Excellent Switching Performance Research Articles

Phase Coexistence Induced Giant Dielectric Tunability and Electromechanical Response in PbZrO3 Epitaxial Thin Films.

PbZrO3 (PZO) thin films, as a classic antiferroelectric material, have attracted tremendous attention for their excellent dielectric, electromechanical, and thermal switching performances. However, several fundamental questions remain unresolved, particularly the existence of an intermediate phase during the transition from the antiferroelectric (AFE) to ferroelectric (FE) state. Here, a phase coexistence configuration of an orthorhombic AFE phase and a tetragonal-like (T-like) phase is reported in epitaxial antiferroelectric PZO thin films, with thickness ranging from 16 to 110nm. This configuration is evidenced both macroscopically by distinct shoulder-cape-shaped dielectric behavior and microscopically through scanning transmission electron microscopy (STEM) analysis. Remarkably, a 49nm PZO film achieves an ultrahigh dielectric tunability of 90.1%, while a 59nm film exhibits significant electromechanical strain of 0.66%. Microscopically, HAADF-STEM reveals the presence of the intermediate phase with a dipole arrangement of vertically diagonal up-up-down-down pattern, and first-principles calculations further confirm the role of this intermediate phase during AFE-to-FE phase transition, which is responsible for the unusual dielectric peaks of ɛr-E curves. These findings not only enhance the understanding of phase transition in antiferroelectric materials but also exhibit great potential for high-performance tunable and nano-electromechanical device applications.

Facile Synthesis of Novel Conducting Copolymers Based on N-Furfuryl Pyrrole and 3,4-Ethylenedioxythiophene with Enhanced Optoelectrochemical Performances Towards Electrochromic Application.

In this article, a series of novel conducting copolymers P(FuPy-co-EDOT) are prepared via cyclic voltammetry electropolymerization method by using N-furfuryl pyrrole (FuPy) and 3,4-ethylenedioxythiophene (EDOT) as comonomers. The molecular structure, surface morphology, electrochemical, and optical properties of the resulting copolymers are characterized in detail upon varying the feed ratios of FuPy/EDOT in the range of 1/1 to 1/9. The results demonstrate that the prepared P(FuPy-co-EDOT) copolymers with a higher proportion of EDOT units (FuPy/EDOT: 2/8~1/9) possess good redox activity, tunable optical absorption performances, and low band gaps (1.75~1.86 eV). Spectroelectrochemistry studies indicate that the resulting copolymers with increased EDOT units show strengthened electrochromic characteristics, exhibiting a red-to-green-to-blue multicolor reversible transition, especially for the P(FuPy1-co-EDOT9) copolymer films. They also show increased optical contrast (9~34%), fast response time (0.8~2.4 s), and good coloring efficiency (110~362 cm2 C-1). Additionally, the complementary bilayer P(FuPy-co-EDOT)/PEDOT electrochromic devices (ECDs) are also assembled and evaluated to hold excellent electrochromic switching performances with relatively high optical contrast (25%), rapid response time (0.9 s), and satisfactory coloring efficiency (416 cm2 C-1). Together with the superior open circuit memory and cycling stability, they can be used as a new type of electrochromic material and have considerable prospects as promising candidates for electrochromic devices.

Outstanding Stability and Resistive Switching Performance through Octa-Amino-Polyhedral Oligomeric Silsesquioxane Modification in Flexible Perovskite Resistive Random-Access Memories.

Resistive random access memory (RRAM) has emerged as a promising candidate for next-generation storage technologies due to its simple structure, high running speed, excellent durability, high integration density, and low power consumption. This paper focuses on the application of organic-inorganic hybrid perovskite (OIHP) materials in RRAM by introducing an innovative three-dimensional POPA modification strategy, which is realized by binding octa-amine-polyhedral oligomeric silsesquioxanes (8NH2-POSS) onto the side chains of poly(acrylic acid) (PAA), thereby enhancing the material's resilience under elevated temperatures and humidity conditions. POPA cross-links with perovskite grains at crystalline boundaries through multiple -NH3+ and -C═O chemical anchoring sites on its branch chain, enhancing the grain adhesion, optimizing the film quality, and improving the cage structure distribution at the perovskite grain boundaries. The experimental results demonstrate that the POPA-modified OIHP RRAM exhibits an excellent resistance switching performance, with an optimal ON/OFF ratio of 5.0 × 105 and a data retention time of 104 s. After 150 days of environmental exposure, the ON/OFF ratio remains at 1.0 × 105, indicating good stability. Furthermore, the POPA modification endows the perovskite film with considerable flexibility, maintaining stable resistance switching performance under various bending radii. This study provides a vital reference for flexible, high-performance, and long-lifespan perovskite memory devices.

