Appl Phys B (2008) 92: 493499 DOI 10.

1007/s00340-008-3138-8

Characterization and comparison of X-ray focusing optics for ultrafast X-ray diffraction experiments
U. Shymanovich M. Nicoul K. Sokolowski-Tinten A. Tarasevitch C. Michaelsen D. von der Linde

Received: 5 November 2007 / Revised version: 3 June 2008 / Published online: 1 August 2008 Springer-Verlag 2008

Abstract We have characterized and compared the performance of different types of multi-layer optics for the focusing of femtosecond X-ray pulses. Using X-ray pulses at 8 keV, from a laser-driven plasma source we have measured the spatial distribution of the diffracted X-rays directly after and in the focal plane of the various X-ray optical devices. For a Montel optic with 7.3 magnication we obtained the largest number of focused X-ray photons per unit angle. The performance of this optic in the X-ray diffraction experiment on a thin germanium lm is demonstrated. PACS 61.10.Nz 41.50.+h 87.59.-e

1 Introduction During the last few years there has been an increasing interest in femtosecond time-resolved X-ray diffraction experiments (TXRD) using accelerator based and laserplasma based X-ray sources [14]. While accelerator based X-ray sources [5, 6] offer well-collimated beams, the X-rays from laser-produced plasma sources are emitted into the full solid angle. In order to use these X-rays in an experiment, they must be collected and focused onto the

U. Shymanovich ( ) M. Nicoul K. Sokolowski-Tinten A. Tarasevitch D. von der Linde Institut fr Experimentelle Physik, Universitt DuisburgEssen, Lotharstr. 1, 47048 Duisburg, Germany e-mail: uladzimir.shymanovich@uni-due.de C. Michaelsen Incoatec GmbH, Max-Planck-Str. 2, 21502 Geesthacht, Germany

sample under investigation using a suitable X-ray focusing optic. Previously, toroidally bent crystals were used successfully for this purpose in a number of experiments [711]. Typically, the bent crystal devices were used in a 1:1 imaging geometry, where a monochromatized image of the source is produced on the sample surface. Recently, other types of X-ray focusing optics have also been studied [12]. Each type of optic has its own specic advantages for certain diffraction experiments or other applications. In order to determine the suitability for TXRD experiments with laserplasma based X-ray sources, Bargheer et al. [12] have measured and compared spatial distributions and other important characteristics of reected or diffracted X-rays from a crystal mirror (toroidally bent germanium platelet), a multi-layer optic, a single ellipsoidal capillary, and a poly-capillary device. One of their conclusions was that the multi-layer optic offers an excellent compromise regarding temporal pulse broadening, spectral selectivity, focal size, and radiation ux. Here we present characterization results of three new hard X-ray multi-layer optics designed for focusing femtosecond pulses, namely a single-bounce mirror and two socalled Montel optics [13]. The latter represent a modication of the well-known KirkpatrickBaez scheme [14]. Our study also includes a comparison of the performances of the Montel optic and the toroidally bent crystal optics, described in reference [11], in a static diffraction experiment for the particular case of the (444) reection from a 150 nm thick germanium lm, hetero-epitaxially grown on a silicon substrate.

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a a

b
Fig. 1 SBM optic: (a) photograph; (b) principle scheme

2 Description of the tested mirrors 2.1 Single-bounce multi-layer mirror

b
Fig. 2 Montel optic: (a) photograph; (b) principle scheme

2.2 Montel optics The single-bounce multi-layer mirror (SBM) has the shape of a rotational ellipsoid. It collects X-rays from a point-like source and forms an image of the source in a focal plane. Figure 1a shows a photograph of the SBM and Fig. 1b illustrates the principle of operation. The substrate of the SBM is covered with a multi-layer reective coating. To ensure high reectivity for hard X-rays the mirror works under grazing incidence. Lateral gradation of the layer thickness guarantees that the Bragg condition is satised over the entire area of the mirror. By manufacturing mirrors with different surface curvature and different lateral gradation the magnication of the devices can be varied. Here, we characterize an SBM device with 3.2 magnication. Montel optics consist of two perpendicular mirrors, each focuses the radiation in one dimension only. Two-dimensional focusing is then achieved by placing the mirrors close to one another as shown in Fig. 2a, b. In this arrangement the X-rays passing through the optic are sequentially reected from the two mirrors. The characteristic paths of the X-rays in this conguration are indicated in Fig. 2b by dark and bright lines. The layer spacing of the multi-layers is again laterally graded along the surface to satisfy the Bragg condition at every point. Thus, the X-rays can be collected and focused over a large solid angle using this type of device. In this report we present the results for two Montel optics with magnications of 2.1 and 7.3, respectively.

