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Register a new userProbing Kondo spin fluctuations with scanning tunneling microscopy and electron spin resonance
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We theoretically analyze a state-of-the-art experimental method based on a combination of electron spin resonance and scanning tunneling microscopy (ESR-STM), to directly probe the spin fluctuations in the Kondo effect. The Kondo impurity is exchange coupled to the probe spin, and the ESR-STM setup detects the small level shifts in the probe spin induced by the spin fluctuations of the Kondo impurity. We use the open quantum system approach by regarding the probe spin as the system and the Kondo impurity spin as the fluctuating bath to evaluate the resonance line shifts in terms of the dynamic spin susceptibility of the Kondo impurity. We consider various common adatoms on surfaces as possible probe spins and estimate the corresponding level shifts. It is found that the sensitivity is most pronounced for the probe spins with transverse magnetic anisotropy.
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We present an extension of the tunneling theory for scanning tunneling microcopy (STM) to include different types of vibrational-electronic couplings responsible for inelastic contributions to the tunnel current in the strong-coupling limit. It allows for a better understanding of more complex scanning tunneling spectra of molecules on a metallic substrate in separating elastic and inelastic contributions. The starting point is the exact solution of the spectral functions for the electronic active local orbitals in the absence of the STM tip. This includes electron-phonon coupling in the coupled system comprising the molecule and the substrate to arbitrary order including the anti-adiabatic strong coupling regime as well as the Kondo effect on a free electron spin of the molecule. The tunneling current is derived in second order of the tunneling matrix element which is expanded in powers of the relevant vibrational displacements. We use the results of an ab-initio calculation for the single-particle electronic properties as an adapted material-specific input for a numerical renormalization group approach for accurately determining the electronic properties of a NTCDA molecule on Ag(111) as a challenging sample system for our theory. Our analysis shows that the mismatch between the ab-initio many-body calculation of the tunnel current in the absence of any electron-phonon coupling to the experiment scanning tunneling spectra can be resolved by including two mechanisms: (i) a strong unconventional Holstein term on the local substrate orbital leads to reduction of the Kondo temperature and (ii) a different electron-vibrational coupling to the tunneling matrix element is responsible for inelastic steps in the $dI/dV$ curve at finite frequencies.
A simple, reliable method for preparation of bulk Cr tips for Scanning Tunneling Microscopy (STM) is proposed and its potentialities in performing high-quality and high-resolution STM and Spin Polarized-STM (SP-STM) are investigated. Cr tips show atomic resolution on ordered surfaces. Contrary to what happens with conventional W tips, rest atoms of the Si(111)-7x7 reconstruction can be routinely observed, probably due to a different electronic structure of the tip apex. SP-STM measurements of the Cr(001) surface showing magnetic contrast are reported. Our results reveal that the peculiar properties of these tips can be suited in a number of STM experimental situations.
Kondo-type zero-bias anomalies have been frequently observed in quantum dots occupied by two electrons and attributed to a spin-triplet configuration that may become stable under particular circumstances. Conversely, zero-bias anomalies have been so far quite elusive when quantum dots are occupied by an even number of electrons greater than two, even though a spin-triplet configuration is more likely to be stabilized there than for two electrons. We propose as an origin of this phenomenon the spin-orbit interaction, and we show how it profoundly alters the conventional Kondo screening scenario in the simple case of a laterally confined quantum dot with four electrons.
Quantum point contacts exhibit mysterious conductance anomalies in addition to well known conductance plateaus at multiples of 2e^2/h. These 0.7 and zero-bias anomalies have been intensively studied, but their microscopic origin in terms of many-body effects is still highly debated. Here we use the charged tip of a scanning gate microscope to tune in situ the electrostatic potential of the point contact. While sweeping the tip distance, we observe repetitive splittings of the zero-bias anomaly, correlated with simultaneous appearances of the 0.7 anomaly. We interpret this behaviour in terms of alternating equilibrium and non-equilibrium Kondo screenings of different spin states localized in the channel. These alternating Kondo effects point towards the presence of a Wigner crystal containing several charges with different parities. Indeed, simulations show that the electron density in the channel is low enough to reach one-dimensional Wigner crystallization over a size controlled by the tip position.
In the last decade, detecting spin dynamics at the atomic scale has been enabled by combining techniques like electron spin resonance (ESR) or pump-probe spectroscopy with scanning tunneling microscopy (STM). Here, we demonstrate an ultra-high vacuum (UHV) STM operational at milliKelvin (mK) and in a vector magnetic field capable of both ESR and pump-probe spectroscopy. By implementing GHz compatible cabling, we achieve appreciable RF amplitudes at the junction while maintaining mK base temperature. We demonstrate the successful operation of our setup by utilizing two experimental ESR modes (frequency sweep and magnetic field sweep) on an individual TiH molecule on MgO/Ag(100) and extract the effective g-factor. We trace the ESR transitions down to MHz into an unprecedented low frequency band enabled by the mK base temperature. We also implement an all-electrical pump-probe scheme based on waveform sequencing suited for studying dynamics down to the nanoseconds range. We benchmark our system by detecting the spin relaxation time T1 of individual Fe atoms on MgO/Ag(100) and note a field strength and orientation dependent relaxation time.
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