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Nonconservative forcing and diffusion in refractive optical traps

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Abstract

Refractive optical trapping forces can be nonconservative in the vicinity of a stable equilibrium point even in the absence of radiation pressure. We discuss how nonconservative 3D force fields reduce, near an equilibrium point, to circular forcing in a plane; a simple model of such forcing is the refractive trapping of a sphere by four rays. We discuss in general the diffusion of an anisotropically trapped, circularly forced particle and obtain its spectrum of motion. Equipartition of potential energy holds, even though the nonconservative flow does not follow equipotentials of the trap. We find that the dissipated nonconservative power is proportional to temperature, providing a mechanism for runaway heating instability in traps.

© 2011 Optical Society of America

1. INTRODUCTION

Nonconservative fields of optical force on optically trapped particles have long been predicted to occur [1]. These force fields are locally nonpotential in character, so that network is done on a particle even in microscopic closed paths. This differs from, say, electromotive force around a circuit where only the global potential is not definable [2]. In a locally nonconservative force field, external power is continuously coupled to particle motion, leading to dissipation and heating even when the particle is localized about a stable point of the force field.

Radiation pressure on trapped particles can be one source of nonconservative forcing. In recent experiments [3, 4], nonconservative toroidal circulation of optically trapped particles caused by axial radiation pressure was observed and theoretically analyzed. Recent theoretical work [5] has shown how, for nonspherical objects, nonconservative motion arises in coordinates of angle and translation.

Here we show that a simple spatial 3D nonconservative force field, circular rather than toroidal, occurs even in the absence of radiation pressure. As a physical model leading to this force, we describe a sphere trapped by refracting rays. Within any such circular-forcing model, and generalizing to an anisotropic trapping force, we derive the spectrum of motion and the thermal signatures of nonconservative circular forcing.

2. GEOMETRY OF NONCONSERVATIVE FORCES

Before narrowing the discussion to optical trapping, we ask what simple generic statements can be made about nonconservative forces. Powerful classification schemes are available from differential geometry [6, 7, 8] but to use these one must correctly identify forces as fields, not of vectors, but of differential 1-forms. This means that force components such as fx, fy, and fz properly take their meaning from the work differential, or work 1-form:

ω=fxdx+fydy+fzdz,
which is the integrand for evaluating work along any chosen path. The 1-form ω is said to be exact if Eq. (1) equals the differential of some potential function, ω=dΦ; otherwise ω is inexact. For our purposes, an exact 1-form is the same thing as a conservative force.

In Euclidean space one can reinterpret fx, fy, and fz as components of a vector. But as a 1-form field, Eq. (1) is constrained by Darboux’s theorem [6, 7], which states that every 1-form field ω can be reduced by some choice of general coordinates (q1,q2,q3,) to a shortest canonical form ω=ω(k) belonging to the sequence

ω(1)=dq1,
ω(2)=q1dq2,
ω(3)=dq1+q2dq3.
In more than three dimensions, the list continues with ω(4)=q1dq2+q3dq4, and so on.

The case ω=ω(1), i.e., ω=dq1, is exact, i.e., conservative. Not only is q1 a coordinate, but q1 is the potential function for ω. The case ω=ω(2), or ω=q1dq2, is reducible to the exact case by an integrating factor (1/q1), because (1/q1)ω=dq2. In two dimensions, this exhausts our list, showing that all 1-forms (i.e., differentials) in 2D are either exact or integrable, a well-known and useful fact in thermodynamics.

In 3D, exact (conservative) and integrable force fields of types ω=ω(1), and ω=ω(2) can still occur, but the most general possibility is the nonintegrable 1-form ω(3), i.e., ω=dq1+q2dq3. The form of a generic force field is thus more restricted than Eq. (1) would suggest. In the case of optical trapping, the optical force field includes a part derivable from a potential, which we use for our first coordinate: q1=Φ. Following Eq. (4), we write

ω=fdθdΦ,
so that q3=θ is a coordinate that we will below take to be an angle and q2=f is the angular force conjugate to θ. The Frobenius theorem [6, 7, 8] states that in terms of the ex terior product ∧ and exterior derivative d, the work 1-form will be of the nonintegrable form of Eq. (5) whenever ωdω=dΦdfdθ0.

In the neighborhood of an equilibrium point, where all components of a force field vanish, it is natural to interpret θ in Eq. (5) as an angular variable, motivated by the reduction ydx+xdy=ρ2dθ. Nonconservative forces near equilibrium are circulations aligned with some plane that contains the equilibrium point. The nonconservative portion of the force can be taken as strictly circular near the equilibrium point in any coordinates, because a noncircular 2D force pattern in x and y can be written as

aydx+bxdy=12(a+b)ρ2dθ12(ab)d(xy),
and the last term can be absorbed into dΦ. Thus the work 1-form of Eq. (6) is actually of the type in Eq. (5), with θ being a circular angle in terms of x and y.

