arXiv subjects

John J. L. Morton

Publications and source records attributed to John J. L. Morton.

90 records · Page 5Linked to original sources

arXiv2010

Storage of multiple coherent microwave excitations in an electron spin ensemble

Electron and nuclear spins have good coherence times and an ensemble of spins is a promising candidate for a quantum memory. By employing holographic techniques via field gradients a single ensemble may be used to store many bits of information. Here we present a coherent memory using a pulsed magnetic field gradient, and demonstrate the storage and retrieval of up to 100 weak 10 GHz coherent excitations in collective states of an electron spin ensemble. We further show that such collective excitations in the electron spin can then be stored in nuclear spin states, which offer coherence times in excess of seconds.

quant-ph↗

arXiv2010

Electron paramagnetic resonance study of ErSc2NC80

We present an electron paramagnetic resonance (EPR) study of ErSc2N@C80 fullerene in which there are two Er3+ sites corresponding to two different configurations of the ErSc2N cluster inside the C80 cage. For each configuration, the EPR spectrum is characterized by a strong anisotropy of the g factors (gx,y = 2.9, gz = 13.0 and gx,y = 5.3, gz = 10.9). Illumination within the cage absorption range (<600 nm) induces a rearrangement of the ErSc2N cluster inside the cage. We follow the temporal dependence of this rearrangement phenomenologically under various conditions.

physics.chem-ph↗

arXiv2010

Entangling remote nuclear spins linked by a chromophore

Molecular nanostructures may constitute the fabric of future quantum technologies, if their degrees of freedom can be fully harnessed. Ideally one might use nuclear spins as low-decoherence qubits and optical excitations for fast controllable interactions. Here, we present a method for entangling two nuclear spins through their mutual coupling to a transient optically-excited electron spin, and investigate its feasibility through density functional theory and experiments on a test molecule. From our calculations we identify the specific molecular properties that permit high entangling power gates under simple optical and microwave pulses; synthesis of such molecules is possible with established techniques.

quant-ph↗

arXiv2010

Electron spin coherence in metallofullerenes: Y, Sc and La@C82

Endohedral fullerenes encapsulating a spin-active atom or ion within a carbon cage offer a route to self-assembled arrays such as spin chains. In the case of metallofullerenes the charge transfer between the atom and the fullerene cage has been thought to limit the electron spin phase coherence time (T2) to the order of a few microseconds. We study electron spin relaxation in several species of metallofullerene as a function of temperature and solvent environment, yielding a maximum T2 in deuterated o-terphenyl greater than 200 microseconds for Y, Sc and La@C82. The mechanisms governing relaxation (T1, T2) arise from metal-cage vibrational modes, spin-orbit coupling and the nuclear spin environment. The T2 times are over 2 orders of magnitude longer than previously reported and consequently make metallofullerenes of interest in areas such as spin-labelling, spintronics and quantum computing.

cond-mat.mtrl-sci↗

arXiv2009

Magnetic field sensing beyond the standard quantum limit using 10-spin NOON states

The concept of entanglement, in which coherent quantum states become inextricably correlated, has evolved from one of the most startling and controversial outcomes of quantum mechanics to the enabling principle of emerging technologies such as quantum computation and quantum sensors. The use of entangled particles in measurement permits the transcendence of the standard quantum limit in sensitivity, which scales as N^1/2 for N particles, to the Heisenberg limit, which scales as N. This approach has been applied to optical interferometry using entangled photons and spin pairs for the measurement of magnetic fields and improvements on atomic clocks. Here, we demonstrate experimentally an 9.4-fold increase in sensitivity to an external magnetic field of a 10-spin entangled state, compared with an isolated spin, using nuclear spins in a highly symmetric molecule. This approach scales in a favourable way compared to systems where qubit loss is prevalent, and paves the way for enhanced precision in magnetic field sensing

quant-ph↗

arXiv2009

A silicon-based cluster state quantum computer

It has been over ten years since Kane's influential proposal for a silicon-based nuclear spin quantum computer using phosphorous donors. Since then, silicon-based architectures have been refined as the experimental challenges associated with the original proposal have become better understood, while simultaneously a number of powerful and generic models for quantum computation have emerged. Here, I discuss how the cluster state or "one-way" model for quantum computing might be advantageously applied to donors in silicon, with the potential to substantially reduce the practical requirements of a successful implementation. The essence of the scheme is to use the electron spin associated with a donor to weave an entangled network between 31P donor nuclear spins. This resource has been shown to have exceptional coherence times and supports universal quantum computation through local measurements on the nuclear spins. Some of the key ingredients, such as global spin manipulation, have been robustly established, while others, such as single spin measurement, have seen much progress in recent years. A key challenge will be the demonstration of electron transfer between donors that preserves spin coherence.

