Text
                    Nano-Scale Imaging With Tabletop Soft X-Ray Lasers:
Sub-38 nm Resolution
C. S. Menoni1,2, G. Vaschenko1,2, F. Brizuela1,2, C. Brewer1,2, Y. Wang1,2,
M. A. Larotonda1,2, B. M. Luther 1,2, M. C. Marconi1,2, and J. J. Rocca1,2,
W. Chao1,3, J. A. Liddle1,3, Y. Liu1,3, E. H. Anderson1,3, and D. T. Attwood1,3,4 A. V. Vinogradov5, I. A. Artioukov5, Y. P. Pershyn6 and V. V.
Kondratenko6
1

NSF ERC for Extreme Ultraviolet Science and Technology
Department of Electrical and Computer Engineering, Colorado State University, Fort Collins, CO 80523
3
Center for X-ray Optics, Lawrence Berkeley National Laboratory,
4
University of California, Berkeley, CA 94720
5
P. N. Lebedev Physical Institute, Russia
6
National Technical University “KhPI”, Ukraine
2

Summary. We report the demonstration of soft x-ray microscopes with resolution
down to sub-38 nm using tabletop soft x-ray laser illumination. One of the compact microscopes combines the 46.9 nm wavelength output from a capillary discharge Ne-like Ar laser with a reflective condenser and a free standing zone plate
objective. High quality images were acquired with this microscope in transmission
mode and reflection mode. The latter includes images of an integrated circuit pattern containing polysilicon features on silicon. The spatial resolution for this microscope is between 120-150 nm. Increased resolution was demonstrated in another microscope using 13.2/13.9 nm wavelength illumination from Ni-like Cd/Ag
transient soft x-ray lasers in combination with diffractive zone plate optics for
both the condenser and objective. Using an objective zone plate with a 50 nm
outer zone width, this optical system achieved a record sub-38 nm spatial resolution. These results demonstrate the feasibility of using compact high repetition
rate soft-x-ray laser sources in nanometer-scale microscopy.

1. Introduction
The development of practical imaging tools with nanometer-scale spatial
resolution are of importance for many applications ranging from material
science and microelectronics to biology. A direct pathway to realize mi-


418 C. S. Menoni et al. croscopy with tens of nanometers resolving power is to use soft x-ray (SXR) light. The best spatial resolution for photon-based microscopes to date, 15 nm, was obtained using soft x-ray illumination from a synchrotron source [1]. Aside from the experiments conducted at synchrotron facilities, a variety of imaging experiments have been carried out using both coherent and incoherent short wavelength sources. Early imaging work with soft x-ray lasers demonstrated submicrometer resolution in reflection mode with a SXR recombination laser at λ=18.2 nm. [2] A resolution of 75 nm was reported using the λ=4.48 nm output from a SXR laser pumped by the very large fusion-driver NOVA which was limited to firing several shots a day. [3] In the last several years smaller-scale short wavelength sources including high order harmonics [4], and incoherent laser-plasma-based sources [5,6], have been used for submicron resolution imaging. Of these experiments, the best performance in terms of spatial resolution, reported as sub-100 nm, was obtained with a laser-created incoherent plasma source emitting at λ = 3.37 nm [6]. In this paper we discuss the implementation and demonstration of soft x-ray microscopy with compact high repetition rate laser sources. We present imaging results in transmission and reflection modes obtained with a microscope that combines the output from a λ = 46.9 nm capillary discharge pumped Ne-like Ar laser with a reflective condenser and objective zone plate. This instrument is capable of acquiring high quality images with a large field of view in exposure times of ~10 - 20 seconds and with a spatial resolution between 120-150 nm. Another transmission mode microscope was developed using a similar geometry but with Fresnel zone plate (FZP) optics for both the condenser and the objective in combination with shorter 13.2/13.9 nm wavelength illumination from laser-pumped Nilike Cd or Ag collisionally excited soft x-ray lasers. This compactable-top photon-based imaging system is shown to have a spatial resolution better than 38 nm. 2. λ=46.9 nm imaging system based on a table-top capillary discharge laser The tabletop soft x-ray microscope implemented using a capillary discharge Ne-like Ar laser as the illumination source is configured to operate either in transmission or in the more versatile reflection mode. In transmission mode, illustrated in Fig. 1a, the laser output is collected and focused onto a sample using a Sc/Si multilayer coated Schwarzschild con-
