Header logo is


2020


A gamified app that helps people overcome self-limiting beliefs by promoting metacognition
A gamified app that helps people overcome self-limiting beliefs by promoting metacognition

Amo, V., Lieder, F.

Virtual, SIG 8 Meets SIG 16, September 2020 (conference) Accepted

Abstract
Previous research has shown that approaching learning with a growth mindset is key for maintaining motivation and overcoming setbacks. Mindsets are systems of beliefs that people hold to be true. They influence a person's attitudes, thoughts, and emotions when they learn something new or encounter challenges. In clinical psychology, metareasoning (reflecting on one's mental processes) and meta-awareness (recognizing thoughts as mental events instead of equating them to reality) have proven effective for overcoming maladaptive thinking styles. Hence, they are potentially an effective method for overcoming self-limiting beliefs in other domains as well. However, the potential of integrating assisted metacognition into mindset interventions has not been explored yet. Here, we propose that guiding and training people on how to leverage metareasoning and meta-awareness for overcoming self-limiting beliefs can significantly enhance the effectiveness of mindset interventions. To test this hypothesis, we develop a gamified mobile application that guides and trains people to use metacognitive strategies based on Cognitive Restructuring (CR) and Acceptance Commitment Therapy (ACT) techniques. The application helps users to identify and overcome self-limiting beliefs by working with aversive emotions when they are triggered by fixed mindsets in real-life situations. Our app aims to help people sustain their motivation to learn when they face inner obstacles (e.g. anxiety, frustration, and demotivation). We expect the application to be an effective tool for helping people better understand and develop the metacognitive skills of emotion regulation and self-regulation that are needed to overcome self-limiting beliefs and develop growth mindsets.

re

A gamified app that helps people overcome self-limiting beliefs by promoting metacognition [BibTex]


no image
How to navigate everyday distractions: Leveraging optimal feedback to train attention control

Wirzberger, M., Lado, A., Eckerstorfer, L., Oreshnikov, I., Passy, J., Stock, A., Shenhav, A., Lieder, F.

Annual Meeting of the Cognitive Science Society, July 2020 (conference) Accepted

Abstract
To stay focused on their chosen tasks, people have to inhibit distractions. The underlying attention control skills can improve through reinforcement learning, which can be accelerated by giving feedback. We applied the theory of metacognitive reinforcement learning to develop a training app that gives people optimal feedback on their attention control while they are working or studying. In an eight-day field experiment with 99 participants, we investigated the effect of this training on people's productivity, sustained attention, and self-control. Compared to a control condition without feedback, we found that participants receiving optimal feedback learned to focus increasingly better (f = .08, p < .01) and achieved higher productivity scores (f = .19, p < .01) during the training. In addition, they evaluated their productivity more accurately (r = .12, p < .01). However, due to asymmetric attrition problems, these findings need to be taken with a grain of salt.

re sf

How to navigate everyday distractions: Leveraging optimal feedback to train attention control DOI Project Page [BibTex]


Event-triggered Learning
Event-triggered Learning

Solowjow, F., Trimpe, S.

Automatica, 117, Elsevier, July 2020 (article)

ics

arXiv PDF DOI Project Page [BibTex]

arXiv PDF DOI Project Page [BibTex]


no image
Leveraging Machine Learning to Automatically Derive Robust Planning Strategies from Biased Models of the Environment

Kemtur, A., Jain, Y. R., Mehta, A., Callaway, F., Consul, S., Stojcheski, J., Lieder, F.

Virtual, CogSci 2020, July 2020, Anirudha Kemtur and Yash Raj Jain contributed equally to this publication. (conference) Accepted

Abstract
Teaching clever heuristics is a promising approach to improve decision-making. We can leverage machine learning to discover clever strategies automatically. Current methods require an accurate model of the decision problems people face in real life. But most models are misspecified because of limited information and cognitive biases. To address this problem we develop strategy discovery methods that are robust to model misspecification. Robustness is achieved by model-ing model-misspecification and handling uncertainty about the real-world according to Bayesian inference. We translate our methods into an intelligent tutor that automatically discovers and teaches robust planning strategies. Our robust cognitive tutor significantly improved human decision-making when the model was so biased that conventional cognitive tutors were no longer effective. These findings highlight that our robust strategy discovery methods are a significant step towards leveraging artificial intelligence to improve human decision-making in the real world.

re

Leveraging Machine Learning to Automatically Derive Robust Planning Strategiesfrom Biased Models of the Environment [BibTex]


Actively Learning Gaussian Process Dynamics
Actively Learning Gaussian Process Dynamics

Buisson-Fenet, M., Solowjow, F., Trimpe, S.

