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Proceedings of the London Mathematical Society

A Problem in Resonance, illustrative of the Theory of Selective Absorption of Light

Horace Lamb

Published Jan 1, 1900• 7 citations
Publisher
DOI
10.1112/plms/s1-32.1.11

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The spectral broadening of incident light that is cw incoherent or pulsed can lead to a redistribution of emission from a near resonantly driven three-level system. The "non-tracking" fluorescence-like peak emerges even when pure dephasing is absent in the system/bath interaction. For the more realistic congested multimode problem, recently introduced transform methods based on the Kramers-Heisenberg expression have proved useful in relating the resonant absorption band (ABS) to experimental Raman excitation profiles (REP’s). Here we shall illustrate the use of a new direct "inverse transform" procedure that is able to take a single observed REP to predict ABS as well as other REP's with extraction of vibronic parameters.

Routledge eBooks•Jan 6, 2026•0 citations
Through photonic mechanisms based on near-field coupling, laser radiation can engage with resonant energy transfer in a variety of suitably designed materials and molecular structures. Energy that has been acquired, through the initial absorption of resonant laser light, undergoes transfer between chromophores only on the throughput of off-resonant light, the process known as laser-assisted resonance energy transfer. The comprehensive results that are presented here extend and generalize the theory for both single and dual beam configurations, producing results that are applicable to media of various types including doped crystals, heterogeneous multichromophore solids, and solutions. The detailed principles, here explained in terms of both energetics and optical selection rule criteria, are specifically illustrated for a variety of materials. It is shown how general application of the theory can facilitate the elucidation of experiments, by clearly interpreting the effects of laser polarization manipulation. On further analysis of the photophysical mechanisms it is also demonstrated that such effects represent an entirely practicable basis for optical switching and logic gate operation. The additional polarization selectivity afforded by a two-beam setup proves to allow the most complete system control. With such a configuration, there is considerable promise for the realization of new optically driven logic and molecular devices.
We investigate optimal states of photon pairs to excite a target transition in a multilevel quantum system. With the help of coherent control theory for two-photon absorption with quantum light, we infer the maximal population achievable by optimal entangled vs separable states of light. Interference between excitation pathways as well as the presence of nearby states may hamper the selective excitation of a particular target state, but we show that quantum correlations can help to overcome this problem and enhance the achievable "selectivity" between two energy levels, i.e., the relative difference in population transferred into each of them. We find that the added value of optimal entangled states of light increases with broadening linewidths of the target states.
The spectral broadening of incident light that is cw incoherent or pulsed can lead to a redistribution of emission from a near resonantly driven three-level system. The "non-tracking" fluorescence-like peak emerges even when pure dephasing is absent in the system/bath interaction. For the more realistic congested multimode problem, recently introduced transform methods based on the Kramers-Heisenberg expression have proved useful in relating the resonant absorption band (ABS) to experimental Raman excitation profiles (REP’s). Here we shall illustrate the use of a new direct "inverse transform" procedure that is able to take a single observed REP to predict ABS as well as other REP's with extraction of vibronic parameters.