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Received 8 December 2020; revised 5 February 2021; accepted 12 February 2021; posted 16 February 2021 (Doc. ID 416923);
published 11 March 2021
We demonstrate an interferometric method to provide frames available, diffraction-limited spatial resolution, and
direct, single-shot measurements of cavitation bubble significant expense and complexity. These limitations place
dynamics with nanoscale spatial and temporal resolution these high-speed photographic and holographic methods out
with results that closely match theoretical predictions. of the reach of most researchers in terms of cost and/or needed
Implementation of this method reduces the need for expen- expertise.
sive and complex ultra-high speed camera systems for the On the other hand, time-resolved photography, achieved
measurement of single cavitation events. This method through combining individual time-gated images from inde-
can capture dynamics over large time intervals with sub- pendent cavitation events, has been used by a larger number
nanosecond temporal resolution and spatial precision of investigators [7,13,25–29]. This approach has enabled the
surpassing the optical diffraction limit. We expect this reconstruction of complex bubble dynamics over long time
method to have broad utility for examination of cavitation intervals with high temporal resolution. However, this approach
bubble dynamics, as well as for metrology applications provides an “average” view of the phenomena, since the data
such as optorheological materials characterization. This acquisition utilizes images from different events. This effectively
method provides an accurate approach for precise mea- blinds the investigator to important factors that may cause
surement of cavitation bubble dynamics suitable for shot-to-shot variability such as the stochastic nature of laser-
metrology applications such as optorheological materi- induced plasma formation and the potential effects of medium
als characterization. © 2021 Optical Society of America under heterogeneity and/or impurities [30,31].
the terms of the OSA Open Access Publishing Agreement
As an alternative, investigators have developed optical
https://doi.org/10.1364/OL.416923 techniques utilizing probe deflection or spatial transmittance
modulation to determine cavitation bubble dynamics [32–
Precise measurement of cavitation dynamics is relevant to 35]. However, these techniques appear to be best suited to
phenomena as diverse as sonoluminescence, sonochemistry, probe millimeter scale sized bubbles and generally lack the
molecular transport, fluidic mixing, and light–tissue inter- precision necessary to allow for detailed analysis. Moreover, to
actions [1–5]. These phenomena have been exploited in obtain quantitative bubble dynamics, these techniques require
numerous applications, including ultrasonic cleaning [6], calibration and/or pairing with photography.
microfluidic mixing [7] and pumping [8], tissue ablation In this Letter, we present a new method for precise mea-
[5], drug delivery [9,10], ocular surgery [11], microrheol- surement of cavitation bubble dynamics with nanoscale
ogy [12,13], screening of cellular mechanosignaling [14,15], temporal resolution and spatial precision. This method uti-
and measurement of mechanical properties of soft materials lizes a heterodyne interferometer in a modified Mach–Zehnder
[13,16,17]. configuration [36,37] as shown in Fig. 1. This configuration was
Empirical studies providing detailed measurement of selected due to its known sensitivity to small phase differences
cavitation bubble dynamics most often utilize high-speed between the reference and sample arm produced by localized
photographic methods [18,19]. Such measurements are critical changes in the refractive index such as those produced by a
to understanding complex fluidic processes, assessing compu- transient cavitation bubble [38].
tational fluid dynamics models, and optimizing applications To demonstrate its capabilities, we formed cavitation bubbles
that utilize cavitation bubbles [20]. While the capabilities of using laser-induced plasma generation by irradiation using a
high-speed photographic and holographic methods have had single 500 ps duration pulse emitted by a frequency-doubled
advanced formidably in recent years, with systems capable Nd:YAG laser (λ = 532 nm, Teem Photonics PNG-M03012)
of imaging rates as large as 1 trillion frames/second [21–24], laser with pulse energies of 2.5–20 µJ. The laser beam output
significant limitations remain, including the total number of was expanded and delivered to a water-filled cuvette using a 40x,
Fig. 2. Measured photodiode signal (blue) and the AOM reference driving signal (orange) from oscilloscope following initiation of a cavitation
bubble using a 20 µJ pulse energy. Iint (blue) and Iaom (orange) are shown in segments corresponding to the (a) beginning, (b) middle, and (c) end of
a 175 µm diameter bubble created by a 20 µJ laser pulse. The AOM reference signal represents the heterodyne interferometer signal in the absence of
a bubble and whose frequency is identical to the photodiode signal prior to the formation of the bubble. Once bubble formation occurs, the detected
intensity of the photodiode signal is altered due to light scattering, and the phase is altered due to the varying optical path lengths. The red arrow on
the horizontal axis indicates the time of laser pulse delivery to the sample.
