Quantitative line shape analysis for arbitrary inhomogeneity in two-dimensional coherent spectroscopy Bhaskar De, Pradeep Kumar, Krishna K. Maurya, Rishabh Tripathi, Rohan Singh Optics Letters, 2025 Two-dimensional coherent spectroscopy (2DCS) provides simultaneous measurement of homogeneous and inhomogeneous linewidths through quantitative line shape analysis. However, conventional line shape analysis methods assume Gaussian inhomogeneity, limiting its applicability to systems with non-Gaussian inhomogeneity. We present a quantitative line shape analysis method incorporating arbitrary inhomogeneity using a bivariate spectral distribution function in 2DCS simulations. An algorithm is developed to extract the homogeneous linewidth and arbitrary inhomogeneous distribution from an experimentally measured 2D spectrum. We demonstrate this framework for a quantum-well (QW)-exciton resonance with non-Gaussian inhomogeneity. This work broadens the scope of quantitative line shape analysis for studying materials with non-Gaussian inhomogeneity.
Coherent nonlinear optical response for high-intensity excitation Rishabh Tripathi, Krishna K. Maurya, Pradeep Kumar, Bhaskar De, Rohan Singh Journal of Chemical Physics, 2025 The calculation of the coherent nonlinear response of a system is essential to correctly interpret results from advanced techniques such as two-dimensional coherent spectroscopy. Usually, even for the simplest systems, such calculations are either performed for low-intensity excitations where perturbative methods are valid and/or by assuming a simplified pulse envelope, such as a δ-function in time. Here, we use the phase-cycling method for the exact calculation of the nonlinear response without making the aforementioned approximations even for high-intensity excitation. We compare the simulation results to several experimental observations to prove the validity of these calculations. The saturation of the photon-echo signal from excitons in a semiconductor quantum well sample is measured. The excitation-intensity dependent measurement shows nonlinear contributions up to twelfth order. Intensity-dependent simulations reproduce this effect without explicitly considering higher-order interactions. In addition, we present simulation results that replicate previously reported experiments with high-intensity excitation of semiconductor quantum dots. By accurately reproducing a variety of phenomena such as higher-order contributions, switching of coherent signals, and changes in photon-echo transients, we prove the efficacy of the phase-cycling method to calculate the coherent nonlinear signal for high-intensity excitation. This method would be particularly useful for systems with multiple, well-separated peaks and/or large inhomogeneities.
Two-Dimensional Coherent Spectroscopy with Arbitrary Inhomogeneous Broadening: Simulations and Analysis Bhaskar De, Krishna K. Maurya, Rishabh Tripathi, Pradeep Kumar, Rohan Singh CLEO Science and Innovations Proceedings CLEO 2025, 2025 We present two-dimensional coherent spectroscopy simulations for arbitrary inhomogeneity. We demonstrate a quantitative fitting procedure, based on these simulations, to extract the homogeneous broadening and non-Gaussian inhomogeneous distribution of excitons in GaAs semiconductor quantum wells.
Two-Dimensional Coherent Spectroscopy with Arbitrary Inhomogeneous Broadening: Simulations and Analysis Bhaskar De, Krishna K. Maurya, Rishabh Tripathi, Pradeep Kumar, Rohan Singh CLEO Fundamental Science Proceedings CLEO 2025, 2025 We present two-dimensional coherent spectroscopy simulations for arbitrary inhomogeneity. We demonstrate a quantitative fitting procedure, based on these simulations, to extract the homogeneous broadening and non-Gaussian inhomogeneous distribution of excitons in GaAs semiconductor quantum wells.
Phase Cycling Beyond Perturbative Limits: Exact Solutions for Nonlinear Response Rishabh Tripathi, Krishna K. Maurya, Pradeep Kumar, Bhaskar De, Rohan Singh Laser Science Proceedings Frontiers in Optics Laser Science 2025, 2025 We present exact simulations of nonlinear optical signals under high-intensity excitation using phase-cycling, validating with experiments and showing accurate modeling beyond perturbative limits without pulse shape or order truncations.
Two- Dimensional Coherent Spectroscopy with Arbitrary Inhomogeneous Broadening: Simulations and Analysis Bhaskar De, Krishna K. Maurya, Rishabh Tripathi, Pradeep Kumar, Rohan Singh 2025 Conference on Lasers and Electro Optics CLEO 2025, 2025 We present two-dimensional coherent spectroscopy simulations for arbitrary inhomogeneity. We demonstrate a quantitative fitting procedure, based on these simulations, to extract the homogeneous broadening and non-Gaussian inhomogeneous distribution of excitons in GaAs semiconductor quantum wells.
