The Study of Pigments in Cultural Heritage: A Review Using Machine Learning
Abstract
:1. Introduction
2. Methods
2.1. Data Collection Process
2.2. Topic Modeling
3. Results
3.1. The Evolution of Literature on the Study of Pigments from 1999–2023
3.2. Analysis of the Topics
- Topic 1 (T1): The spectroscopic and microscopic study of pigments in paintings
- Topic 4 (T4): Raman spectroscopic analysis of pigment samples
- Topic 5 (T5): X-ray techniques dedicated to materials characterization (including pigments) in CH
- Topic 6 (T6): Imaging methods (including hyperspectral imaging) for the examination of paintings
- Topic 7 (T7): Chromatographic and spectroscopic methods for the identification of organic pigments and dyes
- Topic 9 (T9): The analytical study of paint and pigment degradation
- Topic 10 (T10): The technical study of paintings and illuminated manuscripts
- Topic 2 (T2): Fungal deterioration and other types of biodeterioration of CH assets
- Topic 3 (T3): The analysis of mineral compounds contained in CH assets
- Topic 8 (T8): Scientific research for restoration and conservation of CH assets and materials
3.3. The Pigment Cluster
3.3.1. Topic 1 (T1)
3.3.2. Topic 4 (T4)
3.3.3. Topic 5 (T5)
3.3.4. Topic 6 (T6)
3.3.5. Topic 7
3.3.6. Topic 9
3.3.7. Topic 10
3.4. Remaining Unclear Topics
3.4.1. Topic 2
3.4.2. Topic 3
3.4.3. Topic 8
3.5. The Final Labels of the Topics
3.6. Time Trends
4. Discussion and Conclusions
Supplementary Materials
Funding
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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T1 | T2 | T3 | T4 | T5 |
pigments (0.0274) | fungi (0.0123) | glass (0.0106) | Raman (0.0410) | analysis (0.0209) |
spectroscopy (0.0194) | fungal (0.0104) | archaeological (0.0101) | spectroscopy (0.0269) | heritage (0.0203) |
paintings (0.0159) | biodeterioration (0.0082) | mineral (0.0089) | pigments (0.0229) | cultural (0.0196) |
analysis (0.0125) | potential (0.0080) | composition (0.0086) | spectra (0.0198) | materials (0.0178) |
Painting (0.0123) | heritage (0.0080) | black (0.0071) | laser (0.0177) | X-ray (0.0118) |
X-ray (0.0117) | stone (0.0077) | chemical (0.0069) | samples (0.0100) | pigments (0.0115) |
microscopy (0.0115) | paper (0.0076) | minerals (0.0059) | analysis (0.0098) | techniques (0.0107) |
techniques (0.0099) | species (0.0069) | Spain (0.0051) | fluorescence (0.0089) | objects (0.0097) |
white (0.0095) | growth (0.0059) | Italy (0.0049) | different (0.0080) | study (0.0094) |
study (0.0091) | microorganisms (0.0057) | analysis (0.0047) | identification (0.0076) | different (0.0078) |
T6 | T7 | T8 | T9 | T10 |
imaging (0.0322) | organic (0.0198) | restoration (0.0168) | paint (0.0120) | painting (0.0116) |
reflectance (0.0168) | natural (0.0148) | conservation (0.0123) | degradation (0.0112) | manuscripts (0.0113) |
spectral (0.0163) | synthetic (0.0129) | heritage (0.0108) | pigments (0.0106) | century (0.0095) |
pigment (0.0149) | samples (0.0097) | mural (0.0105) | pigment (0.0104) | study (0.0094) |
hyperspectral (0.0121) | identification (0.0090) | paper (0.0097) | color (0.0093) | materials (0.0092) |
paintings (0.0112) | spectrometry (0.0071) | materials (0.0080) | paints (0.0090) | conservation (0.0086) |
using (0.0105) | chromatography (0.0067) | wooden (0.0073) | study (0.0078) | fluorescence (0.0076) |
painting (0.0098) | method (0.0062) | cultural (0.0070) | different (0.0063) | collection (0.0054) |
images (0.0091) | madder (0.0060) | research (0.0069) | cleaning (0.0062) | palette (0.0052) |
spectra (0.0087) | liquid (0.0059) | scientific (0.0068) | results (0.0061) | technical (0.0052) |
Topic 1 (T1) | |||
---|---|---|---|
Article Number | CH Asset Studied | Research Method | Analytical Techniques Used |
Article 1 | Polychrome wooden carpentry | Micro-invasive | EDXRF, OM, XRD, SEM-EDX, Raman, FTIR |
Article 2 | Gouache sketches | Micro-invasive | EDXRF, OM, SEM-EDX, FTIR |
Article 3 | Oil on copper painting | Non-invasive | EDXRF, XRD, Raman, DRIFT |
Article 4 | Wall painting | Micro-invasive | FE-SEM, SEM-EDX, Raman, FTIR |
Article 5 | Easel painting (altarpiece) | Non-invasive | ED-XRF, Raman |
Article 6 | Wall painting (small fragments) | Non-invasive | Raman, FTIR, UV-Vis and chromatic studies |
Article 7 | Painted limestone reliefs | Micro-invasive | OM, UVF imaging, VIL imaging, micro-XRF, LA-ICPMS, micro-XRPD, FTIR |
Article 8 | Wall painting | Micro-invasive | OM, SEM-EDX, FTIR, XRD |
Article 9 | Wall painting | Micro-invasive | OM, SEM-EDX, FTIR, XRD |
