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arXiv:2312.05246 · Nature Communications

SUPER and femtosecond spin-conserving coherent excitation of a tin-vacancy color center in diamond

Cem Güney Torun, Mustafa Gökçe, Thomas K. Bracht, Mariano Isaza-Monsalve, Sarah Benbouabdellah, Özgün Ozan Nacitarhan, Marco E. Stucki, Domenica Bermeo Alvaro, Matthew Markham, Tommaso Pregnolato, J. H. D. Munns, Gregor Pieplow, Doris E. Reiter, Tim Schröder

Published Mar 2, 2026• 4 citations
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Abstract

The coherent excitation of an optically active spin system is one of the key elements in the engineering of a spin-photon interface. Using the novel SUPER scheme, we coherently control the main optical transition of a tin-vacancy color center in diamond with nonresonant ultrashort optical pulses. Furthermore, we implement a femtosecond control scheme using resonant pulses for achieving record short quantum gates applied to diamond color centers. We simulate the applicability of the SUPER scheme to spin qubits and experimentally investigate spin mixing. Finally, we propose a spin-spin entanglement scheme in a scenario where the excitation with broadband pulses is incompatible with spin-selective excitation. The employed ultrafast quantum gates open up a new regime of quantum control with solid-state color centers, enabling multi-gate operations and efficient spectral filtering of the excitation laser from deterministically prepared coherent photons.

DOI
10.1038/s41467-026-69911-1

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The coherent excitation of an optically active spin system is one of the key elements in the engineering of a spin-photon interface. Using the novel SUPER scheme, we coherently control the main optical transition of a tin-vacancy color center in diamond with nonresonant ultrashort optical pulses. Furthermore, we implement a femtosecond control scheme using resonant pulses for achieving record short quantum gates applied to diamond color centers. We simulate the applicability of the SUPER scheme to spin qubits and experimentally investigate spin mixing. Finally, we propose a spin-spin entanglement scheme in a scenario where the excitation with broadband pulses is incompatible with spin-selective excitation. The employed ultrafast quantum gates open up a new regime of quantum control with solid-state color centers, enabling multi-gate operations and efficient spectral filtering of the excitation laser from deterministically prepared coherent photons.
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Optically addressable spin defects in solid-state materials have shown great potential for applications ranging from metrology to quantum information processing. Many of these experiments require a detailed understanding of the full Hamiltonian dynamics in order to develop precise quantum control. Here we use picosecond resonant optical pulses to investigate the coherent orbital and spin dynamics of the nitrogen-vacancy (NV) center in diamond, over timescales spanning six orders of magnitude. We implement an ultrafast optical pump-probe technique to study the NV center’s orbital-doublet, spin-triplet excited state at cryogenic temperatures (T < 20 K), where the excited state becomes stable and optically coherent with the ground state. This technique, coupled with optical polarization selection rules, allows us to probe the coherent orbital dynamics of the NV center’s excited state [1]. These experiments reveal dynamics on femtosecond to nanosecond timescales due to the interplay between the ground and excited state orbital levels. This all-optical technique also provides a method to dynamically control the spin state of the NV center by harnessing the excited state structure. Through studying the spin dynamics of the NV center with coherent pulses of light, we are able to rotate the spin state on sub-nanosecond timescales. Furthermore, by tuning the excited-state spin Hamiltonian with an external magnetic eld, we demonstrate arbitrary-axis spin rotations through controlled unitary evolution of the spin state. Extending this to the full excited-state manifold, we develop a time-domain quantum tomography technique to precisely map the NV center’s excited state Hamiltonian. These techniques generalize to other systems and can be a powerful tool in characterizing and controlling qubits in other optically addressable spin systems.