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Dan Guo, Huiwen Wang, Liu Yang, Weikang Dong, Boyu Xu, Shuang Du, Xuyan Rui, Qingrong Liang, [Kenji Watanabe](https://orcid.org/0000-0003-3701-8119), [Takashi Taniguchi](https://orcid.org/0000-0002-1467-3105), Zhiwei Wang, Yan Xiong, Wei Jiang, Jiadong Zhou, Shoujun Zheng

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This document is the Accepted Manuscript version of a Published Article that appeared in final form in ACS Nano, copyright © 2025 American Chemical Society. To access the final published article, see https://doi.org/10.1021/acsnano.4c13215.[In Copyright](http://rightsstatements.org/vocab/InC/1.0/)

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[Anisotropic Resonant Tunneling in Twist-Stacked van der Waals Heterostructure](https://mdr.nims.go.jp/datasets/b786beed-21e5-4fca-88cf-a49ca6746ca3)

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1Anisotropic resonant tunneling in twist-stackedvan derWaals heterostructureDan Guo1, Huiwen Wang1, Liu Yang1, Weikang Dong1, Boyu Xu1, Shuang Du1, XuyanRui1, Qingrong Liang1, Kenji Watanabe2, Takashi Taniguchi2, Zhiwei Wang1,*, YanXiong3,*, Wei Jiang1,*, Jiadong Zhou1, Shoujun Zheng1,*1Centre for Quantum Physics, Key Laboratory of Advanced Optoelectronic QuantumArchitecture and Measurement (MOE), School of Physics, Beijing Institute ofTechnology, Beijing, 100081, China2National Institute for Materials Science, 1-1 Namiki, Tsukuba 303-0044, Japan3Analysis&Testing center, Beijing Institute of Technology, Beijing, 100081, ChinaCorresponding email: zhiweiwang@bit.edu.cn, xiongyan@bit.edu.cn,wjiang@bit.edu.cn, szheng@bit.edu.cnABSTRACT: Resonant tunneling, with energy and momentumconservation, has been extensively studied in two-dimensional van derWaals heterostructures and has potential applications in band structureprobing, multi-valued logic, and oscillators. Lattice alignment is crucialin resonant tunneling transistors (RTTs) for achieving the negativedifferential resistance (NDR) with a high peak-to-valley ratio (PVR)because twist angle-induced momentum mismatch can break the resonanttunneling condition. Here, we report anisotropic resonant tunneling intwist-stacked ReSe2/h-BN/ReSe2 RTTs, where the PVR exhibits a strongdependence on the twist angle between the two ReSe2 layers, reaching amaximum at the twist angle of 102°. Theoretical calculations suggest thatthe twist angle modulates the joint density of states of the two anisotropicbands in ReSe2 layers during the tunneling process, significantly2suppressing the valley current and thereby enhancing the PVR. DoubleNDR peaks were observed in twist-stacked RTTs, which are attributed tothe interband resonant tunneling. Moreover, our twist-stacked RTTs areutilized in multi-bit inverters and adjustable self-powered photodetectors,shedding light on the design of high-performance RTTs andphotodetectors via twist-stacked engineering.Keywords: two-dimensional material, anisotropic band, resonanttunneling transistor, van der Waals heterostructure, negative differentialresistance, peak-to-valley ratio3INTRODUCTIONResonant tunneling (RT), which involves particle tunneling througha barrier with energy and momentum conservation, exhibits a negativedifferential resistance (NDR), which can be applied in steep-slopeswitches, oscillators, high-frequency amplifiers, multi-valued logic(MVL), and low-power devices.1-6 Traditional three-dimensional (3D) RTdevices with double-barrier quantum well structure face challenges suchas lattice mismatch, impurities, and complex sub-bands,7,8 whichconstrain the peak-to-valley ratio (PVR). In contrast, two-dimensional(2D) RT devices present several advantages for fabricating ideal devicestructures, such as atomically flat transport channels, clean interfaceswithout covalent bonds, and the feasibility of material selections,ensuring superior performances in RT devices.9-12 Consequently, the PVRof 2D resonant tunneling transistors (RTTs) was theoretically predicted tobe several orders of magnitude higher than that of 3D RT devices.13However, the PVR in reported 2D RTTs14,15 remains relatively low due tohigh valley current induced by band tail states, with a maximum of ~9observed in twisted black phosphorus (BP) homostructure via thequantum well tunneling mechanism.16 Therefore, further efforts arerequired to improve PVR by facilitating device quality and exploringnovel RT mechanisms.17Lattice orientation plays a critical role in determining the intrinsic4properties and performances of 2D twistronic devices. Modulating thetwist angle through stacking engineering in 2D van der Waals (vdW)heterostructures has led to significant advancements in superconductivity,ferromagnetism, and ferroelectricity.18-20 However, the large twist angle istypically avoided in RTTs because they can introduce momentummismatch, necessitating compensation through phonons, photons, orplasmons.21-26 For example, precise alignment of lattice orientationsbetween the top and bottom layers is required to achieve NDR inMoS2-based RTT.27 A small twist angle is typically introduced ingraphene/h-BN/graphene devices to observe the NDR peak at a certainvoltage.28,29 Although NDR has been investigated in twisted BP, the PVRin this device is independent on the twist angle.16Actually, the twist angleprovides an additional degree of freedom to precisely control interlayercoupling and band alignment, which has not been thoroughly