Controlling domain wall motion in ferroelectric thin filmsΒ Β· where π0=8.85Γ10β12 F/m is...
Transcript of Controlling domain wall motion in ferroelectric thin filmsΒ Β· where π0=8.85Γ10β12 F/m is...
Controlling domain wall motion in ferroelectric thin films
L. J. McGilly, P. Yudin, L. Feigl, A. K. Tagantsev and N. Setter
Contents
A. Electrode Characterisation
B. Stefan model for DW motion along a linear electrode
B.1 Governing equations from charge conservation and energy balance
B.1.1 Equations in Domains
B.1.2 Conditions on the fixed boundaries
B.1.3 Conditions on the moving boundary
B.1.4 Full set of equations
B.2 Similarity to the Stefan problem for heat
B.3 Solution for stepwise boundary conditions
B.4 Solution for square-pulse boundary conditions
C. Experimental data for DW motion and Stefan problem fits
D. Experimental error and uncertainties
E. References
A. Electrode Characterisation
In order to assess the quality of the Pt electrodes deposited by electron-beam induced deposition (EBID)
a series of switching experiments were carried out. A total of 10,000 hysteresis loops were measured
via piezoresponse force microscopy (PFM) and the positive and negative coercive biases extracted as
can be seen in Supplementary Fig. 1a. From this data it can be seen that the coercive biases (both
positive and negative) change monotonically from initial values of ~ +3.5 V, -3 V to ~ Β±4.5 V. This
means that over a range relevant for experiments i.e. <1000 switching cycles the coercive bias
(Supplementary Fig. 1b) and by extension the domain wall (DW) behaviour changes very little. This
validates the experiments where many switching cycles are used to assess DW motion e.g. Fig. 3 in the
main text.
Controlling domain wall motion in ferroelectric thin films
Controlling domain wall motion in ferroelectric thin films
L. J. McGilly, P. Yudin, L. Feigl, A. K. Tagantsev and N. Setter
Contents
A. Electrode Characterisation
B. Stefan model for DW motion along a linear electrode
B.1 Governing equations from charge conservation and energy balance
B.1.1 Equations in Domains
B.1.2 Conditions on the fixed boundaries
B.1.3 Conditions on the moving boundary
B.1.4 Full set of equations
B.2 Similarity to the Stefan problem for heat
B.3 Solution for stepwise boundary conditions
B.4 Solution for square-pulse boundary conditions
C. Experimental data for DW motion and Stefan problem fits
D. Experimental error and uncertainties
E. References
A. Electrode Characterisation
In order to assess the quality of the Pt electrodes deposited by electron-beam induced deposition (EBID)
a series of switching experiments were carried out. A total of 10,000 hysteresis loops were measured
via piezoresponse force microscopy (PFM) and the positive and negative coercive biases extracted as
can be seen in Supplementary Fig. 1a. From this data it can be seen that the coercive biases (both
positive and negative) change monotonically from initial values of ~ +3.5 V, -3 V to ~ Β±4.5 V. This
means that over a range relevant for experiments i.e. <1000 switching cycles the coercive bias
(Supplementary Fig. 1b) and by extension the domain wall (DW) behaviour changes very little. This
validates the experiments where many switching cycles are used to assess DW motion e.g. Fig. 3 in the
main text.
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The repetitive nature of measurement of DW positions requires many scans to produce the images.
Supplementary Fig. 1c shows the electrode thickness as a function of the number of scans and shows
that the thickness changes little over several hundred scans. It is clear that the EBID Pt top electrodes
are suitably durable and resilient structures to allow for investigation of DW motion.
Supplementary Figure 1 Characterisation of EBID Pt top electrode. (a) The evolution of positive
and negative coercive biases up to 104 switching cycles of which the first 1000 cycles can be seen
clearly in (b). (c) The electrode thickness as a function of the number of PFM scans. (d) The effect of
PFM tip loading force on the coercive bias
The displacement of the DW is limited by the ability of the system to deliver charge to the area of DW
propagation. It is clear that the role of the top electrodesβ conductivity is crucial. Another conductive
bottleneck here may be the contact between the conductive probe tip (Ti/Ir-coated Si) to the EBID Pt.