A Multimodal Perception-Enabled Flexible Memristor with Combined Sensing-Storage-Memory Functions for Enhanced Artificial Injury Recognition.

With the continuous advancement of wearable technology and advanced medical monitoring, there is an increasing demand for electronic devices that can adapt to complex environments and have high perceptual sensitivity. Here, a novel artificial injury perception device based on an Ag/HfOx/ITO/PET flexible memristor is designed to address the limitations of current technologies in multimodal perception and environmental adaptability. The memristor exhibits excellent resistive switching (RS) performance and mechanical flexibility under different bending angles (BAs), temperatures, humid environment, and repetitive folding conditions. Further, the device demonstrates the multimodal perception and conversion capabilities toward voltage, mechanical, and thermal stimuli through current response tests under different conditions, enabling not only the simulation of artificial injury perception but also holds promise for monitoring and controlling the movement of robotic arms. Moreover, the logical operation capability of the memristor-based reconfigurable logic (MRL) gates is also demonstrated, proving the device has great potential applications with sensing, storage, and memory functions. Overall, this study not only provides a direction for the development of the next-generation flexible multimodal sensors, but also has significant implications for technological advancements in many fields such as robotic arms, electronic skin (e-skin), and medical monitoring.

High-speed Ta2O5-based threshold switching memristor for LIF neurons

Due to their high similarity to biological ion channels, low power consumption, small footprint, and the fact that they do not require reset circuits, threshold switching memristors have been intensively studied for simulating neurons in neuromorphic chips. Switching speed is one of the key challenges which limit the application of threshold switching memristors in chips. In this study, Ta2O5 threshold switching memristors with high switching speeds were prepared by doping with silver. The results show that 14 wt. % Ag doped Ta2O5 threshold switching memristors exhibit excellent bi-directional threshold switching performance, featuring fast switching speeds (<20 ns, <18 ns), low leakage currents (<10 pA), and high switching ratio (>107). According to the field nucleation theory, the rapid switching speed can be attributed to the low nucleation energy (0.26 eV) of silver within the Ta2O5 matrix, which is achieved by incorporating 14 wt. % Ag during the doping process. Based on Pspice, a LIF (leaky integrate-and-fire) neuron based on the silver nanoparticles doped Ta2O5 threshold switching memristors is built, and its firing function has been simulated. The results show that the LIF neuron with a short switching time is able to excite pulse spiking with high frequencies. These results demonstrated that the silver nanoparticles doped Ta2O5-based threshold switching memristors hold significant potential for constructing high-speed artificial neural networks.

Reverse Mode Polymer Stabilized Cholesteric Liquid Crystal Flexible Films with Excellent Bending Resistance.

The reverse-mode smart windows, which usually fabricated by polymer stabilized liquid crystal (PSLC), are more practical for scenarios where high transparency is a priority for most of the time. However, the polymer stabilized cholesteric liquid crystal (PSCLC) film exhibits poor spacing stability due to the mobility of CLC molecules during the bending deformation. In this work, a reverse-mode PSCLC flexible film with excellent bending resistance was fabricated by the construction of polymer spacer columns. The effect of the concentration of the polymerizable monomer C6M and chiral dopant R811 on the electro-optical properties and polymer microstructure of the film were studied. The sample B2 containing 3 wt% of C6M and 3 wt% R811 presented the best electro-optical performance. The electrical switch between transparent and opaque state of the flexible PSCLC film after bending not only indicated the excellent electro-optical switching performance, but also demonstrated the outstanding bending resistance of the sample with polymer spacer columns, which makes the PSCLC film containing polymer spacer columns have a great potential to be applied in the field of flexible devices.

