Nano Research Nano Res DOI 10.1007/s12274-014-0652-3 Ultra-sensitive graphene strain sensor for sound signal acquisition and recognition Yan Wang1,2#, Tingting Yang2,3#, Junchao Lao1,2, Rujing Zhang3, Yangyang Zhang3, Miao Zhu2,3, Xiao Li2,3, Xiaobei Zang3, Kunlin Wang3, Hu Jin4, Li Wang1, Hongwei Zhu2,3() Nano Res., Just Accepted Manuscript • DOI: 10.1007/s12274-014-0652-3 http://www.thenanoresearch.com on November 24 2014 © Tsinghua University Press 2014 Just Accepted This is a “Just Accepted” manuscript, which has been examined by the peer-review process and has been accepted for publication. A “Just Accepted” manuscript is published online shortly after its acceptance, which is prior to technical editing and formatting and author proofing. Tsinghua University Press (TUP) provides “Just Accepted” as an optional and free service which allows authors to make their results available to the research community as soon as possible after acceptance. After a manuscript has been technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Please note that technical editing may introduce minor changes to the manuscript text and/or graphics which may affect the content, and all legal disclaimers that apply to the journal pertain. In no event shall TUP be held responsible for errors or consequences arising from the use of any information contained in these “Just Accepted” manuscripts. To cite this manuscript please use its Digital Object Identifier (DOI®), which is identical for all formats of publication. 1 Ultra-sensitive graphene strain sensor for sound signal acquisition and recognition Yan Wang1, Tingting Yang2, Junchao Lao1, Rujing Zhang2, Yangyang Zhang2, Miao Zhu2, Xiao Li2, Xiaobei Zang2, Kunlin Wang2, Hu Jin3, Li Wang1, Hongwei Zhu2* 1Nanchang 2Tsinghua 32D University, China University, China Carbon Graphene Material Co., Ltd., China Page Numbers. The font is ArialMT 16 (automatically A wearable and highly sensitive strain sensor was designed from thin films of graphene woven structures for sound signal acquisition and recognition. inserted by the publisher) 1 Nano Res DOI (automatically inserted by the publisher) Research Article Ultra-sensitive graphene strain sensor for sound signal acquisition and recognition Yan Wang1,2#, Tingting Yang2,3#, Junchao Lao1,2, Rujing Zhang3, Yangyang Zhang3, Miao Zhu2,3, Xiao Li2,3, Xiaobei Zang3, Kunlin Wang3, Hu Jin4, Li Wang1, Hongwei Zhu2,3() 1Department of Physics and Institute for Advanced Study, Nanchang University, Nanchang 330031, China 2Center for Nano and Micro Mechanics, Tsinghua University, Beijing 100084, China 3School of Materials Science and Engineering, State Key Laboratory of New Ceramics and Fine Processing, Key Laboratory of Materials Processing Technology of MOE, Tsinghua University, Beijing 100084, China 42D Carbon Graphene Material Co., Ltd., Changzhou, Jiangsu 213149, China #These authors contributed equally to this work Received: day month year / Revised: day month year / Accepted: day month year (automatically inserted by the publisher) © Tsinghua University Press and Springer-Verlag Berlin Heidelberg 2014 ABSTRACT A wearable and highly sensitive sensor for sound signal acquisition and recognition was fabricated from thin films of special crisscross graphene woven structures. When it was stretched, high-density of random cracks in the network appeared, which decreased the current pathway and increased the resistance. Therefore, the film could act as strain sensors on human throat to measure one’s words through the muscle movement no matter a sound was made or not. The ultra-high sensitivity of the sensor could realize fast and low frequency sampling of speech by extracting the signature characteristics of sound waves. In this study, representative signals of 26 English letters, typical Chinese characters and tones, even phrases and sentences, were tested with obvious resistance changes. Furthermore, resistance changes of graphene sensor responded perfectly with sounds. By future combining artificial intelligence with digital signal processing, we expect that this graphene sensor will be able to deal with