Phase Cycling Beyond Perturbative Limits: Exact Solutions for Nonlinear Response Rishabh Tripathi, Krishna K. Maurya, Pradeep Kumar, Bhaskar De, Rohan Singh Frontiers in Optics Fio 2025 in Proceedings Frontiers in Optics Laser Science 2025 Fio Ls Part of Frontiers in Optics Laser Science 2025, 2025 We present exact simulations of nonlinear optical signals under high-intensity excitation using phase-cycling, validating with experiments and showing accurate modeling beyond perturbative limits without pulse shape or order truncations.
Two-Dimensional Coherent Spectroscopy Simulations with Arbitrary Inhomogeneous Distribution Conference on Lasers and Electro Optics Pacific Rim CLEO PR 2024 in Proceedings 2024 Conference on Lasers and Electro Optics Pacific Rim CLEO PR, 2024
Coherent Control through High-Intensity Excitation: A Simulation of Two-Dimensional Coherent Spectroscopy Conference on Lasers and Electro Optics Pacific Rim CLEO PR 2024 in Proceedings 2024 Conference on Lasers and Electro Optics Pacific Rim CLEO PR, 2024
A Quantitative Study of Excitonic Interactions Using Phenomenological Models Conference on Lasers and Electro Optics Pacific Rim CLEO PR 2024 in Proceedings 2024 Conference on Lasers and Electro Optics Pacific Rim CLEO PR, 2024
Coherent Evolution of Inhomogeneous Exciton/Biexciton System in an InAs Quantum Dot Ensemble Optics Infobase Conference Papers, 2016
Many-body Effects and the Role of Indirect Excitons in Asymmetric InGaAs/GaAs Double Quantum Wells Optics Infobase Conference Papers, 2016
Many-body interactions between excitons in GaAs quantum wells quantified using two-dimensional coherent spectroscopy Conference on Lasers and Electro Optics Europe Technical Digest, 2015
Two dimensional coherent spectroscopy of CdSe/ZnS colloidal quantum dots at cryogenic temperatures Conference on Lasers and Electro Optics Europe Technical Digest, 2015
Exciton-phonon interactions in an InAs quantum dot ensemble studied with 2D coherent spectroscopy Conference on Lasers and Electro Optics Europe Technical Digest, 2014
Excitonic frequency-frequency correlation functions in a gaas quantumwell CLEO QELS Fundamental Science CLEO QELS Fs 2013, 2013
Coupling in InGaAs double quantumwells studied with 2D fourier transform spectroscopy CLEO QELS Fundamental Science CLEO QELS Fs 2013, 2013
Linewidth anisotropy of the heavy hole exciton in (110)-oriented GaAs quantumwells CLEO QELS Fundamental Science CLEO QELS Fs 2013, 2013
Confinement effects on biexciton binding in semiconductor quantum dots measured with 2D coherent spectroscopy CLEO QELS Fundamental Science CLEO QELS Fs 2013, 2013
Excitons, biexcitons, and trions in an InAs quantum dot ensemble studied with 2D Fourier-transform spectroscopy 2012 Conference on Lasers and Electro Optics CLEO 2012, 2012
Coherence of fine-structure states of an InAs quantum dot ensemble studied with 2D Fourier-transform spectroscopy 2012 Conference on Lasers and Electro Optics CLEO 2012, 2012
Coherence of fine-structure states of an InAs quantum dot ensemble studied with 2D fourier-transform spectroscopy Optics Infobase Conference Papers, 2012
Evidence of exciton-trion coherent interactions in a CdTe/CdMgTe quantum well Optics Infobase Conference Papers, 2012
Spectral Tailoring of Inhomogeneous Optical Response Using Two-Dimensional Coherent Spectroscopy P Kumar, R Singh arXiv preprint arXiv:2601.05753 , 2026 2026
Phase Cycling Beyond Perturbative Limits: Exact Solutions for Nonlinear Response R Tripathi, KK Maurya, P Kumar, B De, R Singh Frontiers in Optics, JTu5A. 29 , 2025 2025