explored inRTTs.RT in 2D RTTs provides a valuable means to probe the intrinsicproperties of 2D materials and develop advanced applications as bandalignments and carrier densities of 2D materials can be easily modulatedby electric field and light illumination.30-33 For instance, quantum statesand chirality of graphene can be explored by manipulating latticeorientations in RTTs.34,35 Furthermore, multiple NDR peaks caused by RTcan be leveraged for information storage with multiple logic states,36,375highlighting the potential of RTTs for advanced storage andphotodetection applications.In this study, we fabricated twist-stacked RTTs (TS-RTTs) based onReSe2/hexagonal boron nitride (h-BN)/ReSe2 vdW heterostructures withvarious twist angles between the top and bottom ReSe2 layers. Unliketraditional 2D RT devices, our TS-RTTs devices exhibit twistangle-dependent anisotropic resonant tunneling (ART) with a maximumPVR of 3.2 at a twist angle of 102°. Theoretical calculations reveal thatthe band alignment between anisotropic bands generates twistangle-dependent joint density of states (JDOS), suppressing the valleycurrent and improving the PVR. The NDR behavior is also significantlyinfluenced by temperature and light illumination. Additionally, doubleNDR peaks were observed in TS-RTTs, which is attributed to RT betweenmultiple anisotropic sub-bands of ReSe2. Furthermore, we developed aternary inverter for MVL and a tunable self-powered photodetector basedon the TS-RTTs.RESULTSAND DISCUSSIONAnisotropic Resonant Tunneling.Momentum conservation in vdW heterostructure can be effectivelymanipulated by altering the lattice orientation through the twist angle,providing an additional degree of freedom to modulate RT conditions. Indistorted 1T rhenium diselenide (1T’-ReSe2), rhenium atoms form6Re-chains along the a-axis, resulting in an in-plane anisotropy (shown inFigure 1a). Theoretical calculations indicate that the conduction bands of1T’-ReSe2 exhibit significant band anisotropy, consistent with the C2symmetry of the T’ phase ReSe2 (see Figure 1b). The anisotropy shows a40° angle difference between the first conduction band (CB-1) and thesecond conduction band (CB-2) at Gamma (Γ) point. This uniqueanisotropic band structure enables precise tuning of momentum matchingand interband tunneling by designing vdW heterostructures with tunabletwist angles.ReSe2 is an n-type semiconductor with electron mobility of ~5.66cm2V-1S-1 (see Figure S1) where the conduction band minimum is locatedat the Γ point (shown in Figure 1c). In ReSe₂/h-BN/ReSe₂ vdWheterostructure, electrons near the Γ point can maintain momentumconservation even at a large twist angle of two ReSe₂ layers, enabling aRT. Simultaneously, the momentum mismatch significantly reduces theJDOS in other regions of momentum space, leading to a decrease invalley current (as shown in Figure 1d). Therefore, it is theoreticallyfeasible to enhance the PVR in some specific TS-RTTs via precise controlof the twist angle.7Figure 1. ART based on the anisotropic bands of 1T’-ReSe2. (a) Top viewof the atomic structure of 1T’-ReSe2, exhibiting the anisotropic latticeorientations. (b) Calculated band maps of the first conduction band (CB-1,left) and the second conduction band (CB-2, right), clearly demonstratingthe strong in-plane anisotropy. (c) Band structures of monolayer ReSe2,showing the conduction band minimum at the Γ point. (d) Schematicband alignments of the ReSe2/h-BN/ReSe2 RTTs with 40° (top left) and108° (top right) twist angles. The JDOS in the 108° TS-RTT (red pointsin bottom right) is lower than that in the 40° TS-RTT (red shadow inbottom left). ART is expected in the TS-RTT with a specific twist angleby suppressing the valley current.Negative differential resistance in a 102° TS-RTT.To investigate ART, we prepared a twist-stacked ReSe2/h-BN/ReSe28vdW heterostructure with a twist angle of 102° (device 1). The schematicof TS-RTT is shown in Figure 2a, where a bias voltage is applied to thebottom ReSe2 layer and a back gate voltage is used to tune the carrierdensities and Fermi levels of both the top and bottom ReSe2. The TS-RTTis composed of two ReSe2 flakes and a four-layer h-BN flake (see theoptical image in Figure 2b). The twist angle of the TS-RTT wasdetermined to be 102° by measuring the polarization-dependent Ramanspectra of 127 cm-1 mode (shown in Figure 2c and Figure S1). Figure 2dshows the cross-section image of transmission electron microscopy(TEM), indicating the twist-stacked order between the top and bottomReSe2 layers, and the top and bottom ReSe2 layers were identified toconsist of approximately 5 layers and 4 layers, respectively. Monolayerand bilayer ReSe2 are not working well in our experiments which may bedue to the instability of ReSe2 and interfacial disorders.Clear NDR peaks are observed in the 102° TS-RTT at various gatevoltages of 20 V, 40 V, 60 V, and 80 V at 10 K (shown in Figure 2e). Thepositions of these NDR peaks shift to smaller bias voltages withincreasing gate voltage (as shown in Figure 2g). This trend is furtherevident in the conductance map as a function of bias and gate voltage,illustrated in Figure 2f. Notably, the PVR improves with increasing gatevoltage, as summarized in Figure 2g.It is noteworthy that the NDR behavior in our TS-RTT exhibits a9strong dependence on temperature (shown in Figure 2h), while it isweakly affected by temperature in the previously reported RTTs (Figure2i).15,27 Figure 2h shows