Thus, to study a nonconservative 3D force about an equilibrium point, it is sufficient to consider a circular pattern of force in some 2D plane containing the equilibrium point.

From another point of view, this picture is consistent with equilibrium-point analysis of a vector field f, viewed as flow toward a fixed point [9] (Fig. 1). Briefly, with coordinates qi we have fiMijδqj near the fixed point, defining some real matrix M. The eigenvalues of M are roots of a cubic equation with real coefficients, and they generically yield one real and two complex conjugate roots whose real parts, together with their eigendirections, correspond here to a conservative force field. The imaginary part of the complex pair of eigenvalues defines circulation in some plane. The eigendirections of M may be stretched and skewed, corresponding to the nonorthogonal coordinates in Eq. (4).

From yet another point of view, any vector field restricted to the surface of a sphere (about the equilibrium point) will circulate about the sphere in a 2D fashion, according to the familiar “combed hair on a sphere” theorem of mathematics [8] (Fig. 1).

3. NONCONSERVATIVE TRAPPED-SPHERE MODEL

For a “toy model” realization of a circular nonconservative force, we consider an optically trapped sphere much larger than the wavelength of light, so that geometrical optics applies. In our simplified model, we assume no reflections (perhaps due to a graduated-index boundary) and we trap the sphere with only a few rays passing almost centrally through the sphere, so that the refraction and trapping force can be calculated in a paraxial-ray approximation. Our model is certainly contrived, but it is very simple to analyze. In more realistic situations, whenever there is chirality (handedness) of a system of light rays near an equilibrium point, we still expect some degree of circular nonconservative forcing to occur.

We need only consider rays within the plane of Fig. 2a, containing the sphere center. In Fig. 2a, the displacement of the sphere center from the ray is exaggerated. The force of the refracted ray on the sphere due to momentum trans fer is

f=I0c(k^k^),
where I0 is the power of the ray and k^ and k^ are unit vectors for the original and refracted rays. If Δθ is the angle between k^ and k^, then
f=I0c[(cosΔθ1)k^+(sinΔθ)r^],
where r^ is the direction of r [see Fig. 2a]. We set sinΔθΔθ and cosΔθ1Δθ2/2, and we use paraxial-ray transfer matrices [10] to express Δθ and f in terms of the displacement r of the sphere. These matrices act on a vector (Δθ,h) whose components are the angle with and displacement from the optical axis. If matrices Fin and Fout describe refraction at the convex surfaces of our sphere of radius a, and matrix P2a describes paraxial propagation by a distance 2a, the ray matrix for the sphere is
FoutP2aFin=2n1n/2(n1)/aa1n/2,
with n being the relative refractive index of the sphere. In our case, h=r gives
Δθ=2(n1)nar
for the angular deviation. For simplicity, we set n=2 to find
fI0c[r22a2k^ra].
Equation (11) resolves f into a conservative restoring force, proportional to r, and a nonconservative quadratic force, pushing the sphere along the ray direction k^ whenever the sphere center is displaced off the ray axis.

The system of four rays shown in Fig. 2b results in a purely circular nonconservative force on the sphere. Despite the clockwise circulation of rays, there is no torque on the sphere within this ray-optical model: it is the nonconservative net force on the sphere that we study here. We separate oppositely directed ray pairs by a distance 2b, exaggerated in the figure, with ba so that our paraxial analysis remains valid. The ray in the +x direction is described by

k^=x^,r=(yb)y^+zz^
and similarly for the other rays. Summing the forces from Eq. (11), the total force on the sphere is
f=2I0ca[ba(xy^yx^)(xx^+yy^+2zz^)].
The work differential, or work 1-form, is
ω=2bI0ca2ρdθd[I0ca(x2+y2+2z2)],
which is of the form of Eq. (5), ω=fdθdΦ.

