Comparative Analysis of Spectral Characteristics and Color Origin of Chameleon Diamond and Similar Yellow Diamond
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摘要:
Chameleon钻石（俗称“变色龙钻石”）是一种具有光致变色和热致变色现象的彩色钻石，在受热后或长时间在暗室中会由黄绿色变为黄色，在实际工作中发现与Chameleon钻石颜色相似的黄色钻石并不具有此类“变色”现象。为了研究Chameleon钻石与相似黄色钻石的差异，并进一步探究产生光致变色和热致变色现象的原因，本文选取Chameleon钻石和与其颜色相似的黄色钻石作为研究对象，进行加热实验，观察加热前后钻石颜色、紫外可见光吸收光谱的变化情况，探寻导致热致变色的原因，并对样品的红外吸收光谱及光致发光光谱特征进行详细分析与比较。结果表明：Chameleon钻石受热后由黄绿色变为黄色，在超短波紫外线下显示绿色荧光和磷光，相似黄色钻石样品无磷光及变色现象；所有样品均有从紫外光至510nm逐渐减弱的连续吸收和480nm吸收宽带，Chameleon钻石具650~800nm吸收宽带，相似黄色钻石无该吸收带，加热后吸收带消失是其产生热致变色的主要原因；进一步对样品的缺陷类型进行对比分析，Chameleon钻石红外光谱可见孤氮特征及与片晶无关的1430cm−1宽吸收带，该峰未在相似黄色钻石中出现，但产生该吸收的原因未知，仍需进一步研究，此外与Chameleon钻石相比，相似黄色钻石中氮杂质的聚合程度更高；Chameleon钻石及相似黄色钻石表现出以700nm为中心的特征发光带，此外Chameleon钻石还可检测到H3等与N-V相关缺陷及489、883、884nm等与Ni-N相关缺陷产生的发光峰。综合以上光谱学特征对比分析可知，Chameleon钻石存在与A型氮、孤氮、镍杂质及氢杂质有关的某种缺陷结构，与相似黄色钻石的光谱特征具有明显差异。本次研究对探明Chameleon钻石具热致变色现象的根本原因具有参考意义。
Abstract:BACKGROUNDChameleon diamond is a type of color diamond with photochromic and thermochromic phenomenon. If the chameleon diamond is placed in a dark room or heated for a long time, it can change from greenish yellow to fancy yellow, and return to its original color when it cools. Previous studies on chameleon diamond focus mainly on spectral characteristics. Through testing a large number of samples, the gemological and spectral characteristics of chameleon diamond are summarized. The characteristics of chameleon diamond, include a persistent yellow phosphorescence, a 480nm absorption band, and mainly the A-aggregate of nitrogen. A model to explain the thermochromic and photochromic phenomenon of chameleon diamond was proposed. The characteristics of chameleon diamond discovered by previous studies are also found in a few yellow diamonds. Diamonds colored by the 480nm band show yellow fluorescence and phosphorescence under short wave ultraviolet light, low nitrogen content, high concentrations of defects related to hydrogen and nickel, but no obvious thermochromic and photochromic phenomena. Previous studies of the chameleon diamond and similar yellow diamonds were conducted independently and did not compare the two similar diamonds.
OBJECTIVESTo ascertain the difference of spectral characteristics and defect types between chameleon diamonds and similar yellow diamonds, and then analyze the causes of thermochromic phenomenon of chameleon diamond to gain a deeper understanding of the possible structure of the center responsible for the chameleon effect.
