Quantum Coherent Control of a Single Molecular-Polariton Rotation

Li-Bao Fan, Chuan-Cun Shu, Daoyi Dong, Jun He, Niels E. Henriksen, and Franco Nori

Phys. Rev. Lett. 130, 043604 – Published 25 January 2023

Abstract

We present a combined analytical and numerical study for coherent terahertz control of a single molecular polariton, formed by strongly coupling two rotational states of a molecule with a single-mode cavity. Compared to the bare molecules driven by a single terahertz pulse, the presence of a cavity strongly modifies the postpulse orientation of the polariton, making it difficult to obtain its maximal degree of orientation. To solve this challenging problem toward achieving complete quantum coherent control, we derive an analytical solution of a pulse-driven quantum Jaynes-Cummings model by expanding the wave function into entangled states and constructing an effective Hamiltonian. We utilize it to design a composite terahertz pulse and obtain the maximum degree of orientation of the polariton by exploiting photon blockade effects. This Letter offers a new strategy to study rotational dynamics in the strong-coupling regime and provides a method for complete quantum coherent control of a single molecular polariton. It, therefore, has direct applications in polariton chemistry and molecular polaritonics for exploring novel quantum optical phenomena.

Received 30 March 2022
Accepted 19 December 2022

DOI:https://doi.org/10.1103/PhysRevLett.130.043604

Physics Subject Headings (PhySH)

Atoms, ions, & molecules in cavities Cavity quantum electrodynamics Coherent control Hybrid quantum systems Quantum state engineering

Atomic, Molecular & Optical

Authors & Affiliations

Li-Bao Fan ¹, Chuan-Cun Shu ^1,*, Daoyi Dong ², Jun He¹, Niels E. Henriksen ³, and Franco Nori ^4,5

¹Hunan Key Laboratory of Nanophotonics and Devices, Hunan Key Laboratory of Super-Microstructure and Ultrafast Process, School of Physics and Electronics, Central South University, Changsha 410083, China
²School of Engineering and Information Technology, University of New South Wales, Canberra, Australian Capital Territory 2600, Australia
³Department of Chemistry, Technical University of Denmark, Building 207, DK-2800 Kongens Lyngby, Denmark
⁴Theoretical Quantum Physics Laboratory, RIKEN, Saitama 351-0198, Japan
⁵Physics Department, University of Michigan, Ann Arbor, Michigan 48109, USA