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Springer Theses
Recognizing Outstanding Ph.D. Research

Jan Frederik Totz

Synchronization
and Waves
in Active Media
Springer Theses

Recognizing Outstanding Ph.D. Research


Aims and Scope

The series “Springer Theses” brings together a selection of the very best Ph.D.
theses from around the world and across the physical sciences. Nominated and
endorsed by two recognized specialists, each published volume has been selected
for its scientific excellence and the high impact of its contents for the pertinent field
of research. For greater accessibility to non-specialists, the published versions
include an extended introduction, as well as a foreword by the student’s supervisor
explaining the special relevance of the work for the field. As a whole, the series will
provide a valuable resource both for newcomers to the research fields described,
and for other scientists seeking detailed background information on special
questions. Finally, it provides an accredited documentation of the valuable
contributions made by today’s younger generation of scientists.

Theses are accepted into the series by invited nomination only


and must fulfill all of the following criteria
• They must be written in good English.
• The topic should fall within the confines of Chemistry, Physics, Earth Sciences,
Engineering and related interdisciplinary fields such as Materials, Nanoscience,
Chemical Engineering, Complex Systems and Biophysics.
• The work reported in the thesis must represent a significant scientific advance.
• If the thesis includes previously published material, permission to reproduce this
must be gained from the respective copyright holder.
• They must have been examined and passed during the 12 months prior to
nomination.
• Each thesis should include a foreword by the supervisor outlining the signifi-
cance of its content.
• The theses should have a clearly defined structure including an introduction
accessible to scientists not expert in that particular field.

More information about this series at http://www.springer.com/series/8790


Jan Frederik Totz

Synchronization and Waves


in Active Media
Doctoral Thesis accepted by
the Technische Universität Berlin, Germany

123
Author Supervisor
Dr. Jan Frederik Totz Prof. Harald Engel
Institut für Theoretische Physik Institut für Theoretische Physik
Technische Universität Berlin Technische Universität Berlin
Berlin, Germany Berlin, Germany

ISSN 2190-5053 ISSN 2190-5061 (electronic)


Springer Theses
ISBN 978-3-030-11056-7 ISBN 978-3-030-11057-4 (eBook)
https://doi.org/10.1007/978-3-030-11057-4
Library of Congress Control Number: 2018966380

© Springer Nature Switzerland AG 2019


This work is subject to copyright. All rights are reserved by the Publisher, whether the whole or part
of the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations,
recitation, broadcasting, reproduction on microfilms or in any other physical way, and transmission
or information storage and retrieval, electronic adaptation, computer software, or by similar or dissimilar
methodology now known or hereafter developed.
The use of general descriptive names, registered names, trademarks, service marks, etc. in this
publication does not imply, even in the absence of a specific statement, that such names are exempt from
the relevant protective laws and regulations and therefore free for general use.
The publisher, the authors and the editors are safe to assume that the advice and information in this
book are believed to be true and accurate at the date of publication. Neither the publisher nor the
authors or the editors give a warranty, express or implied, with respect to the material contained herein or
for any errors or omissions that may have been made. The publisher remains neutral with regard to
jurisdictional claims in published maps and institutional affiliations.

This Springer imprint is published by the registered company Springer Nature Switzerland AG
The registered company address is: Gewerbestrasse 11, 6330 Cham, Switzerland
Supervisor’s Foreword

The interplay between synchronization and spatiotemporal pattern formation is


central for understanding a broad variety of phenomena in natural, life, and social
sciences. Examples include associative memory and learning in neural networks,
coordinated contraction of heart tissue, or pathological synchronization during
Parkinson’s disease. Many everyday macroscopic patterns result from self-
organization in non-equilibrium systems that consist of spatially coupled units
displaying excitable or oscillatory nonlinear kinetics. Beyond a critical distance to
equilibrium symmetry-breaking, instabilities give rise to spatiotemporal patterns
and collective modes across vastly different macroscopic space and time scales
selected by the system itself.
Under local spatial coupling between the individual units, remarkable
self-organized spatiotemporal patterns are rotating excitation waves, i.e., spiral
waves in two and scroll waves in three spatial dimensions. Rotating waves are
omnipresent: They have been observed as coverage patterns in heterogeneous
catalysis, intracellular calcium waves, waves of electrical activity in the context of
cardiac arrhythmias, and many other situations.
Against this background, in his thesis, Jan F. Totz addresses three open ques-
tions of basic research in Nonlinear Dynamics: How does geometric confinement
affect the dynamics and the stability of scroll rings? How do traveling excitation
waves spread on oscillator networks? Does the long-predicted spiral wave chimera
state, featuring a spiral arm consisting of synchronized oscillators that rotate around
a core of phase-randomized oscillators, really exist?
The answer to the first question implies modeling and experimental verification
of a new type of autonomous pacemaker representing a scroll ring stabilized due to
its interaction with a nearby no-flux boundary. Answering the second question
reveals the role of permutation symmetries in wave propagation on networks of
weakly heterogeneous relaxation oscillators. Concerning the last question, Jan F.
Totz succeeded to demonstrate the so far elusive spiral wave chimera state, pre-
dicted by Kuramoto and co-workers already in 2002, in a network of 1600 coupled
chemical relaxation oscillators. In all three cases, predictions of theoretical mod-
eling and numerical simulation agree well with experiments. The results highlight

v
vi Supervisor’s Foreword

the similarities and the differences between phase and relaxation oscillators. While
relaxation oscillators are ubiquitous in nature, most analytical results have been
obtained for phase oscillators.
The verification of the spiral wave chimera state imposed most severe chal-
lenges. The developed computer-controlled setup, based on an open chemical
reactor for a large number of optically coupled catalytic Belousov-Zhabotinsky
beads, significantly extends the experimental possibilities for the study of syn-
chronization patterns in large networks of relaxation oscillators. Node dynamics,
frequency distribution, and network topology can be chosen as desired. Moreover,
coupling weights can be time-dependent or even random. This opens new per-
spectives for exploring adaptation and learning in networked oscillatory or excitable
units.
The work reported in this thesis represents a significant advance in synchro-
nization and pattern formation with possible applications in smart materials, soft
robotics, neuromorphic computing, and medical treatment of neurological diseases
as Parkinson’s, tinnitus, and epilepsy.

Berlin, Germany Prof. Harald Engel


December 2018
Abstract

The aim of this thesis is the study and characterization of a number of


self-organized patterns with potential relevance to biological systems and beyond.
To this end, we utilize the well-established oscillating Belousov-Zhabotinsky
(BZ) reaction in chemical experiments as well as numerical simulations of the
underlying model equations on graphics cards.
The first part of this thesis features experiments on spiral-shaped excitation waves
in a three-dimensional oscillatory medium. Their spatiotemporal evolution is gov-
erned by a circular line singularity around which the waves rotate. In the absence of
medium boundaries, the singularity would contract and eventually vanish. Due to the
interaction with the boundary, the singularity may stabilize, such that it acts far
beyond its theoretical lifetime as an autonomous pacemaker. The influence can be
taken into account in a semi-analytical kinematic model, which is in good agreement
with experiments and simulations. Related patterns of electrical activity play a
critical role in ventricular tachycardia, a life-threatening heart arrhythmia.
A small network of discrete BZ oscillators can support periodically spreading
excitation waves. For a narrow distribution of natural oscillation frequencies, the
waves propagate along the permutation symmetries. It is known that comparable
electrical waves in neuronal networks control rhythmic muscle contraction.
In the final part of the thesis, we verify the spiral wave chimera state that was
predicted by Yoshiki Kuramoto in 2002. This particular state exhibits a coherent
spiral wave rotating around a core that consists of incoherent oscillators. Such patterns
might play a role in nonlocally coupled cardiac and cortical tissue as well as in the
photoelectrodissociation on doped silicon wafers and arrays of superconducting
quantum interference devices and opto-mechanical oscillators. The experimental
setup, which we developed for this purpose, furthermore allows for reproducible
experiments under laboratory conditions on networks with N [ 2000 oscillators. It
facilitates the free choice of network topology, coupling function as well as its
strength, range, and time delay, which can even be chosen as time-dependent.

vii
Acknowledgements

Prof. Harald Engel


Prof. Oliver Steinbock, Prof. Kenneth Showalter,
Prof. Vladimir K. Vanag, Prof. Jörn Dunkel

AG Engel (Berlin)
Steffen Martens, Julian Rode, Dumitru Călugăru, Jakob Löber, Fabian Paul,
Markus Radszuweit, Dirk Kulawiak, Florian Buchholz, Christopher Mikolajzak,
Leander Self, Franziska Böhme, Ingeborg Gerdes, Hermann Brandtstädter, Grigory
Bordyugov, Jan Schlesner, Andrea Schulze, Julia Eckert, Yulia Jagodszinski, Peter
Orlowski

AG Steinbock (Florida)
Zulma Jiménez, Sumana Dutta, Laszlo Roszol, Rabih Makki

AG Showalter (West Virginia)


