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- Thermal management of thermoacoustic
Thermoacoustic sound projector: exceeding the sound projectors using a free-standing
carbon nanotube aerogel sheet as a heat
fundamental efficiency of carbon nanotubes source
Ali E Aliev, Nathanael K Mayo, Ray H
Baughman et al.
To cite this article: Ali E Aliev et al 2018 Nanotechnology 29 325704 - Increasing the efficiency of thermoacoustic
carbon nanotube sound projectors
Ali E Aliev, Yuri N Gartstein and Ray H
Baughman

- Thermoacoustic excitation of sonar


View the article online for updates and enhancements. projector plates by free-standing carbon
nanotube sheets
Ali E Aliev, Nathanael K Mayo, Ray H
Baughman et al.

This content was downloaded from IP address 86.27.85.58 on 18/10/2020 at 23:42


Nanotechnology

Nanotechnology 29 (2018) 325704 (17pp) https://doi.org/10.1088/1361-6528/aac509

Thermoacoustic sound projector: exceeding


the fundamental efficiency of carbon
nanotubes
Ali E Aliev1,7 , Daniel Codoluto1, Ray H Baughman1,
Raquel Ovalle-Robles2, Kanzan Inoue2, Stepan A Romanov3,
Albert G Nasibulin3,4, Prashant Kumar5, Shashank Priya5,
Nathanael K Mayo6 and John B Blottman6
1
Alan G. MacDiarmid NanoTech Institute, University of Texas at Dallas, Richardson, TX 75083, United
States of America
2
Nano-Science & Technology Center, LINTEC OF AMERICA, INC. Richardson, TX 75083, United
States of America
3
Skolkovo Institute of Science and Technology, Skolkovo, Moscow Region, 143025, Russia
4
Department of Applied Physics, Aalto University, Puumiehenkuja 2, FI-00076 AALTO, Finland
5
Center for Energy Harvesting Materials and Systems, Virginia Tech, Blacksburg, VA 24061, United
States of America
6
Sensor and Sonar Systems, Naval Undersea Warfare Center, B1170/R109, Newport, RI, United States of America

E-mail: Ali.Aliev@utdallas.edu

Received 2 March 2018, revised 1 May 2018


Accepted for publication 15 May 2018
Published 5 June 2018

Abstract
The combination of smooth, continuous sound spectra produced by a sound source having no
vibrating parts, a nanoscale thickness of a flexible active layer and the feasibility of creating large,
conformal projectors provoke interest in thermoacoustic phenomena. However, at low frequencies,
the sound pressure level (SPL) and the sound generation efficiency of an open carbon nanotube
sheet (CNTS) is low. In addition, the nanoscale thickness of fragile heating elements, their high
sensitivity to the environment and the high surface temperatures practical for thermoacoustic sound
generation necessitate protective encapsulation of a freestanding CNTS in inert gases.
Encapsulation provides the desired increase of sound pressure towards low frequencies. However,
the protective enclosure restricts heat dissipation from the resistively heated CNTS and the interior
of the encapsulated device. Here, the heat dissipation issue is addressed by short pulse excitations
of the CNTS. An overall increase of energy conversion efficiency by more than four orders (from
10−5 to 0.1) and the SPL of 120 dB re 20 μPa @ 1 m in air and 170 dB re 1 μPa @ 1 m in water
were demonstrated. The short pulse excitation provides a stable linear increase of output sound
pressure with substantially increased input power density (>2.5 W cm−2). We provide an extensive
experimental study of pulse excitations in different thermodynamic regimes for freestanding
CNTSs with varying thermal inertias (single-walled and multiwalled with varying diameters and
numbers of superimposed sheet layers) in vacuum and in air. The acoustical and geometrical
parameters providing further enhancement of energy conversion efficiency are discussed.
Supplementary material for this article is available online

Keywords: thermoacoustics, carbon nanotubes, pulse excitation, heat transfer, sound, sonar projectors
(Some figures may appear in colour only in the online journal)

7
Author to whom any correspondence should be addressed.

0957-4484/18/325704+17$33.00 1 © 2018 IOP Publishing Ltd Printed in the UK


Nanotechnology 29 (2018) 325704 A E Aliev et al

1. Introduction multiple: (i) a small duty cycle provides sufficient time for
cooling the active CNT heat source and surrounding gas
Thermoacoustic (TA) sound transduction shows promise to towards ambient temperature within each pulse period;
fill the low frequency niche for light-weight, thin and flexible (ii) the temperature increase in a short pulse and the energy
loudspeakers and underwater sonar systems. Recent studies transfer to the gas medium are nonequilibrium processes,
on TA sound generation using freestanding carbon nanotubes resulting in sharper spatial thermal gradient and an enhanced
(CNTs) [1–8], alternative nanostructures [9–13], and micro- energy conversion efficiency; (iii) the use of a high fre-
fabricated, suspended aluminum nanowires [14, 15] have quency pulsed carrier signal modulated with a low frequency
found that the sound pressure in open systems is proportional sound envelope enables sound generation at the frequency of
to the applied power and frequency. The ultra-small heat the applied current, without the need for additional energy
capacity per unit area of a thin sheet CNT heater, Ch*, and the consuming DC biasing (valid for both open and closed
efficient thermal coupling between CNTs and the surrounding systems); (iv) the electronics for powering the TA device
gas provide a wide frequency response (1 Hz–1 MHz) and with high-power short pulses are more efficient, lighter and
relatively high sound pressure level (SPL) at high frequencies. more compact (like electronic converters) than sinusoidal
However, in the low frequency region, where the demand for signal amplifiers.
large area, flexible sound projectors is high, sound generation Two pulse excitation regimes have been examined: a
efficiency is disappointingly low [3, 6, 16]: ηmax„10−5 for single pulse (SP) per vibrational displacement and a high
f„10 kHz. Other challenges are relate to the air-like density frequency alternating carrier-pulse sequence modulated by an
of CNTS, resulting in low mechanical strength and high acoustical (sinusoidal or arbitrary form) envelope. For both,
sensitivity to the environment at the high surface temperatures an extended linear power dependence of the generated sound
necessary for high-power TA sound generation. pressure and an increased energy conversion efficiency are
TA sound generation combines the principles of a heat observed.
engine, Carnot’s theorem, and fluid dynamics at the nanos- We provide an extensive experimental study of pulse
cale. Expansion and contraction of a gas in vicinity of resis- excitations for different thermodynamic regimes and explain
tively heated CNTS induces sound wave propagation in the our observations within basic theoretical models. The
surrounding medium. Increasing the thermal gradient created acoustical and geometrical parameters providing further
between the surface of the CNTS and the surrounding med- increases in efficiency and transduction performance for
ium results in increased sound pressure intensity. Therefore, resonant and non-resonant systems are discussed.
high electrical power is required to achieve high sound
intensity and high energy conversion efficiency. The extre-
mely low heat capacity of the aerogel density CNTS and the 2. What governs the efficiency of a TA projector:
small, but finite heat capacity of air, are accompanied by low open and closed systems
thermal conductivities to external heat sinks. At high applied
AC power, this leads to an accumulation of heat in the vici- TA sound generation is directly related to the ideal gas law:
nity of the heater, i.e., the CNTS. The elevated background PV=nRT, i.e., the volume, V, occupied by n moles of any
temperature decreases the efficiency of the TA projector. The gas has a pressure, P, at temperature, T, in Kelvin, where R is
heat dissipation issue is even more severe for encapsulated known as the gas constant. For open systems, the boundary
devices [17, 18]. The heat dissipation becomes the main conditions follow dV/V0=dT/T0|P, and the sound pressure
obstacle limiting the acoustic power density of the TA wavelength is much larger than temperature wavelength,
projector. λP?λT, while P remains constant. For closed systems,
For the purpose of benchmarking advances of nanos- dP/P0=dT/T0|V, and the volume remains constant, dV=0
tructured TA materials, like CNTs, wherein the heat capacity [19]. The general solution to spherical TA radiation from any
of the projector material is much less than the surrounding solid pulsating sphere into gas suggests that the heat capacity
gas, we define the fundamental efficiency of sound genera- per unit surface area of the heater, C*h=hρhCh, should be
tion. By fundamental efficiency, we mean the ratio of far field lower than the heat capacitance of the ambient gas involved in
acoustic power output to applied electrical power when the the TA interaction, C*g=lρgCg [6, 20]:
electrical input is a sine wave signal. This fundamental effi-
ciency will depend upon whether the system is open or - iro w 2a2 Ph
prms = ⋅
closed. Hence, we have exceeded the fundamental efficiency 2 k1To r - i4pa2 (wCh* + k1k)
for either an open system or a closed system when the ratio of f 1 1
output acoustic power at a given frequency to the input = ⋅ ⋅ ⋅ Ph. (1 )
2 2 Cg T0 2c + 2c + 1 r
2
electrical power exceeds that for the case where the electrical
input is a single sinusoidal signal.
The heat dissipation issue and the creation of an The root-mean-square (rms) value of sound pressure,
enhanced thermal gradient in encapsulated TA projectors is prms, produced by an applied AC power, Ph=I2oR, is
addressed here by signal processing of the applied AC increased with frequency, f, and the slope of this dependence
power, namely, by short pulse excitation of a nanostructured is a function of material parameters and ambient conditions.
heater. The advantages of short pulse modulation are Here, T0 is the temperature of the surrounding gas, ω=2πf is