2nd Annual Conference on Learning for Dynamics and Control, June 2020 (conference) Accepted

Abstract
Despite the availability of ever more data enabled through modern sensor and computer technology, it still remains an open problem to learn dynamical systems in a sample-efficient way. We propose active learning strategies that leverage information-theoretical properties arising naturally during Gaussian process regression, while respecting constraints on the sampling process imposed by the system dynamics. Sample points are selected in regions with high uncertainty, leading to exploratory behavior and data-efficient training of the model. All results are verified in an extensive numerical benchmark.

ics

ArXiv [BibTex]

ArXiv [BibTex]


Learning Constrained Dynamics with Gauss Principle adhering Gaussian Processes
Learning Constrained Dynamics with Gauss Principle adhering Gaussian Processes

Geist, A. R., Trimpe, S.

In 2nd Annual Conference on Learning for Dynamics and Control, June 2020 (inproceedings) Accepted

Abstract
The identification of the constrained dynamics of mechanical systems is often challenging. Learning methods promise to ease an analytical analysis, but require considerable amounts of data for training. We propose to combine insights from analytical mechanics with Gaussian process regression to improve the model's data efficiency and constraint integrity. The result is a Gaussian process model that incorporates a priori constraint knowledge such that its predictions adhere to Gauss' principle of least constraint. In return, predictions of the system's acceleration naturally respect potentially non-ideal (non-)holonomic equality constraints. As corollary results, our model enables to infer the acceleration of the unconstrained system from data of the constrained system and enables knowledge transfer between differing constraint configurations.

ics

Arxiv preprint [BibTex]

Arxiv preprint [BibTex]


Interface-mediated spontaneous symmetry breaking and mutual communication between drops containing chemically active particles
Interface-mediated spontaneous symmetry breaking and mutual communication between drops containing chemically active particles

Singh, D., Domínguez, A., Choudhury, U., Kottapalli, S., Popescu, M., Dietrich, S., Fischer, P.

Nature Communications, 11(2210), May 2020 (article)

Abstract
Symmetry breaking and the emergence of self-organized patterns is the hallmark of com- plexity. Here, we demonstrate that a sessile drop, containing titania powder particles with negligible self-propulsion, exhibits a transition to collective motion leading to self-organized flow patterns. This phenomenology emerges through a novel mechanism involving the interplay between the chemical activity of the photocatalytic particles, which induces Mar- angoni stresses at the liquid–liquid interface, and the geometrical confinement provided by the drop. The response of the interface to the chemical activity of the particles is the source of a significantly amplified hydrodynamic flow within the drop, which moves the particles. Furthermore, in ensembles of such active drops long-ranged ordering of the flow patterns within the drops is observed. We show that the ordering is dictated by a chemical com- munication between drops, i.e., an alignment of the flow patterns is induced by the gradients of the chemicals emanating from the active particles, rather than by hydrodynamic interactions.

pf icm

link (url) DOI [BibTex]


Data-efficient Auto-tuning with Bayesian Optimization: An Industrial Control Study
Data-efficient Auto-tuning with Bayesian Optimization: An Industrial Control Study

Neumann-Brosig, M., Marco, A., Schwarzmann, D., Trimpe, S.

