1. Introduction
Ultrafast magneto-acoustics investigates peculiarities of ultrafast magnetization dynamics driven by ultrashort, fs-laser-excited acoustic transients [
1,
2,
3,
4,
5]. In most cases the physical interpretation of magneto-elastic interactions roots back to numerically solving the Landau-Lifshitz-Gilbert equations for ferromagnetic resonance (FMR) precession driven by time- and space-dependent magneto-elastic fields. This approach is well justified when the characteristic time scales of the magnetization precession are much longer than the duration of magneto-elastic driving impact. Such simplified approach has been successfully used to describe the phenomenon of ultrafast magnetization switching in magnetostrictive thin films [
6] and nanomagnets [
7]. However, a closer look at the experimental data for magnetic semiconductors deposited on semi-infinite substrates [
8] evidenced some more complicated magnetization dynamics and revealed contributions of the spatially inhomogeneous mod magnetization precession due to perpendicular standing spin wave modes (PSSWs, to be called magnons throughout this paper). The investigated GaMnAs ferromagnetic thin film with a thickness
L=200 nm was too thick for individual modes (to be called magnons) to be spectrally resolved. Another complication was that the acoustic excitation in form of ultrashort acoustic pulses, injected in the GaMnAs layer from a semi-infinite GaAs substrate, was characterized by a continuous acoustic spectrum.
Several steps have been undertaken to get access to and quantify individual phonon-magnon interactions. First, reducing the thickness
L of a ferromagnetic layer below a few tens of nanometers allowed the magnon modes to be well separated in frequency domain [
9,
10]. Under these conditions, the injection of an ultrashort laser pulse from a semi-infinite substrate results in the excitation of multiple spectrally isolated magnon modes within the continuous frequency spectrum of ultrashort acoustic pulses [
11].
Second, Kim and Bigot have conceived and conducted an ultrafast optical experiment in a
300 nm thin freestanding nickel membrane acting as an acoustic cavity [
12]. In this experiment the modes of longitudinal acoustic phonons could be well resolved, each of them interacting with several spectrally overlapping magnon modes. Nevertheless, it was possible to partially discriminate distinct phonon-magnon resonances based on the selection rules for phonon and magnon modes of same/different parity [
13].
Third, a recent purely theoretical study by Vernik et al. discussed the details of resonant phonon-magnon interactions based for freestanding bi-layer and trilayer structures, based on some model parameters for acoustic and magnetic damping.
In the present manuscript we apply the results of quantitative analysis from Ghita et al. [
13], using the extracted frequency-dependent acoustic damping factor
and magnetic Gilbert damping parameter
, to inspect the dynamics of resonantly enhanced phonon-magnon interactions in the ultrahigh frequency range as a function of nickel thickness
L. The purpose of this work is to check the feasibility of experimental observation of this effect in the highest frequencies reaching the THz frequencies, i.e. the range important for studies in fundamental magnetism [
10,
14,
15,
16].
2. Theoretical description of ultrafast magneto-acoustics in freestanding magnetostrictive thin films
Absorption of an ultrashort acoustic pulse excitation in a freestanding nickel membrane results in a nearly instantaneous (on acoustic time scales) spatially inhomogeneous heating profile, which can be approximated by an exponential function
, see
Figure 1a. The characteristic heating depth
h typically exceed the optical penetration depth of laser light due to the diffusion of hot electrons during the picosecond electron-phonon relaxation time [
17,
18]. Since the electron-phonon relaxation time depends on the excitation conditions [
19], the effective heating depth
h becomes experiment-specific and is treated as a fitting parameter [
13,
20]. Throughout this manuscript, we are going to use the value
nm obtained from the comprehensive modeling of recent magneto-acoustic experiments [
13].
Once impulsively heated, the film starts vibrating due to the thermal expansion and the spatio-temporal dynamics of the acoustic strain
can be represented as a superposition of acoustic eigenmodes according to
We assume acoustic eigenmodes to oscillate at frequencies
and decay with damping constants
;
denote their initial phases. In a freestanding film, the acoustic eigenmodes obey the free boundary conditions for the acoustic displacement (corresponding to zero strains at both Ni/air interfaces) resulting in
where
is the wavevector of the
p-th acoustic eigenmode.