Article 10 | Wooden sculpture | Micro-invasive | EDXRF, µXRF, XRD, Raman |
Topic 4 (T4) | |||
---|---|---|---|
Article Number | Test Sample(s) | Considered Issue | Tested Research Technique/Method/Setup |
Article 1 | Cinnabar pigment embedded in wax; sulfur crystal | Fluorescence issue in Raman analysis | shift-excitation Raman difference spectroscopy-difference deconvolution (SERS–DDM) |
Article 2 | Free-standing vermilion oil-paint samples | Low-quality terahertz spectra databases | Terahertz time-domain (THz–TDS) |
Article 3 | Red organic dyes (brazilwood, dragon’s blood, carmine, and madder lake) applied on pulsed ablated gold and silver nanostructured substrates | Weak Raman activity of red organic dyes | SERS; Pulsed laser ablation of gold and silver nanoparticles to produce SERS active substrates |
Article 4 | Pigment samples | Combined use of spectroscopic techniques in a hybrid unit | Laser induced breakdown spectroscopy (LIBS); Raman spectroscopy using a nanosecond pulsed Nd:YAG laser (532 nm) |
Article 5 | Pigment samples (inorganic pigments) | Usage of reflection THz–TDS configuration | THz–TDS |
Article 6 | Paint samples (wall painting) | Combined use of spectroscopic techniques in a hybrid unit | LIBS; Raman spectroscopy using a Q-switched nanosecond Nd:YAG laser (532 nm, 355 nm, 226 nm) |
Article 7 | Paraloid B72; lead white pigment; beeswax; marble | Fluorescence problem in Raman analysis | time-gated pulsed Raman spectroscopy with a ns pulsed laser |
Article 8 | Pigment and paint samples (traditional Korean organic and inorganic pigments mixed animal glue and alum applied on Korean traditional paper) | Absence of complete THz spectral databases for artist’s pigments; lack of analytical methods for the THz-based analysis of heterogenous samples | THz–TDS; FTIR |
Article 9 | Pigment and paint samples (red semi-organic pigments and organic dyes) | Fluorescence problem in Raman analysis | Time-gated Raman spectroscopy based on spectral multiplexed detection; micro-spatially offset Raman spectroscopy (micro-SORS) |
Article 10 | Red organic dyes (carmine lake, garanza lake and brazilwood) applied on silver pulsed ablated silver nanostructured substrates | Weak Raman activity of red organic dyes | SERS; Pulsed laser ablation of silver nanoparticles to produce SERS active substrates |
Topic 6 (T6) | |||
---|---|---|---|
Article Number | CH Material Studied | Issue Considered | Tested, Developed, or Evaluated Experimental Methods/Models/Algorithms |
Article 1 | Film-forming low-gloss wood lacquer for outdoors applied to (1) a reflective silicon wafer, (2) cover glasses positioned on a black-and-white checkerboard, (3) medium-density fiberboard (MDF) | Thickness measurements of paints and coating by means of HSI | Coefficient-independent scattering model for hyperspectral imaging (HSI) |
Article 2 | Oil on copper painting; reference mock-up copper painting | Unmixing of hyperspectral reflectance data for pigment mixture identification | Two Subtractive mixing models (linear mixture and deep learning-based mixture model) used in two spectral reflectance hyperspaces (R hyperspace and log(R) hyperspace) |
Article 3 | Fresco paintings | Reveal frescoes covered by a plaster or limewash layer | Theoretical optimization study of the spatial resolution of cooling-down infrared imaging |
Article 4 | Reference illuminated leaf; mock-up canvas paintings (inorganic pigments bounded in Arabic gum applied to commercially primed canvas; 12 pure pigments and 16 pigment mixtures) | Unmixing of hyperspectral reflectance data for pigment mixture identification | A two-step algorithm using a deep neural network |
Article 5 | Oil on canvas painting | Data reduction and visualization of hyperspectral data (for pigment identification and mapping) | Uniform Manifold Approximation and Projection (UMAP) (i.e., data reduction method using graph layout algorithms to arrange HSI data in low-dimensional space); endmember extraction pipeline |
Article 6 | Illuminated leaves | Automatic endmember determination and the creation of classification maps from reflectance imaging spectroscopy (RIS) for pigment identification | Maximum Distance (MaxD); spectral library matching algorithm; ENVI spectral hourglass wizard (ENVI-SHW) |
Article 7 | Mock-up panel painting with model paint patches consisting of 16 lake pigments mixed in linseed oil or egg yolk | Acquisition of luminescence spectroscopic data with high spectral resolution and megapixel information describing a paint surface | Combining luminescence spot spectroscopy and multispectral imaging; methodology for the preprocessing of the multispectral recording (including noise reduction) and for spectral estimation based on a neural network algorithm |
