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The Journal of Physical Chemistry A

Two-photon Excited Fluorescence of Nitrogen-Vacancy Centers in Proton-Irradiated Type Ib Diamond

Tse-Luen Wee, Yan‐Kai Tzeng, C.-C. Han, Huan‐Cheng Chang, Wunshain S. Fann, Jui‐Hung Hsu, Kuan‐Ming Chen, Yueh‐Chung Yu

Published Aug 18, 2007• 196 citations
Publisher

Abstract

Two-photon fluorescence spectroscopy of negatively charged nitrogen-vacancy [(N-V)-] centers in type Ib diamond single crystals have been studied with a picosecond (7.5 ps) mode-locked Nd:YVO(4) laser operating at 1064 nm. The (N-V)- centers were produced by radiation damage of diamond using a 3 MeV proton beam, followed by thermal annealing at 800 degrees C. Prior to the irradiation treatment, infrared spectroscopy of the C-N vibrational modes at 1344 cm(-1) suggested a nitrogen content of 109 +/- 10 ppm. Irradiation and annealing of the specimen led to the emergence of a new absorption band peaking at approximately 560 nm. From a measurement of the integrated absorption intensity of the sharp zero-phonon line (637 nm) at liquid nitrogen temperature, we determined a (N-V)- density of (4.5 +/- 1.1) x 10(18) centers/cm3 (or 25 +/- 6 ppm) for the substrate irradiated at a dose of 1 x 1016) H(+)/cm(2). Such a high defect density allowed us to observe two-photon excited fluorescence and measure the corresponding fluorescence decay time. No significant difference in the spectral feature and fluorescence lifetime was observed between one-photon and two-photon excitations. Assuming that the fluorescence quantum yields are the same for both processes, a two-photon absorption cross section of sigma(TPA) = (0.45 +/- 0.23) x 10(-50) cm(4).s/photon at 1064 nm was determined for the (N-V)- center based on its one-photon absorption cross section of sigma(OPA) = (3.1 +/- 0.8) x 10(-17) cm2 at 532 nm. The material is highly photostable and shows no sign of photobleaching even under continuous two-photon excitation at a peak power density of 3 GW/cm(2) for 5 min.