Darrell Collison, Desmond Yengi, Razan Snari, Simba Nkomo, Mark Tinsley

AG Vanag (Kaliningrad)
Pavel Smelov, Ivan Proskurkin, Dmitry Safonov

Special Thanks
Georg Engelhardt, Enrico Dietz, Norbert Zielinski, Rinaldo August, Sven-Uwe
Urban, Jörn Six, Fabian Sielaff, Chris Scharfenorth, Sascha Gerloff, Anna
Zakharova, Madeleine Nuck, Annette Taylor, Kathy Lüdge, Delora Gaskins,
Valentin Flunkert, Miran Alic, Christian Hennig, Franz-Josef Schmitt, Philipp
Strasberg, Wassilij Kopylov, Alice Schwarze, Fachreddin Tabataba-Vakili, Farsane
Tabataba-Vakili, Ramona Rothfischer, Julien Olck, Sophie Seidenbecher, Sophie
Ernst, Pirmin Kustin

ix
x Acknowledgements

Funding
Prof. Holger Stark (GRK 1558) and Prof. Eckehard Schöll (SFB 910)

Flora high school (South Carolina)


Physics teacher Mr. Tom Sunday

Family
Cordula & Claus-Dieter & Carl Hendrik & Erika & Werner
Dedicated to my loving wife: Sonja
Contents

1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
2 Confined Scroll Rings . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
2.1 Theoretical Background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
2.2 Chemical Experiments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
2.3 Numerical Simulations and a Kinematical Model . . . . . . . . . . . . . 20
2.4 Chapter Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
2.5 Future Directions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30
3 Target Wave Synchronization on a Network . . . . . . . . . . . . . . . . . . 37
3.1 Theoretical Background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 37
3.2 Experimental Results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 40
3.3 Short Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 51
3.4 Future Directions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 51
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52
4 Spiral Wave Chimera . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 55
4.1 Theoretical Background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56
4.2 Experimental Setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 61
4.3 Numerical Simulations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 66
4.4 Results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 73
4.5 Short Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 86
4.6 Future Directions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 86
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 89
5 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 99
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 100

xi
xii Contents

Appendix A: Dimension Reduction of Oscillators and Oscillatory


Patterns . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 103
Appendix B: Experimental Setups and Numerical Code . . . . . . . . . . . . . 119
Appendix C: Chemistry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 141
Curriculum Vitae . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 161
Chapter 1
Introduction

“... on the shoulders of giants”

Bernard of Chartres

The second law of thermodynamics [1] states, that during an irreversible process the
total entropy S in an isolated system always grows:

di S
> 0. (1.1)
dt
As time passes, matter will decay from an ordered, but improbable state to a dis-
ordered and more probable state. Yet structures of high order, namely life forms,
exist and very successfully so: From the microscopic bacterium Pelagibacter ubique
[2] that measures just about 5 µm but makes up for the largest cumulated species
biomass worldwide to the orders of magnitude larger blue whale (Balaenoptera mus-
culus) reaching about 30 m in size [3]. Life prevails despite inhospitable environ-
ments that are devoid of oxygen [4], below freezing at −20 ◦ C [5] or close to boiling
temperatures [6], to just give a few examples.
This paradox was addressed from the perspective of statistical physics by Erwin
Schrödinger, one of the pioneers of quantum mechanics, in his book “What Is Life?”
[7]. He not only argues for the existence of a biomolecular “asymmetric crystal” as
a carrier of hereditary information, which inspired Crick and Watts to search for the
DNA double helix molecule [8], but also he makes the case that living matter attains
an ordered state and remains in it, due to consuming “negative entropy” from its
environment,

di S de S
+ > 0. (1.2)
dt dt
Put differently, a living being is an open system, which maintains a non-equilibrium
state by entropy exchange de S with its surroundings via nutrients and waste products.
© Springer Nature Switzerland AG 2019 1
J. F. Totz, Synchronization and Waves in Active Media,
Springer Theses, https://doi.org/10.1007/978-3-030-11057-4_1
2 1 Introduction

This notion was formalized mathematically by Ilya Prigogine [9, 10] as a “dissipative
structure”, that exists far from equilibrium and bifurcates off the equilibrium state.
Meanwhile, the dynamics of self-organized structures were elucidated from a
macroscopic viewpoint by Alan Turing and Arthur Winfree who had laid out in their
respective seminal papers the basis for spatial pattern formation [11] and temporal
synchronization of oscillators [12].
Self-organized structures are not only restricted to life. Shortly after the first
working laser [13] was built, Hermann Haken successfully proposed a theory for its
operation based on non-equilibrium dynamics [14]. He and Werner Ebeling went on
to found and popularize the new field of “synergetics” [15, 16] in divided Germany
and throughout the scientific world.
The common thread in all these endeavors is self-organization. Its defining feature
is a structure of high, life-like order that is attained due to its own internal, nonlinear
dynamics. No detailed, external control on the structure is required.
Its continuing success was underscored with two Nobel prizes. One in chemistry
was received by Gerhard Ertl in 2007 for developing the methods of surface chemistry
in general and for observing pattern formation on catalytic platinum surfaces during
CO oxidation in particular [17]. The other was awarded as recently as 2017, when the
Nobel Prize in Physiology or Medicine was shared by Jeffrey Hall, Michael Rosbash
and Michael Young for revealing the basic biomolecular machinery of chronobiology
in virtually all living things, from bacteria, fungi to plants and animals [18, 19].
It was recently proposed [20, 21] that far away from equilibrium the second law
needs to be adapted
 
de S  d pa→b di S
 + ln + >0 (1.3)
dt a→b dt pb→a dt

to account for transition probabilities in and out of a given non-equilibrium state.


This means that the more irreversible a process is, pa→b  pb→a , the larger its asso-
ciated internal entropy production will be. Furthermore this allows for an engineered
dissipative adaptation, by placing suitable driving forces on the system, that will
enable it to reach desired non-equilibrium states, but not escape from them [22].
Future developments in the field of self-organization can be expected to give
insight into life-like non-equlibrium phenomena as well as lead to new applications
in smart materials [23] and soft robotics [24] founded on neuromorphic [25, 26] and
biomimetic structures [27], ultimately opening the door to artificial life forms [28,
29] and new medical therapies [30, 31].
A ubiquitous example for non-equilibrium dynamics is the conversion of a con-
stant energy supply into a non-constant, but periodic motion. This mechanism under-
lies the music played on a violin (Fig. 1.1a) and all other bowed string instruments
[32]. From a physical standpoint, the vibration of a single violin string during a
bow stroke is equivalent to a damped mass-spring oscillator on a moving conveyor
belt (Fig. 1.1b). Both, the string and the mass, perform a stick-slip motion. During
the sticking phase they move in the direction they are pulled by their respective
drivers due to high static contact friction. The slipping phase begins when a large
1 Introduction 3

Fig. 1.1 Real-world examples and simplified physical models of relaxation oscillators. a Violin
strings are brought to oscillate utilizing a violin bow. Their transversal vibrations are amplified in
the instrument body to emit musical tones. b A mass-spring oscillator driven by a moving converyor
belt. c Neurons can periodically generate charge imbalances to communicate with other cells. This
imbalance is attained despite diffusive fluxes via active ion gates in the cell membrane. d A minimal
model of the ion transport across the membrane is given by an equivalent RC circuit, consisting of
a capacitor and batteries in series with voltage-dependent resistors

displacement is reached so that the restoring elastic force surpasses the friction force
and pushes the string or mass in the direction opposite to the driver. During this phase
the contact friction is very small, because there is sliding instead of static friction.
Overall, the net friction composed of internal and contact friction is positive during
the slipping phase and negative during the sticking phase as the net friction opposes
and aligns with the movement, respectively. In the sticking phase the system takes
up as much energy from the external driver as it lost in the slipping phase in order
to maintain a stable recurrent oscillation. The resulting waveform consists only of
harmonics giving rise to a clear and clean pitch.
Another intriguing case are neurons in the mammalian brain (Fig. 1.1c). They
possess the ability to generate short voltage spikes along their membranes for com-
munication with other neurons and muscle cells enabling motor control, emotions
and thoughts [33]. This process can be understood on a molecular level. The cell
membrane of a neuron consists of an impervious lipid bilayer (inset in Fig. 1.1c)
with embedded channel proteins that allow for and regulate transmembrane trans-
port. Depending on the charge imbalance between the intra- and extracellular space,
the channels pump ions, mainly sodium Na+ and potassium K + into or out of the neu-
ron. The molecular pumps consume energy in the form of adenosine triphosphate and
4 1 Introduction

