Ultrathin quasi-2D amorphous carbon dielectric prepared from solution precursor for nanoelectronics

An, Fufei; Wang, Congjun; Pham, Viet Hung; Borisevich, Albina; Qian, Jiangchao; Yin, Kaijun; Pidaparthy, Saran; Robinson, Brian; Chou, Ang-Sheng; Lee, Junseok; Weidman, Jennifer; Natesakhawat, Sittichai; Wang, Han; Schleife, André; Zuo, Jian-Min; Matranga, Christopher; Cao, Qing

doi:10.1038/s44172-023-00141-9

Ultrathin quasi-2D amorphous carbon dielectric prepared from solution precursor for nanoelectronics

Journal Article · Wed Dec 20 00:00:00 EST 2023 · Communications Engineering

DOI:https://doi.org/10.1038/s44172-023-00141-9· OSTI ID:2246990

An, Fufei; ; ; Borisevich, Albina; ; Yin, Kaijun; ; Robinson, Brian; Chou, Ang-Sheng; Lee, Junseok; ; Natesakhawat, Sittichai; ; ; ; Matranga, Christopher;

Abstract

Materials keeping thickness in atomic scale but extending primarily in lateral dimensions offer properties attractive for many emerging applications. However, compared to crystalline counterparts, synthesis of atomically thin films in the highly disordered amorphous form, which avoids nonuniformity and defects associated with grain boundaries, is challenging due to their metastable nature. Here we present a scalable and solution-based strategy to prepare large-area, freestanding quasi-2D amorphous carbon nanomembranes with predominant sp ² bonding and thickness down to 1–2 atomic layers, from coal-derived carbon dots as precursors. These atomically thin amorphous carbon films are mechanically strong with modulus of 400 ± 100 GPa and demonstrate robust dielectric properties with high dielectric strength above 20 MV cm ⁻¹ and low leakage current density below 10 ⁻⁴ A cm ⁻² through a scaled thickness of three-atomic layers. They can be implemented as solution-deposited ultrathin gate dielectrics in transistors or ion-transport media in memristors, enabling exceptional device performance and spatiotemporal uniformity.

View Journal Article

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR); USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Fossil Energy and Carbon Management (FECM); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2246990

Alternate ID(s):: OSTI ID: 2345287

Journal Information:: Communications Engineering, Journal Name: Communications Engineering Journal Issue: 1 Vol. 2; ISSN 2731-3395

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: Country unknown/Code not available

Language:: English

References (65)