Electro-active superposed optical ring vortex beams based on PEDOT: SULF composite metasurface

Electro-active metasurfaces with high efficiency and ultra-small scale active control of integrated components are crucial for developing complex optical devices. Recent attention has focused on vortex beams with ring intensity distribution independent of topological charge, enhancing particle manipulation and fiber optic transmission efficiency. This paper presents a composite metasurface utilizing the conductive polymer PEDOT: SULF, capable of generating and dynamically switching between two types of superposed ring vortex beams. We investigate their characteristics and polarization detection capabilities. Accurate detection of major axis, ellipticity, and handedness of incident polarized light is achieved based on the two superposed ring vortex beams. The metasurface exhibits excellent switching performance, enabling flexible tuning of the ring vortex beams on demand. Additionally, we demonstrate the metasurface's good polarization detection performance for incident polarized light as an application example. The PEDOT: SULF composite metasurface holds great potential in polarization detection, quantum science, and compact photonics-integrated devices.

First-Principles Prediction of High and Low Resistance States in Ta/h-BN/Ta Atomristor.

Two-dimensional (2D) materials have received significant attention for their potential use in next-generation electronics, particularly in nonvolatile memory and neuromorphic computing. This is due to their simple metal-insulator-metal (MIM) sandwiched structure, excellent switching performance, high-density capability, and low power consumption. In this work, using comprehensive material simulations and device modeling, the thinnest monolayer hexagonal boron nitride (h-BN) atomristor is studied by using a MIM configuration with Ta electrodes. Our first-principles calculations predicted both a high resistance state (HRS) and a low resistance state (LRS) in this device. We observed that the presence of van der Waals (vdW) gaps between the Ta electrodes and monolayer h-BN with a boron vacancy (VB) contributes to the HRS. The combination of metal electrode contact and the adsorption of Ta atoms onto a single VB defect (TaB) can alter the interface barrier between the electrode and dielectric layer, as well as create band gap states within the band gap of monolayer h-BN. These band gap states can shorten the effective tunneling path for electron transport from the left electrode to the right electrode, resulting in an increase in the current transmission coefficient of the LRS. This resistive switching mechanism in monolayer h-BN atomristors can serve as a theoretical reference for device design and optimization, making them promising for the development of atomristor technology with ultra-high integration density and ultra-low power consumption.

Realization of Selector‐Memory Bi‐Functionality with Self‐Current Regulation Utilizing Poly‐Crystalline Based GST Electrolyte for Memristor Hardware Development

AbstractConductive bridge random‐access memory (CBRAM) are two terminal devices that offer excellent switching performance. In addition, CBRAM shows various switching modes, including volatile threshold switching (TS) and nonvolatile threshold switching (N‐TS). These properties expand its applications to memory, selector, biological synapses, and neurons. However, due to the uncontrollable behavior of stochastic switching between TS and N‐TS in CBRAM devices, a novel approach is needed to improve the switching performance of CBRAM. Moreover, conventional devices that have different stacking between TS and N‐TS increase fabrication cost and worsen the device yield. Here, the selector‐memory bi‐functionality with self‐current regulation effect of Ag‐inserted Ge2Sb2Te5 (GST) thin films is demonstrated. Selector‐memory bi‐functionality, having TS behavior with an adjustable on/off current, with confined conductive filaments (CFs) improves the uniformity and reduces the fabrication cost by implementing TS/N‐TS in a single stack. From the material analysis, it becomes evident that confined Ag‐based CFs within GST films are key factors for realizing selector‐memory bi‐functionality. The selector‐memory bi‐functionality is achieved through the reaction of Ag metal cations with non‐bonded Te atoms in GST film depending on field polarity. These results suggest that the Ag‐inserted GST film contributes to the development of large‐scale nonvolatile memory and neuromorphic application.

Bandgap regulation and doping modification of Ga2-x Cr x Se3 nanosheets.