METHODSFirstly, two chameleon diamond samples and four similar yellow diamond samples were collected to observe the color changes of the diamonds before and after heating. Top illumination and scattering illumination were used to observe the internal characteristics and color distribution of the samples. The fluorescence and phosphorescence characteristics of diamonds at long wave (365nm) and short wave (254nm) were observed by ordinary fluorescent lamp. The fluorescence and phosphorescent characteristics and growth structure of the samples under ultra-violet light were observed by DiamondViewTM. Secondly, in order to investigate the causes of thermochromism in chameleon diamond, the absorption characteristics of diamond samples in the range of ultraviolet visible light were collected before and after heating and compared with those of similar yellow diamonds. The differences in absorption spectra between chameleon diamond and similar yellow diamond were analyzed, and the causes of thermochromic phenomena were explored. Finally, an infrared spectrometer was used to collect the infrared spectrum of diamond samples and analysis of the types and impurity elements of diamond samples was conducted. Through the comparative analysis of the infrared spectrum of samples, the differences in the types and contents of nitrogen and hydrogen impurities between chameleon diamond and similar yellow diamond were obtained. The laser Raman spectrometer was used to collect PL spectra of the samples at liquid nitrogen temperature by using 473nm, 532nm and 830nm lasers. By comparing the PL characteristics of chameleon diamond and similar yellow diamond, the differences between the two defects were obtained.
RESULTSThe color distribution of the 6 diamond samples is uniform. After heating, the chameleon diamond samples change color from yellow-green to yellow, while similar yellow diamonds have no obvious color change. Under long and short wavelength UV light, the samples are yellow fluorescence without phosphorescence. The performance of the samples in this study is consistent under long and short wavelength ultraviolet light, but it is different from the previous study results that the chameleon diamond has persistent yellow phosphorescence, which further indicates that the chameleon effect is not directly related to the phosphorescence. Under ultra-violet light, the samples have green fluorescence with irregular patterns which are markedly similar to diamonds colored by the 480nm band. Chameleon diamonds show moderate green phosphorescence. All the samples have C defect absorption continuum combined with 480nm absorption band. The specific wide absorption band of 650-800nm is obvious in chameleon diamond. After being heated, the 480nm and 650-800nm absorption band of chameleon diamond completely disappears. However, the 480nm absorption band of similar yellow diamonds is weakened or has no obvious change. Therefore, the poor thermal stability of 480nm and 650-800nm absorption band is responsible for the thermochromic phenomenon of chameleon diamonds. The infrared absorption characteristics of chameleon diamond mainly show A-defect absorption. Isolated nitrogen and hydrogen-related features can be seen, in addition to the characteristic 1430cm−1 wide absorption, which has a different origin than the platelet-related 1430cm−1 feature in Cape diamond. The similar yellow diamond has higher nitrogen content, and the degree of nitrogen aggregation is higher, and does not show any type Ib character. The broadband emission of all samples occurs mainly as one band centered at 700nm, this band consists of a dozen of peaks from 595nm to 725nm in steps of about 10nm. Additionally sharp peaks at 753, 771, 799, 818, 838, 845nm are present in the chameleon diamond samples. This spectrum is virtually identical to that reported previously for diamonds containing the 480nm absorption band. Chameleon diamonds and similar yellow diamonds all contain nitrogen-vacancy, nickel-nitrogen related defects, but the amount of defects is different. Chameleon diamonds cannot be effectively distinguished based on the PL spectral. The PL spectrum analysis shows that the nickel impurity is responsible for the green fluorescence of the samples under ultra-violet light.
CONCLUSIONSThis study focuses on the comparative analysis of gemology, UV-visible absorption, infrared absorption and photoluminescence characteristics of chameleon diamond and its similar yellow diamond. Chameleon diamond is type Ia diamond with low concentration of A defect, and shows some type Ib character, such as 1240cm−1 absorption. Chameleon diamond has 480nm and 650-800nm absorption bands, that are responsible for the chameleon effect. The characteristics of chameleon diamond in this study are consistent with those in previous studies. Absorption bands of 650-800nm and absorption peaks of 1430cm−1 (unrelated to platelet) are the main differences between the chameleon diamond and similar yellow diamond sample. It is inferred that the absorption band of 650-800nm and the absorption peak of 1430cm−1 are related to the center causing the thermochromic phenomenon. Although similar yellow diamond samples also have a 480nm center, their thermal stability is different from that of chameleon diamonds. The reason for this phenomenon is unknown, therefore further studies are needed.
