diff --git "a/dev.txt" "b/dev.txt"
new file mode 100644--- /dev/null
+++ "b/dev.txt"
@@ -0,0 +1,11308 @@
+Complex	B-Process
+Langevin	I-Process
+(	O
+CL	B-Process
+)	O
+dynamics	O
+[	O
+1,2	O
+]	O
+provides	O
+an	O
+approach	O
+to	O
+circumvent	O
+the	O
+sign	B-Task
+problem	I-Task
+in	O
+numerical	B-Process
+simulations	I-Process
+of	I-Process
+lattice	I-Process
+field	I-Process
+theories	I-Process
+with	O
+a	O
+complex	O
+Boltzmann	O
+weight	O
+,	O
+since	O
+it	O
+does	O
+not	O
+rely	O
+on	O
+importance	O
+sampling	O
+.	O
+In	O
+recent	O
+years	O
+a	O
+number	O
+of	O
+stimulating	O
+results	O
+has	O
+been	O
+obtained	O
+in	O
+the	O
+context	O
+of	O
+nonzero	B-Process
+chemical	I-Process
+potential	I-Process
+,	O
+in	O
+both	O
+lower	B-Process
+and	I-Process
+four-dimensional	I-Process
+field	I-Process
+theories	I-Process
+with	O
+a	O
+severe	O
+sign	B-Task
+problem	I-Task
+in	I-Task
+the	I-Task
+thermodynamic	I-Task
+limit	I-Task
+[	O
+3	O
+–	O
+8	O
+]	O
+(	O
+for	O
+two	O
+recent	O
+reviews	O
+,	O
+see	O
+e.g.	O
+Refs.	O
+[	O
+9,10	O
+])	O
+.	O
+However	O
+,	O
+as	O
+has	O
+been	O
+known	O
+since	O
+shortly	O
+after	O
+its	O
+inception	O
+,	O
+correct	O
+results	O
+are	O
+not	O
+guaranteed	O
+[	O
+11	O
+–	O
+16	O
+]	O
+.	O
+This	O
+calls	O
+for	O
+an	O
+improved	B-Task
+understanding	I-Task
+,	I-Task
+relying	I-Task
+on	I-Task
+the	I-Task
+combination	I-Task
+of	I-Task
+analytical	I-Task
+and	I-Task
+numerical	I-Task
+insight	I-Task
+.	O
+In	O
+the	O
+recent	O
+past	O
+,	O
+the	O
+important	O
+role	O
+played	O
+by	O
+the	O
+properties	O
+of	O
+the	O
+real	O
+and	O
+positive	O
+probability	B-Process
+distribution	I-Process
+in	O
+the	O
+complexified	B-Process
+configuration	I-Process
+space	I-Process
+,	O
+which	O
+is	O
+effectively	O
+sampled	O
+during	O
+the	O
+Langevin	B-Process
+process	I-Process
+,	O
+has	O
+been	O
+clarified	O
+[	O
+17,18	O
+]	O
+.	O
+An	O
+important	O
+conclusion	O
+was	O
+that	O
+this	O
+distribution	B-Process
+should	O
+be	O
+sufficiently	O
+localised	O
+in	O
+order	O
+for	O
+CL	B-Process
+to	O
+yield	O
+valid	O
+results	O
+.	O
+Importantly	O
+,	O
+this	O
+insight	O
+has	O
+recently	O
+also	O
+led	O
+to	O
+promising	O
+results	O
+in	O
+nonabelian	B-Task
+gauge	I-Task
+theories	I-Task
+,	O
+with	O
+the	O
+implementation	O
+of	O
+SL	B-Material
+(	I-Material
+N,C	I-Material
+)	I-Material
+gauge	I-Material
+cooling	I-Material
+[	O
+8,10	O
+]	O
+.	O
+
+This	O
+work	O
+shows	O
+how	O
+our	O
+approach	O
+based	O
+on	O
+the	O
+combination	O
+of	O
+Statistical	B-Process
+Mechanics	I-Process
+and	O
+nonlinear	B-Process
+PDEs	I-Process
+theory	I-Process
+provides	O
+us	O
+with	O
+a	O
+novel	O
+and	O
+powerful	O
+tool	O
+to	O
+tackle	O
+phase	B-Task
+transitions	I-Task
+.	O
+This	O
+method	O
+leads	O
+to	O
+solution	O
+of	O
+perhaps	O
+the	O
+most	O
+known	O
+test-case	O
+that	O
+exhibits	O
+a	O
+first	B-Process
+order	I-Process
+phase	I-Process
+transition	I-Process
+(	O
+semi-heuristically	O
+described	O
+)	O
+such	O
+as	O
+the	O
+van	B-Process
+der	I-Process
+Waals	I-Process
+model	I-Process
+.	O
+In	O
+particular	O
+we	O
+have	O
+obtained	O
+the	O
+first	O
+global	O
+mean	O
+field	B-Process
+partition	I-Process
+function	I-Process
+(	O
+Eq.	O
+(	O
+9	O
+))	O
+,	O
+for	O
+a	O
+system	O
+of	O
+finite	O
+number	O
+of	O
+particles	O
+.	O
+The	O
+partition	O
+function	O
+is	O
+a	O
+solution	O
+to	O
+the	O
+Klein	B-Task
+–	I-Task
+Gordon	I-Task
+equation	I-Task
+,	O
+reproduces	O
+the	O
+van	B-Process
+der	I-Process
+Waals	I-Process
+isotherms	I-Process
+away	O
+from	O
+the	O
+critical	O
+region	O
+and	O
+,	O
+in	O
+the	O
+thermodynamic	B-Process
+limit	I-Process
+N	I-Process
+→∞	I-Process
+automatically	O
+encodes	O
+the	O
+Maxwell	B-Process
+equal	I-Process
+areas	I-Process
+rule	I-Process
+.	O
+The	O
+approach	O
+hereby	O
+presented	O
+is	O
+of	O
+remarkable	O
+simplicity	O
+,	O
+has	O
+been	O
+successfully	O
+applied	O
+to	O
+spin	B-Process
+[	O
+17	O
+–	O
+19,14,16	O
+]	O
+and	O
+macroscopic	B-Process
+thermodynamic	I-Process
+systems	I-Process
+[	O
+20,15	O
+]	O
+and	O
+can	O
+be	O
+further	O
+extended	O
+to	O
+include	O
+the	O
+larger	O
+class	O
+of	O
+models	O
+admitting	O
+partition	B-Process
+functions	I-Process
+of	I-Process
+the	I-Process
+form	I-Process
+(	O
+4	O
+)	O
+to	O
+be	O
+used	O
+to	O
+extend	O
+to	O
+the	O
+critical	O
+region	O
+general	B-Process
+equations	I-Process
+of	I-Process
+state	I-Process
+of	I-Process
+the	I-Process
+form	I-Process
+(	O
+7	O
+)	O
+including	O
+a	O
+class	B-Process
+virial	I-Process
+expansions	I-Process
+.	O
+
+We	O
+use	O
+open	O
+and	O
+close	O
+aperture	B-Process
+Z-scan	I-Process
+experiments	I-Process
+,	O
+in	O
+analogy	O
+to	O
+the	O
+saturation	B-Task
+absorption	I-Task
+work	O
+discussed	O
+earlier	O
+in	O
+water	B-Material
+[	O
+8	O
+]	O
+,	O
+to	O
+respectively	O
+measure	O
+the	O
+β	O
+and	O
+n2	O
+for	O
+a	O
+series	O
+of	O
+primary	B-Material
+alcohols	I-Material
+with	O
+the	O
+help	O
+of	O
+1560nm	B-Material
+femtosecond	I-Material
+laser	I-Material
+pulses	I-Material
+,	O
+however	O
+,	O
+with	O
+the	O
+important	O
+inclusion	O
+of	O
+an	O
+optical-chopper	B-Material
+.	O
+The	O
+vibrational	B-Process
+combination	I-Process
+states	I-Process
+of	O
+the	O
+alcohols	B-Material
+are	O
+coupled	O
+by	O
+the	O
+femtosecond	B-Material
+laser	I-Material
+pulses	I-Material
+at	I-Material
+1560nm	I-Material
+.	O
+These	O
+couplings	O
+result	O
+in	O
+the	O
+absorption	B-Process
+of	O
+1560nm	O
+and	O
+the	O
+excited	O
+molecules	B-Material
+undergo	O
+relaxation	O
+through	O
+non-radiative	B-Process
+processes	I-Process
+,	O
+which	O
+gives	O
+rise	O
+to	O
+transient	B-Process
+thermal	I-Process
+effects	I-Process
+.	O
+These	O
+transient	O
+thermal	O
+effects	O
+are	O
+related	O
+to	O
+the	O
+pure	B-Process
+optical	I-Process
+nonlinearity	I-Process
+of	O
+the	O
+samples	O
+and	O
+can	O
+be	O
+measured	O
+as	O
+a	O
+change	O
+in	O
+their	O
+n2	O
+values	O
+[	O
+14	O
+]	O
+.	O
+The	O
+transient	B-Process
+thermal	I-Process
+effects	I-Process
+of	O
+individual	O
+pulses	O
+accumulate	O
+in	O
+case	O
+of	O
+high	B-Material
+repetition-rate	I-Material
+lasers	I-Material
+to	O
+produce	O
+a	O
+cumulative	B-Process
+thermal	I-Process
+effect	I-Process
+at	O
+longer	O
+timescales	O
+.	O
+We	O
+measure	B-Task
+this	I-Task
+cumulative	I-Task
+thermal	I-Task
+effect	I-Task
+with	O
+the	O
+mode-mismatched	B-Process
+two-color	I-Process
+pump	I-Process
+–	I-Process
+probe	I-Process
+experiment	I-Process
+.	O
+
+The	O
+control	O
+of	O
+the	O
+RP	B-Process
+re-encounter	I-Process
+probability	I-Process
+finds	O
+a	O
+direct	O
+application	O
+to	O
+improve	B-Task
+the	I-Task
+performance	I-Task
+of	I-Task
+chemical	I-Task
+devices	I-Task
+.	O
+Here	O
+,	O
+we	O
+show	O
+how	O
+a	O
+simple-to-implement	O
+control	B-Process
+scheme	I-Process
+highly	O
+enhances	O
+the	O
+sensitivity	O
+of	O
+a	O
+model	B-Material
+chemical	I-Material
+magnetometer	I-Material
+by	O
+up	O
+to	O
+two	O
+orders	O
+of	O
+magnitude	O
+.	O
+The	O
+basic	O
+idea	O
+behind	O
+a	O
+chemical	O
+magnetometer	O
+is	O
+that	O
+,	O
+since	O
+a	O
+change	O
+in	O
+the	O
+magnetic	B-Process
+field	I-Process
+modifies	O
+the	O
+amount	O
+of	O
+singlet	B-Material
+products	I-Material
+,	O
+one	O
+can	O
+reverse	O
+the	O
+reasoning	O
+and	O
+measure	O
+the	O
+chemical	B-Material
+yield	I-Material
+to	O
+estimate	O
+B	B-Process
+.	O
+Intuitively	O
+,	O
+the	O
+magnetic	B-Process
+sensitivity	I-Process
+is	O
+high	O
+when	O
+a	O
+small	O
+change	O
+in	O
+the	O
+magnetic	B-Process
+field	I-Process
+intensity	I-Process
+produces	O
+large	O
+effects	O
+on	O
+the	O
+singlet	B-Material
+yield	I-Material
+.	O
+Formally	O
+,	O
+it	O
+is	O
+defined	O
+as	O
+:(	O
+2	O
+)	O
+Λs	O
+(	O
+B	O
+)≡∂	O
+Φs	O
+(	O
+B	O
+)∂	O
+B	O
+=∫	O
+0	O
+∞	O
+pre	O
+(	O
+t	O
+)	O
+gs	O
+(	O
+B,t	O
+)	O
+dt,with	O
+gs	O
+(	O
+B,t	O
+)≡∂	O
+fs	O
+(	O
+B,t	O
+)∂	O
+B	O
+being	O
+the	O
+instantaneous	O
+magnetic	O
+sensitivity	O
+.	O
+The	O
+functional	O
+form	O
+of	O
+fs	O
+(	O
+B,t	O
+)=	O
+Sρel	O
+(	O
+t	O
+)	O
+S	O
+strongly	O
+depends	O
+on	O
+the	O
+specific	O
+realization	O
+of	O
+the	O
+radical	O
+pair	O
+,	O
+in	O
+particular	O
+on	O
+the	O
+number	O
+of	O
+the	O
+surrounding	O
+nuclear	O
+spins	O
+.	O
+Here	O
+,	O
+we	O
+consider	O
+a	O
+radical	O
+pair	O
+in	O
+which	O
+the	O
+first	O
+electron	O
+spin	O
+is	O
+devoid	O
+of	O
+hyperfine	O
+interactions	O
+,	O
+while	O
+the	O
+second	O
+electron	O
+spin	O
+interacts	O
+isotropically	O
+with	O
+one	O
+spin-1	O
+nucleus	O
+,	O
+e.g.	O
+nitrogen	O
+.	O
+In	O
+the	O
+context	O
+of	O
+the	O
+chemical	O
+compass	O
+(	O
+i.e.	O
+when	O
+the	O
+task	O
+is	O
+determining	O
+the	O
+magnetic	O
+field	O
+direction	O
+through	O
+anisotropic	O
+hyperfine	O
+interactions	O
+)	O
+,	O
+an	O
+analogous	O
+configuration	O
+(	O
+with	O
+only	O
+one	O
+spin-1	O
+/	O
+2	O
+nucleus	O
+)	O
+has	O
+been	O
+proposed	O
+[	O
+3	O
+]	O
+,	O
+and	O
+numerically	O
+characterized	O
+[	O
+8	O
+]	O
+,	O
+as	O
+being	O
+optimal	O
+:	O
+Additional	O
+nuclear	O
+spins	O
+would	O
+perturb	O
+the	O
+intuitive	O
+‘	O
+reference	O
+and	O
+probe’	O
+picture	O
+.	O
+The	O
+Hamiltonian	O
+then	O
+simplifies	O
+to	O
+H	O
+=-	O
+γeB	O
+(	O
+S1	O
+(	O
+z	O
+)+	O
+S2	O
+(	O
+z	O
+))+|	O
+γe	O
+|	O
+αS	O
+→	O
+2	O
+·	O
+I	O
+→	O
+,	O
+where	O
+α	O
+is	O
+the	O
+isotropic	O
+hyperfine	O
+coupling	O
+.	O
+
+It	O
+is	O
+well-known	O
+that	O
+the	O
+optical	B-Task
+properties	I-Task
+of	O
+atoms	B-Material
+and	O
+molecules	B-Material
+can	O
+be	O
+influenced	O
+by	O
+their	O
+electronic	B-Process
+environment	I-Process
+.	O
+Local	B-Process
+field	I-Process
+effects	I-Process
+on	O
+spontaneous	O
+emission	O
+rates	O
+within	O
+nanostructured	B-Material
+photonic	I-Material
+materials	I-Material
+for	O
+example	O
+are	O
+familiar	O
+,	O
+and	O
+have	O
+been	O
+well	O
+summarized	O
+[	O
+1	O
+]	O
+.	O
+Optical	B-Process
+processes	I-Process
+,	O
+including	O
+resonance	B-Process
+energy	I-Process
+transfer	I-Process
+are	O
+similarly	O
+dependent	O
+on	O
+the	O
+local	B-Process
+environment	I-Process
+of	I-Process
+molecular	I-Process
+chromophores	I-Process
+[	O
+2	O
+–	O
+4	O
+]	O
+.	O
+Many	O
+biological	O
+systems	O
+are	O
+known	O
+to	O
+contain	O
+complex	O
+organizations	O
+of	O
+molecules	O
+with	O
+absorption	B-Material
+bands	I-Material
+shifted	O
+due	O
+to	O
+the	O
+electronic	B-Process
+influence	I-Process
+of	O
+other	O
+,	O
+nearby	O
+optical	O
+centres	O
+.	O
+For	O
+instance	O
+,	O
+in	O
+widely	O
+studied	O
+light-harvesting	B-Process
+complexes	I-Process
+,	O
+there	O
+are	O
+two	O
+identifiable	O
+forms	O
+of	O
+the	O
+photosynthetic	B-Material
+antenna	I-Material
+molecule	I-Material
+bacteriochlorophyll	I-Material
+,	O
+with	O
+absorption	B-Material
+bands	I-Material
+centred	O
+on	O
+800	O
+and	O
+850nm	O
+;	O
+it	O
+has	O
+been	O
+shown	O
+that	O
+the	O
+most	O
+efficient	O
+forms	O
+of	O
+energy	B-Process
+transfer	I-Process
+between	O
+the	O
+two	O
+occurs	O
+when	O
+there	O
+is	O
+a	O
+neighbouring	O
+carotenoid	B-Material
+species	I-Material
+5	O
+–	O
+7	O
+.	O
+Until	O
+now	O
+,	O
+research	O
+on	O
+the	O
+broader	O
+influence	B-Task
+of	I-Task
+a	I-Task
+neighbouring	I-Task
+,	I-Task
+off-resonant	I-Task
+,	I-Task
+molecule	I-Task
+on	I-Task
+photon	I-Task
+absorption	I-Task
+has	O
+mostly	O
+centred	O
+on	O
+the	O
+phenomenon	O
+of	O
+induced	B-Process
+circular	I-Process
+dichroism	I-Process
+,	O
+where	O
+both	O
+quantum	B-Process
+electrodynamic	I-Process
+(	O
+QED	B-Process
+)	O
+calculations	O
+[	O
+8	O
+–	O
+10	O
+]	O
+and	O
+experimental	B-Process
+procedures	I-Process
+[	O
+11	O
+–	O
+13	O
+]	O
+predict	O
+and	O
+verify	O
+that	O
+a	O
+chiral	B-Material
+mediator	I-Material
+confers	O
+the	O
+capacity	O
+for	O
+an	O
+achiral	B-Material
+acceptor	I-Material
+to	O
+exhibit	O
+circular	B-Process
+differential	I-Process
+absorption	I-Process
+.	O
+
+Since	O
+the	O
+receptors	O
+in	O
+human	O
+biology	O
+mostly	O
+consist	O
+of	O
+chiral	B-Material
+molecules	I-Material
+,	O
+drug	O
+action	O
+mostly	O
+involves	O
+a	O
+specified	O
+enantiomeric	O
+form	O
+.	O
+This	O
+has	O
+spurred	O
+the	O
+development	O
+,	O
+especially	O
+in	O
+the	O
+pharmaceutical	O
+industry	O
+,	O
+of	O
+a	O
+host	O
+of	O
+techniques	O
+to	O
+secure	O
+enantiopure	O
+products	O
+.	O
+Such	O
+methods	O
+,	O
+mostly	O
+multi-step	O
+and	O
+time-consuming	O
+,	O
+can	O
+typically	O
+be	O
+cast	O
+in	O
+one	O
+of	O
+two	O
+distinct	O
+categories	O
+:	O
+synthetic	O
+mechanisms	O
+designed	O
+to	O
+produce	O
+a	O
+single	O
+stereoisomer	O
+,	O
+or	O
+separation	O
+techniques	O
+to	O
+isolate	O
+distinct	O
+enantiomers	O
+from	O
+a	O
+racemic	O
+mixture	O
+.	O
+A	O
+significant	O
+drawback	O
+,	O
+for	O
+either	O
+approach	O
+,	O
+is	O
+a	O
+dependence	O
+on	O
+a	O
+supply	O
+of	O
+enantiopure	O
+reagents	O
+or	O
+substrates	O
+–	O
+synthesis	O
+routes	O
+generally	O
+utilise	O
+chiral	O
+building	O
+blocks	O
+or	O
+enantioselective	O
+catalysts	O
+[	O
+7,8	O
+]	O
+,	O
+while	O
+enantiomer	O
+separation	O
+techniques	O
+typically	O
+incorporate	O
+chiral	O
+selector	O
+molecules	O
+to	O
+form	O
+chemically	O
+distinct	O
+and	O
+distinguishable	O
+diastereomeric	O
+complexes	O
+[	O
+8,9	O
+]	O
+.	O
+A	O
+key	O
+requirement	O
+in	O
+aiming	O
+to	O
+achieve	O
+enantiopure	O
+products	O
+,	O
+irrespective	O
+of	O
+the	O
+synthetic	O
+method	O
+,	O
+is	O
+therefore	O
+a	O
+means	O
+to	O
+measure	O
+,	O
+and	O
+duly	O
+quantitate	O
+the	O
+enantiomeric	O
+excess	O
+–	O
+signifying	O
+the	O
+degree	O
+of	O
+chirality	O
+within	O
+molecular	O
+products	O
+.	O
+Chiral	O
+discrimination	O
+through	O
+optical	O
+means	O
+is	O
+well-known	O
+to	O
+offer	O
+direct	O
+,	O
+non-contact	O
+ways	O
+to	O
+distinguish	O
+between	O
+molecules	O
+of	O
+different	O
+handedness	O
+,	O
+based	O
+on	O
+observations	O
+such	O
+as	O
+the	O
+subtle	O
+differences	O
+in	O
+absorption	O
+of	O
+left	O
+-	O
+and	O
+right-handed	O
+circularly	O
+polarised	O
+light	O
+,	O
+or	O
+indeed	O
+the	O
+twisting	O
+of	O
+polarisation	O
+in	O
+optical	O
+rotation	O
+.	O
+Other	O
+optical	O
+methods	O
+,	O
+under	O
+more	O
+recent	O
+development	O
+,	O
+also	O
+show	O
+some	O
+promise	O
+to	O
+achieve	O
+enantiomer	O
+separation	O
+,	O
+as	O
+will	O
+be	O
+introduced	O
+later	O
+.	O
+
+For	O
+any	O
+quantum	B-Process
+dynamical	I-Process
+method	I-Process
+,	O
+existing	O
+or	O
+emerging	O
+,	O
+reliable	O
+benchmarks	B-Task
+are	O
+required	O
+to	O
+assess	O
+their	O
+accuracy	O
+.	O
+A	B-Process
+model	I-Process
+Hamiltonian	I-Process
+exhibiting	O
+tunnelling	B-Process
+dynamics	I-Process
+through	O
+a	O
+multidimensional	B-Process
+asymmetric	I-Process
+double	I-Process
+well	I-Process
+potential	I-Process
+has	O
+been	O
+used	O
+as	O
+a	O
+test	O
+by	O
+the	O
+MP	B-Process
+/	I-Process
+SOFT	I-Process
+[	O
+18	O
+]	O
+and	O
+CCS	B-Process
+methods	I-Process
+[	O
+19	O
+]	O
+mentioned	O
+above	O
+,	O
+and	O
+also	O