IEEE Transactions on Control Systems Technology, 28(3):730-740, May 2020 (article)

Abstract
Bayesian optimization is proposed for automatic learning of optimal controller parameters from experimental data. A probabilistic description (a Gaussian process) is used to model the unknown function from controller parameters to a user-defined cost. The probabilistic model is updated with data, which is obtained by testing a set of parameters on the physical system and evaluating the cost. In order to learn fast, the Bayesian optimization algorithm selects the next parameters to evaluate in a systematic way, for example, by maximizing information gain about the optimum. The algorithm thus iteratively finds the globally optimal parameters with only few experiments. Taking throttle valve control as a representative industrial control example, the proposed auto-tuning method is shown to outperform manual calibration: it consistently achieves better performance with a low number of experiments. The proposed auto-tuning framework is flexible and can handle different control structures and objectives.

ics

arXiv (PDF) DOI Project Page [BibTex]

arXiv (PDF) DOI Project Page [BibTex]


no image
Automatic Discovery of Interpretable Planning Strategies

Skirzyński, J., Becker, F., Lieder, F.

May 2020 (article) Submitted

Abstract
When making decisions, people often overlook critical information or are overly swayed by irrelevant information. A common approach to mitigate these biases is to provide decisionmakers, especially professionals such as medical doctors, with decision aids, such as decision trees and flowcharts. Designing effective decision aids is a difficult problem. We propose that recently developed reinforcement learning methods for discovering clever heuristics for good decision-making can be partially leveraged to assist human experts in this design process. One of the biggest remaining obstacles to leveraging the aforementioned methods for improving human decision-making is that the policies they learn are opaque to people. To solve this problem, we introduce AI-Interpret: a general method for transforming idiosyncratic policies into simple and interpretable descriptions. Our algorithm combines recent advances in imitation learning and program induction with a new clustering method for identifying a large subset of demonstrations that can be accurately described by a simple, high-performing decision rule. We evaluate our new AI-Interpret algorithm and employ it to translate information-acquisition policies discovered through metalevel reinforcement learning. The results of three large behavioral experiments showed that the provision of decision rules as flowcharts significantly improved people’s planning strategies and decisions across three different classes of sequential decision problems. Furthermore, a series of ablation studies confirmed that our AI-Interpret algorithm was critical to the discovery of interpretable decision rules and that it is ready to be applied to other reinforcement learning problems. We conclude that the methods and findings presented in this article are an important step towards leveraging automatic strategy discovery to improve human decision-making.

re

Automatic Discovery of Interpretable Planning Strategies The code for our algorithm and the experiments is available [BibTex]


Spectrally selective and highly-sensitive UV photodetection with UV-A, C band specific polarity switching in silver plasmonic nanoparticle enhanced gallium oxide thin-film
Spectrally selective and highly-sensitive UV photodetection with UV-A, C band specific polarity switching in silver plasmonic nanoparticle enhanced gallium oxide thin-film

Arora, K., Singh, D., Fischer, P., Kumar, M.

Adv. Opt. Mat., March 2020 (article)

Abstract
Traditional photodetectors generally show a unipolar photocurrent response when illuminated with light of wavelength equal or shorter than the optical bandgap. Here, we report that a thin film of gallium oxide (GO) decorated with plasmonic nanoparticles, surprisingly, exhibits a change in the polarity of the photocurrent for different UV bands. Silver (Ag) nanoparticles are vacuum-deposited onto β-Ga2O3 and the AgNP@GO thin films show a record responsivity of 250 A/W, which significantly outperforms bare GO planar photodetectors. The photoresponsivity reverses sign from +157 µA/W in the UV-C band under unbiased operation to -353 µA/W in the UV-A band. The current reversal is rationalized by considering the charge dynamics stemming from hot electrons generated when the incident light excites a local surface plasmon resonance (LSPR) in the Ag nanoparticles. The Ag nanoparticles improve the external quantum efficiency and detectivity by nearly one order of magnitude with high values of 1.2×105 and 3.4×1014 Jones, respectively. This plasmon-enhanced solar blind GO detector allows UV regions to be spectrally distinguished, which is useful for the development of sensitive dynamic imaging photodetectors.

pf

[BibTex]


no image
Advancing Rational Analysis to the Algorithmic Level

Lieder, F., Griffiths, T. L.

Behavioral and Brain Sciences, 43, E27, March 2020 (article)

Abstract
The commentaries raised questions about normativity, human rationality, cognitive architectures, cognitive constraints, and the scope or resource rational analysis (RRA). We respond to these questions and clarify that RRA is a methodological advance that extends the scope of rational modeling to understanding cognitive processes, why they differ between people, why they change over time, and how they could be improved.

re

Advancing rational analysis to the algorithmic level DOI [BibTex]

Advancing rational analysis to the algorithmic level DOI [BibTex]


Acoustofluidic Tweezers for the 3D Manipulation of Microparticles
Acoustofluidic Tweezers for the 3D Manipulation of Microparticles

Guo, X., Ma, Z., Goyal, R., Jeong, M., Pang, W., Fischer, P., Dian, X., Qiu, T.

