Nanoelectronic Heterodyne Sensor: A New Electronic Sensing Paradigm
Abstract
Nanoelectronic devices based on nanomaterials such as nanowires, carbon nanotubes, graphene, and other 2D nanomaterials offer extremely large surface-to-volume ratios, high carrier mobility, low power consumption, and high compatibility for integration with modern electronic technologies. These distinct advantages promise great potential for nanoelectronic devices as next generation chemical and biological sensors. Currently, majority of existing nanoelectronic sensors are direct current (DC) sensors, which rely ubiquitously on detection of conductance change associated with molecular adsorption. However, despite the simplicity of the conventional DC sensing technology, it also has severe limitations such as the Debye screening effect in ionic solutions, and the speed-sensitivity trade-off for the detection of charge-neutral molecules. Hence, the development of nanoelectronic sensors calls for new sensing platform technologies that can truly showcase the advantages of electronic sensors. In this Account, we will summarize recent efforts from our group on the development of a new electronic sensing paradigm, the nanoelectronic heterodyne sensors. Unlike conventional charge-detection based sensors, the heterodyne sensor explores the frequency mixing response between molecular dipoles and a nanoscale transistor. As an example, we first discuss the capability of heterodyne sensing in gas sensing applications by using graphene devices. Rapid (down to 0.1 s) and sensitive (down to 1 ppb) detection of a wide range of vapor analytes is achieved, representing orders of magnitude improvement over state-of-the-art nanoelectronic sensors. Furthermore, the heterodyne sensing technique enables electrical probing and tuning of the noncovalent physisorption of polar molecules on graphene surface for the first time. These results provide insight into small molecule-nanomaterial interaction dynamics and signify the ability to electrically tailor interactions, which can lead to rational designs of complex chemical processes for catalysis and drug discovery. Finally, we discuss the application of heterodyne sensing in solution for chemical and biological sensors by using carbon nanotube devices. The fundamental ionic screening effect can be mitigated by operating carbon nanotube field effect transistor as a heterodyne biosensor. Electrical detection of streptavidin binding to biotin in 100 mM buffer solution can be achieved at a frequency beyond 1 MHz. The results should promise a new biosensing platform for point-of-care detection, where biosensors functioning directly in physiologically relevant condition are desired.
Integrity signals
Registry
Cites
Statistics
Claims the paper makes
Claims other papers make about this one
Each is checked against this paper’s own text: does it say what the citing paper says it does?
Kulkarni et al. developed a rapid (down to 0.1 s) and sensitive (down to 1 part per billion) nanoelectric graphene vapor sensor that can continuously monitor a wide range of vapor analytes from breath or the environment.
“Kulkarni et al. developed a rapid (down to 0.1 s) and sensitive (down to 1 part per billion) nanoelectric graphene vapor sensor that can continuously monitor a wide range of vapor analytes (e.g., nitric oxide, oxygen) from breath or the environment to monitor for illness or harmful environmental exposures [150,151].”
