Theoretical and Experimental Study of Piezoelectric Modulated AlN Thin Films for Shear Mode BAW Resonators

The use of acoustic resonators for sensors application has opened a new branch in research and applications of piezoelectric materials and devices. The first generation of such sensors is constituted by the quartz crystal microbalance (QCM) based on AT-cut mono-crystalline quartz. High sensitivities of gravimetric sensing in both air and liquids were demonstrated. Since the 1980s, when the first QCM-based sensor was demonstrated for the detection of silver in a liquid solution, many other application in chemical, bio-medical and environmental sensing were realized using the same concept. QCM's exhibit a very good thermal stability. The AT-cut quartz plate leads to the excitation of shear waves when used in parallel capacitor geometry. This is important for achieving high quality factors in the immersed operation of the sensor. A second generation of gravimetric sensors is based on surface acoustic wave (SAW) structures, working for instance with Love waves in a SiO2 layer on top of a LiTaO3 single crystal. SAW devices are mainly used as RF filters in television and mobile phones. SAW sensors are a side product of the much larger telecommunication market. The evolution of thin film and MEMS technology has lead to a third generation of gravimetric sensors that is based on bulk acoustic wave (BAW) resonances in piezoelectric thin films. Again, such sensors are a side product from the large telecommunication market where such resonators are used for RF filters. With every generation, the oscillation frequency increased. While QCM's operate typically at 5 MHz, the SAW resonators work typically at a few 100 MHz, and the thin film BAW resonators (TFBAR) operate typically around 2 GHz. The increase of the frequency goes together with an increase in sensitivity, and a decrease of the thickness and mass range that can be measured. The TFBARs are in some sense miniaturized analogs of QCM's operating at much higher frequencies. They are very promising as they reach higher sensitivities. This attracted the attention of researchers, and experimental evidence of the potential of TFBARs as sensors was delivered. In addition to the higher sensitivity, the miniaturization allows for using arrays of sensors with different immobilization layers as needed for drug screening. However, the application of the same TFBARs as used in telecommunications would not allow a good performance in immersed operation. It would only be good for operation in air. The principal characteristic of TFBARs used in mobile phones is the value of the electromechanical coupling and not the resonance mode at which this coupling is achieved. But for the in-liquid operated sensors, it's rather the opposite – the mode of the resonance should be such that the surface of the resonator, which tis in contact with liquid, should move parallel to the surface (in-plane motion, or transverse motion) to minimize emission of acoustic waves into the liquid. The coupling coefficient is of secondary importance in this case. Therefore, the development of shear mode TFBARs became an interesting task that was challenged by several research groups. One of the most successful solutions is the use of c-axis inclined AlN thin films. Inclination of c-axis in a parallel plate capacitor structure enables the coupling of the electric field to the shear strain, which enables the excitation of a shear mode. Such devices were successfully applied for selective sensing of organic species, such as DNA molecules, suspended in a liquid. Even if the process of deposition of c-axis inclined AlN films doesn't require hardware modification, the quality of the process is still far from the one for deposition of (0001)AlN films used in telecommunications. So the goal of this thesis was to find a solution for the shear mode TFBAR's based on (0001)AlN films. In (0001)AlN films, the shear strain cannot be induced by the electric field produced in a parallel plate geometry as the coefficient e35 and e34 of the piezoelectric tensor are zero. But there are e15 and e24 coefficients that are not zero, meaning that in-plane electric field can be used to excite the shear waves. In the frame of this work, this concept was studied theoretically and experimentally. The in-plane electric field was generated via inter-digitated electrodes (IDE). A first device type was realized in solidly mounted resonator (SMR) design and based on uniform (0001)- oriented AlN thin films. The anti-phase of the electric field in adjacent half-periods of the IDE resulted in an anti-phase movement of the corresponding regions of the film. Finite element modeling and boundary element modeling (FEM-BEM) were carried out to clarify the kind of vibrations present in the device. A kind of shear/lingitudinal mode with elliptic motions was obtained. A device was fabricated and tested both in liquid and air. The resonance of the device was observed in the expected frequency range (1.86 GHz) and high quality factors under operations in air (Q=870) and silicon oil (Q=270) were obtained. The drop of the quality factor was explained by the up and down motion of the regions of the film located directly under the IDE electrodes. Such a motion is due to anti-phase motion of different regions of the film as mentioned above. To prevent this effect, a second device type was studied. It is again based on the use of (0001)AlN thin films, but with modulated piezoelectric properties. Having different piezoelectric properties in the regions corresponding to adjacent half-periods of IDE, breaks the mirror symmetry of the device and allows for coupling the electric field to a pure shear mode. Analytical and numerical models explaining such a device were established and evaluated. The optimal situation is found when perfect Al-polar and N-polar regions of AlN are combined. This maximizes the coupling coefficient k that is derived as being proportional to the difference of e15 coefficients. Finding a way to fabricate the AlN thin film with different piezoelectric properties was thus the next objective. Growth features to decrease the piezoelectric effect were first studied. Providing rougher regions on the otherwise smooth substrate allowed to modify locally the quality of AlN thin films. Device based on such films were fabricated and characterized. The resonance of a pure shear mode was found at the expected frequency (roughly 2GHz) when the piezoelectric effect was modulated. Devices without this modulation failed to show the resonance at the exact frequency, exactly as the theory predicted. We managed to reduce two times the d33 coefficient of the film by inducing a increased roughness to the substrate – from 5.0 pm/V, corresponding to 1.5 degree rocking curve, down to 2.4pm/V, corresponding to 7 degree of rocking curve. The final step of the thesis was the process development for the simultaneous growth of Al-polar and N-polar regions within sputter deposited (0001)AlN, in order to achieve the maximal possible "piezomodulation" effect. As the sputter deposition yielded only N-polar films, we included Al-polar films from another source as seed layers. High temperature epitaxial growth methods of GaN and AlN on Si(111) and Si(100) lead to Ga- and Al-polarities. On such films, the sputter deposited AlN copies polarity from the growth substrate. The selective polarity was then obtained by preventing the expitaxy locally through a patterned oxide layer. Wet etching tests together with PFM measurements were performed to prove the dual polarity in the sputter deposited film. Finally, the integration of this process into the process flow for device fabrication was investigated.