Ga2Se3, an important direct wide bandgap semiconductor with excellent optoelectronic properties, has wide application potential in the fields of photodetectors, photoelectric sensors and solar cells. Herein, we describe the synthesis of Ga2Se3 semiconductor nanoparticles using a high temperature organic liquid phase method. Post-annealing treatment at different temperatures can not only improve the crystallinity of Ga2Se3 nanoparticles, but also regulate its optical band gap ranging from 2.50 to 2.80 eV. We further synthesized Ga2-x Cr x Se3 nanosheets by doping CrCl3·6H2O in the reaction process. By adjusting the Cr doping concentration, Ga2-x Cr x Se3 nanosheets can achieve a continuously tunable band gap in the range of 2.23 eV to 2.42 eV. Both Ga2-x Cr x Se3 nanosheets and Ga2Se3 nanoparticles exhibit excellent and stable photoelectric switching performance. With Cr doping, Ga2-x Cr x Se3 exhibits reduced Nyquist impedance and enhanced electrocatalytic activity, which is attributed to its ultrathin nanosheet morphology and large specific surface area. In addition, the diamagnetic behavior of pure Ga2Se3 changes to ferromagnetism with different Cr doping concentrations, and its magnetization is as high as 18.0 emu g-1 at x = 0.4. These findings demonstrate that Ga2-x Cr x Se3 nanosheets have significant potential in future optoelectronic and magnetoelectric applications.

Controllable analog-to-digital bipolar resistive switching behavior and mechanism analysis in δ-MnO2-based memristor

Memristor is one of the most emerging electronic components to realize synaptic functions in the neuromorphic computing. Memristor with controllable analog-to-digital resistive switching behaviors has the potential to considerably accelerate the realization of high-performance neuromorphic computing. In this work, a memristor with Ag/δ-MnO2/Ti structure was fabricated, and an analog-to-digital resistive switching behavior with voltage regulation was demonstrated. Memristive switching with analogue characteristics can generate a gradual increase in conductance at low voltage of less than 1.3 V to aid in the building of artificial synapses. The Ag/δ-MnO2/Ti memristor with excellent digital resistive switching performance can be applied for data storage and in-memory computation at voltage windows of higher than 1.3 V. Furthermore, the resistive switching mechanism was analyzed by employing the first-principle calculation. The main reason for the emergence of digital memristor characteristics is the Ag+ ions can enter to the δ-MnO2 layer driven by a larger voltage and continue to cluster and form conductive filament. This work enriches the application of analog-to-digital bipolar memristor in neuromorphic computing, and facilitates further realization of memristor in low-power and high-density circuit integration.

Enhanced memristor performance via coupling effect of oxygen vacancy and ferroelectric polarization

As a new type of nonvolatile memory, the resistive memristor has broad application prospects in information storage and neural computing based on its excellent resistive switching (RS) performance. At present, it is still a great challenge to improve both ferroelectric polarization and leakage current to achieve a high RS on/off ratio of ferroelectric memristors. Herein, epitaxial Pb(Zr0.40Ti0.60)O3 (PZT) thin films with low content Ca doping were deposited on the Nb:SrTiO3 substrate to prepare PCZT/NSTO heterostructures and their RS behaviors were studied. The research findings show that compared with pure PZT film, the ferroelectric polarization of 1-mol%-Ca-doped PZT film is slightly improved, while the leakage current is increased by three orders of magnitude. Therefore, the RS on/off ratio reaches 2.5 × 105, about three orders of magnitude higher than pure PZT films. The theoretical analysis reveals that the RS behavior of PCZT/NSTO heterostructures is controlled by the PCZT/NSTO interfacial barrier and the space charge-limited current mechanism. Our results demonstrate that the ferroelectricity and electricity of ferroelectric thin films can be improved simultaneously by doping low-content Ca ions to increase the RS performance, which provides a good reference for the development of high-performance ferroelectric memristor devices.

Improved Hole Injection in Hybrid Light‐Emitting Transistors Incorporating Lithium and Copper(II) Poly(Styrene Sulfonate)

AbstractLight‐emitting transistors (LETs) are optoelectronic devices that perform switching and light‐emitting functions in a single device. Hybrid LETS (HLETs) using inorganic metal oxide semiconductors as the transport layer with organic emissive layers and hole‐injection layers (HILs) combine the excellent switching performance of metal oxides with the flexibility and tunability of organic semiconductors. However, the efficiency of n‐HLETs typically suffers from unbalanced electron and hole injection. To overcome this issue, two hybrid polyelectrolytes—lithium poly(styrene sulfonate) (Li:PSS) and copper(II) poly(styrene sulfonate) (Cu:PSS)—are investigated as HILs in HLETs. HLETs employing Cu:PSS interlayers exhibit significantly enhanced brightness values of up to 4.89 × 103 cd m−2 and an external quantum efficiency (EQE) of 0.45%, compared to HLETs without HIL (no emission) and pristine poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) (2.17 × 102 cd m−2 with an EQE of 0.01%). To understand how the HILs influence the performance, ultraviolet photoelectron spectroscopy (UPS) analysis and photoluminescence (PL) quenching studies are performed, which reveal improved energy band structure and reduced quenching using metal:PSS HILs. This work provides useful information about the function that polyelectrolyte HILs perform in HLET devices which may be exploited to develop new materials and applied in other types of optoelectronic devices.

