IEEE TRANSACTIONS ON MAGNETICS, VOL. 49, NO.

7, JULY 2013 3147

Spin Pumping in Permalloy/Graphene and Permalloy/Graphite Interfaces

Simranjeet Singh , Ajit Kumar Patra , Brett Barin , Enrique del Barco , and Barbaros Özyilmaz
Department of Physics, University of Central Florida, Orlando, FL 32816 USA
Department of Physics, National University of Singapore, Singapore 117542
NanoCore, National University of Singapore, Singapore 117576
Graphene Research Center, National University of Singapore, Singapore 117542
NUS Graduate School for Integrative Sciences and Engineering (NGS), National University of Singapore, Singapore 117456

This article reports a comparative study of the spin pumping induced by graphite and graphene layers adjacent to an extended fer-
romagnetic Permalloy film. The corresponding enhancement of the Gilbert damping in the ferromagnet is determined by analyzing the
frequency dependence of the ferromagnetic resonance linewidth in experiments done with a broad band microwave spectrometer. The
results show that a single graphene layer is more efficient than a thick graphite film in absorbing the angular momentum pumped away
from the Permalloy during the resonant precession of its magnetization. We associate this effect to an enhancement of the spin-orbit cou-
pling in the graphene layer due to Copper adatoms residual from the chemical vapor deposition process used to synthesize the graphene
used in the experiments.
Index Terms— Magnetoelectronics, spin polarized transport.

T HE theoretical prediction of large spin relaxation times

due to the absence of nuclear spins and weak spin-orbit
coupling [1] places graphene as a promising base system for
future spintronics devices. Spin relaxation lengths of the order
of micrometers have been already reported for graphene-based
spin valves [2]–[4]. Therefore, fostering the understanding of
spin dynamics in grapheme is necessary for a potential appli-
cation of this versatile material in future spintronics applica-
tions. Along these lines an exciting research avenue focuses
on advancing efficient means to generate pure spin currents in
graphene. The most widely method used so far is nonlocal spin
injection [5], also known as electrical spin injection, wherein
spin currents are injected into graphene from an adjacent fer-
romagnetic metal layer. As this method involves spin currents
transferred by charge transport across the ferromagnet/graphene
interface, the spin injection efficiency is relatively small due to
the impedance mismatch between the two materials. To circum-
vent this issue a thin insulator can be sandwiched in between the
ferromagnet and the graphene layer to act as a tunnel barrier,
avoiding the impedance mismatch problem and increasing spin
accumulation at the interface. Yet the highest spin efficiency
achieved so far is only about 30% in nonlocal graphene spin
valves with tunnel junctions [6]. In addition, the employment
of spin polarized charge currents through tunnel junctions carry
practical reliability issues. An alternative way of injecting spin
currents in nonmagnetic materials is by means of dynamical
spin pumping, by which the coherent precession of the mag-
netization of a ferromagnetic film pumps spin into an adjacent
nonmagnetic film [7]. Here, instead of a charge current carrying
the spins across the ferromagnetic/nonmagnetic (FM/NM) in-
terface, the net spin angular momentum generated by the mag-
netization precession in the ferromagnet is directly transferred
Manuscript received October 31, 2012; revised January 15, 2013; accepted
January 25, 2013. Date of current version July 15, 2013. Corresponding author:
E. del Barco (e-mail: delbarco@physics.ucf.edu).
Color versions of one or more of the figures in this paper are available online
at http://ieeexplore.ieee.org.
Digital Object Identifier 10.1109/TMAG.2013.2244067
into the nonmagnetic layer by dynamical exchange interaction,
thus rendering this technique free of the impedance mismatch
problem since there is no charge current involved. In addition,
dynamical spin pumping enables spin injection over large meso-
scopic areas.
Although spin pumping has been typically employed to gen-
erate pure spin currents in different metals and semiconductor
materials over the last couple of years, it is only very recently
that this method has been successfully used to generate pure spin
currents in an extended graphene layer [8]. In that work [8] spin
pumping graphene grown by chemical vapor deposition (CVD)
was demonstrated by means of measuring the broadening of
the ferromagnetic resonance (FMR) spectra in extended ferro-
magnet/graphene (FM/Gr) films. The corresponding increase of
the FMR linewidth evidenced a remarkable enhancement of the
Gilbert damping in the ferromagnet due to a transfer (pumping)
of spin angular momentum at the FM/Gr interface. Note that the
pumped spins need to be absorbed by the nonmagnetic material
for the Gilbert damping in the ferromagnet to be affected during
the magnetization dynamics. In fact, the observed effect was
found to be even larger than in equivalent studies with nonmag-
netic layers made up of heavy metals Pt and Pd, where an intrin-
sically strong spin-orbit interaction provides an efficient source
of spin relaxation [9], [10]. NM films of thickness larger than
the corresponding spin relaxation length had to be employed
in the experiments mentioned above to efficiently absorb the
pumped spins. In FM/NM films using thick metallic NM layers
(e.g., Pt) the spins injected can relax perpendicularly to the in-
terface into the thick NM layer. This is not possible in the case
of graphene—a prototypal two-dimensional material with zero
effective thickness. In addition, the large damping enhancement
produced by a single layer graphene in our previous experiments
is surprising attending to the weak spin-orbit coupling theoret-
ically predicted in this material, which eliminates an important
source of spin relaxation apart of coulomb impurities or short
range scatters. We pointed at a potential huge enhancement of
the spin-orbit interaction induced by Cu adatoms residual from
the CVD synthesis of the graphene films.

