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arXiv:2601.05854 · Physical Review A

Optimally driving multi-photon transitions in the perturbative single-mode regime

Frieder Lindel, Stefan Yoshi Buhmann, Andreas Buchleitner, Edoardo G. Carnio

quant-phSubmitted Jan 9, 2026• Announced Jan 12, 2026• 0 citations
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Abstract

The rate of $m$-photon transitions in matter, induced by an incident light field, depends on the field's $m$th order coherence function. Consequently, the coherence properties of the light field may be shaped to increase the rate of multi-photon transitions. Here, we determine the optimal state of a weak fixed-intensity, narrow-band incident light field, with a restricted maximal photon number, that optimally drives $m$-photon transitions in the case of a short-lived atomic multilevel system. We show that, in this case, no quantum properties of the light field need to be exploited, but that classical mixtures of coherent states are optimal.

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The rate of mmm-photon transitions in matter, induced by an incident light field, depends on the field's mmmth order coherence function. Consequently, the coherence properties of the light field may be shaped to increase the rate of multi-photon transitions. Here, we determine the optimal state of a weak fixed-intensity, narrow-band incident light field, with a restricted maximal photon number, that optimally drives mmm-photon transitions in the case of a short-lived atomic multilevel system. We show that, in this case, no quantum properties of the light field need to be exploited, but that classical mixtures of coherent states are optimal.
This work discusses the problem of optimal excitation of a three-level atom of ladder configuration by light in the two-photon state and coherent light carrying an average of two photons. The applied atom-light interaction model is based on the Wigner-Weisskopf approximation. We characterize the properties of the optimal two-photon state that excites an atom perfectly, i.e., with probability equal to one. We find that the spectrotemporal shape of the optimal state of light is determined by the lifetimes of the atomic states, with the degree of photonic entanglement in the optimal state depending on the lifetime ratio. In consequence, two distinct interaction regimes can be identified in which the entanglement of the input state of light has a qualitatively different impact. As the optimal states may be challenging to prepare in general, we compare the results with those obtained for photon pairs of selected experimentally relevant pulse shapes. As these shapes are optimized for maximal atomic excitation probability, the results can be interpreted in terms of the overlap between the optimal and investigated pulse shapes.
We propose a scheme to enhance the light-matter coupling in a cavity QED system where two $\mathrm{\ensuremath{\Lambda}}$ atoms are weakly coupled to a single-mode cavity via multiphoton interaction. By introducing a second-order nonlinear (parametric) driving of the cavity, the original NNN-photon exchanges between the atoms, and the cavity can be reduced to either an effective single- or two-photon transition depending on the odevity of NNN, with the effective atom-field interaction strength being significantly enhanced. This results in an NNN-dependent effective coupling strength on top of the exponential enhancement induced only by the parametric driving. As an example, we demonstrate that our proposal can be exploited for the preparation of high-fidelity steady-state entanglement. The proposed scheme could provide a feasible alternative for diverse applications in quantum technologies.
The resonant absorption, emission, and scattering of light are the fundamental optical processes that have been used both to probe matter and to manipulate light itself. In the last decade there has been essential progress in coherent control of both linear and nonlinear optical responses based on resonant excitation of atomic coherence in multilevel quantum systems. Some interesting and useful phenomena, resulting from coherent control of absorption and the group index, such as electromagnetically induced transparency, lasing without inversion, and ultra-slow group velocity of light have been widely studied. This work is focused on coherent control of refractive index and resonant fluorescence in multilevel medium. \n \nWe suggest two promising schemes for resonant enhancement of the refractive index with eliminated absorption and propose their implementation in transition element doped crystals with excited state absorption and in a cell of Rb atoms at natural abundance. We show how to use one of these schemes for spatial variation of the refractive index via its periodic resonant increase/decrease, remarkably keeping at the same time zero absorption/gain. It opens the way to production of transparent photonic structures (such as distributed Bragg reflectors, holey fibers, or photonic crystals) in a homogeneous resonant atomic media such as dielectrics with homogeneously distributed impurities, atomic, or molecular gases. These optically produced photonic structures could easily be controlled (including switching on/off, changing amplitude and period of modulation) and would be highly selective in frequency, naturally limited by the width of the optical resonance. \n \nWe also derive the optical fluorescence spectra of a three-level medium driven by two coherent fields at the adjacent transitions in a general case when all three transitions are allowed. We show that coherent driving can efficiently control the distribution of intensities between the fluorescent channels. In particular, the total intensity of fluorescence at the transition which is not driven by the optical fields may essentially exceed the fluorescence intensity at the driven transitions under the condition of two-photon resonance. This counter-intuitive effect is due to depletion of the intermediate state via atomic interference.
We examine electromagnetically induced transparency (EIT) in an ensemble of cold $\mathrm{\ensuremath{\Lambda}}$-type atoms induced by a quantum control field in multimode coherent states and compare it with the transparency created by the classical light of the same intensity. We show that the perfect coincidence is achieved only in the case of a single-mode coherent state, whereas the transparency sharply decreases, when the number of the modes exceeds the mean number of control photons in the medium. The origin of the effect is the modification of photon statistics in the control field with increasing the number of the modes that weakens its interaction with atoms resulting in a strong probe absorption. For the same reason, the probe pulse transforms from EIT-based slow light into superluminal propagation caused by the absorption.
The absorption of a single photon that excites a quantum system from a low to a high energy level is an elementary process of light-matter interaction, and a route towards realizing pure single-photon absorption has both fundamental and practical implications in quantum technology. Due to nonlinear optical effects, however, the probability of pure single-photon absorption is usually very low, which is particularly pertinent in the case of strong ultrafast laser pulses with broad bandwidth. Here we demonstrate theoretically a counterintuitive coherent single-photon absorption scheme by eliminating nonlinear interactions of ultrafast laser pulses with quantum systems. That is, a completely linear response of the system with respect to the spectral energy density of the incident light at the transition frequency can be obtained for all transition probabilities between 0 and 100% in multilevel quantum systems. To that end, a multiobjective optimization algorithm is developed to find an optimal spectral phase of an ultrafast laser pulse, which is capable of eliminating all possible nonlinear optical responses while maximizing the probability of single-photon absorption between quantum states. This work not only deepens our understanding of light-matter interactions, but also offers a way to study photophysical and photochemical processes in the ``absence'' of nonlinear optical effects.
The dependence of the multiphoton absorption probability for an atomic system on the statistical properties of the incident light is investigated. It is shown, by means of nthn\mathrm{th}nth-order time-dependent perturbation theory, that the multiphoton absorption probability depends on the (n,n)th(n, n)\mathrm{th}(n,n)th normally ordered correlation functions of the electromagnetic field. For stationary fields, the transition probability per unit time is constant and is directly related to the reduced cross-spectral correlation function of the electromagnetic field. This expression for the transition probability is then analyzed under various conditions of coherence. Explicit calculations are carried out for thermal light and for laser light, and the transition rates are compared when each has a Lorentzian spectrum. In particular, when the width of the final atomic level is much larger than the bandwidth of the field, the transition rate for thermal light is nnn! times higher than with laser light of the same mean intensity. The other extreme case, i.e., when the width of the final atomic level is much smaller than the bandwidth of the field, is also considered in detail. An equation for the density operator of the field is derived; this equation governs the change in the statistical properties of the photon system in nnn-photon absorption processes. On the basis of this equation, the time-dependent properties of the photon system are then studied and some physical consequences of these equations are discussed. Some numerical solutions relating to the time dependence of the factorial moments in two-photon absorption processes are presented.