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Spontaneous Emission Manipulation

Marlan O. Scully, Shi-Yao Zhu, Muhammad Suhail Zubairy

Published Mar 25, 2017• 1 citation
Publisher

Abstract

The earliest studies on the subject of spontaneous emission from an excited atom via interaction with the vacuum modes of the radiation field go back to the early days of quantum mechanics. In view of the fundamental nature of the vacuum fluctuations, it was long thought that spontaneous emission could not be controlled. However, in 1946 Purcell noted that the spontaneous emission rate of the atom inside a resonant cavity can be substantially enhanced (or suppressed) over its free-space value. This is due to the dramatic change of the density of modes of the vacuum field in a cavity. The enhancement and suppression of spontaneous emission in resonant and off-resonant cavities were observed experimentally in the 1980s. It was also realized in the 1950s and 1960s that coherent driving fields can dramatically change the characteristics of the spontaneous emission. The Autler-Townes doublet and Mollow three-peak spectrum are the examples of such behavior. A dramatic narrowing of the spectral peaks were discovered in driven multilevel atomic systems in the early 1990s. The role of atomic coherence in quenching spontaneous emission fluctuations in the context of laser physics was studied in the 1980s, via the correlated spontaneous emission laser (CEL). In this case atomic coherence results in the correlation of two spontaneous emission noise events so that the spontaneous emission quantum noise is eliminated in the relative linewidth. Later, it was “discovered” that the spontaneous emission can be suppressed through quantum interference between decay channels. Properly stated, this was rediscovered since it was first discovered and explained by Lamb in the 1940s. If the dipoles of two transitions from one upper level to two lower levels are parallel, the spontaneous emission in an ordinary vacuum can be cancelled. In a nonuniform vacuum, e.g., a cavity, the quenching of spontaneous emission can be achieved, even for the orthogonal dipoles.