quant-ph↗

arXiv2008

Solid state quantum memory using the 31P nuclear spin

The transfer of information between different physical forms is a central theme in communication and computation, for example between processing entities and memory. Nowhere is this more crucial than in quantum computation, where great effort must be taken to protect the integrity of a fragile quantum bit. Nuclear spins are known to benefit from long coherence times compared to electron spins, but are slow to manipulate and suffer from weak thermal polarisation. A powerful model for quantum computation is thus one in which electron spins are used for processing and readout while nuclear spins are used for storage. Here we demonstrate the coherent transfer of a superposition state in an electron spin 'processing' qubit to a nuclear spin 'memory' qubit, using a combination of microwave and radiofrequency pulses applied to 31P donors in an isotopically pure 28Si crystal. The electron spin state can be stored in the nuclear spin on a timescale that is long compared with the electron decoherence time and then coherently transferred back to the electron spin, thus demonstrating the 31P nuclear spin as a solid-state quantum memory. The overall store/readout fidelity is about 90%, attributed to systematic imperfections in radiofrequency pulses which can be improved through the use of composite pulses. We apply dynamic decoupling to protect the nuclear spin quantum memory element from sources of decoherence. The coherence lifetime of the quantum memory element is found to exceed one second at 5.5K.

quant-ph↗

arXiv2008

Switchable ErSc2N rotor within a C80 fullerene cage: An EPR and photoluminescence excitation study

Systems exhibiting both spin and orbital degrees of freedom, of which Er3+ is one, can offer mechanisms for manipulating and measuring spin states via optical excitations. Motivated by the possibility of observing photoluminescence and electron paramagnetic resonance from the same species located within a fullerene molecule, we initiated an EPR study of Er3+ in ErSc2N@C80. Two orientations of the ErSc2N rotor within the C80 fullerene are observed in EPR, consistent with earlier studies using photoluminescence excitation (PLE) spectroscopy. For some crystal field orientations, electron spin relaxation is driven by an Orbach process via the first excited electronic state of the 4I_15/2 multiplet. We observe a change in the relative populations of the two ErSc2N configurations upon the application of 532 nm illuminations, and are thus able to switch the majority cage symmetry. This photoisomerisation, observable by both EPR and PLE, is metastable, lasting many hours at 20 K.

cond-mat.mtrl-sci↗

arXiv2007

Environmental effects on electron spin relaxation in N@C60

We examine environmental effects of surrounding nuclear spins on the electron spin relaxation of the N@C60 molecule (which consists of a nitrogen atom at the centre of a fullerene cage). Using dilute solutions of N@C60 in regular and deuterated toluene, we observe and model the effect of translational diffusion of nuclear spins of the solvent molecules on the N@C60 electron spin relaxation times. We also study spin relaxation in frozen solutions of N@C60 in CS2, to which small quantities of a glassing agent, S2Cl2 are added. At low temperatures, spin relaxation is caused by spectral diffusion of surrounding nuclear 35Cl and 37Cl spins in the S2Cl2, but nevertheless, at 20 K, T2 times as long as 0.23 ms are observed.

quant-ph↗

arXiv2007

Will spin-relaxation times in molecular magnets permit quantum information processing?

Using X-band pulsed electron spin resonance, we report the intrinsic spin-lattice ($T_1$) and phase coherence ($T_2$) relaxation times in molecular nanomagnets for the first time. In Cr$_7M$ heterometallic wheels, with $M$ = Ni and Mn, phase coherence relaxation is dominated by the coupling of the electron spin to protons within the molecule. In deuterated samples $T_2$ reaches 3 $μ$s at low temperatures, which is several orders of magnitude longer than the duration of spin manipulations, satisfying a prerequisite for the deployment of molecular nanomagnets in quantum information applications.

quant-ph↗

arXiv2006

The effects of a pyrrolidine functional group on the magnetic properties of N@C60

A new stable pyrrolidine functionalized fullerene derivative, C69H10N2O2, has been synthesized, purified by high performance liquid chromatography, and characterized by MALDI mass spectrometry, ultraviolet-visible spectroscopy, Fourier transform infrared, 1H and 13C nuclear magnetic resonance. The magnetic properties of the analogous endohedral species have been studied by both continuous wave (CW) and pulsed EPR. CW-EPR spectra indicated an anisotropic hyperfine interaction and a permanent zero-field-splitting (ZFS). Both CW and pulsed EPR showed the ZFS parameter Deff to be around 17 MHz. Pulsed EPR revealed a biexponential decay in both T1 and T2, yielding a molecular tumbling correlation time of 31.4 +/- 2.5 ps.

physics.chem-ph↗

arXiv2006

Davies ENDOR revisited: Enhanced sensitivity and nuclear spin relaxation

Over the past 50 years, electron-nuclear double resonance (ENDOR) has become a fairly ubiquitous spectroscopic technique, allowing the study of spin transitions for nuclei which are coupled to electron spins. However, the low spin number sensitivity of the technique continues to pose serious limitations. Here we demonstrate that signal intensity in a pulsed Davies ENDOR experiment depends strongly on the nuclear relaxation time T1n, and can be severely reduced for long T1n. We suggest a development of the original Davies ENDOR sequence that overcomes this limitation, thus offering dramatically enhanced signal intensity and spectral resolution. Finally, we observe that the sensitivity of the original Davies method to T1n can be exploited to measure nuclear relaxation, as we demonstrate for phosphorous donors in silicon and for the endohedral fullerene N@C60 in CS2.