Nano-Scale Imaging With Table-Top Soft X-Ray Lasers 419 denser. A free standing FZP objective then forms the image onto a backilluminated CCD detector. Fig. 1. (a) Schematic diagram of the 46.9 nm soft x-ray laser microscope in its transmission mode implementation. (b) Photograph of the inside of the vacuum chamber that houses the microscope. The Sc/Si multilayer coated Schwarzschild condenser contains a primary convex mirror of 10.8 mm in diameter and a 50 mm diameter secondary concave mirror. [7] Together these two mirrors produce a hollow cone of λ = 46.9 nm light that is focused onto the sample, which is positioned at ~ 5 cm from the output of the condenser. The Schwarzschild condenser has a numerical aperture (NA) of 0.18 and a throughput of ~ 1%, due to the less than optimum reflectivity of the coatings at λ = 46.9 nm The FZP objective was fabricated to be “freestanding,” as the use of any substrate material would significantly attenuate the λ = 46.9 nm light. The zone plate, manufactured onto a thin nickel foil attached to a silicon frame, contained pseudo-random bridges connecting the different zones to provide structural stability. [8] The FZP objective has a diameter of 0.5 mm, an outer zone width of 200 nm, a NA of 0.12 and a focal distance of 2.13 mm. To achieve high magnification (~ 750×) the FZP objective to CCD distance was chosen to be 1.6 m, which required the working distance of the objective be very close to its focal distance. For these experiments, the capillary discharge laser was equipped with an Al2O3 capillary 18 cm long, resulting in an average power ~ 0.1 mW. [9,10] This choice of capillary length provided a good compromise between output power and degree of coherence of the source [11]. Although a single laser shot produced discernable images, most images were acquired by accumulating several shots to improve the signal-to-noise ratio. Nevertheless, since the laser can be operated at a repetition rate of several
420 C. S. Menoni et al. Hz, the exposure time was only several seconds. The images were collected with a back-illuminated CCD camera with a 1024×1024 array of 24×24 μm2 pixels. Fig. 2. a) Soft x-ray image of the free standing zone plate objective showing the different zones connected with pseudo-random bridges. The outermost zones of width 200 nm and the corresponding intensity cross-section are shown in (b) and (c) respectively. The test sample used in the transmission imaging experiment was a freestanding FZP similar to the one used as the objective. Fig. 2a is an image of the central portion of this test pattern and was acquired in 20 seconds at a magnification of 250×. The resolution of the imaging system was obtained from the high magnification images of the 200 nm outer edge of the FZP sample, as shown in Fig. 2b (×750 magnification, 10 sec. exposure). From this image the intensity modulation or lineout along the outer edge portion of the FZP was obtained (Fig. 2c). An average of 100 lineout traces shows the intensity modulation is ~ 94 %. This intensity modulation is significantly higher than the 26.5% set by the Rayleigh resolution criterion, suggesting that the resolution of the instrument is significantly better than 200 nm. To estimate the spatial resolution of the imaging system, simulations were performed using the SPLAT program [12]. From the simulations a 120 - 150 nm resolution was estimated. This program assumes the use of incoherent light illumination, which is justifiable for this imaging system when using a short length capillary to ensure low coherence. [11].
