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Versatile Visual Logic Operations Based on Plasmonic Switching in Label-Free Molybdenum Oxide Nanomaterials Wei Huang, Yan Zhou, Jiayan Du, Yuequan Deng, and Yi He Anal. Chem., Just Accepted Manuscript • DOI: 10.1021/acs.analchem.7b05097 • Publication Date (Web): 31 Dec 2017 Downloaded from http://pubs.acs.org on January 1, 2018

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XOR

NaBH4 AA

NaBH4 NaClO

OR

INH

MoO3

AA BR (pH 2.0)

AND

MoO3

Reduction

Oxidation HNO3 NaOH

Na2S

SnCl2

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Analytical Chemistry

XNOR

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Plasmonic MoO3-x H 2O 2 NaClO

Cu2+ H2O2

NOR

Na2S

NAND

MoO3-x MoO3

MoO3-x

BR (pH 2.0)

1:2 demultiplexer

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Analytical Chemistry 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Versatile Visual Logic Operations Based

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on Plasmonic

Switching in Label-Free Molybdenum Oxide Nanomaterials

Wei Huang a, Yan Zhoub, Jiayan Du a, Yuequan Denga, Yi He* b

a School of Materials Science and Engineering, Southwest University of Science and Technology, Mianyang, 621010, P. R. China. b School of National Defence Science & Technology, Southwest University of Science and Technology, Mianyang, 621010, P. R. China. *Corresponding author: Dr. Yi He, Tel: +86-816-6089885, Fax: +86-816-6089889, Email: [email protected].


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ABSTRACT Despite some visual colorimetric chemical logic gates have been reported, a complete set of six basic logic gates have not been realized to date. Moreover, the application of the reported logic gates needs to be further extended. Herein, the label-free molybdenum oxide nanomaterials are presented for the construction of a new visual colorimetric molecular computing system. A complete set of six basic colorimetric logic gates (OR, AND, NOR, NAND, XOR, XNOR) and the INH logic gate are realized based on plasmonic switching in MoO3 nanomaterials. In addition, the rational integration of different logic gates into a 1:2 demultiplexer circuit is also testified.

KEYWORDS: Logic gate, demultiplexer, label-free, MoO3 nanomaterials



INTRODUCTION Molecular computing has emerged as an alternative to traditional silicon-based computer technologies for information processing1. It is capable of performing Boolean functions by using basic molecular logic gates, which has a wide variety of applications, such as chemical/biological sensing, intelligent imaging, memory devices, microfluidics, drug delivery, and protein activity regulation2-9. Molecular logic gates, as the basic building blocks of complex computing systems, have been constructed based on biomacromolecules (e.g. DNA, RNA, enzyme), small organic molecules, stimuli-responsive polymers, and nanoparticles10-18. The assembly of multiple basic logic gates that responses to multiple types of inputs is able to perform advanced logic operations such as multiplexers, demultiplexers, keypad lock, half adders, and half subtractors19. The visual colorimetric logic operation systems are particularly attractive because of their low-cost, rapid response, and visual readout. Traditional plasmonic nanoparticles including gold nanoparticles (AuNPs) and silver nanoparticles (AgNPs) have been widely used for development of various molecular logic gates thanks to their higher absorption extinction coefficient than that of organic dyes20. Although various colorimetric logic gates have been constructed21,22, some great limitations and challenges still remain. For example, AuNPs and AgNPs can not be directly used to perform logic operations, which need to be labeled by other molecules such as DNA, spiropyran, and poly(2-alkyl-2-oxazoline)21,23,24. In addition, only limited logic gates have been developed, while a complete set of six elementary logic gates, including OR, AND, NOR, NAND, XOR, and XNOR, have not been realized up to date. Moreover, the relatively complex colorimetric logic operations such as demultiplexer is not reported as well because it is difficult to connect different logic gates. Recently, two-dimensional molybdenum oxide (MoO3) nanomaterials also show the surface plasmon resonance (SPR) after introduction of lattice vacancies or aliovalent heteroatoms owing to the increase in free charge carrier concentrations25-27. Unlike traditional plasmonic nanoparticles, the SPR of MoO3 nanomaterials is capable ACS Paragon Plus Environment

