Mineral Preservatives in the Wood of Stradivari and

Guarneri
Joseph Nagyvary1*, Renald N. Guillemette2, Clifford H. Spiegelman3
1 Department of Biochemistry and Biophysics, Texas A&M University, College Station, Texas, United States of America, 2 Department of Geology and Geophysics, Texas
A&M University, College Station, Texas, United States of America, 3 Department of Statistics, Texas A&M University, College Station, Texas, United States of America

Abstract
Following the futile efforts of generations to reach the high standard of excellence achieved by the luthiers in Cremona,
Italy, by variations of design and plate tuning, current interest is being focused on differences in material properties. The
long-standing question whether the wood of Stradivari and Guarneri were treated with wood preservative materials could
be answered only by the examination of wood specimens from the precious antique instruments. In a recent
communication (Nature, 2006), we reported about the degradation of the wood polymers in instruments of Stradivari and
Guarneri, which could be explained only by chemical manipulations, possibly by preservatives. The aim of the current work
was to identify the minerals from the small samples of the maple wood which were available to us from the antique
instruments. The ashes of wood from one violin and one cello by Stradivari, two violins by Guarneri, one viola by H. Jay, one
violin by Gand-Bernardel were analyzed and compared with a variety of commercial tone woods. The methods of analysis
were the following: back-scattered electron imaging, X-ray fluorescence maps for individual elements, wave-length
dispersive spectroscopy, energy dispersive X-ray spectroscopy and quantitative microprobe analysis. All four Cremonese
instruments showed the unmistakable signs of chemical treatments in the form of chemicals which are not present in
natural woods, such as BaSO4, CaF2, borate, and ZrSiO4. In addition to these, there were also changes in the common wood
minerals. Statistical evaluation of 12 minerals by discriminant analysis revealed: a. a difference among all four Cremona
instruments, b. the difference of the Cremonese instruments from the French and English antiques, and c. only the
Cremonese instruments differed from all commercial woods. These findings may provide the answer why all attempts to
recreate the Stradivarius from natural wood have failed. There are many obvious implications with regard to how the green
tone wood should be treated, which chould lead to changes in the practice of violin-making. This research should inspire
others to analyze more antique violins for their chemical contents.

Citation: Nagyvary J, Guillemette RN, Spiegelman CH (2009) Mineral Preservatives in the Wood of Stradivari and Guarneri. PLoS ONE 4(1): e4245. doi:10.1371/
journal.pone.0004245
Editor: Xiaoping Pan, Western Illinois University, United States of America
Received November 4, 2008; Accepted December 17, 2008; Published January 22, 2009
Copyright: ß 2009 Nagyvary et al. This is an open-access article distributed under the terms of the Creative Commons Attribution License, which permits
unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.
Funding: This study was not supported by any outside agency.
Competing Interests: The authors have declared that no competing interests exist.
* E-mail: [email protected]

Introduction attention. The 1987 exhibit of documents from the State Archives
of the Serenissima Republic of Venice [5] provided evidence that
For centuries, violin-makers have tried in vain to match the high the wood supply was delivered through the water-ways and could
standards of excellence set in the first half of the 18th century by have been treated with chemical preservatives for the use by all
the two legendary masters of the craft, Antonio Stradivari and sorts of trades. The beneficial effect of salts on the wood of musical
Joseph Guarneri del Gesù in Cremona, Italy. Since craftsmen of instruments was first noted by the French author Palissy in 1580
our age have employed all the traditional know-how of the art and according to the historical research of R. Gug [6].
have also been aided increasingly by volumes of acoustical The wood of the great masters received only little attention by
research, their failure is hard to explain. The mechanical scientists in the past, and the focus was on the area penetrated by
properties of naturally seasoned spruce and maple were thor- the ground layer of the finishing materials [7,8,9]. The varnish and
oughly studied by several investigators [1,2,3] who concluded that the wood of a Stradivarius cello were subjected to analysis by ion
high stiffness and low density should be the criteria in selecting the backscattering [10], but the inaccuracies of the method did not
best wood. Yet the results with the best commercial wood allow conclusions beyond showing the presence of several trace
remained unconvincing. It is possible that, due to the orthotropic elements. The first indication that the entire instrument wood of
nature of the wood [1,3], the given ratio of its mechanical the famous Cremona masters could have received some kind of
constants is not what it should ideally be for the best acoustical special aqueous treatment was advanced by Nagyvary [11] in the
outcome. Such considerations would justify the suggestion that the form of scanning electron microscopic (SEM) images of internal
trees grown during the Maunder Minimum could have had spruce sapwood samples. The micrographs from the violins of
different and better mechanical properties [4]. Stradivari, Guarneri and Guadagnini revealed the remnants of
The proposition that the answer may lie in the material microorganisms, and the Guarneri also showed mineral deposits.
differences caused by an ancient and forgotten practice of wood In contrast, Barlow and Woodhouse found nothing remarkable in
preservation has surfaced many times but it received less than due their SEM study of the morphology of spruce samples from Italian