From Wearables and the Medical Revolution (2018) · cites this paper as [150]
Cites
Geim, A. K., & Novoselov, K. S. (2007) · Nature Materials · doi:10.1038/nmat1849 · Cited by 39,979 · see citing works
Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
Wang, Q. H., Kalantar-Zadeh, K., Kis, A., Coleman, J. N., & Strano, M. S. (2012) · Nature Nanotechnology · doi:10.1038/nnano.2012.193 · Cited by 16,374 · see citing works
Intermolecular and Surface Forces
Israelachvili, J. N. (2011) · Elsevier eBooks · doi:10.1016/c2009-0-21560-1 · Cited by 8,185 · see citing works
Detection of individual gas molecules adsorbed on graphene
Schedin, F., Geim, A. K., Morozov, S. V., Hill, E. W., Blake, P., Katsnelson, M. I., & Novoselov, K. S. (2007) · Nature Materials · doi:10.1038/nmat1967 · Cited by 8,028 · see citing works
Nanowire Nanosensors for Highly Sensitive and Selective Detection of Biological and Chemical Species
Cui, Y., Wei, Q., Park, H., & Lieber, C. M. (2001) · Science · doi:10.1126/science.1062711 · Cited by 5,799 · see citing works
Electronic transport in two-dimensional graphene
Sarma, S. D., Adam, S., Hwang, E. H., & Rossi, E. (2011) · Reviews of Modern Physics · doi:10.1103/revmodphys.83.407 · Cited by 3,404 · see citing works
Noncovalent sidewall functionalization of single-walled carbon nanotubes for protein immobilization
Chen, R. J., Zhang, Y., Wang, D., & Dai, H. (2001) · Journal of the American Chemical Society · doi:10.1021/ja010172b · Cited by 2,534 · see citing works
Multiplexed electrical detection of cancer markers with nanowire sensor arrays
Zheng, G., Patolsky, F., Cui, Y., Wang, W. U., & Lieber, C. M. (2005) · Nature Biotechnology · doi:10.1038/nbt1138 · Cited by 2,430 · see citing works
Carbon Nanotube Sensors for Gas and Organic Vapor Detection
Li, J., Lu, Y., Qi, Y., Cinke, M., Han, J., & Meyyappan, M. (2003) · Nano Letters · doi:10.1021/nl034220x · Cited by 1,812 · see citing works
Nanoelectronics from the bottom up
Lu, W. D., & Lieber, C. M. (2007) · Nature Materials · doi:10.1038/nmat2028 · Cited by 1,547 · see citing works
Introduction to surface chemistry and catalysis
McKee, C. (1994) · Applied Catalysis A General · doi:10.1016/0926-860x(94)85211-1 · Cited by 1,497 · see citing works
Label-free immunodetection with CMOS-compatible semiconducting nanowires
Stern, E., Klemic, J. F., Routenberg, D. A., Wyrembak, P. N., Turner-Evans, D. B., Hamilton, A. D., LaVan, D. A., Fahmy, T. M., & Reed, M. A. (2007) · Nature · doi:10.1038/nature05498 · Cited by 1,352 · see citing works
A tunable carbon nanotube electromechanical oscillator
Sazonova, V., Yaish, Y., Ustunel, H., et al. (2004) · Nature · doi:10.1038/nature02905 · Cited by 1,317 · see citing works
Electrical detection of single viruses
Patolsky, F., Zheng, G., Hayden, O., Lakadamyali, M., Zhuang, X., & Lieber, C. M. (2004) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0406159101 · Cited by 1,256 · see citing works
Single-walled carbon nanotube electronics
McEuen, P. L., Fuhrer, M. S., & Park, H. (2002) · IEEE Transactions on Nanotechnology · doi:10.1109/tnano.2002.1005429 · Cited by 1,201 · see citing works
Chemical Vapor Sensing with Monolayer MoS 2
Perkins, F. K., Friedman, A. L., Cobas, E. D., Campbell, P. M., Jernigan, G. G., & Jonker, B. T. (2013) · Nano Letters · doi:10.1021/nl3043079 · Cited by 1,142 · see citing works