perform work against the charge gradient giving rise to short-lived positive charge
accumulations - the voltage spikes.
This intricate biochemical system is well-captured by an equivalent RC circuit
[34] (Fig. 1.1d). The cell membrane is represented by a capacitor, since it separates the
negatively charged intracellular from the effectively positively charged extracellular
space. An active ion-specific molecular pump is modeled as a battery in series with
a resistor that shows voltage-dependent conductivity. The key-components are the
ion-specific batteries. They represent the native level of ion separation across the
membrane, known as resting potential, that is due to the base activity of each pump
in absence of a spike. For sodium ions the resting potential is very positive and for
potassium ions it is very negative. Depending on the difference between voltage
across the membrane and a resting potential of an ion pump, the corresponding
resistor conductivity will increase or vanish, which is equivalent to an open or closed
ion channel, respectively.
Apart from these cases, there are many more examples permeating biology, chem-
istry and physics: predator and prey population cycles [35], regulatory gene networks
[36], cilia cells [37], sinoatrial pacemaker node [38], glycolytic cycle [39], circadian
rhythm [40], saltwater oscillator [41], Briggs Rauscher-[42], Bray-Liebhafsky-[43],
CIMA-reaction [44], electrochemical cells [45], molecular programs with nucleic
acids [46], mercury beating heart [47], pendulum clocks [48], steam engines [49],
lasers [50], Josephson junction [51], the aeroelastic galloping instability in bridges
[52], organs pipes [53], vocal cords [54], body and wheelset hunting [55], para-
sitic electronic oscillations [56], wheel shimmy [57], geysers [58], earthquakes [59],
ocean circulation [60], ice ages and Dansgaard–Oeschger events [61], chalk squeak-
ing on a blackboard [62], drinking bird toy [63], see-saw with water reservoir [64],
putt putt boat [65], Tantalus’ cup [66], coupled palm glasses [66], thermoacoustic
oscillations in Rijke tubes [67], economic cycles [68], memristors [69], Pearson-
Anson circuit [70] for neon tube oscillators, blinking warning lights and windshield
wipers, astable Abraham-Bloch multivibrator and its modern variant the 555 timer
chip [71], boolean elements with phase locked-loops [72], solar cycle [73], micro-
quasars [74], and variable cepheid stars [75], which were instrumental in discovering
the expansion of the universe [76].
All of the preceding examples have in common, that during one cycle of their
periodic behavior they do not only dissipate energy, but also gain it. This is the
hallmark of a “self oscillator” [49, 62, 64, 77, 78]. Mathematically, this can be
modeled with a damped harmonic oscillator,

d2x dx
m + γ(x) + kx = 0 , (1.4)
dt 2 dt

that allows for positive and negative friction γ(x). Here, the parameters k and m
represent the spring constant and mass. The simplest friction function is given by a
sum over even powers of the displacement x:
1 Introduction 5

Fig. 1.2 Prototypical relaxation oscillator dynamics. a Stable oscillation cycle around an unsta-
ble fixed point at the origin of phase space. The color denotes portions where the oscillator dissipates
(red) or gains (green) energy. b One-dimensional projection of the cycle shows the oscillator accel-
erating during active friction whereas it decelerates and reverses course during dissipative friction.
This leads to a non-sinusoidal time trace composed of many Fourier modes. Parameter choice:
μ = 10

γ(x) = μ(−1 + x 2 + · · · ) . (1.5)

The omission of odd powers guarantees that friction acts identically for positive
and negative displacements x. The negative friction term −μ draws energy into
the system, such that the oscillation amplitudes grows. To counteract the otherwise
unbounded growth there is a positive quadratic term, +μx 2 , that becomes relevant
for large amplitudes. To gain insight into the resulting behavior it is instructive to
apply the Liénard transformation [79] to (1.4). After suitable rescaling, the equation
reads:  
u3
u̇ = μ u −
2
+v ,
3 (1.6)
v̇ = u .

The solution to this system of differential equations is plotted in the phase space
spanned by u and v (Fig. 1.2a). It clearly shows a counterclockwise closed trajectory
around the origin giving rise to the expected oscillatory behavior in one dimension
(Fig. 1.2b). Note that the motion does not decay despite the presence of friction
in the system. At large displacements (red), dissipation pushes the oscillator to its
equilibrium position at u = 0. However, once the displacement amplitude decays and
the oscillator approaches the equilibrium (green), the character of friction switches
from dissipative to active. This pumps energy into the oscillation, so that it overshoots
the equilibrium position and also regains the energy lost at large displacements.
Eventually the oscillator perpetually relaxes back to the equilibrium but is incapable
of reaching it due to active friction. For this reason, oscillators exhibiting this behavior
were coined “relaxation oscillators” by van der Pol [80] and later, in recognition of his
contributions, model (1.6) was named the “van der Pol oscillator” [81]. Overall, the
6 1 Introduction

Fig. 1.3 Experimentally accessible real-world relaxation oscillators. a Spatial fluorescence


signal from fluorescing proteins in a single neuron. The scale bar corresponds to 10 µm. b Mean
fluorescence signal of a single neuron over time showing relaxation oscillations. c Chemical oscilla-
tor based on the Belousov-Zhabotinsky reaction. The scale bar corresponds to 100 µm. d Utilizing
a flourescent catalyst to visualize the evolution of chemical concentrations reveals relaxation oscil-
lations. The raw data of the optogenetic measurement was kindly provided by Yoav Adam of the
Cohen lab [82]

competition between the antagonistic dissipative and active friction forces balances
a relaxation oscillator on a temporally-periodic trajectory. The long-term behavior
of (1.6) can be assessed with standard tools of nonlinear dynamics: linear stability
analysis and the Poincaré-Bendixson theorem [79].
Another important aspect of (1.6) is the time scale separation due to the introduc-
tion of friction. The local dynamics in u-direction evolve faster than the dynamics in
v-direction by a factor of μ2 . This is also clear from Fig. 1.2: The oscillator spends
most of its time on the vertical parts of the cycle, but quickly moves through the
horizontal branches.
To illustrate and verify the value and predictions of theoretical concepts in general,
there are real-world experiments. With the recent rise of optogenetics, it is possible
to genetically modify neurons in such a way as to record and control their activity
with light [83–85]. This is achieved by delivering genetic code for expression of
fluorescent proteins and photosensitive membrane channels into target neurons via
a viral vector. Due to advances in optical technology, it was recently possible to
optically measure the spatially-resolved activity of single neurons [82] (Fig. 1.3a, b).
As expected the neuron shows relaxation oscillations in fluorescent light emission
in the near infrared spectrum.
1 Introduction 7

Fig. 1.4 Excitation wave patterns in different topologies. a Scroll ring in a three-dimensional
continuous domain. b Target wave on a network with symmetry clusters. c Spiral wave chimera on
a discrete two-dimensional grid

Another accessible test bed for predictions on single as well as ensembles of relax-
ation oscillators is the prototypical chemical oscillator, the Belousov-Zhabotinsky
reaction [86] (Fig. 1.3c). Its popularity is due to its neuromorphic character: It exhibits
concentration traces that are strikingly similar to the electrical activity of neurons [87]
(Fig. 1.3b, d). In spatially continuous systems it supports chemical patterns similar to
electrical activity patterns on the heart muscle that usurp its mechanical contraction
before sudden cardiac failure [88–90].
In this thesis the overarching theme is elucidating the peculiar behavior of exci-
tation waves as stable temporally periodic patterns on different topologies (Fig. 1.4).
Unlike waves in a fluid or conservative solitons [91], excitation waves require an
active medium, that is kept far from equilibrium due to energy influx like the gain
medium in a laser [15].
The excitable character of the medium manifests itself in the all-or-nothing
response to an external perturbation: Small perturbations below a threshold have
a negligible consequence, whereas large superthreshold perturbations lead to an
extensive and unique response. This definition is inspired by biological neurons
[34, 92], that remain quiescent in response to small current fluctuations, but emit a
voltage spike once sufficiently perturbed. The response behavior is deeply related to
the slow domains during a relaxation oscillation. When an appropriate perturbation
kicks the oscillator into the fast domain of phase space, a new oscillation is imme-
diately induced. Before another perturbation can successfully trigger an excursion,
the system must pass through its refractory stage and return to its vulnerable state.
Such elements, connected in a chain, support the sequential propagation of a spike
from one end to the other: an excitation wave [93, 94].
Chapter 2 is focused on the formation of a long-living pacemaker, a structure that
acts as a periodic source of excitation waves in three dimensions. For parameters
where stable pacemakers were previously thought impossible, it is shown that they
can exist due to interaction with inherent spatial boundaries that occur in any real
system like the myocardium.
In Chap. 3, the focus shifts to excitation waves on networks. It is found that
underlying network symmetries are intertwined with the way an excitation wave
propagates over the network. During propagation, the nodes in each symmetry cluster
synchronize, such that they fire concurrently.
8 1 Introduction

Finally in Chap. 4, a large grid of discrete oscillators that are nonlocally cou-
pled to each other gives rise to a structure that was predicted 15 years ago by
Yoshiki Kuramoto theoretically [95], but never verified experimentally: the spiral
wave chimera. The distinguishing feature is that a coherent excitation wave rotates
around a central region that consists of seemingly incoherent oscillators even though
all oscillators are coupled identically. This is the first experimental example for the
co-existence of ordered and disordered phases in a robust and reproducible real set-
ting without sensitive dependence on initial conditions.

