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Register a new userSurface single-molecule dynamics controlled by entropy at low temperatures
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Configuration transitions of individual molecules and atoms on surfaces are traditionally described with energy barriers and attempt rates using an Arrhenius law. This approach yields consistent energy barrier values, but also attempt rates orders of magnitude below expected oscillation frequencies of particles in the meta-stable state. Moreover, even for identical systems, the measurements can yield values differing from each other by orders of magnitude. Using low temperature scanning tunnelling microscopy (STM) to measure an individual dibutyl-sulfide molecule (DBS) on Au(111), we show that we can avoid these apparent inconsistencies if we account for the relative position of tip apex and molecule with accuracy of a fraction of the molecule size. Altering the tip position on that scale modifies the transitions barrier and attempt rate in a highly correlated fashion, which on account of the relation between the latter and entropy results in a single-molecular enthalpy-entropy compensation. By appropriately positioning the tip apex the STM tip can be used to select the operating point on the compensation line and modify the transition rates. The results highlight the need to consider entropy in transition rates of a single molecule, even at temperatures where entropy effects are usually neglected.
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Comment on the paper: Magnetization Process of Single Molecule Magnets at Low Temperatures of J.F.Fernandez and J.J.Alonso (PRL 91, 047202 (2003)).
We model magnetization processes that take place through tunneling in crystals of single-molecule magnets, such as Mn_12 and Fe_8. These processes take place when a field H is applied after quenching to very low temperatures. Magnetic dipolar interactions and spin flipping rules are essential ingredients of the model. The results obtained follow from Monte Carlo simulations and from the stochastic model we propose for dipole field diffusion. Correlations established before quenching are shown to later drive the magnetization process. We also show that in simple cubic lattices, m propto sqrt(t) at time t after H is applied, as observed in Fe_8, but only for 1+2log_10(h_d/h_w) time decades, where h_d is some near-neighbor magnetic dipolar field and a spin reversal can occur only if the magnetic field acting on it is within some field window (-h_w,h_w). However, the sqrt(t) behavior is not universal. For BCC and FCC lattices, m propto t^p, but p simeq 0.7 . An expression for p in terms of lattice parameters is derived. At later times the magnetization levels off to a constant value. All these processes take place at approximately constant magnetic energy if the annealing energy epsilon_a is larger than the tunneling windows energy width (i.e., if epsilon_a gtrsim gmu_B h_w S). Thermal processes come in only later on to drive further magnetization growth.
We show that correlations established before quenching to very low temperatures, later drive the magnetization process of systems of single molecule magnets, after a magnetic field is applied at t=0. We also show that in SC lattices, m propto sqrt(t), as observed in Fe_8, but only for 1+2*log_10(h_d/h_w) time decades, where h_d is a nearest neighbor dipolar magnetic field and a spin reversal can occur only if the field on it is within (-h_w,h_w). However, the sqrt(t) behavior is not universal. For BCC and FCC lattices, m propto t^p, but p simeq 0.7. The value to which m finally levels off is also given.
The energy dependent thermoelectric response of a single molecule contains valuable information about its transmission function and its excited states. However, measuring it requires devices that can efficiently heat up one side of the molecule while being able to tune its electrochemical potential over a wide energy range. Furthermore, to increase junction stability devices need to operate at cryogenic temperatures. In this work we report on a new device architecture to study the thermoelectric properties and the conductance of single molecules simultaneously over a wide energy range. We employ a sample heater in direct contact with the metallic electrodes contacting the single molecule which allows us to apply temperature biases up to $Delta T = 60$K with minimal heating of the molecular junction. This makes these devices compatible with base temperatures $T_mathrm{bath} <2$K and enables studies in the linear ($Delta T ll T_mathrm{molecule}$) and non-linear ($Delta T gg T_mathrm{molecule}$) thermoelectric transport regimes.
Electron transport in mesoscopic contacts at low temperatures is accompanied by logarithmically divergent equilibrium noise. We show that this equilibrium noise can be dramatically suppressed in the case of a tunnel junction with modulated (time-dependent) transparency, and identify the optimal protocol. We show how such a contact could be used either as an optimal electron entangler or as a single-electron source with suppressed equilibrium noise at low temperatures.
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