Transmission Spectroscopy of Molecular Spin Ensembles in the Dispersive Regime

The readout in the dispersive regime is originally developed—and it is now largely exploited—for non-demolitive measurement of super- and semiconducting qubits. More recently it has been successfully applied to probe collective spin excitations in ferro(i)magnetic bulk samples or collections of paramagnetic spin centers embedded into microwave cavities. The use of this readout technique within a semiclassical limit of excitation is only marginally investigated although it holds for a wide class of problems, including advanced magnetic resonance techniques. In this work, the coupling between a coplanar microwave resonator and diphenyl-nitroxide organic radical diluted in a fully deuterated benzophenone single crystal is investigated. Two-tone transmission spectroscopy experiments demonstrate the possibility to reconstruct the spectrum of the spin system with little loss of sensitivity with respect to the resonant regime. Likewise, pulse sequences of detuned microwave frequency allow the measurement of the spin-lattice relaxation time (T1). The independent tunability of the probe and the drive power enables one to adjust the signal-to-noise ratio of the spectroscopy. These results suggest that electron spin dispersive spectroscopy can be used as a complementary tool of electron spin resonance to investigate the spin response

Photoswitching of a thermally unswitchable molecular magnet Cu(hfac) 2Li-Pr evidenced by steady-state and time-resolved electron paramagnetic resonance

Most photoswitchable molecular magnets exhibit thermally induced switching, as is typical of spin crossover (SCO), valence tautomerism and SCO-like phenomena. We report a rare case of a copper-nitroxide based molecular magnet Cu(hfac)2Li-Pr that does not exhibit quantitative SCO-like behavior in the temperature range of its chemical stability (2-350 K); however, it can be switched to a metastable thermally inaccessible spin state via visible/near-IR light at cryogenic temperatures. By means of photogeneration, unique information on this otherwise unobservable spin state has been obtained using steady-state Q-band (34 GHz) and time-resolved W-band (94 GHz) electron paramagnetic resonance (EPR) spectroscopy. In particular, we have found that the electronic structure and relaxation properties of the photoinduced state in Cu(hfac)2Li-Pr are very similar to those in its sister compound Cu(hfac)2Ln-Pr that is thermally switchable and has been exhaustively characterized by many analytical methods, previously. The first observation of photoswitchable behavior in a thermally unswitchable copper-nitroxide based molecular magnet Cu(hfac)2Li-Pr paves the way for photoswitching applications of this and similar compounds in the remarkably broad temperature range of 2-350 K. © 2014 American Chemical Society

Self-calibrating Quantum State Tomography

We introduce and experimentally demonstrate a technique for performing quantum state tomography on multiple-qubit states despite incomplete knowledge about the unitary operations used to change the measurement basis. Given unitary operations with unknown rotation angles, our method can be used to reconstruct the density matrix of the state up to local sigma-z rotations as well as recover the magnitude of the unknown rotation angle. We demonstrate high-fidelity self-calibrating tomography on polarization-encoded one- and two-photon states. The unknown unitary operations are realized in two ways: using a birefringent polymer sheet---an inexpensive smartphone screen protector---or alternatively a liquid crystal wave plate with a tuneable retardance. We explore how our technique may be adapted for quantum state tomography of systems such as biological molecules where the magnitude and orientation of the transition dipole moment is not known with high accuracy.Comment: 13 pages, 4 figure