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Chapter 2
Confined Scroll Rings

Among self-organized spatio-temporal patterns rotating spiral-shaped waves are very


common. This suggests, that their emergence must depend on general rules, that
transcend microscopic details. As depicted in Fig. 2.1, an initially planar wave front
can break up due to interaction with inhomogeneities in an active medium. The
resulting wave features an open end far from any boundaries. Still, the excitation
(fire) will spread from the current excited region to any surroundings that are not in
their refractory, unexcitable (burnt) state. This means that the main front will continue
forward, but at the wave tip the excitation can spread upwards in addition. While the
tip continues on its pirouette-like motion, it becomes the source of excitation waves,
that are periodically emitted into the medium. In this sense, the tip is the localized
organizing center [1] of the delocalized spiral wave, that has a wavelength λ and
rotation period T . Note that the oscillations at each location outside the spiral core
are entrained to the rotation period of the spiral wave. Here, the non-equilibrium
character manifests itself in the influx of external energy, that is required to return
oscillators to their rest state (unburnt) so a neighboring excitation can restart the
oscillation cycle.
Apart from this simple example, spiral waves have been observed in an aston-
ishing variety of biological, chemical and physical systems1 : myocardium [21–25],
cardiac cell monolayers [26, 27], optogenetically engineered cell layers [28–30],
giant honey bee colonies [31], mammalian cortex [32], calcium waves in frog
eggs [33], chicken retina [34], single cells and conglomerates of the social amoeba
Dictyostelium discoideum [35, 36], geographical tongue inflammation [37], migra-
tory erythematous lesions [38], human crowds [39], synthetic somatic cell sheets
[40], uterus during labor [41, 42], yeast glycolysis [43], Min proteins [44] and

1 Some vortex patterns in nature are spiral-shaped, but there is no underlying excitable medium.
Some examples are Bose Einstein condensates [3], spin spirals [4], spiral crystal growth [5–7],
drop-induced airflows [8], fluid mixing [9], Bernard convection in gas mixture [10, 11], Faraday
experiments with vertically vibrated viscous fluid and sand [12, 13], Kármán vortex street [14],
hurricanes [15], extraterrestrial storms, such as the Great Red Spot [16] and polar vortices [17] on
Jupiter, galaxy formation [18] and the recent binary black hole as well as neutron star mergers,
which emitted double spiral gravitation waves [19, 20].
© Springer Nature Switzerland AG 2019 13
J. F. Totz, Synchronization and Waves in Active Media,
Springer Theses, https://doi.org/10.1007/978-3-030-11057-4_2
14 2 Confined Scroll Rings

Fig. 2.1 Model for spiral wave formation. A forest consisting of trees that can catch fire, burn
and regrow (unnaturally) fast is a minimal model for an excitable medium. a An excitation wave in
the form of a planar flame front travels from left to right. In the back of the flame front, new trees are
already growing. A rain cloud located in the center of the medium prevents flames from spreading
in the top half, which breaks the front and creates an open end. b While the flame front propagates
in the bottom half, the rain cloud vanishes. The broken flame front continues onward to the right and
now also spreads in the upward direction. This is the genesis of the spiral wave. c After a sufficient
number of rotations, the full-fledged spiral wave pattern is observable. This cellular automaton-like
simulation was realized with the Star Craft II map editor [2]

actin-proteins in electro-fused cell membranes [35, 45], lichen growth [46], cilia
arrays [47], Belousov–Zhabotinsky (BZ) reaction medium [48], BZ-surfactant mix-
tures [49], BZ-infused Langmuir monolayers [50], precipitation reactions [51], CO
oxidation on Pt-110 surface [52], electrodeposition of a binary alloy [53], corrosion
[54], lasers [55–57], combustion [58], liquid crystals [59, 60], plasma [61], dielec-
tric barrier gas-discharge [62], trapped ultracold ion arrays [63], optomechanical
oscillator arrays [64], coupled map lattices [65], and Josephson junction arrays [66].
Among the most striking examples are spiral waves on the heart muscle, where
they are also called rotors or reentry. During the healthy operation of the heart,
the sinoatrial node entrains the beating rhythms of all cells in the myocardium by
emitting a propagating electric excitation wave. Upon arrival at a heart cell, the cell
expands and shortly after contracts again. This synchronized, collective mechanical
deformation underlies the vital heart beat that pumps blood through the body [67].
Due to e.g. unexcitable [68] or highly excitable [69] obstacles, spiral waves may
nucleate. Since they are periodic wave sources, they directly compete with the sinoa-
trial node for the entrainment of the myocardium. If multiple spiral waves form,
the ensuing wave chaos compromises the synchronized, collective deformation and
leads to life-threatening fibrillation [24, 70].
Due to the three-dimensional nature of the heart, the rotating patterns are actually
scroll waves, which are made up of spiral waves stacked up on each other. Accord-
ingly, the center of the spiral core is extended to a line first identified by Winfree as
organizing center of the scroll wave and named filament [46, 71–74].
One of the first reported experimental observations of a filament in the cardiac
muscle, had a ring-shaped form [75]. Indeed, connecting both ends of the filament
and bending it into a ring, leads to a simple structure called the scroll ring [46, 76]
(see Fig. 2.2a). Curiously, the periodic wave pattern of scroll rings was exploited
in oil-immersed BZ drops to drive autonomous periodic motion via changes in the
surface tension [77].
The dynamics of this structure in the presence of boundaries are the focus of this
chapter.
2.1 Theoretical Background 15

Fig. 2.2 Unperturbed dynamics of an axisymmetric, untwisted scroll ring. a A scroll ring is a
toroid formed from a spiral wave. The tip of each spiral wave is attached to a ring with radius R,
called the filament (red). For clarity, here only a single isosurface of the continuous concentration
pattern is shown. b Without perturbations the scroll ring will either decay for filament tension α > 0
(blue) or grow for α < 0 (yellow), see (2.1). Time and space are scaled relative to the rotation period
T and wavelength λ of the waves emitted from the ring

2.1 Theoretical Background

The equations of motion for filaments were first derived in a mathematically rigorous
way by James Keener in 1988 employing techniques from singular perturbation
analysis [78]. His approach is reviewed briefly in Appendix A.2 together with recent
developments.
In the case of a closed filament loop, a scroll ring, the equations of motion
simplify to

dR
= −ακ , (2.1)
dt
dz
= βκ . (2.2)
dt
While the ring drifts along its symmetry axis in z-direction, the radius R of the ring
changes depending on the ring curvature κ = 1/R.2 It will either contract and vanish
or expand depending on the sign of the filament tension α, see Fig. 2.2b. In its later
stages a growing ring will undergo the negative line-tension instability [80]. This
means it will break apart and develop into a highly disorganized pattern known as
Winfree turbulence [81]. The analytical solution to the radius dynamics (2.1) is given
by

R 2 (t) = R02 − 2αt . (2.3)

2 Notethat this is a special case of an arbitrary closed curve r moving under mean curvature flow:
dr/dt = −ακ N , where N is the normal vector at each point of the curve r [79].
16 2 Confined Scroll Rings

Thus unlike its two-dimensional counterpart, the spiral wave, a scroll ring is not
a stationary pattern. Intuitively the non-stationarity is clear: In two dimensions,
a spiral wave will drift under an external perturbation. This can be realized in
the form of a time-periodic external parameter field [82], a parameter gradient
[83], an applied electric field [84], feedback control [85] or a Neumann boundary
[86, 87]. These perturbations lead to a periodic modulation of the excitability in
the core region. However, in three dimensions no external field is necessary, since
the periodic perturbation is due to the pattern itself. During one rotation period, the
filament loop will cycle between a large and a small radius, which have a small and
large curvature, respectively. In the same way the eikonal equation,

cn = c0 − Dκ , (2.4)

dictates how non-planar excitation waves in two dimensions straighten out [88–90],
the rotation speed of the filament increases when it goes from a large circumference
to a small one and decreases on its way back [91]. This periodic curvature-induced
self-modulation forbids stationary scroll ring patterns.
However, the dynamics of the unperturbed scroll ring can be complemented by
considering external perturbations, specifically the effect of Neumann boundaries
that naturally limit the spatial extent in a realistic setting. To this end it is important
to first understand how two-dimensional spiral waves interact with Neumann bound-
aries. One approach is based on the convolution of perturbations with spiral wave
response functions [92–94] (Appendix A.2). While it is highly successful for weak
perturbations, such as spatiotemporal parametric inhomogeneities, it is not applica-
ble to the interaction with Neumann boundaries. Boundaries break the symmetries of
the Euclidean plane and thus the Goldstone modes, whose adjoints are the response
functions, do not exist.
An alternative data-driven semi-analytic approach is described later.