DOI
10.1021/jp073938o

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•Jan 1, 1991•0 citations
Two-photon fluorescence spectroscopy of negatively charged nitrogen-vacancy [(N-V)-] centers in type Ib diamond single crystals have been studied with a picosecond (7.5 ps) mode-locked Nd:YVO(4) laser operating at 1064 nm. The (N-V)- centers were produced by radiation damage of diamond using a 3 MeV proton beam, followed by thermal annealing at 800 degrees C. Prior to the irradiation treatment, infrared spectroscopy of the C-N vibrational modes at 1344 cm(-1) suggested a nitrogen content of 109 +/- 10 ppm. Irradiation and annealing of the specimen led to the emergence of a new absorption band peaking at approximately 560 nm. From a measurement of the integrated absorption intensity of the sharp zero-phonon line (637 nm) at liquid nitrogen temperature, we determined a (N-V)- density of (4.5 +/- 1.1) x 10(18) centers/cm3 (or 25 +/- 6 ppm) for the substrate irradiated at a dose of 1 x 1016) H(+)/cm(2). Such a high defect density allowed us to observe two-photon excited fluorescence and measure the corresponding fluorescence decay time. No significant difference in the spectral feature and fluorescence lifetime was observed between one-photon and two-photon excitations. Assuming that the fluorescence quantum yields are the same for both processes, a two-photon absorption cross section of sigma(TPA) = (0.45 +/- 0.23) x 10(-50) cm(4).s/photon at 1064 nm was determined for the (N-V)- center based on its one-photon absorption cross section of sigma(OPA) = (3.1 +/- 0.8) x 10(-17) cm2 at 532 nm. The material is highly photostable and shows no sign of photobleaching even under continuous two-photon excitation at a peak power density of 3 GW/cm(2) for 5 min.
We report the observation of multiphoton photoluminescence excitation (PLE) below the resonant energies of nitrogen vacancy (NV) centers in diamond. The quadratic and cubic dependence of the integrated fluorescence intensity as a function of excitation power indicates a two-photon excitation pathway for the ${\mathrm{NV}}^{\ensuremath{-}}$ charge state and a three-photon process involved for the neutral NV0{\mathrm{NV}}^{0}NV0 charge state, respectively. Comparing the total multiphoton energy with its single-photon equivalent, the PLE spectra follows the absorption spectrum of single photon excitation. We also observed that the efficiency of photoluminescence for different charge states, as well as the decay time constant, was dependent on the excitation wavelength and power.
We report on the spectroscopic and laser characterization of negatively charged nitrogen-vacancy (NV−) centers in diamond. Spectroscopic properties such as absorption and emission spectra as well as kinetics were studied, and parameters such as cross-sections and lifetimes were estimated. A vibronic band of NV0 with zero phonon line (ZPL) at 575 nm was detected under 532 nm pulsed excitation due to the photoionization of NV−. Transmission of 532 nm pump pulses saturate around ∼10%, which is much smaller than the theoretical level. Δk/k0 kinetics revealed slow recovery of NV− centers after photoionization under 532 nm pumping, which involved different relaxation channels depending on the probe beam wavelengths. Localization of the electrons in the metastable state of NV0 centers resulted in higher saturated transmission of 632 nm pump.
Defects in diamond have evolved as unique object for their potential application for Optical imaging and Nano-photonics. High pressure high temperature (HPHT) grown type-Ib diamond particles were milled down to the size of ~ 80 nm and purified to remove iron & graphitic carbon impurities and irradiated with 35 KeV He+ ions to create vacancies in the diamond lattice. Vacancies diffuse close to substitutional nitrogen impurities of nano-diamond particles upon thermal treatment. Characteristic sharp emission of NV centers were observed at 575.5 nm and 637.9 nm corresponding to NV° and NV− charged states in addition to a broad emission in the range 550-750 nm. Structural and photo-physical behavior of these fluorescent diamonds was found to depend on the method of purification adopted. Samples purified through acid reflux were found suitable for bio-imaging applications while, sample purified through air oxidation shows properties desirable for Nano-photonic applications. Photon-correlation measurements of emission from individual diamond nanoparticles using Hanbury Brown and Twiss interferometer (HBT) shows anti-bunching curve with g2(t)= 0 confirming their suitability as single photon source. Such sources of indistinguishable photons are highly desirable for quantum computation and quantum optics applications.
The development of reliable devices to generate single photons is crucial for applications in quantum cryptography, as well as for fundamental quantum optics experiments. Due to their extremely high photostability at room temperature, optically active defects in solids, the so called color centers, are among the most promising candidates. Single NV (nitrogen-vacancy) centers in diamond have been demonstrated to be able to generate single photons and have already shown advantages compared to attenuated laser pulses in a quantum cryptography experiment. The nitrogen-vacancy center (NV center) in diamond consists of a substitutional nitrogen atom and an adjacent vacancy. This complex exhibits an optical transition with a fluorescence lifetime of 11.6 ns. The room temperature spectrum of the NV center consists of the zero-phonon line at 637 nm and broad phononic sidebands with a FWHM of more than 100 nm. Due to the existence of a shelving level the efficiency of the NV center as a single photon source is limited. Additionally, the high diffraction index of bulk diamond restricts the efficiency to collect the fluorescence light.
We created dense ensembles of negatively charged nitrogen-vacancy (NV-) centers in diamond by neutron and electron irradiation for applications in hybrid quantum systems and magnetometry. We characterize fluorescence intensity, optical and coherence properties of the resulting defects by confocal microscopy, UV/Vis and FTIR spectroscopy, optically detected magnetic resonance and small angle X-ray scattering. We find the highest densities of NV- at neutron fluences on the order of 10^17 cm^-2 and electron doses of 10^18 cm^-2, with spin resonance linewidths of 6 MHz. Lower electron energies increase the ratio of centers in the desired negative charge state to those in the neutral one. Annealing at 900 °C during the irradiation reduces the spin resonance linewidth. Electron irradiation furthermore results in substantially higher optical transparency compared to neutron irradiation.
The nitrogen - vacancy (N-V) center is a point defect found in diamonds containing substitutional nitrogen impurities. It arises after exposure to ionizing radiation and subsequent thermal annealing. The physical structure of the center has previously been identified as a substitutional nitrogen atom located adjacent to a neutral carbon vacancy, but prior to this work knowledge of its electronic structure was very incomplete. The results presented here are intended to establish the energy level structure of the N-V center unambiguously, using nonlinear laser spectroscopy in concert with paramagnetic resonance experiments. A new technique which achieves sub-Hertz resolution in nearly degenerate four-wave mixing (NDFWM) and optical two-beam coupling experiments was applied to determine the decay rates of excited states in the N-V center. Laser-enhanced EPR experiments were performed to assign spin character to the ground state. Fluorescent emission of the center was used to determine excited state energies. In particular, these results resolve earlier conflicting reports of the N-V ground state structure and offer a picture of state energies and dynamics consistent with all observations to date. The principal results of this thesis may be summarized as follows. We show that the ground state of the center consists of a spin triplet ground state with a zero-field splitting of 2.88 GHz and a spin-lattice relaxation time of 1.170 ±\pm± 0.003 ms. The first parity-allowed transition occurs to a triplet excited state at 1.944 eV with a lifetime of 13.3 ±\pm± 0.2 ns. The first metastable singlet excited state is shown to have a lifetime of 265.3 ±\pm± 0.6 ms at room temperature and its temperature dependence measured between 77 and 295 K. Through low temperature studies the mechanism for ground state spin-lattice relaxation is determined to be a two-phonon process involving 63 meV optical phonons. Finally, the origin of satellite lines in the persistent hole-burning spectrum is tentatively explained using our picture of the energy level structure and used to infer a zero-field spin splitting in the excited triplet state of 0.6 GHz.