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Nanotechnology 29 (2018) 325704 A E Aliev et al

the angular output frequency, |k1|=1/l=(ω/2α)1/2 is the Note, an increase of applied AC power (i.e., an increase
real part of the thermal wavenumber, α and κ are the thermal of modulated temperature), increases the efficiency, similar to
diffusivity and the thermal conductivity of the surrounding that of a heat engine. If the input power is totally transferred
gas, respectively, a is the radius of the TA pulsating spherical to the surrounding gas, Ph=2SβTa, the efficiency of an open
heater, and r is the distance to the microphone. The dimen- TA projector in the far field is depends on the intrinsic
sionless coefficient χ=(hρhCh)/(lρgCg) is the ratio of the properties of the ambient gas, υg, ρg, Cg, the mean temper-
heat capacity per unit area, C*h=hρhCh, to the heat capacity ature of the thin TA heater above ambient, Ta, and heat
of the gas layer involved in the TA interaction. Here, C is the exchange coefficient of the TA heater, β:
gravimetric specific heat capacity of the heater (Ch) or gas ug ug b Ta
(Cg), ρ is the corresponding density, h is the thickness of the h= ⋅ Ph = ⋅ . (5 )
2Srg Cg2 T02 rg Cg2 T02
heater and l is the thermal diffusion length in the gas, deter-
mining the thickness of air layer involved in heating process. Thus, the fundamental efficiency of an open system is
The derivation of equation (1) is given in S1 of the supporting much below the thermodynamic limit of the Carnot’s cycle,
information (SI) available online at stacks.iop.org/NANO/ due to the low coupling coefficient. There are a few ways to
29/325704/mmedia. The following conclusions are espe- improve the energy conversion efficiency of a TA projector:
cially important for identifying new TA heaters: first, the low (i) utilize a gas with a low Cg near the TA heater; (ii) increase
density, ρh, and small thickness, h, of the TA sheet are the heat exchange coefficient of the TA heater, β; (iii) increase
essential for having both a lower thermal inertia and a higher the temperature modulation amplitude of the TA heater, Ta.
heat exchange with the surrounding gas; second, for an Among the proper gases, the monoatomic, high mole-
enhanced energy conversion efficiency, the TA material cular weight inert gases show the best performance. For
should withstand a high applied power, i.e., high temperatures example, the thermoacoustically induced sound pressure in
are necessary for a high Carnot’s efficiency, η=1−To/Th; xenon is ∼7 times higher than in air [6]. Moreover, nanos-
third, the heat capacity per unit area of the heater source, C*h, tructured TA heaters, like freestanding CNTS or thin gra-
needs only be small relative to C*g; finally, the effect of the phene sponges, can withstand very high temperatures (>2000
thermal inertia of the heater is diminished at low frequencies K) and enormous applied power densities (>28 W cm−2) [8]
due to an increasing thermal diffusion length in air, in inert gas environments. Thus, an encapsulation in inert
l=(α/πf )1/2. gases provides protection against oxygen in air and severe
At a low applied power (linear regime) and when environmental conditions. At the same time, encapsulation
Ch=C*g, i.e., χ → 0, equation (1) reduces to the well-known
* substantially affects the output sound. For a heater encapsu-
dependence [1], lated in a small rigid enclosure (closed system), the pressure
variation is less sensitive to the gas parameters (except the
f 1 heat capacity ratio, γ=Cp/Cv) and has an opposite fre-
prms = ⋅ ⋅ Ph (2 ) quency dependence compared to the open system [6]
2 2 T0 Cg r
(g - 1 )
prms = Ph. (6 )
and the energy conversion efficiency for a flat TA source 2 pfV
radiating acoustic power Pac in both direction (2S), or for an
omnidirectional source, i.e., for k2a„1 [3], is Here, V is the enclosed volume of gas. The smaller the
heated gas volume, the higher the sound pressure that can be
2 achieved. Encapsulation using resonantly vibrating rigid plates
Pac 2SI 2Sprms p ⋅ f2
h= = = = Ph. (3 ) of density ρp and thickness of hp provides a Q times higher
Ph Ph rg ug Ph rg ug Cg2 T02 external sound pressure and magnifies efficiency by a factor of
Q2, where Q is the mechanical quality factor at a resonance [17]
In the far field, k2a…1 (when the acoustical wave-
rg (a ⋅ b) 1
number k2=2π/λa becomes comparable, or larger than the p (r ) = ⋅Q⋅ ⋅ prms , (7 )
source size a), the directionality of the source and the inter- rp 2ph p r
ference forms a radiation pattern:
(g - 1)2 rg Q 2
h= ⋅ Ph. (8 )
p ⋅ f2 1 2p 3r2p h p2 hg2 f 2 u f
h= 2 2 h
rg ug Cg T0
P ´
2p
∬ D2 sin q dq df ,
Despite the above-mentioned benefits from encapsulation
in an inert gas, the limited heat dissipation from the chamber
where D(θ, j) is the directivity function. For k2a>2 the interior, which increases the ambient temperature, T0, restricts
directivity integral gives I ∝ f −2, which is exactly compen- the applied power density and Carnot’s efficiency. The use of
sated by the TA coupling proportionality, f 2 in equation (3) heat sinks, thermoelectric or water cooling only partially solves
[3]. Therefore, the maximum efficiency in the far field is the problem. This paper describes the merit of pulse excitation
ug that drives the encapsulated TA heater for a short portion of
h= Ph. (4 ) the sound period, thereby allowing sufficient time for heat
2Srg Cg2 T02 dissipation between pulses. Magnification of η by over a factor

3
Nanotechnology 29 (2018) 325704 A E Aliev et al

of 104 is demonstrated by using different short pulse excitation


regimes for thin, flat TA heaters encapsulated in argon gas.
Three orders of this magnification, compared to the open sys-
tem, mostly comes from Q2 and the enhanced heat dissipation,
which allows a higher Ph and a higher temperature gradient,
Ta/T0. The further enhancement of energy conversion effi-
ciency (>10) comes from the reduced filling factor of the input
electrical signal and the shorter time for accelerating fluid
particles, which does not provide enough time for equilibrium
gas heating. The nonequilibrium process reduces the increase
of gas entropy and enhances the one-dimensional expansion of
enclosed gas [21].

