P h y s ic s 1 , 2 2 (2 0 0 8 )

V ie w p o in t
H o w c o llo id a l d is p e rs io n s re la x u n d e r s tre s s
B y N o rm a n J. W a g n e r
D e p a r tm e n t o f C h e m ic a l E n g in e e r in g , U n iv e r s ity o f D e la w a r e , N e w a r k , D E 1 9 7 1 6

P u b lis h e d S e p te m b e r 2 2 , 2 0 0 8
A s h e a r fo r c e c a n m e lt a c o llo id a l g la s s , c a u s in g it to o w in a h ig h ly n o n lin e a r fa s h io n . P h y s ic is ts h a v e n o w fo u n d a w a y to p u t th e d e s c r ip tio n o f th is ty p e o f o w o n a m o r e fo r m a l th e o r e tic a l fo o tin g .

S u b je c t A r e a s : S o f t M a t t e r A V F irs J. M P h y ie w t-P . B s. R p o in rin c ip ra d e r, ev . L e t o le M tt. n : s C o n s titu tiv e E q u a tio n fo r S u s p e n s io n R h e o lo g y . E . C a te s a n d M . F u c h s 1 0 1 , 1 3 8 3 0 1 (2 0 0 8 ) P u b lis h e d S e p te m b e r 2 2 , 2 0 0 8

O f th e m a n y p h y s ic a l s y s te m s th a t w e c a n s tu d y , c o llo id s a n d c o llo id d is p e r s io n s m a y w e ll b e o n e o f th e m o s t p re v a le n t in o u r d a ily liv e s . In k s , p a in ts , c la y s , e m u ls io n s , a n d m ilk , a s w e ll a s s u r fa c ta n t a g g re g a te s (m ic e lle s ) a n d n a n o p a r tic le s u s p e n s io n s a re a ll c o llo id d is p e r s io n s . T h e s tu d y o f h o w th e s e d is p e r s io n s a n d o th e r c o m p le x liq u id s o w a e ld c a lle d rh e o lo g y is e s s e n tia lly a p ro b le m o f n o n e q u ilib r iu m s ta tis tic a l m e c h a n ic s th a t m u s t a c c o u n t fo r m a n y -b o d y in te r a c tio n s . T h e re s p o n s e o f c o llo id d is p e r s io n s to a s h e a r fo rc e is o fte n n o n lin e a r a n d c a n re s u lt in in te re s tin g p h y s ic a l p h e n o m e n a . T h e a p p lic a tio n o f a s h e a r in g fo rc e , fo r e x a m p le , c a n in c re a s e th e v is c o s ity o f a d is p e r s io n , a n e ffe c t th a t c a n b e h a r n e s s e d to m a k e p e r s o n a l p ro te c tiv e d e v ic e s [1 ]. P re d ic tin g h o w a c o llo id d is p e r s io n re s p o n d s to a n e x te r n a l s tre s s a n d c o n n e c tin g th is re la tio n s h ip to th e m ic ro s c o p ic in te r a c tio n s b e tw e e n th e d is p e r s e d p a r tic le s is a k e y g o a l o f th e o re tic a l rh e o lo g y . W r itin g in P h y s ic a l R e v ie w L e tte r s , Jo s e p h B r a d e r a n d M a tth ia s F u c h s o f th e U n iv e r s it t K o n s ta n z in G e r m a n y a n d M ic h a e l C a te s o f T h e U n iv e r s ity o f E d in b u rg h re p o r t th e d e v e lo p m e n t o f a rh e o lo g ic a l c o n s titu tiv e e q u a tio n fo r d e n s e c o llo id a l s u s p e n s io n s a n d g la s s e s [2 ] (h e re , c o n s titu tiv e re fe r s to th e s tre s s -re s p o n s e re la tio n s h ip ). T h e w o r k lin k s a h ig h ly s u c c e s s fu l m ic ro s c o p ic th e o r y , w h ic h d e s c r ib e s h o w c o llo id a l p a r tic le s b e c o m e a r re s te d a t th e g la s s tr a n s itio n o f a c o llo id , to a fo r m a l d e s c r ip tio n o f s u s p e n s io n rh e o lo g y . A lth o u g h th is is n o t th e r s t e ffo r t in th is d ir e c tio n [3 ], th e p a p e r b y B r a d e r e t a l. is a n im p o r ta n t c o n tr ib u tio n b e c a u s e it a p p lie s to b o th c o llo id a l d is p e r s io n a n d g la s s e s , c a n d e s c r ib e th e re s p o n s e fo r n o n lin e a r, a r b itr a r y d e fo r m a tio n e ld s , a n d s a tis e s th e c r ite r io n th a t th e s tre s s e s s h o u ld b e in v a r ia n t fo r d iffe re n t re fe re n c e fra m e s . T h e th e o r y o f th e o w o f c o llo id a l d is p e r s io n u n d e r s h e a r h a s a r ic h h is to r y th a t s p a n s o v e r a c e n tu r y . T h e e ld re a lly b e g in s w ith th e s e m in a l w o r k o f E in D O I: 1 0 . 1 1 0 3 / P h y s i c s . 1 . 2 2 U R L : h t t p : / / l i n k . a p s . o r g / d o i / 1 0 . 1 1 0 3 / P h y s i c s . 1 . 2 2