In 2020 IEEE International Conference on Robotics and Automation (ICRA),, Febuary 2020 (conference)

Abstract
Non-contact manipulation is of great importance in the actuation of micro-robotics. It is challenging to contactless manipulate micro-scale objects over large spatial distance in fluid. Here, we describe a novel approach for the dynamic position control of microparticles in three-dimensional (3D) space, based on high-speed acoustic streaming generated by a micro-fabricated gigahertz transducer. Due to the vertical lifting force and the horizontal centripetal force generated by the streaming, microparticles are able to be stably trapped at a position far away from the transducer surface, and to be manipulated over centimeter distance in all three directions. Only the hydrodynamic force is utilized in the system for particle manipulation, making it a versatile tool regardless the material properties of the trapped particle. The system shows high reliability and manipulation velocity, revealing its potentials for the applications in robotics and automation at small scales.

pf

[BibTex]

[BibTex]


no image
Learning to Overexert Cognitive Control in a Stroop Task

Bustamante, L., Lieder, F., Musslick, S., Shenhav, A., Cohen, J.

Febuary 2020, Laura Bustamante and Falk Lieder contributed equally to this publication. (article) In revision

Abstract
How do people learn when to allocate how much cognitive control to which task? According to the Learned Value of Control (LVOC) model, people learn to predict the value of alternative control allocations from features of a given situation. This suggests that people may generalize the value of control learned in one situation to other situations with shared features, even when the demands for cognitive control are different. This makes the intriguing prediction that what a person learned in one setting could, under some circumstances, cause them to misestimate the need for, and potentially over-exert control in another setting, even if this harms their performance. To test this prediction, we had participants perform a novel variant of the Stroop task in which, on each trial, they could choose to either name the color (more control-demanding) or read the word (more automatic). However only one of these tasks was rewarded, it changed from trial to trial, and could be predicted by one or more of the stimulus features (the color and/or the word). Participants first learned colors that predicted the rewarded task. Then they learned words that predicted the rewarded task. In the third part of the experiment, we tested how these learned feature associations transferred to novel stimuli with some overlapping features. The stimulus-task-reward associations were designed so that for certain combinations of stimuli the transfer of learned feature associations would incorrectly predict that more highly rewarded task would be color naming, which would require the exertion of control, even though the actually rewarded task was word reading and therefore did not require the engagement of control. Our results demonstrated that participants over-exerted control for these stimuli, providing support for the feature-based learning mechanism described by the LVOC model.

re

Learning to Overexert Cognitive Control in a Stroop Task DOI [BibTex]

Learning to Overexert Cognitive Control in a Stroop Task DOI [BibTex]


Investigating photoresponsivity of graphene-silver hybrid nanomaterials in the ultraviolet
Investigating photoresponsivity of graphene-silver hybrid nanomaterials in the ultraviolet

Deshpande, P., Suri, P., Jeong, H., Fischer, P., Ghosh, A., Ghosh, G.

J. Chem. Phys., 152, pages: 044709, January 2020 (article)

Abstract
There have been several reports of plasmonically enhanced graphene photodetectors in the visible and the near infrared regime but rarely in the ultraviolet. In a previous work, we have reported that a graphene-silver hybrid structure shows a high photoresponsivity of 13 A/W at 270 nm. Here, we consider the likely mechanisms that underlie this strong photoresponse. We investigate the role of the plasmonic layer and examine the response using silver and gold nanoparticles of similar dimensions and spatial arrangement. The effect on local doping, strain, and absorption properties of the hybrid is also probed by photocurrent measurements and Raman and UV-visible spectroscopy. We find that the local doping from the silver nanoparticles is stronger than that from gold and correlates with a measured photosensitivity that is larger in devices with a higher contact area between the plasmonic nanomaterials and the graphene layer.

pf

link (url) DOI [BibTex]

link (url) DOI [BibTex]


A High-Fidelity Phantom for the Simulation and Quantitative Evaluation of Transurethral Resection of the Prostate
A High-Fidelity Phantom for the Simulation and Quantitative Evaluation of Transurethral Resection of the Prostate

Choi, E., Adams, F., Gengenbacher, A., Schlager, D., Palagi, S., Müller, P., Wetterauer, U., Miernik, A., Fischer, P., Qiu, T.

