Materials Science and Engineering A 412 (2005) 9396

Measuring elastic properties and anisotropy of microstructural units of laminate composite materials by microacoustical technique
Yu.S. Petronyuk a, , V.M. Levin a , Songping Liu b , Qianlin Zhang c
Laboratory of Acoustic Microscopy, Institute of Biochemical Physics of Russian Academy of Sciences, 4 Kosygin St., 119991 Moscow, Russian Federation b NDT&E Center for Composites, Beijing Aeronautical Manufacturing Technology Research Institute, P.O. Box 863, Beijing 100024, Peoples Republic of China c School of Information Science & Engineering, The Graduate School of CAS, 100039, 19 Yu Quan Road, Beijing, China
a

Abstract The paper is devoted to application of focused ultrasonic beams for measuring bulk elastic properties in advanced ber composite materials, such as carbon ber-reinforced composite (CFRC) laminates. Long-focus convergent beam of 50 MHz ultrasound frequencies provides the exceptional means of measuring elastic properties of microstructural units in composite materials with intricate microstructure as well as their integral properties. The microacoustical measurements reveal high anisotropy of CFR-laminate layers: sonic velocity across plies was found to be equal 3.1 km/s; in ply plane across ber packing7.0 km/s and along bers9.09.8 km/s. 2005 Elsevier B.V. All rights reserved.
Keywords: Fiber-reinforced composites; Laminate composite acoustic microscopy; Ultrasonic measuring

1. Introduction Reinforced composites form a wide class of materials that differ in componentsmaterials of matrix and reinforcing elements, as well as in principles of spatial arrangement of reinforcing elements. Reinforced composites nd ever-widening application in advanced technologies, especially as critical construction elements due to combination of unique elastic and strength properties with small weight, high corrosion resistance and outstanding heat conductivity characteristics [1]. A wide set of research methods is in use to study structure and properties of composite materials. Ultrasonic methods are of special interest because of their non-destructive character. The methods are highly informative and applicable as for measuring elastic properties so for bulk visualization of internal structure and studying defects in the body of reinforced composites [25]. Traditionally, to measure sonic velocities and elastic modules of reinforced composites the relatively low-frequency ultrasonic techniques (115 MHz) is widespread [2,3]. Such experiments provide studying integral values of elastic characteristics since

Corresponding author. E-mail address: julia@sky.chph.ras.ru (Yu.S. Petronyuk).

the ultrasonic wavelength substantially exceeds sizes of structural elements. The reinforced composites are treated by sonic waves as a continuous medium. Low-frequency ultrasonic characterization does not enable to get information on distribution of the elements over the composite medium, their perfection and properties. Acoustic microscopy may be applied to study local elastic properties of reinforced composites with microscopically ordering structure and their individual components, to investigate character of elastic parameter distribution over the material bulk. These data can be the base for following design of composite materials with prescribed properties. In the paper, results of microacoustical measuring for carbon ber-reinforced laminates composites (CFRC) are presented. The CFR composites are manufactured as laminate packages of ordered carbon ber layers (prepreg plies) embedded into a polymer binder (epoxy, bismeleimide or other types of polymer resin) [1]. Thickness of ber layers in CFRC structure is 100150 m. The layers usually are arranged as unidirectional or cross-ply stacks with or without the resin layers between them. Short pulse of focused ultrasound (50 MHz) is sensitive to the interlayer boundaries of such a composite structure. Due to big difference in the pure ber and matrix elastic property it becomes possible to observe obviously the interlayer reections, to measure thickness of the binding (matrix) layers and to determine binder distribution in the matter. Microacoustical

0921-5093/$ see front matter 2005 Elsevier B.V. All rights reserved. doi:10.1016/j.msea.2005.08.038

94

Yu.S. Petronyuk et al. / Materials Science and Engineering A 412 (2005) 9396

technique admits of measuring elastic anisotropy in individual layers of CFR composites. 2. Experimental method and facilities All experimental work has been performed with the wideeld pulse acoustic microscope (WFPAM) designed in Laboratory of Acoustic Microscopy, Institute of Biochemical Physics, RAS. The microscope employs short pulses (11.5 period of oscillations) at frequencies within the 25100 MHz range. The digital output of the microscope is connected with a computer to display echo signal oscillograms or acoustic images, produced by one- (B-scans) or two-coordinate (C-scans) mechanical scanning of the acoustical objective. A set of acoustical objectives with diverse operation frequencies and aperture angles lets us to implement diverse regimes of measuring and visualization with the microscope. In our experiments the low aperture (11 of half-angular aperture) long-focused probe ultrasonic beam have been in use for the bulk elastic property measurements. The experimental setup has provided 60 m resolution of measurements and 2.5 mm depth penetration at the operation ultrasonic frequency of 50 MHz. The ultra-short pulse of focused ultrasound (duration 40 ns) penetrates from the coupling liquid (pure water) into a planeparallel specimen as convergent beams of longitudinal (L) and transverse (T) waves (Fig. 1a). The pulse is reected from the specimen face and bottom as well as from structural elements within the specimen body. Reected echoes are separated in time. Typical echo pattern (Fig. 1b) involves the reference signal F (reection from the specimen face), the L, T and LT signals (reected from the specimen bottom). The signals L and T are caused by round-trip of longitudinal and transverse waves through the specimen; the signal LT results from mode conversion (L T) while wave reecting at the specimen back side. Time intervals L , LT and T between F and L, LT, T signals are used to nd the longitudinal and transverse sound velocities (d is the specimen thickness): cL = cT = 2d ; L 2d ; T (1) (2)

cT =

d . LT 0.5T

(3)