0018-9464/$31.00 © 2013 IEEE

3148 IEEE TRANSACTIONS ON MAGNETICS, VOL. 49, NO. 7, JULY 2013

Fig. 1. Schematics of the three samples studied in this work: Py, Py/HOPG, and
Py/Graphene extended films on substrates. As indicated in the sketch,
the samples are placed upside-down over the central part of the micro-coplanar
waveguide used to perform the FMR measurements.

Fig. 2. (a) 10 GHz FMR absorption spectra for the three samples studied in this
work as a function of a magnetic field applied along the plane of the films. (b)
To better understand the nature of spin injection in FM/Gr in- The field derivative of the waveguide transmission parameter allows the analysis
of the FMR linewidth which is extracted from the peak-to-peak distance.
terfaces in this report we present a comparison study of the dy-
namical spin pumping in extended FM/NM films where highly
ordered pyrolitic graphite (HOPG) is employed as the NM layer.
The 10 GHz FMR spectra (transmission parameter )
Although the FMR linewidth of the FM/HOPG film broadens
recorded for the three samples sweeping the magnetic field
with respect to that of the FM layer alone, the effect is substan-
applied parallel to the film plane (within 0.5 degrees) are
tially smaller than that observed in FM/Gr films, indicating that
shown in Fig. 2(a). The frequency and magnetic field angular
the main spin relaxation processes occur at the interface, where
behaviors of all samples have also been obtained to determine
graphene is expected to present a stronger spin-orbit coupling
the magnetic anisotropy of the films (not shown). Only small
than HOPG due to residual Cu adatoms.
variations in the effective saturation magnetizations have been
Large area graphene was grown by means of CVD on thin
found within the samples, with the effective saturation magne-
foils of Copper [11], [12]. The films were subsequently trans-
tization decreasing from 7.3 kG (in Py) to 6.1 kG (in Py/HOPG)
ferred onto substrates. The organic residues remaining
and to 5.8 kG (in Py/Gr), which explains the different positions
on the surface of the graphene were cleaned by thermal an-
of the FMR resonances in Fig. 2(a) (1.28, 1.43, and 1.55 kG,
nealing in the presence of an optimized flow of Hydrogen and
respectively). This could be done to a successive enhancement
Argon at 300C [13]. The graphene surface was further charac-
of the interface anisotropy due to the presence of the graphite
terized by atomic force microscopy and its single layer nature
and graphene layers or to the creation of a dead magnetic layer
confirmed by Raman spectroscopy. The HOPG sample was pur-
which effectively decreases the magnetization value. Changes
chased from SPI Supplies. The surface of graphite was cleaved
in other characteristic film parameters, such as the gyromag-
with residue-free tape to obtain a fresh and atomically flat sur-
netic ratio (with ), are found to be minor.
face just before depositing the ferromagnetic film atop. Electron
Fig. 2(b) shows the field derivative of the FMR spectra in
beam evaporation in high vacuum conditions was employed to
Fig. 2(a). The FMR linewidth is obtained as the peak-to-peak
deposit a 14 nm thickness Permalloy (Py) film at the same time
field difference of as indicated with arrows in
over the three samples under study: a) a bare sub-
Fig. 2(b). The broadening of the spectra is lower in the
strate (control sample Py), b) extended CVD graphene layer
Py/HOPG sample than in Py/Gr. As mentioned above, the in-
on (sample Py/Gr), and c) extended HOPG film on
crease in the FMR linewidth is associated to an enhancement of
(sample Py/HOPG). The HOPG samples used in the
