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Physical Review X

Deterministic Electrical Charge-State Initialization of Single Nitrogen-Vacancy Center in Diamond

Yuki Doi, Toshiharu Makino, Hiromitsu Kato, Daisuke Takeuchi, Masahiko Ogura, Hideyo Okushi, Hiroki Morishita, Toshiyuki Tashima, Shinji Miwa, Satoshi Yamasaki, Philipp Neumann, Jörg Wrachtrup, Yoshishige Suzuki, Norikazu Mizuochi

Published Mar 31, 2014• 81 citations
Publisher

Abstract

Use of nitrogen-vacancy (NV) centers in diamond for quantum applications requires fast switching between their two different charge states. Using a diamond diode, scientists now demonstrate for the first time deterministic, purely electrical, and room-temperature charge-state control of single NV centers on the time scale of a microsecond.

DOI
10.1103/physrevx.4.011057

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Charge-states modulation of nitrogen-vacancy (NV) centers incorporated into single crystal diamond films attracts increasing attention for solid-state qubits applications. Here, we discuss the electro- and photoluminescence emission properties of NV centers incorporated by gas phase nitrogen delta-doping of the intrinsic diamond layer of a positive-intrinsic-negative (PIN) junction diode. The experiments show that the charge state of NV centers can be intentionally controlled by applying well-defined external bias voltages. It can be switched from the negatively charged state NV− to the neutral charged state NV0 when a strong forward bias potential is applied. This can be switched back by application of reverse potentials. These results will be discussed assuming basic electronic properties of diamond PIN diodes, including the variation of spectral properties as well as the dynamics of charge state transitions.

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Abstract Nitrogen-vacancy (NV) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.

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For quantum information applications, nitrogen-vacancy (NV) centers in diamond combine many of the advantages of atomic systems (optical access, millisecond spin-coherence times) with the engineering flexibility of solid-state devices. Recent demonstrations of coherent coupling between photons and individual NV-center spins [1,2] provide a route to integrating NV-center qubits within photonic networks and for on-demand generation of entangled single-spin/single-photon pairs. Such applications require the ability to tune the NV-center zero-phonon optical transitions, to compensate for natural sample inhomogeneities which perturb the electronic orbital states. Here we demonstrate the ability to electrically control the orbitals of individual NV centers by applying voltages to micron-scale surface gates [3]. Surprisingly, the local electric field experienced by an NV center is significantly enhanced by a photoinduced space charge resulting from photoionization of deep donor impurities within the diamond, even in high-purity single-crystal material (< 5 ppb nitrogen content). Since the photoinduced electric fields are reproducible as a function of gate voltage and are predominantly directed perpendicular to the diamond surface, we can harness them to obtain three-dimensional control of the local electric field vector with surface gates alone. To demonstrate this technique, we tune the excited-state orbital doublet of a strained NV center to degeneracy, as required for some spin-photon entanglement protocols [2], and then adjust the optical transition frequency, showing that we can tune multiple NV centers to have the same degenerate transition energy. This method should enable the coherent coupling of multiple NV center spins to indistinguishable photons within a scalable photonic network.

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In this paper, we demonstrate an active and fast control of the charge state and hence of the optical and electronic properties of single and near-surface nitrogen-vacancy centres (NV centres) in diamond. This active manipulation is achieved by using a two-dimensional Schottky-diode structure from diamond, i.e., by using aluminium as Schottky contact on a hydrogen terminated diamond surface. By changing the applied potential on the Schottky contact, we are able to actively switch single NV centres between all three charge states NV+, NV0 and NV− on a timescale of 10 to 100 ns, corresponding to a switching frequency of 10–100 MHz. This switching frequency is much higher than the hyperfine interaction frequency between an electron spin (of NV−) and a nuclear spin (of 15N or 13C for example) of 2.66 kHz. This high-frequency charge state switching with a planar diode structure would open the door for many quantum optical applications such as a quantum computer with single NVs for quantum information processing as well as single 13C atoms for long-lifetime storage of quantum information. Furthermore, a control of spectral emission properties of single NVs as a single photon emitters – embedded in photonic structures for example – can be realized which would be vital for quantum communication and cryptography.