3. Specimens Specimens were prepared in Beijing Aeronautical Manufacturing Technology Research Institute. The style of the bers is T300/3k, bismeleimide resin QY8911 has been used as a polymer binder. The microacoustical technique has been employed to study elastic properties of resin binder (resin plate 3.18 mm thick), a single prepreg layer and individual layers in a crossply CFR-laminate composite. Two samples of a unidirectional ber prepreg have been used to measure sonic velocity across the prepreg ply. One of them was the free prepreg ply 120 m thick. The other was the same ply embedded into resin; full thickness of the composition was 380 m. Measuring sonic velocities of individual prepreg layers in a ply stacking has been performed with the sample of CFRC laminates composed of 15 layers 200300 m thick. The individual layer consists of two or three prepreg plies with the same orientation of carbon bers 120 m thick each. Neighbour layers differ in ber orientation by 90 (combined cross-ply packing of CFR laminates). We arranged ultrasonic measurements through the specimen in two directionsacross and inside prepreg plies. The measuring inside the composite plies provides two opportunitiesto get value of sonic velocity along ber bundles and across them in the plane of their parallel arrangement. 4. Results and discussions Summary of experimental results is presented in Table 1. Individual specimens of the resin, free single prepreg layer and single prepreg layer embedded into resin have been studied to get information about elastic properties of the main components of CFR-laminate matter. The echo pattern for the solidied bismeleimide plate (d = 3.18 mm) involves the F, L and weak LT signals (Fig. 2a). The measured values of elastic wave velocities in the polymer binder are: cL = 2.71 km/s for longitudinal waves and cT = 1.67 km/s for shear waves. Together with the measured magnitude of density ( = 1.24 g/cm3 ), the data resulted in nding values of elastic module of bismaleimide resin (bulk mod-

Fig. 1. Echo-pulse technique: (a) principal diagram of reections and (b) echo pattern of reected pulses for isotropic plate: (F) echo from the specimen face, (L) echo signal from the specimen bottom formed by longitudinal waves, (T) signal resulted from reection of transverse waves from the bottom, (LT) signal received from the bottom after mode conversion and (2L) signal from the twice bottom reection.

Yu.S. Petronyuk et al. / Materials Science and Engineering A 412 (2005) 9396

95

Fig. 2. Echo pattern of microacoustical measuring for individual elements of CFR composite structure: (a) bismeleimide resin matrix, (b) free prepreg ply and (c) sandwich structure of single prepreg ply in matrix; L time of ight; Fsurface echo; Lbottom echo formed by longitudinal waves; Dinternal defects; PF and PB echoes from surface and bottom of ply within the sandwich system. Table 1 Longitudinal elastic wave velocity cL in CFR-laminate composite and its individual structural elements Sample Direction of measuring Longitudinal elastic wave velocity cL (km/s) 2.71 3.20 3.07 3.10

Polymer binder Free layer of ber threads Sandwich system (ber ply + resin) Cross-ply CFR-laminate composite

Any direction Across composite ply Across composite ply Across plies Inside composite ply Across ber thread Along ber thread

6.927.08 9.009.80

Accuracy of measurement, 2.5%.

ulus K = 6.68 GPa, shear modulus G = 3.46 GPa or for component of the elasticity matrices: C11 = 11.29 GPa, C12 = 4.37 GPa, C44 = 3.46 GPa and Poisson ratio = 0.28). By means of microacoustical technique the unique measurements for basic low-dimensional components of carbon berreinforced systemfree prepreg plies, have been performed. The echo pattern for a single free ply contains the F, L signals and 2L, 3L, etc. echoes formed by repeatedly reected longitudinal waves (Fig. 2b). Across the reinforced ply of 120 m thick the sonic velocity value cL equal to 3.2 km/s has been obtained. Difference between sonic velocities of binding resin

matrix and reinforcing prepreg ply appears essential. This distinction is enough to employ measuring velocity of elastic waves to estimate resin content in the body of composite. The feasibility of estimations has been investigated with a single prepreg ply (120130 m thick) embedded into resin tape. Total thickness of the sandwich system was 380 m; measured value of longitudinal wave velocity cL = 3.07 km/s (Fig. 2c) is intermediate between values of two pure structural componentsthe resin and a free prepreg ply. Increasing resin content in the sandwich system compared to the free prepreg ply causes the reduced value of cL . So microacoustical measurements can be employed as non-destructive method to estimate local resin content in CFRC laminates to nd resin distribution over the specimen bulk. A tested scale for resin content in the composite structure can be obtained by means sonic velocity measuring. The main idea of the studies has been to elucidate potentialities of the microacoustical technique for measuring sonic velocities in individual strata of an ordered system. The technique has been applied to a CFR-laminate specimen with crossply stacking of prepreg layers to get data on longitudinal wave velocities of a single layer along different directions with respect to the ber orientation (Fig. 3). Longitudinal elastic wave velocity that has been measured across individual prepreg ply should be equivalent to the value obtained across the whole laminate specimen. Despite the cross-ply package of neighbour layers the ber orientation in all layers of the stacking is the same, respectively, to the elastic wave polarization and direction of beam