Nonvolatile resistive switching in lead-free La2CoMnO6-based memory device

Dense and flat La2CoMnO6 films as the resistive switching functional layer were deposited on n-type Si substrates by sol–gel method. Excellent bipolar resistive switching performance was observed in the Au/La2CoMnO6/Si device for the first time. The high and low resistance states with a ratio of ∼105 could be maintained for more than 1.4 × 104 s and 750 cycles without significant degradation at room temperature. The bipolar resistive switching effect could be sustained within a wide temperature range of 220 K∼300 K. Electrical conduction analysis indicated that the resistive switching behavior in La2CoMnO6 films was primarily controlled by space-charge-limited current mechanism which originated from the change of oxygen vacancies. Density functional theory calculations indicated that the conductive ability of La2CoMnO6 films was promoted with increasing concentration of oxygen vacancies. Moreover, it is found that the modulation of the barrier located at the Au/La2CoMnO6 interface was responsible for the resistive switching under applied bias voltages.

Nano t-Se Peninsulas Embedded in Natively Oxidized 2D TiSe2 Enable Uniform and Fast Memristive Switching.

Memristive devices, regardless of their potential applications in memory and computing scenarios, still suffer from large cycle-to-cycle and device-to-device variations due to the stochastic growth of conductive filaments (CFs). In this work, we fabricated a crossbar memristor using the 2D TiSe2 material and then oxidized it into TiO2 in the atmosphere at a moderate temperature. Such a mild oxidation approach fails to evaporate all Se into the air, and after further annealing using thermal or electrical stimulations, the remnant Se atoms gather near the interfaces and grow into nanosized crystals with relatively high conductivity. The resulting peninsula-shaped nanocrystals distort the electric field, forcing CFs to grow on them, which could largely confine the location and length of CFs. As a result, this two-terminal TiSe2/TiO2/TiSe2 device exhibits excellent resistive switching performance with a fairly low threshold voltage (Vset < 0.8 V, Vreset > 0.55 V) and high cycle-to-cycle consistency, enabling resistive switching at narrow operating variations, e.g., 500 ± 48 and 845 ± 39 mV. Our work offers a new approach to minimize the cycle-to-cycle stochasticity of the memristive device, paving the way for its applications in data storage and brain-inspired computing.

Geometric, Electronic, and Transport Predictions on Two-Dimensional Semiconducting Silicon with Kagome Lattice: Implications for Nanoscale Field-Effect Transistor Applications

Two-dimensional (2D) semiconducting silicon (Si) is significant for the development of micro/nanoelectronics because of their compatibility with the current Si-based technology and the advantages common to 2D electronic materials. Here, by focusing on the kagome lattice (KL), we design a set of semiconducting 2D KL-Si for nanoscale field-effect transistor (FET) applications. First-principles calculations demonstrate that both stable geometric properties and tunable semiconducting electronic properties can be obtained for the 2D KL-Si with different thicknesses. The 2D KL-Si features electronic band gaps ranging from 2.82 to 1.36 eV as a function of increasing the layer thickness and hole/electron mobility as large as about 103 cm2·V–1·s–1. By applying the KL-Si to nanoscale FETs, we obtain giant negative differential resistances with peak-valley ratios over 107 and excellent switching performance fulfilling the requirements of the International Technology Roadmap for Semiconductors. Our study demonstrates the importance of kagome topology in the design of 2D Si crystals with excellent semiconducting properties as well as their promising application in nanoelectronic devices.

