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Optics Letters

Large prolongation of free-exciton photoluminescence decay in diamond by two-photon excitation

Martin Kozák, F. Trojánek, P. Malý

Published May 29, 2012• 25 citations
Publisher

Abstract

We report on time-resolved photoluminescence of a free-exciton in IIa chemical vapor deposition diamond crystal. Large difference between decay times for one- and two-photon excitation processes was observed. The longest room-temperature exciton photoluminescence lifetime τ(FE)=220 ns was obtained under two-photon excitation with a photon energy of 4.7 eV. The role of diffusion and surface recombination velocity in exciton photoluminescence dynamics was studied using a new optical method based on two-photon excited time-resolved photoluminescence. The measured room-temperature value of diffusion coefficient in diamond was D=40 cm(2)/s.

DOI
10.1364/ol.37.002049

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We report on time-resolved photoluminescence of a free-exciton in IIa chemical vapor deposition diamond crystal. Large difference between decay times for one- and two-photon excitation processes was observed. The longest room-temperature exciton photoluminescence lifetime τ(FE)=220 ns was obtained under two-photon excitation with a photon energy of 4.7 eV. The role of diffusion and surface recombination velocity in exciton photoluminescence dynamics was studied using a new optical method based on two-photon excited time-resolved photoluminescence. The measured room-temperature value of diffusion coefficient in diamond was D=40 cm(2)/s.
Abstract This study presents a detailed investigation into the fluorescence properties of color centers in single-crystal diamond needles (SCDNs) synthesized via chemical vapor deposition. Using steady-state and time-resolved photoluminescence (PL) techniques, we identified color centers with zero-phonon lines at 389 nm, 468 nm, 575 nm (NV0), 637 nm (NV–), and 738 nm (SiV–). PL excitation spectroscopy conducted at room temperature revealed the complex electronic structure of some of these centers, paving the way for further investigation into their fluorescence properties. Lifetime measurements were performed for each center, with the 389 nm one exhibiting the longest decay time (∼30 ns), which is advantageous for enhancing quantum coherence, improving photon emission efficiency, and reducing power consumption. Altogether, these findings highlight the potential of SCDNs for quantum applications and confirm their promise as a platform for next-generation photonic and quantum devices.
We observe exceptionally high diffusion of excitons in diamond using time-resolved photoluminescence imaging. The diffusivity is found to increase with decreasing temperature more rapidly than well-established predictions. The highest diffusion constant, $9.2\ifmmode\times\else\texttimes\fi{}{10}^{3}\phantom{\rule{0.28em}{0ex}}{\mathrm{cm}}^{2}/\text{s}$, measured for thermalized excitons is 150 times that recorded previously in diamond. We elucidate the momentum relaxation mechanisms determining transport: intraband and interband scattering by acoustic phonons in the exciton fine-structure levels. The enhanced diffusivity above 100 K is explained by a free-carrier contribution.
A detailed study of the photophysical properties of several chromium-related color centers produced within chemical vapor deposition diamond is presented. These emitters show narrow luminescence lines in the range of $740\ensuremath{-}770$ nm. Single-photon emission was verified with continuous and pulsed excitation with detected emission rates at saturation in the range of ($2\ensuremath{-}3$) $\ifmmode\times\else\texttimes\fi{}$ 106{10}^{6}106 counts/s, while direct lifetime measurements reveal excited state lifetimes for the distinct centers ranging $1\ensuremath{-}14$ ns. In addition, a number of quantum emitters demonstrate two-level behavior with no bunching present in the second-order correlation function. The three-level systems revealed typically photoluminescence lines with width half-maximum of  4~4 4 nm while the two-level emitters have full width half-maximum of  10~10 10 nm at room temperature. In addition, the quantum efficiency of the two-level system was measured to be four times higher than that of the three-level system.
The fabrication of stable ultrabright single photon sources operating at room temperature is reported. The emitter is based on a color center within a diamond nanocrystal grown on a sapphire substrate by chemical vapor deposition method and exhibits a two-level electronic behavior with a maximum measured count rate of 3.2 x 10(6) counts/s at saturation. The emission is centered at approximately 756 nm with a full width at half-maximum approximately 11 nm and an excited state lifetime of 3.7 ns. These unique properties make it a leading candidate for quantum photonics and communication applications as well as for cellular biomarking.
Abstract We have observed edge emission due to free excitons and electron–hole droplets in diamond by two‐photon excitation using subpicosecond laser pulses at 257 nm. We find that excitonic temperatures under two‐photon excitation are much lower than the case of one‐photon excitation. A minimum excitonic temperature of 3.4 K is extracted by spectral analysis. In order to understand the difference of the excitonic temperatures under two‐photon and one‐photon excitations, we discuss a heating mechanism which depends on the density distribution of the electron–hole pairs in the crystal along the laser beam. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
Optical absorption spectra in the spectral range from 200 nm to 15 μm, Raman spectra in the wavenumber range of 100–3700 cm –1 , and photoluminescence spectra in the spectral range of 200–850 nm have been studied for five nominally “pure” diamond samples synthesized in different ways. The measurements have been carried out in the temperature range of 80–300 K. Photoluminescence was excited by the KrCl laser radiation at a wavelength of 222 nm with a pulse FWHM of 8 ns and a peak intensity on the sample surface of up to 13 MW/cm 2 . It is found that, at absorption coefficients of diamond samples below 10 cm –1 in the spectral range of 225–226 nm, their photoluminescence spectra exhibit a radiative recombination band of electron–hole liquid peaked at 240 nm.