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Nanoscale Heat Transfer at Contact Between A Hot Tip and A Substrate

1) The document analyzes nanoscale heat transfer between a hot tip and substrate using experimental data and modeling. It considers conduction through solid-solid contact, ambient gas, and water meniscus. 2) Experiments use a scanning thermal probe microscope with a heated tip to measure the thermal contact conductance and radii of the three heat transfer modes. 3) Modeling shows the three modes contribute similarly to thermal contact conductance but have distinct contact radii ranging from 30nm to 1micron. Any scanning thermal microscope has 1-3micron resolution in ambient air.

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0% found this document useful (0 votes)
80 views

Nanoscale Heat Transfer at Contact Between A Hot Tip and A Substrate

1) The document analyzes nanoscale heat transfer between a hot tip and substrate using experimental data and modeling. It considers conduction through solid-solid contact, ambient gas, and water meniscus. 2) Experiments use a scanning thermal probe microscope with a heated tip to measure the thermal contact conductance and radii of the three heat transfer modes. 3) Modeling shows the three modes contribute similarly to thermal contact conductance but have distinct contact radii ranging from 30nm to 1micron. Any scanning thermal microscope has 1-3micron resolution in ambient air.

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RashaM.Atwi
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© © All Rights Reserved
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Nanoscale Heat Transfer at Contact Between a Hot Tip

and a Substrate
Stphane Lefvre
Laboratoire dEtude Thermiques, UMR CNRS 6608
Ecole Nationale Suprieure de Mcanique et dArotechnique, 86960
Futuroscope Cedex
Sebastian Volz and Pierre-Olivier Chapuis
Laboratoire dEnergtique Molculaire et Macroscopique, Combustion, UPR
CNRS 288
Ecole Centrale Paris, 92295 Chtenay-Malabry
Corresponding Author :
Sebastian Volz, Ph.D.
EM2C-ECP, 92295 Chtenay Malabry, France
T : 33-1-4113-1049 F : 33-1-4702-8035, volz@em2c.ecp.fr
Abstract
Hot tips are used either for characterizing nanostructures by using
Scanning Thermal Microscopes or for local heating to assist data writing.
The tip-sample thermal interaction involves conduction at solid-solid
contact as well as conduction through the ambient gas and through the
water meniscus. We analyze those three heat transfer modes with
experimental data and modeling. We conclude that the three modes
contribute in a similar manner to the thermal contact conductance but
they have distinct contact radii ranging from 30nm to 1micron. We also
show that any scanning thermal microscope has a 1 to 3 microns
resolution when used in ambient air.

Nomenclature:
A:

accommodation coefficient

a:

thermal diffusivity (m2.s-1)

b:

contact radius (m)

Cv,p:

heat capacities (J.kg-1.K-1)

E:

Young's modulus: (Pa)

e:

film thickness

F:

force between the tip and the surface (N)

G:

thermal conductance (W.K-1)

H:

hardness (Pa)

h:

heat transfer coefficient (W.m-2.K-1)

I:

electrical current (A)

L:

half length of the rhodium-platinum wire (m)

p:

probe perimeter (m)

Pr:

Prandtl number

R:

electrical resistance () Radius (m)

S:

rhodium-platinum wire surface (m2)

T:

temperature (K)

V:

voltage (V)

v:

mean velocity of molecules in air (m.s-1)

x:

coordinate along the Pt-Rh wire axis (m)

x0

coordinate on the Pt-Rh wire surface (m)

y0:

coordinate on the Pt-Rh wire surface (m)

z:

tip altitude (m)

(m)

z0:

coordinate on the Pt-Rh wire surface (m)

Greek symbols:
:

temperature coefficient (K-1)

temperature amplitude (K)

heat capacities ratio

thermal conductivity (W.m-1.K-1)

electrical resistivity (.m)

Subscripts:
A:

air

C:

total contact conductance - probe curvature radius

Eq:

contact and sample conductances in series

P:

probe

S:

solid-solid contact

W:

water meniscus

x:

ellipse small axis

y:

ellipse large axis

Keywords:
Scanning Thermal Microscope, Nanoscale Heat Transfer.