+more	O
+recently	O
+by	O
+a	O
+configuration	B-Process
+interaction	I-Process
+(	I-Process
+CI	I-Process
+)	I-Process
+expansion	I-Process
+method	I-Process
+[	O
+20	O
+]	O
+and	O
+two-layer	B-Process
+version	I-Process
+of	I-Process
+CCS	I-Process
+(	O
+2L-CCS	B-Process
+)	O
+.	O
+[	O
+21	O
+]	O
+The	B-Process
+Hamiltonian	I-Process
+consists	O
+of	O
+a	O
+1-dimensional	B-Process
+tunnelling	I-Process
+mode	I-Process
+coupled	O
+to	O
+an	O
+(	B-Process
+M	I-Process
+−	I-Process
+1	I-Process
+)-	I-Process
+dimensional	I-Process
+harmonic	I-Process
+bath	I-Process
+,	O
+hence	O
+it	O
+is	O
+a	O
+system-bath	B-Task
+problem	I-Task
+which	O
+bears	O
+some	O
+similarity	O
+to	O
+the	O
+Caldeira-Leggett	B-Process
+model	I-Process
+of	I-Process
+tunnelling	I-Process
+in	O
+a	O
+dissipative	O
+system	O
+[	O
+22,23	O
+]	O
+.	O
+This	O
+Hamiltonian	B-Process
+is	O
+non-dissipative	O
+,	O
+however	O
+and	O
+the	O
+harmonic	B-Process
+modes	I-Process
+all	O
+have	O
+the	O
+same	O
+frequency	O
+.	O
+System-bath	B-Process
+models	I-Process
+play	O
+an	O
+important	O
+role	O
+in	O
+physics	B-Task
+,	O
+being	O
+used	O
+to	O
+describe	O
+superconductivity	B-Process
+at	I-Process
+a	I-Process
+Josephson	I-Process
+junction	I-Process
+in	O
+a	O
+superconducting	B-Process
+quantum	I-Process
+interface	I-Process
+device	I-Process
+(	O
+SQUID	B-Process
+)	O
+[	O
+24	O
+]	O
+,	O
+for	O
+which	O
+the	O
+Caldeira-Leggett	B-Process
+model	I-Process
+provides	O
+a	O
+theoretical	O
+basis	O
+,	O
+and	O
+magnetic	B-Process
+and	I-Process
+conductance	I-Process
+phenomena	I-Process
+in	O
+the	O
+spin-bath	B-Task
+regime	I-Task
+[	O
+25	O
+]	O
+.	O
+
+Based	O
+on	O
+the	O
+theoretical	B-Task
+analysis	I-Task
+,	O
+the	O
+value	B-Process
+of	I-Process
+the	I-Process
+measuring	I-Process
+resistor	I-Process
+,	O
+Rm	B-Process
+,	O
+has	O
+no	O
+effect	O
+on	O
+the	O
+corrosion	B-Process
+process	I-Process
+and	O
+on	O
+the	O
+estimated	O
+value	B-Process
+of	I-Process
+noise	I-Process
+resistance	I-Process
+.	O
+In	O
+order	O
+to	O
+validate	B-Task
+this	I-Task
+conclusion	I-Task
+,	O
+the	O
+experiment	O
+of	O
+Fig.	O
+9	O
+was	O
+performed	O
+.	O
+Specifically	O
+,	O
+a	O
+pair	B-Material
+of	I-Material
+nominally	I-Material
+identical	I-Material
+specimens	I-Material
+was	O
+initially	O
+coupled	O
+by	O
+a	O
+4.7kΩ	B-Material
+resistor	I-Material
+and	O
+their	O
+potential	O
+with	O
+respect	O
+to	O
+a	O
+saturated	B-Material
+calomel	I-Material
+electrode	I-Material
+was	O
+recorded	O
+by	O
+using	O
+a	O
+NI-USB	B-Material
+6009	I-Material
+analog-to-digital	I-Material
+converter	I-Material
+.	O
+The	O
+electrochemical	B-Process
+noise	I-Process
+signal	I-Process
+was	O
+recorded	O
+using	O
+in-house	B-Material
+developed	I-Material
+software	I-Material
+,	O
+acquiring	O
+at	O
+1023Hz	O
+segments	O
+of	O
+1000	O
+points	O
+at	O
+each	O
+iteration	O
+.	O
+Between	O
+iterations	O
+,	O
+the	O
+1000	O
+values	O
+acquired	O
+were	O
+averaged	O
+to	O
+obtain	B-Task
+a	I-Task
+single	I-Task
+value	I-Task
+of	I-Task
+potential	I-Task
+,	O
+subsequently	O
+saved	O
+to	O
+the	O
+file	O
+used	O
+for	O
+later	O
+processing	O
+.	O
+The	O
+final	O
+dataset	B-Material
+comprised	O
+potential	O
+values	O
+spaced	O
+1	O
+±	O
+0.05s	O
+in	O
+time	O
+.	O
+Under	O
+the	O
+assumption	O
+that	O
+the	O
+noise	O
+present	O
+above	O
+1023Hz	O
+is	O
+negligible	O
+compared	O
+with	O
+the	O
+noise	O
+present	O
+below	O
+0.5Hz	O
+,	O
+this	O
+procedure	O
+enables	O
+an	O
+accurate	B-Task
+recording	I-Task
+of	I-Task
+the	I-Task
+potential	I-Task
+noise	I-Task
+in	I-Task
+the	I-Task
+frequencies	I-Task
+of	I-Task
+interest	I-Task
+,	O
+avoiding	O
+aliasing	O
+of	O
+frequencies	O
+between	O
+0.5	O
+and	O
+1023Hz	O
+and	O
+minimizing	O
+the	O
+50Hz	O
+interference	O
+from	O
+the	O
+mains	O
+supply	O
+.	O
+
+A	O
+surfactant	B-Material
+is	O
+a	O
+surface	B-Material
+active	I-Material
+agent	I-Material
+.	O
+In	O
+this	O
+work	O
+a	O
+surfactant	B-Material
+term	O
+will	O
+be	O
+used	O
+for	O
+compounds	B-Material
+which	I-Material
+improve	I-Material
+the	I-Material
+dispersability	I-Material
+of	O
+the	O
+CI	B-Material
+in	O
+the	O
+acid	B-Material
+(	O
+as	O
+emulsifiers	B-Material
+providing	O
+dispersed	B-Material
+emulsion	I-Material
+–	O
+not	O
+separated	O
+)	O
+while	O
+wetting	O
+the	O
+surface	O
+of	O
+the	O
+metallic	B-Material
+material	I-Material
+[	O
+14,20,24	O
+]	O
+.	O
+However	O
+,	O
+surfactants	O
+can	O
+offer	O
+corrosion	B-Task
+protection	I-Task
+themselves	O
+.	O
+Some	O
+examples	O
+when	O
+the	O
+same	O
+compound	O
+was	O
+used	O
+as	O
+a	O
+surfactant	B-Material
+or	I-Material
+active	I-Material
+corrosion	I-Material
+inhibitor	I-Material
+ingredient	O
+are	O
+given	O
+below	O
+.	O
+Typical	O
+surfactants	B-Material
+in	O
+the	O
+oilfield	O
+services	O
+industry	O
+are	O
+alkylphenol	B-Material
+ethoxylates	I-Material
+,	O
+e.g.	O
+nonylphenol	B-Material
+ethoxylate	I-Material
+(	O
+NPE	B-Material
+)	O
+[	O
+14,15,30,106,107	O
+]	O
+.	O
+However	O
+,	O
+NPEs	B-Material
+have	O
+been	O
+banned	O
+from	O
+use	O
+in	O
+the	O
+North	O
+Sea	O
+because	O
+of	O
+their	O
+toxicity	O
+.	O
+On	O
+the	O
+other	O
+hand	O
+,	O
+ethoxylated	B-Material
+linear	I-Material
+alcohols	I-Material
+are	O
+more	O
+acceptable	O
+[	O
+20	O
+]	O
+.	O
+The	O
+quaternary	B-Material
+ammonium	I-Material
+salts	I-Material
+and	O
+amines	B-Material
+(	I-Material
+when	I-Material
+protonated	I-Material
+)	I-Material
+are	O
+the	O
+most	O
+used	O
+compounds	O
+of	O
+the	O
+cationic	B-Material
+surfactants	I-Material
+class	I-Material
+,	O
+where	O
+the	O
+cation	B-Material
+is	O
+the	O
+surface	B-Material
+active	I-Material
+specie	I-Material
+.	O
+As	O
+the	O
+amines	B-Material
+only	O
+function	O
+as	O
+a	O
+surfactant	B-Material
+in	O
+the	O
+protonated	B-Process
+state	I-Process
+,	O
+they	O
+cannot	O
+be	O
+used	O
+at	O
+high	O
+pH	O
+.	O
+On	O
+the	O
+other	O
+hand	O
+,	O
+quaternary	B-Material
+ammonium	I-Material
+compounds	I-Material
+,	O
+frequently	O
+abbreviated	O
+as	O
+“	O
+quats	B-Material
+”	O
+,	O
+are	O
+not	O
+pH	O
+sensitive	O
+.	O
+Long-chain	B-Material
+quaternary	I-Material
+ammonium	I-Material
+bromides	I-Material
+were	O
+also	O
+reported	O
+to	O
+work	O
+as	O
+efficient	O
+CIs	B-Material
+for	O
+steel	B-Material
+materials	I-Material
+[	O
+106	O
+]	O
+.	O
+A	O
+frequently	O
+employed	O
+surfactant	B-Material
+was	O
+N-dodecylpyridinium	B-Material
+bromide	I-Material
+(	O
+DDPB	B-Material
+)	O
+[	O
+9,60,61,108,109	O
+]	O
+.	O
+Anionic	B-Material
+sulphates	I-Material
+,	O
+anionic	B-Material
+sulphonates	I-Material
+,	O
+alkoxylated	B-Material
+alkylphenol	I-Material
+resins	I-Material
+,	O
+and	O
+polyoxyethylene	B-Material
+sorbitan	I-Material
+oleates	I-Material
+are	O
+also	O
+useful	O
+surfactants	B-Material
+.	O
+Ali	O
+reported	O
+that	O
+a	O
+particularly	O
+useful	O
+surfactant	B-Material
+is	O
+a	O
+blend	B-Material
+of	I-Material
+polyethylene	I-Material
+glycol	I-Material
+esters	I-Material
+of	I-Material
+fatty	I-Material
+acids	I-Material
+and	I-Material
+ethoxylated	I-Material
+alkylphenols	I-Material
+[	O
+15	O
+]	O
+.	O
+Several	O
+examples	O
+of	O
+the	O
+surfactants	B-Material
+used	O
+are	O
+given	O
+below	O
+in	O
+Section	O
+5.6	O
+.	O
+
+The	O
+related	O
+Volta	B-Process
+potential	I-Process
+(	O
+Ψ	B-Process
+)	O
+is	O
+the	O
+potential	B-Process
+difference	I-Process
+between	O
+a	O
+position	O
+infinitely	O
+far	O
+away	O
+from	O
+the	O
+surface	O
+and	O
+a	O
+position	O
+just	O
+outside	O
+the	O
+surface	O
+,	O
+and	O
+is	O
+the	O
+measureable	B-Process
+quantity	I-Process
+characterising	O
+electrochemical	B-Process
+behaviour	I-Process
+of	I-Process
+a	I-Process
+metal	I-Process
+[	O
+12,17	O
+]	O
+.	O
+The	O
+scanning	B-Process
+Kelvin	I-Process
+probe	I-Process
+force	I-Process
+microscopy	I-Process
+(	O
+SKPFM	B-Process
+)	O
+technique	O
+allows	O
+detection	B-Task
+of	I-Task
+local	I-Task
+EWF	I-Task
+(	O
+if	O
+the	O
+EWF	O
+of	O
+the	O
+tip	O
+is	O
+known	O
+)	O
+,	O
+or	O
+Volta	B-Task
+potential	I-Task
+differences	I-Task
+(	O
+ΔΨ	B-Task
+)	O
+between	O
+an	O
+atomic	B-Material
+force	I-Material
+microscopy	I-Material
+tip	I-Material
+(	O
+usually	O
+Pt	B-Material
+coated	I-Material
+)	O
+and	O
+the	O
+metal	B-Material
+surface	I-Material
+[	O
+14,15,19	O
+]	O
+.	O
+The	O
+lateral	O
+resolution	O
+of	O
+SKPFM	B-Process
+can	O
+be	O
+as	O
+high	O
+as	O
+10	O
+’s	O
+of	O
+nm	O
+in	O
+ambient	B-Material
+air	I-Material
+,	O
+with	O
+a	O
+sensitivity	O
+up	O
+to	O
+10	O
+–	O
+20meV	O
+[	O
+19	O
+]	O
+.	O
+Volta	B-Process
+potential	I-Process
+is	O
+a	O
+characteristic	O
+property	B-Process
+of	I-Process
+a	I-Process
+metal	I-Process
+surface	I-Process
+and	O
+can	O
+be	O
+used	O
+to	O
+understand	B-Task
+electrochemical	I-Task
+processes	I-Task
+[	O
+16	O
+]	O
+.	O
+It	O
+is	O
+sensitive	O
+to	O
+any	O
+kind	O
+of	O
+surface	O
+defects	O
+,	O
+chemical	O
+variations	O
+,	O
+and	O
+residual	O
+stress	O
+[	O
+13,17	O
+]	O
+.	O
+Volta	B-Process
+potential	I-Process
+differences	I-Process
+in	I-Process
+microstructure	I-Process
+have	O
+been	O
+used	O
+to	O
+predict	B-Task
+corrosion	I-Task
+behaviour	I-Task
+[	O
+10,15,18,20	O
+–	O
+22	O
+]	O
+.	O
+Regions	O
+with	O
+larger	B-Process
+(	I-Process
+ΔΨ	I-Process
+)	I-Process
+indicate	I-Process
+increased	I-Process
+surface	I-Process
+reactivity	I-Process
+[	O
+11,15,18	O
+]	O
+,	O
+and	O
+even	O
+a	O
+correlation	O
+between	O
+Volta	B-Process
+potential	I-Process
+differences	I-Process
+measured	O
+in	O
+nominally	O
+dry	B-Material
+air	I-Material
+and	O
+their	O
+free	B-Process
+corrosion	I-Process
+potential	I-Process
+(	O
+Ecorr	B-Process
+)	O
+pre-determined	O
+under	O
+immersed	O
+conditions	O
+has	O
+been	O
+reported	O
+[	O
+18	O
+]	O
+.	O
+
+The	O
+homologous	B-Material
+series	I-Material
+of	I-Material
+n-alkanes	I-Material
+are	O
+represented	O
+here	O
+as	O
+homonuclear	B-Material
+chains	I-Material
+of	I-Material
+tangent	I-Material
+Mie	I-Material
+spherical	I-Material
+CG	I-Material
+segments	I-Material
+.	O
+The	O
+development	B-Task
+of	I-Task
+CG	I-Task
+models	I-Task
+for	I-Task
+long	I-Task
+n-alkanes	I-Task
+such	O
+as	O
+n-decane	B-Material
+(	O
+n-C10H22	B-Material
+)	O
+and	O
+n-eicosane	B-Material
+(	O
+n-C20H42	B-Material
+)	O
+has	O
+already	O
+been	O
+successfully	O
+demonstrated	O
+using	O
+the	O
+SAFT-γ	B-Process
+Mie	I-Process
+formalism	I-Process
+[	O
+118	O
+]	O
+.	O
+The	O
+n-decane	B-Material
+molecule	I-Material
+was	O
+represented	O
+by	O
+chains	O
+of	O
+three	O
+and	O
+n-eicosane	B-Material
+chains	O
+of	O
+six	O
+fully	O
+flexible	O
+tangentially	O
+bonded	O
+Mie	B-Material
+segments	I-Material
+.	O
+A	O
+certain	O
+degree	O
+of	O
+parameter	O
+degeneracy	O
+in	O
+terms	O
+of	O
+overall	O
+performance	O
+is	O
+expected	O
+as	O
+a	O
+consequence	O
+of	O
+the	O
+conformal	O
+nature	O
+of	O
+the	O
+EOS	O
+description	O
+[	O
+132	O
+]	O
+.	O
+In	O
+our	O
+current	O
+work	O
+,	O
+we	O
+use	O
+an	O
+alternative	B-Process
+CG	I-Process
+mapping	I-Process
+for	O
+n-alkanes	B-Material
+developed	O
+in	O
+reference	O
+[	O
+122	O
+]	O
+,	O
+where	O
+each	O
+segment	O
+was	O
+taken	O
+to	O
+represent	O
+three	O
+alkyl	B-Material
+carbon	I-Material
+backbone	I-Material
+atoms	I-Material
+and	O
+their	O
+corresponding	O
+hydrogen	B-Material
+atoms	I-Material
+.	O
+By	O
+applying	O
+this	O
+mapping	O
+,	O
+n-alkanes	B-Material
+chains	I-Material
+containing	O
+multiples	O
+of	O
+three	O
+carbon	B-Material
+units	I-Material
+can	O
+be	O
+represented	O
+directly	O
+:	O
+n-C6H14	B-Material
+,	O
+n-C9H20	B-Material
+,	O
+n-C12H26	B-Material
+,	O
+n-C15H32	B-Material
+,	O
+n-C18H38	B-Material
+,	O
+etc	O
+.	O
+A	O
+good	O
+description	B-Task
+of	I-Task
+the	I-Task
+thermodynamic	I-Task
+properties	I-Task
+of	O
+these	O
+alkanes	B-Material
+is	O
+found	O
+to	O
+be	O
+provided	O
+with	O
+CG	B-Material
+alkyl	I-Material
+beads	I-Material
+characterised	O
+by	O
+the	O
+Mie	B-Process
+(	I-Process
+15	I-Process
+–	I-Process
+6	I-Process
+)	I-Process
+potential	I-Process
+.	O
+For	O
+convenience	O
+,	O
+the	O
+exponent	O
+pair	O
+(	O
+15	O
+–	O
+6	O
+)	O
+is	O
+also	O
+used	O
+to	O
+represent	O
+the	O
+interactions	O
+between	O
+the	O
+CG	B-Material
+beads	I-Material
+of	O
+the	O
+intervening	O
+alkanes	B-Material
+considered	O
+here	O
+;	O
+the	O
+number	O
+of	O
+segments	O
+m	O
+is	O
+taken	O
+to	O
+be	O
+the	O
+nearest	O
+integer	O
+of	O
+the	O
+division	O
+of	O
+the	O
+carbon	B-Material
+number	O
+C	O
+by	O
+three	O
+.	O
+The	O
+size	O
+σ	O
+and	O
+energy	O
+∊	O
+parameters	O
+are	O
+then	O
+estimated	O
+from	O
+the	O
+experimental	O
+saturated-liquid	B-Process
+density	I-Process
+and	O
+vapour	B-Process
+pressure	I-Process
+of	O
+the	O
+individual	O
+alkanes	B-Material
+following	O
+the	O
+usual	O
+SAFT-γ	B-Process
+Mie	I-Process
+procedure	I-Process
+.	O
+The	O
+chosen	O
+mapping	O
+is	O
+by	O
+no	O
+means	O
+unique	O
+,	O
+as	O
+one	O
+can	O
+postulate	O
+parameter	O
+sets	O
+that	O
+fulfil	O
+other	O
+requisites	O
+,	O
+such	O
+as	O
+being	O
+“	O
+universal	O
+”	O
+across	O
+the	O
+entire	O
+homologous	O
+series	O
+[	O
+119	O
+]	O
+or	O
+correlated	O
+to	O
+the	O
+critical	O
+properties	O
+[	O
+125	O
+]	O
+.	O
+
+This	O
+study	O
+proposes	O
+a	O
+new	B-Task
+framework	I-Task
+of	I-Task
+a	I-Task
+numerical	I-Task
+modelling	I-Task
+of	O
+the	O
+gas	B-Process
+exchange	I-Process
+between	O
+air	B-Material
+and	O
+water	B-Material
+across	O
+their	O
+interface	O
+,	O
+and	O
+subsequent	O
+chemical	B-Process
+reaction	I-Process
+in	I-Process
+water	I-Process
+based	O
+on	O
+an	O
+extended	O
+two-compartment	B-Process
+model	I-Process
+.	O
+The	O
+major	O
+purpose	O
+of	O
+this	O
+study	O
+is	O
+to	O
+provide	O
+a	O
+fundamental	B-Process
+concept	I-Process
+for	O
+modelling	B-Task
+physicochemical	I-Task
+processes	I-Task
+of	O
+the	O
+gas	B-Material
+exchange	O
+,	O
+followed	O
+by	O
+the	O
+chemical	B-Process
+reaction	I-Process
+in	I-Process
+water	I-Process
+.	O
+Demonstrating	O
+fundamental	O
+data	O
+and	O
+knowledge	O
+on	O
+the	O
+important	O
+environmental	O
+transport	O
+phenomena	O
+,	O
+especially	O
+the	O
+effects	B-Process
+of	I-Process
+the	I-Process
+Schmidt	I-Process
+number	I-Process
+and	O
+the	O
+chemical	B-Process
+reaction	I-Process
+rate	I-Process
+on	O
+the	O
+gas	B-Process
+exchange	I-Process
+mechanisms	I-Process
+across	I-Process
+the	I-Process
+interface	I-Process
+have	O
+also	O
+been	O
+attempted	O
+.	O
+The	O
+gas	B-Process
+exchange	I-Process
+processes	I-Process
+are	O
+separated	O
+into	O
+two	O
+physicochemical	O
+substeps	O
+,	O
+the	O
+first	O
+is	O
+the	O
+gas	B-Process
+–	I-Process
+liquid	I-Process
+equilibrium	I-Process
+between	O
+the	O
+two	O
+phases	O
+,	O
+and	O
+the	O
+second	O
+is	O
+the	O
+chemical	B-Process
+reaction	I-Process
+in	I-Process
+the	I-Process
+water	I-Process
+phase	I-Process
+.	O
+A	O
+first-order	O
+,	O
+irreversible	B-Process
+chemical	I-Process