2.2 Chemical Experiments

While the Belousov–Zhabotinsky reaction has been utilized to study chemical oscilla-
tions in time, it is also readily employed to study propagating patterns in a continuous
medium in time as well as space (see Appendix C). The applicability of this approach
is well-established by a large body of experiments on scroll rings in BZ media, test-
ing their existence [76], formation [95], dynamics for positive and negative filament
tension [96, 97], behavior influenced by each other [98], temperature and electrical
gradients [99, 100] as well as defect sites [101–103]. However, their interaction with
medium boundaries is less well explored.
Here, chemical waves in the active medium are observed with a simple spec-
trophotometric setup [104] (see Fig. 2.3a). Excitation waves manifest themselves as
narrow, propagating domains of oxidized catalyst surrounded by large regions of
reduced catalyst. Since the absorption spectrum of the ferroin catalyst, Fe(o-phen)3 ,
2.2 Chemical Experiments 17

Fig. 2.3 Experimental setup for boundary stabilized scroll rings. a Pattern formation in the
active medium is monitored spectrophotometrically. Excitation waves of oxidized catalyst absorb
less light than domains with reduced catalyst and thus the concentric waves of a scroll ring appear
in bright blue on an orange background, see photograph in b. The white bar corresponds to
1 cm. c Absorption spectra of the reduced form of the catalyst (Fe3+ ) in orange and the oxidized
form (Fe4+ ) in blue