that NDR peaks progressively weaken andeventually disappear with increasing temperature from 10 K to 300 K at afixed Vg of 40 V. Moreover, both the tunneling current and NDR areinfluenced by light illumination with a 520 nm laser, which is displayedin Figure 2j at various laser powers of 0.6 W, 6.1 W, and 18.2 W at10 K. The sensitivity of NDR peaks to temperature and light illuminationsuggests that the NDR behavior is associated with the specific bandalignment and the twist angle-induced momentum mismatch. The appliedbias voltage drives the Fermi level of the conduction band in the topReSe2 to align with the corresponding conduction band in the bottomReSe2, producing a RT. As the bias voltage increases, band misalignmentand momentum mismatch occur in the TS-RTT, leading to a sharpdecrease of the PVR.10Figure 2. Negative differential resistance in a 102° twist-stacked RTT. (a)Schematic of the ReSe2/h-BN/ReSe2 TS-RTT, where a bias voltage isapplied to the bottom layer of ReSe2 and RT occurs at the overlappingregion (shown in the red region). (b) Optical image of the 102° TS-RTT(device 1), with orange and green pentagons indicating the locations forRaman testing. Two ReSe2 layers are separated by a few-layer h-BN (bluedashed line). (c) Polarization-dependent Raman intensity of both top(orange circles) and bottom (green circles) ReSe2 layers at Raman shift of127 cm-1. Fitted lines (orange and green lines) of Raman data show thatthe twist angle between the two ReSe2 is about 102°. (d) TEMcross-section image of the TS-RTT, showing the relative latticeorientation of two ReSe2. (e) Tunneling current as a function of bias11voltage at different gate voltages with T=10 K, clearly demonstrating thegate-dependent NDR. (f) Conductance map of the 102° TS-RTT withT=10 K, showing a trend of NDR peak with gate voltage. (g) Summary ofPVR and NDR peak positions as a function of gate voltage with T=10 K.(h) Tunneling current as a function of bias voltage at various temperatureswith Vg=40 V, showing that NDR is sensitive to temperature. (i)Comparison of temperature-dependent PVR between the TS-RTT withVg=80 V and an untwisted RTT based on monolayer MoS2. (j) Tunnelingcurrent as a function of bias voltage under 520 nm light illumination withvarious laser powers at Vg=40 V and T=10 K.Double NDR Peaks in TS-RTT.Based on the ART between anisotropic conduction bands in ReSe2,multiple NDR peaks in TS-RTTs are expected. TS-RTTs with varioustwist angles were fabricated and double NDR peaks were observed(device 2 and device 3). Twist angles of device 2 and device 3 aredetermined to be 87° (Figure S2) and 37° (Figure S4) bypolarization-dependent Raman spectra. In contrast to device 1, bothdevice 2 and device 3 exhibit two gate-dependent NDR peaks (as shownin Figures 3a and 3d) and distinguishable NDR regions (Figures 3b and3e) at 10 K. Although the NDR peaks weaken with increasingtemperature in Figure 3c at a fixed gate voltage of 80 V, it is worth notingthat the second NDR peak decays faster than the first, suggesting the12different origins between the two peaks (more information of devices 2and 3 can be found in Figures S3 and S5). Similar to device 1, doubleNDR peaks and conductance of devices 2 and 3 show a strongdependence on gate voltage, temperature, and light illumination.Capacitance-voltage (C-V) measurement is also an efficient tool to probeNDR peaks as RT-induced conductance variation affects the capacitanceof vdW heterostructure. Even though only two NDR peaks were observedin the I-V measurement in device 3, three NDR peaks were observed inthe C-V measurement at 10 K (Figure S5g), suggesting that C-Vmeasurement is a more sensitive tool to identify the conduction band ofReSe2.The observed double NDR peaks can be attributed to the RTbetween different conduction bands of ReSe2. There are severalconduction bands at the Γ point according to our theoretical calculations(Figure 1c). The second NDR peak arises from the band alignmentbetween CB-1 in the top layer and CB-2 or the higher conduction bandsin the bottom layer (shown in Figure 3f). The band dispersion relationdetermines the RT condition, resulting in the NDR peaks being sensitiveto temperature and light illumination. Specifically, the second NDR peakin the RTT with the twist angle of 37˚ is attributed to the 40° anisotropicangular difference between the first and second conduction bands ofReSe2. The double peak observed at twist angle of 87° might originate13from RT between the first conduction band at the Γ point of one ReSe2layer and other conduction bands (like the third conduction band) of theother ReSe2 layer, which needs further investigation.Figure 3. Double NDR peaks in TS-RTTs. (a) Tunneling current as afunction of bias voltage at different gate voltages in an 87° TS-RTT withT=10 K, showing double NDR peaks. (b) Conductance map of the 87°TS-RTT with T=10 K, showing NDR peaks change with gate voltage. (c)Tunneling current as a function of bias voltage for the 87° TS-RTT atdifferent temperatures with Vg=80 V, exhibiting that the second peak ismore sensitive to temperature. (d) Tunneling current as a function of biasvoltage at different gate voltages for a 37° TS-RTT with T=10 K,showing similar double NDR peaks. (e) Summary of PVR and NDR peakpositions as a function of gate voltage for the 37° TS-RTT with T=10 K.