Letter Vol. 46, No. 6 / 15 March 2021 / Optics Letters 1411
Phase [krad/2
Phase [rad/2
120
3
100
50 2 80
60
1
40
0 0
0 5 10 15 20 25 30 35 40 20
Time [µs] 0
Fig. 3. Measured ϕref and ϕint corresponding to the formation of a
0 10 20 30 40 50
141.3 µm diameter cavitation bubble using a 10 µJ laser pulse. ϕbub is Time [µs]
the phase difference between the reference and interferometer signals. Fig. 4. Time-resolved bubble dynamics for bubbles formed using
pulse energies of 2.5, 10, and 20 µJ resulting in maximum bubble radii
λϕbub (t) of 77, 136, and 172 µm, respectively, are shown with theoretical bub-
R B (t) = , (1) ble radius predicted by the Rayleigh–Plesset model. In the case of 10 µJ
4π(n G − n W )
pulse energy, we also show data acquired using images captured from
where λ is the wavelength of the probe beam, and n G and n W are separate events using an intensified CCD camera (Stanford Computer
the refractive indices of the gas within the bubble and surround- Optics, 4Picos).
ing water, respectively.
Once the bubble is initiated and growing in size, the instanta-
maximum radius can range from ±3 µm at times when the
neous frequency of the interferometer signal Iint falls below the
bubble is changing size slowly, to a maximum bubble radius of
110 MHz heterodyne frequency, since the optical path length
±40 µm during bubble collapse [27,29]. This large variation
in the sample arm is decreasing with time. Conversely, once the
is primarily due to shot-to-shot variability in the phenomena.
bubble reaches its maximum size and begins to collapse, the
However, we do find that our interferometric method has dif-
instantaneous frequency of the interferometer signal Iint rises
ficulty unwrapping the phase during the final stages of bubble
above a 110 MHz heterodyne signal. The detection limit of our
collapse once the velocity of the bubble wall exceeds approx-
bubble measurement is dependent on the root-mean-square
imately 84–94 m/s. This collapse velocity corresponds to a
(RMS) phase noise associated with the baseline interferometer
heterodyne detection frequency in excess of 154–159 MHz.
signal without bubble formation. This phase noise amounts to
0.1 radians and corresponds to a detection limit of 15 nm. Interestingly, we have an unidentified source of ambient elec-
To assess the measurement accuracy of the interferometer, we tronic noise located at 156 MHz. This leads us to believe that
compare the bubble dynamics measurements with predictions our difficulty in resolving the bubble collapse is not intrinsic to
provided by the Rayleigh–Plesset model [41], which has been our overall approach, but may instead be resolved through better
demonstrated to provide accurate predictions for the cavitation electrical isolation or by using an AOM operating at a lower
bubble dynamics in this case [13,27]: modulation frequency.
In summary, we have demonstrated an accurate interfero-
metric method for obtaining the complete cavitation bubble
" #
d 2R B 3 dR B 2
2σ 4µ dR B
ρ RB + = p B − p∞ − − , dynamics from a single cavitation event with 15 nm radial preci-
dt2 2 dt RB RB dt sion and sub-nanosecond temporal resolution. This approach is
(2) more accurate, less costly, and simpler to operate as compared to
where R B (t) represents the time-resolved bubble radius, µ rep- fast-frame photographic and holographic methods. Moreover,
resents the viscosity of water, ρ represents the density of water, unlike probe beam methods, our method requires no calibration
and σ represents the surface tension at water/vapor interface, to obtain quantitative measurements. This approach allows for
with p B and p ∞ representing the pressure inside the bubble and capturing of the full cavitation bubble dynamics extending over
surrounding liquid, respectively. Figure 4 shows excellent agree- tens of microseconds while retaining sub-nanosecond temporal
ment between the predictions made by the Rayleigh–Plesset resolution. We anticipate these capabilities will be of broad
model and the interferometric measurement. As a point of com- utility for examination of cavitation bubble dynamics, as well
parison, we also provide bubble dynamics data obtained under as for metrology applications such as optorheological materials
similar conditions obtained by taking a single bubble image at characterization.
different time points using time-resolved photography [13,27].
A comparison of the two data sets clearly illustrates the Funding. National Institutes of Health/National Institute of General
increased measurement uncertainty that is incurred when Medical Sciences (R01 GM129426); National Science Foundation (Graduate
Research Fellowship Program (BGW)).
determining the bubble dynamics using time-resolved images
obtained using multiple independent trials. Specifically, typical Acknowledgment. B. G. Wilson acknowledges support of a National
measurement uncertainties for cavitation bubbles of ∼140 µm Science Foundation (NSF) Graduate Research Fellowship.
1412 Vol. 46, No. 6 / 15 March 2021 / Optics Letters Letter
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