Critical Casimir Effect Research Articles

Critical Casimir effect in a disordered O(2)-symmetric model.

The critical Casimir effect appears when critical fluctuations of an order parameter interact with classical boundaries. We investigate this effect in the setting of a Landau-Ginzburg model with continuous symmetry in the presence of quenched disorder. The quenched free energy is written as an asymptotic series of moments of the model's partition function. Our main result is that, in the presence of a strong disorder, Goldstone modes of the system contribute either with either an attractive or a repulsive force. This result was obtained using the distributional zeta-function method without relying on any particular ansatz in the functional space of the moments of the partition function.

Robust orbital diamagnetism in correlated Dirac fermions

We study orbital diamagnetism at zero temperature in (2 + 1)-dimensional Dirac fermions with a short-range interaction which exhibits a quantum phase transition to a charge density wave (CDW) phase. We introduce orbital magnetic fields into spinless Dirac fermions on the π-flux square lattice, and analyze them by using infinite density matrix renormalization group. It is found that the diamagnetism remains intact in the Dirac semimetal regime, while it is monotonically suppressed in the CDW regime. Around the quantum critical point of the CDW phase transition, we find a scaling behavior of the diamagnetism characteristic of the chiral Ising universality class. Besides, the scaling analysis implies that the robust orbital diamagnetism at weak magnetic fields in a Dirac semimetal regime would hold not only in our model but also in other interacting Dirac fermion systems as long as scaling regions are wide enough. The scaling behavior may also be regarded as a quantum, magnetic analogue of the critical Casimir effect which has been widely studied for classical phase transitions.

Controlled deposition of nanoparticles with critical Casimir forces.

Nanocrystal assembly represents the key fabrication step to develop next-generation optoelectronic devices with properties defined from the bottom-up. Despite numerous efforts, our limited understanding of nanoscale interactions has so far delayed the establishment of assembly conditions leading to reproducible superstructure morphologies, therefore hampering integration with large-scale, industrial processes. In this work, we demonstrate the deposition of a layer of semiconductor nanocrystals on a flat and unpatterned silicon substrate as mediated by the interplay of critical Casimir attraction and electrostatic repulsion. We show experimentally and rationalize with Monte Carlo and molecular dynamics simulations how this assembly process can be biased towards the formation of 2D layers or 3D islands and how the morphology of the deposited superstructure can be tuned from crystalline to amorphous. Our findings demonstrate the potential of the critical Casimir interaction to direct the growth of future artificial solids based on nanocrystals as the ultimate building blocks.

Gelation of Anisotropic Colloids with Short-Range Attraction

Gels are dilute connected networks that form solids at very low particle volume fraction with rich rheological properties. The kinetic process of gelation is central to understand the flow of complex fluids. Here, we report a simulation study of colloidal gelation formed by anisotropic colloids with attractive Lennard-Jones potential. These forces quasi-model the critical Casimir effect far from the critical solvent fluctuations acting on colloidal patches. By tuning the depths of the patch-to-patch particle interactions and the selected colloidal patches, we dynamically arrest the colloids to form gels. We find that thermal density fluctuation is the key factor to activate colloidal cluster space spanning: the balance between clustering and break-up mechanism plays a major role in the gelation process of anisotropic systems. These results offer new opportunities for studying the structural modifications of colloidal gels formed by anisotropic particles, and shed light on non-equilibrium behavior of anisotropic colloidal building blocks.

Simulation of lattice statistical models with defects: Critical Casimir Effect

The influence of lattice structure defects on phase transition phenomena was studied in framework of 2D spin model. Effective mass of defect was proposed for investigation of conformal properties of the model at critical point. The volume dependence of defect’s mass at critical point and the Critical Casimir interaction of two defects were studied. It was shown that this Casimir interaction is attraction for any value of hopping parameter. The confinement of the defect on the defects line and the process of defects line collapse were studied. Applications in nanophysics and biophysics were discussed.

Nanoparticle separation based on size-dependent aggregation of nanoparticles due to the critical Casimir effect.

Nanoparticles typically have an inherent wide size distribution that may affect the performance and reliability of many nanomaterials. Because the synthesis and purification of nanoparticles with desirable sizes are crucial to the applications of nanoparticles in various fields including medicine, biology, health care, and energy, there is a great need to search for more efficient and generic methods for size-selective nanoparticle purification/separation. Here we propose and conclusively demonstrate the effectiveness of a size-selective particle purification/separation method based on the critical Casimir force. The critical Casimir force is a generic interaction between colloidal particles near the solvent critical point and has been extensively studied in the past several decades due to its importance in reversibly controlling the aggregation and stability of colloidal particles. Combining multiple experimental techniques, we found that the critical Casimir force-induced aggregation depends on relative particle sizes in a system with larger ones aggregating first and the smaller ones remaining in solution. Based on this observation, a new size-dependent nanoparticle purification/separation method is proposed and demonstrated to be very efficient in purifying commercial silica nanoparticles in the lutidine/water binary solvent. Due to the ubiquity of the critical Casimir force for many colloidal particles in binary solvents, this method might be applicable to many types of colloidal particles.