(f) Schematic of the band alignment, explaining the origin of the double14NDR peaks.Twist Angle Dependent PVR.Interestingly, NDR is also observed at 10 K in TS-RTTs with varioustwist angles, including 1.8° (Figures S9 and S10), 31° (Figures S12 andS13), 45° (Figures S14 and S15) and 158° (Figures S6-S8) shown inFigures 4a-d. More devices encapsulated with h-BN were also fabricatedincluding twist angles of 7.5° (Figure S16 and S17), 10° (Figure S18 andS19), 140° (Figure S20 and S21), and 160° (Figure S22 and S23). Thethicknesses of ReSe2 in those devices are around 4~5 layers, which issimilar to that of device 1 (see the AFM images in the supportinginformation). NDR of all devices exhibits a strong dependence on gatevoltage, temperature, and light illumination.We can see that the tunneling current of 1.8° TS-RTT is the largest(Figure 4a), which can be attributed to the largest JDOS with momentumconservation. It is clear that PVR strongly depends on the twist angle andreaches a maximum of 102° by summarizing PVR values of TS-RTTswith different twist angles (shown in Figure 4e). Note that the absolutevalue of tunneling current decreases by two orders of magnitude when alarge twist angle is introduced. However, the valley current decreasesfaster than the peak current, resulting in an enhancement of PVR.To simulate the tunneling current through the h-BN layer, wecalculated the tunneling probability between the top and bottom ReSe215layers of a 108° device as shown in Figure 4f (see details in methods).The external electric field drives the Fermi level to the second conductionband, leading to the appearance of the second NDR peak, which agreesvery well with double NDR peaks observed in the experimental results(Figure 4e). Further, we calculated the tunneling probability by varyingthe twist angle between the top and bottom ReSe2 layers (shown inFigures S24 and S25), where the valley current is determined by thetunneling probability of all conduction bands between the top and bottomReSe2 layers. Due to the anisotropy of the ReSe2 structure, the tunnelingprobability depends not only on the energy matching condition but alsothe twist angle-induced momentum matching condition. The bandsbetween the top and bottom ReSe2 layers can reach the largest (smallest)momentum mismatch when the anisotropic angle is about perpendicular(parallel) to each other. For example, the PVR reaches a maximum whenthe valley current reaches its minimum value at the twist angle of 108° asJDOS is lowest (shown in Figure 4g and Figure S26), which qualitativelyagrees well with our experimental results.PVR in our tunneling devices is determined by both the peak andvalley currents. Due to the nature of the Γ point (k=0), the momentum ofelectrons near the Γ point is insensitive to the twist angle so that we canobserve RT at the Γ point even with a large twist angle between the twolayers of ReSe2 (Figure S27). The high PVR is attributed to the16suppression of valley current via twist angle-induced momentummismatch and twist angle-dependent JDOS between the top and bottomlayers. In addition, two bands are predicted to be the largest mismatch atthe twist angle of 18° which can also result in the smallest valleytunneling probability and a large PVR. However, the PVR inexperimental devices around 18° is not greatly improved, which might beattributed to the high valley current produced by the RT from othermomentum spaces. The quantitative mismatch between experimental andtheoretical results at smaller twisting angles close to 0° might beattributed to interfacial scattering-induced direct tunneling and largeleakage current. Moreover, the momentum match in all momentum spacein the RTT with a 1.8° twist angle increases the tunneling probability ofelectrons, resulting in a large valley tunneling current and the mismatchbetween experimental and theoretical results.17Figure 4. Summary of NDR at various twist angles at 10 K. (a-d)Tunneling currents as a function of bias voltage for TS-RTTs with twistangles about 1.8° (a), 31° (b), 45° (c), and 158° (d), respectively. (e)Summary of PVR as a function of twist angle, showing that PVR isenhanced in the TS-RTT with a large twist angle. The green dashed line isfor guidance. (f) Calculated tunneling probability as a function of energyshift for TS-RTT with a twist angle of 108°. (g) Calculated PVR as afunction of twist angle, which is consistent with the experimental resultsin (e).Ternary MVL and Photo Response of TS-RTTs.MVL has garnered significant attention due to its potential forstoring more data in smaller spaces compared to binary logic. Ingate-controlled RT devices, negative transconductance can be achievedthrough NDR. Interestingly, the transfer curve of device 4 (with a twistangle of 158°) exhibits anti-bipolarity at 10 K (as shown in Figures S8aand S8b). Inspired by this, we constructed a ternary inverter with threelogic states as depicted in Figure 5a to achieve MVL applications.The ternary inverter consists of a ReSe2 field-effect transistor (FET)and our TS-RTT (device 4) in series. A bias voltage is applied to theReSe2 FET which is connected in series with the bottom ReSe2 layer ofthe TS-RTT, and the top ReSe2 layer is grounded as the source. The inputvoltage (Vin) serves as the back gate for device 4, and the output voltage18(Vout) is measured at the shared electrode between ReSe2 FET and device4. The input-output characteristic (Vout versus Vin) of the inverter isshown in Figure 5b. As Vin varies from 0 V to 60 V, Vout exhibits threedistinct states: (i) Vout is 5 V when 0 V < Vin < 10 V (State “2”), (ii) Vout is4.5 V when 20 V < Vin < 35 V (State “1”), and (iii) Vout is 0 V when 55 V< Vin < 60 V (State “0”). The inset in Figure 5b depicts the input-outputvoltage equivalent table for our ternary inverter. Figure 5c plots thecorresponding gains of the inverter at different bias voltages. Two peaksare clearly observed, corresponding to the voltage gains from logic “2” to“1” and “1” to “0”. Notably, the gain of the TS-RTT increases with biasvoltage, indicating its potential applications in storage and computing.However, due to the low output voltage, our inverter is not scalable. Todrive the next logic gate, the output voltage of the inverter must beamplified. Therefore, improving the output voltage of the inverter will beour focus in the future.Since light illumination significantly affects the negative resistancepeak position and PVR, our TS-RTTs are also promising inphotodetection applications. We conducted a detector of photo responseand photovoltaic response of device 5 (1.8 ° ) at room temperature. Thephotocurrent increases with increasing the laser power at an applied gatevoltage of -40 V, with an on/off ratio of ~106 and responsivity of 1.2mA/W at P = 13.8 W (shown in Figure 5d and Figure S11). It is worth19noting that our device shows a responsivity that gradually increases withincreasing laser power, which is different from typical photodetectors. Webelieve this is due to the presence of the h-BN barrier in our tunnelingdevice, which makes it difficult for photoelectrons to be collected at lowoptical power. Only when the optical power increases to a level whereenough photoelectrons are generated can they overcome the barrier andbe collected by the device’s source-drain electrodes. Furthermore, theincreased optical power may also lead to a more significant photothermaleffect, which could be another reason for the higher responsivity.Additionally, we found that the device has a tunable photovoltaic effectwhich can be adjusted by changing gate voltage as shown in Figure 5e.The adjustable photovoltaic current can also be confirmed by endurancemeasurement under periodic illumination at Vg = ± 40 V (shown inFigure 5f), showing its potential applications in self-poweredoptoelectronic devices, real-time imaging and artificial synapses, etc.20Figure 5. MVL inverter and adjustable self-powered photodetectorapplications of TS-RTTs. (a) Schematic of a ternary inverter composed ofa 158° TS-RTT and a ReSe2 FET. (b) Output voltage as a function ofinput voltage for the inverter at 10 K, demonstrating the recognition ofternary values. (c) Gain as a function of input voltage. (d)Power-dependent photocurrent as a function of bias voltage for a 1.8°TS-RTT. (e) Gate-dependent photovoltaic current, showing the tunabilityof the self-powered photodetector. (f) Endurance measurement ofphotovoltaic current at ±40 V gate voltages.CONCLUSIONSIn summary, we reported the ART in ReSe2/h-BN/ReSe2 TS-RTTswith various twist angles between the two ReSe2 layers in terms of thein-plane anisotropy of ReSe2. Due to the band anisotropy of ReSe2, ourdevices exhibited distinct NDR peaks and improved PVR by modulating21the twist angle. This enhancement of PVR is attributed to the suppressionof valley current within the tunneling process with a specific twist angleof 102°, achieved through unique band alignments and JDOS decrease, ascorroborated by our theoretical calculations. Furthermore, wedemonstrated that our TS-RTTs have potential applications in MVLinverters with three logic states and in adjustable self-poweredphotodetectors. Our findings not only introduce a twist-stackingtechnique to improve the performance of RTTs through twist angle andmomentum matching, but also demonstrate its potential applications inprogrammable optoelectronics and neuromorphic devices.METHODSTS-RTTs Fabrication. ReSe2/h-BN/ReSe2 twist-stackedheterojunctions were prepared using a dry transfer technique. The bottomReSe2 was mechanically exfoliated using 3M scotch tape on flake blocksonto a silicon/silicon dioxide (285 nm) (Si/SiO2) substrate for opticalmicroscopy examination (Olympus). Subsequently, h-BN wasmechanically exfoliated and transferred onto the bottom ReSe2 to serve asthe barrier layer. Poly (Bisphenol A carbonate) (PC) film coated onpolydimethylsiloxane (PDMS) was used to pick up h-BN flakes andrelease them at 180°C. The PC was prepared by dispersing 1 g ofpolycaprolactone in 10 mL of chloroform (Aladdin Tech. Co.). The PC22was then removed by soaking in chloroform for 5 minutes. Finally, thetop ReSe2 was mechanically exfoliated and transferred onto the h-BNlayer. The entire device was fabricated through a step-by-step transfermethod from bottom to top and the edge of the top ReSe2 layer is rotatedwith respect to the edge of the bottom ReSe2 layer to ensure a twist anglebetween two layers. Use electron-beam lithography technology (Zeisssupra 55 and Raith ELPHY Quantum) to pattern the electrons of thedevice, and deposit Cr/Au (5 nm/50 nm) with thermal evaporation in ahigh vacuum of 10−5 Pa by a thermal evaporation coater (ChineseAcademy of Sciences Shenyang Scientific Instruments Co.).Optical Measurement. The thickness of materials was performedusing atomic force microscopy (Dimension Icon, Bruker). Raman and thepolarization-dependent Raman spectra measurements were characterizedusing confocal Raman microscopy (WITec). The TEM image wasobtained by an FEI Themis Z with double aberration correctors, and thedata was processed by the Velox software.Photoelectronic Measurement. Photoelectric measurements wereperformed in a probe (CRX-6.5K, Lakeshore) using a semiconductoranalyzer (Keysight B1500A). 