AIN Thin Film Structures for High-Q Resonators

Alvaro Artieda

The development of wireless and mobile communication in the last decade led to the elaboration of new components based on thin films with continually increasing performance and reduced fabrication cost. A fundamental element for mobile communication is the passband filter defining the total bandwidth, the so-called RF filter. Thanks to outstanding characteristics, thin film bulk acoustic wave resonators (TFBAR's) based on piezoelectric AlN thin films have conquered parts of this market against surface acoustic wave devices based on piezoelectric crystals. AlN is today the most favoured material for such these devices, thanks to its excellent electro-acoustic properties. This thesis explores paths for a new type of application in oscillators for time and frequency control in frequency range of several GHz. In portable applications, this domain is largely dominated by quartz crystals. Their resonance frequency – typically around 33 kHz – is multiplied to reach higher frequency domains. For such applications, the main issues are high quality factors and temperature stability of the resonators. This exploration implied two research directions, the first focused on AlN thin film property-process relationships for films grown on amorphous substrates, and the second on the property-design relations of such new devices. High quality factors and temperature stability are key issues in oscillator applications. We proposed to apply symmetric composite resonators (composite TFBAR) including two amorphous SiO2 thin films sandwiching high quality piezoelectric thin films of AlN. This required the growth of AlN on amorphous and insulating surfaces. We thus studied the growth of AlN on such substrates to evaluate the impact on film microstructure and morphology, mechanical stress, quality of orientation, piezoelectric constant d33,f , and polarization uniformity. Substrate roughness and substrate bias power (voltage) were identified as crucial growth parameters. In parallel, we also optimized Mo-electrode thin films for optimal AlN/Mo thin film structures. This was necessary to derive properties from pure AlN TFBAR's, and to produce HBAR's for comparison with our composite BAR's. The impact of the general device design, comprising active area surface, apodization and lateral edge design, was investigated concerning the Q-factor, kt2 and parasitic behaviour of devices. The important role of excitation of parasitic resonances was highlighted. We could show that also the microstructure of AlN plays a key role in their excitation and propagation. AlN exhibits a polar structure with one polar axis (c-axis). The growth process has to provide mechanisms to align the polar axis of all grains. No reorientation is possible by external means. The stability of the piezoelectric AlN layer with applied electric field guarantees a linear response for sensors and actuators. The high stiffness, combined with low density leads to a high longitudinal acoustic velocity of AlN, thus enabling the use of very high application frequencies. Almost all the reports so far have concentrated on depositing AlN on metallic layers, such as Mo, or Pt. The ability to grow high quality AlN thin film on amorphous substrates increases the possibility of developing new devices and applications. The orientation and stress properties, as well as the piezoelectric constant and the polarization of polycrystalline AlN thin films deposited on amorphous substrates, were investigated. Thin sputtered amorphous silicon layers of defined nanoscale roughness were assessed for their ability to manipulate the mechanical stress in AlN thin films that need to be grown on thermal oxide. With a roughness variation from 1 to 11 Å in the Si film, a stress variation from -700 to +200 MPa was observed in the AlN film, which shows the high impact of substrate roughness on the stress in AlN films. The rocking curve width of the 1.2 µm AlN deposited on the Si layers showed a pronounced, linear increase as a function of Si layer roughness. Low density