s te in in 1 9 0 6 [4 , 5 ], in w h ic h h e s tu d ie d h o w s in g le p a r tic le m o tio n c o n tr ib u te s to th e v is c o s ity o f a s u s p e n s io n . A ro u n d th e s a m e tim e , S m o lu c h o w s k i d e v e lo p e d a s ta tis tic a l d e s c r ip tio n o f B ro w n ia n m o tio n o f c o llo id a l p a r tic le s [6 ]. In th e e a r ly 1 9 7 0 s , B a tc h e lo r fo r m u la te d th e s tre s s te n s o r a m a tr ix w h o s e c o m p o n e n ts d e s c r ib e th e fo rc e s a c tin g o n th e m a te r ia l in a ll th re e s p a tia l c o o rd in a te s fo r b o th h y d ro d y n a m ic (th a t is , m e d ia te d b y th e u id b e tw e e n th e p a r tic le s ) a n d c o n s e r v e d in te ra c tio n s [7 9 ]. T h e p a s t th ir ty y e a r s o f th e o re tic a l d e v e lo p m e n t h a v e la rg e ly fo c u s e d o n h a n d lin g th e fa c t th a t a c o n c e n tr a te d c o llo id d is p e r s io n is a m a n y -b o d y p ro b le m , th o u g h th e c h a lle n g e o f m a n y -b o d y h y d ro d y n a m ic in te r a c tio n s is , in p r a c tic e , la rg e ly re s o lv e d [1 0 1 2 ]. W ith a d v a n c e d s im u la tio n m e th o d s , it is p o s s ib le to o b ta in a c c u r a te s o lu tio n s fo r s u f c ie n tly la rg e e n s e m b le s o f p a r tic le s [1 3 , 1 4 ], e v e n if a n a ly tic a l c a lc u la tio n s a re in tr a c ta b le fo r a ll b u t re g u la r a r r a y s . O n e w a y th a t m a n y -b o d y in te r a c tio n s a ffe c t p a r tic le d y n a m ic s is th ro u g h e x c lu d e d v o lu m e e ffe c ts th a t re s u lt fro m th e n ite s iz e o f th e d is p e r s e d p a r tic le s (s e e F ig 1 , le ft p a n e l). In a s u f c ie n tly d e n s e s u s p e n s io n o f h a rd s p h e re s , th e s e e ffe c ts c a n le a d to th e fo r m a tio n o f a c o llo id a l g la s s , a k in e tic tr a n s itio n c h a r a c te r iz e d b y d y n a m ic a l a r re s t o f th e p a r tic le m o tio n [1 5 ]. H o w e v e r, w h e n th e o r ie s th a t a re b a s e d o n o n ly p a ir-w is e in te r a c tio n s b e tw e e n p a r tic le s (r a th e r th a n a m a n y -b o d y p ic tu re ) a re e x te n d e d to c o n c e n tr a te d d is p e r s io n s , th e y d o n o t c a p tu re th is d iv e rg e n c e in th e v is c o s ity a t th e id e a l g la s s tr a n s itio n , b u t a t m u c h h ig h e r c o n c e n tr a tio n s [1 6 , 1 7 ]. A p ro m is in g a p p ro a c h fo r d e s c r ib in g c o llo id a l d y n a m ic s ju s t a b o v e a n d b e lo w t h e c o llo id a l g la s s t r a n s itio n h a s p ro v e n to b e m o d e -c o u p lin g th e o r y (M C T ). T h is th e o r y is a n a n s a tz p ro p o s e d to h a n d le h ig h ly c o rre la te d s y s te m s a n d c a n th e re fo re a c c o u n t fo r th e p a rtic le c a g in g s h o w n in th e le ft p a n e l o f F ig . 1 . T h e re la x a tio n m o d e s o f th e te s t p a r tic le (th e re d p a r tic le ) a re c 2 0 0 8 A m e r ic a n P h y s ic a l S o c ie ty