Chlorination of Reduced Graphene Oxide Enhances the Dielectric Constant of Reduced Graphene Oxide/Polymer Composites Kim, Jin-Young; Lee, Wi Hyoung; Suk, Ji Won Advanced Materials, Vol. 25, Issue 16 https://doi.org/10.1002/adma.201300385	journal	February 2013
Atomically Thin Femtojoule Memristive Device Zhao, Huan; Dong, Zhipeng; Tian, He Advanced Materials, Vol. 29, Issue 47 https://doi.org/10.1002/adma.201703232	journal	October 2017
Pyrolysis field desorption mass spectrometry of polymers. III. Aliphatic polyamides Bahr, U.; Lüderwald, I.; Müller, R. Die Angewandte Makromolekulare Chemie, Vol. 120, Issue 1 https://doi.org/10.1002/apmc.1984.051200110	journal	February 1984
Chemically Tailoring Coal to Fluorescent Carbon Dots with Tuned Size and Their Capacity for Cu(II) Detection Hu, Chao; Yu, Chang; Li, Mingyu Small, Vol. 10, Issue 23 https://doi.org/10.1002/smll.201401328	journal	July 2014
Direct evaluation of the sp3 content in diamond-like-carbon films by XPS Mérel, P.; Tabbal, M.; Chaker, M. Applied Surface Science, Vol. 136, Issue 1-2 https://doi.org/10.1016/S0169-4332(98)00319-5	journal	October 1998
Diamond as an electronic material Wort, Chris J. H.; Balmer, Richard S. Materials Today, Vol. 11, Issue 1-2 https://doi.org/10.1016/S1369-7021(07)70349-8	journal	January 2008
Gentle STEM: ADF imaging and EELS at low primary energies Krivanek, Ondrej L.; Dellby, Niklas; Murfitt, Matthew F. Ultramicroscopy, Vol. 110, Issue 8 https://doi.org/10.1016/j.ultramic.2010.02.007	journal	July 2010
Ligand Pyrolysis during Air-Free Inorganic Nanocrystal Synthesis Sperry, Breena M.; Luscombe, Christine K. Chemistry of Materials, Vol. 33, Issue 1 https://doi.org/10.1021/acs.chemmater.0c03088	journal	December 2020
Atomristor: Nonvolatile Resistance Switching in Atomic Sheets of Transition Metal Dichalcogenides Ge, Ruijing; Wu, Xiaohan; Kim, Myungsoo Nano Letters, Vol. 18, Issue 1 https://doi.org/10.1021/acs.nanolett.7b04342	journal	December 2017
Dielectric Breakdown in Single-Crystal Hexagonal Boron Nitride Ranjan, Alok; Raghavan, Nagarajan; Holwill, Matthew ACS Applied Electronic Materials, Vol. 3, Issue 8 https://doi.org/10.1021/acsaelm.1c00469	journal	August 2021
Restoring the Electrical Properties of CVD Graphene via Physisorption of Molecular Adsorbates Thodkar, Kishan; Thompson, Damien; Lüönd, Felix ACS Applied Materials & Interfaces, Vol. 9, Issue 29 https://doi.org/10.1021/acsami.7b05143	journal	July 2017
Rapid Purification and Size Separation of Gold Nanoparticles via Diafiltration Sweeney, Scott F.; Woehrle, Gerd H.; Hutchison, James E. Journal of the American Chemical Society, Vol. 128, Issue 10 https://doi.org/10.1021/ja0558241	journal	March 2006
Softened Elastic Response and Unzipping in Chemical Vapor Deposition Graphene Membranes Ruiz-Vargas, Carlos S.; Zhuang, Houlong L.; Huang, Pinshane Y. Nano Letters, Vol. 11, Issue 6 https://doi.org/10.1021/nl200429f	journal	June 2011
Electron Tunneling through Ultrathin Boron Nitride Crystalline Barriers Britnell, Liam; Gorbachev, Roman V.; Jalil, Rashid Nano Letters, Vol. 12, Issue 3 https://doi.org/10.1021/nl3002205	journal	February 2012
Synthesis and Characterization of Hexagonal Boron Nitride Film as a Dielectric Layer for Graphene Devices Kim, Ki Kang; Hsu, Allen; Jia, Xiaoting ACS Nano, Vol. 6, Issue 10 https://doi.org/10.1021/nn301675f	journal	September 2012
How 2D semiconductors could extend Moore’s law Li, Ming-Yang; Su, Sheng-Kai; Wong, H. -S. Philip Nature, Vol. 567, Issue 7747 https://doi.org/10.1038/d41586-019-00793-8	journal	March 2019
Two-dimensional semiconductors for transistors Chhowalla, Manish; Jena, Debdeep; Zhang, Hua Nature Reviews Materials, Vol. 1, Issue 11 https://doi.org/10.1038/natrevmats.2016.52	journal	August 2016
High-frequency, scaled graphene transistors on diamond-like carbon Wu, Yanqing; Lin, Yu-ming; Bol, Ageeth A. Nature, Vol. 472, Issue 7341 https://doi.org/10.1038/nature09979	journal	April 2011
Coal as an abundant source of graphene quantum dots Ye, Ruquan; Xiang, Changsheng; Lin, Jian Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3943	journal	December 2013
Oxygenated amorphous carbon for resistive memory applications Santini, Claudia A.; Sebastian, Abu; Marchiori, Chiara Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9600	journal	October 2015
Synthesis of large-area multilayer hexagonal boron nitride for high material performance Kim, Soo Min; Hsu, Allen; Park, Min Ho Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9662	journal	October 2015
A fast, high-endurance and scalable non-volatile memory device made from asymmetric Ta₂O_5−x/TaO_2−x bilayer structures Lee, Myoung-Jae; Lee, Chang Bum; Lee, Dongsoo Nature Materials, Vol. 10, Issue 8, p. 625-630 https://doi.org/10.1038/nmat3070	journal	July 2011
