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Physical Review A

Suppression of the spontaneous emission of atoms and molecules

Einat Frishman, Moshe Shapiro

Published Sep 19, 2003• 22 citations
Publisher

Abstract

We present an experimentally viable approach for suppressing the spontaneous emission in several atomic and molecular systems. We have shown [E. Frishman and M. Shapiro, Phys. Rev. Lett. 87, 253001 (2001)] that a coherent excitation of overlapping resonances followed by the application of infrequent interruptions can result in complete suppression of spontaneous emission. In the present work, the overlapping resonances result from splitting a single resonance with an external (spectator) field. An optimized superposition of the two components is formed by a shaped pulse excitation from the ground state.

DOI
10.1103/physreva.68.032717

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We present an experimentally viable approach for suppressing the spontaneous emission in several atomic and molecular systems. We have shown [E. Frishman and M. Shapiro, Phys. Rev. Lett. 87, 253001 (2001)] that a coherent excitation of overlapping resonances followed by the application of infrequent interruptions can result in complete suppression of spontaneous emission. In the present work, the overlapping resonances result from splitting a single resonance with an external (spectator) field. An optimized superposition of the two components is formed by a shaped pulse excitation from the ground state.
Spontaneous emission can be modified if the atom is driven by an external coherent field. Such modification include the three-peak spectrum of resonance fluorescence from a two level atom. The spectral line elimination and cancellation of spontaneous emission is possible under conditions that the spontaneous emission from an excited atom can be trapped in the upper states without decaying. The amount of fluorescence in this case as well as the population of the upper levels can be controlled. If spontaneous emission along with atomic transition is suppressed, it is possible to create a population in version on this transition by using a very weak incoherent pumping.
It has been shown recently [see, for example, S.-Y. Zhu and M. O. Scully, Phys. Rev. Lett. 76, 388 (1996)] that a dynamical suppression of spontaneous emission can occur in a three-level system when an external field drives transitions between a metastable state and two decaying states. What is unusual in the decay scheme is that the decaying states are coupled directly by the vacuum radiation field. It is shown that the decay dynamics required for total suppression of spontaneous emission necessarily implies that the level scheme is isomorphic to a three-level \ensuremath{\Lambda} system, in which the lower two levels are both metastable and each is coupled to the decaying state. As such, the total suppression of spontaneous emission can be explained in terms of conventional dark states and coherent population trapping.
Abstract In a previous paper [Deb and Agarwal 2014 Phys. Rev. A 90 063417], it was theoretically shown that, magneto-optical manipulation of low energy scattering resonances and atom-molecule transitions could lead to the formation of a bound state in continuum (BIC), provided there is no spontaneous emission. We find that even an exceedingly small spontaneous decay from exited molecular states can spoil the BIC. In this paper, we show how to circumvent the detrimental effect of spontaneous emission by making use of vacuum-induced coherence (VIC) which results in the cancellation or suppression of spontaneous emission. VIC occurs due to the destructive interference between two spontaneous decay pathways. An essential condition for VIC is the non-orthogonality of two transition dipole moments associated with the radiative decays form two excited states. Furthermore, the interference between two decay pathways requires that the spacing between the two decaying states must be comparable to or smaller than the square root of the product of the two spontaneous linewidths. We demonstrate that these conditions can be fulfilled by optically manipulating appropriately chosen molecular excited states, opening a promising prospect for the experimental realization of BIC of cold atoms.
We experimentally investigate various processes present in the photoassociative interaction of an ultracold atomic sample with shaped femtosecond laser pulses as an detailed extension of previous work [W. Salzmann et al., Phys. Rev. Lett. 100, 233003 (2008)]. We demonstrate the photoassociation of pairs of rubidium atoms into electronically excited, bound molecular states using spectrally cut femtosecond laser pulses tuned below the rubidium D1{D}_{1}D1​ or D2{D}_{2}D2​ asymptote. Time-resolved pump-probe spectra reveal oscillations of the molecular formation rate, which are due to coherent transient dynamics in the electronic excitation. The oscillation frequency corresponds to the detuning of the spectral cut position to the asymptotic transition frequency of the rubidium D1{D}_{1}D1​ or D2{D}_{2}D2​ lines, respectively. Measurements of the molecular photoassociation signal as a function of the pulse energy reveal a nonlinear dependence and indicate a nonperturbative excitation process. Chirping the association laser pulse allowed us to change the phase of the coherent transients. Furthermore, a signature for molecules in the electronic ground state is found, which is attributed to molecule formation by femtosecond photoassociation followed by spontaneous decay. In a subsequent article [A. Merli et al., Phys. Rev. A 80, 063417 (2009)] quantum mechanical calculations are presented, which compare well with the experimental data and reveal further details about the observed coherent transient dynamics.