Supplementary Fig. 1d shows that this interface is neither a limit or critical to the system. As the probe
loading force is increased, the contact area changes correspondingly, achieving a large contact radius
and overall βbetterβ contact however the coercive bias is not altered by this change in the contact area
a b
d c
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leading to the assumption that the interface is not a limiting factor. Hereafter we assume perfect
electrical contact of the PFM tip with the electrode. This determines the Dirichlet boundary condition
for voltage in the charge transport problem. As we will demonstrate below this charge transport problem
is mathematically equivalent to propagation of heat in the classical Stefan problem [1].
In the classic case the Stefan problem is used to describe the motion of a pre-existing (i.e. meaning
nucleation is not considered) phase front that separates a liquid from a solid phase. In particular we will
draw an analogy from a heat problem of a rod initially resting at a constant temperature, πππππ‘ below the
melting temperature, ππ when one end is instantaneously subjected to a temperature ππΏ > ππ. The
thermal conductivity of the material (in the liquid phase) determines the amount of heat that reaches the
phase front, thus allowing it to propagate further due to the subsequent further melting. It is clear that
far from the melting front the temperature in the solid phase will be a minimum i.e. the initial value
before introduction of heat. As such there will be a large temperature distribution along the rod, from a
maximum at the heating end to a minimum at the opposite end (for the case of a finite rod).
The Stefan model is sufficient to describe the motion of DWs in ferroelectric thin films with EBID Pt
top electrodes. Supplementary Fig. 2 shows a comparison between the classic form of the model and
the DW motion analogue. Each quantity in the classic form of the model can be found to have an
analogue as outlined in Tables S1 & S2. As can be seen from Table S2 there are several quantities that
describe the temperature and their analogues for voltage within the Stefan model. This clearly
demonstrates that there is a voltage distribution where the maximum value must be ππ‘ and the minimum,
far away from the tip position is π0 = 0.
B. Stefan model for DW motion along a linear electrode
Here we develop a mathematical description for the DW motion in a thin ferroelectric film along a
linear electrode driven by a voltage pulse applied to one end of the electrode. This problem allows for
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a one-dimensional (1D) treatment, where the voltage distribution π’(π₯, π‘) and DW position π(π‘) are
found as functions of the applied voltage ππ‘(π‘), coordinate π₯ (distance along the electrode measured
from the point of contact with the PFM tip) and time π‘. Essentially, we address the propagation of charge
from the PFM tip into and along the electrode (see Supplementary Fig. 2a). As we will demonstrate, a
direct similarity can be drawn to the classical Stefan problem describing propagation of heat into a
material, where the position of a melting front is found as a function of the surface temperature ππΏ
(Supplementary Fig. 2b).
Supplementary Figure 2 Schematics of DW motion along a linear electrode. (a) A cross-sectional
view of the experimental setup showing partial switching of the capacitor structure. Polarisation is given
by red arrows, free charges are pluses and minuses whilst bound charges are circled. (b) The analogue
to the DW motion example in (a) for heat conduction in a rod which is described by the classical Stefan
problem. The meanings of the symbols in bold are given in Tables S1 & S2.
B.1 Governing equations from charge conservation and energy balance
In this section we develop equations for the voltage distribution from basic laws: charge conservation,
Ohmβs law and energy balance. First we will develop differential equation for the voltage inside
(a)
(b)
Domain wall Domain1Domain2
PFM tip
Pt
PbZr0.1Ti0.9O3
SrRuO3
SrTiO3
Phase front Phase1Phase2
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domains then we will discuss boundary conditions including conditions on the DW (phase front)
between domains (phases) 1 & 2.
B.1.1 Equations in Domains
Inside the domains the charge conservation law yields
βπ½β² = ποΏ½ΜοΏ½
(S1)
where π½ is the electric current in the electrode, π is the systemβs capacitance per unit length. Hereafter
(ββ²) and (βΜ) denote derivation with respect to coordinate (π₯) and time (π‘) respectively. The capacitance
per unit length may be estimated as
π =ππ0π€
β
(S2)
where π0 = 8.85 Γ 10β12 F/m is electric permittivity of vacuum, π is relative permittivity of the
ferroelectric material, β is the thickness of the ferroelectric layer and π€ is the width of the electrode.