the Gilbert damping in the ferromagnetic film due to pumping
experiments are about 300–400 um thick, well above the spin
of angular momentum into the adjacent nonmagnetic layer.
diffusion length of the material. Sketches representing the three
To analyze this effect in detail we measured the frequency
samples are shown in Fig. 1. A broadband micro coplanar wave-
dependence of the FMR linewidths over a wide microwave
guide ( -CPW) FMR spectrometer [14] (50 ohm impedance)
frequency range with the external field applied in the film
was used to study the FMR response of the sample upon mi-
plane. The observed results on the three studied samples are
crowave stimuli of frequencies ranging from 1 to 20 GHz. The
compared in Fig. 3, where one can clearly see that the broad-
FM/NM samples were placed upside-down over the central con-
ening in the Py/HOPG sample is not as pronounced as the one
stricted part of the waveguide [15]–[17] (see Fig. 1) to max-
observed in Py/Gr. The fact that the linewidth increases linearly
imize the intensity of the microwave field and signal-to-noise
with frequency for all samples indicates that damping in the
ratio. The -CPW was covered with a 100 nm hardened insu-
ferromagnetic film follows the phenomenological Landau-Lif-
lating e-beam resist to avoid any possible external damping pro-
shitz-Gilbert damping model. According to this model, the
duced by the proximity of the waveguide. A 1.4-Tesla rotatable
frequency behavior of the FMR linewidth can be written as
split electromagnet and an Agilent PNA Vector Network Ana-
lyzer were used to perform the FMR characterization at room
(1)
temperature.
SINGH et al.: SPIN PUMPING IN PERMALLOY/GRAPHENE AND PERMALLOY/GRAPHITE INTERFACES
Fig. 3. Frequency dependence of the FMR linewidth for the three samples
studied. The respective slopes are proportional to the Gilbert damping param-
eter in the Permalloy film, which is maximally increased by the CVD graphene
layer underneath the ferromagnet.
The first term on the right hand side of (1) is independent of the
frequency and represents the inhomogeneity of the polycrys-
talline ferromagnetic film (i.e., not all the magnetization pre-
cesses coherently throughout the whole film). The results show
that the inhomogeneous broadening is indeed negligible in our
samples (the data extrapolates to zero linewidth at ). The
second term is linear with frequency and represents the dynam-
ical broadening of the FMR, which is directly associated with
the Gilbert damping , being the damping pa-
rameter. Fitting of the data in Fig. 3 to (1) provides the fol-
lowing values for the damping parameters: and
for the Py sample [8],
and for the Py/HOPG sample, and
and for the Py/Gr
sample [8]. These values represent an increase in the Gilbert
damping in Py/HOPG and Py/Graphene of 37% and 88% with
respect to the Py film, respectively. These results confirm the re-
markable enhancement of the ferromagnetic damping induced
by a single CVD graphene layer, which is surprisingly high rel-
ative to the damping enhancement generated by other nonmag-
netic metals reported so far. Importantly, the present results in-
dicate that the effect obtained with graphene is even larger than
with graphite, which can be considered the three-dimensional
extension of graphene. Although the slight reduction in the sat-
uration magnetizations of the Py/HOPG and Py/Graphene could
contribute to increasing damping in these samples, we exclude
this possibility as the main source for the following reasons: a)
there is no evidence of a noticeable increase of inhomogeneous
broadening, which would be expected from a more inhomoge-