grain boundaries appeared, and the overall stress changed to positive values. A study of the piezoelectricity and the grain polarity of AlN thin films grown on amorphous SiO2 thin films has been done. d33,f of 5.0 pm/V were achieved at low substrate roughness and low mechanical AlN film stress. This value is comparable to values reached on oriented Pt. Increasing substrate roughness and stress leads to a deterioration of d33,f which is correlated with a higher density of opposite polarity grains detected by piezoresponse force microscopy (PFM). Extrapolating to 100% uniform polarity, a maximum d33,f value of 6.1 pm/V is derived. High-Q, bulk acoustic wave composite resonators based on a symmetric layer sequence of SiO2-AlN-SiO2 sandwiched between electrodes have been developed. The SiO2 film thickness was varied while the piezoelectric AlN film had a constant thickness of 1.2 µm. Experimental results of quality factors (Q) and coupling coefficients (kt2) are in agreement with finite element calculations. Q-factors of about 2000 were observed for the first harmonic of the 310 nm oxide devices. Third harmonic resonances were very intense for devices with 770 nm oxide double layers. The temperature drift reveals the impact of the SiO2 layers, which is more pronounced on the first harmonic, reducing the TCF to about 0 ppm/K. Hybrid harmonic bulk acoustic resonators (HBAR) based on an AlN/Si structure were fabricated. In order to increase the coupling kt2 of the simple device, an additional film of AlN was deposited on the top of the HBAR to optimize the excitation energy localization in the stack. The gain of the coupling was more than a factor of 2. A general study of the TFBAR performance is given in this work. The performance of circular, polygonal and elliptical electrodes were compared according to the area. The figure of merit Q · kt2 is higher in the case of elliptical design electrodes in comparison with others. Due to its high acoustic impedance and low electrical resistivity molybdenum is the best electrode material used in this work. The use of the lateral edge design on symmetric SiO2-AlN-SiO2 composite resonators slightly reduces the strength of spurious resonances of the third harmonic, but decreases the Q-factor of the resonances. This composite design has the advantage of attenuating the spurious resonances. In order to study the impact of the microstructure of AlN films on electroacoustic properties of TFBARs, simple Mo-AlN-Mo devices with different values of AlN in-plane stress (from -500 MPa to +500 MPa) were developed. These devices showed a clear correlation between the stress and the intensity of the spurious resonances, devices with tensile stressed AlN films reached Q-factors of about 1800. The impact of the microstructure on the transmission of in-plane acoustic waves is responsible for this phenomena. Voided grain boundaries, that are correlated with tensile films, reduce this transmission. These devices showed that the use of amorphous SiO2 thin films in the stack of resonators increased the Q-factor and the figure of merit Q · f to (∼8.0 ·1012 Hz), which is close to the ultimate value of Quartz (∼1.6·1013 Hz). The reached value compares also well with a novel improved HBAR structure reaching a Q · f of (∼2.7·1012 Hz). The composite resonator in addition exhibits a much higher coupling coefficient, which facilitates the implementation of the electronics. The admittance curves of the composite resonators could be well simulated by combining finite element modelling with simple circuits including parasitic elements. The derived materials quality factors of SiO2 and for the Al/AlN/Pt stack amounted to 50'000 and 3'000, respectively. Finally, composite resonators working at 3.4 GHz, corresponding to the half ground state hyperfine separation of rubidium atoms, were developed. The Q-factor was equal to 2300 and the TCF equal to 1.5 ppm/K. A figure of merit Q · f of ∼0.8 ·1013 Hz and a kt2 of 1% were reached. This device will be implemented in an oscillator as planned to realize an atomic clock control circuit.