complex acoustic systems and large quantities of audio data. KEYWORDS Graphene, strain sensors, sound detectors, high sensitivity 1. Introduction mechanical wave of pressure and displacement, Sensing strain and vibration with soft materials in through a medium such as air, water and solids, small scale has attracted increasing attention. Sound and its perception and processing is an integral part is a vibration that propagates as a typically audible of human intelligence. Traditional sound collection ———————————— Address correspondence to Hongwei Zhu, [email protected] 2 and recognition involve the process of taking carbon nanotube (CNT)/polymer composite is samples of an analog sound and storing the results 0.06~0.82 [17], that of traditional metal is 1~5 [18], in storage mediums or as binary data. Human can that of semiconductor is ~100 [19], that of use auditory sensor to receive external sounds CNT-based sensor is ~1000 [20], and that of single through vibration of the spreading air. However, nanowire-based sensor is ~1250 [21]. While the GF when one cannot make voice physically due to of graphene woven fabrics (GWFs) from our some diseases, how could others know what one research group can be as high as 103 with 2-6% wants to say? Therefore, it is necessary to develop a strains, 106 with higher strains (>7%), and ~35 with new device and method to collect and recognize the tiny strain of 0.2%, which are the best up to present communications and enough to measure with a normal digital through some other signals instead of sounding voice. Multimeter. Additionally, due to the high sensitivity, Signals, as well as voice, are characterized as excellent flexibility and no irritation to human real-world’s Voice bodies, the GWFs had been used as stain gauge, the phonological or prosodic features include loudness, key component in many monitoring sensors (finger jitter, fundamental frequency, zero-crossing rate and bending, hand clenching, expression change, breath energy frequency ratios, etc [2]. Normally, audio and pulse monitoring) [8, 22, 23]. the observable output [1]. recorder or computer recording software (like voiceprint) can nearly perfectly collect In this study, we demonstrate one interesting and example of potential applications of graphene recognize the human speech sound through the woven structure in highly sensitive sensing as a greatly reduced spectral information. However, wearable these severely restrict the listener to obtain the full graphene) from chemical vapor deposition (CVD) information according to the distribution of spectral on copper meshes were transferred onto a thin, energy [3]. When someone is difficult to make or biocompatiblly hear a sound, commercial artificial electronic throat polydimethylsiloxane (PDMS) [24, 25] and double [4] and electronic ear [5, 6] can be used to produce sided tape, assembling a highly sensitive GWFs or collect and recognize speech sound. based strain sensor. When some stress was applied acoustic detector. and GWFs elastic (crisscross polymer, e.g., Recently, another type of strain sensor stuck on on the GWFs, high-density and random cracks throat skin could record the muscular movement appeared in the network, leading to the decrease of (see Fig. 1) to collect and recognize speech sound current pathway and the increase of resistance. because different-degreed Because vocalization of human is based on the stretching or shrinking strains with different words muscle movement/vibration and different contents spoken [7, 8]. As a voice recognition sensor in the correspond throat, sensitivity, flexibility, stretchability and compression, a new GWFs sensor has been softness of the sensor are very important [9-12]. In established to monitor throat muscle movements in strain sensors [13-15], the gauge factor (GF) is voice collection and recognition based on the defined as resistance changing with mechanical relationship between GWFs stress and its resistance, deformation to express the sensitivity, and the compared with the traditional method based on relationship between the change of electrical acoustic spectrum. When the assembled sensor is resistance (dR/R) and the variation of mechanical affixed onto throat, GWFs will be stretched or strain (dL/L) is GF=(dR/R)/(dL/L), which means the compressed along with the skin to change the strain sensor is more sensitive with a larger GF resistance value [16]. It has been reported that the GF of Furthermore, because of the excellent electrical throat muscle has to then different to collect muscles the tension voice or signals. 