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Journal of Physics B Atomic and Molecular Physics

AC Stark splitting of bound-continuum decays

P. L. Knight

Published Oct 28, 1979• 52 citations
Publisher

Abstract

The effects of saturation of a bound-bound atomic resonance on bound-continuum decays in investigated using the dressed state concept. Two special cases are discussed: the modification of spontaneous radiative decay by coupling to a third bound atomic state, and the changes in single-photon photoionisation when the initial discrete state is coupled by an external field to another bound state. For strong external fields Rabi oscillations and dynamic Stark splittings profoundly alter the 'decay'; but for weak fields the alterations at line centre are no less dramatic.

DOI
10.1088/0022-3700/12/20/010

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The effects of saturation of a bound-bound atomic resonance on bound-continuum decays in investigated using the dressed state concept. Two special cases are discussed: the modification of spontaneous radiative decay by coupling to a third bound atomic state, and the changes in single-photon photoionisation when the initial discrete state is coupled by an external field to another bound state. For strong external fields Rabi oscillations and dynamic Stark splittings profoundly alter the 'decay'; but for weak fields the alterations at line centre are no less dramatic.
The dressed eigenstates of an atom interacting with a near-resonant radiation field are used to study the dynamics and final-state photoelectron spectra of resonant two-photon ionisation for arbitrary initial conditions and detunings. The authors find that under some circumstances (and particularly for intense fields) the dressed states preserve their integrity whilst decaying as distinguishable states, leading to AC Stark-split photoelectron energy spectra. In general, however, there exists an off-diagonal coupling between dressed states via the continuum so that each dressed state cannot decay independently of the existence of the other. This can modify lowest order expectations, particularly for weak fields and can entirely alter final-state spectra.
A theory describing the radiative decay of an autoionizing state under strong pumping by a coherent field is developed. The theory systematically takes into account the radiative decay of the unperturbed continuum. The problem at hand corresponds to the case of strongly coupled bound states decaying to electron and photon continua with the two continua also weakly coupled to each other. A master equation describing the time evolution of the atomic system is derived, and its exact solution under arbitrary initial conditions is given. The effect of radiative decay on the Fano profiles and photoelectron spectra is analyzed in detail. The time development of the system is also examined. The radiative decay of the autoionizing state and the unperturbed continuum changes the spectra in a significant way. The characteristics of the spectra are correlated with the dressed states (with complex energies) of the system. The changes in the structure of the dressed states as a function of the system parameters such as the spontaneous-emission rate and laser intensity are discussed in detail.
Complex dressed states and photoelectron spectra are considered for a model system containing two discrete states that are coupled by separate lasers to a continuum that supports a resonance such as an autoionizing state. Spontaneous radiative decay from the structured continuum has been included and its effects are examined. It is shown that population can be trapped within the model atom even when radiative decay is included provided (1) the two Fano q values which characterize the discrete-state--continuum interactions are equal, and (2) the two-photon resonance condition is satisfied.
We investigate a ionising electronic transition under resonant pumping. We demonstrate that, above a critical value of the pump intensity, a novel metastable electronic bound state is created, which can decay into the free electron continuum by two-photon ionization. We calculate the system's resonant fluorescence spectrum, finding results qualitatively different from the Mollow triplet expected in a bound-to-bound transition. The fluorescent emission can be used to measure the time-resolved population of the novel metastable state. Contrary to Kramers-Hennenberger atoms, stabilised by non-perturbative, non-resonant laser pulses, the physics we observe is inherently resonant and relies on perturbative level repulsion. In analogy to how the AC-Stark shift is a semiclassical version of the single-photon Rabi splitting observed in photonic cavity, the phenomenon we describe is better understood as a semiclassical version of recently observed excitons bound by a single cavity photon. Our results demonstrate a novel way to stabilise electronic states with intense laser fields, increasing our capability to design and engineer non-classical states of matter.
We present a comprehensive quantum electrodynamical analysis of the interaction between a continuum with photonic band gaps (PBGs) or frequency cut-off and an excited two-level atom, which can be either ‘bare’ or ‘dressed’ by coupling to a near-resonant field mode. A diversity of novel features in the atom and field dynamics is shown to arise from the non-Markovian character of radiative decay into such a continuum of modes. Firstly the excited atom is shown to evolve, by spontaneous decay, into a superposition of non-decaying single-photon dressed states, each having an energy in a different PBG, and a decaying component. This superposition is determined by the atomic resonance shift, induced by the spontaneously emitted photon, into or out of a PBG. The main novel feature exhibited by the decaying excited-state component is the occurrence of beats between the shifted atomic resonance frequency and the PBG cut-off frequencies, corresponding to a non-Lorentzian emission spectrum. Secondly the induced decay of a resonantly driven atom into such a continuum exhibits a cascade of transitions down the ladder of dressed states, which are labelled by decreasing photon numbers of the driving mode. Remarkably, this cascade is terminated at the dressed-state doublet, from which all subsequent transitions to lower doublets are forbidden because they fall within the PBG. This doublet then becomes an attractor state for the populations of higher-lying doublets. As a result, the photon-number distribution of the driving mode becomes strongly sub-Poissonian.
Stabilizing atoms exposed to intense laser fields has been a central topic in atomic physics for decades, inspiring several theoretical frameworks that describe the phenomenon under different resonance conditions and coupling regimes. Here, we theoretically investigate an ionizing electronic transition driven by a resonant pump field, in contrast to Kramers–Henneberger atoms, which are stabilized by non-perturbative, non-resonant laser pulses. We show that, above a critical pump intensity, the drive creates a metastable electronic bound state emerging from the continuum, which decays via two-photon ionization. We calculate the resulting resonant fluorescence spectrum and find a qualitatively different structure from the familiar Mollow triplet associated with bound-to-bound transitions. This fluorescence provides a time-resolved probe of the population in the metastable state. In analogy to how the AC Stark shift is a semiclassical counterpart of the single-photon Rabi splitting observed in optical cavities, the phenomenon we describe is best understood as a semiclassical analog of recently observed excitons bound by a single cavity photon.