800 Adenine Guanine. Gate Voltage (V)

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1 I. SUPPLEMENTARY FIGURES Surce-Drain Current (µa) 14 Thymine cverage (M.L.) Cytsine cverage (M.L.) Adenine cverage (M.L.) Guanine cverage (M.L.) Gate Vltage (V) Supplementary Figure 1: Electrical transprt measurements fr thymine, adenine, cytsine and guanine. Electrical transprt measurements f GFETs with increasing cverage f fur nuclebases. The psitin (vltage) f the I SD minima were used t determine the shifts f CNP in Figure 2. Due t changes in the asymmetry f the curve slpes, we did nt use the linear fit methd t btain CNP. The psitive gate vltage data fr the lw cverage cytsine measurements is clipped due t a data cllectin errr, but the minimum in I SD is still visible. 1

2 2. Intensity (16 CPS) Graphene C1s 1.5 T cverage (M.L.) Thymine N1s.5 Thymine C1s Phtelectrn Kinetic Energy (ev) 4 38 Supplementary Figure 2: XPS data at a range f cverages fr Thymine adsrbed n SLG. High reslutin XPS C 1s (hν = 33 ev) and N 1s (hν = 45 ev) cre level spectra fr thymine adsrbed n SLG. The results are pltted n the less cmmn phtelectrn kinetic energy scale t demnstrate the similar phtelectrn energies as seen by the analyzer. The minimal kinetic energy difference between these tw phtelectrn peaks allwed fr the use f the rati f C 1s and N 1s peak areas in the calculatin mlecular cverage withut knwledge f the analyzer transmissin as a functin f energy. 2

3 a Nrmalised Intensity (arb. units) 3. Guanine π 2.5 Graphene σ Graphene π NEXAFS Angle Phtn Energy (ev) b Nrmalised Peak Intensity (arb. units) Guanine π * fit Guanine π * fit Graphene σ * + 5 fit NEXAFS Angle Supplementary Figure 3: Angle reslved C K-edge NEXAFS measurements f 1 mnlayer f Guanine n graphene. (a) C K-edge NEXAFS spectra at 5 different NEXAFS angles (9 represents beam incident nrmal t the surface). Identificatin f guanine peaks was achieved by cmparisn with the NEXAFS f the bare graphene. The tw π guanine peaks used fr tilt angle calculatins are indicated by the clured lines. (b) Fits fr tilt angle calculatins f tw guanine π peaks and a graphene σ peak [1]. 3

4 14 Cytsine 16 Guanine Mbility (cm 2 V -1 s -1 ) Thymine Adenine Cverage (M.L.) Hle Mbility Electrn Mbility Supplementary Figure 4: Cverage dependent electrn (red) and hle (black) mbility f graphene as a functin f increasing cverage f DNA nuclebases n the surface. The graphene electrn and hle mbilities were estimated via linear fits t the measured transprt curves either side f the Dirac pint. 4

5 II. SUPPLEMENTARY TABLE Nuclebase Unit Cell Size (Å 2 ) Nitrgen atms per unit cell n N nc Ref. Adenine [2] Cytsine [3] Guanine [2] Thymine [4] Supplementary Table I: Tabulated values f the unit cell size fr mnlayer cverage f different nuclebases adsrbed n graphite, btained frm literature. These values were used t calculate the mlecular cverage f XPS samples frm the rati f mlecular N1s peak area t graphene C1s peak area (n N /n C ). 5

6 III. SUPPLEMENTARY DISCUSSION In additin t the reprted changes in the graphene dping (shift f the Dirac pint in Fig. 2) in the main manuscript, the transprt characteristics f graphene FETs demnstrate als changes in the shape f the I-Vg curves with increasing cverage f the nuclebases. In supplementary figure 3, we analyze the changes in the slpe f the electrn and hle cnductivity sides using linear fits which are related t charge carrier mbility f graphene [5]. The electrn and hle mbility (µ) was estimated via linear fits f I SD V SD = µne t the data away frm the minimum cnductivity regin. Prir t mlecular adsrptin a significant asymmetry between electrn mbility and hle mbility is bserved, the magnitude and directin f the asymmetry is nt cnsistent acrss the devices measured. This magnitude f the asymmetry between electrn and hle transprt is further increased by the adsrptin each f the fur nuclebases measured. Additinal adsrptin f guanine and cytsine results in an verall decrease in the graphene mbility, whilst thymine causes an increase in the device mbility. Reductins f graphene mbility have been theretically [6] and experimentally [7] attributed t lng range charge carrier scattering sites in the frm f lcalised electric fields nearby the graphene surface. Analgusly, the diple mment f the adsrbed nuclebases will result in the frmatin f additinal charged scattering sites further decreasing the graphene mbility. The bserved rder in magnitude f mbility reductin agrees with the predicted diple mments fr the nuclebases studied; guanine 7.2 D, cytsine 6.6 D, thymine 4.3 D and adenine 2.3 D. Hwever, the bserved increase in device mbility with thymine cverage is nt cnsistent with this explanatin. As there is already a high density f charge scattering sites nearby the graphene fr clean samples, evidenced by the lw mbility and brad cnductivity minimum in clean devices, the plarisability f the nuclebases effects hw well they will effectively screen ther charged scattering sites [5]. The nuclebase plarizabilites are all similar and the relative magnitude f diple mments culd pssibly explain why we see a decrease fr adsrbed G and C but an increase in T. Hwever, as A has the smallest diple mment it wuld als be expected t cause an increase in device mbility. Interactins between the mlecules and the metal cntact-graphene interface culd be anther explanatin f the bserved changes in the graphene mbility. Adsrptin f nuclebases at the metal-graphene interface culd lead t band re-alignment changing the cntact ptential, which in turn alters the cntact resistance and cnsequently the estimated graphene mbility. Cntact effects culd als explain the bserved variability in clean device asymmetry, as the devices were nt prduced simultaneusly. As mentined in the paper the metal-cntact graphene interface can dminate the bserved transprt, hwever, as tw prbe devices were used the effects f cntact resistance culd nt be explred. 6

7 IV. SUPPLEMENTARY REFERENCES [1] Stöhr, J. & Outka, D. A. Determinatin f mlecular rientatins n surfaces frm the angular dependence f near-edge x-ray-absrptin fine-structure spectra. Phys. Rev. B 36, (1987). [2] Ta, N. J. & Shi, Z. Mnlayer guanine and adenine n graphite in nacl slutin: A cmparative stm and afm study. The Jurnal f Physical Chemistry 98, (1994). [3] Mamduh, W., Kelly, R. E. A., Dng, M., Kantrvich, L. N. & Besenbacher, F. Tw-dimensinal supramlecular nanpatterns frmed by the cadsrptin f guanine and uracil at the liquid/slid interface. Jurnal f the American Chemical Sciety 13, (28). [4] Swerby, S. J. & Petersen, G. B. Scanning tunneling micrscpy f uracil mnlayers self-assembled at the slid liquid interface. Jurnal f Electranalytical Chemistry 433, 85 9 (1997). [5] Newaz, A., Puzyrev, Y. S., Wang, B., Pantelides, S. T. & Bltin, K. I. Prbing charge scattering mechanisms in suspended graphene by varying its dielectric envirnment. Nature Cmmunicatins 3, 734 (212). [6] Adam, S., Hwang, E. H., Galitski, V. M. & Sarma, S. D. A self-cnsistent thery fr graphene transprt. PNAS 14, (27). [7] Chen, J.-H. et al. Charged-impurity scattering in graphene. Nature Physics 4, 377 (28). 7

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