By driving photoassociation transitions, we form electronically excited molecules $({\mathrm{Na}}_{2}^{*})$ from ultracold $(50--300\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{K})$ Na atoms. Using a second laser to drive transitions from the excited state to a level in the molecular ground state, we are able to split the photoassociation line and observe features with a width smaller than the natural linewidth of the excited molecular state. The quantum interference which gives rise to this effect is analogous to that which leads to electromagnetically induced transparency in three-level atomic $\ensuremath{\Lambda}$ systems, but here one of the ground states is a pair of free atoms while the other is a bound molecule. The linewidth is limited primarily by the finite temperature of the atoms.By driving photoassociation transitions, we form electronically excited molecules $({\mathrm{Na}}_{2}^{*})$ from ultracold $(50--300\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{K})$ Na atoms. Using a second laser to drive transitions from the excited state to a level in the molecular ground state, we are able to split the photoassociation line and observe features with a width smaller than the natural linewidth of the excited molecular state. The quantum interference which gives rise to this effect is analogous to that which leads to electromagnetically induced transparency in three-level atomic $\ensuremath{\Lambda}$ systems, but here one of the ground states is a pair of free atoms while the other is a bound molecule. The linewidth is limited primarily by the finite temperature of the atoms.

arXiv:cond-mat/0508077Physical Review AOct 7, 200545 citations

Extension of the Local Approach to excited states of molecules

Peter Horsch

The European Physical Journal BMar 1, 19796 citations

A method of determining molecular excited-states using quantum computation

Pejman Jouzdani, Stefan A. Bringuier, Mark Kostuk

arXiv:1908.05238MRS AdvancesJul 26, 20218 citations

Vacuum-induced coherence in ultracold photoassociative rovibrational excitations

Sumanta Das, Arpita Rakshit, Bimalendu Deb

We show that coherence between two excited rovibrational states belonging to the same molecular electronic configuration arises quite naturally due to their interaction with electromagnetic vacuum. For initial preparation of a molecule in the desired rovibrational states, we propose to employ the method of ultracold photoassociation. Spontaneous decay of the excited molecule then gives rise to vacuum-induced coherence between the excited ro-vibrational states. We demonstrate theoretically an interesting interplay of effects due to vacuum-induced coherence and photoassociation. We apply our theory to photoassociation of bosonic ytterbium ( ${}^{174}$ Yb) atoms, which appear to be a promising system for exploring such interplay. The effects discussed here can be important for controlling decoherence and dissipation in molecular systems.We show that coherence between two excited rovibrational states belonging to the same molecular electronic configuration arises quite naturally due to their interaction with electromagnetic vacuum. For initial preparation of a molecule in the desired rovibrational states, we propose to employ the method of ultracold photoassociation. Spontaneous decay of the excited molecule then gives rise to vacuum-induced coherence between the excited ro-vibrational states. We demonstrate theoretically an interesting interplay of effects due to vacuum-induced coherence and photoassociation. We apply our theory to photoassociation of bosonic ytterbium (${}^{174}$Yb) atoms, which appear to be a promising system for exploring such interplay. The effects discussed here can be important for controlling decoherence and dissipation in molecular systems.

arXiv:1109.0588Physical Review AJan 3, 201210 citations

The Excited States of Atoms

Karl Taylor Compton

Scientific AmericanNov 1, 19260 citations

Strong‐field dressing of vibrational manifolds within ultrafast coherent Raman excitation

Stefanie Gräfe, Denis Akimov, Belinda Böhm +5 more

Abstract The mechanism of ultrafast, coherent Raman transitions driven at high field strengths is explored in theory and experiment. The study addresses the possibility of maintaining control of a vibrational wavepacket that is guided to a desired final state during the course of a Raman excitation by significantly perturbing the participating molecular states on the time scale of the dynamics under manipulation. Variations in the sequence and amplitude of the pulsed laser fields give direct insight into the nature of the perturbation as well as the population flow within vibrational manifolds of the electronic states involved in the transition. The excitation scheme realized in this work demonstrates control over the dynamics of a molecular system through a non‐adiabatic pathway that utilizes the full manifold of dressed states induced by the laser fields driving the transition rather than isolating the system in a decoupled dressed state common for the adiabatic passage scheme. By preparing highly excited virbrational states in molecular iodine with this scheme, it is shown that a vibrational wavepacket can be steered by controlling the phase with which the character of the field‐free states is introduced into the manifold of dressed states participating in the transition. This scheme seeks to open the possibility of using ultrafast Raman excitation for initiating and observing chemical reactions in the electronic ground state of a molecular system. Copyright © 2007 John Wiley & Sons, Ltd.Abstract The mechanism of ultrafast, coherent Raman transitions driven at high field strengths is explored in theory and experiment. The study addresses the possibility of maintaining control of a vibrational wavepacket that is guided to a desired final state during the course of a Raman excitation by significantly perturbing the participating molecular states on the time scale of the dynamics under manipulation. Variations in the sequence and amplitude of the pulsed laser fields give direct insight into the nature of the perturbation as well as the population flow within vibrational manifolds of the electronic states involved in the transition. The excitation scheme realized in this work demonstrates control over the dynamics of a molecular system through a non‐adiabatic pathway that utilizes the full manifold of dressed states induced by the laser fields driving the transition rather than isolating the system in a decoupled dressed state common for the adiabatic passage scheme. By preparing highly excited virbrational states in molecular iodine with this scheme, it is shown that a vibrational wavepacket can be steered by controlling the phase with which the character of the field‐free states is introduced into the manifold of dressed states participating in the transition. This scheme seeks to open the possibility of using ultrafast Raman excitation for initiating and observing chemical reactions in the electronic ground state of a molecular system. Copyright © 2007 John Wiley & Sons, Ltd.

Journal of Raman SpectroscopyApr 11, 200718 citations

By driving photoassociation transitions, we form electronically excited molecules

({\mathrm{Na}}_{2}^{*})

from ultracold $(50--300\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{K})$ Na atoms. Using a second laser to drive transitions from the excited state to a level in the molecular ground state, we are able to split the photoassociation line and observe features with a width smaller than the natural linewidth of the excited molecular state. The quantum interference which gives rise to this effect is analogous to that which leads to electromagnetically induced transparency in three-level atomic $\ensuremath{\Lambda}$ systems, but here one of the ground states is a pair of free atoms while the other is a bound molecule. The linewidth is limited primarily by the finite temperature of the atoms.

{}^{174}

Yb) atoms, which appear to be a promising system for exploring such interplay. The effects discussed here can be important for controlling decoherence and dissipation in molecular systems.