physics.chem-ph↗

arXiv2006

Bang-bang control of fullerene qubits using ultra-fast phase gates

Quantum mechanics permits an entity, such as an atom, to exist in a superposition of multiple states simultaneously. Quantum information processing (QIP) harnesses this profound phenomenon to manipulate information in radically new ways. A fundamental challenge in all QIP technologies is the corruption of superposition in a quantum bit (qubit) through interaction with its environment. Quantum bang-bang control provides a solution by repeatedly applying `kicks' to a qubit, thus disrupting an environmental interaction. However, the speed and precision required for the kick operations has presented an obstacle to experimental realization. Here we demonstrate a phase gate of unprecedented speed on a nuclear spin qubit in a fullerene molecule (N@C60), and use it to bang-bang decouple the qubit from a strong environmental interaction. We can thus trap the qubit in closed cycles on the Bloch sphere, or lock it in a given state for an arbitrary period. Our procedure uses operations on a second qubit, an electron spin, in order to generate an arbitrary phase on the nuclear qubit. We anticipate the approach will be vital for QIP technologies, especially at the molecular scale where other strategies, such as electrode switching, are unfeasible.

quant-ph↗

arXiv2006

Electron spin relaxation of N@C60 in CS2

We examine the temperature dependence of the relaxation times of the molecules N@C60 and N@C70 (which comprise atomic nitrogen trapped within a carbon cage) in liquid CS2 solution. The results are inconsistent with the fluctuating zero field splitting (ZFS) mechanism, which is commonly invoked to explain electron spin relaxation for S > 1/2 spins in liquid solution, and is the mechanism postulated in the literature for these systems. Instead, we find a clear Arrhenius temperature dependence for N@C60, indicating the spin relaxation is driven primarily by an Orbach process. For the asymmetric N@C70 molecule, which has a permanent non-zero ZFS, we resolve an additional relaxation mechanism caused by the rapid reorientation of its ZFS. We also report the longest coherence time (T2) ever observed for a molecular electron spin, being 0.25 ms at 170K.

cond-mat.mtrl-sci↗

arXiv2005

High Fidelity Single Qubit Operations using Pulsed EPR

Systematic errors in spin rotation operations using simple RF pulses place severe limitations on the usefulness of the pulsed magnetic resonance methods in quantum computing applications. In particular, the fidelity of quantum logic operations performed on electron spin qubits falls well below the threshold for the application of quantum algorithms. Using three independent techniques, we demonstrate the use of composite pulses to improve this fidelity by several orders of magnitude. The observed high-fidelity operations are limited by pulse phase errors, but nevertheless fall within the limits required for the application of quantum error correction.

quant-ph↗

arXiv2005

Brokered Graph State Quantum Computing

We describe a procedure for graph state quantum computing that is tailored to fully exploit the physics of optically active multi-level systems. Leveraging ideas from the literature on distributed computation together with the recent work on probabilistic cluster state synthesis, our model assigns to each physical system two logical qubits: the broker and the client. Groups of brokers negotiate new graph state fragments via a probabilistic optical protocol. Completed fragments are mapped from broker to clients via a simple state transition and measurement. The clients, whose role is to store the nascent graph state long term, remain entirely insulated from failures during the brokerage. We describe an implementation in terms of NV-centres in diamond, where brokers and clients are very naturally embodied as electron and nuclear spins.

quant-ph↗

arXiv2004

A new mechanism for electron spin echo envelope modulation

Electron spin echo envelope modulation (ESEEM) has been observed for the first time from a coupled hetero-spin pair of electron and nucleus in liquid solution. Previously, modulation effects in spin echo experiments have only been described in liquid solutions for a coupled pair of homonuclear spins in NMR or a pair of resonant electron spins in EPR. We observe low-frequency ESEEM (26 and 52 kHz) due to a new mechanism present for any electron spin with S>1/2 that is hyperfine coupled to a nuclear spin. In our case these are electron spin (S=3/2) and nuclear spin (I=1) in the endohedral fullerene N@C60. The modulation is shown to arise from second order effects in the isotropic hyperfine coupling of an electron and 14N nucleus.

quant-ph↗

arXiv2004

Measuring errors in single qubit rotations by pulsed electron paramagnetic resonance

The ability to measure and reduce systematic errors in single-qubit logic gates is crucial when evaluating quantum computing implementations. We describe pulsed electron paramagnetic resonance (EPR) sequences that can be used to measure precisely even small systematic errors in rotations of electron-spin-based qubits. Using these sequences we obtain values for errors in rotation angle and axis for single-qubit rotations using a commercial EPR spectrometer. We conclude that errors in qubit operations by pulsed EPR are not limiting factors in the implementation of electron-spin based quantum computers.

quant-ph↗