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of being tailored according to changing dopant concentrations. Meanwhile, this plasmonic property is highly reversible and switchable, which is able to response to the external stimuli, such as pH and oxidants28. These factors make this nanomaterial a good candidate for use in molecular computing without any labeling. Herein, we utilize the label-free MoO3 nanomaterials as the signal transducer to construct molecular computing system. Various reducing agents are demonstrated to transform colorless MoO3 nanosheets to blue plasmonic MoO3-x nanomaterials with oxygen vacancies. Simultaneously, the plasmonic MoO3-x nanomaterials are in a position to turn to MoO3 nanomaterials again. Based on the plasmonic switching, a complete set of six basic logic gates (OR, AND, NOR, NAND, XOR, and NXOR) and the INH logic gate are established using the same threshold. Besides, an advanced logic operation (1:2 demultiplexer) is performed as well.

EXPERIMENTAL SECTION Chemicals and Apparatus α-MoO3 powder, tin(II) chloride dehydrate (SnCl2·2H2O) were purchased from Sangon Biotech (Shanghai) Co., Ltd.. L-ascorbic acid (AA), hydrogen peroxide (H2O2), sodium borohydride (NaBH4), sodium hypochlorite solution (NaClO), sodium sulfide nonahydrate (Na2S·9H2O), copper(II) sulfate petahydrate (CuSO4·5H2O), acetonitrile (CH3CN), ethanol (EtOH), acetic acid (HAc), phosphoric acid (H3PO4), and boric acid (H3BO3) were obtained from ChengDu KeLong Chemical Co., Ltd.. All the materials were of analytical grade and used as received. Britton-Robinson (BR) buffer was prepared by dissolving NaOH and mixtures of acids containing H3PO4, H3BO3, and HAc in deionized water, and the real pH of BR buffer was measured with a pH meter. Ultraviolet-visible (UV-vis) absorption spectra of each sample were recorded on a UV-vis spectrophotometer (UV-1800, Shimadzu, Japan). Atomic force microscope (AFM) images were collected using a SPA300HV scanning probe microscopy. Preparation of MoO3 nanosheets. MoO3 nanosheets were synthesized by the reported method with a slight modification29. Briefly, 0.2 g bulk α-MoO3 powder is firstly grinded with 0.2 mL acetonitrile for 15 min. Subsequently, the powder is



dispersed in a mixture of water and ethanol (25 mL, v/v=1), followed by ultra-sonication for 120 min (100 W). After that, the dispersion is centrifuged at 3,000 r.p.m, and the supernatant is collected. Preparation of plasmonic MoO3-x nanodots. MoO3-x nanodots are prepared by direct reduction of MoO3 nanosheets by NaBH4. Briefly, 25 mL MoO3 nanosheet dispersion are mixed with 10 mL NaBH4 solution (10 mM), followed by reaction for 30 min at room temperature, during which a distinct color change from colorless to blue appears. The obtained MoO3-x nanodots are stored at 4°C before use. Experimental procedure for AND, OR, XOR, INH logic gate and 1:2 demultiplexer based on MoO3 nanosheets. AND logic gate. Four glass vials each contained 0.6 mL MoO3 nanosheet dispersion (0.9 mM) and then mixed with four possible input combinations for 30 min: 1.2 mL H2O (0 0); 0.5 mL BR buffer (pH 2.0) and 0.7 mL H2O (1 0); 0.5 mL H2O and 0.7 mL 1 mM AA (0 1); 0.5 mL BR buffer (pH 2.0) and 0.7 mL 1 mM AA (1 1). After that, the UV-vis absorption spectra of each vial were recorded. OR logic gate. Four glass vials each contained 0.6 mL MoO3 nanosheet dispersion (0.9 mM) and then mixed with four possible input combinations for 30 min: 1 mL H2O (0 0); 0.7 mL 1 mM AA and 0.3 mL H2O (1 0); 0.7 mL H2O and 0.3 mL 1 mM NaBH4 (0 1); 0.7 mL 1 mM AA and 0.3 mL 1 mM NaBH4 (1 1). Afterwards, the UV-vis absorption spectra of each vial were gathered. XOR logic gate. Four glass vials each contained 0.6 mL MoO3 nanosheet dispersion (0.9 mM) and then mixed with four possible input combinations for 30 min: 0.4 ml H2O (0 0); 0.2 mL H2O and 0.2 mL 10 mM Na2S (0 1); 0.2 mL 10 mM SnCl2 and 0.2 mL H2O (1 0); 0.2 mL 10 mM SnCl2 and 0.2 mL 10 mM Na2S (1 1). Afterwards, the UV-vis absorption spectra of each vial were collected. INH logic gate. Four glass vials each contained 0.6 mL MoO3 nanosheet dispersion (0.9 mM) and then mixed with four possible input combinations for 30 min: 0.45 mL of H2O (0 0); 0.3 mL H2O and 0.15 mL 10 mM NaClO (0 1); 0.3 mL 1 mM NaBH4 and 0.15 mL H2O (1 0); 0.3 mL 1 mM NaBH4 and 0.15 mL 10 mM NaClO (1 1). Subsequently, the UV-vis absorption spectra of each vial were recorded. ACS Paragon Plus Environment

