Quantum Coherent Control of a Single Molecular-Polariton Rotation
arXiv:2212.11649 · doi:10.1103/PhysRevLett.130.043604
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 post-pulse 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 work 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.
16 pages, 5 figures , accepted by Physical Review Letters on 19 December, 2022
References in corpus (15)
- Microwave photonics with superconducting quantum circuits
- Realizing strong light-matter interactions between single nanoparticle plasmons and molecular excitons at ambient conditions
- Climbing the Jaynes-Cummings Ladder and Observing its Sqrt(n) Nonlinearity in a Cavity QED System
- Nonlinear response of the vacuum Rabi resonance
- Field-free orientation of CO molecules by femtosecond two-color laser fields
- Nonlinear spectroscopy of photons bound to one atom
- Two-photon probe of the Jaynes-Cummings model and symmetry breaking in circuit QED
- Resolution of Gauge Ambiguities in Molecular Cavity Quantum Electrodynamics
- Reaching optimally oriented molecular states by laser kicks
- Efficient and long-lived field-free orientation of molecules by a single hybrid short pulse
- Two-state wave packet for strong field-free molecular orientation
- Pulsed Rabi oscillations in quantum two-level systems: beyond the Area Theorem
- Optimal three-state field-free molecular orientation with terahertz pulses
- Complete quantum coherent control of ultracold molecular collisions
- Carrier-wave Rabi flopping signatures in high-order harmonic generation for alkali atoms
Cited by in corpus (7)
- Coupling Polyatomic Molecules to Lossy Nanocavities: Lindblad versus Schrödinger description
- Quantum Speed Limit under Brachistochrone Evolution
- Impact of Cavity on Molecular Ionization Spectra
- Single site-controlled inverted pyramidal InGaAs QD-nanocavity operating at the onset of the strong coupling regime
- Anisotropic Rabi model with two-photon relaxation
- Environment-limited transfer of angular momentum in Bose liquids
- Topological enhancement of a PT-symmetric Su-Schrieffer-Heeger quantum battery