+reaction	I-Process
+of	O
+the	O
+gaseous	B-Material
+material	I-Material
+after	O
+its	O
+uptake	O
+into	O
+the	O
+water	B-Material
+phase	I-Material
+is	O
+assumed	O
+here	O
+to	O
+simplify	O
+interactions	O
+of	O
+the	O
+chemical	B-Process
+reactions	I-Process
+and	O
+turbulent	B-Process
+transport	I-Process
+phenomena	I-Process
+in	I-Process
+water	I-Process
+.	O
+While	O
+a	O
+traditional	O
+two-compartment	B-Process
+model	I-Process
+assumes	O
+uniform	O
+concentration	O
+of	O
+a	O
+material	O
+in	O
+each	O
+compartment	O
+,	O
+the	O
+present	O
+two-compartment	O
+model	O
+uses	O
+a	O
+computational	B-Process
+fluid	I-Process
+dynamics	I-Process
+(	O
+CFD	B-Process
+)	O
+technique	O
+in	O
+the	O
+water	B-Material
+compartment	O
+to	O
+evaluate	B-Task
+temporal	I-Task
+development	I-Task
+of	I-Task
+three-dimensional	I-Task
+profiles	I-Task
+of	I-Task
+the	I-Task
+velocity	I-Task
+and	I-Task
+concentration	I-Task
+fields	I-Task
+.	O
+A	O
+direct	B-Process
+numerical	I-Process
+simulation	I-Process
+(	O
+DNS	B-Process
+)	O
+approach	O
+is	O
+used	O
+to	O
+evaluate	B-Task
+profiles	I-Task
+of	I-Task
+fluid	I-Task
+velocities	I-Task
+and	I-Task
+concentrations	I-Task
+in	I-Task
+water	I-Task
+,	O
+and	O
+several	O
+important	O
+turbulence	O
+statistics	O
+have	O
+been	O
+evaluated	O
+without	O
+using	O
+turbulent	O
+closures	O
+,	O
+and	O
+subgrid-scale	B-Process
+models	I-Process
+.	O
+We	O
+assume	O
+that	O
+a	O
+fluid	B-Process
+flow	I-Process
+in	I-Process
+the	I-Process
+water	I-Process
+phase	I-Process
+is	O
+a	O
+well-developed	O
+turbulent	O
+water	O
+layer	O
+of	O
+a	O
+low	O
+Reynolds	O
+number	O
+,	O
+and	O
+the	O
+Schmidt	O
+number	O
+is	O
+varied	O
+from	O
+1	O
+to	O
+8	O
+to	O
+observe	B-Task
+the	I-Task
+effects	I-Task
+of	I-Task
+the	I-Task
+molecular	I-Task
+diffusion	I-Task
+of	O
+the	O
+gas	B-Material
+in	O
+sub-interface	O
+water	B-Material
+on	O
+the	O
+gas	B-Material
+exchange	O
+rate	O
+at	O
+the	O
+interface	O
+.	O
+Six	O
+degrees	O
+of	O
+the	O
+nondimensional	B-Process
+chemical	I-Process
+reaction	I-Process
+rate	I-Process
+are	O
+used	O
+to	O
+find	O
+the	O
+effect	B-Task
+of	I-Task
+the	I-Task
+chemical	I-Task
+reaction	I-Task
+rate	I-Task
+on	I-Task
+the	I-Task
+gas	I-Task
+exchange	I-Task
+mechanisms	I-Task
+.	O
+Extrapolations	O
+of	O
+the	O
+gas	B-Process
+exchange	I-Process
+rates	I-Process
+and	O
+the	O
+related	O
+transport	B-Process
+phenomena	I-Process
+toward	O
+larger	O
+Schmidt	O
+number	O
+and	O
+the	O
+faster	O
+chemical	B-Process
+reaction	I-Process
+rate	O
+will	O
+also	O
+be	O
+examined	O
+to	O
+predict	B-Task
+the	I-Task
+gas	I-Task
+exchange	I-Task
+processes	I-Task
+of	O
+the	O
+actual	O
+gases	B-Material
+of	O
+Sc	B-Material
+∼	I-Material
+O	I-Material
+(	I-Material
+102	I-Material
+)	I-Material
+based	O
+on	O
+results	O
+from	O
+the	O
+present	O
+numerical	B-Task
+experiments	I-Task
+.	O
+
+Although	O
+the	O
+free	B-Task
+Kelvin	I-Task
+wave	I-Task
+problem	I-Task
+is	O
+of	O
+considerable	O
+theoretical	O
+importance	O
+,	O
+problems	B-Task
+with	I-Task
+forcing	I-Task
+and	I-Task
+damping	I-Task
+have	O
+greater	O
+practical	O
+importance	O
+.	O
+In	O
+nature	O
+,	O
+the	O
+forcing	O
+could	O
+be	O
+due	O
+to	O
+a	O
+wind	B-Material
+stress	O
+at	O
+the	O
+free	O
+surface	O
+or	O
+an	O
+astronomical	B-Process
+tidal	I-Process
+potential	I-Process
+,	O
+and	O
+the	O
+damping	B-Process
+could	O
+be	O
+due	O
+to	O
+the	O
+turbulent	B-Process
+stress	I-Process
+of	I-Process
+a	I-Process
+bottom	I-Process
+boundary	I-Process
+layer	I-Process
+.	O
+Regardless	O
+of	O
+the	O
+details	O
+,	O
+the	O
+forced	B-Process
+response	I-Process
+is	O
+composed	O
+of	O
+shallow-water	B-Material
+waves	I-Material
+,	O
+possibly	O
+including	O
+Kelvin	B-Material
+waves	I-Material
+,	O
+with	O
+the	O
+largest	O
+amplitudes	O
+in	O
+waves	O
+with	O
+a	O
+natural	B-Process
+frequency	I-Process
+ωf	B-Process
+close	O
+to	O
+that	O
+of	O
+the	O
+forcing	B-Process
+frequency	I-Process
+ω	B-Process
+;	O
+various	O
+examples	O
+of	O
+this	O
+sort	O
+are	O
+given	O
+in	O
+Chapters	O
+9	O
+and	O
+10	O
+of	O
+Gill	O
+[	O
+16	O
+]	O
+.	O
+When	O
+ω	O
+≈	O
+ωf	B-Process
+,	O
+there	O
+is	O
+a	O
+large	O
+amplitude	O
+near-resonant	O
+response	O
+,	O
+the	O
+size	O
+of	O
+which	O
+is	O
+sensitive	O
+to	O
+the	O
+weak	B-Process
+damping	I-Process
+and	O
+|	B-Process
+ω	I-Process
+−	I-Process
+ωf	I-Process
+|	I-Process
+.	O
+Thus	O
+,	O
+in	O
+numerical	B-Task
+solutions	I-Task
+of	O
+near-resonantly	B-Material
+forced	I-Material
+waves	I-Material
+,	O
+we	O
+anticipate	O
+that	O
+errors	O
+in	O
+ωf	B-Process
+(	O
+associated	O
+with	O
+the	O
+spatial	B-Process
+discretisation	I-Process
+)	O
+could	O
+lead	O
+to	O
+non-trivial	O
+errors	O
+in	O
+the	O
+forced	O
+response	O
+.	O
+
+A	O
+fully-coupled	B-Process
+numerical	I-Process
+framework	I-Process
+for	O
+two-phase	B-Process
+flows	I-Process
+with	O
+an	O
+implicit	O
+implementation	O
+of	O
+surface	B-Process
+tension	I-Process
+has	O
+been	O
+introduced	O
+in	O
+this	O
+article	O
+.	O
+This	O
+fully-coupled	B-Process
+framework	I-Process
+has	O
+then	O
+been	O
+used	O
+to	O
+compare	B-Task
+the	I-Task
+influence	I-Task
+of	O
+the	O
+surface	B-Process
+tension	I-Process
+treatment	I-Process
+on	O
+the	O
+time-step	B-Process
+restrictions	I-Process
+resulting	I-Process
+from	I-Process
+capillary	I-Process
+waves	I-Process
+.	O
+The	O
+conducted	O
+study	O
+demonstrates	O
+that	O
+restrictions	B-Process
+on	I-Process
+the	I-Process
+numerical	I-Process
+time-step	I-Process
+resulting	I-Process
+from	I-Process
+capillary	I-Process
+waves	I-Process
+are	O
+valid	O
+and	O
+unchanged	O
+regardless	O
+of	O
+the	O
+numerical	B-Process
+treatment	I-Process
+of	I-Process
+surface	I-Process
+tension	I-Process
+.	O
+Since	O
+surface	O
+tension	O
+is	O
+not	O
+a	O
+function	O
+of	O
+pressure	O
+or	O
+velocity	O
+,	O
+the	O
+change	O
+in	O
+implementation	O
+does	O
+not	O
+affect	O
+the	O
+matrix	O
+coefficients	O
+of	O
+the	O
+primitive	O
+variables	O
+and	O
+,	O
+thus	O
+,	O
+numerical	O
+stability	O
+is	O
+independent	O
+of	O
+the	O
+treatment	B-Task
+of	I-Task
+surface	I-Task
+tension	I-Task
+.	O
+Further	O
+analysis	O
+shows	O
+that	O
+the	O
+capillary	O
+time-step	O
+constraint	O
+is	O
+a	O
+requirement	O
+imposed	O
+by	O
+the	O
+spatiotemporal	B-Task
+sampling	I-Task
+of	I-Task
+capillary	I-Task
+waves	I-Task
+,	O
+which	O
+is	O
+independent	O
+of	O
+the	O
+applied	B-Process
+numerical	I-Process
+methodology	I-Process
+.	O
+
+The	O
+remainder	O
+of	O
+our	O
+discussion	O
+proceeds	O
+as	O
+follows	O
+.	O
+In	O
+Section	O
+2	O
+we	O
+briefly	O
+describe	O
+the	O
+problem	B-Task
+of	I-Task
+cell	I-Task
+tracking	I-Task
+and	O
+introduce	B-Task
+our	I-Task
+approach	I-Task
+to	I-Task
+cell	I-Task
+tracking	I-Task
+,	O
+which	O
+may	O
+be	O
+regarded	O
+as	O
+fitting	O
+a	O
+mathematical	B-Process
+model	I-Process
+to	O
+experimental	B-Material
+image	I-Material
+data	I-Material
+sets	I-Material
+.	O
+We	O
+present	O
+the	O
+geometric	B-Process
+evolution	I-Process
+law	I-Process
+model	I-Process
+we	O
+seek	O
+to	O
+fit	O
+,	O
+which	O
+is	O
+a	O
+simplification	O
+of	O
+recently	O
+developed	O
+models	O
+in	O
+the	O
+literature	O
+that	O
+show	O
+good	O
+agreement	O
+with	O
+experiments	O
+[	O
+8,10	O
+–	O
+12,4,13,9	O
+]	O
+.	O
+We	O
+finish	O
+Section	O
+2	O
+by	O
+reformulating	O
+our	B-Process
+model	I-Process
+into	O
+the	O
+phase	B-Process
+field	I-Process
+framework	I-Process
+,	O
+which	O
+appears	O
+more	O
+suitable	O
+for	O
+the	O
+problem	O
+in	O
+hand	O
+,	O
+and	O
+we	O
+formulate	O
+the	O
+cell	B-Task
+tracking	I-Task
+problem	I-Task
+as	O
+a	O
+PDE	B-Task
+constrained	I-Task
+optimisation	I-Task
+problem	I-Task
+.	O
+In	O
+Section	O
+3	O
+we	O
+propose	O
+an	O
+algorithm	B-Process
+for	O
+the	O
+resolution	O
+of	O
+the	O
+PDE	B-Task
+constrained	I-Task
+optimisation	I-Task
+problem	I-Task
+and	O
+we	O
+discuss	O
+some	O
+practical	O
+aspects	O
+related	O
+to	O
+the	O
+implementation	O
+.	O
+In	O
+particular	O
+we	O
+note	O
+that	O
+the	O
+theoretical	B-Process
+and	I-Process
+computational	I-Process
+framework	I-Process
+may	O
+be	O
+applied	O
+directly	O
+to	O
+multi-cell	B-Material
+image	I-Material
+data	I-Material
+sets	I-Material
+and	O
+raw	B-Material
+image	I-Material
+data	I-Material
+sets	I-Material
+(	O
+of	O
+sufficient	O
+quality	O
+)	O
+without	O
+segmentation	B-Process
+.	O
+In	O
+Section	O
+4	O
+we	O
+present	O
+some	O
+numerical	O
+examples	O
+for	O
+the	O
+case	O
+of	O
+2d	O
+single	O
+and	O
+multi-cell	O
+image	B-Material
+data	I-Material
+sets	I-Material
+.	O
+Finally	O
+in	O
+Section	O
+5	O
+we	O
+present	O
+some	O
+conclusions	O
+of	O
+our	O
+study	O
+and	O
+discuss	O
+future	O
+extensions	O
+and	O
+applications	O
+of	O
+the	O
+work	O
+.	O
+
+The	B-Task
+dynamics	I-Task
+of	I-Task
+various	I-Task
+physical	I-Task
+phenomena	I-Task
+,	O
+such	O
+as	O
+the	O
+movement	B-Process
+of	I-Process
+pendulums	I-Process
+,	I-Process
+planets	I-Process
+,	I-Process
+or	I-Process
+water	I-Process
+waves	I-Process
+can	O
+be	O
+described	O
+in	O
+a	O
+variational	B-Process
+framework	I-Process
+.	O
+The	O
+development	O
+of	O
+variational	B-Process
+principles	I-Process
+for	O
+classical	O
+mechanics	O
+traces	O
+back	O
+to	O
+Euler	O
+,	O
+Lagrange	O
+,	O
+and	O
+Hamilton	O
+;	O
+an	O
+overview	O
+of	O
+this	O
+history	O
+can	O
+be	O
+found	O
+in	O
+[	O
+1,19	O
+]	O
+.	O
+This	O
+approach	B-Process
+allows	O
+to	O
+express	B-Task
+all	I-Task
+the	I-Task
+dynamics	I-Task
+of	I-Task
+a	I-Task
+system	I-Task
+in	O
+a	O
+single	B-Process
+functional	I-Process
+–	O
+the	O
+Lagrangian	B-Process
+–	O
+which	O
+is	O
+an	O
+action	B-Process
+integral	I-Process
+.	O
+Hamiltonian	B-Process
+mechanics	I-Process
+is	O
+a	O
+reformulation	B-Process
+of	I-Process
+Lagrangian	I-Process
+mechanics	I-Process
+which	O
+provides	O
+a	O
+convenient	O
+framework	B-Material
+to	O
+study	B-Task
+the	I-Task
+symmetry	I-Task
+properties	I-Task
+of	I-Task
+a	I-Task
+system	I-Task
+.	O
+This	O
+is	O
+expressed	O
+by	O
+Noether	O
+'s	O
+theorem	O
+which	O
+establishes	O
+the	O
+direct	O
+connection	O
+between	O
+the	O
+symmetry	O
+properties	O
+of	O
+Hamiltonian	B-Process
+systems	I-Process
+and	O
+conservation	O
+laws	O
+.	O
+When	O
+one	O
+approximates	O
+the	O
+system	B-Process
+numerically	O
+,	O
+it	O
+is	O
+advantageous	O
+to	O
+preserve	O
+the	O
+Hamiltonian	O
+structure	O
+also	O
+at	O
+the	O
+discrete	O
+level	O
+.	O
+Given	O
+that	O
+Hamiltonian	B-Process
+systems	I-Process
+are	O
+abundant	O
+in	O
+nature	O
+,	O
+their	O
+numerical	B-Task
+approximation	I-Task
+is	O
+therefore	O
+a	O
+topic	O
+of	O
+significant	O
+relevance	O
+.	O
+
+As	O
+discussed	O
+above	O
+,	O
+proper	B-Task
+inclusion	I-Task
+of	I-Task
+these	I-Task
+interactions	I-Task
+requires	O
+segment	B-Process
+synchronization	I-Process
+after	I-Process
+every	I-Process
+iteration	I-Process
+.	O
+In	O
+order	O
+to	O
+minimize	B-Task
+simulation	I-Task
+errors	I-Task
+due	O
+to	O
+incorrect	O
+values	O
+of	O
+the	O
+interactions	O
+potential	O
+,	O
+segments	B-Process
+are	I-Process
+synchronized	I-Process
+after	I-Process
+every	I-Process
+iteration	I-Process
+.	O
+Although	O
+relatively	O
+long	O
+communication	O
+times	O
+between	O
+remote	O
+processors	B-Material
+may	O
+hinder	O
+this	O
+process	O
+in	O
+typical	O
+parallel	B-Material
+computers	I-Material
+,	O
+this	O
+is	O
+not	O
+the	O
+case	O
+for	O
+GPGPU	B-Material
+architectures	I-Material
+.	O
+Still	O
+,	O
+full	O
+recalculation	B-Process
+of	I-Process
+the	I-Process
+interaction	I-Process
+potential	I-Process
+after	O
+each	O
+iteration	O
+is	O
+time	O
+consuming	O
+.	O
+Instead	O
+,	O
+the	O
+algorithm	B-Process
+corrects	B-Process
+the	I-Process
+current	I-Process
+potential	I-Process
+by	O
+adding	B-Process
+dipole	I-Process
+contributions	I-Process
+for	O
+every	O
+nearby	O
+charge	O
+that	O
+hopped	O
+during	O
+the	O
+previous	O
+iteration	O
+.	O
+Full	O
+updates	O
+of	O
+the	O
+interaction	B-Process
+potential	I-Process
+are	O
+only	O
+required	O
+for	O
+the	O
+grid	O
+points	O
+that	O
+are	O
+related	O
+to	O
+charges	O
+that	O
+hopped	O
+during	O
+the	O
+last	O
+iteration	O
+.	O
+Accumulative	O
+rounding	O
+errors	O
+that	O
+arise	O
+due	O
+to	O
+repetitive	O
+addition	O
+and	O
+subtraction	O
+are	O
+solve	O
+this	O
+by	O
+rounding	O
+all	O
+interaction	O
+potentials	O
+to	O
+a	O
+uniformly	O
+spaced	O
+range	O
+of	O
+floating	O
+point	O
+numbers	O
+.	O
+
+The	O
+need	O
+to	O
+represent	B-Task
+scale	I-Task
+interactions	I-Task
+in	O
+weather	B-Process
+and	I-Process
+climate	I-Process
+prediction	I-Process
+models	I-Process
+has	O
+,	O
+for	O
+many	O
+decades	O
+,	O
+motivated	O
+research	O
+into	O
+the	O
+use	O
+of	O
+adaptive	B-Material
+meshes	I-Material
+[	O
+3,34,38	O
+]	O
+.	O
+R-adaptivity	B-Process
+–	O
+mesh	B-Material
+redistribution	O
+–	O
+involves	O
+deforming	B-Process
+a	I-Process
+mesh	I-Process
+in	O
+order	O
+to	O
+vary	O
+local	O
+resolution	O
+and	O
+was	O
+first	O
+considered	O
+for	O
+atmospheric	B-Process
+modelling	I-Process
+more	O
+than	O
+twenty	O
+years	O
+ago	O
+by	O
+Dietachmayer	O
+and	O
+Droegemeier	O
+[	O
+14	O
+]	O
+.	O
+It	O
+is	O
+an	O
+attractive	O
+form	O
+of	O
+adaptivity	B-Process
+since	O
+it	O
+does	O
+not	O
+involve	O
+altering	B-Process
+the	I-Process
+mesh	I-Process
+connectivity	I-Process
+,	O
+does	O
+not	O
+create	O
+load	O
+balancing	O
+problems	O
+because	O
+points	O
+are	O
+never	O
+created	O
+or	O
+destroyed	O
+,	O
+does	O
+not	O
+require	O
+mapping	B-Process
+of	I-Process
+solutions	I-Process
+between	I-Process
+meshes	I-Process
+[	O
+26	O
+]	O
+,	O
+does	O
+not	O
+lead	O
+to	O
+sudden	O
+changes	O
+in	O
+resolution	O
+and	O
+can	O
+be	O
+retro-fitted	O
+into	O
+existing	O
+models	O
+.	O
+Variational	B-Process
+methods	I-Process
+exist	O
+which	O
+attempt	O
+to	O
+control	B-Task
+resolution	I-Task
+in	I-Task
+different	I-Task
+directions	I-Task
+for	I-Task
+r-adaptive	I-Task
+meshes	I-Task
+(	O
+e.g.	O
+[	O
+23,25	O
+])	O
+.	O
+Alternatively	O
+,	O
+the	O
+solution	O
+of	O
+the	O
+Monge	B-Process
+–	I-Process
+Ampère	I-Process
+equation	I-Process
+to	O
+generate	O
+an	O
+optimally	B-Material
+transported	I-Material
+(	I-Material
+OT	I-Material
+)	I-Material
+mesh	I-Material
+based	O
+on	O
+a	O
+scalar	B-Process
+valued	I-Process
+monitor	I-Process
+function	I-Process
+is	O
+a	O
+useful	O
+form	O
+of	O
+r-adaptive	B-Process
+mesh	I-Process
+generation	I-Process
+because	O
+it	O
+generates	O
+a	O
+mesh	O
+equidistributed	O
+with	O
+respect	O
+to	O
+a	O
+monitor	B-Process
+function	I-Process
+and	O
+does	O
+not	O
+lead	O
+to	O
+mesh	B-Process
+tangling	I-Process
+[	O
+7	O
+]	O
+.	O
+We	O
+will	O
+see	O
+that	O
+the	O
+optimal	B-Task
+transport	I-Task
+problem	I-Task
+on	I-Task
+the	I-Task
+sphere	I-Task
+leads	O
+to	O
+a	O
+slightly	O
+different	O
+equation	O
+of	O
+Monge	B-Process
+–	I-Process
+Ampère	I-Process
+type	O
+,	O