depends on the oxidation state of the Fe-ion (Fe3+ /Fe4+ ), it is possible to optically
record the concentration waves with a CCD camera. Waves appear as bright blue on
an orange background (Fig. 2.3b), because the reduced catalyst strongly absorbs blue
and green parts of the VIS spectrum (λ = 380−560 nm), whereas the oxidized form
is nearly transparent to all wavelengths, except for a weak absorption of red wave-
lengths with λ = 580−620 nm (Fig. 2.3c). The optical contrast is further enhanced
with a bandpass filter that only transmits light into the camera with a wavelength
of λ = 400−500 nm. Further details on the experiment instrumentation are given in
Appendix B.1.1.
The chemical medium consists of two layers to allow for a reproducible nucleation
protocol of scroll rings [101] (Fig. 2.4). On the solid BZ reagent-infused hydrogel
layer rests another layer of liquid BZ solution. The agarose hydrogel is solid enough
to prevent convective instabilities and also sufficiently porous, such that the diffusion
of chemical species in both layers is approximately identical. The first step of the
initiation procedure is placing the clean end of a pure silver wire (99% Ag) at the
gel-liquid interface for about 15 s. Adding silver to the BZ solution allows for the
formation of small amounts of AgBr [105]. This locally perturbs the chemical balance
due to the removal of the inhibitor Br− . Thus shortly after the silver wire is removed,
a spherical wave starts to expand from the former location of the wire end. Similar to
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[522] Bunting, 59, 62, 43, 51, 52, and 61, respectively; also first
volume of records for each meeting.
[523] See map.
[524] Bunting, 49.
[525] Min. Kennett Mo. Mtg., 11-7-1715, 28.
[526] Min. Kennett Mo. Mtg., 12-3-1727, 188.
[527] Futhey & Cope, Hist. Chester Co., 302f.; Jordan, Hist.
Del. Co., II, 423ff.
[528] See page 42, Philadelphia 107, Abington 154, Darby.
[529] Min. Kennett Mo. Mtg., 12-11-1777, 625.
[530] Ibid., 1-15-1778, 626.
[531] Ibid., 1-14-1779, 658.
[532] Min. Kennett Mo. Mtg., 2-15-1781, 730.
[533] Ibid., 7-12-1781, 741.
[534] Ibid., 10-11-1781, 746.
[535] Ibid., 9-11-1783, 787.
[536] Ibid., 5-13-1783, 795.
[537] Ibid., 5-12-1785, 814.
[538] Min. Kennett Mo. Mtg., 8-11-1785, 820.
[539] Ibid., 2-14-1788, 874.
[540] Ibid., 1-14-1790, 914.
[541] Min. Kennett Mo. Mtg., 1-12-1792, 14.
[542] Horsham School Com. Minutes, 1-27-1783.
[543] Min. Kennett Mo. Mtg., 7-12-1792, 25.
[544] Ibid., 3-14-1793, 39.
[545] Ibid., 2-12-1795, 83.
[546] Min. Kennett Mo. Mtg., 4-16-1795, 88.
[547] Ibid., 5-14-1795, 91.
[548] Futhey & Cope, Hist. Chester Co., 302.
[549] Min. Kennett Mo. Mtg., 12-15-1796, 146.
[550] Ibid., 8-16-1798, 199.
[551] Min. New Garden Mo. Mtg., 3-6-1773, 174.
[552] Min. Kennett Mo. Mtg., 6-6-1778, 388.
[553] Ibid., 5-1-1779, 22.
[554] Ibid., 8-7-1779, 34.
[555] Ibid., 3-5-1785, 234.
[556] Ibid., 8-6-1785, 256.
[557] Ibid., 1-7-1786, 275.
[558] Ibid., 4-1-1786, 290.
[559] Ibid., 8-5-1786, 312.
[560] Min. Kennett Mo. Mtg., 8-4-1787, 355.
[561] Deed No. 88, Chester Co. (the deed is deposited in a
fireproof at Orthodox Meeting House, custody of Edgar Haines,
West Grove, Pa.).
[562] Min. Horsham Sch. Com., 1-27-1783.
[563] Min. Chester Q. Mtg., 12-2-1701.
[564] Ibid., 9-1-1703.
[565] Ibid., 12-2-1707.
[566] See page 122.
[567] See first book of Goshen Mo. Mtg. Records.
[568] Advices of the Yr. Mtg., 250.
[569] Min. Goshen Mo. Mtg., 1-8-1779.
[570] Ibid., 6-11-1779.
[571] Futhey and Cope mention a school at Birmingham as
early as 1753, Hist. Chester Co., 302.
[572] Min. Goshen Mo. Mtg., 6-11-1779.
[573] Ibid.
[574] Ibid., 1-11-1782.
[575] Min. Goshen Mo. Mtg., 3-8-1782.
[576] Ibid., 1-9-1784.
[577] Ibid.
[578] Ibid., 8-6-1784.
[579] Ibid., 8-5-1785.
[580] Min. Goshen Mo. Mtg., 8-11-1786.
[581] Ibid., 8-10-1787.
[582] Ibid., 7-6-1792.
[583] See page 132.
[584] Min. Goshen Mo. Mtg., 4-10-1795.
[585] Ibid., 8-5-1796.
[586] See page 132.
[587] Min. Goshen Mo. Mtg., 8-11-1797.
[588] Ibid.
[589] Ibid., 8-10-1798.
[590] See page 131.
[591] See page 73f.
[592] Min. Goshen Mo. Mtg., 1-6-1797.
[593] Min. Chester Q. Mtg., 9-9-1719.
[594] Ibid., 3-10-1725.
[595] See page 122; also Bunting, 51.
[596] Min. Bradford Mo. Mtg., 6-18-1762.
[597] Ibid.
[598] Ibid., 12-13-1765.
[599] Ibid., 4-7-1767.
[600] Ibid., 8-14-1767.
[601] Min. Bradford Mo. Mtg., 12-15-1778.
[602] Ibid., 2-12-1779.
[603] See page 133f.
[604] Min. Bradford Mo. Mtg., 5-12-1780.
[605] Min. Bradford Mo. Mtg., 2-16-1781.
[606] Ibid., 6-16-1781.
[607] Ibid., 2-16-1781.
[608] Ibid., 6-16-1781.
[609] Ibid., 9-14-1781.
[610] Ibid., 2-15-1782.
[611] Ibid., 8-15-1783.
[612] Ibid., 2-13-1784.
[613] Min. Bradford Mo. Mtg., 9-14-1792.
[614] Min. Uwchlan Mo. Mtg., 8-3-1763, 22.
[615] Ibid., 3-1-1765, 66.
[616] Ibid., 11-7-1782, 132.
[617] Ibid., 12-5-1782, 106.
[618] Min. Uwchlan Mo. Mtg., 12-4-1783, 158.
[619] Ibid., 2-5-1784, 162.
[620] Ibid., 2-10-1785, 184.
[621] Min. Bradford Mo. Mtg., 8-9-1787, 235.
[622] Min. London Grove Mtg., 12-3-1794, 56.
[623] Ibid., 3-4-1795, 62.
[624] Ibid., 7-1-1795, 73.
[625] Min. London Grove Mtg., 11-4-1795, 78.
[626] Futhey and Cope, Hist. Chester Co., 239.
[627] Min. Sadsbury Mo. Mtg., 3-6-1739, 7.
[628] Ibid., 6-21-1769, 180.
[629] Ibid., 1-20-1779, 297.
[630] Ibid., 2-20-1779, 298.
[631] Min. Sadsbury Mo. Mtg., 6-19-1782, 337.
[632] Ibid.
[633] Ibid., 3-21-1787, 39f.
[634] Ibid., 6-17-1789, 70.
[635] Ibid.
[636] Futhey and Cope, Hist. Chester Co., 239.
[637] Min. Sadsbury Mo. Mtg., 2-22-1792, 106.
[638] Min. Sadsbury Mo. Mtg., 3-21-1792, 107.
[639] Ibid., 5-23-1792, 109.
[640] Ibid., 7-10-1792, 112.
[641] Min. Sadsbury Mo. Mtg., 4-17-1793. 120.
[642] Ibid., 5-13-1793, 121.
[643] Ibid., 9-18-1793, 125.
[644] Ibid., 12-10-1793, 128.
[645] Ibid., 1-7-1798, 175.
[646] Min. Sadsbury Mo. Mtg., 7-19-1797, 168.
[647] Ibid., 4-24-1799, 187.
[648] Bunting, 40, 39, 19 and 42, respectively; also first vols. of
each respective meeting’s records.
[649] Smith, Hist. Del. Co., 138; see also page 41, chapter on
Philadelphia.
[650] Ibid., 139.
[651] Clarkson’s Penn, I, 259; Hazard’s Annals, 695.
[652] Rec. Upland Court, 121; Smith, Hist. Del. Co., 121;
Hazard, Annals, 462.
[653] Would not likely take the case to court.
[654] It appears from a record of sale that the court house was
sold to Robert Wade, 1686. (Record of sale quoted in Jordan,
Hist. Del. Co., I, 112.)
[655] Jordan, Hist. Del. Co., I, 104; Smith, Hist. Del. Co., 137.
[656] Smith, Hist. Del. Co., 166.
[657] Rec. of Chester Mo. Mtg., 1687, I.; Smith, 166.
[658] Smith, 188.
[659] Jordan, II, 441.
[660] Jordan, II, 441.
[661] Ibid.
[662] Ibid.
[663] Min. Chester Mo. Mtg., 1-27-1800.
[664] Jordan, II, 43-45.
[665] Ibid.
[666] The absence of any mention of it in the meeting records.
[667] The writer was unable to find a record of this deed.
[668] No committee reports were noted before that date.
[669] See chapter on Negroes, page 228.
[670] Min. Chester Mo. Mtg., 1-28-1782, 87.
[671] Ibid.
[672] Ibid.
[673] Ibid., 4-29-1782.
[674] Ibid.
[675] Ibid., 7-28-1783, 130.
[676] Ibid.
[677] Min. Chester Mo. Mtg., 4-30-1792, 347.
[678] Ibid., 12-26-1796, 447.
[679] Ibid., 1-27-1800, 508.
[680] Ibid., 5-30-1791, 319.
[681] Min. Chester Mo. Mtg.
[682] Ibid., 9-23-1785, 177.
[683] Min. Chester Q. Meeting, 12-3-1689, 7.
[684] Min. Chester Q. Mtg., 6-14-1732, 128.
[685] Ibid., 9-13-1732, 129.
[686] Ibid., 6-13-1739, 154.
[687] Advices, 250.
[688] Min. Chester Q. Mtg., 5-13-1754, 218.
[689] Smith, Hist. of Del. Co., 166.
[690] Ibid.
[691] Ibid.
[692] Min. Darby Mo. Mtg., 7-7-1692, 54.
[693] Ibid., 9-20-1693, 56.
[694] See Falls p. 87f.; Abington, p. 105ff.; and Buckingham, p.
96f.
[695] Min. Darby Mo. Mtg. 7-5-1758, 441; 7-5-1750, 322.
[696] Ibid., 12-3-1778, 263.
[697] Min. Darby Mo. Mtg.
[698] Ibid.
[699] Ibid., 2-25-1779, 259.
[700] See page 154.
[701] Ibid., 3-1-1781, 319.
[702] Ibid., 3-29-1781, 320.
[703] Ibid., 1-1-1784, 10.
[704] Ibid., 7-29-1784, 22.
[705] Min. Darby Mo. Mtg., 3-29-1787, 68.
[706] Ibid., 11-1-1787, 79.
[707] Ibid., 4-2-1789, 99f.
[708] Min. Darby Mo. Mtg., 1-28-1790, 114. (For entire report
see page 23).
[709] Ibid., 8-2-1792, 157.
[710] Ibid., 11-29-1792, 160.
[711] Ibid., 3-28-1793, 165.
[712] Ibid., 5-2-1793, 166.
[713] Ibid.
[714] Ibid., 7-26-1796, 207.
[715] Min. Darby Mo. Mtg., 8-2-1798, 243.
[716] Jordan, II, 432.
[717] Min. Darby Mo. Mtg. 1739, 258; 7-5-1750, 322.
[718] Ibid., 8-3-1797, 226.