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 Wood Minerals of Stradivari

musical instruments [12]. They concluded that the wood of the Sample preparation. Ash samples were prepared from the
masters had not been submerged in water for a prolonged period wood shavings using the following technique. Between 20 and
of time, as done in the present process of ‘‘ponding’’ of logs. 80 mg of wood shavings were weighed and transferred to Coors
However, SEM by itself is not a suitable method to prove the point porcelain covered crucibles; only 13 mg of Cremona soot was used
and exclude the possibility of past aqueous treatments with because of the smaller expected loss of volatiles. The crucibles
chemicals, including boiling for short periods of time, which could were inserted into a cold Lindberg muffle furnace and the furnace
cause important chemical and morphological changes on a smaller was set to 500uC and turned on. After 2 hours, crucibles were
scale. The conclusion of the British workers was not backed up by removed from the furnace and allowed to cool. Ash was removed
mineral analysis, which would have been the simplest way to prove from the crucibles and pressed between 2 highly-polished
the absence of aqueous treatment. (0.25 mm surface finish) stainless steel cylinders to form a 1–
More recently, the powerful methods of solid-state NMR and 3 mm diameter pellet. Each pellet was transferred onto the surface
FTIR spectroscopy were employed by Nagyvary et al. [13] for the of conductive carbon tape and coated with 15 nm of
study of maple wood from the backs of instruments made by spectroscopically pure amorphous carbon in a Ladd carbon
Stradivari and Guarneri del Gesù in comparison with the maple evaporator to make the pellet conductive under an electron beam.
from antique French and English instruments. The Italian samples
revealed massive chemical changes in the wood polymers while the Analytical Methods
others differed only slightly from the recent natural wood. The Analyses were carried out on a Cameca sx50 electron
observed changes went well beyond what one could see after microprobe equipped with four wavelength dispersive X-ray
boiling in water. Thus, there could be no doubt that these spectrometers (WDS) and an energy dispersive X-ray spectrometer
particular woods were chemically treated, and the only question (EDS) using standard microprobe imaging and microanalytical
concerns the specifics of the chemical treatment. methods [15,16]. The WDS spectrometers are capable of
In the present study we report on the mineral analysis of the ashes detecting and qualitatively and quantitatively analyzing elements
from the previously used maple samples [13], to which we could also from Z = 4 (Be) through Z = 92 (U). The Li-drifted Si detector with
add an additional sample from an early Guarneri del Gesù violin. ultra-thin window in the EDS system is capable of detecting and
Some years ago, the mineral composition of various trees was qualitatively analyzing elements from Z = 6 (C) through Z = 92
determined by classical methods requiring relatively large quantities (U). Electron imaging was performed using a six component
of wood [14]. We have employed the methods of backscattered backscattered electron (BSE) detector operated in atomic number
electron (BSE) imaging, X-ray qualitative analysis by energy mode, where the brightness in an image is proportional to the
dispersive spectroscopy (EDS), X-ray quantitative analysis by mean atomic number of the area being imaged. X-ray elemental
wavelength dispersive spectroscopy (WDS), and WDS X-ray distribution images (‘‘maps’’) were acquired by moving the stage
element distribution imaging. The results suggest that the wood containing the sample in 2 mm steps in a 512 by 512 grid beneath
used by Stradivari and Guarneri was indeed treated by mineral the fixed 1 mm diameter beam; dwell time at each step (pixel) was
preservatives. Such a process could have caused extensive chemical 15 ms. Each of the four WDS spectrometers was set to the major
changes in the organic matrix and, therefore, could have impacted X-ray emission line of an element, with an additional pass required
the acoustical properties of the wood. These findings have far- for each additional set of four elements. The brightness of each
reaching consequences for the art of violin-making if the goal is pixel in the image is proportional to the number of X-rays from
indeed the reproduction of the great Cremonese standards. that element detected at that point on the sample.
EDS qualitative analyses in the form of X-ray spectra were
Materials and Methods acquired on the pressed powder pellets. The sizes of the areas analyzed
varied from about 1 mm up to 1 mm. The smaller sizes were used to
Materials examine different BSE heterogeneous areas, while the larger sizes
Wood samples from the instruments of Stradivari and Guarneri were used to average as large an area as possible on the pellets. EDS
del Gesù were taken from the interior of the backs during the quantitative analyses were not attempted because of the larger errors
repair of cracks when the restorer removed thin shavings of old associated with EDS analyses compared to WDS analyses.
wood several millimeter deep from an area approx. 6 to 8 cm2; the WDS quantitative analyses were performed on the samples
outer discolored layers were excluded. The samples were derived using standard methods after careful calibration using well
from the maple backs of the following provenance: (a) a violin by characterized Smithsonian [17,18] and C. M. Taylor Inc. [19]
Stradivari, 1717 CE, (b) a cello of Stradivari, 1731 CE, (c) a violin reference standards. Calibration for all elements was performed at
by Guarneri del Gesù, 1741 CE, (d) a violin by Guarneri del Gesù the beginning of each analytical session, followed by the analysis of
from the mid-1730s, (e) a violin by Gand-Bernardel of Paris, mid- known compounds as standard checks. WDS analyses were carried
1840s, (f) a viola by Henry Jay from London, 1769 CE. The last out on 20 mm diameter spots distributed over the surface of the
two instruments were salvaged from a house fire and were exposed pressed powder pellets in as representative a manner as possible;
to a brief period of heat. For comparisons, we used maple tone 20 mm is the largest area that can be analyzed in a single WDS
wood from all important European regions such as Bosnia, analysis as determined by the constraints of spectrometer
Slovenia, Slovakia, Germany and also from southwest China. geometry. A larger number of points was selected on the more
Such samples were either purchased from commercial companies heterogeneous samples (as determined by BSE imaging) in order to
such as International Violin Co., Baltimore, MD; David Morse obtain better averages for those samples.
Violins, Soquel, CA; Rivolta Co., Desio, Italy; ViolinMaple Co., Boron was detected semi-quantitatively using WDS spectral scans
Bratislava, Slovakia, or they were donated by private individuals centered on the boron K alpha X-ray emission line and carried out
who acquired them on locations. Although we asked for naturally under identical conditions on the pressed powder pellets.
seasoned wood, some contamination could not be excluded since
the practice in some locations includes spraying of the logs with Statistical analysis
fungicides. Unusual Na values found in one Bosnian and one Only elements that were measured for all instruments and
Slovenian samples could be due to such contamination. woods in Tables 1 and 2 were used in the multivariate statistical