EPFL2010

Piezoelectric thin films for bulk acoustic wave resonator applications

Roman Lanz

Bandpass filters for microwave frequencies realized with thin film bulk acoustic wave resonators (FBAR) are a promising alternative to current dielectric or surface acoustic wave filters for use in mobile telecommunication applications. With equivalent performance, FBAR filters are significantly smaller than dielectric filters and allow for a larger power operation than SAW filters. In addition, FBARs offer the possibility of on-chip integration, which will result in substantial volume and cost reduction. The first passive FBAR devices are now appearing on the market. They mainly cover needs in miniaturized RF-filters for the new bands around 2 GHz. A FBAR is essentially a thin piezoelectric plate sandwiched between two electrodes and acoustically isolated from the environment for energy trapping purposes. If the isolation is effectuated by an acoustic Bragg reflector, one speaks of solidly mounted resonators (SMR). Piezoelectric aluminum nitride (AlN) thin films are predominantly used in the emerging FBAR technology because AlN exhibits a sufficient electromechanical coupling coefficient kt2 , low acoustic losses at microwave frequencies, a low temperature coefficient of frequency, and its chemical composition is compatible with CMOS requirements. This thesis has two research directions. In the first part, FBAR structures based on AlN thin films were investigated for applications at X-band frequencies (7.2-8.5 GHz), i.e. operating at much higher frequencies than the ones used for present products. The goal was to identify property limitations related to such high frequencies, and to demonstrate to industry high performing SMR filters at 8 GHz. In the second part, a new material for FBAR devices was studied. The motivation is that AlN allows for a restricted filter bandwidth only, limited by its coupling factor of maximal 7%. Monocrystalline KNbO3 appears as an ideal alternative with its high coupling factor kt2 of 47%, and relatively large sound velocity of 8125m/s for longitudinal waves along the [101] direction. Piezoelectricity of KNbO3 films grown on electrodes has never been characterized. Single crystal results indicate that the optimal film texture would be (101). In this thesis, the growth of KNbO3 films on Pt electrodes was studied with the goal to achieve this texture uniformly, and to characterize piezoelectric properties. X-band FBAR's were first studied with numerical simulations based on a one-dimensional theory of the thickness-extensional bulk acoustic wave (BAW). Thickness, acoustic properties and electrical conductivity of the electrodes have a large impact on the resonator characteristics. There are conflicting requirements with respect to optimum acoustic and electrical properties of the electrode materials. An optimum thickness was calculated for 8GHz FBARs that use Pt bottom and Al top electrodes. The characteristics of ladder filters have been calculated based on the impedances of single resonators. The adjustable filter parameters, i.e. the areas of series and shunt resonators, frequency de-tuning between series and parallel resonators, and number of π-sections were screened for a process window offering maximum filter bandwidth with lowest ripple and low insertion loss for a given out-of-band rejection. An important result of the numerical simulations was that the bandwidth of ladder filters can be doubled by de-tuning the series and parallel resonators by more (1.3 times) than the difference of resonance and anti-resonance frequency. This also leads to a flatter passband while keeping the ripples below ±0.2dB. Solidly mounted resonators