Annals of Biomed. Eng., 48, pages: 437-446, January 2020 (article)

Abstract
Transurethral resection of the prostate (TURP) is a minimally invasive endoscopic procedure that requires experience and skill of the surgeon. To permit surgical training under realistic conditions we report a novel phantom of the human prostate that can be resected with TURP. The phantom mirrors the anatomy and haptic properties of the gland and permits quantitative evaluation of important surgical performance indicators. Mixtures of soft materials are engineered to mimic the physical properties of the human tissue, including the mechanical strength, the electrical and thermal conductivity, and the appearance under an endoscope. Electrocautery resection of the phantom closely resembles the procedure on human tissue. Ultrasound contrast agent was applied to the central zone, which was not detectable by the surgeon during the surgery but showed high contrast when imaged after the surgery, to serve as a label for the quantitative evaluation of the surgery. Quantitative criteria for performance assessment are established and evaluated by automated image analysis. We present the workflow of a surgical simulation on a prostate phantom followed by quantitative evaluation of the surgical performance. Surgery on the phantom is useful for medical training, and enables the development and testing of endoscopic and minimally invasive surgical instruments.

pf

link (url) DOI [BibTex]

link (url) DOI [BibTex]


no image
Sliding Mode Control with Gaussian Process Regression for Underwater Robots

Lima, G. S., Trimpe, S., Bessa, W. M.

Journal of Intelligent & Robotic Systems, January 2020 (article)

ics

DOI [BibTex]

DOI [BibTex]


Interactive Materials – Drivers of Future Robotic Systems
Interactive Materials – Drivers of Future Robotic Systems

Fischer, P.

Adv. Mat., January 2020 (article)

Abstract
A robot senses its environment, processes the sensory information, acts in response to these inputs, and possibly communicates with the outside world. Robots generally achieve these tasks with electronics-based hardware or by receiving inputs from some external hardware. In contrast, simple microorganisms can autonomously perceive, act, and communicate via purely physicochemical processes in soft material systems. A key property of biological systems is that they are built from energy-consuming ‘active’ units. Exciting developments in material science show that even very simple artificial active building blocks can show surprisingly rich emergent behaviors. Active non-equilibrium systems are therefore predicted to play an essential role to realize interactive materials. A major challenge is to find robust ways to couple and integrate the energy-consuming building blocks to the mechanical structure of the material. However, success in this endeavor will lead to a new generation of sophisticated micro- and soft-robotic systems that can operate autonomously.

pf

link (url) DOI [BibTex]


Hierarchical Event-triggered Learning for Cyclically Excited Systems with Application to Wireless Sensor Networks
Hierarchical Event-triggered Learning for Cyclically Excited Systems with Application to Wireless Sensor Networks

Beuchert, J., Solowjow, F., Raisch, J., Trimpe, S., Seel, T.

IEEE Control Systems Letters, 4(1):103-108, January 2020 (article)

ics

arXiv PDF DOI Project Page [BibTex]

arXiv PDF DOI Project Page [BibTex]


Toward a Formal Theory of Proactivity
Toward a Formal Theory of Proactivity

Lieder, F., Iwama, G.

