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Conference on Lasers and Electro-Optics

Raman excited spin coherences in N-V diamond

Philip Hemmer, Alexey V. Turukhin, M. S. Shahriar, J. A. Musser

Published Jan 1, 2001• 2 citations
Publisher

Abstract

Summary form only given. The use of optical Raman interactions to excite spin coherences in solids has numerous potential applications, ranging from low-power nonlinear optics to high-temperature spectral hole burning memories to solid-state quantum computing. The interest in Raman excitation lies in the fact that the spin coherences can be efficiently excited and manipulated using optical laser fields yet are weakly coupled to the environment and hence have the long coherence lifetimes needed for optical memories and quantum computing. The interest in nitrogen-vacancy (N-V) color centers in diamond is its large optical oscillator strength. For memory, a large oscillator strength is important for high temperature operation. For quantum computing, the high optical transition rate enables the higher gate speed and the larger number of quantum logic operations that can be performed within the spin coherence lifetime.

DOI
10.1109/cleo.2001.947938

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Summary form only given. The use of optical Raman interactions to excite spin coherences in solids has numerous potential applications, ranging from low-power nonlinear optics to high-temperature spectral hole burning memories to solid-state quantum computing. The interest in Raman excitation lies in the fact that the spin coherences can be efficiently excited and manipulated using optical laser fields yet are weakly coupled to the environment and hence have the long coherence lifetimes needed for optical memories and quantum computing. The interest in nitrogen-vacancy (N-V) color centers in diamond is its large optical oscillator strength. For memory, a large oscillator strength is important for high temperature operation. For quantum computing, the high optical transition rate enables the higher gate speed and the larger number of quantum logic operations that can be performed within the spin coherence lifetime.
Summary form only given.Optical spectral hole-burning has demonstrated the ability to achieve high-capacity, high-speed data storage. Unfortunately, widespread application of this technique has been limited by the requirement for low temperature operation. To circumvent this problem, we have been investigating the possibility of using Raman-excited spin coherences to store and recall optical data. The motivation is that optical Raman excitation allows storage densities and response times characteristic of optical hole-burning memories, but because it is based on long-lived spin coherences, it can maintain these characteristics at much higher operating temperatures. For the initial experiments we chose to use N-V color centers in diamond as the Raman hole-burning material because it is comparatively well studied.
Raman excited spin coherences were experimentally observed in nitrogen-vacancy (N-V) diamond color centers via nondegenerate four-wave mixing (NDFWM) and electromagnetically induced transparency (EIT). The maximal EIT-induced absorption suppression was found to be 17%, which corresponds to 70% of what is possible given the four possible geometric orientations of the N-V center in diamond. The properties of these coherences are discussed in the context of potential applications to solid-state quantum computing and high-temperature spectral hole burning memories.
The possibility of using Raman excited spin coherences to increase the operating temperature of spectral hole burning memories and processors is being explored experimentally. The approach is to store and/or process data using spin coherences excited by optical Raman transitions. This is motivated by the fact that spin coherence lifetimes are much less sensitive to temperature than optical coherence lifetimes. However, direct microwave excitation of spin coherences does not give a high storage density because of the large microwave wavelength. By using optical Raman fields to excite the spin coherences, full optical spatial resolution can be achieved. Initial experiments in Pr doped YSO demonstrated potential for higher temperature operation. Current experiments are concentrating on further increasing the operating temperature using this and other materials.
Raman-excited spin coherences were experimentally observed in nitrogen-vacancy (N-V) diamond color centers by means of nondegenerate four-wave mixing and electromagnetically induced transparency. The maximal absorption suppression was found to be 17%, which corresponds to 70% of what is possible given the random geometric orientation of the N-V center in diamond. In the context of quantum computing in solids, this level of transparency represents efficient preparation of quantum bits, as well as the ability to perform arbitrary single-quantum-bit rotations.
Quantum memories are a key technology enabling arbitrarily-scalable optical quantum information processing architectures via active synchronisation and multiplexing of quantum information. Optically active confined impurities, called colour centres, in a spin-free and highly transparent diamond host material are promising systems to realise such devices in the solid-state, suitable for integration in a scalable guided-wave on-chip photonic platform. In this thesis, the transition from optical Raman quantum memories in atomic vapours to solid-state systems is prepared, exploring two diamond-based systems: On the basis of ensembles of neutrally charged nitrogen vacancy centres, desirable properties and criteria of solid-state systems used for optical quantum memories are developed. These include non-vanishing off-resonant Raman coupling, variable acceptance bandwidth for broadband pulses and cross-linear polarised optical transitions to prevent the generation of noise during the Raman memory protocol, which have been realised experimentally by applying external uniaxial stress to the system. However, attempts to measure the very short orbital ground state lifetime affirmed unfavourable theoretical estimations, rendering this centre unsuitable for memory applications. As a potential alternative, the negatively charged silicon vacancy centre has been investigated, which offers a large ground state splitting with extended life and coherence times and narrow inhomogeneous spectral lines due to its inversion symmetry. In an ensemble of silicon vacancy centres, the ground state lifetime is measured and coherent manipulation via resonant Ramsey interference and Hahn echo is demonstrated. In a second step, off-resonant two-photon transitions are achieved implementing stimulated Raman adiabatic passage between the orbital ground states. Finally, strong light-matter interaction of a weak signal field with the ensemble via phase-sensitive four-wave mixing is shown forming the basis for integrated Raman-based memories and single photon nonlinearities in ensembles of silicon vacancy centres and closely related defects.
The nitrogen-vacancy (NV) center in diamond has emerged as a versatile atom-like system, finding diverse applications at both ambient and cryogenic temperatures. At room temperature, the NV center's spin-triplet electronic ground state has a long coherence time and can be read out and initialized using nonresonant optical excitation, which has enabled a wide range of metrology and quantum information applications. At cryogenic temperatures, the NV center exhibits a variety of narrow, atom-like optical transitions, which has made the NV center a promising platform for quantum optics applications. We use coherent optical manipulation of the NV center at cryogenic temperatures to probe its internal dynamics and aspects of its interactions with its environment.\nFirst, we investigate the intersystem crossing (ISC) process, which is a spin-dependent nonradiative decay mechanism that enables the electronic spin state to be optically initialized and read out at room temperature. We measure the ISC rates from different excited states as well as the rate at which interactions with phonons redistribute population between these states. Based on these measurements, we develop a theoretical model that unifies the phonon-induced mixing and ISC mechanisms. We find that our model is in excellent agreement with experiment and that it can be used to predict unknown elements of the NV center's electronic structure.\nSecond, we investigate a novel method of using coherent optical manipulation of the NV center's electronic spin to control a nearby nuclear spin. Coherent interactions between the NV center and nearby nuclear spins have enabled the development of NV center-based, multi-qubit quantum registers, but these techniques have generally required the application of microwave or radio-frequency radiation. We demonstrate control of the nuclear spin using an all-optical Raman technique and theoretically evaluate the extent to which the intrinsic physics of the NV center limits the coherence of this Raman-based manipulation technique.