Solvent-mediated forces in critical fluids.

The effective interaction between two planar walls immersed in a fluid is investigated by use of density functional theory in the supercritical region of the phase diagram. A hard core Yukawa model of fluid is studied with special attention to the critical region. To achieve this goal a formulation of the weighted density approximation coupled with the hierarchical reference theory, able to deal with critical long wavelength fluctuations, is put forward and compared with other approaches. The effective interaction between the walls is seen to change character on lowering the temperature: The strong oscillations induced by layering of the molecules, typical of the depletion mechanism in hard core systems, are gradually smoothed and, close to the critical point, a long range attractive tail emerges leading to a scaling form which agrees with the expectations based on the critical Casimir effect. Strong corrections to scaling are seen to affect the results up to very small reduced temperatures. By use of the Derjaguin approximation, this investigation has natural implications for the aggregation of colloidal particles in critical solvents.

Critical Casimir effect in the Ising strips with standard normal and ordinary boundary conditions and the grain boundary

We consider critical Casimir force in the Ising strips with boundary conditions defined by standard normal and ordinary surface universality classes containing also the internal grain boundary. Using exact variational approach of Mikheev and Fisher we have elaborated on behaviors of Casimir amplitudes Δ++(g), ΔOO(g) and Δ+O(g), corresponding to normal–normal, ordinary–ordinary and mixed normal–ordinary boundary conditions, respectively, with g as a strength of the grain boundary. Closed analytic results describe Casimir amplitudes Δ++(g) and ΔOO(g) as continuous functions of the grain boundary’s strength g, changing the character of the Casimir force from repulsive to attractive and vice versa for certain domains of g. Present results reveal a new type of symmetry between Casimir amplitudes Δ++(g) and ΔOO(g). Unexpectedly simple constant result for the Casimir amplitude Δ+O(g)=π12 we have comprehensively interpreted in terms of equilibrium states of the present Ising strip as a complex interacting system comprising two sub-systems. Short-distance expansions of energy density profiles in the vicinity of the grain boundary reveal new distant-wall correction amplitudes that we examined in detail. Analogy of present considerations with earlier more usual short-distance expansions near one of the (N), (O) and (SB) boundaries, as well as close to surfaces with variable boundary conditions refers to the set of scaling dimensions appearing in the present calculations but also to the discovery of the de Gennes–Fisher distant wall correction amplitudes.

Critical Casimir interactions between Janus particles.

Recently there has been strong experimental and theoretical interest in studying the self-assembly and the phase behavior of patchy and Janus particles, which form colloidal suspensions. Although in this quest a variety of effective interactions have been proposed and used in order to achieve a directed assembly, the critical Casimir effect stands out as being particularly suitable in this respect because it provides both attractive and repulsive interactions as well as the potential of a sensitive temperature control of their strength. Specifically, we have calculated the critical Casimir force between a single Janus particle and a laterally homogeneous substrate as well as a substrate with a chemical step. We have used the Derjaguin approximation and compared it with results from full mean field theory. A modification of the Derjaguin approximation turns out to be generally reliable. Based on this approach we have derived the effective force and the effective potential between two Janus cylinders as well as between two Janus spheres.

Formation probabilities in quantum critical chains and Casimir effect

We find a connection between logarithmic formation probabilities of two disjoint intervals of quantum critical spin chains and the Casimir energy of two aligned needles in two-dimensional classical critical systems. Using this connection we provide a formula for the logarithmic formation probability of two disjoint intervals in generic (1 + 1)-dimensional critical systems. The quantity is depenedent on the full structure of the underlying conformal field theory and so useful to find the universality class of the critical system. The connection that we find also provides a very efficient numerical method to calculate the Casimir energy between needles using quantum critical chains. The agreement between numerical results performed on the critical transverse-field Ising model and the XX chain with our exact results is very good. We also comment on the mutual Rényi information of two disjoint intervals.

