Dense pentacene cocrystal demonstrates room-temperature coherent control

Abstract

Maximizing the number of addressable spins within a fixed volume can improve ensemble quantum sensor sensitivity, but dense packing usually increases dipolar interactions and excited-state transport, shortening coherence and suppressing optical readout. Here we report a 2:1 cocrystal of 6,13-dihydropentacene and pentacene (DHP/Pc) containing 33.3 mol% pentacene (3.3×10⁵ ppm; 9.51×10²⁰ cm⁻³), a volumetric spin-site density more than two orders of magnitude above previous benchmarks, NV-diamond and pentacene-doped p-terphenyl (PDP). Despite this density, DHP/Pc exhibits microsecond spin coherence, room-temperature optically detected magnetic resonance and coherent control. Time-resolved measurements indicate that the long-lived triplet population is generated predominantly by intersystem crossing and exhibits strong, non-thermal sublevel polarization. Density-functional theory calculations further suggest that the native cocrystal geometry weakens electronic coupling between neighboring pentacenes, while the higher DHP triplet energy creates a barrier to triplet migration. These results identify molecular packing and coformer triplet energetics as complementary design parameters for preserving coherence in high spin-site density systems, demonstrating cocrystallization as a promising route to dense, optically addressable spin materials for room-temperature ensemble quantum sensing.

Optical Detection of Coherent Nuclear Spin Control in a Molecular System at Room Temperature
Eoin O. Irving, Ziqiu Huang, Max Attwood +2
arXiv12 Oct 2026PreprintCC BY 4.0Full textPhysical chemistry Quantum physics & quantum informationarXiv
Plasmon-assisted coherent control of a four-level semiconductor quantum dot: operating window and fidelity limits
Ameenah Al-Ahmadi
Optics Express2 Nov 2026Peer-reviewedLicence not statedOptics & photonicsCrossref
Coherent control of spinmons
Johanne Bratland Tjernshaugen, Florinda Viñas Boström, Jeroen Danon +3
arXiv29 Oct 2026PreprintarXiv licenceFull textCondensed matter Quantum physics & quantum informationarXiv
Chiral Unidirectional Resonances Enabled by Complete Coherent Radiation Control
Keren Wang, Wei Wang
arXiv1 Nov 2026PreprintarXiv licenceFull textOptics & photonicsarXiv
Coherent control of subradiant excitations in atomic rings
Milena Djatchkova, Igor Lesanovsky, Beatriz Olmos
arXiv4 Nov 2026PreprintCC BY-NC-SA 4.0Full textQuantum physics & quantum informationarXiv

Cite

BibTeX RIS

BibTeX

@misc{dsouza2026dense,
  title = {{Dense pentacene cocrystal demonstrates room-temperature coherent control}},
  author = {Noella D'Souza and Guangzhao Chen and Madhur Parashar and Wern Ng and Brandon Wallace and Tatiana Lindahl and Tanner S. Volek and Lam Lam and Joseph Garrett and Emanuel Druga and Sean T. Roberts and Jeffrey Reimer and Harpreet Singh and Liang Z. Tan and Riccardo Montis and Ashok Ajoy},
  howpublished = {arXiv},
  year = {2026},
  month = sep,
  doi = {10.48550/arxiv.2609.28912},
  eprint = {2609.28912},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2609.28912},
  note = {CC BY 4.0},
}

RIS

TY  - UNPB
TI  - Dense pentacene cocrystal demonstrates room-temperature coherent control
AU  - Noella D'Souza
AU  - Guangzhao Chen
AU  - Madhur Parashar
AU  - Wern Ng
AU  - Brandon Wallace
AU  - Tatiana Lindahl
AU  - Tanner S. Volek
AU  - Lam Lam
AU  - Joseph Garrett
AU  - Emanuel Druga
AU  - Sean T. Roberts
AU  - Jeffrey Reimer
AU  - Harpreet Singh
AU  - Liang Z. Tan
AU  - Riccardo Montis
AU  - Ashok Ajoy
PY  - 2026
DA  - 2026/09/24
PB  - arXiv
DO  - 10.48550/arxiv.2609.28912
UR  - https://arxiv.org/abs/2609.28912
AB  - Maximizing the number of addressable spins within a fixed volume can improve ensemble quantum sensor sensitivity, but dense packing usually increases dipolar interactions and excited-state transport, shortening coherence and suppressing optical readout. Here we report a 2:1 cocrystal of 6,13-dihydropentacene and pentacene (DHP/Pc) containing 33.3 mol% pentacene (3.3×10^5 ppm; 9.51×10^20 cm^−3), a volumetric spin-site density more than two orders of magnitude above previous benchmarks, NV-diamond and pentacene-doped p-terphenyl (PDP). Despite this density, DHP/Pc exhibits microsecond spin coherence, room-temperature optically detected magnetic resonance and coherent control. Time-resolved measurements indicate that the long-lived triplet population is generated predominantly by intersystem crossing and exhibits strong, non-thermal sublevel polarization. Density-functional theory calculations further suggest that the native cocrystal geometry weakens electronic coupling between neighboring pentacenes, while the higher DHP triplet energy creates a barrier to triplet migration. These results identify molecular packing and coformer triplet energetics as complementary design parameters for preserving coherence in high spin-site density systems, demonstrating cocrystallization as a promising route to dense, optically addressable spin materials for room-temperature ensemble quantum sensing.
ER  -

Abstract

Related

Cite