[719] Ibid., 8-2-1798, 243.
[720] Min. Darby Mo. Mtg., 1739, 258. (Other bequests were
made by Blunston and ... the value of which in 1791, amounted to
£97 15/6; the committee reporting thereon, add: “we are united in
opinion it will be best to lay out the money in a building on the
meeting lot and in order thereto have had an estimate made for a
house 16 ft. by 26 ft. from out to out, two stories high with a cellar
under the whole, which amounts to £160 or thereabouts.” A
Committee was appointed to see whether this would be according
to the wish of the donor, Darby Minutes 12-29-1791, 145. In 1792
the committee reported it would be best to build the house for the
master’s accommodation with the money of the legacies, and use
the rents arising therefrom for the schooling of poor children,
Darby Minutes, 2-2-1792, 147.)
[721] Smith, Hist. of Del. County, 347.
[722] Min. Radnor Mo. Mtg., 1-11-1731, 189.
[723] Ibid., 1-11-1757, 300.
[724] Min. Radnor Mo. Mtg., see also page 228, chapter on
Negro education.
[725] Min. Radnor Mo. Mtg., 4-10-1759, 28.
[726] Ibid., 12-8-1768, 220.
[727] Ibid., 1-7-1759, 18.
[728] Advices, 250.
[729] Min. Radnor Mo. Mtg., 8-14-1778, 133.
[730] Min. Radnor Mo. Mtg., 10-13-1778, 139.
[731] Ibid., 7-13-1779, 169.
[732] Ibid., 7-10-1781, 233.
[733] Min. Phila. Q. Mtg., 8-6-1781, 235.
[734] Min. Radnor Mo. Mtg., 9-7-1782, 260.
[735] Ibid., 7-11-1786, 4.
[736] Ibid., 7-13-1790, 8.
[737] Min. Radnor Mo. Mtg., 7-12-1791, 24.
[738] Jordan, II, 429.
[739] Min. Concord Mo. Mtg., 8-4-1779, 94.
[740] Jordan, II, 430.
[741] Min. Concord Mo. Mtg., 8-4-1779, 94.
[742] Ibid., 12-5-1781, 193.
[743] Ibid.
[744] Ibid., 3-3-1784, 275.
[745] Ibid., 8-4-1779, 94.
[746] Ibid., 8-9-1786, 370.
[747] Min. Concord Mo. Mtg., 8-8-1787, 397.
[748] Ibid., 6-5-1782, 213.
[749] Ibid., 8-9-1786, 370; see page 164.
[750] For example, the plan suggested in 1746 and elaborated
in the years following.
[751] Advices, 250.
[752] Advices, 250.
[753] Min. Concord Q. Mtg., 8-12-1754, 218.
[754] Ibid., 8-10-1778, 358.
[755] Ibid., 8-9-1784, 413.
[756] Ibid., 8-12-1793, 477; Min. Warrington and Fairfax Q.
Mtg., 9-20-1784, 175ff.
[757] Phila. Q. Mtg. in the earliest years transacted
considerable detail business, which, years later, it did not touch.
[758] Several definite references are: Min. Middletown Mo.
Mtg., 6-6-1778, 409 and 12-4-1783, 562; Min. Horsham Mo. Mtg.,
II, 12-28-1796.
[759] Min. London Grove Mo. Mtg., 11-4-1795, 78; Min. Darby
Mo. Mtg., 2-3-1791, 133.
[760] To turn to the text of a plan of subscription, see “school
support” in index.
[761] See page 168.
[762] Min. Kennett Mo. Mtg., 12-15-1796, 146.
[763] Ibid., 8-16-1798, 199.
[764] Min. London Grove Mo. Mtg., 11-4-1795, 78.
[765] Min. Darby Mo. Mtg., 2-3-1791, 133.
[766] Min. Sadsbury Mo. Mtg., 12-10-1793, 128.
[767] Min. Buckingham Mo. Mtg., 4-1-1793, 302.
[768] Min. Kennett Mo. Mtg., 12-15-1796, 146.
[769] Min. Phila. Mo. Mtg., 10-26-1701, 316.
[770] To find the text of legacies granted, turn to legacies, in the
index.
[771] Min. Uwchlan Mo. Mtg., 8-3-1763, 22.
[772] Attention is called to the fact that during the years
mentioned in the following table currency greatly depreciated.
This depreciation was most marked in 1779, when, in January,
the ratio was 8 to 1; and in November of the same year 38½ to 1.
See Dewey, D. R., Financial History of U. S., 39; also page 212.
[773] Min. Penn Charter School Overseers, I, 301.
[774] Buckingham Mo. Mtg., 12-7-1778, 194.
[775] Ibid., 4-1-1793, 302.
[776] Min. Wrightstown Mo. Mtg., 12-7-1790, 60.
[777] Min. Falls Mo. Mtg., 11-6-1799, 288.
[778] Min. Uwchlan Mo. Mtg., 2-5-1784, 162.
[779] Min. Horsham School Committee, 3-18-1793.
[780] See page 14ff.
[781] Min. London Yr. Mtg., 3-16-1692, 68.
[782] The yearly meetings also established schools; such was
the case in London Yearly, and Philadelphia followed in 1799 with
the establishment of Westtown Boarding School in Chester
County. Justice cannot be done to that institution in this work. The
reader is referred to Dewes, A History of Westtown Boarding
School.
[783] Min. London Yr. Mtg., 3-17 to 24-1703, 114; 5-26 to 31-
1760, 339.
[784] Min. London Yr. Mtg., 3-16 to 19-1692, 68.
[785] Ibid., 4-2 to 7-1745, 268.
[786] Ibid., 4-9 to 11-1690, 52; 4-1 to 4-1691, 60.
[787] Ibid., 3-13 to 17-1695, 89.
[788] Ibid.
[789] Ibid., 4-2 to 10-1718, 160.
[790] Ibid., 5-31 to 6-5-1773, 399.
[791] Ibid., 3-29 to 4-3-1732, 210; 4-9 to 11-1690, 52.
[792] Min. Phila. Yr. Mtg., 7-16 and 17-1694, 39.
[793] Advices from Burlington and Philadelphia Yr. Mtg., 1746,
1750, 1753, 1755, 1777, and so forth, page 250ff. Also the yearly
meeting minutes records for those years, deposited at 304 Arch
Street, Phila. (The first reference is the more accessible.)
[794] The reader is referred to the account of establishing
schools in Bucks, Montgomery, Delaware Counties, etc.
[795] These references are, respectively, to the five points
stated below:
a. Min. Westland Mo. Mtg., 11-11-1786, 12; 3-10-1787, 19.
b. Min. Horsham Mo. Mtg., 4-28-1784.
c. Min. Phila. Mo. Mtg., 11-29-1719, 57.
d. Min. Kennett Mo. Mtg., 12-15-1796, 146.
e. Min. Chester Mo. Mtg., 1-27-1800, 508; Min. Concord Mo.
Mtg., 8-9-1786, 370.
[796] See the Advices, 250; or the Book of Discipline which
has, under the head of schools, a statement of the various
recommendations of the yearly meetings. See also Yearly
Meeting Minute Books at 4th and Arch Streets, Phila., for years
1746, 1753, 1755, 1777, and 1778.
[797] Min. Phila. Mo. Mtg., 2-29-1698, 229; P. C. S. M., I, 13.
[798] Deed No. 33, mentioned in P. C. S. M., I, 13.
[799] Ibid., 40.
[800] Ibid., 147.
[801] Friends’ Intelligencer, 8-15-1896, 539; Min. Abington Mo.
Mtg., 1-26-1722, 124.
[802] Min. Warrington and Fairfax Q. Mtg., 9-20-1779, 73.
[803] Ibid., 77; Warrington Mo. Mtg., 8-7-1779, 46.
[804] Deed No. 88 New Garden Township, Chester County.
(The original is in Orthodox Friends Meeting House, West Grove,
Pa.)
[805] Min. New Garden Mo. Mtg., 8-6-1785, 256.
[806] Min. Kennett Mo. Mtg., 1-12-1792, 14.
[807] Min. Goshen Mo. Mtg., 4-10-1795.
[808] Ibid., 3-8-1782.
[809] Min. Darby Mo. Mtg., 3-28-1793, 165.
[810] Min. Buckingham Mo. Mtg., 4-10-1794, 314.
[811] Jenkins, Historical Col. of Gwynedd, 396.
[812] Ibid.
[813] Min. Middletown Mo. Mtg., 12-1-1693-4, 64.
[814] Ibid., 1-1-1699, 114.
[815] Min. Phila. Mo. Mtg., 5-25-1740, 318.
[816] In 1701 they had begun a school house which was to be
60 by 24 feet. Min. Phila. Mo. Mtg., 4-27-1701, 298.
[817] The schoolroom described is in Merion Meeting House,
which may be reached from Philadelphia via P.R.R. to Narberth,
Pa.; from thence a ten-minute walk.
[818] Min. Goshen Mo. Mtg., 3-8-1782.
[819] Min. Falls Mo. Mtg., 12-3-1794, 169; for value of money
see page 212.
[820] Ibid., 9-4-1799, 283.
[821] Min. Phila. Mo. Mtg., 4-27-1701, 298.
[822] Ibid., 11-25-1744, 379; P. C. S. M., I, 40. Parts of the
school buildings were at times used as tenant property thus
affording a supporting income, P. C. S. M., I, 22.
[823] P. C. S. M., I, 56.
[824] Ibid., I, 39.
[825] Min. Phila. Mo. Mtg., 9-25-1715, 10ff.
[826] P. C. S. M., I, 95 and 37.
[827] Min. Bradford Mo. Mtg., 6-18-1762; 4-7-1767; 8-14-1767.
[828] P. C. S. M., I, 29 and 25.
[829] Ibid., 31.
[830] Ibid., 95.
[831] Ibid., 37.
[832] P. C. S. M., 72.
[833] Ibid., 151ff.
[834] Ibid.
[835] Min. Phila. Mo. Mtg., 1-30-1784, 123ff.
[836] P. C. S. M., I, 76 and 79; also I, 198.
[837] P. C. S. M., see list of scholars; number is approximate.
[838] Pemberton Mss., Vol. 3, p. 2.
[839] P. C. S. M., I, 102f. (Rules adopted in 1748.)
[840] Robert Proud Mss. Collection, No. 20, pp. 3-7. The rules,
he states, were drawn up for his use in the school in 1780.
[841] The rules presented, taken from records of the Overseers
of the Schools in Philadelphia, are quite like those later drawn up
by Horsham School Committee. There is nothing additional in the
later ones and they were doubtless patterned after them.
(Horsham Sch. Com. Min., 1-27-1783).
[842] Robert Proud Mss., No. 156, 45.
[843] Logan Mss. Letter for 4th month, 12th, 1704. Vol. I, 49. (J.
Dickinson was away on a voyage of some length.)
[844] Vaux, Memoirs of Benezet, 15f.
[845] Watson, Annals, I, 291-2.
[846] See page 181.
[847] P. C. S. M., I, 137.
[848] Ibid., 150.
[849] Min. Horsham Sch. Com., 3-16-1792.
[850] See page 78.
[851] Page 78.
[852] See list of printed rules for the school in custody of P.C.S.
[853] Min. Horsham Sch. Com., 1-27-1783 (also mentioned in