Nano-Scale Imaging With Table-Top Soft X-Ray Lasers 421 Fig. 3. Soft x-ray image of a silicon wafer patterned with 100 nm polysilicon lines (top right) and 250 nm half-period lines with equal lines and spaces (bottom right). This image was obtained with the 200 nm outer zone objective using a 20 second exposure (20 laser shots) and a magnification of 750×. To acquire images in reflection mode the object was rotated by 45º with respect to the incoming beam, and the FZP objective and CCD were rotated by 90º. In this configuration, the depth of focus of the objective FZP limited the area of the image in focus at the CCD to 3×30 μm2. This was overcome by digitally compensating the images. We imaged a test pattern consisting of polysilicon lines on a silicon substrate. This test pattern was originally produced for optimization of the lithography process for chip manufacturing. Fig. 3 shows an image of this sample obtained with a 20 second exposure. The condenser was scanned during acquisition to ensure complete illumination of the sample and to reduce coherence effects on the image. In the upper right corner of Fig. 3, 100 nm polysilicon lines separated by 800 nm spaces are clearly discernible, and in the lower right region, 250 nm lines with 250 nm separations are well resolved. A more compact “desk-top” size version of this microscope is currently under development. It will utilize the desk-top size Ne-like Ar capillary discharge laser developed at CSU in combination with an objective FZP with a 120 nm outer-most zone to obtain sub 100 nm resolution images.
422 C. S. Menoni et al. 3. Imaging at 13 nm with a laser-pumped tabletop laser We have also demonstrated the operation of a microscope at wavelengths near 13.5 nm. The shorter wavelength of the illumination coupled with aberration free zone plate optics allowed a record spatial resolution to be obtained for a tabletop photon-based full-field microscope system. The illumination is provided by either a 13.2 nm Ni-like Cd or a 13.9 nm Nilike Ag laser-pumped transient collisional laser generating highly monochromatic light (Δλ/λ < 1 × 10-4) with microwatt average power. [13,14] The condenser and objective FZPs were fabricated by electron beam lithography in a ~ 120 nm thick nickel film supported by a 100 nm Si3N4 layer that is ~ 40 % transparent to the incident 13 nm light. The condenser FZP has a diameter of 5 mm and consists of 12,500 zones of decreasing width down to 100 nm. It has a numerical aperture NA = 0.07 and a focal distance of 38 mm for the wavelength of 13.2 nm. Two different objective zone plates were used. One has a diameter of 0.2 mm and contains 625 zones with an outer zone width of Δr = 80 nm. The second one has a 0.1 mm diameter with Δr = 50 nm. Microscope magnifications of 290 – 1750× were obtained by selecting the objective working distance very close to its focal length and by selecting the distance between the objective zone plate and the CCD camera in the 0.335 to 0.635 m range. The spatial resolution of the microscope was determined by imaging a series of dense grating test patterns of period ranging from 38 to 310 nm. The sample also contains a set of 64 radial spokes decreasing in width down to ~ 40 nm as they converge towards the center of a circular pattern. Figure 4 shows an image of the radial spokes pattern obtained with the objective zone plate of Δr = 80 nm, using λ = 13.9 nm illumination and an exposure time of 20 sec (100 laser pulses at 5 Hz). The central part of the image contains 60 nm half-period lines that are clearly visible. The acquisition of images with a relatively large field of view (~ 12 × 20 µm2) is facilitated by the high brightness of the laser, which allows the condenser to efficiently collect the laser emission and focus it onto the test pattern. The spatial resolution of the microscope was experimentally determined from the images of grating patterns with different periods, all of them with nominal 1:1 line/space ratio. Figure 5 shows a soft x-ray image of gratings with 50 nm dense lines obtained with the FZP of Δr = 50 nm and λ = 13.2 nm illumination. The intensity lineout corresponding to the 38 nm grating image is also shown in Fig. 5. The ~ 70 % intensity modulation clearly demonstrates that the spatial resolution of the microscope is better than 38 nm.