3 performance and high sensitivity of GWFs, every did the same action with a voice or without a voice, English letters, Chinese characters, tone or phrases which could help the patient who has trouble in can readily be distinguished based on their different voicing out. resistance changes and the characteristic peak of In order to achieve better performance in voice each vocalization. Additionally, the low sampling collection and recognition, the strain sensor should point in this study, also simplified the traditional be able to distinguish every letter and the minimum speech recognition. Interestingly, it was found that structural unit of a word. Figure 2 shows test signal the signal waveforms between vocalization and waveforms of all 26 English letters, and the inset is a un-vocalization were nearly overlapped with same real test photograph. As expected, the wave-forms speaking action. are unique and repeatable for all letters. Every 2. Results and Discussion specific letter has its own different amplitude, Fig. 1a shows the key processes to fabricate and duration time and resistivity variation. Since each operate the GWFs strain sensor. During the CVD individual speech organ is different, people can growth of graphene [26], GWFs was formed when a easily distinguish whether the voice comes from the crisscross copper mesh was used [22]. During the same person. Similarly, we tested three females and transferring of GWFs, PDMS was used as an ideal a male speaking the same English letter “A”. As adhesive on double-sided tape due to the flexibility, shown in Fig. S2(a), the key features of the test biocompatibility, chemical signal waveforms were similar. Placing sensors in inertness and stability of PDMS over a wide range the same spot each time on different people with of temperatures [27]. Additionally, the double sided different anatomy got very similar shapes of tape was only 100 μm thick and much thinner than responses for the letter, while same person who the previous medical tape [8], which led more repeats his/her own words generates relatively precise signals to distinguish different words from different patterns and magnitudes. Louder sound the tester. Though the strain sensor device was requires multi-layered, the total thickness is about 200 μm, amplitude of the signal is expected to change. which was thin enough to get ideal signals and Compared decrease attenuation. From the image of an recognition, integrated strain sensor in Fig. 1(c), it could be particularly lower (less data points) than those from found that the wearable device was very thin and sound spectrum, but one could still get the could be bent with excellent flexibility. As shown in characteristic signal waveform of each letter, which Fig. S1, this flexible strain sensor could fit human simplified the sound collection compared with skins very well only with a sizable strain from any other traditional ways. high transparency, direction. In Fig. 1(d) of a scanning electron more muscle with our movement, other methods sampling thus of frequency the sound were After the clearly identification of every English microscopy (SEM) image, the wafers on the stripe letter, surface a different English phrases and sentences was done. polycrystalline structure. If the assembled strain As shown in Fig. 3, the resistance changed sensor was stuck onto a human throat, signals of significantly when a tester said different words or resistance changing could be obtained with the phrases, such as “Graphene”, “Lab of Science”, movement of throat muscle to monitor vocalization, “Strain which is shown in Fig. 1(e). Furthermore and Sensors”. It was also found that each