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1:2 Demultiplexer. Four glass vials each contained 0.6 mL MoO3 nanosheet dispersion (0.9 mM) and then mixed with four possible input combinations for 30 min: 0.7 ml of H2O (0 0); 0.5 mL H2O and 0.2 mL 10 mM Na2S (0 1); 0.5 mL of BR buffer (pH 2.0) and 0.2 mL of H2O (1 0); 0.5 mL of BR buffer (pH 2.0) and 0.2 mL 10 mM Na2S (1 1). Afterwards, the UV-vis absorption spectra of each vial were recorded. Experimental procedure for NOR, NAND and XNOR logic gate based on MoO3-x nanodots NOR logic gate. Four glass vials each contained 0.3 mL MoO3-x nanodot dispersion and then mixed with four possible input combinations for 30 min: 0.75 mL H2O (0 0); 0.6 mL H2O and 0.15 mL 10 mM NaClO (0 1); 0.6 mL 10 mM H2O2 and 0.15 mL H2O (1 0); 0.6 mL 10 mM H2O2 and 0.15 mL 10 mM NaClO (1 1). Subsequently, the UV-vis absorption spectra of each vial were recorded. NAND logic gate. Four glass vials each contained 0.3 mL MoO3-x nanodot dispersion and then mixed with four possible input combinations for 30 min: 0.65 mL H2O (0 0); 0.15 mL 10 mM H2O2 and 0.5 mL H2O (1 0); 0.15 mL H2O and 0.5 mL 1 mM CuSO4 (0 1); 0.15 mL 10 mM H2O2 and 0.5 mL 1 mM CuSO4 (1 1). Then, the UV-vis absorption spectra of each vial were collected. XNOR logic gate. Four glass vials each contained 0.3 mL MoO3-x nanodot dispersion and then mixed with four possible input combinations for 30 min: 0.6 ml H2O (0 0); 0.3 mL 1 M HNO3 and 0.3 ml H2O (1 0); 0.3 ml H2O and 0.3 mL 1 M NaOH (0 1); 0.3 mL 1 M HNO3 and 0.3 ml 1 M NaOH (1 1). After that, the measurement of UV-vis absorption spectra of each vial was carried out.

