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PreprintarXiv licencearXiv

Dark state preparation in a zero-field-split molecular triplet

  • Maria Pfahler
  • Andrea Donarini
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Abstract

We propose a protocol to prepare and probe dark states in a single-molecule electron spin resonance based on atomic force microscopy (ESR-AFM), thus extending existing techniques developed to address Rabi oscillations. To this end, we simulate in analogy to atomic physics the coherent manipulation of a three-level system in the V-configuration using a multifrequency magnetic field. More specifically, we consider a neutral molecule with a zero-field-split (ZFS) first excited triplet and analyze within a pump-probe scheme the dynamics of the total triplet population. In the triplet subspace, the dark state is a coherent superposition formed by two ZFS states which does not evolve in time despite a continuous resonant driving towards the third one. We characterize the properties of this state comparing it to its fully incoherent counterpart. Within a density-matrix formalism for open systems, we then compute the expected dark state signatures both for ideal scenarios and for the realistic parameterization of ESR-AFM on pentacene.

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Cite

BibTeXRIS
BibTeX
@misc{pfahler2026dark,
  title = {{Dark state preparation in a zero-field-split molecular triplet}},
  author = {Maria Pfahler and Andrea Donarini},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2610.18661},
  eprint = {2610.18661},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2610.18661},
}
RIS
TY  - UNPB
TI  - Dark state preparation in a zero-field-split molecular triplet
AU  - Maria Pfahler
AU  - Andrea Donarini
PY  - 2026
DA  - 2026/10/13
PB  - arXiv
DO  - 10.48550/arxiv.2610.18661
UR  - https://arxiv.org/abs/2610.18661
AB  - We propose a protocol to prepare and probe dark states in a single-molecule electron spin resonance based on atomic force microscopy (ESR-AFM), thus extending existing techniques developed to address Rabi oscillations. To this end, we simulate in analogy to atomic physics the coherent manipulation of a three-level system in the V-configuration using a multifrequency magnetic field. More specifically, we consider a neutral molecule with a zero-field-split (ZFS) first excited triplet and analyze within a pump-probe scheme the dynamics of the total triplet population. In the triplet subspace, the dark state is a coherent superposition formed by two ZFS states which does not evolve in time despite a continuous resonant driving towards the third one. We characterize the properties of this state comparing it to its fully incoherent counterpart. Within a density-matrix formalism for open systems, we then compute the expected dark state signatures both for ideal scenarios and for the realistic parameterization of ESR-AFM on pentacene.
ER  -