signal curve interestingly, it was found that the nearly same was apparently different and the repeatability was signal waveforms were obtained when the tester very good by contrasting the same word of indicated that the GWF had the voice Sensors” recognition or through “Graphene-based testing Strain 4 “Graphene” in Fig. 3(a) and 3(d) or the same phrase response to loudspeakers that are relying on current of “Strain Sensors” in Fig. 3(c) and 3(d). Some other signal-caused magnetic energy changing. As shown tests on monitoring English sentences are shown in in Fig. 5, some audio experiments with English and Fig. S2(e). The signal proportion obtained from our Chinese music with the GWFs-based sensor on the multiple strain sensors was at least 4% in resistance vibrating membrane of a loudspeaker were done. It change, which was enough to measure with normal was found that GWFs’ collecting signals had a instrument Keithley and even digital Multimeter. synchronous response to audio frequency, and Compared with ZnO (the maximal signal of current could retain almost every characteristic peak. change was about 5 nA or voltage change was about However, the volume of the loudspeaker also 50 mV) [28, 29] and CNTs (the maximal resistance played an important role on the signal strength. As change was about 2%) [17, 30] or molded graphene shown in Fig. S2(d), with a louder loudspeaker film-based sensors (the maximal current change volume, the loudspeaker vibration amplitude was was less 0.8 μA) [7, 31],] our GWFs-based strain larger sensor Comprehensively, same sentence signals could be has absolute predominance in voice recognition in the near future. and then the signal was stronger. obtained with GWFs-based sensor directly on Different from English alphabets or phonetic throat (red) and the loudspeaker (black), compared symbols with differences in monosyllabic and with the original recorded data (inset), and every polysyllabic, basic characteristic peak had been well recorded. monosyllabic Chinese with characters four are pronunciation all tones. As mentioned previously, although the Therefore, it is necessary to identify Chinese sampling frequencies of our GWFs-based strain characters and phrases with our GWFs-based voice sensor were far lower than that from any existing recognition sensors, and the test results are shown recording software, it still could keep every sound’s in Fig. 4. In Fig. 4(a) and 4(b), respectively, the most characteristic peaks very well. Fig. 6 shows the test frequently used Chinese characters of “东”, “西”, data of four typical animal sounds (dog, cow, bird “南”, “北” and Chinese tones of “ā”, “á”, “ǎ”, “à” and horse) and the insets are the original recorded were tested. From the results, a conclusion could be audio data. Compared with the original recorded made that every Chinese character had its own data, each measured signal from our GWFs-based characteristic peak and different Chinese tones had strain sensor had a high degree of consistency. different signals. Generally, signal waveforms of the Additionally, due to the excellent flexibility and third tone often had up and down, and signal high sensitivity, our GWFs-based strain might be amplitudes of the forth tone always were the used in not only the recognition of human sounds, maximum. And another experiment of “前”, “后”, monitoring of acoustic activity of animals, but also “左”, “右” and “ō”, “ó”, “ǒ”, “ò” was done (Fig. various deformations or vibrations monitoring in S-2(b) and S-2(c)) to confirm the reliability of the robotics, fatigue detection, etc. data generated from our GWFs-based voice This work provides an interesting beginning of recognition sensors. As shown in Fig. 4(c) and 4(d), a proof of concept to the ability of the graphene Chinese phrases and sentences could also be sensors to generate different signals for different recognized with our GWFs-based sensitive sensors. tones and words. However, the results still require Because the collected signals for GWFs-based further validation, repetition and cross-validation sensors came from different degrees of stretching or between different