Materials Science and Engineering A 460461 (2007) 95100

Single crystal bulk material micro/nano indentation hardness testing by nanoindentation instrument and AFM
Liang Zhou a,b, , Yingxue Yao a
a

School of Mechanical and Electrical Engineering, Harbin Institute of Technology, Harbin 150001,PR China b School of Material Science and Engineering, Harbin Institute of Technology, Harbin 150001,PR China Received 4 June 2006; received in revised form 2 January 2007; accepted 11 January 2007

Abstract The micro/nano indentation hardness of single crystal aluminium and single crystal silicon are investigated. Loaddepth curves can be obtained by nanoindentation instrument, and materials indentation hardness can be calculated by OliverPharr method and work of indentation method directly from these curves. The hardness that obtained by OliverPharr method is overestimate because of material pile-up effect, and the hardness that obtained by work of indentation method is not very correct because of its empirical equations inaccurate. The true hardness can be calculated by plastic work of indentation and plastic volume that obtained by integrating tted polynomial according to loaddepth curves and atomic force microscopy, respectively. Comparison and analysis of the results that obtained by these methods are made. 2007 Elsevier B.V. All rights reserved.
Keywords: Nanoindentation; Hardness; OliverPharr method; Work of indentation method; Atomic force microscopy

1. Introduction As an indicator of the materials ability against deformation, hardness has been studied for more than 100 years [1,2]. During the last 20 years, researches have become more and more interested in mechanical properties of smaller volumes, and the mechanical properties under micro/nano scale may differ from the macro scale properties due to the size effect and surface effect, etc. [1]. Nanoindentation as an instrumented indentation method is widely used to determine the mechanical properties of both bulk solids and thin lms. The loaddepth curves including loading and unloading process can be obtained by nanoindentation technology. It has been shown that the OliverPharr method [3,4] and work-of-indentation method [5,6], which are commonly used to measure hardness from loaddepth curves. Fig. 1 shows the typical loaddepth relationship curves from nanoindentation experiments, where Pmax is the peak indentation load, hmax the indenter depth at peak load, and hr is the nal depth of contact impression after unloading [3].

The hardness usually dened as the ratio of Pmax to project area of hardness impression Ac (Eq. (1)), and perhaps the most widely used method is OliverPharr method [3]. Hop = Pmax Ac (1)

The OliverPharr method analysis procedure begins by tting the unloading curve to an empirical power-law relation [3,7]. P = (h hr )m (2)

where P is the indentation load, h the indenter depth, and m are empirically determined tting parameters. Once the parameters and m are obtained by curve tting, the initial unlading stiffness, S, can be established by differentiating Eq. (2) at the maximum depth of penetration, h = hmax . The contact depth, hc , is estimated from the loaddepth data [3,7]. hc = hmax Pmax S (3)

Corresponding author at: School of Mechanical and Electrical Engineering, Harbin Institute of Technology, Harbin 150001,PR China. Tel.: +86 451 86402543/608; fax: +86 451 86413810. E-mail address: lzhou75@163.com (L. Zhou). 0921-5093/$ see front matter 2007 Elsevier B.V. All rights reserved. doi:10.1016/j.msea.2007.01.029

where is a constant dependent on the indenter geometry. For the generally employed Berkovich indenter, it has been shown that has an empirical value of 0.75 [3,7]. The project area of hardness impression function is made by tting the Ac versus hc

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(8) [6,8]. Wp hr We =1 =1 Wt Wt hmax (8)

Tuck et al. [5] suggested that the hardness could be calculated on the basis work-of-indentation alone, and can be represented by HWt =
3 Pmax 9Wt2

(9)

where is a constant equal to 0.0408 for Berkovich indenter. Alternatively, by taking the hardness to be concerned with the plastic work of indentation, then the total work term is replaced with the plastic work and the hardness is obtained also [5] (Eq. (10)).
Fig. 1. Typical loaddepth curves from nanoindentation experiments.