+which	O
+has	O
+not	O
+before	O
+been	O
+solved	O
+numerically	O
+on	O
+the	O
+surface	O
+of	O
+a	O
+sphere	B-Material
+,	O
+which	O
+would	O
+be	O
+necessary	O
+for	O
+weather	B-Task
+and	I-Task
+climate	I-Task
+prediction	I-Task
+using	O
+r-adaptivity	B-Process
+.	O
+
+The	O
+four	O
+bounding	B-Material
+PCM	I-Material
+wastes	I-Material
+,	O
+given	O
+in	O
+Table	O
+1	O
+,	O
+were	O
+simulated	O
+using	O
+the	O
+most	O
+appropriate	O
+materials	O
+and	O
+geometries	O
+.	O
+“	B-Material
+Mock	I-Material
+up	I-Material
+”	I-Material
+PCM	I-Material
+drums	I-Material
+were	O
+assembled	O
+using	O
+the	O
+following	O
+components	O
+:	O
+PCM	O
+drums	O
+were	O
+simulated	O
+using	O
+mild	B-Material
+steel	I-Material
+paint	I-Material
+cans	I-Material
+and	I-Material
+lids	I-Material
+(	O
+Fenton	O
+Packaging	O
+Ltd.	O
+)	O
+;	O
+PVC	B-Material
+bags	I-Material
+were	O
+replicated	O
+using	O
+identical	B-Material
+PVC	I-Material
+sheeting	I-Material
+(	O
+Romar	O
+Workwear	O
+Ltd.	O
+)	O
+;	O
+the	O
+metallic	B-Material
+waste	I-Material
+was	O
+simulated	O
+using	O
+commercial	B-Material
+grade	I-Material
+18	I-Material
+/	I-Material
+8	I-Material
+stainless	I-Material
+steel	I-Material
+,	O
+aluminium	B-Material
+and	O
+copper	B-Material
+(	O
+Avus	O
+Metals	O
+&	O
+Plastics	O
+Ltd.	O
+)	O
+,	O
+and	O
+lead	B-Material
+shot	I-Material
+(	O
+Aldrich	O
+)	O
+;	O
+the	O
+inorganic	B-Material
+waste	I-Material
+was	O
+simulated	O
+using	O
+waste	B-Material
+Pyrex	I-Material
+labware	I-Material
+,	O
+crushed	O
+masonry	B-Material
+,	O
+concrete	B-Material
+and	O
+window	B-Material
+glass	I-Material
+;	O
+CeO2	B-Material
+(	O
+from	O
+Acros	O
+Organics	O
+,	O
+>	O
+99.9	O
+%	O
+;	O
+dried	O
+15h	O
+at	O
+600	O
+°	O
+C	O
+)	O
+was	O
+used	O
+as	O
+a	O
+PuO2	B-Material
+surrogate	I-Material
+.	O
+Commercially	O
+available	O
+ground	O
+,	O
+granulated	O
+blast-furnace	B-Material
+slag	I-Material
+“	I-Material
+Calumite	I-Material
+”	I-Material
+was	O
+used	O
+as	O
+an	O
+additive	O
+[	O
+27	O
+]	O
+.	O
+The	O
+analysed	O
+chemical	O
+composition	O
+is	O
+given	O
+in	O
+Table	O
+3	O
+.	O
+Calumite	O
+is	O
+a	O
+powdered	B-Material
+material	I-Material
+,	O
+with	O
+a	O
+typical	O
+particle	B-Material
+size	O
+distribution	O
+between	O
+limits	O
+of	O
+ca	O
+.	O
+40	O
+to	O
+ca	O
+.	O
+400μm	O
+.	O
+
+There	O
+is	O
+still	O
+some	O
+debate	O
+about	O
+the	O
+crystal	B-Material
+structure	O
+and	O
+composition	O
+of	O
+the	O
+fine	B-Material
+oxides	I-Material
+found	O
+in	O
+ODS	B-Material
+steels	I-Material
+and	O
+a	O
+number	O
+of	O
+different	O
+phases	O
+have	O
+been	O
+both	O
+proposed	O
+and	O
+identified	O
+.	O
+A	O
+complete	B-Task
+characterisation	I-Task
+of	I-Task
+the	I-Task
+oxide	I-Task
+particles	I-Task
+,	O
+including	O
+crystal	B-Material
+structure	O
+and	O
+composition	O
+,	O
+is	O
+needed	O
+as	O
+different	O
+phases	O
+and	O
+chemical	O
+variants	O
+of	O
+a	O
+single	O
+structure	O
+have	O
+been	O
+shown	O
+to	O
+respond	O
+differently	O
+to	O
+high	O
+temperatures	O
+and	O
+irradiation	B-Process
+.	O
+Ribis	O
+and	O
+de	O
+Carlan	O
+[	O
+6	O
+]	O
+have	O
+studied	O
+the	O
+coarsening	O
+characteristics	O
+of	O
+Y2O3	B-Material
+and	O
+Y2Ti2O7	B-Material
+oxides	I-Material
+at	O
+high	O
+temperatures	O
+.	O
+They	O
+show	O
+that	O
+the	O
+increase	O
+in	O
+particle	B-Material
+size	O
+is	O
+greater	O
+for	O
+the	O
+non-Ti	O
+containing	O
+phase	O
+.	O
+Similarly	O
+,	O
+Ratti	O
+et	O
+al	O
+.	O
+[	O
+9	O
+]	O
+,	O
+although	O
+they	O
+do	O
+not	O
+allude	O
+to	O
+specific	O
+oxide	O
+phases	O
+,	O
+have	O
+shown	O
+that	O
+small	O
+Ti	B-Material
+additions	O
+to	O
+an	O
+18	O
+%	O
+Cr	O
+ODS	O
+alloy	O
+dramatically	O
+reduces	O
+the	O
+coarsening	O
+rates	O
+of	O
+dispersoids	O
+when	O
+compared	O
+to	O
+an	O
+equivalent	O
+alloy	O
+without	O
+titanium	O
+.	O
+For	O
+example	O
+,	O
+Ribis	O
+indicates	O
+that	O
+coarsening	O
+rates	O
+may	O
+be	O
+controlled	O
+by	O
+interfacial	O
+energy	O
+between	O
+the	O
+secondary	O
+phase	O
+particles	O
+and	O
+the	O
+matrix	O
+;	O
+he	O
+points	O
+out	O
+that	O
+the	O
+resistance	O
+to	O
+coarsening	O
+observed	O
+in	O
+the	O
+Y	O
+,	O
+Ti	O
+,	O
+O	O
+system	O
+is	O
+probably	O
+the	O
+result	O
+of	O
+a	O
+very	O
+low	O
+interface	O
+energy	O
+and	O
+this	O
+would	O
+differ	O
+from	O
+one	O
+phase	O
+to	O
+another	O
+.	O
+Whittle	O
+et	O
+al	O
+.	O
+[	O
+10	O
+]	O
+have	O
+shown	O
+that	O
+pyrochlore	O
+and	O
+structures	O
+closely	O
+related	O
+to	O
+the	O
+pyrochlore	O
+structure	O
+respond	O
+in	O
+different	O
+ways	O
+to	O
+irradiation	O
+.	O
+They	O
+revealed	O
+that	O
+oxide	B-Material
+structure	O
+and	O
+variations	O
+in	O
+composition	O
+can	O
+affect	O
+their	O
+ability	O
+to	O
+withstand	O
+and	O
+recover	O
+from	O
+irradiation	O
+induced	O
+damage	O
+.	O
+
+Zirconium	B-Material
+alloys	I-Material
+are	O
+used	O
+as	O
+fuel	O
+cladding	O
+in	O
+pressurised	O
+and	O
+boiling	O
+water	O
+nuclear	B-Material
+reactors	I-Material
+.	O
+As	O
+such	O
+these	O
+materials	O
+are	O
+exposed	O
+to	O
+a	O
+large	O
+number	O
+of	O
+environmental	O
+factors	O
+that	O
+will	O
+promote	O
+degradation	B-Process
+mechanisms	I-Process
+such	O
+as	O
+oxidation	B-Process
+.	O
+At	O
+high	O
+burn-ups	O
+,	O
+i.e.	O
+extended	O
+service	O
+life	O
+,	O
+oxidation	O
+and	O
+the	O
+associated	O
+hydrogen	B-Process
+pick-up	I-Process
+can	O
+be	O
+a	O
+limiting	O
+factor	O
+in	O
+terms	O
+of	O
+fuel	B-Material
+efficiency	O
+and	O
+safety	O
+.	O
+The	O
+oxidation	B-Process
+kinetics	O
+for	O
+many	O
+zirconium	B-Material
+alloys	I-Material
+are	O
+cyclical	O
+,	O
+demonstrating	O
+a	O
+series	O
+of	O
+approximately	O
+cubic	O
+kinetic	O
+curves	O
+separated	O
+by	O
+transitions	O
+[	O
+1	O
+–	O
+5	O
+]	O
+.	O
+These	O
+transitions	O
+are	O
+typified	O
+by	O
+a	O
+breakdown	O
+in	O
+the	O
+protective	O
+character	O
+of	O
+the	O
+oxide	B-Material
+and	O
+are	O
+potentially	O
+linked	O
+to	O
+a	O
+number	O
+of	O
+mechanical	O
+issues	O
+.	O
+Understanding	B-Task
+how	I-Task
+these	I-Task
+issues	I-Task
+influence	I-Task
+oxidation	I-Task
+is	O
+a	O
+key	O
+to	O
+developing	B-Task
+a	I-Task
+full	I-Task
+mechanistic	I-Task
+understanding	I-Task
+of	I-Task
+the	I-Task
+corrosion	I-Task
+process	I-Task
+.	O
+
+The	O
+formulation	O
+in	O
+Table	O
+1	O
+was	O
+derived	O
+by	O
+an	O
+empirical	O
+approach	O
+and	O
+led	O
+to	O
+a	O
+non-classical	B-Material
+glass	I-Material
+matrix	I-Material
+.	O
+Carter	O
+et	O
+al	O
+.	O
+[	O
+3	O
+]	O
+and	O
+Zhang	O
+et	O
+al	O
+.	O
+[	O
+4	O
+]	O
+took	O
+a	O
+more	O
+systematic	O
+approach	O
+to	O
+such	O
+glass-ceramic	B-Material
+wasteforms	I-Material
+.	O
+These	O
+wasteforms	O
+were	O
+targeted	O
+at	O
+Hanford	B-Material
+K-basin	I-Material
+sludges	I-Material
+and	O
+the	O
+immobilisation	B-Task
+of	I-Task
+the	I-Task
+primary	I-Task
+waste	I-Task
+stream	I-Task
+from	I-Task
+production	I-Task
+of	I-Task
+molybdenum-99	I-Task
+at	O
+the	O
+Australian	O
+Nuclear	O
+Science	O
+and	O
+Technology	O
+Organisation	O
+site	O
+in	O
+Sydney	O
+respectively	O
+.	O
+In	O
+the	O
+work	O
+of	O
+Carter	O
+et	O
+al.	O
+and	O
+Zhang	O
+et	O
+al.	O
+the	O
+intended	O
+crystalline	B-Material
+phase	O
+was	O
+the	O
+closely	O
+related	O
+titanate	B-Material
+pyrochlore	I-Material
+,	O
+CaUTi2O7	B-Material
+.	O
+The	O
+glass	B-Material
+matrix	I-Material
+was	O
+formulated	O
+such	O
+that	O
+the	O
+trivalent	O
+species	O
+in	O
+the	O
+glass	B-Material
+network	I-Material
+,	O
+boron	B-Material
+and	O
+aluminium	B-Material
+,	O
+were	O
+charge	O
+compensated	O
+on	O
+a	O
+molar	O
+basis	O
+by	O
+sodium	B-Material
+.	O
+The	O
+stoichiometric	O
+composition	O
+of	O
+the	O
+glass	B-Material
+in	O
+this	O
+wasteform	O
+was	O
+Na2AlBSi6O16	B-Material
+.	O
+This	O
+glass	B-Material
+provides	O
+a	O
+method	O
+by	O
+which	O
+the	O
+glass	B-Material
+composition	I-Material
+can	O
+be	O
+varied	O
+systematically	O
+.	O
+Given	O
+that	O
+the	O
+initial	O
+observations	O
+inferred	O
+an	O
+important	O
+role	O
+played	O
+by	O
+alumina	B-Material
+,	O
+it	O
+was	O
+decided	O
+to	O
+prepare	O
+a	O
+suite	O
+of	O
+zirconolite	B-Material
+glass-ceramics	I-Material
+in	O
+which	O
+the	O
+glass	B-Material
+matrix	I-Material
+was	O
+defined	O
+by	O
+Na2Al1	B-Material
++	I-Material
+xB1	I-Material
+–	I-Material
+xSi6O16	I-Material
+to	O
+investigate	B-Task
+the	I-Task
+role	I-Task
+played	I-Task
+by	I-Task
+glass	I-Task
+composition	I-Task
+in	I-Task
+controlling	I-Task
+crystalline	I-Task
+phase	I-Task
+stability	I-Task
+.	O
+The	O
+x	O
+=	O
+1	O
+end	O
+member	O
+gives	O
+the	O
+mineral	B-Material
+albite	I-Material
+,	O
+NaAlSi3O8	B-Material
+.	O
+The	O
+melting	O
+point	O
+of	O
+albite	B-Material
+is	O
+1120	O
+°	O
+C	O
+[	O
+5	O
+]	O
+and	O
+the	O
+composition	O
+cools	O
+to	O
+a	O
+glass	B-Material
+at	O
+the	O
+cooling	O
+rates	O
+that	O
+occur	O
+during	O
+a	O
+HIP	O
+cycle	O
+.	O
+From	O
+the	O
+available	O
+phase	O
+diagrams	O
+,	O
+[	O
+6	O
+]	O
+no	O
+boron	B-Material
+analogue	O
+for	O
+albite	B-Material
+was	O
+shown	O
+,	O
+and	O
+the	O
+liquidus	O
+estimated	O
+from	O
+the	O
+relevant	O
+phase	O
+diagram	O
+is	O
+1100	O
+–	O
+1200	O
+°	O
+C	O
+.	O
+No	O
+phase	O
+diagrams	O
+for	O
+the	O
+quaternary	O
+system	O
+Na2O	B-Material
+–	I-Material
+Al2O3	I-Material
+–	I-Material
+B2O3	I-Material
+–	I-Material
+SiO2	I-Material
+could	O
+be	O
+found	O
+.	O
+
+Structural	O
+properties	O
+are	O
+well	O
+reproduced	O
+by	O
+all	O
+models	O
+(	O
+Table	O
+2	O
+)	O
+,	O
+but	O
+the	O
+significant	O
+improvement	O
+of	O
+our	O
+potential	O
+stands	O
+in	O
+the	O
+elastic	O
+constants	O
+which	O
+relate	O
+to	O
+how	O
+the	O
+system	O
+responds	O
+to	O
+stress	O
+.	O
+Indeed	O
+,	O
+structure	O
+and	O
+elasticity	O
+are	O
+important	O
+parameters	O
+for	O
+elucidating	B-Task
+grain	I-Task
+boundary	I-Task
+stability	I-Task
+.	O
+All	O
+potential	O
+models	O
+correctly	O
+predict	B-Task
+the	I-Task
+relative	I-Task
+stability	I-Task
+of	I-Task
+the	I-Task
+defect	I-Task
+energies	I-Task
+.	O
+The	O
+Morelon	B-Process
+potential	I-Process
+model	I-Process
+performed	O
+best	O
+as	O
+it	O
+was	O
+specifically	O
+derived	O
+to	O
+replicate	B-Task
+defect	I-Task
+formation	I-Task
+energies	I-Task
+,	O
+but	O
+it	O
+largely	O
+underestimates	O
+the	O
+bulk	O
+modulus	O
+.	O
+The	O
+energies	O
+calculated	O
+with	O
+the	O
+Morl	B-Process
+and	I-Process
+the	I-Process
+Arima	I-Process
+potential	I-Process
+models	I-Process
+are	O
+overestimated	O
+;	O
+this	O
+is	O
+a	O
+known	O
+disadvantage	O
+of	O
+using	O
+rigid	B-Process
+ion	I-Process
+models	I-Process
+as	O
+the	O
+ionic	O
+polarisability	O
+is	O
+not	O
+taken	O
+into	O
+account	O
+.	O
+For	O
+completeness	O
+,	O
+we	O
+report	O
+two	O
+shell	B-Process
+models	I-Process
+with	O
+the	O
+best	O
+results	O
+given	O
+by	O
+the	O
+Catlow	B-Process
+potential	I-Process
+model	I-Process
+.	O
+The	O
+Morl	B-Process
+,	I-Process
+along	I-Process
+with	I-Process
+the	I-Process
+Grimes	I-Process
+shell	I-Process
+potential	I-Process
+model	I-Process
+,	O
+accurately	O
+reproduce	B-Task
+the	I-Task
+activation	I-Task
+energy	I-Task
+of	I-Task
+oxygen	I-Task
+migration	I-Task
+(	O
+the	O
+migration	B-Process
+path	I-Process
+was	O
+the	O
+lowest	O
+energy	O
+and	O
+most	O
+favourable	O
+diffusion	B-Process
+mechanism	I-Process
+observed	O
+in	O
+bulk	O
+UO2	B-Material
+[	O
+1	O
+])	O
+.	O
+The	O
+major	O
+deficiency	O
+of	O
+the	O
+Morl	B-Process
+potential	I-Process
+is	O
+that	O
+the	O
+cation	B-Material
+defect	O
+energies	O
+are	O
+high	O
+,	O
+and	O
+hence	O
+the	O
+number	O
+of	O
+cation	O
+defects	O
+will	O
+be	O
+underestimated	O
+.	O
+However	O
+,	O
+this	O
+should	O
+not	O
+be	O
+an	O
+issue	O
+unless	O
+this	O
+model	O
+was	O
+applied	O
+to	O
+processes	O
+such	O
+as	O
+grain	B-Process
+growth	I-Process
+where	O
+cation	O
+mobility	O
+will	O
+contribute	O
+.	O
+
+Hydrides	B-Material
+,	O
+once	O
+precipitated	O
+in	O
+zirconium	B-Material
+,	O
+degrade	O
+the	O
+mechanical	O
+properties	O
+of	O
+a	O
+component	O
+,	O
+leading	O
+to	O
+reductions	O
+in	O
+tensile	O
+strength	O
+,	O
+ductility	O
+and	O
+fracture	O
+toughness	O
+[	O
+35	O
+–	O
+40	O
+]	O
+.	O
+These	O
+changes	O
+can	O
+ultimately	O
+compromise	O
+the	O
+integrity	O
+of	O
+cladding	B-Process
+during	O
+normal	O
+operating	O
+life	O
+,	O
+accident	O
+conditions	O
+and	O
+fuel	B-Material
+storage	O
+[	O
+13	O
+]	O
+.	O
+As	O
+well	O
+as	O
+the	O
+degradation	O
+of	O
+mechanical	O
+properties	O
+,	O
+the	O
+presence	O
+of	O
+hydrides	B-Material
+can	O
+also	O
+affect	O
+phenomena	O
+like	O
+pellet	B-Process
+cladding	I-Process
+mechanical	I-Process
+interaction	I-Process
+(	O
+PCMI	B-Process
+)	O
+;	O
+or	O
+introduce	O
+mechanisms	O
+for	O
+failure	O
+,	O
+such	O
+as	O
+delayed	B-Process
+hydride	I-Process
+cracking	I-Process
+(	O
+DHC	B-Process
+)	O
+.	O
+The	O
+former	O
+mechanism	O
+is	O
+the	O
+product	O
+of	O
+thermal	B-Process
+expansion	I-Process
+in	O
+fuel	B-Material
+pellets	I-Material
+introducing	O
+stresses	O
+into	O
+the	O
+cladding	B-Process
+,	O
+which	O
+may	O
+then	O
+lead	O
+to	O
+the	O
+formation	O
+of	O
+cracks	O
+in	O
+areas	O
+made	O
+brittle	O
+by	O
+large	O
+hydride	B-Material
+concentrations	O
+[	O
+13	O
+]	O
+.	O
+The	O
+latter	O
+mechanism	O
+,	O
+DHC	B-Process
+,	O
+is	O
+a	O
+sub-critical	O
+,	O
+time	O
+dependent	O
+cracking	B-Process
+phenomenon	I-Process
+that	O
+requires	O
+long	O
+range	O
+hydrogen	B-Material
+diffusion	O
+for	O
+repeated	O
+local	B-Task
+hydride	I-Task
+growth	I-Task
+and	O
+fracture	O
+at	O
+a	O
+hydrostatic	B-Process
+tensile	I-Process
+stress	I-Process
+raiser	I-Process
+[	O
+5,41,42	O
+]	O
+.	O
+The	O
+process	O
+occurs	O
+over	O
+an	O
+extended	O
+period	O
+of	O
+time	O
+under	O
+a	O
+continuously	O
+applied	O
+load	O
+that	O
+is	O
+below	O
+the	O
+yield	O
+stress	O
+of	O
+the	O
+material	O
+[	O
+5,41,42	O
+]	O
+.	O
+
+Uranium	B-Material
+carbide	I-Material
+was	O
+traditionally	O
+used	O
+as	O
+fuel	B-Material
+kernel	I-Material
+for	O
+the	O
+US	O
+version	O
+of	O
+pebble	B-Material
+bed	I-Material
+reactors	I-Material
+as	O
+opposed	O
+to	O
+the	O
+German	O
+version	O
+based	O
+on	O
+uranium	B-Material
+dioxide	I-Material
+.	O
+For	O
+the	O
+Generation	B-Material
+IV	I-Material
+nuclear	I-Material
+systems	I-Material
+,	O
+mixed	B-Material
+uranium	I-Material
+–	I-Material
+plutonium	I-Material
+carbides	I-Material
+(	B-Material
+U	I-Material
+,	I-Material
+Pu	I-Material
+)	I-Material
+C	I-Material
+constitute	O
+the	O
+primary	O
+option	O
+for	O
+the	O
+gas	B-Material
+fast	I-Material
+reactors	I-Material
+(	O
+GFR	B-Material
+)	O
+and	O
+UCO	B-Material
+is	O
+the	O
+first	O
+candidate	O
+for	O
+the	O
+very	B-Material
+high	I-Material
+temperature	I-Material
+reactor	I-Material
+(	O
+VHTR	B-Material
+)	O
+.	O
+In	O
+the	O
+former	O
+case	O
+the	O
+fuel	B-Material
+high	O
+actinide	B-Material
+density	O
+and	O
+thermal	O
+conductivity	O
+are	O
+exploited	O
+in	O
+view	O