RESULTS AND DISCUSSION Characterization of MoO3 nanosheets and MoO3-x nanodots. The MoO3 nanosheets are prepared by ultrasonic exfoliation of MoO3 powders29. Figure S1A shows the typical AFM image of the obtained MoO3 nanosheets with micrometer lateral dimensions, which possess a thickness of ~1.2 nm, suggesting that they have a single-layer structure26,30. The MoO3 nanosheets are transparent and absorbs UV light merely (Figure S2A). On the contrary, the addition of NaBH4 to MoO3 nanosheet



dispersion generates a strong UV-vis absorption in the visible and NIR region with a peak at 760 nm, demonstrating the formation of plasmonic MoO3-x nanomaterials (Figure S2B)31. As shown in Figure S1B, the resulted MoO3-x nanodots show a small lateral dimension (40 nm), indicating that a chemical etching process occurs. The plasmonic property is originating the oxygen vacancies which are from the deoxidation of MoO3 nanosheet during the reduction process28. The Mo6+ ions in MoO3 nanosheet is partially reduced by NaBH4, and some oxygen react with hydrogen ion to produce water, therefore producing oxygen vacancies in MoO3. Construction of OR, AND, XOR, and INH logic gates based on MoO3 nanosheets. We find that some common reducing agents such as AA, SnCl2 and Na2S apart from NaBH4 can also reduce MoO3 nanosheets to generate MoO3-x nanodots because the protons in solution are propitious to generate water and oxygen vacancies during the reduction process, accompanying a color change from colorless to blue (Figure 1A). Based on the transformation of MoO3 nanosheets into plasmonc MoO3-x nanodots induced by reducing agents, we constructed a series of logic gates containing OR, AND, XOR and INH (Figure 1 and Figure S3). The OR logic gate is fabricated using NaBH4 and acidic AA solution as the two input signals. The absorbance at 760 nm of 0.05 is defined as the threshold level for all the logic gates. As shown in Figure 1B, either (0 1, 1 0) or both input signals (1 1) cause produce a strong absorption output (1).


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Figure 1. (A) Schematic representation, UV-vis absorption spectra, bar chart presentation, optical image of MoO3 nanosheet dispersion in the (a) absence and presence of (b) NaBH4, (c) AA, (d) Na2S, and (e) SnCl2, respectively. Schematic representation, UV-vis absorption spectra, bar chart presentation, truth table, and output optical image of (B) OR, (C) AND and (D) XOR logic gates based on MoO3 nanosheets. The threshold was set at 0.05.

Figure 1C shows the construction of AND logic gates. The reduction of MoO3 nanosheet by AA is highly dependent on the pH value. The AA and BR buffer (pH 2.0) as the two inputs of the AND logic gate. In the absence of both inputs (0 0) or in the presence of ether input (0 1, 1 0), the output signal can not be observed due to the lack of AA or BR buffer. In the presence of both inputs (1 1), MoO3 nanosheets are reduced to yield MoO3-x nanomaterials effectively, resulting in an apparent absorption and colorless-to-blue change. The XOR logic gate makes use of the incompatibility of two reducing agents (SnCl2 and Na2S) as the input signals. There is an output (strong optical absorption) only if the two inputs are different (0 1, 1 0) because they can react with each other to form SnS precipitation as illustrated in Figure 1D. Also, the INH logic gate is realized by introduction of NaClO which inhibits the reaction ACS Paragon Plus Environment


between NaBH4 and MoO3-x nanosheets. There is an output of 1 only if one input signal is 1 (Figure S3). Fabrication of NAND, NOR and XNOR logic gates based on MoO3-x nanodots. After successfully developing the four visual chemical logic gates (OR, AND, XOR, and INH), other logic gates (NAND, NOR, and XNOR) also have been created based on MoO3-x nanodots (Figure 2). The plasmonic resonance of the MoO3-x nanodots is easily switchable upon oxidation by several oxidants, in which the oxidation reaction decreases the free charge carrier concentrations to below the threshold, leading to the disappearance of the plasmonic resonance28 as shown in Figure 2A. For the NOR logic gate, two oxidants (H2O2 and NaClO) are introduced to oxidize MoO3-x nanodots. As shown in Figure 2B, it has an output signal of 1 only if both input signals are 0.