Thermoelectric energy conversion was improved by a factor of 2 in the


year 2001 by using nanostructured materials [1], the future of data
storage is believed to rely on nanoscale heating [2], and nanomaterials are
to be used for building insulation. Those examples emphasize the key role
of heat transfer in nanotechnologies, especially regarding to the energy
field. A review on the scientific challenges in microscale heat transfer can
be found in several references [3,4].
A complex heat transfer issue is clearly encountered when predicting the
heat flux between a hot tip and a sample. In the ambient air, heat
conductions through solid-solid contact, through the gas and through the
water meniscus are combined as illustrated by Figure 1. The tip sample
contact conductance Gc is defined as the sum of the three thermal
conductances:
GC GS G A GW .

(1)

The thermal transport is governed on the quantitative and geometrical


point of views by those three contributions. Those contributions can not be
ignored when using the scanning probe microscopes. The spatial extension
of the thermal interaction between the tip probe and a nanostructure is
crucial. The flux value is also a keypoint when a tip heating is used to
lower the local coercitive magnetic field or to melt a substrate in the case
of data storage.
Previous works have reported a detailed analysis of the thermal
mechanisms at point contact between a thermocouple tip and a hot
substrate [5]. The air contribution is found to be dominant because the tip
cantilever is heated through air. We propose to use a hot tip so that the

measurements are not dependent on the temperature distribution on the


sample surface.
Gomes et al [6] suggested that the water meniscus might be the dominant
heat transfer mode but that this contribution should depend on the sample
thermal conductivity.
In our previous papers [7-9], we identified the contact radius as being 1
micron when the tip temperature is larger than 100C and about 200nm
when it is lower. We presume that the change in the contact radius
produces a change in the modes contributions.
We use a Scanning Thermal Probe Microscope to provide quantitative data
for the thermal contact conductance and the contact radii of the three
main modes. A presentation of the microscope is provided in the first
paragraph. We address the solid-solid thermal interaction in the second
part. The water meniscus contribution is studied based on a simple
modeling in the third part. In the last section, the air contribution is
analyzed with experimental and modeling tools.

1. The SThM based on a Hot Tip


The basis of most SThMs is the Atomic Force Microscope. Its principle is to
maintain a constant force between a tip and a sample. A piezoelectric
crystal controls the force by monitoring the height of the tip cantilever.
The piezocrystal voltage is then directly related to the sample topography
when the probe scans the surface. The original function of those systems
was to provide the samples topography with the atomic resolution. Those
devices were rapidly developed to also measure a large variety of local

properties magnetic, electric, elastic, -. And in 1986, K. Wickramasinghe


[10] proposed to mount a thermocouple tip in a conventional AFM. While
the temperature was the feedback signal to control the tip height, it is
until now used to measure the local temperature [11] when the tip is
brought in contact with the surface. Those techniques however require an
external heating [12] and the knowledge of the sample geometry to
provide local thermal properties.
Our probe consists in an electrical resistance that is thermally controlled
through Joule dissipation. The probe temperature is directly deduced from
the probe electrical resistance. Those active tips also measure the local
thermal conductivity without any external heat source: the input current is
controlled so that the tip temperature is maintained to a constant value,
the feedback current then reflects the capacity of the sample to conduct
heat. In the present paper, we used the 3-omega technique to measure
the tip temperature [13,9]. An AC current at frequency is heating the tip
at the frequency 2. The tip electrical resistance is linearly dependent to
the temperature amplitude 2, R=R0(1+2where is the temperature
coefficient. The tip voltage V=R(2).I() therefore includes a thermal
component at 3:
V3

I0
R ,
2 0 2

(2)

where I0 is the current amplitude. This technique allows us to remove the


dependence of the measurement to the ambient temperature and ensures
a high signal to noise ratio.
As illustrated in Figure 2, the tip is made of a wollaston wire of diameter

75microns and shaped as a tip. The silver coating is removed at the tipsample contact to uncover the platinum/rhodium wire of diameter 5
microns. Due to the Joule heating, the temperature profile in the tip is
parabolic. The temperatures at both ends are set to the ambient because
the silver is assimilated to a heat sink. The detailed solving of the thermal
problem is proposed in references [7,9]. The expression of the probesample conductance Geq including the contact GC and the sample GS
contributions writes:
1
1
1