HWp = data to the relationship:

7

3 Pmax 2 9Wp

(10)

Ac =

24.56h2 c

+
i=0

/2i Ci h1 c

(4)

where Ci are constants, the lead term describes a perfect Berkovich indenter, the other parameters describe deviations from the Berkovich geometry due to blunting at the tip [3]. Work of indentation method describes indentation experiments process as the use of the energy dissipated or work done during the indentation. The energies are based on the integral of the loading and unloading curves. The area under the loading curve gives the total work Wt (gray region in Fig. 1) done during indentation, while the elastic contribution, We (weak gray region in Fig. 1), is given by the area under the unloading curve. Thus, the plastic work Wp (deep gray region in Fig. 1) is the difference between Wt and We (Fig. 1) [5,6,8]. W p = Wt W e (5)

The work of indentation method to estimate material hardness was rst proposed by Stilwell and Tabor [8]. It was shown that the conventional representation of hardness, indentation load divided by the projected area of permanent impression, is equivalent to the ratio of plastic work to plastically deformed volume [5,6,8]: plastic work, Wp (J) load, P (N) = plastic area, Ap (m2 ) plastic volume, Vp (m3 ) (6)

Although nanoindentation technology give signicant information concerning the mechanical response to indentation and without the need for indent image, the effects of material pileup that often was found at the indent edges [4,6,9] can seriously affect the calculated values. In addition to atomic force microscopy (AFM) high resolution, three dimensional imaging capability, the use of AFM for imaging residual indentations has already proved to be one of the only methods presently available for obtaining accurate dimensional information from an image area of only a few microns [9]. Combining Matlab soft, the real plastic deformation volume of micro/nano indentation can be obtained according to AFM image. In this paper, the indentation hardness of single crystal aluminium and single crystal silicon are investigated. The hardness of these materials is initially determined using OliverPharr method and work-of-indentation method. In order to determine the actual deformation volume and area, the indentations are directly measured via AFM and Matlab soft. The effect of pile-up on hardness values is investigated also. 2. Experimental Bulk materials such as single crystal silicon (10 mm 10 mm 1 mm) and single crystal aluminium ( 25 mm 5 mm) were used for this experiment. Single crystal silicon surface roughness is less than 5 nm after electropolishing, and single crystal aluminium surface roughness is less than 10 nm after turning by diamond cutting tool in ultraprecise machine tool. The indentation experiments were conducted with a Berkovich indenter using Nano II (manufactured by MTS nanoinstruments). It has load and displacement resolutions of 75 nN and 0.04 nm, respectively. In each testing run, the indenter was driven into the specimen surface under a load gradually increased to the predetermined depth, then unloaded after being hold at peak load for 10 s. Such a procedure repeated with different predetermined depths as 500 nm, 800 nm, 1000 nm, 1200 nm and 1500 nm for single

The total work Wt can be obtained by integrating the loading curve. In general, it is found that for sharp indentation of an elasticplastic material the loading response is governed by P = Ch2 , where C is a constant and h is the penetration depth [6] (Eq. (7)). Wt =
0 hmax

P (h) dh =
0

hmax

Ch2 dh =

Pmax hmax 3

(7)

It has been shown that the ratio of hr /hmax is equivalent to that of Wp /Wt . Thus, the plastic work Wp can be obtained by Eq.

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Fig. 2. Loaddepth curves of single crystal silicon. Fig. 5. AFM images of single crystal aluminium.

indentation. The materials pile-up appears in Figs. 4 and 5, we can see that single crystal aluminium indents pile-up higher than single crystal silicon. 3. Results and discussion The hardness values, Hop , HWt and HWp , of single crystal aluminium and single crystal silicon that are calculated directly from loaddepth curve using OliverPharr method and work of indentation method have been plotted as a function of maximum depth in Figs. 6 and 7, respectively. Figs. 6 and 7 show that plastic hardness HWp is too large to accept especially in smaller depth. In addition, the plastic work must be less than total work, but the hardness of plastic work HWp larger than HWt . So, a simple way to use plastic work term Wp replacing Wt perhaps is unreasonable in Eq. (10).