P h y s ic s 1 , 2 2 (2 0 0 8 )
m a n y -b o d y d ire c t c o r re la tio n fu n c tio n re d u c e s b a c k to th e p a ir p o te n tia l). D iffe re n c e s s h o u ld a r is e fo r s tro n g ly c o r re la te d s y s te m s a n d th e y c a n n o w b e r ig o ro u s ly te s te d a g a in s t s im u la tio n s a n d e x p e r im e n ta l m e a s u re m e n ts . It a ls o re m a in s to fo r m a lly d e te r m in e if th e s tr e s s te n s o r a n d d y n a m ic a l e q u a tio n th a t B r a d e r e t a l. h a v e c a lc u la te d fo r th e n o n e q u ilib r iu m m ic ro s tr u c tu re a re th e r m o d y n a m ic a lly c o n s is te n t [2 6 ]. A fu r th e r c h a lle n g e fo r th e th e o r y w ill b e to re p ro d u c e e x p e r im e n ta l m e a s u re m e n ts o f th e d iv e rg e n c e in th e v is c o s ity fo r h a rd -s p h e re d is p e r s io n s [2 7 ]. T h e s e d is p e rs io n s h a v e a la r g e , b u t n ite v is c o s ity fo r v o lu m e fr a c tio n s a b o v e th e id e a l g la s s tr a n s itio n , s u g g e s tin g th a t p a r tic le m o tio n is a c tiv a te d in a w a y th a t is n o t c a p tu re d b y M C T [2 8 ]. F in a lly , it w ill a t s o m e p o in t b e n e c e s s a r y to in c lu d e in th e th e o r y th e e ffe c ts o f h y d ro d y n a m ic in te r a c tio n s , w h ic h a re m o re s ig n i c a n t in s tro n g ly s h e a rin g o r d e fo r m in g d is p e r s io n s . T h e p h a s e b e h a v io r a n d d y n a m ic s o f c o llo id a l d is p e rs io n s w ith a ttr a c tiv e in te r a c tio n s a re a c u r re n t to p ic o f g re a t s c ie n ti c in te re s t b u t o f e v e n g re a te r im p o r ta n c e in te c h n o lo g ic a l p r a c tic e [2 9 ]. T h e re c e n t s u c c e s s e s o f M C T in d e s c r ib in g th e a ttr a c tiv e d r iv e n g la s s tr a n s itio n in c o llo id a l d is p e r s io n s [3 0 3 3 ] o r th e fo r m a tio n o f a c o llo id a l g e l [3 4 ] s u g g e s t th a t th e n e w fo r m a lis m p re s e n te d h e re m ig h t le a d to a c c u r a te rh e o lo g ic a l c o n s titu tiv e e q u a tio n s fo r th e s e s y s te m s , to o . F u r th e r, w ith th e fo r m a lis m d e v e lo p e d b y B r a d e r e t a l. it m a y b e p o s s ib le to d e s c r ib e tim e -d e p e n d e n t v is c o s itie s th a t o c c u r in u id s e x p o s e d t o c h a n g in g s h e a r ( i.e ., t h ix o t r o p y ) [ 3 5 , 3 6 ] a s w e ll a s a g e in g e ffe c ts [3 7 ]. T h u s , th is th e o re tic a l a d v a n c e o p e n s n u m e ro u s o p p o r tu n itie s fo r fu r th e r e x p lo r a tio n s o f th e r ic h b e h a v io r o f c o n c e n tr a te d c o llo id a l d is p e r s io n s .

