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1 S10 S ,.. 1,.. 1, , :. : 1) - ; ) - 3) -.,, -,. -,,. :,,,. - [ 1, ]. d,, k B T m T m 10 ( d /k B T m 10). - [ ]. -,, - [ ].. - -,, [ 3 ].,. -., - [ 4 ]., [ 5 7 ].,. - [ 8 ], -. [ 8 ],..,..,..,.., 013
2 , S11, ;, t = 0,9, t = 0,5. : 1) - ) -. -.,,.,,, , -,.. -. [ 9 ] 0, é , [ 10, 11 ]. 0 >> 1,, ,. -. t - f a/ T, - a T. 0 / f [ 1, 13 ] , - Tm T TH, Tm 73 K, TH 315 K, T H, - -. T > T H. -, -, [ 14, 15 ]. - [ 14 ] [ 15 ] ( / f, f , [ 9, 10 ]
3 S1..,..,..,.. 1 : Sd ( S Sl ) Sc, S S l - ; S c ). - [ 16, 17 ]. [ 17 ]., d. - [, 18 0 ]. : T < T H, -, T > T H,., T > T H -. r / T, T ~ kt B / I - ; I ~ mhoh r (m H r OH ). r 0,510 1., -.., d (), t t = T/T c, T c, 0,6 < t < 1. d () t, -. d () t t < 0,5 (. 3). - d () t (. 3): (0) (0) 4 d d H t d H exp( / ), 5,110, 4,71, (1) [ 9 ] ( H = E H /k B T c ). - t d 0,480,49, d (). t.. - d() t d()/ t r: - [18] (), d d () t d ()/ t r, d : [ ] (+), [ 18 ] (), [ 19 ] (), [ 0 ] () d
4 , S H () t ( ); - H() t 0exp( H / t) , (1), - w (t), [ 14 ]., w (t), - Ar w() t w () t H(), t Ar w () t ; H () t, , : ( ) ( ) H () e p t H () t H (). t ( e) ( e) ( H ( t) 0 exp( H / t)),. H = 4,71,. [ 14 ],. ( e ) H () t d () t t < t H ( e) 4. 5, c H / d 10 ( e) * /. H () t d () t -,. M -.,, -, [ ].,, - h. h, -. [ 1 ] - f (,, t) [ 19 ]: f Dr, f, t D r = 1/, -. Y nm (,): f(,, t) anm exp( n( n1) Dr ) Ynm(, ), () nm,
5 S14..,..,..,.. a nm,., n-, n- : r n. (3) nn ( 1), n = 1, d r /. (4) n n = 6, - h = d /1.,, M = h, M d / 1. H (t)/ M t H()/ t M 1 c*. c *,. 5, : c t 1, /c. c l 1, /c [ ]. : c t 1, /c c l 3, /c., G = t 1, /. 0 d T < T H 315 K , 0,,, d,., 0., [ 3 ],. -., - 0 T (70 300) K. d / 0 ~ ,. 0 d. - n- - d nn ( 1) d nn ( 1). n n n = 0, d n ( n 1) (5) 0 0 n 0, - -., d / 0 10,, n 0 4,.. T ( / f. 0 : [ 3 ] (), [ 4 ] (+), [ 5 ] ()
6 , S15 Ta 1 1 d d 10 c 1 1 d c 1,, n, (5) T d [19] 0 [4] 0 [5] 0 [6] n 0 [4] n 0 [5] n 0 [6] 73 17,85, 1,15,9 3,56 5,09 3, ,6 1,3 0,85 1,9 3,93 4,97 3, ,33 0,9 0,7 1,3 4,08 4,69 3, , 0,65 0,5 1,1 4,4 4,89 3, ,7 0,45 0,4 0,9 4,56 4,86 3,09 300) K. n K < T < 315 K.,.,,,. [ 6 ]. (T > T H ) n 0 4, -,. f a/ T. -., - - :,,.., : 1 4 eff, 3 n ; n. [ 7 ], : ( L) 1 teff () t eff () t e, (6) 3 t deff () t eff () 3 B c OO t t = ktr (7), d eff (t) ; r OO - ; T c. (6) - [, 7 ] - : 0,055. e
7 S16..,..,.., ( L) eff () t - [ 8 ]. 8. () - d eff () t ( ) (7) (8) -. 7., eff (t) : d eff () t teff ()/ t t0 0,8 teff (), t (8) d () t d ()/ t d, d 0 eff eff 0 d0 0 3 B c OO t =. ktr,. 8, d eff () t - t: d eff () t abt a = 0,15 b = 0,61., a b, [ 9, 30 ], - : a = 0,150,16 b = 0,610,63. 0,93 < t < 1 t eff () t -. t eff (0,93) 0,75 d eff (0,93) 1,334 D, (7) (8), - [ 31 ]: ( V ) ( V ) teff (0,93) 1,48 deff (0,93) d0,63 D , ,..,, -.