Article 8 | Mock-up canvas painting with model paint patches consisting of inorganic pigments and one synthetic organic pigment (i.e., Novoperm Carmine Red) mixed with linseed oil | Pigment classification based HSI data | Evaluating the effect of HSI imaging acquisition parameters (i.e., focus distance, signal-to-noise ratio, integration time and illumination geometry) on the accuracy of pigment classification |
Article 9 | Mock-up painting | Pigment classification based HSI data | Evaluating the performance of supervised-based algorithms and machine learning models for pigment classification |
Topic 7 (T7) | |||
---|---|---|---|
Article Number | CH Material Studied | Research Objective(s) | Analytical Techniques Used/Developed/Tested |
Article 1 | Carthamin | Improve synthesis of a C-Glycisyl quinochalcone | Synthesis method |
Article 2 | Dragon’s blood resin (laboratory and historical samples) | Authentication of dragon’s blood resins by identifying marker compounds | High-performance liquid chromatography with photodiode-array detection (HPLC–PAD); extraction protocol; HPLC–PAD database |
Article 3 | Indigo and carthamin red and yellow extracted from dyed wool laboratory samples | Extraction methods; identification of the best conditions for the extraction of marker compounds of organic dyes | High-performance liquid chromatography with photodiode-array detection connected to mass spectrometry (HPLC–PAD–MS) |
Article 4 | Cochineal (laboratory and historical samples extracted from painting and silk textile) | Dye identification; Structure elucidation of minor marker compounds of cochineal | Medium pressure liquid chromatography (MPLC); HPLC–PAD; HPLC–PAD–MS; Nuclear Magnetic Resonance (NMR) |
Article 5 | Carthamin (historical silk textile samples) | Dye identification; Structure elucidation of compounds of carthamin | HPLC with UV detection coupled with electrospray ionization tandem mass spectrometry (UV–vis–ESI–MS/MS) and high-resolution Orbitrap mass spectrometry (HPLC–HESI–HRMS) |
Article 6 | Madder dye | Field research to record indigenous method of cloth dyeing using madder dye | Field research; phytochemical analysis, UV-visible spectroscopy; Fourier transform infrared spectroscopy (FTIR) |
Article 7 | Reference samples of shellfish purple and archaeological samples consisted of residues of a pink-violet substance acquired from ceramic fragments | Dye identification; Applicability of laser-based ionization techniques for the identification of purple dyes in historical and archaeological objects | Negative-mode laser desorption/ionization mass spectrometry (LDI–MS) |
Article 8 | Winsor and Newton 19th-century madder pigments | Study of synthesis methods | UV–vis spectroscopy, colorimetry, EDXRF, FTIR; HPLC–PAD |
Article 9 | Dyes and metal thread (historical samples extracted from silk textiles) | Dye and metal identification | HPLC–PAD; field-emission scanning electron microscopy (FESEM) with energy dispersive X-ray spectroscopy (EDX) for the identification of metal |
Article 10 | Synthetic organic dyes (e.g., eosin Y and carmine) used in printing and painting (reference and historical samples) | Sample pretreatment method; develop a new sample pretreatment method with nitric acid for SERS analysis of dyes used as artists’ materials | Surface-enhanced Raman spectroscopy (SERS) |
Topic 9 (T9) | |||
---|---|---|---|
Article Number | CH Material Studied | Research Objective | Analytical Techniques Used/Developed/Tested |
Article 1 | Inorganic pigments (Fe2O3, Pb3O4, PbCrO4, TiO2) used in Dancheong (polychromed wooden building and artefacts) (laboratory pigment samples) | Impact of gamma irradiation procedure on the optical and structural properties of inorganic pigments | 1, 5 and 20 kGy gamma radiation, colorimetry (study changes in CIE color values); XRD (study changes in crystal structure) |
Article 2 | Acrylic emulsion paint on canvas (laboratory samples, i.e., young, light aged and aged model paints) | Measuring the rate of water penetration from conservation treatment gels into acrylic emulsion paints on canvas; applicability of unilateral NMR for comparing depth penetration of water | Nuclear Magnetic Resonance unilateral sensor (unilateral NMR) |
