Quantum adiabatic evolutions find a broad range of applications in quantum physics and quantum technologies. The traditional form of the quantum adiabatic theorem limits the speed of adiabatic evolution by the minimum energy gaps of the system Hamiltonian. Here, we experimentally show using a nitrogen-vacancy center in diamond that, even in the presence of vanishing energy gaps, quantum adiabatic evolution is possible. This verifies a recently derived necessary and sufficient quantum adiabatic theorem and offers paths to overcome the conventionally assumed constraints on adiabatic methods. By fast modulation of dynamic phases, we demonstrate near-unit-fidelity quantum adiabatic processes in finite times. These results challenge traditional views and provide deeper understanding on quantum adiabatic processes, as well as promising strategies for the control of quantum systems.
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http://dx.doi.org/10.1126/sciadv.aax3800 | DOI Listing |
J Chem Phys
January 2025
Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan.
The quantum-electrodynamic non-adiabatic emission (QED-NAE) is a type of radiatively assisted vibronic de-excitation due to electromagnetic vacuum fluctuations on non-adiabatic processes. Building on our previous work [Tsai et al., J.
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 Phys Chem Lett
January 2025
Key Laboratory of Quantum Materials and Devices of Ministry of Education, School of Physics, Southeast University, Nanjing 211189, China.
Single-atom manipulation has emerged as an effective strategy for enhancing the photocatalytic efficiency. However, the mechanism of photogenerated carrier dynamics under single-atom modulation remains unclear. Combining first-principles calculations and non-adiabatic molecular dynamics simulations, we systematically studied carrier transfer and recombination in the oxygen reduction reaction of single-atom-doped CN systems.
View Article and Find Full Text PDFCommun Chem
January 2025
Institute of Chemical Sciences, Heriot-Watt University, Edinburgh, UK.
Various photoactive molecules contain motifs built on aza-aromatic heterocycles, although a detailed understanding of the excited state photophysics and photochemistry in such systems is not fully developed. To help address this issue, the non-adiabatic dynamics operating in azanaphthalenes under hexane solvation was studied following 267 nm excitation using ultrafast transient absorption spectroscopy. Specifically, the species quinoline, isoquinoline, quinazoline, quinoxaline, 1,6-naphthyridine, and 1,8-naphthyridine were investigated, providing a systematic variation in the relative positioning of nitrogen heteroatom centres within a bicyclic aromatic structure.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Department of Chemistry, University of Rochester, Rochester, New York 14627, USA.
We outline two general theoretical techniques to simulate polariton quantum dynamics and optical spectra under the collective coupling regimes described by a Holstein-Tavis-Cummings (HTC) model Hamiltonian. The first one takes advantage of sparsity of the HTC Hamiltonian, which allows one to reduce the cost of acting polariton Hamiltonian onto a state vector to the linear order of the number of states, instead of the quadratic order. The second one is applying the well-known Chebyshev series expansion approach for quantum dynamics propagation and to simulate the polariton dynamics in the HTC system; this approach allows us to use a much larger time step for propagation and only requires a few recursive operations of the polariton Hamiltonian acting on state vectors.
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