Ultralow Operating Voltage Nb2O5-Based Multilevel Resistive Memory with Direct Observation of Cu Conductive Filament

Amorphous Nb2O5 is proposed as the resistive switching layer for conductive bridge random access memory. The Nb2O5 device is fabricated with the top Cu and bottom Au electrodes, which is fabricated at a fully room temperature process, exhibiting excellent resistive switching performance with an on/off ratio of up to 105 and ultralow operating voltage. The multilevel resistive switching characteristic can be rationally demonstrated by changing the compliance current in the Nb2O5 device. Each level of the resistance state is uniform with distinguishable read windows. The reset voltage reduces significantly as the compliance current decreases, which is merely 0.002 V when the compliance current is 10–5 A. An approach of the broken-down device is elaborately developed to firmly identify the migration of Cu and the existence of a Cu conductive filament and to explain the ultralow operating voltage. Amorphous Nb2O5 devices exhibit excellent resistive switching performance, proving it is a promising material for memory applications.

An Integrated Gate Driver Based on SiC MOSFETs Adaptive Multi-Level Control Technique

In HV (high-voltage) and HF (high-frequency) applications, SiC (silicon carbide) MOSFET is widely used for its small parasitic characteristics and fast switching speed. Using discrete devices on PCB, the active gate driver is usually adopted to restrict EMI (electromagnetic interference) noise. This method could achieve a limited switching performance improvement, and many disadvantages still exist. In this paper, the integrated adaptive multi-level gate driver is presented to improve the switching performance of SiC MOSFET in HV and HF applications. The proposed gate driver is realized on the chip using critical techniques such as <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">dV/dt</i> noise attenuation, high-speed circuit, and anti-false triggering mechanism. Then, the proposed gate drive is fabricated in a 0.18 <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$\mu$</tex-math> </inline-formula> m BCD process and occupies a 4.16 mm <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$^{2}$</tex-math> </inline-formula> active area. The experimental results show that SiC MOSFET can achieve a 200 ns switching time, 0.8 mJ energy losses, no more than 15 V/ns average <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">dV/dt</i> noises, and 1.5 A/ns average <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">di/dt</i> noises under a 600 V power supply and a 33 A load. SiC MOSFET can also realize the excellent switching performance at different load currents from 15 A to 90 A by using the proposed adaptive multi-level gate driver.

Inorganic Solid-State Nonlinear Optical Switch with a Linearly Tunable Tc Spanning a Wide Temperature Range.

Nonlinear optical (NLO) switch materials that turn on/off second-harmonic generation (SHG) at a phase transition temperature (Tc ) are promising for applications in the fields of photoswitching and optical computing. However, precise control of Tc remains challenging, mainly because a linearly tunable Tc has not been reported to date. Herein, we report a unique selenate, tetragonal P 21 c [Ag(NH3 )2 ]2 SeO4 with a=b=8.5569(2) Å and c=6.5208(2) Å that exhibits a strong SHG intensity (1.3×KDP) and a large birefringence (Δnobv. =0.08). This compound forms a series of isostructural solid-solution crystals [Ag(NH3 )2 ]2 Sx Se1-x O4 (x=0-1.00) that exhibit excellent NLO switching performance and an unprecedented linearly tunable spanning 430 to 356 K. The breaking of localized hydrogen bonds between SeO4 2- and the cation triggers a phase transition accompanied by hydrogen bond length changes with increasing x and a linear change in the enthalpy .

Inorganic Solid‐State Nonlinear Optical Switch with a Linearly TunableTcSpanning a Wide Temperature Range

AbstractNonlinear optical (NLO) switch materials that turn on/off second‐harmonic generation (SHG) at a phase transition temperature (Tc) are promising for applications in the fields of photoswitching and optical computing. However, precise control ofTcremains challenging, mainly because a linearly tunableTchas not been reported to date. Herein, we report a unique selenate, tetragonalP21c[Ag(NH3)2]2SeO4witha=b=8.5569(2) Å andc=6.5208(2) Å that exhibits a strong SHG intensity (1.3×KDP) and a large birefringence (Δnobv.=0.08). This compound forms a series of isostructural solid‐solution crystals [Ag(NH3)2]2SxSe1−xO4(x=0–1.00) that exhibit excellent NLO switching performance and an unprecedented linearly tunablespanning 430 to 356 K. The breaking of localized hydrogen bonds between SeO42−and the cation triggers a phase transition accompanied by hydrogen bond length changes with increasingxand a linear change in the enthalpy.