Boron nitride substrates for high-quality graphene electronics Dean, C. R.; Young, A. F.; Meric, I. Nature Nanotechnology, Vol. 5, Issue 10, p. 722-726 https://doi.org/10.1038/nnano.2010.172	journal	August 2010
Tunable sieving of ions using graphene oxide membranes Abraham, Jijo; Vasu, Kalangi S.; Williams, Christopher D. Nature Nanotechnology, Vol. 12, Issue 6 https://doi.org/10.1038/nnano.2017.21	journal	April 2017
Vapor–liquid–solid growth of large-area multilayer hexagonal boron nitride on dielectric substrates Shi, Zhiyuan; Wang, Xiujun; Li, Qingtian Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-14596-3	journal	February 2020
Insulators for 2D nanoelectronics: the gap to bridge Illarionov, Yury Yu.; Knobloch, Theresia; Jech, Markus Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16640-8	journal	July 2020
SiGe epitaxial memory for neuromorphic computing with reproducible high performance based on engineered dislocations Choi, Shinhyun; Tan, Scott H.; Li, Zefan Nature Materials, Vol. 17, Issue 4 https://doi.org/10.1038/s41563-017-0001-5	journal	January 2018
Memristive crossbar arrays for brain-inspired computing Xia, Qiangfei; Yang, J. Joshua Nature Materials, Vol. 18, Issue 4 https://doi.org/10.1038/s41563-019-0291-x	journal	March 2019
Alloying conducting channels for reliable neuromorphic computing Yeon, Hanwool; Lin, Peng; Choi, Chanyeol Nature Nanotechnology, Vol. 15, Issue 7 https://doi.org/10.1038/s41565-020-0694-5	journal	June 2020
Atomically precise control in the design of low-nuclearity supported metal catalysts Mitchell, Sharon; Pérez-Ramírez, Javier Nature Reviews Materials, Vol. 6, Issue 11 https://doi.org/10.1038/s41578-021-00360-6	journal	September 2021
Synthesis and properties of free-standing monolayer amorphous carbon Toh, Chee-Tat; Zhang, Hongji; Lin, Junhao Nature, Vol. 577, Issue 7789 https://doi.org/10.1038/s41586-019-1871-2	journal	January 2020
Ultralow-dielectric-constant amorphous boron nitride Hong, Seokmo; Lee, Chang-Seok; Lee, Min-Hyun Nature, Vol. 582, Issue 7813 https://doi.org/10.1038/s41586-020-2375-9	journal	June 2020
Disorder-tuned conductivity in amorphous monolayer carbon Tian, Huifeng; Ma, Yinhang; Li, Zhenjiang Nature, Vol. 615, Issue 7950 https://doi.org/10.1038/s41586-022-05617-w	journal	March 2023
Dielectric properties of hexagonal boron nitride and transition metal dichalcogenides: from monolayer to bulk Laturia, Akash; Van de Put, Maarten L.; Vandenberghe, William G. npj 2D Materials and Applications, Vol. 2, Issue 1 https://doi.org/10.1038/s41699-018-0050-x	journal	March 2018
Wafer-scale integration of two-dimensional materials in high-density memristive crossbar arrays for artificial neural networks Chen, Shaochuan; Mahmoodi, Mohammad Reza; Shi, Yuanyuan Nature Electronics, Vol. 3, Issue 10 https://doi.org/10.1038/s41928-020-00473-w	journal	October 2020
The performance limits of hexagonal boron nitride as an insulator for scaled CMOS devices based on two-dimensional materials Knobloch, Theresia; Illarionov, Yury Yu.; Ducry, Fabian Nature Electronics, Vol. 4, Issue 2 https://doi.org/10.1038/s41928-020-00529-x	journal	February 2021
Understanding the catalyst-free transformation of amorphous carbon into graphene by current-induced annealing Barreiro, Amelia; Börrnert, Felix; Avdoshenko, Stanislav M. Scientific Reports, Vol. 3, Issue 1 https://doi.org/10.1038/srep01115	journal	January 2013
Synthesis and Characterization of Hexagonal Boron Nitride as a Gate Dielectric Jang, Sung Kyu; Youn, Jiyoun; Song, Young Jae Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep30449	journal	July 2016
Purification technologies for colloidal nanocrystals Shen, Yi; Gee, Megan Y.; Greytak, A. B. Chemical Communications, Vol. 53, Issue 5 https://doi.org/10.1039/C6CC07998A	journal	January 2017
Wafer-scale MoS2 thin layers prepared by MoO3 sulfurization Lin, Yu-Chuan; Zhang, Wenjing; Huang, Jing-Kai Nanoscale, Vol. 4, Issue 20 https://doi.org/10.1039/c2nr31833d	journal	January 2012
A climbing image nudged elastic band method for finding saddle points and minimum energy paths Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904 https://doi.org/10.1063/1.1329672	journal	December 2000
High speed resistive switching in Pt∕TiO2∕TiN film for nonvolatile memory application Yoshida, Chikako; Tsunoda, Kohji; Noshiro, Hideyuki Applied Physics Letters, Vol. 91, Issue 22 https://doi.org/10.1063/1.2818691	journal	November 2007
