arXiv subjects

Ajay Ram Srimath Kandada

Publications and source records attributed to Ajay Ram Srimath Kandada.

35 records · Page 2Linked to original sources

arXiv2020

Stochastic scattering theory for excitation induced dephasing: Time-dependent nonlinear coherent exciton lineshapes

We develop a stochastic theory that treats time-dependent exciton-exciton s-wave scattering and that accounts for dynamic Coulomb screening, which we describe within a mean-field limit. With this theory, we model excitation-induced dephasing effects on time-resolved two-dimensional coherent optical lineshapes and we identify a number of features that can be attributed to the many-body dynamics occurring in the background of the exciton, including dynamic line narrowing, mixing of real and imaginary spectral components, and multi-quantum states. We test the model by means of multidimensional coherent spectroscopy on a two-dimensional metal-halide semiconductor that hosts tightly bound excitons and biexcitons that feature strong polaronic character. We find that the exciton nonlinear coherent lineshape reflects many-body correlations that give rise to excitation-induced dephasing. Furthermore, we observe that the exciton lineshape evolves with population time over time windows in which the population itself is static, in a manner that reveals the evolution of the multi-exciton many-body couplings. Specifically, the dephasing dynamics slow down with time, at a rate that is governed by the strength of exciton many-body interactions and on the dynamic Coulomb screening potential. The real part of the coherent optical lineshape displays strong dispersive character at zero time, which transforms to an absorptive lineshape on the dissipation timescale of excitation-induced dephasing effects, while the imaginary part displays converse behavior. Our microscopic theoretical approach is sufficiently flexible to allow for a wide exploration of how system-bath dynamics contribute to linear and non-linear time-resolved spectral behavior.

physics.chem-ph↗

arXiv2020

Stochastic scattering theory for excitation induced dephasing: Comparison to the Anderson-Kubo lineshape

In this paper we present a quantum stochastic model for spectroscopic line-shapes in the presence of a co-evolving and non-stationary background population of excitations. Starting from a field theory description for interacting bosonic excitons, we derive a reduced model whereby optical excitons are coupled to an incoherent background via scattering as mediated by their screened Coulomb coupling. The Heisenberg equations of motion for the optical excitons are then driven by an auxiliary stochastic population variable, which we take to be the solution of an Ornstein-Uhlenbeck process. Itô's Lemma then allows us to easily construct and evaluate correlation functions and response functions. Focusing on the linear response, we compare our model to the classic Anderson-Kubo model. While similar in motivation, there are profound differences in the predicted lineshapes, notably in terms of asymmetry, and variation with increasing background population.

physics.chem-ph↗

arXiv2020

Exciton-polaron spectral structures in two dimensional hybrid lead-halide perovskites

Owing to both electronic and dielectric confinement effects, two-dimensional organic-inorganic hybrid perovskites sustain strongly bound excitons at room temperature. Here, we demonstrate that there are non-negligible contributions to the excitonic correlations that are specific to the lattice structure and its polar fluctuations, both of which are controlled via the chemical nature of the organic counter-cation. We present a phenomenological, yet quantitative framework to simulate excitonic absorption lineshapes in single-layer organic-inorganic hybrid perovskites, based on the two-dimensional Wannier formalism. We include four distinct excitonic states separated by $35\pm5$\,meV, and additional vibronic progressions. Intriguingly, the associated Huang-Rhys factors and the relevant phonon energies show substantial variation with temperature and the nature of the organic cation. This points to the hybrid nature of the lineshape, with a form well described by a Wannier formalism, but with signatures of strong coupling to localized vibrations, and polaronic effects perceived through excitonic correlations. Our work highlights the complexity of excitonic properties in this class of nanostructured materials.

cond-mat.mtrl-sci↗

arXiv2020

Probing exciton/exciton interactions with entangled photons: theory

Quantum entangled photons provide a sensitive probe of many-body interactions and offer an unique experimental portal for quantifying many-body correlations in a material system. In this paper, we present a theoretical demonstration of how photon-photon entanglement can be generated via interactions between coupled qubits. Here we develop a model for the scattering of an entangled pair of photons from a molecular dimer. We develop a diagrammatic theory for the scattering matrix and show that one can correlate the von Neumann entropy of the outgoing bi-photon wave function to exciton exchange and repulsion interactions. We conclude by discussing possible experimental scenarios for realizing these ideas.