Nano-Scale Imaging With Table-Top Soft X-Ray Lasers 423 Fig. 4. Image of a pattern consisting of radial spokes of width increasing outwards obtained at λ = 13.9 nm with the Δr= 80 nm FZP and a 6 sec. exposure. Fig. 5. Soft x-ray image of 50 nm dense lines (left) obtained at λ=13.2 nm with the Δr = 50 nm FZP. The image of the 38 nm dense lines and its lineout are shown on the right. The ~ 70% intensity modulation shows that the spatial resolution of the system is better than 38 nm. 4. Summary We have demonstrated high resolution full field imaging at soft x-ray wavelengths by combining the output from high repetition rate tabletop lasers at λ = 46.9, 13.9 and 13.2 nm with diffractive FZP optics. The λ = 46.9 nm microscope renders images in transmission and in the challenging reflection mode of operation. Its spatial resolution has been determined to
424 C. S. Menoni et al. be 120-150 nm. The best spatial resolution, 38 nm, was realized with an all zone plate imaging system at λ = 13.2 nm using an objective FZP with an outer zone width of Δr = 50 nm. The spatial resolution of these microscopes could be readily improved by using objective zone plates with smaller outer zone widths and increased numerical apertures. 5. Acknowledgments This work was supported by the Engineering Research Centers Program of the National Science Foundation under NSF Award Number EEC0310717. References 1. Chao, W., Harteneck, B. D., Liddle, J. A., Anderson, E. H. and Attwood, D. T., “Soft X-ray microscopy at a spatial resolution better than 15 nm.” Nature 435, 1210-1213, 2005. 2. DiCicco, D. S., Kim, D., Rosser, R. and Suckewer, S., “First stage in development of a soft-x-ray reflection imaging microscope in the Schwarzschild configuration using a soft-x-ray laser at 18.2 nm.” Opt. Lett. 17, 157-159, 1992. 3. Da Silva, L. B. et al. “Demonstration of x-ray microscopy with an x-ray laser operating near the carbon K edge.” Opt. Lett. 17, 754-756, 1992. 4. Wieland, M. et al. “Towards time-resolved soft X-ray microscopy using pulsed fs-high-harmonic radiation.” Ultramicoscopy 102, 93-100, 2005. 5. Artioukov I.A. et al., “Schwarzschild soft-x-ray microscope for imaging of nonradiating objects.” Opt. Lett. 20, 2451-2453, 1995. 6. Berglund, M., Rymell, L., Peuker, M., Wilhein, T. & Hertz, H. M., “Compact water-window x-ray microscopy.” J. Microsc. 197, 268-273, 2000. 7. Artioukov I.A., Krymski K.M., “Schwarzschild objective for soft x-rays,” Optical Engineering 39, 2163-2170, 2000 8. Anderson E.H., “Specialized electron beam nanolithography for EUV and Xray diffractive optics,” IEEE Journal Of Quantum Electronics 42, 27-35, 2006. 9. Benware B.R., Macchietto C.D., Moreno C.H., Rocca J.J., “Demonstration of a high average power tabletop soft X-ray laser,” Phys. Rev. Lett. 81, 58045807 1998. 10. Macchietto CD, Benware BR, Rocca JJ, “Generation of millijoule-level softx-ray laser pulses at a 4-Hz repetition rate in a highly saturated tabletop capillary discharge amplifier,” Opt. Lett. 24, 1115-1117, 1999.
Nano-Scale Imaging With Table-Top Soft X-Ray Lasers 425 11. Liu Y., Seminario M., Tomasel F.G., Chang C., Rocca J.J., Attwood D.T., “Achievement of essentially full spatial coherence in a high-average-power soft-x-ray laser,” Physical Review A 63, Art. No. 033802, 2001. 12. Heck, J. M., Attwood, D. T., Meyer-Ilse, W. & Anderson, E. H., “Resolution determination in X-ray microscopy: an analysis of the effects of partial coherence and illumination spectrum,” J. X-ray Sci. Technol. 8, 95-104, 1998. 13. Wang Y., Larotonda M.A., Luther B.M., Alessi D., Berrill M., Shlyaptsev V.N., Rocca J.J., “Demonstration of high-repetition-rate tabletop soft-x-ray lasers with saturated output at wavelengths down to 13.9 nm and gain down to 10.9 nm,” Phys. Rev. A 72, Art. No. 053807, 2005. 14. Rocca J.J., Wang Y., Larotonda M.A., Luther B.M., Berrill M., Alessi D., “Saturated 13.2 nm high-repetition-rate laser in nickellike cadmium (vol 30, pg 2581, 2005)”, Opt. Lett. 31, 129-129, 2006.