Realization of a high mobility dual-gated graphene field-effect transistor with Al2O3 dielectric Kim, Seyoung; Nah, Junghyo; Jo, Insun Applied Physics Letters, Vol. 94, Issue 6 https://doi.org/10.1063/1.3077021	journal	February 2009
Nonvolatile resistive switching in graphene oxide thin films He, C. L.; Zhuge, F.; Zhou, X. F. Applied Physics Letters, Vol. 95, Issue 23 https://doi.org/10.1063/1.3271177	journal	December 2009
Electron tunneling through atomically flat and ultrathin hexagonal boron nitride Lee, Gwan-Hyoung; Yu, Young-Jun; Lee, Changgu Applied Physics Letters, Vol. 99, Issue 24 https://doi.org/10.1063/1.3662043	journal	December 2011
A density-functional theory study of the Al/AlO _x /Al tunnel junction Kim, Chang-Eun; Ray, Keith G.; Lordi, Vincenzo Journal of Applied Physics, Vol. 128, Issue 15 https://doi.org/10.1063/5.0020292	journal	October 2020
Synthesis of linked carbon monolayers: Films, balloons, tubes, and pleated sheets Schultz, Mitchell J.; Zhang, Xiaoyu; Unarunotai, Sakulsuk Proceedings of the National Academy of Sciences, Vol. 105, Issue 21 https://doi.org/10.1073/pnas.0710081105	journal	May 2008
Electric Breakdown of Glasses and Crystals as a Function of Temperature von Hippel, A.; Maurer, R. J. Physical Review, Vol. 59, Issue 10 https://doi.org/10.1103/PhysRev.59.820	journal	May 1941
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Separation of the sp 3 and sp 2 components in the C1 s photoemission spectra of amorphous carbon films Díaz, Javier; Paolicelli, Guido; Ferrer, Salvador Physical Review B, Vol. 54, Issue 11 https://doi.org/10.1103/PhysRevB.54.8064	journal	September 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Resonant Raman spectroscopy of disordered, amorphous, and diamondlike carbon Ferrari, A. C.; Robertson, J. Physical Review B, Vol. 64, Issue 7 https://doi.org/10.1103/PhysRevB.64.075414	journal	July 2001
Electron knock-on cross section of carbon and boron nitride nanotubes Zobelli, A.; Gloter, A.; Ewels, C. P. Physical Review B, Vol. 75, Issue 24 https://doi.org/10.1103/PhysRevB.75.245402	journal	June 2007
From Point Defects in Graphene to Two-Dimensional Amorphous Carbon Kotakoski, J.; Krasheninnikov, A. V.; Kaiser, U. Physical Review Letters, Vol. 106, Issue 10 https://doi.org/10.1103/PhysRevLett.106.105505	journal	March 2011
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/S0021889811038970	journal	October 2011
HfOx based vertical resistive random access memory for cost-effective 3D cross-point architecture without cell selector Chen, Hong-Yu; Yu, Shimeng; Gao, Bin 2012 International Electron Devices Meeting https://doi.org/10.1109/IEDM.2012.6479083	conference	December 2012
A Physical Model for the Hysteresis in MoS₂ Transistors Knobloch, Theresia; Rzepa, Gerhard; Illarionov, Yury Yu. IEEE Journal of the Electron Devices Society, Vol. 6 https://doi.org/10.1109/JEDS.2018.2829933	journal	January 2018
Atomically Thin CBRAM Enabled by 2-D Materials: Scaling Behaviors and Performance Limits Dong, Zhipeng; Zhao, Huan; DiMarzio, Don IEEE Transactions on Electron Devices, Vol. 65, Issue 10 https://doi.org/10.1109/TED.2018.2830328	journal	October 2018
The Great Crystallite Versus Random Network Controversy: A Personal Perspective Wright, Adrian C. International Journal of Applied Glass Science, Vol. 5, Issue 1 https://doi.org/10.1111/ijag.12039	journal	October 2013
Realization of continuous Zachariasen carbon monolayer Joo, Won-Jae; Lee, Jae-Hyun; Jang, Yamujin Science Advances, Vol. 3, Issue 2 https://doi.org/10.1126/sciadv.1601821	journal	February 2017
Neat monolayer tiling of molecularly thin two-dimensional materials in 1 min Matsuba, Kazuaki; Wang, Chengxiang; Saruwatari, Kazuko Science Advances, Vol. 3, Issue 6 https://doi.org/10.1126/sciadv.1700414	journal	June 2017
Measurement of the Elastic Properties and Intrinsic Strength of Monolayer Graphene Lee, C.; Wei, X.; Kysar, J. W. Science, Vol. 321, Issue 5887, p. 385-388 https://doi.org/10.1126/science.1157996	journal	July 2008
(Invited) Resistive Memories (RRAM) Variability: Challenges and Solutions Molas, Gabriel; Sassine, Gilbert; Nail, Cecile ECS Transactions, Vol. 86, Issue 3 https://doi.org/10.1149/08603.0035ecst	journal	July 2018

Similar Records

Solution-Based Synthesis of Ultrathin Quasi-2D Amorphous Carbon for Nanoelectronics

Conference · Sat Nov 30 23:00:00 EST 2024 · OSTI ID:2479102

2D Amorphous Carbon Dielectric Prepared from Solution Precursor for Nanoelectronics

Conference · Wed Oct 09 00:00:00 EDT 2024 · OSTI ID:2460431

Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY

Ultrathin quasi-2D amorphous carbon dielectric prepared from solution precursor for nanoelectronics

Citation Formats

References (65)

Similar Records

Related Subjects