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数据可视化[1]是关于数据视觉表现形式的科学技术研究，研究如何真实、准确地将相对晦涩的数据通过可视的方式进行展示，从而形象、直观地表达数据蕴含的信息和规律。文献作为重要的信息载体，积累了大量有研究价值的信息，文献资料的可视化研究对知识的传播具有重要意义。
课题组对中国主要科技文献数据库中收录的文献可视化应用研究成果进行搜集整理发现，当前文献资料的可视化分析应用多与文献计量分析方法[2]相结合，运用数学和统计学方法，对文献资料进行定量分析，再采用可视化工具[3]，以聚类图谱、时间线图谱、统计图表等多种方式，将文献之间的关系以科学知识图谱[4]的方式可视化地展现[5-6]，这一技术方法的应用在挖掘文献数据蕴含的信息和规律上发挥了重要作用，但是在其空间属性挖掘展现上稍显不足，需要采用新的技术方法在这一领域开展深入研究。
GIS技术[7]是对空间数据进行相关处理分析的技术，具有采集、管理、分析、输出展示空间信息的能力，得到广泛的应用。GIS以其强大的空间信息管理与分析能力，在基础地质、矿产地质、环境地质、灾害地质等领域中发挥着重要作用。尤其是近年来“地质云”的建设，更是将GIS技术深入地融合应用到地质数据的汇聚和共享利用中。研究基于GIS技术的文献资料可视化分析方法，可以进一步拓展对文献资料的空间信息挖掘[8]和可视化应用。GIS技术如何在文献资料可视化应用中发挥作用，需要挖掘出文献资料的空间特征，确定GIS技术和文献数据之间的结合点。地质科学研究相关的文献资料记录了该领域的很多有价值成果，此类文献具备非常明显的时空特征，非常适合利用GIS技术进行可视化研究。
本研究搜集整理了2015—2020年以来公开发表的140多篇Re-Os同位素定年[9]文献资料，探索了如何运用GIS技术，挖掘此类文献的空间特征信息并进行可视化应用，开发了Re-Os同位素数据可视化服务系统，实现了对近年来发表的Re-Os同位素定年文献数据成果的空间可视化应用展现。
1. 文献数据空间可视化研究方法
文献数据的可视化研究主要有两个方面的研究内容。第一，在数据资源层面研究文献资料的共性内容特征和空间特征，其目标是汇聚一定体量的、具备空间特征信息的可结构化的文献数据，为可视化研究奠定数据基础。第二，开展可视化技术研究，从数据资源层面和GIS可视化技术两个维度进行融合探索，找到两者之间在可视化应用中的结合点，将GIS的空间可视化能力充分服务于目标信息的可视化应用需求。设计的文献资料空间可视化总体架构见图 1。
总体架构设计为包含支撑层、数据层、服务层、应用层、用户层在内的五层架构体系。其中，支撑层包含GIS数据处理分析软件、数据库软件、GIS开发组件、空间数据服务器、Web应用中间件等；数据层主要是对文献资料进行特征信息提取、规范化、空间化处理后建设的文献数据库；服务层包含空间可视化应用需要调用的空间底图数据服务和文献数据服务；应用层是面向用户提供可视化功能的文献资料可视化共享服务平台；用户层主要分为行业用户和社会公众这两大类。该架构的特点是以服务层为媒介，可以实现数据层和应用层之间的松耦合关系，保证数据库的稳定性，同时增强应用层的可灵活扩展性。
2. 文献信息挖掘
以CNKI文献资料库为数据源，以“Re”、“Os”作为关键词进行主题检索，对检索出的2015—2020年公开发表的140多篇Re-Os同位素定年文献进行收集整理并建立数据库，挖掘文献的共性特征信息和空间特征信息这两部分的内容[10-11]。通过对文献内容的分析，提出文献信息、矿产地信息、测试信息是此类文献的共性特征信息组成部分，这一发现为后续的结构化处理提供了可行性，数据内容特征信息的提取也主要以这三类信息为主，提取内容见图 2。
对此类文献的空间特征信息进行分析发现，全部140多篇文献都可以通过研究区矿产地的经纬度来进行空间定位，基于文献本身对空间位置的记载详细程度和方式，具体的定位方法包括以下三种：①直接以文献记载的经纬度进行定位；②通过文献记载的地质简图进行定位；③通过搜集研究区矿产地位置信息进行定位。
文献数据库可采用地理数据库模型Geodatabase完成数据存储，采用UML(Unified Modeling Language)建模语言[12]完成数据模型设计工作。数据库模型设计以论文、矿产地、样品为实体，结合文献资料记载的内容特征信息，每类实体延伸各自的属性内容，并在此基础上研究各类实体之间的联系，形成数据库E-R图[13]，见图 3。数据库建设方法详见文献[14]。
3. 文献数据可视化技术实现
按照前述设计的文献数据可视化五层架构体系，以Re-Os同位素定年文献数据作为数据基础，选取空间数据服务器完成文献数据服务的制作和发布，运用GIS技术开发配套的空间可视化共享服务平台，实现对文献资料的空间可视化展现。
文献数据空间可视化的核心需求是将已实现空间定位的文献数据以地图的形式进行可视化展现。为了达到更优的可视化效果和交互体验，研究重点聚焦空间数据服务展示、图例展示、空间查询等功能实现，平台实现的核心功能见表 1。