,
Geq GC 2S b

(3)

where S and b are the sample thermal conductivity and the thermal
contact radius. Geq is related to the measured temperature through:
L

1
x dx
L 0 2
J0

A.Geq B.GP mL

(4)

Lm3 exp 2mL 1 Geq 1 exp 2mL GP mL

where J 0

I 02
, being the probe electrical resistivity, P and SP the probe thermal
2 P S P2

conductivity and section. Gp represents the probe conductance. The A and B coefficients are
defined as:

A 2 mL 4exp mL 2exp 2mL mLexp 2mL

B 1 mL exp 2mL mLexp 2mL ,


2
where L is the half length of the platinum wire. m

(5)
(6)
hpP 2i

represents
P S P aP

the probe fin parameter where h is the heat transfer coefficient between

the tip and the ambient. pp and ap are the probe perimeter and thermal
diffusivity.

2. The solid-solid and water meniscus contact conductances


The contact between two bodies is achieved through constrictions and
spacing including gas and water. A thermal resistance appears due to the
lower thermal conductivity of air and water but also due to the change of
the flux lines that preferably pass through the constrictions. As illustrated
in figure 1, the solid-solid contact between the tip and the sample is
described by the same morphology. Consequently, we use the same model
to describe the dependence of the conductance to the applied force [14]:
GS C.F n C '.I n ,

(7)

where C and C are coefficients, F represents the force applied by the tip
on the sample and I is the current that controls the piezoelectric crystal
extension. This current is proportional to the force. The literature [14]
proposes a value of n between 0.63 and 0.99. Increasing the force
smashes the constrictions and increases their conductance as well as the
overall solid-solid contact conductance. We shall assume that the tip
shape is not modified on the microscale so that the force dependence of
the total conductance writes:
Geq

2S b C ' I n G A GW

2S b C ' I G A GW
n

(8)

Thermal mapping were performed on the surface of an Hafnium sample


under different forces. The total conductance was identified based on Eqs.
(4-6) and averaged on the surface. Figure 3 reports the comparison

between experimental results and the prediction of Eq. (7). The fit provides
GS=6.8.10-5 W.K-1, GA+GW=9.8 10-6 W.K-1, n=1 and C=2.1 10-7 W.K-1.A-1. A
change in the sample modifies the solid-solid contact conductance through
its contact radius. Those are modelled through the Hertz law in the elastic
domain:
6RF
bs
E

1/ 3

(9)

RP being the Pt-Rh wire radius, and in the plastic domain:


4F
bs
H

1/ 2

(10)

where RC=5-15m is the tip curvature radius, E the Youngs Modulus and H
the hardness. An estimation of bs-s with typical values for E and H is 20nm.
The power laws 1/3 and 1/2 emphasize a low sensitivity of the radius b s-s to
the materials. We therefore believe that a variation of G s in the range of 05 10-6 W.K-1 is a reasonable general estimation. A 8nA current is usually
applied when using the SThM tip so that G s1.7 10-6 W.K-1. This is 17% of
the total conductance as learnt from the value of G A+GW. The reference
value of S=23 W.m-1.K-1 also leads to a mean contact radius b = 740 nm
>>20nm. We deduce that the air and the meniscus conductances might
have contact radii much larger than the solid-solid one.
In ambient air, the hygrometric rate ranges from 35% to 65% and water
molecules are adsorbed on samples surfaces. In AFM measurements, this
water film is observed when measuring the cantilever deflection when the
voltage of the piezoelectric crystal varies. When approaching the surface,
the tip is brought down by capillarity forces. The film thickness can be

estimated to 0.25-1nm from this signal. 0.25nm is the water molecule


radius. The water meniscus was indicated as the main heat transfer
channel in several studies [6]. We propose an estimation of the meniscus
conductance including the tip geometry. The tip is assimilated to a halftore and the sample as a plane surface. The tore equation has to include
the curvature radius of the Pt-Rh wire RC and the wire radius RP:

z0 RC RP RC2 RP2 y02 x02 2RC RP2 x02 .