quant-ph↗

arXiv2019

Quantum process tomography of entangled photons as a probe of intermediates of singlet fission in a tetracene derivative

Spin-entaglement has been proposed and extensively used in the case of correlated triplet pairs which are intermediate states in singlet fission process in select organic semiconductors. Here, we employ quantum process tomography of polarization entangled photon-pairs resonant with the excited state absorption of these states to investigate the nature of the inherent quantum correlations and to explore for an unambiguous proof for the existence of exciton entanglement.

physics.chem-ph↗

arXiv2019

Perspective: Exciton polarons in two-dimensional hybrid metal-halide perovskites

While polarons --- charges bound to a lattice deformation induced by electron-phonon coupling --- are primary photoexcitations at room temperature in bulk metal-halide hybrid organic-inorganic perovskites (HOIP), excitons --- Coulomb-bound el\-ectron-hole pairs --- are the stable quasi-particles in their two-dimensional (2D) analogues. Here we address the fundamental question: are polaronic effects consequential for excitons in 2D-HIOPs? Based on our recent work, we argue that polaronic effects are manifested intrinsically in the exciton spectral structure, which is comprised of multiple non-degenerate resonances with constant inter-peak energy spacing. We highlight our own measurements of population and dephasing dynamics that point to the apparently deterministic role of polaronic effects in excitonic properties. We contend that an interplay of long-range and short-range exciton-lattice couplings give rise to exciton polarons, a character that fundamentally establishes their effective mass and radius, and consequently, their quantum dynamics. Finally, we highlight opportunities for the community to develop the rigorous description of exciton polarons in 2D-HIOPs to advance their fundamental understanding as model systems for condensed-phase materials in which lattice-mediated correlations are fundamental to their physical properties.

cond-mat.mtrl-sci↗

arXiv2019

Electron-phonon couplings inherent in polarons drive exciton dynamics in two-dimensional metal-halide perovskites

We report on the exciton formation and relaxation dynamics following photocarrier injection in a single-layer two-dimensional lead-iodide perovskite. We probe the time evolution of four distinct exciton resonances by means of time-resolved photoluminescence and transient absorption spectroscopies, and find that at 5\,K a subset of excitons form on a $\lesssim$ 1-ps timescale, and that these relax subsequently to lower-energy excitons on $\sim$ 5--10\,ps with a marked temperature dependence over $<$ 100\,K. We implement a mode projection analysis that determines the relative contribution of all observed phonons with frequency $\leq$50\,cm$^{-1}$ to inter-exciton nonadiabatic coupling, which in turn determines the rate of exciton relaxation. This analysis ranks the relative contribution of the phonons that participate in polaronic lattice distortions to the exciton inter-conversion dynamics and thus establishes their role in the nonadiabatic mixing of exciton states, and this in the exciton relaxation rate.

cond-mat.mtrl-sci↗

arXiv2019

Phonon coherences reveal the polaronic character of excitons in two-dimensional lead-halide perovskites

Hybrid organic-inorganic semiconductors feature complex lattice dynamics due to the ionic character of the crystal and the softness arising from non-covalent bonds between molecular moieties and the inorganic network. Here we establish that such dynamic structural complexity in a prototypical two-dimensional lead iodide perovskite gives rise to the coexistence of diverse excitonic resonances, each with a distinct degree of polaronic character. By means of high-resolution resonant impulsive stimulated Raman spectroscopy, we identify vibrational wavepacket dynamics that evolve along different configurational coordinates for distinct excitons and photocarriers. Employing density functional theory calculations, we assign the observed coherent vibrational modes to various low-frequency ($\lesssim 50$\,cm$^{-1}$) optical phonons involving motion in the lead-iodide layers. We thus conclude that different excitons induce specific lattice reorganizations, which are signatures of polaronic binding. This insight on the energetic/configurational landscape involving globally neutral primary photoexcitations may be relevant to a broader class of emerging hybrid semiconductor materials.

