Enhancing the Optically Detected Magnetic Resonance Signal of Organic Molecular Qubits

Poh, Yong Rui; Yuen-Zhou, Joel

doi:10.1021/acscentsci.4c01632

Enhancing the Optically Detected Magnetic Resonance Signal of Organic Molecular Qubits

Journal Article · Thu Jan 02 04:00:00 EST 2025 · ACS Central Science

DOI:https://doi.org/10.1021/acscentsci.4c01632· OSTI ID:2999597

Poh, Yong Rui ^[1]; ^[1]

University of California San Diego, La Jolla, CA (United States)

In quantum information science and sensing, electron spins are often purified into a specific polarization through an optical-spin interface, a process known as optically detected magnetic resonance (ODMR). Diamond-NV centers and transition metals are both excellent platforms for these so-called color centers, while metal-free molecular analogues are also gaining popularity for their extended polarization lifetimes, milder environmental impacts, and reduced costs. In our earlier attempt at designing such organic high-spin π-diradicals, we proposed to spin-polarize by shelving triplet M_S = ±1 populations as singlets. This was recently verified by experiments albeit with low ODMR contrasts of <1% at temperatures above 5 K. In this work, we propose to improve the ODMR signal by moving singlet populations back into the triplet M_S = 0 sublevel, designing a true carbon-based molecular analogue to the NV center. Our proposal is based upon transition-orbital and group-theoretical analyses of beyond-nearest-neighbor spin–orbit couplings, which are further confirmed by ab initio calculations of a realistic trityl-based radical dimer. Microkinetic analyses point toward high ODMR contrasts of around 30% under experimentally feasible conditions, a stark improvement from previous works. Finally, in our quest toward ground-state optically addressable molecular spin qubits, we exemplify how our symmetry-based design avoids Zeeman-induced singlet–triplet mixings, setting the scene for realizing electron spin qubit gates.

View Accepted Manuscript (DOE)

Research Organization:: California Institute of Technology, Pasadena, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0022089

OSTI ID:: 2999597

Journal Information:: ACS Central Science, Journal Name: ACS Central Science Journal Issue: 1 Vol. 11; ISSN 2374-7951; ISSN 2374-7943

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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