Time-Resolved Activation of pH Sensing and Imaging in Vivo by a Remotely Controllable DNA Nanomachine

Construction of probes or nanodevices capable of sensing pH with high spatial and temporal precision remains a challenge, despite their importance in monitoring of diverse physiological and pathological processes. Here we disclose the first remotely and noninvasively controlled DNA nanomachine that can monitor pH in live cells and animals in a temporally programmable manner. The nanomachine is designed by rational engineering of the DNA motif with a light-responsive element and further combination with an upconversion nanoparticle that works as a transducer to manipulate the nanomachine with the high precision of NIR light. The nanomachine not only allows for activated fluorescent imaging of intracellular pH, but it also can exert spatiotemporal control over its pH sensing activity in tumor-bearing mice by NIR light irradiation at a chosen time and place. This work illustrates the potential of combining DNA nanotechnology with upconversion tools to yield a precisely controlled nanomachine for temporally resolved pH sensing and imaging.