The next generation of optoelectronic and photonic systems—with wide-ranging potential applications in image transmission, light-guiding-light signal processing, logic gates for computing, and medicine—may be realized through the invention of circuitry-free, rapidly reconfigurable systems powered by solitons. Optical spatial solitons are self-trapped optical beams of finite spatial cross section that travel without diverging like freely diffracting beams. These nonlinear waves propagate in photoresponsive materials through self-inscribed waveguides, which are generated when the materials locally change their refractive index in response to light intensity. In conventional nonlinear materials, self-trapping requires high-powered lasers or external electric fields.

Now, a team of researchers from the University of Pittsburgh, Harvard University, and McMaster University have developed a pH-responsive poly(acrylamide-co-acrylic acid) hydrogel, a hydrophilic three-dimensionally connected polymer network, in which light self-trapping can be turned rapidly on and off many times in a controllable and reversible way using a low-intensity visible laser. They report their work in a recent issue of Proceedings of the National Academy of Sciences.

Developed by Joanna Aizenberg’s group at Harvard University, the hydrogel contains critical covalently-tethered chromophores that absorb specific wavelengths of visible light and thereby transform their structure. In the absence of light, the gel is relaxed and the chromophores are predominantly in a ring-open merocyanine form. When the hydrogel is irradiated with visible light, the isomerization of merocyanine to its closed-ring spiropyran form triggers a local expulsion of water, a contraction of the hydrogel, and ultimately an increase in the refractive index along the irradiated path.

The novelty of this work is that this isomerization process is reversible. In the absence of light, the hydrogel reverts back to its original state.

The researchers demonstrated the reversible self-trapping process with experiments led by Kalaichelvi Saravanamuttu’s team at McMaster University—measuring the diameter and peak intensity of the beam over time using a 532 nm laser, optical lenses, neutral density filters, and a CCD camera. They also performed a series of control experiments, such as testing the hydrogel matrix without chromophores, to determine which parameters are critical for self-trapping.

“We determined it was important to have a hydrogel matrix that became more hydrophobic in the presence of light. It was important to have the chromophores covalently-tethered to the three-dimensional matrix to localize the refractive index change. And photoisomerization was critical in triggering this sequence of events,” says Saravanamuttu, an associate professor of chemistry and chemical biology and a senior author on the paper.

Schematic representation of optical self-trapping within spiropyran-functionalized hydrogels with two remote beams; each beam is switched on and off to control the interaction. Credit: PNAS doi.org/10.1073/pnas.1902872117

More surprising, when the researchers irradiated the hydrogel with two parallel lasers, the self-trapping beams interacted with each other when separated by distances up to 10 times the beam width. “They modulated each other, reducing their self-trapping efficiency, at remote distances through the interconnected and flexible network of the hydrogel,” Saravanamuttu says.

Being able to reversibly, predictably, and remotely control one self-trapped beam with another opens up the possibility of applications like all-optical computing using beams of ambient light. Traditional computations are performed using hard materials such as wires, semiconductors, and photodiodes to couple electronics to light. Instead, the researchers hope to control light with light. So far, they have already used the interactions of self-trapped beams to do basic binary arithmetic, says Saravanuamuttu.

These experimental results were confirmed by numerical simulations developed by senior authors Aizenberg, a professor of materials science and of chemistry and chemical biology at Harvard University, and Anna Balazs, a professor of chemical and petroleum engineering at the University of Pittsburgh, and their groups. Their model dynamically calculated the spatial and temporal evolution of the optical field as it propagated through the hydrogel, whose index of refraction was changing. Consistent with experiments, the model accurately captured the self-trapping dynamics and efficiency when using the single or double laser beams.

“This paper marks an interesting step forward that is indicative of the potential of one disruptive technology,” says John Sheridan, a professor of electrical and electronic engineering at the University College of Dublin, who was not involved in the research. “Technologies like this will provide core hardware components enabling the three-dimensional, all-optical connection and switching hardware needed for ‘Internet of things’ data integration and the 5G/6G telecommunications systems of the future.”

Currently, the speed of the waveguide formation and switching happens in seconds, though, rather than the nanoseconds typical of optoelectronic switches. So the researchers plan to investigate what parameters are slowing down the process and how to change them. For example, they will explore making the hydrogel more flexible to give the chromophores greater freedom to undergo isomerization in hopes of eliciting a faster response. They will also look at different types of isomerizable chromophores.

However, Saravanamuttu emphasizes they are not trying to replace digital computers that use conventional electronics, so speed may not be critical. Other potential applications include autonomous stimuli-responsive soft robotic systems for drug delivery or dynamic optics.

“This is particularly exciting because we see it as a material that can reciprocally interact with an environmental stimulus. It isn’t just turned on and off, but it actually changes its behavior in a dynamic way,” she says.

Read the article in Proceedings of the National Academy of Sciences.