Equation (S2) is applicable for wide electrodes, where π€ β« β. Using β = 7 Γ 10β8 m, π€ =
3 Γ 10β7 m, π = 80 one obtains π = 3 Γ 10β9 F/m.
Additionally Ohmβs law states
π’β² = βππ½
(S3)
π = π/π€π
(S4)
where π is electric resistance of the electrode per unit length, π is the thickness of the electrode, π is the
resistivity of the electrode. In our system the resistivity of the electrode is strongly dependent on the
thickness of the electrode. We expect for electrodes with thickness π around 10 nm to have resistivity
π in the range from 1 to 10 Ξ©m, thus (for π€ = 3 Γ 10β7m) leading to π ~1014 β 1016 Ξ©/m.
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Eliminating electric current between (S1) and (S3) one obtains
οΏ½ΜοΏ½ =π’β²β²
ππ
(S5)
B.1.2 Conditions on the fixed boundaries
We assume that the probe tip has a perfect electrical contact with the electrode, thus the voltage under
the tip (at π₯ = 0) is equal to the tip voltage ππ‘. The other edge of the electrode is assumed to be far from
the zone of interest and voltage on it equal to zero. This implies boundary conditions
π’(0, π‘) = ππ‘(π‘)
(S6)
π’(β, π‘) = 0
(S7)
B.1.3 Conditions on the moving boundary
From the requirement that electric current must be finite, one obtains that voltage is a continuous
function, implying
π’|πβ = π’|π+ β‘ π
(S8)
Here |πβ denotes the limit at the DW approaching from the left (domain 2) and right (domain 1)
respectively. At the same time the current undergoes a jump at the domain wall. This jump is defined
from the charge balance at the DW. Consider infinitesimal displacement of the DW, πΏπ which is
essentially switching of the area π€πΏπ under the electrode. The bound charge in this area will increase
by πΏππ = β2ππ π€πΏπ, where ππ is spontaneous polarization. Assuming perfect screening one obtains
πΏππ = βπΏππ = (π½2 β π½1)πΏπ‘. Here π½2 and π½1 are electric currents on the left and right hand sides (LHS
& RHS respectively) of the DW respectively.
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Thus from charge conservation one obtains:
π½2 β π½1 = 2ππ π€π Μ
(S9)
π½2 =π’β²
π|πβ
(S10)
π½1 =π’β²
π|π+
(S11)
The voltage π above the DW may be found from the energy balance for the DW having infinitesimal
displacement πΏπ. The work done by the current source will be π΄π = 2ππππ π€πΏπ. In the frame of our
model, one part of this work will be spent on elongation of the DW, the other part is dissipated by
different friction mechanisms mainly related to the Peierls potential, pinning by defects and switching
dynamics. The work done against DW surface tension may be written as 2πβπΏπ, while the work against
dissipative forces may be combined into a term ππβπ€πΏπ, where π is the domain wall energy per unit
area, and ππ is a pressure on the moving domain wall exerted from different friction mechanisms. In the
general case ππ is a function of the DW speed οΏ½ΜοΏ½. For sufficiently slow motion a βdry frictionβ model is
applicable where ππ = πππππ₯ β
οΏ½ΜοΏ½
|π|Μ on a moving DW, while ππ compensates other forces on the DW at
rest. The energy balance (after eliminating the displacement πΏπ) yields:
2ππππ€ = 2πβ + ππβπ€
(S12)
From equation (S12) one derives the equilibrium voltage above the DW
π = {
ππ β, π Μ < 0
π β (ππ β, ππ
+), π Μ = 0
ππ +, π Μ > 0
(S13)
ππ Β± =
πβ
π€ππΒ±πππππ₯β
2ππ
(S14)
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Here we introduce switching voltages ππ Β±, where β+β and β-β stand for growing and shrinking domain
2. Note that under the assumption of validity of the dry friction model the switching voltage does not
depend on the DW velocity. As a criterion of applicability of the dry friction model we suggest
π‘πππ = πππ2 β« π‘πππ
(S15)
where π‘πππ & π‘πππ are the characteristic times of the electrical circuit and the load (ferroelectric capacitor
structure) and where π‘πππ ~10β11 β 10β12 s is the polarization switching time limited by polarization
dynamics (estimated as inverse soft-mode frequency). Using π = 1014 Ξ©/m and π = 3 Γ 10β9 F/m one
checks that the dry friction model is safely applicable for our system for π >10 nm.
