. These analytic results will be used to recover frequencies and dephasing times in a series of experiments on multiply resonant mixtures.The theory for coherent Raman scattering (CRS) with broadband incoherent light is presented for a multiply resonant, multicomponent mixture of molecules that exhibits simultaneous multiple resonances with the frequencies of the driving fields. All possible pairwise hyperpolarizability contributions to the signal intensity are included in the theoretical treatment---(resonant-resonant, resonant-nonresonant, and nonresonant-nonresonant correlations between chromophores) and it is shown how the different types of correlations manifest themselves as differently behaved components of the signal intensity. The Raman resonances are modeled as Lorentzians in the frequency domain, as is the spectral density of the incoherent light. The analytic results for this multiply resonant mixture are presented and applied to a specific binary mixture. These analytic results will be used to recover frequencies and dephasing times in a series of experiments on multiply resonant mixtures.

Physical Review AFeb 1, 19988 citations

Theoretical aspects of the resonant scattering of light by molecules

Frank A. Novak

Jan 1, 19771 citation

Enhancing photoassociation rates by nonresonant-light control of shape resonances

Rosario González‐Férez, Christiane P. Koch

Photoassociation, assembling molecules from atoms using laser light, is limited by the low density of atom pairs at sufficiently short interatomic separations. Here we show that nonresonant light with intensities of the order of ${10}^{10}\phantom{\rule{0.16em}{0ex}}$ W/cm ${}^{2}$ modifies the thermal cloud of atoms, enhancing the Boltzmann weight of shape resonances and pushing scattering states below the dissociation limit. This leads to an enhancement of photoassociation rates by several orders of magnitude and opens the way to significantly larger numbers of ground-state molecules in a thermal ensemble than achieved so far.Photoassociation, assembling molecules from atoms using laser light, is limited by the low density of atom pairs at sufficiently short interatomic separations. Here we show that nonresonant light with intensities of the order of ${10}^{10}\phantom{\rule{0.16em}{0ex}}$W/cm${}^{2}$ modifies the thermal cloud of atoms, enhancing the Boltzmann weight of shape resonances and pushing scattering states below the dissociation limit. This leads to an enhancement of photoassociation rates by several orders of magnitude and opens the way to significantly larger numbers of ground-state molecules in a thermal ensemble than achieved so far.

arXiv:1301.1143Physical Review ADec 26, 201227 citations

Scattering of adiabatically aligned molecules by nonresonant optical standing waves

Lee Yeong Kim, Byung Gwun Jin, Tae Woo Kim +2 more

molecules in their lowest few rotational states are adiabatically aligned and transversely accelerated by a nonresonant optical standing wave. The width of the measured transverse velocity distribution increases to 160 m/s with the field intensity, while its central peak position moves from 10 to -10 m/s. These changes are well reproduced by numerical simulations based on the rotational state-dependent alignment but cannot be modeled when ignoring these effects. Moreover, the molecular scattering by an off-resonant optical field amounts to manipulating the translational motion of molecules in a rotational state-specific way. Conversely, our results demonstrate that scattering from a nonresonant optical standing wave is a viable method for rotational state selection of nonpolar molecules.molecules in their lowest few rotational states are adiabatically aligned and transversely accelerated by a nonresonant optical standing wave. The width of the measured transverse velocity distribution increases to 160 m/s with the field intensity, while its central peak position moves from 10 to -10 m/s. These changes are well reproduced by numerical simulations based on the rotational state-dependent alignment but cannot be modeled when ignoring these effects. Moreover, the molecular scattering by an off-resonant optical field amounts to manipulating the translational motion of molecules in a rotational state-specific way. Conversely, our results demonstrate that scattering from a nonresonant optical standing wave is a viable method for rotational state selection of nonpolar molecules.

Science AdvancesApr 3, 20201 citation

{10}^{10}\phantom{\rule{0.16em}{0ex}}

W/cm

{}^{2}

modifies the thermal cloud of atoms, enhancing the Boltzmann weight of shape resonances and pushing scattering states below the dissociation limit. This leads to an enhancement of photoassociation rates by several orders of magnitude and opens the way to significantly larger numbers of ground-state molecules in a thermal ensemble than achieved so far.