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Register a new userPump-Probe Experiments on the Single-Molecule Magnet Fe8 : Measurement of Excited Level Lifetimes
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We present magnetization measurements on the single molecule magnet Fe8 in the presence of pulsed microwave radiation. A pump-probe technique is used with two microwave pulses with frequencies of 107 GHz and 118 GHz and pulse lengths of several nanoseconds to study the spin dynamics via time-resolved magnetization measurements using a Hall probe magnetometer. We find evidence for short spin-phonon relaxation times of the order of one microsecond. The temperature dependence of the spin-phonon relaxation time in our experiments is in good agreement with previously published theoretical results. We also established the presence of very short energy diffusion times, that act on a timescale of about 70 ns.
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We present pump-probe measurements on the single-molecule magnet Fe_8 with microwave pulses having a length of several nanoseconds. The microwave radiation in the experiments is located in the frequency range between 104 GHz and 118 GHz. The dynamics of the magnetization of the single Fe_8 crystal is measured using micrometer-sized Hall sensors. This technique allows us to determine the level lifetimes of excited spin states, that are found to be in good agreement with theoretical calculations. The theory, to which we compare our experimental results, is based on a general spin-phonon coupling formalism, which involves spin transitions between nearest and next-nearest energy levels. We show that good agreement between theory and experiments is only obtained when using both the Delta m_S = +-1 transition as well as Delta m_S = +-2, where Delta m_S designates a change in the spin quantum number m_S. Temperature dependent studies of the level lifetimes of several spin states allow us finally to determine experimentally the spin-phonon coupling constants.
The low temperature spin dynamics of a Fe8 Single-Molecule Magnet was studied under circularly polarized electromagnetic radiation allowing us to establish clearly photon-assisted tunneling. This effect, while linear at low power, becomes highly non-linear above a relatively low power threshold. This non-linearity is attributed to the nature of the coupling of the sample to the thermostat.These results are of great importance if such systems are to be used as quantum computers.
We measure magnetization changes in a single crystal of the single-molecule magnet Fe8 when exposed to intense, short (<20 $mu$s) pulses of microwave radiation resonant with the m = 10 to 9 transition. We find that radiation induces a phonon bottleneck in the system with a time scale of ~5 $mu$s. The phonon bottleneck, in turn, drives the spin dynamics, allowing observation of thermally assisted resonant tunneling between spin states at the 100-ns time scale. Detailed numerical simulations quantitatively reproduce the data and yield a spin-phonon relaxation time of T1 ~ 40 ns.
The interplay between the oxidation state and the optical properties of molecules plays a key role for applications in displays, sensors or molecular-based memories. The fundamental mechanisms occurring at the level of a single-molecule have been difficult to probe. We used a scanning tunneling microscope (STM) to characterize and control the fluorescence of a single Zn-phthalocyanine radical cation adsorbed on a NaCl-covered Au(111) sample. The neutral and oxidized states of the molecule were identified on the basis of their fluorescence spectra that revealed very different emission energies and vibronic fingerprints. The emission of the charged molecule was controlled by tuning the thickness of the insulator and the plasmons localized at the apex of the STM tip. In addition, sub-nanometric variations of the tip position were used to investigate the charging and electroluminescence mechanisms.
We theoretically investigate quantum transport through single-molecule magnet (SMM) junctions with ferromagnetic and normal-metal leads in the sequential regime. The current obtained by means of the rate-equation gives rise to the tunneling anisotropic magnetoresistance (TAMR), which varies with the angle between the magnetization direction of ferromagnetic lead and the easy axis of SMM. The angular dependence of TAMR can serve as a probe to determine experimentally the easy axis of SMM. Moreover, it is demonstrated that both the magnitude and sign of TAMR are tunable by the bias voltage, suggesting a promising TAMR based spintronic molecule-device.
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