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Super-resolution techniques to simulate electronic spectra of large molecular systems

Author

Listed:
  • Matthias Kick

    (Massachusetts Institute of Technology)

  • Ezra Alexander

    (Massachusetts Institute of Technology)

  • Anton Beiersdorfer

    (Technical University of Munich)

  • Troy Voorhis

    (Massachusetts Institute of Technology)

Abstract

An accurate treatment of electronic spectra in large systems with a technique such as time-dependent density functional theory is computationally challenging. Due to the Nyquist sampling theorem, direct real-time simulations must be prohibitively long to achieve suitably sharp resolution in frequency space. Super-resolution techniques such as compressed sensing and MUSIC assume only a small number of excitations contribute to the spectrum, which fails in large molecular systems where the number of excitations is typically very large. We present an approach that combines exact short-time dynamics with approximate frequency space methods to capture large narrow features embedded in a dense manifold of smaller nearby peaks. We show that our approach can accurately capture narrow features and a broad quasi-continuum of states simultaneously, even when the features overlap in frequency. Our approach is able to reduce the required simulation time to achieve reasonable accuracy by a factor of 20-40 with respect to standard Fourier analysis and shows promise for accurately predicting the whole spectrum of large molecules and materials.

Suggested Citation

  • Matthias Kick & Ezra Alexander & Anton Beiersdorfer & Troy Voorhis, 2024. "Super-resolution techniques to simulate electronic spectra of large molecular systems," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52368-5
    DOI: 10.1038/s41467-024-52368-5
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    References listed on IDEAS

    as
    1. Tamar Goldzak & Alexandra R. McIsaac & Troy Van Voorhis, 2021. "Colloidal CdSe nanocrystals are inherently defective," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    2. Takumi Kinoshita & Kazuteru Nonomura & Nam Joong Jeon & Fabrizio Giordano & Antonio Abate & Satoshi Uchida & Takaya Kubo & Sang Il Seok & Mohammad Khaja Nazeeruddin & Anders Hagfeldt & Michael Grätzel, 2015. "Spectral splitting photovoltaics using perovskite and wideband dye-sensitized solar cells," Nature Communications, Nature, vol. 6(1), pages 1-8, December.
    3. Nicola Gasparini & Franco V. A. Camargo & Stefan Frühwald & Tetsuhiko Nagahara & Andrej Classen & Steffen Roland & Andrew Wadsworth & Vasilis G. Gregoriou & Christos L. Chochos & Dieter Neher & Michae, 2021. "Adjusting the energy of interfacial states in organic photovoltaics for maximum efficiency," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    4. Irena Orović & Vladan Papić & Cornel Ioana & Xiumei Li & Srdjan Stanković, 2016. "Compressive Sensing in Signal Processing: Algorithms and Transform Domain Formulations," Mathematical Problems in Engineering, Hindawi, vol. 2016, pages 1-16, October.
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