January 2020 (article) Submitted

Abstract
Beyond merely reacting to their environment and impulses, people have the remarkable capacity to proactively set and pursue their own goals. But the extent to which they leverage this capacity varies widely across people and situations. The goal of this article is to make the mechanisms and variability of proactivity more amenable to rigorous experiments and computational modeling. We proceed in three steps. First, we develop and validate a mathematically precise behavioral measure of proactivity and reactivity that can be applied across a wide range of experimental paradigms. Second, we propose a formal definition of proactivity and reactivity, and develop a computational model of proactivity in the AX Continuous Performance Task (AX-CPT). Third, we develop and test a computational-level theory of meta-control over proactivity in the AX-CPT that identifies three distinct meta-decision-making problems: intention setting, resolving response conflict between intentions and automaticity, and deciding whether to recall context and intentions into working memory. People's response frequencies in the AX-CPT were remarkably well captured by a mixture between the predictions of our models of proactive and reactive control. Empirical data from an experiment varying the incentives and contextual load of an AX-CPT confirmed the predictions of our meta-control model of individual differences in proactivity. Our results suggest that proactivity can be understood in terms of computational models of meta-control. Our model makes additional empirically testable predictions. Future work will extend our models from proactive control in the AX-CPT to proactive goal creation and goal pursuit in the real world.

re

Toward a formal theory of proactivity DOI [BibTex]


Control-guided Communication: Efficient Resource Arbitration and Allocation in Multi-hop Wireless Control Systems
Control-guided Communication: Efficient Resource Arbitration and Allocation in Multi-hop Wireless Control Systems

Baumann, D., Mager, F., Zimmerling, M., Trimpe, S.

IEEE Control Systems Letters, 4(1):127-132, January 2020 (article)

ics

arXiv PDF DOI [BibTex]

arXiv PDF DOI [BibTex]


no image
ACTrain: Ein KI-basiertes Aufmerksamkeitstraining für die Wissensarbeit [ACTrain: An AI-based attention training for knowledge work]

Wirzberger, M., Oreshnikov, I., Passy, J., Lado, A., Shenhav, A., Lieder, F.

66th Spring Conference of the German Ergonomics Society, 2020 (conference)

Abstract
Unser digitales Zeitalter lebt von Informationen und stellt unsere begrenzte Verarbeitungskapazität damit täglich auf die Probe. Gerade in der Wissensarbeit haben ständige Ablenkungen erhebliche Leistungseinbußen zur Folge. Unsere intelligente Anwendung ACTrain setzt genau an dieser Stelle an und verwandelt Computertätigkeiten in eine Trainingshalle für den Geist. Feedback auf Basis maschineller Lernverfahren zeigt anschaulich den Wert auf, sich nicht von einer selbst gewählten Aufgabe ablenken zu lassen. Diese metakognitive Einsicht soll zum Durchhalten motivieren und das zugrunde liegende Fertigkeitsniveau der Aufmerksamkeitskontrolle stärken. In laufenden Feldexperimenten untersuchen wir die Frage, ob das Training mit diesem optimalen Feedback die Aufmerksamkeits- und Selbstkontrollfertigkeiten im Vergleich zu einer Kontrollgruppe ohne Feedback verbessern kann.

re sf

link (url) Project Page [BibTex]


Spatial Scheduling of Informative Meetings for Multi-Agent Persistent Coverage
Spatial Scheduling of Informative Meetings for Multi-Agent Persistent Coverage

Haksar, R. N., Trimpe, S., Schwager, M.

IEEE Robotics and Automation Letters, 2020 (article) Accepted

ics

DOI [BibTex]

DOI [BibTex]


Safe and Fast Tracking on a Robot Manipulator: Robust MPC and Neural Network Control
Safe and Fast Tracking on a Robot Manipulator: Robust MPC and Neural Network Control

Nubert, J., Koehler, J., Berenz, V., Allgower, F., Trimpe, S.

IEEE Robotics and Automation Letters, 2020 (article) Accepted

Abstract
Fast feedback control and safety guarantees are essential in modern robotics. We present an approach that achieves both by combining novel robust model predictive control (MPC) with function approximation via (deep) neural networks (NNs). The result is a new approach for complex tasks with nonlinear, uncertain, and constrained dynamics as are common in robotics. Specifically, we leverage recent results in MPC research to propose a new robust setpoint tracking MPC algorithm, which achieves reliable and safe tracking of a dynamic setpoint while guaranteeing stability and constraint satisfaction. The presented robust MPC scheme constitutes a one-layer approach that unifies the often separated planning and control layers, by directly computing the control command based on a reference and possibly obstacle positions. As a separate contribution, we show how the computation time of the MPC can be drastically reduced by approximating the MPC law with a NN controller. The NN is trained and validated from offline samples of the MPC, yielding statistical guarantees, and used in lieu thereof at run time. Our experiments on a state-of-the-art robot manipulator are the first to show that both the proposed robust and approximate MPC schemes scale to real-world robotic systems.

am ics

arXiv PDF DOI [BibTex]

arXiv PDF DOI [BibTex]

2005


Nonlinear optical spectroscopy of chiral molecules
Nonlinear optical spectroscopy of chiral molecules

Fischer, P., Hache, F.