表 1 文献数据空间可视化共享服务平台核心功能Table 1. Basic function of literature data visualized share and service system.平台核心功能点 功能描述 文献数据展示 文献数据空间可视化展示 地理底图服务展示 地理底图服务空间可视化展示 图例展示 当前加载空间数据服务所对应图例的可视化展示 空间查询 对当前加载空间数据服务的点查询、多边形查询、矩形查询 3.1 技术架构
技术选型方面，采用GIS数据处理分析软件ArcGIS Desktop完成数据加工处理，采用地理数据模型Geodatabase完成空间数据存储，采用空间数据服务器ArcGIS Server完成空间数据服务的发布，发布的地图服务遵循OGC空间数据服务标准[15]，GIS开发组件采用ArcGIS API for JS开发组件，前端开发采用HTML+JavaScript+CSS技术。系统技术路线见图 4。
3.2 数据可视化
数据可视化是系统的核心功能，包含文献数据可视化、地理底图可视化、图例可视化等方面内容。
(1) 文献数据可视化
文献数据可视化采用的技术路线为: 首先将数据库中的空间数据进行渲染[16-17]并保存为MXD工程文件，然后采用ArcGIS Server[18-19]服务器将工程文件发布为MapService地图服务，最后在应用端采用JavaScript语言编程实现展示页面对地图服务的加载。通过ArcGIS API for JS开发组件提供的esri/layers/MapImageLayer接口实现对地图服务的定义和调取；通过esri/Map接口的add方法来实现对定义好的地图服务的页面加载。
(2) 地理底图可视化
系统提供对符合OGC空间数据服务标准的不同的地理底图服务的加载展示。通过esri/layers/TileLayer接口实现对地图服务的定义；通过esri/Basemap的baseLayers属性定义底图图层；通过esri/Map接口的basemap属性的定义实现对地理底图服务的页面加载。
(3) 图例可视化
系统提供对当前展示地图服务相应图例的加载和展示。通过esri/widgets/Legend接口实现对图例的定义，通过esri/views/MapView接口实现对图例的页面加载。
3.3 空间查询
系统提供对空间数据的点查询、多边形查询、矩形查询等功能。这三种方式的空间查询功能[20]主要通过对三个核心接口的调用和关键属性赋值来实现。各类查询方式实现的功能和调用的核心接口见表 2。
表 2 查询功能及核心接口说明Table 2. Specification of search function and basic API.查询功能 功能说明 核心接口 核心接口使用说明 点查询 在地图上选择要查询的点要素，以表格的形式展示当前所选要素的属性信息 esri/layers/MapImageLayer 对该接口的popupTemplate属性的定义来完成对点查询结果弹窗的内容赋值 多边形查询 在地图上绘制多边形查询范围，以表格的形式展示查询范围内所有要素的属性信息 esri/widgets/Sketch 通过该接口的layer属性定义图形绘制图层；通过view属性定义绘制的地图窗口。通过该接口的create方法激活绘图工具，绘制多边形。 esri/tasks/support/Query 通过该接口的outFields属性来获取图层的字段信息 矩形查询 在地图上绘制矩形查询范围，以表格的形式展示查询范围内所有要素的属性信息 esri/widgets/Sketch 通过该接口的layer属性定义图形绘制图层；通过view属性定义绘制的地图窗口。通过该接口的create方法激活绘图工具，绘制矩形。 esri/tasks/support/Query 通过该接口的outFields属性获取图层的字段信息 4. 文献可视化分析
按照上述可视化方法，对140多篇Re-Os同位素定年文献进行了数据挖掘和可视化分析，研究区覆盖中国东中西部地区的140多个矿产地，主要矿种包括铜、钼、钨、金等共19种，实现了对Re-Os同位素定年文献的空间可视化展现，以及对属性信息的点、矩形、多边形综合查询。
4.1 论文发表信息
系统展示了Re-Os同位素定年文献发表时间、发表刊物的分布情况，可视化结果详见图 5。通过可视化的数据分析，Re-Os同位素定年研究数量在2015—2016年尤为突出，相关论文主要发表于38种刊物。
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图 5 (a) 论文发表数量按发表时间统计(2015—2020)；(b)论文发表数量按发表刊物统计(2015—2020)Figure 5. (a) Numbers of published papers counted according to the time of publication (2015—2020); (b) Numbers of published papers counted according to the published journals (2015—2020).4.2 矿产地信息