B.1.4 Full set of equations
In full we obtain the following equations for the pair of functions, π’(π₯, π‘) & π(π‘):
οΏ½ΜοΏ½(π₯, π‘) = (ππ)β1π’β²β²(π₯, π‘), 0 < π₯ β π
(S16)
π’(0, π‘) = ππ‘ (π‘)
(S17)
π’(β, π‘) = 0
(S18)
π’|πβ = π’|π+ = π’(π, π‘) = {
ππ β, π Μ < 0
π β (ππ β, ππ
+), π Μ = 0
ππ +, π Μ > 0
(S19)
π’β²
π|πβ β
π’β²
π|π+ = 2ππ π€π Μ
(S20)
From equations (S16)-(S20) we can describe the voltage evolution along the length of the electrode.
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B.2 Similarity to the Stefan problem for heat
The classical Stefan problem [1] describes the evolution of temperature and the position of the melting
front in a semi-infinite material. We will draw an analogy between our problem and the melting of a
rod by heating from the LHS (Supplementary Fig. 2b).
The governing equations for the problem [1] are:
οΏ½ΜοΏ½(π₯, π‘) =πΎ
ππ πΆπβ²β²(π₯, π‘), 0 < π₯ β π
(S21)
π(0, π‘) = ππΏ (π‘) > ππ
(S22)
π(β, π‘) = πππππ‘ < ππ
(S23)
π(π, π‘) = ππ
(S24)
πΎπβ²|πβ β πΎπβ²|π+ = ππ πΆπΏπ Μ
(S25)
The physical values that describe the heat problem are listed in Table S1, where we also introduce
values and complexes that we will need for conversion to our charge transport analogue; our problem
corresponds to the case where physical properties (specific heat, thermal conductivity and density) in
the liquid and solid phases are the same.
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Temperature, melting temperature , [K]
Density π [Kg/m3]
Cross-sectional area of the rod πΊ [m2]
Specific heat πͺ [J/Kg K]
Thermal conductivity π² [J/Kms]
Latent heat [J/kg]
Heat capacitance per length πͺβ = π πΊπͺ [J/mK]
Latent heat per length β = π πΊ [J/m]
Supplementary Table 1: Some physical values from the classical Stefan problem and their
relevant complexes
Analysis of equations (S16)-(S20) & (S21)-(S25) reveals direct similarity of the problem with the
classical Stefan problem [1] for heat. Thus the existing solutions can be used with respect to
substitutions reflected in Table S2.
Classical Stefan problem DW motion analogue
Temperature. πΏ, , [K] , , =
[V]
Voltage
Heat [J] [C] Charge
Heat Flux [J/s] [A] Current
Latent heat per length β [J/m] = ππ· π[C/m] Switching charge
Thermal conductivity π² [J/Kms] π πβ [C/Vms] Electrical conductivity
Heat capacitance per length πͺβ [J/mK] π [F/m] Capacitance per length
Stefan no.- solid phase πΊ =πͺ( β )
πΊπ =
π ππ· π
Stefan no.- domain1
Stefan no.- liquid phase πΊπ =πͺ( β )
πΊπ =
π( β )
ππ· π Stefan no.- domain2
Supplementary Table 2: Correspondence between physical values describing the classical Stefan
problem (left column) and the present problem (right column)
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However there is one essential difference between the models. This difference is reflected in equation
(S19) which is modified with respect to the corresponding equation (S24) for the classical Stefan
problem. This modification rises from the fact that in the classical Stefan problem the difference
between temperatures for freezing and melting is typically negligible1. In our case, since we are
applying voltages comparable with the coercive voltage, the difference needed for switching and back-
switching is crucial. However for the DW travelling in only one direction our problem is fully equivalent
to the classical heat-related Stefan problem.