neous interface. In fact, the inhomogeneous broadening is neg-
ligible in all samples, indicating the quality of the interfaces;
b) the gyromagnetic ratio does not change (same frequency vs.
field slopes); c) similar FMR broadening is obtained when the
field is applied perpendicular to the film, a configuration where
common damping sources (i.e. magnons) are less effective. And
finally, c) results obtained in other samples (not shown) in where
different reductions of the saturation magnetization were ob-
served led to a similar damping enhancement.
3149
Let us conclude by focusing on the differences observed
in damping between the graphene and the graphite samples,
which is the objective of this article. In a standard Py/NM
metallic system the spin current injected into the NM layer
decays mainly perpendicularly to the interface, causing the
enhancement of the damping parameter to depend on the ratio
between the layer thickness and the spin-diffusion length in
the NM film. This is because some of the angular momentum
transmitted into the NM layer can flow back into the Py due to
the out-of-equilibrium spin accumulation in the NM layer and,
consequently, effectively decrease the amount of momentum
pumped out of the Py [18]. For heavy metals with strong
spin-orbit coupling pumped spins quickly diffuse in the NM
decreasing the probability to backflow into the Py, even when
using thin NM layers, such as in the case of Pt and Pd. In
metals with larger spin diffusion times, e.g., metals in where
the spin-orbit coupling is small such as in the case of Cu, the
enhancement of the Gilbert damping will be less pronounced
and thicker NM layers will be necessary to efficiently absorb
the angular momentum pumped away from the Py [19]. This is
what makes the observed enhancement of the Gilbert damping
in Py/Gr so special, since graphene has effectively zero thick-
ness and, at least theoretically, a very weak intrinsic spin-orbit
coupling. Consequently, one would expect the effect to be
stronger when using graphite, contrary to the observations.
Furthermore, some sizable spin-orbit coupling must exist in
CVD graphene films to explain our results, and this should
overcome the one provided by thick films made up of HOPG
and even heavy metals. The latter may also explain the gener-
ally observed very short spin relaxation times in lateral CVD
graphene spin valves [20]. Indeed, small levels of hydrogen
[21] and copper adatoms [22], [23] (as well as other transition
metal ions [24], [25]) have been predicted to lead to a strong
enhancement of the spin-orbit coupling, bringing it into the
meV range. Small levels of Cu adatoms are likely to remain
from the synthesis of the CVD samples utilized in our exper-
iments, pointing at a possible explanation for the remarkably
large spin pumping effect observed in the Py/Gr bilayer, since
this kind of scattering centers are not found in HOPG films.
Nevertheless, the remarkable enhancement of spin pumping
provided by graphene when compared to graphite and other
thicker NM systems remains to be quantitatively explained.
Theoretical efforts designed to understand the nature of spin
pumping in a FM/Gr system are also needed since current
theories cannot be applied for zero-thickness NM layers.
ACKNOWLEDGMENT
S. Singh, B.Barin, and E. del Barco acknowledge support
from the National Science Foundation (Grant DMR-0747587).
A. K. Patra and B. Özyilmaz acknowledge support from the Sin-
gapore National Research Foundation (NRF-RF2008-07) and
NUS-Young Investigator Award (R144-000-283-101).
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