Electrical Cross-Correlation Spectroscopy: Measuring Picoliter-per-Minute Flows in Nanochannels

We introduce all-electrical cross-correlation spectroscopy of molecular number fluctuations in nanofluidic channels. Our approach is based on a pair of nanogap electrochemical transducers located downstream from each other in the channel. When liquid is driven through this device, mesoscopic fluctuations in the local density of molecules are transported along the channel. We perform a time-of-flight measurement of these fluctuations by cross-correlating current-time traces obtained at the two detectors. Thereby we are able to detect ultralow liquid flow rates below 10  pL/min⁡. This method constitutes the electrical equivalent of fluorescence cross-correlation spectroscopy.