+of	O
+high	O
+burnup	B-Process
+performance	O
+.	O
+In	O
+the	O
+latter	O
+,	O
+UCO	B-Material
+is	O
+a	O
+good	O
+compromise	O
+between	O
+oxides	B-Material
+and	O
+carbides	B-Material
+both	O
+in	O
+terms	O
+of	O
+thermal	O
+conductivity	O
+and	O
+fissile	O
+density	O
+.	O
+However	O
+,	O
+in	O
+the	O
+American	O
+VHTR	B-Material
+design	O
+,	O
+the	O
+fuel	B-Material
+is	O
+a	O
+3:1	O
+ratio	O
+of	O
+UO2	B-Material
+:	O
+UC2	B-Material
+for	O
+one	O
+essential	O
+reason	O
+,	O
+well	O
+explained	O
+by	O
+Olander	O
+[	O
+2	O
+]	O
+in	O
+a	O
+recent	O
+publication	O
+.	O
+During	O
+burnup	B-Process
+,	O
+pure	O
+UO2	B-Material
+fuel	I-Material
+tends	O
+to	O
+oxidize	O
+to	O
+UO2	B-Material
++	I-Material
+x	I-Material
+.	O
+UO2	O
++	O
+x	O
+reacts	O
+with	O
+the	O
+pyrocarbon	B-Material
+coating	I-Material
+layer	I-Material
+according	O
+to	O
+the	O
+equilibrium	O
+:(	O
+1	O
+)	O
+UO2	B-Material
++	I-Material
+x	I-Material
++	O
+xC	B-Material
+→	O
+UO2	B-Material
++	O
+xCO	O
+
+The	O
+Magnox	B-Material
+reactors	I-Material
+represent	O
+the	O
+first	O
+generation	O
+of	O
+gas-cooled	B-Material
+reactors	I-Material
+in	O
+the	O
+UK	O
+that	O
+used	O
+carbon	B-Material
+dioxide	I-Material
+(	O
+CO2	B-Material
+)	O
+as	O
+the	O
+primary	O
+coolant	B-Material
+and	O
+a	O
+honeycomb	B-Material
+network	I-Material
+of	I-Material
+graphite	I-Material
+bricks	I-Material
+to	O
+provide	O
+neutron	B-Process
+moderation	I-Process
+.	O
+During	O
+reactor	B-Material
+operation	O
+significant	O
+amounts	O
+of	O
+carbon	B-Material
+monoxide	I-Material
+(	O
+CO	B-Material
+)	O
+was	O
+produced	O
+from	O
+the	O
+CO2	B-Material
+coolant	I-Material
+.	O
+This	O
+CO	B-Material
+in	O
+turn	O
+can	O
+be	O
+radiolytically	B-Process
+polymerised	I-Process
+to	O
+form	B-Task
+a	I-Task
+carbonaceous	I-Task
+deposit	I-Task
+on	I-Task
+free	I-Task
+surfaces	I-Task
+[	O
+12	O
+]	O
+.	O
+This	O
+non-graphitic	B-Material
+carbon	I-Material
+deposit	I-Material
+is	O
+significantly	O
+more	O
+chemically	O
+reactive	O
+to	O
+air	B-Material
+than	O
+the	O
+underlying	O
+graphite	B-Material
+[	O
+12,13	O
+]	O
+.	O
+During	O
+the	O
+lifetime	O
+of	O
+some	O
+Magnox	B-Material
+reactors	I-Material
+,	O
+small	O
+quantities	O
+of	O
+methane	B-Material
+gas	I-Material
+were	O
+injected	O
+into	O
+the	O
+coolant	B-Material
+gas	I-Material
+to	O
+inhibit	B-Task
+weight	I-Task
+loss	I-Task
+of	I-Task
+the	I-Task
+graphite	I-Task
+core	I-Task
+due	I-Task
+to	I-Task
+radiolytic	I-Task
+oxidation	I-Task
+[	O
+14	O
+]	O
+.	O
+Methane	B-Material
+(	O
+CH4	B-Material
+)	O
+is	O
+a	O
+precursor	O
+for	O
+carbonaceous	B-Material
+deposits	I-Material
+that	O
+form	O
+a	O
+sacrificial	O
+layer	O
+protecting	O
+the	O
+underlying	O
+graphite	B-Material
+from	O
+excessive	B-Process
+weight	I-Process
+loss	I-Process
+[	O
+15	O
+]	O
+and	O
+reduction	B-Process
+in	I-Process
+mechanical	I-Process
+strength	I-Process
+[	O
+16	O
+]	O
+.	O
+It	O
+is	O
+assumed	O
+nitrogen	B-Material
+incorporation	O
+during	O
+deposit	O
+formation	O
+is	O
+the	O
+subsequent	O
+production	O
+route	O
+for	O
+the	O
+high	O
+14C	O
+levels	O
+observed	O
+.	O
+
+An	O
+essential	O
+part	O
+of	O
+nuclear	B-Task
+reactor	I-Task
+analysis	I-Task
+is	O
+the	O
+prediction	B-Task
+of	I-Task
+the	I-Task
+three-dimensional	I-Task
+space-time	I-Task
+kinetics	I-Task
+of	I-Task
+neutrons	I-Task
+in	O
+a	O
+relatively	O
+large	O
+,	O
+finite	O
+,	O
+heterogeneous	O
+,	O
+three-dimensional	O
+reactor	B-Material
+core	I-Material
+.	O
+In	O
+a	O
+majority	O
+of	O
+safety	B-Task
+analyses	I-Task
+the	O
+prediction	B-Task
+of	I-Task
+reactor	I-Task
+physics	I-Task
+responses	I-Task
+is	O
+performed	O
+using	O
+neutron	B-Material
+diffusion	O
+theory	O
+applied	O
+to	O
+three-dimensional	O
+systems	O
+,	O
+with	O
+inputs	O
+usually	O
+derived	O
+from	O
+deterministic	B-Process
+neutron	I-Process
+transport	I-Process
+solutions	I-Process
+of	O
+two-dimensional	B-Process
+lattice	I-Process
+geometries	I-Process
+.	O
+There	O
+has	O
+been	O
+increased	O
+activity	O
+related	O
+to	O
+uncertainty	O
+and	O
+sensitivity	O
+in	O
+reactor	B-Task
+physics	I-Task
+calculations	I-Task
+,	O
+and	O
+the	O
+Organization	O
+for	O
+Economic	O
+Cooperation	O
+and	O
+Development	O
+–	O
+Nuclear	O
+Energy	O
+Agency	O
+(	O
+OECD-NEA	O
+)	O
+has	O
+sponsored	O
+an	O
+ongoing	O
+benchmark	O
+entitled	O
+“	O
+Uncertainty	B-Material
+Analysis	I-Material
+in	I-Material
+Modelling	I-Material
+”	O
+(	O
+UAM	B-Material
+)	O
+related	O
+to	O
+these	O
+efforts	O
+.	O
+The	O
+goal	O
+of	O
+this	O
+work	O
+is	O
+to	O
+offer	O
+a	O
+strategy	B-Task
+for	I-Task
+computing	I-Task
+lattice	I-Task
+sensitivities	I-Task
+using	O
+the	O
+DRAGON	B-Material
+lattice	I-Material
+code	I-Material
+and	O
+WIMS-D4	B-Material
+multi-group	I-Material
+library	I-Material
+.	O
+Results	O
+are	O
+presented	O
+with	O
+comparison	O
+to	O
+those	O
+from	O
+TSUNAMI	B-Process
+,	O
+developed	O
+by	O
+Oak	O
+Ridge	O
+National	O
+Laboratories	O
+.	O
+
+The	O
+pipes	B-Material
+under	O
+pressure	O
+in	O
+the	O
+RCS	B-Material
+or	O
+connected	O
+to	O
+RCS	O
+are	O
+usually	O
+made	O
+of	O
+austenitic	B-Material
+or	I-Material
+austenitic	I-Material
+&	I-Material
+ferritic	I-Material
+stainless	I-Material
+steel	I-Material
+.	O
+Most	O
+connections	O
+are	O
+welded	O
+.	O
+The	O
+pipes	B-Material
+may	O
+be	O
+exposed	O
+to	O
+various	O
+degradation	O
+phenomena	O
+(	O
+diverse	O
+hazards	O
+,	O
+mechanical	O
+fatigue	O
+,	O
+thermal	O
+fatigue	O
+,	O
+stress	O
+corrosion	O
+,	O
+etc.	O
+)	O
+.	O
+Event	B-Task
+screening	I-Task
+in	O
+the	O
+databases	O
+showed	O
+a	O
+total	O
+of	O
+116	O
+events	O
+(	O
+33	O
+related	O
+to	O
+cracks	O
+and	O
+83	O
+to	O
+leaks	O
+)	O
+.	O
+Three	O
+main	O
+causes	O
+for	O
+failure	O
+were	O
+identified	O
+,	O
+namely	O
+,	O
+fatigue	O
+,	O
+corrosion	O
+and	O
+the	O
+presence	O
+of	O
+manufacturing	O
+defects	O
+.	O
+Human	O
+factor	O
+induced	O
+defects	O
+proved	O
+to	O
+have	O
+little	O
+impact	O
+–	O
+less	O
+than	O
+10	O
+%	O
+of	O
+the	O
+cases	O
+could	O
+be	O
+attributed	O
+to	O
+operation	O
+errors	O
+.	O
+Fatigue	O
+was	O
+found	O
+being	O
+induced	O
+by	O
+several	O
+factors	O
+:	O
+excessive	O
+vibration	O
+,	O
+pressure	O
+shocks	O
+and	O
+the	O
+thermal	O
+regime	O
+of	O
+operating	O
+the	O
+pipe	B-Material
+,	O
+as	O
+well	O
+as	O
+by	O
+combinations	O
+of	O
+these	O
+factors	O
+.	O
+Corrosion	O
+was	O
+induced	O
+,	O
+in	O
+most	O
+of	O
+the	O
+cases	O
+,	O
+by	O
+a	O
+non-appropriate	O
+choice	O
+of	O
+alloys	B-Material
+while	O
+not	O
+taking	O
+into	O
+account	O
+the	O
+chemical	O
+parameters	O
+of	O
+the	O
+fluid	B-Material
+inside	O
+pipes	B-Material
+.	O
+Manufacturing	O
+defects	O
+mostly	O
+dealt	O
+with	O
+welding	O
+related	O
+problems	O
+and	O
+deviation	O
+from	O
+the	O
+design	O
+documentation	O
+during	O
+post-weld	O
+heat	O
+treatment	O
+.	O
+
+Historically	O
+,	O
+the	O
+interest	O
+in	O
+accurate	O
+measurement	O
+of	O
+DNI	O
+started	O
+decades	O
+ago	O
+.	O
+Early	O
+studies	O
+(	O
+e.g.	O
+,	O
+Linke	O
+,	O
+1931	O
+;	O
+Linke	O
+and	O
+Ulmitz	O
+,	O
+1940	O
+)	O
+identified	O
+the	O
+difficulty	O
+of	O
+separating	B-Task
+the	I-Task
+measurement	I-Task
+of	I-Task
+DNI	I-Task
+from	I-Task
+that	I-Task
+of	I-Task
+the	I-Task
+diffuse	I-Task
+irradiance	I-Task
+in	I-Task
+the	I-Task
+immediate	I-Task
+vicinity	I-Task
+of	I-Task
+the	I-Task
+sun	I-Task
+,	O
+hereafter	O
+referred	O
+to	O
+as	O
+circumsolar	O
+irradiance	O
+.	O
+Pastiels	O
+(	O
+1959	O
+)	O
+conducted	O
+a	O
+detailed	O
+study	B-Task
+of	I-Task
+the	I-Task
+geometry	I-Task
+of	I-Task
+pyrheliometers	I-Task
+,	I-Task
+and	I-Task
+how	I-Task
+that	I-Task
+geometry	I-Task
+interacted	I-Task
+with	I-Task
+circumsolar	I-Task
+radiance	I-Task
+,	O
+using	O
+simplified	O
+representations	O
+of	O
+the	O
+latter	O
+.	O
+Various	O
+communications	O
+were	O
+then	O
+presented	O
+at	O
+a	O
+WMO	O
+Task	O
+Group	O
+meeting	O
+held	O
+in	O
+Belgium	O
+in	O
+1966	O
+(	O
+WMO	O
+,	O
+1967	O
+)	O
+to	O
+improve	B-Task
+the	I-Task
+accuracy	I-Task
+of	I-Task
+pyrheliometric	I-Task
+measurements	I-Task
+,	I-Task
+including	I-Task
+estimates	I-Task
+of	I-Task
+the	I-Task
+circumsolar	I-Task
+enhancement	I-Task
+.	O
+Ångström	O
+(	O
+1961	O
+)	O
+and	O
+Ångström	O
+and	O
+Rohde	O
+(	O
+1966	O
+)	O
+later	O
+contributed	O
+to	O
+the	O
+same	O
+topic	O
+,	O
+followed	O
+years	O
+later	O
+by	O
+Major	O
+(	O
+1973	O
+,	O
+1980	O
+)	O
+.	O
+The	O
+whole	O
+issue	O
+of	O
+instrument	O
+geometry	O
+vs.	O
+circumsolar	O
+irradiance	O
+was	O
+complex	O
+and	O
+confusing	O
+at	O
+the	O
+time	O
+because	O
+different	O
+makes	O
+and	O
+models	O
+of	O
+instruments	O
+had	O
+differing	O
+geometries	O
+.	O
+This	O
+was	O
+considerably	O
+simplified	O
+after	O
+WMO	O
+issued	O
+guidelines	O
+about	O
+the	O
+recommended	O
+geometry	O
+of	O
+pyrheliometers	B-Material
+,	O
+which	O
+led	O
+to	O
+a	O
+relatively	O
+“	O
+standard	O
+”	O
+geometry	O
+used	O
+in	O
+all	O
+recent	O
+instruments	O
+.	O
+The	O
+experimental	O
+issues	O
+related	O
+to	O
+the	O
+measurement	O
+of	O
+DNI	O
+are	O
+discussed	O
+in	O
+Section	O
+3.2	O
+.	O
+
+The	O
+wind	B-Process
+speed	I-Process
+and	I-Process
+cloud	I-Process
+height	I-Process
+Markov	I-Process
+chains	I-Process
+are	O
+produced	O
+accounting	O
+for	O
+seasonal	O
+variations	O
+.	O
+A	O
+Markov	B-Process
+chain	I-Process
+is	O
+used	O
+for	O
+each	O
+variable	O
+representing	O
+each	O
+of	O
+the	O
+four	O
+seasons	O
+,	O
+capturing	O
+the	O
+variability	O
+at	O
+different	O
+times	O
+of	O
+the	O
+year	O
+,	O
+totalling	O
+four	O
+chains	O
+each	O
+.	O
+The	O
+okta	B-Process
+number	I-Process
+Markov	I-Process
+chains	I-Process
+also	O
+consider	O
+the	O
+effect	O
+of	O
+season	O
+,	O
+with	O
+the	O
+inclusion	O
+of	O
+impacts	O
+from	O
+pressure	O
+and	O
+diurnal	O
+variation	O
+.	O
+Eight	O
+okta	B-Process
+Markov	I-Process
+chains	I-Process
+are	O
+produced	O
+that	O
+are	O
+split	O
+by	O
+above	O
+and	O
+below	O
+average	O
+pressure	O
+for	O
+each	O
+season	O
+,	O
+and	O
+four	O
+additional	O
+morning	O
+okta	O
+Markov	O
+chains	O
+are	O
+produced	O
+to	O
+capture	O
+the	O
+diurnal	O
+variation	O
+for	O
+okta	O
+transitions	O
+between	O
+00:00	O
+and	O
+05:00am	O
+for	O
+each	O
+season	O
+.	O
+The	O
+intent	O
+is	O
+to	O
+capture	B-Task
+the	I-Task
+variation	I-Task
+in	I-Task
+transition	I-Task
+probability	I-Task
+that	O
+occurs	O
+as	O
+a	O
+result	O
+of	O
+weather	O
+changes	O
+due	O
+to	O
+the	O
+presence	O
+of	O
+solar	O
+energy	O
+.	O
+5am	O
+is	O
+considered	O
+the	O
+cut-off	O
+because	O
+it	O
+is	O
+a	O
+typical	O
+sunrise	O
+in	O
+the	O
+summer	O
+for	O
+the	O
+applied	O
+study	O
+locations	O
+.	O
+5h	O
+represents	O
+5	O
+okta	O
+transitions	O
+and	O
+is	O
+considered	O
+an	O
+appropriate	O
+duration	O
+for	O
+the	O
+slight	O
+propensity	O
+to	O
+shift	O
+towards	O
+an	O
+increased	O
+okta	O
+to	O
+be	O
+represented	O
+,	O
+Fig.	O
+8	O
+demonstrates	O
+the	O
+diurnal	O
+transition	O
+differences	O
+.	O
+Fig.	O
+2	O
+visually	O
+demonstrates	O
+the	O
+mean	O
+okta	B-Process
+Markov	I-Process
+chain	I-Process
+for	O
+the	O
+entire	O
+year	O
+,	O
+whilst	O
+the	O
+effect	O
+of	O
+season	O
+can	O
+be	O
+seen	O
+in	O
+Fig.	O
+11	O
+.	O
+
+In	O
+addition	O
+,	O
+the	O
+prediction	B-Task
+of	I-Task
+solar	I-Task
+cell	I-Task
+’s	I-Task
+temperature	I-Task
+is	O
+very	O
+important	O
+for	O
+the	O
+electrical	O
+characterisation	O
+of	O
+CPV	B-Process
+modules	O
+.	O
+Rodrigo	O
+et	O
+al	O
+.	O
+(	O
+2014	O
+)	O
+reviewed	O
+various	O
+methods	O
+for	O
+the	O
+calculation	B-Task
+of	I-Task
+the	I-Task
+cell	I-Task
+temperature	I-Task
+in	O
+High	B-Process
+Concentrator	I-Process
+PV	I-Process
+(	O
+HCPV	B-Process
+)	O
+modules	O
+.	O
+The	O
+methods	O
+were	O
+categorised	O
+based	O
+on	O
+:	O
+(	O
+1	O
+)	O
+heat	O
+sink	O
+temperature	O
+,	O
+(	O
+2	O
+)	O
+electrical	O
+parameters	O
+and	O
+(	O
+3	O
+)	O
+atmospheric	O
+parameters	O
+.	O
+The	O
+first	O
+two	O
+categories	O
+are	O
+based	O
+on	O
+direct	O
+measurements	O
+of	O
+CPV	B-Process
+modules	O
+in	O
+indoor	O
+or	O
+outdoor	O
+experimental	O
+setups	O
+and	O
+presented	O
+the	O
+highest	O
+degree	O
+of	O
+accuracy	O
+(	O
+Root	O
+Mean	O
+Square	O
+Error	O
+(	O
+RMSE	O
+)	O
+1.7	O
+–	O
+2.5K	O
+)	O
+.	O
+Most	O
+of	O
+the	O
+methods	O
+reviewed	O
+by	O
+Rodrigo	O
+et	O
+al	O
+.	O
+(	O
+2014	O
+)	O
+calculate	B-Task
+the	I-Task
+cell	I-Task
+temperature	I-Task
+at	O
+open-circuit	B-Process
+conditions	I-Process
+.	O
+Methods	O
+that	O
+predict	O
+the	O
+cell	O
+temperature	O
+at	O
+maximum	B-Process
+power	I-Process
+point	I-Process
+(	O
+MPP	B-Process
+)	O
+operation	O
+offer	O
+a	O
+more	O
+realistic	O
+approach	O
+since	O
+they	O
+include	O
+the	O
+electrical	B-Process
+energy	I-Process
+generation	I-Process
+of	O
+the	O
+solar	B-Material
+cells	I-Material
+(	O
+i.e.	O
+real	O
+operating	O
+conditions	O
+)	O
+;	O
+Yandt	O
+et	O
+al	O
+.	O
+(	O
+2012	O
+)	O
+described	O
+a	O
+method	O
+predicting	B-Task
+the	I-Task
+cell	I-Task
+temperature	I-Task
+at	I-Task
+MPP	I-Task
+based	O
+on	O
+electrical	O
+parameters	O
+and	O
+Fernández	O
+et	O
+al	O
+.	O
+(	O
+2014b	O
+)	O
+based	O
+on	O
+heat	O
+sink	O
+temperature	O
+with	O
+absolute	O
+RMSE	O
+0.55	O
+–	O
+1.44K	O
+.	O
+Fernández	O
+et	O
+al	O
+.	O
+(	O
+2014a	O
+)	O
+also	O
+proposed	O
+an	O
+artificial	B-Process
+neural	I-Process
+network	I-Process
+model	I-Process
+to	O
+estimate	B-Task
+the	I-Task
+cell	I-Task
+temperature	I-Task
+based	O
+on	O
+atmospheric	O
+parameters	O
+and	O
+an	O
+open-circuit	B-Process
+voltage	I-Process
+model	I-Process
+based	O
+on	O
+electrical	O
+parameters	O
+(	O
+Fernandez	O
+et	O
+al.	O
+,	O
+2013a	O
+)	O
+offering	O
+good	O
+accuracy	O
+(	O
+RMSE	O
+3.2K	O
+and	O
+2.5K	O
+respectively	O
+(	O
+Rodrigo	O
+et	O
+al.	O
+,	O
+2014	O
+))	O
+.	O
+The	O
+main	O
+disadvantage	O
+of	O
+the	O
+aforementioned	O
+methods	O
+is	O
+that	O
+an	O
+experimental	O
+setup	O
+is	O
+required	O
+to	O
+obtain	O
+the	O
+parameters	O
+used	O
+for	O
+the	O
+cell	B-Task
+temperature	I-Task
+calculation	I-Task
+.	O
+
+Our	O
+procedure	O
+does	O
+not	O
+address	O
+the	O
+issue	O
+of	O
+how	O
+parameterizations	B-Process
+can	O
+vary	O
+for	O
+different	O
+flow	B-Process
+types	O
+.	O
+However	O
+,	O
+Edeling	O
+et	O
+al	O
+.	O
+[	O
+9	O
+]	O
+carried	O
+out	O
+separate	O
+calibrations	O
+for	O
+a	O
+set	O
+of	O
+13	O
+boundary-layer	B-Process
+flows	I-Process
+.	O
+They	O
+summarized	O
+this	O
+information	O
+across	O
+calibrations	O
+by	O
+computing	O
+Highest	B-Process
+Posterior-Density	I-Process
+(	O
+HPD	B-Process
+)	O
+intervals	O
+,	O
+and	O
+subsequently	O
+represent	O
+the	O
+total	O
+solution	O
+uncertainty	O
+with	O
+a	O
+probability-box	B-Material
+(	O
+p-box	B-Material
+)	O
+.	O
+This	O
+p-box	O
+represents	O
+both	O
+parameter	O
+variability	O
+across	O
+flows	B-Process
+,	O
+and	O
+epistemic	O
+uncertainty	O
+within	O
+each	O
+calibration	O
+.	O
+A	O
+prediction	O