520nm laser (NBeT) was introduceddirectly into the probe shore cavity through an optical fiber and the lightintensity was measured by a power meter (THORLABS GmbH).DFT Calculation Details. The calculations of electronic properties23were carried out based on the density functional theory (DFT). We usedthe PAW pseudo potential38 and PBE exchange-correlation functional,39as implemented in the Vienna ab initio simulation package (VASP).40 Toavoid the interaction between slabs, we introduced a vacuum layer largerthan 15 Å along the z direction. Considering vdW interactions betweenReSe2 layers, we applied the DFT-D3 functional when calculatingmultilayer ReSe2 systems. To obtain accurate electronic band structureswhere free carriers are located, we chose 0.4 × 0.4 reciprocal patch withrespect to reciprocal vectors centered around the Γ point with a 7 × 7 × 1k-mesh. The lattice parameters were chosen as a=6.64 Å , b=6.77 Å ,c=38.96 Å, α=90.0°, β=90.0°, and γ=118.9°.Tunneling current simulations: To simulate the tunneling currentbetween the top and bottom ReSe2 layers through the middle insulatingh-BN layers. We calculated the tunneling probability between theelectronic states of these two ReSe2 layers under different electric fieldsand rotational angles. For simplicity, we consider only the conductionband and tunneling between the same wave vectors. Given that the freecarriers are mainly located at the bottom of the conduction band, which iscentered around the Gamma (Γ) point, we focused on a small 0.4 × 0.4 kpatch. We shifted the chemical potential of the top layer electronic statesto simulate the gating field. Furthermore, under the large gating field, weassumed that when the energy of electronic field equals the energy24difference between the two conduction bands, electrons will tunnel fromthe first conduction band to the second conduction band. As the top andbottom layers are widely separated by the large-gap insulating layer, thelattice rotation-induced interlayer coupling is neglected, which results inonly the rotation of the k-space electronic band structure. To obtain thedirect tunneling probability, we calculate the energy difference betweenthe top and bottom layer electronic states (first and second conductionbands) with the same k points. The tunneling probability reads� �� =1� ��� −��� −�� /��� + 1where we take T=300 K, kB is the Boltzmann constant, ΔE is the electricfield strength, and ��� , ��� denote the energy of different bands for thetop and bottom ReSe2 layers, respectively. For example, for themonolayer case, i = 1, 2 correspond to the first and second conductionbands.ASSOCIATED CONTENTSupporting InformationSupporting Information: Figures S1-S27.AUTHOR INFORMATIONCorresponding AuthorsShoujun Zheng - Centre for Quantum Physics, Key Laboratory ofAdvanced Optoelectronic Quantum Architecture and Measurement25(MOE), School of Physics, Beijing Institute of Technology, Beijing,100081, China; Email: szheng@bit.edu.cnWei Jiang - Centre for Quantum Physics, Key Laboratory of AdvancedOptoelectronic Quantum Architecture and Measurement (MOE), Schoolof Physics, Beijing Institute of Technology, Beijing, 100081, China;Email: wjiang@bit.edu.cnYan Xiong - Analysis&Testing center, Beijing Institute of technology,Beijing, 100081, China; Email: xiongyan@bit.edu.cnZhiwei Wang - Centre for Quantum Physics, Key Laboratory ofAdvanced Optoelectronic Quantum Architecture and Measurement(MOE), School of Physics, Beijing Institute of Technology, Beijing,100081, China; Email: zhiweiwang@bit.edu.cnAuthorsDan Guo - Centre for Quantum Physics, Key Laboratory of AdvancedOptoelectronic Quantum Architecture and Measurement (MOE), Schoolof Physics, Beijing Institute of Technology, Beijing 100081, ChinaHuiwen Wang - Centre for Quantum Physics, Key Laboratory ofAdvanced Optoelectronic Quantum Architecture and Measurement(MOE), School of Physics, Beijing Institute of Technology, Beijing100081, ChinaLiu Yang - Centre for Quantum Physics, Key Laboratory of Advancedmailto:szheng@bit.edu.cnmailto:wjiang@bit.edu.cnmailto:xiongyan@bit.edu.cnmailto:zhiweiwang@bit.edu.cn26Optoelectronic Quantum Architecture and Measurement (MOE), Schoolof Physics, Beijing Institute of Technology, Beijing 100081, ChinaWeikang Dong - Centre for Quantum Physics, Key Laboratory ofAdvanced Optoelectronic Quantum Architecture and Measurement(MOE), School of Physics, Beijing Institute of Technology, Beijing100081, ChinaBoyu Xu - Centre for Quantum Physics, Key Laboratory of AdvancedOptoelectronic Quantum Architecture and Measurement (MOE), Schoolof Physics, Beijing Institute of Technology, Beijing 100081, ChinaShuang Du - Centre for Quantum Physics, Key Laboratory of AdvancedOptoelectronic Quantum Architecture and Measurement (MOE), Schoolof Physics, Beijing Institute of Technology, Beijing 100081, ChinaXuyan Rui - Centre for Quantum Physics, Key Laboratory of AdvancedOptoelectronic Quantum Architecture and Measurement (MOE), Schoolof Physics, Beijing Institute of Technology, Beijing 100081, ChinaQingrong Liang - Centre for Quantum Physics, Key Laboratory ofAdvanced Optoelectronic Quantum Architecture and Measurement(MOE), School of Physics, Beijing Institute of Technology, Beijing100081, ChinaKenji Watanabe - National Institute for Materials