矿产地信息主要展示了Re-Os同位素定年文献记载的研究区矿产地分布情况，可视化结果详见图 6。可以看出，在搜集的文献范围内，近年来开展的Re-Os同位素定年研究在地理上中国东中西部地区都有分布，尤其在东南区域分布较集中。研究区主要矿种共19种，以铜[21-24](29.0%)、钼[25-27](28.3%)、钨[28-30](12.4%)、金[31-33](11.0%)为主。
4.3 分析测试信息
分析测试信息主要展示了Re-Os同位素定年文献记载的检测单位、检测设备、检测对象、检测年龄等信息的分布情况，可视化结果详见图 7、图 8。
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图 7 (a) 样品检测数量按检测单位统计(2015—2020)；(b)样品检测数量按检测设备统计(2015—2020)；(c)样品检测数量按检测对象统计(2015—2020)Figure 7. (a) Numbers of tested samples according to the laboratories (2015—2020); (b) Numbers of tested samples according to the analytical instruments (2015—2020); (c) Numbers of tested samples according to the detected objects (2015—2020).在搜集的文献范围内，Re-Os同位素定年样品测试工作主要在11家单位进行，较为集中在国家地质实验测试中心，测试样品地理分布上遍布东中西矿产地，占比达79.9%。Re-Os同位素定年测试仪器多采用电感耦合等离子体质谱仪(ICP-MS)[34]，占比达86.0%，少量采用热电离质谱仪(TIMS)[35-36]。质谱仪型号多为TJA X-series ICP-MS，占比70.8%。检测对象共计12种，包括辉钼矿、黄铁矿、黄铜矿、磁黄铁矿、灰岩、油砂岩、碳质泥岩、石墨、钼矿、黑色页岩、固体沥青、毒砂。其中，以辉钼矿作为检测对象的研究在数量上明显突出，占比达80.7%，表明辉钼矿仍是Re-Os同位素定年法的首选研究对象，这与辉钼矿的高Re/Os值特性密不可分。
考虑到分布的均衡性，检测年龄划分为五个区间：0~100Ma、100~200Ma、200~300Ma、300~600Ma、600~1522Ma。其中，落在0~200Ma较新年龄区间的矿产地多分布在中国东北和东南区域，该年龄区间矿产地占比达62.1%，表明东部地区的Re-Os同位素年龄集中分布在中生代，这与中国东部地区存在中生代大规模成矿事件[37]是相一致的；落在200Ma以上较老年龄区间的矿产地多分布在中国中部和西部区域，该年龄区间矿产地占比达37.9%，表明中西部地区的Re-Os同位素年龄集中分布在中生代以前，且具有多期次成矿的特点。
5. 结论
本研究探索了基于GIS技术对文献资料进行可视化的技术方法，形成了对文献数据进行信息挖掘和空间可视化的策略和技术路线。并以Re-Os同位素定年文献数据为例，对该技术方法进行了应用验证，建设了具有GIS空间特征的铼锇同位素定年数据库和空间可视化共享服务平台。研究表明GIS技术在文献资料的可视化应用中可发挥特殊作用，该可视化方法具备可视化对象的空间性、可视化过程的交互性、可视化方式的融合性、可视化展示的直观性等特点。
本研究提出的技术方法，可挖掘出文献资料的空间特性，拓展文献资料在空间可视化领域的应用性，解决文献资料如何进行共性信息分析提取、空间特征信息定位、空间可视化技术实现等问题。在后续研究中，建议从数据资源和可视化方法方面进行深入研究，在数据资源层面，从广度和深度丰富数据内容，挖掘数据价值；在可视化方法方面，研究多种可视化技术的综合运用，增强文献资料信息的可利用价值。
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图 1 Chameleon钻石及相似黄色钻石样品加热前后颜色变化及在DiamondViewTM下的发光图像
Figure 1. Color change of chameleon diamond and similar yellow diamond samples before and after heating and luminescence images by ultra-violet light of DiamondViewTM. After heating, the chameleon diamonds showed obvious change, while the similar yellow diamond did not. Under ultra-violet light of DiamondViewTM, all samples showed green fluorescence, the chameleon diamond showed green phosphorescence, while sectional yellow diamond samples were phosphorescent inertia.
