“…34,36,37 An increased dopant concentration can lead to a decreased dC/dV signal due to a lower thermal voltage and thinner depletion layer leading to a smaller change in capacitance as a function of voltage. 27,34 However, at concentrations below the peak, the dC/dV signal decreases with decreasing concentration because of other effects like a shift in the flat band voltage or a spreading resistance in series with the capacitance. 27,34 Moreover, dC/dV amplitude signals can be different for ntype and p-type carriers even at the same concentration.…”
Section: Memcapacitance Enhancement and Resistivementioning
confidence: 99%
“…26 However, little is known about the local capacitive and resistive behavior of PdSe 2 nanosheets (NSs) on mesoscopic lateral scales as well as the role of stacking on the electrical behavior. We use scanning microwave impedance microscopy (SMIM) 27,28 to investigate local capacitive and resistive behavior of orthorhombic PdSe 2 nanosheets (NSs) and NS stacks on the nanoscale. This mesoscale technique bridges the gap between atomic scale behavior and macroscopic device performance.…”
Section: Introductionmentioning
confidence: 99%
“…We use scanning microwave impedance microscopy (SMIM) , to investigate local capacitive and resistive behavior of orthorhombic PdSe 2 nanosheets (NSs) and NS stacks on the nanoscale. This mesoscale technique bridges the gap between atomic scale behavior and macroscopic device performance.…”
Section: Introductionmentioning
confidence: 99%
“…This mesoscale technique bridges the gap between atomic scale behavior and macroscopic device performance. SMIM is an atomic force microscopy technique where a nanoscale tip scans across a sample surface. ,− In addition to providing information about the topography, SMIM measures local electrical properties by sending microwaves at ∼3 GHz through a nanoscale tip that is in contact with the sample, creating a near-field electromagnetic wave. The microwave signal that is reflected back into the probe depends on the tip–sample contact impedance, and demodulation provides information on nanoscale capacitive (SMIM-C) and resistive (SMIM-R) material properties.…”
Tunable electronic materials that can be switched between different impedance states are fundamental to the hardware elements for neuromorphic computing architectures. This "brain-like" computing paradigm uses highly paralleled and colocated data processing, leading to greatly improved energy efficiency and performance compared to traditional architectures in which data have to be frequently transferred between processor and memory. In this work, we use scanning microwave impedance microscopy for nanoscale electrical and electronic characterization of twodimensional layered semiconductor PdSe 2 to probe neuromorphic properties. The local resolution of tens of nanometers reveals significant differences in electronic behavior between and within PdSe 2 nanosheets (NSs). In particular, we detected both n-type and p-type behaviors, although previous reports only point to ambipolar n-type dominating characteristics. Nanoscale capacitance−voltage curves and subsequent calculation of characteristic maps revealed a hysteretic behavior originating from the creation and erasure of Se vacancies as well as the switching of defect charge states. In addition, stacks consisting of two NSs show enhanced resistive and capacitive switching, which is attributed to trapped charge carriers at the interfaces between the stacked NSs. Stacking n-and p-type NSs results in a combined behavior that allows one to tune electrical characteristics. As local inhomogeneities of electrical and electronic behavior can have a significant impact on the overall device performance, the demonstrated nanoscale characterization and analysis will be applicable to a wide range of semiconducting materials.
“…34,36,37 An increased dopant concentration can lead to a decreased dC/dV signal due to a lower thermal voltage and thinner depletion layer leading to a smaller change in capacitance as a function of voltage. 27,34 However, at concentrations below the peak, the dC/dV signal decreases with decreasing concentration because of other effects like a shift in the flat band voltage or a spreading resistance in series with the capacitance. 27,34 Moreover, dC/dV amplitude signals can be different for ntype and p-type carriers even at the same concentration.…”
Section: Memcapacitance Enhancement and Resistivementioning
confidence: 99%
“…26 However, little is known about the local capacitive and resistive behavior of PdSe 2 nanosheets (NSs) on mesoscopic lateral scales as well as the role of stacking on the electrical behavior. We use scanning microwave impedance microscopy (SMIM) 27,28 to investigate local capacitive and resistive behavior of orthorhombic PdSe 2 nanosheets (NSs) and NS stacks on the nanoscale. This mesoscale technique bridges the gap between atomic scale behavior and macroscopic device performance.…”
Section: Introductionmentioning
confidence: 99%
“…We use scanning microwave impedance microscopy (SMIM) , to investigate local capacitive and resistive behavior of orthorhombic PdSe 2 nanosheets (NSs) and NS stacks on the nanoscale. This mesoscale technique bridges the gap between atomic scale behavior and macroscopic device performance.…”
Section: Introductionmentioning
confidence: 99%
“…This mesoscale technique bridges the gap between atomic scale behavior and macroscopic device performance. SMIM is an atomic force microscopy technique where a nanoscale tip scans across a sample surface. ,− In addition to providing information about the topography, SMIM measures local electrical properties by sending microwaves at ∼3 GHz through a nanoscale tip that is in contact with the sample, creating a near-field electromagnetic wave. The microwave signal that is reflected back into the probe depends on the tip–sample contact impedance, and demodulation provides information on nanoscale capacitive (SMIM-C) and resistive (SMIM-R) material properties.…”
Tunable electronic materials that can be switched between different impedance states are fundamental to the hardware elements for neuromorphic computing architectures. This "brain-like" computing paradigm uses highly paralleled and colocated data processing, leading to greatly improved energy efficiency and performance compared to traditional architectures in which data have to be frequently transferred between processor and memory. In this work, we use scanning microwave impedance microscopy for nanoscale electrical and electronic characterization of twodimensional layered semiconductor PdSe 2 to probe neuromorphic properties. The local resolution of tens of nanometers reveals significant differences in electronic behavior between and within PdSe 2 nanosheets (NSs). In particular, we detected both n-type and p-type behaviors, although previous reports only point to ambipolar n-type dominating characteristics. Nanoscale capacitance−voltage curves and subsequent calculation of characteristic maps revealed a hysteretic behavior originating from the creation and erasure of Se vacancies as well as the switching of defect charge states. In addition, stacks consisting of two NSs show enhanced resistive and capacitive switching, which is attributed to trapped charge carriers at the interfaces between the stacked NSs. Stacking n-and p-type NSs results in a combined behavior that allows one to tune electrical characteristics. As local inhomogeneities of electrical and electronic behavior can have a significant impact on the overall device performance, the demonstrated nanoscale characterization and analysis will be applicable to a wide range of semiconducting materials.