3. Experimental methods

3.1. Temperature and blackbody radiation in vacuum and air

The precise measurement of temperature on the surface of


Figure 1. Schematic diagram of the experimental setup. The
nanostructured materials is challenging. The temperature on loudspeaker testing chamber is acoustically insulated from the
the surface of freestanding CNTS is controlled using an laboratory environment and ‘noisy’ high-power amplifiers using
infrared thermal imaging camera FLIR T650-sc (FLIR Sys- absorptive fabric and anechoic foam wedges.
tems, Inc.) with a preinstalled emissivity, ε. This temperature
from the thermal camera is compared with the temperature The temperature, T, and the intensity of the blackbody
obtained from the measurement of resistance change (R/R0 radiation, UIR, in air and in a high vacuum (P<0.1 mTorr)
versus T) in the supported CNTS [8, 12]. The emissivity of were measured in optical cryostat (VPF-475 from Janis
the CNTS was obtained from the optical transmission, τ, Research Company, LLC). One glass window of the cryostat
using Kirchhoff’s law for thermal radiation (ε=α=1−τ). was substituted with an infrared-transparent germanium
Here, the dimensionless coefficient of absorption (or the window (2 mm thick and 50 mm in diameter) coated with an
absorptivity), α, is the fraction of incident light (power) that is antireflection film (Edmunds Optics Inc.) which has a wave-
absorbed by the body when it is radiating and absorbing in length range of 3–12 μm. An absorption factor of 1.0424 was
thermodynamic equilibrium. used to correct the radiation intensity transmitted through the
The thermal infrared camera is designed for precision Ge window.
measurements of steady or slowly changing temperatures
with a frame rate of 30 Hz. The response frequency of the
3.2. Acoustic setup
microbolometer matrix in the T650-sc is 125 Hz (time
constant<8 ms). For periodic temperature waves with a The schematic diagram of the setup is shown in figure 1. A
frequency higher than 30 Hz, the thermal camera measures sine or pulsed signal of frequency f (0–80 MHz) generated by
the mean value of temperature, which for pure sinusoidal a Digital Function/Arbitrary Waveform Generator (Agilent
waves, corresponds to half of the peak value (the same as the 33250A), G, is amplified by a high-power amplifier, A, and
power, Ph=UpIp/2). For example, by applying 30 V (the applied to the TA projector, TA, which is grounded through a
peak value is 42.4 V) of sinusoidal rms voltage to a free- reference resistor (Rref=1 Ω) to control the applied current.
standing CNTS (S=1.25×2.3 cm2, R0=841 Ω) in air at IntuiLink software was used for bipolar short pulses and
f>60 Hz, one can obtain Ta=T0−Tb=100 °C above the complex waveforms created and edited on a personal comp-
ambient (background) temperature, Tb. But the peak value of uter, PC. Three high-power amplifiers were used in this work
Ta measured at a frequency of 1 mHz is 186 °C, which is 7% for different experimental conditions: (1) a wide frequency
lower than the expected 200 °C, because of increasing power range (DC to 250 kHz) high-voltage (±350 V) piezo-driver
consumption by blackbody radiation at peak temperatures. By amplifier PZD350-M/S (Trek Inc.) was used for high-impe-
applying square wave signals of 30 V (Upeak=Urms= 30 V), dance projectors (R0=100 Ω–100 kΩ, output current of
which creates constant, non-alternating temperature, the ±0.4 A); (2) a AE-Techron 8102 (AE-Techron Inc.) power
thermal camera shows a temperature of 100 °C, the same as supply amplifier with a frequency bandwidth from DC to
for 30 V DC. 5 kHz and a maximum power output of about 1100 W was
To control the shape of the thermal signal, the instant used for low-impedance projectors (R0<100 Ω); and (3) a
amplitude of the modulated part of the temperature and the AG1012 (T&C Power Conversion, Inc.) 10 kHz to 10 MHz
evolution of the background temperature, we used a high- RF generator and amplifier with an output RF power up to
speed infrared photo-detector (InAsSb amplified detector 1000 W was used for ultra-short pulse sequences (Δτ<
PDA10PT from ThorLabs Inc., which has a wavelength range 100 ns). The thermoacoustically generated sound pressure
from 1.0 to 5.8 μm, and a maximum sensitivity at 4.9 μm). was measured using precision microphones, Mic., with

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Nanotechnology 29 (2018) 325704 A E Aliev et al

different apertures, A, and sensitivities, S:A=12.5 mm for an Table 1. Physical parameters of the studied CNTS.
ACO Pacific Model 7046 (2 Hz–20 kHz, S=54.3 mV Pa−1);
SWNT-2 MWNT-10 MWNT-50
A=6.25 mm for an ACO Pacific Model 7016 (5 Hz–
120 kHz, S=5.43 mV Pa−1); and A=3.1 mm for a B&K
25 22
Diameter of individual 2.2 10 50
pressure-field microphone 4138-A-015 (6 Hz–140 kHz, CNTs, nm
S=0.543 mV Pa−1). The SPL in air was measured using an Length of individual 1.5–3 200 600
CNTs, μm
impulse SPL-meter (Quest Technologies, Model 2700) pro-
Number of shells 1 7–8 40–50
vided with a QC-10 acoustic calibrator.
Sheet thickness, μm 0.05825 2022 ∼30
The charge conditioning preamplifier, CA (B&K Type Areal density, μg cm−2 6.025 1.522 9
2670 or ‘Sound Connect’ Listen Inc.), amplifies the 2f signal Optical transparency, % 85 82 44
and sends it to another high-gain, low-noise amplifier marked Sheet resistance, Ω/square 260 1000 150
LNA, which increases the detected signal further and sends it Thermal coefficient of +1.0 −0.7 −0.4
to the SR830 lock-in amplifier, LA (Stanford Research resistivity, ×10−3 K−1
Instruments, Inc.). The rms amplitude and phase delay of the Thermal conductivity, 500 50 28
second harmonic signal are read from the lock-in amplifier W m−1 K−1
displays. Simultaneously, the signal goes to a four-channel Rate of temperature rise, 53 63 8
digital oscilloscope DPO4104B-L, Osc. (Tektronix, Inc.), for K ms−1 (figure 5)
visualization and recording the shape of the received signal.
The detection of the second harmonic signal using the phase-
sensitive lock-in amplifier substantially enhances the signal/ DC, AC, and pulsed electrical power were applied to the
noise ratio. In addition to the reference resistor, Rref=1 Ω, freestanding CNTS and the dependence of temperature on
the shape of the pulse current was controlled by 120 MHz area-normalized input power was recorded in vacuum and in
air. Figure 2 shows that in air (a) and in vacuum (a) and (b)
bandwidth AC/DC current probe TCP0030A (Tek-
the temperature on the surface of resistively heated free-
tronix, Inc).
standing CNTS is a nonlinear function of applied power. In
vacuum, the main heat dissipation channel at T>100 °C is
blackbody radiation. In air, this nonlinearity is caused mainly
by the temperature dependent thermal conductivity of air,
4. Results and discussion
convection, and by blackbody radiation at elevated tempera-
tures. For aerogel-type transparent sheets at low frequencies
4.1. Thermal inertia of a freestanding TA heater
( f<1 kHz), we can neglect the heat capacitance of the
To provide results that enable optimization of signal proces- heater, Ch=0. Thus, in equilibrium, for a large heater
sing conditions (signal shape, duty cycle, number of pulses k1a?1 [6], the main dissipative mechanism of the applied
per period), we first studied the dynamics of temperature power, Ph, in air is the thermal conduction to air, κτ:
development on the surface of freestanding CNTS having Ph Ph
different average CNT diameters, sheet densities and number Ta = » . (9 )
- i4pa2 (wCh* + k1k) pf
of superimposed layers: (i) a single layer of a highly aligned 2Sk
multiwalled CNTS (MWNT-10) drawn from a chemical a
vapor deposition (CVD) grown forest (the height of the In the linearized energy balance equations [6, 8] we
aligned forest is ∼200 μm, the average diameter of the omitted the temperature dependence of the thermal conductivity
nanotubes is ∼10 nm, the optical transparency of the sheet (thermal diffusivity) of the gas. However, for large temperature
between 0.5 and 20 μm is ∼82%, and the thermal radiation variations, the temperature dependence of the thermal con-
emissivity is 0.18) [22, 23]; (ii) a single layer of an aligned ductivity, κτ ∝ T½ [28], and the thermal diffusivity, α=
multiwalled CNTS (MWNT-50) drawn from a forest grown κτ/ρgCg ∝ T3/2, should be restored. The substitution for an
by the floating catalyst based CVD method (the forest height ideal gas (ρ ∝ T−1 and Cg=(7/2)R, where R is the ideal gas
is 600 μm, the average diameter of the nanotubes is ∼50 nm, constant) gives Ta ∝ Ph/(ρgCgκτ)1/2 ∝ PhT1/4. However, for
the optical transparency of the sheet is ∼44%, and the air, which contains mainly the molecular gases N2 and O2, the
emissivity is 0.56) [24]; (iii) six layers of MWNT-10 sheets thermal conductivity has a much sharper temperature depend-
stacked parallel to each other, (MWNT-6L) (wherein the ence above 200 K (κτ =0.026 24·(T/300)0.8646 W m−1 K−1)
optical transparency of the sheet assembly is ∼44%, and the and the heat capacity gradually increases (Cg=1002.6+
emissivity is 0.56) [8]; and (iv) a single layer of a randomly 275×10−6·(T – 200)2 J kg−1 K−1) [29]. As a result, the
deposited freestanding single-walled CNTS (SWNT-2) grown strong increase in the thermal conductivity enhanced by an
by the floating catalyst based CVD method (the average increase in the heat capacity is almost totally balanced by the
diameter of the nanotubes is ∼2.2 nm, the optical transpar- decrease of air density, ρ ∝ 1/T. Thus, the power dependence
ency of the studied sheet is 85%, and the emissivity is ∼0.15) of Ta should deviate little from the linear dependence, Ta ∝
[25–27]. Some useful parameters of these CNTS are shown in Ph·T−1/20. In fact, we observe a much stronger deviation, Ta ∝
table 1 and details are described in S2 of SI. PhT−1/4. This behavior is shown in the inset of figure 2(a) as

