Electrocaloric (EC) materials show promise in eco-friendly solid-state refrigeration and integrable on-chip thermal management. While direct measurement of EC thin-films still remains challenging, a generic theoretical framework for quantifying the cooling properties of rich EC materials including normal-, relaxor-, organic- and anti-ferroelectrics is imperative for exploiting new flexible and room-temperature cooling alternatives. Here, we present a versatile theory that combines Master equation with Maxwell relations and analytically relates the macroscopic cooling responses in EC materials with the intrinsic diffuseness of phase transitions and correlation characteristics. Under increased electric fields, both EC entropy and adiabatic temperature changes increase quadratically initially, followed by further linear growth and eventual gradual saturation. The upper bound of entropy change (∆S_max) is limited by distinct correlation volumes (V _cr ) and transition diffuseness. The linearity between V _cr and the transition diffuseness is emphasized, while ∆S_max = 300 kJ/(K.m³) is obtained for Pb_0.8Ba_0.2ZrO₃. The ∆S_max in antiferroelectric Pb_0.95Zr_0.05TiO₃, Pb_0.8Ba_0.2ZrO₃ and polymeric ferroelectrics scales proportionally with V _cr^-2.2, owing to the one-dimensional structural constraint on lattice-scale depolarization dynamics; whereas ∆S_max in relaxor and normal ferroelectrics scales as ∆S_max ~ V _cr^-0.37, which tallies with a dipolar interaction exponent of 2/3 in EC materials and the well-proven fractional dimensionality of 2.5 for ferroelectric domain walls.

A combination of ultrafast, long-range, and low-loss excitation energy transfer from the photoreceptor location to a functionally active site is essential for cost-effective polymeric semiconductors. Delocalized electronic wavefunctions along π-conjugated polymer (CP) backbone can enable efficient intrachain transport, while interchain transport is generally thought slow and lossy due to weak chain-chain interactions. In contrast to the conventional strategy of mitigating structural disorder, amorphous layers of rigid CPs, exemplified by highly planar poly(indacenodithiophene-co-benzothiadiazole) (IDT-BT) donor-accepter copolymer, exhibit trap-free transistor performance and charge-carrier mobilities similar to amorphous silicon. Here, we report long-range exciton transport in HJ-aggregated IDTBT thin-film, in which the competing exciton transport and exciton-exciton annihilation (EEA) dynamics are spectroscopically separated using a phase-cycling-based scheme and shown to depart from the classical diffusion-limited and strong-coupling regime. In the thin film, we find an annihilation-limited mechanism with ≪100% per-encounter annihilation probability, facilitating the minimization of EEA-induced excitation losses. In contrast, excitons on isolated IDTBT chains diffuse over 350 nm with 0.56 cm² s^-1 diffusivity, before eventually annihilating with unit probability on first contact. We complement the pump-probe studies with temperature-dependent photocurrent and EEA measurements from 295 K to 77 K and find a remarkable correspondence of annihilation rate and photocurrent activation energies in the 140 K to 295 K temperature range.

Abstract: Wavefront shaping, which is often achieved using liquid crystal (LC) spatial light modulators, is particularly important for a wide range of applications including laser microfabrication and micromanipulation, microscopy, and quantum optics. In this work, results are presented for the first integrated LC phase modulator that combines a flexoelectro‐optic LC layer (that behaves as a switchable λ/2 waveplate) with a polymerized reactive mesogen layer (which acts as a λ/4 waveplate) and a mirrored substrate that creates a double‐pass geometry. For a flexoelectro‐optic LC layer that exhibits switching angles of ±45° at a voltage of ±85 V a full 2π phase modulation is observed when driven by a 1 kHz waveform. Experimental results are also compared with modeling using Jones calculus of the amplitude and phase variation when the LC and the polymer layer deviate from their desired waveplate conditions. The development and demonstration of an integrated device is particularly significant for applications where size and cost are critical factors such as in LiDAR for the Space and Automotive industries, respectively.