4. NONCONSERVATIVE MOTION OF A DIFFUSING PARTICLE

To look for spectral features of trapping in a nonconservative field, we consider diffusion through a fluid of a particle with drag coefficient γ. At temperature T, the diffusion coefficient is γ/kBT, an Einstein relation [11]. Near an equilibrium point we consider 2D motion r(t) in a plane of circulation where the nonconservative component of force is

f=ξz^×r=ξρθ^,
where ξ, the strength of the circular forcing, has units of force per distance. As a 1-form
ω=ξρdθ.
First we check that there is no pathology regarding work done by the nonconservative force at short scales, where a diffusing particle executes spatial cycles with a diverging frequency. For this, imagine the particle constrained to move on a circle of radius ϵ, like a bead sliding on a circular wire. In the absence of the external force, the time to diffuse around the circle is δt(γ/kBT)ϵ2. In the presence of a nonconservative force, the rates of positive and negative circling are enhanced and suppressed according to
ν±kBTγϵ2exp(±ΔWkBT),
where ΔW is the work done by the nonconservative force in a “+” cycle; for our force this is ΔW=2πϵfξϵ2. The net “+” rate is Δν=ν+νΔW/γϵ2, implying that the dissipated power is
ΔνΔWξ2ϵ2γ.
We conclude that the power supplied by the nonconservative force vanishes at small scales, as the square of the spatial scale of the motion.

We turn to the spectral properties of the diffusing particle, and we first establish formalism [12] with force and motion only in the x direction. For a force f(t) and motion x(t) that extend over all time, the spectral density (fx)ω is defined by [13]

fωxω*=2π(fx)ωδ(ωω),
where fω and xω are Fourier transforms of functions truncated outside of a time T. Throughout, ()ω specifies a spectral density, whereas is an average. Standard manipulations [13], or more simply the formal replacement fωxω*=T(fx)ω, give the rate of work done by f as
dWdt=12π(fv)ωdω=12πiω(fx)ωdω.
Spectral densities integrate to correlations or mean squared fluctuations [13]. In the 1D case, if a thermal Nyquist force N(t) acts on the object, with (N2)ω=2γkBT (with γ being the drag coefficient), then in an external conservative force f=κxx, with αx=κx/γ, the equation of motion N=κxx+γx˙ gives us
Nω=iγ(ω+iαx)xω,
NωNω*=γ2(αx2+ω2)xωxω*.
The replacements NωNω*=T(N2)ω and xωxω*=T(x2)ω immediately lead to
(x2)ω=2kBT/γαx2+ω2.
This Lorentzian spectrum integrates to
x2=12π(x2)ωdω=kBTκx,
as it should by the equipartition theorem [12]. Because (fx)ω=κx(x2)ω is an even function of ω, the rate of external work vanishes.

Now include a circular external force. With an isotropic conservative force κr, the vector equation of motion N=κrξz^×r+γr˙ gives us

Nω=(αiωηz^×)rω,
with “×” being a cross product and where α=κ/γ and η=ξ/γ. In the absence of thermal forces, the particle spirals to the origin with angular frequency η and a radius proportional to exp(αt), similar to Fig. 1a. Using the column vectors
Nω=[Nx,ωNy,ω],rω=[xωyω],
we can analyze an anisotropic confining potential, with Eq. (21) generalized to
Nω=iγMrω,M=[ω+iαxiηiηω+iαy]
and αy=κy/γ. To find the power spectrum, we form the averaged product
NωNω=γ2MrωrωM,
a generalization of Eq. (22). In terms of spectral densities, we have
2γkBT1=γ2M(rr)ωM,
where 1 is the identity matrix, and the spectral density matrix is
(rr)ω=[(x2)ω(xy)ω(yx)ω(y2)ω].
Equation (29) is easily solved for (rr)ω, giving diagonal elements
(x2)ω=2kBTγω2+αy2+η2[ω4+(αx2+αy22η2)ω2+(η2+αxαy)2],
which generalizes Eq. (23); (y2)ω is the same with αx and αy interchanged.

Equation (31) represents the power spectrum of the x motion of a trapped particle with a nonconservative force (η0) and 2D anisotropy (αxαy) both in the xy plane. Nonconservative forces make this power spectrum non-Lorentzian, even in an isotropic trap. Other interesting effects, such as inertial hydrodynamics and material properties [14, 15], will of course also invalidate a simple Lorentzian spectrum. Carrying out the ω integral in Eq. (24), we obtain

x2=kBTκx+κy[1+ξ2+κy2ξ2+κxκy].
For y2, κx and κy are interchanged. In the isotropic case, κx=κy=κ, the nonconservative circulation preserves x2=kBT/κ. For large values of ξ,
x2=2kBTκx+κy,ξκx,κy,
and the potential is effectively being averaged by rapid circulation. However, for all values of ξ, κx, and κy we find
12κxx2+12κyy2=kBT,
so that the equipartition of potential energy is unaffected by nonconservative circulation, even though the nonconservative flows do not follow equipotentials in an anisotropic trap.