According to Ghita et al. [
13], in the frequency range 0 - 80 GHz, the damping coefficient
scaled as
. As this is coherent with a model of damping due to phonon-phonon scattering processes, we will extrapolate this scaling to frequencies up to 200 GHz, which is the highest frequency of a fundamental mode involved in our study.
In the same study, it was revealed that assuming an exponential heating profile, with penetration depth
h = 60 nm, offers a satisfactory description of the mode amplitudes extracted from the experiment of Kim and Bigot. Assuming that for
, the initial strain in the film is given by
, the individual mode amplitudes read
In the following, we will assume that the amplitude
and the characteristic length scale
h of the strain are constant and do not depend on the thickness
L of the freestanding thin film. This assumption neglects thin-film effects in light absorption and reflection of heat at the back nickel-air interface. Possible (minor) corrections due to the aforementioned effects do not change the conclusions in this manuscript.
With this in mind, we can examine the dependence of the first three mode amplitudes on the film thickness
L. It can be seen that, when going down to thinner films, the first acoustic mode becomes over-represented with respect to the higher-order harmonics. As shown in panel (d) of
Figure 2, the evolution of the strain amplitude of modes
and
is monotonous with respect to the increase of thickness
L. On the contrary, the acoustic mode
displays a maximum at
nm. While these modes start with comparable values around
nm, the first mode steeper increase than the others respect as
L decreases. Therefore, it is reasonable to assume that at lower film thicknesses, interactions governed by the first acoustic mode will dominate.
In a thin film of thickness
L the general form of the
spatially inhomogeneous magnetization precession
can be represented as a superposition in magnetic eigenmodes, i.e. PSSWs or exchange magnons superimposed on the FMR-precession (see
Figure 1a,c):
for
across the film with quantized wave vectors
and eigenfrequencies
where
is the exchange stiffness (the numerical value
=430 [meV Å
] for Ni is taken from Ref. [
9]),
stands for the gyromagnetic ratio,
is vacuum permeability and
ℏ is the Planck’s constant.
It has been shown recently [
11,
21] that in the linear approximation when the acoustic strains are small, the magneto-elastically driven dynamics for each magnon mode satisfy the equation of a damped driven harmonic oscillator,
The external magneto-elastic driving force
is proportional to the overlap integral between the magnon eigenmode with the acoustic strain pulse
. For our experimental geometry the prefactor
is proportional to the magnetostriction coefficient
and depends both on the magnitude and orientation of an external magnetic field
.
Using the decomposition of the acoustic strain in its respective eigenmodes, the expression of the magneto-elastic driving force becomes
Here we have introduced the overlap integral [
21]
between the
n-th magnetic and
p-th acoustic eigenmodes.
Therefore, the theoretical modeling in ultrafast magnetoacoustics is reduced to solving Eq. (
6) driven by a superposition of acoustic eigenmodes. The latter are quantified by amplitudes
, frequencies
and damping constants
. In order to evaluate the overall efficiency of magneto-elastic interactions it is sufficient to inspect the analytical solutions for each magnon mode
n driven by an individual phonon mode with index
p, as a function of nickel thickness
L. For the purposes of numerical simulations, we use the valid experimental parameters used in [
13], namely
T,
m/s and
.
We note that the change in thickness of the film leads to a shift of acoustic frequencies with respect to the magnon modes, thus drifting away from the resonant regime. In order to preserve the resonant behavior, one needs to adjust the magnetic field . In the following, we will preserve the orientation of at an angle with respect to the normal, while varying its modulus. Furthermore, we will focus in our numerical studies on the interactions of the and acoustic mode with the and magnon modes, as well as that of acoustic mode with and magnon modes.
This resonant tuning of to the acoustic frequencies induces a change in the prefactor , which in turn changes the driving force amplitude.
In the case of resonant interaction between a phonon and a magnon mode (
), the precession of magnetization in time is given by
The expression for the maximum amplitude of magnetization precession of the
nth magnon mode resonantly driven by the
pth acoustic mode reads:
The damping-dependent factor
can be understood in terms of the quality factors
and
for magnon and phonon modes, respectively:
Therefore we conclude that resonant phonon-magnon interactions are enhanced by the
smaller Q-factor.