Characterization and comparison of X-ray focusing optics for ultrafast X-ray diffraction experiments

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3 Testing of the optics X-ray pulses were produced with the help of a terawatt CPA (chirped pulse amplication) Titanium Sapphire laser ( = 800 nm) with the following parameters: pulse duration = 120 fs, energy Ep = 110 mJ, repetition rate = 10 Hz. To produce X-rays the laser pulses were focused onto a copper wire of 250 m in diameter using a lens with a 30 cm focal length, producing peak intensities of several times 1017 W/cm2 . A large portion of the X-rays from the laser-produced micro-plasma consists of characteristic K -radiation of copper ( = 0.154 nm). This radiation was used for testing the X-ray optics. The principle scheme of the experiment for characterization of the optics is shown in Fig. 3. For each type of X-ray optics we measured the X-ray intensity distribution in the

b
Fig. 3 Schemes of the experiments for testing of optics: (a) measurement of the intensity distribution in the focal spot of the X-ray optic; (b) measurement of the topography

image plane (Fig. 3a) and in a plane located directly after the device (Fig. 3b). The spatial distributions of the X-rays were measured using a camera equipped with a thinned, backilluminated CCD (charge-coupled device) chip. The actual distances between the X-ray source, the focusing optics, and the CCD camera shown in the scheme in Fig. 3 were determined by the properties of the devices as dened by the manufacturer. These distances and some other parameters of the optics under test are listed in Table 1. Table 2 summarizes the measured data. As a typical crystalline sample diffracts X-rays only in a narrow angular range determined by the width of its rocking curve, it is important to guide as many X-rays into this angular range as possible, that is, to maximize the angular ux density (number of focused Xray photons per unit angle). As one can see from Table 2 the Montel-E19 optic has the largest angular ux density and in this respect it is the most attractive one for diffraction experiments. Another important characteristic of X-ray optics is the size of the focal spot. In an excite-and-probe experiment with laser excitation and X-ray probing, the X-ray spot size on the sample should be much smaller than the spot size of the optical excitation beam to ensure that a homogeneously excited portion of the sample is probed. A small spot size of the optical excitation can be important in non-reversible experiments when raster scanning must be applied and the sample size is limited. For all devices tested in this work the X-rays could be focused onto a spot with a diameter in the range of 100 200 m. The actual focal spot size is determined by the convolution of the point spread function of the imaging device and the size of the X-ray source.

Table 1 Geometrical properties of the tested multi-layer optics

Type of optic Source-optic distance dso [mm] Optic-image distance doi [mm] Length of the device l [mm] Capturing angle Magnication M Hor. convergence h [mrad] [mrad2 ]

SBM 90 350 60 12 36 3.2 11.2

Montel-E17 90 250 100 17 17 2.1 8.0

Montel-E19 20 400 80 31 31 7.3 4.2

Table 2 Measured parameters of the tested multi-layer optics. The following parameters of the optics are presented: Flux in the focus is the total number of K photons per pulse detected in the focus of the optic, normalized to the Montel-E17 mirror (magnication of M = 2.1); Angular ux density is the number of photons per pulse and unit angle detected in the focus; Size of the focus is the full width at half maximum of the distribution of diffracted X-rays in the image plane Type of optic Flux in the focus [norm] Angular ux density [norm] Size of the focus (sx sy ) [m2 ] SBM 4.3 3.1 180 120 Montel-E17 1 1 90 90 Montel-E19 4.9 9.4 250 140

496 Fig. 4 Spatial distributions of the X-rays after they have passed through different optics: (a) SBM optic; (b) Montel optic with a magnication of M = 2.1; (c) Montel optic with a magnication of M = 7.3. The upper section shows the X-ray intensity distributions directly after passing through the optic. The lower section depicts the distributions in the image planes

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The measured spatial distributions of the X-rays are presented in Fig. 4. The upper section shows the distributions with the X-ray detector placed directly after the optics (near eld; topography), providing information about the uniformity of the reected X-rays over the mirror surface. The results of the measurements in the image plane (far eld; focus) are depicted in the lower section. These distributions yield information about size, shape and intensity of the focused radiation. In the pictures showing the topography and the focus of the SBM (Fig. 4a), both the reected X-rays and the X-rays passing directly through the aperture of the optic without touching the mirror surface can be recognized. In the focal plane the reected X-rays form a small spot (see lower part of Fig. 4a), while in the topography plane they are spread over an extended, arch-shaped distribution (upper part of Fig. 4a). The distribution of X-rays going through the optic unaffected gives rise to the large circle segment seen in both pictures. The distribution of the X-rays reected by the optic and measured in the topography conguration reveals small variations of the reection coefcient over the mirror surface. The output radiation of the Montel optics consists of three components. The rst component in the shape of a square is the direct radiation passing without reection. The second component consists of two rectangular areas or lines formed by a single reection from either the rst or the second multi-layer mirror. The third component is the radiation of interest, i. e. the actual focal spot located at the intersection of the two lines. This spot is formed by a twofold

reection of the X-rays from both mirrors. For the MontelE19 optic with a magnication of M = 7.3 the three components overlap in the topography plane (Fig. 4c, upper section). These components separate as the observation plane moves towards the image plane (see Fig. 4c lower section). The measured near-eld distributions for the two Montel optics give evidence for a good uniformity of the X-ray reectivity across the mirror surfaces. Expanded views of the pictures of the measured focal distributions are shown in Fig. 5, together with the proles in the vertical and horizontal directions. It can be seen from Fig. 5 that all our tested focusing devices produce smooth X-ray intensity distributions in the focal plane.