Fig. 3. Loaddepth curves of single crystal aluminium.

crystal silicon and 400 nm, 500 nm, 800 nm, 1000 nm, 1500 nm and 1700 nm for single crystal aluminium. Figs. 2 and 3 show the loaddepth curves of the single crystals silicon and single crystal aluminium, respectively. AFM is Dimension 3100 (manufactured by Digital Instruments). Its integral nonlinearity (X, Y) is 1%, XY imaging area is 90 m, Z range is 6 m, and RMS vertical noise oor is <0.05 nm. Figs. 4 and 5 show one of AFM images for single crystal silicon and single crystal aluminium at different indentation depths. We can see that the elastic recovery appears in loaddepth curves during unloading processing from Figs. 2 and 3, but the elastic recovery of single crystal aluminium is less than single crystal silicon indicating that the deformation occurs mainly by plastic processes for single crystal aluminium. And the same phenomena can be seen from Figs. 4 and 5, the edges of single crystal silicon bend to center because of elastic recovery, but the edges of single crystal aluminium nearly linearity except smaller

Fig. 6. Hardnessdepth curves of single crystal silicon.

Fig. 4. AFM images of single crystal silicon.

Fig. 7. Hardnessdepth curves of single crystal aluminium.

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Fig. 8. Workdepth curves of single crystal silicon.

Fig. 10. Plot of pile-up height with indentation depth.

We can see that all hardness values increasing with the depth decreasing from Figs. 6 and 7. This phenomenon knows as the indentation size effect (ISE). And it is clear that the HWt < Hop from Figs. 6 and 7, the reason is likely to be caused by the elastic contribution to the total work-of-indentation. To single crystal aluminium, the hardness values HWt and Hop are very similar because that indentation deformation mainly is plastic deformation in it. For further analysis, Tuck and Korsunsky suggesting P = Ch2 (Eq. (7)) perhaps is not reasonable. If the suggestion is true, then there is inexistent ISE and hardness is a constant, but ISE phenomenon exists in many materials micro/nano indentation experiment and existing in this testing also. So, we use polynomial tting loading curves and unloading curves of Figs. 2 and 3, the total work and elastic work are obtained by integrating the tted polynomial, and the plastic work are obtained by the difference between total work and elastic work (Eq. (5)) in this experiment. The total work, elastic work and plastic work that obtained by integrating tted polynomial are named as Wt1 , We1 and Wp1 , respectively, in this paper to distinguish with Wt , We and Wp that calculated by Eqs. (7) and (8). Figs. 8 and 9 show the work of indentation plot against the indenter depth of single crystal silicon and single crystal aluminium. In Figs. 8 and 9, there is large elastic work contribution to the total work of single crystal silicon indentation process and the elastic work contribution to the total work of single crystal aluminium is very small. The work that obtained by Eqs. (7) and (8) (Wt , We and Wp ) not as same as the work that obtained by integrating tted polynomial (Wt1 , We1 and Wp1 ), the maximum

Fig. 11. Workvolume curves of single crystal silicon.

percentage of the ratio (Wt Wt1 )/Wt is nearly 20%, and the deviation must be affect hardness calculation. The material pile-up in crystals indent edges may affect the area and volume calculation when using OliverPharr method and work-of-indentation method. If we look at Fig. 10 we see that the pile-up height increases with increasing penetration depth for the two crystals, and the pile-up height of single crystal aluminium is higher than single crystal silicon at any indentation depth because of the single crystal aluminium plastic property better than single crystal silicon. The pile-up height is obtained by AFM images also. Combining Matlab program, we can obtain the total plastic deformation volume, including the volume of material above and below the surface, i.e. the pile-up volume and three-sides pyramidal indent volume. The total volume, pile-up volume and indent volume are named as Vt , Va and Vb in this paper, respectively. The relationship curves of work and volume are shown in Figs. 11 and 12.

Fig. 9. Workdepth curves of single crystal aluminium.

Fig. 12. Workvolume curves of single crystal aluminium.

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Fig. 13. Plots of hardness vs. depth of single crystal silicon.