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 Wood Minerals of Stradivari

analysis. These 12 elements (cations as oxides) were Cl, Na2O, P, S, Si and Zn. These images were useful to show the uneven
K2O, CaO, MgO, SiO2, Al2O3, P2O5, SO3, FeO, MnO, TiO2. distribution of elements within the ash pellet, and they also helped in
The full set of data, compiled in Supplemental Information (Table identifying some chemical compounds that were originally applied to
S1), included 95612 values for the Stradivarius violin, 75612 for the wood, such as CaSO4, BaSO4, Na-borate and CaF2. In general,
the early Guarneri and 30612 for the rest, with the exception of the distribution of the major elements Ca, K, and Na is more even
the German maple which had only 15612 data points. The than those of the minor elements. Fig. 2 shows some representative
differences between the wood samples could be best seen in plots images of elements from the ash of the Stradivari violin wood.
based on canonical axes designed to separate the instruments as Noteworthy is the presence of boron, an element normally not found
much as possible. These axes are linear combinations of the in wood, which can be easily overlooked because of its low energy X-
elements that were measured in all the instruments and ray emission line which must be detected using a WDS spectrometer
commercial woods under study. The statistical technique used to equipped with a special large d-spacing pseudocrystal. The
construct the axes is known as discriminant analysis; see Johnson comparison of its map with that of Na suggests that it was probably
and Wichern [20]. All calculations were done using JMP [21] applied as Na-borate (borax). The presence of BaSO4 is also
statistical software and the quadratic discriminant analysis module. indicated by the coincidence of the Ba and S images. It is not a
We used these axes only for plotting. It was not our purpose to constituent of wood, and its presence must be due to a deliberate
create an assignment rule for new measurements to one of these chemical manipulation.
instrument types as is typical with discriminant analysis. When a similar WDS-based imaging was applied to the late
period Guarneri violin ash, it led to the discovery of CaF2, a
Results compound otherwise not found in wood (Fig. 3). It is interesting to
note that none of the other violins had any significant amounts of
Backscattered electron (BSE) imaging fluoride, as it could be determined by WDS X-ray distribution maps.
The controlled burning of the wood shavings yielded approx- Particular care was taken to search for borate in all samples
imately 0.5 to 1.0 mg quantities of ashes, which were pressed into because of its role as an insecticide-fungicide of long-standing
pellets as described above. The first preliminary assessment of the usage. Boron was found in both instruments of Stradivari and the
possible differences was made by backscattered electron (BSE) early period Guarneri; it was absent in the late Guarneri and in all
imaging targeting an area of 1 mm2. These are shown in Fig. 1 for the commercial maple samples. The amount of borate in the
the Stradivari violin (A), the early Guarneri violin (B) and one of Gand-Bernardel and perhaps in the Henry Jay was slightly beyond
the 12 recent commercial wood samples (C). On these gray-scale its natural abundance in wood. This is apparent in Fig. 4 which
images the degree of contrast correlates with chemical heteroge- shows WDS spectral scans over the boron peak on the Stradivari
neity, and the brightness is a function of the mean atomic number violin, early Guarneri violin, Gand-Bernardel violin, Henry Jay
of the elements. By these criteria, one can see significant viola, and recent commercial Bosnian maple ash pellets.
differences among these images.
EDS Spectra
Elemental distribution images The EDS method was useful in identifying elements of mineral
The use of WDS detectors allowed for the imaging of individual clusters in small areas, and thus establishing the degree of
elements. We acquired such X-ray maps covering an area of 1 mm2 heterogeneity of the ashes. At the largest setting of 1 mm2 and
for the anticipated elements Al, B, Ba, Ca, Cl, Cu, F, Fe, K, Mg, Na, repeated sampling, the average spectrum has become a reasonable

Table 1. Quantitative analyses of musical instrument ashes.

Norm Anal F Cl Na2O K2 O CaO MgO SiO2 Al2O3 P2 O 5 SO3 BaO FeO MnO CuO ZnO TiO2

LLD 0.27 0.04 0.10 0.05 0.08 0.07 0.10 0.06 0.10 0.11 0.18 0.15 0.15 0.28 0.35 0.22
StradCello(15) 1.26 6.11 15.93 40.17 10.15 4.62 1.98 4.76 13.54 1.32 0.16 0.21
Strad Cello SD 0.50 2.00 7.06 9.46 4.00 3.40 2.05 1.79 3.24 1.90 0.08 0.34
Strad Vln(95) 0.84 11.34 23.26 25.26 15.45 4.48 3.89 0.50 1.59 9.70 1.26 0.81 0.11 1.11 0.32 0.08
Strad Violin SD 0.63 6.59 12.14 8.57 6.51 3.11 9.51 0.61 0.87 4.17 5.33 0.87 0.11 2.47 0.56 0.12
Guarneri(80) 0.08 0.19 7.61 15.70 24.63 3.27 6.81 5.29 1.89 23.11 0.14 8.06 0.17 0.14 0.34 0.55
Guarneri SD 0.06 0.06 2.02 2.72 5.86 1.27 3.99 3.12 0.72 4.01 0.12 5.25 0.12 0.08 0.23 0.48
HenryJay(29) 0.22 0.35 4.63 34.18 37.66 8.11 2.05 0.62 6.71 4.26 0.31 0.27 0.24 0.18 0.16 0.05
HenryJay SD 0.12 0.09 2.22 3.89 3.74 1.07 2.50 1.12 1.77 0.83 0.11 0.33 0.06 0.13 0.17 0.08
Gand-Bern(30) 0.18 0.24 5.18 19.95 50.89 10.66 0.81 0.14 5.00 5.06 0.18 0.98 0.31 0.18 0.18 0.06
Gand-Bern SD 0.09 0.04 1.42 4.38 5.46 1.55 1.51 0.26 0.89 1.37 0.14 4.13 0.09 0.09 0.13 0.10
Soot (30) 0.26 1.07 0.70 9.79 40.17 5.76 5.60 1.94 4.76 27.79 0.08 0.81 0.07 0.13 0.96 0.12
Soot SD 0.10 0.36 0.17 1.68 4.41 1.74 3.56 1.21 0.84 4.15 0.05 0.36 0.04 0.08 0.21 0.18