Phosphorene as a Superior Gas Sensor: Selective Adsorption and Distinct I – V Response
Kou, L., Frauenheim, T., & Chen, C. (2014) · The Journal of Physical Chemistry Letters · doi:10.1021/jz501188k · Cited by 1,056 · see citing works
Intrinsic Response of Graphene Vapor Sensors
Dan, Y., Lu, Y., Kybert, N. J., Luo, Z., & Johnson, A. T. C. (2009) · Nano Letters · doi:10.1021/nl8033637 · Cited by 974 · see citing works
Chemical Detection with a Single-Walled Carbon Nanotube Capacitor
Snow, E. S., Perkins, F. K., Houser, E. J., Bǎdescu, Ş. C., & Reinecke, T. L. (2005) · Science · doi:10.1126/science.1109128 · Cited by 953 · see citing works
All‐Organic Vapor Sensor Using Inkjet‐Printed Reduced Graphene Oxide
Dua, V., Surwade, S. P., Ammu, S., Agnihotra, S. R., Jain, S., Roberts, K. E., Park, S., Ruoff, R. S., & Manohar, S. K. (2010) · Angewandte Chemie International Edition · doi:10.1002/anie.200905089 · Cited by 934 · see citing works
Detection of NO 2 down to ppb Levels Using Individual and Multiple In 2 O 3 Nanowire Devices
Zhang, D., Liu, Z., Li, C., Tang, T., Liu, X., Han, S. H., Lei, B., & Zhou, C. (2004) · Nano Letters · doi:10.1021/nl0489283 · Cited by 867 · see citing works
Patolsky, F., Timko, B. P., Yu, G., Fang, Y., Greytak, A. B., Zheng, G., & Lieber, C. M. (2006) · Science · doi:10.1126/science.1128640 · Cited by 832 · see citing works
Carbon Nanotube Gas and Vapor Sensors
Kauffman, D. R., & Star, A. (2008) · Angewandte Chemie International Edition · doi:10.1002/anie.200704488 · Cited by 827 · see citing works
Importance of the Debye Screening Length on Nanowire Field Effect Transistor Sensors
Stern, E., Wagner, R., Sigworth, F. J., Breaker, R., Fahmy, T. M., & Reed, M. A. (2007) · Nano Letters · doi:10.1021/nl071792z · Cited by 806 · see citing works
Label-free detection of DNA hybridization using carbon nanotube network field-effect transistors
Star, A., Tu, E. L., Niemann, J., Gabriel, J. P., Joiner, C. S., & Valcke, C. (2006) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0504146103 · Cited by 670 · see citing works
Zhang, A., & Lieber, C. M. (2015) · Chemical Reviews · doi:10.1021/acs.chemrev.5b00608 · Cited by 629 · see citing works
Nanoelectronic biosensors based on CVD grown graphene
Huang, Y., Dong, X., Shi, Y., et al. (2010) · Nanoscale · doi:10.1039/c0nr00142b · Cited by 442 · see citing works
Chemical Sensors and Biosensors
Banica, F. G. (2012) · Wiley eBooks · doi:10.1002/9781118354162 · Cited by 428 · see citing works
Current and Developing Technologies for Monitoring Agents of Bioterrorism and Biowarfare
Lim, D. V., Simpson, J. M., Kearns, E. A., et al. (2005) · Clinical Microbiology Reviews · doi:10.1128/cmr.18.4.583-607.2005 · Cited by 422 · see citing works
Selective Gas Sensing with a Single Pristine Graphene Transistor
Rumyantsev, S., Liu, G., Shur, M. S., Potyrailo, R. A., & Balandin, A. A. (2012) · Nano Letters · doi:10.1021/nl3001293 · Cited by 405 · see citing works
Full and Modulated Chemical Gating of Individual Carbon Nanotubes by Organic Amine Compounds
Kong, J., & Dai, H. (2001) · The Journal of Physical Chemistry B · doi:10.1021/jp0101312 · Cited by 332 · see citing works
Optical heterodyne detection of laser-induced gratings.
