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RF harvesting circuits have been demonstrated for more than 50 years, but only a few have been able to harvest energy from freely available ambient (i.e., non-dedicated) RF sources. In this paper, our objectives were to realize harvester operation at typical ambient RF power levels found within urban and semi-urban environments. To explore the potential for ambient RF energy harvesting, a city-wide RF spectral survey was undertaken from outside all of the 270 London Underground stations at street level. Using the results from this survey, four harvesters (comprising antenna, impedance-matching network, rectifier, maximum power point tracking interface, and storage element) were designed to cover four frequency bands from the largest RF contributors (DTV, GSM900, GSM1800, and 3G) within the ultrahigh frequency (0.3-3 GHz) part of the frequency spectrum. Prototypes were designed and fabricated for each band. The overall end-to-end efficiency of the prototypes using realistic input RF power sources is measured; with our first GSM900 prototype giving an efficiency of 40%. Approximately half of the London Underground stations were found to be suitable locations for harvesting ambient RF energy using our four prototypes. Furthermore, multiband array architectures were designed and fabricated to provide a broader freedom of operation. Finally, an output dc power density comparison was made between all the ambient RF energy harvesters, as well as alternative energy harvesting technologies, and for the first time, it is shown that ambient RF harvesting can be competitive with the other technologies.