Analyses were carried out on a Cameca sx50 electron microprobe equipped with four WDS spectrometers. All analyses were performed with a 15 kV, 10 nA, 20 mm
diameter beam; standardization and standard checks using well-characterized reference materials were done before each analytical session. The numbers represent
average wt% values, normalized to 100%; number of sites analyzed is in parentheses. SD: standard deviation. It is customary to present the values as oxides. The lower
limit of detection (LLD) for each element or oxide is given at the top of the table. Abbreviations: Guarneri designates the ash of the early Guarneri violin, Gand-Bern that
of the Gand-Bernardel violin.
doi:10.1371/journal.pone.0004245.t001

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 Wood Minerals of Stradivari

Table 2. Quantitative analyses of various commercial maple ashes.

Norm Anal F Cl Na2O K2O CaO MgO SiO2 Al2O3 P2O5 SO3 BaO FeO MnO CuO ZnO TiO2

LLD 0.27 0.04 0.10 0.05 0.08 0.07 0.10 0.06 0.10 0.11 0.18 0.15 0.15 0.28 0.35 0.22
Grmn(15) 0.86 3.67 46.61 32.37 7.34 1.27 0.50 2.44 1.24 0.03 3.68 0.04
Grmn SD 0.36 2.86 6.70 6.47 1.50 0.85 0.25 1.54 0.63 0.06 0.70 0.07
Slvk_ht(30) 0.34 2.23 3.74 15.71 52.79 15.17 1.06 0.14 3.76 3.87 0.04 0.54 0.23 0.16 0.15 0.07
Slvk_ht SD 0.20 1.18 3.18 7.84 8.08 3.44 2.23 0.44 0.90 0.96 0.04 1.07 0.10 0.11 0.14 0.07
Slvk_sp(30) 0.35 0.65 1.80 40.46 31.36 9.92 1.70 0.21 9.01 3.54 0.05 0.52 0.11 0.15 0.10 0.07
Slvk_sp SD 0.25 0.33 1.24 6.71 4.75 1.74 2.67 0.45 2.61 0.84 0.05 1.21 0.06 0.14 0.11 0.07
Slvk_95(30) 0.50 0.78 3.23 33.02 34.50 14.14 1.05 0.07 7.72 2.28 2.02 0.14 0.20 0.19 0.12 0.03
Slvk_95 SD 0.18 0.37 2.24 4.42 3.98 3.19 1.08 0.18 1.51 0.43 2.69 0.32 0.07 0.11 0.10 0.05
Slvn1_ht(30) 0.32 0.93 3.66 26.45 44.46 7.82 5.31 1.69 4.29 3.67 0.27 0.54 0.22 0.14 0.14 0.10
Slvn1_ht SD 0.19 0.59 2.53 8.70 7.23 1.65 5.50 2.03 1.15 0.90 0.09 0.56 0.08 0.09 0.14 0.12
Slvn1_sp(30) 0.25 2.93 11.72 14.09 44.55 9.52 1.54 0.30 4.90 7.62 0.22 0.94 0.25 0.20 0.92 0.04
Slvn1_sp SD 0.15 1.63 4.01 3.88 9.74 2.47 1.71 0.60 1.58 2.44 0.09 1.24 0.08 0.12 0.43 0.06
Slvn2_ht(30) 0.21 0.36 3.50 32.00 42.26 7.34 4.33 1.30 3.82 3.38 0.51 0.35 0.20 0.16 0.12 0.13
Slvn2_ht SD 0.09 0.13 1.70 5.28 3.97 1.45 4.55 1.70 1.04 0.58 1.34 0.42 0.06 0.07 0.11 0.23
Slvn2_sp(30) 0.19 1.37 4.86 30.05 38.78 8.13 1.78 0.18 8.59 4.86 0.32 0.13 0.26 0.19 0.24 0.04
Slvn2_sp SD 0.11 2.40 2.69 8.20 6.40 1.57 1.67 0.45 2.44 0.94 0.10 0.17 0.06 0.10 0.19 0.07
Chns(30) 0.52 0.27 2.58 16.66 54.91 12.29 1.44 0.21 4.21 4.69 0.34 0.35 1.11 0.25 0.10 0.07
Chns SD 0.28 0.06 1.15 4.53 3.90 1.06 2.20 0.26 0.63 1.46 0.14 0.51 0.21 0.13 0.15 0.07
Bosn1(30) 0.08 0.11 12.55 16.11 31.24 28.59 0.14 0.02 4.98 3.56 0.28 0.07 1.93 0.14 0.18 0.02
Bosn1 SD 0.06 0.05 1.17 1.99 1.37 1.88 0.15 0.03 0.87 0.67 0.08 0.11 0.40 0.10 0.10 0.03
Bosn2(30) 0.08 0.18 1.10 27.41 33.38 30.10 0.17 0.03 4.33 2.14 0.22 0.04 0.49 0.16 0.15 0.02
Bosn2 SD 0.08 0.16 0.24 4.08 2.47 1.95 0.15 0.09 1.17 0.38 0.09 0.05 0.09 0.10 0.13 0.02
Bosn3(30) 0.13 0.16 1.58 15.95 47.65 26.45 0.36 0.03 4.13 2.38 0.21 0.05 0.58 0.13 0.15 0.04
Bosn3 SD 0.09 0.03 1.23 4.87 4.35 3.50 0.18 0.04 1.21 0.35 0.08 0.06 0.07 0.11 0.11 0.05
Bosn4 30) 0.06 0.19 4.35 8.90 46.45 30.87 0.44 0.01 4.21 3.96 0.05 0.07 0.12 0.16 0.14 0.02
Bosn4 SD 0.06 0.03 1.12 2.38 1.68 1.93 0.26 0.02 0.78 0.35 0.04 0.06 0.06 0.10 0.10 0.03
Bosn5(30) 0.04 0.17 1.53 20.99 35.43 33.99 0.18 0.02 4.42 2.17 0.17 0.04 0.49 0.18 0.16 0.03
Bosn5 SD 0.04 0.04 0.73 5.68 6.16 5.06 0.21 0.02 1.23 0.52 0.07 0.05 0.10 0.09 0.12 0.04
Bosn(30) 0.09 0.32 1.25 22.59 39.15 27.87 0.21 0.02 4.90 2.41 0.27 0.04 0.60 0.16 0.10 0.03
Bosn6 SD 0.05 0.04 0.46 5.85 2.87 3.11 0.17 0.03 1.30 0.49 0.07 0.04 0.09 0.09 0.10 0.04

