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In the last decade, detecting spin dynamics at the atomic scale has beenenabled by combining techniques like electron spin resonance (ESR) orpump-probe spectroscopy with scanning tunneling microscopy (STM). Here, wedemonstrate an ultra-high vacuum (UHV) STM operational at milliKelvin (mK) andin a vector magnetic field capable of both ESR and pump-probe spectroscopy. Byimplementing GHz compatible cabling, we achieve appreciable RF amplitudes atthe junction while maintaining mK base temperature. We demonstrate thesuccessful operation of our setup by utilizing two experimental ESR modes(frequency sweep and magnetic field sweep) on an individual TiH molecule onMgO/Ag(100) and extract the effective g-factor. We trace the ESR transitionsdown to MHz into an unprecedented low frequency band enabled by the mK basetemperature. We also implement an all-electrical pump-probe scheme based onwaveform sequencing suited for studying dynamics down to the nanoseconds range.We benchmark our system by detecting the spin relaxation time T1 of individualFe atoms on MgO/Ag(100) and note a field strength and orientation dependentrelaxation time.

A scanning tunneling microscope capable of electron spin resonance and pump-probe spectroscopy at mK temperature and in vector magnetic field