5
Nanotechnology 29 (2018) 325704 A E Aliev et al

Figure 2. (a) Temperature at the middle of MWNT-10 surface in air (open blue circles) and in vacuum (open green circles for AC excitation
with f=100 Hz and open red squares for the DC excitation) versus applied power (normalized to the surface area of the sheet, S=1.25×2
cm2). The solid blue circles show the dependence of temperature on the power consumed only by thermal conduction to air, Ph−Pε (Pε is
the radiated power). The inset shows the linear dependence of T5/4 on the power consumed by air transport. (b) The temperature on the
surface of four freestanding CNTS in vacuum: SWNT-2; MWNT-10; MWNT-6L; and MWNT-50, as a function of the area-normalized input
power.

T5/4
a versus (Ph−Pε)/S. The quantity Ph−Pε is the power The 1 W of applied power heats up the 1.25×2 cm2
consumed only by the thermal conduction to air, Pκ. To plot freestanding MWNT-10 sheet in air to ∼130 °C. The heat loss
Pκ(T), the power consumed by blackbody radiation for each by thermal conductivity along the sheet to the current elec-
temperature point measured in vacuum (open green circles) was trodes is the smallest term in equation (10), Pκl =
subtracted from the applied power, Ph, for the corresponding −2Aκl(∂Ta/∂x)≈0.0009 W, where κl =50 W m−1 K−1,
temperature measured in air (open blue circles). Apparently, the A=8×10−10 m2 is the cross-section area of the sheet with
small decline of the resulting curve from the linear dependence thickness h=20 μm (h=40 nm for the densified structure),
(<5% for solid blue circles in the main panel of figure 2(a)) is and x=L/2=6.25×10−3 m is the distance from the sheet
caused by a convective heat loss (air motion in a gravitational center to the electrodes. The heat loss through radiation from
field) from the vertically (or horizontally) oriented sheet. Note, both sides of the sheet can be estimated as Pσ =2Sεσ
that convection is a secondary process producing a redistribu- (Ta 4 - T0 4 )=0.096 W, where ε=0.18, S=2.5 cm2 and
tion of the accumulated part of the heat. The natural convection T0=295 K. Assuming that the contribution of the convective
can be substantially reduced by partitioning the space near the part is lower than 10% (the power that is needed to linearize
sheet using short fins (i.e., reducing the Rayleigh number [30]) the solid blue dotted curve in figure 2(a)) and the contribution
or by placing the heater in a closed chamber, which is the case of the thermal conduction along the nanotubes together with a
for encapsulated TA projectors. The natural convection for the radiation heat loss at Ta =130 °C do not exceed 9.7%, one
vertically aligned MWNT-10 sheet (1.25×2 cm2) creates a can conclude that more than 80% of an applied AC power in
temperature gradient between the bottom and top edges of equilibrium is consumed by heat conduction to the sur-
∼25 °C for Ph=1 W and Ta=130 °C. Enclosing the sheet in rounding gas. In the case of a negligible heat capacity of the
an aluminum foil chamber of 5×5×2 cm3 partially reduces heater, Ch=0, the heat exchange coefficient, β, can be
the temperature gradient to ∼15 K. At the same time, the par- directly estimated from the slope of T(Ph) at low tempera-
tition increases the absolute temperature in the center of the tures. For the MWNT-10 sheet (see figure 2(a)), β=(Ph−
sheet by ∼3%. Pκl−Pσ−Pconv)/2S(T−T0)≈18 W m−2 K−1.
In general, the total heat loss from a TA heater includes Despite the higher surface temperatures found for
three components: the heat loss through thermal conduction SWNT-2 sheet at high input power (figure 2(b)), the slope at
along the TA heater to the electrodes, Q0=−Aκl (∂T/∂x), low input power is essentially the same as for the MWNT-10
where κl is the thermal conductivity along the sheet having sheet suggesting very close thermal inertia. However, the heat
cross-section A; blackbody radiation 2SεσT4, where ε is the exchange coefficient, β=0.16 W m−2 K−1, for the SWNT-2
thermal radiation emissivity of the surface and σ=5.6× sheet (with 85% transparency) is little lower than for the
10−8 W m−2 K−4 is the Stefan–Boltzmann constant; and the MWNT-10 sheet, mostly due to the higher density of the
heat loss through thermal conduction (κτ) to the surrounding SWNT-2 sheet, ρ=6 μg cm−2 [25], and the extremely high
fluid, 2Sκτ [(Ta−T0)/l]=2SβT. Thus thermal conductivity along the sheet, κl ≈500 W m−1 K−1,
which provides a one order higher heat dissipation to the
dT dT electrodes, Pκl =0.012 W (ΔT=100 °C). Note, the thinner
Ph = I 2R = rVCh - Akl + 2SesT 4 + 2SbT . (10)
dt dx SWNT-2-90% and SWNT-2-95% sheets, having the same

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Nanotechnology 29 (2018) 325704 A E Aliev et al

