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arXiv:2504.09845

Simultaneous Multiphoton-Multiatom Processes in Atomic Gases and Their Application in Enhancing Ultraweak Atomic Absorption Transitions

Yu, Yongle

Published Apr 14, 2025• 0 citations
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Abstract

We investigate simultaneous multiphoton-multiatom (MPMA) processes in atomic gases subjected to laser fields. Our study reveals that the composite factor governing the transition rate of these processes can reach extraordinarily high magnitudes, with an intrinsic regulation mechanism causing the rate to exhibit near-saturation behavior. By integrating an MPMA process into an ultraweak atomic absorption transition, a substantial enhancement of the overall transition rate can be achieved. This enhancement enables the detection of transitions that would otherwise remain undetectable, thereby opening new avenues for exploring ultraweak quantum phenomena in atomic systems.

DOI
10.48550/arxiv.2504.09845

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We investigate simultaneous multiphoton-multiatom (MPMA) processes in atomic gases subjected to laser fields. Our study reveals that the composite factor governing the transition rate of these processes can reach extraordinarily high magnitudes, with an intrinsic regulation mechanism causing the rate to exhibit near-saturation behavior. By integrating an MPMA process into an ultraweak atomic absorption transition, a substantial enhancement of the overall transition rate can be achieved. This enhancement enables the detection of transitions that would otherwise remain undetectable, thereby opening new avenues for exploring ultraweak quantum phenomena in atomic systems.
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The non linear interaction between an intense laser radiation and atoms leads to ionization through the absorption of N photons from the laser radiation via laser-induced virtual states. The multiphoton ionization rate varies as a function of the laser intensity I as IN. We discuss the two most important effects which govern multiphoton ionization processes : resonance effects and laser-coherence effects. In a moderate laser intensity range (107 - 109 W cm-2) corresponding to the two, three or four-photon ionization of atoms, resonance effects play a dominant role while the photon statistics of the laser radiation are relatively unimportant. On the contrary, in the very high intensity range (1012 - 1013 W cm-2) required to observe large Nth - order ionization processes, coherence effects play a dominant role through N! enhancement in the N-photon ionization rate, while resonance effects are completely damped due to the high laser intensity. We conclude by reviewing the possible applications of multiphoton absorption processes in other fields.
We have demonstrated an interference between multiphoton ionization processes that results in a phase-sensitive enhancement or inhibition of the net ionization rate. We focus two laser beams, either of which can induce an atomic transition between the same two states, into a cell containing atomic mercury. One of the fields is at a wavelength of 185 nm and can linearly induce the 6s 1S0 → 6p 1P1 transition in mercury. The other field is at a wavelength precisely three times as long, and it can excite the 6p resonance by a three-photon process. The absorption of two additional visible photons ionizes the mercury. In the presence of both fields, the transition amplitudes interfere, and their relative phases become very important. Their phases can be controlled by controlling the phases of the optical fields inducing the transitions. Coherence between the two fields, vital for the interference, is ensured by generating one field from the other using a nonlinear third-harmonic process. We have also demonstrated the effect of spatial phase variations between the two fields on the local photo-ionization rate.
In the strong-field regime a single multiphoton resonance can enhance many harmonics of the fundamental laser frequency simultaneously. We demonstrate that an alkali-metal atom driven by an intense, ultrafast midinfrared pulse is an ideal system for observing this effect by calculating the response of potassium atoms to radiation that is nearly three or five photon resonant with the $4s\ensuremath{-}4p$ transition. We find that all the harmonics through at least the 17th are enhanced over a wide range of intensities, and that the resonance width of the enhanced harmonics is governed by the lifetime of the multiphoton resonance.
Multiphoton spectroscopy The subject of multiphoton excitation spectroscopy began in 1931 when Göppert-Mayer [450] wrote a theoretical paper in which she calculated the transition rate for an atom in the presence of two photons rather than just one. At the time, the process seemed rather exotic, and it was reassuring that the calculated rate was so low as to guarantee that it could not readily be observed in the laboratory with conventional sources. This conclusion was reassuring because it implies that a simple perturbative theory (one photon per transition is the weak-field limit) is adequate for most purposes. The subject came to life with the advent of lasers, when it became easy to create intense beams of light. Since the probability of excitation by two photons grows as the square of the photon density, whereas the probability of single-photon excitation grows only linearly with photon density, two-photon transitions gain in relative strength with increasing intensity despite the small value of the rate coefficient. The development of multiphoton spectroscopy has followed that of lasers: as the available power has increased, so has the number of photons involved in individual transitions. More significantly, it has become apparent that the physics of the interaction between radiation and matter is not the same at high laser powers as under weak illumination, i.e. that there is a qualitative change which sets in at strong laser fields. This is normally expressed by saying that perturbative approximations break down.