Seeking a quantum advantage with trapped-ion quantum simulations of condensed-phase chemical dynamics

Kang, Mingyu; Nuomin, Hanggai; Chowdhury, Sutirtha N.; Yuly, Jonathon L.; Sun, Ke; Whitlow, Jacob; Valdiviezo, Jesús; Zhang, Zhendian; Zhang, Peng; Beratan, David N.; Brown, Kenneth R.

doi:10.1038/s41570-024-00595-1

Cited by 5 publications

(2 citation statements)

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“…Nonadiabatic electron–phonon coupling facilitates charge carrier transitions, playing a crucial role in technologies such as solar cells, , quantum information systems, , and spintronic devices. − Typically, nonadiabatic coupling (NAC) is computed at a single k -point in momentum space, which constrains nonadiabatic molecular dynamics (NA-MD) to only manage vertical transitions of charge carriers. , This limitation prevents the NA-MD from addressing nonvertical transitions among multiple k-points, which requires additional nonzero phonons to conserve the momentum of electrons during electronic transitions. On the basis of the harmonic approximation and using the electron–phonon coupling, the nonvertical transitions can be handled by the real-time Boltzmann transport equation − or surface hopping based quantum dynamics .…”

Section: Introductionmentioning

confidence: 99%

“…Nonadiabatic electron−phonon coupling facilitates charge carrier transitions, playing a crucial role in technologies such as solar cells, 1,2 quantum information systems, 3,4 and spintronic devices. 5−7 Typically, nonadiabatic coupling (NAC) is computed at a single k-point in momentum space, which constrains nonadiabatic molecular dynamics (NA-MD) to only manage vertical transitions of charge carriers.…”

Section: Introductionmentioning

confidence: 99%

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Nonadiabatic Molecular Dynamics in Momentum Space Beyond Harmonic Approximation: Hot Electron Relaxation in Photoexcited Black Phosphorus

Lu,

Fang,

Long

2024

J. Am. Chem. Soc.

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We simulated hot-electron relaxation in black phosphorus using the nonadiabatic molecular dynamics (NA-MD) approach with a non-Condon effect in momentum space beyond the harmonic approximation. By comparing simulations at the Γ point in a large supercell with those using a few k-points in a smaller supercell�while maintaining the same number of electronic states within the same energy range, we demonstrate that both setups yield remarkably consistent energy relaxation times, regardless of the initial state energy. This consistency arises from the complementary effects of supercell size in real space and the number of k-points in the reciprocal space. This finding confirms that simulations at a single k-point in large size supercells are an effective approximation for NA-MD with a non-Condon effect. This approach offers significant advantages for complex photophysics, such as intervalley scattering and indirect bandgap charge recombination, and is particularly suitable for large systems without the need for a harmonic approximation.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Nonadiabatic Molecular Dynamics in Momentum Space Beyond Harmonic Approximation: Hot Electron Relaxation in Photoexcited Black Phosphorus

Lu,

Fang,

Long

2024

J. Am. Chem. Soc.

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Coherence in Chemistry: Foundations and Frontiers

Schultz,

Yuly,

Arsenault

et al. 2024

Chem. Rev.

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Coherence refers to correlations in waves. Because matter has a wave-particle nature, it is unsurprising that coherence has deep connections with the most contemporary issues in chemistry research (e.g., energy harvesting, femtosecond spectroscopy, molecular qubits and more). But what does the word "coherence" really mean in the context of molecules and other quantum systems? We provide a review of key concepts, definitions, and methodologies, surrounding coherence phenomena in chemistry, and we describe how the terms "coherence" and "quantum coherence" refer to many different phenomena in chemistry. Moreover, we show how these notions are related to the concept of an interference pattern. Coherence phenomena are indeed complex, and ambiguous definitions may spawn confusion. By describing the many definitions and contexts for coherence in the molecular sciences, we aim to enhance understanding and communication in this broad and active area of chemistry.

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