F IG . 1 : T h e c a r to o n a t le ft s h o w s h o w th e m o tio n o f p a rtic le s c a n b e c o m e a r re s te d in a c o llo id a l d is p e r s io n . T h e c a g in g m e c h a n is m o c c u r s in c o n c e n tr a te d d is p e r s io n s : a re fe re n c e p a r tic le (re d ) is h in d e re d fro m m o v in g b y e x c lu d e d v o lu m e in te r a c tio n s w ith its n e ig h b o r s (b lu e ), th a t a re in tu r n a re h in d e re d b y th e ir n e ig h b o r s (g re y ). C a g in g e ffe c ts c a n m a k e th e re s p o n s e o f th e c o llo id a l d is p e r s io n to a tim e v a r y in g s h e a r fo rc e ( ) h ig h ly n o n lin e a r. T h e im a g e o n th e r ig h t s h o w s a s im u la tio n o f h o w th e m ic ro s tr u c tu re is d is to r te d in th e p la n e o f s h e a r fo r a c o n c e n tr a te d h a rd s p h e re d is p e rs io n u n d e r s h e a r o w a t a re la tiv e ly m o d e r a te s h e a r r a te (s e e [1 1 ]) [C o u r te s y o f J. F . B r a d y , C a lT e c h ] (Illu s tr a tio n : A la n S to n e b ra k e r/ s t o n e b r a k e r d e s i g n w o r k s . c o m )

fo r m a lly c o u p le d to th o s e o f th e n e ig h b o r s (b lu e ) c o m p r is in g th e c a g e , w h ic h th e m s e lv e s a re c a g e d b y th e ir n e ig h b o r s (g r e y ), a d in n itu m . In d e e d , M C T h a s b e e n s h o w n to a c c u r a te ly m o d e l th e d iffu s io n o f p a r tic le s , a t e q u ilib r iu m , a n d th e v is c o e la s tic ity fo r c h a rg e d s p h e re d is p e r s io n s w h e re h y d ro d y n a m ic in te r a c tio n s a re n o t d o m in a n t [3 , 1 8 2 0 ] T h e th e o r y a ls o p ro v id e s a q u a lita tiv e fr a m e w o r k fo r u n d e r s ta n d in g th e lin k a g e b e tw e e n v is c o e la s tic ity a n d p a r tic le c a g in g in h a rd -s p h e re d is p e r s io n s [2 1 , 2 2 ]. In th e ir n e w w o r k , B r a d e r, C a te s , a n d F u c h s p u t th e ir e a r lie r a n s a tz e x te n d in g M C T fo r c o llo id a l s u s p e n s io n s to n o n lin e a r s h e a r d e fo r m a tio n s o n a m o re fo r m a l fo o tin g . A s ig n i c a n t a d v a n ta g e o f th e ir a p p ro a c h is th a t th e y fo ld th e s u c c e s s fu l M C T d e s c r ip tio n o f p a r tic le d y n a m ic s in to a g e n e r a liz e d fo r m u la tio n o f th e s tre s s te n s o r (in p a r tic u la r, th e y u s e th e G re e n -K u b o fo r m a lis m [3 ]). T h e ir id e n ti c a tio n o f th e fu ll te n s o r ia l s tr u c tu re o f th e th e o r y m e a n s it is n o t re s tr ic te d to s im p le s h e a r d e fo r m a tio n . T o illu s tr a te th e ir a p p r o a c h , B r a d e r e t a l. c o n s id e r a h a rd -s p h e re c o llo id a l g la s s a n d c a lc u la te th e d y n a m ic y ie ld s t r e s s , i.e ., t h e f o r c e r e q u ir e d t o m e lt t h e g la s s a n d c a u s e th e d is p e r s io n to o w , u n d e r s h e a r a s w e ll a s u n ia x ia l a n d p la n a r e x te n s io n o w s . T h e th e o r y p re d ic ts w h a t h a p p e n s to th e m ic ro s tr u c tu re o f a c o llo id a l s u s p e n s io n u n d e r a n a p p lie d d e fo rm a tio n (a n e x a m p le o f th is s o r t o f c a lc u la tio n is s h o w n in th e r ig h t p a n e l o f F ig . 1 ). T h e re s u lts c o u ld b e d ire c tly c o m p a re d w ith n e u tro n s c a tte r in g m e a s u re m e n ts o f th e d e n s ity d is tr ib u tio n in th e c o llo id a l s u s p e n s io n u n d e r s h e a r o w [2 3 ], a s w e ll a s a g a in s t m e a s u re m e n ts o f th e v is c o e la s tic p ro p e r tie s [2 4 ]. T h e c a lc u la te d s tre s s te n s o r a g re e s w ith p re v io u s e x a c t d e r iv a tio n s b a s e d o n m ic r o m e c h a n ic s [ 2 5 ] in t h e d ilu t e lim it ( i.e ., w h e n t h e
D O I: 1 0 . 1 1 0 3 / P h y s i c s . 1 . 2 2 U R L : h t t p : / / l i n k . a p s . o r g / d o i / 1 0 . 1 1 0 3 / P h y s i c s . 1 . 2 2