CHIRALITY, 17(8):421-437, 2005 (article)

Abstract
We review nonlinear optical processes that are specific to chiral molecules in solution and on surfaces. In contrast to conventional natural optical activity phenomena, which depend linearly on the electric field strength of the optical field, we discuss how optical processes that are nonlinear (quadratic, cubic, and quartic) functions of the electromagnetic field strength may probe optically active centers and chiral vibrations. We show that nonlinear techniques open entirely new ways of exploring chirality in chemical and biological systems: The cubic processes give rise to nonlinear circular dichroism and nonlinear optical rotation and make it possible to observe dynamic chiral processes at ultrafast time scales. The quadratic second-harmonic and sum-frequency-generation phenomena and the quartic processes may arise entirely in the electric-dipole approximation and do not require the use of circularly polarized light to detect chirality: They provide surface selectivity and their observables can be relatively much larger than in linear optical activity. These processes also give rise to the generation of light at a new color, and in liquids this frequency conversion only occurs if the solution is optically active. We survey recent chiral nonlinear optical experiments and give examples of their application to problems of biophysical interest. (C) 2005 Wiley-Liss, Inc.

pf

DOI [BibTex]

2005


DOI [BibTex]


Negative refraction at optical frequencies in nonmagnetic two-component molecular media
Negative refraction at optical frequencies in nonmagnetic two-component molecular media

Chen, Y., Fischer, P., Wise, F.

PHYSICAL REVIEW LETTERS, 95(6), 2005 (article)

Abstract
There is significant motivation to develop media with negative refractive indices at optical frequencies, but efforts in this direction are hampered by the weakness of the magnetic response at such frequencies. We show theoretically that a nonmagnetic medium with two atomic or molecular constituents can exhibit a negative refractive index. A negative index is possible even when the real parts of both the permittivity and permeability are positive. This surprising result provides a route to isotropic negative-index media at optical frequencies.

pf

DOI [BibTex]

DOI [BibTex]

2001


Isotropic second-order nonlinear optical susceptibilities
Isotropic second-order nonlinear optical susceptibilities

Fischer, P., Buckingham, A., Albrecht, A.

PHYSICAL REVIEW A, 64(5), 2001 (article)

Abstract
The second-order nonlinear optical susceptibility, in the electric dipole approximation, is only nonvanishing for materials that are noncentrosymmetric. Should the medium be isotropic, then only a chiral system. such as an optically active liquid, satisfies this symmetry requirement. We derive the quantum-mechanical form of the isotropic component of the sum- and difference-frequency susceptibility and discuss its unusual spectral properties. We show that any coherent second-order nonlinear optical process in a system of randomly oriented molecules requires the medium to be chiral. and the incident frequencies to be different and nonzero. Furthermore, a minimum of two nondegenerate excited molecular states are needed for the isotropic part of the susceptibility to be nonvanishing. The rotationally invariant susceptibility is zero in the static field limit and shows exceptionally sensitive resonance and dephasing effects that are particular to chiral centers.

pf

DOI [BibTex]

2001


DOI [BibTex]


Reply to ``Comment on `Phenomenological damping in optical response tensors'{''}
Reply to “Comment on ‘Phenomenological damping in optical response tensors’”

Buckingham, A., Fischer, P.

PHYSICAL REVIEW A, 63(4), 2001 (article)

Abstract
We show that damping factors must not be incorporated in the perturbation of the ground state by a static electric field. If they are included, as in the theory of Stedman et al. {[}preceding Comment. Phys. Rev. A 63, 047801 (2001)], then there would be an electric dipole in the y direction induced in a hydrogen atom in the M-s = + 1/2 state by a static electric field in the x direction. Such a dipole is excluded by symmetry.

pf

DOI [BibTex]