Analyses were carried out on a Cameca sx50 electron microprobe equipped with four WDS spectrometers. All analyses were performed with a 15 kV, 10 nA, 20 mm
diameter beam; standardization and standard checks using well-characterized reference materials were done before each analytical session. The numbers represent
average wt% values, normalized to 100%; number of sites analyzed is in parentheses. SD: standard deviation. The lower limit of detection (LLD) for each element or
oxide is given at the top of the table. Abbreviations of wood ashes. Grmn: German; Slvk_ht: Slovak heartwood; sp: sapwood; Slvk_95: Slovakian wood from 1995; Slvn_1
and Slvn_2 are samples from the same Slovenian maple board but from different depth; Chns: Chinese; Bosn1–Bosn6 designate samples from 6 different Bosnian trees.
doi:10.1371/journal.pone.0004245.t002

Figure 1. Backscattered electron images. BSE images of 1 mm2 areas of the pressed powder pellets made from the ash of the (A) Stradivari
violin, (B) early Guarneri violin, and (C) one of the commercial Bosnian maples. The two violin ash samples exhibit a higher degree of the BSE
brightness variability and hence compositional heterogeneity than the Bosnian maple.
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 Wood Minerals of Stradivari

Figure 2. Elemental distribution images in the Stradivari violin

ash. WDS-based imaging of 1 mm2 areas was employed for the
elements Na, B, Ca, Ba, S, and Si. Note the higher degree of variability in
the distribution of the elements B, Ba, S, and Si. Partial overlapping
images suggest the presence of BaSO4, CaSO4 and Na-borate.
doi:10.1371/journal.pone.0004245.g002
Figure 4. The detection of boron. WDS spectral scans over the
boron peak are shown on the ash pellets of the Stradivari violin (blue),
early Guarneri violin (green), Gand-Bernardel violin (red), Henry Jay viola
(orange) and commercial Bosnian maple (black).
doi:10.1371/journal.pone.0004245.g004

only minor deviations from those of the 11 commercial samples

tested in this study.

Quantitative measurements
Electron microprobe WDS analysis was employed for the
Figure 3. Elemental distribution images in the late Guarneri
violin. WDS-based imaging of 1 mm2 areas was employed for the quantitative determination of the elements from all the above
elements Ca and F. Note that all F-bearing regions also contain Ca. Thus samples, with one exception. Due to a temperature control
the particles constitute CaF2. problem, the late Guarneri sample was overheated to almost
doi:10.1371/journal.pone.0004245.g003 700uC and lost most of its K; this sample was not used in this
analysis. Because of the volatility of K [22], we had to keep the
semi-quantitative representation of the overall elemental compo- combustion temperature under 550uC. We also analyzed the
sition. The EDS spectrum of Figure 5A represents the average of composition of chimney soot from Cremona. The results of the
10 spectra taken on the ash of the Stradivari cello, which is elemental analysis of the musical instruments ash are compiled in
noticeably different from the average spectrum of recent maple of Table 1, those of the commercial woods in Table 2, where the
Fig. 5B, albeit not so obviously different as the 3 violins of numbers represent wt% elements or oxides normalized to 100%
Cremona. The spectra of the Stradivari violin taken at several total. The number of 20 mm diameter circular areas that were
locations show the presence of NaCl well above its natural analyzed and averaged was 95 for the Stradivarius violin, 80 for
occurrence in wood (Fig. 6A). The survey of the ash pellets of both the early Guarneri and 30 for the rest. The noticeable feature of
Guarneri violins revealed a trove of unusual components. A this data set is the high standard deviation for several elements
particular site of the early period Guarneri contains crystals of which can be due to several factors, such as the uneven
ZrSiO4 besides Fe and Cr salts (Fig. 6B). The spectra of the Gand- distribution of the natural minerals in the wood, and the uneven
Bernardel and Henry Jay instruments (not shown here) revealed uptake of extraneous minerals. Particles of the insoluble BaSO4

Figure 5. EDS spectra of ash from the Stradivari cello and from new maple. A: ash from Stradivari cello, B: recent maple. Each spectrum
represents the average of ten spectra acquired at different .100 mm diameter areas on each pellet over a total acquisition time of 1200 seconds.
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 Wood Minerals of Stradivari

