Telecom-Luminescent and Room Temperature Coherent Tetrathiafulvalene-Based Qubits in Spin-Rich Solids
Lauren E. McNamara, Ai-Mei Zhou, Alexandra Krupinski, Yin Yang, Sophie W. Anferov, Christopher Melnychuk, Matthew D. Krzyaniak, Michael R. Wasielewski, Jan-Niklas Boyn, Richard D. Schaller, Lei Sun, John Stuart Anderson
One of the main challenges facing quantum information science (QIS) is the development of robust qubits that can be operated under ambient conditions. Current state-of-the-art anionic nitrogen-vacancy center (NV – ) defect qubits are robust enough to be operated at room temperature but lack scalability and tunability. These are areas where molecular qubits excel, although, in contrast, they typically suffer from poor air stability and fast decoherence at elevated temperatures and in magnetically noisy environments. Organic-based systems offer possible advantages to this end, although examples retaining room temperature coherence are still rare. Furthermore, most organic-based systems lack optical transitions similar to NV – centers that could allow for optical initialization and readout. Here we report two new organic-based qubit candidates that demonstrate room temperature coherence in nuclear and electron spin-rich environments. These qubits luminesce far into the near-infrared (NIR, 700–1700 nm) and telecom (∼1260–1625 nm) regions, ideal for biological sensing and communications applications, respectively.
One of the main challenges facing quantum information science (QIS) is the development of robust qubits that can be operated under ambient conditions. Current state-of-the-art anionic nitrogen-vacancy center (NV – ) defect qubits are robust enough to be operated at room temperature but lack scalability and tunability. These are areas where molecular qubits excel, although, in contrast, they typically suffer from poor air stability and fast decoherence at elevated temperatures and in magnetically noisy environments. Organic-based systems offer possible advantages to this end, although examples retaining room temperature coherence are still rare. Furthermore, most organic-based systems lack optical transitions similar to NV – centers that could allow for optical initialization and readout. Here we report two new organic-based qubit candidates that demonstrate room temperature coherence in nuclear and electron spin-rich environments. These qubits luminesce far into the near-infrared (NIR, 700–1700 nm) and telecom (∼1260–1625 nm) regions, ideal for biological sensing and communications applications, respectively.
We propose a quantum repeater architecture that can operate under ambient conditions. Our proposal builds on recent progress towards non-cryogenic spin-photon interfaces based on nitrogen-vacancy centers, which have excellent spin coherence times even at room temperature, and optomechanics, which allows to avoid phonon-related decoherence and also allows the emitted photons to be in the telecom band. We apply the photon number decomposition method to quantify the fidelity and the efficiency of entanglement established between two remote electron spins. We describe how the entanglement can be stored in nuclear spins and extended to long distances via quasi-deterministic entanglement swapping operations involving the electron and nuclear spins. We furthermore propose schemes to achieve high-fidelity readout of the spin states at room temperature using the spin-optomechanics interface. Our work shows that long-distance quantum networks made of solid-state components that operate at room temperature are within reach of current technological capabilities.
This work investigates the applicability of the nitrogen-vacancy (NV) defect center in diamond for quantum computation and metrology purposes. The NV center is a molecule like defect in the diamond lattice which is optically active and possesses an electron spin in its ground state. The spin can be used as a quantum bit and as a field sensor. The NV center has three major properties enabling individual control of single defects. Its optical properties depend on the spin state, the spin can be polarized optically and the spin state has an exceptionally long lifetime. Single NV centers can be controlled by optical and microwave radiation. Generally, the research on individually controllable quantum systems is not only motivated by quantum computation and communication. With the ongoing miniaturization nowadays electronic and electro-optic devices will soon reach the limit of single quantum building blocks. While in these applications the full complexity of single quantum systems might not be needed, small sensors based on single atoms or molecules might very well take advantage of the susceptibility of quantum coherences to environmental conditions. Major challenges for all approaches towards single quantum system control are the individual addressing, the measurement of the quantum state and the protection of quantum coherence from environmental noise. Today, there is a variety of systems (including the NV center) that allow control on the single quantum level. These are for example single photons, single ions and atoms in traps, single spins in semiconductors or single molecules in solid state systems. Rather mesoscopic examples are superconducting devices, nanomechanical oscillators or surface plasmon polaritons. Regarding the NV center it has been shown that the magnetic moment of its electron spin allows individual sensing and coupling to other surrounding electron and nuclear spins. Especially single nuclear spins were shown to be exceptional quantum memories. In this work small quantum registers of up to 5 spins have been used to test major requirements for a feasible quantum processor. Therefore, mainly artificially created high purity diamond samples with controlled spin and impurity concentration were used. The NV centers were either grown in or created via ion implantation techniques in a controlled fashion. As a first requirement for quantum computation entanglement among up to three spins has been generated and was verified by quantum state tomography. This proves the access of the full Hilbert space. Especially, entanglement among nuclear spins was very long-living. In further experiments this