Indirect excitons and many-body interactions in InGaAs double quantum wells CL Smallwood, R Owen, MW Day, T Suzuki, R Singh, TM Autry, ... Physical Review B 112 (3), 035305 , 2025 2025
Quantitative line shape analysis for arbitrary inhomogeneity in two-dimensional coherent spectroscopy B De, P Kumar, KK Maurya, R Tripathi, R Singh Optics Letters 50 (14), 4502-4505 , 2025 2025
Excitation-Pulse Intensity Mediated Coherent Control in V-Type Systems R Tripathi, KK Maurya, R Singh arXiv preprint arXiv:2506.13371 , 2025 2025
Two-Dimensional Coherent Spectroscopy with Arbitrary Inhomogeneous Broadening: Simulations and Analysis B De, KK Maurya, R Tripathi, P Kumar, R Singh CLEO: Fundamental Science, JPS100_3 , 2025 2025
Simulating Two-Dimensional Coherent Spectroscopy with Arbitrary Inhomogeneity Beyond Gaussian Distributions B De, R Singh SMT 2025 , 2025 2025
Coherent nonlinear optical response for high-intensity excitation R Tripathi, KK Maurya, P Kumar, B De, R Singh The Journal of Chemical Physics 162 (11) , 2025 2025 Citations: 4
A Quantitative Study of Excitonic Interactions Using Phenomenological Models P Kumar, B De, R Tripathi, R Singh Conference on Lasers and Electro-Optics/Pacific Rim, P1_042 , 2024 2024
Coherent Control through High-Intensity Excitation: A Simulation of Two-Dimensional Coherent Spectroscopy R Tripathi, KK Maurya, R Singh Conference on Lasers and Electro-Optics/Pacific Rim, P1_041 , 2024 2024
Two-Dimensional Coherent Spectroscopy Simulations with Arbitrary Inhomogeneous Distribution B De, R Singh Conference on Lasers and Electro-Optics/Pacific Rim, P1_056 , 2024 2024
Exciton-exciton interaction: A quantitative comparison between complimentary phenomenological models P Kumar, B De, R Tripathi, R Singh Physical Review B 109 (15), 155423 , 2024 2024 Citations: 4
Transient Spectroscopy of Glass-Embedded Perovskite Quantum Dots: Novel Structures in an Old Wrapping R Singh Zeitschrift für Physikalische Chemie , 2023 2023
Spectroscopic insights into high defect tolerance of Zn: CuInSe 2 quantum-dot-sensitized solar cells J Du, R Singh, I Fedin, AS Fuhr, VI Klimov Nature Energy 5 (5), 409-417 , 2020 2020 Citations: 136
Coherent control of a semiconductor quantum dot ensemble T Suzuki, R Singh Semiconductors and Semimetals 105, 347-385 , 2020 2020 Citations: 1
Hot-electron dynamics in quantum dots manipulated by spin-exchange Auger interactions R Singh, W Liu, J Lim, I Robel, VI Klimov Nature nanotechnology 14 (11), 1035-1041 , 2019 2019 Citations: 66
Trap-Insensitive Quantum Dot-Sensitized Solar Cells J Du, R Singh, VI Klimov Los Alamos National Laboratory (LANL), Los Alamos, NM (United States) , 2019 2019
Dephasing of InAs quantum dot -shell excitons studied using two-dimensional coherent spectroscopy T Suzuki, R Singh, G Moody, M Aßmann, M Bayer, A Ludwig, AD Wieck, ... Physical Review B 98 (19), 195304 , 2018 2018 Citations: 10
Transient Spectroscopy of Glass-Embedded Perovskite Quantum Dots: Novel Structures in an Old Wrapping OV Kozlov, R Singh, B Ai, J Zhang, C Liu, VI Klimov Zeitschrift für Physikalische Chemie 232 (9-11), 1495-1511 , 2018 2018 Citations: 21
MOST CITED SCHOLAR PUBLICATIONS
Spectroscopic insights into high defect tolerance of Zn: CuInSe 2 quantum-dot-sensitized solar cells J Du, R Singh, I Fedin, AS Fuhr, VI Klimov Nature Energy 5 (5), 409-417 , 2020 2020 Citations: 136
Coherent Excitonic Coupling in an Asymmetric Double InGaAs Quantum Well Arises from Many-Body Effects G Nardin, G Moody, R Singh, TM Autry, H Li, F Morier-Genoud, ST Cundiff Physical Review Letters 112 (4), 046402 , 2014 2014 Citations: 89
Coherent Coupling of Excitons and Trions in a Photoexcited CdTe/CdMgTe Quantum Well G Moody, IA Akimov, H Li, R Singh, DR Yakovlev, G Karczewski, M Wiater, ... Physical Review Letters 112 (9), 097401 , 2014 2014 Citations: 72