R e fe re n c e s
[1 ] M p [2 ] J 1 [3 ] G [4 ] A [5 ] A [6 ] M [7 ] G [8 ] G [9 ] G 1 0 ] B B 1 1 ] D 1 2 ] A 1 3 ] A 1 4 ] A 1 1 5 ] W 1 6 ] J 1 7 ] J 1 8 ] A 3 [ [ [ [ [ [ [ [ [ . D e c k e r, C . H a lb a c h , C . N a m , N . W a g n e r, a n d E . W e tz e l, C o o s ite s S c ie n c e a n d T e c h n o lo g y 6 7 , 5 6 5 (2 0 0 7 ). . M . B ra d e r, M . E . C a te s , a n d M . F u c h s , P h y s. R ev . L ett. 1 3 8 3 0 1 (2 0 0 8 ). . N g e le a n d J. B e rg e n h o ltz , J. C h e m . P h y s . 1 0 8 , 9 8 9 3 (1 9 9 8 ). . E in s te in , A n n . P h y s . 3 2 4 , 2 8 9 (1 9 0 6 ). . E in s te in , A n n . P h y s . 3 3 9 , 5 9 1 (1 9 1 1 ). . v o n S m o lu c h o w s k i, A n n . P h y s . 3 2 6 , 7 5 6 (1 9 0 6 ). . K . B a tc h e lo r, J. F lu id M e c h . 4 1 , 5 4 5 (1 9 7 0 ). . K . B a tc h e lo r a n d J. T . G r e e n , J. F lu id M e c h . 5 6 , 4 0 1 (1 9 7 2 ). . K . B a tc h e lo r a n d J. T . G r e e n , J. F lu id M e c h . 5 6 , 3 7 5 (1 9 7 2 ). . C ic h o c k i, B . U . F e ld e r h o f , K . H in s e n , E . W a jn r y b , a n d a w z d z ie w ic z , J. C h e m . P h y s . 1 0 0 , 3 7 8 0 (1 9 9 4 ). R . F o s s a n d J. F . B r a d y , J. F lu id M e c h . 4 0 7 , 1 6 7 . . S ie r o u a n d J. F . B r a d y , J. R h e o l. 4 6 , 1 0 3 1 (2 0 0 2 ). . J. B a n c h io a n d J. F . B r a d y , J. C h e m . P h y s . 1 1 8 , 1 0 3 2 3 (2 0 0 3 ). . J. C . L a d d a n d R . V e r b e r g , Jo u r n a l o f S ta tis tic a l P h y s ic s 1 1 9 1 . . v a n M e g e n a n d P . N . P u s e y , P h y s. R ev . A 4 3 , 5 4 2 9 (1 9 9 1 ). . F . B ra d y , J. C h em . P h y s. 9 9 , 5 6 7 (1 9 9 3 ). . F . B ra d y , J. C h em . P h y s. 9 8 , 3 3 3 5 (1 9 9 3 ). . J. B a n c h io , G . N g e le , a n d J. B e rg e n h o ltz , J. C h e m . P h y s . 1 3 8 1 (2 0 0 0 ). m 0 1 ,

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c 2 0 0 8 A m e r ic a n P h y s ic a l S o c ie ty

P h y s ic s 1 , 2 2 (2 0 0 8 )
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[2 8 [2 9 [3 0 [3 1 [3 2 [3 3 [3 4 [3 5 [3 6 [3 7

iz e r, P h y s . R e v . E 7 7 , 0 5 1 5 0 4 (2 0 0 8 ). M a t. 1 9 , 3 , A . B . S c 0 0 8 ). h y s. R ev . . P h y s. C o n d M . F u . B o n n , S e o l. 4 9 , 1 2 . P ia u , J. 2 3 1 0 1 (2 0 0 7 ). h o e ld , F . S c io r tin o , a n d E 5 9 , 5 7 0 6 (1 9 n d en s. M a t. 1 1 c h s , L a n g m u ir o ft M a tte r 2 , 2 1 3 (2 0 0 5 ). R h e o l. 4 2 , 1 3 4 9 9 ). , 1 0 1 7 1 . 1 9 , 4 4 9 3 . 7 4 (2 0 0 6 ). 9 (1 9 9 8 ).

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