volumetric density as SWNT-2-85% but much better access


to the fluid, show superior TA performance (will be published
elsewhere).
In vacuum, there are only two heat dissipation channels:
thermal conduction along the nanotube sheet to the electrodes
and blackbody radiation. At a low applied power
(Ph/S<0.1 W cm−2), the TA heater temperature, that is
mainly determined by the heat capacitance of the sheet, ρhCh,
increases linearly. We will use this fact for a direct mea-
surement of ρhCh for a freestanding sheet. At higher tem-
peratures, blackbody radiation becomes the main contributor
to the T(Ph) decline.
To avoid the development of a temperature background
in the above experiments, we intentionally used a low fre-
Figure 3. The shape of the blackbody radiation signal (open blue
quency excitations (an applied AC voltage of frequency circles) and the temperature rise (open red squares) versus pulse duty
100 Hz corresponds to a temperature modulation frequency of cycle for a MWNT-10 TA heater. The temperature was recovered
200 Hz). At the same time, to obtain a stable reading (to avoid from blackbody radiation intensities using the mechanically chopped
the flickering of the thermal camera image), the temperature radiation of a DC excited TA heater. The black dashed line shows
the shape of the applied voltage for a duty cycle of 10%, f=10 Hz,
modulation frequency was chosen much above the frame rate
and Ph=0.35 W. T∞=220 °C for a duty cycle of 100%.
of the thermal camera ( ffr=30 Hz) and the response fre-
quency of the microbolometer matrix of T650-sc, f∼125 Hz.
The measured temperature versus applied AC power, both in using the reduced equation (9), to be ρhCh=Ph/SωTa, is
air and in vacuum, is consistent with the temperature com- ∼0.01 J m−2 K−1. Hence, the specific heat capacity of the
puted from the resistance change technique that correlates a MWNT-10 sheet for the previously measured density per unit
decrease in resistance (for MWNT-10) to increasing area, ρ=0.015 g m−2, is Ch=670±30 J kg−1 K−1. The
temperature. heat capacitance of the air layer involved in the heating process
depends upon the pulse duration, Cg·H, where Cg=
4.2. Shape of the thermal pulse 1006.3 J kg−1 K−1=1191.5 J m−3 K−1 is the specific heat
capacity of air at T=295 K and H=h+2l is the thickness
To improve heat dissipation from the interior of the nanos- of the heater, h=∼20 μm, and l = 2a/w = 2at is the
tructured heater, the pulse duration should be short enough to thermal diffusion length. For a pulse width of 1 ms (1% duty
give sufficient time for heat relaxation to return to the back- cycle at pulse repetition rate of 10 Hz), l=0.21 mm and
ground level. Following the sampling theorem of digital Cg·H=0.52 J m−2 K−1. Hence, the heat capacitance of air is
signal processing, we introduce here a thermal sampling cri- ∼50 times greater than the heat capacitance of the TA heater.
teria for short pulse excitation of an encapsulated TA pro- In the case of a pulse width for a high frequency alternating
jector. The sampling interval, Δt, depends on the acoustical carrier-pulse sequence of 1% duty cycle at f=35 kHz, that
signal bandwidth, Δfa, the thermal inertia of the filled gas, corresponds to a 286 ns pulse, in which the pulse amplitude is
ρgCg, and the heat exchange coefficient, β: modulated by an acoustic frequency envelope, l=3.5 μm.
1 Hrg Cg Hrg Cg Now the heat capacitance of the air layer, H=27 μm, is much
Dt = + » . (11) lower,∼0.032 J m−2 K−1, and comparable with the heat
2Dfa 2b 2b
capacitance of the CNT heater.
The new term, HρgCg/2β, derived from the heat balance Figure 3 shows the infrared signal, UIR, radiated from the
equation (10) in the equilibrium state surface of the MWNT-10 TA heater and the temperature, T,
dT recovered from peak amplitudes of the radiated signal by
VrCh = 2 S bT , (12) comparing it with mechanically chopped radiation from a DC
dt
excited heater, over a range of pulse duty cycles in vacuum.
introduces the time that is necessary for the temperature to The linear increase of temperature (highlighted by green
return to the background level after each pulse excitation. dashed line) and the quadratic rise of blackbody radiation
Since Cg?Ch, here we replace Ch with Cg. The temperature signal (for a given spectrum of infrared detector) are typical
response for a short electrical pulse is limited by the heat for low applied power.
capacitance of the gas layer within the thermal diffusion For TA sheets in vacuum, figure 4(a) shows the rise of an
length and the heat exchange coefficient. infrared signal’s pulse front from the surface of SWNT-2,
The development of the thermal pulse measured for three MWNT-10, MWNT-6L, and MWNT-50 sheets (S=2.5 cm2)
types of freestanding CNTS in high vacuum and air shows that as a function of pulse width (duty cycle in %). Since the
the heat capacitance of the gas governs the rising and falling intensity of the infrared signal for a narrow bandwidth receiver
edges of the heat pulse. The heat capacitance of a single (1–5.8 μm) is proportional to the square of the applied power
freestanding MWNT-10 sheet (S=1.25×2.0 cm2), estimated (which was verified for all studied CNTS), the normalization to
in vacuum from the slope of the T(Ph) plot in figure 2(a), and Ph2 allows comparison between different TA heaters. The

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Nanotechnology 29 (2018) 325704 A E Aliev et al

Figure 4. (a) The shape of the radiated signal at an increasing pulse width for four CNTS placed in vacuum. The frequency of the pulse
sequence is 10 Hz. The applied pulse power of 0.61 W, 0.48 W, 0.85 W, and 0.8 W are chosen to reach the maximum temperature of 220 °C
at a 100% duty cycle. (b) The comparison of the pulse shape for MWNT-10 placed in vacuum and air.

Figure 5. The shape of the received blackbody radiated signal recorded for increasing duty cycles: (a) MWNT-10 sheet excited by 20 V
pulses; (b) SWNT-2 sheet excited by 13 V pulses; and (c) MWNT-50 sheet excited by 10 V pulses. The duty cycle in % for a pulse sequence
of 10 Hz corresponds to the pulse width in ms, i.e., a 1% duty cycle corresponds to a pulse width of 1 ms.

obtained pulse development curves show the highest rate of temperature rise versus time using equation (10):
temperature increase for MWNT-10 with a lower density of Ph/S=ρhCh(dT/dt). The temperature slope in figure 3 at
sheet than for SWNT-2 with smaller diameter of nanotubes, but input power of 0.35 W gives ρhCh=0.01 J m−2 K−1 for the
much higher density of the sheet. Along with small diameter, above MWNT-10 sheet. Control measurement of pulse slope
the spacing between adjacent nanotubes is a crucial property in air gives the precise specific heat capacity of air,
for TA heaters. 1010 J kg−1 K−1 (ρhCh=150 J m−2 K−1, where the thick-
Figure 4(b) shows the development of the infrared signal ness of the air layer involved in the heating process is
as a function of pulse width for MWNT-10 in vacuum l=(2αΔt)1/2=0.8 mm, and Ta=100 °C). Thus, monitor-
(UDC=16.24 V, Ph=0.376 W, T∞=220 °C) and air ing the blackbody radiation from the freestanding TA heater
(UDC=41.2 V, Ph=2.2 W, T∞=220 °C). For clarity, the in air and vacuum is a very sensitive and powerful tool for
signal intensity in air is magnified by a factor of 100. characterization of nanostructured materials and the thermal
Figures 5(a)–(c) show the shape of the front and rear edge of management of TA devices.
the infrared signal for MWNT-10, SWNT-2, and MWNT-50
in vacuum for an increased pulse duty cycle recorded directly
4.3. Pulse excitations of encapsulated TA projectors
from the digital oscilloscope. For details of light-to-voltage
conversion, see S8 in the SI. Two pulse excitation regimes have been examined and
For low temperatures on the surface of a TA source compared with a continuous sinusoidal excitation: (1) SP per
(Δt<2 ms in figures 3–5), when the blackbody radiation can vibration displacement with a constant amplitude; (2) high
be neglected and two other heat dissipation channels in the frequency alternating carrier-pulse sequence in which the
vacuum are canceled, one can again estimate the heat capa- pulse amplitude is modulated by an acoustic envelope. In both
citance of the freestanding sheet from the slope of the regimes, an extended linear dependence of the acoustic

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Nanotechnology 29 (2018) 325704 A E Aliev et al

Figure 6. Excitation of a TA transducer by short pulses (blue lines show the pulse sequences and black dashed lines show the displacement of
the vibrating plates): (a) constant amplitude and width bipolar pulses (SP) synchronized with the resonant vibration of the plate; (b) single
(bipolar or unipolar) constant amplitude and width pulses per several periods of mechanical vibration; (c) pulse width modulation (PWM)
using constant pulse amplitude; (d) high frequency alternating carrier-pulse sequence in which the pulse amplitude is modulated by an
acoustical envelope (PAM).

pressure with respect to the applied power and an increased


energy conversion efficiency were observed.

4.3.1. Single pulse (SP) per vibration displacement. SP


excitation with constant width and amplitude is the simplest
excitation suitable for encapsulated TA projectors to generate
monochromatic sound. Several regimes are available,
depending on the quality factor, Q, of the vibrating plates:
(i) single bipolar pulses per period for low Q (figure 6(a)); and
(ii) SP per several periods for high Q (figure 6(b)). Bipolar
excitation is preferable at high frequencies to avoid the
development of a mean voltage (current). Despite significant
distortions, this regime is extremely efficient in air and Figure 7. The amplitude-modulated carrier sinusoidal signal has a
underwater. 1.4 times lower filling factor than the directly applied sound
envelope.
4.3.2. Short pulse sequence modulated by an acoustical
signal. In a previous paper [6] we have demonstrated that applied power. The enhancement depends on the quality
the sound pressure generated by an encapsulated TA projector factor of the vibrating plates averaging the internal pressure
is enhanced nearly two-fold by using a high frequency oscillations. This mode of excitation enables generation of
sinusoidal carrier signal ( fc∼50 kHz), whose amplitude is any arbitrary acoustic signal defined by the modulated signal.
modulated by an acoustic signal envelope (AM) (figure 7). If the sinusoidal carrier filler is substituted with short,
The enhancement results from the reduced filling factor of the uni- or bipolar pulses, then the fill-factor can be substantially
envelope, which is (2)1/2 for voltage and a factor of 2 for reduced. For the optimized carrier signal frequency, the pulse

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Nanotechnology 29 (2018) 325704 A E Aliev et al