(11)

Equation (11) relates the altitude z0 of the tip to the coordinates x 0 and y0
of a point M on the sample surface. z 0

also represents the meniscus

thickness under the tip when z0<ew, ew being the film thickness. The heat
transfer is assumed to be vertical so that a heat transfer coefficient can be
defined as:

h x0 , y0

z0 x0 , y0

(12)

The thermal conductivity of water w is set to 0.61 W.m-1.K-1. The water


conductance then writes:

GW h x, y dx.dy

(13)

where is the surface defined by (x 0,y0) points for which 0.25nm<z0<ew.


The water conductance ranges from 10-6 W.K-1 for a one molecule thick film
to 3.10-5 W.K-1 when ew=1nm 4 molecules thick film - as reported in figure
4. This contribution remains of the same order of magnitude than the
solid-solid contact conductance. The contact radii as a function of e w are
derived from analytical calculations and presented in Table 1. They are one
order of magnitude larger than the solid-solid contact conductance.

3.Conduction through air


We will show that the thermal signal varies far before the tip is brought in
contact with the sample. The radiation conductance can be overestimated
to 10nanoW.K-1 which is clearly negligible. We therefore presume that
conduction through air is the key channel. The diffusive, slip and ballistic
regimes of heat transfer were already modelled [15] to describe the
rarefied gas effect on energy exchange between the tip and the sample. A
1D vertical conduction is also assumed. A local heat transfer coefficient is
modelled as:

h x0 , y0

A
,
z0

(14)

in the diffusive regime when z 0 is much larger than air mean free path
(MFP) =100nm. In the slip regime when z<100, molecules temperature
is strongly different from the one of the sample surface when colliding it.
The heat transfer coefficient writes:

h x0 , y0

z0 2 (2 A) / A 1 Pr

(15)

where A=0.9 is the rate of the molecule energy left to the surface,
=Cp/Cv=1.4 and Pr=0.7 is the Prandtl number in air. This complex

expression fits the diffusive regime when z0 >> (2 A) / A 1 Pr


and also to the ballistic regime when air molecules do not collide between
themselves. In this case, MFP is set to z0 and:

h x0 , y0

Cv v.z0 / 3

z0 1 2(2 A) / A 1 Pr

(16)

where the kinetic expression of the thermal conductivity A=Cv.v.z0/3 was


introduced with the mean molecule velocity v. In the ballistic case, h A is
not z0 dependent anymore. The air conductance is then derived from
expression (16).
We apply this modelling to the specific shape of the wollaston probe. The
results are compared to experimental signals obtained when the tip
altitude ranges from 150 microns to contact.
The landing of the tip on the surface starts at altitude 150 microns. The
maximum dilatation of the piezoelectric crystal is of a few microns. We
therefore use the vertical displacement generated by the motorized screw.
This screw performs the tip approach before contact in a conventional AFM
imaging. To measure the vertical displacement, another z probe was put in
contact with the screw head. G eq was derived from Eq. (4) and from the 3
tip voltage.
A silver sample was used to keep the air resistance larger than the sample
one so that Geq=GA. Figure 5 reports the thermal resistance 1/G eq versus
the altitude z.
Beyond 20 m, we presume that a convective regime is observed in Figure
5(a), i.e. lifting Archimedes forces become larger than viscous forces. Heat
conduction mostly occurs in the viscous layer at the probe vicinity. The
thickness of the viscous layer is approximated from A and the heat

transfer coefficient h between the Pt-Rh wire and the ambient [9]

A
h

=25m. This thickness precisely corresponds to the limit of air conduction


regime where Req is linearly dependent to z.
A deviation to this linear dependence appears in Figure 5(b) below z =
1m. This trend is relevant to the slip regime and the small plateau when
z<300 nm might correspond to the ballistic regime. Just before contact,
the air conductance GA=2.5 W.K-1 and GA=2W.K-1 when the deviation
appears. Consequently, the slip and ballistic regimes might contribute to
20% of the conductance through air when the tip is in contact.
The intersection between a plane of altitude =100nm and the tore
representing the tip is an oval. Its mean radius b can be defined with the
two axis lengths bx=2.5m and by=9m according to:

bx2 by2
2

(17)

