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Physical Chemistry Chemical Physics

Chromium( iii )-based potential molecular quantum bits with long coherence times

Samuel Lenz, Heiko Bamberger, Philipp P. Hallmen, Yannick M. Thiebes, S. Otto, Katja Heinze, Joris van Slageren

Published Jan 1, 2019• 41 citations
Publisher

Abstract

Molecular quantum bits based on copper(ii) or vanadium(iv) have been shown to possess long coherence times on multiple occasions. In contrast, studies in which non-spin-½ ions are employed are relatively scarce. High-spin ions provide additional states that can be used to encode further quantum bits. Furthermore, an optical rather than a microwave readout of molecular quantum bits is highly desirable, because in principle it could allow addressing at the single quantum bit level. The chromium(iii) complex [Cr(ddpd)2]3+ (ddpd = N,N'-dimethyl-N,N'-dipyridine-2-yl-pyridine-2,6-diamine) combines both the large spin (S = 3/2) and optical activity (strong, long lived luminescence). Here we demonstrate that the compound possesses coherence times of up to 8.4(1) μs, which are much longer (at least three times) than those for other chromium(iii)-based compounds. On the other hand, it is proved to be impossible to read out or influence the quantum state by optical means, underlining that further work is needed in this direction.

DOI
10.1039/c9cp00745h

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The coordination complexes of Yb(III) exhibit some of the longest spin coherence times among 4f compounds, making them a promising platform for molecular quantum technologies. While spin-phonon relaxation remains a limiting factor for coherence times even at low temperature, its control through chemical design has the potential to push these spin qubits prototypes beyond current limits. With the aim of providing insights on how to chemically control spin-phonon relaxation, we here present a full ab initio study of spin-phonon dynamics for three Yb(III) molecules exhibiting minimal chemical differences, yet quantitatively different spin relaxation times. Results show that low-temperature relaxation is governed by Raman processes triggered by a small group of largely delocalized low-energy phonons. The analysis of these contributions highlights that the modulation of spin-phonon coupling by molecular structure modifications beyond the first coordination shell are highly non-trivial in nature and hard to rationalize in simple chemical terms. These findings call for a conceptual step change from the attempt to use simple magneto-structural correlations to interpret the effect of molecular structural modifications on spin-phonon relaxation, and present predictive first-principles frameworks as a potential driving force of future chemical design strategies