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Charge State Control of Single Nitrogen-Vacancy Centers in Diamond

悠生 土井

Quantum information in which spin is used as a source of non-classical computation and communication, attracts considerable interest.A long spin coherence (T 2 ) are required toward quantum processing.In addition, small spectral diffusion of single photon for realization of quantum cryptography and building quantum network is needed.The nitrogen-vacancy center (NV) in diamond have long T 2 (up to several milliseconds at room temperature) and become single-photon emitter.Now a days, optically induced charge state interconversion on NV significantly extend T 2 of proximal nuclear spin owing to hyperfine interaction is weaken by motion narrowing.Theory predicts that T 2 exceeding 1 min with preventing heating of diamond due to high laser power excitation.This demonstration show potential of charge state and its non-optical control for spin properties of the NV center.Despite optical illumination is essential for NV to initialize and readout spin, optically induced charge state interconversion causes error in quantum control and spectral diffusion in emitted single photons.In this study, charge state of single NV centers are deterministically controlled by non-optical method.Charge state of single NVs formed in the intrinsic layer of p-in diode are modulated by current injection.Transition rate and its dependence on current is revealed.Recent controllable direction of charge state is limited; however this non-optical charge state control on spin-active negatively charged state (NV -) open the new way to spin related experiments.This study also realize purely populated charge state on the single NVs in phosphorus doped n-type diamond.Charge state is perfectly stabilized into NV -state even under optical illumination (1 µW, 593 nm).After NV - charge state is disturbed by strong laser excitation, state recovered to NV -state under dark condition.This result pave the way to the single spin manipulation in high efficiency and suppress spectral diffusion of single emitted photons. 概要この NV 中心は光励起下(波長: 593 nm, 強度: 1 µW) においても電荷状態が変化しない。また強い光励起によって電荷状態の変化が引き起こ されても、その後 0.28 ms -1 のレートで完全に NV -へと回復することがわかった。この 成果は単一スピン操作の精度、並びに単一光子のスペクトルの安定性向上に繋がる。 Contents 5.2.Raster scan images and fluorescence time traces . . . . . . . . . . . . . .5.3.Single-shot charge-state measurements . . . . . . . . . . . . . . . . . . .5.4.Recombination/recharge rate in the dark condition . . . . . . . . . . . .5.5.Charge-state population and recombination rate under laser excitation .5.6.ODMR and spin coherence measurements . . . . . . . . . . . . . . . . .