Line contribution to the critical Casimir force between a homogeneous and a chemically stepped surface

Recent experimental realizations of the critical Casimir effect have been implemented by monitoring colloidal particles immersed in a binary liquid mixture near demixing and exposed to a chemically structured substrate. In particular, critical Casimir forces have been measured for surfaces consisting of stripes with periodically alternating adsorption preferences, forming chemical steps between them. Motivated by these experiments, we analyze the contribution of such chemical steps to the critical Casimir force for the film geometry and within the Ising universality class. By means of Monte Carlo simulations, mean-field theory and finite-size scaling analysis we determine the universal scaling function associated with the contribution to the critical Casimir force due to individual, isolated chemical steps facing a surface with homogeneous adsorption preference or with Dirichlet boundary condition. In line with previous findings, these results allow one to compute the critical Casimir force for the film geometry and in the presence of arbitrarily shaped, but wide stripes. In this latter limit the force decomposes into a sum of the contributions due to the two homogeneous parts of the surface and due to the chemical steps between the stripes. We assess this decomposition by comparing the resulting sum with actual simulation data for the critical Casimir force in the presence of a chemically striped substrate.

Alignment of cylindrical colloids near chemically patterned substrates induced by critical Casimir torques

Recent experiments have demonstrated a fluctuation-induced lateral trapping of spherical colloidal particles immersed in a binary liquid mixture near its critical demixing point and exposed to chemically patterned substrates. Inspired by these experiments, we study this kind of effective interaction, known as the critical Casimir effect, for elongated colloids of cylindrical shape. This adds orientational degrees of freedom. When the colloidal particles are close to a chemically structured substrate, a critical Casimir torque acting on the colloids emerges. We calculate this torque on the basis of the Derjaguin approximation. The range of validity of the latter is assessed via mean-field theory. This assessment shows that the Derjaguin approximation is reliable in experimentally relevant regimes, so that we extend it to Janus particles endowed with opposing adsorption preferences. Our analysis indicates that critical Casimir interactions are capable of achieving well-defined, reversible alignments both of chemically homogeneous and of Janus cylinders.

Nonequilibrium Critical Casimir Effect in Binary Fluids

Colloids immersed in a critical binary liquid mixture are subject to critical Casimir forces (CCFs) because they confine its concentration fluctuations and influence the latter via effective surface fields. To date, CCFs have been primarily studied in thermodynamic equilibrium. However, due to the critical slowing down, the order parameter around a particle can easily be perturbed by any motion of the colloid or by solvent flow. This leads to significant but largely unexplored changes in the CCF. Here we study the drag force on a single colloidal particle moving in a near-critical fluid mixture and the relative motion of two colloids due to the CCF acting on them. In order to account for the kinetic couplings among the order parameter field, the solvent velocity field, and the particle motion, we use a fluid particle dynamics method. These studies extend the understanding of CCFs from thermal equilibrium to nonequilibrium processes, which are relevant to current experiments, and show the emergence of significant effects near the critical point.

Statistics of the work done by splitting a one-dimensional quasicondensate

Motivated by experiments on splitting one-dimensional quasicondensates, we study the statistics of the work done by a quantum quench in a bosonic system. We discuss the general features of the probability distribution of the work and focus on its behavior at the lowest energy threshold, which develops an edge singularity. A formal connection between this probability distribution and the critical Casimir effect in thin classical films shows that certain features of the edge singularity are universal as the postquench gap tends to zero. Our results are quantitatively illustrated by an exact calculation for noninteracting bosonic systems. The effects of finite system size, dimensionality, and nonzero initial temperature are discussed in detail.

Controlling colloidal phase transitions with critical Casimir forces

The critical Casimir force provides a thermodynamic analogue of the quantum mechanical Casimir force that arises from the confinement of electromagnetic field fluctuations. In its thermodynamic analogue, two surfaces immersed in a critical solvent mixture attract each other due to confinement of solvent concentration fluctuations. Here, we demonstrate the active assembly control of colloidal equilibrium phases using critical Casimir forces. We guide colloidal particles into analogues of molecular liquid and solid phases via exquisite control over their interactions. By measuring the critical Casimir pair potential directly from density fluctuations in the colloidal gas, we obtain insight into liquefaction at small scales. We apply the van der Waals model of molecular liquefaction and show that the colloidal gas-liquid condensation is accurately described by the van der Waals theory, even on the scale of a few particles. These results open up new possibilities in the active assembly control of micro and nanostructures.

Large Deviations and Universality in Quantum Quenches

We study the large deviation statistics of the intensive work done by globally changing a control parameter in a thermally isolated quantum many-body system. We show that, upon approaching a critical point, large deviations well below the mean work display universal features related to the critical Casimir effect in the corresponding classical system. Large deviations well above the mean are, instead, of quantum nature and not captured by the quantum-to-classical correspondence. For a bosonic system we show that in this latter regime a transition from exponential to power-law statistics, analogous to the equilibrium Bose-Einstein condensation, may occur depending on the parameters of the quench and on the spatial dimensionality.