Details of the flow pattern follow from the off-diagonal element of (rr)ω,

(xy)ω=2kBTγη(αyαx)2iηω[ω4+(αx2+αy22η2)ω2+(η2+αxαy)2],
obtained by solving Eq. (29). Integrating this over ω yields
xy=kBTκx+κyξ(κyκx)ξ2+κxκy.
Using this result, we can generalize Eq. (32) to the mean squared radius at any 2D angle. For Gaussian statistics such as we have here, the probability distribution
P(x,y)exp[12rGr]
yields a matrix of averages rr=G1, and a unit ellipse defined by
rGr=rrr1r=1.
As a function of angular direction θ, the squared radius of the ellipse is
r2=x2y2xy2y2cos2θ2xycosθsinθ+x2sin2θ,
into which x2, y2, and xy can be inserted from Eqs. (32, 36). The resulting ellipses are plotted in Fig. 3 for various values of ξ. The rms radius drawn in the figure is necessarily a line of flow. For increasing ξ, the flow pattern does not follow the ξ=0 equipotential lines, but tilts by θξ in the direction of the circular forcing, with
tan2θξ=2ξ(κx+κy).
The flow pattern also decreases in eccentricity with ξ until, at high circular forcing, we recover the circularly symmetric distribution described by Eq. (33).

The rate at which work is done on the system is

dWdt=12π(f·v)ωdω,
where (f·v)ω is a spectral density. In terms of Fourier transforms,
fω·vω*=iωξ[xωyω][0110][xω*yω*]=iωξ(xωyω*yωxω*)=2ξωImxωyω*,
from which we infer the spectral density
(f·v)ω=2ξωIm(xy)ω.
Using Eq. (35) for the right-hand side and performing the integral in Eq. (41) gives
dWdt=4kBTξ2κx+κy.
We find that the rate of work dissipated in the system by the circular nonconservative force is directly proportional to temperature, reflecting the enhancement of induced drift velocities by thermal spreading from the zero-force point. In contrast, nonconservative toroidal circulation due to axial radiation pressure [3, 4] leads to a squared dependence on temperature. Depending on the rate of outward heat flow from the optical focus [16] the proportionality of dissipation to temperature raises the possibility of an instability toward runaway heating by a nonconservative component of the trapping force.

5. SUMMARY

We have characterized the simplest 3D nonconservative force field, near a stable fixed point, as an anisotropic conservative force plus a nonconservative circular force. We constructed a simple trapping model exhibiting such forcing, and we presented signatures of particle displacement and nonconservative dissipation in the presence of nonconservative forcing. In most optical trapping experiments, simple circular forcing about a stationary point may not be easily observable given the more dominant radiation pressure effects that have been observed by others [3, 4]. Specifically designing chiral trapping geometries for particles and minimizing reflections may allow observation of circular forcing. More generally, however, the geometrical picture we have constructed and the thermal and spectral results we have obtained may be useful in other situations, even outside of optics, where locally nonconservative microscopic forces act.

ACKNOWLEDGMENTS

The authors would like to thank their colleagues in the Department of Physics and Astronomy at Washington State University for support and helpful conversations.

 figure: Fig. 1

Fig. 1 Nonconservative 3D force field near a stable equilibrium point. The circulation of force may be viewed as purely circular in some plane. (a) Vector flow-field point of view. (b) Combed-hair-on-a-sphere point of view.

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 figure: Fig. 2

Fig. 2 (a) Refraction of a single ray by a sphere. In the paraxial limit, r is much smaller than the radius of the sphere. The force f acts to return the sphere center to the line of k^, but it also has a component along k^. (b) System of four rays for nonconservative trapping. The limit ba allows a paraxial approximation for each ray.

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 figure: Fig. 3

Fig. 3 Rms radius r21/2 (solid curves) of the position distribution P(x,y) of a diffusing particle in a trap with stiffness anisotropy κy/κx=5, for various values ξ of counterclockwise circular forcing in the xy plane. The solid curves are lines of flow, which, for ξ0, do not follow the ξ=0 equipotential contour (dotted curves). Circular flow at ξ= (final panel, solid curve) has the rms radius [2kBT/(κx+κy)]1/2.