•Mar 28, 2016•0 citations
Use of nitrogen-vacancy (NV) centers in diamond for quantum applications requires fast switching between their two different charge states. Using a diamond diode, scientists now demonstrate for the first time deterministic, purely electrical, and room-temperature charge-state control of single NV centers on the time scale of a microsecond.
Charge-states modulation of nitrogen-vacancy (NV) centers incorporated into single crystal diamond films attracts increasing attention for solid-state qubits applications. Here, we discuss the electro- and photoluminescence emission properties of NV centers incorporated by gas phase nitrogen delta-doping of the intrinsic diamond layer of a positive-intrinsic-negative (PIN) junction diode. The experiments show that the charge state of NV centers can be intentionally controlled by applying well-defined external bias voltages. It can be switched from the negatively charged state NV− to the neutral charged state NV0 when a strong forward bias potential is applied. This can be switched back by application of reverse potentials. These results will be discussed assuming basic electronic properties of diamond PIN diodes, including the variation of spectral properties as well as the dynamics of charge state transitions.
Abstract Nitrogen-vacancy (NV) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.
For quantum information applications, nitrogen-vacancy (NV) centers in diamond combine many of the advantages of atomic systems (optical access, millisecond spin-coherence times) with the engineering flexibility of solid-state devices. Recent demonstrations of coherent coupling between photons and individual NV-center spins [1,2] provide a route to integrating NV-center qubits within photonic networks and for on-demand generation of entangled single-spin/single-photon pairs. Such applications require the ability to tune the NV-center zero-phonon optical transitions, to compensate for natural sample inhomogeneities which perturb the electronic orbital states. Here we demonstrate the ability to electrically control the orbitals of individual NV centers by applying voltages to micron-scale surface gates [3]. Surprisingly, the local electric field experienced by an NV center is significantly enhanced by a photoinduced space charge resulting from photoionization of deep donor impurities within the diamond, even in high-purity single-crystal material (< 5 ppb nitrogen content). Since the photoinduced electric fields are reproducible as a function of gate voltage and are predominantly directed perpendicular to the diamond surface, we can harness them to obtain three-dimensional control of the local electric field vector with surface gates alone. To demonstrate this technique, we tune the excited-state orbital doublet of a strained NV center to degeneracy, as required for some spin-photon entanglement protocols [2], and then adjust the optical transition frequency, showing that we can tune multiple NV centers to have the same degenerate transition energy. This method should enable the coherent coupling of multiple NV center spins to indistinguishable photons within a scalable photonic network.
In this paper, we demonstrate an active and fast control of the charge state and hence of the optical and electronic properties of single and near-surface nitrogen-vacancy centres (NV centres) in diamond. This active manipulation is achieved by using a two-dimensional Schottky-diode structure from diamond, i.e., by using aluminium as Schottky contact on a hydrogen terminated diamond surface. By changing the applied potential on the Schottky contact, we are able to actively switch single NV centres between all three charge states NV+, NV0 and NV− on a timescale of 10 to 100 ns, corresponding to a switching frequency of 10–100 MHz. This switching frequency is much higher than the hyperfine interaction frequency between an electron spin (of NV−) and a nuclear spin (of 15N or 13C for example) of 2.66 kHz. This high-frequency charge state switching with a planar diode structure would open the door for many quantum optical applications such as a quantum computer with single NVs for quantum information processing as well as single 13C atoms for long-lifetime storage of quantum information. Furthermore, a control of spectral emission properties of single NVs as a single photon emitters – embedded in photonic structures for example – can be realized which would be vital for quantum communication and cryptography.
Nitrogen-vacancy centers in diamond are considered to be promising building blocks for emerging quantum technologies. At the same time, practical applications require them to be excited and controlled electrically. However, there is a lack of knowledge about their behavior in electrical driven systems. Here, we introduce a physical model to address the single-photon emission dynamics of electrically pumped NV center in diamond in a quantitative manner and present a detailed study of the single-photon emitting diode based on NV centers.
Quantum information in which spin is used as a source of non-classical computation and communication, attracts considerable interest.A long spin coherence (T 2 ) are required toward quantum processing.In addition, small spectral diffusion of single photon for realization of quantum cryptography and building quantum network is needed.The nitrogen-vacancy center (NV) in diamond have long T 2 (up to several milliseconds at room temperature) and become single-photon emitter.Now a days, optically induced charge state interconversion on NV significantly extend T 2 of proximal nuclear spin owing to hyperfine interaction is weaken by motion narrowing.Theory predicts that T 2 exceeding 1 min with preventing heating of diamond due to high laser power excitation.This demonstration show potential of charge state and its non-optical control for spin properties of the NV center.Despite optical illumination is essential for NV to initialize and readout spin, optically induced charge state interconversion causes error in quantum control and spectral diffusion in emitted single photons.In this study, charge state of single NV centers are deterministically controlled by non-optical method.Charge state of single NVs formed in the intrinsic layer of p-in diode are modulated by current injection.Transition rate and its dependence on current is revealed.Recent controllable direction of charge state is limited; however this non-optical charge state control on spin-active negatively charged state (NV -) open the new way to spin related experiments.This study also realize purely populated charge state on the single NVs in phosphorus doped n-type diamond.Charge state is perfectly stabilized into NV -state even under optical illumination (1 µW, 593 nm).After NV - charge state is disturbed by strong laser excitation, state recovered to NV -state under dark condition.This result pave the way to the single spin manipulation in high efficiency and suppress spectral diffusion of single emitted photons. 概要この NV 中心は光励起下(波長: 593 nm, 強度: 1 µW) においても電荷状態が変化しない。また強い光励起によって電荷状態の変化が引き起こ されても、その後 0.28 ms -1 のレートで完全に NV -へと回復することがわかった。この 成果は単一スピン操作の精度、並びに単一光子のスペクトルの安定性向上に繋がる。 Contents 5.2.Raster scan images and fluorescence time traces . . . . . . . . . . . . . .5.3.Single-shot charge-state measurements . . . . . . . . . . . . . . . . . . .5.4.Recombination/recharge rate in the dark condition . . . . . . . . . . . .5.5.Charge-state population and recombination rate under laser excitation .5.6.ODMR and spin coherence measurements . . . . . . . . . . . . . . . . .