Supercritical Casimir effect in carbon dioxide

We present the first measurement of surface forces across supercritical carbon dioxide. An important finding is that long-range attractive surface forces are detected not just near the critical point, but along the supercritical extension of the coexistence line, which is commonly discussed as the supercritical ridge.Using a precisely adjustable model slit pore, our experiment can measure the change of thermodynamic potential together with changes in refractive index (mass density) in the confined CO2. The model slit pore is realized between two atomically smooth mica surfaces in a specially designed high-pressure surface forces apparatus. Our data suggest that thermal fluctuations of higher density are selectively depleted, which results in observation of a time- and space-averaged density reduction in the confined film. Direct observation of this confinement effect has consequences for theoretical understanding as well as technological applications of CO2 in porous materials.In the presence of small amounts of an acrylate solute (polyethyleneglycol-dimethacrylate), we found that multiple stable menisci of solute can be created between the surfaces and stretched out several micrometers. These liquid-liquid bridges are observed as an apparent birefringence effect. We demonstrate the critical character of the phenomena and discuss our findings in terms of a (super)critical Casimir effect.

The critical Casimir effect in films for generic non-symmetry-breaking boundary conditions

Systems described by an O(n) symmetrical ϕ4 Hamiltonian are considered in a d-dimensional film geometry at their bulk critical points. A detailed renormalization group (RG) study of the critical Casimir forces induced between the film's boundary planes , by thermal fluctuations is presented for the case where the O(n) symmetry remains unbroken by the surfaces. The boundary planes are assumed to cause short-range disturbances of the interactions that can be modelled by standard surface contributions ∝ϕ2 corresponding to subcritical or critical enhancement of the surface interactions. This translates into mesoscopic boundary conditions of the generic symmetry-preserving Robin type . RG-improved perturbation theory and Abel–Plana techniques are used to compute the L-dependent part fres of the reduced excess free energy per film area A → ∞ to two-loop order. When d < 4, it takes the scaling form fres ≈ D(c1LΦ/ν,c2LΦ/ν)/Ld−1 as L → ∞, where ci are scaling fields associated with the surface-enhancement variables c˚i, while Φ is a standard surface crossover exponent. The scaling function D(c1,c2) and its analogue for the Casimir force are determined via expansion in ϵ = 4 − d and extrapolated to d = 3 dimensions. In the special case c1 = c2 = 0, the expansion becomes fractional. Consistency with the known fractional expansions of D(0,0) and to order ϵ3/2 is achieved by appropriate reorganization of RG-improved perturbation theory. For appropriate choices of c1 and c2, the Casimir forces can have either sign. Furthermore, crossovers from attraction to repulsion and vice versa may occur as L increases.

Radiative dark–bright instability and the critical Casimir effect in DQW exciton condensates

It is already well known that radiative interband interaction in the excitonic normal liquid in semiconducting double quantum wells is responsible for a negligible splitting between the energies of the dark and bright excitons enabling us to consider a four fold spin degeneracy. This has also lead many workers to naively consider the same degeneracy in studying the condensate. On the other hand, the non-perturbative aspects of this interaction in the condensed phase, e.g. its consequences on the order parameter and the dark–bright mixture in the ground state have not been explored. In this work, we demonstrate that the ground state concentrations of the dark and the bright exciton condensates are dramatically different beyond a sharp interband coupling threshold where the contribution of the bright component in the ground state vanishes. This shows that the effect of the radiative interband interaction on the condensate is nonperturbative. We also observe in the free energy a discontinuous derivative with respect to the layer separation at the entrance to the condensed phase, indicating a strong critical Casimir force. An estimate of its strength shows that it is measurable. Measuring the Casimir force is challenging, but at the same time it has a conclusive power about the presence of the long sought for condensed phase.

Solvation forces in Ising films with long-range boundary fields: density-matrix renormalization-group study

Using the quasi-exact density-matrix renormalization-group method we calculate the solvation forces in two-dimensional Ising films of thickness L subject to identical algebraically decaying boundary fields with various decay exponents p. At the bulk critical point the solvation force acquires a universal contribution which is long-ranged in L due to the critical fluctuations, a phenomenon known as the critical Casimir effect. For p = 2, 3 and 50, we study the scaling behaviour of the solvation force along the pseudo-phase coexistence and along the critical and sub-critical isotherms.