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Acta Physica Polonica A

Fluorescence Correlation and Low Temperature Linewidth of Single Defect Centers in Diamond

A. Dräbenstedt, C. Tietz, Fedor Jelezko, Jörg Wrachtrup, S. Ya. Kilin, A. Nizovtzev

Published Nov 1, 1999• 8 citations
Publisher

Abstract

Low temperature fluorescence excitation spectroscopy was carried out on single , nitrogen vacancy defect centers.At temperatures below 90, K; the fluorescence intensity of individual centers drastically diminishes because of the population of a metastable singlet state in near resonance with the .optically excited state.Low temperature fluorescence excitation spectroscopy , down to 5 K becomes possible via deshelving of this state with a second laser source.Surprisingly individual centers reveal low temperature fluorescence excitation line widths around 0.6 meV.

DOI
10.12693/aphyspola.96.665

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Low temperature fluorescence excitation spectroscopy was carried out on single , nitrogen vacancy defect centers.At temperatures below 90, K; the fluorescence intensity of individual centers drastically diminishes because of the population of a metastable singlet state in near resonance with the .optically excited state.Low temperature fluorescence excitation spectroscopy , down to 5 K becomes possible via deshelving of this state with a second laser source.Surprisingly individual centers reveal low temperature fluorescence excitation line widths around 0.6 meV.
Individual nitrogen-vacancy defect centers have been investigated by low-temperature confocal microscopy and fluorescence excitation spectroscopy. At temperatures below 90 K the fluorescence intensity of individual centers drastically diminishes because of the population of a metastable singlet state in near resonance with the optically excited state. Low-temperature fluorescence excitation spectroscopy down to 5 K becomes possible via deshelving of this state with a second laser source. Surprisingly individual centers reveal low-temperature fluorescence excitation line widths around 0.6 meV, more than two orders of magnitude larger than expected from previous high resolution laser spectroscopy on bulk samples.
Over the past few years, the detection of single N-V centers in diamond has attracted much interest, since it is expected to lead to innovative applications in various domains of quantum information. The N-V center in diamond is a defectconsisting of a substitutional nitrogen atom adjacent to a carbon-atom vacancy. The optical transition between the 3A ground state and the 3E excited state has a very high quantum efficiency allowing single defect spectroscopy. Because of the paramagnetic nature of the ground electronic state, single N-V defects are believed to be promising candidates for solid state quantum computation. To date, however, the photophysics of the defect is not entirely understood. The existence of a singlet metastable state 1A was challenged in a series of papers reporting hole-burning, optically detected magnetic resonance and single molecule experiments. We present here an overview of recent low and room temperature data, indicating the important role of a metastable state of the defect in single center experiments.
The spin-selective photokinetics of a single matrix-isolated impurity molecule with a triplet-triplet optical transition, T 0–T 1, is considered and the manifestations of the photokinetics in the fluorescence excitation spectra and intensity autocorrelation functions g (2)(τ) of the molecule undergoing narrow-band optical excitation is studied to resolve the fine structure of the transition. The rates of intersystem crossings (ISCs) T 1→S→T 0 to and from a nonradiating singlet state S of the molecule and the rate of population relaxation among the ground (T 0) state sublevels can be obtained from the spectra and g (2)(τ) using the analytical expressions obtained. New experiments on an individual NV defect center in nanocrystals of diamond, where, for the first time, the fine structure of its triplet-triplet 3 A-3 E zero-phonon optical transition (~637 nm) at 1.4 K was resolved, are interpreted. It is concluded that the rate of the ISC transition from the m S =0 sublevel of the excited 3 E state to the singlet 1 A state (~1 kHz) is much slower than the rates from the m S =±1 substates, while the rates of ISC transitions to different m S substates of the ground 3 A state are close to each other (~1 Hz). As a result, only the optical transition between m S =0 sublevels in the 3 A-3 E manifold contributes strongly to the fluorescence. The experimentally observed double-exponential decay of the g (2)(τ) function is explained by the two pathways available to the center for it to leave the S state: (i) the S→ T 0(m S )=0) transition and (ii) the S→T 0(m S =±1) transitions followed by the slow spin-lattice relaxation T 0(m S =±1)→T 0(m S =0) (rate ~0.1 Hz). The work is important for studies where the NV center is used as a single photon source or for quantum information processing.
Silicon-vacancy (SiV) color centers in diamond offer a promising system for quantum information applications owing to their intense narrowband emission and optically detectable spin states. Here, the fluorescent properties of ensembles and single SiV centers in diamonds obtained by high-pressure high-temperature synthesis from adamantane (below referred to as adamantane diamonds) are investigated at liquid-helium temperatures. Ensembles of SiV centers (~10 3 ) are studied in large diamond crystals (1–2 µm in size). Despite the large number of excited centers, the fine structure of the zero-phonon line, corresponding to four allowed optical transitions between the ground- and excited-state doublets of the SiV center, can be observed in the fluorescence spectra of these crystals. The width of individual lines is in the range of 60–80 GHz, which is explained by their inhomogeneous broadening. Single SiV centers are studied in diamond crystallites with sizes of about 200 nm. The width of the narrowest transition lines observed in the fluorescence spectra of single SiV centers under resonant excitation is almost three orders of magnitude smaller than linewidths in the spectra of SiV ensembles and is as small as 94 MHz; i.e., these lines are so narrow that their width is determined by the lifetime of the upper state of the transition. Therefore, adamantane nanodiamond features the narrowest emission line width of a single SiV center at cryogenic temperatures among other types of SiV-con-taining nanodiamonds of similar sizes obtained by the high-pressure high-temperature and chemical vapor deposition techniques.
Summary form only given. Fluorescence excitation method of single molecule spectroscopy has been applied recently to study individual nitrogen-vacancy (N-V) defect centers in diamond. These objects are of great interest owing to the proposal to build quantum computer at /sup 13/C nuclear spins neighboring the N-V center. Based on new spectroscopic information we have developed simple models of the N-V center and used them to describe a wide range of experiments dealing both with single centers and with their ensembles. The first model emphasizes possible tunneling of N atom into vacancy and describes that in terms of double well potentials. The second model takes into account the spin-triplet character of the ground electronic state of the center and allows to describe a variety of fluorescence detected magnetic resonance phenomena.
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.