4 Diffraction test with the Montel focusing optic As mentioned in the previous section, among the three tested devices the Montel-E19 optic with 7.3 magnication provides the highest angular ux density for the focused X-rays. Because the Bragg diffraction signal from a monocrystalline sample is proportional to the angular ux density, the Montel-E19 optic was used to perform diffraction experiments on a 150 nm thick, single-crystalline germanium lm grown on a silicon substrate [15]. The sample was placed in the focal spot of the Montel-E19 optic. The Ge (444) reection was observed (Bragg = 70.6 ). The measured diffracted signal represents a spot with an angular full width of about 3 mrad at half maximum. Figure 6a contains a horizontal

Characterization and comparison of X-ray focusing optics for ultrafast X-ray diffraction experiments Fig. 5 Images and cross-sections of the optics foci: (a) SBM optic; (b) Montel-E17 optic with a magnication of M = 2.1; (c) Montel-E19 optic with a magnication of M = 7.3

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cross-section of the diffraction signal (the latter is depicted in the inset of the graph in Fig. 6a). The angular width of the diffracted signal is mostly determined by the angular range of the X-rays focused on the sample (see Table 2). In this case the broad spectrum of the focused radiation (including K1 and K2 ) allows the Bragg condition to be satised for all angles of incidence at the sample. The measured diffraction signal was compared to the signal when X-rays were focused onto the sample by a toroidally bent crystal described in reference [11]. The corresponding horizontal cross-section and the diffracted signal are presented in Fig. 6b. In the latter case, the diffracted signal exhibits a large spread in vertical direction determined by the angular range of the X-rays focused by a toroidally crystal (around 80 mrad in vertical direction). The measured angular width in horizontal direction is approximately 2 mrad, determined by the rocking curve width of the thin lm sample. This value is approximately an order of magnitude smaller than the horizontal angular range of the incident radiation (around 30 mrad). This difference is due to the fact, that the focused radiation is strongly monochromatic and the

Bragg condition can be satised only for a very narrow angular range of the incident radiation. The Ge (444) diffraction signal was measured to be approximately 25 5 times larger with the Montel optic compared to focusing with the toroidally bent crystal. The accuracy of this signal ratio was limited by the relatively poor signal-to-noise ratio (Fig. 6b) of the experiment with the crystal optic, where the diffraction signal on the CCD camera corresponded to less than one detected photon per pulse. The radiation ux from the X-ray source was kept the same during both diffraction experiments. For a theoretical estimate of the signal ratio for the two diffraction experiments one should keep in mind that with the Montel optic the sample can diffract only the K1 component ( = 0.15406 nm), because the Bragg condition is not fullled for the K2 line ( = 0.15444 nm) due to the small total angular range of the focused X-rays. Thus, the K2 component does not contribute to the diffraction signal. With this correction included, the ratio of the diffraction signals for the two different focusing devices estimated as a ratio of the angular ux densities of the incident radiation should be 20, which is in reasonable agreement with the measured ratio of 25 5.

498 Fig. 6 Measured diffraction signals of the (444) reection from a (111) oriented 150 nm thick germanium lm: (a) X-ray focused by the Montel-E19; (b) X-ray focused by toroidally bent crystal

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We would like to nish this section with a remark on the inuence these optics can have on the effective duration of the X-ray pulses in the focus. As it has been discussed in references [12, 16], an ultrashort X-ray pulse may be temporally broadened depending on the experimental geometry and the properties of the optic. Three effects can lead to an increase of the X-ray pulse duration: (1) the nite size of the imaged X-ray source, (2) (deep) penetration of the X-rays into the optics and (3) the shape and the quality of the surface. For the optics discussed here, where total thicknesses of the reecting multi-layers are less than 1 m, typical values for the slope and height error are 15 arcsec and 1 m, respectively, and with a source size of about 25 m, all three mentioned effects will lead to a negligible pulse broadening of a few femtoseconds at most.

Acknowledgements Financial support by the Deutsche Forschungsgemeinschaft (Collaborative Research Center SFB 616 and Priority Program 1134) and the European Community (research and training networks XPOSE and FLASH) is gratefully acknowledged.

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5 Conclusion We have characterized and compared different types of multi-layer X-ray focusing optics. It was found that all of the tested optics allow the X-ray radiation to be focused onto a spot with a diameter of about 100200 m. The X-ray yield in the focal spot of each optic was measured using femtosecond Cu-K pulses produced by a laserplasma based X-ray source. The small focal spot size and the large ux of the focused X-rays make it possible to use these devices for focusing in femtosecond time-resolved X-ray diffraction experiments. The performance in the actual diffraction experiment was demonstrated with the Montel-E19 optic with a magnication of M = 7.3. Optics with large magnication provide a high angular ux density in a relatively small angular range and are therefore excellent candidates for experiments, where angular shifts and changes of the shape of the rocking curve are relatively small or negligible and where the integrated reectivity of the sample is of interest.

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