Mathematical derivation of equations (11-13) is provided in the Appendix A. The rest of the manuscript will be devoted to their numerical analysis for nickel membranes of arbitrary thickness L.
3. Numerical results for acoustically driven magnetization dynamics and their discussion
In this section, we show the numerical results obtained through the prism of the above-mentioned theoretical treatment.
Figure 3 shows the results for driven magnon oscillator equations, for the
,
and
,
magnon-phonon pairs, respectively. The expected behavior of the rise and subsequent decay is recovered. We notice that both of the rise and decay time scales are decreasing as the film thickness decreases. Naturally, the frequency of these excitations increases, reaching values of up to 160 GHz.
We can already notice that in case of the FMR-mode driven by the phonon mode, the maximal magnetization displays the non-monotonous dependence on the film thickness L. Furthermore, the magnetic field needed to achieve this resonance increases with the decreasing thickness. For the considered values of the thickness ( nm, nm, nm, nm and nm), there is no clear conclusion on the dependence of this maximal magnetization in the case of the magnon mode driven by the phonon mode. As such, it is interesting to study the dependence of the maximal magnetization achieved, as well as the magnetic field needed for the resonant interaction, as a function of the film thickness L.
Figure 4 shows the thickness dependence of the resonant magnetic field (lower panel) and the maximal magnetization (upper panel) for six distinct phonon-magnon resonances. We start our discussion from two phonon-magnon resonances observed in the Kim & Bigot experiment performed for
nm [
13]: the
-excited
FMR precession and the
-excited
magnon. In the first case, one can see that for
nm the FMR precession can be amplified by a factor of 10 as compared with Kim & Bigot experiment. Meanwhile, for the driving of
mode, a peak precession amplitude is achieved for
nm, but the increase in precession with respect to the Kim-Bigot experiment is marginal (only a factor of 1.25).
One can furthermore see that these two
low-order phonon-magnon resonances are the ones with the largest amplitudes when going towards smaller thicknesses. Furthermore, in terms of the required resonant magnetic fields, for film thicknesses
nm the fields stay in the range below 10 T (and below 5 T for low-order resonances). These experimentally achievable magnetic fields suggest that for this range of thicknesses, resonant phonon-magnon interaction can be observed and measured. The problem arises when considering the behaviour at very small film thicknesses (or, equivalently, at very high frequencies, exceeding 100 GHz). One notices that the required resonant required magnetic fields diverge to unreasonably high values. However, for certain phonon-magnon pairs (evidenced with dotted lines in
Figure 4), there is a sharp decrease toward zero of these required magnetic fields. As such, at certain very low thicknesses, one can again find high-frequency phonon-magnon resonances at experimentally reasonable magnetic fields.
We will focus our analysis on one of these cases, namely, that of a
nm film thickness.
Figure 5b shows the magneto-acoustic interaction landscape, given by the dependence of the magnitude of the Fourier transform of
on the external magnetic field. One notices a rather faint, yet visible trace of resonant behavior at the intersection of the
and
phonon and magnon curves. This resonant enhancement is achieved for the external magnetic field value
T, at a frequency of approximately 200 GHz. Numerical simulation of magnetization dynamics at this set of experimental parameters shows indeed a behaviour as expected, with the typical rise and decay time being evident on the magnetization dynamics. As such we have achieved the main goal of this paper to demonstrate that previously anticipated higher-order phonon-magnon resonances in hybrid metal-ferromagnet membranes [
21] can be indeed achieved using realistic parameters [
13] in much simpler structures, i.e. thin nickel membranes.
It is worth mentioning that the resonant curve is described by the analytical expression Eq.
12. As such, Eq.
12 represents a powerful tool to engineer arbitrary phonon-magnon resonances as a function of magnetic and acoustic material parameters. For example, experiments with magnetic dielectrics BiYIG [
15,
22,
23,
24,
25], characterized by orders-of-magnitude lower values of the Gilbert damping parameter
, may seem better candidates to observe large-amplitude phonon-magnon interactions at first glance. However, in the limit
Eq.
14 converges towards
indicating the crucial role of the acoustic damping
in this case. This rather straightforward example demonstrates that the choice of an optimum combination of membrane’s material and thickness represents a rather nontrivial multiparameter optimization problem.