Article 3 | Zinc oxide (ZnO) in oil paintings (laboratory samples) | Study the interaction between of (a) ZnO and oil carboxylic acids and acetates, and (b) the formation of ZnO degradation products (Zn soaps/carboxylates); test the applicability of DFT for the study of oil paint degradation | Density functional theory (DFT) modeling |
Article 4 | Linseed oil and tung oil binders used for historical armor paints (naturally aged and accelerated aged replica armor paint, historical samples) | Ageing and degradation reactions of oil-based binding media in anticorrosive armor paint; study the interaction between the pigments and binding media, and the formation of degradation products | Gas chromatography–mass spectrometry (GC–MS); FTIR; contact angel measurements, colorimetry |
Article 5 | Linseed oil and tung oil binders used for historical armor paints (fresh drying oils, air blown oils, heat bodied oils and oil in paint laboratory samples) | Study the ageing characteristics of oil binders to understand their technical function as part of anticorrosive armor paints; identification of the chemical composition of commercially available refined and bodied linseed and tung oils | GC–MS; FTIR; water immersion test; testing chemical and physical properties of oils executed by a quality-certified oil laboratory |
Article 6 | Prussian blue (pigment, paper, textile, paint, ducos du Hauron, cyanotype laboratory samples) | Understanding the roles of the substrate in the fading behavior of Prussian blue; protocol to investigate the fading process of Prussian bule on a substrate | Scanning electron microscopy (SEM); XRD; spectrophotometry; X-ray absorption near edge structure (XANES); Raman spectroscopy |
Article 7 | Oil canvas paintings (laboratory samples) | Study the impact of repeated relative humidity variations on the viscoelastic behavior of paint films; development of a nanoindentation protocol to evaluate the mechanical properties of paint films at microscale | Nanoindentation |
Article 8 | Casein paint (laboratory paint samples) | Systematic study of the influence of pigments and protein aging on casein identification | Protein extraction with ammonium bicarbonate and trifluoro-ethanal; NanoOrange method before and after artificial aging; Enzyme-linked immunosorbent assay (ELISA) method |
Article 9 | Proteinaceous paint binders (laboratory binder and paint samples) | Study of UV ageing process of proteinaceous paint binders and the role of non-proteinaceous painting materials (i.e., lipids from linseed oil, terpenic compounds from varnish, inorganic pigments) | FTIR; principal component analysis |
Article 10 | Eosin Y-based lakes (laboratory samples) | The characterization of photodegradation of Eosin Y under different illumination and in oxic and anoxic conditions; identification different degradation pathways | UV–Vis spectrophotometry; liquid chromatography quadrupole time-of-flight mass spectrometry (LC–QToF–MS); electrochemistry techniques |
Topic 10 (T10) | ||||
---|---|---|---|---|
Article Number | CH Object Studied | Research Aim | Research Approach | Analytical Technique(S) Used |
Article 1 | Oil painting on panel | Characterization of the pigment palette and techniques of Raffaello Sanzio (1483–1520) | Non-invasive | Macro X-ray fluorescence (MA–XRF) scanning |
Article 2 | Oil paintings on canvas and cardboard (cross-sectioned samples) | Characterization of the pigment palette of Pio Collivadino (1869–1945) from a corpus of representative works of different time periods; comparison between Collivadino’s palette and contemporary European artists | Micro-invasive | Raman spectroscopy |
Article 3 | Oil painting on copper | Characterization of the pigment palette and techniques of the painting Venus with Mars and Cupids, attributed to Carlo Saraceni (1579–1620); Assess the painting’s state of conservation (including identifying old restorations) | Non-invasive | Visual analysis; visible and raking light photography; ultraviolet induced fluorescence (UVIF) photography infrared reflectography (IRR), portable EDXRF |
Article 4 | Illuminated manuscripts and hand-written books | Identification of inks, pigments and supporting materials (paper and parchments) present in 15th and 16th century manuscripts; Provide knowledge on the history of different inks used in the manuscripts, the conservation and degradation of supporting materials; characterization of restoration materials and techniques, and deliberate falsification processes | Non-invasive | Raman spectroscopy |