cond-mat.mtrl-sci↗

arXiv2019

Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites

In two-dimensional hybrid organic-inorganic metal-halide perovskites, the intrinsic optical lineshape reflects multiple excitons with distinct binding energies, each dressed differently by the hybrid lattice. Given this complexity, a fundamentally far-reaching issue is how Coulomb-mediated many-body interactions --- elastic scattering such as excitation-induced dephasing, inelastic exciton bimolecular scattering, and multi-exciton binding --- depend upon the specific exciton-lattice coupling. We report the intrinsic and density-dependent exciton pure dephasing rates and their dependence on temperature by means of a coherent nonlinear spectroscopy. We find exceptionally strong screening effects on multi-exciton scattering relative to other two-dimensional single-atomic-layer semiconductors. Importantly, the exciton-density dependence of the dephasing rates is markedly different for distinct excitons. These findings establish the consequences of particular lattice dressing on exciton many-body quantum dynamics, which critically define fundamental optical properties that underpin photonics and quantum optoelectronics in relevant exciton density regimes.

cond-mat.mtrl-sci↗

arXiv2018

Lattice vibrations and dynamic disorder in two-dimensional hybrid lead-halide perovskites

By means of non-resonant Raman spectroscopy and density functional theory calculations, we measure and assign the vibrational spectrum of two distinct two-dimensional lead-iodide perovskite derivatives. These two samples are selected in order to probe the effects of the organic cation on lattice dynamics. One templating cation is composed of a phenyl-substituted ammonium derivative, while the other contains a linear alkyl group. We find that modes that directly involve the organic cation are more prevalent in the phenyl-substituted derivative. Comparison of the temperature dependence of the Raman spectra reveals differences in the nature of dynamic disorder, with a strong dependence on the molecular nature of the organic moiety.

cond-mat.mtrl-sci↗

arXiv2018

Photon entanglement entropy as a probe of many-body correlations and fluctuations

Recent theoretical and experiments have explored the use of entangled photons as a spectroscopic probe of material systems. We develop here a theoretical description for entropy production in the scattering of an entangled biphoton state within an optical cavity. We develop this using perturbation theory by expanding the biphoton scattering matrix in terms of single-photon terms in which we introduce the photon-photon interaction via a complex coupling constant, $ξ$. We show that the von Neumann entropy provides a succinct measure of this interaction. We then develop a microscopic model and show that in the limit of fast fluctuations, the entanglement entropy vanishes whereas in the limit the coupling is homogeneous broadened, the entanglement entropy depends upon the magnitude of the fluctuations and reaches a maximum.

quant-ph↗

arXiv2018

Stable biexcitons in two-dimensional metal-halide perovskites with strong dynamic lattice disorder

With strongly bound and stable excitons at room temperature, single-layer, two-dimensional organic-inorganic hybrid perovskites are viable semiconductors for light-emitting quantum optoelectronics applications. In such a technological context, it is imperative to comprehensively explore all the factors --- chemical, electronic and structural --- that govern strong multi-exciton correlations. Here, by means of two-dimensional coherent spectroscopy, we examine excitonic many-body effects in pure, single-layer (PEA)$_2$PbI$_4$ (PEA = phenylethylammonium). We determine the binding energy of biexcitons --- correlated two-electron, two-hole quasiparticles --- to be $44 \pm 5$\,meV at room temperature. The extraordinarily high values are similar to those reported in other strongly excitonic two-dimensional materials such as transition-metal dichalchogenides. Importantly, we show that this binding energy increases by $\sim25$\% upon cooling to 5\,K. Our work highlights the importance of multi-exciton correlations in this class of technologically promising, solution-processable materials, in spite of the strong effects of lattice fluctuations and dynamic disorder.

cond-mat.mtrl-sci↗

arXiv2017

Probing dynamical symmetry breaking using quantum-entangled photons

We present an input/output analysis of photon-correlation experiments whereby a quantum mechanically entangled bi-photon state interacts with a material sample placed in one arm of a Hong-Ou-Mandel (HOM) apparatus. We show that the output signal contains detailed information about subsequent entanglement with the microscopic quantum states in the sample. In particular, we apply the method to an ensemble of emitters interacting with a common photon mode within the open-system Dicke Model. Our results indicate considerable dynamical information concerning spontaneous symmetry breaking can be revealed with such an experimental system.

