Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Journal of Lightwave Technology

Replica Symmetry Breaking Reveals the Emission Mechanism of FRET-Assisted Random Laser

Jiangying Xia, Xiaojuan Zhang, Erlei Wang, Lei Hu, Tianyu Yang, Wenyu Du, Jiajun Ma, Kaiming Zhou, Lin Zhang, Kang Xie, Benli Yu, Junxi Zhang, Zhijia Hu

Published Aug 20, 2024• 8 citations
Publisher

Abstract

Fȍrster resonance energy transfer (FRET) is a fundamental approach for fabricating widely tunable (≥100 nm) random lasers and cascaded ones, which are the fundamental direction for achieving applications breakthroughs of random lasers in multi-fields, such as speckle-free imaging and biosensing. However, it is challenging to realize due to a lack of method to investigate the emission mechanism and emission characteristics of FRET-assisted random laser. In this work, the replica symmetry breaking and the Lévy flight are introduced to investigate the dynamical emission mechanism of FRET-assisted random laser. It is revealed that FRET can induce the disorder in random laser to frustrate coherently oscillating modes, resulting in a non-trivial interaction between the modes, which generates discrete emission field. This emission field exhibits low spatiotemporal coherence, which is essential for using random laser in super-resolution spectroscopy and even photolithography. Meanwhile, the phase diagram of dynamics during the FRET is derived to reveal the dynamical evolution of the interaction between random laser modes during FRET, which illustrates how FRET influences the emissions properties of random laser. This work broadens not only the approach for exploring order physical principles in disorder random laser based on statistical analysis methods, but also provides the theoretical support for the design of complex energy level random lasers with special application properties.

DOI
10.1109/jlt.2024.3446824

Related papers

Photon Statistics and Dynamics of Fluorescence Resonance Energy Transfer

Andrew J. Berglund, Andrew C. Doherty, Hideo Mabuchi

We report high time-resolution measurements of photon statistics from pairs of dye molecules coupled by fluorescence resonance energy transfer (FRET). In addition to quantum-optical photon antibunching, we observe photon bunching on a time scale of several nanoseconds. We show by numerical simulation that configuration fluctuations in the coupled fluorophore system could account for minor deviations of our data from predictions of basic Förster theory. With further characterization we believe that FRET photon statistics could provide a unique tool for studying DNA mechanics on time scales from 10(-9)-10(-3) s.

arXiv:cond-mat/0206301•Physical Review Letters•Jul 18, 2002•74 citations

A Self-Consistent Quantum Field Theory for Random Lasing

Andreas Lubatsch, Regine Frank

The spatial formation of coherent random laser modes in strongly scattering disordered random media is a central feature in the understanding of the physics of random lasers. We derive a quantum field theoretical method for random lasing in disordered samples of complex amplifying Mie resonators which is able to provide self-consistently and free of any fit parameter the full set of transport characteristics at and above the laser phase transition. The coherence length and the correlation volume respectively is derived as an experimentally measurable scale of the phase transition at the laser threshold. We find that the process of stimulated emission in extended disordered arrangements of active Mie resonators is ultimately connected to time-reversal symmetric multiple scattering in the sense of photonic transport while the diffusion coefficient is finite. A power law is found for the random laser mode diameters in stationary state with increasing pump intensity.

arXiv:1509.01873•Applied Sciences•Jun 18, 2019•17 citations

Time sequence variation of incoherent and coherent random laser based on positive replica of abalone shell

Jiawei Li, Juntao Li, Shu Hu +4 more

Besides the scattering structures, the energy transfer (ET) process in the gain medium plays a significant role in the competition between coherent (comprising strongly coherent components) and incoherent (consisting of weakly coherent or "hidden" coherent components) modes of random lasers. In this study, bichromatic emission random lasers were successfully created using polydimethylsiloxane (PDMS) replicas with grooved structures that imitate the inner surface of abalone shells as scattering substrates. The influence mechanism of the ET process from the monomer to dimer in the Rhodamine 640 dye on the competition of random laser modes was thoroughly investigated from both spectral and temporal dimensions. It was confirmed that the ET process can reduce the gain of monomers while amplifying the gain of dimers. By considering the dominant high-efficiency ET processes, an energy transfer factor associated with the pump energy density was determined. Notably, for the first time, it was validated that the statistical distribution characteristics of the time sequence variations in the coherent random laser generated by dimers closely resemble a normal distribution. This finding demonstrates the feasibility of producing high-quality random number sequences.