Figure 8. (a) The spectra of the input power-normalized sound pressure for four types of excitations of a glass plate TA projector which has a
mechanical resonance of the vibrating plates at ∼750 Hz: (1) the blue line is for the simple sinusoidal excitation at an applied frequency of
375 Hz; (2) the red line is for a 35 kHz sinusoidal carrier signal modulated by a 750 Hz sinusoidal sound envelope (AM); (3) the green line is
for single bipolar pulse excitation at 750 Hz, with a pulse duty cycle of 1% (SP); (4) the brown line is for a 35 kHz pulse sequence with a duty
cycle of 1% AM modulated by a 750 Hz sinusoidal signal (PAM). The distance between the vibrating plate and the microphone (model 7046
with type 2618 preamplifier) was 3 cm. (b) The vertically placed two-glass-plate TA projector comprises two 12.7×17.8 cm2 glass plates
with a thickness of 1.85 mm and four layers of freestanding MWNT-10 sheets (R=370 Ω) suspended 1 mm apart between the two-glass
plates.

duty cycle can be adjusted so that after each short pulse, the 1.8 mm thick glass plates sealed at the edges by highly elastic
system has ample time to cool down to near room temperature silicone strips (see for details S2 in SI) provided a high quality
(see equation (11)). Hence, the large temperature gradient and factor, Q≈36. PAM is found to be the most efficient
energy conversion efficiency is preserved. excitation for the given combination of Q and impedance
There are three types of pulse modulation to consider: mismatch for this device.
(i) amplitude modulation of a short pulse sequence (PAM, The sound pressure for a simple sinusoidal excitation,
see figure 6(d); (ii) pulse width modulation (PWM, see which should linearly increase with applied power for low
figure 6(c), and (iii) the pulse density modulation (PDM), power levels (equations (6) and (7)), starts to degrade at a
where the frequency of constant width short pulses is relatively low power (open blue circles in figure 9(a)). In
modulated by a sound wave. While PWM and PDM permit contrast, SP excitation maintains the expected linear depend-
very simple, efficient electronic circuitry, and commonly used ence up to the highest power (∼65 W) available for this TA
for excitations of flat, coil loudspeakers (like found in projector, which has a high input resistance (two electrode
postcards), here we focus attention on PAM for potentially a devices). The acoustic sensitivity (prms/Ph) increased by a factor
more efficient excitation providing much lower distortion. of 1.8 times for the SP excitations (figure 9(b)) compared to a
In what follows, we examine short pulse excitation by sinusoidal excitation. The sensitivity of the device increases for
spectra, acoustical sensitivity, and efficiency for MWNT-10 shorter pulses and saturates at duty cycles below 10% (see
based encapsulated TA projectors with vibrating plates of figure S2.3(a) in SI). SP excitation at sub-harmonic frequencies
various size, stiffness and mass. (see S3.1 in SI for 375, 250, 187. 5, 150 and 125 Hz) does not
change sensitivity. Due to the high mass of the vibrating plates,
4.3.3. 12.7×17.8 cm2 two-glass-plate TA projector. The the highest achieved sensitivity, prms/Ph=0.73 Pa W−1 (r=
enhanced output sound pressure and efficiency of 3 cm)=60.8 dB W−1 (r= 1 m), and efficiency, η=1.4% (for
encapsulated TA projectors results from an optimal balance Ph=65 W), are relatively low.
between elastic modulus and mass of the vibrating plates, The theoretical value for sound pressure can be estimated
providing a high quality factor, Q, and an acoustical impedance from equations (6) and (7): the internal pressure generated by
mismatch (∝ ρf υf/ρpυp), according to equations (7) and (8). the encapsulated TA heater at an applied power of 1 W at
Figure 8(a) demonstrates the increases of sound pressure at f=750 Hz is ∼2.65 Pa, whereas the external sound pressure
resonance ( fr∼750 Hz) for four different types of excitations. at the centers of two resonantly vibrating plates calculated at a
Sound pressure for the TA projector shown in figure 8(b) was distance of 3 cm is ∼3.3 Pa W−1 (see calculations on page 12
measured when the device was horizontally suspended on a in S3 of SI). The measured value for a horizontally suspended
marble table covered with a sound absorber (1 cm separation TA projector driven by the most efficient PAM excitation was
between the bottom plate and the absorber). Large area, ∼1.56 Pa W−1 (see figure 8(a)). Apparently, the damping of

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Nanotechnology 29 (2018) 325704 A E Aliev et al

Figure 9. (a) The dependence of sound pressure on input power that is provided by a two-glass-plate TA projector using SP excitation at
f=750 Hz for an increasing duty cycle: 1%; 2%; 4%; and 10%. The sound pressure generated by continuous sinusoidal excitation (open
blue circles) is shown for comparison. (b) The acoustic sensitivity versus applied power for the TA projector vertically suspended in an
anechoic room. The distance to microphone is 3 cm.

Figure 10. (a) The sound spectrum of a single plate TA projector comprising the 15×15 cm2 carbon-fiber composite plate shows broad
resonance peaks at 430 Hz and 910 Hz. The inset shows an extended view at the main resonance peak. (b) A picture of the TA projector with
the microphone (model 7046, ACO Pacific, Inc.) placed 3 cm above the projector. The inset shows a thermal image of the projector at
Ph=20 W.

plate vibrations by the silicone sealant and the entrained device and a heatsink (15×15 cm2, Aavid thermalloy LLC)
gas substantially reduces the external sound pressure, causing on the bottom (figure 10 (b)). The input resistance of the
this discrepancy. Note the contribution of the entrained gas device was 18.4 Ω (the sheet resistance of MWNT-10 is 2000
increases for thinner enclosures (see equation (S3.3) in [6]). Ω/,) and fr=910 Hz (see details in S4 of SI).
The sound pressure and efficiency (figure 11(a)) linearly
4.3.4. 15×15 cm2 carbon-fiber composite plate on a increase with increasing power up to the highest applied power
heatsink. The relatively lighter 15×15 cm2 carbon-fiber available for short, SPs (164 W) and for a modulated sequence
composite plate has a much lower quality factor (Q=18.2) of pulses (156 W). Despite the lower sound pressure achieved
and a much broader resonance peak (figure 10(a)). This TA for sinusoidal excitation, the prms(Ph) curve departs from a
projector comprised five superimposed layers of freestanding linear dependence at a relatively high applied power of ∼20 W.
MWNT-10 sheets attached to an array of interdigitated This is attributed to the enhanced heat dissipation through the
copper-foil electrodes. The MWNT sheets were encapsulated sink. Note, the higher carrier frequency for AM excitation (open
in argon gas between a carbon-fiber composite plate (15× green triangles for fc=5 kHz and solid green triangles for
15× 0.08 cm3, Dragon Plate Inc.) placed on the top of the fc=50 kHz in figure 11(b)) results in a higher sound pressure.

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Nanotechnology 29 (2018) 325704 A E Aliev et al

Figure 11. (a) The sound pressure and efficiency of the carbon-fiber-plate TA projector versus applied power for three different types of
excitations: continuous sine wave (blue circles, open for sound pressure and solid for efficiency, respectively); SP with duty cycles of 10%
(red circles); and PAM with fc=50 kHz and duty cycles of 10% (green squares). (b) The sensitivity of a TA projector versus applied power
for Sine, AM, SP and PAM excitations. For these measurements, fr=910 Hz and r=3 cm.

Figure 12. (a) The sound spectra of the single plate TA projector #3, comprising a 7.6×6.6 cm thin (250 μm) AlN ceramic plate on top
2

and an aluminum heatsink on the bottom. The fundamental resonance peak is at 1366 Hz. (b) Top view of the ceramic plate TA projector.

