Project description:Quantum information processing (QIP) could revolutionize areas ranging from chemical modeling to cryptography. One key figure of merit for the smallest unit for QIP, the qubit, is the coherence time (T 2), which establishes the lifetime for the qubit. Transition metal complexes offer tremendous potential as tunable qubits, yet their development is hampered by the absence of synthetic design principles to achieve a long T 2. We harnessed molecular design to create a series of qubits, (Ph4P)2[V(C8S8)3] (1), (Ph4P)2[V(β-C3S5)3] (2), (Ph4P)2[V(α-C3S5)3] (3), and (Ph4P)2[V(C3S4O)3] (4), with T 2s of 1-4 μs at 80 K in protiated and deuterated environments. Crucially, through chemical tuning of nuclear spin content in the vanadium(IV) environment we realized a T 2 of ∼1 ms for the species (d 20-Ph4P)2[V(C8S8)3] (1') in CS2, a value that surpasses the coordination complex record by an order of magnitude. This value even eclipses some prominent solid-state qubits. Electrochemical and continuous wave electron paramagnetic resonance (EPR) data reveal variation in the electronic influence of the ligands on the metal ion across 1-4. However, pulsed measurements indicate that the most important influence on decoherence is nuclear spins in the protiated and deuterated solvents utilized herein. Our results illuminate a path forward in synthetic design principles, which should unite CS2 solubility with nuclear spin free ligand fields to develop a new generation of molecular qubits.
Project description:We herein investigate the heterobimetallic lantern complexes [PtVO(SOCR)4] as charge neutral electronic qubits based on vanadyl complexes (S = 1/2) with nuclear spin-free donor atoms. The derivatives with R = Me (1) and Ph (2) give highly resolved X-band EPR spectra in frozen CH2Cl2/toluene solution, which evidence the usual hyperfine coupling with the 51V nucleus (I = 7/2) and an additional superhyperfine interaction with the I = 1/2 nucleus of the 195Pt isotope (natural abundance ca. 34%). DFT calculations ascribe the spin density delocalization on the Pt2+ ion to a combination of π and δ pathways, with the former representing the predominant channel. Spin relaxation measurements in frozen CD2Cl2/toluene-d8 solution between 90 and 10 K yield Tm values (1-6 μs in 1 and 2-11 μs in 2) which compare favorably with those of known vanadyl-based qubits in similar matrices. Coherent spin manipulations indeed prove possible at 70 K, as shown by the observation of Rabi oscillations in nutation experiments. The results indicate that the heavy Group 10 metal ion is not detrimental to the coherence properties of the vanadyl moiety and that Pt-VO lanterns can be used as robust spin-coherent building blocks in materials science and quantum technologies.
Project description:We report on an example of confined magnetic ions with long spin coherence near room temperature. This was achieved by confining single Mn(2+) spins in colloidal semiconductor quantum dots (QDs) and by dispersing the QDs in a proton-spin free matrix. The controlled suppression of Mn-Mn interactions and minimization of Mn-nuclear spin dipolar interactions result in unprecedentedly long phase memory (TM ~ 8 ?s) and spin-lattice relaxation (T1 ~ 10 ms) time constants for Mn(2+) ions at T = 4.5 K, and in electron spin coherence observable near room temperature (TM ~ 1 ?s).
Project description:Single electron spins coupled to multiple nuclear spins provide promising multi-qubit registers for quantum sensing and quantum networks. The obtainable level of control is determined by how well the electron spin can be selectively coupled to, and decoupled from, the surrounding nuclear spins. Here we realize a coherence time exceeding a second for a single nitrogen-vacancy electron spin through decoupling sequences tailored to its microscopic nuclear-spin environment. First, we use the electron spin to probe the environment, which is accurately described by seven individual and six pairs of coupled carbon-13 spins. We develop initialization, control and readout of the carbon-13 pairs in order to directly reveal their atomic structure. We then exploit this knowledge to store quantum states in the electron spin for over a second by carefully avoiding unwanted interactions. These results provide a proof-of-principle for quantum sensing of complex multi-spin systems and an opportunity for multi-qubit quantum registers with long coherence times.
Project description:Spin resonance of individual spin centers allows applications ranging from quantum information technology to atomic-scale magnetometry. To protect the quantum properties of a spin, control over its local environment, including energy relaxation and decoherence processes, is crucial. However, in most existing architectures, the environment remains fixed by the crystal structure and electrical contacts. Recently, spin-polarized scanning tunneling microscopy (STM), in combination with electron spin resonance (ESR), allowed the study of single adatoms and inter-atomic coupling with an unprecedented combination of spatial and energy resolution. We elucidate and control the interplay of an Fe single spin with its atomic-scale environment by precisely tuning the phase coherence time T2 using the STM tip as a variable electrode. We find that the decoherence rate is the sum of two main contributions. The first scales linearly with tunnel current and shows that, on average, every tunneling electron causes one dephasing event. The second, effective even without current, arises from thermally activated spin-flip processes of tip spins. Understanding these interactions allows us to maximize T2 and improve the energy resolution. It also allows us to maximize the amplitude of the ESR signal, which supports measurements even at elevated temperatures as high as 4 K. Thus, ESR-STM allows control of quantum coherence in individual, electrically accessible spins.