Optics Express•Apr 29, 2024•2 citations

Mathematical Modeling and Experimental Verification of Resonance Energy Transfer Networks: Applications in Cryptography and Biological Sensing

Vishwa Nellore

FRET between pairs of fluorophores is widely used as a biological assay. However, the properties of larger fluorophore networks are poorly understood and their application space has not yet been fully explored. This dissertation introduces DNA self-assembled FÖrster Resonance Energy Transfer (FRET) networks that provide a unique optical output when probed by a series of light pulses. We create a Markov model of the FRET networks and analyze over 1200 time-resolved fluorescence measurements on 300 prototypical networks. Our results show that the optical responses of FRET networks are highly repeatable and minor variations between the FRET networks can be discriminated resulting in a total of 10375 unique responses. These results are used in the following breakthrough applications: 1. Unclonable Cryptographic Key for Secure Authentication and Communication Modern authentication protocols rely on an asymmetry in the effort required by a legitimate user and an adversary to accurately decrypt an encoded message. These protocols ensure that communication between legitimate users is possible in polynomial time using a private key but a user without access to the exact key cannot compute the function using a probabilistic polynomial-time algorithm. Private-key cryptographic techniques currently employ physical keys based on algorithmic one-way functions, which are conjectured mathematical objects that are easy to compute but difficult to invert. Well-known examples of such one-way functions include the RSA and the Rabin functions. Although algorithmic one-way functions are widely used for authentication, their reliance on computational difficulty to provide security implies that they are not protected against future advances in computational capacity or speed. Also, use of a highly parallel network of conventional computers could potentially reverse engineer a key from the challenge-response pairs used in past communications. The key may also be obtained by duplicating the device. Most of the current physical embodiments of algorithmic one-way functions come with a tamper resistant packaging but remain vulnerable to sophisticated attacks. We develop a RET based physical key to overcome the limitations of conventional security keys. The key exploits resonance energy transfer between a network of fluorophores placed on a nanostructure. The fluorophores provide a unique, unpredictable output when probed by a series of light pulses of specific wavelengths and delays. A critical advantage of the RET key over existing keys is that the manufacturing process allows two identical devices to be produced allowing us to exploit the advantages of symmetric key encryption, for the first time, without the need to physically transfer the device between the two communicating parties. It is infeasible to model, characterize or replicate our key using modern cryptographic attacks including unfettered physical access to the device. This is because of the difficulty in characterizing the nanoscale structure and the large number of challenge-response pairs achievable for each key. Atomic force microscopy and time -resolved fluorescence measurements are performed to characterize the nanoscale structures. From over 1200 measurements on 300 prototypical keys, we estimate that a legitimate user would have a computational advantage of 10340 years over an attacker even if the attacker uses all the computational resources available in the world. Thus, the computational advantage of our key ensures perfect theoretical security for the foreseeable future. We provide an authentication protocol for use of the key and demonstrate that legitimate users are successfully authenticated 99.48% of the time with two trials. 2. Multiplexed Fluorescence Sensor for Cancer Detection Fluorescence microscopy is one of the most widely used assays in biological systems. However, the technique suffers from limited multiplexing capability with previous attempts at detecting more than 11 fluorophores simultaneously resulting in barcodes that are too big for in vivo analysis, expensive and involve time-consuming detection schemes. Here, we introduce DNA self-assembled FRET networks that provide a unique, optical output when probed by a series of light pulses. Markov and entropy modeling of the nanoscale FRET sensors show that 125 fluorophores can be observed simultaneously. Furthermore, experimental analyses of over 1200 time-resolved fluorescence signatures show that the optical responses are repeatable 99.48% of the time and that minor variations between FRET networks can be discriminated resulting in a total of 10375 unique responses. This enormous increase in spatial information density enabled by FRET networks allowed us to identify molecular signatures in lung and breast cancer tumors. It is now known that the presence of aberrant DNA/RNA secondary structure in the regulatory regions of genes involved in cell proliferation, cells growth and apoptosis can lead to cancer. The FRET sensor we designed, self-assembles DNA probes labeled with acceptor fluorophores to the target DNA/RNA secondary structure forming an optical network. A DNA strand labeled with a donor fluorophore triplex binds to a unique sequence adjacent to the secondary structure. When the donor fluorophore is excited, the optical network results in a different optical signal based on the presence of the wild-type or the aberrant secondary structure, through which we identified lung and breast cancer cells with high specificity and over 99.9% repeatability. The small size of fluorophores results in molecular scale spatial resolution while the optical sensing mechanism enables in vitro and in vivo characterization of the structure at picosecond resolution.