+of	O
+a	O
+new	O
+boundary-layer	B-Process
+flow	I-Process
+is	O
+made	O
+with	O
+uncertainty	O
+bars	O
+generated	O
+from	O
+this	O
+uncertainty	O
+information	O
+,	O
+and	O
+the	O
+resulting	O
+error	O
+estimate	O
+is	O
+shown	O
+to	O
+be	O
+consistent	O
+with	O
+measurement	O
+data	O
+.	O
+This	O
+approach	O
+is	O
+helpful	O
+,	O
+but	O
+it	O
+might	O
+be	O
+extended	O
+further	O
+by	O
+modelling	B-Process
+proximity	I-Process
+across	I-Process
+flows	I-Process
+through	O
+a	O
+distance	O
+that	O
+would	O
+relate	O
+to	O
+the	O
+flow	B-Process
+characteristics	O
+in	O
+order	O
+to	O
+borrow	O
+strength	O
+across	O
+calibrations	O
+instead	O
+of	O
+splitting	B-Process
+the	I-Process
+calibrations	I-Process
+and	I-Process
+then	I-Process
+merging	I-Process
+the	I-Process
+outcomes	I-Process
+afterwards	O
+.	O
+This	O
+is	O
+a	O
+challenging	O
+but	O
+attractive	O
+venue	O
+for	O
+future	O
+research	O
+.	O
+
+One	O
+of	O
+the	O
+most	O
+important	O
+outcomes	O
+of	O
+the	O
+comparative	B-Task
+analysis	I-Task
+is	O
+the	O
+fact	O
+that	O
+in	O
+all	O
+tested	O
+cases	O
+the	O
+use	O
+of	O
+FM	B-Process
+is	O
+associated	O
+with	O
+a	O
+dramatic	O
+reduction	O
+in	O
+computational	O
+time	O
+when	O
+compared	O
+with	O
+FE	B-Process
+,	O
+generally	O
+being	O
+in	O
+the	O
+order	O
+of	O
+seconds	O
+for	O
+FM	B-Process
+and	O
+in	O
+the	O
+order	O
+of	O
+hours	O
+for	O
+FE	B-Process
+.	O
+Table	O
+1	O
+reports	O
+the	O
+timings	O
+of	O
+the	O
+simulations	O
+for	O
+both	O
+methods	O
+.	O
+Free	O
+expansion	O
+is	O
+the	O
+fastest	O
+case	O
+,	O
+where	O
+FM	B-Process
+reaches	O
+the	O
+load-free	O
+configuration	O
+in	O
+just	O
+2	O
+s	O
+,	O
+while	O
+simulations	B-Process
+inside	O
+the	O
+vessels	B-Material
+with	O
+the	O
+diameter	O
+of	O
+around	O
+30	O
+mm	O
+take	O
+approximately	O
+30	O
+s	O
+.	O
+Most	O
+of	O
+the	O
+execution	O
+time	O
+of	O
+the	O
+FM	B-Process
+deployment	I-Process
+algorithm	I-Process
+is	O
+dedicated	O
+to	O
+the	O
+contact	O
+check	O
+and	O
+calculations	O
+of	O
+the	O
+implications	O
+the	O
+vessel	B-Material
+wall	I-Material
+has	O
+on	O
+the	O
+stent	O
+structure	O
+.	O
+Interestingly	O
+,	O
+in	O
+both	O
+methods	O
+,	O
+the	O
+highest	O
+computational	O
+time	O
+(	O
+i.e.	O
+,	O
+curved	B-Material
+vessels	I-Material
+)	O
+is	O
+not	O
+associated	O
+with	O
+the	O
+most	O
+complex	O
+geometry	O
+(	O
+i.e.	O
+,	O
+patient-specific	O
+case	O
+of	O
+aortic	O
+dissection	O
+)	O
+.	O
+Another	O
+fact	O
+worth	O
+mentioning	O
+is	O
+the	O
+relation	O
+of	O
+the	O
+computational	O
+time	O
+to	O
+the	O
+diameter	O
+of	O
+the	O
+vessel	B-Material
+in	O
+both	O
+methods	O
+.	O
+While	O
+the	O
+computational	O
+time	O
+of	O
+FM	B-Process
+appeared	O
+to	O
+be	O
+directly	O
+related	O
+to	O
+the	O
+diameter	O
+of	O
+the	O
+vessel	B-Material
+,	O
+no	O
+immediate	O
+relation	O
+was	O
+found	O
+for	O
+the	O
+FE	B-Process
+simulations	I-Process
+.	O
+Such	O
+outcome	O
+is	O
+probably	O
+related	O
+to	O
+the	O
+simplified	B-Process
+contact	I-Process
+model	I-Process
+used	O
+by	O
+FM	B-Process
+,	O
+which	O
+makes	O
+the	O
+stent-graft	B-Process
+expansion	I-Process
+terminate	O
+once	O
+the	O
+nodes	B-Material
+come	O
+in	O
+contact	O
+with	O
+the	O
+vessel	B-Material
+wall	I-Material
+.	O
+On	O
+the	O
+contrary	O
+,	O
+it	O
+is	O
+well	O
+known	O
+that	O
+the	O
+contact	B-Process
+algorithm	I-Process
+used	O
+in	O
+the	O
+FE	B-Process
+analyses	I-Process
+increases	O
+the	O
+computational	O
+cost	O
+of	O
+the	O
+simulations	B-Process
+.	O
+
+Gas	B-Process
+sorption	I-Process
+,	I-Process
+storage	I-Process
+and	I-Process
+separation	I-Process
+in	O
+carbon	B-Material
+materials	I-Material
+are	O
+mainly	O
+based	O
+on	O
+physisorption	B-Process
+on	O
+the	O
+surfaces	O
+and	O
+particularly	O
+depend	O
+on	O
+the	O
+electrostatic	B-Process
+and	I-Process
+dispersion	I-Process
+(	I-Process
+i.e.	I-Process
+,	I-Process
+vdW	I-Process
+)	I-Process
+interactions	I-Process
+.	O
+The	O
+former	O
+can	O
+be	O
+tuned	O
+by	O
+introducing	B-Process
+charge	I-Process
+variations	I-Process
+in	I-Process
+the	I-Process
+material	I-Process
+,	O
+and	O
+the	O
+latter	O
+by	O
+chemical	B-Process
+substitution	I-Process
+.	O
+The	O
+strength	O
+of	O
+the	O
+interaction	O
+is	O
+determined	O
+by	O
+the	O
+surface	O
+characteristics	O
+of	O
+the	O
+adsorbent	B-Material
+and	O
+the	O
+properties	O
+of	O
+targeted	O
+adsorbate	B-Material
+molecule	I-Material
+,	O
+including	O
+but	O
+not	O
+limited	O
+to	O
+the	O
+size	O
+and	O
+shape	O
+of	O
+the	O
+adsorbate	O
+molecule	O
+along	O
+with	O
+its	O
+polarizability	O
+,	O
+magnetic	O
+susceptibility	O
+,	O
+permanent	O
+dipole	O
+moment	O
+,	O
+and	O
+quadrupole	O
+moment	O
+.	O
+Li	O
+et	O
+al.	O
+summarise	O
+the	O
+adsorption-related	O
+physical	O
+parameters	O
+of	O
+many	O
+gas	B-Material
+or	I-Material
+vapour	I-Material
+adsorbates	I-Material
+,	O
+and	O
+herein	O
+Table	O
+1	O
+we	O
+show	O
+a	O
+few	O
+of	O
+those	O
+of	O
+interest	O
+,	O
+H2	B-Material
+,	O
+N2	B-Material
+,	O
+CO	B-Material
+,	O
+CO2	B-Material
+,	O
+CH4	B-Material
+,	O
+NH3	B-Material
+,	O
+SO2	B-Material
+and	O
+H2S	B-Material
+[	O
+90	O
+]	O
+.	O
+For	O
+instance	O
+,	O
+an	O
+adsorbent	B-Material
+with	O
+a	O
+high	O
+specific	O
+surface	O
+area	O
+is	O
+a	O
+good	O
+candidate	O
+for	O
+adsorption	O
+of	O
+a	O
+molecule	B-Material
+with	O
+high	O
+polarizability	O
+but	O
+no	O
+polarity	O
+.	O
+Adsorbents	B-Material
+with	O
+highly	O
+polarised	O
+surfaces	O
+are	O
+good	O
+for	O
+adsorbate	B-Material
+molecules	I-Material
+with	O
+a	O
+high	O
+dipole	O
+moment	O
+.	O
+The	O
+adsorbents	B-Material
+with	O
+high	O
+electric	O
+field	O
+gradient	O
+surfaces	O
+are	O
+found	O
+to	O
+be	O
+ideal	O
+for	O
+the	O
+high	B-Material
+quadrupole	I-Material
+moment	I-Material
+adsorbate	I-Material
+molecules	I-Material
+[	O
+91	O
+]	O
+.	O
+Normally	O
+,	O
+the	O
+binding	O
+or	O
+adsorption	O
+strength	O
+with	O
+a	O
+carbon	O
+nanostructure	O
+is	O
+relatively	O
+low	O
+for	O
+H2	B-Material
+and	O
+N2	B-Material
+;	O
+intermediate	O
+for	O
+CO	B-Material
+,	O
+CH4	B-Material
+and	O
+CO2	B-Material
+;	O
+and	O
+relatively	O
+high	O
+for	O
+H2S	B-Material
+,	O
+NH3	B-Material
+and	O
+H2O	B-Material
+.	O
+Thus	O
+,	O
+surface	B-Process
+modifications	I-Process
+,	O
+such	O
+as	O
+doping	B-Process
+,	O
+functionalization	B-Process
+and	O
+improving	B-Process
+the	I-Process
+pore	I-Process
+structure	I-Process
+and	I-Process
+specific	I-Process
+surface	I-Process
+area	I-Process
+of	I-Process
+nanocarbons	I-Process
+,	O
+are	O
+important	O
+to	O
+enhance	B-Task
+gas	I-Task
+adsorption	I-Task
+.	O
+For	O
+this	O
+purpose	O
+,	O
+graphene	B-Material
+offers	O
+a	O
+great	O
+scope	O
+for	O
+tailor-made	O
+carbonaceous	B-Material
+adsorbents	I-Material
+.	O
+
+When	O
+dominated	O
+by	O
+surface	B-Process
+shadowing	I-Process
+mechanisms	I-Process
+,	O
+the	O
+aggregation	B-Process
+of	I-Process
+vapor	I-Process
+particles	I-Process
+onto	I-Process
+a	I-Process
+surface	I-Process
+is	O
+a	O
+complex	O
+,	O
+non-local	O
+phenomenon	O
+.	O
+In	O
+the	O
+literature	O
+,	O
+there	O
+have	O
+been	O
+many	O
+attempts	O
+to	O
+analyze	B-Task
+the	I-Task
+growth	I-Task
+mechanism	I-Task
+by	O
+means	O
+of	O
+pure	O
+geometrical	B-Process
+considerations	I-Process
+;	O
+i.e.	O
+,	O
+by	O
+assuming	O
+that	O
+vapor	B-Material
+particles	I-Material
+arrive	O
+at	O
+the	O
+film	B-Material
+surface	I-Material
+along	O
+a	O
+single	B-Process
+angular	I-Process
+direction	I-Process
+[	O
+38,41	O
+]	O
+.	O
+Continuum	B-Process
+approaches	I-Process
+,	O
+which	O
+are	O
+based	O
+on	O
+the	O
+fact	O
+that	O
+the	O
+geometrical	B-Process
+features	I-Process
+of	O
+the	O
+film	B-Material
+(	O
+i.e.	O
+,	O
+the	O
+nanocolumns	B-Process
+)	O
+are	O
+much	O
+larger	O
+than	O
+the	O
+typical	O
+size	O
+of	O
+an	O
+atom	B-Material
+[	O
+42,266,267	O
+]	O
+,	O
+have	O
+been	O
+also	O
+explored	O
+.	O
+For	O
+instance	O
+,	O
+Poxson	O
+et	O
+al	O
+.	O
+[	O
+228	O
+]	O
+developed	O
+an	O
+analytic	B-Process
+model	I-Process
+that	O
+takes	O
+into	O
+account	O
+geometrical	B-Process
+factors	I-Process
+as	O
+well	O
+as	O
+surface	B-Process
+diffusion	I-Process
+.	O
+This	O
+model	O
+accurately	O
+predicted	O
+the	O
+porosity	O
+and	O
+deposition	O
+rate	O
+of	O
+thin	B-Material
+films	I-Material
+using	O
+a	O
+single	O
+input	O
+parameter	O
+related	O
+to	O
+the	O
+cross-sectional	O
+area	O
+of	O
+the	O
+nanocolumns	B-Material
+,	O
+the	O
+volume	O
+of	O
+material	O
+and	O
+the	O
+thickness	O
+of	O
+the	O
+film	B-Material
+.	O
+Moreover	O
+,	O
+in	O
+Ref	O
+.	O
+[	O
+39	O
+]	O
+,	O
+an	O
+analytical	B-Process
+semi-empirical	I-Process
+model	I-Process
+was	O
+presented	O
+to	O
+quantitatively	B-Task
+describe	I-Task
+the	I-Task
+aggregation	I-Task
+of	I-Task
+columnar	I-Task
+structures	I-Task
+by	O
+means	O
+of	O
+a	O
+single	O
+parameter	O
+dubbed	O
+the	O
+fan	O
+angle	O
+.	O
+This	O
+material-dependent	O
+quantity	O
+can	O
+be	O
+experimentally	O
+obtained	O
+by	O
+performing	O
+deposition	O
+at	O
+normal	O
+incidence	O
+on	O
+an	O
+imprinted	O
+groove	B-Material
+seeded	I-Material
+substrate	I-Material
+,	O
+and	O
+then	O
+measuring	O
+the	O
+increase	O
+in	O
+column	O
+diameter	O
+with	O
+film	B-Material
+thickness	O
+.	O
+This	O
+model	O
+was	O
+tested	O
+under	O
+various	O
+conditions	O
+[	O
+40	O
+]	O
+,	O
+which	O
+returned	O
+good	O
+results	O
+and	O
+an	O
+accurate	O
+prediction	B-Task
+of	I-Task
+the	I-Task
+relation	I-Task
+between	I-Task
+the	I-Task
+incident	I-Task
+angle	I-Task
+of	I-Task
+the	I-Task
+deposition	I-Task
+flux	I-Task
+and	I-Task
+the	I-Task
+tilt	I-Task
+angle	I-Task
+of	I-Task
+the	I-Task
+columns	I-Task
+for	O
+several	O
+materials	O
+.	O
+
+A	O
+bond	B-Process
+failure	I-Process
+is	O
+thought	O
+of	O
+as	O
+a	O
+micro-crack	B-Process
+nucleation	I-Process
+,	O
+specifically	O
+as	O
+a	O
+separation	B-Process
+between	I-Process
+the	I-Process
+adjacent	I-Process
+cells	I-Process
+in	I-Process
+the	I-Process
+cellular	I-Process
+structure	I-Process
+along	I-Process
+their	I-Process
+common	I-Process
+face	I-Process
+.	O
+Initially	O
+,	O
+the	O
+micro-cracks	B-Material
+may	O
+be	O
+dispersed	O
+in	O
+the	O
+model	O
+reflecting	O
+the	O
+random	O
+distribution	O
+of	O
+pore	B-Material
+sizes	O
+and	O
+the	O
+low	O
+level	O
+of	O
+interaction	O
+due	O
+to	O
+force	O
+redistribution	O
+.	O
+Interaction	O
+and	O
+coalescence	O
+may	O
+follow	O
+as	O
+the	O
+population	O
+of	O
+micro-cracks	B-Material
+increases	O
+.	O
+These	O
+situations	O
+are	O
+illustrated	O
+in	O
+Fig.	O
+3.	O
+The	O
+structure	O
+of	O
+the	O
+failed	B-Material
+surface	I-Material
+can	O
+be	O
+represented	O
+with	O
+a	O
+mathematical	B-Process
+graph	I-Process
+,	O
+where	O
+graph	O
+nodes	O
+represent	O
+failed	B-Material
+faces	I-Material
+and	O
+graph	O
+edges	O
+exist	O
+between	O
+failed	O
+faces	O
+with	O
+common	O
+triple	O
+line	O
+in	O
+the	O
+cellular	B-Material
+structure	I-Material
+,	O
+i.e.	O
+where	O
+two	O
+micro-cracks	B-Material
+formed	O
+a	O
+continuous	O
+larger	O
+crack	B-Material
+.	O
+With	O
+reference	O
+to	O
+Fig.	O
+3	O
+,	O
+each	O
+failed	B-Material
+face	I-Material
+is	O
+a	O
+graph	O
+node	O
+and	O
+each	O
+pair	O
+of	O
+neighbouring	O
+failed	B-Material
+faces	I-Material
+is	O
+a	O
+graph	O
+edge	O
+.	O
+
+Half	B-Material
+metallic	I-Material
+ferromagnets	I-Material
+(	O
+HMF	B-Material
+)	O
+have	O
+attracted	O
+enormous	O
+interest	O
+due	O
+to	O
+their	O
+applications	O
+in	O
+spintronic	B-Task
+devices	I-Task
+[	O
+1	O
+]	O
+.	O
+Dilute	B-Material
+magnetic	I-Material
+semiconductors	I-Material
+(	O
+DMSs	B-Material
+)	O
+are	O
+considered	O
+to	O
+be	O
+the	O
+best	O
+materials	B-Material
+to	I-Material
+show	I-Material
+half	I-Material
+metallicity	I-Material
+.	O
+These	O
+materials	O
+have	O
+two	O
+components	O
+,	O
+one	O
+being	O
+a	O
+semiconducting	B-Material
+material	I-Material
+with	O
+diamagnetic	O
+properties	O
+while	O
+the	O
+other	O
+is	O
+a	O
+magnetic	B-Material
+dopant	I-Material
+such	O
+as	O
+transition	B-Material
+metal	I-Material
+having	O
+un-paired	B-Material
+d	I-Material
+electrons	I-Material
+[	O
+2	O
+]	O
+.	O
+The	O
+major	O
+advantage	O
+of	O
+these	O
+materials	O
+is	O
+utilization	B-Process
+of	I-Process
+electron	I-Process
+'s	I-Process
+spin	I-Process
+as	I-Process
+information	I-Process
+carrier	I-Process
+since	O
+advanced	O
+functionalities	O
+in	O
+spintronic	B-Task
+devices	I-Task
+can	O
+be	O
+viable	O
+by	O
+the	O
+use	O
+of	O
+spin	O
+degree	O
+of	O
+freedom	O
+along	O
+with	O
+the	O
+charge	O
+of	O
+electrons	B-Material
+[	O
+3	O
+]	O
+.	O
+The	O
+major	O
+issue	O
+regarding	O
+the	O
+applicability	O
+of	O
+these	O
+materials	O
+is	O
+to	O
+enhance	B-Task
+the	I-Task
+Curie	I-Task
+temperature	I-Task
+above	I-Task
+room	I-Task
+temperature	I-Task
+.	O
+That	O
+'s	O
+why	O
+the	O
+research	O
+interest	O
+shifted	O
+towards	O
+large	B-Material
+band	I-Material
+gap	I-Material
+materials	I-Material
+.	O
+A	O
+lot	O
+of	O
+work	O
+has	O
+been	O
+reported	O
+on	O
+DMSs	B-Material
+with	O
+different	O
+II	B-Material
+–	I-Material
+VI	I-Material
+and	I-Material
+III	I-Material
+–	I-Material
+V	I-Material
+semiconductors	I-Material
+as	O
+host	B-Material
+material	I-Material
+such	O
+as	O
+,	O
+ZnS	B-Material
+,	O
+CdS	B-Material
+,	O
+GaN	B-Material
+,	O
+ZnO	B-Material
+,	O
+ZnSe	B-Material
+,	O
+ZnTe	B-Material
+,	O
+TiO2	B-Material
+,	O
+SnO2	B-Material
+[	O
+4	O
+–	O
+12	O
+]	O
+.	O
+
+It	O
+has	O
+been	O
+known	O
+[	O
+9,14,18,22	O
+]	O
+that	O
+the	O
+fragmentation	B-Process
+processes	I-Process
+in	O
+polyatomic	B-Material
+molecules	I-Material
+induced	O
+by	O
+an	O
+intense	B-Material
+ultrafast	I-Material
+laser	I-Material
+field	I-Material
+can	O
+sometimes	O
+exhibit	O
+sensitive	O
+dependence	O
+on	O
+the	O
+instantaneous	O
+phase	O
+characteristics	O
+of	O
+the	O
+laser	O
+field	O
+.	O
+Depending	O
+on	O
+the	O
+change	O
+in	O
+sign	O
+the	O
+chirped	B-Material
+laser	I-Material
+pulses	I-Material
+,	O
+fragmentation	B-Task
+could	O
+be	O
+either	O
+enhanced	O
+or	O
+suppressed	O
+[	O
+14,18,22	O
+]	O
+.	O
+Controlling	O
+the	O
+outcome	O
+of	O
+such	O
+laser	B-Process
+induced	I-Process
+molecular	I-Process
+fragmentation	I-Process
+with	O
+chirped	B-Material
+femtosecond	I-Material
+laser	I-Material
+pulses	I-Material
+has	O
+brought	O
+forth	O
+a	O
+number	O
+of	O
+experimental	O
+and	O
+theoretical	O
+effects	O
+in	O
+the	O
+recent	O
+years	O
+.	O
+However	O
+,	O
+efforts	O
+are	O
+continuing	O
+for	O
+a	O
+specific	O
+fragment	B-Task
+channel	I-Task
+enhancement	I-Task
+,	O
+which	O
+is	O
+difficult	O
+since	O
+it	O
+also	O
+is	O
+a	O
+function	O
+of	O
+the	O
+molecular	B-Process
+system	I-Process
+under	O
+study	O
+[	O
+20,22	O
+–	O
+24	O
+]	O
+.	O
+Here	O
+we	O
+report	O
+the	O
+observation	B-Task
+of	I-Task
+a	I-Task
+coherently	I-Task
+enhanced	I-Task
+fragmentation	I-Task
+pathway	I-Task