quant-ph↗

arXiv2017

Incoherent population mixing contributions to phase-modulation two-dimensional coherent excitation spectra

We present theoretical and experimental results showing the effects of incoherent population mixing on two-dimensional (2D) coherent excitation spectra that are measured via a time-integrated population and phase-sensitive detection. The technique uses four collinear ultrashort pulses and phase modulation to acquire two-dimensional spectra by isolating specific nonlinear contributions to the photoluminescence or photocurrent excitation signal. We demonstrate that an incoherent contribution to the measured lineshape, arising from nonlinear population dynamics over the entire photoexcitation lifetime, generates a similar lineshape to the expected 2D coherent spectra in condensed-phase systems. In those systems, photoexcitations are mobile such that inter-particle interactions are important on any timescale, including those long compared to the 2D coherent experiment. Measurements on a semicrystalline polymeric semiconductor film at low temperature show that, in some conditions in which multi-exciton interactions are suppressed, the technique predominantly detects coherent signal and can be used, in our example, to extract homogeneous linewidths. The same method used on a lead-halide perovskite photovoltaic cell shows that incoherent population mixing of mobile photocarriers can dominate the measured signal since carrier-carrier bimolecular scattering is active even at low excitation densities, which hides the coherent contribution to the spectral lineshape.

cond-mat.mtrl-sci↗

arXiv2017

Integrated perovskite lasers on silicon nitride waveguide platform by cost-effective high throughput fabrication

Metal-halide perovskites are a class of solution processed materials with remarkable optoelectronic properties such as high photoluminescence quantum yields and long carrier lifetimes, which makes them promising for a wide range of efficient photonic devices. In this work, we demonstrate the first successful integration of a perovskite laser onto a silicon nitride photonic chip. High throughput, low cost optical lithography is used followed by indirect structuring of the perovskite waveguide. We embed methylammonium lead tri-iodide (MAPbI3) in a pre-patterned race-track microresonator and couple the emitted light to an integrated photonic waveguide. We clearly observe the build-up of spectrally narrow lasing modes at room temperature upon a pump threshold fluence of $19.6 μJcm^{-2}$. Our results evidence the possibility of on-chip lasers based on metal-halide perovskites with industry relevance on a commercially available dielectric photonic platform, which is a step forward towards low-cost integrated photonic devices.

physics.optics↗

arXiv2017

Probing Femtosecond Lattice Displacement upon Photo-carrier generation in Lead Halide Perovskite

Electronic properties and lattice vibrations are supposed to be strongly correlated in metal-halide perovskites, due to the "soft" fluctuating nature of their crystal lattice. Thus, unveiling electron-phonon coupling dynamics upon ultra-fast photoexcitation is necessary for understanding the optoelectronic behaviour of the semiconductor. Here, we use impulsive vibrational spectroscopy to reveal ground and excited state vibrational modes of methylammonium lead-bromide perovskite. We observe a coherent phonon at 106 cm-1 (13 meV), pertaining to the inorganic octahedral, which is peculiar of the electronic excited state and generated via displacive excitation mechanism. This indicates the formation of a new geometry, reached after a quarter of the phonon period T/4=80 fs, and fully equilibrated within the phonon lifetime of about 1 ps. Our observations unambiguously prove that this mode drives the crystalline distortion occurring upon carrier generation, implying the presence of polaronic effects.

cond-mat.mtrl-sci↗

arXiv2013

Plasmonics in heavily-doped semiconductor nanocrystals

Heavily-doped semiconductor nanocrystals characterized by a tunable plasmonic band have been gaining increasing attention recently. Herein, we introduce this type of materials focusing on their structural and photo physical properties. Beside their continuous-wave plasmonic response, depicted both theoretically and experimentally, we also review recent results on their transient, ultrafast response. This was successfully interpreted by adapting models of the ultrafast response of gold nanoparticles.

cond-mat.mes-hall↗