B.3 Solution for stepwise boundary conditions
Consider the problem with the initial condition
π’(π₯, 0) = 0
(S26)
and boundary condition
π’(0, π‘) = ππ‘π(π‘)
(S27)
Here π(π‘) is Heaviside theta-function, which is 1 if π‘ β₯ 0 and 0 if π‘ < 0. The solution to this problem
may be adapted from Ref. [1] with substitutions in accordance with Table S1 to obtain for the DW
position
π(π‘) = 2πΎβπ‘
ππ
(S28)
and for the voltage distribution in domain 2 (0 < π₯ < π)
π’(π₯, π‘) = ππ‘ β (ππ‘ β ππ ) [
erf (π₯
2βπ‘/ππ)
erf (πΎ)]
(S29)
1 The difference in melting and freezing temperatures becomes essential for impure materials
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and in domain 1 (π₯ > π)
π’(π₯, π‘) = ππ [
erfc (π₯
2βπ‘/ππ)
erfc (πΎ)]
(S30)
where πΎ is the only positive root for the transcendental equation (obtained from requirement that
solutions (S29) and (S30) satisfy (S9)-(S11)
π2πππ (πΎ)
βπ1
ππππ(πΎ)= βπππΎ
2
(S31)
π2 =π(ππ‘ β ππ )
2ππ π€
(S32)
π1 =πππ 2ππ π€
(S33)
Here π1 and π2 are Stefan numbers for the first and second domains respectively, as introduced in Table
S2. It is instructive to rewrite these numbers in terms of thermodynamic coercive field
πΈπ β 0.2ππ ππ0
(S34)
Here we used the approximate relationship for 2nd order ferroelectrics from Ref. [2]. Eliminating π and
ππ in (S32) and (S33) using (S34) and (S2) one derives
π2 β 0.1(ππ‘ β ππ )/β
πΈπ= 0.1
(ππ‘ β ππ )
ππ
(S35)
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π1 β 0.1ππ /β
πΈπ= 0.1
ππ ππ
(S36)
Here we introduced coercive voltage ππ = πΈπβ for the given film thickness. In view of the numerical
factor 0.1 in expressions (S35) and (S36), in case if the applied voltage is of the order of coercive
voltage, Stefan numbers may be considered as small parameters. For typical values of our experiment
using π = 3 Γ 10β9 F/m, ππ‘ = 8 V, ππ = 3 V, ππ = 0.8 C/m2, π€ = 3 Γ 10β7 m one evaluates π2 β 0.03
and π1 β 0.02.
The voltage distribution along the electrode, given by equations (S28)-(S30) is used to show the
distribution for different times in Fig. 2h in the main text.
In the case of small Stefan numbers (when charge needed for charging the capacitor is negligible
compared with the switching charge needed for the displacement of the DW) πΎ becomes small and by
decomposing equation (S31) into a Taylor series and keeping only the most important terms one obtains
πΎ βS1 +β2πS2 + S1
2
2βπβ β
S22
(S37)
Combining equation (S28) with equation (S37) one obtains expressions for the domain wall
displacement
π =βπ‘ππ (
βπ(πVπ 2 + 4πPs(Vt β Vs)π€) β πVπ )
2βπPsπ€β β
(ππ‘ β ππ )π‘
πππ π€
(S38)
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This expression for the DW displacement as a function of time has been used to fit the experimental
data as seen in Fig. 2e and appears in the main text as equation 1. The DW velocity, π£ can be determined
from differentiation of equation (S38) so that
π£ =1
2β(ππ‘ β ππ )
πππ π€π‘
(S39)
and expressed in terms of DW position along the electrode by use of equation (S38) to give
π£ =(ππ‘ β ππ )
2πππ π€β1
π
(S40)
which is used as the fit to describe the experimental results of Fig. 2f in the main text.