and filters were fabricated using an acoustic multilayer reflector consisting of AlN and SiO2 λ/4 layers. All films were sputter deposited in a high vacuum sputter cluster system with 4 process chambers. The films were patterned using standard photolithography and dry etching processes. The SMR exhibited a strong and spurious-free resonance at 8GHz with a high quality factor of 360 and electromechanical coupling coefficient of 6.0%. The temperature coefficient of frequency was -18ppm/K, and the voltage coefficient of frequency was -72ppm/V. Passband ladder filters with T- and π-topology consisting of 3 to 14 SMR were successfully demonstrated with a center frequency of 8GHz. These filters were optimized for maximum bandwidth and exhibited an insertion loss of 5.5dB, a rejection of 32dB, a 0.2dB bandwidth of 99MHz (1.3%), and a 3dB bandwidth of 224MHz (2.9%). There was good correspondence between measured and simulated filter and resonator characteristics. For perfect agreement, parasitic elements needed to be taken into account. These were a series resistance of 5Ω and a parallel conductance of 2mS in case of single resonators. The series resistance can be explained with resistive losses in the electrodes, whereas the parallel conduction was due to conduction along the surface. For π-filters, an additional series inductance of 100pH was needed to obtain a satisfactory fit. This inductance increased the out-of band rejection and insertion loss. Besides the group delay variation, all industrial specifications were met. KNbO3 was in-situ sputter deposited at 500 to 600°C using a rf magnetron source. A dedicated sputter chamber with load-lock and oxygen resistant substrate heater was built for this purpose. The high volatility of potassium oxide requires a potassium enrichment of the target. Targets with several excess concentrations (in the form of K2CO3) were studied. Stoichiometric KNbO3 films were obtained with targets containing 25 and 40% excess K. Zero and 10% excess yielded K deficient films, whereas 100% and 200% excess K led to highly unstable targets with K accumulation on the target surface, resulting in K rich second phases. The potassium-to-niobium ratio in the films depends strongly on sputter pressure and substrate temperature. Dense films, nucleated with cubic {100} texture, were obtained on platinized silicon substrates with a 10nm thick IrO2 seed layer at substrate temperatures of 520°C. At lower temperatures the films were amorphous, and at higher temperatures the films were composed of individual and facetted KNbO3 grains. The cubic high-temperature {100} texture results in a mixed (101)/(010) texture in the orthorhombic room temperature phase. The measured relative permitivity of 420 indicates that both orientations are equally present. Micro-Raman confirms the orthorhombic line splitting. Piezoelectrical and ferroelectrical activity were verified by means of a piezoelectric sensitive atomic force microscope. A very large piezoelectric activity was observed on some of the grains, and the polarization could be switched on most of the grains. However, the average d33,f = e33/c33, as measured by means of laser interferometry, showed a modest value of 24pm/V. The effective coupling factor is derived as kt2=2.8%, which is small relative to the theoretical value of 47%. The high dielectric constant and the absence of piezoelectric activity along the [010] direction are responsible for the reduction of the kt2 factor. Film roughness, complexity of deposition process and open poling issue make KNbO3 integration into BAW devices a difficult task.

EPFL2004

Micromachined tunable devices based on silicon integrated BaxSr1-xTiO3 thin films

