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Controlling Particle Diffusion Controlling Particle Diffusion on the Nanoscales Nanoscales on the Fabio Marchesoni 1,2 1 Physics Department, University of Camerino, Italy 2 Physics Department, University of Augsburg, Germany University Augsburg


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SLIDE 1

Controlling Particle Diffusion Controlling Particle Diffusion

  • n the
  • n the Nanoscales

Nanoscales

Fabio Marchesoni1,2

1 Physics Department, University of Camerino, Italy 2 Physics Department, University of Augsburg, Germany

KIAS, July 2008 KIAS, July 2008

in collaboration with

University Augsburg

and

RIKEN

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SLIDE 2

Brownian Motors Brownian Motors

Astumian & Hanggi, Physics Today (2002)

Flashing ratchet: substrate switches on and off periodically Role of noise: rectification is assisted by noise

kinesin ATP hydrolysis

Diffusion Diffusion

‹x2›

= 2 Dα t α spread around mean α = 1 normal diffusion Impacts efficiency: long

  • bservation times tobs

> 2 D1 / ‹|v|›2

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SLIDE 3

One One-

  • species mixtures

species mixtures

PRL 99 PRL 01 Bras & Kets PRL 04

Binary mixtures Binary mixtures

Repulsive interaction: feel ratchet potential; don’t.; both species get rectified in opposite direction

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SLIDE 4

Diffusion Enhancement Diffusion Enhancement

Model: single Brownian particle in a tilted washboard potential

) ( sin t F x x ξ + + − = &

F t x V x x m + + ′ − − = ) ( ) ( ξ γ & & &

ξ(t): thermal noise 〈ξ〉 = 0, 〈ξ(t)ξ(0)〉 = 2γ kTδ(t) V(x)=V(x+L): periodic substrate Overdamped regime (m = 0, γ = 1): most used for applications

  • ne depinning

threshold: F3

‹x2(t)›

̶ ‹x(t)›2 = 2 D t normal diffusion with D = D (F,T) L=2π μ=v/F v∞ =F/γ

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SLIDE 5

D/D0 F/F3 Numerics: D(F) peaks at F = F3 to compare with free diffusion D0 = kT

[Costantini, FM, EPL 48 (1999) 491]

Renewal process: diffusion due to uncorrelated hops between adjacent wells Cox' formula yields: ‹t n (a → b)› n-th moment of the a→b FPT in good agreement with numerics.

[Reimann et al, PRL 87 010602 (2001)]

kT=0.1 kT=0.01

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SLIDE 6

Underdamped regime: effect further enhanced [Costantini, FM, EPL 48 (1999) 491] Threshold effect: peaks located by approximate formula γ= 0.01 γ = 0.1 kT=1 Consequence: diffusion enhancement occurs at current onset, eg, in ratchet devices; efficiency gets degraded.

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SLIDE 7

Single Single-

  • File Diffusion

File Diffusion

Constrained geometries: from 1D to “narrow” channels. Single file (SF): N non-passing particles diffusing over a line

  • f length L: N,L →∞

with ρ = N/L = const [Jepsen gas, 1965] Initial vi and xi : randomly distributed Thermal noise: OFF (ballistic SF); ON (stochastic SF)

SFD: the diffusion of a single particle gets suppressed; independently of F ballistic SFD: normal diffusion stochastic SFD: anomalous diffusion with FD = √D0/π

[Harris 1975, Percus 1974]

D

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SLIDE 8

SFD Enhancement SFD Enhancement

V(x) = d[1– cos (2πx/L)]

Corrugated walls: ion channels, zeolites, laser traps, etc for a single particle driven on a periodic substrate Anomalous diffusion: ‹Δx2(t)› = 2FD √t/ρ with FD = √D(F) /π

D F=1 F=0

L V(x) F=1

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SLIDE 9

Entropic Effects Entropic Effects

Bona fide 2D, 3D geometry: suspended

point-like Brownian particles in a “narrow” channel. Channel radius: w(x) = a cos(2πx/L)+b Wmax = 2(b+a); Wmin = 2(b-a) ∝ kT

  • P(x,y,z;t) → P(x;t)
  • ±w(x) boundaries & V(x) = 0 →

Ventropic (x) = – kT ln A(x) with A(x) = 2w(x) (2D); π w2(x) (3D)

  • T → Teff

(x) = T/[1+w'(x)2]α A(x) Wmax Approximate reduction to 1D

[Zwanzig 1992, Reguera Rubi 2001]

Veff (x) α = 1/2, 1/3

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SLIDE 10

Entropic Diffusion Enhancement Entropic Diffusion Enhancement

Replacing Ventropic (x) and Teff (x) into Cox' formula fits closely numerics Deviations for large F/T: asymptotes ≠ 1; particle piles up against bottlenecks [Hanggi

et al, 2006, 2007]

μ

kT = 0.01, 0.1, 0.2, 04 L=2π a/L=1; b/L=1.02

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SLIDE 11

Resonant Diffusion Resonant Diffusion

  • flashing

substrate – ATP power strokes,

  • ptical lattice traps, etc
  • side-wise sieves

– by unbiased forcing 2 x0 (t) ) ( ) ( sin

kick

t F t F y y ξ + + + − = & with x0 (t) = ± x0 ; either periodic

  • r random

with residence time τ

  • kicked particles:

by x → y = x – x0 (t)

) ( )] ( sin[ t F t x x x ξ + + − − = &

with Fkick (t) = (–1)n x0 δ(t – tn ); either periodic

  • r random

with residence time τ

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SLIDE 12

π+ π- Resonant diffusion: τ ~ 1: particle hops right/left by steps

  • f 2x0

and 2(π-x0 ); hence

D = L2/(2τ) π+ (1– π+ )

π+ ,π

right/left probabilities Diffusion coefficient τ → ∞: kicking is irrelevant, τ → 0: potential gets renormalized – cos x → – (cos x0 ) cos x

D (F=0)

for the relevant potential amplitude

diffusion peak D = (L/2)2/2τ

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SLIDE 13

Conclusions Conclusions

Work done also in collaboration with: Nori and Savel’ev (RIKEN): PRL 91 010601 (2003); 92 160602 (2004); Taloni (now IoP-AS, Taiwan): 96 020601 (2006); 97 106101 (2006); Borromeo (INFN, Perugia): 99 150605 (2007)

Diffusion plays a crucial role in the control of particle transport at the nanoscales. Relevance for applications in nanotechnology. RMP 2009