cond-mat.mtrl-sciCross-listedarXiv:2603.12160•Mar 13, 2026
Molecular quantum bits based on copper(ii) or vanadium(iv) have been shown to possess long coherence times on multiple occasions. In contrast, studies in which non-spin-½ ions are employed are relatively scarce. High-spin ions provide additional states that can be used to encode further quantum bits. Furthermore, an optical rather than a microwave readout of molecular quantum bits is highly desirable, because in principle it could allow addressing at the single quantum bit level. The chromium(iii) complex [Cr(ddpd)2]3+ (ddpd = N,N'-dimethyl-N,N'-dipyridine-2-yl-pyridine-2,6-diamine) combines both the large spin (S = 3/2) and optical activity (strong, long lived luminescence). Here we demonstrate that the compound possesses coherence times of up to 8.4(1) μs, which are much longer (at least three times) than those for other chromium(iii)-based compounds. On the other hand, it is proved to be impossible to read out or influence the quantum state by optical means, underlining that further work is needed in this direction.
The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ions (REIs) are suitable candidates for QIP protocols due to their extraordinary photo-physical and magnetic quantum properties such as long optical and spin coherence lifetimes (T2T_2T2​). However, molecules incorporating REIs, despite having advantageous properties such as atomically exact quantum tunability, inherent scalability, and large portability, have not yet been studied for QIP applications. As a first testimony of the usefulness of REI molecules for optical QIP applications, we demonstrate in this study that narrow spectral holes can be burned in the inhomogeneously broadened 5^55D0→7_0\to^70​→7F0_00​ optical transition of a binuclear Eu(III) complex, rendering a homogeneous linewidth (ΓhΓ_hΓh​) = 22 ±\pm± 1 MHz, which translates as T2=14.5T_2 = 14.5T2​=14.5 ±\pm± 0.7 ns at 1.4 K. Moreover, long-lived spectral holes are observed, demonstrating efficient polarization of Eu(III) ground state nuclear spins, a fundamental requirement for all-optical spin initialization and addressing. These results elucidate the usefulness of REI-based molecular complexes as versatile coherent light-spin interfaces for applications in quantum communications and processing.
Efforts to harness quantum hardware relying on quantum mechanical principles have been steadily progressing. The search for novel material platforms that could spur the progress by providing new functionalities for solving the outstanding technological problems is however still active. Any physical property presenting two distinct energy states that can be found in a long-lived superposition state can serve as a quantum bit (qubit), the basic information processing unit in quantum technologies. Molecular systems that can feature electron and/or nuclear spin states together with optical transitions are one of the material platforms that can serve as optically addressable qubits. The attractiveness of molecular systems for quantum technologies relies on the fact that molecular structures of atomically defined nature can be obtained in endless diversity of chemical compositions. Crucially, by harnessing the molecular design protocols, the optical and spin (electronic and nuclear) properties of molecules can be tailored, aiding the design of optically addressable spin qubits and quantum sensors. In this contribution, we present a concise and collective discussion of optically addressable spin-bearing molecules - namely, organic molecules, transition metal (TM) and rare-earth ion (REI) complexes - and highlight recent results such as chemical tuning of optical and electron spin quantum coherence, optical spin initialization and readout, intramolecular quantum teleportation, optical coherent storage, and photonic-enhanced optical addressing. We envision that optically addressable spin-carrying molecules could become a scalable building block of quantum hardware for applications in the fields of quantum sensing, quantum communication and quantum computing.
Abstract The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ion (REI)- based molecular systems, whose quantum properties could be tuned taking advantage of molecular engineering strategies, are one of the systems actively pursued for the implementation of QIP schemes. Herein, we demonstrate the efficient polarization of 2 ground-state nuclear spins—a fundamental requirement for all-optical spin initialization and addressing—in a binuclear Eu(III) complex, featuring inhomogeneously broadened 5D0→7 F0 optical transition. At 1.4 K, long-lived spectral holes have been burnt in the transition: homogeneous linewidth (Γh) = 22 +/- 1 MHz, which translates as optical coherence lifetime (T2opt) = 14.5 +/- 0.7 ns, and ground-state spin population lifetime (T1spin) = 1.6 +/- 0.4 s have been obtained. The results presented in this study are a progressive step towards the realization of molecule-based coherent light-spin QIP interfaces.
ingle luminescent molecules provide a unique approach in the development of quantum technologies utilizing single photon sources. This includes quantum metrology by using a molecule’s sensitivity of its emission and magnetic properties to the local environment. In this thesis, we present our investigation of the optical properties of several different classes of luminescent molecules. We begin by providing some theoretical background of single quantum emitters as well as a brief description of the experimental methodologies and equipment. Next, we present an optical investigation of an ensemble of iron phthalocyanines molecules. This molecule possesses a ground state triplet, which is a desirable property for optically active spin qubits, but has a very weak optical emission. Diffraction limited spots displayed photo-instability in the form of blinking and irreversible bleaching. In ensemble form however, their optical stability allowed us to identify a possible Raman peak where we calculated the associated phonon frequency. Next, we present our single molecule study of vanadium phthalocyanine. This molecule has been documented as displaying very long spin coherence times even at room temperatures. We confirmed the presence of a single molecule by measuring the second order correlation function. Additionally, we looked at the intensity and spectral response as a function of the excitation laser polarization. The spectrum was fitted to a two Gaussian function, which may correspond to the two dipole transitions as suggested by theoretical calculations. Lastly, we looked at the optical properties of rare earth europium complexes known for having very sharp optical transitions in the emission spectrum, with each having varying levels of sensitivity to the local environment. Motivated by techniques to investigate non-radiative decay channels, we looked at the optical response of four different europium complexes under two 1 µs pulses of 515 nm laser separated by 1 µs. Each displayed a very different results and allowed us to identify the best candidates for single molecule studies. Finally, we looked at the emission spectrum as well as the optical response under a 6 µs long pulse using time-correlation single photon spectroscopy.
Molecular electron spin qubits with optical manipulation schemes are some of the most promising candidates for modern quantum technologies. Key values that determine a compound’s viability for optical-spin initialization and readout include its singlet-triplet gap and zero-field splitting (ZFS) parameters. Generally, these values are very small in magnitude and are thus difficult to reproduce with theoretical methods. Here we study a previously identified optically addressable molecular qubit, (C6F5)3trenVCNtBu (tren = tris(2-aminoethyl)amine), using the complete active space self-consistent field (CASSCF) and post-CASSCF methods (CASPT2, MC-PDFT, and HMC-PDFT). Of those methods, we successfully reproduce the singlet-triplet gap and ZFS parameters with reasonable accuracy using 0.5 HMC-PDFT and CASPT2. Four additional V3+ complexes with differing ligands were also investigated. We found that the ligands have minimal effect on the spin properties of the molecule and propose them to be optically addressable qubit candidates. These potential qubits are further analyzed in terms of ab initio ligand field theory (AILFT) to understand the influence of the ligands on the singlet-triplet gap and ZFS parameters.
The coordination complexes of Yb(III) exhibit some of the longest spin coherence times among 4f compounds, making them a promising platform for molecular quantum technologies. While spin-phonon relaxation remains a limiting factor for coherence times even at low temperature, its control through chemical design has the potential to push these spin qubits prototypes beyond current limits. With the aim of providing insights on how to chemically control spin-phonon relaxation, we here present a full ab initio study of spin-phonon dynamics for three Yb(III) molecules exhibiting minimal chemical differences, yet quantitatively different spin relaxation times. Results show that low-temperature relaxation is governed by Raman processes triggered by a small group of largely delocalized low-energy phonons. The analysis of these contributions highlights that the modulation of spin-phonon coupling by molecular structure modifications beyond the first coordination shell are highly non-trivial in nature and hard to rationalize in simple chemical terms. These findings call for a conceptual step change from the attempt to use simple magneto-structural correlations to interpret the effect of molecular structural modifications on spin-phonon relaxation, and present predictive first-principles frameworks as a potential driving force of future chemical design strategies