Andreas Nöth

Thin Film Bulk Acoustic Wave Resonators (TFBARs) had been developed a decade ago and since then were implemented extensively in mobile communications devices. The "heart" of a TFBAR consists of a piezoelectric film that operates as an acousto-electric transducer, stabilizing the transmission at a given predetermined frequency. For reasons such as space economy in hand-held devices, it is of interest to make these TFBARs tunable, so that a single TFBAR is multi-band responsive. This thesis demonstrates for the first time electrically tunable, single-component TFBARs. A theory describing the tuning behavior of dc bias induced acoustic resonances was developed. Then we made the hypothesis that dc bias induced piezoelectric BaxSr1-xTiO3 (BST) thin films – namely, paraelectric, non-piezoelectric films operating under dc bias – can be used to make electrically tunable TFBARs and that the devices can be switched on or off depending on the dc bias state. The devices were then fabricated: We integrated BST lms onto silicon substrates, micromachined the substrate to create the TFBARs and a new type of suspended planar capacitor which were then characterized, analyzed, and modeled, demonstrating successfully the new concept: We developed a theory describing the electrical tuning behavior of the dc bias induced acoustic resonances in paraelectric thin lms in terms of material parameters. The field dependent constitutive piezoelectric equations were derived from the Landau free energy P-expansion by taking the linear and nonlinear electrostrictive terms as well as the background permittivity into account. We considered two modes of excitation for the tuning of the acoustic resonances, namely the thickness excitation (TE) mode and the lateral field excitation (LFE) mode. The tuning behavior of the two types of resonators based on BST thin films was modeled and discussed. For the modeling we calculated the relevant tensor components controlling the tuning of the BST resonators from the available literature data. The fabrication of the membrane-type TFBARs was realized by integrating BST thin films onto silicon substrates and using micromaching technologies. We showed that the developed TFBARs can be switched on or off with a dc bias. At a dc electric field of 615 kV/cm we observed a tuning of -2.4% (-66 MHz) and -0.6% (-16 MHz) for the resonance and antiresonance frequencies of the device, while the resonance frequency at a dc electric field extrapolated to 0 kV/cm was 2.85 GHz. The effective electromechanical coupling factor k2eff of the device increased up to 4.4%. The tuning was non-hysteretic. The Quality-factor (Q-factor) of the device was about 200. The developed micromaching processes for the TFBARs were used to fabricate coplanar BST capacitors on silicon. Micromaching was used to remove the Si substrate under the active area of the device. Comparing this new micromachined coplanar capacitor with conventional non-micromachined capacitors, we demonstrated that the removal of the substrate from the active device area resulted in a reduction of parasitic effects. The micromachined coplanar capacitor showed an increased tunability and a reduced loss tangent in comparison to the non-micromachined capacitor. The micromachined capacitor showed a relative tunability of 37% at a dc electric field of 1100 kV/cm. The loss tangent was 0.08 and 0.06 at zero and maximum dc bias, respectively, at a measurement frequency of 20 GHz. The integration of epitaxial BST thin films on silicon was studied as well because of its potential improvement of the device performance in comparison to devices based on polycrystalline films. Two different electrode/buffer layer systems, YBa2Cu3O7-x (YBCO) / CeO2 / YxZr1-xO2-x/2 (YSZ) and TiN were used for the integration. Epitaxial BST thin films were grown with both structures. For the BST / YBCO / CeO2 / YSZ / Si structure, the BST unit cell was rotated by 45° in the in-plane dimension with respect to the substrate. The BST layer exhibited good structural quality as indicated by a Full Width at Half Maximum (FWHM) of 0.5° of the rocking curve of the BST(002) diffraction peak. For the BST / TiN / Si structure, the BST layer was grown with a cube-on-cube epitaxial relationship on the silicon substrate, thus demonstrating epitaxially grown BST on silicon using conventional bottom electrode that is easily acceptable by the microelectronic industry. However, in this case, the structural quality of the BST layer was reduced in comparison to the BST / YBCO / CeO2 / YSZ / Si structure. The FWHM of the rocking curve of the BST(002) diffraction peak was 2.2°. We established the temperature (T=550 to 600 °C) and pressure (p ≈ 10-7 to 5 × 10-4 Torr) conditions for the growth of epitaxial BST thin films on TiN-buffered Si. At too high temperatures and/or oxygen pressures epitaxial BST thin film growth was impeded due to the oxidation of the TiN layer. By introducing experimental results from the electrical characterization of the micromachined devices with the polycrystalline BST into our developed theory, we could successfully model the tuning behavior of our fabricated TFBARs. The modeling allowed us to de-embed the intrinsic electromechanical properties of a freestanding BST layer. The effect of increasing mechanical load on the tuning performance of the device was modeled and studied experimentally. Under strong mechanical load, the tuning of both resonance and antiresonance frequency was reduced. The effect was attributed to a reduction in the tuning of k2eff of the device and of the sound velocity of the BST layer.

EPFL2009