transfer was repeated several times (typically ∼3) in order to further improve the conductance of the electrodes, therefore forming a multilayer graphene (MLG) stack. An optical graph of the glass substrate with the MLG fi lm on top is displayed in Figure 1 b, showing high transparency. Subsequently, the MLG fi lm was patterned into bottom electrodes (BEs) with widths of 1-5 µm by photolithography and O 2 plasma etching (Figure 1 a2). Au/Ti metal contacts (B1 and B2) were then deposited onto the two ends of the MLG BE afterwards to minimize the contact resistance to the external probes in electrical measurements (Figure 1 a3). Following BE defi nition, a bilayer oxide structure consisting of an oxygen rich Ta 2 O 5-x layer (∼5 nm) and an oxygen defi cient TaO y layer (∼40 nm) serving as the switching medium of the RRAM devices was successively deposited by radio-frequency (RF) sputtering and reactive sputtering (400 °C, O 2 /Ar = 3%), respectively, without breaking the vacuum (Figure 1 a4). Similar to steps 1-3 in Figure 1 a, multiple monolayer graphene transfer, O 2 plasma etching and Au/Ti metal contacts deposition were conducted again to fabricate the top electrodes (TEs) that complete the crossbar memory structure ( Figure 1 a5-7). Finally, a pad opening step was performed through a timed reactive ion etching (RIE) process to remove the Ta 2 O 5-x /TaO y bilayer on top of the bottom contact Au/Ti pads (Figure 1 a8). The sizes of the RRAM devices in this work range from 1-5 µm × 1-5 µm, and during measurements the voltage was applied on the TE with the BE grounded. Since resistive switching in Ta 2 O 5-x /TaO y bilayer devices is driven by internal oxygen vacancy redistribution, the change in deposition sequence should in principle only lead to a reversal of the switching polarity, as has been verifi ed by studies on devices with inert metal electrodes. [ 25 ] However, in the case of devices with MLG electrodes, the stacking sequence of the bilayer was found to be critical in determining the device behavior, as shown in Figure 1 d,e. When the Ta 2 O 5-x layer was deposited fi rst on the graphene BE followed by TaO y deposition, the MLG/TaO y /Ta 2 O 5-x /MLG (top to bottom) devices exhibited conventional bipolar resistive switching characteristics similar to the results obtained with metal electrodes, [ 25,26 ] as shown in Figure 1 d. Such switching behavior can be well understood in the picture of V O exchange between the Ta 2 O 5-x and the V O -rich TaO y layers, [ 8,26,27 ] and the switching polarity with positive SET and negative RESET voltages is a natural result of the device confi guration since the V O reservoir (the oxygen defi cient TaO y layer) sits on top in this case. The linear on-state behavior is also consistent with Ohmic conduction for the V O -based conducting fi laments in Ta 2 O 5-x /TaO y RRAMs. [ 8,26,27 ] Driven by the continuing demand for improved computing capability, the semiconductor industry has been constantly looking for a fast, reliable, scalable yet nonvolatile memory technolo...