Maznev, A., Nelson, K., & Rogers, J. A. (1998) · Optics Letters · doi:10.1364/ol.23.001319 · Cited by 289 · see citing works
Charge Transfer from Adsorbed Proteins
Bradley, K., Briman, M., Star, A., & Gruner, G. (2004) · Nano Letters · doi:10.1021/nl0349855 · Cited by 282 · see citing works
Gao, N., Zhou, W. M., Jiang, X., et al. (2015) · Nano Letters · doi:10.1021/acs.nanolett.5b00133 · Cited by 268 · see citing works
Biorecognition Layer Engineering: Overcoming Screening Limitations of Nanowire-Based FET Devices
Elnathan, R., Kwiat, M., Pevzner, A., Engel, Y., Burstein, L., Khatchtourints, A., Lichtenstein, A., Kantaev, R., & Patolsky, F. (2012) · Nano Letters · doi:10.1021/nl302434w · Cited by 232 · see citing works
Screening-Limited Response of NanoBiosensors
Nair, P. R., & Alam, M. A. (2008) · Nano Letters · doi:10.1021/nl072593i · Cited by 228 · see citing works
Frequency Domain Detection of Biomolecules Using Silicon Nanowire Biosensors
Zheng, G., Gao, X., & Lieber, C. M. (2010) · Nano Letters · doi:10.1021/nl1020975 · Cited by 211 · see citing works
Star, A., Han, T., Gabriel, J. P., et al. (2003) · Nano Letters · doi:10.1021/nl0346833 · Cited by 210 · see citing works
Detection beyond the Debye Screening Length in a High-Frequency Nanoelectronic Biosensor
Kulkarni, G. S., & Zhong, Z. (2012) · Nano Letters · doi:10.1021/nl203666a · Cited by 209 · see citing works
Self-citationMcNair, H. M., & Miller, J. M. (2008) · Wiley eBooks · doi:10.1002/9780470480106 · Cited by 199 · see citing works
Graphene nanoelectronic heterodyne sensor for rapid and sensitive vapour detection
Kulkarni, G. S., Reddy, K., Zhong, Z., & Fan, X. (2014) · Nature Communications · doi:10.1038/ncomms5376 · Cited by 189 · see citing works
Self-citationNon-covalent interactions: Key to biological flexibility and specificity
Frieden, E. (1975) · Journal of Chemical Education · doi:10.1021/ed052p754 · Cited by 188 · see citing works
Single molecule detection with graphene and other two-dimensional materials: nanopores and beyond
Arjmandi‐Tash, H., Belyaeva, L. A., & Schneider, G. F. (2015) · Chemical Society Reviews · doi:10.1039/c5cs00512d · Cited by 178 · see citing works
Real-time imaging of microparticles and living cells with CMOS nanocapacitor arrays
Laborde, C., Pittino, F., Verhoeven, H. A., Lemay, S. G., Selmi, L., Jongsma, M. A., & Widdershoven, F. (2015) · Nature Nanotechnology · doi:10.1038/nnano.2015.163 · Cited by 163 · see citing works
Mixing at 50GHz using a single-walled carbon nanotube transistor
Rosenblatt, S., Lin, H. Q., Sazonova, V., Tiwari, S., & McEuen, P. L. (2005) · Applied Physics Letters · doi:10.1063/1.2103391 · Cited by 148 · see citing works
The Role of External Defects in Chemical Sensing of Graphene Field-Effect Transistors
Kumar, B., Min, K., Bashirzadeh, M., Farimani, A. B., Bae, M., Estrada, D., Kim, Y. D., Yasaei, P., Park, Y. D., Pop, E., et al. (2013) · Nano Letters · doi:10.1021/nl304734g · Cited by 141 · see citing works
Dielectric Relaxation in the Electric Double Layer
Bockris, J. O., Gileadi, E., & Müller, K. J. (1966) · The Journal of Chemical Physics · doi:10.1063/1.1726876 · Cited by 94 · see citing works
Scaling issues in chemical and biological sensors
Madou, M. J., & Cubicciotti, R. (2003) · Proceedings of the IEEE · doi:10.1109/jproc.2003.813577 · Cited by 83 · see citing works
A tunable carbon nanotube resonator
Sazonova, V. A. (2006) · eCommons (Cornell University) · Cited by 76 · see citing works
Identification of A/H5N1 Influenza Viruses Using a Single Gene Diagnostic Microarray
Dawson, E. D., Moore, C. L., Dankbar, D. M., et al. (2006) · Analytical Chemistry · doi:10.1021/ac061920o · Cited by 72 · see citing works
Nonthermal Current-Stimulated Desorption of Gases from Carbon Nanotubes
