Sequential optical response suppression for chemical mixture characterization

Alicia B. Magann1,2, Gerard McCaul3, Herschel A. Rabitz4, and Denys I. Bondar3

1Department of Chemical & Biological Engineering, Princeton University, Princeton, New Jersey 08544, USA
2Center for Computing Research, Sandia National Laboratories, Albuquerque, New Mexico 87185, USA
3Department of Physics, Tulane University, New Orleans, LA 70118, USA
4Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA

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The characterization of mixtures of non-interacting, spectroscopically similar quantum components has important applications in chemistry, biology, and materials science. We introduce an approach based on quantum tracking control that allows for determining the relative concentrations of constituents in a quantum mixture, using a single pulse which enhances the distinguishability of components of the mixture and has a length that scales linearly with the number of mixture constituents. To illustrate the method, we consider two very distinct model systems: mixtures of diatomic molecules in the gas phase, as well as solid-state materials composed of a mixture of components. A set of numerical analyses are presented, showing strong performance in both settings.

Our ability to accurately characterize the composition of chemical mixtures has widespread applications spanning chemistry, physics, biology, and materials science. This article proposes a new procedure for characterizing chemical mixtures that utilizes a single laser pulse, which is tailored to increase the distinguishability of mixture components by rendering them sequentially invisible, by turning off their optical responses one-by-one. Then, by measuring how the total optical response of the mixture varies in time, the relative concentrations of the components can be determined, allowing for the characterization of the mixture composition. Numerical demonstrations are performed that confirm that this procedure enhances the distinguishability of the components of the molecular and materials mixtures under consideration.

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Cited by

[1] Gerard McCaul, Kurt Jacobs, and Denys I. Bondar, "Towards single atom computing via high harmonic generation", The European Physical Journal Plus 138 2, 123 (2023).

[2] Abdallah AlShafey, Gerard McCaul, Yuan-Ming Lu, Xu-Yan Jia, Shou-Shu Gong, Zachariah Addison, Denys I. Bondar, Mohit Randeria, and Alexandra S. Landsman, "Ultrafast laser-driven dynamics in metal/magnetic-insulator interfaces", Physical Review B 108 14, 144434 (2023).

[3] Jacob Masur, Denys I. Bondar, and Gerard McCaul, "Optical distinguishability of Mott insulators in the time versus frequency domain", Physical Review A 106 1, 013110 (2022).

[4] Gerard McCaul, Alexander F. King, and Denys I. Bondar, "Non‐Uniqueness of Driving Fields Generating Non‐Linear Optical Response", Annalen der Physik 534 10, 2100523 (2022).

[5] Alicia B. Magann, Tak-San Ho, Christian Arenz, and Herschel A. Rabitz, "Quantum tracking control of the orientation of symmetric-top molecules", Physical Review A 108 3, 033106 (2023).

[6] Gerard McCaul, Peisong Peng, Monica Ortiz Martinez, Dustin R. Lindberg, Diyar Talbayev, and Denys I. Bondar, "Superoscillations Deliver Superspectroscopy", Physical Review Letters 131 15, 153803 (2023).

[7] Gerard McCaul, Alexander F. King, and Denys I. Bondar, "Optical Indistinguishability via Twinning Fields", Physical Review Letters 127 11, 113201 (2021).

[8] Gerard McCaul, Kurt Jacobs, and Denys I. Bondar, "Towards Single Atom Computing via High Harmonic Generation", arXiv:2104.06322, (2021).

[9] Gerard McCaul, Alexander F. King, and Denys I. Bondar, "Non-Uniqueness of Non-Linear Optical Response", arXiv:2110.06189, (2021).

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