We obtain a very large value for b= 1.3m. According to the previous


modelling, this radius defines the surface on which the tip heating through
air is governed by the efficient ballistic regime. The true value of b A has to
be larger than 1.3m.
Between z=1m and 25m the diffusive regime is observed. The 3 regimes
model (3RM) assumes a diffusive behaviour above z=10 m only.
Understanding that the diffusive behaviour might be relevant on a wide z
range, we perform a 3D finite elements modelling (FEM) of the tip-sample
interaction based on the Fourier heat conduction equation. We neglect the

enhancement of heat flux in the ballistic area because the FEM predictions
show that the heat transfer in the ballistic area is much less than the total
heat transfer. The tip is assimilated to an ellipsoid with small and large
axis bx and by. Joule heating generates a parabolic temperature distribution
in the probe. Therefore, the area of the probe that is in contact with the
sample is the hottest part and the one that contributes most to heat
transfer. The sample and the air are simulated by two adjacent cubes of
100m in edge.

The temperature on the ellipsoid boundaries is set to

400K, the ellipsoid is positioned in air at various altitudes from the sample.
The temperatures of the outer boundaries of the two cubes are set to
300K. Geq is the ratio between the heat flux crossing the whole sample/air
interface and 100K.

We checked that changing the ellipse temperature

would not change the value of Geq. Our simulations includes about 60 000
elements. The mesh is refined around the ellipsoid volume.
Figures 6(a) and 6(b) reports the comparison between experimental
measurements (diamonds), the simplified 3RM (continuous grey line) and
the finite element modelling (black triangles). Discrepancies between 3RM
and measurements mostly occur between 2 and 15 microns. This confirms
that the slip regime is introduced at too high altitudes in the 3RM. The slip
regime underestimates the conductance as shown in Figure 7. But there is
a good agreement when z<1m. The assumption of vertical conductance
used in the 3RM is valid in the range of small z values indeed. The FEM
and the experimental data have the same evolution but the FEM
overestimates the measurements values by a factor of 2 when z<0.2m
and by 0.5 W.K-1 for higher altitudes. We emphasize that the diffusive

conductance is higher than the ballistic one when z<as indicated by Figure 7.
The Fourier heat exchange coefficient follows a 1/z law and is diverging
when z goes to zero whereas the ballistic conductance is constant. Of
course, using the Fourier law when z< is not physically relevant. This
however explains why the FEM predictions are drastically overestimating
measurements when z<0.2m.
The thermal conductivity of the sample is dependent on the roughness
and surface oxydation, it therefore might be lower than the reference
value of 428 W.m-1.K-1 for Ag. The FEM calculation for S=0.1 W.m-1.K-1 was
performed and reported in Figure 6a (empty triangles). The FEM values
then match measurements better when z>20m.
The FEM data do not follow the linear behaviour when z<3m as seen in
Figure 6(b). The vertical heat transfer coefficient approximation 1/hz is
yet more reliable near contact. We presume that heat flux from the surface
of the ellipsoid becomes non-homogeneous when z is small. This
behaviour is z-dependent. The Taylor expansion of h1/z-(z(d)-z)/z2 where
d is the surface element on proves that h is much z(d) dependent
when z is of the order of z(d)-z, i.e. about RP=2.5m. The deviation
observed in the experimental data might also be due to this effect so that
the slip regime is likely to start for even lower altitude than 1 m.
The predominance of the heat diffusion in air on the contact conductance
implies that the contact radius and the microscope resolution depends on
the sample thermal conductivity. The flux lines spread when the sample
thermal conductivity decreases. We computed the spatial distribution of

the heat flux crossing the sample surface by using our FEM. The tip height
is 20nm so that no solid-solid heat conduction is involved. Figure 8 reports
a slight difference in the flux distributions when s ranges from 100 to 5
W.m-1.K-1. But the maximum flux values then decreases by a factor of 5
when s reaches 0.1 W.m-1.K-1. The contact radius can be identified as the
radius for which the heat flux density reaches 50% or 90% of its maximum
value. The insert of Figure 8 shows that the radius increases by a factor of
2 (90%) or 25% (50%) when the sample thermal conductivity decreases to
the air thermal conductivity. In those conditions, the range of radius values
is 1.5-3.3m (90%) and 4 -5.4m (50%). A value of 1m for b was obtained
in previous works [7] from experimental data when the tip temperature is
higher than 100C. In those conditions, the meniscus disappears and air
conduction

becomes

predominant.