In Figs. 11 and 12, we can see that the work either obtained by Eqs. (7) and (8) or obtained by integrating tted polynomial have a good linearity with volume, but the slopes of these tting lines are different, i.e. the hardness values are different because of work of indentation obtained by different method. Thus, we can obtain the hardness of crystals by work of indentation divided by plastic volume. When discussing the hardness results, the following nomenclature is used to distinguish the hardness values (Hop , HWt and HWp ) that have been described in this paper. The hardness that obtained by Wt1 /Vt is named HWt1 , the hardness obtained by Wp1 /Vt is named HWp1 , and the hardness obtained by Wp1 /Vb is named HWp2 . Plots of hardness, Hop , HWt , HWt1 , HWp1 and HWp2 versus depth are drawn for crystals examined in the present study and are now shown in Figs. 13 and 14. Whether the hardness calculated by OliverPharr method or work-of-indentation method, and whether the work of indentation directly obtained by empirical equations or integrating tted polynomial, the hardness values existing ISE phenomenon. But the hardness values that obtained by the ratio of plastic work to total plastic deformation volume, i.e. HWp1 = Wp1 /Vt variation is smoother than others. Fig. 13 shows that single crystal silicon indentation hardness HWt1 in excess of two times of HWp1 , this means the large elastic work mainly contribution to the total work of indentation that calculated by integrating tted polynomial. Reversely, in Fig. 14, HWt1 is almost similar with HWp1 of single crystal aluminium because of the deformation in indentation processing almost only plastic deformation happening.

Further analysis, the hardness values HWp2 , i.e. plastic work divided by indent plastic volume only, is very nearly the hardness values Hop that obtained by OliverPharr method for all examined crystals in present study. Hence, the OliverPharr method hardness yields values have not considering the material pile-up plastic volume that would seriously affect the results. Due to the plastic contact depth is greatly underestimated in OliverPharr method because of ignoring materials pile-up, lead to overestimate hardness values. To HWt , the hardness values that obtained by work of indentation method (Eqs. (7) and (9)) are similar with Hop of single crystal aluminium, but similar with HWp1 of single crystal silicon, so, the hardness value HWt is more suitable elasticplastic materials not plastic materials, the reason is under the understanding that Hop is overestimate the indentation hardness and HWp1 is nearest the true hardness of materials. The constant = 0.0408 of Eq. (9) using in work of indentation method and = 0.75 of Eq. (3) using in OliverPharr method are dependent on the indenter geometry, but under micro/nano scale, the indenter geometry did not self-similar. So, the two constant will generate errors under different indentation depths. And the project area Ac (Eq. (4)) of OliverPharr method and the hardness HWt (Eq. (9)) of work-of-indentation method are empirical equation or semi-empirical equation that will seriously affects by testing condition, testing instruments, irregularities of material, initial state of material surface and so on. To HWp1 , the plastic work is calculated by integrating tted polynomial according to loaddepth curves, the plastic volume including material pile-up volume and indent volume are obtained by real indent AFM images, so, the results of HWp1 perhaps are more accurate and believable than other results, and the effects of pileup are eliminated because of considering the pile-up volume in calculation. 4. Conclusions Under micro/nano scale, loaddepth curve can be obtained by nanoindentation instrument, and real indent image can be obtained by AFM. Materials indentation hardness can be calculated directly from loaddepth curves by OliverPharr method and work of indentation method. But the hardness values are overestimated by OliverPharr method because of pile-up effect, and the hardness values are inaccurate by work of indentation method because of its suggestions are not completely correctly. Plastic work can be obtained integrating tted polynomial based on loaddepth curve and real plastic volume including pile-up volume and indent volume obtained by AFM images. The hardness values that using plastic work divided by plastic volume are more smoother than other results, and also perhaps more accurate and believable. Acknowledgements Support for this work by the Scientic Research Foundation of Harbin Institute of Technology (Project: HIT.2003.23) and Doctor Research Startup Foundation of Harbin Institute of Technology.

Fig. 14. Plots of hardness vs. depth of single crystal aluminium.

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