“…The spatial resolution is therefore mainly governed by geometry. SMM has received a growing interest from the research community to address a wide range of applications, including semiconductor materials such as 1D and 2D materials [14][15][16][17], biology [18][19][20][21][22][23][24][25], quantum physics [26][27][28][29][30] or energy materials [31][32][33]. There is an urgent need to develop SMM traceability to yield quantitative and calibrated data.…”
Section: Description Of the Scanning Microwave Microscope Built Inside A Scanning Electron Microscopementioning
The main objectives of this work are the development of fundamental extensions to existing scanning microwave microscopy (SMM) technology to achieve quantitative complex impedance measurements at the nanoscale. We developed a SMM operating up to 67 GHz inside a scanning electron microscope, providing unique advantages to tackle issues commonly found in open-air SMMs. Operating in the millimeter-wave frequency range induces high collimation of the evanescent electrical fields in the vicinity of the probe apex, resulting in high spatial resolution and enhanced sensitivity. Operating in a vacuum allows for eliminating the water meniscus on the tip apex, which remains a critical issue to address modeling and quantitative analysis at the nanoscale. In addition, a microstrip probing structure was developed to ensure a transverse electromagnetic mode as close as possible to the tip apex, drastically reducing radiation effects and parasitic apex-to-ground capacitances with available SMM probes. As a demonstration, we describe a standard operating procedure for instrumentation configuration, measurements and data analysis. Measurement performance is exemplarily shown on a staircase microcapacitor sample at 30 GHz.
photoconductive and photovoltaic properties. [3] Moreover, the material exhibits a substantial polarization of ≈15 µC cm −2 , [4,5] while being lead-free.A fundamentally intriguing question is that of the role of the polarization potential of Sn 2 P 2 S 6 in its known and prospective functionalities. The crystal structure of Sn 2 P 2 S 6 in its ferroelectric state is shown in Figure 1a. [6] As is typical for ferroelectric thiophosphates, the ferroelectricity originates from a relative displacement of the Sn 2+ cations with regard to the framework of (P 2 S 6 ) 4− anions. The driving force for the transition is the second-order Jan-Teller effect [7] due to electron lonepair stereoactivity of the Sn 2+ cations, together with possible valence fluctuations within the (P 2 S 6 ) 4− anions. [5,8,9] Unlike more ubiquitous double-well ferroelectrics (Figure 1b), Sn 2 P 2 S 6 has been reported to exhibit a uniaxial triple-well (Figure 1d) wherein a metastable nonpolar state coexists with polarized structures well below the phase transition to the ferroelectric state at ≈338 K. [4,8,10] Despite early reports of a possible triple-well potential in Sn 2 P 2 S 6 , direct experimental evidence for its existence remains scarce and controversial. Experimentally, Kiselev et al. have shown piezoresponse force microscopy (PFM) images of Sn 2 P 2 S 6 containing areas of suppressed piezoresponse around domain boundaries that appeared much broader than expected Polarization dynamics in ferroelectric materials is governed by the effective potential energy landscape of the order parameter. The unique aspect of ferroelectrics compared to many other transitions is the possibility of more than two potential wells, leading to complicated energy landscapes with new fundamental and functional properties. Here, direct dynamic evidence is revealed of a triple-well potential in the metal thiophosphate Sn 2 P 2 S 6 compound using multivariate scanning probe microscopy combined with theoretical simulations. The key finding is that the metastable zero polarization state can be accessed through a gradual switching process and is stabilized over a broad range of electric fields. Simulations confirm that the observed zero polarization state originates from a kinetic stabilization of the nonpolar state of the triple-well, as opposed to domain walls. Dynamically, the triple-well of Sn 2 P 2 S 6 becomes equivalent to antiferroelectric hysteresis loops. Therefore, this material combines the robust and well-defined domain structure of a proper ferroelectric with dynamic hysteresis loops present in antiferroelectrics. Moreover, the triple-well enhances mem-capacitive effects in Sn 2 P 2 S 6 , which are forbidden for ideal double-well ferroelectrics. These findings provide a path to tunable electronic elements for beyond binary high-density computing devices and neuromorphic circuits based on dynamic properties of the triple-well.
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