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arXiv:1809.10116 · Physical Review Letters

Echo Trains in Pulsed Electron Spin Resonance of a Strongly Coupled Spin Ensemble

Stefan Weichselbaumer, Matthias Zens, Christoph W. Zollitsch, Martin S. Brandt, Stefan Rotter, Rudolf Groß, Hans Huebl

Published Sep 22, 2020• 30 citations
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Abstract

We report on a novel dynamical phenomenon in electron spin resonance experiments of phosphorus donors. When strongly coupling the paramagnetic ensemble to a superconducting lumped element resonator, the coherent exchange between these two subsystems leads to a train of periodic, self-stimulated echoes after a conventional Hahn echo pulse sequence. The presence of these multiecho signatures is explained using a simple model based on spins rotating on the Bloch sphere, backed up by numerical calculations using the inhomogeneous Tavis-Cummings Hamiltonian.

DOI
10.1103/physrevlett.125.137701

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cond-mat.mes-hallCross-listedarXiv:2603.26255•Mar 30, 2026
We report on a novel dynamical phenomenon in electron spin resonance experiments of phosphorus donors. When strongly coupling the paramagnetic ensemble to a superconducting lumped element resonator, the coherent exchange between these two subsystems leads to a train of periodic, self-stimulated echoes after a conventional Hahn echo pulse sequence. The presence of these multiecho signatures is explained using a simple model based on spins rotating on the Bloch sphere, backed up by numerical calculations using the inhomogeneous Tavis-Cummings Hamiltonian.
We show experimentally and describe theoretically how a conventional magnetic resonance Hahn echo sequence can lead to a self-stimulated pulse echo train when an inhomogeneously broadened spin ensemble is coupled to a resonator. Effective strong coupling between the subsystems assures that the first Hahn echo can act as a refocusing pulse on the spins, leading to self-stimulated secondary echoes. Within the framework of mean field theory, we show that this process can continue multiple times leading to a train of echoes. We introduce an analytical model that explains the shape of the first echo and numerical results that account well for the experimentally observed shape and strength of the echo train and provides insights into the collective effects involved.
Self-stimulated echoes have recently been reported in the high cooperativity and inhomogeneous coupling regime of spin ensembles with superconducting resonators. In this work, we study their relative amplitudes using echo-silencing made possible by a fast frequency tunable resonator. The highly anisotropic spin linewidth of Er3+ electron spins in the CaWO4 crystal also allows to study the dependence on spin-resonator ensemble cooperativity. It is demonstrated that self-stimulated echoes primarily result from a combination of two large control pulses and the echo preceding it.
The use of superconducting microresonators together with quantum-limited Josephson parametric amplifiers has enhanced the sensitivity of pulsed electron spin resonance (ESR) measurements by more than four orders of magnitude. So far, the microwave resonators and amplifiers have been designed as separate components due to the incompatibility of Josephson junction–based devices with magnetic fields. This has produced complex spectrometers and raised technical barriers toward adoption of the technique. Here, we circumvent this issue by coupling an ensemble of spins directly to a weakly nonlinear and magnetic field–resilient superconducting microwave resonator. We perform pulsed ESR measurements with a 1-pL mode volume containing 6 × 10 7 spins and amplify the resulting signals within the device. When considering only those spins that contribute to the detected signals, we find a sensitivity of 2.8 × 1 0 3 spins / Hz for a Hahn echo sequence at a temperature of 400 mK. In situ amplification is demonstrated at fields up to 254 mT, highlighting the technique’s potential for application under conventional ESR operating conditions.
The electrical detection of spin echoes via echo tomography is used to observe coherent processes associated with the electrical readout of the spin state of phosphorus donor electrons in silicon near a SiO2 interface. Using the Carr-Purcell pulse sequence, an echo decay with a time constant of 1.7+/-0.2 micros is observed and discussed in terms of decoherence and recombination times. Electrical spin echo tomography thus can be used to study the dynamics of the spin-dependent transport processes, e.g., in realistic spin qubit devices for quantum information processing.
We report on electron spin resonance measurements of phosphorus donors localized in a 200 μm^{2} area below the inductive wire of a lumped element superconducting resonator. By combining quantum limited parametric amplification with a low impedance microwave resonator design, we are able to detect around 2×10^{4} spins with a signal-to-noise ratio of 1 in a single shot. The 150 Hz coupling strength between the resonator field and individual spins is significantly larger than the 1-10 Hz coupling rates obtained with typical coplanar waveguide resonator designs. Because of the larger coupling rate, we find that spin relaxation is dominated by radiative decay into the resonator and dependent upon the spin-resonator detuning, as predicted by Purcell.
Electron spin resonance scanning tunneling microscopy (ESR-STM) has become a powerful tool for probing spin dynamics and coherence of individual atoms and molecules on surfaces. In this work, we perform Rabi oscillation and Hahn echo pulse protocols on individual iron phthalocyanine (FePc) molecules on MgO/Ag(001) using ESR-STM. While Hahn echo protocols are widely used to extract spin coherence times, we show that in ESR-STM they are particularly susceptible to misinterpretation due to tunneling electrons generated by the applied radio-frequency (RF) voltage. The RF voltage not only drives the spin, but simultaneously probes and relaxes it, which consequently leads to an exponential decay that reflects spin relaxation rather than intrinsic phase coherence. We moreover show that varying both delay times in the refocusing pulse sequence is a reliable way to ensure a coherent nature of the echo signal. The extracted decay for the latter protocol suggests that T2 is approximately 30 ns and is thus closer to the decoherence time observed in Rabi oscillation measurements. This is significantly shorter than values reported in previous echo measurements. Our findings underscore the need for caution in interpreting T2 times from Hahn echo and Carr-Purcell protocols in ESR-STM and provide practical criteria for distinguishing true spin echoes from tunneling-induced relaxometry signals.