Salehi‐Khojin, A., Lin, K., Field, C. R., & Masel, R. I. (2010) · Science · doi:10.1126/science.1194210 · Cited by 50 · see citing works
Radio-frequency electronics: circuits and applications
(1997) · Choice Reviews Online · doi:10.5860/choice.34-4496 · Cited by 41 · see citing works
Peer Reviewed: Responsive Drug Delivery Systems
Deo, S. K., Moschou, E. A., Peteu, S. F., et al. (2003) · Analytical Chemistry · doi:10.1021/ac0313217 · Cited by 40 · see citing works
A pathway sensor for genome-wide screens of intracellular proteolytic cleavage
Ketteler, R., Sun, Z., Kovacs, K. F., He, W.-W., & Seed, B. (2008) · Genome biology · doi:10.1186/gb-2008-9-4-r64 · Cited by 32 · see citing works
Electrical Probing and Tuning of Molecular Physisorption on Graphene
Kulkarni, G. S., Reddy, K., Zang, W., Lee, K., Fan, X., & Zhong, Z. (2015) · Nano Letters · doi:10.1021/acs.nanolett.5b04500 · Cited by 26 · see citing works
Self-citationSynthetic-array heterodyne detection: a single-element detector acts as an array
Strauss, C. E. M. (1994) · Optics Letters · doi:10.1364/ol.19.001609 · Cited by 17 · see citing works
Ligler, F. S., & Erickson, J. S. (2006) · Nature · doi:10.1038/440159a · Cited by 15 · see citing works
Adsorption of linear chain molecules on carbon nanotubes
Alldredge, E., Bǎdescu, Ş. C., Bajwa, N., et al. (2008) · Physical Review B · doi:10.1103/physrevb.78.161403 · Cited by 14 · see citing works
Kulkarni, G. S., & Zhong, Z. (2013) · Journal of Visualized Experiments · doi:10.3791/50438 · Cited by 7 · see citing works
Self-citationA microfabricated work-function gas sensor for semiconductor process gas detection.
Bergstrom, P. L. (1996) · Deep Blue (University of Michigan) · Cited by 3 · see citing works
Carbon Nanoelectronic Heterodyne Sensors : A New Paradigm for Chemical and Biological Detection.
Kulkarni, G. S. (2014) · Deep Blue (University of Michigan) · Cited by 1 · see citing works
Self-citation
Flagged first, then by citations
Cited by
Sorted by citations
Wearables and the Medical Revolution
Dunn, J., Runge, R., & Snyder, M. (2018) · Personalized Medicine · doi:10.2217/pme-2018-0044 · Cited by 654 · see citing works
- Authors
- Kulkarni, G. S., Zang, W., & Zhong, Z.
- Affiliations
- University of Michigan (US)
- Corresponding author
- Zhong, Zhaohui
- Venue
- Accounts of Chemical Research
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-09-26
- Volume
- 49
- Issue
- 11
- Pages
- 2578-2586
- ISSN
- 0001-4842 (ISSN-L)
- 1520-4898
- OpenAlex
- W2524478725
- Cited by
- 32
- References
- 61
- Citations by year
- 2025: 1 · 2024: 1 · 2023: 2 · 2022: 5 · 2021: 5 · 2020: 4 · 2019: 4 · 2018: 7 · 2017: 2 · 2016: 1
- FWCI
- 2.15
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Accounts of Chemical Research (publishedVersion)
- PubMed (publishedVersion)
- Funders
- Division of Electrical, Communications and Cyber Systems (ECCS-1405870)
- Division of Materials Research (DMR-1120187)
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Gas Sensing Nanomaterials and Sensors
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Electrochemical sensors and biosensors
- Physical Sciences › Chemical Engineering › Bioengineering › Analytical Chemistry and Sensors
- Keywords
- frequency mixing, molecular dipoles, graphene gas sensors, carbon nanotube field-effect transistors, polar molecule adsorption, Debye screening, ionic screening, biosensors, biotin-streptavidin binding, point-of-care detection, vapor sensing, nanomaterials
- MeSH terms
- Adsorption, Graphite, Ions, Transistors, Electronic, Biosensing Techniques, Nanotubes, Carbon, Nanostructures, Volatile Organic Compounds, Electrochemical Techniques, Electromagnetic Radiation
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review
