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The Journal of Physical Chemistry Letters

Selective Elimination of Homogeneous Broadening by Multidimensional Spectroscopy in the Electromagnetically Induced Transparency Regime

Guangyu Liu, Андрій Сіжук, Konstantin E. Dorfman

Published Jun 15, 2020• 4 citations
Publisher

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.

DOI
10.1021/acs.jpclett.0c01481

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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.
We have shown that electromagnetically induced transparency can be achieved by control-probe interferometry using two delayed phase-locked ultrashort pulses. Two vibrational wavepackets on the excited state, excited by two delayed phase-locked ultrashort pulses, interfere constructively or destructively leading to enhancement or suppression of absorption to a selective set of vibrational levels. Depending on the phase difference and the delay between the pulses with same carrier frequency, one can design different transparency windows between absorption peaks at consecutive even(odd) vibrational levels by eliminating absorption at odd(even) vibrational levels. We have shown that by switching the phase difference of two delayed femtosecond pulses, one can switch to complete elimination of absorption from enhanced absorption to a particular set of vibrational levels in the excited state. Thus, switching of transparency through window between odd vibrational levels to that between even vibrational levels is possible. By properly choosing the temporal width and the carrier frequency of the pulses, lossless transmission of complete or bands of frequencies of the pulses can be achieved through these transparency windows. Hence, designing of single- or multi-mode transparency windows in NaH molecule is feasible by control-probe quantum interferometry.
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Optical spectroscopy using ultrafast light pulses has undergone a revolution in the last decade due to the introduction and development of multidimensional coherent techniques. These methods build on established coherent spectroscopic techniques, such as photon echoes, but go beyond them by correlating the coherent dynamics during two time periods. The resulting multidimensional spectra have a number of advantages including disentangling congested spectra, revealing coupling between resonances, and removing the effects of inhomogeneous broadening. Similar ideas are currently being used for imaging. The papers in this 'focus on' collection document some of the current areas of activity in these fields.
The interplay between dynamically induced coherence (DIC) and spontaneously generated coherence (SGC) can induce electromagnetically induced transparency (EIT) in a three-level closed Λ system. When the contributions from these two coherences are equal in magnitude and opposite in sign at the resonances of both the coherent and probe fields, transparency of the probe light occurs at the resonance with absorption humps away from the resonance. We have demonstrated here that the broadening of the EIT window can be controlled by changing the strength of incoherent pumping. This is a new approach for achieving wide EIT window for lossless and distortionless transmission of light of large spectral width. The most attractive feature of this new method is that the FWHM (full width at half-maximum) of the EIT window is further increased when the broadening due to homogeneous/inhomogeneous decay is taken into consideration. This scheme can be applied in atoms/molecules where SGC can be invoked by dressing two closely spaced levels ( e.g. hyperfine levels in atoms or rovibrational levels in molecules) by an external field. This effect has been demonstrated in a heteronuclear molecule ( e.g. LiH) and examined the role of incoherent pumping for controlling the width of the EIT window in the presence and absence of homogeneous/inhomogeneous decay. The experimental realization of the widening of the EIT window in molecules has been discussed.
Spectroscopic properties of coherently prepared, optically dense atomic media are studied experimentally and analyzed theoretically. It is shown that in such media the power broadening of the resonances can be substantially reduced. A density-dependent spectral narrowing of the electromagnetically induced transparency (EIT) window and novel, even narrower, resonances superimposed on the EIT line are observed in dense Rb vapor. A nonlinear two-photon spectroscopic technique based on coherent atomic media and combining high resolution with a large signal-to-noise ratio seems feasible.
Bose-Einstein condensates (BEC) serve as a model system for the study of the dynamic and spectroscopic response of a quantum system to momentum excitation. However, high -resolution spectroscopy of BEC has suffered from various finite-size (Doppler broadening) and inhomogeneous density effects [1]. We propose and demonstrate experimentally [2] a momentum space echo method using two and four -photon Bragg pulses, in order to overcome these broadening mechanisms. This method is pre sented in Fig. 1, where the excitation scheme and resulting populations in momentum space are shown. We demonstrate this scheme experimentally by using a four -photon echo pulse to reflect the initi ally populated excitations. The spectroscopic response of t he echo pulse is narrower than that of a regular Bragg pulse, as shown in Fig. 2.