B.4 Solution for square-pulse boundary conditions
The experimental measurement of the DW position corresponded to a square pulse of voltage. In our
simplest approximation where electric capacitance of the system is fully neglected, the domain wall is
expected to stop abruptly when the voltage is off. However in case of small but finite capacitance a
further motion βby inertiaβ (driven by charge stored in the capacitance of domain 2) will occur. The
displacement of the domain wall πΏπ caused by this effect may be evaluated using
πΏπ =πΏπ
2πππ€
(S41)
πΏπ = π(ππ‘ β ππ )ππ
2
(S42)
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Here πΏπ is the charge stored in the capacitance of the 2nd domain2, π < 1 β 1/3 is the fraction of the
charge that will flow to the DW but not to the tip, approximate relationship holds for the limiting case
{ ππ
ππ‘β 0, π2 β 0}. From (S41) and (S42) one obtains
πΏπ
π=π
2
(ππ‘ β ππ )π
2πππ€β1
6S2
(S43)
One concludes that the relative displacement of the wall after the voltage is off is of the order of Stefan
number. This validates use of (S38) to evaluate the displacement of the DW under the square voltage
pulse with duration π‘. For the parameters of our system the relative error will be of the order of 1% as
controlled by equation (S43).
2 Here we use only part of the charge from charging the capacitor above ππ (subtracting the charge πππ π) since
this part is βtrappedβ under the barrier of the DW and will flow into the tip.
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C. Experimental data for DW motion and Stefan problem fits
In Supplementary Fig. 3 the full data set for both positive and negative switching is shown. The DW
displacement and calculated DW velocity are shown for several different tip voltages.
Supplementary Figure 3 DW motion and fits from the Stefan problem. In (a) the DW displacement
as a function of time and negative applied voltage is shown and (b) is the associated DW velocity as a
function of displacement along the line electrode. (c) DW displacement as a function of time for positive
applied voltages and the associated DW velocities (d). The inset in (d) is a magnified view. The solid
lines in all charts are the Stefan model fits to the experiment data.
D. Experimental error and uncertainties
In this section we will discuss the uncertainty in the measurements and calculations presented in the
main text.
a b
c d
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The most basic measurement and one of the most vital is the position of the DW after a voltage pulse
i.e. π(π‘). The AR Cypher atomic force microscope used in this study is an extremely accurate and stable
machine. Therefore we assume that the major source of uncertainty in our measurement of DW position
is the resolution of the image captured i.e. the pixel size. For the experiments shown in Fig. 2-4 of the
main text we know that the pixel size is 21.5 nm therefore we assign an error of βπ = Β±22 nm. In fact
this error in the DW position is much smaller than the size of the data points presented in Fig. 2e, 3c-e
4e-g.
In a similar approach the error in the voltage pulse duration will be equal to half the smallest increment
of the signal generator so that βπ‘ = Β±0.25 ms; again smaller than the data point size. For Fig. 3d,e the
time increment was changed for precise DW placement and the associated error is βπ‘ = Β±0.02 ms.
Therefore the error in the velocity is βπ£ = |π
π‘| β(
βπ
π)2+ (
βπ‘
π‘)2. This equation has been used to
calculate the uncertainty in velocity and gives the error bars in Fig. 2f in the main text. The uncertainty
in the velocity will decrease as the fractional uncertainty (βπ‘
π‘) decreases as π‘ β π‘πππ₯.
For Fig. 4f,g the values βdβ and βDW regressionβ are simply π = π1 β π2 so βπ = β(βπ1)2 + (βπ2)
2
= 31 nm. This is smaller than the size of the data points.
For the average DW velocity data presented in Fig. 2g the error is propagated from the error in the DW
velocity such that βοΏ½Μ οΏ½ = 1
2(π£πππ₯Μ Μ Μ Μ Μ Μ Μ β π£πππΜ Μ Μ Μ Μ Μ ) where π£πππ₯ = π£ + βπ£ and π£πππ = π£ β βπ£. This has been
calculated for each voltage and gives the error bars visible in Fig. 2g for positive and negative voltages.
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The voltage required to move an existing DW, ππ is taken from the x-intercept of the line fits from the
Stefan model seen in Fig. 2g. The uncertainty, Ξππ , is obtained from fitting to the οΏ½Μ οΏ½ Β± βοΏ½Μ οΏ½ data sets.
Calculation of the values of the resistance per unit length, π and resistivity Ξ© both depend on the
propagation of the error in the value of ππ .
E. References
[1] Gupta, S. C. The classical Stefan problem: basic concepts, modelling and analysis. Elsevier,
Amsterdam (2003)
[2] Tagantsev, A. K., Cross, L. E. & Fousek, J. Domains in Ferroic Crystals and Thin Films. Springer
(2010)
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