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Figures (3)

Fig. 1
Fig. 1 Nonconservative 3D force field near a stable equilibrium point. The circulation of force may be viewed as purely circular in some plane. (a) Vector flow-field point of view. (b) Combed-hair-on-a-sphere point of view.
Fig. 2
Fig. 2 (a) Refraction of a single ray by a sphere. In the paraxial limit, r is much smaller than the radius of the sphere. The force f acts to return the sphere center to the line of k ^ , but it also has a component along k ^ . (b) System of four rays for nonconservative trapping. The limit b a allows a paraxial approximation for each ray.
Fig. 3
Fig. 3 Rms radius r 2 1 / 2 (solid curves) of the position distribution P ( x , y ) of a diffusing particle in a trap with stiffness anisotropy κ y / κ x = 5 , for various values ξ of counterclockwise circular forcing in the x y plane. The solid curves are lines of flow, which, for ξ 0 , do not follow the ξ = 0 equipotential contour (dotted curves). Circular flow at ξ = (final panel, solid curve) has the rms radius [ 2 k B T / ( κ x + κ y ) ] 1 / 2 .

Equations (44)

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ω = f x d x + f y d y + f z d z ,
ω ( 1 ) = d q 1 ,
ω ( 2 ) = q 1 d q 2 ,
ω ( 3 ) = d q 1 + q 2 d q 3 .
ω = f d θ d Φ ,
a y d x + b x d y = 1 2 ( a + b ) ρ 2 d θ 1 2 ( a b ) d ( x y ) ,
f = I 0 c ( k ^ k ^ ) ,
f = I 0 c [ ( cos Δ θ 1 ) k ^ + ( sin Δ θ ) r ^ ] ,
F out P 2 a F in = 2 n 1 n / 2 ( n 1 ) / a a 1 n / 2 ,
Δ θ = 2 ( n 1 ) n a r
f I 0 c [ r 2 2 a 2 k ^ r a ] .
k ^ = x ^ , r = ( y b ) y ^ + z z ^
f = 2 I 0 c a [ b a ( x y ^ y x ^ ) ( x x ^ + y y ^ + 2 z z ^ ) ] .
ω = 2 b I 0 c a 2 ρ d θ d [ I 0 c a ( x 2 + y 2 + 2 z 2 ) ] ,
f = ξ z ^ × r = ξ ρ θ ^ ,
ω = ξ ρ d θ .
ν ± k B T γ ϵ 2 exp ( ± Δ W k B T ) ,
Δ ν Δ W ξ 2 ϵ 2 γ .
f ω x ω * = 2 π ( f x ) ω δ ( ω ω ) ,
d W d t = 1 2 π ( f v ) ω d ω = 1 2 π i ω ( f x ) ω d ω .
N ω = i γ ( ω + i α x ) x ω ,
N ω N ω * = γ 2 ( α x 2 + ω 2 ) x ω x ω * .
( x 2 ) ω = 2 k B T / γ α x 2 + ω 2 .
x 2 = 1 2 π ( x 2 ) ω d ω = k B T κ x ,
N ω = ( α i ω η z ^ × ) r ω ,
N ω = [ N x , ω N y , ω ] , r ω = [ x ω y ω ] ,
N ω = i γ M r ω , M = [ ω + i α x i η i η ω + i α y ]
N ω N ω = γ 2 M r ω r ω M ,
2 γ k B T 1 = γ 2 M ( r r ) ω M ,
( r r ) ω = [ ( x 2 ) ω ( x y ) ω ( y x ) ω ( y 2 ) ω ] .
( x 2 ) ω = 2 k B T γ ω 2 + α y 2 + η 2 [ ω 4 + ( α x 2 + α y 2 2 η 2 ) ω 2 + ( η 2 + α x α y ) 2 ] ,
x 2 = k B T κ x + κ y [ 1 + ξ 2 + κ y 2 ξ 2 + κ x κ y ] .
x 2 = 2 k B T κ x + κ y , ξ κ x , κ y ,
1 2 κ x x 2 + 1 2 κ y y 2 = k B T ,
( x y ) ω = 2 k B T γ η ( α y α x ) 2 i η ω [ ω 4 + ( α x 2 + α y 2 2 η 2 ) ω 2 + ( η 2 + α x α y ) 2 ] ,
x y = k B T κ x + κ y ξ ( κ y κ x ) ξ 2 + κ x κ y .
P ( x , y ) exp [ 1 2 r Gr ]
r Gr = r r r 1 r = 1.
r 2 = x 2 y 2 x y 2 y 2 cos 2 θ 2 x y cos θ sin θ + x 2 sin 2 θ ,
tan 2 θ ξ = 2 ξ ( κ x + κ y ) .
d W d t = 1 2 π ( f · v ) ω d ω ,
f ω · v ω * = i ω ξ [ x ω y ω ] [ 0 1 1 0 ] [ x ω * y ω * ] = i ω ξ ( x ω y ω * y ω x ω * ) = 2 ξ ω Im x ω y ω * ,
( f · v ) ω = 2 ξ ω Im ( x y ) ω .
d W d t = 4 k B T ξ 2 κ x + κ y .
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