8 , S n p d p p, 3 p1 p 3kT B n p p- ; d p.,, - -. (6), ( p) ( dp / p) t 3 ktr B c OO, - d p,, p /p e (. [ 31 ]): ct p p 1 4 p1 e. 3 3t (9),, c p = n p /n w p-. pnp nw, : p1 eff () 3 3 p1 pc, p- - (. ). -,,.,,,., 0,8 1,3 D [ 33, 34 ]. [ 31, 3 ] (. - ),, d d0,63d, d3 0,5d0 0,9D dp 0, p 4. (10) - : 1) ) t (), t (3) t eff (t). 9. d 3 1,3 D. 9, - t (3), 0,4. t > 0,5, - : ( cl) ( L) 1 teff () t eff () t e, 3 t ( cl) t t c d c d, d p, d p = ktr 3 B c OO p 1. : c +3c 3 = t eff (t) t (), t (3)
9 S18..,..,.., cal c () t () exp c () t () -, c c 3 : 1 c t t c3 (1 c ). 3, 1 ( tt ) d d 3 d3 ( abt) a d b ab 3 3,,, Z d d 3. Z Z Z 3 (10), : d,97, d 3 0,37 11 Z d 0,7. 6 c 0, t 0,1t 0, 03. (11) c (0,4) = 0,05, c (0,9) = 0,,.. (c ) 10 % - 44 %.. 10 c cal (), t exp (1) 0,4 t 0,85, c (), t (11) : 0,4 t 1.,,... [ 35 ]., c 0,9 t 1,... ( cl) ( L) 1 teff () t ( cl) () eff () t e, teff () t c d, 3 t.. -., c c : () c () t c () t (1 c ()). t () 3 d 3d,, : () 4 c () ( )) 4c 1. (13) (c (t) c t 1,. 11., (), c 4c4 1,,.,. (1)
10 , S c (t), c ( t ) 4c 4, - (11), (1) (13) (),. [ 8 ], -, -. i Q = C V /k B N A (C V - ; N A ),., -. -., -. i Q. -. i Q = 6,. i Q,, : iq i (tr) (or) ( ) Q iq i Q. (14) (14) -, 1 (. [ 8 ]). - i ( ) Q,,. 1,., ( ) 6,5, t tm, iq () t (15) 3, t 0,9., (a) -,, (17) ()
11 S0..,..,..,.. (,..)., : - -, -. - i () =, ( ) i Q 3. (15), -. -, [ 35 ] -., -, i ( ) Q ,, - i ( ) Q : i ( ) 6 c 6 pc. (16) Q,. - (16) i ( ) 6 () Q c 6 pcp i ( ) Q p3 p4 p. 1, (11) (1) - pcp., - p4, 4c : 1 ( ) () 4 c i ( t) 6c 0,117t 1, 68t 1, 697. (17) 4 6 Q 4c 4. 1,. - : 1). 90 %; ),.. t 0,9,. 60 %., -,. (. ). -,, -. -, : -.,, -, [ 5, 7 ] [ 35 ].
12 , S1,...,.,,, ().,,,., [ ] ,....,., [ 36 ] - (H O) n n = 1,, 0. n = 3,,. [ 37 ]. -,,,,,, -,. -., n n, n 1., -,.,,,.,,.. 13, -,.. -.,,.,,,. - [ 36 ].. 13.
13 S..,..,..,.. d D dd / d0 (H O) (H O) 3 (H O) 4 0,57 0 [ 38 ] 1,59 0,81 0 [ 39 ] 1,5 0,69 0 [ 40 ] 3 E n En / kbtm [41] n TIP4P TIP3P 47,98 50, ,78 134,4 4 14,5 5,51, -,. 3..,,, -,.. (. [ 47 5 ]).,, 50 %., -. -., - -., T tr < T < 400 K [ 48, 49, ] - [ 56 ]. 400 K < T < 650 K,.,. [ 8 ]., -., -. [ 8 ] -.,. i Q (t), i Q (t) : (1) () (4) Q 1 Q Q 4 Q i () t ci ci 4 ci, (18). -, : (1) () (4) i 6, i 10, i 15,5. Q Q Q. 14., (0) (), -
14 , S3 i Q. 14, (i Q = 6). i Q = 10,, t 0,75 (T = 485 K). i Q t tr < t < 0,75 : iq 6 c1( t) 10 (1 c1( t)) 10 4 c1( t). (19) c 1 (t) -. 14, : c 1 ( t ),71 t,48 t 0,4. (0) (t) = 1 c 1 (t) c D (t) = = c (t) c D (t) : c PK p c1c 1. (1) c1,, K p (. [ 57 ]): Kp ( T) exp( b/ t), () t a b,, (3) 400 K < T < 650 K, -., - K p (t),, [56].. 15, (t) c D (t) 0,4 < t < 0,6., (0),,. t > 0,6 (t) c D (t), :,.. -,.,, (0), c 4 (t) = = (t) c D (t). 4c 4 (t) (t) ( ) c D (t), : a b, [ 49 ], [ 53 ], [ 54 ], [55]. 16. : c D (t) [ 49 ] (), [ 53 ] ()
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