The device concept of ferroelectric-based negative capacitance (NC) transistors offers a promising route for achieving energy-efficient logic applications that can outperform the conventional semiconductor technology, while viable operation mechanisms remain a central topic of debate. In this work, we report steep slope switching in MoS2transistors back-gated by single-layer polycrystalline PbZr0.35Ti0.65O3. The devices exhibit current switching ratios up to 8 × 106within an ultra-low gate voltage window of
Controllable single‐molecule logic operations will enable development of reliable ultra‐minimalistic circuit elements for high‐density computing but require stable currents from multiple orthogonal inputs in molecular junctions. Utilizing the two unique adjacent conductive molecular orbitals (MOs) of gated Au/S‐(CH2)3‐Fc‐(CH2)9‐S/Au (Fc = ferrocene) single‐electron transistors (≈2 nm), a stable single‐electron logic calculator (SELC) is presented, which allows real‐time modulation of output current as a function of orthogonal input bias (
- Award ID(s):
- 1916874
- NSF-PAR ID:
- 10445326
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 34
- Issue:
- 26
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
Abstract $$V_{{{\mathrm{g}}}} = \pm \! 0.5$$ -
more » « less
Abstract Pivotal to functional van der Waals stacked flexible electronic/excitonic/spintronic/thermoelectric chips is the synergy amongst constituent layers. However; the current techniques viz. sequential chemical vapor deposition, micromechanical/wet‐chemical transfer are mostly limited due to diffused interfaces, and metallic remnants/bubbles at the interface. Inter‐layer‐coupled 2+
δ ‐dimensional materials, as a new class of materials can be significantly suitable for out‐of‐plane carrier transport and hence prompt response in prospective devices. Here, the discovery of the use of exotic electric field ≈106 V cm−1(at microwave hot‐spot) and 2 thermomechanical conditions i.e. pressure ≈1 MPa, T ≈ 200 °C (during solvothermal reaction) to realize 2+δ ‐dimensional materials is reported. It is found that PzPzchemical bonds form between the component layers, e.g., CB and CN in G‐BN, MoN and MoB in MoS2‐BN hybrid systems as revealed by X‐ray photoelectron spectroscopy. New vibrational peaks in Raman spectra (BC ≈1320 cm–1for the G‐BN system and MoB ≈365 cm–1for the MoS2‐BN system) are recorded. Tunable mid‐gap formation, along with diodic behavior (knee voltage ≈0.7 V, breakdown voltage ≈1.8 V) in the reduced graphene oxide‐reduced BN oxide (RGO‐RBNO) hybrid system is also observed. Band‐gap tuning in MoS2‐BN system is observed. Simulations reveal stacking‐dependent interfacial charge/potential drops, hinting at the feasibility of next‐generation functional devices/sensors. -
more » « less
Abstract Au‐mediated exfoliation of 2D transition‐metal dichalcogenides (TMDs) has received significant attention due to its ability to produce large‐area monolayer (ML) flakes. This process has been attributed to strong TMD/Au binding energy (BE) as well as the uniform strain between the TMDs and Au. However, large‐area exfoliation of TMDs with other metals that have even stronger theoretical BE than Au/TMD is not successful, leading to question whether the BE plays any role in the exfoliation process. Here, successful demonstration of large‐area ML MoS2using Cu, Ni, and Ag with various predicted strain, including Pd with almost no strain, but stronger BE than Au/MoS2is demonstrated. Optical micrographs show MoS2flakes with 100s of µm in size with a yield of several tens to hundreds of ML flakes per exfoliation. Photoluminescence and Raman spectroscopy confirm the ML nature of the flakes, while electrical transport measurements show mobilities of
≈ 6 cm2 V−1 s−1with a current on‐off ratio≈ 108consistent with high‐quality ML MoS2. Given that MoS2can be exfoliated with metals that have strong BE irrespective of their strain values suggests that BE is the primary mechanism in successful exfoliation of large‐area ML MoS2. -
more » « less
Neurotransmitters are small molecules involved in neuronal signaling and can also serve as stress biomarkers.1Their abnormal levels have been also proposed to be indicative of several neurological diseases such as Alzheimer’s disease, Parkinson’s disease, Huntington disease, among others. Hence, measuring their levels is highly important for early diagnosis, therapy, and disease prognosis. In this work, we investigate facile functionalization methods to tune and enhance sensitivity of printed graphene sensors to neurotransmitters. Sensors based on direct laser scribing and screen-printed graphene ink are studied. These printing methods offer ease of prototyping and scalable fabrication at low cost.
