Classical to quantum mechanical tunneling mechanism crossover in thermal transitions between magnetic states
| Autor: | Valery M. Uzdin, Sergei M. Vlasov, Pavel F. Bessarab, Hannes Jónsson |
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| Přispěvatelé: | St. Petersburg National Research University of Information Technologies, Mechanics and Optics (ITMO), St. Petersburg State University, Department of Applied Physics, Aalto-yliopisto, Aalto University |
| Rok vydání: | 2016 |
| Předmět: |
ta114
Condensed matter physics Chemistry Crossover 02 engineering and technology Activation energy 021001 nanoscience & nanotechnology 01 natural sciences Transition state theory Saddle point 0103 physical sciences Physical and Theoretical Chemistry 010306 general physics 0210 nano-technology Anisotropy Quantum Quantum tunnelling Spin-½ |
| Zdroj: | Faraday Discussions. 195:93-109 |
| ISSN: | 1364-5498 1359-6640 |
| DOI: | 10.1039/c6fd00136j |
| Popis: | Transitions between states of a magnetic system can occur by jumps over an energy barrier or by quantum mechanical tunneling through the energy barrier. The rate of such transitions is an important consideration when the stability of magnetic states is assessed for example for nanoscale candidates for data storage devices. The shift in transition mechanism from jumps to tunneling as the temperature is lowered is analyzed and a general expression derived for the crossover temperature. The jump rate is evaluated using a harmonic approximation to transition state theory. First, the minimum energy path for the transition is found with the geodesic nudged elastic band method. The activation energy for the jumps is obtained from the maximum along the path, a saddle point on the energy surface, and the eigenvalues of the Hessian matrix at that point as well as at the initial state minimum used to estimate the entropic pre-exponential factor. The crossover temperature for quantum mechanical tunneling is evaluated from the second derivatives of the energy with respect to orientation of the spin vector at the saddle point. The resulting expression is applied to test problems where analytical results have previously been derived, namely uniaxial and biaxial spin systems with two-fold anisotropy. The effect of adding four-fold anisotropy on the crossover temperature is demonstrated. Calculations of the jump rate and crossover temperature for tunneling are also made for a molecular magnet containing an Mn4group. The results are in excellent agreement with previously reported experimental measurements on this system. |
| Databáze: | OpenAIRE |
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