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arXiv:1503.03956 · Physical Review B

Electron-phonon processes of the nitrogen-vacancy center in diamond

Taras Plakhotnik, Marcus W. Doherty, Neil B. Manson

Published Aug 21, 2015• 38 citations
arXivHTMLPDF

Abstract

Applications of the negatively charged nitrogen-vacancy center in diamond exploit the center's unique optical and spin properties, which at ambient temperature are predominately governed by electron-phonon interactions. Here, we investigate these interactions at ambient and elevated temperatures by observing the motional narrowing of the center's excited-state spin resonances. We determine that the center's Jahn-Teller dynamics are much slower than currently believed and that they do not solely account for the broadening of the center's optical resonance above cryogenic temperatures. We show that the inclusion of interactions with symmetric phonon modes can explain the observed broadening and resolve the current inconsistencies in the literature. However, our model also reveals unexpected features of the electron-phonon processes that coincide with other poorly understood vibronic features of the center and require further investigation.

DOI
10.1103/physrevb.92.081203

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Applications of the negatively charged nitrogen-vacancy center in diamond exploit the center's unique optical and spin properties, which at ambient temperature are predominately governed by electron-phonon interactions. Here, we investigate these interactions at ambient and elevated temperatures by observing the motional narrowing of the center's excited-state spin resonances. We determine that the center's Jahn-Teller dynamics are much slower than currently believed and that they do not solely account for the broadening of the center's optical resonance above cryogenic temperatures. We show that the inclusion of interactions with symmetric phonon modes can explain the observed broadening and resolve the current inconsistencies in the literature. However, our model also reveals unexpected features of the electron-phonon processes that coincide with other poorly understood vibronic features of the center and require further investigation.
The negatively charged nitrogen vacancy (NV) center in diamond is an optically accessible material defect with a unique combination of spin and optical properties that has attracted interest in quantum-information sciences and as a design candidate for nanoscale quantum sensors. Here, we present time-resolved nonlinear optical spectroscopy measurements, conducted with ultrabroadband laser pulses, that reveal strong modulation of the excited-state by the longitudinal optical (LO) phonon of the diamond lattice. The LO phonon and its overtones geometrically distort neighboring NV centers, driving long lived (3.5 ps) excited state relaxation of coupled NV centers after the initial excitation and ultrafast (<150 fs) decay of the Jahn-Teller distortion. These observations elevate the LO phonon to an important tuning mode of the Jahn-Teller conical intersection and help resolve previous spectroscopy experiments that noted longer-lived excited-state dynamics.
The negatively charged nitrogen-vacancy (NV(-)) center in diamond is considered to be one of the most promising solid state systems for quantum information applications. Excited states of the NV(-) center play a center role in the proposed applications. Using a combination of first-principles calculations and vibronic interaction model analysis, we establish the presence of a dynamic Jahn-Teller effect in the (3)E excited state. The calculated temperature-dependent dephasing rate for the zero phonon line as well as the splitting of the first two vibronic states are in good agreement with experiment.
The understanding of the coherence properties of photons emitted from negatively charged nitrogen-vacancy (NV) centers in diamond is essential for the success of quantum information applications based on indistinguishable photons. Here we study both the polarization of photons emitted from and the linewidth of photons absorbed by single NV centers as a function of temperature T. We find that for T < 100 K the main dephasing mechanism contributing to the linewidth broadening is phonon-mediated population transfer between the two excited orbital states. The observed T5 temperature dependence of the population transfer rate and linewidth is experimental evidence of a dynamic Jahn-Teller effect in the excited states.
Negatively charged nitrogen-vacancy (NV${}^{\ensuremath{-}}$) color centers in diamond have generated much interest for use in quantum technology. Despite the progress made in developing their applications, many questions about the basic properties of NV${}^{\ensuremath{-}}$ centers remain unresolved. Understanding these properties can validate theoretical models of NV${}^{\ensuremath{-}}$, improve their use in applications, and support their development into competitive quantum devices. In particular, knowledge of the phonon modes of the 1A1{}^{1}{A}_{1}1A1​ electronic state is key for understanding the optical pumping process. Using pump-probe spectroscopy, we measured the phonon sideband of the ${}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}$ electronic transition in the NV${}^{\ensuremath{-}}$ center. From this we calculated the ${}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}$ one-phonon absorption spectrum and found it to differ from that of the ${}^{3}E\ensuremath{\rightarrow}{}^{3}{A}_{2}$ transition, a result which is not anticipated by previous group-theoretical models of the NV${}^{\ensuremath{-}}$ electronic states. We identified a high-energy 169-meV localized phonon mode of the 1A1{}^{1}{A}_{1}1A1​ level.
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.
The nitrogen vacancy (NV) center in diamond is well known for its outstanding optical and spin properties, enabling various applications in quantum sensing and quantum information at both cryogenic and ambient temperatures. Despite a large body of work, however, the NV center's dynamics at intermediate temperatures are incompletely understood. This paper describes a basic rate model able to explain the NV population dynamics over the full parameter space of temperature, crystallographic strain, and magnetic field. Numerical simulations of the model are in excellent agreement with experiments discussed in the accompanying PRL.