the monthly meeting minutes very frequently).
[854] See page 78f.
[855] P.C.S.M., I, 84.
[856] Pa. Gazette, No. 1449, 1756.
[857] Ibid., No. 824, 1744.
[858] Pa. Pocket and Daily Advertiser, No. 2385, 1786.
[859] Ibid., No. 2386, 1786.
[860] A list of printed rules issued by the Board, found in the
depository for the P.C.S.M., in the Provident Life and Trust
Building, Phila.
[861] Darby Meeting employed B. Clift to teach a whole year
with the exception of two weeks. (Darby Min., 7-7-1692, 54).
[862] Ibid.
[863] See page 183f.
[864] Min. Phila. Mo. Mtg., 1-30-1784, 123ff.
[865] P. C. S. M., I, 117.
[866] Min. Phila. Mo. Mtg., 1-30-1784, 123ff.
[867] Some copies and volumes of these illustrious news
sheets are found in the Norris Ms. Collection.
[868] Norris Ms. Collection—The Student’s Magazine. The little
volumes are unpaged; page references are impossible.
[869] Norris Ms. Collection.
[870] Ibid.
[871] P. C. S. M., I, 135.
[872] Phila. Mo. Min., 1-25-1771, 430.
[873] London Yr. Mtg. Min., 4-2 to 10-1718, 160. Phila. Advices
XXX, page 250 (for years from 1746-1778). Also a copy of the
Discipline containing the digested recommendations on schools,
p. 386ff. (In first National Bank, Newtown, Pa.).
[874] Col. Rec., I, LXVI.
[875] Extracts from London Yr. Mtg. Min., pub. 1802, 124.
[876] Crouch, Collection of His Papers, 183.
[877] Col. Rec., I, 36.
[878] P. C. S. M., I, 33.
[879] P. C. S. M., 14.
[880] Ibid., 90.
[881] Ibid., 117.
[882] Ibid., 145.
[883] Ibid., 221.
[884] A letter written to John Penn, Penn Ms. Collections, I,
233.
[885] Min. Phila. Mo. Mtg., 7-30-1779, 151; 1-30-1784, 123ff.
Also, Min. Horsham Sch. Com., 1-27-1783; Min. Horsham Prep.
Mtg., 1-24-1783, and Min. Darby Mo. Mtg., 2-28-1793, 165, give
some of the books which were used in the schools.
[886] P. C. S. M., I, 138.
[887] Hildeburn, II, 332.
[888] Ibid., I, 39.
[889] Pa. Gaz., No. 1245, 1752.
[890] Ibid., No. 1499, 1757.
[891] Ibid., No. 1861, 1764.
[892] Ibid., No. 1556, 1758.
[893] Min. Phila. Mo. Mtg., 3-30-1770, 370.
[894] P. C. S. M., I, 138.
[895] Min. Darby Mo. Mtg., 2-28-1793, 165.
[896] Min. Horsham Sch. Com., 1-11-1793.
[897] Min. Sadsbury Mo. Mtg., 2-20-1793, 118.
[898] Min. Byberry Prep. Mtg., 12-26-1792.
[899] Ibid., 8-26-1789.
[900] Min. Radnor Mo. Mtg., 5-8-1789, 55.
[901] Min. Sadsbury Mo. Mtg., 6-17-1789, II, 70.
[902] Hildeburn, I, 39 (published in London 1697).
[903] Ibid., II, 100.
[904] Prowell, I, 540.
[905] In 1689 Phila. Mo. Mtg. authorized W. Bradford to print
certain of G. Fox’s papers. These are not named and it hardly
seems probable that Fox’s Primmer was in the list. Bradford’s
request for permission (Genealogical Publications, II, 139), H. S.
P.
[906] Min. Phila. Mo. Mtg., 12-25-1697-8, p. 227 (G. S. P. P.)
[907] Hildeburn, I, 38.
[908] Smith, Supplement to Catalogue of Friends Books, 262.
[909] Min. Phila. Mo. Mtg., 11-29-1696-7, 211. (G. S. P. P., Vol.
4).
[910] Pastorius’s Common Place Book (Mss.) H. S. P.
[911] The Primer of Stephen Crisp is also mentioned frequently
with that of Fox, as being used in the schools. (Min. Abington Mo.
Mtg., 8-27-1735, 207).
[912] Hildeburn, II, 21, 114, 341, 340, and 343, respectively.
[913] Hildeburn, I, 318.
[914] P. C. S. M., I, 240.
[915] Prowell, I, 541.
[916] See page 191.
[917] Chiefly in the Norris Mss. Collections.
[918] A scale, having units of known value, which is used in
measuring accomplishment in handwriting.
[919] Hildeburn, II, 164.
[920] Prowell, I, 540.
[921] Elihu Underwood was teacher at Warrington in York
County in 1784 (See Warrington Mo. Mtg. Min., 1-10-1784, 47.)
[922] Norris Ms. Collection, H. S. P.
[923] P. C. S. M., I, 64.
[924] Ibid., 26; also Min. Phila. Mo. Mtg., 7-30-1779, 151.
[925] In 1741 Buller advertised the teaching of writing,
arithmetic, merchants’ accounts, navigation, algebra, and other
parts of the mathematics to be taught at the “Public School.” (Pa.
Gaz. No. 673, 1741).
[926] Ibid., 84.
[927] Ibid., 101.
[928] Ibid., 122.
[929] Ibid., 131.
[930] Ibid., 133.
[931] Min. Phila. Mo. Mtg., 1-30-1784, 123ff.
[932] Ibid., 7-30-1779, 151.
[933] P. C. S. M., I, 33.
[934] Ibid., 14.
[935] Alexander Seaton, who came to the English School about
1754 (P. C. S. M. I, 117) had been teaching a school of the same
nature in the upper part of the city, in which he taught
mathematics. That school was also under the direction of the
Board. (P. C. S. M., I, 90).
[936] Ibid., 80.
[937] Ibid., 104f.
[938] Ibid.
[939] A list of the rules for the government of the schools,
printed, in the P. C. S. depository.
[940] See page 189.
[941] Hildeburn, II, 266.
[942] Ibid., 464.
[943] P. C. S. M., I, 235.
[944] See page 57.
[945] Pa. Gaz., Apr. 16, 1730.
[946] Hildeburn, II, 342.
[947] Pastorius, Common Place Book (Mss.) H. S. P.
[948] Books of Charles and Isaac Norris in Norris Ms.
Collection.
[949] Books chiefly of Norris, I. Griffiths, and King, in the Norris
Ms. Collection.
[950] P. C. S. M., I, 104f.
[951] See page 195.
[952] See Norris Ms. Collection, H. S. P.
[953] P. C. S. M., I, 239.
[954] Ibid., 75.
[955] For instance, F. D. Pastorius, Anthony Benezet, Robert
Proud, Christopher Taylor, and many others.
[956] Min. London Yr. Mtg., 4-9 to 11-1690, 52; 4-1 to 4-1691,
60; 3-13 to 17-1695, 89; also collected Advices of Philadelphia
and Burlington Yr. Mtg., 250ff.
[957] Min. Byberry Prep. Mtg., 2-22-1786.
[958] Min. Goshen Mo. Mtg., 7-6-1792; Min. Kennett Mo. Mtg.,
5-12-1785, 814; Min. Radnor Mo. Mtg., 7-11-1786, 4; Min.
Uwchlan Mo. Mtg., 12-5-1782, 136; 11-7-1782, 132.
[959] Deed No. 88, New Garden, Tp., Chester Co. (In Fireproof
of Orthodox Friends in West Grove, Pa.).
[960] Min. Goshen Mo. Mtg., 8-11-1797; Min. Ken. Mo. Mtg., 3-
14-1793, 39.
[961] Min. Goshen Mtg., 8-5-1796.
[962] P. C. S. M., 1, 3, 33, and 90; Min. Darby Mo. Mtg., 7-17-
1692, 54; Min. Phila. Mo. Mtg., 1-29-1700, 254; 4-24-1720, 63.
[963] Col. Rec. I, 36.
[964] Min. Phila. Mo. Mtg., 6-26-1784, 64.
[965] P. C. S. M., I, 58.
[966] Ibid., 5f.
[967] Ibid., 175.
[968] Ibid., 208.
[969] Ibid., 139.
[970] Ibid., 141.
[971] Ibid., 265.
[972] P. C. S. M., I, 237.
[973] Ibid., 245.
[974] Ibid., 116.
[975] See Yearly Meetings’ Advices, 250.
[976] Min. Darby Mo. Mtg., 7-7-1692, 54; 9-20-1693, 56.
[977] 2 Pa. Arch. XIX, 248.
[978] Bean, 680.
[979] There is found no record of his removal by letter, though
he may have done so without, which, however, was not according
to practice.
[980] Min. Phila. Mo. Mtg., 5-26-1689, 154.
[981] Ibid., 3-29-1691, 146.
[982] Weekly Mercury, Nov. 29, 1733.
[983] Min. Phila. Mo. Mtg., 11-28-1697, 227.
[984] Ibid., 1-29-1700, 254.
[985] P. C. S. M., I, 64.
[986] Ibid., 101.
[987] Ibid., 90.
[988] Ibid., 266.
[989] Ibid., 175.
[990] Ibid., 334.
[991] Min. Phila. Mo. Mtg., 1-30-1784, 123.
[992] P. C. S. M., I, 33.
[993] Simpson’s Lives of Eminent Philadelphians, 53. Min.
Phila. Mo. Mtg., 1-30-1784, 128.
[994] Ibid., 1-31-1699, 244.
[995] Ibid., 1-27-1702, 326.
[996] P. C. S. M., I, 126.
[997] Ibid., 221.
[998] P. C. S. M., I, 130.
[999] Ibid., 161.
[1000] Ibid., 158.
[1001] Min. Darby Mo. Mtg., 7-7-1692, 54.
[1002] P. C. S. M., I, 133.
[1003] Ibid., 274.
[1004] Ibid., 131.
[1005] P. C. S. M., I., 123.
[1006] Ibid., 131.
[1007] Min. Phila. Mo. Mtg., 5-26-1689.
[1008] In the references at the right hand margin of the table
“Ph” refers to Minutes of Philadelphia Monthly Meeting for the
date given; Darby refers to Minutes of Darby Monthly Meeting.
[1009] Futhey and Cope, 308.
[1010] From an old account book in possession of Albert Cook
Myers, Moylan, Pa.
[1011] Dewey, D. R., Financial History of the U. S., 39.
The reader is reminded of the fact that because of greatly
depreciated currency the amounts paid, as shown in the above
table, did not represent so much absolute increase. That some
exact idea of the extent of depreciation of the continental currency
may be gained, there is given the following table for the year
1779, when the depreciation became most marked.

Jan. 14, 1779 8 to 1


Feb. 3 10 to 1
Apr. 2 17 to 1
May 5 24 to 1
June 4 20 to 1
Sept. 17 24 to 1
Oct. 14 30 to 1
Nov. 17 38½ to 1

The fact of such depreciation was not officially recognized by


Congress until March 18, 1780, it being then provided that paper
be accepted for silver at a ratio of 40 to 1.
[1012] See page 20.
[1013] Min. London Grove Mtg., 3-4-1795, 62.
[1014] Ibid., 1-31-1699, 244.
[1015] Ibid., 1-27-1702, 326.
[1016] P. C. S. M., I, 130.
[1017] Ibid., 158.

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