subjects as well as an explanation shrinking strain, it is worth to checking whether the regarding the origin of these signals (muscle signals of GWFs-based sensors have the same movement or response to voice vibrations). In 5 addition, signal processing should be done through Copper mesh (100 mesh, woven with wires of 100 mathematical extraction of signal shapes and μm in diameter) was used as the CVD growing features automated substrate. H2 (~50 mL/min) and Ar (300 mL/min) than just was flowed until 1000 oC was reached. Then, CH4 comparison of signal shape. For example, Fast (30 mL/min) was introduced into the reactor while Fourier Transformation (FFT) can be applied to both the flow of H2 was turned down to 5 mL/min and signals and get the Pearson Correlation to extract Ar was stopped to increase the number of graphene features of the given voice signal for comparing two nucleation because the GWFs would more sensitive audio signals to check the audio signal similarity. to deformation with smaller graphene grain. After 2 Utilization of machine learning algorithms on the min, 200 mL/min of Ar was introduced for another extracted features could provide a good proof that 18 min. After GWFs were completely grown around the different signals can indeed be differentiated the copper mesh, GWFs could be obtained after the and identified as letters and words. copper was etched away with FeCl3 and HCl 3. Conclusion aqueous solution. In summary, a flexible and wearable acoustic 4.2 Fabrication of GWFs-based strain sensor detector was assembled by adhering graphene A small amount of PDMS (the weight ratio of base woven elastic to cross linker was 10:1) was spin-coated on a polymer/double-sided tape film. The detector based microns double-sided tape (100 μm in thickness). on strain sensing exhibited ultra-high sensitivity to As-made materials were degassed under vacuum tiny strains/vibrations and could be used as for 20 min to remove bubbles and solidified at 80 oC electronic skin covering human throat to detect for 1 h. A PDMS-double sided tape composite sound waves at low sampling frequencies. The substrate (about 200 μm in thickness) for GWFs was results completed. and mathematical their analysis algorithms, structures showed that using rather on the the graphene sensor After GWFs were transferred to successfully collected and recognized all 26 English PDMS-tape substrate, silver wires were connected letters, some typical Chinese characters, phrases, with silver paste and the multilayer device was and sentences with wearability, excellent flexibility assembled. and high sensitivity. The graphene sensor could 4.3 Custom-made data processing system perfectly retain every signal characteristic of all Surface of the GWFs was observed with an optical peaks, which was highly consistent with that from microscope (Axio Scope A1) and scanning electron the loudspeaker. Furthermore and interestingly, it microscopy (LEO 1530). Audio tests of the strain was found that the nearly same signal waveforms sensors were performed with a computer-controlled were obtained when the tester did the same action loudspeaker. Voice collection and recognition of the with a voice or without a voice, which could help GWFs-based sensor were performed with a digital the patient who has trouble in voicing out. Because meter (Keithley 4200-SCS) with a test step of 5 ms of the excellent flexibility, ultra-high sensitivity, and a Source-Drain voltage of 1V DC. good reversibility, friendly biocompatibility, the GWFs-based sensor might have great potentials in Acknowledgements earthquake monitoring, animal communication, This work was supported by Beijing Science and and robot voice development. Technology Program (D141100000514001), National 4. Materials and Methods 4.1 Preparation of GWFs Science Foundation of China (51372133), and National Program on Key Basic Research Project (2011CB013000, 2014CB932401). 6 S. D.; Wu J.; Won S. 