Science, 1-1 Namiki,Tsukuba 303-0044, JapanTakashi Taniguchi - National Institute for Materials Science, 1-1 Namiki,27Tsukuba 303-0044, JapanJiadong Zhou - Centre for Quantum Physics, Key Laboratory ofAdvanced Optoelectronic Quantum Architecture and Measurement(MOE), School of Physics, Beijing Institute of Technology, Beijing100081, ChinaAuthor ContributionsD.G. fabricated all the devices and obtained the data. H.W. and W.J.performed the first-principles calculation and theoretical analysis. L.Y.and Z.W. synthesized the ReSe2 sample via chemical vapor transportmethod. W.D. finished the TEM measurements. B.X., S.D., X.R. and Q.L.assisted the device fabrications and optical and electronic tests. K.W. andT.T. synthesized h-BN samples. S.Z. and J.Z. supervised the project. Allauthors participated in scientific discussion and contributed on themanuscript.NotesThe authors declare no competing financial interest.ACKNOWLEDGMENTSThis work was supported by Natural Science Foundation of China grants(No.12104050 and No. 62375018), National Key Research and28Development Program of China (No. 2022YFA1203900) and BeijingInstitute of Technology Research Fund Program for Young Scholars.29REFERENCES(1) Mishchenko, A.; Tu, J. S.; Cao, Y.; Gorbachev, R. V.; Wallbank, J. R.; Greenaway, M. T.;Morozov, V. E.; Morozov, S. V.; Zhu, M. J.; Wong, S. L.; Withers, F.; Woods, C. R.; Kim, Y. J.;Watanabe, K.; Taniguchi, T.; Vdovin, E. E.; Makarovsky, O.; Fromhold, T. M.; Fal'ko, V. I.; Geim, A. K.,et al. Twist-Controlled Resonant Tunnelling in Graphene/Boron Nitride/GrapheneHeterostructures. Nat. Nanotechnol. 2014, 9, 808-813.(2) Asada, M.; Suzuki, S.;Kishimoto, N. Resonant Tunneling Diodes for Sub-Terahertz andTerahertz Oscillators. Jpn. J. of Appl. Phys. 2008, 47, 4375.(3) Sun, M.; Fang, Q.; Xie, D.; Sun, Y.; Xu, J.; Teng, C.; Dai, R.; Yang, P.; Li, Z.; Li, W.;Zhang, Y. NovelTransfer Behaviors in 2D MoS2/WSe2 Heterotransistor and Its Applications in Visible-Near InfraredPhotodetection. Adv. Electron. Mater. 2017, 3, 1600502.(4) Qiu, C.; Liu, F.; Xu, L.; Deng, B.; Xiao, M.; Si, J.; Lin, L.; Zhang, Z.; Wang, J.; Guo, H.; Peng,H.;Peng, L.-M. Dirac-Source Field-Effect Transistors as Energy-Efficient, High-PerformanceElectronic Switches. Science (New York, N.Y.) 2018, 361, 387-392.(5) Ma, Z.; Zhang, Q.; Tao, L.; Wang, Y.; Sando, D.; Zhou, J.; Guo, Y.; Lord, M.; Zhou, P.; Ruan, Y.;Wang, Z.; Hamilton, A.; Gruverman, A.; Tsymbal, E. Y.; Zhang, T.;Valanoor, N. ARoom-Temperature Ferroelectric Resonant Tunneling Diode. Adv. Mater. 2022, 34, 2205359.(6) Broekaert, T. P. E.; Brar, B.; Wagt, J. P. A. v. d.; Seabaugh, A. C.; Morris, F. J.; Moise, T. S.; Beam,E. A.;Frazier, G. A. A Monolithic 4-Bit 2-Gsps Resonant Tunneling Analog-to-Digital Converter.IEEE J. Solid-State Circuits 1998, 33, 1342-1349.(7) Cao, H.; Klimovitch, G.; Björk, G.;Yamamoto, Y. Direct Creation of Quantum Well Excitons byElectron Resonant Tunneling. Phys. Rev. Lett. 1995, 75, 1146-1149.(8) Sun, J. P.; Haddad, G. I.; Mazumder, P.;Schulman, J. N. Resonant Tunneling Diodes: Modelsand Properties. Proc. IEEE 1998, 86, 641-660.(9) Wang, L.; Papadopoulos, S.; Iyikanat, F.; Zhang, J.; Huang, J.; Taniguchi, T.; Watanabe, K.;Calame, M.; Perrin, M. L.; García de Abajo, F. J.;Novotny, L. Exciton-Assisted Electron Tunnelling invan der Waals Heterostructures. Nat. Mater. 2023, 22, 1094-1099.(10) Xu, K.; Wynne, E.;Zhu, W. Resonant Tunneling and Negative Differential Resistance in BlackPhosphorus Vertical Heterostructures. Adv. Electron. Mater. 2020, 6, 2000318.(11) Shi, J.; Liu, M.; Wen, J.; Ren, X.; Zhou, X.; Ji, Q.; Ma, D.; Zhang, Y.; Jin, C.; Chen, H.; Deng, S.; Xu,N.; Liu, Z.;Zhang, Y. All Chemical Vapor Deposition Synthesis and Intrinsic Bandgap Observationof MoS2/Graphene Heterostructures. Adv. Mater. 2015, 27, 7086-7092.(12) Nguyen, L.-N.; Lan, Y.-W.; Chen, J.-H.; Chang, T.-R.; Zhong, Y.-L.; Jeng, H.-T.; Li, L.-J.;Chen,C.-D. Resonant Tunneling through Discrete Quantum States in Stacked Atomic-Layered MoS2.Nano Lett. 2014, 14, 2381-2386.(13) Campbell, P. M.; Tarasov, A.; Joiner, C. A.; Ready, W. J.;Vogel, E. M. Enhanced ResonantTunneling in Symmetric 2D Semiconductor Vertical Heterostructure Transistors. ACS Nano 2015,9, 5000-5008.(14) Kim, K.; Prasad, N.; Movva, H. C. P.; Burg, G. W.; Wang, Y.; Larentis, S.; Taniguchi, T.;Watanabe, K.; Register, L. F.;Tutuc, E. J. N. l. Spin-Conserving Resonant Tunneling inTwist-Controlled WSe2-hBN-WSe2 Heterostructures. Nano Lett. 2018, 18, 5967-5973.(15) Britnell, L.; Gorbachev, R. V.; Geim, A. K.; Ponomarenko, L. A.; Mishchenko, A.; Greenaway, M.T.; Fromhold, T. M.; Novoselov, K. S.;Eaves, L. Resonant Tunnelling and Negative Differential30Conductance in Graphene Transistors. Nat. Commun. 2013, 4, 1794.(16) Srivastava, P. K.; Hassan, Y.; de Sousa, D. J. P.; Gebredingle, Y.; Joe, M.; Ali, F.; Zheng, Y.; Yoo,W. J.; Ghosh, S.; Teherani, J. T.; Singh, B.; Low, T.;Lee, C. Resonant Tunnelling Diodes Based onTwisted Black Phosphorus Homostructures. Nat. Electron. 2021, 4, 269-276.(17) Xiong, X.; Huang, M.; Hu, B.; Li, X.; Liu, F.; Li, S.; Tian, M.; Li, T.; Song, J.;Wu, Y. A TransverseTunnelling Field-Effect Transistor Made From a van der Waals Heterostructure. Nat. Electron.2020, 3, 106-112.(18) Cao, Y.; Fatemi, V.; Fang, S.; Watanabe, K.; Taniguchi, T.; Kaxiras, E.;Jarillo-Herrero, P.Unconventional Superconductivity in Magic-Angle Graphene Superlattices. Nature 2018, 556,43-50.(19) Song, T.; Cai, X.; Tu, M. W.