The striking nonlinear effects exhibited by cavity QED systems make them a powerful tool in modern condensed matter and atomic physics. A recently discovered example is the quantized pumping of energy into a cavity by a strongly coupled, periodically driven spin. We uncover a remarkable feature of these energy pumps: they coherently translate, or boost, a quantum state of the cavity in the Fock basis. Current optical cavity and circuit QED experiments can realize the required Hamiltonian in a rotating frame. Boosting thus enables the preparation of highly excited nonclassical cavity states in near-term experiments.
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http://dx.doi.org/10.1103/PhysRevLett.128.183602 | DOI Listing |
ACS Nano
January 2025
Institute of Physics, Ecole Polytechnique Fédérale de Lausanne (EPFL), 1015 Lausanne, Switzerland.
Controlling the light emitted by individual molecules is instrumental to a number of advanced nanotechnologies ranging from super-resolution bioimaging and molecular sensing to quantum nanophotonics. Molecular emission can be tailored by modifying the local photonic environment, for example, by precisely placing a single molecule inside a plasmonic nanocavity with the help of DNA origami. Here, using this scalable approach, we show that commercial fluorophores may experience giant Purcell factors and Lamb shifts, reaching values on par with those recently reported in scanning tip experiments.
View Article and Find Full Text PDFJ Comput Chem
January 2025
Department of Chemistry, Molecular Sciences Research Hub, Imperial College London, London, UK.
We report nonadiabatic dynamics computations on CH initiated on a coherent superposition of the five lowest cationic states, employing the Quantum Ehrenfest method. In addition to the totally symmetric carbon-carbon double bond stretch and carbon-hydrogen stretches, we see that the three non-totally symmetric modes become stimulated; torsion and three different CH stretching patterns. Thus, a coherent superposition of states, of the type involved in an attochemistry experiment, leads to the stimulation of specific non-totally symmetric motions.
View Article and Find Full Text PDFJ Comput Chem
January 2025
Nantes Université, CNRS, CEISAM UMR 6230, Nantes, France.
Carbonyl complexes of metals with an α-diimine ligand exhibit both emission and ligand-selective photodissociation from MLCT states. Studying this photodissociative mechanism is challenging for experimental approaches due to an ultrafast femtosecond timescale and spectral overlap of multiple photoproducts. The photochemistry of a prototypical system is investigated with non-adiabatic dynamic simulations.
View Article and Find Full Text PDFJ Comput Chem
January 2025
Instituto de Química, Universidade de Brasília, Brasília, Brazil.
This study aims to shed light on the mechanism and kinetics of 1,4-dioxane degradation by hydroxyl radical (OH) across various solvation conditions to evaluate electronic and structural properties at the MP2/aug-cc-pVTZ level. Transition states (TS) structures determined in the gas phase and SMD solvation model reveal similar hydrogen abstraction patterns. In contrast, the explicit solvation model (ES) introduces significant changes, suggesting a kinetic preference for axial pathways.
View Article and Find Full Text PDFSmall
January 2025
Key Laboratory of Advanced Technologies of Materials, Ministry of Education, School of Materials Science and Engineering, Southwest Jiaotong University, Chengdu, 610031, China.
A novel polymer electrolyte based on CsPbI quantum dots (QDs) reinforced polyacrylonitrile (PAN), named as PIL, is exploited to address the low room-temperature (RT) ion conductivity and poor interfacial compatibility of polymer solid-state electrolytes. After optimizing the content of CsPbI QDs, RT ion conductivity of PIL largely increased from 0.077 to 0.
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