•Jan 1, 2014•0 citations

Topological Anderson Random Laser

Hang-Zheng Shen, Xian-Hao Wei, Xi-Wang Luo +1 more

Topological lasers and random lasers embody two contrasting strategies for disorder management in photonics: the former suppresses disorder via protected edge transport, while the latter exploits multiple scattering for feedback. Here, we theoretically demonstrate that these seemingly incompatible paradigms can be unified through a topological Anderson random laser (TARL), where disorder itself induces a topological phase that enables robust lasing. Starting from a trivial photonic lattice, we show that engineered disorder drives the system into a topological Anderson insulator regime, generating emergent chiral edge states that serve as boundary-selective lasing channels. Remarkably, the TARL exhibits rapid mode selection toward a single edge state, producing an ultranarrow emission spectrum and enhanced slope efficiency optimized near disorder strength with maximal topological mobility gap. Furthermore, they exhibit single-mode-like coherence properties, deviating from Kardar-Parisi-Zhang behavior in conventional chiral topological lasers, while remaining significantly more robust against local perturbations than conventional random lasers. Our findings establish a disorder-enabled flexible route to topologically protected single-mode lasing and introduce a fundamentally new design principle for robust, high-coherence photonic light sources.

physics.opticsCross-listedarXiv:2604.02364•Mar 24, 2026

Coherent fluorescence resonance energy transfer between two dipoles: Full quantum electrodynamics approach

В. В. Климов, Sergey K. Sekatskii, Giovanni Dietler

The quantum electrodynamical theory of coherent fluorescence resonance energy transfer (FRET) between two dipoles (free atoms, molecules or dopant centres in crystalline matrices at low temperature conditions) in an arbitrary non-dissipative environment is elaborated using a canonical quantization scheme. It is shown that population dynamics of both atoms can be expressed in terms of a classical Green function. This general theory corresponds well to the problem of description of controllable quantum manipulations under the donor-acceptor system (e.g. its application for FRET scanning near-field optical microscopy-based quantum computing). In addition, its usefulness is illustrated for the case of coherent FRET in free space and for the case when atoms are placed near an ideally conducting plane. The possibility of creating an entangled state of three atoms is demonstrated.

