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1.
J Chem Phys ; 155(4): 044105, 2021 Jul 28.
Article in English | MEDLINE | ID: mdl-34340365

ABSTRACT

Quantum optical theory of absorption properties of interacting atoms is developed. The concept of local absorptance is introduced as a derivative of the logarithm of intensity with respect to the distance in the vicinity of a given spatial point and a moment of time. The intensity is represented by the quantum and statistically averaged normal product of creation and annihilation operators of the electromagnetic field. The development of an analytical method of the estimation for the kinetic and optical parameters for the system is proposed here. The calculation method of the absorption coefficient includes thermal atomic motion, Doppler effect, and the short-range interaction between atoms. The absorption coefficient explicitly takes into account the quantum nature of the optical field. The ability of the system to absorb or emit quanta is quantitatively expressed through the special form of interaction integrals. The specific form of integrals results from the structure of the quantum brackets. The interplay between the collective (virtual photon exchange) and binary (optically induced inter-particle bonding) processes determines the system behavior. The spectral profile of the local absorption coefficient for different atomic densities and time intervals is simulated for realistic parameters.

2.
J Phys Chem Lett ; 11(14): 5504-5509, 2020 Jul 16.
Article in English | MEDLINE | ID: mdl-32539404

ABSTRACT

The key feature of photon echo-based spectroscopies is a selective elimination of the inhomogeneous broadening. Fast homogeneous dephasing typical for large macromolecules makes it difficult to resolve the congested spectra even if the inhomogeneous component is eliminated. We propose a novel two-dimensional spectroscopy in which a series of temporally separated probe pulses are combined with the strong narrowband control pulse. Using electromagnetically induced transparency originating from the interference between the control and probe pulses, we achieve an observation window for molecular response in narrow spectral intervals significantly smaller than the homogeneous dephasing limit.

3.
Nanoscale Res Lett ; 9(1): 203, 2014.
Article in English | MEDLINE | ID: mdl-24860278

ABSTRACT

In this work, a chain of N identical two-level atoms coupled with a quantized electromagnetic field, initially prepared via a single-photon Fock state, is investigated. The N-particle state amplitude of the system is calculated for several space configurations of the atoms in the Weisskopf-Wigner approximation. It was shown that the space configuration of an atomic chain, the total number of atoms, and even the available volume for the field modes define the behavior of the system state amplitude with time. Applying the condition of 'cyclic bonds', presented in this work, to the elaborated theory allows to describe the system time evolution, practically, for any space configuration.

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