We

therefore

believe

that

our

estimation of b remains reasonable.


4. Conclusion
We have presented experimental and modelling results to understand and
quantify the heat transfer mechanisms between a micrometer tip and a
sample surface. The conventional law was retrieved for the heat transfer
due to the solid-solid contact. Values of 1.7 W.K-1 and 20nm were
obtained for the thermal conductance and the radius. Conduction in the
meniscus was estimated from the probe geometry. A 1 to 30 W.K-1 was
obtained for water film thicknesses as small as 4 water molecules. The
order of magnitude of the radius is 100nm. Air conduction between the tip
and the sample was studied in details. A thermal conductance of 2.5 W.K-1

and we proved that the corresponding radius ranges from 1.5 to 3 m


depending on the sample thermal conductivity. As shown in Table 2 and in
Figure 9, the three heat transfer modes have similar contributions with a
predominance of the water meniscus depending on the hygrometric rate.
The radii have very different order of magnitudes. Working with a hot tip
removes the meniscus and the tip contact radius then becomes of the
order of the micron: a nanoscale contact requires working in vacuum.

REFERENCES
[1]R.Venkatasubramanian,E.Siivola,T.ColpittsandB.OQuinn,Thinfilmthermoelectric
deviceswithhighroomtemperaturefiguresofmerit,Nature,413,(2001),597.
[2] P. Vettiger et al., The Millipedenanotechnology entering data storage, IEEE
TransactiononNanotechnology,1,(2002),39.
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ASMEJ.HeatTransfer,116,(1994),799.
[4]D.G.Cahilletal.,Nanoscalethermaltransport,JournalofAppliedPhysics,93,(2003),
793818.
[5] L. Shi and A. Majumdar, Thermal transport mechanisms at nanoscale point contact,
Journal of Heat Transfer, 124, (2002), 329.
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locale: calibration dune pointe thermorsistive, analyse des divers couplages thermiques,
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thermalcontrol,49,(1976),381396.
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CAPTIONS
Table 1: Contact radius bW corresponding to heat conduction in the water meniscus for
differentwaterfilmthickness.
Table2:Thermalconductancesandradiiforthefourheattransfermodesinvolvedinthetip
sampleheattransfer.
Figure 1: Schematic of the probesample interaction including conduction through air,
throughthewatermeniscusandthroughthesolidsolidcontact.
Figure2:ScanningElectronicMicroscopeimageofthethermalprobe.TheWollastonwireis
asilvercoating75micronsindiameterandaPtRhcore5micronsindiameter.Themirror
ensuresthelaserreflectiontocontrolthetipdeflection.
Figure3:Thermalconductancesofthecontactandthesampleversustheforceappliedbythe
tiponthesample.
Figure 4: Thermal contact conductance through the water meniscus versus the meniscus
thickness.
Figures 5(a) and 5(b): Thermal resistance of the contact and the sample versus the tip
altitude. Figure 5(a) reveals a convective regime when z>20m and a linear regime
correspondingtoconductioninairwhenz<20m.
Figures6(a)and6(b):Comparisonbetweenthemeasuredconductanceandthepredicted
ones.Themodelingisbasedona3Dfiniteelementmethodscheme(FEM)andasimplified3
regimesdescription(model).Thefigure6(b)reportstheresistanceversusaltitude.Thelinear
regime corresponds to conduction in air. The three approaches predict the same thermal
conductancethroughairasshownbytheextrapolationforz=0.
Figure7:Heattransfercoefficientsinthe3regimesmodel.

Figure8:Fluxversusradius(smallellipseaxisdirection)whenthetipisincontactandfor
differentvaluesofsamplethermalconductivities.Theinsertrevealsthatthecontactradius
duetoairconductionmayvarywiththesamplethermalconductivitybyafactorof2.
.

Table1:

Film Thickness W (nm)

bW (nm)

0.25

100

0.5

140

200

Table2:

Heat Transfer Mode

Conductance (W.K-1)

Contact Radius b (nm)

Radiation

10-3

Solid-solid

0 1.8

20

Conduction through air

2.5

1000 3000

5 - 30

100 - 200

Water Meniscus

Fig1:

Fig2:

Fig3:

Fig4:

Fig5:

Fig6:

Fig7:

Fig8:

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