Influence of confinement on biexciton binding in semiconductor quantum dot ensembles measured with two-dimensional spectroscopy G Moody, R Singh, H Li, IA Akimov, M Bayer, D Reuter, AD Wieck, ... Physical Review B 87 (4), 041304 , 2013 2013 Citations: 67
Hot-electron dynamics in quantum dots manipulated by spin-exchange Auger interactions R Singh, W Liu, J Lim, I Robel, VI Klimov Nature nanotechnology 14 (11), 1035-1041 , 2019 2019 Citations: 66
Fifth-order nonlinear optical response of excitonic states in an InAs quantum dot ensemble measured with two-dimensional spectroscopy G Moody, R Singh, H Li, IA Akimov, M Bayer, D Reuter, AD Wieck, ... Physical Review B 87 (4), 045313 , 2013 2013 Citations: 55
Coherent Control of the Exciton-Biexciton System in an InAs Self-Assembled Quantum Dot Ensemble T Suzuki, R Singh, M Bayer, A Ludwig, AD Wieck, ST Cundiff Physical Review Letters 117 (15), 157402 , 2016 2016 Citations: 51
Multi-dimensional coherent optical spectroscopy of semiconductor nanostructures: Collinear and non-collinear approaches G Nardin, TM Autry, G Moody, R Singh, H Li, ST Cundiff Journal of Applied Physics 117 (11), 112804 , 2015 2015 Citations: 36
Anisotropic homogeneous linewidth of the heavy-hole exciton in (110)-oriented GaAs quantum wells R Singh, TM Autry, G Nardin, G Moody, H Li, K Pierz, M Bieler, ST Cundiff Physical Review B 88 (4), 045304 , 2013 2013 Citations: 34
Correlation and dephasing effects on the non-radiative coherence between bright excitons in an InAs QD ensemble measured with 2D spectroscopy G Moody, R Singh, H Li, IA Akimov, M Bayer, D Reuter, AD Wieck, ... Solid State Communications 163, 65-69 , 2013 2013 Citations: 34
Quantifying spectral diffusion by the direct measurement of the correlation function for excitons in semiconductor quantum wells R Singh, G Moody, ME Siemens, H Li, ST Cundiff Journal of the Optical Society of America B 33 (7), C137-C143 , 2016 2016 Citations: 28
Localization dynamics of excitons in disordered semiconductor quantum wells R Singh, M Richter, G Moody, ME Siemens, H Li, ST Cundiff Physical Review B 95 (23), 235307 , 2017 2017 Citations: 22
Polarization-dependent exciton linewidth in semiconductor quantum wells: A consequence of bosonic nature of excitons R Singh, T Suzuki, TM Autry, G Moody, ME Siemens, ST Cundiff Physical Review B 94 (8), 081304 , 2016 2016 Citations: 22
Transient Spectroscopy of Glass-Embedded Perovskite Quantum Dots: Novel Structures in an Old Wrapping OV Kozlov, R Singh, B Ai, J Zhang, C Liu, VI Klimov Zeitschrift für Physikalische Chemie 232 (9-11), 1495-1511 , 2018 2018 Citations: 21
Deconvolution of optical multidimensional coherent spectra M Richter, R Singh, M Siemens, ST Cundiff Science advances 4 (6), eaar7697 , 2018 2018 Citations: 19
Detuning dependence of Rabi oscillations in an InAs self-assembled quantum dot ensemble T Suzuki, R Singh, M Bayer, A Ludwig, AD Wieck, ST Cundiff Physical Review B 97 (16), 161301 , 2018 2018 Citations: 12
Biexcitons in semiconductor quantum dot ensembles G Moody, R Singh, H Li, IA Akimov, M Bayer, D Reuter, AD Wieck, ... physica status solidi (b) 250 (9), 1753-1759 , 2013 2013 Citations: 12
Dephasing of InAs quantum dot -shell excitons studied using two-dimensional coherent spectroscopy T Suzuki, R Singh, G Moody, M Aßmann, M Bayer, A Ludwig, AD Wieck, ... Physical Review B 98 (19), 195304 , 2018 2018 Citations: 10
Coherent nonlinear optical response for high-intensity excitation R Tripathi, KK Maurya, P Kumar, B De, R Singh The Journal of Chemical Physics 162 (11) , 2025 2025 Citations: 4