Journal of Modern Optics•May 8, 2004•11 citations
Fȍrster resonance energy transfer (FRET) is a fundamental approach for fabricating widely tunable (≥100 nm) random lasers and cascaded ones, which are the fundamental direction for achieving applications breakthroughs of random lasers in multi-fields, such as speckle-free imaging and biosensing. However, it is challenging to realize due to a lack of method to investigate the emission mechanism and emission characteristics of FRET-assisted random laser. In this work, the replica symmetry breaking and the Lévy flight are introduced to investigate the dynamical emission mechanism of FRET-assisted random laser. It is revealed that FRET can induce the disorder in random laser to frustrate coherently oscillating modes, resulting in a non-trivial interaction between the modes, which generates discrete emission field. This emission field exhibits low spatiotemporal coherence, which is essential for using random laser in super-resolution spectroscopy and even photolithography. Meanwhile, the phase diagram of dynamics during the FRET is derived to reveal the dynamical evolution of the interaction between random laser modes during FRET, which illustrates how FRET influences the emissions properties of random laser. This work broadens not only the approach for exploring order physical principles in disorder random laser based on statistical analysis methods, but also provides the theoretical support for the design of complex energy level random lasers with special application properties.
We report high time-resolution measurements of photon statistics from pairs of dye molecules coupled by fluorescence resonance energy transfer (FRET). In addition to quantum-optical photon antibunching, we observe photon bunching on a time scale of several nanoseconds. We show by numerical simulation that configuration fluctuations in the coupled fluorophore system could account for minor deviations of our data from predictions of basic Förster theory. With further characterization we believe that FRET photon statistics could provide a unique tool for studying DNA mechanics on time scales from 10(-9)-10(-3) s.
The spatial formation of coherent random laser modes in strongly scattering disordered random media is a central feature in the understanding of the physics of random lasers. We derive a quantum field theoretical method for random lasing in disordered samples of complex amplifying Mie resonators which is able to provide self-consistently and free of any fit parameter the full set of transport characteristics at and above the laser phase transition. The coherence length and the correlation volume respectively is derived as an experimentally measurable scale of the phase transition at the laser threshold. We find that the process of stimulated emission in extended disordered arrangements of active Mie resonators is ultimately connected to time-reversal symmetric multiple scattering in the sense of photonic transport while the diffusion coefficient is finite. A power law is found for the random laser mode diameters in stationary state with increasing pump intensity.
Besides the scattering structures, the energy transfer (ET) process in the gain medium plays a significant role in the competition between coherent (comprising strongly coherent components) and incoherent (consisting of weakly coherent or "hidden" coherent components) modes of random lasers. In this study, bichromatic emission random lasers were successfully created using polydimethylsiloxane (PDMS) replicas with grooved structures that imitate the inner surface of abalone shells as scattering substrates. The influence mechanism of the ET process from the monomer to dimer in the Rhodamine 640 dye on the competition of random laser modes was thoroughly investigated from both spectral and temporal dimensions. It was confirmed that the ET process can reduce the gain of monomers while amplifying the gain of dimers. By considering the dominant high-efficiency ET processes, an energy transfer factor associated with the pump energy density was determined. Notably, for the first time, it was validated that the statistical distribution characteristics of the time sequence variations in the coherent random laser generated by dimers closely resemble a normal distribution. This finding demonstrates the feasibility of producing high-quality random number sequences.
FRET between pairs of fluorophores is widely used as a biological assay. However, the properties of larger fluorophore networks are poorly understood and their application space has not yet been fully explored. This dissertation introduces DNA self-assembled FÖrster Resonance Energy Transfer (FRET) networks that provide a unique optical output when probed by a series of light pulses. We create a Markov model of the FRET networks and analyze over 1200 time-resolved fluorescence measurements on 300 prototypical networks. Our results show that the optical responses of FRET networks are highly repeatable and minor variations between the FRET networks can be discriminated resulting in a total of 10375 unique responses. These results are used in the following breakthrough applications: 1. Unclonable Cryptographic Key for Secure Authentication and Communication Modern authentication protocols rely on an asymmetry in the effort required by a legitimate user and an adversary to accurately decrypt an encoded message. These protocols ensure that communication between legitimate users is possible in polynomial time using a private key but a user without access to the exact key cannot compute the function using a probabilistic polynomial-time algorithm. Private-key cryptographic techniques currently employ physical keys based on algorithmic one-way functions, which are conjectured mathematical objects that are easy to compute but difficult to invert. Well-known examples of such one-way functions include the RSA and the Rabin functions. Although algorithmic one-way functions are widely used for authentication, their reliance on computational difficulty to provide security implies that they are not protected against future advances in computational capacity or speed. Also, use of a highly