Perhaps at higher carrier frequencies, when the acoustical 4.3.5. 6.6×7.6 cm2 AlN ceramic plate on heatsink. The
wavelength of carrier excitation becomes comparable to the argon-filled aluminum nitride (AlN) ceramic plate TA projector
heater-plate distance, both regimes of open and closed systems comprises four superimposed layers of freestanding MWNT-10
described by equations (2) and (6) are combined. sheets attached to an array of interdigitated copper-foil
The efficiency of a carbon-fiber-plate TA projector in air electrodes. The MWNT sheets were encapsulated between an
reaches 0.24% at the highest available applied power of AlN ceramic plate on top (7.6×6.6×0.025 cm3) and an
164 W (solid green squares in figure 11(a)). This efficiency aluminum heatsink on the bottom. Six TA projectors with an
was calculated using a direct method for near field sound input resistance between 40 and 60 Ω were assembled with
pressure (see figure S4.2(b) in SI). The sensitivity of the different attachments of the ceramic plate to the supporting
device is twice as higher for a SP and PAM excitations sealing silicone strips (see details in S5 of SI). The low mass
(0.47 and 0.48 Pa W−1 in figure 11(b)) than for sinusoidal and thickness of the plate and the high bending modulus of the
excitations. However, the lower density of the vibrating plate used AlN ceramic results in a high resonance frequency,
(∼1.33 g cm−3) is totally canceled by two-times lower quality fr=1366 Hz, and a high quality factor for mechanical
factor of plates in this device, and results in a sensitivity close vibrations, Q=43 (figure 12(a)).
to the glass plate TA projector. Nevertheless, at a maximum The encapsulated AlN ceramic TA projector generates a
applied power of 164 W driven with the SP-10% excitation, a sound pressure that is 33 times higher than for an equivalent
SPL reached 120.5 dB re 20 μPa @ 1 m distance. open system (green dashed line in figure 13(b)) for a sinusoidal

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Nanotechnology 29 (2018) 325704 A E Aliev et al

Figure 13. The sound pressure (a), sensitivity (b) and efficiency (c) of the encapsulated AlN ceramic plate TA projector (Pyramid #3) versus
applied AC power for four types of excitations measured in air: a continuous sine wave (open blue circles); AM excitation with sinusoidal
carrier signal ( fc=35 kHz) modulated with a sinusoidal envelope of fr=1366 Hz (open red squares); SP excitation using three different
duty cycles: 0.1%; 1%; and 10% (green triangles); and PAM excitation with a duty cycle of the short pulse sequence of 10% at fc=50 kHz.
For these measurements fr=1366 Hz and r=3 cm. (d) The sound pressure in water versus applied AC power for sinusoidal and SP types of
excitations with fr=315 Hz, where the sound pressure was measured at a distance of r=3 cm (Pyramid #4).

drive, mostly due to a high quality factor of the vibrating plate, field at the front of the TA projector (20 Pa at r=1 m) is an
Q=43. Further enhancement of sound transduction sensitivity overestimated value due to the radiation pattern of the flat
(figure 13(b)) and energy conversion efficiency (figure 13(c)) projector [31].
were achieved by lowering the filling factor of the excitation The double-plate radiating TA projector composed the
signals, which provides another factor of ∼2.9 increase in same AlN ceramic plates placed in water shows broad-band
sensitivity and more than one order in efficiency. A deviation spectra (Q<26) with a resonance frequency reduced down to
of pulse shape from rectangular at a duty cycle <1% results in ∼328 Hz (see details in S6 of SI). Apparently, much higher
a decline of the sound pressure (top curve, open dark-green sound pressure (prms>10.6 kPa at r=3 cm), sound pressure
triangles) at a high applied power. The PAM excitation with a level (SPL=170 dB re 1 μPa @ 1 m) and sensitivity
pulse duty cycle of 10% at fc=50 kHz produced a sound (prms/Ph>250 Pa W−1) results in water from the improved
pressure of ∼140 Pa (r=3 cm) and a SPL of ∼120 dB re impedance matching and cooling conditions. At a sound
20 μPa @ 1 m. The energy conversion efficiency calculated by pressure of ∼10 kPa ( f=315 Hz) we observed bubble
the direct method using equation (3), with the sound pressure nucliation (cavitation) at the center of the vibrating plate,
measured at the surface of the vibrating plate (r=1 mm and which spreads across the whole plate at prms∼10.5 kPa (see
S=50 cm2) and an applied power of 42 W (open brown figure S5.4 (d) in SI). Above this sound pressure the cavitation
squares in figures 13(a)–(c)) reaches 8.7%. Note, an efficiency cloud penetrates deeper into the water medium (up to 10 cm)
of 15% obtained from the sound pressure measured in the far and limits the radiated acoustic power. Rough estimation of

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Nanotechnology 29 (2018) 325704 A E Aliev et al

Figure 14. (a) The sound spectra of a two-plate TA projector comprising a single layer of a freestanding MWNT-10 sheet encapsulated
between two thin (96 μm) mica plates (5×5 cm2). The insets show the expanded spectrum of the main resonance peak at 6110 Hz. (b) The
first three plate vibration modes. The insets show the modal patterns whose relative frequencies are shown on the bottom of the squares.

cavitation limited sound intensity in the near field for a rigid them a suitable for vibrating membranes of flexible and
clamped plate [32] confirms that the acoustic pressure transparent loudspeakers and underwater TA projectors.
amplitude exceeds atmospheric pressure (101 kPa). The resonance frequency of a square plate with rigid
A larger size TA projector (11.43×11.43 cm2), with clamped edges for the first fundamental (0, 0) mode is
0.5 mm thick AlN ceramic plate on a heatsink driven with SP- fr=B·υl·h/L2=457 Hz, where h=96 μm is the plate
10% excitation provides superior sound power at lower thickness, Lx=Ly=5 cm are the plate dimensions, υl =
frequencies (890 Hz in air and 240 Hz in water), with sound 7200 m s−1 is the longitudinal sound velocity, and B=1.654
pressures above 12 kPa in water limited by intense cavitation is the coefficient of the Bessel function, determined by the
(see details in S7 of SI). In this device we modified the boundary conditions [33]. The longitudinal sound velocity
attachment of MWNT sheet to the interdigitated copper was chosen from a list of 36 different Muscovites [34] to fit a
electrodes by densification. At high applied AC current or measured 457 Hz resonance frequency for the first funda-
voltage the abundance of free dangling CNTs and nanotube mental mode. The layered structure of the mica plates
bundles in a freestanding aerogel sheet creates uncontrollable provides a low bending modulus. The sound pressure of the
nanoscale shortages at terminals. Tiny sparks eventually first three resonances, corresponding to the (0, 0), (1, 0), and
(1, 1) modes, is low (see figure 14(b)).
develop into larger openings, which propagate along the
The main resonance peak of the device at 6110 Hz has
electrodes. To avoid the dangling CNTs we densified the
relatively high sound pressure per input power and a quality
freestanding sheets by using methanol vapor. The densifica-
factor Q=18 (see details in S8 of SI). The short pulse
tion at electrodes (see figure S7.1(c)) substantially enhanced
excitation of these light and thin mica membranes
the robustness of the TA heater’s structure and significantly
(h=96 μm, S=5×5 cm2) significantly increases the
increased the power limit. sensitivity of the encapsulated device (open squares in
The sound pressure, sensitivity and efficiency enhance- figure 15). The increase of energy conversion efficiency to
ments in water by using rigid vibrating plates and short pulse 0.45% at an applied power of 35.7 W is due to the mechanical
excitations is the same as in air. This might be attributed to response of the light membrane to the pressure variation
the high density and thicknes of studied vibrating plates (see created by short thermal pulses. With a total weight of 2.5 g,
equation (7)). Below, we evaluate the short pulse excitations the 5×5 cm2 TA projector radiates in air the SPL of 100 dB
in encapsulated TA projectors composed light-weight mica re 20 μPa at 1 m and 170 dB re 1 μPa at 1 m underwater.
membranes. For all above examples of flat encapsulated TA
projectors excited with single short pulses (SP excitation) or
sequence of short pulses modulated with a sound envelope
4.3.6. Light-weight mica membranes. Highly transparent (PAM excitation), we observed enhancement of sound
(T=90%) plates of mica (H20-5691BS from Fire pressure and energy conversion efficiency compared to
Mountain Gems and Beads Inc.) with a thickness of sinusoidal excitation. For the case of a thin, light AlN
80–160 μm, show excellent mechanical and thermal ceramic plate (see Pyramid #3 in figure 13), this enhance-
properties. The low density (ρ=1.6–3 g cm−3), excellent ment reaches 2.7 and 7.2 fold, respectively. For sinusoidal
flexural strength (>180 MPa) and high thermal resistance excitation, the slow motion of the flat piston provides enough
(>750 °C) of muscovite and phlogopite mica sheets make time to thermalize the energy of excited gas particles across