processor was used for first quantum algorithms like super-dense coding and the Deutsch algorithm. In addition, this work demonstrates new methods to initialize nuclear spin qubits into a desired quantum state. This is particularly important as improper initialization inhibits quantum computation. One of these methods is related to dynamic nuclear spin polarization and the other to measurement based state preparation. Nuclear spins in the diamond lattice originate mainly from the C-13 isotope. By artificially altering its content the influence on the NV center spin was investigated. The coherence times of the NV center were increasing inversely with the nuclear spin density. Even increasing nuclear spin density to offer more nuclear spin qubits to an operational quantum register was possible. As an alternative route of scaling up the quantum register pairs of closely spaced NV centers were investigated. For the first time two qubit gates among two NV centers mediated by magnetic dipolar coupling have been realized. Furthermore the sensing ability was demonstrated by measuring the relative distance of the two centers (10 nm) with sub-nm precision. Eventually, this work contains new insight into the electronically excited state of the NV center which allowed a more advanced control of the electron and nuclear spins. A comparably high magnetic field was used to decouple electron and nuclear spins. Finally, this allowed quantum nondemolition measurements on single nuclear spins which manifests in the observation of quantum jumps. The new insight was used to drastically improve the performance of quantum state readout. Summarizing, it was shown that single NV centers and proximal nuclear spins form versatile small quantum registers which can be interconnected with neighboring such NV quantum registers. Although the number of qubits used in this work is still small the experimental results propose a way of how to proceed when building a quantum computer. Regarding quantum metrology, however, the use of such a small register which can sense fields and store and process the results would already outperform a single NV electron spin by orders of magnitude.
Solid-state color centers with manipulatable spin qubits and telecom-ranged fluorescence are ideal platforms for quantum communications and distributed quantum computations. In this work, we coherently control the nitrogen-vacancy (NV) center spins in silicon carbide at room temperature, in which telecom-wavelength emission is detected. We increase the NV concentration sixfold through optimization of implantation conditions. Hence, coherent control of NV center spins is achieved at room temperature, and the coherence time T_{2} can be reached to around 17.1 μs. Furthermore, an investigation of fluorescence properties of single NV centers shows that they are room-temperature photostable single-photon sources at telecom range. Taking advantage of technologically mature materials, the experiment demonstrates that the NV centers in silicon carbide are promising platforms for large-scale integrated quantum photonics and long-distance quantum networks.
Molecular qubits, owing to their designability and tunability, have emerged as fundamental units for quantum technologies. Among them, molecular qubit frameworks (MQFs) offer unique advantages in long-range ordered lattices and microporosity that provide well-defined phonon environments and guest-tunable spin dynamics. These features greatly enhance qubit performance and enable room temperature quantum operations, holding promise for quantum sensing applications. Herein, we compare the qubit performance of 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) and tetrathiafulvalene tetrabenzoic acid (H4TTFTB), which form stable radicals upon spontaneous oxidation in the air. We found that optical phonons dominate spin relaxation in HHTP, whereas H4TTFTB exhibits stronger spin-orbit coupling and higher acoustic phonon population that account for its shorter spin relaxation time. Meanwhile, H4TTFTB features a nuclear-spin-free core and in turn a prolonged phase memory time, making it a favorable qubit candidate. Furthermore, we synthesized three MQFs using H4TTFTB as the ligand, which not only retain the superior room-temperature qubit performance but also possess porous channels, establishing a viable platform for future quantum information applications.
The key challenge in experimental quantum information science is to identify isolated quantum mechanical systems with long coherence times that can be manipulated and coupled together in a scalable fashion. We describe the coherent manipulation of an individual electron spin and nearby individual nuclear spins to create a controllable quantum register. Using optical and microwave radiation to control an electron spin associated with the nitrogen vacancy (NV) color center in diamond, we demonstrated robust initialization of electron and nuclear spin quantum bits (qubits) and transfer of arbitrary quantum states between them at room temperature. Moreover, nuclear spin qubits could be well isolated from the electron spin, even during optical polarization and measurement of the electronic state. Finally, coherent interactions between individual nuclear spin qubits were observed and their excellent coherence properties were demonstrated. These registers can be used as a basis for scalable, optically coupled quantum information systems.
Stable quantum bits, capable both of storing quantum information for macroscopic time scales and of integration inside small portable devices, are an essential building block for an array of potential applications. We demonstrate high-fidelity control of a solid-state qubit, which preserves its polarization for several minutes and features coherence lifetimes exceeding 1 second at room temperature. The qubit consists of a single (13)C nuclear spin in the vicinity of a nitrogen-vacancy color center within an isotopically purified diamond crystal. The long qubit memory time was achieved via a technique involving dissipative decoupling of the single nuclear spin from its local environment. The versatility, robustness, and potential scalability of this system may allow for new applications in quantum information science.