# Parity Effect in the Resonant Tunneling

## Abstract

A mechanism of the parity effect in the thermally assisted resonant tunneling is proposed in the view point of nonadiabatic transitions of thermally excited states. In this mechanism, alternating enhancement of the relaxation is naturally understood as a general property of quantum relaxation of uniaxial magnets at finite temperatures where appreciable populations are pumped up to excited states. It is also found that the enhanced sequence depends on the sweeping rate of the field.

PACS number: 75.40.Gb,76.20.+q

As to the relaxation of metastable magnetization of uniaxial nanoscale molecular magnets such as Mn<sub>12</sub> and Fe<sub>8</sub>, the resonant tunneling phenomena have been paid attention and various interesting properties of the phenomena have been reported. The key mechanism of the relaxation comes from their discrete energy structure due to a finite number of degrees of freedom. The eigenvalues of the system are functions of the parameters of the system, such as an external field. If we change a parameter infinitesimally small, then the system changes adiabatically, i.e., if the system is initially in the ground state, then it stays in the ground state of the system with the current value of the parameter. On the other hand, if the changing rate is finite, the system cannot completely follow the change of parameter and then so-called nonadiabatic transition occurs. For example in uniaxial magnetic systems, if we sweep the field very slowly from parallel to antiparallel to the initial magnetization, the magnetization adiabatically follows the field and reverses its direction. This change of magnetization corresponds to the tunneling (the adiabatic transition). If the sweeping rate is fast, then the magnetization only partially changes (the nonadiabatic transition).

In uniaxial magnets, quantum fluctuation is relevant only at avoided level crossing points and changes of magnetization only occur at those points. The sweeping rate dependence of the probability of staying in the original state in this type of nonadiabatic transition has been given by Landau , Zener , and Stükelberg  (LZS). We have studied changes of magnetization in a sweeping field from the view point of the LZS mechanism and proposed to obtain the tunneling gap from the magnetization change in a sweeping field and also explained the step-like magnetization process as a characteristic feature of nanoscale magnets. The LZS mechanism is pure quantum mechanical and it is independent of the temperature. However in experiments, strong temperature dependences have been observed, which brought an idea “thermally assisted resonant tunneling”. In order to explain this temperature dependence, various theoretical attempts have been done.

The sweeping rate dependences of magnetization process have been also observed in experiments at very low temperatures in Mn<sub>12</sub> and also in Fe<sub>8</sub>. There data do not depend on the temperature any more. We have pointed out that even in such cases there is still inevitable effect of the environment, and that we could nevertheless estimate the pure quantum transition probability.

Recently new aspects of the resonant tunneling have been reported, e.g., the parity effect of the resonant tunneling where amount of relaxation changes at the resonant points alternately, and $`\sqrt{t}`$-dependence of the initial relaxation of the magnetization at the resonant points. In the present Letter, we would like to propose a mechanism of the parity effect as a universal property of the thermally assisted resonant tunneling.

In order to investigate characteristics of temperature dependence of the resonant tunneling, we have constructed an equation of motion of the density matrix where effects of a thermal bath are taken into account (the quantum master equation):

$`{\displaystyle \frac{\rho (t)}{t}}`$ $`=`$ $`i[,\rho (t)]\lambda \left([X,R\rho (t)]+[X,R\rho (t)]^{}\right),`$ (1)   
where $``$ is the Hamiltonian, $`\rho (t)`$ is the density matrix of the system and $`X`$ is a system operator through which the system and the bath couple with the constant $`\lambda `$. Here we set $`\mathrm{}`$ to be unity. The first term of the right-hand side describes the pure quantum dynamics of the system while the second term represents effects of environments at a temperature $`T(=\beta ^1)`$. There $`R`$ is defined as follows:

$`k|R|m`$ $`=`$ $`\zeta (E_kE_m)n_\beta (E_kE_m)k|X|m,`$ (2)   
$`\zeta (\omega )`$ $`=`$ $`I(\omega )I(\omega ),\mathrm{and}n_\beta (\omega )=(e^{\beta \omega }1)^1,`$ (3)   
where $`|k`$ and $`|m`$ represent the eigenstates of $``$ with the eigenenergies $`E_k`$ and $`E_m`$, respectively. Here we adopt a thermal bath which consists of an infinite number of bosons $`_\mathrm{B}=_\omega \omega b_\omega ^{}b_\omega `$, where $`b_\omega `$ and $`b_\omega ^{}`$ are the annihilation and creation boson operators of the frequency $`\omega `$. We adopt the spectral density of the boson bath $`I(\omega )`$ in the form $`I(\omega )=I_0\omega ^2`$, which is associated with phonon reservoir. As to the interaction between the system and the bath we adopt a form $`X_\omega (b_\omega +b_\omega ^{})`$.

As a more relevant source of a noise at very low temperatures, we may consider the dipole field from other molecules or$`/`$and the hyperfine interaction from nuclear spins. For such noises we have to take into account another contribution to $`R`$. In this sense the bath treating here does not represent the experimental situation very appropriately. In the present Letter, however, we discuss only general natures which do not depend on the detail of the thermal bath.

Equation (1) with $`X=S_x+S_z`$ was used to study the aforementioned inevitable effects of environments in the magnetization process under a sweeping field at a very low temperature . For the process the existence of interaction is essential but detailed nature of the mechanism of the dissipation is not important. Thus we could discuss the property of the process as a universal property of the relaxation on nanoscale magnets. 

