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Optics and Spectroscopy

Optical spectra and electron–Hole liquid in diamond

E. I. Lipatov, D. E. Genin, В. Ф. Тарасенко

Published Dec 1, 2015• 12 citations
Publisher

Abstract

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.

DOI
10.1134/s0030400x15120164

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In our work we investigated different optical characteristics of five diamond samples that were supposed to be pure. The characteristics were the following: optical absorption spectra in the range 200 nm – 15μm, Raman scattering spectra in the range 100-3700 cm-1 and photoluminescence spectra in the range 200 – 850 nm. The temperature of diamond samples was varied from 80 to 300 K. Photoluminescence was excited by KrCl*-laser radiation (λ=222 nm) with pulsewidth of 8 ns (FWHM) and peak intensity of 13 MW/cm2. We found out that the band of radiative recombination of the electron-hole liquid (with the maximum at 240 nm) can be observed in the photoluminescence spectra if the absorption coefficient of the diamond sample is less than 10 cm-1 in the range 225-226 nm.

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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.
In our work we investigated different optical characteristics of five diamond samples that were supposed to be pure. The characteristics were the following: optical absorption spectra in the range 200 nm – 15μm, Raman scattering spectra in the range 100-3700 cm-1 and photoluminescence spectra in the range 200 – 850 nm. The temperature of diamond samples was varied from 80 to 300 K. Photoluminescence was excited by KrCl*-laser radiation (λ=222 nm) with pulsewidth of 8 ns (FWHM) and peak intensity of 13 MW/cm2. We found out that the band of radiative recombination of the electron-hole liquid (with the maximum at 240 nm) can be observed in the photoluminescence spectra if the absorption coefficient of the diamond sample is less than 10 cm-1 in the range 225-226 nm.
In the light of the creation of a diamond laser [1], an urgent task is to determine the characteristics of diamonds in order to determine the range in which such lasers can be created not in isolated cases. This work is aimed at studying the mechanisms of creating superluminescence in diamond under the action of optical pumping by the second harmonic of an ND:YAG laser (λ = 532 nm). It was found that, upon pulsed excitation of a diamond by an ND:YAG laser with a pump intensity above ~2.0 MW/cm2 in the spectral range 700–750 nm, a nonlinear increase in intensity appears against the background of the spontaneous photoluminescence spectrum, which, with a further increase in the pump intensity, turns into a pronounced superluminescence peak with a maximum at about 718 nm. An increase in the pump intensity from 2.7 to 46 MW/cm2leads to the broadening of this peak at half maximum from 13 to 19 nm. At high levels of pump intensity, nonlinear absorption of pump radiation and accumulation of NV centers in the excited state were found. The position of the photoluminescence band was calculated as a function of various values of the inversion density of the populations of color centers, taking into account the intrinsic absorption spectrum of diamond. The calculation results are close to the experimental data.
The photoluminescence spectra of two synthetic diamond samples containing 1-10 ppm NV centers and 100-200 ppm substitutional nitrogen were studied under optical pumping at 532, 560, and 575 nm. At pump intensities less than 0.5-1.0 MW/cm2, a vibronic photoluminescence band of NV- centers in the negative charge state was observed. With an increase in the pump intensity above 0.5-1.0 MW/cm2, a superluminescence band was observed on the long-wavelength shoulder of the phonon wing in the range 700-760 nm. The intensity of superluminescence band increased with increasing pump intensity. It is shown that the position of the superluminescence band with maxima in the range 715-720 nm is unchanged at all of optical pump wavelengths.
Abstract Superluminescence of NV centres with a band peaking at λ = 718 nm in the phonon wing of the photoluminescence spectrum of a high-pressure high-temperature (HPHT) diamond sample under pulsed optical excitation at λ = 532 nm with an intensity of 2 – 46 MW cm−2 is demonstrated. Superluminescence is observed in the diamond crystal region containing 6 ppm NV centres and 150 ppm substituent nitrogen; it is absent in the crystal part with a lower nitrogen content. Superluminescence pulses are observed on the leading edge of the optical excitation pulse at λ = 532 nm and have an FWHM value of 4 ns. The enhancement of the photoluminescence of NV centres is suggested to be due to the total internal reflection in the diamond plate (waveguide effect).
Abstract— A comparative analysis has been made of the superluminescence spectra of two HPHT diamond samples with NV¯-centers with the concentration in the growth sectors {111} of NV¯-centers ≈10 ppm and of C-centers ≈ 45 ppm. A broad structureless superluminescence band with a maximum about 706 nm and a narrow band in the region of 705 to 720 nm were identified in the spectral range of 650–750 nm when excited by pulsed laser radiation at λ = 532 nm. It was found that the narrow-band superluminescence was not excited by pumping with continuous radiation at λ = 532 nm and the intensities of both types of superluminescence were summated under simultaneous pumping by continuous and pulsed radiation at λ = 532 nm. These data indicate either the different nature of the two types of superluminescence or that they belonged to NV¯ centers but with different excitation mechanisms. The existence of connection between the shape of the spectra of narrow-band superluminescence and of radiation pulses has been demonstrated. The observed features of narrow-band superluminescence are explained for the first time by the occurrence of mode-locking laser generation. The mode-locking laser generation without the use of reflective coatings on the sample or an external resonator on other laser materials has not been observed before.
Abstract In the context of the NV− diamond laser creation [1], an urgent task is to determine the characteristics of diamonds that can affect the laser generation. This work is aimed at investigating the mechanisms of the creation of superluminescence in diamond under the action of optical pumping by the second harmonic of the Nd:YAG laser (λ = 532nm). It was found that when the HPHT diamond is irradiated by 532 nm radiation with an intensity above ~ 2.0 MW/cm2, a nonlinear intensity increasing in the spectral region 700–750 nm is manifested against the background of the spontaneous photoluminescence spectrum, which, with a further pumping intensity increasing turns into a pronounced peak of superluminescence with a maximum of about 718 nm. An increase in the pumping intensity from 2.7 to 46 MW/cm2 widened this peak at half-maximum from 13 to 19 nm. At high levels of pumping intensity, nonlinear pumping radiation absorption and accumulation of NV centers in the excited state were detected. The position of the photoluminescence band was calculated depending on different values of the population inversion density of the color centers, taking into account the diamond's own absorption spectrum. The calculation results are close to the experimental data.