Fig. 3. Sketch of CFR-laminate sample orientation to measure sonic velocity: (a) across composite plies and (b) inside composite plies. In the last case, scanning of an acoustic lens allows to measure the longitudinal elastic wave velocity cL along ber package as well as across it (by shifting the lens position).

96

Yu.S. Petronyuk et al. / Materials Science and Engineering A 412 (2005) 9396

Fig. 4. Study of the 0 and 90 layers distribution in cross-ply composite structure by means of microacoustical technique: (a) echo pattern nearby the strata boundary: L1 signal from bottom of a 0 -oriented layer and L2 echo from bottom of a 90 -oriented layer; (b) acoustic imaging of the sample bottom, acoustical contrast is results in difference in elastic property for neighbour layers.

propagation (Fig. 3a). The value of sonic velocity cL = 3.10 km/s obtained in the case of beam propagation across composite plies is close to the value that was as a result of measuring across a ply, embedded into the resin. To measure elastic wave velocities inside individual composite layers the thin plates of cross-ply CFR laminate (2.11 mm) have been cut off as shown in Fig. 3b. The focal waist length (lF 23 mm) was compared with a thickness of the cut sample; the diameter dF of the focal spot (dF 80 m) was sufciently smaller than the width (200300 m) of an individual stratum in the ply stack. So the probe beam was able to reach the bottom of the cut sample being inside the individual composite stratum. In cut sample the neighbour plies have a different ber orientationnormal to the sample side surface or parallel to it. Different position of the focal spot on the surface provides measuring sonic velocity along and across bers within an individual stratum of the stack. Echo patterns obtained for neighbour layers demonstrate markedly different values of delay times and, respectively, different magnitudes of sonic velocities along carbon bers (cL = 9.69.8 km/s) and across them in the plane of ber plies (cL = 6.937.05 km/s). The longitudinal wave velocity for along ber orientation is signicantly higher than the velocity for across ber orientation in the same ply. Both of these values are essentially larger than sonic velocity across plies. Elastic and acoustic properties of particular components of CFRC laminatespolymer binder, single plies and their combinations; are of special interest for investigating mechanisms of acoustic contrast in CFRC imaging, for developing principles for acoustic images (C- and B-scans) interpretation in CFRC laminates and for interpretation of results of measuring sonic velocities and elastic properties of such materials. The received data are in good agreement with results of measuring integral values of sonic velocities and elastic module for different orientations of unidirectional CFRC laminate specimens performed by low-frequency ultrasonic methods (see, for instance, papers [2,3]). Different delay times L and, respectively, different positions of echo pulses reected from specimen backside can be employed to display distribution of layers with distinct orientation of ber packing over the specimen body. In Fig. 4, we present the acoustic image (C-scan) of the specimen bottom

for different positions of an electronic gate. The electronic gate allows picking from the received echoes only part, which can be taken for visualizing the level of the signal in depth (Fig. 4a). White colour in acoustical images corresponds to the high level of reection pulse. The C-scan in Fig. 4b has been done when the electronic gate involves only the distant pulse L1 resulted from reection at the bottom of layers with ber orientation parallel to the sample surface. 5. Conclusion Acoustic microscopy is a powerful non-destructive method for quantitative characterization of CFR-laminate composites. It provides measuring the local elastic properties and visualization of their distribution over the material body. The method can be applied also to estimate topological characteristics of laminatesthickness of layers, etc. Penetrating ability of high frequency ultrasound make it possible to apply of this technique to fairly thick (28 mm) specimens of CFRC laminates. The work demonstrates the acoustic microscopy, besides of potentialities of imaging internal microstructure of non-transparent advanced ber materials, gives an effective technique for quantitative characterization of ordered composites. Acknowledgements The work has been supported by Grant OXHM PAH No. 04-PAH-07 Development of methods and facilities for microacoustical investigation of structure and properties of advanced materials of Russian Academy of Sciences and by the program KJCXZ-N12 of Chinese Academy of Sciences. References
[1] D.D. Edie, J.J. McHugh, High performance carbon bers, in: T.D. Burchell (Ed.), Carbon Materials for Advanced Technologies, Pergamon, 1999, pp. 183221. [2] Y.C. Chu, S.I. Rokhlin, J. Acoust. Soc. Am. 95 (1994) 3204 3212. [3] S.I. Rokhlin, W. Huang, Y.C. Chu, Ultrasonics 33 (1995) 351364. [4] F. Aymerich, S. Meili, Composites: Part B 31 (2000) 16. [5] L. Wang, Ultrasonics 37 (1999) 283289.