CommuniCation(1 of 8) 1600784However, O 2 plasma treatment results in an increase of stamp surface adhesive energy, preventing efficient layer transfer from the PDMS to the substrate.To address these problems, we introduce double transfer stamping (DTS) to promote interdiffusion between donor and acceptor layers to form well-defined interdiffused bilayer heterojunction (BiHJ) OPDs sandwiched between donor and acceptor layers that are in direct contact with their respective metal electrodes. The thermal annealing step is used to enable interdiffusion between the donor and acceptor layers, forming the active layer. Using this approach, we demonstrate an inverted interdiffused P3HT/PCBM bilayer photodiode whose dark current density is 7.7 ± 0.3 nA cm −2 with an external quantum efficiency of 60% ± 1% and a peak specific detectivity of (4.8 ± 0.2) × 10 12 cm Hz 1/2 W −1 .In Figure 1, we show the energy level diagram for the OPD to illustrate how donor and acceptor bilayer interdiffusion can effectively suppress the dark current under reverse bias while maintaining a high quantum efficiency; the energy values shown are found elsewhere. [21] Although other approaches have been demonstrated to suppress dark current injection such as addition of a hole blocking layer (e.g., ZnO) [21,22] at the anode, or an electron blocking layer (e.g., poly[N,N′-bis(4butylphenyl)-N,N′-bis(phenyl)-benzidine]) at the cathode, [2] the success of these methods are fabrication process dependent since the additional layers can introduce interface states that adversely affect device performance. [23][24][25] A simple and reliable means to suppress the reverse-biased dark current, therefore, is to have only the acceptor material in contact with the cathode, while only donor material contacts the anode. [4,10] In the inverted BHJ in Figure 1a, the hole injection barrier at the cathode is ΔE hole = 1.4 eV (equal to the difference between the highest occupied molecular orbital (HOMO) energy of P3HT at 5.0 eV [26] and Φ ITO/PEIE = 3.6 eV [27] ), and the electron injection barrier at the anode is ΔE electron = 2.6 eV (equal to the difference between Φ MoO3 6.9 eV [28] and the lowest unoccupied MO (LUMO) energy of PCBM of 4.3 eV [26] ). A significant increase of the barrier height is obtained by the formation of the bilayer HJ in Figure 1b. Then, the hole injection barrier at the cathode/PCBM interface is ΔE hole = 2.5 eV (equal to the difference between the HOMO energy of PCBM of 6.1 eV [26] and Φ ITO/PEIE ) and the electron injection barrier at the anode/P3HT layer is ΔE electron = 3.9 eV (equal to the difference between Φ MoO3[28] and the LUMO energy of P3HT of 3.0 eV [26] ). We expect that the increased ΔE hole and ΔE electron at cathode/anode interfaces reduce the dark leakage current, while the lower energetic barrier (e.g., ΔE hole ) encourages current injection. The device structure is shown in Figure 1c. The structure maximizes the area of the D/A interfaces within a given volume via thermal interdiffusion, while maintaining undiluted electron