Figure 6. EDS spectra of ash from violins of Stradivari and Guarneri. The Stradivari violin spectrum A was acquired over a large
representative 400 mm diameter area of the pellet, while the Guarneri violin spectrum B represents a small BSE bright Zr rich area.
doi:10.1371/journal.pone.0004245.g006

and silica would be capable of deep penetration only within the the local soil. The only way to reconcile the Ca/Mg ratios of the
vessels of the wood, and this explains the rare occurrence of such Stradivari and Guarneri wood with a Bosnian origin would be to
particles within the ash. The heterogeneity of the ash, especially assume that the excess Mg-salts had been extracted. Slovenian
that from the musical instruments, can clearly be seen in X-ray maple would have been a more likely source for Stradivari and
maps (Fig. 2, Fig. 3) and in BSE images (Fig. 1). Guarneri on the basis of the respective Ca/Mg ratios. Although
The composition of the Stradivari violin ash differs significantly our intention was to include only natural and unadulterated wood
from those of the commercial wood samples in several regards. Its in our analyses, it appears that our Bosnian sample no. 1 and the
Na2O content is 11 times that of the Bosnian average, 5 times that Slovenian wood could have been treated by salt. Their ash
of the Slovenian and 8 times that of the Slovakian maple. The revealed the presence of NaCl well beyond those seen in the other
respective ratios for Cl are 52, 11 and 7. Both of these sets of samples. We also included Chinese and Slovakian maple woods in
comparisons are supported by the relevant unequal variance t-test our study since they are commonly available these days.
for equality of means and all have p-values less than 0.0001. In Finally, we analyzed chimney soot from Cremona by several types
addition the Strad violin has a much larger variance than the other of analysis including the microprobe, and its composition was
wood samples for Na2O and Cl, p,0.0001. It also contains more included in Table 2. According to a historical source [23], alcoholic
SiO2, SO3, BaO, FeO and CuO but less of CaO, MgO and extract of soot was liberally applied to the wood of violins. The ash
phosphate. It exhibits an unnatural K/Na ratio. Borate data were from the soot reflected the very fine particle size of the original fly-
not included in this table. ash. Unfortunately, our 30-year old soot sample was probably
The Stradivarius cello ash was analyzed ten years ago, and at deposited from a combination of wood and coal burning, and it may
that time we did not include the elements Ba, F, Cu and Zn. The not be representative of soot produced in the 18th century. The high
main differences to natural wood are apparent in the values for value of SO3 could be best explained by assuming low-grade coal as
SO3, SiO2, and FeO. Unlike the Stradivari violin, the cello ash a major source. Even with this caveat, the similarities of the soot and
retained its phosphate. These findings suggest that the cello wood violin values are intriguing and give some credence for the possible
was treated differently from the violin wood, and this might have use of soot in the processing of the old violin wood.
had something to do with the practical aspect of soaking a large
piece of wood. Statistical analysis
Of the two Guarneri violins, only the early period Guarneri was The complete set of elemental analysis data of all musical
subjected to quantitative microprobe analysis. Unlike the later instruments and commercial wood samples that were subjected to
Guarneri, this one had very little fluoride and chloride in its ash. statistical analysis can be found in the Supplemental Information
This makes it unlikely that it had ever been in sea water. It had (Table S1). The results of the multivariate statistical analysis are
more Na2O, SiO2, Al2O3, SO3, FeO and ZnO than any of the shown in two figures which depict the clusters of data in elliptical
commercial woods. It also contained boron, chromium and forms, for each sample a small one and a large one. Figure 7 shows
zirconium, which were not included in Table 1. The early the separation of the mineral clusters from the woods taken from
Guarneri violin also differs from the Stradivari violin, notably with Stradivarius, Guarneri, Gand-Bernardel, and Jay instruments. In
regard to the respective Na2O, Cl, Al2O3, and FeO contents. The each instance, the small centroid ellipses represent 95%confidence
wood minerals of the instruments of H. Jay and Gand-Bernardel for the mean chemical content, and the large ellipses contain about
are significantly different from the Cremona instruments; 50% of the measurements. The separation of the Stradivari violin
otherwise the values fall within the range of natural woods. and the Guarneri violin clusters is very obvious, and they are also
In a few of our maple samples from commercial stocks, we well distanced from the Stradivarius cello, the Henry Jay viola and
analyzed both the sapwood and the heartwood, whenever we the Gand-Bernardel violin. Fig. 7 shows a small degree of overlap
could identify them, since their values are often different. We between the Stradivari cello and the Gand-Bernardel violin.
assume, but cannot be fully certain, that our antique samples Figure 8 shows 95% confidence ellipses for the mean chemical
derived from sapwood or a transitional area between sapwood and content for the Stradivarius and Guarneri instruments as well as
heartwood. Since tradition had it that the maple of Stradivari was for various commercial woods. Again, the plots used canonical
of Bosnian origin, we analyzed 6 different Bosnian maple samples. axes which were designed to separate the instruments and woods
The most distinctive feature of their elemental composition is the as much as possible. These axes are different from those of Figure 7
high values of Mg, which must be due to the dolomite minerals of as a separate optimization was done using the same method. The

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 Wood Minerals of Stradivari