+of	O
+n-propyl	B-Material
+benzene	I-Material
+,	O
+which	O
+seems	O
+to	O
+have	O
+such	O
+specific	O
+fragmentation	B-Material
+channel	I-Material
+available	O
+.	O
+We	O
+found	O
+that	O
+for	O
+n-propyl	B-Material
+benzene	I-Material
+,	O
+the	O
+relative	O
+yield	O
+of	O
+C3H3	B-Material
++	I-Material
+is	O
+extremely	O
+sensitive	O
+to	O
+the	O
+phase	O
+of	O
+the	O
+laser	B-Material
+pulse	I-Material
+as	O
+compared	O
+to	O
+any	O
+of	O
+the	O
+other	O
+possible	O
+channels	B-Material
+.	O
+In	O
+fact	O
+,	O
+there	O
+is	O
+almost	O
+an	O
+order	O
+of	O
+magnitude	O
+enhancement	O
+in	O
+the	O
+yield	O
+of	O
+C3H3	B-Material
++	I-Material
+when	O
+negatively	B-Material
+chirped	I-Material
+pulses	I-Material
+are	O
+used	O
+,	O
+while	O
+there	O
+is	O
+no	O
+effect	O
+with	O
+the	O
+positive	B-Material
+chirp	I-Material
+.	O
+Moreover	O
+,	O
+the	O
+relative	O
+yield	O
+of	O
+all	O
+the	O
+other	O
+heavier	B-Material
+fragment	I-Material
+ions	I-Material
+resulting	O
+from	O
+interaction	O
+of	O
+the	O
+strong	O
+field	O
+with	O
+the	O
+molecule	B-Material
+is	O
+not	O
+sensitive	O
+to	O
+the	O
+sign	O
+of	O
+the	O
+chirp	B-Material
+,	O
+within	O
+the	O
+noise	O
+level	O
+.	O
+
+The	O
+vibrational	O
+spectra	O
+of	O
+l-cysteine	B-Material
+have	O
+been	O
+recorded	O
+and	O
+assigned	O
+in	O
+both	O
+solution	O
+[	O
+8,9	O
+]	O
+and	O
+the	O
+solid	O
+state	O
+[	O
+10	O
+–	O
+14	O
+]	O
+.	O
+Spectral	B-Process
+assignments	I-Process
+have	O
+been	O
+made	O
+using	O
+empirical	B-Process
+force	I-Process
+fields	I-Process
+[	O
+15	O
+]	O
+,	O
+Hartree	B-Process
+–	I-Process
+Fock	I-Process
+calculations	I-Process
+[	O
+10,16,17	O
+]	O
+based	O
+on	O
+the	O
+isolated	B-Process
+molecule	I-Process
+approximation	I-Process
+.	O
+For	O
+systems	O
+that	O
+exhibit	O
+strong	O
+intermolecular	O
+interactions	O
+,	O
+this	O
+approximation	O
+often	O
+leads	O
+to	O
+poor	O
+agreement	O
+between	O
+experiment	O
+and	O
+theory	O
+.	O
+A	O
+striking	O
+example	O
+is	O
+purine	B-Material
+[	O
+18	O
+]	O
+,	O
+where	O
+a	O
+study	B-Task
+of	I-Task
+the	I-Task
+solid	I-Task
+state	I-Task
+vibrational	I-Task
+spectra	I-Task
+by	O
+isolated	B-Process
+molecule	I-Process
+and	I-Process
+periodic	I-Process
+calculations	I-Process
+,	O
+gave	O
+almost	O
+quantitative	O
+agreement	O
+between	O
+theory	O
+and	O
+experiment	O
+for	O
+the	O
+latter	O
+,	O
+whereas	O
+the	O
+former	O
+gave	O
+only	O
+modest	O
+agreement	O
+and	O
+was	O
+unable	O
+to	O
+distinguish	O
+between	O
+the	O
+tautomers	B-Material
+.	O
+In	O
+the	O
+present	O
+case	O
+,	O
+where	O
+the	O
+structure	O
+consists	O
+of	O
+ions	B-Material
+linked	O
+by	O
+hydrogen	B-Material
+bonds	O
+,	O
+periodic	B-Process
+calculations	I-Process
+based	O
+on	O
+the	O
+complete	B-Material
+primitive	I-Material
+cell	I-Material
+are	O
+essential	O
+[	O
+19	O
+]	O
+.	O
+The	O
+only	O
+work	O
+[	O
+20	O
+]	O
+that	O
+includes	O
+some	O
+solid	O
+state	O
+effects	O
+used	O
+molecular	B-Process
+dynamics	I-Process
+but	O
+from	O
+which	O
+it	O
+is	O
+difficult	O
+to	O
+extract	O
+assignments	O
+.	O
+The	O
+aim	O
+of	O
+this	O
+paper	O
+is	O
+to	O
+provide	B-Task
+a	I-Task
+complete	I-Task
+assignment	I-Task
+of	I-Task
+the	I-Task
+vibrational	I-Task
+spectra	I-Task
+of	I-Task
+l-cysteine	I-Task
+in	O
+both	O
+the	O
+orthorhombic	O
+and	O
+monoclinic	O
+forms	O
+by	O
+the	O
+use	O
+of	O
+a	O
+combination	O
+of	O
+computational	B-Process
+and	I-Process
+experimental	I-Process
+methods	I-Process
+.	O
+
+It	O
+is	O
+critical	O
+to	O
+the	O
+success	O
+of	O
+the	O
+NPD	B-Process
+technique	I-Process
+that	O
+the	O
+MOF	B-Material
+complex	I-Material
+adsorbs	O
+a	O
+significant	O
+amount	O
+of	O
+D2	B-Material
+to	O
+boost	O
+the	O
+observed	O
+signal	O
+.	O
+This	O
+technique	O
+therefore	O
+has	O
+disadvantages	O
+when	O
+studying	O
+the	O
+binding	B-Process
+interaction	I-Process
+within	O
+MOFs	B-Material
+with	O
+low	O
+uptakes	O
+.	O
+Furthermore	O
+,	O
+static	B-Task
+crystallographic	I-Task
+studies	I-Task
+cannot	O
+provide	O
+insights	O
+into	O
+the	O
+dynamics	O
+of	O
+the	O
+adsorbed	B-Material
+gas	I-Material
+molecules	I-Material
+.	O
+Thus	O
+,	O
+it	O
+is	O
+very	O
+challenging	O
+to	O
+probe	O
+experimentally	O
+the	O
+H2	B-Process
+binding	I-Process
+interactions	I-Process
+within	O
+a	O
+porous	O
+host	O
+system	O
+which	O
+has	O
+very	O
+low	O
+gas	B-Material
+uptake	O
+due	O
+to	O
+the	O
+lack	O
+of	O
+suitable	O
+characterisation	B-Process
+techniques	I-Process
+.	O
+We	O
+report	O
+herein	O
+the	O
+application	O
+of	O
+the	O
+in	B-Process
+situ	I-Process
+inelastic	I-Process
+neutron	I-Process
+scattering	I-Process
+(	O
+INS	B-Process
+)	O
+technique	O
+to	O
+permit	B-Task
+direct	I-Task
+observation	I-Task
+of	I-Task
+the	I-Task
+dynamics	I-Task
+of	I-Task
+the	I-Task
+binding	I-Task
+interactions	I-Task
+between	O
+adsorbed	B-Material
+H2	I-Material
+molecules	I-Material
+and	O
+an	O
+aluminium-based	B-Material
+porous	I-Material
+MOF	I-Material
+,	O
+NOTT-300	B-Material
+,	O
+exhibiting	O
+moderate	O
+porosity	O
+,	O
+narrow	O
+pore	O
+window	O
+and	O
+very	O
+low	O
+uptake	O
+of	O
+H2	B-Material
+.	O
+This	O
+neutron	B-Task
+spectroscopy	I-Task
+study	O
+reveals	O
+that	O
+adsorbed	B-Material
+H2	I-Material
+molecules	I-Material
+do	O
+not	O
+interact	O
+with	O
+the	O
+organic	B-Material
+ligand	I-Material
+within	O
+the	O
+pore	O
+channels	O
+,	O
+and	O
+form	O
+very	O
+weak	O
+interactions	O
+with	O
+[	B-Material
+Al	I-Material
+(	I-Material
+OH	I-Material
+)	I-Material
+2O4	I-Material
+]	I-Material
+moieties	I-Material
+via	O
+a	O
+type	O
+of	O
+through-spacing	B-Process
+interaction	I-Process
+(	O
+Al-O	B-Process
+⋯	I-Process
+H2	I-Process
+)	O
+.	O
+Interestingly	O
+,	O
+the	O
+very	O
+low	O
+H2	B-Process
+adsorption	I-Process
+has	O
+been	O
+successfully	O
+characterised	O
+as	O
+weak	B-Process
+binding	I-Process
+interactions	I-Process
+and	O
+,	O
+for	O
+the	O
+first	O
+time	O
+,	O
+we	O
+have	O
+found	O
+that	O
+the	O
+adsorbed	B-Material
+H2	I-Material
+in	O
+the	O
+pore	O
+channel	O
+has	O
+a	O
+liquid	B-Material
+type	O
+recoil	O
+motion	O
+at	O
+5K	O
+(	O
+below	O
+its	O
+melting	O
+point	O
+)	O
+as	O
+a	O
+direct	O
+result	O
+of	O
+this	O
+weak	B-Process
+interaction	I-Process
+to	O
+the	O
+MOF	B-Material
+host	O
+.	O
+
+The	O
+sodium	B-Material
+trimer	I-Material
+has	O
+a	O
+long	O
+history	O
+of	O
+theoretical	O
+and	O
+experimental	O
+studies	O
+.	O
+A	O
+pioneering	O
+theoretical	O
+paper	O
+of	O
+Martin	O
+and	O
+Davidson	O
+published	O
+in	O
+1978	O
+showed	O
+that	O
+the	O
+obtuse	B-Process
+isosceles	I-Process
+geometry	I-Process
+is	O
+lower	O
+in	O
+energy	O
+than	O
+the	O
+linear	B-Process
+conformation	I-Process
+[	O
+6	O
+]	O
+.	O
+Several	O
+extended	O
+PES	B-Process
+scans	I-Process
+of	O
+Na3	B-Material
+and	O
+other	O
+alkali	B-Material
+trimers	I-Material
+followed	O
+this	O
+initial	O
+study	O
+,	O
+employing	O
+DFT	B-Process
+[	O
+7	O
+]	O
+,	O
+complete	B-Process
+active	I-Process
+space	I-Process
+SCF	I-Process
+[	O
+8	O
+]	O
+,	O
+or	O
+a	O
+configuration	B-Process
+interaction	I-Process
+approach	I-Process
+based	O
+on	O
+valence	B-Process
+bond	I-Process
+wave	I-Process
+functions	I-Process
+[	O
+9	O
+]	O
+.	O
+Recently	O
+,	O
+the	O
+applicability	O
+of	O
+density	B-Process
+functional	I-Process
+theory	I-Process
+(	O
+DFT	B-Process
+)	O
+to	O
+JT-distorted	B-Process
+systems	I-Process
+has	O
+also	O
+been	O
+tested	O
+for	O
+Na3	B-Material
+[	O
+10	O
+]	O
+,	O
+and	O
+the	O
+B-X	B-Process
+transition	I-Process
+has	O
+been	O
+revisited	O
+as	O
+well	O
+,	O
+applying	O
+state-averaged	B-Process
+multi-reference	I-Process
+configuration	I-Process
+interaction	I-Process
+with	O
+a	O
+large	O
+active	O
+space	O
+in	O
+order	O
+to	O
+derive	B-Task
+more	I-Task
+accurate	I-Task
+non-adiabatic	I-Task
+coupling	I-Task
+terms	I-Task
+for	O
+an	O
+improved	O
+interpretation	O
+of	O
+photoabsorption	B-Material
+spectra	I-Material
+[	O
+11	O
+–	O
+13	O
+]	O
+.	O
+
+Alternatively	O
+to	O
+H-atom	B-Process
+photodetachment	I-Process
+from	O
+the	O
+intermediate	B-Material
+radicals	I-Material
+,	O
+the	O
+latter	O
+may	O
+serve	O
+as	O
+reducing	B-Material
+agents	I-Material
+.	O
+Evidence	O
+has	O
+been	O
+reported	O
+in	O
+recent	O
+years	O
+that	O
+the	O
+pyridinyl	B-Material
+radical	I-Material
+(	O
+PyH	B-Material
+)	O
+is	O
+an	O
+exceptionally	O
+strong	O
+reducing	B-Material
+agent	I-Material
+which	O
+can	O
+even	O
+reduce	O
+CO2	B-Material
+to	O
+formaldehyde	B-Material
+,	O
+formic	B-Material
+acid	I-Material
+or	O
+methanol	B-Material
+with	O
+suitable	O
+catalyzers	B-Material
+[	O
+27	O
+–	O
+29	O
+]	O
+,	O
+albeit	O
+the	O
+mechanisms	O
+of	O
+these	O
+reactions	O
+are	O
+currently	O
+poorly	O
+understood	O
+[	O
+30	O
+–	O
+32	O
+]	O
+.	O
+The	O
+theoretically	O
+predicted	O
+dissociation	O
+thresholds	O
+of	O
+the	O
+AcH	B-Material
+,	I-Material
+AOH	I-Material
+and	I-Material
+BAH	I-Material
+radicals	I-Material
+are	O
+about	O
+2.7eV	O
+,	O
+2.5eV	O
+and	O
+3.0eV	O
+,	O
+respectively	O
+(	O
+see	O
+Fig.	O
+4	O
+)	O
+,	O
+while	O
+the	O
+predicted	O
+dissociation	O
+threshold	O
+of	O
+the	O
+pyridinyl	B-Material
+radical	I-Material
+is	O
+much	O
+lower	O
+,	O
+about	O
+1.7eV	O
+[	O
+1	O
+]	O
+.	O
+Pyridinyl	B-Material
+is	O
+thus	O
+a	O
+significantly	O
+stronger	O
+reductant	B-Material
+than	O
+acridinyl	B-Material
+and	O
+related	O
+radicals	B-Material
+.	O
+It	O
+is	O
+therefore	O
+not	O
+expected	O
+that	O
+the	O
+latter	O
+will	O
+be	O
+able	O
+to	O
+reduce	B-Task
+carbon	I-Task
+dioxide	I-Task
+in	I-Task
+dark	I-Task
+reactions	I-Task
+.	O
+
+As	O
+already	O
+discussed	O
+,	O
+in	O
+dilute	B-Material
+flows	I-Material
+the	O
+choice	O
+between	O
+the	O
+hard	B-Process
+sphere	I-Process
+and	I-Process
+soft	I-Process
+sphere	I-Process
+models	I-Process
+largely	O
+depends	O
+on	O
+the	O
+computational	O
+time	O
+spent	O
+to	O
+solve	B-Task
+the	I-Task
+particle	I-Task
+equation	I-Task
+of	I-Task
+motion	I-Task
+.	O
+For	O
+very	O
+dilute	B-Material
+flows	I-Material
+,	O
+the	O
+hard	B-Process
+sphere	I-Process
+model	I-Process
+is	O
+the	O
+most	O
+natural	O
+choice	O
+.	O
+However	O
+,	O
+when	O
+the	O
+collisions	O
+can	O
+no	O
+longer	O
+be	O
+assumed	O
+as	O
+binary	O
+and	O
+instantaneous	O
+,	O
+the	O
+soft	B-Process
+sphere	I-Process
+model	I-Process
+is	O
+the	O
+only	O
+realistic	O
+option	O
+.	O
+It	O
+is	O
+interesting	O
+to	O
+know	O
+whether	O
+the	O
+choice	O
+of	O
+the	O
+collision	B-Process
+model	I-Process
+affects	O
+the	O
+statistics	O
+.	O
+Fig.	O
+14	O
+compares	O
+the	O
+mean	O
+velocity	O
+obtained	O
+from	O
+both	O
+models	O
+with	O
+the	O
+experimental	O
+data	O
+.	O
+The	O
+same	O
+comparison	O
+is	O
+performed	O
+for	O
+the	O
+smooth	B-Material
+walls	I-Material
+.	O
+The	O
+differences	O
+between	O
+the	O
+hard	B-Process
+and	I-Process
+soft	I-Process
+sphere	I-Process
+models	I-Process
+for	O
+the	O
+smooth	B-Material
+walls	I-Material
+are	O
+almost	O
+negligible	O
+.	O
+However	O
+,	O
+the	O
+differences	O
+between	O
+the	O
+hard	B-Process
+and	I-Process
+soft	I-Process
+sphere	I-Process
+models	I-Process
+for	O
+the	O
+rough	B-Material
+walls	I-Material
+are	O
+minor	O
+.	O
+This	O
+is	O
+because	O
+the	O
+rough	B-Task
+wall	I-Task
+treatment	I-Task
+in	O
+the	O
+soft	B-Process
+sphere	I-Process
+implementation	I-Process
+adds	O
+extra	O
+virtual	B-Material
+walls	I-Material
+during	O
+the	O
+collision	O
+of	O
+a	O
+particle	B-Material
+with	O
+a	O
+wall	B-Material
+,	O
+which	O
+is	O
+a	O
+more	O
+realistic	O
+representation	O
+of	O
+a	O
+rough	B-Material
+wall	I-Material
+compared	O
+to	O
+the	O
+hard	B-Task
+sphere	I-Task
+rough	I-Task
+wall	I-Task
+treatment	I-Task
+where	O
+one	O
+random	B-Material
+wall	I-Material
+is	O
+considered	O
+.	O
+This	O
+is	O
+because	O
+,	O
+a	O
+soft	B-Process
+sphere	I-Process
+collision	I-Process
+is	O
+not	O
+instantaneous	O
+and	O
+occurs	O
+over	O
+a	O
+finite	O
+amount	O
+of	O
+time	O
+.	O
+Similarly	O
+,	O
+the	O
+same	O
+effects	O
+are	O
+observed	O
+on	O
+the	O
+fluid	B-Material
+statistics	O
+.	O
+However	O
+,	O
+Fig.	O
+15	O
+,	O
+which	O
+compares	O
+the	O
+particle	B-Material
+velocity	O
+fluctuations	O
+,	O
+shows	O
+that	O
+the	O
+differences	O
+are	O
+somewhat	O
+larger	O
+.	O
+Additionally	O
+,	O
+the	O
+differences	O
+in	O
+both	O
+particle	O
+mean	O
+and	O
+RMS	O
+velocity	O
+profiles	O
+are	O
+because	O
+the	O
+hard	B-Process
+sphere	I-Process
+collisions	I-Process
+are	O
+unfortunately	O
+heavily	O
+dependent	O
+on	O
+the	O
+tangential	O
+coefficient	O
+of	O
+restitution	O
+(	O
+ψ	O
+)	O
+;	O
+the	O
+effects	O
+by	O
+varying	O
+this	O
+quantity	O
+are	O
+shown	O
+in	O
+Figs.	O
+16	O
+and	O
+17	O
+.	O
+
+In	O
+the	O
+current	O
+CLSVOF	B-Process
+method	I-Process
+,	O
+the	O
+normal	O
+vector	O
+is	O
+calculated	O
+directly	O
+by	O
+discretising	O
+the	O
+LS	B-Process
+gradient	O
+using	O
+a	O
+finite	B-Process
+difference	I-Process
+scheme	I-Process
+.	O
+By	O
+appropriately	O
+choosing	O
+one	O
+of	O
+three	O
+finite	B-Process
+difference	I-Process
+schemes	I-Process
+(	O
+central	B-Process
+,	I-Process
+forward	I-Process
+,	I-Process
+or	I-Process
+backward	I-Process
+differencing	I-Process
+)	O
+,	O
+it	O
+has	O
+been	O
+demonstrated	O
+that	O
+thin	B-Material
+liquid	I-Material
+ligaments	I-Material
+can	O
+be	O
+well	O
+resolved	O
+see	O
+Xiao	O
+(	O
+2012	O
+)	O
+.	O
+Although	O
+a	O
+high	B-Process
+order	I-Process
+discretisation	I-Process
+scheme	I-Process
+(	O
+e.g.	O
+5th	B-Process
+order	I-Process
+WENO	I-Process
+)	O
+has	O
+been	O
+found	O
+necessary	O
+for	O
+LS	B-Process
+evolution	O
+in	O
+pure	O
+LS	B-Process
+methods	I-Process
+to	O
+reduce	B-Task
+mass	I-Task
+error	I-Task
+,	O
+low	B-Process
+order	I-Process
+LS	I-Process
+discretisation	I-Process
+schemes	I-Process
+(	O
+2nd	O
+order	O
+is	O
+used	O
+here	O
+)	O
+can	O
+produce	O
+accurate	O
+results	O
+when	O
+the	O
+LS	O
+equation	O
+is	O
+solved	O
+and	O
+constrained	O
+as	O
+indicated	O
+above	O
+in	O
+a	O
+CLSVOF	B-Process
+method	I-Process
+(	O
+see	O
+Xiao	O
+,	O
+2012	O
+)	O
+,	O
+since	O
+the	O
+VOF	B-Process
+method	I-Process
+maintains	O
+2nd	O
+order	O
+accuracy	O
+.	O
+This	O
+is	O
+a	O
+further	O
+reason	O
+to	O
+adopt	O
+the	O
+CLSVOF	B-Process
+method	I-Process
+,	O
+which	O
+has	O
+been	O
+used	O
+for	O
+all	O
+the	O
+following	O
+simulations	B-Task
+of	I-Task
+liquid	I-Task
+jet	I-Task
+primary	I-Task
+breakup	I-Task
+.	O
+
+The	O
+aim	O
+of	O
+this	O
+paper	O
+is	O
+to	O
+investigate	B-Task
+the	I-Task
+influence	I-Task
+of	I-Task
+the	I-Task
+particle	I-Task
+shape	I-Task
+on	I-Task
+interacting	I-Task
+particles	I-Task
+flowing	I-Task
+in	I-Task
+a	I-Task
+horizontal	I-Task
+turbulent	I-Task
+channel	I-Task
+flow	I-Task
+,	O
+for	O
+particles	O
+with	O
+a	O
+significant	O
+Stokes	O
+number	O
+.	O
+To	O
+achieve	O
+this	O
+,	O
+large	B-Process
+eddy	I-Process
+simulations	I-Process
+(	O