-Y.; Zhang, X.; Huang, B.; Wilson, N. P.; Seyler, K. L.; Zhu, L.;Taniguchi, T.; Watanabe, K.; McGuire, M. A.; Cobden, D. H.; Xiao, D.; Yao, W.;Xu, X. GiantTunneling Magnetoresistance in Spin-Filter van der Waals Heterostructures. Science (New York,N.Y.) 2018, 360, 1214-1218.(20) Zheng, Z.; Ma, Q.; Bi, Z.; de la Barrera, S.; Liu, M.-H.; Mao, N.; Zhang, Y.; Kiper, N.; Watanabe,K.; Taniguchi, T.; Kong, J.; Tisdale, W. A.; Ashoori, R.; Gedik, N.; Fu, L.; Xu, S.-Y.;Jarillo-Herrero, P.Unconventional Ferroelectricity in Moiré Heterostructures. Nature 2020, 588, 71-76.(21) Dai, Y.; Qi, P.; Tao, G.; Yao, G.; Shi, B.; Liu, Z.; Liu, Z.; He, X.; Peng, P.; Dang, Z.; Zheng, L.;Zhang, T.; Gong, Y.; Guan, Y.; Liu, K.;Fang, Z. Phonon-Assisted Upconversion in TwistedTwo-Dimensional Semiconductors. Light Sci. Appl. 2023, 12, 6.(22) Fallahazad, B.; Lee, K.; Kang, S.; Xue, J.; Larentis, S.; Corbet, C.; Kim, K.; Movva, H. C. P.;Taniguchi, T.; Watanabe, K.; Register, L. F.; Banerjee, S. K.;Tutuc, E. Gate-Tunable ResonantTunneling in Double Bilayer Graphene Heterostructures. Nano Lett. 2015, 15, 428-433.(23) Hu, G.; Ou, Q.; Si, G.; Wu, Y.; Wu, J.; Dai, Z.; Krasnok, A.; Mazor, Y.; Zhang, Q.; Bao, Q.; Qiu,C.-W.;Alù, A. Topological Polaritons and Photonic Magic Angles in Twisted α-MoO3 Bilayers.Nature 2020, 582, 209-213.(24) Liao, M.; Wei, Z.; Du, L.; Wang, Q.; Tang, J.; Yu, H.; Wu, F.; Zhao, J.; Xu, X.; Han, B.; Liu, K.; Gao,P.; Polcar, T.; Sun, Z.; Shi, D.; Yang, R.;Zhang, G. Precise Control of the Interlayer Twist Angle inLarge Scale MoS2 Homostructures. Nat. Commun. 2020, 11, 2153.(25) Sun, T.; Chen, R.; Ma, W.; Wang, H.; Yan, Q.; Luo, J.; Zhao, S.; Zhang, X.;Li, P. Van der WaalsQuaternary Oxides for Tunable Low-Loss Anisotropic Polaritonics. Nat. Nanotechnol. 2024, 19,758-765.(26) Sun, X.; Suriyage, M.; Khan, A. R.; Gao, M.; Zhao, J.; Liu, B.; Hasan, M. M.; Rahman, S.; Chen,R.-s.; Lam, P. K.;Lu, Y. Twisted van der Waals Quantum Materials: Fundamentals, Tunability, andApplications. Chem. Rev. 2024, 124, 1992-2079.(27) Zheng, S.; Jo, S.; Kang, K.; Sun, L.; Zhao, M.; Watanabe, K.; Taniguchi, T.; Moon, P.; Myoung,N.;Yang, H. Resonant Tunneling Spectroscopy to Probe the Giant Stark Effect in Atomically ThinMaterials. Adv. Mater. 2020, 32, 1906942.(28) Ghazaryan, D. A.; Misra, A.; Vdovin, E. E.; Watanabe, K.; Taniguchi, T.; Morozov, S. V.;Mishchenko, A.;Novoselov, K. S. Twisted Monolayer and Bilayer Graphene for Vertical TunnelingTransistors. Appl. Phys. Lett. 2021, 118, 183106.(29) Kuzmina, A.; Parzefall, M.; Back, P.; Taniguchi, T.; Watanabe, K.; Jain, A.;Novotny, L. ResonantLight Emission from Graphene/Hexagonal Boron Nitride/Graphene Tunnel Junctions. Nano Lett.2021, 21, 8332-8339.31(30) Jang, J.; Yoo, H. M.; Pfeiffer, L. N.; West, K. W.; Baldwin, K. W.;Ashoori, R. C. Full Momentum-and Energy-Resolved Spectral Function of a 2D Electronic System. Science (New York, N.Y.) 2017,358, 901-906.(31) Keren, I.; Dvir, T.; Zalic, A.; Iluz, A.; LeBoeuf, D.; Watanabe, K.; Taniguchi, T.;Steinberg, H.Quantum-Dot Assisted Spectroscopy of Degeneracy-Lifted Landau Levels in Graphene. Nat.Commun. 2020, 11, 3408.(32) Kim, E.; Hwang, G.; Kim, D.; Won, D.; Joo, Y.; Zheng, S.; Watanabe, K.; Taniguchi, T.; Moon, P.;Kim, D.-W.; Sun, L.;Yang, H. Orbital Gating Driven by Giant Stark Effect in TunnelingPhototransistors. Adv. Mater. 2022, 34, 2106625.(33) Takeyama, K.; Moriya, R.; Okazaki, S.; Zhang, Y.; Masubuchi, S.; Watanabe, K.; Taniguchi, T.;Sasagawa, T.;Machida, T. Resonant Tunneling Due to van der Waals Quantum-Well States ofFew-Layer WSe2 in WSe2/h-BN/p+-MoS2 Junction. Nano Lett. 2021, 21, 3929-3934.(34) Greenaway, M. T.; Vdovin, E. E.; Mishchenko, A.; Makarovsky, O.; Patanè, A.; Wallbank, J. R.;Cao, Y.; Kretinin, A. V.; Zhu, M. J.; Morozov, S. V.; Fal’ko, V. I.; Novoselov, K. S.; Geim, A. K.;Fromhold, T. M.;Eaves, L. Resonant Tunnelling Between the Chiral Landau States of TwistedGraphene Lattices. Nat. Phys. 2015, 11, 1057-1062.(35) Wallbank, J. R.; Ghazaryan, D.; Misra, A.; Cao, Y.; Tu, J. S.; Piot, B. A.; Potemski, M.; Pezzini, S.;Wiedmann, S.; Zeitler, U.; Lane, T. L. M.; Morozov, S. V.; Greenaway, M. T.; Eaves, L.; Geim, A. K.;Fal'ko, V. I.; Novoselov, K. S.;Mishchenko, A. Tuning the Valley and Chiral Quantum State of DiracElectrons in van der Waals Heterostructures. Science (New York, N.Y.) 2016, 353, 575-579.(36) Shim, J.; Oh, S.; Kang, D.-H.; Jo, S.-H.; Ali, M. H.; Choi, W.-Y.; Heo, K.; Jeon, J.; Lee, S.; Kim, M.;Song, Y. J.;Park, J.-H. Phosphorene/Rhenium Disulfide Heterojunction-Based NegativeDifferential Resistance Device for Multi-Valued Logic. Nat. Commun. 2016, 7, 13413.(37) Shim, J.; Jo, S.-H.; Kim, M.; Song, Y. J.; Kim, J.;Park, J.-H. Light-Triggered Ternary Device andInverter Based on Heterojunction of van der Waals Materials. ACS Nano 2017, 11, 6319-6327.(38) Blöchl, P. E. Projector Augmented-Wave Method. Phys. Rev. B 1994, 50, 17953-17979.(39) Perdew, J. P.; Burke, K.;Ernzerhof, M. Generalized Gradient Approximation Made Simple.Phys. Rev. Lett. 1996, 77, 3865-3868.(40) Kresse, G.;Hafner, J. Ab Initio Molecular Dynamics for Liquid Metals. Phys. Rev. B 1993, 47,558-561.32ToC imageToC caption: An anisotropic resonant tunneling transistor based onanisotropic ReSe2 is reported, where peak-to-valley ratio exhibits a strongdependence on the twist angle between the two ReSe2 layers, reaching amaximum at the twist angle of 102° due to the modulation of the jointdensity of states and suppression of the valley current.