“…In filter paper,c ellulose chains organize into microfibrils that consist of crystalline and non-crystalline domains,a nd microfibrils further pack into fibers. [11] Ink for optode fabrication could access and modify the surface of fibers with ease.H owever,c rystalline domains are impenetrable toward water and most solvents,i ncluding cyclohexanone,b ecause of substantial inter-a nd intra-molecular hydrogen bonding.Therefore,the crystalline bulk of cellulose fibers is difficult to dope with the sensing ingredients.I n contrast, penetration of ink into the fiber bulk could take place through loosely-ordered non-crystalline domains.T he thin layer surface modification and limited bulk modification through non-crystalline defects is further supported by the following observations:1 )XPS depth profiling analysis (see inset of Figure 2) shows that al arge portion of sensing ingredients were eliminated by only 20 sofion beam etching (corresponding to an etching thickness of afew nm or less [12] ) but the amount of sensing ingredients levels off for the subsequent etching cycles (resulting from in-depth modification);2 )inm icroscopic pictures (Supporting Information, Figure S1), large fibers show an accumulated reddish color on the surface,b ut only limited reddish domains are observed from the fiber bulk.…”