Figure 7. Canonical plot of musical instruments. The results of

discriminant analysis are shown for the violin and cello of Stradivari, the
Figure 8. Canonical plot of Cremona instruments and com-
early period Guarneri violin, the violin of Gand-Bernardel and the viola
mercial woods. The results of discriminant analysis are shown on the
of Jay. The small ellipses represent the area of 95% confidence; the
violin and cello of Stradivari, the early period Guarneri violin, and a
large ellipses contain 50% of the measurements.
variety of commercial woods. The small ellipses represent the area of
doi:10.1371/journal.pone.0004245.g007
95%confidence.
doi:10.1371/journal.pone.0004245.g008
centroids for Stradivarius, Guarneri instruments are very different
from the commercial woods with the exception of the Stradivarius
cello. commercial woods, on the other hand. According to this analysis,
there is no commercial wood that comes even remotely close to the
violins of Stradivari and Guarneri, while the cello of Stradivari has
Discussion some similarities to one of the commercial woods, the Slovenian
The above results, however limited in the numbers of the precious wood. The commercial woods themselves reveal a considerable
specimens, offer the first real insight into the condition of the wood degree of variation which may be due to differences in the soil
used by the two greatest violinmakers, Stradivari and Guarneri. It minerals and surface contaminations. It should be noted that the
would be highly unlikely that out of the approx. 800 extant Stradivari suppliers could not rule out the possibility that the logs could have
and Guarneri instruments we would have come across the only four been sprayed with fungicides.
that possess unusual material compositions. All four samples from An important insight one can gain from the above body of
the instruments of these two masters have provided evidence of evidence is the apparent absence of a specific formula that would
chemical manipulations. This conclusion rests foremost on the have been commonly used in Cremona. The chemicals found in
presence of a few minerals which are not known to exist in detectable the violin and the cello of Stradivari have quite different
quantities in natural woods. Most significant is the finding of borate proportions. Perhaps this could be explained by the size difference
in the violin and the cello of Stradivari and also in the early period of these instruments. The large plank of wood for the cello would
violin of Guarneri. The latter also contained a most unexpected have been hard to boil in a large vat, and its penetration by
material, crystals of ZrSiO4. The late period Guarneri did not chemicals would have been limited. There are several differences
contain borate, but it had a small amount of the mineral fluorite, between the two Guarneri violins, one of which relates to the
CaF2. The uptake of salts and especially the insoluble particles, like borate and fluorite content. If we consider the primitive state of
BaSO4, SiO2, and CaF2, may vary slightly according to the chemistry in the early 18th century, it would not be surprising that
distribution of the vessels and the curvature of the violin surface. these two minerals could have been misidentified. Under those
Unfortunately, we did not have the luxury of getting samples from circumstances, it could have been almost impossible to reproduce
different parts of the same instrument. the intended chemical mixture over the years.
The four Cremona maple samples also differ from the others If we scrutinize the extraneous chemicals found in the
with regards to the amounts and the ratios of the common Cremonese woods, there seems to be a probable intent in their
minerals of the wood. This seems to be the case if we examine the being compounded in this particular fashion. They might have
Na, K, Ca and SO3 contents listed in Tables 1 and 2. When been intended for the purpose of wood preservation. The practice
considering a large number of the minerals, it requires statistical of employing borax as an insecticide and fungicide is so ancient
methods to assign varying degrees of significance to the that one cannot assign credit for its discovery [24]. It is interesting
differences. The results of the statistical evaluation relying on the that similar uses of soluble fluorides and even their combination
method of discriminant analysis, shown in Figures 7 and 8, provide with borax can be found in current literature [25]. Other salts
a graphic representation of the differences between the individual commonly sprayed on trees, like those of Zn, Cr, Cu and Fe, could
instruments on one hand and between the instruments and have been included by design or as contaminants.

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 Wood Minerals of Stradivari