DOI
10.1117/3.2265059.ch15

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The earliest studies on the subject of spontaneous emission from an excited atom via interaction with the vacuum modes of the radiation field go back to the early days of quantum mechanics. In view of the fundamental nature of the vacuum fluctuations, it was long thought that spontaneous emission could not be controlled. However, in 1946 Purcell noted that the spontaneous emission rate of the atom inside a resonant cavity can be substantially enhanced (or suppressed) over its free-space value. This is due to the dramatic change of the density of modes of the vacuum field in a cavity. The enhancement and suppression of spontaneous emission in resonant and off-resonant cavities were observed experimentally in the 1980s. It was also realized in the 1950s and 1960s that coherent driving fields can dramatically change the characteristics of the spontaneous emission. The Autler-Townes doublet and Mollow three-peak spectrum are the examples of such behavior. A dramatic narrowing of the spectral peaks were discovered in driven multilevel atomic systems in the early 1990s. The role of atomic coherence in quenching spontaneous emission fluctuations in the context of laser physics was studied in the 1980s, via the correlated spontaneous emission laser (CEL). In this case atomic coherence results in the correlation of two spontaneous emission noise events so that the spontaneous emission quantum noise is eliminated in the relative linewidth. Later, it was “discovered” that the spontaneous emission can be suppressed through quantum interference between decay channels. Properly stated, this was rediscovered since it was first discovered and explained by Lamb in the 1940s. If the dipoles of two transitions from one upper level to two lower levels are parallel, the spontaneous emission in an ordinary vacuum can be cancelled. In a nonuniform vacuum, e.g., a cavity, the quenching of spontaneous emission can be achieved, even for the orthogonal dipoles.
We review the physics underlying the process of spontaneous emission, with a special focus on spontaneous emission into a resonator mode. We define the mode volume, verify the fundamental modal dimensions, present the spectral mode profile, the coherence time, the Q-factor, the Füchtbauer-Ladenburg equation, and the Purcell factor, and discuss their influence on different types of lasers. We obtain the relation between peak emission cross section, radiative lifetime, and emission linewidth. By interpreting spontaneous emission as stimulated emission driven by vacuum fluctuations, we derive the spontaneous-emission rate into a resonator mode and establish physical expressions for the fractions of spontaneous emission and total decay from the upper laser level into this mode. Furthermore, we discuss coupling of the atomic system with the coherent field inside a lasing resonator mode, resulting in the formation of a Mollow triplet, and demonstrate that it leads to a reduction of the spontaneous-emission rate by a factor of 2.
Possibility of coherent control of spontaneous emission from four- and five-level systems in the laser radiation field is studied. The four-level system consists of two levels resonantly driven by laser radiation where either of levels may decay to a separate level. For such a system we show that the presence of the second decay channel may deteriorate the destructive interference occurring because of Autler-Townes effect in case of one decay channel. The five-level system represents two two-level resonantly driven systems with the upper levels decaying to a common level. For this case, the interference between the two decay channels is partially or completely destructive or constructive depending on the initial conditions and on the mutual orientation of the transition dipole moments. It is shown that population transfer takes place by the same quantum vacuum via spontaneous emission. The populations are shown to have damping oscillatory nature.
Quantum interference and coherence lead to many interesting phenomenon and applications in quantum optics. In this dissertation, we study the quantum coherent properties in the following systems and aspects. We first investigate the optical bistability in a combined cavity-cold atoms system. In such a system the atom-photon interaction provides an optical lattice to the atoms and affects the mechanical motion of the atoms while atoms induce a position dependent phase shift on the cavity field. This highly nonlinearity induces optical bistability of intra-cavity photon number with respect to the pumping light added along the cavity axis. We show that the presence of this bistability can be controlled by a second pumping field added perpendicular to the cavity axis. It is also found that the critical input intensity of switching from one branch of bistability to the other depends on the the way of the field being added. This behavior is similar to the anomalous switching of the dispersive optical bistability of atomic media in the cavity. We also study the effect of counter-rotating terms in the control of spontaneous emission. We make use of a unitary transformation method and investigate the effect of dynamic energy shifts on the spontaneous emission modification via quantum interference in a four-level atomic system. We show that the counter-rotating terms, which are normally neglected in the usual investigation of atomic systems, do produce a significant influence on the evolution of the atomic amplitudes and the emission spectrum. This effect of counter-rotating terms can be observed in the time scale of the decay rate even when the dipole moments of the two upper levels are orthogonal to each other. The effect of counter-rotating terms on the spontaneous emission in a 3-D anisotropic photonic crystal is also discussed. It is shown that the behavior of the emission is similar to the case making rotating wave approximation, i.e., the localized and propagating fields are also separated by two characteristic atomic transition frequencies. However, the two characteristic frequencies are shifted due to the full Lamb shift which is obtained with counter-rotating terms being included in the Hamiltonian. We also utilize the unitary transformation method to show how the Lamb shift in a multi-level atom can be controlled by a driving field. Finally, we propose a subwavelength atom localization scheme for an atom located in a standing-wave field. The strategy is based on the observation that the photon statistics of resonance fluorescence depends on the position-dependent Rabi frequency.
We study the spontaneous-emission properties of a coherently driven four-level atom, and show a few interesting phenomena such as fluorescence quenching, spectral-line narrowing, spectral-line enhancement, and spectral-line elimination. These phenomena can be observed in experiment since the rigorous condition of near-degenerate levels with nonorthogonal dipole moments is not required here. Qualitatively, these phenomena can be attributed to the quantum interference between competitive spontaneous-decay channels in the bare-state picture or the spontaneously generated coherence between two close-lying levels in the dressed-state picture.
It was first realized by Purcell (1) that the spontaneous emission rate of a quantum system can be enhanced or suppressed by placing it in a resonant radiofrequency cavity. Spontaneous emission as it was first theoretically described by Einstein (2) is not a pure property of matter. It is described by matter coupled to quantized radiation field modes, which can be manipulated in an artificial structure such as a cavity. Cavity quantum electrodynamics (QED) is used to describe such effects that intimately depend on the fact that light is made of photons. Cavity QED has been extensively studied in atoms and the experimental proof was awarded with the Nobel Prize in 2012 (3). It has been applied to cooling of single atoms and for the detection of single atoms and creating and studying states with few photons and few atoms (4). In more recent developments these ideas have been extended to manipulate electronic states (5) and vibrations in molecules (6, 7). In PNAS, Flick et al. (8) introduce recent theoretical developments for the application of cavity QED to molecules and suggest possible novel applications to photochemistry. These include nonadiabatic dynamics of molecules in cavities, the modification of molecular properties, and the integration of QED with density functional theory. A quantized electromagnetic field mode can be described as a harmonic oscillator whose coordinate is the electric field displacement (Fig. 1 A ). The zero point energy translates into a nonvanishing field intensity ⟨ e 2 ⟩ in the ground state | 0 ⟩ (vacuum fluctuations). The electric vacuum field increases for a small cavity volume e c = ℏ ω c V ϵ 0 , [1] Fig. 1. ( A ) Illustration of the standing wave cavity mode and the resulting field quantization (Fock states). ( B ) Combined matter-field states (dressed states, | ± , n ⟩ … [↵][1]1To whom correspondence should be addressed. Email: smukamel{at}uci.edu. [1]: #xref-corresp-1-1
The spontaneous emission property of a five-level atom with a loop structure driven by three optical fields and a microwave field is intensively studied. Several quantum interference effects can be observed in the spontaneous emission spectra, such as spectral-line narrowing, spectral-line enhancement, spectral-line suppression, partial cancellation and fluorescence quenching. The number of emission peaks, the positions of dark lines can be controlled by varying the intensities of driving fields or the phase of the microwave field coupling the two lower levels in the atomic system. Furthermore, since no rigorous conditions are required, the expected phenomena may easily be achieved experimentally in atomic systems.