Figure 2. (A) Schematic representation, UV-vis absorption spectra, bar chart presentation, and optical image of MoO3-x nanodot dispersion in the (a) absence and presence of (b) H2O2, (c) HNO3, and (d) NaClO, respectively. Schematic representation, UV-vis absorption spectra, bar chart presentation, truth table, and output optical image of (B) NOR, (C) XNOR and (D) NAND logic gates based on MoO3-x nanodots. The threshold was set at 0.05. ACS Paragon Plus Environment

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The alkaline environment will promotes the reaction between MoO3-x nanodots and dissolved oxygen32. On the other hand, some oxidizing acids such as HNO3 can simultaneously react with both base and MoO3-x nanodots thanks to both acidic and oxidative properties. Based on these properties, NaOH and HNO3 are chosen as two inputs to develop a XNOR logic gate. There is an output of 0 only if the two inputs are different (Figure 2C). In order to fabricate the NAND logic gate, we decrease the H2O2 concentration as an input signal to below the threshold level which can not react with plasmonic MoO3-x nanodots anymore. The Cu2+ is introduced as another input signal to trigger the decomposition reaction of H2O2 to form hydroxyl radicals with a high oxidation property33,34, which easily oxidize MoO3-x nanodots. It has an output of 0 only if both input signals are 1 (Figure 2D). 1:2 demultiplexer. Next, we demonstrate the integration of the AND and INH logic gates to generate a 1:2 demultiplexer (Figure 3). The plasmonic peak of MoO3-x nanomaterials are dependent on the density of oxygen vacancies. More oxygen vacancies in the nanomaterials will lead to a blueshift of the plasmonic peak because of the increase in free charge carrier concentrations28. Additionally, the reduction capacity of Na2S is sensitive to the pH value, and it has a relatively weak reduction activity in an acidic environment. Thus, Na2S is able to reduce MoO3 nanosheets to generate MoO3-x nanomaterials with distinct two plasmonic peaks under different pH environment. Under this condition, Na2S can be considered as the data input signal, the absorbance values at two peaks are regarded as two output signals, and the BR buffer (pH 2.0) is chosen as addressing input signal, which performs a 1:2 demultiplexer operation. The high and low absorbance values at 440 nm and 880 nm are defined as two outputs, with a threshold of 0.2. As shown in Figure 3, either in the absence of Na2S (data input=0) and BR buffer at pH 2.0 (addressing input=0) or in the absence of Na2S (data input=0) and presence of BR buffer at pH 2.0 (addressing input=1), there is no obvious absorption (output 1=0, output 2=0). However, in the presence of Na2S (data input=1) and in the absence of BR buffer at pH 2.0 (addressing input=0), the computing system shows a strong absorption at 440 nm ACS Paragon Plus Environment


(output 1=1), while the absorbance at 880 nm is approximately zero (output 2=0). In the presence of Na2S (data input=1) and BR buffer at pH 2.0 (addressing input=1), the absorbance at 440 nm is low (output 1=0), while the absorbance at 880 nm is high (output 2=1).

Figure 3. Integration of AND and INH logic gates into a 1:2 demultiplexer for molecular computing. Figure shows the schematic, UV-vis absorption spectra, bar chart presentation, truth table, and output optical image of the 1:2 demultiplexer.

CONCLUSIONS In conclusion, we have successfully designed and developed six basic chemical logic gates (AND, NAND, OR, NOR, XOR, and XNOR) and the INH logic gate based on plasmonic switching in label-free MoO3 nanomaterials. A 1:2 demultiplexer is also constructed by rational integration of the AND and INH logic gates. Compared with the traditional labeled metal nanoparticle-based computing systems, the distinct advantage of this system is that it is label-free, highly switchable, and low-cost, which makes it quite versatile for various logical operations. Taken together, in the light of these advantages, we believe the present logic operations to have a variety of


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applications in molecular computing, sensing, drug delivery, and so forth.

ASSOCIATED CONTENT Supporting Information Figure S1-S3. This material is available free of charge via the Internet at http://pubs.acs.org.

AUTHOR INFORMATION Corresponding Author * Email: [email protected] Notes The authors declare no competing financial interests.

ACKNOWLEDGEMENTS The support of this research by the by the National Natural Science Foundation of China (Grant No. 21705134), Foundation of Science and Technology Department of Sichuan Province (Grant No. 2015JY0053), and Longshan Scholars Programme of Southwest University of Science and Technology (Grant No. 17LZX449) is gratefully acknowledged.

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