Project description:The interaction of single quantum emitters with an optical cavity enables the realization of efficient spin-photon interfaces, an essential resource for quantum networks. The dynamical control of the spontaneous emission rate of quantum emitters in cavities has important implications in quantum technologies, e.g., for shaping the emitted photons' waveform or for driving coherently the optical transition while preventing photon emission. Here we demonstrate the dynamical control of the Purcell enhanced emission of a small ensemble of erbium ions doped into a nanoparticle. By embedding the nanoparticles into a fully tunable high finesse fiber based optical microcavity, we demonstrate a median Purcell factor of 15 for the ensemble of ions. We also show that we can dynamically control the Purcell enhanced emission by tuning the cavity on and out of resonance, by controlling its length with sub-nanometer precision on a time scale more than two orders of magnitude faster than the natural lifetime of the erbium ions. This capability opens prospects for the realization of efficient nanoscale quantum interfaces between solid-state spins and single telecom photons with controllable waveform, for non-destructive detection of photonic qubits, and for the realization of quantum gates between rare-earth ion qubits coupled to an optical cavity.
Project description:The gate fidelity and the coherence time of a quantum bit (qubit) are important benchmarks for quantum computation. We construct a qubit using a single electron spin in an Si/SiGe quantum dot and control it electrically via an artificial spin-orbit field from a micromagnet. We measure an average single-qubit gate fidelity of ∼99% using randomized benchmarking, which is consistent with dephasing from the slowly evolving nuclear spins in the substrate. The coherence time measured using dynamical decoupling extends up to ∼400 μs for 128 decoupling pulses, with no sign of saturation. We find evidence that the coherence time is limited by noise in the 10-kHz to 1-MHz range, possibly because charge noise affects the spin via the micromagnet gradient. This work shows that an electron spin in an Si/SiGe quantum dot is a good candidate for quantum information processing as well as for a quantum memory, even without isotopic purification.
Project description:Isolated solid-state atomic defects with telecom optical transitions are ideal quantum photon emitters and spin qubits for applications in long-distance quantum communication networks. Prototypical telecom defects, such as erbium, suffer from poor photon emission rates, requiring photonic enhancement using resonant optical cavities. Moreover, many of the traditional hosts for erbium ions are not amenable to direct incorporation with existing integrated photonics platforms, limiting scalable fabrication of qubit-based devices. Here, we present a scalable approach toward CMOS-compatible telecom qubits by using erbium-doped titanium dioxide thin films grown atop silicon-on-insulator substrates. From this heterostructure, we have fabricated one-dimensional photonic crystal cavities demonstrating quality factors in excess of 5 × 104 and corresponding Purcell-enhanced optical emission rates of the erbium ensembles in excess of 200. This easily fabricated materials platform represents an important step toward realizing telecom quantum memories in a scalable qubit architecture compatible with mature silicon technologies.
Project description:Conventional superconductors were long thought to be spin inert; however, there is now increasing interest in both (the manipulation of) the internal spin structure of the ground-state condensate, as well as recently observed long-lived, spin-polarized excitations (quasiparticles). We demonstrate spin resonance in the quasiparticle population of a mesoscopic superconductor (aluminium) using novel on-chip microwave detection techniques. The spin decoherence time obtained (∼100 ps), and its dependence on the sample thickness are consistent with Elliott-Yafet spin-orbit scattering as the main decoherence mechanism. The striking divergence between the spin coherence time and the previously measured spin imbalance relaxation time (∼10 ns) suggests that the latter is limited instead by inelastic processes. This work stakes out new ground for the nascent field of spin-based electronics with superconductors or superconducting spintronics.
Project description:X-ray reflectometry (XRR) is a powerful tool for probing the structural characteristics of nanoscale films and layered structures, which is an important field of nanotechnology and is often used in semiconductor and optics manufacturing. This study introduces a novel approach for conducting quantitative high-resolution millisecond monochromatic XRR measurements. This is an order of magnitude faster than in previously published work. Quick XRR (qXRR) enables real time and in situ monitoring of nanoscale processes such as thin film formation during spin coating. A record qXRR acquisition time of 1.4 ms is demonstrated for a static gold thin film on a silicon sample. As a second example of this novel approach, dynamic in situ measurements are performed during PMMA spin coating onto silicon wafers and fast fitting of XRR curves using machine learning is demonstrated. This investigation primarily focuses on the evolution of film structure and surface morphology, resolving for the first time with qXRR the initial film thinning via mass transport and also shedding light on later thinning via solvent evaporation. This innovative millisecond qXRR technique is of significance for in situ studies of thin film deposition. It addresses the challenge of following intrinsically fast processes, such as thin film growth of high deposition rate or spin coating. Beyond thin film growth processes, millisecond XRR has implications for resolving fast structural changes such as photostriction or diffusion processes.