14
Nanotechnology 29 (2018) 325704 A E Aliev et al

Figure 15. The power dependence of sound pressure (a) and sensitivity (b) for an argon-filled two-plate TA projector comprising a single
freestanding MWNT-10 sheet (R=1680 Ω) encapsulated between two 96 μm thick mica membranes (S=5×5 cm2) for two types of
excitations: a continuous sine wave (open blue circles) and pulsed sine wave (tone burst) with a pulse frequency of 10 Hz and duty cycle of
7% (PS-7%); and SP excitation using two different duty cycles: 2% and 10% (open green and red squares, respectively). The sound pressure
and sensitivity measured in air at a resonance frequency of 6110 Hz and at a distance of 3 cm. The inset to (a) shows the shape of the sound
pressure signal for the sine tone burst excitation PS-7%.

the enclosure. In this case, the gas particles can be treated as a similar to MWNT-10 optical transparency, ∼85%, SWNT-2
three-dimensional thermodynamic system, reaching equili- has much denser sheet structure (two orders thinner) and one
brium during the sound period. Equation (6) with γ=5/3 order higher thermal conductivity along the sheet. However,
(for monoatomic gas as argon) well describes this case. For the thinner SWNT-2%-90% and SWNT-2%-95% sheets,
short pulse excitations, the motion of accelerated particles can having the same volumetric density as SWNT-2%-85% but
be treated as effectively a one-dimensional gas in none- much better access to the fluid, show enhanced TA perfor-
quilibrium state, since insufficient time is provided for mance. Moreover, the metallic temperature dependence of
thermalization across the thin, flat enclosure. Accelerated resistivity, the one order lower sheet resistance, and the
particles do not lose energy by thermalizing the system in the unique mechanical properties of the studied SWNT films
horizontal direction and behave as an adiabatically expanding make them very attractive for high frequency TA transduction
gas with γ=3 [21]. The rate of entropy increase is also (>100 kHz) and underwater applications (higher hydro-
reduced. The sound pressure and efficiency for this none- phobicity). On the other hand, the ability of large diameter
quilibrium one-dimensional thermodynamic system, as nanotubes, like MWNT-50 (D≈50 nm), to avoid bundling
roughly estimated by equation (6), are increased by factor 3 and the extended length of individual nanotubes (∼0.6 mm)
and 9, respectively, which are very close to the observed make them very attractive for low frequency TA projectors
results. ( f<1 kHz) working in harsh conditions of high static
potentials and strong vibrations.
It was demonstrated that blackbody radiation from the
5. Conclusions resistively heated CNTS can be used as a very sensitive tool
for examining the modulated and accumulated parts of the
Small diameter CNTs in a low density, porous, freestanding heat on freestanding nanostructured TA heaters and for
sheet are preferable for TA sound generation. Therefore, extracting the thermal inertia and heat capacity of the heater
aerogel structures enabling enhanced fluid accessibility to the material. The precise control of heat dissipation channels
inner parts of the freestanding sheet provide the highest TA (internal heating of the sheet, thermal conduction to the
performance. To minimize internal thermal interaction, the electrodes along the heater and to the fluid, and blackbody
distance between separate nanostructures in an aerogel TA radiation) allows direct estimation of the TA (heat-to-sound)
heater should exceed the thermal diffusion length of the coupling coefficient.
surrounding fluid. The comparison of three aerogel CNTS Encapsulation of a nanostructured TA projector heater
containing differing diameter nanotubes shows that the working in harsh conditions in air and underwater is neces-
aerogel structure of MWNT-10 sheets (D=10 nm with 7–8 sary to achieve desirable robustness and efficiency. Employ-
shells) which has an average distance between individual ing rigid, vibrating plates softly clamped on the edges, an
nanotubes and bundles in the freestanding sheet greater than approximately 50-fold improvement of device sensitivity
20 μm, provides superior TA performance to SWNT-2 (prms/Ph) and a more than four order enhancement in energy
(D=2.2 nm) and MWNT-50 (D=50 nm) sheets. Despite conversion efficiency, compared to the open system, were

15
Nanotechnology 29 (2018) 325704 A E Aliev et al

demonstrated. These enhancements were achieved by using


short pulse excitation that mostly improves the heat dissipa-
tion conditions from the interior of the encapsulated device
and allows higher input power densities.
There are a number of geometric and thermodynamic
parameters of the projector heater, chamber and the vibrating
plate to consider in the design of high-performance TA pro-
jector. However, the crucial step to overcoming the steady-
state fundamental efficiency limit of open TA system is in
encapsulation and using short pulses having a low duty cycle
(<1%). The rapid acceleration of fluid particles within the
front of short thermal pulses creates nonequilibrium one-
dimensional expansion of the filled gas. The accelerated Figure A1. The time dependence of the normalized temperature
particles do not have enough time to create an equilibrium modulation of a CNT sheet when driven by an AC current,
state. Hence, the entropy of the system is lower than for the I0·sin(ωt), is shown for different values of ωτ, where τ is the
equilibrated system. These particles create stronger impact on characteristic heat dissipation time constant. The fluctuation
a vibrating plate placed within the thermal diffusion length. amplitude reaches a maximum of 2 at the limit ωτ→0, and shrinks
to a narrow line on the background of [T(x, t)−T0]/Δ0=1
The energy conversion efficiency of this non-ergodic engine as ωτ?1.
is still below the thermodynamic limit of Carnot’s cycle, but it
is much higher than the fundamental efficiency of either open
or closed systems. Notes
Short temperature pulses at an applied power of 10 kW
per pulse can permit over 10% energy conversion efficiency The authors declare no competing financial interest.
in air and over 60% efficiency underwater. Since the SPL for
an encapsulated device is independent of the properties of
enclosed inert gas, other than the heat capacity ratio Appendix
γ=Cp/Cv, the use of helium should improve heat dissipa-
tion [35] for extreme conditions of high-power >10 kW per The applied current Io·sin(ωt+jo) generates heat at an
pulse. angular frequency of 2ω. The power applied to the sheet,
Using a pulse excitation (PAM, PWM, PDM), one can Ph=I2·R·sin2(ωt)=I2·R·(1−cos(2ωt))/2, results in
generate an acoustic output having the same shape as the a temperature increase, ρh·Ch(dT/dt), if there are no other
input signal, and use linear signal processing techniques to heat dissipation channels, where ρh is the density and Ch is the
avoid the distortions specific to second harmonic signals and heat capacity of a resistively heated TA heater. The full heat
the need for biased excitation current. balance equation in vacuum is:
The obtained SPL at relatively low volume and mass of
encapsulated TA projectors by using short pulse excitations ¶ ¶2
I 2R sin2 wt = r h Vh Ch T (x , t ) - k 2 T (x , t )
show promising opportunities for noise cancelation, fire ¶t ¶x
extinction and low frequency sonars. + 2AesT 4 (x , t ) , (A1)
where κ is the thermal conductivity along the sheet, ε is the
emissivity, and σ is the Stefan–Boltzmann constant.
Acknowledgments For small temperature fluctuations, the temperature
change on the surface of CNT sheet is [36]:
We thank JNC Corp. for providing spinnable MWNT-50,
Juan Pablo Oviedo Robles (Material Science Engineering, UT ⎡ ⎤
sin (2wt + j) ⎥
Dallas) for the TEM images of MWNT-50. SAR and AGN T (x , t ) - T0 = D 0 ⎢1 - , (A2)
⎢⎣ 1 + (2wt )2 ⎥⎦
acknowledge the Russian Science Foundation for the support
by project # 17-19-01787. This research work was supported where Δ0 is the maximum temperature change. At low tem-
by the Office of Naval Research grants N00014-14-1-0152, peratures in vacuum, Δ0 depends only upon the thermal
N00014-17-1-2521, Army Research Office STTR Contract conduction along the TA heater, Δ0=2I20R/(πκS/L), and τ
#W911NF-15-P-0023, and the Robert A Welch Foundation is the characteristic heat dissipation time constant, determined
Grant AT-0029. exclusively by the thermal diffusivity, α, along the length of
the nanotubes and nanotube bundles, namely, τα =L2/π2α.
However, for temperatures above 400 K and the sample
Author contributions length above 2 mm, the contribution of blackbody radiation
should also be considered.
The manuscript was written with contributions from all The temperature, normalized to Δ0, alternates between 0
authors. All authors have given approval to the final version and 2 as ωτ→0, i.e., when the heat accumulation during a
of the manuscript. temperature oscillation period is negligible. However, this

16
Nanotechnology 29 (2018) 325704 A E Aliev et al

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