Article 5 | Oil painting on canvas | Assess the authenticity of a painting attributed to Salvator Rosa (1615–1673) by studying the painting’s materials and techniques | Micro-invasive | Raman spectroscopy; polarized light microscopy; 14C dating by accelerator mass spectrometry; SEM-EDX |
Article 6 | Oil painting on panel | Applicability of a new lightweight MA–XRF scanner for in situ research on paintings; Characterization of the pigment palette and techniques of The Entombment of Christ by Rogier van der Weyden (1399/1400–1464); Confirm the Flemish production of the painting | Non-invasive | MA–XRF scanning |
Article 7 | Glue-size painting (tüchlein) on canvas | Identification of overpaints executed by Guiseppe Molteni (1800–1867) on Madonna with Child by Andrea Mantegna (1431–1506) by means of MA–XRF; characterization of the pigment palette and techniques of Mantegna | Non-invasive | MA–XRF scanning |
Article 8 | Illuminated manuscript | Applicability of a new lightweight MA–XRF scanner for in situ research on illuminated manuscripts; characterization of pigments and painting techniques; attribution of individual illuminations to different hands | Non-invasive | MA–XRF scanning |
Article 9 | Oil paintings on canvas | Optimize a novel multi-analytical approach for the in-situ technical study of contemporary paintings; characterization of painting materials, techniques, and state of conservation | Non-invasive | Multiband technical photography (MTP) (including visible light, UV, reflected UV, IR and false color IR); IRR; HIS; portable light microscopy; portable EDXRF |
Article 10 | Oil painting on canvas | Characterization of painting materials and techniques of employed by Remo Brindisi (1918–1996) in the painting Ragazzo seduto (Seated boy); evaluation of the state of conservation and preliminary assessment of the deterioration processes caused by the employed industrial materials | Micro-invasive | Visible, raking light, UVIF, near infrared photography; optical microscopy (OM); SEM; μFTIR |
Topic | Preliminary Label | Final Label |
---|---|---|
T1 | The spectroscopic study of pigments in paintings | The spectroscopic and microscopic study of the stratigraphy of painted CH assets |
T2 | Fungal deterioration and other types of biodeterioration of CH assets | Identification of fungi in CH assets and the assessment of their degrading abilities (including pigment production) |
T3 | The analysis of mineral compounds in CH assets | Not identifiable topic |
T4 | Raman spectroscopic analysis of pigment samples | Vibrational spectroscopic techniques: their development and improvement for pigment identification and characterization |
T5 | X-ray techniques dedicated to materials characterization (including pigments) in cultural heritage | X-ray based techniques for CH, conservation science and archaeometry: their application, development, and contribution to the characterization of CH materials (including pigments) |
T6 | Imaging methods (including hyperspectral imaging) for the examination of paintings | Spectral imaging techniques: their development and improvement for surface chemical mapping of easel paintings, wall paintings, and illuminated leaves |
T7 | Chromatographic and spectroscopic methods for the identification of organic pigments and dyes | Chromatographic and spectroscopic methods for the identification and characterization of natural and synthetic organic dyes and pigments |
T8 | Scientific research for restoration and conservation of CH assets and materials | Restoration and conservation methods, materials, and treatments: Their developments and improvement for CH |
T9 | The analytical study of paint and pigment degradation | The analytical study of aging and degradation of paint films, pigments and organic binders, and the roles of light, paint materials and conservation treatments in these processes |
T10 | The technical study of paintings and illuminated manuscripts | The technical study of pigments and painting methods employed by historical and contemporary painters and illuminators |
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Harth, A. The Study of Pigments in Cultural Heritage: A Review Using Machine Learning. Heritage 2024, 7, 3664-3695. https://doi.org/10.3390/heritage7070174
Harth A. The Study of Pigments in Cultural Heritage: A Review Using Machine Learning. Heritage. 2024; 7(7):3664-3695. https://doi.org/10.3390/heritage7070174
Chicago/Turabian StyleHarth, Astrid. 2024. "The Study of Pigments in Cultural Heritage: A Review Using Machine Learning" Heritage 7, no. 7: 3664-3695. https://doi.org/10.3390/heritage7070174