When the temperature goes up and the effect of the bath increases, the dissipative process becomes to depend on specific features of the bath and the coupling. Thus it becomes difficult to treat relaxation without specifying nature of the bath. However, in the present Letter, we will point out that the aforementioned parity effect is a universal property of the resonant tunneling at finite temperatures, which is independent of detailed nature of the bath.

Let us consider a general model of an $`S=10`$ uniaxial magnet in an external field:

$$=DS_z^2\mathrm{\Gamma }S_xH(t)S_z+Q,$$
(4)   
where $`Q`$ represents extra terms such as $`(S^+)^4+(S^{})^4`$, etc. We will propose a mechanism of the parity effect as a general property of uniaxial magnets. Thus we put $`Q=0`$.

In Fig. 1(a) we show a magnetization process $`M(t)=S_z/S`$ for the case with $`T=1.0`$, $`\lambda =0.00005`$, $`\mathrm{\Gamma }=0.45`$. We sweep the magnetic field $`H(t)=ctH_0`$ with $`c=0.0001`$ and $`H_0=0.3`$. In Fig. 1(b), the derivative $`dM/dH(=c^1dM/dt)`$ is also shown. In these figures, we find an alternate change of the amount of changes of the magnetization clearly. 

In Fig. 2, energy levels as a function of the field are shown. Here we see straight lines along which the magnetization is approximately given by $`m`$ or $`m^{}`$. These lines denoting energy levels for the diagonal parts of the Hamiltonian are called diabatic states. At each crossing point, a small energy gap is created by the off-diagonal terms and so-called avoided level crossing is formed, where large enhancement of relaxation occurs (resonant tunneling). The energy gaps of avoided level crossing points are listed in Table I, where we denote avoided level crossing points of levels of $`m`$ and $`m^{}`$ by $`(m,m^{})`$. There we find that the energy gaps at the same horizontal level in Fig. 2 (denoted by the same symbols) are about the same. This is easily understood from the fact that the gap is of order $`\mathrm{\Gamma }^{|mm^{}|}`$ where $`m`$ and $`m^{}`$ are the magnetizations of the crossing levels for $`\mathrm{\Gamma }=0`$ .

In order to see what processes are going, we show, in Fig. 3, the time evolution of distribution of occupation probabilities at the $`i`$th level, which is expressed by $`i|\rho |i`$.

This figure shows that the population along the line of $`m=8`$ decays at $`(8,5)`$ in Fig. 2 and the populations along the line $`m=9`$ and $`10`$ decay at $`(9,4)`$ and $`(10,3)`$, respectively. These points are shown by squares in Fig. 2.

If the system has an equilibrium distribution in the initial state, the population distributes on levels. The population at each line decays at an avoided level crossing point where the LZS transition probability 

$$p=1\mathrm{exp}\left[\frac{\pi (\mathrm{\Delta }E)^2}{2c|mm^{}|}\right]$$
(5)   
has an appreciable value. Here $`\mathrm{\Delta }E`$ is the energy gap at $`(m,m^{})`$. In Table I the transition probabilities are listed. For example the transition probability for $`c=0.0001`$ at $`(m,m^{})=(8,5)`$ (see Fig. 3) is 0.913, while at the point $`(8,6)`$ it is $`0.07`$. Thus most of the population of the line of $`m=8`$ decays at $`(8,5)`$. The population of the line of $`m=9`$ decays very little until $`(9,4)`$ because the transition probabilities at $`(9,6)`$ and $`(9,5)`$ are very small, i.e., 0.0006 and 0.04, respectively. The population of the line of $`m=10`$ decays at the point $`(10,3)`$.

As we found here, the parity effect simply comes from the structure of the energy levels. The structure of energy levels in Fig. 2 is inherent to the systems of the uniaxial Hamiltonian (4) regardless of the form $`Q`$ and we expect that the parity effect is observed generally in uniaxial magnets.

Here it should be noted that the relevant sequence of decays (in the above case $`H=0.3,0.5`$, and $`0.7`$) depends on the sweeping rate $`c`$. If $`c`$ decreases, then the transition probabilities increase. Thus the populations on the lines decay at the circled avoided level crossing points before reaching the points of squares. Thus in this case relaxation is enhanced at $`H=0.2,0.4`$, and $`0.6`$ instead of $`H=0.3,0.5`$, and $`0.7`$ in the case of $`c=0.0001`$. In Fig. 4, we plot the time evolution of the magnetization process in case of 20 times slower sweeping rate $`c=0.000005`$. In Fig. 5, we show the time evolution of probabilities at levels, where we actually find large decreases of the population at $`H=0.2,0.4`$, and $`0.6`$. Furthermore, in case of much slower sweeping rate $`c=0.00000005`$, we expect that the transitions occur at the points of triangles in Fig. 2 (see also Table I). We do not demonstrate it because it takes $`100`$ times longer simulation time. This sweeping rate dependence is also a general property of uniaxial magnets and we expect the shift of the sequence to be also found in experiments.

Finally we would like to point out a strange property of the system when the Hamiltonian (4) includes the interaction

$$Q=C[(S^+)^4+(S^{})^4]$$
(6)   
which has been discussed in literatures. As has been pointed out by Wernsdorfer and Sessoli, in the present model energy gaps at the avoided level crossing point change nonmonotonically with the value of $`C`$ ($`\mathrm{\Gamma }`$ is fixed) and even gapless points exist, which causes irregular behavior of resonant tunneling and simple parity effect is disturbed. The reason why gapless points appear is not clear at this moment, which would be an interesting problem. 

We would like to thank B. Barbara, H. De Raedt and W. Wernsdorfer for their valuable discussions. The present work is partially supported by the Grant-in-Aid from the Ministry of Education.