Apart from the above conclusions, one can make only educated Breaking with the conventional practices, during the years since
guesses about the actual method of wood treatment in Cremona 1975, Nagyvary and his associates have built approximately 200
that harkens back to the alchemist practices of Paracelsus [26], violins from wood that was treated by a variety of chemicals,
who used an undefined mix of ‘‘salt of gems’’ for hardening of the including borax, microorganisms and hemicellulase enzymes [30].
wood. We can get now a glimpse into the possible composition of Undoubtedly, other violinmakers have followed suit. These
such mixture when inspecting the data of Table 1. The Cremona treatments were designed to lower the hemicellulose content,
‘‘salt of gems’’ could have contained crushed crystals of calcite, and therefore, also the moisture content and the density [30–32].
gypsum, barite, fluorite, and quartz, in addition to some water- The increase of porosity and permeability of chemically and
soluble salts like borax and the sulfates of Zn, Cu, Cr and Fe. microbially treated wood was noted by several investigators
Possibly, the plank of wood could have been immersed in an [33,11]. It was also reported by Bucur [34] that boiling of the
aqueous slurry of the above materials and most likely boiled—a wood led to a decrease of its density which is beneficial for the
guaranteed way to kill the woodworm. It is not possible to radiation of the sound. According to Nagyvary [11], the full
ascertain if there had been only one such treatment or more, and benefit of the aqueous wood treatment includes an increase of
whether the excessive soluble salt was extracted with ordinary porosity and permeability, which is apparent on staining of the
water. One can assume that a thick slurry of minerals could have wood and, especially, the early wood.
been also applied directly to the surfaces of the carved instruments Two recent reports published this year (2008) seem to have a
as fillers. The fine particles could have penetrated into the interior strong bearing on our conclusions concerning the Cremonese
of the maple mainly via the vessels [27] and a limited number of wood treatment. Schwarze et al. [35] employed specific fungi for
extracellular openings, and hence they could be found only the controlled degradation of Norway spruce and sycamore and
sporadically in our ash samples. One cannot rule out the possibility achieved a substantial reduction of density and an increase of
that an alcoholic solution of chimney soot was also applied to the permeability, especially in the early wood. While this treatment
wood, this having been the practice of the last great Cremona reduced the elasticity modulus of the wood, nevertheless it
trained violin-maker, G.B. Guadagnini [23]. improved its acoustical properties with respect to the radiation
Regrettably, our work had to be restricted to maple samples from ratio. Even more recently, Stoel and Borman [36] applied
the backs of instruments. There is much less spruce in the violin than computed tomography to study the densities of early wood and
maple, and we were unable to acquire samples in sufficient amounts late wood in five Cremona violins and eight violins made by
for this set of analyses. The preliminary results on the few spruce distinguished contemporary makers. With one exception beyond
samples we examined [11] by neutron-activation analysis suggested a the maker’s control, the modern violins were made of natural
higher concentration of minerals than in natural spruce. There wood. The density differential between the early wood and the late
would be no reason to assume that the spruce for musical wood was found significantly less in the Cremona violins than in
instruments was not preserved the same way as the maple. the modern violins. The authors did not offer a convincing
The question whether the minerals found in the four Cremona interpretation of their finding, but they assumed it could have been
instruments were responsible for the previously reported degradation an outcome of an aqueous treatment of the wood.
of the organic matrix of the wood [13] cannot be answered with The limitations of our study are obvious: our measurements and
sufficient confidence, but they could be an important factor. The statistics encompassed only materials from a square inch of surface
Stradivarius cello exhibits the least deviation from the natural from a few musical instruments. In an ideal world of scientist-
mineral composition, and it also shows the least damage to its collector cooperation, one would like to have several areas of the
hemicellulose and lignin components. Similarly, the samples from same instrument sampled, and one would like to have several
the instruments of Gand-Bernardel and Jay did not deviate much samples from all creative periods of Stradivari and Guarneri. It is
from natural wood in either their organic components or their our hope that others would now be attracted to this promising field
mineral content. Since the violins of Stradivari and Guarneri of research and would be more successful than we were in
revealed the greatest damage to their wood while their mineral acquiring precious samples.
composition differed substantially both from commercial wood and In summary, several lines of evidence suggest that the wood of
from each other, it would be hard to assert which of the chemicals the great Italian masters of Cremona was chemically and
were responsible for the changes. Sea salt by itself was shown to cause physically different from those of the later makers. These new
degradation when sprayed on live trees; salts of Fe, Cu, Cr, Sn, and insights strengthen the case for the postulated chemical/material
Zn were also known to cause degradation [28]. An assortment of paradigm of the Cremona violin [37,38], which posits chemical
soluble salts, some of them being also oxidizing agents, were most manipulations as a sine-qua-non towards the successful reproduction
likely involved in the degradation of the Cremona maples. of the old standards. It follows then that natural wood may not be
Our findings may have far-reaching implications for the a suitable material if the goal is to make violins with the old
direction of violin research since they seem to validate the Cremona-type tone. This recognition may instigate a major
assumptions of the minority view of what is essential for the change in how the commercial wood should be processed and also
production of fine violins. Much of the work during the last two in the state of the art of violin-making.
centuries was focused on the geometry and the acoustical
adjustment of the various elements of the violin. The selection of Supporting Information
wood with the highest possible stiffness was considered essential,
but the idea of using anything but unadulterated, natural wood has Table S1 Data for multivariate discriminant analysis. The full
been an anathema to most violin-makers and researchers. Soaking set of data included 95612 values for the Stradivarius violin,
of the wood and the addition of mineral preservatives appeared 75612 for the early Guarneri and 30612 for the rest, with the
counter-intuitive since they had a negative effect on the elasticity exception of the German maple which had only 15612 data
modulus [2,29]. However, one can also register a number of points. The data set from the pellets from each musical instrument
beneficial physical changes that would accompany the hypothet- was analyzed in its entirety as one group, while the commercial
ical Cremonese treatment of the wood based on research from woods were analyzed as sets of 15. Abbreviations: Guarn: the early
several laboratories. Guarneri violin; Strad: Stradivari; StrCello: Stradivari cello;

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 Wood Minerals of Stradivari

Gand: Gand-Bernardel violin. The following commercial wood Found at: doi:10.1371/journal.pone.0004245.s001 (1.90 MB
ashes were analyzed: Bosn2M1 and Bosn2M2 are 2 groups of 15 DOC)
sites each from the Bosnian tree no. 2; similarly, Bosn3M1,
Bosn3M2 are 2 groups of 15 from the Bosnian tree no. 3 tree and Acknowledgments
so on up to Bosn6M1 and Bosn6M2; ChinaM1 and ChinaM2 are
We thank two past presidents of the American Chemical Society, Dr. E. K.
2 groups of 15 sites from the ash pellet of one Chinese maple; Fields and Dr. A. E. Pavlath for their encouragement and support over the
GerMaple has only15 sites from the pellet of the German maple; past 25 years. We thank Dr. Peter Valko for technical advice and Dr.
slven1-ht and slven1-sp are groups of 15 sites from the heartwood Andrew Dipper for a sample of chimney soot. We are foremost indebted to
and sapwood of a Slovenian maple, and slven2-ht and slven2-sp the restorers and collectors who supplied the materials and wish to remain
are 2 groups of 15 from the same board but a deeper layer of anonymous.
wood; slvk1-ht and slvk1-sp are 15 sites each from the heartwood
and sapwood of a Slovakian maple, and slvk2-ht and slvk2-sp Author Contributions
represent sites from the same board but a deeper layer; slvk1995-1 Conceived and designed the experiments: JN RG. Performed the
and slvk1995-2 designate 2 groups of 15 sites from a different experiments: RG. Analyzed the data: JN RG CHS. Contributed
Slovakian maple board obtained in 1995. reagents/materials/analysis tools: JN RG. Wrote the paper: JN RG CHS.

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