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S.; Riveline D.; Goichberg P.; 8 Figures a CVD Copper mesh Etching Graphene growth Transferring Graphene woven fabric b 200 µm Ag Air vibration Muscular movement c d Ag Graphene woven fabric PDMS Double sided tape e Vocalized Not vocalized (R-R0)/R0 0.2 0.1 0.0 0.0 0.8 1.6 2.4 Time (s) Figure 1 GWFs-on-PDMS strain sensor. (a) Key steps of preparing the graphene strain sensor; (b) Three ways of collecting and recognizing human voices; (c) Photograph of a bent strain sensor; (d) SEM image of GWFs; (e) Signals of vocalization (black) and un-vocalization (red) are nearly overlapped when a tester made the same speech action. 9 0.16 0.20 0.04 0.00 (R-R0)/R0 (R-R0)/R0 (R-R0)/R0 0.08 0.08 0.04 0.5 1.0 1.5 2.0 0.5 1.0 1.5 2.0 2.5 E -0.04 2 3 1.0 1.5 2.0 0 1 2 3 4 Time (s) G 0.16 0.08 0.00 1 0.04 0.04 (R-R0)/R0 (R-R0)/R0 0.00 0 0.5 F 0.24 0.04 0.08 Time (s) 0.32 0.08 0.12 0.00 0.0 Time (s) Time (s) D 0.16 0.00 0.0 2.5 C 0.04 0.00 0.0 (R-R0)/R0 0.08 B 0.12 (R-R0)/R0 A 0.12 0.00 -0.04 0.0 0.5 Time (s) 1.0 1.5 0.0 2.0 0.5 1.0 1.5 2.0 2.5 Time (s) Time (s) 0.16 0.06 0.00 0.10 0.05 0.0 0.5 1.0 0 1 Time (s) 0.24 0.04 0.08 0.04 0.00 0 1 2 0.0 3 0.5 0.20 M 0.12 0.06 1.5 2.0 N 0.15 0.18 1.0 Time (s) Time (s) 0.10 0.05 0.00 0.00 0.00 0.0 0.5 0.0 1.0 0.5 1.0 1.5 2.0 -0.05 2.5 0 Time (s) Time (s) 1 2 Time (s) 0.20 0.24 (R-R0)/R0 0.18 0.12 0.06 Q 0.12 P 0.15 0.10 0.05 R 0.18 (R-R0)/R0 O (R-R0)/R0 0.24 (R-R0)/R0 0.04 -0.04 3 (R-R0)/R0 (R-R0)/R0 (R-R0)/R0 0.08 Time (s) L 0.12 2 K 0.08 0.00 0.00 -0.06 J 0.12 0.15 (R-R0)/R0 (R-R0)/R0 (R-R0)/R0 0.12 I (R-R0)/R0 0.20 H 0.18 0.08 0.04 0.12 0.06 0.00 0.00 0.00 0 1 2 0.00 0 3 1 2 0 3 1 0 1 2 Time (s) Time (s) Time (s) Time (s) 2 0.16 0.08 0.00 (R-R0)/R0 0.16 0.04 0.00 -0.08 0.5 0 Time (s) 0.08 0.04 0.24 0 (R-R0)/R0 0.08 1 2 0.16 X 0.16 0.04 0 Time (s) (R-R0)/R0 W 0.08 0.00 2 Time (s) 0.12 0.00 1 V 0.12 0.12 0.00 1.0 0.06 U 1 2 Time (s) Y Z 0.08 0.12 (R-R0)/R0 0.0 (R-R0)/R0 0.16 T (R-R0)/R0 0.08 S (R-R0)/R0 (R-R0)/R0 0.24 0.08 0.04 0.04 0.00 0.00 -0.06 0 1 0 Time (s) Figure 2 1 Time (s) 0.00 0 1 Time (s) 2 0 1 2 3 Time (s) Recognition of 26 English letters. 10 a 0.12 b “graphene” “lab of science” 0.08 (R-R0)/R0 0.08 (R-R0)/R0 0.12 0.04 0.00 0.04 0.00 -0.04 -0.04 0 1 0 2 1 c 0.08 d “strain sensors” 0.24 “graphene based strain sensors” 0.16 (R-R0)/R0 (R-R0)/R0 0.04 0.00 0.08 0.00 -0.04 0 1 Time (s) Figure 3 2 Time (s) Time (s) 2 0 1 2 3 4 Time (s) Recognition of English words and phrases. Relative resistance changes with throat muscle motions when the tester said (a) “graphene”; (b) “lab of science”; (c) “strain sensors”; and (d) “graphene based strain sensors”. 11 a b 0.08 0.08 à 北 南 (R-R0)/R0 (R-R0)/R0 东 0.04 西 ā á 0.04 0.00 0.00 0 5 10 15 20 25 0 5 10 Time (s) c ǎ 0.18 15 20 25 30 Time (s) d “石墨烯” “石墨烯传感器” 0.08 (R-R0)/R0 (R-R0)/R0 0.12 0.06 0.00 -0.08 0.00 -0.16 0 1 Time (s) Figure 4 2 3 0 1 2 3 4 Time (s) Recognition of Chinese characters, tones, phrases. Relative resistance changes for (a) Chinese characters and (b) tones. Relative resistance changes with throat muscle motions when the tester said (c) “石墨烯” and (d) “石墨烯传感器”. 12 c a 2.0 Music 0.2 (R-R0)/R0 (R-R0)/R0 e 2.5 0.3 0.1 English audio 1.5 1.0 0.5 0.0 0.0 0 b 10 20 Time (s) 30 0 20 Time (s) 30 40 d 0.6 3 0.5 0.4 Chinese audio (R-R0)/R0 (R-R0)/R0 10 0.3 0.2 2 1 0.1 0.0 0 0 10 20 Time (s) Figure 5 30 0 2 4 6 8 10 Time (s) Recognition signals compared with the sounds from the loudspeaker. Relative changes of resistance when the loudspeaker played (a) music; (b) Chinese audio and (c) English audio, respectively; (d) A same sentence tested by the sensors stuck on the throat (red), on the loudspeaker (black). The insets show the original recording data; (e) Photograph of a strain sensor stuck on the vibrating membrane of a loudspeaker. 13 0.6 (R-R0)/R0 0.4 Dog 0.2 b 0.6 (R-R0)/R0 a 0.4 0.0 Cow 0.2 0.0 0 4 8 12 16 0 4 0.06 0.04 d Bird 0.02 0.00 12 16 0.10 Horse 0.05 0.00 0 4 8 12 16 0 Time (s) Figure 6 8 Time (s) (R-R0)/R0 c (R-R0)/R0 Time (s) 4 8 12 Time (s) Recognition of animal sound records. Relative resistance changes when the loudspeaker played sound records of (a) dog, (b) cow, (c) bird and (d) horse, respectively. The insets show the original recording data. 14
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