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单晶化学气相沉积合成金刚石中的电荷转移效应、热致变色和光致变色

Charge transfer effects, thermo and photochromism in single crystal CVD synthetic diamond.

作者信息

Khan R U A, Martineau P M, Cann B L, Newton M E, Twitchen D J

机构信息

Diamond Trading Company, DTC Research Centre, Maidenhead, Berkshire SL6 6JW, UK.

出版信息

J Phys Condens Matter. 2009 Sep 9;21(36):364214. doi: 10.1088/0953-8984/21/36/364214. Epub 2009 Aug 19.

DOI:10.1088/0953-8984/21/36/364214
PMID:21832320
Abstract

We report on the effects of thermal treatment and ultraviolet irradiation on the point defect concentrations and optical absorption profiles of single crystal CVD synthetic diamond. All thermal treatments were below 850 K, which is lower than the growth temperature and unlikely to result in any structural change. UV-visible absorption spectroscopy measurements showed that upon thermal treatment (823 K), various broad absorption features diminished: an absorption band at 270 nm (used to deduce neutral single substitutional nitrogen (N(S)(0)) concentrations) and also two broad features centred at approximately 360 and 520 nm. Point defect centre concentrations as a function of temperature were also deduced using electron paramagnetic resonance (EPR) spectroscopy. Above ∼500 K, we observed a decrease in the concentration of N(S)(0) centres and a concomitant increase in the negatively charged nitrogen-vacancy-hydrogen (NVH) complex (NVH(-)) concentration. Both transitions exhibited an activation energy between 0.6 and 1.2 eV, which is lower than that for the N(S)(0) donor (∼1.7 eV). Finally, it was found that illuminating samples with intense short-wave ultraviolet light recovered the N(S)(0) concentration and also the 270, 360 and 520 nm absorption features. From these results, we postulate a valence band mediated charge transfer process between NVH and single nitrogen centres with an acceptor trap depth for NVH of 0.6-1.2 eV. Because the loss of N(S)(0) concentration is greater than the increase in NVH(-) concentration we also suggest the presence of another unknown acceptor existing at a similar energy to NVH. The extent to which the colour in CVD synthetic diamond is dependent on prior history is discussed.

摘要

我们报告了热处理和紫外线照射对单晶化学气相沉积(CVD)合成金刚石中点缺陷浓度和光吸收谱的影响。所有热处理温度均低于850K,该温度低于生长温度,不太可能导致任何结构变化。紫外-可见吸收光谱测量表明,经过热处理(823K)后,各种宽吸收特征减弱:270nm处的吸收带(用于推断中性单取代氮(N(S)(0))浓度)以及以约360和520nm为中心的两个宽吸收特征。还使用电子顺磁共振(EPR)光谱推断了点缺陷中心浓度随温度的变化。在约500K以上,我们观察到N(S)(0)中心浓度降低,同时带负电荷的氮-空位-氢(NVH)络合物(NVH(-))浓度增加。这两种转变的激活能均在0.6至1.2eV之间,低于N(S)(0)施主的激活能(约1.7eV)。最后,发现用强短波紫外光照射样品可恢复N(S)(0)浓度以及270、360和520nm的吸收特征。根据这些结果,我们推测在NVH和单个氮中心之间存在一个价带介导的电荷转移过程,NVH的受主陷阱深度为0.6 - 1.2eV。由于N(S)(0)浓度的损失大于NVH(-)浓度的增加,我们还认为存在另一种未知受主,其能量与NVH相似。讨论了CVD合成金刚石中的颜色对先前历史的依赖程度。

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