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图 2 样品ChaD1、YD1和 YD3紫外可见光吸收特征
a—样品ChaD1、YD1和 YD3加热前后紫外可见光吸收特征对比； b—样品ChaD1加热前后紫外可见光吸收特征对比； c—样品YD1加热前后紫外可见光吸收特征对比； d—样品YD3加热前后紫外可见光吸收特征对比。
Figure 2. UV-Vis absorption characteristics of ChaD1, YD1 and YD3 samples. a: Prior to heating, the samples have C defect absorption continuum and 480nm absorption band. In addition, the chameleon diamond has 650-800nm band. b: After heating the chameleon diamond ChaD1, the 650-800nm band disappeared, and the 480nm band significantly weakened. c and d: The change of similar yellow diamond sample was not obvious before and after heating.
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图 3 样品ChaD1、YD1和 YD3红外光谱吸收特征
a—样品ChaD1、YD1、YD3红外光谱特征； b—样品ChaD1、YD1、YD3一声子区红外吸收特征； c—样品ChaD1、YD1、YD3中与氢杂质相关缺陷吸收特征。
Figure 3. The FTIR spectra of tested samples ChaD1, YD1 and YD3. a: ChaD1, YD1 and YD3 are all type Ia diamonds, the nitrogen concentration of similar yellow diamonds is significantly higher than that of chameleon diamonds. b: Chameleon diamond has the 1430cm−1 absorption, which has a different origin from the platelet-related 1430cm−1 feature. In addition, the similar yellow diamond has obvious aggregates of nitrogen absorption, while chameleon diamond shows a weak type Ib character. c: The hydrogen-related absorptions indicates chameleon diamond has a type Ib character.
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图 4 样品ChaD1、YD1和 YD3的PL光谱特征
a—532nm激光源下样品的PL光谱特征; b—473nm激光源下样品的PL光谱特征; c—830nm激光源下样品的PL光谱特征。
Figure 4. PL spectra of ChaD1, YD1 and YD3 samples. a. PL spectral characteristics of samples with 532nm excitation. The main feature is a broad emission band centered at about 700nm, this band consists of a dozen of peaks from 595nm to 725nm in steps of about 10nm. Additionally sharp peaks at 753, 771, 799, 818, 838, 845nm present in the chameleon diamond. b, c: PL spectral characteristics of samples with 473nm, 830nm excitation, respectively. The peaks at 503.2, 489, 883, 884nm are detected in the samples, indicating the presence of N-V and Ni-N related defects.
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