+LES	B-Process
+)	O
+of	O
+a	O
+horizontal	B-Process
+turbulent	I-Process
+channel	I-Process
+flow	I-Process
+laden	O
+with	O
+five	O
+different	O
+particle	B-Material
+shapes	O
+,	O
+incorporating	O
+the	O
+drag	B-Process
+,	I-Process
+lift	I-Process
+and	I-Process
+toque	I-Process
+model	I-Process
+derived	O
+in	O
+Zastawny	O
+et	O
+al	O
+.	O
+(	O
+2012	O
+)	O
+,	O
+are	O
+performed	O
+.	O
+The	O
+well-documented	O
+horizontal	B-Process
+channel	I-Process
+flow	I-Process
+case	O
+described	O
+in	O
+Kussin	O
+and	O
+Sommerfeld	O
+(	O
+2002	O
+)	O
+,	O
+who	O
+study	O
+spherical	B-Material
+particles	I-Material
+,	O
+is	O
+used	O
+as	O
+a	O
+reference	O
+case	O
+.	O
+The	O
+measurements	O
+in	O
+their	O
+work	O
+was	O
+done	O
+with	O
+phase	B-Process
+Doppler	I-Process
+anemometry	I-Process
+(	O
+PDA	B-Process
+)	O
+,	O
+to	O
+measure	O
+the	O
+fluid	B-Material
+and	O
+particle	B-Material
+velocity	O
+simultaneously	O
+.	O
+The	O
+numerical	B-Process
+framework	I-Process
+applied	O
+in	O
+this	O
+paper	O
+has	O
+been	O
+previously	O
+validated	O
+for	O
+spherical	B-Material
+particles	I-Material
+in	O
+Mallouppas	O
+and	O
+van	O
+Wachem	O
+(	O
+2013	O
+)	O
+.	O
+In	O
+that	O
+paper	O
+,	O
+it	O
+is	O
+shown	O
+that	O
+the	O
+comprehensive	B-Process
+discrete	I-Process
+element	I-Process
+model	I-Process
+(	O
+DEM	B-Process
+)	O
+is	O
+more	O
+accurate	O
+in	O
+determining	B-Task
+the	I-Task
+behaviour	I-Task
+of	I-Task
+the	I-Task
+particles	I-Task
+in	I-Task
+this	I-Task
+horizontal	I-Task
+gas	I-Task
+–	I-Task
+solid	I-Task
+channel	I-Task
+flow	I-Task
+that	O
+the	O
+hard-sphere	B-Process
+model	I-Process
+.	O
+Moreover	O
+,	O
+this	O
+paper	O
+showed	O
+that	O
+the	O
+fluid	B-Material
+mechanics	O
+are	O
+accurately	O
+modelled	O
+using	O
+the	O
+LES	B-Process
+framework	I-Process
+.	O
+In	O
+the	O
+current	O
+paper	O
+,	O
+this	O
+framework	O
+is	O
+extended	O
+to	O
+account	O
+for	O
+non-spherical	B-Material
+particles	I-Material
+.	O
+
+The	O
+Statistical	B-Process
+Associating	I-Process
+Fluid	I-Process
+Theory	I-Process
+(	O
+SAFT	B-Process
+)	O
+is	O
+a	O
+well-developed	O
+perturbation	B-Process
+theory	I-Process
+used	O
+to	O
+describe	O
+quantitatively	O
+the	O
+volumetric	O
+properties	O
+of	O
+fluids	B-Material
+.	O
+The	O
+reader	O
+is	O
+referred	O
+to	O
+several	O
+reviews	O
+on	O
+the	O
+topic	O
+which	O
+describe	O
+the	O
+various	O
+stages	O
+of	O
+its	O
+development	O
+and	O
+the	O
+multiple	O
+versions	O
+available	O
+[	O
+50	O
+–	O
+53	O
+]	O
+.	O
+The	O
+fundamental	O
+difference	O
+between	O
+the	O
+versions	O
+is	O
+in	O
+the	O
+underlying	O
+intermolecular	B-Process
+potential	I-Process
+employed	O
+to	O
+describe	O
+the	O
+unbounded	B-Material
+constituent	I-Material
+particles	I-Material
+.	O
+Hard	B-Material
+spheres	I-Material
+,	O
+square	B-Material
+well	I-Material
+fluids	I-Material
+,	O
+LJ	B-Material
+fluids	I-Material
+,	O
+argon	B-Material
+,	O
+alkanes	B-Material
+have	O
+all	O
+been	O
+employed	O
+as	O
+reference	B-Material
+fluids	I-Material
+in	O
+the	O
+different	O
+incarnations	O
+of	O
+SAFT	B-Process
+.	O
+For	O
+the	O
+purpose	O
+of	O
+this	O
+work	O
+we	O
+will	O
+center	O
+on	O
+a	O
+particular	O
+version	O
+of	O
+the	O
+SAFT	B-Process
+EoS	I-Process
+,	O
+i.e.	O
+the	O
+SAFT-VR	B-Process
+Mie	I-Process
+recently	O
+proposed	O
+by	O
+Laffitte	O
+et	O
+al	O
+.	O
+[	O
+54	O
+]	O
+and	O
+expanded	O
+into	O
+a	O
+group	B-Process
+contribution	I-Process
+approach	I-Process
+,	O
+SAFT-γ	B-Process
+,	O
+by	O
+Papaioannou	O
+et	O
+al	O
+.	O
+[	O
+55	O
+]	O
+.	O
+This	O
+particular	O
+version	O
+of	O
+SAFT	B-Process
+provides	O
+a	O
+closed	B-Process
+form	I-Process
+EoS	I-Process
+that	O
+describes	O
+the	O
+macroscopical	O
+properties	O
+of	O
+the	O
+Mie	B-Process
+potential	I-Process
+[	O
+56	O
+]	O
+,	O
+also	O
+known	O
+as	O
+the	O
+(	B-Process
+m,n	I-Process
+)	I-Process
+potential	I-Process
+;	O
+a	O
+generalized	O
+form	O
+of	O
+the	O
+LJ	B-Process
+potential	I-Process
+(	O
+albeit	O
+predating	O
+it	O
+by	O
+decades	O
+)	O
+.	O
+The	O
+Mie	B-Process
+potential	I-Process
+has	O
+the	O
+form	O
+(	O
+1	O
+)	O
+ϕ	O
+(	O
+r	O
+)=	O
+Cεσrλr	O
+−	O
+σrλawhere	O
+C	O
+is	O
+an	O
+analytical	O
+function	O
+of	O
+the	O
+repulsive	O
+and	O
+attractive	O
+exponents	O
+,	O
+λa	O
+and	O
+λr	O
+,	O
+respectively	O
+,	O
+σ	O
+is	O
+a	O
+parameter	O
+that	O
+defines	O
+the	O
+length	O
+scale	O
+and	O
+is	O
+loosely	O
+related	O
+to	O
+the	O
+average	O
+diameter	O
+of	O
+a	O
+Mie	O
+bead	B-Material
+;	O
+ɛ	O
+defines	O
+the	O
+energy	O
+scale	O
+and	O
+corresponds	O
+to	O
+the	O
+minimum	O
+potential	O
+energy	O
+between	O
+two	O
+isolated	O
+beads	B-Material
+;	O
+expressed	O
+here	O
+as	O
+a	O
+ratio	O
+to	O
+the	O
+Boltzmann	O
+constant	O
+,	O
+kB	O
+.	O
+The	O
+Mie	O
+function	O
+,	O
+as	O
+written	O
+above	O
+,	O
+deceivingly	O
+suggests	O
+that	O
+four	O
+parameters	O
+are	O
+needed	O
+to	O
+characterize	O
+the	O
+behaviour	O
+of	O
+an	O
+isotropic	B-Material
+molecule	I-Material
+,	O
+however	O
+the	O
+exponents	O
+λa	O
+and	O
+λr	O
+are	O
+intimately	O
+related	O
+,	O
+and	O
+for	O
+fluid	B-Material
+phase	O
+equilibria	O
+,	O
+one	O
+needs	O
+not	O
+consider	O
+them	O
+as	O
+independent	O
+parameters	O
+[	O
+57	O
+]	O
+.	O
+Accordingly	O
+,	O
+we	O
+choose	O
+herein	O
+to	O
+fix	O
+the	O
+attractive	O
+exponent	O
+to	O
+λa	O
+=	O
+6	O
+which	O
+would	O
+be	O
+expected	O
+to	O
+be	O
+representative	O
+of	O
+the	O
+dispersion	O
+scaling	O
+of	O
+most	O
+simple	B-Material
+fluids	I-Material
+and	O
+refer	O
+from	O
+here	O
+on	O
+to	O
+the	O
+repulsive	O
+parameter	O
+as	O
+λ	O
+=	O
+λr	O
+.	O
+The	O
+potential	O
+simplifies	O
+to	O
+(	O
+2	O
+)	O
+ϕ	O
+(	O
+r	O
+)=	O
+λλ	O
+−	O
+6λ66	O
+/(	O
+λ	O
+−	O
+6	O
+)	O
+εσrλ	O
+−	O
+σr6	O
+
+The	O
+data	B-Process
+acquisition	I-Process
+strategies	I-Process
+must	O
+balance	O
+the	O
+relevant	O
+scales	O
+and	O
+volumes	O
+of	O
+the	O
+datasets	O
+to	O
+be	O
+used	O
+in	O
+the	O
+physical	B-Task
+and	I-Task
+statistical	I-Task
+modeling	I-Task
+.	O
+Approaches	O
+for	O
+extraction	B-Task
+of	I-Task
+the	I-Task
+necessary	I-Task
+information	I-Task
+must	O
+be	O
+able	O
+to	O
+disregard	O
+spurious	O
+information	O
+,	O
+so	O
+as	O
+to	O
+develop	O
+a	O
+working	O
+network	B-Process
+of	I-Process
+models	I-Process
+for	O
+each	O
+active	O
+mechanism	O
+related	O
+to	O
+each	O
+degradation	O
+pathway	O
+on	O
+the	O
+mesoscopic	O
+physical	O
+level	O
+and	O
+the	O
+data-driven	O
+statistical	B-Process
+model	I-Process
+level	O
+.	O
+To	O
+capture	B-Task
+the	I-Task
+temporal	I-Task
+evolution	I-Task
+of	O
+the	O
+energy	B-Material
+material	I-Material
+over	O
+long	O
+time	O
+frames	O
+,	O
+appropriate	B-Process
+informatics	I-Process
+methods	I-Process
+are	O
+needed	O
+to	O
+balance	O
+data	O
+volume	O
+(	O
+e.g.	O
+,	O
+simple	O
+univariate	B-Material
+time-series	I-Material
+data	I-Material
+streams	I-Material
+with	O
+high-dimensional	B-Material
+volumetric	I-Material
+imaging	I-Material
+datasets	I-Material
+)	O
+while	O
+considering	O
+their	O
+respective	O
+information	O
+contents	O
+[	O
+68,69	O
+]	O
+.	O
+The	O
+raw	O
+data	O
+and	O
+extracted	O
+information	O
+must	O
+be	O
+accessible	O
+for	O
+query	B-Task
+and	O
+modeling	B-Task
+.	O
+Similarly	O
+,	O
+the	O
+modeling	B-Process
+approaches	I-Process
+used	O
+to	O
+understand	O
+and	O
+parameterize	O
+active	O
+mechanisms	O
+and	O
+phenomena	O
+over	O
+lifetime	O
+fall	O
+into	O
+the	O
+broad	O
+categories	O
+of	O
+micro	B-Process
+-	I-Process
+,	I-Process
+meso	I-Process
+-	I-Process
+and	I-Process
+macroscopic	I-Process
+approaches	I-Process
+.	O
+Laboratory	B-Task
+and	I-Task
+real-world	I-Task
+experimentation	I-Task
+,	O
+informatics	B-Task
+,	O
+analytics	B-Task
+,	O
+and	O
+the	O
+development	B-Task
+of	I-Task
+network	I-Task
+models	I-Task
+for	O
+mesoscopic	O
+evolution	O
+of	O
+energy	B-Material
+materials	I-Material
+over	O
+lifetime	O
+together	O
+constitute	O
+the	O
+field	O
+of	O
+degradation	B-Task
+science	I-Task
+.	O
+
+There	O
+are	O
+some	O
+relevant	O
+studies	O
+on	O
+information	B-Task
+dissemination	I-Task
+in	I-Task
+transportation	I-Task
+systems	I-Task
+using	O
+simulations	B-Process
+.	O
+One	O
+category	O
+of	O
+studies	O
+look	O
+at	O
+how	O
+either	O
+local	O
+information	O
+(	O
+only	O
+about	O
+the	O
+neighbours	O
+)	O
+or	O
+global	O
+information	O
+(	O
+about	O
+the	O
+entire	O
+network	O
+)	O
+affects	O
+the	O
+global	O
+network	O
+performance	O
+.	O
+Our	O
+approach	O
+is	O
+different	O
+in	O
+the	O
+sense	O
+that	O
+we	O
+investigate	B-Process
+the	I-Process
+impact	I-Process
+of	I-Process
+information	I-Process
+on	I-Process
+the	I-Process
+global	I-Process
+network	I-Process
+performance	I-Process
+depending	O
+on	O
+the	O
+fraction	O
+of	O
+people	O
+that	O
+receive	O
+information	O
+.	O
+We	O
+analyse	B-Task
+what	I-Task
+is	I-Task
+the	I-Task
+effect	I-Task
+of	I-Task
+real	I-Task
+time	I-Task
+information	I-Task
+dissemination	I-Task
+and	O
+explain	O
+why	O
+this	O
+effect	O
+appears	O
+.	O
+Information	O
+is	O
+disseminated	O
+in	O
+real	O
+time	O
+and	O
+contains	O
+global	O
+details	O
+about	O
+how	O
+congested	O
+the	O
+roads	O
+are	O
+.	O
+This	O
+approach	O
+is	O
+important	O
+as	O
+it	O
+gives	O
+insights	O
+on	O
+the	O
+impact	O
+that	O
+massive	B-Process
+use	I-Process
+of	I-Process
+real-time	I-Process
+information	I-Process
+can	O
+have	O
+on	O
+traffic	O
+.	O
+This	O
+can	O
+be	O
+useful	O
+for	O
+building	B-Task
+more	I-Task
+intelligent	I-Task
+traffic	I-Task
+control	I-Task
+mechanisms	I-Task
+where	O
+information	O
+is	O
+a	O
+steering	O
+tool	O
+.	O
+
+Generalized	B-Process
+polynomial	I-Process
+chaos	I-Process
+expansions	I-Process
+.	O
+One	O
+approach	O
+to	O
+model	B-Task
+densities	I-Task
+with	O
+stochastically	O
+dependent	O
+components	O
+numerically	O
+,	O
+is	O
+to	O
+reformulate	O
+the	O
+uncertainty	B-Task
+problem	I-Task
+as	O
+a	O
+set	O
+of	O
+independent	O
+components	O
+through	O
+generalised	B-Process
+polynomial	I-Process
+chaos	I-Process
+expansion	I-Process
+[	O
+34	O
+]	O
+.	O
+As	O
+described	O
+in	O
+detail	O
+in	O
+Section	O
+3.1	O
+,	O
+a	O
+Rosenblatt	B-Process
+transformation	I-Process
+allows	O
+for	O
+the	O
+mapping	O
+between	O
+any	O
+domain	O
+and	O
+the	O
+unit	O
+hypercube	O
+[	O
+0	O
+,	O
+1	O
+]	O
+D	O
+.	O
+With	O
+a	O
+double	O
+transformation	O
+we	O
+can	O
+reformulate	O
+the	O
+response	O
+function	O
+f	O
+asf	O
+(	O
+x,t,Q	O
+)=	O
+f	O
+(	O
+x,t,TQ	O
+−	O
+1	O
+(	O
+TR	O
+(	O
+R	O
+)))≈	O
+fˆ	O
+(	O
+x,t,R	O
+)=∑	O
+n	O
+∈	O
+INcn	O
+(	O
+x,t	O
+)	O
+Φn	O
+(	O
+R	O
+)	O
+,	O
+where	O
+R	O
+is	O
+any	O
+random	O
+variable	O
+drawn	O
+from	O
+pR	O
+,	O
+which	O
+for	O
+simplicity	O
+is	O
+chosen	O
+to	O
+consists	O
+of	O
+independent	O
+components	O
+.	O
+Also	O
+,	O
+{	O
+Φn	O
+}	O
+n	O
+∈	O
+IN	O
+is	O
+constructed	O
+to	O
+be	O
+orthogonal	O
+with	O
+respect	O
+to	O
+LR	O
+,	O
+not	O
+LQ	O
+.	O
+In	O
+any	O
+case	O
+,	O
+R	O
+is	O
+either	O
+selected	O
+from	O
+the	O
+Askey-Wilson	B-Process
+scheme	I-Process
+,	O
+or	O
+calculated	O
+using	O
+the	O
+discretized	B-Process
+Stieltjes	I-Process
+procedure	I-Process
+.	O
+We	O
+remark	O
+that	O
+the	O
+accuracy	O
+of	O
+the	O
+approximation	O
+deteriorate	O
+if	O
+the	O
+transformation	O
+composition	O
+TQ	O
+−	O
+1	O
+∘	O
+TR	O
+is	O
+not	O
+smooth	O
+[	O
+34	O
+]	O
+.	O
+Dakota	O
+,	O
+Turns	O
+,	O
+and	O
+Chaospy	O
+all	O
+support	O
+generalized	B-Process
+polynomial	I-Process
+chaos	I-Process
+expansions	I-Process
+for	O
+independent	O
+stochastic	O
+variables	O
+and	O
+the	O
+Normal	O
+/	O
+Nataf	O
+copula	O
+listed	O
+in	O
+Table	O
+2	O
+.	O
+Since	O
+Chaospy	O
+has	O
+the	O
+Rosenblatt	B-Process
+transformation	I-Process
+underlying	O
+the	O
+computational	B-Material
+framework	I-Material
+,	O
+generalized	B-Process
+polynomial	I-Process
+chaos	I-Process
+expansions	I-Process
+are	O
+in	O
+fact	O
+available	O
+for	O
+all	O
+densities	O
+.	O
+
+The	O
+main	O
+drawback	O
+of	O
+thermo-oxidation	B-Process
+in	O
+most	O
+actual	O
+devices	O
+and	O
+ITER	B-Material
+is	O
+its	O
+limitation	O
+to	O
+maintenance	O
+periods	O
+,	O
+when	O
+the	O
+vessel	B-Material
+walls	O
+can	O
+be	O
+heated	O
+up	O
+around	O
+300	O
+–	O
+400	O
+°	O
+C	O
+by	O
+hot	O
+helium	B-Material
+injection	O
+through	O
+the	O
+cooling	B-Material
+system	I-Material
+[	O
+19,20	O
+]	O
+,	O
+and	O
+also	O
+because	O
+of	O
+the	O
+required	O
+reconditioning	B-Task
+of	O
+the	O
+walls	O
+before	O
+plasma	B-Task
+operation	I-Task
+to	O
+remove	O
+the	O
+absorbed	O
+oxygen	B-Material
+[	O
+10	O
+]	O
+.	O
+However	O
+,	O
+the	O
+temperature	O
+achieved	O
+is	O
+not	O
+homogeneous	O
+over	O
+the	O
+vessel	B-Material
+,	O
+as	O
+it	O
+is	O
+limited	O
+to	O
+the	O
+distance	O
+to	O
+the	O
+cooling	B-Material
+tubes	I-Material
+,	O
+and	O
+thus	O
+to	O
+the	O
+device	O
+design	O
+.	O
+The	O
+analysis	O
+of	O
+this	O
+study	O
+is	O
+a	O
+continuation	O
+of	O
+previous	O
+works	O
+done	O
+for	O
+the	O
+treatment	B-Task
+of	I-Task
+ITER	I-Task
+carbon	I-Task
+co-deposits	I-Task
+[	O
+1	O
+–	O
+3	O
+]	O
+,	O
+so	O
+the	O
+temperatures	O
+studied	O
+are	O
+in	O
+the	O
+range	O
+of	O
+350	O
+°	O
+C	O
+for	O
+divertor	B-Material
+and	O
+200	O
+–	O
+275	O
+°	O
+C	O
+for	O
+main	B-Material
+wall	I-Material
+and	O
+remote	B-Material
+parts	I-Material
+.	O
+At	O
+present	O
+,	O
+due	O
+to	O
+budget	O
+restrains	O
+as	O
+well	O
+as	O
+due	O
+to	O
+tritium	B-Material
+trapped	O
+in	O
+co-deposited	O
+carbon	B-Material
+layers	I-Material
+,	O
+ITER	B-Material
+will	O
+not	O
+use	O
+carbon	B-Material
+materials	I-Material
+at	O
+the	O
+divertor	B-Material
+strike	O
+points	O
+in	O
+spite	O
+of	O
+their	O
+excellent	O
+resilience	O
+against	O
+large	O
+heat	O
+loads	O
+.	O
+Nevertheless	O
+,	O
+many	O
+present	O
+experimental	O
+nuclear	B-Material
+fusion	I-Material
+devices	I-Material
+(	O
+DIII-D	B-Material
+,	O
+TCV	B-Material
+,	O
+etc.	O
+)	O
+and	O
+new	O
+ones	O
+(	O
+JT-60SA	B-Material
+,	O
+KSTAR	B-Material
+,	O
+Wenderstein-7X	B-Material
+)	O
+use	O
+carbon	B-Material
+elements	I-Material
+,	O
+so	O
+the	O
+removal	B-Task
+of	I-Task
+carbon	I-Task
+co-deposits	I-Task
+is	O
+still	O
+necessary	O
+for	O
+a	O
+better	O
+device	O
+operation	O
+—	O
+plasma	B-Task
+density	I-Task
+control	I-Task
+,	O
+dust	B-Material
+events	O
+,	O
+etc	O
+.	O
+The	O
+temperatures	O
+used	O
+in	O
+this	O
+work	O
+are	O
+not	O
+very	O
+different	O
+from	O
+the	O
+ones	O
+achievable	O
+in	O
+present	O
+devices	O
+,	O
+such	O
+that	O
+the	O
+results	O
+can	O
+be	O
+extrapolated	O
+to	O
+them	O
+.	O
+Moreover	O
+,	O
+even	O
+for	O
+ITER	B-Material
+this	O
+study	O
+could	O
+be	O
+useful	O
+if	O
+carbon	B-Material
+materials	I-Material
+have	O
+to	O
+be	O
+eventually	O
+installed	O
+in	O
+the	O
+case	O
+that	O
+operation	O
+with	O
+tungsten	B-Material
+tiles	I-Material
+at	O
+the	O
+strike	O
+points	O
+is	O
+precluded	O
+by	O
+unexpected	O
+reasons	O
+.	O
+