parallel network of conventional computers could potentially reverse engineer a key from the challenge-response pairs used in past communications. The key may also be obtained by duplicating the device. Most of the current physical embodiments of algorithmic one-way functions come with a tamper resistant packaging but remain vulnerable to sophisticated attacks. We develop a RET based physical key to overcome the limitations of conventional security keys. The key exploits resonance energy transfer between a network of fluorophores placed on a nanostructure. The fluorophores provide a unique, unpredictable output when probed by a series of light pulses of specific wavelengths and delays. A critical advantage of the RET key over existing keys is that the manufacturing process allows two identical devices to be produced allowing us to exploit the advantages of symmetric key encryption, for the first time, without the need to physically transfer the device between the two communicating parties. It is infeasible to model, characterize or replicate our key using modern cryptographic attacks including unfettered physical access to the device. This is because of the difficulty in characterizing the nanoscale structure and the large number of challenge-response pairs achievable for each key. Atomic force microscopy and time -resolved fluorescence measurements are performed to characterize the nanoscale structures. From over 1200 measurements on 300 prototypical keys, we estimate that a legitimate user would have a computational advantage of 10340 years over an attacker even if the attacker uses all the computational resources available in the world. Thus, the computational advantage of our key ensures perfect theoretical security for the foreseeable future. We provide an authentication protocol for use of the key and demonstrate that legitimate users are successfully authenticated 99.48% of the time with two trials. 2. Multiplexed Fluorescence Sensor for Cancer Detection Fluorescence microscopy is one of the most widely used assays in biological systems. However, the technique suffers from limited multiplexing capability with previous attempts at detecting more than 11 fluorophores simultaneously resulting in barcodes that are too big for in vivo analysis, expensive and involve time-consuming detection schemes. Here, we introduce DNA self-assembled FRET networks that provide a unique, optical output when probed by a series of light pulses. Markov and entropy modeling of the nanoscale FRET sensors show that 125 fluorophores can be observed simultaneously. Furthermore, experimental analyses of over 1200 time-resolved fluorescence signatures show that the optical responses are repeatable 99.48% of the time and that minor variations between FRET networks can be discriminated resulting in a total of 10375 unique responses. This enormous increase in spatial information density enabled by FRET networks allowed us to identify molecular signatures in lung and breast cancer tumors. It is now known that the presence of aberrant DNA/RNA secondary structure in the regulatory regions of genes involved in cell proliferation, cells growth and apoptosis can lead to cancer. The FRET sensor we designed, self-assembles DNA probes labeled with acceptor fluorophores to the target DNA/RNA secondary structure forming an optical network. A DNA strand labeled with a donor fluorophore triplex binds to a unique sequence adjacent to the secondary structure. When the donor fluorophore is excited, the optical network results in a different optical signal based on the presence of the wild-type or the aberrant secondary structure, through which we identified lung and breast cancer cells with high specificity and over 99.9% repeatability. The small size of fluorophores results in molecular scale spatial resolution while the optical sensing mechanism enables in vitro and in vivo characterization of the structure at picosecond resolution.
Topological lasers and random lasers embody two contrasting strategies for disorder management in photonics: the former suppresses disorder via protected edge transport, while the latter exploits multiple scattering for feedback. Here, we theoretically demonstrate that these seemingly incompatible paradigms can be unified through a topological Anderson random laser (TARL), where disorder itself induces a topological phase that enables robust lasing. Starting from a trivial photonic lattice, we show that engineered disorder drives the system into a topological Anderson insulator regime, generating emergent chiral edge states that serve as boundary-selective lasing channels. Remarkably, the TARL exhibits rapid mode selection toward a single edge state, producing an ultranarrow emission spectrum and enhanced slope efficiency optimized near disorder strength with maximal topological mobility gap. Furthermore, they exhibit single-mode-like coherence properties, deviating from Kardar-Parisi-Zhang behavior in conventional chiral topological lasers, while remaining significantly more robust against local perturbations than conventional random lasers. Our findings establish a disorder-enabled flexible route to topologically protected single-mode lasing and introduce a fundamentally new design principle for robust, high-coherence photonic light sources.
The quantum electrodynamical theory of coherent fluorescence resonance energy transfer (FRET) between two dipoles (free atoms, molecules or dopant centres in crystalline matrices at low temperature conditions) in an arbitrary non-dissipative environment is elaborated using a canonical quantization scheme. It is shown that population dynamics of both atoms can be expressed in terms of a classical Green function. This general theory corresponds well to the problem of description of controllable quantum manipulations under the donor-acceptor system (e.g. its application for FRET scanning near-field optical microscopy-based quantum computing). In addition, its usefulness is illustrated for the case of coherent FRET in free space and for the case when atoms are placed near an ideally conducting plane. The possibility of creating an entangled state of three atoms is demonstrated.