The effect of functionalization of laser induced graphene (LIG) by electrodeposition and solution-based deposition of TMDs (molybdenum disulfide2and tungsten disulfide) and metal nanoparticles is studied. For different processing methods, electrochemical characteristics (such as electrochemically active surface area: ECSA and heterogenous electron transfer rate: k0) are extracted and correlated to surface chemistry and defect density obtained respectively using X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. These functionalization methods are observed to directly impact the sensitivity and limit of detection (LOD) of the graphene sensors for the studied neurotransmitters. For example, as compared to bare LIG, it is observed that electrodeposition of MoS2on LIG improves ECSA by 3 times and k0by 1.5 times.3Electrodeposition of MoS2also significantly reduces LOD of serotonin and dopamine in saliva, enabling detection of their physiologically relevant concentrations (in pM-nM range). In addition, chemical treatment of LIG sensors is carried out in the form of acetic acid treatment. Acetic acid treatment has been shown previously to improve C-C bonds improving the conductivity of LIG sensors.4In our work, in particular, acetic acid treatment leads to larger improvement of LOD of norepinephrine compared to MoS2electrodeposition.
In addition, we investigate the effect of plasma treatment to tune the sensor response by modifying the defect density and chemistry. For example, we find that oxygen plasma treatment of screen-printed graphene ink greatly improves LOD of norepinephrine up to three orders of magnitude, which may be attributed to the increased defects and oxygen functional groups on the surface as evident by XPS measurements. Defects are known to play a key role in enhancing the sensitivity of 2D materials to surface interactions, and have been explored in tuning/enhancing the sensor sensitivity.5Building on our previous work,3we apply a custom machine learning-based data processing method to further improve that sensitivity and LOD, and also to automatically benchmark different molecule-material pairs.
Future work includes expanding the plasma chemistry and conditions, studying the effect of precursor mixture in laser-induced solution-based functionalization, and understanding the interplay between molecule-material system. Work is also underway to improve the machine learning model by using nonlinear learning models such as neural networks to improve the sensor sensitivity, selectivity, and robustness.
References A. J. Steckl, P. Ray, (2018), doi:10.1021/acssensors.8b00726.
Y. Lei, D. Butler, M. C. Lucking, F. Zhang, T. Xia, K. Fujisawa, T. Granzier-Nakajima, R. Cruz-Silva, M. Endo, H. Terrones, M. Terrones, A. Ebrahimi,
Sci. Adv. 6 , 4250–4257 (2020).V. Kammarchedu, D. Butler, A. Ebrahimi,
Anal. Chim. Acta .1232 , 340447 (2022).H. Yoon, J. Nah, H. Kim, S. Ko, M. Sharifuzzaman, S. C. Barman, X. Xuan, J. Kim, J. Y. Park,
Sensors Actuators B Chem. 311 , 127866 (2020).T. Wu, A. Alharbi, R. Kiani, D. Shahrjerdi,
Adv. Mater. 31 , 1–12 (2019). -
more » « less
Abstract The crystal structures of the charge‐transfer (CT) cocrystals formed by the π‐electron acceptor 1,3,4,5,7,8‐hexafluoro‐11,11,12,12‐tetracyanonaphtho‐2,6‐quinodimethane (F6TNAP) with the planar π‐electron‐donor molecules triphenylene (TP), benzo[
b ]benzo[4,5]thieno[2,3‐d ]thiophene (BTBT), benzo[1,2‐b :4,5‐b ′]dithiophene (BDT), pyrene (PY), anthracene (ANT), and carbazole (CBZ) have been determined using single‐crystal X‐ray diffraction (SCXRD), along with those of two polymorphs of F6TNAP. All six cocrystals exhibit 1:1 donor/acceptor stoichiometry and adopt mixed‐stacking motifs. Cocrystals based on BTBT and CBZ π‐electron donor molecules exhibit brickwork packing, while the other four CT cocrystals show herringbone‐type crystal packing. Infrared spectroscopy, molecular geometries determined by SCXRD, and electronic structure calculations indicate that the extent of ground‐state CT in each cocrystal is small. Density functional theory calculations predict large conduction bandwidths and, consequently, low effective masses for electrons for all six CT cocrystals, while the TP‐, BDT‐, and PY‐based cocrystals are also predicted to have large valence bandwidths and low effective masses for holes. Charge‐carrier mobility values are obtained from space‐charge limited current (SCLC) measurements and field‐effect transistor measurements, with values exceeding 1 cm2V−1s1being estimated from SCLC measurements for BTBT:F6TNAP and CBZ:F6TNAP cocrystals.
